WorldWideScience

Sample records for submicron aerosol composition

  1. Chemical compositions, sources and evolution processes of the submicron aerosols in Nanjing, China during wintertime

    Science.gov (United States)

    Wu, Y.; He, Y.; Ge, X.; Wang, J.; Yu, H.; Chen, M.

    2016-12-01

    Elevated atmospheric particulate matter pollution is one of the most significant environmental issues in the Yangtze River Delta (YRD), China. Thus it is important to unravel the characteristics, sources and evolution processes of the ambient aerosols in order to improve the air quality. In this study, we report the real-time monitoring results on submicron aerosol particles (PM1) in suburban Nanjing during wintertime of 2015, using an Aerodyne soot particle aerosol mass spectrometer (SP-AMS). This instrument allows the fast measurement of refractory black carbon simultaneously with other aerosol components. Results show that organics was on average the most abundant species of PM1 (25.9%), but other inorganic species, such as nitrate (23.7%) and sulfate (23.3%) also comprised large mass fractions. As the sampling site is heavily influenced by various sources including industrial, traffic and other anthropogenic emissions, etc., six organic aerosol (OA) factors were identified from Positive matrix factorization (PMF) analysis of the SP-AMS OA mass spectra. These factors include three primary OA factors - a hydrocarbon-like OA, an industry-related OA (IOA) and a cooking OA (COA), and three secondary OA factors, i.e., a local OOA (LSOA), a semi-volatile OOA (SV-OOA) and a low-volatility OOA (LV-OOA). Overall, the primary organic aerosol (POA) (HOA, IOA and COA) dominated the total OA mass. Behaviors and evolution processes of these OA factors will be discussed in combining with the other supporting data.

  2. Penetration of sub-micron aerosol droplets in composite cylindrical filtration elements

    NARCIS (Netherlands)

    Geurts, Bernardus J.; Pratte, Pascal; Stolz, S.; Stabbert, Regina; Poux, Valerie; Nordlund, Markus; Winkelmann, Christoph

    Advection–diffusion transport of aerosol droplets in composite cylindrical filtration elements is analyzed and compared to experimental data. The penetration, characterizing the fraction of droplets that passes through the pores of a filtration element, is quantified for a range of flow rates. The

  3. Variations in the chemical composition of the submicron aerosol and in the sources of the organic fraction at a regional background site of the Po Valley (Italy)

    Science.gov (United States)

    Bressi, Michael; Cavalli, Fabrizia; Belis, Claudio A.; Putaud, Jean-Philippe; Fröhlich, Roman; Martins dos Santos, Sebastiao; Petralia, Ettore; Prévôt, André S. H.; Berico, Massimo; Malaguti, Antonella; Canonaco, Francesco

    2016-10-01

    Fine particulate matter (PM) levels and resulting impacts on human health are in the Po Valley (Italy) among the highest in Europe. To build effective PM abatement strategies, it is necessary to characterize fine PM chemical composition, sources and atmospheric processes on long timescales (> months), with short time resolution (organic fraction. Although previous studies have been conducted in this region, none of them addressed all these aspects together. For the first time in the Po Valley, we investigate the chemical composition of nonrefractory submicron PM (NR-PM1) with a time resolution of 30 min at the regional background site of Ispra during 1 full year, using the Aerodyne Aerosol Chemical Speciation Monitor (ACSM) under the most up-to-date and stringent quality assurance protocol. The identification of the main components of the organic fraction is made using the Multilinear-Engine 2 algorithm implemented within the latest version of the SoFi toolkit. In addition, with the aim of a potential implementation of ACSM measurements in European air quality networks as a replacement of traditional filter-based techniques, parallel multiple offline analyses were carried out to assess the performance of the ACSM in the determination of PM chemical species regulated by air quality directives. The annual NR-PM1 level monitored at the study site (14.2 µg m-3) is among the highest in Europe and is even comparable to levels reported in urban areas like New York City and Tokyo. On the annual basis, submicron particles are primarily composed of organic aerosol (OA, 58 % of NR-PM1). This fraction was apportioned into oxygenated OA (OOA, 66 %), hydrocarbon-like OA (HOA, 11 % of OA) and biomass burning OA (BBOA, 23 %). Among the primary sources of OA, biomass burning (23 %) is thus bigger than fossil fuel combustion (11 %). Significant contributions of aged secondary organic aerosol (OOA) are observed throughout the year. The unexpectedly high degree of oxygenation

  4. Seasonal variations in high time-resolved chemical compositions, sources, and evolution of atmospheric submicron aerosols in the megacity Beijing

    Science.gov (United States)

    Hu, Wei; Hu, Min; Hu, Wei-Wei; Zheng, Jing; Chen, Chen; Wu, Yusheng; Guo, Song

    2017-08-01

    A severe regional haze problem in the megacity Beijing and surrounding areas, caused by fast formation and growth of fine particles, has attracted much attention in recent years. In order to investigate the secondary formation and aging process of urban aerosols, four intensive campaigns were conducted in four seasons between March 2012 and March 2013 at an urban site in Beijing (116.31° E, 37.99° N). An Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) was deployed to measure non-refractory chemical components of submicron particulate matter (NR-PM1). The average mass concentrations of PM1 (NR-PM1+black carbon) were 45.1 ± 45.8, 37.5 ± 31.0, 41.3 ± 42.7, and 81.7 ± 72.4 µg m-3 in spring, summer, autumn, and winter, respectively. Organic aerosol (OA) was the most abundant component in PM1, accounting for 31, 33, 44, and 36 % seasonally, and secondary inorganic aerosol (SNA, sum of sulfate, nitrate, and ammonium) accounted for 59, 57, 43, and 55 % of PM1 correspondingly. Based on the application of positive matrix factorization (PMF), the sources of OA were obtained, including the primary ones of hydrocarbon-like (HOA), cooking (COA), biomass burning OA (BBOA) and coal combustion OA (CCOA), and secondary component oxygenated OA (OOA). OOA, which can be split into more-oxidized (MO-OOA) and less-oxidized OOA (LO-OOA), accounted for 49, 69, 47, and 50 % in four seasons, respectively. Totally, the fraction of secondary components (OOA+SNA) contributed about 60-80 % to PM1, suggesting that secondary formation played an important role in the PM pollution in Beijing, and primary sources were also non-negligible. The evolution process of OA in different seasons was investigated with multiple metrics and tools. The average carbon oxidation states and other metrics show that the oxidation state of OA was the highest in summer, probably due to both strong photochemical and aqueous-phase oxidations. It was indicated by the good correlations

  5. Seasonal characterization of submicron aerosol chemical composition and organic aerosol sources in the southeastern United States: Atlanta, Georgia,and Look Rock, Tennessee

    Science.gov (United States)

    Hapsari Budisulistiorini, Sri; Baumann, Karsten; Edgerton, Eric S.; Bairai, Solomon T.; Mueller, Stephen; Shaw, Stephanie L.; Knipping, Eladio M.; Gold, Avram; Surratt, Jason D.

    2016-04-01

    A year-long near-real-time characterization of non-refractory submicron aerosol (NR-PM1) was conducted at an urban (Atlanta, Georgia, in 2012) and rural (Look Rock, Tennessee, in 2013) site in the southeastern US using the Aerodyne Aerosol Chemical Speciation Monitor (ACSM) collocated with established air-monitoring network measurements. Seasonal variations in organic aerosol (OA) and inorganic aerosol species are attributed to meteorological conditions as well as anthropogenic and biogenic emissions in this region. The highest concentrations of NR-PM1 were observed during winter and fall seasons at the urban site and during spring and summer at the rural site. Across all seasons and at both sites, NR-PM1 was composed largely of OA (up to 76 %) and sulfate (up to 31 %). Six distinct OA sources were resolved by positive matrix factorization applied to the ACSM organic mass spectral data collected from the two sites over the 1 year of near-continuous measurements at each site: hydrocarbon-like OA (HOA), biomass burning OA (BBOA), semi-volatile oxygenated OA (SV-OOA), low-volatility oxygenated OA (LV-OOA), isoprene-derived epoxydiols (IEPOX) OA (IEPOX-OA) and 91Fac (a factor dominated by a distinct ion at m/z 91 fragment ion previously observed in biogenic influenced areas). LV-OOA was observed throughout the year at both sites and contributed up to 66 % of total OA mass. HOA was observed during the entire year only at the urban site (on average 21 % of OA mass). BBOA (15-33 % of OA mass) was observed during winter and fall, likely dominated by local residential wood burning emission. Although SV-OOA contributes quite significantly ( ˜ 27 %), it was observed only at the urban site during colder seasons. IEPOX-OA was a major component (27-41 %) of OA at both sites, particularly in spring and summer. An ion fragment at m/z 75 is well correlated with the m/z 82 ion associated with the aerosol mass spectrum of IEPOX-derived secondary organic aerosol (SOA). The

  6. Variations in the chemical composition of the submicron aerosol and in the sources of the organic fraction at a regional background site of the Po Valley (Italy

    Directory of Open Access Journals (Sweden)

    M. Bressi

    2016-10-01

    Full Text Available Fine particulate matter (PM levels and resulting impacts on human health are in the Po Valley (Italy among the highest in Europe. To build effective PM abatement strategies, it is necessary to characterize fine PM chemical composition, sources and atmospheric processes on long timescales (> months, with short time resolution (< day, and with particular emphasis on the predominant organic fraction. Although previous studies have been conducted in this region, none of them addressed all these aspects together. For the first time in the Po Valley, we investigate the chemical composition of nonrefractory submicron PM (NR-PM1 with a time resolution of 30 min at the regional background site of Ispra during 1 full year, using the Aerodyne Aerosol Chemical Speciation Monitor (ACSM under the most up-to-date and stringent quality assurance protocol. The identification of the main components of the organic fraction is made using the Multilinear-Engine 2 algorithm implemented within the latest version of the SoFi toolkit. In addition, with the aim of a potential implementation of ACSM measurements in European air quality networks as a replacement of traditional filter-based techniques, parallel multiple offline analyses were carried out to assess the performance of the ACSM in the determination of PM chemical species regulated by air quality directives. The annual NR-PM1 level monitored at the study site (14.2 µg m−3 is among the highest in Europe and is even comparable to levels reported in urban areas like New York City and Tokyo. On the annual basis, submicron particles are primarily composed of organic aerosol (OA, 58 % of NR-PM1. This fraction was apportioned into oxygenated OA (OOA, 66 %, hydrocarbon-like OA (HOA, 11 % of OA and biomass burning OA (BBOA, 23 %. Among the primary sources of OA, biomass burning (23 % is thus bigger than fossil fuel combustion (11 %. Significant contributions of aged secondary organic aerosol (OOA

  7. Seasonal characterization of submicron aerosol chemical composition and organic aerosol sources in the southeastern United States: Atlanta, Georgia,and Look Rock, Tennessee

    Directory of Open Access Journals (Sweden)

    S. H. Budisulistiorini

    2016-04-01

    Full Text Available A year-long near-real-time characterization of non-refractory submicron aerosol (NR-PM1 was conducted at an urban (Atlanta, Georgia, in 2012 and rural (Look Rock, Tennessee, in 2013 site in the southeastern US using the Aerodyne Aerosol Chemical Speciation Monitor (ACSM collocated with established air-monitoring network measurements. Seasonal variations in organic aerosol (OA and inorganic aerosol species are attributed to meteorological conditions as well as anthropogenic and biogenic emissions in this region. The highest concentrations of NR-PM1 were observed during winter and fall seasons at the urban site and during spring and summer at the rural site. Across all seasons and at both sites, NR-PM1 was composed largely of OA (up to 76 % and sulfate (up to 31 %. Six distinct OA sources were resolved by positive matrix factorization applied to the ACSM organic mass spectral data collected from the two sites over the 1 year of near-continuous measurements at each site: hydrocarbon-like OA (HOA, biomass burning OA (BBOA, semi-volatile oxygenated OA (SV-OOA, low-volatility oxygenated OA (LV-OOA, isoprene-derived epoxydiols (IEPOX OA (IEPOX-OA and 91Fac (a factor dominated by a distinct ion at m∕z 91 fragment ion previously observed in biogenic influenced areas. LV-OOA was observed throughout the year at both sites and contributed up to 66 % of total OA mass. HOA was observed during the entire year only at the urban site (on average 21 % of OA mass. BBOA (15–33 % of OA mass was observed during winter and fall, likely dominated by local residential wood burning emission. Although SV-OOA contributes quite significantly ( ∼  27 %, it was observed only at the urban site during colder seasons. IEPOX-OA was a major component (27–41 % of OA at both sites, particularly in spring and summer. An ion fragment at m∕z 75 is well correlated with the m∕z 82 ion associated with the aerosol mass spectrum of IEPOX

  8. Beschrijving van een verdampings-condensatie aerosol generator voor de produktie van submicron aerosol

    NARCIS (Netherlands)

    Feijt; A.*; Meulen; A.van der

    1985-01-01

    Dit rapport is een handleiding voor een bedrijfszeker, routinematig gebruik van een zgn. Evaporation-Condensation aerosol Conditioner. Met deze aerosol generatie apparatuur kunnen op stabiele, reproduceerbare manier zeer hoge concentraties (tot 1 miljoen deeltjes per cc) monodispers submicron

  9. Evaluating model parameterizations of submicron aerosol scattering and absorption with in situ data from ARCTAS 2008

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    M. J. Alvarado

    2016-07-01

    Full Text Available Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS campaign. The four models are the NASA Global Modeling Initiative (GMI Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT, and the Optical Properties of Aerosol and Clouds (OPAC v3.1 package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1 to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10–23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass

  10. Characteristics of Submicron Aerosols in 2013 summer of Beijing

    Science.gov (United States)

    Guo, Song; Hu, Min; Shang, Dongjie; Zheng, Jing; Du, Zhuofei; Wu, Yusheng; Lu, Sihua; Zeng, Limin; Zhang, Renyi

    2016-04-01

    To characterize the air pollution of North China Plain of China, CAREBEIJING-2013 field campaign (Campaigns of Air quality REsearch in BEIJING and surrounding region) was conducted in summer of 2013. Submicron aerosols were measured at an urban site PKU (Peking University, 39° 59'21"N, 116° 18'25"E) from July 28th to September 31st 2013. A suite of integrated instruments was used to measure the size distribution, effective density and hygroscopicity of ambient particles. The chemical composition of submicron particles were measured by using an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) (Billerica, MA, USA). The average PM2.5 concentration was 73.0±70.7 μg m-3 during the measurement. The particulate pollution showed distinct 4-7 days cycles controlled by the meteorological conditions. Each cycle started with low PM2.5 mass concentrations (air mass was from relatively clean mountainous area. The particle number concentrations were high, but and the sizes were small (60 μg day-1, and the particle mean diameter grew to >100 nm. It is interesting to note that the mean diameters showed similar trend to PM2.5 mass concentrations, indicating the particle pollution attributed to the growth of the newly formed small particles. During the measurement, the average particle densities are between 1.3-1.5 g cm-3, indicating organics and sulfate were dominant in the particles. The densities of smaller particles, i.e. 46 nm, 81nm, showed single peak at 1.3-1.5 g cm-3, indicating the particles are internal mixed sulfate and organics. While the 150nm and 240 nm particle densities exhibited bimodal distribution with an additional small peak at ˜1.1 g cm-3, which is considered as external mixed organic particles or aged soot particles. The particle hygroscopic growth factor for all the measured sizes at RH of 90% showed bimodal distribution, attributing to external mixed organics (or aged soot) and internal mixed organics and sulfate. Both the

  11. Effects of chemical composition and mixing state on size-resolved hygroscopicity and cloud condensation nuclei activity of submicron aerosols at a suburban site in northern Japan in summer

    Science.gov (United States)

    Müller, Astrid; Miyazaki, Yuzo; Aggarwal, Shankar G.; Kitamori, Yasuyuki; Boreddy, Suresh K. R.; Kawamura, Kimitaka

    2017-09-01

    Ambient hygroscopic properties, numbers of size-segregated cloud condensation nuclei (CCN) at different supersaturations (0.1%-0.8%), and the chemical composition of submicron particles were simultaneously measured at a suburban site in northern Japan in summer. Two distinct periods with different growth factors (GF), CCN activation diameters, and chemical compositions were observed. The data suggest that internally mixed sulfate aerosols dominated the accumulation size mode in relatively aged aerosols during the first period, whereas particles observed during the latter periods showed external mixing dominated by organics, which was linked to low hygroscopicity and CCN activity. In particular, the higher loading of water-soluble organic matter (WSOM; 60% of OM by mass) with increased WSOM/sulfate ratios corresponded to a low hygroscopicity parameter derived from the CCN measurement (κCCN = 0.15 ± 0.02) at a dry diameter (Ddry) of 146 nm. The results suggest that WSOM, likely dominated by the influence of biogenic sources, contributed to reducing the hygroscopicity and CCN activation at this particle size. Temporal variations in the number concentrations for low GF mode at Ddry = 49.6 nm were similar to those in the elemental carbon (EC) concentration, suggesting that EC contributed to reducing hygroscopicity at this smaller size. Our results suggest that chemical composition and mixing state are important factors controlling the hygroscopicity and CCN activation of submicron particles. These results provide useful data sets of size-resolved subsaturated and supersaturated hygroscopicity and highlight the importance of the abundance of OM relative to sulfate in predicting the effects on climate change.

  12. Characterization and source apportionment of submicron aerosol with aerosol mass spectrometer during the PRIDE-PRD 2006 campaign

    Directory of Open Access Journals (Sweden)

    R. Xiao

    2011-07-01

    Full Text Available Size-resolved chemical compositions of non-refractory submicron aerosol were measured using an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS at the rural site Back Garden (BG, located ~50 km northwest of Guangzhou in July 2006. This paper characterized the submicron aerosol particles of regional air pollution in Pearl River Delta (PRD in the southern China. Organics and sulfate dominated the submicron aerosol compositions, with average mass concentrations of 11.8 ± 8.4 μg m−3 and 13.5 ± 8.7 μg m−3, respectively. Unlike other air masses, the air masses originated from Southeast-South and passing through the PRD urban areas exhibited distinct bimodal size distribution characteristics for both organics and sulfate: the first mode peaked at vacuum aerodynamic diameters (Dva ∼200 nm and the second mode occurred at Dva from 300–700 nm. With the information from AMS, it was found from this study that the first mode of organics in PRD regional air masses was contributed by both secondary organic aerosol formation and combustion-related emissions, which is different from most findings in other urban areas (first mode of organics primarily from combustion-related emissions. The analysis of AMS mass spectra data by positive matrix factorization (PMF model identified three sources of submicron organic aerosol including hydrocarbon-like organic aerosol (HOA, low volatility oxygenated organic aerosol (LV-OOA and semi-volatile oxygenated organic aerosol (SV-OOA. The strong correlation between HOA and EC indicated primary combustion emissions as the major source of HOA while a close correlation between SV-OOA and semi-volatile secondary species nitrate as well as between LV-OOA and nonvolatile secondary species sulfate suggested secondary aerosol formation as the major source of SV-OOA and LV-OOA at the BG site. However, LV-OOA was more aged than SV-OOA as its spectra was highly

  13. Characterization and source apportionment of submicron aerosol with aerosol mass spectrometer during the PRIDE-PRD 2006 campaign

    Science.gov (United States)

    Xiao, R.; Takegawa, N.; Zheng, M.; Kondo, Y.; Miyazaki, Y.; Miyakawa, T.; Hu, M.; Shao, M.; Zeng, L.; Gong, Y.; Lu, K.; Deng, Z.; Zhao, Y.; Zhang, Y. H.

    2011-07-01

    Size-resolved chemical compositions of non-refractory submicron aerosol were measured using an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) at the rural site Back Garden (BG), located ~50 km northwest of Guangzhou in July 2006. This paper characterized the submicron aerosol particles of regional air pollution in Pearl River Delta (PRD) in the southern China. Organics and sulfate dominated the submicron aerosol compositions, with average mass concentrations of 11.8 ± 8.4 μg m-3 and 13.5 ± 8.7 μg m-3, respectively. Unlike other air masses, the air masses originated from Southeast-South and passing through the PRD urban areas exhibited distinct bimodal size distribution characteristics for both organics and sulfate: the first mode peaked at vacuum aerodynamic diameters (Dva) ∼200 nm and the second mode occurred at Dva from 300-700 nm. With the information from AMS, it was found from this study that the first mode of organics in PRD regional air masses was contributed by both secondary organic aerosol formation and combustion-related emissions, which is different from most findings in other urban areas (first mode of organics primarily from combustion-related emissions). The analysis of AMS mass spectra data by positive matrix factorization (PMF) model identified three sources of submicron organic aerosol including hydrocarbon-like organic aerosol (HOA), low volatility oxygenated organic aerosol (LV-OOA) and semi-volatile oxygenated organic aerosol (SV-OOA). The strong correlation between HOA and EC indicated primary combustion emissions as the major source of HOA while a close correlation between SV-OOA and semi-volatile secondary species nitrate as well as between LV-OOA and nonvolatile secondary species sulfate suggested secondary aerosol formation as the major source of SV-OOA and LV-OOA at the BG site. However, LV-OOA was more aged than SV-OOA as its spectra was highly correlated with the reference spectra of fulvic acid, an indicator of aged and

  14. The role of jet and film drops in controlling the mixing state of submicron sea spray aerosol particles

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Xiaofei; Deane, Grant B.; Moore, Kathryn A.; Ryder, Olivia S.; Stokes, M. Dale; Beall, Charlotte M.; Collins, Douglas B.; Santander, Mitchell V.; Burrows, Susannah M.; Sultana, Camille M.; Prather, Kimberly A.

    2017-06-19

    Covering 71% of the Earth’s surface, oceans represent a significant global source of atmospheric aerosols. The size and composition of sea spray aerosols (SSA) affect their ability to serve as cloud seeds and thus understanding the factors controlling their composition is critical to predicting their impact on clouds and climate. SSA particles have been shown to be an external mixture of particles with different compositions. Film and jet drop production mechanisms ultimately determine the individual particle compositions which are comprised of an array of salt/organic mixtures ranging from pure sea salt to nearly pure organic particles. It is often assumed that the majority of submicron SSA are formed by film drops produced from bursting hydrophobic organic-rich bubble film caps at the sea surface, and in contrast, jet drops are postulated to produce larger supermicron particles from underlying seawater comprised largely of salts and water soluble organic species. However, here we show that jet drops produced by bursting sub-100 m bubbles account for up to 40 % of all submicron particles. They have distinct chemical compositions, organic volume fractions and ice nucleating activities from submicron film drops. Thus a substantial fraction of submicron particles will not necessarily be controlled by the composition of the sea surface microlayer as has been assumed in many studies. This finding has significant ramifications for the size-resolved mixing states of SSA particles which must be taken into consideration when accessing SSA impacts on clouds.

  15. Submicron organic aerosol in Tijuana, Mexico, from local and Southern California sources during the CalMex campaign

    Science.gov (United States)

    Takahama, S.; Johnson, A.; Guzman Morales, J.; Russell, L. M.; Duran, R.; Rodriguez, G.; Zheng, J.; Zhang, R.; Toom-Sauntry, D.; Leaitch, W. R.

    2013-05-01

    The CalMex campaign was conducted from May 15 to June 30 of 2010 to study the properties and sources of air pollution in Tijuana, Mexico. In this study, submicron organic aerosol mass (OM) composition measured by Fourier Transform Infrared Spectroscopy (FTIR), Aerosol Chemical Speciation Monitor (ACSM), and X-ray spectromicroscopy are combined with statistical analysis and measurements of other atmospheric constituents. The average (±one standard deviation) OM concentration was 3.3 ± 1.7 μg m-3. A large source of submicron aerosol mass at this location was determined to be vehicular sources, which contributed approximately 40% to the submicron OM; largely during weekday mornings. The O/C ratio estimated from ACSM measurements was 0.64 ± 0.19; diurnal variations in this value and the more oxygenated fraction of OM as determined from Positive Matrix Factorization and classification analyses suggest the high degree of oxygenation originates from aged OM, rather than locally-produced secondary organic aerosol. A large contribution of this oxygenated aerosol to Tijuana from various source classes was observed; some fraction of this aerosol mass may be associated with non-refractory components, such as dust or BC. Backtrajectory simulations using the HYSPLIT model suggest that the mean wind vector consistently originated from the northwest region, over the Pacific Ocean and near the Southern California coast, which suggests that the origin of much of the oxygenated organic aerosol observed in Tijuana (as much as 60% of OM) may have been the Southern California Air Basin. The marine aerosol contribution to OM during the period was on average 23 ± 24%, though its contribution varied over synoptic rather than diurnal timescales. BB aerosol contributed 20 ± 20% of the OM during the campaign period, with notable BB events occurring during several weekend evenings.

  16. Chemical characteristics of submicron particles at the central Tibetan Plateau: insights from aerosol mass spectrometry

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    J. Xu

    2018-01-01

    Full Text Available Recent studies have revealed a significant influx of anthropogenic aerosol from South Asia to the Himalayas and Tibetan Plateau (TP during pre-monsoon period. In order to characterize the chemical composition, sources, and transport processes of aerosol in this area, we carried out a field study during June 2015 by deploying a suite of online instruments including an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS and a multi-angle absorption photometer (MAAP at Nam Co station (90°57′ E, 30°46′ N; 4730 m a.s.l. at the central of the TP. The measurements were made at a period when the transition from pre-monsoon to monsoon occurred. The average ambient mass concentration of submicron particulate matter (PM1 over the whole campaign was  ∼  2.0 µg m−3, with organics accounting for 68 %, followed by sulfate (15 %, black carbon (8 %, ammonium (7 %, and nitrate (2 %. Relatively higher aerosol mass concentration episodes were observed during the pre-monsoon period, whereas persistently low aerosol concentrations were observed during the monsoon period. However, the chemical composition of aerosol during the higher aerosol concentration episodes in the pre-monsoon season was on a case-by-case basis, depending on the prevailing meteorological conditions and air mass transport routes. Most of the chemical species exhibited significant diurnal variations with higher values occurring during afternoon and lower values during early morning, whereas nitrate peaked during early morning in association with higher relative humidity and lower air temperature. Organic aerosol (OA, with an oxygen-to-carbon ratio (O ∕ C of 0.94, was more oxidized during the pre-monsoon period than during monsoon (average O ∕ C ratio of 0.72, and an average O ∕ C was 0.88 over the entire campaign period, suggesting overall highly oxygenated aerosol in the central TP. Positive matrix factorization of the

  17. Characterization of near-highway submicron aerosols in New York City with a high-resolution aerosol mass spectrometer

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    Y. L. Sun

    2012-02-01

    Full Text Available Knowledge of the variations of mass concentration, chemical composition and size distributions of submicron aerosols near roadways is of importance for reducing exposure assessment uncertainties in health effects studies. The goal of this study is to deploy and evaluate an Atmospheric Sciences Research Center-Mobile Laboratory (ASRC-ML, equipped with a suite of rapid response instruments for characterization of traffic plumes, adjacent to the Long Island Expressway (LIE – a high-traffic highway in the New York City Metropolitan Area. In total, four measurement periods, two in the morning and two in the evening were conducted at a location approximately 30 m south of the LIE. The mass concentrations and size distributions of non-refractory submicron aerosol (NR-PM1 species were measured in situ at a time resolution of 1 min by an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer, along with rapid measurements (down to 1 Hz of gaseous pollutants (e.g. HCHO, NO2, NO, O3, and CO2, etc., black carbon (BC, and particle number concentrations and size distributions. Particulate organics varied dramatically during periods with high traffic influences from the nearby roadway. The variations were mainly observed in the hydrocarbon-like organic aerosol (HOA, a surrogate for primary OA from vehicle emissions. The inorganic species (sulfate, ammonium, and nitrate and oxygenated OA (OOA showed much smoother variations indicating minor impacts from traffic emissions. The concentration and chemical composition of NR-PM1 also varied differently on different days depending on meteorology, traffic intensity and vehicle types. Overall, organics dominated the traffic-related NR-PM1 composition (>60% with HOA accounting for a major fraction of OA. The traffic-influenced organics showed two distinct modes in mass-weighted size distributions, peaking at ∼120 nm and 500 nm (vacuum

  18. Rapid heterogeneous oxidation of organic coatings on submicron aerosols

    Science.gov (United States)

    Lim, C. Y.; Browne, E. C.; Sugrue, R. A.; Kroll, J. H.

    2017-03-01

    Laboratory studies have found that heterogeneous oxidation can affect the composition and loading of atmospheric organic aerosol particles over time scales of several days, but most studies have examined pure organic particles only. In this study, in order to probe the reactivity of organic species confined near the particle surface, the rates and products of the OH-initiated oxidation of pure squalane particles are compared to oxidation of thin coatings of squalane on ammonium sulfate particles. The squalane reaction rate constant shows a linear dependence on the organic surface area-to-volume ratio, with rate constants for coated particles up to 10 times larger than for pure particles. Changes in the carbon oxidation state and fraction of particulate carbon remaining show similar enhancements, implying that heterogeneous oxidation may exhibit a stronger effect on the loadings and properties of organic aerosol than previously estimated from laboratory studies.

  19. Volatility measurement of atmospheric submicron aerosols in an urban atmosphere in southern China

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    L.-M. Cao

    2018-02-01

    Full Text Available Aerosol pollution has been a very serious environmental problem in China for many years. The volatility of aerosols can affect the distribution of compounds in the gas and aerosol phases, the atmospheric fates of the corresponding components, and the measurement of the concentration of aerosols. Compared to the characterization of chemical composition, few studies have focused on the volatility of aerosols in China. In this study, a thermodenuder aerosol mass spectrometer (TD-AMS system was deployed to study the volatility of non-refractory submicron particulate matter (PM1 species during winter in Shenzhen. To our knowledge, this paper is the first report of the volatilities of aerosol chemical components based on a TD-AMS system in China. The average PM1 mass concentration during the experiment was 42.7±20.1 µg m−3, with organic aerosol (OA being the most abundant component (43.2 % of the total mass. The volatility of chemical species measured by the AMS varied, with nitrate showing the highest volatility, with a mass fraction remaining (MFR of 0.57 at 50 °C. Organics showed semi-volatile characteristics (the MFR was 0.88 at 50 °C, and the volatility had a relatively linear correlation with the TD temperature (from the ambient temperature to 200 °C, with an evaporation rate of 0.45 % °C−1. Five subtypes of OA were resolved from total OA using positive matrix factorization (PMF for data obtained under both ambient temperature and high temperatures through the TD, including a hydrocarbon-like OA (HOA, accounting for 13.5 %, a cooking OA (COA, 20.6 %, a biomass-burning OA (BBOA, 8.9 %, and two oxygenated OAs (OOAs: a less-oxidized OOA (LO-OOA, 39.1 % and a more-oxidized OOA (MO-OOA, 17.9 %. Different OA factors presented different volatilities, and the volatility sequence of the OA factors at 50 °C was HOA (MFR of 0.56  >  LO-OOA (0.70  >  COA (0.85  ≈  BBOA (0.87

  20. Aerodynamics and deposition effects of inhaled submicron drug aerosol in airway diseases.

    Science.gov (United States)

    Faiyazuddin, Md; Mujahid, Md; Hussain, Talib; Siddiqui, Hefazat H; Bhatnagar, Aseem; Khar, Roop K; Ahmad, Farhan J

    2013-01-01

    Particle engineering is the prime focus to improve pulmonary drug targeting with the splendor of nanomedicines. In recent years, submicron particles have emerged as prettyful candidate for improved fludisation and deposition. For effective deposition, the particle size must be in the range of 0.5-5 μm. Inhalers design for the purpose of efficient delivery of powders to lungs is again a crucial task for pulmonary scientists. A huge number of DPI devices exist in the market, a significant number are awaiting FDA approval, some are under development and a large number have been patented or applied for patent. Even with superior design, the delivery competence is still deprived, mostly due to fluidisation problems which cause poor aerosol generation and deposition. Because of the cohesive nature and poor flow characteristics, they are difficult to redisperse upon aerosolization with breath. These problems are illustrious in aerosol research, much of which is vastly pertinent to pulmonary therapeutics. A technical review is presented here of advances that have been utilized in production of submicron drug particles, their in vitro/in vivo evaluations, aerosol effects and pulmonary fate of inhaled submicron powders.

  1. Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China during 2014 APEC summit

    Science.gov (United States)

    Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

    2015-08-01

    The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the 325 m Beijing Meteorological Tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition at near ground level using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3-/SO42- mass ratios illustrate an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed by secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors such as SO2, NOx, and volatile organic compounds (VOCs). In addition to emission controls, the routine

  2. Characteristics and sources of submicron aerosols above the urban canopy (260 m) in Beijing, China, during the 2014 APEC summit

    Science.gov (United States)

    Chen, C.; Sun, Y. L.; Xu, W. Q.; Du, W.; Zhou, L. B.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Gao, Z. Q.; Zhang, Q.; Worsnop, D. R.

    2015-11-01

    The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the Beijing 325 m meteorological tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition near ground level using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3- / SO42- mass ratios illustrates an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed of secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia-Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40-80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors. In addition to emission controls, the routine circulations of mountain-valley breezes were also found to play

  3. Airborne measurements of submicron aerosols across the coastline ...

    Indian Academy of Sciences (India)

    track in the east–west direction extended partly over land and partly over ocean. 2. Instrumentation. A Scanning Mobility Particle Sizer (SMPS), Model. 3080, of TSI, installed onboard a beachcraft air- craft is used to make measurements of the number concentration and size distribution of aerosol par- ticles in the size range ...

  4. Measurements of Natural Radioactivity in Submicron Aerosols in Mexico City.

    Science.gov (United States)

    Gaffney, J. S.; Marley, N. A.; Sterling, K.; Sturchio, N. C.

    2003-12-01

    Natural radionuclides can be useful in evaluating the transport of ozone and aerosols in the troposphere. Beryllium-7, which is produced by cosmic ray interactions in the upper troposphere and lower stratosphere and becomes adsorbed on fine aerosols, can be a useful indicator of upper air transport into a region. Lead-210 is produced by the decay of radon-222 out-gassed into the lower atmosphere from ground-based uranium deposits. Potassium-40, found in soils, can act as a measure of wind-blown dust and also comes from burning of wood and other biomass that is enriched in this natural radioisotope. Thus, both lead-210 and potassium-40 can aid in identification of aerosols sourced in the lower atmosphere. As part of our continuing interest in the lifetimes and sources of aerosols and their radiative effects, we report here measurements of fine aerosol radioactivity in Mexico City, one of the largest megacities in the world. Samples were collected on quartz fiber filters by using cascade impactors (Sierra type, Anderson Instruments) and high-volume air samplers from the rooftop of the main laboratory of El Centro Nacional de Investigacion y Capacitacion Ambiental (CENICA). By using stage 4 of the impactor and timers, we were able to collect integrated samples of sizes > 1 micrometer and < 1 micrometer over 12-hr time periods daily for approximately one month in April 2003. Samples were counted at the University of Illinois at Chicago by using state-of-the-art gamma counting (beryllium-7, 477.6 keV; potassium-40, 1460.8 keV; lead-210, 46.5 keV). The beryllium-7 data indicate one possible upper-air transport event during April 2003. As expected, the lead-210 data indicate very little soil contribution to the fine aerosol. The potassium-40 data showed an increase in fine aerosol potassium during Holy Week that might be attributed to local combustion of biomass fuels. The data will be presented and discussed in light of future data analysis and comparison with other

  5. Airborne studies of submicron aerosol in the troposphere over West Siberia

    Energy Technology Data Exchange (ETDEWEB)

    Panchenko, M.V.; Zuev, V.E.; Belan, B.D.; Terpugova, S.A. [Institute of Atmospheric Optics, Tomsk (Russian Federation)

    1996-04-01

    Submicron fraction particles that have the longest lifespan and are included in almost all atmospheric processes are of special importance among the great variety of sizes of particles present in the atmosphere. Submicron particles mainly determine the opticle state of the atmosphere in the visible spectral range, essentially cause the absorption of infrared radiation and, since they are the products and participants in all aerosol-to-gas transformations, accumulate of a lot of various chemical compounds and transfer them to large distances. Investigation of the processes of the spatial-temporal variability of aerosol particles for different climatic zones of the earth is the experimental base for studying their effect on climatically and ecologically significant factors and estimating their unfavorable tendencies. The increasing anthropogenic loading of the earth`s atmosphere is creating an urgency for aerosol research. Regardless of how perfect the analytical and numerical methods of solving radiation problems may be, success in forecasting climatic change is mainly determined by the reliability of the experimental data on optical parameters of the atmosphere and of the description of their variability under the effect of external factors.

  6. Toward Quantifying the Mass-Based Hygroscopicity of Individual Submicron Atmospheric Aerosol Particles with STXM/NEXAFS and SEM/EDX

    Science.gov (United States)

    Yancey Piens, D.; Kelly, S. T.; OBrien, R. E.; Wang, B.; Petters, M. D.; Laskin, A.; Gilles, M. K.

    2014-12-01

    The hygroscopic behavior of atmospheric aerosols influences their optical and cloud-nucleation properties, and therefore affects climate. Although changes in particle size as a function of relative humidity have often been used to quantify the hygroscopic behavior of submicron aerosol particles, it has been noted that calculations of hygroscopicity based on size contain error due to particle porosity, non-ideal volume additivity and changes in surface tension. We will present a method to quantify the hygroscopic behavior of submicron aerosol particles based on changes in mass, rather than size, as a function of relative humidity. This method results from a novel experimental approach combining scanning transmission x-ray microscopy with near-edge x-ray absorption fine spectroscopy (STXM/NEXAFS), as well as scanning electron microscopy with energy dispersive x-ray spectroscopy (SEM/EDX) on the same individual particles. First, using STXM/NEXAFS, our methods are applied to aerosol particles of known composition ‒ for instance ammonium sulfate, sodium bromide and levoglucosan ‒ and validated by theory. Then, using STXM/NEXAFS and SEM/EDX, these methods are extended to mixed atmospheric aerosol particles collected in the field at the DOE Atmospheric Radiation Measurement (ARM) Climate Research Facility at the Southern Great Planes sampling site in Oklahoma, USA. We have observed and quantified a range of hygroscopic behaviors which are correlated to the composition and morphology of individual aerosol particles. These methods will have implications for parameterizing aerosol mixing state and cloud-nucleation activity in atmospheric models.

  7. Aerosols in the tropical and subtropical UT/LS: in-situ measurements of submicron particle abundance and volatility

    Directory of Open Access Journals (Sweden)

    S. Borrmann

    2010-06-01

    Full Text Available Processes occurring in the tropical upper troposphere (UT, the Tropical Transition Layer (TTL, and the lower stratosphere (LS are of importance for the global climate, for stratospheric dynamics and air chemistry, and for their influence on the global distribution of water vapour, trace gases and aerosols. In this contribution we present aerosol and trace gas (in-situ measurements from the tropical UT/LS over Southern Brazil, Northern Australia, and West Africa. The instruments were operated on board of the Russian high altitude research aircraft M-55 "Geophysica" and the DLR Falcon-20 during the campaigns TROCCINOX (Araçatuba, Brazil, February 2005, SCOUT-O3 (Darwin, Australia, December 2005, and SCOUT-AMMA (Ouagadougou, Burkina Faso, August 2006. The data cover submicron particle number densities and volatility from the COndensation PArticle counting System (COPAS, as well as relevant trace gases like N2O, ozone, and CO. We use these trace gas measurements to place the aerosol data into a broader atmospheric context. Also a juxtaposition of the submicron particle data with previous measurements over Costa Rica and other tropical locations between 1999 and 2007 (NASA DC-8 and NASA WB-57F is provided. The submicron particle number densities, as a function of altitude, were found to be remarkably constant in the tropical UT/LS altitude band for the two decades after 1987. Thus, a parameterisation suitable for models can be extracted from these measurements. Compared to the average levels in the period between 1987 and 2007 a slight increase of particle abundances was found for 2005/2006 at altitudes with potential temperatures, Θ, above 430 K. The origins of this increase are unknown except for increases measured during SCOUT-AMMA. Here the eruption of the Soufrière Hills volcano in the Caribbean caused elevated particle mixing ratios. The vertical profiles from Northern hemispheric mid-latitudes between 1999 and 2006 also are

  8. Enhancements of the refractory submicron aerosol fraction in the Arctic polar vortex: feature or exception?

    Science.gov (United States)

    Weigel, R.; Volk, C. M.; Kandler, K.; Hösen, E.; Günther, G.; Vogel, B.; Grooß, J.-U.; Khaykin, S.; Belyaev, G. V.; Borrmann, S.

    2014-11-01

    In situ measurements with a four-channel stratospheric condensation particle counter (CPC) were conducted at up to 20 km altitude on board the aircraft M-55 Geophysica from Kiruna, Sweden, in January through March (EUPLEX 2003, RECONCILE 2010) and in December (ESSenCe 2011). During all campaigns air masses from the upper stratosphere and mesosphere were subsiding inside the Arctic winter vortex, thus initializing a transport of refractory aerosol into the lower stratosphere (Θ content of nitrous oxide (70 nmol mol-1 of N2O). This indicates that refractory aerosol originates from the upper stratosphere or the mesosphere. Derived from the mixing ratio of the simultaneously measured long-lived tracer N2O, an empirical index serves to differentiate probed air masses according to their origin: inside the vortex, the vortex edge region, or outside the vortex. Previously observed high fractions of refractory submicron aerosol in the 2003 Arctic vortex were ascribed to unusually strong subsidence during that winter. However, measurements under perturbed vortex conditions in 2010 and during early winter in December 2011 revealed similarly high values. Thus, the abundance of refractory aerosol in the lower stratosphere within the Arctic vortices appears to be a regular feature rather than the exception. During December, the import from aloft into the lower stratosphere appears to be developing; thereafter the abundance of refractory aerosol inside the vortex reaches its highest levels in March. The correlations of refractory aerosol with N2O suggest that, apart from mean subsidence, diabatic dispersion inside the vortex significantly contributes to the transport of particles to the Arctic lower stratosphere. A measurement-based estimate of the total mass of refractory aerosol inside the vortex is provided for each campaign. Based on the derived increase of particle mass in the lower stratospheric vortex (100-67 hPa pressure altitude) by a factor of 4.5 between early and

  9. A statistical analysis of North East Atlantic (submicron aerosol size distributions

    Directory of Open Access Journals (Sweden)

    M. Dall'Osto

    2011-12-01

    Full Text Available The Global Atmospheric Watch research station at Mace Head (Ireland offers the possibility to sample some of the cleanest air masses being imported into Europe as well as some of the most polluted being exported out of Europe. We present a statistical cluster analysis of the physical characteristics of aerosol size distributions in air ranging from the cleanest to the most polluted for the year 2008. Data coverage achieved was 75% throughout the year. By applying the Hartigan-Wong k-Means method, 12 clusters were identified as systematically occurring. These 12 clusters could be further combined into 4 categories with similar characteristics, namely: coastal nucleation category (occurring 21.3 % of the time, open ocean nucleation category (occurring 32.6% of the time, background clean marine category (occurring 26.1% of the time and anthropogenic category (occurring 20% of the time aerosol size distributions. The coastal nucleation category is characterised by a clear and dominant nucleation mode at sizes less than 10 nm while the open ocean nucleation category is characterised by a dominant Aitken mode between 15 nm and 50 nm. The background clean marine aerosol exhibited a clear bimodality in the sub-micron size distribution, with although it should be noted that either the Aitken mode or the accumulation mode may dominate the number concentration. However, peculiar background clean marine size distributions with coarser accumulation modes are also observed during winter months. By contrast, the continentally-influenced size distributions are generally more monomodal (accumulation, albeit with traces of bimodality. The open ocean category occurs more often during May, June and July, corresponding with the North East (NE Atlantic high biological period. Combined with the relatively high percentage frequency of occurrence (32.6%, this suggests that the marine biota is an important source of new nano aerosol particles in NE Atlantic Air.

  10. Modelling size and structure of nanoparticles formed from drying of submicron solution aerosols

    Science.gov (United States)

    Bandyopadhyay, Arpan A.; Pawar, Amol A.; Venkataraman, Chandra; Mehra, Anurag

    2015-01-01

    Drying of submicron solution aerosols, under controlled conditions, has been explored to prepare nanoparticles for drug delivery applications. A computational model of solution drop evaporation is developed to study the evolution of solute gradients inside the drop and predict the size and shell thickness of precipitating nanoparticles. The model considers evaporation as a two-stage process involving droplet shrinkage and shell growth. It was corroborated that droplet evaporation rate controls the solute distribution within a droplet and the resulting particle structure (solid or shell type). At higher gas temperatures, rapid build-up of solute near drop surface from high evaporation rates results in early attainment of critical supersaturation solubility and a steeper solute gradient, which favours formation of larger, shell-type particles. At lower gas temperatures, formation of smaller, solid nanoparticles is indicated. The computed size and shell thickness are in good agreement with experimentally prepared lipid nanoparticles. This study indicates that solid or shell structure of precipitated nanoparticles is strongly affected by evaporation rate, while initial solute concentration in the precursor solution and atomized droplet size affect shell thickness. For the gas temperatures considered, evaporative cooling leads to droplet temperature below the melting point of the lipid solute. Thus, we conclude that control over nanoparticle size and structure, of thermolabile precursor materials suitable for drug delivery, can be achieved by controlling evaporation rates, through selection of aerosol processing conditions.

  11. Enhanced hydrophobicity and volatility of submicron aerosols under severe emission control conditions in Beijing

    Science.gov (United States)

    Wang, Yuying; Zhang, Fang; Li, Zhanqing

    2017-04-01

    A series of strict emission control measures were implemented in Beijing and the surrounding seven provinces to ensure good air quality during the 2015 China Victory Day parade, rendering a unique opportunity to investigate anthropogenic impact of aerosol properties. Submicron aerosol hygroscopicity and volatility were measured during and after the control period using a hygroscopic and volatile tandem differential mobility analyzer (H/V-TDMA) system. Three periods, namely, the control clean period (Clean1), the non-control clean period (Clean2), and the non-control pollution period (Pollution), were selected to study the effect of the emission control measures on aerosol hygroscopicity and volatility. Aerosol particles became more hydrophobic and volatile due to the emission control measures. The hygroscopicity parameter (κ) of 40-200 nm particles decreased by 32.0%-8.5% during the Clean1 period relative to the Clean2 period, while the volatile shrink factor (SF) of 40-300 nm particles decreased by 7.5%-10.5%. The emission controls also changed the diurnal variation patterns of both the probability density function of κ (κ-PDF) and the probability density function of SF (SF-PDF). During Clean1 the κ-PDF showed one nearly-hydrophobic (NH) mode for particles in the nucleation mode, which was likely due to the dramatic reduction in industrial emissions of inorganic trace gases. Compared to the Pollution period, particles observed during the Clean1 and Clean2 periods exhibited a more significant non-volatile (NV) mode throughout the day, suggesting a more externally-mixed state particularly for the 150 nm particles. Aerosol hygroscopicities increased as particle sizes increased, with the greatest increases seen during the Pollution period. Accordingly, the aerosol volatility became weaker (i.e., SF increased) during the Clean1 and Clean2 periods, but no apparent trend was observed during the Pollution period. Based on a correlation analysis of the number fractions

  12. Chemical characterization and source apportionment of submicron aerosols measured in Senegal during the 2015 SHADOW campaign

    Directory of Open Access Journals (Sweden)

    L.-H. Rivellini

    2017-09-01

    Full Text Available The present study offers the first chemical characterization of the submicron (PM1 fraction in western Africa at a high time resolution, thanks to collocated measurements of nonrefractory (NR species with an Aerosol Chemical Speciation Monitor (ACSM, black carbon and iron concentrations derived from absorption coefficient measurements with a 7-wavelength Aethalometer, and total PM1 determined by a TEOM-FDMS (tapered element oscillating microbalance–filtered dynamic measurement system for mass closure. The field campaign was carried out over 3 months (March to June 2015 as part of the SHADOW (SaHAran Dust Over West Africa project at a coastal site located in the outskirts of the city of Mbour, Senegal. With an averaged mass concentration of 5.4 µg m−3, levels of NR PM1 in Mbour were 3 to 10 times lower than those generally measured in urban and suburban polluted environments. Nonetheless the first half of the observation period was marked by intense but short pollution events (NR PM1 concentrations higher than 15 µg m−3, sea breeze phenomena and Saharan desert dust outbreaks (PM10 up to 900 µg m−3. During the second half of the campaign, the sampling site was mainly under the influence of marine air masses. The air masses on days under continental and sea breeze influences were dominated by organics (36–40 %, whereas sulfate particles were predominant (40 % for days under oceanic influence. Overall, measurements showed that about three-quarters of the total PM1 were explained by NR PM1, BC (black carbon and Fe (a proxy for dust concentrations, leaving approximately one-quarter for other refractory species. A mean value of 4.6 % for the Fe ∕ PM1 ratio was obtained. Source apportionment of the organic fraction, using positive matrix factorization (PMF, highlighted the impact of local combustion sources, such as traffic and residential activities, which contribute on average to 52 % of the total organic

  13. Chemical characterization and source apportionment of submicron aerosols measured in Senegal during the 2015 SHADOW campaign

    Science.gov (United States)

    Rivellini, Laura-Hélèna; Chiapello, Isabelle; Tison, Emmanuel; Fourmentin, Marc; Féron, Anaïs; Diallo, Aboubacry; N'Diaye, Thierno; Goloub, Philippe; Canonaco, Francesco; Prévôt, André Stephan Henry; Riffault, Véronique

    2017-09-01

    The present study offers the first chemical characterization of the submicron (PM1) fraction in western Africa at a high time resolution, thanks to collocated measurements of nonrefractory (NR) species with an Aerosol Chemical Speciation Monitor (ACSM), black carbon and iron concentrations derived from absorption coefficient measurements with a 7-wavelength Aethalometer, and total PM1 determined by a TEOM-FDMS (tapered element oscillating microbalance-filtered dynamic measurement system) for mass closure. The field campaign was carried out over 3 months (March to June 2015) as part of the SHADOW (SaHAran Dust Over West Africa) project at a coastal site located in the outskirts of the city of Mbour, Senegal. With an averaged mass concentration of 5.4 µg m-3, levels of NR PM1 in Mbour were 3 to 10 times lower than those generally measured in urban and suburban polluted environments. Nonetheless the first half of the observation period was marked by intense but short pollution events (NR PM1 concentrations higher than 15 µg m-3), sea breeze phenomena and Saharan desert dust outbreaks (PM10 up to 900 µg m-3). During the second half of the campaign, the sampling site was mainly under the influence of marine air masses. The air masses on days under continental and sea breeze influences were dominated by organics (36-40 %), whereas sulfate particles were predominant (40 %) for days under oceanic influence. Overall, measurements showed that about three-quarters of the total PM1 were explained by NR PM1, BC (black carbon) and Fe (a proxy for dust) concentrations, leaving approximately one-quarter for other refractory species. A mean value of 4.6 % for the Fe / PM1 ratio was obtained. Source apportionment of the organic fraction, using positive matrix factorization (PMF), highlighted the impact of local combustion sources, such as traffic and residential activities, which contribute on average to 52 % of the total organic fraction. A new organic aerosol (OA) source

  14. Simulation of hurricane response to suppression of warm rain by sub-micron aerosols

    Directory of Open Access Journals (Sweden)

    D. Rosenfeld

    2007-07-01

    Full Text Available The feasibility of hurricane modification was investigated for hurricane Katrina using the Weather Research and Forecasting Model (WRF. The possible impact of seeding of clouds with submicron cloud condensation nuclei (CCN on hurricane structure and intensity as measured by nearly halving of the area covered by hurricane force winds was simulated by "turning–off" warm rain formation in the clouds at Katrina's periphery (where wind speeds were less than 22 m s−1. This simplification of the simulation of aerosol effects is aimed at evaluating the largest possible response. This resulted in the weakening of the hurricane surface winds compared to the "non-seeded" simulated storm during the first 24 h within the entire tropical cyclone (TC area compared to a control simulation without warm rain suppression. Later, the seeding-induced evaporative cooling at the TC periphery led to a shrinking of the eye and hence to some increase in the wind within the small central area of the TC. Yet, the overall strength of the hurricane, as defined by the area covered by hurricane force winds, decreased in response to the suppressed warm rain at the periphery, as measured by a 25% reduction in the radius of hurricane force winds. In a simulation with warm rain suppression throughout the hurricane, the radius of the hurricane force winds was reduced by more than 42%, and although the diameter of the eye shrunk even further the maximum winds weakened. This shows that the main mechanism by which suppressing warm rain weakens the TC is the low level evaporative cooling of the un-precipitated cloud drops and the added cooling due to melting of precipitation that falls from above.

  15. Aerosol Chemical Speciation Monitor (ACSM) Instrument Handbook

    Energy Technology Data Exchange (ETDEWEB)

    Watson, Thomas B. [Brookhaven National Lab. (BNL), Upton, NY (United States)

    2017-08-15

    The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) measures particle mass loading and chemical composition in real time for non-refractory sub-micron aerosol particles. The ACSM is designed for long-term unattended deployment and routine monitoring applications.

  16. Characteristics of submicron particulate matter at the urban roadside in downtown Hong Kong—Overview of 4 months of continuous high-resolution aerosol mass spectrometer measurements

    Science.gov (United States)

    Lee, Berto P.; Li, Yong Jie; Yu, Jian Zhen; Louie, Peter K. K.; Chan, Chak K.

    2015-07-01

    Hong Kong, one of the world's most densely populated cities and an international financial center, has been suffering from traffic-related air pollution. This study presents the first real-time high-resolution aerosol mass spectrometry measurements of submicron nonrefractory particulate matter (NR-PM1) at the urban roadside in Hong Kong from March to July 2013 with the aim to identify major sources, to assess local and nonlocal emissions, and to characterize trends at different time scales. Organics were dominant, with fresh primary organic aerosol representing two thirds of the total measured organics. Cooking contributions in organic aerosol were assessed directly for the first time in Hong Kong and exceeded those related to vehicles although traffic was still the major PM1 source when elemental carbon was included. These findings were supported by additional measurements including traffic data, elemental/organic carbon, and VOC data. Springtime concentrations were about double of those in summer, due to a strong seasonal transition which affected meteorological conditions and street-level circulation. Local formation of secondary species was not clearly discernible in either season. The elemental composition of organic aerosol remained stable with similar elemental ratios across the covered seasons: OM/OC: 1.49 ± 0.13, O/C: 0.25 ± 0.10, H/C: 1.68 ± 0.08 for spring and OM/OC: 1.43 ± 0.14, O/C: 0.21 ± 0.11, H/C: 1.69 ± 0.08 for summer. Diurnal changes in H/C and O/C as a result of mixing of primary organic aerosol and secondary organic aerosol were evident in the van Krevelen plot.

  17. Contribution of wood combustion in winter submicron ambient aerosols over Athens

    Science.gov (United States)

    Stavroulas, Iasonas; Fourtziou, Luciana; Zarmpas, Pavlos; Bougiatioti, Aikaterini; Liakakou, Eleni; Sciare, Jean; Mihalopoulos, Nikos

    2014-05-01

    Given that a smog pollution problem, mostly attributed to wood burning in fireplaces and stoves, is currently emerging in the Athens metropolitan area, several monitoring instruments were deployed at the National Observatory of Athens facilities in the region of Thissio, downtown Athens . These included an Aerodyne Aerosol Chemical Speciation Monitor with 30 minute time resolution and a Particle Into Liquid Sampler coupled with Ion Chromatography with 15 minute time resolution. The campaign duration was from December 2013 to February 2014 and the aim was to investigate the chemical composition of ultrafine aerosols connected to biomass burning.. Many events of high particulate matter concentrations (exceeding the 50 μg/m3 daily limit) were observed during night-time, with maximum concentrations occurring when stagnant atmospheric conditions prevailed. Potassium measured by the PILS - IC, and the m/z = 60 fragment measured by the ACSM, was initially used as a tracer of biomass burning events. A good correlation was determined for those two factors, allowing for safe conclusions concerning the identification of these aforementioned biomass burning events. For utmost certainty, Black Carbon measurements coming from three different instruments, was also used. As a second step, Positive Matrix Factorization analysis was performed, using the SoFi interface, which utilizes the generalized multilinear engine (ME-2) (Canonaco et Al., Atmos. Meas. Tech., 6, 3649-3661, 2013), for the source apportionment of the organic particulate matter, determined by the ACSM. This analysis revealed a very important Biomass Burning Organic Aerosol (BBOA) factor with a clear diurnal cycle, showing maxima in the time interval from 21:00 in the evening to 02:00 in the morning. A Hydrocarbon-like Organic Aerosol (HOA) factor is also present with a maximum during the same time interval, attributed to fossil fuel used in central heating systems, and a secondary maximum during the day, attributed

  18. Effects of brief and intermediate exposures to sulfate submicron aerosols and sulfate injections on cardiopulmonary function of dogs and tracheal mucous velocity of sheep

    Energy Technology Data Exchange (ETDEWEB)

    Sackner, M.A. (Mount Sinai Medical Center, Miami Beach, FL); Dougherty, R.L.; Chapman, G.A.; Cipley, J.; Perez, D.; Kwoka, M.; Reinhart, M.; Brito, M.; Schreck, R.

    1981-06-01

    Pulmonary mechanics of anesthetized dogs were not changed or were minimally altered by breathing the following compounds as submicron aerosols in concentrations up to 17.3 mg/m/sup 3/ for 7.5 min: (1) sodium chloride (as a control), (2) sodium sulfate, (3) ammonium sulfate, (4) zinc sulfate, (5) zinc ammonium sulfate, (6) ammonium bisulfate, (7) aluminum sulfate, (8) manganese sulfate, (9) nickel sulfate, (10) copper sulfate, (11) ferrous fulfate, and (12) ferric sulfate. Submicron aerosols of these compounds in concentrations of 4.1 to 8.8 mg/m/sup 3/, administered for 4 h to anesthetized dogs, did not affect mechanics of breathing, hemodynamics, and arterial blood gases. In conscious sheep, tracheal mucous velocity was not altered by exposure to the submicron aerosols of the sulfate compounds. None of these compounds, injected iv in a dose of 1 mg, had adverse effects on mechanics of breathing, pulmonary and systemic hemodynamics, or arterial blood gases. In 100-mg injections, zinc sulfate and zinc ammonium sulfate produced a fall in cardiac output, systemic hypotension, hypoxemia, and metabolic acidosis. Copper sulfate at this dose produced pulmonary hypertension, a fall in cardiac output, hypoxemia, respiratory acidosis, and a decrease of specific total respiratory conductance. It is concluded that submicron aerosols of sulfate salts do not have adverse cardiopulmonary effects when administered in high concentrations for up to 4 h. However, prolonged exposure to high concentrations of zinc sulfate, zinc ammonium sulfate, and copper sulfate aerosols might have adverse cardiopulmonary effects.

  19. Fluxes of Submicron Organic Aerosol above London Measured by Eddy Covariance using the Aerodyne HR-ToF-AMS

    Science.gov (United States)

    Phillips, G. J.; di Marco, C. F.; Farmer, D.; Kimmel, J. R.; Jimenez, J. L.; Nemitz, E.

    2009-12-01

    Urban centres are large sources of sub-micron particles. The myriad of emission sources combined with the complex interaction between regional aerosol and the particulate and gaseous photochemistry make for a complex system. It is evident that particulate emissions from cities will affect the regional atmosphere as well as the environment within the urban area. Aerosol particles have been associated with respiratory and cardio-vascular disease and are also linked with the climate through scattering of radiation and indirect effects such as cloud formation. The Aerodyne Aerosol Mass Spectrometer (AMS) provides a powerful tool to elucidate the sources and processing of organic aerosol in the urban atmosphere. Normally this is done through concentration measurements, by statistical analysis of the organic mass spectra, e.g. using Positive Matrix Factorization (PMF). Recently the quadrupole based AMS (Q-AMS) has been used for the micrometeorological measurement of organic aerosol fluxes above several cities, based on high frequency measurements of individual masses (m/z) representative of different organic mass fractions. While providing a major step forward towards quantification of urban organic aerosol emissions and processing, the interpretation of Q-AMS flux data requires assumptions to scale up signals on individual m/z to total organic mass fluxes. In this paper we present chemically-speciated and size-segregated number aerosol fluxes measured using the next generation eddy covariance flux system based on the Aerodyne HR-ToF-AMS, now capable of recording fast-response eddy-covariance time-series of all m/z simultaneously. This allows organic mass fluxes to be calculated more quantitatively and provides 'flux mass spectra' in addition to concentration mass spectra, which produces novel information on the local emission and processing of organic aerosols in the urban environment, while concentration analysis includes the regional background. The measurements were

  20. Aerosol composition of the tropical upper troposphere

    Directory of Open Access Journals (Sweden)

    K. D. Froyd

    2009-07-01

    Full Text Available Aerosol composition was measured by the NOAA single-particle mass spectrometer (PALMS aboard the NASA WB-57 high altitude aircraft platform during two Aura Validation Experiment (AVE campaigns based in Costa Rica in 2004 and 2006. These studies yielded the most complete set of aerosol composition measurements to date throughout the tropical tropopause layer (TTL and tropical lower stratosphere. We describe the aerosol properties of the tropical atmosphere and use composition tracers to examine particle sources, the role of recent convection, and cirrus-forming potential in the TTL. Tropical dynamics and regional air sources played principal roles in dictating tropospheric aerosol properties. There was a sharp change in aerosol chemical composition at about 12 km altitude coincident with a change in convective influence. Below this level, maritime convection lofted condensable material that generated acidic, sulfate-rich aerosol. These particles contained significant amounts of methanesulfonic acid (MSA and showed evidence of cloud processes. In contrast, continental convection injected particles and precursors directly into the TTL, yielding a population of neutralized, organic-rich aerosol. The organics were often highly oxidized and particles with oxidized organics also contained nitrate. Above the tropopause, chemical composition gradually changed toward sulfuric acid particles but neutralized particles were still abundant 2 km above the tropopause. Deep continental convection, though sporadic and geographically localized, may strongly influence TTL aerosol properties on a global scale. The abundance of organic-rich aerosol may inhibit ice nucleation and formation of tropopause level cirrus.

  1. Biogenic influence on the composition and growth of summertime Arctic aerosol

    Science.gov (United States)

    Willis, M. D.; Burkart, J.; Thomas, J. L.; Koellner, F.; Schneider, J.; Bozem, H.; Hoor, P. M.; Aliabadi, A. A.; Schulz, H.; Herber, A. B.; Leaitch, R.; Abbatt, J.

    2016-12-01

    The summertime Arctic lower troposphere is a relatively pristine background aerosol environment dominated by nucleation and Aitken mode particles. Understanding the mechanisms that control the formation and growth of aerosol is crucial for our ability to predict cloud properties and therefore radiative balance and climate. We present aircraft-based observations of submicron aerosol composition from an aerosol mass spectrometer made during the NETCARE 2014 summertime arctic campaign, based in the Canadian High Arctic, at Resolute Bay, NU (74°N). Under stable and regionally influenced atmospheric conditions with low carbon monoxide and black carbon concentrations ( 6 with evidence for enhancement within the lower boundary layer. Methanesulfonic acid (MSA), a marker for the contribution of ocean-derived biogenic sulphur, was also observed in submicron aerosol. MSA-to-sulfate ratios ranged from near zero to 0.3 and tended to increase within the lower boundary layer, suggesting a contribution to aerosol loading from the ocean. In one notable case while flying in the lower boundary layer above open water in Lancaster Sound, we observed growth of small particles, <20 nm in diameter, into sizes above 50 nm. Aerosol growth was correlated with the presence of organic species, trimethylamine, and MSA in particles 80 nm and larger, where the organics were similar to those previously observed in marine settings. The organic-rich aerosol contributed significantly to particles active as cloud condensation nuclei (CCN, supersaturation = 0.6%). Our results highlight the potential importance of secondary organic aerosol formation and its role in growing nucleation mode aerosol into CCN-active sizes in this remote marine environment.

  2. Trends and sources of ozone and sub-micron aerosols at the Mt. Bachelor Observatory during 2004-2015

    Science.gov (United States)

    Zhang, L.; Jaffe, D. A.; Hee, J.

    2016-12-01

    Tropospheric ozone (O3) and airborne particles have significant impacts on human health and the environment. The Mt. Bachelor Observatory (MBO, 2.8 km a.s.l.) in Central Oregon, USA, now has one of the longest continuous free tropospheric records of O3, CO and aerosols in North America. In this study, we report on sources and trends of O3 and sub-micron aerosol scattering at MBO for 2004-2015. For O3, the seasonal cycle shows a bimodal pattern with peaks in April and July, while aerosol scattering (σsp) is lognormally distributed with a very high average in August and a smaller maximum in May. Mean O3 concentrations show a positive and significant trend in all seasons except winter, with an increase of approximately 0.6 ppb/year. This trend appears to be driven by Asian pollution in spring and regional wildfires in summer. For aerosol scattering, we see a significant increase only in summer, driven by recent increases in wildfire activity in the western US. Monthly criteria for isolating free troposphere (FT) and boundary layer (BL) air masses at MBO were obtained based on comparison of MBO water vapor (WV) distributions to those of Salem (SLE) and Medford (MFR), Oregon at equivalent pressure level. In all seasons, FT O3 is, on average, higher than BL O3, but the seasonal patterns are rather similar. For σsp the mean in summer is significantly higher than the FT, indicating the importance of regional wildfire smoke. We have identified four types of air masses that impact O3, CO and aerosols: Asian long range transport (ALRT), regional wildfires, regional industrial pollution, and upper troposphere and lower stratosphere (UTLS) intrusions. Over the 12 years of observations, we have identified 204 individual plume events based on the criteria of 8 consecutive polluted hours with elevated σsp, O3 or CO. Multi-pollutant correlations and backward trajectories were used to differentiate background source categories. A series of enhancement ratios (ERs) including

  3. Source apportionment of submicron organic aerosol collected from Atlanta, Georgia, during 2014-2015 using the aerosol chemical speciation monitor (ACSM)

    Science.gov (United States)

    Rattanavaraha, Weruka; Canagaratna, Manjula R.; Budisulistiorini, Sri Hapsari; Croteau, Philip L.; Baumann, Karsten; Canonaco, Francesco; Prevot, Andre S. H.; Edgerton, Eric S.; Zhang, Zhenfa; Jayne, John T.; Worsnop, Douglas R.; Gold, Avram; Shaw, Stephanie L.; Surratt, Jason D.

    2017-10-01

    The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) was redeployed at the Jefferson Street (JST) site in downtown Atlanta, Georgia (GA) for 1 year (March 20, 2014-February 08, 2015) to chemically characterize non-refractory submicron particulate matter (NR-PM1) in near real-time and to assess whether organic aerosol (OA) types and amounts change from year-to-year. Submicron organic aerosol (OA) mass spectra were analyzed by season using multilinear engine (ME-2) to apportion OA subtypes to potential sources and chemical processes. A suite of real-time collocated measurements from the Southeastern Aerosol Research and Characterization (SEARCH) network was compared with ME-2 factor solutions to aid in the interpretation of OA subtypes during each season. OA tracers measured from high-volume filter samples using gas chromatography interfaced with electron ionization-mass spectrometry (GC/EI-MS) also aided in identifying OA sources. The initial application of ME-2 to the yearlong ACSM dataset revealed that OA source apportionment by season was required to better resolve sporadic OA types. Spring and fall OA mass spectral datasets were separated into finer periods to capture potential OA sources resulting from non-homogeneous emissions during transitioning periods. NR-PM1 was highest in summer (16.7 ± 8.4 μg m-3) and lowest in winter (8.0 ± 5.7 μg m-3), consistent with prior studies. OA dominated NR-PM1 mass (56-74% on average) in all seasons. Hydrocarbon-like OA (HOA) from primary emissions was observed in all seasons, averaging 5-22% of total OA mass. Strong correlations of HOA with carbon monoxide (CO) (R = 0.71-0.88) and oxides of nitrogen (NOx) (R = 0.55-0.79) indicated that vehicular traffic was the likely source. Biomass burning OA (BBOA) was observed in all seasons, with lower contributions (2%) in summer and higher in colder seasons (averaging 8-20% of total OA mass). BBOA correlated strongly with levoglucosan (R = 0.78-0.95) during colder seasons

  4. Trends and sources of ozone and sub-micron aerosols at the Mt. Bachelor Observatory (MBO) during 2004-2015

    Science.gov (United States)

    Zhang, Lei; Jaffe, Daniel A.

    2017-09-01

    In this paper, we report the climatology of tropospheric ozone (O3) and sub-micron aerosol scattering at the Mt. Bachelor Observatory (MBO, 2.8 km asl) in central Oregon, USA, during 2004-2015. The seasonal cycle for O3 showed a bimodal pattern with peaks in April and July, while aerosol scattering (σsp) was lognormally distributed with a very high peak in August and a smaller peak in May. The mean O3 concentrations showed positive and significant trends in all seasons except winter, with a slope of 0.6-0.8 ppbv yr-1. Monthly criteria for isolating free tropospheric (FT) and boundary layer influenced (BLI) air masses at MBO were obtained based on comparison of MBO water vapor (WV) distributions to those of Salem (SLE) and Medford (MFR), Oregon, at equivalent pressure level. In all seasons, FT O3 was, on average, higher than BLI O3, but the seasonal patterns were rather similar. For σsp the FT mean in spring was higher, but the BLI mean in summer was significantly higher, indicating the importance of regional wildfire smoke. To better understand the causes for the seasonal and interannual trends at MBO, we identified four major categories of air masses that impact O3, carbon monoxide (CO) and aerosols: upper troposphere and lower stratosphere (UTLS) O3 intrusion, Asian long-range transport (ALRT), Arctic air pollution (AAP) and plumes from the Pacific Northwest region (PNW). ALRT and PNW plumes can be further divided into wildfires (WF), industrial pollution (IP) and mineral dust (MD). Over the 12 years of observations, 177 individual plume events have been identified. Enhancement ratios (ERs) and Ångström exponents (AEs) of aerosols were calculated for all events. The lowest slope of Δσsp/ΔO3 is a unique feature of UTLS events. PNW-WF events have the highest averages for Δσsp/ΔCO, Δσsp/ΔO3 and Δσsp/ΔNOy compared to other events. These ERs decrease during long-range transport due to the shorter residence time of aerosols compared to the other

  5. Assessment of the diffusion battery for determining low concentration submicron aerosol distributions in microelectronics clean rooms

    Energy Technology Data Exchange (ETDEWEB)

    Locke, B.R.; Donovan, R.P.; Ensor, D.S.; Caviness, A.L.

    Traditional particle size determinations for aerosols below 0.1 ..mu..m diameter have been made by both electrical mobility and diffusional methods. Difficulties in determining particle size spectra in the sub-0.1-..mu..m diameter range arise when air from microelectronics manufacturing cleanrooms is sampled because of the low concentration of particulates and the low sampling rates of currently available instruments. Previously reported data indicate that the differential electrical mobility method does not provide reliable aerosol distributions for concentrations below about 1 particle/cm/sup 3/. Laboratory and operating cleanroom measurements with the collimated hole diffusion battery gave particle distributions spanning the range from about 0.001 particles/cm/sup 3/ to 1 x 10/sup 5/ particles/cm/sup 3/. The low concentration particle spectra in cleanrooms at rest showed peak aerosol concentrations at about 0.1 ..mu..m with few particles at sizes below this peak.

  6. Relative contribution of submicron and supermicron particles to aerosol light scattering in the marine boundary layer

    NARCIS (Netherlands)

    Kleefeld, C.; O'Dowd, C.D.; O'Reilly, S.; Jennings, S.G.; Aalto, P.; Becker, E.; Kunz, G.J.; Leeuw, G. de

    2002-01-01

    Measurements of the aerosol light scattering coefficient (σsp) at a wavelength of λ - 550 nm were conducted at a coastal atmospheric research station in the east Atlantic Ocean during June 1999. Size distribution measurements between diameters of 3 nm and 40 um (at ambient humidity) were used to

  7. Quantification of the carbonaceous matter origin in submicron marine aerosol particles by dual carbon isotope analysis

    OpenAIRE

    D. Ceburnis; A. Garbaras; S. Szidat; M. Rinaldi; S. Fahrni; N. Perron; L. Wacker; S. Leinert; V. Remeikis; M. C. Facchini; A. S. H. Prevot; S. G. Jennings; C. D. O'Dowd

    2011-01-01

    Dual carbon isotope analysis has been performed for the first time demonstrating a potential in organic matter apportionment between three principal sources: marine, terrestrial (non-fossil) and fossil fuel due to unique isotopic signatures. The results presented here, utilising combinations of dual carbon isotope analysis, provides a conclusive evidence of a dominant biogenic organic fraction to organic aerosol over biologically active oceans. In particular, the NE Atlantic, which is...

  8. Light induced uptake of NO{sub 2} on submicron humic acid aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Kleffmann, Joerg; Elshorbany, Yasin [Bergische Universitaet Wuppertal (Germany); Ammann, Markus; Stemmler, Konrad [Paul Scherrer Institut, Villigen (Switzerland); Bohn, Birger [Forschungszentrum Juelich (Germany); George, Christian; Ndour, Marieme [University Claude Bernard, (UCBL-CNRS), Villeurbanne (France)

    2007-07-01

    Recent field studies have demonstrated that the contribution of HONO to the OH radical production during daytime has been underestimated and indicated the existence of strong photolytic sources of HONO. A potential source is the light induced heterogeneous conversion of NO{sub 2} into HONO on humic acid surfaces, which was recently investigated on bulk surfaces. In the present laboratory study, we extended these studies to humic acid aerosols, which were generated by a nebulizer. The aerosol was transferred into a flow reactor and irradiated (300-700 nm) under controlled atmospheric conditions (humidity, NO{sub 2} concentration, etc.). HONO was detected using a selective and sensitive instrument (LOPAP), while the particle surface was quantified by a SMPS and an electrostatic precipitator. Similar to our recent study on bulk surfaces, a clearly photoinduced formation of HONO was observed, which was linear correlated with the aerosol surface and the reaction time. The experimental results are compared with the bulk study and a mechanism is presented to explain the experimental observations. In addition, the contribution to the primary production of OH radicals in the atmosphere is estimated.

  9. The role of jet and film drops in controlling the mixing state of submicron sea spray aerosol particles.

    Science.gov (United States)

    Wang, Xiaofei; Deane, Grant B; Moore, Kathryn A; Ryder, Olivia S; Stokes, M Dale; Beall, Charlotte M; Collins, Douglas B; Santander, Mitchell V; Burrows, Susannah M; Sultana, Camille M; Prather, Kimberly A

    2017-07-03

    The oceans represent a significant global source of atmospheric aerosols. Sea spray aerosol (SSA) particles comprise sea salts and organic species in varying proportions. In addition to size, the overall composition of SSA particles determines how effectively they can form cloud droplets and ice crystals. Thus, understanding the factors controlling SSA composition is critical to predicting aerosol impacts on clouds and climate. It is often assumed that submicrometer SSAs are mainly formed by film drops produced from bursting bubble-cap films, which become enriched with hydrophobic organic species contained within the sea surface microlayer. In contrast, jet drops formed from the base of bursting bubbles are postulated to mainly produce larger supermicrometer particles from bulk seawater, which comprises largely salts and water-soluble organic species. However, here we demonstrate that jet drops produce up to 43% of total submicrometer SSA number concentrations, and that the fraction of SSA produced by jet drops can be modulated by marine biological activity. We show that the chemical composition, organic volume fraction, and ice nucleating ability of submicrometer particles from jet drops differ from those formed from film drops. Thus, the chemical composition of a substantial fraction of submicrometer particles will not be controlled by the composition of the sea surface microlayer, a major assumption in previous studies. This finding has significant ramifications for understanding the factors controlling the mixing state of submicrometer SSA particles and must be taken into consideration when predicting SSA impacts on clouds and climate.

  10. The role of jet and film drops in controlling the mixing state of submicron sea spray aerosol particles

    Science.gov (United States)

    Wang, Xiaofei; Deane, Grant B.; Moore, Kathryn A.; Ryder, Olivia S.; Stokes, M. Dale; Beall, Charlotte M.; Collins, Douglas B.; Santander, Mitchell V.; Burrows, Susannah M.; Sultana, Camille M.; Prather, Kimberly A.

    2017-07-01

    The oceans represent a significant global source of atmospheric aerosols. Sea spray aerosol (SSA) particles comprise sea salts and organic species in varying proportions. In addition to size, the overall composition of SSA particles determines how effectively they can form cloud droplets and ice crystals. Thus, understanding the factors controlling SSA composition is critical to predicting aerosol impacts on clouds and climate. It is often assumed that submicrometer SSAs are mainly formed by film drops produced from bursting bubble-cap films, which become enriched with hydrophobic organic species contained within the sea surface microlayer. In contrast, jet drops formed from the base of bursting bubbles are postulated to mainly produce larger supermicrometer particles from bulk seawater, which comprises largely salts and water-soluble organic species. However, here we demonstrate that jet drops produce up to 43% of total submicrometer SSA number concentrations, and that the fraction of SSA produced by jet drops can be modulated by marine biological activity. We show that the chemical composition, organic volume fraction, and ice nucleating ability of submicrometer particles from jet drops differ from those formed from film drops. Thus, the chemical composition of a substantial fraction of submicrometer particles will not be controlled by the composition of the sea surface microlayer, a major assumption in previous studies. This finding has significant ramifications for understanding the factors controlling the mixing state of submicrometer SSA particles and must be taken into consideration when predicting SSA impacts on clouds and climate.

  11. Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

    Science.gov (United States)

    Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

    2015-10-06

    Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.

  12. Aerosol carbon isotope composition over Baltic Sea

    Science.gov (United States)

    Garbaras, Andrius; Pabedinskas, Algirdas; Masalaite, Agne; Petelski, Tomasz; Gorokhova, Elena; Sapolaite, Justina; Ezerinskis, Zilvinas; Remeikis, Vidmantas

    2017-04-01

    Particulate carbonaceous matter is significant contributor to ambient particulate matter originating from intervening sources which contribution is difficult to quantify due to source diversity, chemical complexity and processes during atmospheric transport. Carbon isotope analysis can be extremely useful in source apportionment of organic matter due to the unique isotopic signatures associated with anthropocentric (fossil fuel), continental (terrestrial plants) and marine sources, and is particularly effective when these sources are mixed (Ceburnis et al., 2011;Ceburnis et al., 2016). We will present the isotope ratio measurement results of aerosol collected during the cruise in the Baltic Sea. Sampling campaign of PM10 and size segregated aerosol particles was performed on the R/V "Oceania" in October 2015. Air mass back trajectories were prevailing both from the continental and marine areas during the sampling period. The total carbon concentration varied from 1 µg/m3 to 8 µg/m3. Two end members (δ13C = -25‰ and δ13C = -28 ‰ ) were established from the total stable carbon isotope analysis in PM10 fraction. δ13C analysis in size segregated aerosol particles revealed δ13C values being highest in the 1 - 2.5 µm range (δ13C = -24.9 ‰ ) during continental transport, while lowest TC δ13C values (δ13C ≈ -27 ‰ ) were detected in the size range D50 matter origin in submicron marine aerosol by 13 C and 14 C isotope analysis, Atmospheric Chemistry and Physics, 11, 8593-8606, 2011. Ceburnis, D., Masalaite, A., Ovadnevaite, J., Garbaras, A., Remeikis, V., Maenhaut, W., Claeys, M., Sciare, J., Baisnée, D., and O'Dowd, C. D.: Stable isotopes measurements reveal dual carbon pools contributing to organic matter enrichment in marine aerosol, Scientific Reports, 6, 2016. Masalaite, A., Remeikis, V., Garbaras, A., Dudoitis, V., Ulevicius, V., and Ceburnis, D.: Elucidating carbonaceous aerosol sources by the stable carbon δ13C TC ratio in size

  13. Source apportionment of submicron organic aerosol at an urban background and a road site in Barcelona (Spain during SAPUSS

    Directory of Open Access Journals (Sweden)

    M. Alier

    2013-10-01

    Full Text Available This study investigates the contribution of potential sources to the submicron (PM1 organic aerosol (OA simultaneously detected at an urban background (UB and a road site (RS in Barcelona during the 30 days of the intensive field campaign of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies, September–October 2010. A total of 103 filters at 12 h sampling time resolution were collected at both sites. Thirty-six neutral and polar organic compounds of known emission sources and photo-chemical transformation processes were analyzed by gas chromatography–mass spectrometry (GC-MS. The concentrations of the trace chemical compounds analyzed are herein presented and discussed. Additionally, OA source apportionment was performed by multivariate curve resolution–alternating least squares (MCR-ALS and six OA components were identified at both sites: two were of primary anthropogenic OA origin and three of secondary OA origin, while a sixth one was not clearly defined. Primary organics from emissions of local anthropogenic activities (urban primary organic aerosol, or POA Urban, mainly traffic emissions but also cigarette smoke, contributed 43% (1.5 μg OC m−3 and 18% (0.4 μg OC m−3 to OA at RS and UB, respectively. A secondary primary source – biomass burning (BBOA – was found in all the samples (average values 7% RS; 12% UB; 0.3 μg OC m−3, but this component was substantially contributing to OA only when the sampling sites were under influence of regional air mass circulation (REG.. Three secondary organic aerosol (SOA components (describing overall 60% of the variance were observed in the urban ambient PM1. Products of isoprene oxidation (SOA ISO – i.e. 2-methylglyceric acid, C5 alkene triols and 2-methyltetrols – showed the highest abundance at both sites when the city was under influence of inland air masses. The overall concentrations of SOA ISO were similar at both sites (0.4 and 0.3 μg m−3, or 16% and 7%, at

  14. Do nanofill or submicron composites show improved smoothness and gloss? A systematic review of in vitro studies

    NARCIS (Netherlands)

    Kaizer, M.R.; Oliveira-Ogliari, A. de; Cenci, M.S.; Opdam, N.J.M.; Moraes, R.R.

    2014-01-01

    OBJECTIVES: Despite nanofill and submicron composites' aim to provide high initial polishing combined with superior smoothness and gloss retention, the question still remains whether clinicians should consider using these new materials over traditional microhybrids. The aim of this paper was to

  15. Seasonal variations of ultra-fine and submicron aerosols in Taipei, Taiwan: implications for particle formation processes in a subtropical urban area

    Directory of Open Access Journals (Sweden)

    H. C. Cheung

    2016-02-01

    Full Text Available The aim of this study is to investigate the seasonal variations in the physicochemical properties of atmospheric ultra-fine particles (UFPs, d ≤ 100 nm and submicron particles (PM1, d ≤ 1 µm in an east Asian urban area, which are hypothesized to be affected by the interchange of summer and winter monsoons. An observation experiment was conducted at TARO (Taipei Aerosol and Radiation Observatory, an urban aerosol station in Taipei, Taiwan, from October 2012 to August 2013. The measurements included the mass concentration and chemical composition of UFPs and PM1, as well as the particle number concentration (PNC and the particle number size distribution (PSD with size range of 4–736 nm. The results indicated that the mass concentration of PM1 was elevated during cold seasons with a peak level of 18.5 µg m−3 in spring, whereas the highest concentration of UFPs was measured in summertime with a mean of 1.64 µg m−3. Moreover, chemical analysis revealed that the UFPs and PM1 were characterized by distinct composition; UFPs were composed mostly of organics, whereas ammonium and sulfate were the major constituents of PM1. The seasonal median of total PNCs ranged from 13.9  ×  103 cm−3 in autumn to 19.4  ×  103 cm−3 in spring. Median concentrations for respective size distribution modes peaked in different seasons. The nucleation-mode PNC (N4 − 25 peaked at 11.6  ×  103 cm−3 in winter, whereas the Aitken-mode (N25 − 100 and accumulation-mode (N100 − 736 PNC exhibited summer maxima at 6.0  ×  103 and 3.1  ×  103 cm−3, respectively. The change in PSD during summertime was attributed to the enhancement in the photochemical production of condensable organic matter that, in turn, contributed to the growth of aerosol particles in the atmosphere. In addition, clear photochemical production of particles was observed, mostly in the summer season

  16. Characterization of aerosol chemical composition with aerosol mass spectrometry in Central Europe: an overview

    Directory of Open Access Journals (Sweden)

    V. A. Lanz

    2010-11-01

    Full Text Available Real-time measurements of non-refractory submicron aerosols (NR-PM1 were conducted within the greater Alpine region (Switzerland, Germany, Austria, France and Liechtenstein during several week-long field campaigns in 2002–2009. This region represents one of the most important economic and recreational spaces in Europe. A large variety of sites was covered including urban backgrounds, motorways, rural, remote, and high-alpine stations, and also mobile on-road measurements were performed. Inorganic and organic aerosol (OA fractions were determined by means of aerosol mass spectrometry (AMS. The data originating from 13 different field campaigns and the combined data have been utilized for providing an improved temporal and spatial data coverage.

    The average mass concentration of NR-PM1 for the different campaigns typically ranged between 10 and 30 μg m−3. Overall, the organic portion was most abundant, ranging from 36% to 81% of NR-PM1. Other main constituents comprised ammonium (5–15%, nitrate (8–36%, sulfate (3–26%, and chloride (0–5%. These latter anions were, on average, fully neutralized by ammonium. As a major result, time of the year (winter vs. summer and location of the site (Alpine valleys vs. Plateau could largely explain the variability in aerosol chemical composition for the different campaigns and were found to be better descriptors for aerosol composition than the type of site (urban, rural etc.. Thus, a reassessment of classifications of measurements sites might be considered in the future, possibly also for other regions of the world.

    The OA data was further analyzed using positive matrix factorization (PMF and the multi-linear engine ME (factor analysis separating the total OA into its underlying components, such as oxygenated (mostly secondary organic aerosol (OOA, hydrocarbon-like and freshly emitted organic aerosol (HOA, as well as OA from biomass

  17. Airborne measurement of submicron aerosol number concentration and CCN activity in and around the Korean Peninsula and their comparison to ground measurement in Seoul

    Science.gov (United States)

    Park, M.; Kim, N.; Yum, S. S.

    2016-12-01

    Aerosols exert impact not only on human health and visibility but also on climate change directly by scattering or absorbing solar radiation and indirectly by acting as cloud condensation nuclei (CCN) and thus altering cloud radiative and microphysical properties. Aerosol indirect effects on climate has been known to have large uncertainty because of insufficient measurement data on aerosol and CCN activity distribution. Submicron aerosol number concentration (NCN, TSI CPC) and CCN number concentration (NCCN, DMT CCNC) were measured on board the NASA DC-8 research aircraft and at a ground site at Olympic Park in Seoul from May 2nd to June 10th, 2016. CCNC on the airborne platform was operated with the fixed internal supersaturation of 0.6% and CCNC at the ground site was operated with the five different supersaturations (0.2%, 0.4%, 0.6%, 0.8%, and 1.0%). The NASA DC-8 conducted 20 research flights (about 150 hours) in and around the Korean Peninsula and the ground measurement at Olympic Park was continuously made during the measurement period. Both airborne and ground measurements showed spatially and temporally varied aerosol number concentration and CCN activity. Aerosol number concentration in the boundary layer measured on airborne platform was highly affected by pollution sources on the ground. The average diurnal distribution of ground aerosol number concentration showed distinct peaks are located at about 0800, 1500, and 2000. The middle peak indicates that new particle formation events frequently occurred during the measurement period. CCN activation ratio at 0.6% supersaturation (NCCN/NCN) of the airborne measurement ranged from 0.1 to 0.9, indicating that aerosol properties in and around the Korean Peninsula varied so much (e. g. size, hygroscopicity). Comprehensive analysis results will be shown at the conference.

  18. Change in global aerosol composition since preindustrial times

    NARCIS (Netherlands)

    Tsigaridis, K.; Krol, M.C.; Dentener, F.; Balkanski, Y.; Lathiere, J.; Metzger, S.; Hauglustaine, D.; Kanakidou, M.

    2006-01-01

    To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. The present 3-D modeling study focuses on aerosol chemical composition change since preindustrial

  19. Change in global aerosol composition since preindustrial times

    Directory of Open Access Journals (Sweden)

    K. Tsigaridis

    2006-01-01

    Full Text Available To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. The present 3-D modeling study focuses on aerosol chemical composition change since preindustrial times considering the secondary organic aerosol formation together with all other main aerosol components including nitrate. In particular, we evaluate non-sea-salt sulfate (nss-SO4=, ammonium (NH4+, nitrate (NO3−, black carbon (BC, sea-salt, dust, primary and secondary organics (POA and SOA with a focus on the importance of secondary organic aerosols. Our calculations show that the aerosol optical depth (AOD has increased by about 21% since preindustrial times. This enhancement of AOD is attributed to a rise in the atmospheric load of BC, nss-SO4=, NO3, POA and SOA by factors of 3.3, 2.6, 2.7, 2.3 and 1.2, respectively, whereas we assumed that the natural dust and sea-salt sources remained constant. The nowadays increase in carbonaceous aerosol loading is dampened by a 34–42% faster conversion of hydrophobic to hydrophilic carbonaceous aerosol leading to higher removal rates. These changes between the various aerosol components resulted in significant modifications of the aerosol chemical composition. The relative importance of the various aerosol components is critical for the aerosol climatic effect, since atmospheric aerosols behave differently when their chemical composition changes. According to this study, the aerosol composition changed significantly over the different continents and with height since preindustrial times. The presence of anthropogenically emitted primary particles in the atmosphere facilitates the condensation of the semi-volatile species that form SOA onto the aerosol phase, particularly in the boundary layer. The SOA burden that is dominated by the natural component has increased by 24% while its contribution to the AOD

  20. Quantification of the carbonaceous matter origin in submicron marine aerosol by 13C and 14C isotope analysis

    Directory of Open Access Journals (Sweden)

    M. Ramonet

    2011-08-01

    Full Text Available Dual carbon isotope analysis of marine aerosol samples has been performed for the first time demonstrating a potential in organic matter apportionment between three principal sources: marine, terrestrial (non-fossil and fossil fuel due to unique isotopic signatures. The results presented here, utilising combinations of dual carbon isotope analysis, provides conclusive evidence of a dominant biogenic organic fraction to organic aerosol over biologically active oceans. In particular, the NE Atlantic, which is also subjected to notable anthropogenic influences via pollution transport processes, was found to contain 80 % organic aerosol matter of biogenic origin directly linked to plankton emissions. The remaining carbonaceous aerosol was of terrestrial origin. By contrast, for polluted air advected out from Europe into the NE Atlantic, the source apportionment is 30 % marine biogenic, 40 % fossil fuel, and 30 % continental non-fossil fuel. The dominant marine organic aerosol source in the atmosphere has significant implications for climate change feedback processes.

  1. The heterogeneous reaction of hydroxyl radicals with sub-micron squalane particles: a model system for understanding the oxidative aging of ambient aerosols

    Science.gov (United States)

    Smith, J. D.; Kroll, J. H.; Cappa, C. D.; Che, D. L.; Liu, C. L.; Ahmed, M.; Leone, S. R.; Worsnop, D. R.; Wilson, K. R.

    2009-05-01

    The heterogeneous reaction of OH radicals with sub-micron squalane particles, in the presence of O2, is used as a model system to explore the fundamental chemical mechanisms that control the oxidative aging of organic aerosols in the atmosphere. Detailed kinetic measurements combined with elemental mass spectrometric analysis reveal that the reaction proceeds sequentially by adding an average of one oxygenated functional group per reactive loss of squalane. The reactive uptake coefficient of OH with squalane particles is determined to be 0.3±0.07 at an average OH concentration of ~1×1010 molecules cm-3. Based on a comparison between the measured particle mass and model predictions it appears that significant volatilization of a reduced organic particle would be extremely slow in the real atmosphere. However, as the aerosols become more oxygenated, volatilization becomes a significant loss channel for organic material in the particle-phase. Together these results provide a chemical framework in which to understand how heterogeneous chemistry transforms the physiochemical properties of particle-phase organic matter in the troposphere.

  2. The heterogeneous reaction of hydroxyl radicals with sub-micron squalane particles: a model system for understanding the oxidative aging of ambient aerosols

    Directory of Open Access Journals (Sweden)

    J. D. Smith

    2009-05-01

    Full Text Available The heterogeneous reaction of OH radicals with sub-micron squalane particles, in the presence of O2, is used as a model system to explore the fundamental chemical mechanisms that control the oxidative aging of organic aerosols in the atmosphere. Detailed kinetic measurements combined with elemental mass spectrometric analysis reveal that the reaction proceeds sequentially by adding an average of one oxygenated functional group per reactive loss of squalane. The reactive uptake coefficient of OH with squalane particles is determined to be 0.3±0.07 at an average OH concentration of ~1×1010 molecules cm−3. Based on a comparison between the measured particle mass and model predictions it appears that significant volatilization of a reduced organic particle would be extremely slow in the real atmosphere. However, as the aerosols become more oxygenated, volatilization becomes a significant loss channel for organic material in the particle-phase. Together these results provide a chemical framework in which to understand how heterogeneous chemistry transforms the physiochemical properties of particle-phase organic matter in the troposphere.

  3. Surfactants and submicron sea spray generation

    NARCIS (Netherlands)

    Sellegri, K.; O'Dowd, C.D.; Yoon, Y.J.; Jennings, S.G.; Leeuw, G. de

    2006-01-01

    Laboratory experiments have been carried out to elucidate the role of surfactants on the primary marine aerosol production of submicron marine aerosols. A synthetic surfactant SDS was used in conjunction with artificially generated seawater, and the resultant bubble-mediated aerosol produced was

  4. Molecular Diversity of Sea Spray Aerosol Particles: Impact of Ocean Biology on Particle Composition and Hygroscopicity

    Energy Technology Data Exchange (ETDEWEB)

    Cochran, Richard E.; Laskina, Olga; Trueblood, Jonathan; Estillore, Armando D.; Morris, Holly S.; Jayarathne, Thilina; Sultana, Camile M.; Lee, Christopher; Lin, Peng; Laskin, Julia; Laskin, Alexander; Dowling, Jackie; Qin, Zhen; Cappa, Christopher; Bertram, Timothy; Tivanski, Alexei V.; Stone, Elizabeth; Prather, Kimberly; Grassian, Vicki H.

    2017-05-01

    The impact of sea spray aerosol (SSA) on climate depends on the size and chemical composition of individual particles that make-up the total SSA ensemble. While the organic fraction of SSA has been characterized from a bulk perspective, there remains a lack of understanding as to the composition of individual particles within the SSA ensemble. To better understand the molecular components within SSA particles and how SSA composition changes with ocean biology, simultaneous measurements of seawater and SSA were made during a month-long mesocosm experiment performed in an ocean-atmosphere facility. Herein, we deconvolute the composition of freshly emitted SSA devoid of anthropogenic and terrestrial influences by characterizing classes of organic compounds as well as specific molecules within individual SSA particles. Analysis of SSA particles show that the diversity of molecules within the organic fraction varies between two size fractions (submicron and supermicron) with contributions from fatty acids, monosaccharides, polysaccharides and siliceous material. Significant changes in the distribution of these compounds within individual particles are observed to coincide with the rise and fall of phytoplankton and bacterial populations within the seawater. Furthermore, water uptake is impacted as shown by hygroscopicity measurements of model systems composed of representative organic compounds. Thus, the how changes in the hygroscopic growth of SSA evolves with composition can be elucidated. Overall, this study provides an important connection between biological processes that control the composition of seawater and changes in single particle composition which will enhances our ability to predict the impact of SSA on climate.

  5. Thermal, structural and morphological properties of High Density Polyethylene matrix composites reinforced with submicron agro silica particles and Titania particles

    Directory of Open Access Journals (Sweden)

    Oluyemi O. Daramola

    2017-07-01

    Full Text Available HDPE—based composites samples filled with 2, 4, 6, 8 and 10 wt.% submicron agro-waste silica particles extracted from rice husk ash (RHA at constant 0.3 wt.% Titania loading were prepared using rapra single screw extruder at temperature of 200–230 °C. The extrudates were compressed with a laboratory carver press at a temperature of 230 °C for 10 min under applied pressure of 0.2 kPa and water cooled at 20 °C min−1. Thermal, structural and morphological properties of the composites were studied. The results of the thermogravimetric analysis (TGA revealed that the composites with 10 wt.% SiO2 have the best maximum thermal degradation temperature of 438.73 °C. The crystal structure of neat HDPE, and the siliceous composites developed revealed two obvious diffractive peaks of about 21.3° and 23.7° corresponding to typical crystal plane (1 1 0 and (2 0 0 of orthorhombic phase respectively. The diffractive peaks do not shift with the addition of silica particles; this clearly indicates that the addition of silica particles did not exert much effect on the crystalline structure of HDPE. There is no much difference in the interplanar distance (d-value. Lamellar thickness (L of HDPE increases with the addition of silica particles, which implies that silica particles aid the formation of more perfect crystals. Scanning electron microscopy studies indicated that there were chains inter diffusion and entanglement between HDPE matrix and the silica particles at lower weight fraction (2–4 wt.% of submicron silica particles which resulted into homogeneous dispersion of the particles within the matrix.

  6. Chemical composition of free tropospheric aerosol for PM1 and coarse mode at the high alpine site Jungfraujoch

    Directory of Open Access Journals (Sweden)

    J. Cozic

    2008-01-01

    Full Text Available The chemical composition of submicron (fine mode and supermicron (coarse mode aerosol particles has been investigated at the Jungfraujoch high alpine research station (3580 m a.s.l., Switzerland as part of the GAW aerosol monitoring program since 1999. A clear seasonality was observed for all major components throughout the period with low concentrations in winter (predominantly free tropospheric aerosol and higher concentrations in summer (enhanced vertical transport of boundary layer pollutants. In addition, mass closure was attempted during intensive campaigns in March 2004, February–March 2005 and August 2005. Ionic, carbonaceous and non-refractory components of the aerosol were quantified as well as the PM1 and coarse mode total aerosol mass concentrations. A relatively low conversion factor of 1.8 for organic carbon (OC to particulate organic matter (OM was found in winter (February–March 2005. Organics, sulfate, ammonium, and nitrate were the major components of the fine aerosol fraction that were identified, while calcium and nitrate were the only two measured components contributing to the coarse mode. The aerosol mass concentrations for fine and coarse mode aerosol measured during the intensive campaigns were not typical of the long-term seasonality due largely to dynamical differences. Average fine and coarse mode concentrations during the intensive field campaigns were 1.7 μg m−3 and 2.4 μg m−3 in winter and 2.5 μg m−3 and 2.0 μg m−3 in summer, respectively. The mass balance of aerosols showed higher contributions of calcium and nitrate in the coarse mode during Saharan dust events (SDE than without SDE.

  7. Influence of biomass burning on mixing state of sub-micron aerosol particles in the North China Plain

    Science.gov (United States)

    Kecorius, Simonas; Ma, Nan; Teich, Monique; van Pinxteren, Dominik; Zhang, Shenglan; Gröβ, Johannes; Spindler, Gerald; Müller, Konrad; Iinuma, Yoshiteru; Hu, Min; Herrmann, Hartmut; Wiedensohler, Alfred

    2017-09-01

    Particulate emissions from crop residue burning decrease the air quality as well as influence aerosol radiative properties on a regional scale. The North China Plain (NCP) is known for the large scale biomass burning (BB) of field residues, which often results in heavy haze pollution episodes across the region. We have been able to capture a unique BB episode during the international CAREBeijing-NCP intensive field campaign in Wangdu in the NCP (38.6°N, 115.2°E) from June to July 2014. It was found that aerosol particles originating from this BB event showed a significantly different mixing state compared with clean and non-BB pollution episodes. BB originated particles showed a narrower probability density function (PDF) of shrink factor (SF). And the maximum was found at shrink factor of 0.6, which is higher than in other episodes. The non-volatile particle number fraction during the BB episode decreased to 3% and was the lowest measured value compared to all other predefined episodes. To evaluate the influence of particle mixing state on aerosol single scattering albedo (SSA), SSA at different RHs was simulated using the measured aerosol physical-chemical properties. The differences between the calculated SSA for biomass burning, clean and pollution episodes are significant, meaning that the variation of SSA in different pollution conditions needs to be considered in the evaluation of aerosol direct radiative effects in the NCP. And the calculated SSA was found to be quite sensitive on the mixing state of BC, especially at low-RH condition. The simulated SSA was also compared with the measured values. For all the three predefined episodes, the measured SSA are very close to the calculated ones with assumed mixing states of homogeneously internal and core-shell internal mixing, indicating that both of the conception models are appropriate for the calculation of ambient SSA in the NCP.

  8. Size-specific composition of aerosols in the El Chichon volcanic cloud

    Science.gov (United States)

    Woods, D. C.; Chuan, R. L.

    1983-01-01

    A NASA U-2 research aircraft flew sampling missions in April, May, July, November, and December 1982 aimed at obtaining in situ data in the stratospheric cloud produced from the March-April 1982 El Chichon eruptions. Post flight analyses provided information on the aerosol composition and morphology. The particles ranged in size from smaller than 0.05 m to larger than 20 m diameter and were quite complex in composition. In the April, May, and July samples the aerosol mass was dominated by magmatic and lithic particles larger than about 3 m. The submicron particles consisted largely of sulfuric acid. Halite particles, believed to be related to a salt dome beneath El Chichon, were collected in the stratosphere in April and May. On the July 23 flight, copper-zinc oxide particles were collected. In July, November, and December, in addition to the volcanic ash and acid particles, carbon-rich particles smaller than about 0.1 m aerodynamic diameter were abundant.

  9. Efficiency of five chemical protective clothing materials against nano and submicron aerosols when submitted to mechanical deformations.

    Science.gov (United States)

    Ben Salah, Mehdi; Hallé, Stéphane; Tuduri, Ludovic

    2016-01-01

    Due to their potential toxicity, the use of nanoparticles in the workplace is a growing concern. Some studies indicate that nanoparticles can penetrate the skin and lead to adverse health effects. Since chemical protective clothing is the last barrier to protect the skin, this study aims to better understand nanoparticle penetration behaviour in dermal protective clothing under mechanical deformation. For this purpose, five of the most common types of fabrics used in protective clothing, one woven and four nonwoven, were chosen and submitted to different simulated exposure conditions. They were tested against polydispersed NaCl aerosols having an electrical-mobility diameter between 14 and 400 nm. A bench-scale exposure setup and a sampling protocol was developed to measure the level of penetration of the aerosols through the material samples of disposable coveralls and lab coat, while subjecting them to mechanical deformations to simulate the conditions of usage in the workplace. Particle size distribution of the aerosol was determined upstream and downstream using a scanning mobility particle sizer (SMPS). The measured efficiencies demonstrated that the performances of nonwoven materials were similar. Three nonwovens had efficiencies above 99%, while the woven fabric was by far, the least effective. Moreover, the results established that mechanical deformations, as simulated for this study, did not have a significant effect on the fabrics' efficiencies.

  10. Mexico City Aerosol Analysis During Milagro Using High Resolution Aerosol Mass Spectrometry at the Urban Supersite (T0) - Part 1: Fine Particle Composition and Organic Source Apportionment.

    OpenAIRE

    Aiken, A. C.; Foy, B. de; Wiedinmyer, C.; Ulbrich, I. M.; Wehrli, M. N.; Szidat, S.; Prevot, A. S. H.; Noda, J.; Wacker, L.; Volkamer, R.; Fortner, E. C.; Wang, J.; Laskin, A.; Shutthanandan, V.; Zheng, J.

    2010-01-01

    Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Aerosol Mass Spectrometer (AMS) and complementary instrumentation. Positive Matrix Factorization (PMF) of high resolution AMS spectra identified a biomass burning organic aerosol (BBOA) component, which includes several large plumes that appear to be from forest fires within the region. Here, we show that the AMS BBOA concentration at T0 correlates wit...

  11. Relating hygroscopicity and composition of organic aerosol particulate matter

    CERN Document Server

    Duplissy, J; Prevot, A S H; Barmpadimos, I; Jimenez, J L; Gysel, M; Worsnop, D R; Aiken, A C; Tritscher, T; Canagaratna, M R; Collins, D R; Alfarra, M R; Metzger, A; Tomlinson, J; DeCarlo, P F; Weingartner, E; Baltensperger, U

    2011-01-01

    A hygroscopicity tandem differential mobility analyzer (HTDMA) was used to measure the water uptake (hygroscopicity) of secondary organic aerosol (SOA) formed during the chemical and photochemical oxidation of several organic precursors in a smog chamber. Electron ionization mass spectra of the non-refractory submicron aerosol were simultaneously determined with an aerosol mass spectrometer (AMS), and correlations between the two different signals were investigated. SOA hygroscopicity was found to strongly correlate with the relative abundance of the ion signal m/z 44 expressed as a fraction of total organic signal (f(44)). m/z 44 is due mostly to the ion fragment CO(2)(+) for all types of SOA systems studied, and has been previously shown to strongly correlate with organic O/C for ambient and chamber OA. The analysis was also performed on ambient OA from two field experiments at the remote site Jungfrau-joch, and the megacity Mexico City, where similar results were found. A simple empirical linear relation b...

  12. Facile synthesis and stable cycling ability of hollow submicron silicon oxide–carbon composite anode material for Li-ion battery

    Energy Technology Data Exchange (ETDEWEB)

    Kim, Joong-Yeon; Nguyen, Dan Thien [Department of Fine Chemical Engineering & Applied Chemistry, Chungnam National University, Daejeon 305-764 (Korea, Republic of); Kang, Joon-Sup [Department of Energy Science and Technology, Chungnam National University, Daejeon 305-764 (Korea, Republic of); Song, Seung-Wan, E-mail: swsong@cnu.ac.kr [Department of Fine Chemical Engineering & Applied Chemistry, Chungnam National University, Daejeon 305-764 (Korea, Republic of); Department of Energy Science and Technology, Chungnam National University, Daejeon 305-764 (Korea, Republic of)

    2015-06-05

    Highlights: • Hollow submicron SiO{sub 2}–carbon composite material was synthesized using Si{sup 4+}-citrate chelation. • Composite material possessed a homogeneous distribution of SiO{sub 2} and carbon. • Composite electrode delivered ⩾600 mAh/g with a stable cycling stability. • This materials design and synthesis provides a useful platform for scalable production. - Abstract: Advanced SiO{sub 2}–carbon composite anode active material for lithium-ion battery has been synthesized through a simple chelation of silicon cation with citrate in a glyme-based solvent. The resultant composite material demonstrates a homogeneous distribution of constituents over the submicron particles and a unique hollow spherical microstructure, which provides an enhanced electrical conductivity and better accommodation of volume change of silicon during electrochemical charge–discharge cycling, respectively. As a result, the composite electrode exhibits a high cycling stability delivering the capacity retention of 91% at the 100th cycle and discharge capacities of 662–602 mAh/g and coulombic efficiencies of 99.8%. This material synthesis is scalable and cost-effective in preparing various submicron or micron composite electrode materials.

  13. Towards a quasi-complete reconstruction of past atmospheric aerosol load and composition (organic and inorganic over Europe since 1920 inferred from Alpine ice cores

    Directory of Open Access Journals (Sweden)

    S. Preunkert

    2013-07-01

    Full Text Available Seasonally resolved chemical ice core records available from the Col du Dôme glacier (4250 m elevation, French Alps, are here used to reconstruct past aerosol load and composition of the free European troposphere from before World War II to present. Available ice core records include inorganic (Na+, Ca2+, NH4+, Cl−, NO3−, and SO42− and organic (carboxylates, HCHO, humic-like substances, dissolved organic carbon, water-insoluble organic carbon, and black carbon compounds and fractions that permit reconstructing the key aerosol components and their changes over the past. It is shown that the atmospheric load of submicron aerosol has been increased by a factor of 3 from the 1921–1951 to 1971–1988 years, mainly as a result of a large increase of sulfate (a factor of 5, ammonium and water-soluble organic aerosol (a factor of 3. Thus, not only growing anthropogenic emissions of sulfur dioxide and ammonia have caused the enhancement of the atmospheric aerosol load but also biogenic emissions producing water-soluble organic aerosol. This unexpected change of biospheric source of organic aerosol after 1950 needs to be considered and further investigated in scenarios dealing with climate forcing by atmospheric aerosol.

  14. Aerosol characterization over the southeastern United States using high resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition, sources, and organic nitrates

    Science.gov (United States)

    Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

    2015-04-01

    We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particles (NR-PM1) in the southeastern US. Measurements were performed in both rural and urban sites in the greater Atlanta area, GA and Centreville, AL for approximately one year, as part of Southeastern Center of Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important but not dominant contributions to total OA in urban sites. Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA (Isoprene-OA) is only deconvolved in warmer months and contributes 18-36% of total OA. The presence of Isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79%) of OA in all sites. MO-OOA correlates well with ozone in summer, but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based on the HR-ToF-AMS measurements, we estimate that the nitrate functionality from organic nitrates

  15. Experimental investigation of aerosol composition and growth rates

    Science.gov (United States)

    Wimmer, Daniela; Winkler, Paul; Kulmala, Markku; Petäjä, Tuukka

    2017-04-01

    Atmospheric aerosol particles have relevant influence on human lives. Human health is affected, as by breathing in the aerosol particles, they deposit in the lungs causing various health problems. Also they interfere indirectly and directly with sunlight, which affects the climate on Earth. Primary aerosol particles originate for example from anthropogenic sources, such as Diesel cars or natural sources such as dessert dust. Secondary aerosol particles are formed via condensation of low volatile gas phase compounds. First, small clusters consisting of a few gas molecules only are formed, which can then grow to bigger aerosol particles. These then form seeds for cloud droplets. The chemical composition of the cloud particles determines whether the cloud absorbs or scatters sunlight more. Intensive experimental and theoretical work has been put into understanding the details of the initial processes leading to the natural formation of these secondary aerosol particles. According to modelling studies, aerosol particles formed via the nucleation process are responsible for about 50% of the global cloud condensation nuclei concentration. With currently used methods, the chemical composition of small molecular clusters (up to 2nm in diameter) can be resolved. Also standard methods to determine aerosol particle composition at sizes >10 nm are available. Within this project, the aerosol particle composition in the 2-4 nm size range will be investigated experimentally. The setup will consist of a combination of an electrical method that allows determine the electrical mobility of the particles which then can be converted to a diameter. By letting the charged particles travel through a changing electrical field, they travel at different speeds according to their mobility. That allows to particles with certain mobilities, which then can be converted to a diameter. After the size selection, the particles are counted by means of optical detection. Condensation particle counters

  16. Reconstruction of Aerosol Concentration and Composition from Glacier Ice Cores

    Science.gov (United States)

    Vogel, Alexander; Dällenbach, Kaspar; El-Haddad, Imad; Wendl, Isabel; Eichler, Anja; Schwikowski, Margit

    2017-04-01

    Reconstruction of the concentration and composition of natural aerosol in an undisturbed atmosphere enables the evaluation of the understanding of aerosol-climate effects, which is currently based on highly uncertain emission inventories of the biosphere under pre-industrial conditions. Understanding of the natural state of the pre-industrial atmosphere and evaluating the atmospheric perturbations by anthropogenic emissions, and their potential feedbacks, is essential for accurate model predictions of the future climate (Boucher et al., 2013). Here, we present a new approach for the chemical characterization of the organic fraction preserved in cold-glacier ice cores. From this analysis historic trends of atmospheric organic aerosols are reconstructed, allowing new insights on organic aerosol composition and mass in the pre-industrial atmosphere, which can help to improve climate models through evaluation of our current understanding of aerosol radiative effects. We present results from a proof-of-principal study, analyzing an 800 year ice core record from the Lomonosovfonna glacier ice core, drilled in 2009 in Svalbard, Norway, using a setup that has until then only been applied on offline measurements of aerosol filter extracts (Dällenbach et al., 2016): The melted ice was nebulized and dried, such that aerosols are formed from the soluble and insoluble organic and inorganic compounds that are preserved in the ice. To improve the sensitivity, the aerosol stream was then enriched by the application of an online aerosol concentrator, before the aerosol was analyzed by electron ionization within a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). We were able to demonstrate that this setup is a quantitative method toward nitrate and sulfate when internal inorganic standards of NH415NO3 and (NH4)234SO4 are added to the sample. Comparison between AMS and IC measurements of nitrate and sulfate resulted in an excellent agreement. The analysis of

  17. SiO2/ZnO Composite Hollow Sub-Micron Fibers: Fabrication from Facile Single Capillary Electrospinning and Their Photoluminescence Properties.

    Science.gov (United States)

    Song, Guanying; Li, Zhenjiang; Li, Kaihua; Zhang, Lina; Meng, Alan

    2017-02-24

    In this work, SiO2/ZnO composite hollow sub-micron fibers were fabricated by a facile single capillary electrospinning technique followed by calcination, using tetraethyl orthosilicate (TEOS), polyvinylpyrrolidone (PVP) and ZnO nanoparticles as raw materials. The characterization results of the scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FT-IR) spectra indicated that the asprepared composite hollow fibers consisted of amorphous SiO2 and hexagonal wurtzite ZnO. The products revealed uniform tubular structure with outer diameters of 400-500 nm and wall thickness of 50-60 nm. The gases generated and the directional escaped mechanism was proposed to illustrate the formation of SiO2/ZnO composite hollow sub-micron fibers. Furthermore, a broad blue emission band was observed in the photoluminescence (PL) of SiO2/ZnO composite hollow sub-micron fibers, exhibiting great potential applications as blue light-emitting candidate materials.

  18. SiO2/ZnO Composite Hollow Sub-Micron Fibers: Fabrication from Facile Single Capillary Electrospinning and Their Photoluminescence Properties

    Directory of Open Access Journals (Sweden)

    Guanying Song

    2017-02-01

    Full Text Available In this work, SiO2/ZnO composite hollow sub-micron fibers were fabricated by a facile single capillary electrospinning technique followed by calcination, using tetraethyl orthosilicate (TEOS, polyvinylpyrrolidone (PVP and ZnO nanoparticles as raw materials. The characterization results of the scanning electron microscopy (SEM, transmission electron microscopy (TEM, X-ray diffraction (XRD and Fourier transform infrared spectroscopy (FT-IR spectra indicated that the asprepared composite hollow fibers consisted of amorphous SiO2 and hexagonal wurtzite ZnO. The products revealed uniform tubular structure with outer diameters of 400–500 nm and wall thickness of 50–60 nm. The gases generated and the directional escaped mechanism was proposed to illustrate the formation of SiO2/ZnO composite hollow sub-micron fibers. Furthermore, a broad blue emission band was observed in the photoluminescence (PL of SiO2/ZnO composite hollow sub-micron fibers, exhibiting great potential applications as blue light-emitting candidate materials.

  19. Relating hygroscopicity and composition of organic aerosol particulate matter

    Energy Technology Data Exchange (ETDEWEB)

    Duplissy, J.; DeCarlo, P. F.; Dommen, J.; Alfarra, M. R.; Metzger, A.; Barmpadimos, I.; Prevot, A. S. H.; Weingartner, E.; Tritscher, T.; Gysel, M.; Aiken, A. C.; Jimenez, J. L.; Canagaratna, M. R.; Worsnop, D. R.; Collins, D. R.; Tomlinson, J.; Baltensperger, U.

    2011-01-01

    A hygroscopicity tandem differential mobility analyzer (HTDMA) was used to measure the water uptake (hygroscopicity) of secondary organic aerosol (SOA) formed during the chemical and photochemical oxidation of several organic precursors in a smog chamber. Electron ionization mass spectra of the non-refractory submicron aerosol were simultaneously determined with an aerosol mass spectrometer (AMS), and correlations between the two different signals were investigated. SOA hygroscopicity was found to strongly correlate with the relative abundance of the ion signal m/z 44 expressed as a fraction of total organic signal (f44). m/z 44 is due mostly to the ion fragment CO2+ for all types of SOA systems studied, and has been previously shown to strongly correlate with organic O/C for ambient and chamber OA. The analysis was also performed on ambient OA from two field experiments at the remote site Jungfraujoch, and the megacity Mexico City, where similar results were found. A simple empirical linear relation between the hygroscopicity of OA at subsaturated RH, as given by the hygroscopic growth factor (GF) or "κorg" parameter, and f44 was determined and is given by κorg = 2.2 × f44 - 0.13. This approximation can be further verified and refined as the database for AMS and HTDMA measurements is constantly being expanded around the world. Finally, the use of this approximation could introduce an important simplification in the parameterization of hygroscopicity of OA in atmospheric models, since f44 is correlated with the photochemical age of an air mass.

  20. Relating hygroscopicity and composition of organic aerosol particulate matter

    Directory of Open Access Journals (Sweden)

    J. Duplissy

    2011-02-01

    Full Text Available A hygroscopicity tandem differential mobility analyzer (HTDMA was used to measure the water uptake (hygroscopicity of secondary organic aerosol (SOA formed during the chemical and photochemical oxidation of several organic precursors in a smog chamber. Electron ionization mass spectra of the non-refractory submicron aerosol were simultaneously determined with an aerosol mass spectrometer (AMS, and correlations between the two different signals were investigated. SOA hygroscopicity was found to strongly correlate with the relative abundance of the ion signal m/z 44 expressed as a fraction of total organic signal (f44. m/z 44 is due mostly to the ion fragment CO2+ for all types of SOA systems studied, and has been previously shown to strongly correlate with organic O/C for ambient and chamber OA. The analysis was also performed on ambient OA from two field experiments at the remote site Jungfraujoch, and the megacity Mexico City, where similar results were found. A simple empirical linear relation between the hygroscopicity of OA at subsaturated RH, as given by the hygroscopic growth factor (GF or "ϰorg" parameter, and f44 was determined and is given by ϰorg = 2.2 × f44 − 0.13. This approximation can be further verified and refined as the database for AMS and HTDMA measurements is constantly being expanded around the world. The use of this approximation could introduce an important simplification in the parameterization of hygroscopicity of OA in atmospheric models, since f44 is correlated with the photochemical age of an air mass.

  1. Influence of locational states of submicron fibers added into matrix on mechanical properties of plain-woven Carbon Fiber Composite

    National Research Council Canada - National Science Library

    Soichiro Kumamoto; Kazuya Okubo; Toru Fujii

    2016-01-01

    The aim of this study was to show the influence of locational states of submicron fibers added into epoxy matrix on mechanical properties of modified plane-woven carbon fiber reinforced plastic (CFRP...

  2. The Hohenpeissenberg aerosol characterization experiment (HAZE2002): Aerosol composition derived from mass spectrometry

    Science.gov (United States)

    Hock, N.; Berresheim, H.; Borrmann, S.; Poeschl, U.; Roempp, A.; Schneider, J.

    2003-04-01

    The HAZE Experiment was conducted between 17.05.2002 and 31.05.2002, at the meteorological observatory of the Deutsche Wetterdienst (DWD) at Hohenpeissenberg (47^o48'N,11^o02'E, 985m). The objective was to make essential progress in understanding of the physical and chemical properties of the atmospheric aerosol, in particular relating to the Gas-To-Particle-Conversion and the interaction with meteorological processes. The measurements included online mass spectrometric analysis using the Aerosol Mass Spectrometer (AMS), filter samples with GC analyses of organic compounds, particle size distribution (Electrical Low Pressure Impactor (ELPI), SMPS, OPC), as well as the total particle concentration (CPC). Additionally, several gas-phase substances were measured (e.g. Benzene, Acetone). The measurements obtained with the AMS show a strong variability of the aerosol composition. The non-refractory aerosol composition was dominated by nitrate, sulphate, and organics, whereas ammonium was surprisingly low. High number concentration of up to 14000 particles/cm^3 were observed. These particles mostly had diameters between 200 nm and 400 nm and were mainly composed of ammonium sulphate and ammonium nitrate. Various meteorological conditions allowed to study their influence on the aerosol. For example, on rainy days the concentrations of ammonium sulphate particles decreased, whereas the concentrations of ammonium nitrate particles increased.

  3. Linking Remotely Sensed Aerosol Types to Their Chemical Composition

    Science.gov (United States)

    Dawson, Kyle William; Kacenelenbogen, Meloe S.; Johnson, Matthew S.; Burton, Sharon P.; Hostetler, Chris A.; Meskhidze, Nicholas

    2016-01-01

    Aerosol types measured during the Ship-Aircraft Bio-Optical Research (SABOR) experiment are related to GEOS-Chem model chemical composition. The application for this procedure to link model chemical components to aerosol type is desirable for understanding aerosol evolution over time. The Mahalanobis distance (DM) statistic is used to cluster model groupings of five chemical components (organic carbon, black carbon, sea salt, dust and sulfate) in a way analogous to the methods used by Burton et al. [2012] and Russell et al. [2014]. First, model-to-measurement evaluation is performed by collocating vertically resolved aerosol extinction from SABOR High Spectral Resolution LiDAR (HSRL) to the GEOS-Chem nested high-resolution data. Comparisons of modeled-to-measured aerosol extinction are shown to be within 35% +/- 14%. Second, the model chemical components are calculation into five variables to calculate the DM and cluster means and covariances for each HSRL-retrieved aerosol type. The layer variables from the model are aerosol optical depth (AOD) ratios of (i) sea salt and (ii) dust to total AOD, mass ratios of (iii) total carbon (i.e. sum of organic and black carbon) to the sum of total carbon and sulfate (iv) organic carbon to black carbon, and (v) the natural log of the aerosol-to-molecular extinction ratio. Third, the layer variables and at most five out of twenty SABOR flights are used to form the pre-specified clusters for calculating DM and to assign an aerosol type. After determining the pre-specified clusters, model aerosol types are produced for the entire vertically resolved GEOS-Chem nested domain over the United States and the model chemical component distributions relating to each type are recorded. Resulting aerosol types are Dust/Dusty Mix, Maritime, Smoke, Urban and Fresh Smoke (separated into 'dark' and 'light' by a threshold of the organic to black carbon ratio). Model-calculated DM not belonging to a specific type (i.e. not meeting a threshold

  4. Linking remotely sensed aerosol types to their chemical composition

    Science.gov (United States)

    Dawson, K. W.; Kacenelenbogen, M. S.; Johnson, M. S.; Burton, S. P.; Hostetler, C. A.; Meskhidze, N.

    2016-12-01

    Aerosol types measured during the Ship-Aircraft Bio-Optical Research (SABOR) experiment are related to GEOS-Chem model chemical composition. The application for this procedure to link model chemical components to aerosol type is desirable for understanding aerosol evolution over time. The Mahalanobis distance (DM) statistic is used to cluster model groupings of five chemical components (organic carbon, black carbon, sea salt, dust and sulfate) in a way analogous to the methods used by Burton et al. [2012] and Russell et al. [2014]. First, model-to-measurement evaluation is performed by collocating vertically resolved aerosol extinction from SABOR High Spectral Resolution LiDAR (HSRL) to the GEOS-Chem nested high-resolution data. Comparisons of modeled-to-measured aerosol extinction are shown to be within 35% ± 14%. Second, the model chemical components are calculation into five variables to calculate the DM and cluster means and covariances for each HSRL-retrieved aerosol type. The layer variables from the model are aerosol optical depth (AOD) ratios of (i) sea salt and (ii) dust to total AOD, mass ratios of (iii) total carbon (i.e. sum of organic and black carbon) to the sum of total carbon and sulfate (iv) organic carbon to black carbon, and (v) the natural log of the aerosol-to-molecular extinction ratio. Third, the layer variables and at most five out of twenty SABOR flights are used to form the pre-specified clusters for calculating DM and to assign an aerosol type. After determining the pre-specified clusters, model aerosol types are produced for the entire vertically resolved GEOS-Chem nested domain over the United States and the model chemical component distributions relating to each type are recorded. Resulting aerosol types are Dust/Dusty Mix, Maritime, Smoke, Urban and Fresh Smoke (separated into `dark' and `light' by a threshold of the organic to black carbon ratio). Model-calculated DM not belonging to a specific type (i.e. not meeting a threshold

  5. Characterization of submicron particles influenced by mixed biogenic and anthropogenic emissions using high-resolution aerosol mass spectrometry: results from CARES

    Energy Technology Data Exchange (ETDEWEB)

    Setyan, Ari; Zhang, Qi; Merkel, M.; Knighton, Walter B.; Sun, Y.; Song, Chen; Shilling, John E.; Onasch, Timothy B.; Herndon, Scott C.; Worsnop, Douglas R.; Fast, Jerome D.; Zaveri, Rahul A.; Berg, Larry K.; Wiedensohler, A.; Flowers, B. A.; Dubey, Manvendra K.; Subramanian, R.

    2012-09-11

    The Carbonaceous Aerosols and Radiative Effects Study (CARES) took place in the Sacramento Valley of California in summer 2010. We present results obtained at Cool, CA, the T1 site of the project ({approx}40 km downwind of urban emissions from Sacramento), where we deployed an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) in parallel with complementary instrumentation to characterize the sources and processes of submicron particles (PM1). Cool is located at the foothill of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. The particle mass loading was low (3.0 {micro}gm{sup -3} on average) and dominated by organics (80% of the PM1 mass) followed by sulfate (9.9 %). Organics and sulfate appeared to be externally mixed, as suggested by their different time series (r2 = 0.13) and size distributions. Sulfate showed a bimodal distribution with a droplet mode peaking at {approx}400nm in vacuum aerodynamic diameter (Dva), and a condensation mode at {approx}150 nm, while organics generally displayed a broad distribution in 60-600nm (Dva). New particle formation and growth events were observed almost every day, emphasizing the roles of organics and sulfate in new particle growth, especially that of organics. The organic aerosol (OA) had a nominal formula of C{sub 1}H{sub 1.38}N{sub 0.004}O{sub 0.44}, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two different oxygenated OA (OOA, 90% of total OA mass) and a hydrocarbon-like OA (HOA, 10 %) were identified by Positive matrix factorization (PMF) of the high resolution mass spectra. The more oxidized MO-OOA (O/C = 0.54) corresponded to secondary OA (SOA) primarily influenced by biogenic emissions, while the less oxidized LO-OOA (O/C = 0.42) corresponded to SOA associated with urban transport. The HOA factor corresponded to primary emissions mainly

  6. Aerosol source apportionment from 1-year measurements at the CESAR tower in Cabauw, the Netherlands

    NARCIS (Netherlands)

    Schlag, Patrick; Kiendler-Scharr, Astrid; Blom, Marcus Johannes; Canonaco, Francesco; Henzing, Jeroen Sebastiaan; Moerman, Marcel; Prevot, Andre Stephan Henry; Holzinger, Rupert

    2016-01-01

    Intensive measurements of submicron aerosol particles and their chemical composition were performed with an Aerosol Chemical Speciation Monitor (ACSM) at the Cabauw Experimental Site for Atmospheric Research (CESAR) in Cabauw, the Netherlands, sampling at 5 m height above ground. The campaign lasted

  7. The Chemical Composition and Mixing State of Sea Spray Aerosol and Organic Aerosol in the Winter-Spring Arctic

    Science.gov (United States)

    Kirpes, R.; Bondy, A. L.; Bonanno, D.; Moffet, R.; Wang, B.; Laskin, A.; Ault, A. P.; Pratt, K.

    2016-12-01

    The Arctic region is undergoing rapid transformations and loss of sea ice due to climate change. With increased sea ice fracturing resulting in greater open ocean surface, winter emissions of sea spray aerosol (SSA) are expected to be increasing. Additionally, during the winter-spring transition, Arctic haze contributes to the Arctic aerosol budget. The magnitude of aerosol climate effects depends on the aerosol composition and mixing state (distribution of chemical species within and between particles). However, few studies of aerosol chemistry have been conducted in the winter Arctic, despite it being a time when aerosol impacts on clouds are expected to be significant. To study aerosol composition and mixing state in the winter Arctic, atmospheric particles were collected near Barrow, Alaska in January and February 2014 for off-line individual particle chemical analysis. SSA was the most prevalent particle type observed. Sulfate and nitrate were observed to be internally mixed with SSA and organic aerosol. Greater than 98% of observed SSA particles contained organic content, with 15-35% organic volume fraction on average for individual particles. The SSA organic compounds consisted of carbohydrates, lipids, and fatty acids found in the seawater surface microlayer. SSA was determined to be emitted from open leads, while transported sulfate and nitrate contributed to aging of SSA and organic aerosol. Determining the aerosol chemical composition and mixing state in the winter Arctic will further the understanding of how individual aerosol particles impact climate through radiative effects and cloud formation.

  8. Influence of locational states of submicron fibers added into matrix on mechanical properties of plain-woven Carbon Fiber Composite

    Science.gov (United States)

    Kumamoto, Soichiro; Okubo, Kazuya; Fujii, Toru

    2016-01-01

    The aim of this study was to show the influence of locational states of submicron fibers added into epoxy matrix on mechanical properties of modified plane-woven carbon fiber reinforced plastic (CFRP). To change the locational states of submicron fibers, two kinds of fabrication processes were applied in preparing specimen by hand lay-up method. Submicron fibers were simply added into epoxy resin with ethanol after they were stirred by a dispersion process using homogenizer to be located far from the interface between reinforcement and matrix. In contrast, submicron fibers were attached onto the carbon fibers by injecting from a spray nozzle accompanying with ethanol to be located near the interface, after they were tentatively contained in ethanol. The plain-woven CFRP plates were fabricated by hand lay-up method and cured at 80 degree-C for 1 hour and then at 150 degree-C for 3 hours. After curing, the plain-woven CFRP plates were cut into the dimension of specimen. Tensile shear strength and Mode-II fracture toughness of CFRP were determined by tensile lap-shear test and End-notched flexure(ENF) test, respectively. When submicron fibers were located far from the interface between carbon fibers and epoxy resin, tensile shear strength and Mode-II fracture toughness of CFRP were improved 30% and 18% compared with those of unmodified case. The improvement ratio in modified case was rather low (about few percentages) in the case where submicron fibers were located near the interface. The result suggested that crack propagation should be prevented when submicron fibers were existed far from the interface due to the effective stress state around the crack tip.

  9. Influence of locational states of submicron fibers added into matrix on mechanical properties of plain-woven Carbon Fiber Composite

    Directory of Open Access Journals (Sweden)

    Kumamoto Soichiro

    2016-01-01

    Full Text Available The aim of this study was to show the influence of locational states of submicron fibers added into epoxy matrix on mechanical properties of modified plane-woven carbon fiber reinforced plastic (CFRP. To change the locational states of submicron fibers, two kinds of fabrication processes were applied in preparing specimen by hand lay-up method. Submicron fibers were simply added into epoxy resin with ethanol after they were stirred by a dispersion process using homogenizer to be located far from the interface between reinforcement and matrix. In contrast, submicron fibers were attached onto the carbon fibers by injecting from a spray nozzle accompanying with ethanol to be located near the interface, after they were tentatively contained in ethanol. The plain-woven CFRP plates were fabricated by hand lay-up method and cured at 80 degree-C for 1 hour and then at 150 degree-C for 3 hours. After curing, the plain-woven CFRP plates were cut into the dimension of specimen. Tensile shear strength and Mode-II fracture toughness of CFRP were determined by tensile lap-shear test and End-notched flexure(ENF test, respectively. When submicron fibers were located far from the interface between carbon fibers and epoxy resin, tensile shear strength and Mode-II fracture toughness of CFRP were improved 30% and 18% compared with those of unmodified case. The improvement ratio in modified case was rather low (about few percentages in the case where submicron fibers were located near the interface. The result suggested that crack propagation should be prevented when submicron fibers were existed far from the interface due to the effective stress state around the crack tip.

  10. The continuous field measurements of soluble aerosol compositions at the Taipei Aerosol Supersite, Taiwan

    Science.gov (United States)

    Chang, Shih-Yu; Lee, Chung-Te; Chou, Charles C.-K.; Liu, Shaw-Chen; Wen, Tian-Xue

    The characteristics of ambient aerosols, affected by solar radiation, relative humidity, wind speed, wind direction, and gas-aerosol interaction, changed rapidly at different spatial and temporal scales. In Taipei Basin, dense traffic emissions and sufficient solar radiation for typical summer days favored the formation of secondary aerosols. In winter, the air quality in Taipei Basin was usually affected by the Asian continental outflows due to the long-range transport of pollutants carried by the winter monsoon. The conventional filter-based method needs a long time for collecting aerosols and analyzing compositions, which cannot provide high time-resolution data to investigate aerosol sources, atmospheric transformation processes, and health effects. In this work, the in situ ion chromatograph (IC) system was developed to provide 15-min time-resolution data of nine soluble inorganic species (Cl -, NO 2-, NO 3-, SO 42-, Na +, NH 4+, K +, Mg 2+ and Ca 2+). Over 89% of all particles larger than approximately 0.056 μm were collected by the in situ IC system. The in situ IC system is estimated to have a limit of detection lower than 0.3 μg m -3 for the various ambient ionic components. Depending on the hourly measurements, the pollutant events with high aerosol concentrations in Taipei Basin were associated with the local traffic emission in rush hour, the accumulation of pollutants in the stagnant atmosphere, the emission of industrial pollutants from the nearby factories, the photochemical secondary aerosol formation, and the long-range transport of pollutants from Asian outflows.

  11. Primary marine aerosol physical flux and chemical composition during a nutrient enrichment experiment in mesocosms in the Mediterranean Sea

    Science.gov (United States)

    Schwier, Allison N.; Sellegri, Karine; Mas, Sébastien; Charrière, Bruno; Pey, Jorge; Rose, Clémence; Temime-Roussel, Brice; Jaffrezo, Jean-Luc; Parin, David; Picard, David; Ribeiro, Mickael; Roberts, Greg; Sempéré, Richard; Marchand, Nicolas; D'Anna, Barbara

    2017-12-01

    While primary marine aerosol (PMA) is an important part of global aerosol total emissions, its chemical composition and physical flux as a function of the biogeochemical properties of the seawater still remain highly uncharacterized due to the multiplicity of physical, chemical and biological parameters that are involved in the emission process. Here, two nutrient-enriched mesocosms and one control mesocosm, both filled with Mediterranean seawater, were studied over a 3-week period. PMA generated from the mesocosm waters were characterized in term of chemical composition, size distribution and size-segregated cloud condensation nuclei (CCN), as a function of the seawater chlorophyll a (Chl a) concentration, pigment composition, virus and bacteria abundances. The aerosol number size distribution flux was primarily affected by the seawater temperature and did not vary significantly from one mesocosm to the other. The aerosol number size distribution flux was primarily affected by the seawater temperature and did not vary significantly from one mesocosm to the other. Particle number and CCN aerosol fluxes increase by a factor of 2 when the temperature increases from 22 to 32 °C, for all particle submicron sizes. This effect, rarely observed in previous studies, could be specific to oligotrophic waters and/or to this temperature range. In all mesocosms (enriched and control mesocosms), we detected an enrichment of calcium (+500 %) and a deficit in chloride (-36 %) in the submicron PMA mass compared to the literature inorganic composition of the seawater. There are indications that the chloride deficit and calcium enrichment are linked to biological processes, as they are found to be stronger in the enriched mesocosms. This implies a non-linear transfer function between the seawater composition and PMA composition, with complex processes taking place at the interface during the bubble bursting. We found that the artificial phytoplankton bloom did not affect the CCN

  12. Primary marine aerosol physical flux and chemical composition during a nutrient enrichment experiment in mesocosms in the Mediterranean Sea

    Directory of Open Access Journals (Sweden)

    A. N. Schwier

    2017-12-01

    Full Text Available While primary marine aerosol (PMA is an important part of global aerosol total emissions, its chemical composition and physical flux as a function of the biogeochemical properties of the seawater still remain highly uncharacterized due to the multiplicity of physical, chemical and biological parameters that are involved in the emission process. Here, two nutrient-enriched mesocosms and one control mesocosm, both filled with Mediterranean seawater, were studied over a 3-week period. PMA generated from the mesocosm waters were characterized in term of chemical composition, size distribution and size-segregated cloud condensation nuclei (CCN, as a function of the seawater chlorophyll a (Chl a concentration, pigment composition, virus and bacteria abundances. The aerosol number size distribution flux was primarily affected by the seawater temperature and did not vary significantly from one mesocosm to the other. The aerosol number size distribution flux was primarily affected by the seawater temperature and did not vary significantly from one mesocosm to the other. Particle number and CCN aerosol fluxes increase by a factor of 2 when the temperature increases from 22 to 32 °C, for all particle submicron sizes. This effect, rarely observed in previous studies, could be specific to oligotrophic waters and/or to this temperature range. In all mesocosms (enriched and control mesocosms, we detected an enrichment of calcium (+500 % and a deficit in chloride (−36 % in the submicron PMA mass compared to the literature inorganic composition of the seawater. There are indications that the chloride deficit and calcium enrichment are linked to biological processes, as they are found to be stronger in the enriched mesocosms. This implies a non-linear transfer function between the seawater composition and PMA composition, with complex processes taking place at the interface during the bubble bursting. We found that the artificial phytoplankton bloom

  13. On the sub-micron aerosol size distribution in a coastal-rural site at El Arenosillo Station (SW – Spain

    Directory of Open Access Journals (Sweden)

    M. Sorribas

    2011-11-01

    Full Text Available This study focuses on the analysis of the sub-micron aerosol characteristics at El Arenosillo Station, a rural and coastal environment in South-western Spain between 1 August 2004 and 31 July 2006 (594 days. The mean total concentration (NT was 8660 cm−3 and the mean concentrations in the nucleation (NNUC, Aitken (NAIT and accumulation (NACC particle size ranges were 2830 cm−3, 4110 cm−3 and 1720 cm−3, respectively. Median size distribution was characterised by a single-modal fit, with a geometric diameter, median number concentration and geometric standard deviation of 60 nm, 5390 cm−3 and 2.31, respectively. Characterisation of primary emissions, secondary particle formation, changes to meteorology and long-term transport has been necessary to understand the seasonal and annual variability of the total and modal particle concentration. Number concentrations exhibited a diurnal pattern with maximum concentrations around noon. This was governed by the concentrations of the nucleation and Aitken modes during the warm seasons and only by the nucleation mode during the cold seasons. Similar monthly mean total concentrations were observed throughout the year due to a clear inverse variation between the monthly mean NNUC and NACC. It was related to the impact of desert dust and continental air masses on the monthly mean particle levels. These air masses were associated with high values of NACC which suppressed the new particle formation (decreasing NNUC. Each day was classified according to a land breeze flow or a synoptic pattern influence. The median size distribution for desert dust and continental aerosol was dominated by the Aitken and accumulation modes, and marine air masses were dominated by the nucleation and Aitken modes. Particles

  14. Chemical composition of atmospheric aerosols resolved via positive matrix factorization

    Science.gov (United States)

    Äijälä, Mikko; Junninen, Heikki; Heikkinen, Liine; Petäjä, Tuukka; Kulmala, Markku; Worsnop, Douglas; Ehn, Mikael

    2017-04-01

    Atmospheric particulate matter is a complex mixture of various chemical species such as organic compounds, sulfates, nitrates, ammonia, chlorides, black carbon and sea salt. As aerosol chemical composition strongly influences aerosol climate effects (via cloud condensation nucleus activation, hygroscopic properties, aerosol optics, volatility and condensation) as well as health effects (toxicity, carcinogenicity, particle morphology), detailed understanding of atmospheric fine particle composition is widely beneficial for understanding these interactions. Unfortunately the comprehensive, detailed measurement of aerosol chemistry remains difficult due to the wide range of compounds present in the atmosphere as well as for the miniscule mass of the particles themselves compared to their carrier gas. Aerosol mass spectrometer (AMS; Canagaratna et al., 2007) is an instrument often used for characterization of non-refractive aerosol types: the near-universal vaporization and ionisation technique allows for measurement of most atmospheric-relevant compounds (with the notable exception of refractory matter such as sea salt, black carbon, metals and crustal matter). The downside of the hard ionisation applied is extensive fragmentation of sample molecules. However, the apparent loss of information in fragmentation can be partly offset by applying advanced statistical methods to extract information from the fragmentation patterns. In aerosol mass spectrometry statistical analysis methods, such as positive matrix factorization (PMF; Paatero, 1999) are usually applied for aerosol organic component only, to keep the number of factors to be resolved manageable, to retain the inorganic components for solution validation via correlation analysis, and to avoid inorganic species dominating the factor model. However, this practice smears out the interactions between organic and inorganic chemical components, and hinders the understanding of the connections between primary and

  15. Quantifying the Relationship between Organic Aerosol Composition and Hygroscopicity/CCN Activity

    Energy Technology Data Exchange (ETDEWEB)

    Ziemann, Paul J. [Univ. of California, Riverside, CA (United States); Kreidenweis, Sonia M. [Colorado State Univ., Fort Collins, CO (United States); Petters, Markus D. [North Carolina State Univ., Raleigh, NC (United States)

    2013-06-30

    The overall objective for this project was to provide the data and underlying process level understanding necessary to facilitate the dynamic treatment of organic aerosol CCN activity in future climate models. The specific objectives were as follows: (1) employ novel approaches to link organic aerosol composition and CCN activity, (2) evaluate the effects of temperature and relative humidity on organic aerosol CCN activity, and (3) develop parameterizations to link organic aerosol composition and CCN activity.

  16. Impact of aerosol composition on cloud condensation nuclei activity

    Directory of Open Access Journals (Sweden)

    Q. Zhang

    2012-04-01

    Full Text Available The impact of aerosol composition on cloud condensation nuclei (CCN activity were analyzed in this study based on field experiments carried out at downtown Tianjin, China in September 2010. In the experiments, the CCN measurements were performed at supersaturation (SS of 0.1%, 0.2% and 0.4% using a thermal-gradient diffusion chamber (DMT CCNC, whereas the aerosol size distribution and composition were simultaneously measured with a TSI SMPS and an Aerodyne Aerosol Mass Spectrometer (AMS, respectively. The results show that the influence of aerosol composition on CCN activity is notable under low SS (0.1%, and their influence decreased with increasing SS. For example, under SS of 0.1%, the CCN activity increases from 4.5±2.6% to 12.8±6.1% when organics fraction decrease from 30–40% to 10–20%. The rate of increase reached up to 184%. While under SS of 0.4%, the CCN activity increases only from 35.7±19.0% to 46.5±12.3% correspondingly. The calculated NCCN based on the size-resolved activation ratio and aerosol number size distribution correlated well with observed NCCN at high SS (0.4%, but this consistence decreased with the falling of SS. The slopes of linear fitted lines between calculated and observed NCCN are 0.708, 0.947, and 0.995 at SS of 0.1%, 0.2% and 0.4% respectively. Moreover, the stand deviation (SD of calculated NCCN increased with the decreasing of SS. A case study of CCN closure analyses indicated that the calculated error of NCCN could reach up to 34% at SS of 0.1% if aerosol composition were not included, and the calculated error decreased with the raising of SS. It is decreased to 9% at SS of 0.2%, and further decreased to 4% at SS of 0.4%.

  17. Atmospheric aerosol over Vermont: chemical composition and sources

    Energy Technology Data Exchange (ETDEWEB)

    Polissar, A.V.; Hopke, P.K. [Clarkson University, Potsdam, NY (United States). Dept. of Chemical Engineering

    2001-12-01

    Aerosol chemical composition data for PM{sub 2.5} samples collected during the period from 1988 to 1995 at Underhill, VT were analyzed. The six sources representing wood burning, coal and oil combustion, coal combustion emissions plus photochemical sulfate production, metal production plus municipal wastes incineration, and emissions from motor vehicles were identified. Emissions from smelting of nonferrous metal ores, arsenic smelting, and soil particles and particles with high concentrations of Na were also identified by PMF. Potential source contribution function (PSCF) analysis for the black carbon factor shows high probabilities in the area surrounding the sampling wood combustion in northern New England and southwestern Quebec. Similar large potential source areas in the midwestern United States were identified for the coal combustion factors. The oil combustion factor was associated with the east coast of the United States. canadian Ni smelters are the main sources for the As factor, although there is some contribution from coal-fired power plants to the south and west of Underhill, VT. It is concluded that the combination of the two receptor modeling methods, PMF and PSCF, provides an effective way in identifying atmospheric aerosol sources and their likely locations. Emissions from different anthropogenic activities as well as secondary aerosol production are the main sources of aerosol measured in Vermont. Fuel combustion, local wood smoke, municipal waste incineration and the secondary sulfate production collectively accounted for about 87% of the fine mass concentrations measured in Vermont. 29 refs., 18 figs., 2 tabs.

  18. Characterization of aerosol composition and sources in the greater Atlanta area by aerosol mass spectrometry

    Science.gov (United States)

    Ng, N. L.; Xu, L.; Suresh, S.; Weber, R. J. J.; Baumann, K.; Edgerton, E. S.

    2014-12-01

    An important and uncertain aspect of biogenic secondary organic aerosol (SOA) formation is that it is often associated with anthropogenic pollution tracers. Prior studies in Atlanta suggested that 70-80% of the carbon in water-soluble organic carbon (WSOC) is modern, yet it is well-correlated with the anthropogenic CO. In this study, we deployed a High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) at multiple sites in different seasons (May 2012-February 2013) to characterize the sources and chemical composition of aerosols in the greater Atlanta area. This area in the SE US is ideal to investigate anthropogenic-biogenic interactions due to high natural and anthropogenic emissions. These extensive field studies are part of the Southeastern Center for Air Pollution and Epidemiology study (SCAPE). The HR-ToF-AMS is deployed at four sites (~ 3 weeks each) in rotation: Jefferson Street (urban), Yorkville (rural), roadside site (near Highway 75/85), and Georgia Tech site (campus), with the urban and rural sites being part of the SEARCH network. We obtained seven HR-ToF-AMS datasets in total. During the entire measurement period, the ACSM is stationary at the GIT site and samples continuously. We perform positive matrix factorization (PMF) analysis on the HR-ToF-AMS and ACSM data to deconvolve the OA into different components. While the diurnal cycle of the total OA is flat as what have been previously observed, the OA factors resolved by PMF analysis show distinctively different diurnal trends. We find that the "more-oxidized oxygenated OA" (MO-OOA) constitutes a major fraction of OA at all sites. In summer, OA is dominated by SOA, e.g., isoprene-OA and OOA with different degrees of oxidation. In contrary, biomass burning OA is more prominent in winter data. By comparing HR-ToF-AMS and ACSM data during the same sampling periods, we find that the aerosol time series are highly correlated, indicating the

  19. Changes in organic aerosol composition with aging inferred from aerosol mass spectra

    Directory of Open Access Journals (Sweden)

    N. L. Ng

    2011-07-01

    Full Text Available Organic aerosols (OA can be separated with factor analysis of aerosol mass spectrometer (AMS data into hydrocarbon-like OA (HOA and oxygenated OA (OOA. We develop a new method to parameterize H:C of OOA in terms of f43 (ratio of m/z 43, mostly C2H3O+, to total signal in the component mass spectrum. Such parameterization allows for the transformation of large database of ambient OOA components from the f44 (mostly CO2+, likely from acid groups vs. f43 space ("triangle plot" (Ng et al., 2010 into the Van Krevelen diagram (H:C vs. O:C (Van Krevelen, 1950. Heald et al. (2010 examined the evolution of total OA in the Van Krevelen diagram. In this work total OA is deconvolved into components that correspond to primary (HOA and others and secondary (OOA organic aerosols. By deconvolving total OA into different components, we remove physical mixing effects between secondary and primary aerosols which allows for examination of the evolution of OOA components alone in the Van Krevelen space. This provides a unique means of following ambient secondary OA evolution that is analogous to and can be compared with trends observed in chamber studies of secondary organic aerosol formation. The triangle plot in Ng et al. (2010 indicates that f44 of OOA components increases with photochemical age, suggesting the importance of acid formation in OOA evolution. Once they are transformed with the new parameterization, the triangle plot of the OOA components from all sites occupy an area in Van Krevelen space which follows a ΔH:C/ΔO:C slope of ~ −0.5. This slope suggests that ambient OOA aging results in net changes in chemical composition that are equivalent to the addition of both acid and alcohol/peroxide functional groups without fragmentation (i.e. C-C bond breakage, and/or the addition of acid groups with fragmentation

  20. Composition and Particle Size Retrievals for Homogeneous Binary Aerosols

    Science.gov (United States)

    Niedziela, R. F.; Argon, P.; Bejcek, L.

    2014-12-01

    Tropospheric aerosols have widely varying compositions, shapes, and sizes. The ability to measure these physical characteristics, coupled with knowledge about their optical properties, can provide insight as to how these particles might participate in atmospheric processes, including their interaction with light. Over the past several years, our laboratory has been involved in developing methods to determine basic physical properties of laboratory-generated particles based on the analysis of infrared extinction spectra of multi-component aerosols. Here we report the results of a complete study on the applicability of well-known refractive index mixing rules to homogeneous binary liquid organic aerosols in an effort to yield in situ measurements of particle size and composition. In particular, we present results for terpenoid (carvone/nopinone) and long-chain hydrocarbon (squalane/squalene) mixtures. The included image shows model carvone/nopinone extinction spectra that were computed using the Lorentz-Lorenz mixing rule on complex refractive index data for the pure components.

  1. Fine aerosol bulk composition measured on WP-3D research aircraft in vicinity of the Northeastern United States – results from NEAQS

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    C. Warneke

    2007-06-01

    Full Text Available During the New England Air Quality Study (NEAQS in the summer of 2004, airborne measurements were made of the major inorganic ions and the water-soluble organic carbon (WSOC of the submicron (PM1.0 aerosol. These and ancillary data are used to describe the overall aerosol chemical characteristics encountered during the study. Fine particle mass was estimated from particle volume and a calculated density based on measured particle composition. Fine particle organic matter (OM was estimated from WSOC and a mass balance analysis. The aerosol over the northeastern United States (U.S. and Canada was predominantly sulfate and associated ammonium, and organic components, although in unique plumes additional ionic components were also periodically above detection limits. In power generation regions, and especially in the Ohio River Valley region, the aerosol tended to be predominantly sulfate (~60% μg μg−1 and apparently acidic, based on an excess of measured anions compared to cations. In all other regions where sulfate concentrations were lower and a smaller fraction of overall mass, the cations and anions were balanced suggesting a more neutral aerosol. In contrast, the WSOC and estimated OM were more spatially uniform and the fraction of OM relative to PM mass was largely influenced by sources of sulfate. The study median OM mass fraction was 40%. Throughout the study region, sulfate and organic aerosol mass were highest near the surface and decreased rapidly with increasing altitude. The relative fraction of organic mass to sulfate was similar throughout all altitudes within the boundary layer (altitude less than 2.5 km, but was significantly higher at altitude layers in the free troposphere (above 2.5 km. A number of distinct biomass burning plumes from fires in Alaska and the Yukon were periodically intercepted, mostly at altitudes between 3 and 4 km. These plumes were associated with highest aerosol concentrations of the study and were

  2. Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

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    S. D. Forestieri

    2016-07-01

    Full Text Available The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 % of predominately submicron SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs. One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. Optically weighted GF(85 % values for SSA particles were derived from measurements of light scattering and particle size distributions. The mean optically weighted SSA diameters were 530 and 570 nm for the indoor and outdoor MARTs, respectively. The GF(85 % measurements were made concurrently with online particle composition measurements, including bulk composition (using an Aerodyne high-resolution aerosol mass spectrometer and single particle (using an aerosol time-of-flight mass spectrometer measurement, and a variety of water-composition measurements. During both microcosm experiments, the observed optically weighted GF(85 % values were depressed substantially relative to pure inorganic sea salt by 5 to 15 %. There was also a time lag between GF(85 % depression and the peak chlorophyll a (Chl a concentrations by either 1 (indoor MART or 3-to-6 (outdoor MART days. The fraction of organic matter in the SSA particles generally increased after the Chl a peaked, also with a time lag, and ranged from about 0.25 to 0.5 by volume. The observed depression in the GF(85 % values (relative to pure sea salt is consistent with the large observed volume fractions of non-refractory organic matter (NR-OM comprising the SSA. The GF(85 % values

  3. Absorption Angstrom Exponent in AERONET and related data as an indicator of aerosol composition

    Directory of Open Access Journals (Sweden)

    P. B. Russell

    2010-02-01

    Full Text Available Recent results from diverse air, ground, and laboratory studies using both radiometric and in situ techniques show that the fractions of black carbon, organic matter, and mineral dust in atmospheric aerosols determine the wavelength dependence of absorption (often expressed as Absorption Angstrom Exponent, or AAE. Taken together, these results hold promise of improving information on aerosol composition from remote measurements. The main purpose of this paper is to show that AAE values for an Aerosol Robotic Network (AERONET set of retrievals from Sun-sky measurements describing full aerosol vertical columns are also strongly correlated with aerosol composition or type. In particular, we find AAE values near 1 (the theoretical value for black carbon for AERONET-measured aerosol columns dominated by urban-industrial aerosol, larger AAE values for biomass burning aerosols, and the largest AAE values for Sahara dust aerosols. These AERONET results are consistent with results from other, very different, techniques, including solar flux-aerosol optical depth (AOD analyses and airborne in situ analyses examined in this paper, as well as many other previous results. Ambiguities in aerosol composition or mixtures thereof, resulting from intermediate AAE values, can be reduced via cluster analyses that supplement AAE with other variables, for example Extinction Angstrom Exponent (EAE, which is an indicator of particle size. Together with previous results, these results strengthen prospects for determining aerosol composition from space, for example using the Glory Aerosol Polarimetry Sensor (APS, which seeks to provide retrievals of multiwavelength single-scattering albedo (SSA and aerosol optical depth (and therefore aerosol absorption optical depth (AAOD and AAE, as well as shape and other aerosol properties. Multidimensional cluster analyses promise additional information content, for example by using the Ozone Monitoring Instrument (OMI to add AAOD

  4. Seasonal variations in aerosol particle composition at the puy-de-Dôme research station in France

    Directory of Open Access Journals (Sweden)

    E. J. Freney

    2011-12-01

    Full Text Available Detailed investigations of the chemical and microphysical properties of atmospheric aerosol particles were performed at the puy-de-Dôme (pdD research station (1465 m in autumn (September and October 2008, winter (February and March 2009, and summer (June 2010 using a compact Time-of-Flight Aerosol Mass Spectrometer (cToF-AMS. Over the three campaigns, the average mass concentrations of the non-refractory submicron particles ranged from 10 μg m−3 up to 27 μg m−3. Highest nitrate and ammonium mass concentrations were measured during the winter and during periods when marine modified airmasses were arriving at the site, whereas highest concentrations of organic particles were measured during the summer and during periods when continental airmasses arrived at the site. The measurements reported in this paper show that atmospheric particle composition is strongly influenced by both the season and the origin of the airmass. The total organic mass spectra were analysed using positive matrix factorisation to separate individual organic components contributing to the overall organic particle mass concentrations. These organic components include a low volatility oxygenated organic aerosol particle (LV-OOA and a semi-volatile organic aerosol particle (SV-OOA. Correlations of the LV-OOA components with fragments of m/z 60 and m/z 73 (mass spectral markers of wood burning during the winter campaign suggest that wintertime LV-OOA are related to aged biomass burning emissions, whereas organic aerosol particles measured during the summer are likely linked to biogenic sources. Equivalent potential temperature calculations, gas-phase, and LIDAR measurements define whether the research site is in the planetary boundary layer (PBL or in the free troposphere (FT/residual layer (RL. We observe that SV-OOA and nitrate particles are associated with air masses arriving from the PBL where as particle composition measured from RL

  5. Influence of seawater and its aerosols on copper patina composition

    Energy Technology Data Exchange (ETDEWEB)

    Veleva, L., E-mail: veleva@mda.cinvestav.mx [Applied Physics Department, Center for Investigation and Advanced Study, CINVESTAV-Merida, Carr. Ant. a Progreso, Km. 6, 97310 Merida (Mexico); Farro, W. [Department of Chemistry, Universidad Nacional de Trujillo, Av. Juan Pablo II s/n, Ciudad Universitaria, Urb. San Andres, Trujillo (Peru)

    2012-10-01

    Highlights: Black-Right-Pointing-Pointer Copper patina was grown during one-year period on samples exposed to splash, tidal, full immersion sea zone and atmospheric aerosols. Black-Right-Pointing-Pointer The cuprite and atacamite contributed most to patina formation. Black-Right-Pointing-Pointer Atacamite became the sole majority phase in the full immersion zone. Black-Right-Pointing-Pointer Cuprite decreased over time and posnjakite and chalcanthite appeared as minority phases. Black-Right-Pointing-Pointer Copper patina composition is strongly influenced by chloride pollution and specific zone conditions. - Abstract: X-ray diffraction analysis was used to monitor patina composition on copper samples exposed during one-year period to different seawater zones (splash, tidal and full immersion) and marine atmospheric aerosols. Two phases contributed most to patina formation: cuprite (copper oxide) and atacamite (copper chloride compound). Their relative XRD spectra intensities were very similar in patina formed in the tidal sea zone, but atacamite became the sole majority phase in the full immersion zone. The cuprite phase decreased over time, and two minority copper sulfates phases appeared: posnjakite and chalcanthite (CuSO{sub 4}). The results revealed that copper patina composition is strongly influenced by chloride pollution and specific zone conditions. Additional factors, such as wind-blown sand, continuous dredging in coastal areas and vessel docking, influenced degree of pollutant compound adherence to patinas and consequently their structure (porous or compact).

  6. Aircraft-borne aerosol chemical composition measurements in the lower to middle troposphere over southern West Africa: Biomass burning, urban outflow plumes, and long-range transport.

    Science.gov (United States)

    Batenburg, Anneke; Schulz, Christiane; Schneider, Johannes; Sauer, Daniel; Schlager, Hans; Borrmann, Stephan

    2017-04-01

    During the DACCIWA field campaign in June and July 2016, aircraft-borne in-situ aerosol chemical composition measurements were performed over southern West Africa (SWA). This presentation will focus on the submicron particle measurements done with a Compact Time-of-Flight Aerosol Mass Spectrometer (C-ToF-AMS) on board of the DLR Falcon aircraft during twelve research flights from Lomé, Togo, covering the altitude range from the boundary layer (BL) to the middle troposphere (12 km). A preliminary analysis of the results shows typical baseline total non-refractory aerosol mass loadings of 1.5 to 2.8 μg m-3 in the BL, and 0.4 to 1.1 μg m-3above. Up to half of the baseline aerosol mass in the BL appears to consist of sulphate, compared to only 10 to 35 % above the BL; organic matter dominates in the middle troposphere. During several flights, the DLR Falcon crossed a pronounced and seemingly widespread aerosol layer at 2—4.5 km altitude, partly in or slightly above the BL. The AMS data indicate that about half of the non-refractory aerosol mass in the middle of this layer consisted of organic matter. We consider it likely that these aerosol particles were produced by biomass burning in Central Africa. Emissions from cities and industrial areas were also intercepted, as well as enhancements in some species at higher altitudes. Trajectory analysis suggests that an increase of the organics to more than 2.5 μg m-3 observed at 8 km during one flight came from the Arabian Peninsula. Several ammonium peaks during the same flight at higher altitudes were traced back to the Asian Summer Monsoon Anticyclone (ASMA).

  7. The composition of ambient and fresh biomass burning aerosols at a savannah site, South Africa

    Directory of Open Access Journals (Sweden)

    Minna Aurela

    2016-05-01

    Full Text Available Atmospheric aerosols play a key role in climate change, and have adverse effects on human health. Given South Africa�s status as a rapidly-developing country with increasing urbanisation and industrial growth, information on the quality of ambient air is important. In this study, the chemical composition of ambient particles and the particles in fresh biomass burning plumes were studied at a savannah environment in Botsalano, South Africa. The results showed that Botsalano was regularly affected by air masses that had passed over several large point sources. Air masses that had passed over the coal-fired Matimba power station in the Waterberg, or over the platinum group metal smelters in the western Bushveld Igneous Complex, contained high sulfate concentrations in the submicron ranges. These concentrations were 14 to 37 times higher compared with air masses that had passed only over rural areas. Because of the limited nature of this type of data in literature for the interior regions of southern Africa, our report serves as a valuable reference for future studies. In addition, our biomass burning study showed that potassium in the fresh smoke of burning savannah grass was likely to take the form of KCl. Clear differences were found in the ratios for potassium and levoglucosan in the smouldering and flaming phases. Our findings highlight the need for more comprehensive chamber experiments on various fuel types used in southern Africa, to confirm the ratio of important biomass burning tracer species that can be used in source apportionment studies in the future.

  8. Aerosol Composition in the Los Angeles Basin Studied by High Resolution Aerosol Mass Spectrometry

    Science.gov (United States)

    Hayes, P. L.; Ortega, A. M.; Cubison, M.; Hu, W.; Toohey, D. W.; Flynn, J. H.; Grossberg, N.; Lefer, B. L.; Alvarez, S. L.; Rappenglueck, B.; Allan, J. D.; Taylor, J.; Holloway, J. S.; Gilman, J. B.; Kuster, W. C.; De Gouw, J. A.; Massoli, P.; Zhang, X.; Weber, R.; Zhao, Y.; Cliff, S. S.; Wexler, A. S.; Isaacman, G. A.; Worton, D. R.; Kreisberg, N. M.; Hering, S. V.; Goldstein, A. H.; Jimenez, J. L.

    2011-12-01

    Atmospheric aerosols impact climate and health, but their sources and composition are poorly understood. To address this knowledge gap, a high-resolution aerosol mass spectrometer (AMS) and complementary instrumentation were deployed during the 2010 CalNex campaign to characterize aerosol composition in the Los Angeles (LA) area. Total mass concentrations as well as the species concentrations measured by the AMS compare well with most other instruments. Nitrate dominates in the mornings, but its concentration is reduced in the afternoon when organic aerosols (OA) increase and dominate. The diurnal variations in concentrations are strongly influenced by emission transport from the source-rich western basin. The average OA to enhanced CO ratio increases with photochemical age from 25 to 80 μg m-3 ppm-1, which indicates significant secondary OA (SOA) production and that a large majority of OA is secondary in aged air. The ratio values are similar to those from Mexico City as well as New England and the Mid-Atlantic States. Positive matrix factorization (PMF) is used to assess the concentrations of different OA components. The major OA classes are oxygenated OA (OOA, a surrogate for total SOA), and hydrocarbon-like OA (HOA, a surrogate for primary combustion OA). Several subclasses of OA are identified as well including diesel-influenced HOA (DI-HOA) and non-diesel HOA. DI-HOA exhibits low concentrations on Sundays consistent with the well-known weekday/weekend effect in LA. PMF analysis finds that OOA is 67% of the total OA concentration. A strong correlation between OOA and Ox (O3 + NO2) concentrations is observed with a slope of 0.15 that suggests the production of fresh SOA in Pasadena. Plotting the OA elemental ratios in a Van Krevelen diagram (H:C vs. O:C) yields a slope of -0.6, which is less steep than that observed in Riverside during the SOAR-2005 campaign. The difference in slopes may be attributed to the highly oxidized HOA present in Pasadena that is

  9. Multielemental composition of atmospheric aerosol in the South of West Siberia

    CERN Document Server

    Koutsenogii, K P; Smirnova, A I; Makarov, V I; Kirov, E I

    2000-01-01

    The data on the multielemental composition of atmospheric aerosols for the typical landscapes of Novosibirsk region have been obtained using SR XRF. The peculiarities of seasonal variations in the multielemental composition of atmospheric aerosols in the South of West Siberia have been analyzed.

  10. A model study of the size and composition distribution of aerosols in an aircraft exhaust

    Energy Technology Data Exchange (ETDEWEB)

    Sorokin, A.A. [SRC `ECOLEN`, Moscow (Russian Federation)

    1997-12-31

    A two-dimensional, axisymmetric flow field model which includes water and sulphate aerosol formation represented by moments of the size and composition distribution function is used to calculate the effect of radial turbulent jet mixing on the aerosol size distribution and mean modal composition. (author) 6 refs.

  11. Realtime chemical characterization of post monsoon organic aerosols in a polluted urban city: Sources, composition, and comparison with other seasons.

    Science.gov (United States)

    Chakraborty, Abhishek; Mandariya, Anil Kumar; Chakraborti, Ruparati; Gupta, Tarun; Tripathi, S N

    2018-01-01

    Real time chemical characterization of non-refractory submicron aerosols (NR-PM1) was carried out during post monsoon (September-October) via Aerosol Mass Spectrometer (AMS) at a polluted urban location of Kanpur, India. Organic aerosol (OA) was found to be the dominant species with 58% contribution to total NR-PM1 mass, followed by sulfate (16%). Overall, OA was highly oxidized (average O/C = 0.66) with the dominance of oxidized OAs (60% of total OA) as revealed by source apportionment. Oxidized nature of OA was also supported by very high OC/EC ratios (average = 8.2) obtained from simultaneous offline filter sampling. High and low OA loading periods have very dramatic effects on OA composition and oxidation. OA O/C ratios during lower OA loading periods were on average 30% higher than the same from high loading periods with significant changes in types and relative contribution from oxidized OAs (OOA). Comparison of OA sources and chemistry among post monsoon and other seasons revealed significant differences. Characteristics of primary OAs remain very similar, but features of OOAs showed substantial changes from one season to another. Winter had lowest OOA contribution to total OA but similar overall O/C ratios as other seasons. This reveals that processing of primary OAs, local atmospheric chemistry, and regional contributions can significantly alter OA characteristics from one season to another. This study provides interesting insights into the seasonal variations of OA sources and evolution in a very polluted and complex environment. Copyright © 2017 Elsevier Ltd. All rights reserved.

  12. Atmospheric aerosol over Vermont: chemical composition and sources.

    Science.gov (United States)

    Polissar, A V; Hopke, P K; Poirot, R L

    2001-12-01

    Aerosol chemical composition data for PM2.5 samples collected during the period from 1988 to 1995 at Underhill, VT, were analyzed. Sulfur and black carbon mass concentrations ranged from 0.01 to 6.5 microg m(-3) and from 0.05 to 2.2 microg m(-3), respectively, while the total fine aerosol mass concentration ranged from 0.2 to 51.1 microg m(-3). Seasonal variations with maxima during the summer and minima in winter/spring were observed for sulfur and the fine mass concentrations. No annual pattern was observed for black carbon. Seasonal variations for most of the other anthropogenic species had maxima in winter and spring and minima in the summer. A factor analysis method, positive matrix factorization (PMF), utilizing error estimates of the data to provide optimum data point scaling was used to obtain information about possible sources of the aerosol. An 11-factor solution was obtained. The six sources representing wood burning, coal and oil combustion, coal combustion emissions plus photochemical sulfate production, metal production plus municipal waste incineration, and emissions from motor vehicles were identified. Emissions from smelting of nonferrous metal ores, arsenic smelting, and soil particles and particles with high concentrations of Na were also identified by PMF. Potential source contribution function (PSCF) analysis combines the aerosol data with the air parcel backward trajectories. PSCF was applied to identify possible source areas and pathways that give rise to the observed high particulate mass concentrations from these 11 sources. The CAPITA Monte Carlo trajectory model was used to obtain 10 sets of 5-day air parcel back trajectories arriving every 2 h for the 7-yr period from 1988 to 1995. The PSCF plot for the black carbon factor shows high probabilities in the area surrounding the sampling site, indicating a strong local influence from residential wood combustion in northern New England and southwestern Quebec. Similar large potential source

  13. Role of ammonium ion and transition metals in the formation of secondary organic aerosol and metallo-organic complex within fog processed ambient deliquescent submicron particles collected in central part of Indo-Gangetic Plain.

    Science.gov (United States)

    Singh, Dharmendra Kumar; Gupta, Tarun

    2017-08-01

    In this study we observed the role of ammonium ion (NH4+) and transition metals (Fe, Mn, Cr, and Cu) present in ambient submicron particles in stabilizing and enhancing the yield of water soluble organic carbon (WSOC). A good correlation of WSOC with transition metals and NH4+ was found (R2 = 0.87 and 0.71), respectively within foggy episode collected ambient PM1 (particles having aerodynamic diameter ≤1.0 μm) suggesting plausibleness of alternate oxidation (primarily various carbonyls into their respective organic acids, esters and other derivatives.) and aging mechanisms. Molar concentration of ammonium ion was observed to be exceeded over and above to require in neutralizing the sulphate and nitrate which further hints its role in the neutralization, stabilization and enhancement of subset of WSOC such as water soluble organic acids. Transition metals were further apportioned using enrichment factor analysis. The source of Fe, Mn, and Cr was found to be crustal and Cu was tagged to anthropogenic origin. This study also described the plausible role of significant predictors (Fe and Cu) in the secondary organic aerosol (SOA) formation through effect of Fenton chemistry. Mass-to-charge ratio of identified oxalic acid from our published recent field study (carried out from same sampling location) was used for understanding the possible metallo-organic complex with Fe supports the substantial role of Fe in SOA formation in the deliquescent submicron particles facilitated by aqueous-phase chemistry. Copyright © 2017 Elsevier Ltd. All rights reserved.

  14. Characterization of the organic composition of aerosols from Rondônia, Brazil, during the LBA-SMOCC 2002 experiment and its representation through model compounds

    Directory of Open Access Journals (Sweden)

    S. Decesari

    2006-01-01

    Full Text Available The chemical composition of carbonaceous aerosols collected during the LBA-SMOCC field experiment, conducted in Rondônia, Brazil, in 2002 during the transition from the dry to the wet season, was investigated by a suite of state-of-the-art analytical techniques. The period of most intense biomass burning was characterized by high concentrations of submicron particles rich in carbonaceous material and water-soluble organic compounds (WSOC. At the onset of the rainy period, submicron total carbon (TC concentrations decreased by about 20 times. In contrast, the concentration of supermicron TC was fairly constant throughout the experiment, pointing to a constant emission of coarse particles from the natural background. About 6–8% of TC (9–11% of WSOC was speciated at the molecular level by GC-MS and liquid chromatography. Polyhydroxylated compounds, aliphatic and aromatic acids were the main classes of compounds accounted for by individual compound analysis. Functional group analysis by proton NMR and chromatographic separation on ion-exchange columns allowed characterization of ca. 50–90% of WSOC into broad chemical classes (neutral species/light acids/humic-like substances. In spite of the significant change in the chemical composition of tracer compounds from the dry to the wet period, the functional groups and the general chemical classes of WSOC changed only to a small extent. Model compounds representing size-resolved WSOC chemical composition for the different periods of the campaign are then proposed in this paper, based on the chemical characterization by both individual compound analysis and functional group analysis deployed during the LBA-SMOCC experiment. Model compounds reproduce quantitatively the average chemical structure of WSOC and can be used as best-guess surrogates in microphysical models involving organic aerosol particles over tropical areas affected by biomass burning.

  15. Cloud Nucleating Properties of Aerosols During TexAQS - GoMACCS 2006: Influence of Aerosol Sources, Composition, and Size

    Science.gov (United States)

    Quinn, P. K.; Bates, T. S.; Coffman, D. J.; Covert, D. S.; Onasch, T. B.; Alllan, J. D.; Worsnop, D.

    2006-12-01

    TexAQS - GoMACCS 2006 was conducted from July to September 2006 in the Gulf of Mexico and Houston Ship Channel to investigate sources and processing of gas and particulate phase species and to determine their impact on regional air quality and climate. As part of the experiment, the NOAA R.V. Ronald H. Brown transited from Charleston, S.C. to the study region. The ship was equipped with a full compliment of gas and aerosol instruments. To determine the cloud nucleating properties of aerosols, measurements were made of the aerosol number size distribution, aerosol chemical composition, and cloud condensation nuclei (CCN) concentration at five supersaturations. During the transit and over the course of the experiment, a wide range of aerosol sources and types was encountered. These included urban and industrial emissions from the S.E. U.S. as the ship left Charleston, a mixture of Saharan dust and marine aerosol during the transit around Florida and across the Gulf of Mexico, urban emissions from Houston, and emissions from the petrochemical industries, oil platforms, and marine vessels in the Gulf coast region. Highest activation ratios (ratio of CCN to total particle number concentration at 0.4 percent supersaturation) were measured in anthropogenic air masses when the aerosol was composed primarily of ammonium sulfate salts and in marine air masses with an aerosol composed of sulfate and sea salt. A strong gradient in activation ratio was measured as the ship moved from the Gulf of Mexico to the end of the Houston Ship Channel (values decreasing from about 0.8 to less than 0.1) and the aerosol changed from marine to industrial. The activation ratio under these different regimes in addition to downwind of marine vessels and oil platforms will be discussed in the context of the aerosol size distribution and chemical composition. The discussion of composition will include the organic mass fraction of the aerosol, the degree of oxidation of the organics, and the water

  16. Year-round record of bulk and size-segregated aerosol composition in central Antarctica (Concordia site – Part 2: Biogenic sulfur (sulfate and methanesulfonate aerosol

    Directory of Open Access Journals (Sweden)

    M. Legrand

    2017-11-01

    Full Text Available Multiple year-round (2006–2015 records of the bulk and size-segregated composition of aerosol were obtained at the inland site of Concordia located in East Antarctica. The well-marked maximum of non-sea-salt sulfate (nssSO4 in January (100 ± 28 ng m−3 versus 4.4 ± 2.3 ng m−3 in July is consistent with observations made at the coast (280 ± 78 ng m−3 in January versus 16 ± 9 ng m−3 in July at Dumont d'Urville, for instance. In contrast, the well-marked maximum of MSA at the coast in January (60 ± 23 ng m−3 at Dumont d'Urville is not observed at Concordia (5.2 ± 2.0 ng m−3 in January. Instead, the MSA level at Concordia peaks in October (5.6 ± 1.9 ng m−3 and March (14.9 ± 5.7 ng m−3. As a result, a surprisingly low MSA-to-nssSO4 ratio (RMSA is observed at Concordia in mid-summer (0.05 ± 0.02 in January versus 0.25 ± 0.09 in March. We find that the low value of RMSA in mid-summer at Concordia is mainly driven by a drop of MSA levels that takes place in submicron aerosol (0.3 µm diameter. The drop of MSA coincides with periods of high photochemical activity as indicated by high ozone levels, strongly suggesting the occurrence of an efficient chemical destruction of MSA over the Antarctic plateau in mid-summer. The relationship between MSA and nssSO4 levels is examined separately for each season and indicates that concentration of non-biogenic sulfate over the Antarctic plateau does not exceed 1 ng m−3 in fall and winter and remains close to 5 ng m−3 in spring. This weak non-biogenic sulfate level is discussed in the light of radionuclides (210Pb, 10Be, and 7Be also measured on bulk aerosol samples collected at Concordia. The findings highlight the complexity in using MSA in deep ice cores extracted from inland Antarctica as a proxy of past dimethyl sulfide emissions from the Southern Ocean.

  17. Comprehensive modeling study of ozonolysis of oleic acid aerosol based on real-time, online measurements of aerosol composition

    Science.gov (United States)

    Gallimore, P. J.; Griffiths, P. T.; Pope, F. D.; Reid, J. P.; Kalberer, M.

    2017-04-01

    The chemical composition of organic aerosols profoundly influences their atmospheric properties, but a detailed understanding of heterogeneous and in-particle reactivity is lacking. We present here a combined experimental and modeling study of the ozonolysis of oleic acid particles. An online mass spectrometry (MS) method, Extractive Electrospray Ionization (EESI), is used to follow the composition of the aerosol at a molecular level in real time; relative changes in the concentrations of both reactants and products are determined during aerosol aging. The results show evidence for multiple non-first-order reactions involving stabilized Criegee intermediates, including the formation of secondary ozonides and other oligomers. Offline liquid chromatography MS is used to confirm the online MS assignment of the monomeric and dimeric products. We explain the observed EESI-MS chemical composition changes, and chemical and physical data from previous studies, using a process-based aerosol chemistry simulation, the Pretty Good Aerosol Model (PG-AM). In particular, we extend previous studies of reactant loss by demonstrating success in reproducing the time dependence of product formation and the evolving particle size. This advance requires a comprehensive chemical scheme coupled to the partitioning of semivolatile products; relevant reaction and evaporation parameters have been refined using our new measurements in combination with PG-AM.

  18. Aerosol composition from Tlaxcoapan, Hidalgo in central Mexico

    Energy Technology Data Exchange (ETDEWEB)

    Martinez C, M. A.; Solis, C.; Andrade, E. [UNAM, Instituto de Fisica, Circuito Exterior, Ciudad Universitaria, 04510 Mexico D. F. (Mexico); Issac O, K. [Universidad Autonoma del Estado de Mexico, Facultad de Medicina, Paseo Tollocan y Jesus Carranza s/n, 50120 Toluca, Estado de Mexico (Mexico); Beltran H, R. I. [Universidad Autonoma del Estado de Hidalgo, Centro de Investigaciones Quimicas, Carretera Pachuca-Tulancingo Km. 4.5, 42174 Pachuca, Hidalgo (Mexico); Medina M, S. A.; Martinez R, G.; Ramirez R, A.; Lucho C, C. A. [Universidad Politecnica de Pachuca, Programa de Ingenieria en Biotecnologia, Carretera Pachuca-Cd. Sahagun Km. 20, Ex-Hacienda de Santa Barbara, Municipio de Zempoala, Hidalgo (Mexico); Del Razo, L. M. [IPN, Centro de Investigacion y de Estudios Avanzados, Seccion Externa de Toxicologia, Ticoman, 07360 Mexico D. F. (Mexico)

    2010-02-15

    Air quality mexican regulations about atmospheric aerosols refer to particle sizes and to the total suspended particle. None of these norms establishes the allowed values based on the particulate chemical composition. Mexican environmental legislation also considers as critical zones those with high concentration of contaminants in the atmosphere. One of these zones is the Tula-Vito-Apasco corridor where no chemical composition characterization in terms of trace metal associated to the air particulate matter has been made. Along this corridor near Tlaxcoapan there are important contaminant sources as petrochemical and electric power plants, metal-mechanical industry, limestone quarry and contaminated soils. In this work PIXE and Sem-EDS were applied to the PM{sub 10} fraction collected on filters. The trace element values thus determined were compared with those of a similar critical zone. It was found that most of the coarse particles come from limestone quarry as fugitive dusts while V, Ni, Cr and Pb values are moderately high and seems to be associated to industrial activities and contaminated soil as well. (Author)

  19. Chemical composition, sources and secondary processes of aerosols in Baoji city of northwest China

    Science.gov (United States)

    Wang, Y. C.; Huang, R.-J.; Ni, H. Y.; Chen, Y.; Wang, Q. Y.; Li, G. H.; Tie, X. X.; Shen, Z. X.; Huang, Y.; Liu, S. X.; Dong, W. M.; Xue, P.; Fröhlich, R.; Canonaco, F.; Elser, M.; Daellenbach, K. R.; Bozzetti, C.; El Haddad, I.; Prévôt, A. S. H.; Canagaratna, M. R.; Worsnop, D. R.; Cao, J. J.

    2017-06-01

    Particulate air pollution is a severe environmental problem in China, affecting visibility, air quality, climate and human health. However, previous studies focus mainly on large cities such as Beijing, Shanghai, and Guangzhou. In this study, an Aerodyne Aerosol Chemical Speciation Monitor was deployed in Baoji, a middle size inland city in northwest China from 26 February to 27 March 2014. The non-refractory submicron aerosol (NR-PM1) was dominated by organics (55%), followed by sulfate (16%), nitrate (15%), ammonium (11%) and chloride (3%). A source apportionment of the organic aerosol (OA) was performed with the Sofi (Source Finder) interface of ME-2 (Multilinear Engine), and six main sources/factors were identified and classified as hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), coal combustion OA (CCOA), less oxidized oxygenated OA (LO-OOA) and more oxidized oxygenated OA (MO-OOA), which contributed 20%, 14%, 13%, 9%, 23% and 21% of total OA, respectively. The contribution of secondary components shows increasing trends from clean days to polluted days, indicating the importance of secondary aerosol formation processes in driving particulate air pollution. The formation of LO-OOA and MO-OOA is mainly driven by photochemical reactions, but significantly influenced by aqueous-phase chemistry during periods of low atmospheric oxidative capacity.

  20. Aerosol emissions from prescribed fires in the United States: A synthesis of laboratory and aircraft measurements

    Science.gov (United States)

    A. A. May; G. R. McMeeking; T. Lee; J. W. Taylor; J. S. Craven; I. Burling; A. P. Sullivan; S. Akagi; J. L. Collett; M. Flynn; H. Coe; S. P. Urbanski; J. H. Seinfeld; R. J. Yokelson; S. M. Kreidenweis

    2014-01-01

    Aerosol emissions from prescribed fires can affect air quality on regional scales. Accurate representation of these emissions in models requires information regarding the amount and composition of the emitted species. We measured a suite of submicron particulate matter species in young plumes emitted from prescribed fires (chaparral and montane ecosystems in California...

  1. Atmo-metabolomics: a new measurement approach for investigating aerosol composition and ecosystem functioning.

    Science.gov (United States)

    Rivas-Ubach, A.; Liu, Y.; Sardans, J.; Tfaily, M. M.; Kim, Y. M.; Bourrianne, E.; Paša-Tolić, L.; Penuelas, J.; Guenther, A. B.

    2016-12-01

    Aerosols play crucial roles in the processes controlling the composition of the atmosphere and the functioning of ecosystems. Gaining a deeper understanding of the chemical composition of aerosols is one of the major challenges for atmospheric and climate scientists and is beginning to be recognized as important for ecological research. Better comprehension of aerosol chemistry can potentially provide valuable information on atmospheric processes such as oxidation of organics and the production of cloud condensation nuclei as well as provide an approximation of the general status of an ecosystem through the measurement of certain stress biomarkers. In this study, we describe an efficient aerosol sampling method, the metabolite extraction and the analytical procedures for the chemical characterization of aerosols, namely, the atmo-metabolome. We used mass spectrometry (MS) coupled to liquid chromatography (LC-MS), gas chromatography (GC-MS) and Fourier transform ion cyclotron resonance (FT-ICR-MS) to characterize the atmo-metabolome of two marked seasons; spring and summer. Our sampling and extraction methods demonstrated to be suitable for aerosol chemical characterization with any of the analytical platforms used in this study. The atmo-metabolome between spring and summer showed overall statistically differences. We identified several metabolites that can be attributed to pollen and other plant-related aerosols. Spring aerosols exhibit higher concentrations of metabolites linked to higher plant activity while summer samples had higher concentrations of metabolites that may reflect certain oxidative stresses in primary producers. Moreover, the elemental composition of aerosols showed clear different between seasons. Summer aerosols were generally higher in molecular weight and with higher O/C ratios, indicating higher oxidation levels and condensation of compounds relative to spring. Our method represents an advanced approach for characterizing the composition of

  2. Comparison of advanced offline and in situ techniques of organic aerosol composition measurement during the CalNex campaign

    NARCIS (Netherlands)

    Tsimkouski, I.|info:eu-repo/dai/nl/330541676; Dorst, T; Goldstein, AH; Oyama, B.S.; Holzinger, R.|info:eu-repo/dai/nl/337989338; Chan, AWH

    2015-01-01

    Our understanding of formation processes, physical properties, and climate/health effects of organic aerosols is still limited in part due to limited knowledge of organic aerosol composition. We present speciated measurements of organic aerosol composition by two methods: in situ thermaldesorption

  3. Combustion-related pollutants of polydisperse single-composition aerosols and advection fog formation

    Science.gov (United States)

    Hung, R. J.; Liaw, G. S.

    1982-01-01

    The most noticeable effect of air pollution on the properties of the atmosphere is the reduction in visibility, with and without the occurrence of condensation, which frequently accompanies polluted air. The present study concerns the formation of advection fog associated with aerosols, due to combustion-related pollutants, with a polydisperse population distribution and a single composition model. The results show that an aerosol population with high particle concentration-shifted distribution provides a more favorable condition for the formation of dense fog than an aerosol population with a low particle concentration-shifted distribution if the value of the mass concentration of the aerosols is kept constant.

  4. Organic composition of single and submicron particles in different regions of western North America and the eastern Pacific during INTEX-B 2006

    Directory of Open Access Journals (Sweden)

    D. A. Day

    2009-08-01

    Full Text Available Single particles were collected from an aircraft platform as part of the Intercontinental Chemical Transport Experiment – Phase B (INTEX-B conducted over the eastern Pacific and western North America. Single particle spectra were obtained using scanning transmission X-ray microscopy-near edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS. Bulk submicron particles were also collected and organic functional group and elemental concentrations were quantified with Fourier transform infrared (FTIR spectroscopy and X-ray fluorescence (XRF. Single particle spectra were classified into metaclasses associated with different sources and atmospheric processing. Particles with spectra indicative of secondary organic aerosol production and combustion sources were found at several locations and a range of altitudes. At lower altitudes, particles with spectra resembling soil dust and biomass burning fingerprints were commonly observed. The types of particle spectra most commonly observed aloft were similar to those observed during a previous study over the northwestern Pacific, indicating that long-range transport may have been an important particle source. Single particle spectra provided evidence that condensation and surface-limited oxidation contributed to particle growth. Organic mass (OM concentrations ranged from 1 to 7 μg m−3 and averaged 2.4–4.1 μg m−3. Alkane functional groups were the largest fraction of OM, averaging 1.9–2.1 μg m−3 or 50–76% of OM, followed by alcohol functional groups (0.35–0.39 μg m−3, 9–14%. Organic and elemental concentrations are compared within and among geographical air mass regions: "Pacific" free troposphere, "Continental" free troposphere, "Seattle" metropolitan region, and the California "Central Valley". OM concentrations were highest and most variable in the Central Valley (3.5±2 μg m−3. Oxygen-to-carbon ratios were

  5. CARVE: Fire-Related Aerosol and Soil Elemental and Isotopic Composition, Alaska, 2013

    Data.gov (United States)

    National Aeronautics and Space Administration — This data set provides measurements of the isotopic composition of black carbon and organic carbon aerosols collected at two locations in interior Alaska during the...

  6. Comparative Mineralogy, Microstructure and Compositional Trends in the Sub-Micron Size Fractions of Mare and Highland Lunar Soils

    Science.gov (United States)

    Thompson, M. S.; Christoffersen, R.; Noble, S. K.; Keller, L. P.

    2012-01-01

    The morphology, mineralogy, chemical composition and optical properties of lunar soils show distinct correlations as a function of grain size and origin [1,2,3]. In the mineralogy type, microstructure and major element compositions of grains in this important size range in lunar soils.

  7. Direct aerosol chemical composition measurements to evaluate the physicochemical differences between controlled sea spray aerosol generation schemes

    Science.gov (United States)

    Collins, D. B.; Zhao, D. F.; Ruppel, M. J.; Laskina, O.; Grandquist, J. R.; Modini, R. L.; Stokes, M. D.; Russell, L. M.; Bertram, T. H.; Grassian, V. H.; Deane, G. B.; Prather, K. A.

    2014-11-01

    Controlled laboratory studies of the physical and chemical properties of sea spray aerosol (SSA) must be under-pinned by a physically and chemically accurate representation of the bubble-mediated production of nascent SSA particles. Bubble bursting is sensitive to the physico-chemical properties of seawater. For a sample of seawater, any important differences in the SSA production mechanism are projected into the composition of the aerosol particles produced. Using direct chemical measurements of SSA at the single-particle level, this study presents an intercomparison of three laboratory-based, bubble-mediated SSA production schemes: gas forced through submerged sintered glass filters ("frits"), a pulsed plunging-waterfall apparatus, and breaking waves in a wave channel filled with natural seawater. The size-resolved chemical composition of SSA particles produced by breaking waves is more similar to particles produced by the plunging waterfall than those produced by sintered glass filters. Aerosol generated by disintegrating foam produced by sintered glass filters contained a larger fraction of organic-enriched particles and a different size-resolved elemental composition, especially in the 0.8-2 μm dry diameter range. Interestingly, chemical differences between the methods only emerged when the particles were chemically analyzed at the single-particle level as a function of size; averaging the elemental composition of all particles across all sizes masked the differences between the SSA samples. When dried, SSA generated by the sintered glass filters had the highest fraction of particles with spherical morphology compared to the more cubic structure expected for pure NaCl particles produced when the particle contains relatively little organic carbon. In addition to an intercomparison of three SSA production methods, the role of the episodic or "pulsed" nature of the waterfall method on SSA composition was under-taken. In organic-enriched seawater, the continuous

  8. Glassy aerosols with a range of compositions nucleate ice heterogeneously at cirrus temperatures

    Directory of Open Access Journals (Sweden)

    T. W. Wilson

    2012-09-01

    Full Text Available Atmospheric secondary organic aerosol (SOA is likely to exist in a semi-solid or glassy state, particularly at low temperatures and humidities. Previously, it has been shown that glassy aqueous citric acid aerosol is able to nucleate ice heterogeneously under conditions relevant to cirrus in the tropical tropopause layer (TTL. In this study we test if glassy aerosol distributions with a range of chemical compositions heterogeneously nucleate ice under cirrus conditions. Three single component aqueous solution aerosols (raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA and levoglucosan and one multi component aqueous solution aerosol (raffinose mixed with five dicarboxylic acids and ammonium sulphate were studied in both the liquid and glassy states at a large cloud simulation chamber. The investigated organic compounds have similar functionality to oxidised organic material found in atmospheric aerosol and have estimated temperature/humidity induced glass transition thresholds that fall within the range predicted for atmospheric SOA. A small fraction of aerosol particles of all compositions were found to nucleate ice heterogeneously in the deposition mode at temperatures relevant to the TTL (<200 K. Raffinose and HMMA, which form glasses at higher temperatures, nucleated ice heterogeneously at temperatures as high as 214.6 and 218.5 K respectively. We present the calculated ice active surface site density, ns, of the aerosols tested here and also of glassy citric acid aerosol as a function of relative humidity with respect to ice (RHi. We also propose a parameterisation which can be used to estimate heterogeneous ice nucleation by glassy aerosol for use in cirrus cloud models up to ~220 K. Finally, we show that heterogeneous nucleation by glassy aerosol may compete with ice nucleation on mineral dust particles in mid-latitudes cirrus.

  9. Infrared studies of temperature-dependent phase transitions in ammonium sulfate aerosol and the development of a visible light scattering technique to measure atmospheric particle compositions

    Science.gov (United States)

    Onasch, Timothy Bruce

    1999-10-01

    Sulfate containing particles exist globally throughout the atmosphere and impact its chemistry and radiative properties. Under the low temperature conditions found in the upper troposphere and lower stratosphere, sulfate particles act as nuclei for cirrus clouds and facilitate heterogeneous reactions which affect ozone chemistry. Both of these processes are dependent upon the chemical composition and phase of the background aerosol, and thus the behavior of these particles at low temperatures. This thesis represents two approaches undertaken to investigate the composition and phase of atmospheric aerosols. First, a flow tube system has been developed to study the low temperature behavior of atmospherically relevant particles within a controlled laboratory environment. Second, a visible light scattering technique has been developed to characterize the physical properties of particles in situ from an aircraft platform. The relative humidities of temperature-dependent phase transitions in ammonium sulfate aerosols were measured within a flow tube system. A chilled-mirror hygrometer measured the relative humidity and Fourier transform infrared spectroscopy was utilized to probe the phase of the particles and to characterize their microphysical properties. The relative humidity of deliquescence changed from 80% to 82% over the temperature range from 294.8 K to 258.0 K, in agreement with thermodynamic theory. The efflorescence relative humidity of submicron ammonium sulfate particles increased slightly from 32% to 39% as the temperature decreased from 294.8 K to 234.3 K. The latter result suggests that salt particles may exist as metastable solution droplets under low relative humidity conditions for significant time periods in the upper troposphere. To measure particle refractive indices in situ, a visible light scattering technique based on NCAR's Multiangle Aerosol Spectrometer Probe (MASP) was developed. The MASP was calibrated with monodisperse particles having

  10. Determination of Chemical Composition of Marine Aerosol Particles and its Effects on Aerosol and Cloud Properties During the 2005 MASE Field Campaign

    Science.gov (United States)

    Lee, Y.; Jayne, J.; Alexander, M.; Springston, S.; Wang, J.; Senum, G.; Hubbe, J.; Daum, P.

    2005-12-01

    Marine stratus clouds play an important role in Earth's radiation budget. Cloud microphysical properties such as size distribution and liquid water concentration which govern the aerosol indirect radiative effects are influenced in part by chemical composition of the pre-cloud aerosol particles. To investigate the role aerosol particles play in the properties of marine stratus clouds, we measured aerosol and cloud properties on board the DOE G1 aircraft in the marine atmosphere between Point Reyes and Monterey Peninsula, California in the month of July as part of the 2005 Marine Stratus Experiment (MASE, http://www.asp.bnl.gov/MASE/, supported by the DOE Atmospheric Science and Atmospheric Radiation Measurement Programs). Aerosol chemical composition was measured using a PILS-IC and an Aerodyne AMS. The PILS-IC measured sodium, chloride, ammonium, nitrate, sulfate, potassium, calcium, magnesium, methanesulfonic acid, and format/acetate with a time resolution of 4 minutes and a limit of detection of ca. 0.2 microgram per cubic meter. The AMS measured size-resolved total organic compounds as well as ammonium, nitrate and sulfate at a one-minute time resolution. Other aerosol properties measured included size distribution, light scattering, light absorption and cloud condensation nuclei concentration. Measured cloud properties were cloud droplet size spectrum and liquid water concentration. We will report the chemical composition of aerosol particles and discuss the mechanisms governing their distributions and the relationships between aerosol chemical composition and aerosol and cloud properties.

  11. Nano-sized aerosol classification, collection and analysis--method development using dental composite materials.

    Science.gov (United States)

    Bogdan, Axel; Buckett, Mary I; Japuntich, Daniel A

    2014-01-01

    This article presents a methodical approach for generating, collecting, and analyzing nano-size (1-100 nm) aerosol from abraded dental composite materials. Existing aerosol sampling instruments were combined with a custom-made sampling chamber to create and sample a fresh, steady-state aerosol size distribution before significant Brownian coagulation. Morphological, size, and compositional information was obtained by Transmission Electron Microscopy (TEM). To create samples sizes suitable for TEM analysis, aerosol concentrations in the test chamber had to be much higher than one would typically expect in a dental office, and therefore, these results do not represent patient or dental personnel exposures. Results show that nano-size aerosol was produced by the dental drill alone, with and without cooling water drip, prior to abrasion of dental composite. During abrasion, aerosol generation seemed independent of the percent filler load of the restorative material and the operator who generated the test aerosol. TEM investigation showed that "chunks" of filler and resin were generated in the nano-size range; however, free nano-size filler particles were not observed. The majority of observed particles consisted of oil droplets, ash, and graphitic structures.

  12. Characterization of submicron particles influenced by mixed biogenic and anthropogenic emissions using high-resolution aerosol mass spectrometry: results from CARES

    Directory of Open Access Journals (Sweden)

    A. Setyan

    2012-09-01

    Full Text Available An Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS was deployed during the Carbonaceous Aerosols and Radiative Effects Study (CARES that took place in northern California in June 2010. We present results obtained at Cool (denoted as the T1 site of the project in the foothills of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. During this study, the average mass loading of submicrometer particles (PM1 was 3.0 μg m−3, dominated by organics (80% and sulfate (9.9%. The organic aerosol (OA had a nominal formula of C1H1.38N0.004OM0.44, thus an average organic mass-to-carbon (OM/OC ratio of 1.70. Two distinct oxygenated OA factors were identified via Positive matrix factorization (PMF of the high-resolution mass spectra of organics. The more oxidized MO-OOA (O/C = 0.54 was interpreted as a surrogate for secondary OA (SOA influenced by biogenic emissions whereas the less oxidized LO-OOA (O/C = 0.42 was found to represent SOA formed in photochemically processed urban emissions. LO-OOA correlated strongly with ozone and MO-OOA correlated well with two 1st generation isoprene oxidation products (methacrolein and methyl vinyl ketone, indicating that both SOAs were relatively fresh. A hydrocarbon like OA (HOA factor was also identified, representing primary emissions mainly due to local traffic. On average, SOA (= MO-OOA + LO-OOA accounted for 91% of the total OA mass and 72% of the PM1 mass observed at Cool. Twenty three periods of urban plumes from T0 (Sacramento to T1 (Cool were identified using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem. The average PM1 mass loading was considerably higher in urban plumes than in air masses dominated by biogenic SOA. The change in OA

  13. Identification of key aerosol populations through their size and composition resolved spectral scattering and absorption

    Directory of Open Access Journals (Sweden)

    F. Costabile

    2013-03-01

    Full Text Available Characterizing chemical and physical aerosol properties is important to understand their sources, effects, and feedback mechanisms in the atmosphere. This study proposes a scheme to classify aerosol populations based on their spectral optical properties (absorption and scattering. The scheme is obtained thanks to the outstanding set of information on particle size and composition these properties contain. The spectral variability of the aerosol single scattering albedo (dSSA, and the extinction, scattering and absorption Angstrom exponents (EAE, SAE and AAE, respectively were observed on the basis of two-year measurements of aerosol optical properties (scattering and absorption coefficients at blue, green and red wavelengths performed in the suburbs of Rome (Italy. Optical measurements of various aerosol types were coupled to measurements of particle number size distributions and relevant optical properties simulations (Mie theory. These latter allowed the investigation of the role of the particle size and composition in the bulk aerosol properties observed. The combination of simulations and measurements suggested a general "paradigm" built on dSSA, SAE and AAE to optically classify aerosols. The paradigm proved suitable to identify the presence of key aerosol populations, including soot, biomass burning, organics, dust and marine particles. The work highlights that (i aerosol populations show distinctive combinations of SAE and dSSA times AAE, these variables being linked by a linear inverse relation varying with varying SSA; (ii fine particles show EAE > 1.5, whilst EAE 0.8, whilst ultrafine urban Aitken mode and soot particles show SSA < 0.8. The proposed paradigm agrees with aerosol observations performed during past major field campaigns, this indicating that relations concerning the paradigm have a general validity.

  14. The impacts of aerosol loading, composition, and water uptake on aerosol extinction variability in the Baltimore-Washington, D.C. region

    Science.gov (United States)

    Beyersdorf, A. J.; Ziemba, L. D.; Chen, G.; Corr, C. A.; Crawford, J. H.; Diskin, G. S.; Moore, R. H.; Thornhill, K. L.; Winstead, E. L.; Anderson, B. E.

    2016-01-01

    In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type - such as composition, size, and hygroscopicity - and to the surrounding atmosphere, such as temperature, relative humidity (RH), and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in situ atmospheric profiling in the Baltimore, MD-Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs). The average black carbon concentrations were 240 ng m-3 in the lowest 1 km, decreasing to 35 ng m-3 in the free troposphere (above

  15. The impacts of aerosol loading, composition, and water uptake on aerosol extinction variability in the Baltimore–Washington, D.C. region

    Directory of Open Access Journals (Sweden)

    A. J. Beyersdorf

    2016-01-01

    Full Text Available In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites and mass measurements of aerosol loading (PM2.5 used for air quality monitoring must be understood. This connection varies with many factors including those specific to the aerosol type – such as composition, size, and hygroscopicity – and to the surrounding atmosphere, such as temperature, relative humidity (RH, and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality project, extensive in situ atmospheric profiling in the Baltimore, MD–Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 % and organics (57 %. A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs. The average black carbon concentrations were 240 ng m−3 in the lowest 1 km, decreasing to 35

  16. Aged organic aerosol in the Eastern Mediterranean: the Finokalia Aerosol Measurement Experiment – 2008

    Directory of Open Access Journals (Sweden)

    L. Hildebrandt

    2010-05-01

    Full Text Available Aged organic aerosol (OA was measured at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2008 (FAME-2008, which was part of the EUCAARI intensive campaign of May 2008. The site at Finokalia is influenced by air masses from different source regions, including long-range transport of pollution from continental Europe. A quadrupole aerosol mass spectrometer (Q-AMS was employed to measure the size-resolved chemical composition of non-refractory submicron aerosol (NR-PM1, and to estimate the extent of oxidation of the organic aerosol. Factor analysis was used to gain insights into the processes and sources affecting the OA composition. The particles were internally mixed and liquid. The largest fraction of the dry NR-PM1 sampled was ammonium sulfate and ammonium bisulfate, followed by organics and a small amount of nitrate. The variability in OA composition could be explained with two factors of oxygenated organic aerosol (OOA with differing extents of oxidation but similar volatility. Hydrocarbon-like organic aerosol (HOA was not detected. There was no statistically significant diurnal variation in the bulk composition of NR-PM1 such as total sulfate or total organic aerosol concentrations. However, the OA composition exhibited statistically significant diurnal variation with more oxidized OA in the afternoon. The organic aerosol was highly oxidized, regardless of the source region. Total OA concentrations also varied little with source region, suggesting that local sources had only a small effect on OA concentrations measured at Finokalia. The aerosol was transported for about one day before arriving at the site, corresponding to an OH exposure of approximately 4×1011 molecules cm−3 s. The constant extent of oxidation suggests that atmospheric aging results in a highly oxidized OA at these OH exposures, regardless of the aerosol source.

  17. Characterization of ambient aerosol composition and formation mechanisms and development of quantification methodologies utilizing ATOFMS

    Science.gov (United States)

    Qin, Xueying

    Aerosols are solid or liquid particles suspended in the air. They are generated from a range of natural and anthropogenic sources. Aerosols also experience various reactions such as photo-oxidation and aqueous-phase processing, which constantly change their physical and chemical properties. Therefore, in order to determine the emission inventory, it is important to study aerosol reactions and transformation mechanisms in ambient atmosphere. The research described in this dissertation aimed to characterize temporal, spatial, and seasonal variations on ambient aerosol chemical compositions and formation mechanisms. The results contribute to the understanding of air pollution, climate change, and human health problems, and to devising necessary strategies and policies to resolve these problems. The main experimental technique utilized in the current work is Aerosol time-of-flight mass spectrometry (ATOFMS). It measures the size and chemical composition of individual particles in real-time, and can thus provide high time resolution information on aerosol mixing states, reaction mechanisms, and sources. Continuous ATOFMS measurements have been conducted to study the ambient aerosol properties in several highly polluted regions of California, including the Fresno and Angiola area and the Riverside area. The results provide important insights on the characteristics, distinct diurnal temporal trends, and seasonal variations of aerosols in both urban and rural locations. The second focus of this dissertation is on the quantification capability of ATOFMS, which had been limited by several factors including the size-dependant particle transmission loss and shot-to-shot variability of the desorption/ionization laser. It is demonstrated that, by scaling the ATOFMS measurements using the results from an aerodynamic particle sizer (APS) or a micro-orifice uniform deposit impactor (MOUDI) measurements, it is possible to obtain high temporal resolution mass concentrations from

  18. Characterization of aerosol composition, concentrations, and sources at Baengnyeong Island, Korea using an aerosol mass spectrometer

    Science.gov (United States)

    Lee, Taehyoung; Choi, Jinsoo; Lee, Gangwoong; Ahn, Junyoung; Park, Jin Soo; Atwood, Samuel A.; Schurman, Misha; Choi, Yongjoo; Chung, Yoomi; Collett, Jeffrey L.

    2015-11-01

    To improve understanding of the sources and chemical properties of particulate pollutants on the western side of the Korean Peninsula, an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) measured non-refractory fine (PM1) particles from May to November, 2011 at Baengnyeong Island, South Korea. Organic matter and sulfate were generally the most abundant species and exhibited maximum concentrations of 36 μg/m3 and 39 μg/m3, respectively. Nitrate concentrations peaked at 32 μg/m3 but were typically much lower than sulfate and organic matter concentrations. May, September, October, and November featured the highest monthly average concentrations, with lower concentrations typically observed from June through August. Potential source contribution function (PSCF) analysis and individual case studies revealed that transport from eastern China, an area with high SO2 emissions, was associated with high particulate sulfate concentrations at the measurement site. Observed sulfate aerosol sometimes was fully neutralized by ammonium but often was acidic; the average ammonium to sulfate molar ratio was 1.49. Measured species size distributions revealed a range of sulfate particle size distributions with modes between 100 and 600 nm. Organic aerosol source regions were widespread, including contributions from eastern China and South Korea. Positive matrix factorization (PMF) analysis indicated three "factors," or types of organic aerosol, comprising one primary, hydrocarbon-like organic aerosol (HOA) and two oxidized organic aerosol (OOA) components, including a more oxidized (MO-OOA) and a less oxidized (LO-OOA) oxidized organic aerosol. On average, HOA and OOA contributed 21% and 79% of the organic mass (OM), respectively, with the MO-OOA fraction nearly three times as abundant as the LO-OOA fraction. Biomass burning contributions to observed OM were low during the late spring/early summer agricultural burning season in eastern China, since

  19. Predicting the Mineral Composition of Dust Aerosols. Part 1; Representing Key Processes

    Science.gov (United States)

    Perlwitz, J. P.; Garcia-Pando, C. Perez; Miller, R. L.

    2015-01-01

    Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wetsieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to

  20. Quantifying compositional impacts of ambient aerosol on cloud droplet formation

    Science.gov (United States)

    Lance, Sara

    It has been historically assumed that most of the uncertainty associated with the aerosol indirect effect on climate can be attributed to the unpredictability of updrafts. In Chapter 1, we analyze the sensitivity of cloud droplet number density, to realistic variations in aerosol chemical properties and to variable updraft velocities using a 1-dimensional cloud parcel model in three important environmental cases (continental, polluted and remote marine). The results suggest that aerosol chemical variability may be as important to the aerosol indirect effect as the effect of unresolved cloud dynamics, especially in polluted environments. We next used a continuous flow streamwise thermal gradient Cloud Condensation Nuclei counter (CCNc) to study the water-uptake properties of the ambient aerosol, by exposing an aerosol sample to a controlled water vapor supersaturation and counting the resulting number of droplets. In Chapter 2, we modeled and experimentally characterized the heat transfer properties and droplet growth within the CCNc. Chapter 3 describes results from the MIRAGE field campaign, in which the CCNc and a Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) were deployed at a ground-based site during March, 2006. Size-resolved CCN activation spectra and growth factor distributions of the ambient aerosol in Mexico City were obtained, and an analytical technique was developed to quantify a probability distribution of solute volume fractions for the CCN in addition to the aerosol mixing-state. The CCN were shown to be much less CCN active than ammonium sulfate, with water uptake properties more consistent with low molecular weight organic compounds. The pollution outflow from Mexico City was shown to have CCN with an even lower fraction of soluble material. "Chemical Closure" was attained for the CCN, by comparing the inferred solute volume fraction with that from direct chemical measurements. A clear diurnal pattern was observed for the CCN solute

  1. Compositional and temporal analysis of urban and regional aerosols in Norway

    Science.gov (United States)

    Indresand, Hege

    Two sampling campaigns in Norway were undertaken to characterize fine aerosols (PM2.5). Two types of collection methods were used to capture aerosols, namely DRUM impactors and filter collectors. The DRUM impactor achieves samples that can be analyzed by high time resolution. A measurement can be taken every three hours, by non-destructive methods such as Synchrotron X-ray Fluorescence and Laser Desorption Ionization Time-of-Flight Mass Spectrometry. In June and July of 2002 3-DRUM aerosol samples were attained at rural sites, Birkenes and Kjeller, to gain insight to the aerosol composition in Southern Norway as influenced by regional transport events. The summer study at Birkenes and Kjeller gave insights to long-range transport events of aerosols from the European continent, aerosol composition, chemistry and dynamics. The high time resolution greatly added insights to diurnal cycling of the aerosols and the correlation to temperature and relative humidity. An urban winter sampling campaign was completed in Sofienberg Park in Oslo February and March 2004 with two 8-DRUM impactors. Filter measurements with a time resolution of 48 hours were used to quantify the PM2.5 mass and carbon fractions associated with wood burning. The goal of the urban campaign was to characterize size-separated aerosols with high time resolution during wintertime, where especially high concentrations of aerosols are occurring and speciation of PM2.5 in Norwegian urban settings are lacking. In Oslo, elevated aerosol concentrations from local sources are a function of traffic and inversion layers. The carbon analysis found that wood burning is a significant source of aerosol carbon. The results from the Sofienberg Park winter 2004 analysis will be submitted to the international scientific journal Atmospheric Environment. The following dissertation is organized into six chapters. The first chapter is an introduction to aerosols and measurement tools used. The second chapter covers the summer

  2. The composition and variability of atmospheric aerosol over Southeast Asia during 2008

    Science.gov (United States)

    Trivitayanurak, W.; Palmer, P. I.; Barkley, M. P.; Robinson, N. H.; Coe, H.; Oram, D. E.

    2012-01-01

    We use a nested version of the GEOS-Chem global 3-D chemistry transport model to better understand the composition and variation of aerosol over Borneo and the broader Southeast Asian region in conjunction with aircraft and satellite observations. Our focus on Southeast Asia reflects the importance of this region as a source of reactive organic gases and aerosols from natural forests, biomass burning, and food and fuel crops. We particularly focus on July 2008 when the UK BAe-146 research aircraft was deployed over northern Malaysian Borneo as part of the ACES/OP3 measurement campaign. During July 2008 we find using the model that Borneo (defined as Borneo Island and the surrounding Indonesian islands) was a net exporter of primary organic aerosol (42 kT) and black carbon aerosol (11 kT). We find only 13% of volatile organic compound oxidation products partition to secondary organic aerosol (SOA), with Borneo being a net exporter of SOA (15 kT). SOA represents approximately 19% of the total organic aerosol over the region. Sulphate is mainly from aqueous-phase oxidation (68%), with smaller contributions from gas-phase oxidation (15%) and advection into the regions (14%). We find that there is a large source of sea salt, as expected, but this largely deposits within the region; we find that dust aerosol plays only a relatively small role in the aerosol burden. In contrast to coincident surface measurements over Northern Borneo that find a pristine environment with evidence for substantial biogenic SOA formation we find that the free troposphere is influenced by biomass burning aerosol transported from the northwest of the Island and further afield. We find several transport events during July 2008 over Borneo associated with elevated aerosol concentrations, none of which coincide with the aircraft flights. We use MODIS aerosol optical depths (AOD) data and the model to put the July campaign into a longer temporal perspective. We find that Borneo is where the model

  3. The composition and variability of atmospheric aerosol over Southeast Asia during 2008

    Directory of Open Access Journals (Sweden)

    W. Trivitayanurak

    2012-01-01

    Full Text Available We use a nested version of the GEOS-Chem global 3-D chemistry transport model to better understand the composition and variation of aerosol over Borneo and the broader Southeast Asian region in conjunction with aircraft and satellite observations. Our focus on Southeast Asia reflects the importance of this region as a source of reactive organic gases and aerosols from natural forests, biomass burning, and food and fuel crops. We particularly focus on July 2008 when the UK BAe-146 research aircraft was deployed over northern Malaysian Borneo as part of the ACES/OP3 measurement campaign. During July 2008 we find using the model that Borneo (defined as Borneo Island and the surrounding Indonesian islands was a net exporter of primary organic aerosol (42 kT and black carbon aerosol (11 kT. We find only 13% of volatile organic compound oxidation products partition to secondary organic aerosol (SOA, with Borneo being a net exporter of SOA (15 kT. SOA represents approximately 19% of the total organic aerosol over the region. Sulphate is mainly from aqueous-phase oxidation (68%, with smaller contributions from gas-phase oxidation (15% and advection into the regions (14%. We find that there is a large source of sea salt, as expected, but this largely deposits within the region; we find that dust aerosol plays only a relatively small role in the aerosol burden. In contrast to coincident surface measurements over Northern Borneo that find a pristine environment with evidence for substantial biogenic SOA formation we find that the free troposphere is influenced by biomass burning aerosol transported from the northwest of the Island and further afield. We find several transport events during July 2008 over Borneo associated with elevated aerosol concentrations, none of which coincide with the aircraft flights. We use MODIS aerosol optical depths (AOD data and the model to put the July campaign into a longer temporal perspective. We find that Borneo is where

  4. Compositional Analysis of Aerosols Using Calibration-Free Laser-Induced Breakdown Spectroscopy.

    Science.gov (United States)

    Boudhib, Mohamed; Hermann, Jörg; Dutouquet, Christophe

    2016-04-05

    We demonstrate that the elemental composition of aerosols can be measured using laser-induced breakdown spectroscopy (LIBS) without any preliminary calibration with standard samples. Therefore, a nanosecond Nd:YAG laser beam was focused into a flux of helium charged with alumina aerosols of a few micrometers diameter. The emission spectrum of the laser-generated breakdown plasma was recorded with an echelle spectrometer coupled to a gated detector. The spectral features including emission from both the helium carrier gas and the Al2O3 aerosols were analyzed on the base of a partial local thermodynamic equilibrium. Thus, Boltzmann equilibrium distributions of population number densities were assumed for all plasma species except of helium atoms and ions. By analyzing spectra recorded for different delays between the laser pulse and the detector gate, it is shown that accurate composition measurements are only possible for delays ≤1 μs, when the electron density is large enough to ensure collisional equilibrium for the aerosol vapor species. The results are consistent with previous studies of calibration-free LIBS measurements of solid alumina and glass and promote compositional analysis of aerosols via laser-induced breakdown in helium.

  5. Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates

    Science.gov (United States)

    Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

    2015-07-01

    We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particulate matter (NR-PM1) in the southeastern USA. Measurements were performed in both rural and urban sites in the greater Atlanta area, Georgia (GA), and Centreville, Alabama (AL), for approximately 1 year as part of Southeastern Center for Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR-PM1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important, but not dominant, contributions to total OA in urban sites (i.e., 21-38 % of total OA depending on site and season). Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA factor (isoprene-OA) is only deconvolved in warmer months and contributes 18-36 % of total OA. The presence of isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79 %) of OA in all sites. MO-OOA correlates well with ozone in summer but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based

  6. Aerosol sources and their contribution to the chemical composition of aerosols in the Eastern Mediterranean Sea during summertime

    Directory of Open Access Journals (Sweden)

    J. Sciare

    2003-01-01

    Full Text Available A detailed study on the temporal variability of compounds important in controlling aerosol chemical composition was performed during a one-month experiment conducted during summer 2000 at a background site on Crete, in the Eastern Mediterranean Sea. Contribution of different aerosol sources in the Eastern Mediterranean Basin could be investigated at this location since the site is influenced by a wide range of air masses originating mainly in Europe and Africa. Chemical apportionment was performed for various air mass origins and showed a strong impact of anthropogenic emissions in the Turkey and Central Europe sectors, with black carbon (BC and non-sea-salt sulfate (nss-SO4 concentrations higher than observed in the Eastern and Western Europe sectors. High levels of non-sea-salt calcium (nss-Ca were associated with air masses from Africa but also from Central Turkey. Evidence was found that BC calculation based on light absorbance during dust events was biased. This quality-controlled high temporal resolution dataset allowed to investigate in detail the source-receptor relationships responsible for the levels of BC, nss-SO4 and sulfur dioxide (SO2, observed in Crete. Among the results obtained from this model, the major contribution of Turkey and Central Europe was confirmed in terms of anthropogenic emissions. Comparisons with remote optical properties obtained from Satellite observations (SEAWIFS north of Crete indicates that our ground based aerosol characterization was suitable for describing aerosol properties in the atmospheric column for most of the time during the campaign.

  7. Organic Mass Fragments and Organic Functional Groups in Aged Biomass Burning and Fossil Fuel Combustion Aerosol

    Science.gov (United States)

    Day, D. A.; Hawkins, L. N.; Russell, L. M.

    2009-12-01

    Organic functional group concentrations in submicron aerosol particles collected from 27 June to 17 September at the Scripps Pier in La Jolla, California as part of AeroSCOPE 2008 were quantified using Fourier Transform Infrared (FTIR) spectroscopy. Organic and inorganic non-refractory components in the same air masses were quantified using a Quadrupole Aerosol Mass Spectrometer (Q-AMS). Previous measurements at the Scripps pier indicate that a large fraction of submicron particle mass originates in Los Angeles and the port of Long Beach. Additional particle sources to the region include local urban emissions and periodic biomass burning during large wildfires. Three distinct types of organic aerosol components were identified from organic composition and elemental tracers, including biomass burning, fossil fuel combustion, and polluted marine components. Fossil fuel combustion organic aerosol was dominated by unsaturated alkane and was correlated with sulfur, vanadium, and nickel supporting ship and large trucks in and around the Los Angeles/Long Beach region as the dominant source. Biomass burning organic aerosol comprised a smaller unsaturated alkane fraction and larger fractions of non-acid carbonyl, amine, and carboxylic acid and was correlated with potassium and bromine. Polluted marine organic aerosol was dominated by organic hydroxyl and unsaturated alkane and was not correlated with any elemental tracers. Mass spectra of the organic aerosol support the aerosol sources determined by organic functional groups and elemental tracers and contain fragments commonly attributed to oxygenated organic aerosol (OOA), hydrocarbon-like organic aerosol (HOA), and biomass burning organic aerosol (BBOA). Comparisons of the PMF-derived Q-AMS source spectra with FTIR source spectra and functional group composition provide additional information on the relationship between commonly reported organic aerosol factors and organic functional groups in specific organic aerosol

  8. Production Mechanism, Number Concentration, Size Distribution, Chemical Composition, and Optical Properties of Sea Spray Aerosols Workshop, Summer 2012

    Energy Technology Data Exchange (ETDEWEB)

    Meskhidze, Nicholas [NCSU

    2013-10-21

    The objective of this workshop was to address the most urgent open science questions for improved quantification of sea spray aerosol-radiation-climate interactions. Sea spray emission and its influence on global climate remains one of the most uncertain components of the aerosol-radiation-climate problem, but has received less attention than other aerosol processes (e.g. production of terrestrial secondary organic aerosols). Thus, the special emphasis was placed on the production flux of sea spray aerosol particles, their number concentration and chemical composition and properties.

  9. Aerosol accumulation intensity and composition variations under different weather conditions in urban environment

    Science.gov (United States)

    Steinberga, Iveta; Bikshe, Janis; Eindorfa, Aiva

    2014-05-01

    During the last decade aerosol (PM10, PM2.5) mass and composition measurements were done in different urban environments - parallel street canyons, industrial sites and at the background level in Riga, Latvia. Effect of meteorological parameters on the accumulation and ventilation intensity was investigated in order to understand microclimatological parameters affecting aerosol pollution level and chemical composition changes. In comparison to industrial sites (shipping activities, bulk cargo, oil and naphtha processing), urban street canyon aerosol mass concentration was significantly higher, for PM10 number of daily limit exceedances are higher by factor 3.4 - 3.9 in street canyons. Exceedances of PM2.5 annual limits were identified only in street canyons as well. Precipitation intensity, wind speed, days with mist highly correlates with aerosol concentration; in average during the year about 1 - 2 % presence of calm wind days, 20 - 30 days with mist facilitate accumulation of aerosols and mitigating growing of secondary aerosols. It has been assessed that about 25 % of daily exceedances in street canyons are connected with sea salt/street sanding factor. Strong dependency of wind speed and direction were identified in winter time - low winds (0.4 - 1.7 m/s) blowing from south, south-east (cross section of the street) contributing to PM10 concentrations over 100 - 150 ug/m3. Seasonal differences in aerosol concentrations were identified as a result of recombination of direct source impact, specific meteorological and synoptical conditions during the period from January until April when usually dominates extremely high aerosol concentrations. While aerosol mass concentration levels in monitoring sites significantly differs, concentrations of heavy metals (Pb, Ni, Cd, and As) are almost at the same level, even more - concentration of Cd for some years was higher in industrial area where main pollution is caused by oil processing and storage, heavy traffic

  10. A seasonal time history of the size resolved composition of fine aerosol in Manchester UK

    Science.gov (United States)

    Choularton, Thomas; Martin, Claire; Allan, James; Coe, Hugh; Bower, Keith; Gallagher, Martin

    2010-05-01

    Numerous studies have been conducted in urban centres now using sophisticated instruments that measure aerosol properties needed to determine their effects on human health, air quality and climate change) showing that a significant fraction of urban aerosols (mainly from automotive sources) are composed of organic compounds with implications for human health. In this project we have produced the first seasonal aerosol composition and emission database for the City of Manchester in the UK Several recent projects have been conducted by SEAES looking at fundamental properties of urban atmospheric aerosol to understand their influence on climate. This work is now expanding through collaboration with the School of Geography & Centre for Occupational & Environmental Health to investigate urban aerosol emission impacts on human health In this paper we present a compendium of data from field campaigns in Manchester city centre over the past decade. The data are from six different campaigns, between 2001 - 2007, each campaign was between 2 weeks and 2 months long predominantly from January and June periods . The data analysis includes air parcel trajectory examination and comparisons with external data, including PM10, CO and NOx data from AURN fixed monitoring sites Six Manchester fine aerosol datasets from the past decade have been quality controlled and analysed regarding averages of the size distributions of Organic, NO3, NH4 and SO4 mass loadings. It was found that: Organic material is the largest single component of the aerosol with primary aliphatic material dominating the smallest sizes, but with oxygenated secondary organic material being important in the accumulation mode. In the accumulation mode the organic material seems to be internally mixed with sulphate and nitrate. The accumulation mode particles were effective as cloud condensation nuclei. Seasonal effects surrounding atmospheric stability and photochemistry were found to play an important role in the

  11. Chemical composition of aerosol in the atmospheric surface layer of the East Antarctica coastal zone

    Directory of Open Access Journals (Sweden)

    L. P. Golobokova

    2016-01-01

    Full Text Available Chemical composition of aerosol in the ground layer of the coastal zone in East Antarctica is analyzed in the article. The aerosol samples were taken in 2006–2015 during seasonal works of the Russian Antarctic Expeditions (RAE, namely, these were 52nd–53rd, 55th, and 58th–60th expeditions. Samples were taken in the 200‑km band of the sea-shore zone along routes of the research vessels (REV «Akademik Fedorov» and «Akademik Treshnikov» as well as on territories of the Russian stations Molodezhnaya and Mirny. Although the results obtained did show the wide range of the aerosol concentrations and a certain variability of their chemical composition, some common features of the variability were revealed. Thus, during the period from 2006 to 2014 a decrease of average values of the sums were noted. Spatially, a tendency of decreasing of the ion concentrations was found in the direction from the station Novolazarevskaya to the Molodezhnaya one, but the concentrations increased from the Molodezhnaya to the station Mirny. The sum of ions of the aerosol in the above mentioned coastal zone was, on the average, equal to 2.44 μg/m3, and it was larger than that on the territory of the Antarctic stations Molodezhnaya (0,29 μg/m3 and Mirny (0,50 ág / m3. The main part to the sum of the aerosol ions on the Antarctic stations was contributed by Na+, Ca2+, Cl−, SO4 2−. The main ions in aerosol composition in the coastal zone are ions Na+ and Cl−. The dominant contribution of the sea salt and SO4 2− can be traced in not only the composition of atmospheric aerosols, but also in the chemical composition of the fresh snow in the coastal areas of East Antarctica: at the Indian station Maitri, on the Larsemann Hills, and in a boring located in 55.3 km from the station Progress (K = 1.4÷6.1. It was noted that values of the coefficient of enrichment K of these ions decreases as someone moves from a shore to inland. Estimation of

  12. Combustion aerosols from potassium-containing fuels

    Energy Technology Data Exchange (ETDEWEB)

    Balzer Nielsen, Lars

    1998-12-31

    The scope of the work presented in this thesis is the formation and evolution of aerosol particles in the submicron range during combustion processes, in particular where biomass is used alone or co-fired with coal. An introduction to the formation processes of fly ash in general and submicron aerosol in particular during combustion is presented, along with some known problems related to combustion of biomass for power generation. The work falls in two parts. The first is the design of a laboratory setup for investigation of homogeneous nucleation and particle dynamics at high temperature. The central unit of the setup is a laminar flow aerosol condenser (LFAC), which essentially is a 173 cm long tubular furnace with an externally cooled wall. A mathematical model is presented which describes the formation and evolution of the aerosol in the LFAC, where the rate of formation of new nuclei is calculated using the so-called classical theory. The model includes mass and energy conservation equations and an expression for the description of particle growth by diffusion. The resulting set of nonlinear second-order partial differential equations are solved numerically using the method of orthogonal collocation. The model is implemented in the FORTRAN code MONAERO. The second part of this thesis describes a comprehensive investigation of submicron aerosol formation during co-firing of coal and straw carried out at a 380 MW{sub Th} pulverized coal unit at Studstrup Power Plant, Aarhus. Three types of coal are used, and total boiler load and straw input is varied systematically. Straw contains large amounts of potassium, which is released during combustion. Submicron aerosol is sampled between the two banks of the economizer at a flue gas temperature of 350 deg. C using a novel ejector probe. The aerosol is characterized using the SMPS system and a Berner-type low pressure impactor. The chemical composition of the particles collected in the impactor is determined using

  13. Ground and Airborne Aerosol Composition Measurements of California Coastal Chaparral Smoke Emissions

    Science.gov (United States)

    Craven, J. S.; Sorooshian, A.; Hersey, S. P.; Metcalf, A. R.; Schilling-Fahnestock, K.; Newman, S.; Akagi, S. K.; Taylor, J.; McMeeking, G.; Coe, H.; Tang, P.; Cocker, D. R., III; Yokelson, R. J.; Flagan, R. C.; Seinfeld, J.

    2014-12-01

    Wildfire smoke has large local to global pollution impacts. We present aerosol composition data from two fires in southern California. We measured organic aerosol (OA) of nascent and aged (4 h) smoke from the Williams Fire during the 2009 airborne San Luis Obispo Biomass Burning Campaign (SLOBB). The net ΔOA/ΔCO2 decreased by ~20%; however, positive matrix factorization (PMF) analysis of the organic mass spectra supports two factors that enable the OA emissions to be separated into fresh and oxidized OA. The Δfresh BBOA/ΔCO2 had a steeper decline than the ΔOA/ΔCO2 consistent with outgassing of semi-voltile organic compounds (SVOCs) due to dilution, whereas the Δoxidized BBOA/ΔCO2 increased from its initial value, consist with formation of secondary organic aerosol (SOA). We compare these fresh and oxidized mass spectral signatures, along with chaparral smoke samples measured in the Missoula Fire Lab, to ground-based aerosol measurements made during the Station Fire that occurred one month earlier than the Williams Fire during the Pasadena Aerosol Characterization Observatory Campaign (PACO). Night and daytime aerosol smoke emissions were sampled for one week during the Station Fire. Daytime organic aerosol smoke emissions exhibited larger variability both in mass concentration and composition than nighttime smoke emissions. Both levoglucosan and potassium, known biomass burning tracers, were measured and had distinct time series, supporting diversity in the flaming vs. smoldering initial burning conditions. Similar to the Williams Fire, PMF of the Station Fire mass spectra also reveal two biomass burning factors, one that is less oxidized and correlates strongly with levoglucosan measurements and one that is heavily oxidized and correlates in time with the potassium signal. These two campaigns have allowed us to probe fresh and oxidized smoke in both night and daytime conditions, and PMF results have revealed that at least two emission factors are useful to

  14. Decadal trends in aerosol chemical composition at Barrow, Alaska: 1976–2008

    Directory of Open Access Journals (Sweden)

    G. E. Shaw

    2009-11-01

    Full Text Available Aerosol measurements at Barrow, Alaska during the past 30 years have identified the long range transport of pollution associated with Arctic Haze as well as ocean-derived aerosols of more local origin. Here, we focus on measurements of aerosol chemical composition to assess (1 trends in Arctic Haze aerosol and implications for source regions, (2 the interaction between pollution-derived and ocean-derived aerosols and the resulting impacts on the chemistry of the Arctic boundary layer, and (3 the response of aerosols to a changing climate. Aerosol chemical composition measured at Barrow, AK during the Arctic haze season is compared for the years 1976–1977 and 1997–2008. Based on these two data sets, concentrations of non-sea salt (nss sulfate (SO4= and non-crustal (nc vanadium (V have decreased by about 60% over this 30 year period. Consistency in the ratios of nss SO4=/ncV and nc manganese (Mn/ncV between the two data sets indicates that, although emissions have decreased in the source regions, the source regions have remained the same over this time period. The measurements from 1997–2008 indicate that, during the haze season, the nss SO4= aerosol at Barrow is becoming less neutralized by ammonium (NH4+ yielding an increasing sea salt aerosol chloride (Cl deficit. The expected consequence is an increase in the release of Cl atoms to the atmosphere and a change in the lifetime of volatile organic compounds (VOCs including methane. In addition, summertime concentrations of biogenically-derived methanesulfonate (MSA and nss SO4= are increasing at a rate of 12 and 8% per year, respectively. Further research is required to assess the environmental factors behind the increasing concentrations of biogenic aerosol.

  15. Aerosol hygroscopcity, volatility and chemical composition between the Pearl River Delta Region and Okinawa: a comparison

    Science.gov (United States)

    Cai, M.; Tan, H.; Zhao, J.; Hatakeyama, S.; Mochida, M.; Kondo, Y.; Xu, H.; Li, F.; Shimada, K.; Deng, Y.; Liu, L.

    2016-12-01

    Aerosol physical and chemical properties play important roles in affecting visibility and cloud formation, and the direct and indirect effects of Earth's radiative forcing. It is hence vital to understand aerosol properties in order to assess impacts of atmospheric aerosol particles. Aerosol hygroscopicity, volatility and chemical composition were measured at an urban site in the Pearl River Delta (PRD) Region of China and at a marine site in Okinawa of Japan in November 2014 and November 2016, respectively. A hygroscopic/volatile tandem differential mobility analyzer (H/V-TDMA) and aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) were used to measure hygroscopicity/volatility and chemical composition respectively during the campaign. Aerosol particles were apportioned to more complex emission sources in the PRD than in Okinawa, resulting in about an order of magnitude higher number concentrations of particles (10nm-400nm) in the PRD than in Okinawa. The HR-ToF-AMS measurements show much higher total non-refractory PM1 (NR-PM1) in the PRD than in Okinawa. The two sites represent distinctly different chemical compositions in the total NR-PM1: organics was dominant in the PRD, while sulfate is the major component in Okinawa, reflecting different emission sources. The V-TDMA measurements showed almost no non-volatile (NV) species in 40-300nm particles, while particles in the same size range might contain black carbon or low volatile organics in the PRD. Size-resolved particles hygroscopicity and mixing state between the two measurement sites are also compared in the presentation.

  16. Probing Aerosol Mixing State and Composition via Direct Hygroscopicity Measurements of Highly-Representative, Laboratory-Generated Sea-Spray Aerosol

    OpenAIRE

    Schill, Steven Robert

    2017-01-01

    Aerosol particles impact global climate in large part by acting as cloud condensation nuclei (CCN) and seeding cloud formation events in the atmosphere, which alters the Earth’s albedo. The cloud formation ability of aerosol particles is determined by their water uptake tendencies, which is defined by their chemicophysical properties. Detailed composition information, such as the distribution of chemical components within the particles know as mixing state, is therefore essential for assessin...

  17. Exploration of the seasonal variation of organic aerosol composition using an explicit modeling approach

    Science.gov (United States)

    Ouzebidour, Farida; Camredon, Marie; Stéphanie La, Yuyi; Madronich, Sasha; Taylor, Julia Lee; Hodzic, Alma; Beekmann, Matthias; Siour, Guillaume; Aumont, Bernard

    2014-05-01

    Organic compounds account for a major fraction of fine aerosols in the atmosphere. This organic fraction is dominated by secondary organic aerosol (SOA). Processes leading to SOA formation are however still uncertain and SOA composition is far from being fully characterized. The goals of this study are to evaluate our current understanding of SOA formation and explore its composition. For this purpose, a box-model that describes explicitly processes involved in SOA formation has been developed. This model includes the emission of 183 gaseous and particulate organic compounds. The oxidation of these emitted organic compounds is described using the Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A). Gas/particle partitioning has been implemented considering an ideal homogeneous condensed phase. The generated chemical scheme contains 500,000 species and the gas/particle partitioning is performed for 90,000 of them. Simulations have been performed for summer and winter scenarios representative of continental and urban conditions. NOx and ozone simulated concentrations reproduce the expected winter and summer diurnal evolutions. The predicted organic aerosol composition is a mixture of primary and secondary organic aerosols during the winter and is largely dominated by SOA during the summer.

  18. Two year-long continuous monitoring of PM1 aerosol chemical composition at the Cyprus Atmospheric Observatory. Source apportionment of the Organic content and geographic origins.

    Science.gov (United States)

    Stavroulas, Iasonas; Pikridas, Michael; Oikonomou, Kostantina; Vasiliadou, Emily; Savvides, Chrysanthos; Vrekoussis, Mihalis; Mihalopoulos, Nikolaos; Gros, Valerie; Sciare, Jean

    2017-04-01

    Particulate matter with diameter smaller than 1{μ}m (PM1) induces direct and indirect effects on local and regional pollution, global climate and health. As of the beginning of 2015, the chemical composition of submicron aerosols, is continuously being monitored at the newly established Cyprus Atmospheric Observatory (CAO, http://www.cyi.ac.cy/index.php/cao.html), a national facility of the ACTRIS Research Infrastructure operated by The Cyprus Institute. Cyprus, an island located in the Eastern Mediterranean Middle East region and influenced by diverse air masses throughout the year, is ideal for monitoring photochemically aged aerosols and gaseous pollutants of both natural and anthropogenic origin. Furthermore this is a unique dataset for this area in such proximity to the Middle East, a poorly documented area in terms of atmospheric aerosol observations. An Aerodyne Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) is currently deployed at the CAO premises (35.04N - 33.06E) situated at the rural area of Agia Marina Xyliatou on the foothill of mount Troodos at an elevation of 532m above sea level (asl). The ACSM delivers chemical composition of the major non-refractory aerosol (PM1) chemical constituents (organics, sulfate, nitrate, ammonium, chloride) with an effective (close to 100{%}) collection efficiency for particles in the diameter range of 65-700 nm at a 30 minute temporal resolution. Black Carbon (BC) was also monitored using both Magee Scientific AE-31 and AE-33 aethalometers. Quality control of the PM chemical dataset was conducted by comparison with chemical analysis performed on collocated 24-h filter samples (PM1) and comparison with 1-h PM2.5 derived from a Thermo Scientific TEOM (1400a) Monitor. Positive Matrix Factorization (PMF) was conducted and different organic aerosol factors were distinguished using the Igor based SoFi toolkit utilizing the ME-2 multilinear engine. Air mass origin was investigated for each measurement day using the

  19. On the relation between the size and chemical composition of aerosol particles and their optical properties

    Science.gov (United States)

    Molnár, A.; Mészáros, E.

    The light scattering and absorption coefficients of fine atmospheric aerosol particles were recorded in Hungary under rural conditions in 1998-1999 by an integrating nephelometer and particle soot absorption photometer, respectively. In some cases optical properties in the fine size range were compared to those in the coarse particles. Results obtained indicate, as expected, that fine particles control the scattering and absorption caused by the aerosol. In 1999 the size distribution of aerosol particles was also monitored by means of an electric low pressure impactor (ELPI). This makes it possible the study of the relationship between the number, surface and mass concentration in the size range of 0.1-1.0 μm and the optical characteristics by also considering the chemical composition of the particles.

  20. Impact of North America on the aerosol composition in the North Atlantic free troposphere

    Science.gov (United States)

    García, M. Isabel; Rodríguez, Sergio; Alastuey, Andrés

    2017-06-01

    In the AEROATLAN project we study the composition of aerosols collected over ˜ 5 years at Izaña Observatory (located at ˜ 2400 m a.s.l. in Tenerife, the Canary Islands) under the prevailing westerly airflows typical of the North Atlantic free troposphere at subtropical latitudes and midlatitudes. Mass concentrations of sub-10 µm aerosols (PM10) carried by westerly winds to Izaña, after transatlantic transport, are typically within the range 1.2 and 4.2 µg m-3 (20th and 80th percentiles). The main contributors to background levels of aerosols (PM10 within the 1st-50th percentiles = 0.15-2.54 µg m-3) are North American dust (53 %), non-sea-salt sulfate (14 %) and organic matter (18 %). High PM10 events (75th-95th percentiles ≈ 4.0-9.0 µg m-3) are prompted by dust (56 %), organic matter (24 %) and non-sea-salt sulfate (9 %). These aerosol components experience a seasonal evolution explained by (i) their spatial distribution in North America and (ii) the seasonal shift of the North American outflow, which migrates from low latitudes in winter (˜ 32° N, January-March) to high latitudes in summer (˜ 52° N, August-September). The westerlies carry maximum loads of non-sea-salt sulfate, ammonium and organic matter in spring (March-May), of North American dust from midwinter to mid-spring (February-May) and of elemental carbon in summer (August-September). Our results suggest that a significant fraction of organic aerosols may be linked to sources other than combustion (e.g. biogenic); further studies are necessary for this topic. The present study suggests that long-term evolution of the aerosol composition in the North Atlantic free troposphere will be influenced by air quality policies and the use of soils (potential dust emitter) in North America.

  1. Nature, Origin, Potential Composition, and Climate Impact of the Asian Tropopause Aerosol Layer (ATAL)

    Science.gov (United States)

    Fairlie, T. D.; Vernier, J.-P.; Thomason, L. W.; Natarajan, M.; Bedka, K.; Wienhold, F.; Bian J.; Martinsson, B.

    2015-01-01

    Satellite observations from SAGE II and CALIPSO indicate that summertime aerosol extinction has more than doubled in the Asian Tropopause Aerosol Layer (ATAL) since the late 1990s. Here we show remote and in-situ observations, together with results from a chemical transport model (CTM), to explore the likely composition, origin, and radiative forcing of the ATAL. We show in-situ balloon measurements of aerosol backscatter, which support the high levels observed by CALIPSO since 2006. We also show in situ measurements from aircraft, which indicate a predominant carbonaceous contribution to the ATAL (Carbon/Sulfur ratios of 2- 10), which is supported by the CTM results. We show that the peak in ATAL aerosol lags by 1 month the peak in CO from MLS, associated with deep convection over Asia during the summer monsoon. This suggests that secondary formation and growth of aerosols in the upper troposphere on monthly timescales make a significant contribution to ATAL. Back trajectory calculations initialized from CALIPSO observations provide evidence that deep convection over India is a significant source for ATAL through the vertical transport of pollution to the upper troposphere.

  2. Predicting the mineral composition of dust aerosols – Part 1: Representing key processes

    Directory of Open Access Journals (Sweden)

    J. P. Perlwitz

    2015-10-01

    Full Text Available Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A

  3. Size-resolved chemical composition of aerosol particles during a monsoonal transition period over the Indian Ocean

    Science.gov (United States)

    Spencer, M. T.; Holecek, J. C.; Corrigan, C. E.; Ramanathan, V.; Prather, K. A.

    2008-08-01

    An aerosol time-of-flight mass spectrometer (ATOFMS) was used to measure the size-resolved mixing state of particles over the northern Indian Ocean in October and November 2004. This period was chosen to observe the impact of the monsoonal transition on the size, chemistry, sources, and radiative properties of atmospheric aerosols in the region. Overall, elemental carbon with sulfate (EC-sulfate), biomass/biofuel burning, fresh sea salt (SS), aged sea salt, fly ash, and EC mixed with sea salt were the dominant supermicron particle types, whereas EC-sulfate, biomass/biofuel burning, and fly ash were the dominant submicron particle types. Interestingly, particles composed mostly of aged organic carbon and nitrate were virtually absent during the campaign. This is possibly from low ozone formation in the region or selective scavenging during transport. Notably, during long-range transport periods when an aethalometer measured the highest black carbon concentrations, 77% of submicron particles between 0.5 and 2.5 μm and 71% of EC/soot particles contained an intense 39K+ ion (a known tracer for biomass/biofuel combustion). These observations suggest when the air mass originated from India, biofuel combustion represented a significant source of the regional atmospheric brown cloud. The majority (˜80%) of EC and biomass/biofuel burning particles were mixed with significant amounts of sulfate due to extensive secondary processing of these particles during transport. EC mixed with sea salt was also observed suggesting the particles had undergone cloud processing and become internally mixed during transport. These measurements support the use of an internal mixture of sulfate with EC/soot and biomass/biofuel burning in models to accurately calculate radiative forcing by aerosols in this region.

  4. Composite study of aerosol export events from East Asia and North America

    Science.gov (United States)

    Luan, Y.; Jaeglé, L.

    2013-02-01

    We use satellite observations of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectrometer (MODIS) together with the GEOS-Chem global chemical transport model to contrast export of aerosols from East Asia and North America during 2004-2010. The GEOS-Chem model reproduces the spatial distribution and temporal variations of Asian aerosol outflow generally well, although a low bias (-30%) is found in the model fine mode AOD, particularly during summer. We use the model to identify 244 aerosol pollution export events from E. Asia and 251 export events from N. America over our 7-year study period. When these events are composited by season, we find that the AOD in the outflow is enhanced by 50-100% relative to seasonal mean values. The composite Asian plume splits into one branch going poleward to the Arctic in 3-4 days, with the other crossing the Pacific Ocean in 6-8 days. A fraction of the aerosols is trapped in the subtropical Pacific High during spring and summer. The N. American plume travels to the northeast Atlantic, reaching Europe after 4-5 days. Part of the composite plume turns anticyclonically in the Azores High, where it slowly decays. Both the Asian and N. American export events are favored by a dipole structure in sea-level pressure anomalies, associated with mid-latitude cyclone activity over the respective source regions. This dipole structure during outflow events is a strong feature for all seasons except summer, when convection becomes more important. The observed AOD in the E. Asian outflow exhibits stronger seasonality, with a spring maximum, than the N. American outflow, with a broad spring/summer maximum. The large spring AOD in the Asian outflow is the result of enhanced sulfate and dust aerosol concentrations, but is also due to a larger export efficiency of sulfate and SO2 from the Asian boundary layer relative to the N. American boundary layer. While the N. American sulfate outflow is mostly found in the lower troposphere

  5. Composite study of aerosol export events from East Asia and North America

    Directory of Open Access Journals (Sweden)

    Y. Luan

    2013-02-01

    Full Text Available We use satellite observations of aerosol optical depth (AOD from the Moderate Resolution Imaging Spectrometer (MODIS together with the GEOS-Chem global chemical transport model to contrast export of aerosols from East Asia and North America during 2004–2010. The GEOS-Chem model reproduces the spatial distribution and temporal variations of Asian aerosol outflow generally well, although a low bias (−30% is found in the model fine mode AOD, particularly during summer. We use the model to identify 244 aerosol pollution export events from E. Asia and 251 export events from N. America over our 7-year study period. When these events are composited by season, we find that the AOD in the outflow is enhanced by 50–100% relative to seasonal mean values. The composite Asian plume splits into one branch going poleward to the Arctic in 3–4 days, with the other crossing the Pacific Ocean in 6–8 days. A fraction of the aerosols is trapped in the subtropical Pacific High during spring and summer. The N. American plume travels to the northeast Atlantic, reaching Europe after 4–5 days. Part of the composite plume turns anticyclonically in the Azores High, where it slowly decays. Both the Asian and N. American export events are favored by a dipole structure in sea-level pressure anomalies, associated with mid-latitude cyclone activity over the respective source regions. This dipole structure during outflow events is a strong feature for all seasons except summer, when convection becomes more important. The observed AOD in the E. Asian outflow exhibits stronger seasonality, with a spring maximum, than the N. American outflow, with a broad spring/summer maximum. The large spring AOD in the Asian outflow is the result of enhanced sulfate and dust aerosol concentrations, but is also due to a larger export efficiency of sulfate and SO2 from the Asian boundary layer relative to the N. American boundary layer. While the N. American sulfate outflow

  6. Constraining the atmospheric composition of the day-night terminators of HD 189733b: Atmospheric retrieval with aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Jae-Min [Institute for Computational Science, University of Zürich, Winterthurerstrasse 190, CH-8057 Zürich (Switzerland); Irwin, Patrick G. J.; Fletcher, Leigh N.; Barstow, Joanna K. [Department of Atmospheric, Oceanic, and Planetary Physics, University of Oxford, OX1 3PU Oxford (United Kingdom); Heng, Kevin, E-mail: lee@physik.uzh.ch [Center for Space and Habitability, University of Bern, Sidlerstrasse 5, CH-3012 Bern (Switzerland)

    2014-07-01

    A number of observations have shown that Rayleigh scattering by aerosols dominates the transmission spectrum of HD 189733b at wavelengths shortward of 1 μm. In this study, we retrieve a range of aerosol distributions consistent with transmission spectroscopy between 0.3-24 μm that were recently re-analyzed by Pont et al. To constrain the particle size and the optical depth of the aerosol layer, we investigate the degeneracies between aerosol composition, temperature, planetary radius, and molecular abundances that prevent unique solutions for transit spectroscopy. Assuming that the aerosol is composed of MgSiO{sub 3}, we suggest that a vertically uniform aerosol layer over all pressures with a monodisperse particle size smaller than about 0.1 μm and an optical depth in the range 0.002-0.02 at 1 μm provides statistically meaningful solutions for the day/night terminator regions of HD 189733b. Generally, we find that a uniform aerosol layer provide adequate fits to the data if the optical depth is less than 0.1 and the particle size is smaller than 0.1 μm, irrespective of the atmospheric temperature, planetary radius, aerosol composition, and gaseous molecules. Strong constraints on the aerosol properties are provided by spectra at wavelengths shortward of 1 μm as well as longward of 8 μm, if the aerosol material has absorption features in this region. We show that these are the optimal wavelengths for quantifying the effects of aerosols, which may guide the design of future space observations. The present investigation indicates that the current data offer sufficient information to constrain some of the aerosol properties of HD189733b, but the chemistry in the terminator regions remains uncertain.

  7. Individual aerosol particle composition variations in air masses crossing the North Sea

    OpenAIRE

    De Bock, L.A.; Van Malderen, H.; Van Grieken, R.

    1994-01-01

    Single-particle analysis on North Sea and rainwater samples was performed by electron-probe X-ray microanalysis (EPXMA). The analysis was mainly focused on the determination of the inorganic composition of giant particles with diameters above 1 µm. Multivariate techniques were used for the reduction of the data set and for source apportion. Based on the relative abundances found by hierarchical cluster analyses according to the Ward error sum method, three to eight different aerosol types wer...

  8. Impacts of aerosol-cloud interactions on past and future changes in tropospheric composition

    Energy Technology Data Exchange (ETDEWEB)

    Unger, N.; Menon, S.; Shindell, D. T.; Koch, D. M.

    2009-02-02

    The development of effective emissions control policies that are beneficial to both climate and air quality requires a detailed understanding of all the feedbacks in the atmospheric composition and climate system. We perform sensitivity studies with a global atmospheric composition-climate model to assess the impact of aerosols on tropospheric chemistry through their modification on clouds, aerosol-cloud interactions (ACI). The model includes coupling between both tropospheric gas-phase and aerosol chemistry and aerosols and liquid-phase clouds. We investigate past impacts from preindustrial (PI) to present day (PD) and future impacts from PD to 2050 (for the moderate IPCC A1B scenario) that embrace a wide spectrum of precursor emission changes and consequential ACI. The aerosol indirect effect (AIE) is estimated to be -2.0 Wm{sup -2} for PD-PI and -0.6 Wm{sup -2} for 2050-PD, at the high end of current estimates. Inclusion of ACI substantially impacts changes in global mean methane lifetime across both time periods, enhancing the past and future increases by 10% and 30%, respectively. In regions where pollution emissions increase, inclusion of ACI leads to 20% enhancements in in-cloud sulfate production and {approx}10% enhancements in sulfate wet deposition that is displaced away from the immediate source regions. The enhanced in-cloud sulfate formation leads to larger increases in surface sulfate across polluted regions ({approx}10-30%). Nitric acid wet deposition is dampened by 15-20% across the industrialized regions due to ACI allowing additional re-release of reactive nitrogen that contributes to 1-2 ppbv increases in surface ozone in outflow regions. Our model findings indicate that ACI must be considered in studies of methane trends and projections of future changes to particulate matter air quality.

  9. Systematic Relationships Between Lidar Observables and Sizes And Mineral Composition Of Dust Aerosols

    Science.gov (United States)

    Van Diedenhoven, Bastiaan; Stangl, Alexander; Perlwitz, Jan; Fridlind, Ann M.; Chowdhary, Jacek; Cairns, Brian

    2015-01-01

    The physical and chemical properties of soil dust aerosol particles fundamentally affect their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates on the surface of dust particles, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Lidar measurements, such as extinction-to-backscatter, color and depolarization ratios, are frequently used to distinguish between aerosol types with different physical and chemical properties. The chemical composition of aerosol particles determines their complex refractive index, hence affecting their backscattering properties. Here we present a study on how dust aerosol backscattering and depolarization properties at wavelengths of 355, 532 and 1064 nm are related to size and complex refractive index, which varies with the mineral composition of the dust. Dust aerosols are represented by collections of spheroids with a range of prolate and oblate aspect ratios and their optical properties are obtained using T-matrix calculations. We find simple, systematic relationships between lidar observables and the dust size and complex refractive index that may aid the use of space-based or airborne lidars for direct retrieval of dust properties or for the evaluation of chemical transport models using forward simulated lidar variables. In addition, we present first results on the spatial variation of forward-simulated lidar variables based on a dust model that accounts for the atmospheric cycle of eight different mineral types plus internal mixtures of seven mineral types with iron oxides, which was recently implemented in the NASA GISS Earth System ModelE2.

  10. Elucidating determinants of aerosol composition through particle-type-based receptor modeling

    Directory of Open Access Journals (Sweden)

    M. L. McGuire

    2011-08-01

    Full Text Available An aerosol time-of-flight mass spectrometer (ATOFMS was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007

  11. Characterization of size, morphology and elemental composition of nano-, submicron, and micron particles of street dust separated using field-flow fractionation in a rotating coiled column.

    Science.gov (United States)

    Fedotov, Petr S; Ermolin, Mikhail S; Karandashev, Vasily K; Ladonin, Dmitry V

    2014-12-01

    For the first time, nano- and submicron particles of street dust have been separated, weighted, and analyzed. A novel technique, sedimentation field-flow fractionation in a rotating coiled column, was applied to the fractionation of dust samples with water being used as a carrier fluid. The size and morphology of particles in the separated fractions were characterized by electronic microscopy before digestion and the determination of the concentration of elements by ICP-AES and ICP-MS. The elements that may be of anthropogenic origin (Zn, Cr, Ni, Cu, Cd, Sn, Pb) were found to concentrate mainly in particles present only about 0.1 mass% of the sample they are of special concern due to their increased mobility and ability to penetrate into the deepest alveolar area of the lungs. For rare earth elements (La, Ce, Pr, Nd, Sm) that are evidently of natural source and may be found in soil minerals, in contrary, higher concentrations were observed in large particles (10-100 μm). Sc was an exception that needs further studies. The proposed approach to the fractionation and analysis of nano-, submicron, and micron particles can be a powerful tool for risk assessment related to toxic elements in dust, ash, and other particulate environmental samples. Copyright © 2014 Elsevier B.V. All rights reserved.

  12. Composition and evolution of volcanic aerosol following three eruptions in 2008 - 2010

    Science.gov (United States)

    Andersson, S. M.; Martinsson, B. G.; Friberg, J.; Brenninkmeijer, C. A. M.; Hermann, M.; Heue, K. P.; van Velthoven, P. F. J.; Zahn, A.

    2012-04-01

    Measurements of atmospheric aerosols by the CARIBIC (Civil Aircraft for Regular Investigation of the atmosphere Based on an Instrument Container) platform following the Kasatochi (Alaska), Sarychev (Russia) and Eyjafjallajökull (Iceland) eruptions in the period 2008-2010 are presented. The CARIBIC platform operates on a Lufthansa passenger aircraft usually on monthly inter-continental flights, measuring the atmospheric composition in the UT/LS at 8-12 km altitude (Brenninkmeijer et al., 2007). After the eruption of Kasatochi, analyses of the stratospheric aerosol composition showed enhanced concentrations of sulfur and carbon for several months. On the other hand the ash component, clearly seen in a sample seven days after the eruption, was not detected a month later (Martinsson et al., 2009). To further investigate the composition of the volcanic aerosol three flights trough the volcanic plume of the Eyjafjallajökull eruption were carried out on April 20, May 16 and May 19, 2010. Aerosol sampling was performed by an impaction technique with a cut-off diameter of 2 μm (Nguyen et al., 2006). Collected samples were analyzed by quantitative multi-elemental analysis by PIXE (Particle-Induced X-ray Emission), to obtain concentrations of elements with atomic number larger than 13, and PESA (Particle Elastic Scattering Analysis) for concentrations of hydrogen, carbon, nitrogen and oxygen (Nguyen and Martinsson, 2007). Three samples taken during the special flights to study the Eyjafjallajökull eruption contained unusually high concentrations of elements pointing to crustal origin. The composition of these samples was compared to ash from a fall out sample (Sigmundsson et al., 2010). The ratio of detected elements to iron in both sample types showed good agreement for most of the elements for all three aerosol samples. Volcanically influenced aerosol following the eruptions of Sarychev and Kasatochi were identified by high concentrations of sulfur and by using air mass

  13. Active and passive smoking - New insights on the molecular composition of different cigarette smoke aerosols by LDI-FTICRMS

    Science.gov (United States)

    Schramm, Sébastien; Carré, Vincent; Scheffler, Jean-Luc; Aubriet, Frédéric

    2014-08-01

    The aerosol generated when a cigarette is smoked is a significant indoor contaminant. Both smokers and non-smokers can be exposed to this class of pollutants. Nevertheless, they are not exposed to the same kind of smoke. The active smoker breathes in the mainstream smoke (MSS) during a puff, whereas the passive smoker inhales not only the smoke generated by the lit cigarette between two puffs (SSS) but also the smoke exhaled by active smokers (EXS). The aerosol fraction of EXS has until now been poorly documented; its composition is expected to be different from MSS. This study aims to investigate the complex composition of aerosol from EXS to better understand the difference in exposure between active and passive smokers. To address this, the in-situ laser desorption ionisation Fourier transform ion cyclotron mass spectrometry (LDI-FTICRMS) was used to characterise the aerosol composition of EXS from two different smokers. Results clearly indicated many similarities between EXS samples but also significant differences with MSS and SSS aerosol. The comparison of MSS and EXS aerosol allowed the chemicals retained by the active smoker's lungs to be identified, whereas the convolution of the EXS and SSS aerosol compositions were considered relevant to the exposition of a passive smoker. As a consequence, active smokers are thought to be mainly exposed to polar and poorly unsaturated oxygenated and nitrogenated organics, compared with poorly oxygenated but highly unsaturated compounds in passive smokers.

  14. The importance of aerosol mixing state and size-resolved composition on CCN concentration and the variation of the importance with atmospheric aging of aerosols

    Directory of Open Access Journals (Sweden)

    J. Wang

    2010-08-01

    Full Text Available Aerosol microphysics, chemical composition, and CCN concentrations were measured at the T0 urban supersite in Mexico City during Megacity Initiative: Local and Global Research Observations (MILAGRO in March 2006. The aerosol size distribution and composition often showed strong diurnal variation associated with traffic emissions and aging of aerosols through coagulation and local photochemical production of secondary aerosol species. CCN concentrations (NCCN are derived using Köhler theory from the measured aerosol size distribution and various simplified aerosol mixing state and chemical composition, and are compared to concurrent measurements at five supersaturations ranging from 0.11% to 0.35%. The influence of assumed mixing state on calculated NCCN is examined using both aerosols observed during MILAGRO and representative aerosol types. The results indicate that while ambient aerosols often consist of particles with a wide range of compositions at a given size, NCCN may be derived within ~20% assuming an internal mixture (i.e., particles at a given size are mixtures of all participating species, and have the identical composition if great majority of particles has an overall κ (hygroscopicity parameter value greater than 0.1. For a non-hygroscopic particle with a diameter of 100 nm, a 3 nm coating of sulfate or nitrate is sufficient to increase its κ from 0 to 0.1. The measurements during MILAGRO suggest that the mixing of non-hygroscopic primary organic aerosol (POA and black carbon (BC particles with photochemically produced hygroscopic species and thereby the increase of their κ to 0.1 take place in a few hours during daytime. This rapid process suggests that during daytime, a few tens of kilometers away for POA and BC sources, NCCN may be derived with sufficient accuracy by assuming an internal mixture, and using bulk chemical composition. The rapid mixing also

  15. The importance of aerosol mixing state and size-resolved composition on CCN concentration and the variation of the importance with atmospheric aging of aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Wang, J.; Cubison, M. J.; Aiken, A. C.; Jimenez, J. L.; Collins, D. R.

    2010-05-01

    Aerosol microphysics, chemical composition, and CCN concentrations were measured at the T0 urban supersite in Mexico City during Megacity Initiative: Local and Global Research Observations (MILAGRO) in March 2006. The aerosol size distribution and composition often showed strong diurnal variation associated with traffic emissions and aging of aerosols through coagulation and local photochemical production of secondary aerosol species. CCN concentrations (N{sub CCN}) are derived using Kohler theory from the measured aerosol size distribution and various simplified aerosol mixing state and chemical composition, and are compared to concurrent measurements at five supersaturations ranging from 0.11% to 0.35%. The influence of assumed mixing state on calculated N{sub CCN} is examined using both aerosols observed during MILAGRO and representative aerosol types. The results indicate that while ambient aerosols often consist of particles with a wide range of compositions at a given size, N{sub CCN} may be derived within {approx}20% assuming an internal mixture (i.e., particles at a given size are mixtures of all participating species, and have the identical composition) if great majority of particles has an overall {kappa} (hygroscopicity parameter) value greater than 0.1. For a non-hygroscopic particle with a diameter of 100 nm, a 3 nm coating of sulfate or nitrate is sufficient to increase its {kappa} from 0 to 0.1. The measurements during MILAGRO suggest that the mixing of non-hygroscopic primary organic aerosol (POA) and black carbon (BC) particles with photochemically produced hygroscopic species and thereby the increase of their {kappa} to 0.1 take place in a few hours during daytime. This rapid process suggests that during daytime, a few tens of kilometers away for POA and BC sources, N{sub CCN} may be derived with sufficient accuracy by assuming an internal mixture, and using bulk chemical composition. The rapid mixing also indicates that, at least for very active

  16. Impact of aerosol composition and foliage characteristics on forest canopy deposition rates: A laboratory study

    Science.gov (United States)

    Hornsby, K. E.; Pryor, S. C.

    2013-12-01

    Forests are a major sink for atmospheric aerosols. Hence it has been suggested that (i) increased tree planting in urban areas might lead to a reduction in aerosol particle concentrations and thus a reduction in respiratory conditions and heart complications, and (ii) forests may be responsible for removing a disproportionately large fraction of potentially climate-relevant fine and ultra-fine aerosol particles from the atmosphere. However, larger uncertainties remain with respect to controls on uptake rates for forests. E.g. the deposition flux partitioning between foliage and non-foliage elements, the influence of particle size and composition, the role of leaf surface morphology and stomatal aperture in surface uptake. Improved understanding of the relative importance of these factors and the variability across different tree species should help determine how much of a sink naturally occurring and planted forests can provide downstream of fine particle production. In this study, a sample of trees native to southern Indiana were exposed to ultra-fine aerosol particle populations in a 1.5 m x 1.5 m x 1.5 m Teflon chamber. Stable particle size distributions (PSD) with geometric mean diameters (GMD) ranging from 40 to 80 nm were generated from sodium chloride, ammonium nitrate, ammonium sulfate and sodium sulfite solutions using a TSI model 3940 Aerosol Generation System (AGS). The aerosol stream was diluted using scrubbed and dried zero air to allow a variation of total number concentration across two orders of magnitude. PSD in the chamber are continuously measured using a TSI Scanning Mobility Particle Spectrometer (SMPS) comprising an Electrostatic Classifier (EC model 3080) attached to a Long DMA (LDMA model 3081) and a TSI model 3025A Butanol Condensation Particle Counter (CPC) operated with both the internal diffusion loss and multiple charge corrections turned on. The composition of the chamber air was also monitored for carbon dioxide (CO2) and water vapor

  17. Aerosol composition, chemistry, and source characterization during the 2008 VOCALS Experiment

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Y.; Springston, S.; Jayne, J.; Wang, J.; Senum, G.; Hubbe, J.; Alexander, L.; Brioude, J.; Spak, S.; Mena-Carrasco, M.; Kleinman, L.; Daum, P.

    2010-03-15

    Chemical composition of fine aerosol particles over the northern Chilean coastal waters was determined onboard the U.S. DOE G-1 aircraft during the VOCALS (VAMOS Ocean-Cloud-Atmosphere-Land Study) field campaign between October 16 and November 15, 2008. SO42-, NO3-, NH4+, and total organics (Org) were determined using an Aerodyne Aerosol Mass Spectrometer, and SO42-, NO3-, NH4+, Na+, Cl-, CH3SO3-, Mg2+, Ca2+, and K+ were determined using a particle-into-liquid sampler-ion chromatography technique. The results show the marine boundary layer (MBL) aerosol mass was dominated by non- sea-salt SO42- followed by Na+, Cl-, Org, NO3-, and NH4+, in decreasing importance; CH3SO3-, Ca2+, and K+ rarely exceeded their respective limits of detection. The SO42- aerosols were strongly acidic as the equivalent NH4+ to SO42- ratio was only {approx}0.25 on average. NaCl particles, presumably of sea-salt origin, showed chloride deficits but retained Cl- typically more than half the equivalency of Na+, and are externally mixed with the acidic sulfate aerosols. Nitrate was observed only on sea-salt particles, consistent with adsorption of HNO3 on sea-salt aerosols, responsible for the Cl- deficit. Dust particles appeared to play a minor role, judging from the small volume differences between that derived from the observed mass concentrations and that calculated based on particle size distributions. Because SO42- concentrations were substantial ({approx}0.5 - {approx}3 {micro}g/m3) with a strong gradient (highest near the shore), and the ocean-emitted dimethylsulfide and its unique oxidation product, CH3SO3-, were very low (i.e., {le} 40 parts per trillion and <0.05 {micro}g/m3, respectively), the observed SO42- aerosols are believed to be primarily of terrestrial origin. Back trajectory calculations indicate sulfur emissions from smelters and power plants along coastal regions of Peru and Chile are the main sources of these SO4- aerosols. However, compared to observations, model

  18. Aerosol microphysics simulations of the Mt. Pinatubo eruption with the UKCA composition-climate model

    Science.gov (United States)

    Dhomse, S. S.; Emmerson, K. M.; Mann, G. W.; Bellouin, N.; Carslaw, K. S.; Chipperfield, M. P.; Hommel, R.; Abraham, N. L.; Telford, P.; Braesicke, P.; Dalvi, M.; Johnson, C. E.; O'Connor, F.; Morgenstern, O.; Pyle, J. A.; Deshler, T.; Zawodny, J. M.; Thomason, L. W.

    2014-01-01

    We have enhanced the capability of a microphysical aerosol-chemistry module to simulate the atmospheric aerosol and precursor gases for both tropospheric and stratospheric conditions. Using the Mount Pinatubo eruption (June 1991) as a test case, we evaluate simulated aerosol properties in a composition-climate model against a range of satellite and in-situ observations. Simulations are performed assuming an injection of 20 Tg SO2 at 19-27 km in tropical latitudes, without any radiative feedback from the simulated aerosol. In both quiescent and volcanically perturbed conditions, simulated aerosol properties in the lower stratosphere show reasonable agreement with the observations. The model captures the observed timing of the maximum aerosol optical depth (AOD) and its decay timescale in both tropics and Northern Hemisphere (NH) mid-latitudes. There is also good qualitative agreement with the observations in terms of spatial and temporal variation of the aerosol effective radius (Reff), which peaks 6-8 months after the eruption. However, the model shows significant biases against some observational data sets. Simulated AOD and Surface Area Density (SAD) in the tropics are substantially higher than the gap-filled satellite data products during the first 6 months after the eruption. The model shows consistently weaker enhancement in Reff compared to satellite and in-situ measurements. Simulated aerosol particle size distribution is also compared to NH mid-latitude in-situ balloon sounding measurements of size-resolved number concentrations. Before the eruption, the model captures the observed profiles of lower stratospheric particle number concentrations with radii larger than 5, 150 and 250 nm (N5, N150 and N250) very well. However, in the first 6 months after the eruption, the model shows high bias in N5 concentrations in the lower stratosphere, suggesting too strong nucleation. Following particle growth via condensation and coagulation, this bias in the finest

  19. Atmospheric Aerosol Chemical Composition Measurements for the Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS)

    Science.gov (United States)

    Talbot, Robert W.; Dibb, Jack E.

    1998-01-01

    We received funding to provide measurements of the chemical composition of aerosols aboard the NASA Ames DC-8 research aircraft during the SUCCESS mission. These measurements were successfully completed and the final data resides in the Cloud I computer archive at NASA Ames Research Center. The interpretation of the data obtained on this mission over the central United States has been published in special issues of Geophysical Research Letters. The papers with the University of New Hampshire as first author constitute this report and summarize the salient features of our data. The paper by Talbot et al. discusses the impact of vertical transport on free tropospheric chemistry over the the central USA in springtime. This transport was a dominant feature of the aerosol chemistry during SUCCESS. The paper by Dibb et al. discusses aerosol chemistry specifically as it related to free tropospheric sulfate related to jet exhaust and surface sources. Somewhat surprisingly, we found that surface sources appeared to dominant the distribution of aerosol sulfate in the free troposphere. In addition to these first authored papers, researchers from the University of New Hampshire were co-authors on numerous other companion papers in the special issues.

  20. Sea Spray Aerosol Structure and Composition Using Cryogenic Transmission Electron Microscopy.

    Science.gov (United States)

    Patterson, Joseph P; Collins, Douglas B; Michaud, Jennifer M; Axson, Jessica L; Sultana, Camile M; Moser, Trevor; Dommer, Abigail C; Conner, Jack; Grassian, Vicki H; Stokes, M Dale; Deane, Grant B; Evans, James E; Burkart, Michael D; Prather, Kimberly A; Gianneschi, Nathan C

    2016-01-27

    The composition and surface properties of atmospheric aerosol particles largely control their impact on climate by affecting their ability to uptake water, react heterogeneously, and nucleate ice in clouds. However, in the vacuum of a conventional electron microscope, the native surface and internal structure often undergo physicochemical rearrangement resulting in surfaces that are quite different from their atmospheric configurations. Herein, we report the development of cryogenic transmission electron microscopy where laboratory generated sea spray aerosol particles are flash frozen in their native state with iterative and controlled thermal and/or pressure exposures and then probed by electron microscopy. This unique approach allows for the detection of not only mixed salts, but also soft materials including whole hydrated bacteria, diatoms, virus particles, marine vesicles, as well as gel networks within hydrated salt droplets-all of which will have distinct biological, chemical, and physical processes. We anticipate this method will open up a new avenue of analysis for aerosol particles, not only for ocean-derived aerosols, but for those produced from other sources where there is interest in the transfer of organic or biological species from the biosphere to the atmosphere.

  1. Temporal variation of "solar dimming" induced by composite and carbonaceous aerosols: Observations from mineral-rich eastern Indian region

    Science.gov (United States)

    Latha, R.; Murthy, B. S.; Lipi, K.; Kumar, Manoj; Das, S. K.; Mahanti, N. C.

    2014-05-01

    Composite and carbonaceous aerosol radiative forcing (RF) over Ranchi (23.5°N, 85.3°E) in eastern India at monthly and seasonal scales during February 2011 to January 2012 is derived from mean optical properties obtained from Sun-sky radiometer and a radiative transfer model. Ranchi is located on the Chotanagpur plateau at 650 m above mean sea level; the region is unique with dense open active mines, a source of mineral aerosols with opposing optical properties such as coal and limestone. Diurnal mean composite aerosol RF at the surface, in the spectral band 0.3-3.0 µm increases from winter (December, January, February) to premonsoon (March, April, May) with maximum (-65 Wm-2) aerosol RF in March that is associated with highest black carbon (BC) aerosol optical depth (AOD), 0.05. Minimum surface aerosol RF occurs in July with minimum values of AOD and AODBC. Aerosol RF at top of the atmosphere is maximum (-17 Wm-2) in April, and is positive (+1.2 Wm-2) in March. On an average, carbonaceous aerosols (BC) contribute ~8.8% to total AOD and about 60% to total atmospheric absorption. A rapid increase of BC is seen in the postmonsoon with 1.0 µg m-3 in September to 3.0 µg m-3 in October. Aerosol-induced solar dimming is about 9.4% (premonsoon), 7.0% (monsoon), 10.6% (postmonsoon), and 10.2% (winter) of the surface radiation. Seasonal mean aerosol heating rate is observed to be maximum in premonsoon (~1.15°K/d-1), followed by postmonsoon, while winter and monsoon experience minimum (~0.45°K/d-1) heating, assuming typical aerosol profiles of the model.

  2. Influence of sugar cane burning on aerosol soluble ion composition in Southeastern Brazil

    Science.gov (United States)

    Allen, A. G.; Cardoso, A. A.; da Rocha, G. O.

    2004-09-01

    Seasonal variability in the major soluble ion composition of atmospheric particulate matter in the principal sugar cane growing region of central São Paulo State indicates that pre-harvest burning of sugar cane plants is an important influence on the regional scale aerosol chemistry. Samples of particulate matter were collected between April 1999 and February 2001 in coarse (> 3.5 μm) and fine (polluted urban environments, the massive increases during much of the year, due to a single anthropogenic activity (sugar cane burning) are indicative of a very large perturbation of the lower troposphere in the region relative to the natural condition. These aerosols are suspected of promoting respiratory disease. They also represent an important mechanism for the tropospheric transport of species relevant to surface acidification (sulphates, nitrates, ammonium and organic acids) and soil nutrient status (potassium, nitrogen, ammonium, calcium), so their impact on fragile natural ecosystems (following deposition) needs to be considered.

  3. Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Dron, J.; El Haddad, I.; Temime-Roussel, B.; Wortham, H.; Marchand, N. [Univ Aix Marseille, CNRS, Lab Chim Provence, Equipe Instrumentat and React Atmospher, UMR 6264, F-13331 Marseille 3 (France); Jaffrezo, J.L. [Univ Grenoble 1, CNRS, UMR 5183, Lab Glaciol and Geophys Environm, F-38402 St Martin Dheres (France)

    2010-07-01

    The functional group composition of various organic aerosols (OA) is investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCIMS/MS). The determinations of three functional groups contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups, R-COOH and R-CO-R' respectively) and precursor ion (nitro groups, R-NO{sub 2}) scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA) produced through photooxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounts for 1.7% (vehicular) to 13.5% (o-xylene photooxidation) of the organic carbon. Diagnostic functional group ratios are then used to tentatively discriminate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France) during a strong winter pollution event. The three functional groups under study account for a total functionalization rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also dominated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitro- and carbonyl-to-carboxylic diagnostic ratios can be a useful tool to discriminate sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assess a wood burning organic carbon contribution of about 60%. Finally, examples of functional

  4. Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

    Directory of Open Access Journals (Sweden)

    J. Dron

    2010-08-01

    Full Text Available The functional group composition of various organic aerosols (OA is investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCI-MS/MS. The determinations of three functional groups contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups, R-COOH and R-CO-R´ respectively and precursor ion (nitro groups, R-NO2 scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA produced through photooxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounts for 1.7% (vehicular to 13.5% (o-xylene photooxidation of the organic carbon. Diagnostic functional group ratios are then used to tentatively discriminate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France during a strong winter pollution event. The three functional groups under study account for a total functionalisation rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also dominated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitro- and carbonyl-to-carboxylic diagnostic ratios can be a useful tool to discriminate sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assess a wood burning organic carbon contribution of about 60

  5. The time evolution of aerosol composition over the Mexico City plateau

    Directory of Open Access Journals (Sweden)

    J. Hubbe

    2008-03-01

    Full Text Available The time evolution of aerosol concentration and chemical composition in a megacity urban plume was determined based on 8 flights of the DOE G-1 aircraft in and downwind of Mexico City during the March 2006 MILAGRO field campaign. A series of selection criteria are imposed to eliminate data points with non-urban emission influences. Biomass burning has urban and non-urban sources that are distinguished on the basis of CH3CN and CO. In order to account for dilution in the urban plume, aerosol concentrations are normalized to CO which is taken as an inert tracer of urban emission, proportional to the emissions of aerosol precursors. Time evolution is determined with respect to photochemical age defined as −Log10 (NOx/NOy. The geographic distribution of photochemical age and CO is examined, confirming the picture that Mexico City is a source region and that pollutants become more dilute and aged as they are advected towards T1 and T2, surface sites that are located at the fringe of the City and 35 km to the NE, respectively. Organic aerosol (OA per ppm CO is found to increase 7 fold over the range of photochemical ages studied, corresponding to a change in NOx/NOy from nearly 100% to 10%. In the older samples the nitrate/CO ratio has leveled off suggesting that evaporation and formation of aerosol nitrate are in balance. In contrast, OA/CO increases with age in older samples, indicating that OA is still being formed. The amount of carbon equivalent to the deduced change in OA/CO with age is 56 ppbC per ppm CO. At an aerosol yield of 5% and 8% for low and high yield aromatic compounds, it is estimated from surface hydrocarbon observations that only ~9% of the OA formation can be accounted for. A comparison of OA/CO in Mexico City and the eastern U.S. gives no evidence that aerosol yields are higher in a more polluted environment.

  6. Impact of North America on the aerosol composition in the North Atlantic free troposphere

    Directory of Open Access Journals (Sweden)

    M. I. García

    2017-06-01

    Full Text Available In the AEROATLAN project we study the composition of aerosols collected over  ∼  5 years at Izaña Observatory (located at  ∼  2400 m a.s.l. in Tenerife, the Canary Islands under the prevailing westerly airflows typical of the North Atlantic free troposphere at subtropical latitudes and midlatitudes. Mass concentrations of sub-10 µm aerosols (PM10 carried by westerly winds to Izaña, after transatlantic transport, are typically within the range 1.2 and 4.2 µg m−3 (20th and 80th percentiles. The main contributors to background levels of aerosols (PM10 within the 1st–50th percentiles  =  0.15–2.54 µg m−3 are North American dust (53 %, non-sea-salt sulfate (14 % and organic matter (18 %. High PM10 events (75th–95th percentiles  ≈  4.0–9.0 µg m−3 are prompted by dust (56 %, organic matter (24 % and non-sea-salt sulfate (9 %. These aerosol components experience a seasonal evolution explained by (i their spatial distribution in North America and (ii the seasonal shift of the North American outflow, which migrates from low latitudes in winter (∼  32° N, January–March to high latitudes in summer (∼  52° N, August–September. The westerlies carry maximum loads of non-sea-salt sulfate, ammonium and organic matter in spring (March–May, of North American dust from midwinter to mid-spring (February–May and of elemental carbon in summer (August–September. Our results suggest that a significant fraction of organic aerosols may be linked to sources other than combustion (e.g. biogenic; further studies are necessary for this topic. The present study suggests that long-term evolution of the aerosol composition in the North Atlantic free troposphere will be influenced by air quality policies and the use of soils (potential dust emitter in North America.

  7. Predicting the mineral composition of dust aerosols: Insights from elemental composition measured at the Izaña Observatory

    Science.gov (United States)

    Pérez García-Pando, Carlos; Miller, Ron L.; Perlwitz, Jan P.; Rodríguez, Sergio; Prospero, Joseph M.

    2016-10-01

    Regional variations of dust mineral composition are fundamental to climate impacts but generally neglected in climate models. A challenge for models is that atlases of soil composition are derived from measurements following wet sieving, which destroys the aggregates potentially emitted from the soil. Aggregates are crucial to simulating the observed size distribution of emitted soil particles. We use an extension of brittle fragmentation theory in a global dust model to account for these aggregates. Our method reproduces the size-resolved dust concentration along with the approximately size-invariant fractional abundance of elements like Fe and Al in the decade-long aerosol record from the Izaña Observatory, off the coast of West Africa. By distinguishing between Fe in structural and free forms, we can attribute improved model behavior to aggregation of Fe and Al-rich clay particles. We also demonstrate the importance of size-resolved measurements along with elemental composition analysis to constrain models.

  8. Aerosol size and chemical composition measurements at the Polar Environment Atmospheric Research Lab (PEARL) in Eureka, Nunavut

    Science.gov (United States)

    Hayes, P. L.; Tremblay, S.; Chang, R. Y. W.; Leaitch, R.; Kolonjari, F.; O'Neill, N. T.; Chaubey, J. P.; AboEl Fetouh, Y.; Fogal, P.; Drummond, J. R.

    2016-12-01

    This study presents observations of aerosol chemical composition and particle number size distribution at the Polar Environment Atmospheric Research Laboratory (PEARL) in the Canadian High Arctic (80N, 86W). The current aerosol measurement program at PEARL has been ongoing for more than a year providing long-term observations of Arctic aerosol size distributions for both coarse and fine modes. Particle nucleation events were frequently observed during the summers of 2015 and 2016. The size distribution data are also compared against similar measurements taken at the Alert Global Atmospheric Watch Observatory (82N, 62W) for July and August 2015. The nucleation events are correlated at the two sites, despite a distance of approximately 500 km, suggesting regional conditions favorable for particle nucleation and growth during this period. Size resolved chemical composition measurements were also carried out using an aerosol mass spectrometer. The smallest measured particles between 40 and 60 nm are almost entirely organic aerosol (OA) indicating that the condensation of organic vapors is responsible for particle growth events and possibly particle nucleation. This conclusion is further supported by the relatively high oxygen content of the OA, which is consistent with secondary formation of OA via atmospheric oxidation.Lastly, surface measurements of the aerosol scattering coefficient are compared against the coefficient values calculated using Mie theory and the measured aerosol size distribution. Both the actual and the calculated scattering coefficients are then compared to sun photometer measurements to understand the relationship between surface and columnar aerosol optical properties. The measurements at PEARL provide a unique combination of surface and columnar data sets on aerosols in the High Arctic, a region where such measurements are scarce despite the important impact of aerosols on Arctic climate.PEARL research is supported by the Natural Sciences and

  9. Estimation of aerosol particle composition using ground-based sun-sky radiometer measurements at typical sites in China

    Science.gov (United States)

    Li, Z.; Gu, X.; Wang, L.; Li, D.; Xing, X.; Gai, J.; Wang, Q.; Li, K.; Li, L.; Zhang, Y.

    2011-12-01

    Atmospheric aerosol affects climate and environment through radiative and health effects determined by its physical and chemical properties. In this study, we modeled aerosol by an internal mixture of different components like water, sulfate and black carbon following Maxwell-Garnett effective medium approximation theory. In order to deal with complex aerosol mixing situation in China, we considered extra mineral dust component in case of large particles. Remote sensing data obtained from ground-based CE318 sun-sky radiometers in typical China sites are used to derive the aerosol mixture model. Measurements are firstly calibrated by using intercomparison and vicarious calibration methods and then retrieved by using AErosol RObotic NETwork (AERONET) inversion algorithm to obtain refractive indices of the mixture, which are then used to yield aerosol component fraction. Results at typical China regions like megacity, industrial, arid, oceanic and background sites show considerable difference between their aerosol particle compositions and agree with a priori information like regional aerosol sources and formation processes.

  10. Seasonality of New Particle Formation in Vienna, Austria - Influence of Air Mass Origin and Aerosol Chemical Composition

    Czech Academy of Sciences Publication Activity Database

    Wonaschütz, A.; Demattio, A.; Wagner, R.; Burkart, J.; Zíková, Naděžda; Vodička, Petr; Ludwig, W.; Steiner, G.; Schwarz, Jaroslav; Hitzenberger, R.

    2015-01-01

    Roč. 118, OCT 2015 (2015), s. 118-126 ISSN 1352-2310 R&D Projects: GA MŠk 7AMB12AT021; GA ČR(CZ) GBP503/12/G147 Grant - others:FWF(AT) P19515-N20 Institutional support: RVO:67985858 Keywords : urban aerosol * aerosol chemical composition * new particle formation Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.459, year: 2015

  11. Variations in Aerosol Chemical Composition during New Particle Formation and Growth Events Downwind of Seoul, Korea

    Science.gov (United States)

    Park, J.; Choi, Y.; Ghim, Y. S.

    2016-12-01

    New particle formation and growth has been characterized through various field studies using scanning mobility particle sizer (SMPS). However, there is insufficient knowledge of the variation of aerosol chemical compositions during those events. We investigated the variation of aerosol chemical composition during new particle formation and growth events downwind of Seoul. New particle formation and growth events were identified based on the evolution of the number size distribution measured by SMPS. The concentrations of inorganic ions and black carbon were measured using a particle-into-liquid sampler (PILS) coupled with an ion chromatograph (IC) and multi-angle absorption photometer (MAAP), respectively. We also measured concentrations of gaseous precursors (SO2, NO2) along with meteorological parameters using an automatic weather station. The measurements were conducted on the rooftop of a five-story building on a hill (37.34°N, 127.27°E, 167 m above sea level) at the Global Campus of Hankuk University of Foreign Studies, located about 35 km southeast of downtown Seoul. The measurement periods were from February 12 to April 1, 2015 and from April 13 to June 12, 2016. We investigated the difference in chemical compositions between event and non-event days and its association with the variations in precursor concentrations and meteorological parameters.

  12. CCN predictions using simplified assumptions of organic aerosol composition and mixing state: a synthesis from six different locations

    Directory of Open Access Journals (Sweden)

    B. Ervens

    2010-05-01

    Full Text Available An accurate but simple quantification of the fraction of aerosol particles that can act as cloud condensation nuclei (CCN is needed for implementation in large-scale models. Data on aerosol size distribution, chemical composition, and CCN concentration from six different locations have been analyzed to explore the extent to which simple assumptions of composition and mixing state of the organic fraction can reproduce measured CCN number concentrations.

    Fresher pollution aerosol as encountered in Riverside, CA, and the ship channel in Houston, TX, cannot be represented without knowledge of more complex (size-resolved composition. For aerosol that has experienced processing (Mexico City, Holme Moss (UK, Point Reyes (CA, and Chebogue Point (Canada, CCN can be predicted within a factor of two assuming either externally or internally mixed soluble organics although these simplified compositions/mixing states might not represent the actual properties of ambient aerosol populations, in agreement with many previous CCN studies in the literature. Under typical conditions, a factor of two uncertainty in CCN concentration due to composition assumptions translates to an uncertainty of ~15% in cloud drop concentration, which might be adequate for large-scale models given the much larger uncertainty in cloudiness.

  13. Aerosol composition and microstructure in the smoky atmosphere of Moscow during the August 2010 extreme wildfires

    Science.gov (United States)

    Popovicheva, O. B.; Kistler, M.; Kireeva, E. D.; Persiantseva, N. M.; Timofeev, M. A.; Shoniya, N. K.; Kopeikin, V. M.

    2017-01-01

    This is a comprehensive study of the physicochemical characterization of multicomponent aerosols in the smoky atmosphere of Moscow during the extreme wildfires of August 2010 and against the background atmosphere of August 2011. Thermal-optical analysis, liquid and ion chromatography, IR spectroscopy, and electron microscopy were used to determine the organic content (OC) and elemental content (EC) of carbon, organic/inorganic and ionic compounds, and biomass burning markers (anhydrosaccharides and the potassium ion) and study the morphology and elemental composition of individual particles. It has been shown that the fires are characterized by an increased OC/EC ratio and high concentrations of ammonium, potassium, and sulfate ions in correlation with an increased content of levoglucosan as a marker of biomass burning. The organic compounds containing carbonyl groups point to the process of photochemical aging and the formation of secondary organic aerosols in the urban atmosphere when aerosols are emitted from forest fires. A cluster analysis of individual particles has indicated that when the smokiest atmosphere is characterized by prevailing soot/tar ball particles, which are smoke-emission micromarkers.

  14. Morphology, Composition, and Mixing State of Individual Aerosol Particles in Northeast China during Wintertime

    Directory of Open Access Journals (Sweden)

    Liang Xu

    2017-02-01

    Full Text Available Northeast China is located in a high latitude area of the world and undergoes a cold season that lasts six months each year. Recently, regional haze episodes with high concentrations of fine particles (PM2.5 have frequently been occurring in Northeast China during the heating period, but little information has been available. Aerosol particles were collected in winter at a site in a suburban county town (T1 and a site in a background rural area (T2. Morphology, size, elemental composition, and mixing state of individual aerosol particles were characterized by transmission electron microscopy (TEM. Aerosol particles were mainly composed of organic matter (OM and S-rich and certain amounts of soot and K-rich. OM represented the most abundant particles, accounting for 60.7% and 53.5% at the T1 and T2 sites, respectively. Abundant spherical OM particles were likely emitted directly from coal-burning stoves. Soot decreased from 16.9% at the T1 site to 4.6% at the T2 site and sulfate particles decrease from 35.9% at the T2 site to 15.7% at the T1 site, suggesting that long-range transport air masses experienced more aging processes and produced more secondary particles. Based on our investigations, we proposed that emissions from coal-burning stoves in most rural areas of the west part of Northeast China can induce regional haze episodes.

  15. Estimation of atmospheric aerosol composition from ground-based remote sensing measurements of Sun-sky radiometer

    Science.gov (United States)

    Xie, Y. S.; Li, Z. Q.; Zhang, Y. X.; Zhang, Y.; Li, D. H.; Li, K. T.; Xu, H.; Zhang, Y.; Wang, Y. Q.; Chen, X. F.; Schauer, J. J.; Bergin, M.

    2017-01-01

    Remote sensing provides aerosol loading information, but to address climate and air quality model validation, there are additional needs to acquire aerosol composition information. In this study, a comprehensive aerosol composition model is established to quantify black carbon (BC), brown carbon (BrC), mineral dust (DU), particulate organic matters, ammonium sulfate like (AS), sea salt, and aerosol water uptake. We develop forward modeling of aerosol components, including microphysical parameters (real and imaginary refractive indices, volume fraction ratio of fine to coarse mode, and sphericity) and hygroscopic growth models, and propose an optimization scheme to estimate the components. The uncertainties caused by input parameters are also assessed. Sun-sky radiometer measurements and meteorological data obtained during a campaign in Huairou, Beijing, are processed to estimate aerosol components, which are further compared with synchronous in situ chemical measurements. The results show generally good consistencies between remotely estimated and measured components (e.g., correlation coefficients for BC, BrC, AS, and PM2.5 lie in about 0.8-0.9). The comparisons between modeled and observed microphysical parameters also show good agreements, with the exception of sphericity, which is likely caused by high uncertainties of this parameter. Sensitivity studies show that BC and BrC are highly sensitive to imaginary refractive index, while DU is strongly correlated to both volume size and sphericity. The performance of composition retrieval is expected to be improved when the sphericity uncertainty is significantly reduced.

  16. Photoacoustic measurements of photokinetics in single optically trapped aerosol droplets

    Science.gov (United States)

    Covert, Paul; Cremer, Johannes; Signorell, Ruth; Thaler, Klemens; Haisch, Christoph

    2017-04-01

    It is well established that interaction of light with atmospheric aerosols has a large impact on the Earth's climate. However, uncertainties in the magnitude of this impact remain large, due in part to broad distributions of aerosol size, composition, and chemical reactivity. In this context, photoacoustic spectroscopy is commonly used to measure light absorption by aerosols. Here, we present photoacoustic measurements of single, optically-trapped nanodroplets to reveal droplet size-depencies of photochemical and physical processes. Theoretical considerations have pointed to a size-dependence in the magnitude and phase of the photoacoustic response from aerosol droplets. This dependence is thought to originate from heat transfer processes that are slow compared to the acoustic excitation frequency. In the case of a model aerosol, our measurements of single particle absorption cross-section versus droplet size confirm these theoretical predictions. In a related study, using the same model aerosol, we also demonstrate a droplet size-dependence of photochemical reaction rates [1]. Within sub-micron sized particles, photolysis rates were observed to be an order of magnitude greater than those observed in larger droplets. [1] J. W. Cremer, K. M. Thaler, C. Haisch, and R. Signorell. Photoacoustics of single laser-trapped nanodroplets for the direct observation of nanofocusing in aerosol photokinetics. Nat. Commun., 7:10941, 2016.

  17. Influence of Heterogeneous OH Oxidation on the Evaporation Behavior and Composition of a Model Organic Aerosol

    Science.gov (United States)

    Kolesar, K. R.; Cappa, C. D.; Wilson, K. R.

    2011-12-01

    Heterogeneously oxidized squalane particles are used here as a model system to investigate the interplay between chemical composition and particle volatility. Reaction of squalane particles by OH radicals leads to the production of oxygenated products. Here we use the vacuum ultra-violet Aerosol Mass Spectrometer (VUV-AMS) at beamline 9.0.2 at the Advanced Light Source to monitor the evolution of specific oxidation products that result from increasing OH exposures, and how the composition changes as the oxidized particles evaporate. The soft ionization in the VUV-AMS allows us to uniquely track the parent squalane molecule and the various oxidation products over multiple generations of oxidation. Compositional changes of the oxidized particles resulting from evaporation have been measured in three sets of laboratory experiments. In the first set, a thermodenuder at varying temperatures was used to induce evaporation of particles at a fixed OH exposure. Second, the OH exposure was varied along with temperature to create a cross-sectional observation of particle composition at 50% mass fraction remaining for ten different oxidation levels. The combination of these two experiments provides information as to the compositional changes that occur during evaporation due to heating. In the third set of experiments, VUV-AMS spectra of oxidized squalane particles following dilution-induced evaporation were measured for comparison with the thermodenuder experiments. These experiments provide insights into the relationships between particle oxidation, composition and evaporation kinetics.

  18. Effect of humidity on the composition of isoprene photooxidation secondary organic aerosol

    Directory of Open Access Journals (Sweden)

    T. B. Nguyen

    2011-07-01

    Full Text Available The effect of relative humidity (RH on the composition and concentrations of gas-phase products and secondary organic aerosol (SOA generated from the photooxidation of isoprene under high-NOx conditions was investigated. Experiments were performed with hydrogen peroxide as the OH precursor and in the absence of seed aerosol. The relative yields of most gas-phase products were the same regardless of initial water vapor concentration with exception of hydroxyacetone and glycolaldehyde, which were considerably affected by RH. A significant change was observed in the SOA composition, with many unique condensed-phase products formed under humid (90 % RH vs. dry (<2 % RH conditions, without any detectable effect on the rate and extent of the SOA mass growth. There is a 40 % reduction in the number and relative abundance of distinct particle-phase nitrogen-containing organic compounds (NOC detected by high resolution mass spectrometry. The suppression of condensation reactions, which produce water as a product, is the most important chemical effect of the increased RH. For example, the total signal from oligomeric esters of 2-methylglyceric acid was reduced by about 60 % under humid conditions and the maximum oligomer chain lengths were reduced by 7–11 carbons. Oligomers formed by addition mechanisms, without direct involvement of water, also decreased at elevated RH but to a much smaller extent. The observed reduction in the extent of condensation-type oligomerization at high RH may have substantial impact on the phase characteristics and hygroscopicity of the isoprene aerosol. The reduction in the amount of organic nitrates in the particle phase has implications for understanding the budget of NOC compounds.

  19. Hygroscopicity of Chemically Aged, sub-micron Squalane Particles: On the Role of Size and Composition towards the Hygroscopicity Parameter κ

    Science.gov (United States)

    Harmon, C. W.; Smith, J. D.; Che, D. L.; Leone, S. R.; Wilson, K. R.

    2010-12-01

    Measurements presented herein explore cloud condensation nuclei (CCN) activity of sub-micron squalane particles chemically aged by hydroxyl radicals as a function of size and OH exposure. As squalane particles are exposed to OH radicals, size-selected 100, 150, and 200 nm particles monotically decrease in size with increasing OH exposure. Concurrently, their CCN derived hygroscopicity parameter values, κ, increase with OH exposure until saturating at 0.165 in the 100 nm data set, 0.140 in the 150 nm data set, and reach a maximum value of 0.075 in the 200 nm data set at the highest level of OH exposure. The critical super-saturation relative humidity (RH) at which CCN activity is achieved decreases initially with increasing OH exposure and then increases with OH exposure, most notably for the 100 nm data set and weakly with the 150 nm data set. Chemically aged squalane particles from the 200 nm data set show a monotonic decrease in critical super-saturation RH with all values of increasing OH exposure between 0.1-2.5 × 10^13 s molec./cc. The measured O:C ratios of 160 nm chemically aged squalane particles, which were reported previously, are compared to κ values by the CCN derived relationship reported in literature: κ = 0.30*O:C and reasonable agreement is attained in the size-selected 150 nm data set. These values are also compared with the hygroscopic growth factor derived relationship in literature: κ = 0.49*(O:C -0.25) and reasonable agreement is attained at O:C > 0.35.

  20. PHYSICOCHEMICAL PROPERTIES OF THE SOLID COMPONENT OF WELDING AEROSOL. I. PHASE COMPOSITION

    Directory of Open Access Journals (Sweden)

    T. L. Rakitskaya

    2015-02-01

    Full Text Available The phase composition of the solid component of welding aerosol (SCWA obtained as a result of metal welding with electrodes of ANO-4 and TsL-11 types manufactured according to ISO 2560 E432R 21 and ISO E19.9NbB20 standards, respectively, and differing in com-position of their wires and coatings was determined with the help of a Siemens D500 diffrac- a Siemens D500 diffrac-tometer supplied with the manufacturer’s software. Four and thirteen phases were identified in SCWA-ANO-4 and SCWA-TsL-11, respectively. Evaluation of crystallite sizes by the use of the Scherer equation showed that the crystallites formed in the course of welding with a TsL-11 type electrode are larger than those in the case of an ANO-4 type one: 65-89 nm and 30-49 nm, respectively.

  1. Submicron particle chemistry: Vapor condensation analogous to liquid solidification

    Science.gov (United States)

    Jenkins, Neil T.; Eagar, Thomas W.

    2003-06-01

    The chemical composition of submicron particles condensed from vapor can vary with particle size. This chemical variation with size affects industrial health estimates and technological innovation. A model based on similar behavior during the solidification of liquids is proposed to explain this behavior.

  2. Optical properties and chemical composition of the atmospheric aerosol in urban Guangzhou, China

    Science.gov (United States)

    Andreae, Meinrat O.; Schmid, Otmar; Yang, Hong; Chand, Duli; Zhen Yu, Jian; Zeng, Li-Min; Zhang, Yuan-Hang

    During the Pearl River Delta measurement campaign (Program of Regional Integrated Experiments of Air Quality over Pearl River Delta 2004, PRIDE-PRD2004, 4 October-5 November 2004), we measured aerosol light absorption and scattering (PM2.5) in urban Guangzhou, using a photoacoustic spectrometer and two integrating nephelometers (at ambient and dry humidity). In addition, 12-h averages of elemental carbon (EC a), organic carbon (OC), and inorganic species concentrations were determined. Aerosol concentrations in urban Guangzhou were extremely high, with average PM2.5, OC, and EC a concentrations of 103, 22.4, and 7.1 μg m -3, respectively. The chemical composition of the aerosol was dominated by particulate organic matter, EC a, sulfate and ammonium. Elevated levels of potassium indicated significant contributions from biomass burning to the regional haze. The high average OC/EC a ratio of 3.6±1.1 resulted from a mixture of regional haze with high OC content and local emissions with low OC/EC a, mostly from vehicular sources. The average scattering and absorption coefficients for dry aerosol were 418 and 91 Mm -1 ( λ˜540 nm), and the mean mass scattering and absorption efficiencies 4.2±1.0 and 0.78±0.19 m 2 g -1. During some episodes resulting from the trapping of local emissions in a nocturnal boundary layer, extreme values of aerosol absorption were reached (up to 490 Mm -1). The average single scattering albedo ( ω0, λ˜540 nm) at dry conditions was about 0.83, representing a mixture of fresh, strongly absorbing, urban pollution, and a more scattering regional haze. Because of the prevailing low humidity, the ambient ω0 was not significantly higher. The mass absorption efficiency of EC a was 7.7 m 2 g -1; an additional contribution to absorption was associated with OC, either as a result of light absorption by OC or the effects of internal mixing. The observed diurnal trends of the optical and chemical properties are consistent with aged regional haze

  3. Measurement of Ambient Aerosol Composition Using an Aerosol Mass Spectrometer: New York 2001 Supersite Summer Intensive Study

    Science.gov (United States)

    Drewnick, F.; Schwab, J. J.; Demerjian, K. L.

    2002-12-01

    A summer field measurement campaign in Queens, New York during July 2001 was operated as part of the PM2.5 Technology Assessment and Characterization Study in New York (PMTACS-NY) Supersite program. During this study several state-of-the art aerosol instruments were deployed including an Aerosol Mass Spectrometer (AMS, Aerodyne Research, Inc.). This AMS is designed to deliver quantitative information on mass loadings and size-resolved mass distributions of volatile and semi-volatile aerosol chemical species. AMS aerosol mass concentration measurements made during the campaign indicated significant contributions of sulfate and organic species to the total aerosol mass concentration. Sulfate, ranging from 0.05 μg/m3 for clean days to 53 μg/m3 for the most polluted period, had a median concentration of 2.6 μg/m3. The total organics mass concentration, with a median mass concentration of 2.7 μg/m3, ranged from 0.5 μg/m3 up to 29 μg/m3. In addition species-resolved size distribution measurements for sulfate, nitrate and organic aerosol particles indicate that sulfate and nitrate occur mainly internally mixed while the organic particles show a completely different size distribution, reflecting their different sources. AMS mass concentration measurements combined with total aerosol mass concentration data from a co-located TEOM are used to provide a continuous mass balance with 10-min time resolution. Diurnal patterns of absolute sulfate, nitrate and organics mass concentration as well as diurnal patterns of relative contributions of different types of organic particles are calculated using the AMS mass concentration data. Typical size distributions as well as the evolution processes of particulate sulfate size distributions are presented, measured during high background concentrations of organic particles. In addition, capabilities and limitations of the AMS instrument, as indicated by laboratory testing and evaluation studies in the laboratory and in the field

  4. Chemical composition based aerosol optical properties according to size distribution and mixture types during smog and Asian dust events in Seoul, Korea

    Science.gov (United States)

    Jung, Chang Hoon; Lee, Ji Yi; Um, Junshik; Lee, Seung Soo; Kim, Yong Pyo

    2017-09-01

    This study investigated the optical properties of aerosols involved in different meteorological events, including smog and Asian dust days. Carbonaceous components and inorganic species were measured in Seoul, Korea between 25 and 31 March 2012. Based on the measurements, the optical properties of aerosols were calculated by considering composition, size distribution, and mixing state of aerosols. To represent polydisperse size distributions of aerosols, a lognormal size distribution with a wide range of geometric mean diameters and geometric standard deviations was used. For the optical property calculations, the Mie theory was used to compute single-scattering properties of aerosol particles with varying size and composition. Analysis of the sampled data showed that the water-soluble components of organic matter increased on smog days, whereas crustal elements increased on dust days. The water content significantly influenced the optical properties of aerosols during the smog days as a result of high relative humidity and an increase in the water-soluble component. The absorption coefficients depended on the aerosol mixture type and the aerosol size distributions. Therefore, to improve our knowledge on radiative impacts of aerosols, especially the regional impacts of aerosols in East Asia, accurate measurements of aerosols, such as size distribution, composition, and mixture type, under different meteorological conditions are required.

  5. Chemical, physical, and optical evolution of biomass burning aerosols: a case study

    Directory of Open Access Journals (Sweden)

    G. Adler

    2011-02-01

    Full Text Available In-situ chemical composition measurements of ambient aerosols have been used for characterizing the evolution of submicron aerosols from a large anthropogenic biomass burning (BB event in Israel. A high resolution Time of Flight Aerosol Mass Spectrometer (HR-RES-TOF-AMS was used to follow the chemical evolution of BB aerosols during a night-long, extensive nationwide wood burning event and during the following day. While these types of extensive BB events are not common in this region, burning of agricultural waste is a common practice. The aging process of the BB aerosols was followed through their chemical, physical and optical properties. Mass spectrometric analysis of the aerosol organic component showed that aerosol aging is characterized by shifting from less oxidized fresh BB aerosols to more oxidized aerosols. Evidence for aerosol aging during the day following the BB event was indicated by an increase in the organic mass, its oxidation state, the total aerosol concentration, and a shift in the modal particle diameter. The effective broadband refractive index (EBRI was derived using a white light optical particle counter (WELAS. The average EBRI for a mixed population of aerosols dominated by open fires was m = 1.53(±0.03 + 0.07i(±0.03, during the smoldering phase of the fires we found the EBRI to be m = 1.54(±0.01 + 0.04i(±0.01 compared to m = 1.49(±0.01 + 0.02i(±0.01 of the aged aerosols during the following day. This change indicates a decrease in the overall aerosol absorption and scattering. Elevated levels of particulate Polycyclic Aromatic Hydrocarbons (PAHs were detected during the entire event, which suggest possible implications for human health during such extensive event.

  6. Aerosol composition and properties variation at the ground and over the column under different air masses advection in South Italy.

    Science.gov (United States)

    Pavese, G; Lettino, A; Calvello, M; Esposito, F; Fiore, S

    2016-04-01

    Aerosol composition and properties variation under the advection of different air masses were investigated, as case studies, by contemporary measurements over the atmospheric column and at the ground in a semi-rural site in South Italy. The absence of local strong sources in this area allowed to characterize background aerosol and to compare particle mixing effects under various atmospheric circulation conditions. Aerosol optical depth (AOD) and Ǻngström parameters from radiometric measurements allowed the detection and identification of polluted, dust, and volcanic atmospheric conditions. AODs were the input for a suitable model to evaluate the columnar aerosol composition, according to six main atmospheric components (water-soluble, soot, sea salt accumulation, sea salt coarse, mineral dus,t and biological). Scanning electron microscope (SEM) analysis of particulate sampled with a 13-stage impactor at the ground showed not only fingerprints typical of the different air masses but also the effects of transport and aging on atmospheric particles, suggesting processes that changed their chemical and optical properties. Background columnar aerosol was characterized by 72% of water-soluble and soot, in agreement with ground-based findings that highlighted 60% of contribution from anthropogenic carbonate particles and soot. In general, a good agreement between ground-based and columnar results was observed. Under the advection of trans-boundary air masses, water-soluble and soot were always present in columnar aerosol, whereas, in variable percentages, sea salt and mineral particles characterized both dust and volcanic conditions. At the ground, sulfates characterized the amorphous matrix produced in finer stages by the evaporation of solutions of organic and inorganic aerosols. Sulfates were also one of the key players involved in heterogeneous chemical reactions, producing complex secondary aerosol, as such clay-sulfate internally mixed particle externally mixed

  7. Characterization of aerosol optical properties, chemical composition and mixing states in the winter season in Shanghai, China.

    Science.gov (United States)

    Tang, Yong; Huang, Yuanlong; Li, Ling; Chen, Hong; Chen, Jianmin; Yang, Xin; Gao, Song; Gross, Deborah S

    2014-12-01

    Physical and chemical properties of ambient aerosols at the single particle level were studied in Shanghai from December 22 to 28, 2009. A Cavity-Ring-Down Aerosol Extinction Spectrometer (CRD-AES) and a nephelometer were deployed to measure aerosol light extinction and scattering properties, respectively. An Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) was used to detect single particle sizes and chemical composition. Seven particle types were detected. Air parcels arrived at the sampling site from the vicinity of Shanghai until mid-day of December 25, when they started to originate from North China. The aerosol extinction, scattering, and absorption coefficients all dropped sharply when this cold, clean air arrived. Aerosol particles changed from a highly aged type before this meteorological shift to a relatively fresh type afterwards. The aerosol optical properties were dependent on the wind direction. Aerosols with high extinction coefficient and scattering Ångström exponent (SAE) were observed when the wind blew from the west and northwest, indicating that they were predominantly fine particles. Nitrate and ammonium correlated most strongly with the change in aerosol optical properties. In the elemental carbon/organic carbon (ECOC) particle type, the diurnal trends of single scattering albedo (SSA) and elemental carbon (EC) signal intensity had a negative correlation. We also found a negative correlation (r=-0.87) between high mass-OC particle number fraction and the SSA in a relatively clean period, suggesting that particulate aromatic components might play an important role in light absorption in urban areas. Copyright © 2014. Published by Elsevier B.V.

  8. OCEANFILMS-2: Representing coadsorption of saccharides in marine films and potential impacts on modeled marine aerosol chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Burrows, Susannah M. [Atmospheric Science and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Gobrogge, Eric [Department of Chemistry and Biochemistry, Montana State University, Bozeman Montana USA; Fu, Li [Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland Washington USA; Link, Katie [Department of Chemistry and Biochemistry, Montana State University, Bozeman Montana USA; Elliott, Scott M. [Climate, Ocean, and Sea Ice Modelling Group, Los Alamos National Laboratory, Los Alamos New Mexico USA; Wang, Hongfei [Environmental and Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland Washington USA; Walker, Rob [Department of Chemistry and Biochemistry, Montana State University, Bozeman Montana USA

    2016-08-10

    Here we show that the addition of chemical interactions of soluble polysaccharides with a surfactant monolayer improves agreement of modeled sea spray chemistry with observed marine aerosol chemistry. In particular, the fraction of hydroxyl functional groups in modeled sea spray organic matter is increased, improving agreement with FTIR observations of marine aerosol composition. The overall organic fraction of submicron sea spray also increases, allowing organic mass fractions in the range 0.5 – 0.7 for submicron sea spray particles over highly active phytoplankton blooms. We show results from Sum Frequency Generation (SFG) experiments that support the modeling approach, by demonstrating that soluble polysaccharides can strongly adsorb to a lipid monolayer via columbic interactions under appropriate conditions.

  9. Chemical composition and hygroscopic properties of aerosol particles over the Aegean Sea

    Science.gov (United States)

    Bezantakos, S.; Barmpounis, K.; Giamarelou, M.; Bossioli, E.; Tombrou, M.; Mihalopoulos, N.; Eleftheriadis, K.; Kalogiros, J.; Allan, J. D.; Bacak, A.; Percival, C. J.; Coe, H.; Biskos, G.

    2013-11-01

    The chemical composition and water uptake characteristics of sub-micrometre atmospheric particles over the region of the Aegean Sea were measured between 25 August and 11 September 2011 within the framework of the Aegean-Game campaign. High temporal-resolution measurements of the chemical composition of the particles were conducted using an airborne compact time-of-flight aerosol mass spectrometer (cToF-AMS). These measurements were performed during two flights from the island of Crete to the island of Lemnos and back. A hygroscopic tandem differential mobility analyser (HTDMA) located on the island of Lemnos was used to measure the ability of the particles to take up water. The HTDMA measurements showed that the particles in the dominant mode were internally mixed, having hygroscopic growth factors that ranged from 1.00 to 1.59 when exposed to 85% relative humidity. When the aircraft flew near the ground station on Lemnos, the cToF-AMS measurements showed that the organic volume fraction of the particles ranged from 43 to 56%. These measurements corroborate the range of hygroscopic growth factors measured by the HTDMA during that time. Good closure between HTDMA and cToF-AMS measurements was achieved when assuming that the organic species were less hygroscopic and had an average density that corresponds to aged organic species. Using the results from the closure study, the cToF-AMS measurements were employed to determine vertical profiles of a representative aerosol hygroscopic parameter κmix. Calculated κmix values ranged from 0.19 to 0.84 during the first flight and from 0.22 to 0.80 during the second flight. Air masses of different origin as determined by back trajectory calculations can explain the spatial variation in chemical composition and κmix values of the particles observed in the region.

  10. Water uptake and chemical composition of fresh aerosols generated in open burning of biomass

    Directory of Open Access Journals (Sweden)

    C. M. Carrico

    2010-06-01

    Full Text Available As part of the Fire Lab at Missoula Experiments (FLAME in 2006–2007, we examined hygroscopic properties of particles emitted from open combustion of 33 select biomass fuels. Measurements of humidification growth factors for subsaturated water relative humidity (RH conditions were made with a hygroscopic tandem differential mobility analyzer (HTDMA for dry particle sizes of 50, 100 and 250 nm. Results were then fit to a single-parameter model to obtain the hygroscopicity parameter, κ. Particles in freshly emitted biomass smoke exhibited a wide range of hygroscopicity (individual modes with 0<κ<1.0, spanning a range from the hygroscopicity of fresh diesel soot emissions to that of pure inorganic salts commonly found in the ambient aerosol. Smoke aerosols dominated by carbonaceous species typically had a unimodal growth factor with corresponding mean κ=0.1 (range of 0<κ<0.4. Those with a substantial inorganic mass fraction typically separated into less- and more-hygroscopic modes at high RH, the latter with mean κ=0.4 (range of 0.1<κ<1. The bimodal κ distributions were indicative of smoke chemical heterogeneity at a single particle size, whereas heterogeneity as a function of size was indicated by typically decreasing κ values with increasing dry particle diameters. Hygroscopicity varied strongly with biomass fuel type and, to a lesser extent, with combustion conditions. Among the most hygroscopic smokes were those from palmetto, rice straw, and sawgrass, while smoke particles from coniferous species such as spruces, firs, pines, and duffs were among the least hygroscopic. Overall, hygroscopicity decreased with increasing ratios of total carbon to inorganic ions as measured in PM2.5 filter samples. Despite aerosol heterogeneity, reconstructions of κ using PM2.5 bulk chemical composition data fell along a 1:1 line with measured ensemble κ values.

  11. Size distribution and chemical composition of secondary organic aerosol formed from C1-initiated oxidation of toluene.

    Science.gov (United States)

    Huang, Mingqiang; Zhang, Weijun; Gu, Xuejun; Hu, Changjin; Zhao, Weixiong; Wang, Zhenya; Fang, Li

    2012-01-01

    Secondary organic aerosol (SOA) formed from C1-initiated oxidation of toluene was investigated in a home-made smog chamber. The size distribution and chemical composition of SOA particles were measured using aerodynamic particle sizer spectrometer and the aerosol laser time-of-flight mass spectrometer (ALTOFMS), respectively. According to a large number of single aerosol diameter and mass spectra, the size distribution and chemical composition of SOA were obtained statistically. Experimental results showed that SOA particles created by C1-initiated oxidation of toluene is predominantly in the form of fine particles, which have diameters less than 2.5 microm (i.e., PM2.5), and glyoxal, benzaldehyde, benzyl alcohol, benzoquinone, benzoic acid, benzyl hydroperoxide and benzyl methyl nitrate are the major products components in the SOA. The possible reaction mechanisms leading to these products are also proposed.

  12. Size and composition measurements of background aerosol and new particle growth in a Finnish forest during QUEST 2 using an Aerodyne Aerosol Mass Spectrometer

    Directory of Open Access Journals (Sweden)

    J. D. Allan

    2006-01-01

    Full Text Available The study of the growth of nucleation-mode particles is important, as this prevents their loss through diffusion and allows them to reach sizes where they may become effective cloud condensation nuclei. Hyytiälä, a forested site in southern Finland, frequently experiences particle nucleation events during the spring and autumn, where particles first appear during the morning and continue to grow for several hours afterwards. As part of the QUEST 2 intensive field campaign during March and April 2003, an Aerodyne Aerosol Mass Spectrometer (AMS was deployed alongside other aerosol instrumentation to study the particulate composition and dynamics of growth events and characterise the background aerosol. Despite the small mass concentrations, the AMS was able to distinguish the grown particles in the <100 nm regime several hours after an event and confirm that the particles were principally organic in composition. The AMS was also able to derive a mass spectral fingerprint for the organic species present, and found that it was consistent between events and independent of the mean particle diameter during non-polluted cases, implying the same species were also condensing onto the accumulation mode. The results were compared with those from offline analyses such as GC-MS and were consistent with the hypothesis that the main components were alkanes from plant waxes and the oxidation products of terpenes.

  13. Overview and preliminary results of the Surface Ocean Aerosol Production (SOAP campaign

    Directory of Open Access Journals (Sweden)

    C. S. Law

    2017-11-01

    , contaminant markers and a common aerosol inlet facilitated multi-sensor measurement of uncontaminated air. Aerosol characterization identified variable Aitken mode and consistent submicron-sized accumulation and coarse modes. Submicron aerosol mass was dominated by secondary particles containing ammonium sulfate/bisulfate under light winds, with an increase in sea salt under higher wind speeds. MBL measurements and chamber experiments identified a significant organic component in primary and secondary aerosols. Comparison of SOAP aerosol number and size distributions reveals an underprediction in GLOMAP (GLObal Model of Aerosol Processes-mode aerosol number in clean marine air masses, suggesting a missing marine aerosol source in the model. The SOAP data will be further examined for evidence of nucleation events and also to identify relationships between MBL composition and surface ocean biogeochemistry that may provide potential proxies for aerosol precursors and production.

  14. Measurements of Hygroscopicity- and Size-Resolved Sea Spray Aerosol

    Science.gov (United States)

    Phillips, B.; Dawson, K. W.; Royalty, T. M.; Reed, R. E.; Petters, M.; Meskhidze, N.

    2015-12-01

    Atmospheric aerosols play a central role in many environmental processes by influencing the Earth's radiative balance, tropospheric chemistry, clouds, biogeochemical cycles, and visibility as well as adversely impacting human health. Based on their origin, atmospheric aerosols can be defined as anthropogenic or natural. Recent studies have shown that a large fraction of uncertainty in the radiative effects of anthropogenic aerosols is related to uncertainty in natural—background—aerosols. Marine aerosols are of particular interest due to the abundance of oceans covering the Earth's surface. Despite their importance, limited information is currently available for size- and composition-resolved marine aerosol emission fluxes. Our group has designed and built an instrument for measuring the size- and hygroscopicity-resolved sea spray aerosol fluxes. The instrument was first deployed during spring 2015 at the end of the 560 m pier of the US Army Corps of Engineers' Field Research Facility in Duck, NC. Measurements include 200 nm-sized diameter growth factor (hygroscopicity) distributions, sea spray particle flux measurements, and total sub-micron sized aerosol concentration. Ancillary ocean data includes salinity, pH, sea surface temperature, dissolved oxygen content, and relative fluorescence (proxy for [Chl-a]). Hygroscopicity distribution measurements show two broad peaks, one indicative of organics and sulfates and another suggestive of sea salt. The fraction of 200 nm-sized salt particles having hygroscopicity similar to that of sea-spray aerosol contributes up to ~24% of the distribution on days with high-speed onshore winds and up to ~3% on calm days with winds blowing from the continent. However, the total concentration of sea-spray-like particles originating from offshore versus onshore winds was relatively similar. Changes in the relative contribution of sea-salt to number concentration were caused by a concomitant changes in total aerosol concentration

  15. Continuous measurement of elemental composition of ambient aerosol by induction-coupled plasma mass spectrometry.

    Science.gov (United States)

    Mishra, Santosh K; Chattopadhyay, Bhargab; Kadjo, Akinde F; Dasgupta, Purnendu K

    2018-01-15

    There is presently no instrumentation that can provide (near) real time information on elemental composition of atmospheric aerosols. We describe an arrangement where air is sampled through a cyclone @30L/min with a 50% cutoff @ ~250nm. The particles deposit into a cup through which deionized water is continuously flowing. High purity HNO3 is added downstream and the mixed stream optionally flows through a quartz photo reactor (185nm, ~90°C, tR ~1.2min) and is aspirated by an induction coupled plasma mass spectrometer (ICP-MS). Comparative batch experiments in which samples were not photodigested at all or thermally digested off-line for an extended period indicated no statistically significant difference in the results. This observation agrees with early theoretical and experimental work. Some 22 elements were quantifiable (S/N > 10) at all times in the aerosol samples collected in our highly urban sampling location; an additional 4 elements were quantifiable at times of construction activity in the general area. Presently attained system limits of detection (LODs) are orders of magnitude higher than the instrumental LOD, both because of the purity of the acid and pump-induced contamination. These aspects can be vastly improved and will need to be improved to determine background concentrations. Copyright © 2017 Elsevier B.V. All rights reserved.

  16. submitter On the composition of ammonia–sulfuric-acid ion clusters during aerosol particle formation

    CERN Document Server

    Schobesberger, S; Bianchi, F; Rondo, L; Duplissy, J; Kürten, A; Ortega, I K; Metzger, A; Schnitzhofer, R; Almeida, J; Amorim, A; Dommen, J; Dunne, E M; Ehn, M; Gagné, S; Ickes, L; Junninen, H; Hansel, A; Kerminen, V -M; Kirkby, J; Kupc, A; Laaksonen, A; Lehtipalo, K; Mathot, S; Onnela, A; Petäjä, T; Riccobono, F; Santos, F D; Sipilä, M; Tomé, A; Tsagkogeorgas, G; Viisanen, Y; Wagner, P E; Wimmer, D; Curtius, J; Donahue, N M; Baltensperger, U; Kulmala, M; Worsnop, D R

    2015-01-01

    The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new-particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia $(NH_3)$ and sulfuric acid $(H-2SO_4)$. Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small $NH_3–H_2SO_4$ clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH3] in the range from 10. Positively charged clusters grew on average by Δm/Δn = 1.05 and were only observed at sufficiently high $[NH_3]$ / $[H_2SO_4]$. The $H_2SO_4$ molecules of these clusters are partially neutralized by $NH_3$, in close resemblance...

  17. On the composition of ammonia-sulfuric acid clusters during aerosol particle formation

    CERN Document Server

    Schobesberger, S; Bianchi, F; Rondo, L; Duplissy, J; Kürten, A; Ortega, I K; Metzger, A; Schnitzhofer, R; Almeida, J; Amorim, A; Dommen, J; Dunne, E M; Ehn, M; Gagné, S; Ickes, L; Junninen, H; Hansel, A; Kerminen, V-M; Kirkby, J; Kupc, A; Laaksonen, A; Lehtipalo, K; Mathot, S; Onnela, A; Petäjä, T; Riccobono, F; Santos, F D; Sipilä, M; Tomé, A; Tsagkogeorgas, G; Viisanen, Y; Wagner, P E; Wimmer, D; Curtius, J; Donahue, N M; Baltensperger, U; Kulmala, M; Worsnop, D R

    2014-01-01

    The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH3) and sulfuric acid (H2SO4). Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small NH3-H2SO4 clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH3] in the range from 10. Positively charged clusters grew on average by Δm / Δn = 1.05 and were only observed at sufficiently high [NH3] / [H2SO4]. The H2SO4 molecules of these clusters are partially neutralized by NH3, in close resemblance to the acid-base bindings ...

  18. Changes in the concentration and composition of anthropogenic and biogenic aerosols in the Finnish Arctic

    Science.gov (United States)

    Yli-Tuomi, Tarja

    In this study, historical samples of Arctic haze collected between 1964 and 1978 from northern Finland have been analyzed. The aim has been to determine the sources of the particles, as well as the temporal variation in the source contributions and the source regions. There is no other long-term data available from this early time period and overall, more information about the occurrence, nature, origin and transport of anthropogenic and biogenic aerosols in the European Arctic is needed in order to protect the vulnerable Arctic environment. In addition, evidence for climate/biosphere interaction observed in a previous study of the Arctic aerosol has been sought. The chemical composition data was analyzed with a Multilinear Engine using two different models, pure bilinear and a mixed 2-way/3-way model. The results of receptor modeling were connected with back trajectory data in a Potential Source Contribution Function analysis to determine the likely source areas. Nine sources, namely silver emissions, coal combustion, biomass burning, nonferrous smelters (two sources), crustal elements from remote sources, excess silicon from local sources, sea salt particles and biogenic sulfur emissions from marine algae were found. Although the emissions from industrial areas in the Kola Peninsula have an effect on the concentration of anthropogenic pollutants at Kevo, the highest concentrations during winter are transported from the sources in the mid-latitudes. The yearly strength of the biogenic sulfur emissions showed no dependence on the Northern Hemisphere temperature anomaly and thus, a climatic feedback loop can not be confirmed.

  19. Assessing the radiative forcing from sea-spray geoengineering using a composition-climate model with an aerosol microphysics scheme

    Science.gov (United States)

    Parkes, Ben; Mann, Graham; Carslaw, Ken; Pringle, Kirsty; Gadian, Alan; West, Rosalind; Stier, Philip; Johnson, Colin; Dalvi, Mohit

    2013-04-01

    Marine Cloud Brightening (MCB) is one of several suggested solar radiation management geoengineering schemes proposed to counteract changes in climate resulting from anthropogenically increased greenhouse gas concentrations. Such changes include precipitation changes, increasing global average temperatures and an associated reduction in sea ice cover. In contrast to most previous climate model studies of MCB which quantify the climate impacts of imposed changes to the cloud droplet number concentration. In this work we explicitly resolve the injection of a size-resolved source of sea salt aerosol into the boundary layer. We use the UK Chemistry and Aerosol (UKCA) composition-climate model which is an extension of the UK Met Office Hadley Centre Global Environmental Model (HadGEM) and includes the GLOMAP-mode aerosol microphysics scheme coupled to a mechanistic cloud droplet activation module. In this study, we quantify the aerosol direct and 1st indirect forcings from MCB without applying the aerosol radiative effects to the atmosphere model, ensuring identical meteorology in the control and perturbation experiments, consistent with the IPCC defined forcing. We carry out several sensitivity runs seeding several different regions of persistent marine stratocumulus clouds with soluble sea salt aerosol of varying radius.

  20. Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area

    Science.gov (United States)

    Xu, L.; Williams, L. R.; Young, D. E.; Allan, J. D.; Coe, H.; Massoli, P.; Fortner, E.; Chhabra, P.; Herndon, S.; Brooks, W. A.; Jayne, J. T.; Worsnop, D. R.; Aiken, A. C.; Liu, S.; Gorkowski, K.; Dubey, M. K.; Fleming, Z. L.; Visser, S.; Prévôt, A. S. H.; Ng, N. L.

    2016-02-01

    The composition of PM1 (particulate matter with diameter less than 1 µm) in the greater London area was characterized during the Clean Air for London (ClearfLo) project in winter 2012. Two high-resolution time-of-flight aerosol mass spectrometers (HR-ToF-AMS) were deployed at a rural site (Detling, Kent) and an urban site (North Kensington, London). The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM1. We find that the organic aerosol (OA) concentration is comparable between the rural and urban sites, but the contribution from different sources is distinctly different between the two sites. The concentration of solid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA) are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that the biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD) to investigate the volatility of PM1 species at the rural Detling site. After heating at 250 °C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC; measured by a soot-particle aerosol mass spectrometer) only accounts for organics have similar sources or have undergone similar chemical processing as rBC in the atmosphere. Although the atomic O : C ratio of OOA is substantially larger than that of solid fuel OA and

  1. Sources of atmospheric aerosol from long-term measurements (5 years) of chemical composition in Athens, Greece.

    Science.gov (United States)

    Paraskevopoulou, D; Liakakou, E; Gerasopoulos, E; Mihalopoulos, N

    2015-09-15

    To identify the sources of aerosols in Greater Athens Area (GAA), a total of 1510 daily samples of fine (PM 2.5) and coarse (PM 10-2,5) aerosols were collected at a suburban site (Penteli), during a five year period (May 2008-April 2013) corresponding to the period before and during the financial crisis. In addition, aerosol sampling was also conducted in parallel at an urban site (Thissio), during specific, short-term campaigns during all seasons. In all these samples mass and chemical composition measurements were performed, the latest only at the fine fraction. Particulate organic matter (POM) and ionic masses (IM) are the main contributors of aerosol mass, equally contributing by accounting for about 24% of the fine aerosol mass. In the IM, nss-SO4(-2) is the prevailing specie followed by NO3(-) and NH4(+) and shows a decreasing trend during the 2008-2013 period similar to that observed for PM masses. The contribution of water in fine aerosol is equally significant (21 ± 2%), while during dust transport, the contribution of dust increases from 7 ± 2% to 31 ± 9%. Source apportionment (PCA and PMF) and mass closure exercises identified the presence of six sources of fine aerosols: secondary photochemistry, primary combustion, soil, biomass burning, sea salt and traffic. Finally, from winter 2012 to winter 2013 the contribution of POM to the urban aerosol mass is increased by almost 30%, reflecting the impact of wood combustion (dominant fuel for domestic heating) to air quality in Athens, which massively started in winter 2013. Copyright © 2015 Elsevier B.V. All rights reserved.

  2. Physical properties of aerosols at Maitri, Antarctica

    Indian Academy of Sciences (India)

    Measurements of the submicron aerosol size distribution made at the Indian Antarctic station, Maitri (70° 45′S, 11° 44′E) from January 10th to February 24th, 1997, are reported. Total aerosol concentrations normally range from 800 to 1200 particles cm-3 which are typical values for the coastal stations at Antarctica in ...

  3. Chemical and isotopic composition of secondary organic aerosol generated by α-pinene ozonolysis

    Science.gov (United States)

    Meusinger, Carl; Dusek, Ulrike; King, Stephanie M.; Holzinger, Rupert; Rosenørn, Thomas; Sperlich, Peter; Julien, Maxime; Remaud, Gerald S.; Bilde, Merete; Röckmann, Thomas; Johnson, Matthew S.

    2017-05-01

    Secondary organic aerosol (SOA) plays a central role in air pollution and climate. However, the description of the sources and mechanisms leading to SOA is elusive despite decades of research. While stable isotope analysis is increasingly used to constrain sources of ambient aerosol, in many cases it is difficult to apply because neither the isotopic composition of aerosol precursors nor the fractionation of aerosol forming processes is well characterised. In this paper, SOA formation from ozonolysis of α-pinene - an important precursor and perhaps the best-known model system used in laboratory studies - was investigated using position-dependent and average determinations of 13C in α-pinene and advanced analysis of reaction products using thermal-desorption proton-transfer-reaction mass spectrometry (PTR-MS). The total carbon (TC) isotopic composition δ13C of the initial α-pinene was measured, and the δ13C of the specific carbon atom sites was determined using position-specific isotope analysis (PSIA). The PSIA analysis showed variations at individual positions from -6.9 to +10. 5 ‰ relative to the bulk composition. SOA was formed from α-pinene and ozone in a constant-flow chamber under dark, dry, and low-NOx conditions, with OH scavengers and in the absence of seed particles. The excess of ozone and long residence time in the flow chamber ensured that virtually all α-pinene had reacted. Product SOA was collected on two sequential quartz filters. The filters were analysed offline by heating them stepwise from 100 to 400 °C to desorb organic compounds that were (i) detected using PTR-MS for chemical analysis and to determine the O : C ratio, and (ii) converted to CO2 for 13C analysis. More than 400 ions in the mass range 39-800 Da were detected from the desorbed material and quantified using a PTR-MS. The largest amount desorbed at 150 °C. The O : C ratio of material from the front filter increased from 0.18 to 0.25 as the desorption temperature was

  4. A sea spray aerosol flux parameterization encapsulating wave state

    NARCIS (Netherlands)

    Ovadnevaite, J.; Manders, A.; De Leeuw, G.; Ceburnis, D.; Monahan, C.; Partanen, A.I.; Korhonen, H.; O'Dowd, C.D.

    2014-01-01

    A new sea spray source function (SSSF), termed Oceanflux Sea Spray Aerosol or OSSA, was derived based on in-situ sea spray aerosol measurements along with meteorological/physical parameters. Submicron sea spray aerosol fluxes derived from particle number concentration measurements at the Mace Head

  5. Organic aerosol composition and sources in Pasadena, California, during the 2010 CalNex campaign

    Science.gov (United States)

    Hayes, P. L.; Ortega, A. M.; Cubison, M. J.; Froyd, K. D.; Zhao, Y.; Cliff, S. S.; Hu, W. W.; Toohey, D. W.; Flynn, J. H.; Lefer, B. L.; Grossberg, N.; Alvarez, S.; Rappenglück, B.; Taylor, J. W.; Allan, J. D.; Holloway, J. S.; Gilman, J. B.; Kuster, W. C.; de Gouw, J. A.; Massoli, P.; Zhang, X.; Liu, J.; Weber, R. J.; Corrigan, A. L.; Russell, L. M.; Isaacman, G.; Worton, D. R.; Kreisberg, N. M.; Goldstein, A. H.; Thalman, R.; Waxman, E. M.; Volkamer, R.; Lin, Y. H.; Surratt, J. D.; Kleindienst, T. E.; Offenberg, J. H.; Dusanter, S.; Griffith, S.; Stevens, P. S.; Brioude, J.; Angevine, W. M.; Jimenez, J. L.

    2013-08-01

    Organic aerosols (OA) in Pasadena are characterized using multiple measurements from the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign. Five OA components are identified using positive matrix factorization including hydrocarbon-like OA (HOA) and two types of oxygenated OA (OOA). The Pasadena OA elemental composition when plotted as H : C versus O : C follows a line less steep than that observed for Riverside, CA. The OOA components from both locations follow a common line, however, indicating similar secondary organic aerosol (SOA) oxidation chemistry at the two sites such as fragmentation reactions leading to acid formation. In addition to the similar evolution of elemental composition, the dependence of SOA concentration on photochemical age displays quantitatively the same trends across several North American urban sites. First, the OA/ΔCO values for Pasadena increase with photochemical age exhibiting a slope identical to or slightly higher than those for Mexico City and the northeastern United States. Second, the ratios of OOA to odd-oxygen (a photochemical oxidation marker) for Pasadena, Mexico City, and Riverside are similar, suggesting a proportional relationship between SOA and odd-oxygen formation rates. Weekly cycles of the OA components are examined as well. HOA exhibits lower concentrations on Sundays versus weekdays, and the decrease in HOA matches that predicted for primary vehicle emissions using fuel sales data, traffic counts, and vehicle emission ratios. OOA does not display a weekly cycle—after accounting for differences in photochemical aging —which suggests the dominance of gasoline emissions in SOA formation under the assumption that most urban SOA precursors are from motor vehicles.

  6. Fuel composition and secondary organic aerosol formation: gas-turbine exhaust and alternative aviation fuels.

    Science.gov (United States)

    Miracolo, Marissa A; Drozd, Greg T; Jathar, Shantanu H; Presto, Albert A; Lipsky, Eric M; Corporan, Edwin; Robinson, Allen L

    2012-08-07

    A series of smog chamber experiments were performed to investigate the effects of fuel composition on secondary particulate matter (PM) formation from dilute exhaust from a T63 gas-turbine engine. Tests were performed at idle and cruise loads with the engine fueled on conventional military jet fuel (JP-8), Fischer-Tropsch synthetic jet fuel (FT), and a 50/50 blend of the two fuels. Emissions were sampled into a portable smog chamber and exposed to sunlight or artificial UV light to initiate photo-oxidation. Similar to previous studies, neat FT fuel and a 50/50 FT/JP-8 blend reduced the primary particulate matter emissions compared to neat JP-8. After only one hour of photo-oxidation at typical atmospheric OH levels, the secondary PM production in dilute exhaust exceeded primary PM emissions, except when operating the engine at high load on FT fuel. Therefore, accounting for secondary PM production should be considered when assessing the contribution of gas-turbine engine emissions to ambient PM levels. FT fuel substantially reduced secondary PM formation in dilute exhaust compared to neat JP-8 at both idle and cruise loads. At idle load, the secondary PM formation was reduced by a factor of 20 with the use of neat FT fuel, and a factor of 2 with the use of the blend fuel. At cruise load, the use of FT fuel resulted in no measured formation of secondary PM. In every experiment, the secondary PM was dominated by organics with minor contributions from sulfate when the engine was operated on JP-8 fuel. At both loads, FT fuel produces less secondary organic aerosol than JP-8 because of differences in the composition of the fuels and the resultant emissions. This work indicates that fuel reformulation may be a viable strategy to reduce the contribution of emissions from combustion systems to secondary organic aerosol production and ultimately ambient PM levels.

  7. How much information do extinction and backscattering measurements contain about the chemical composition of atmospheric aerosol?

    Science.gov (United States)

    Kahnert, Michael; Andersson, Emma

    2017-03-01

    We theoretically and numerically investigate the problem of assimilating multiwavelength lidar observations of extinction and backscattering coefficients of aerosols into a chemical transport model. More specifically, we consider the inverse problem of determining the chemical composition of aerosols from these observations. The main questions are how much information the observations contain to determine the particles' chemical composition, and how one can optimize a chemical data assimilation system to make maximum use of the available information. We first quantify the information content of the measurements by computing the singular values of the scaled observation operator. From the singular values we can compute the number of signal degrees of freedom, Ns, and the reduction in Shannon entropy, H. As expected, the information content as expressed by either Ns or H grows as one increases the number of observational parameters and/or wavelengths. However, the information content is strongly sensitive to the observation error. The larger the observation error variance, the lower the growth rate of Ns or H with increasing number of observations. The right singular vectors of the scaled observation operator can be employed to transform the model variables into a new basis in which the components of the state vector can be partitioned into signal-related and noise-related components. We incorporate these results in a chemical data assimilation algorithm by introducing weak constraints that restrict the assimilation algorithm to acting on the signal-related model variables only. This ensures that the information contained in the measurements is fully exploited, but not overused. Numerical tests show that the constrained data assimilation algorithm provides a solution to the inverse problem that is considerably less noisy than the corresponding unconstrained algorithm. This suggests that the restriction of the algorithm to the signal-related model variables suppresses

  8. Estimation of aerosol water and chemical composition from AERONET Sun-sky radiometer measurements at Cabauw, the Netherlands

    NARCIS (Netherlands)

    Van Beelen, A. J.; Roelofs, G. J H; Hasekamp, O. P.; Henzing, J. S.; Röckmann, T.

    2014-01-01

    Remote sensing of aerosols provides important information on atmospheric aerosol abundance. However, due to the hygroscopic nature of aerosol particles observed aerosol optical properties are influenced by atmospheric humidity, and the measurements do not unambiguously characterize the aerosol dry

  9. Observational evidence for the formation of DMS-derived aerosols during Arctic phytoplankton blooms

    Science.gov (United States)

    Park, Ki-Tae; Jang, Sehyun; Lee, Kitack; Yoon, Young Jun; Kim, Min-Seob; Park, Kihong; Cho, Hee-Joo; Kang, Jung-Ho; Udisti, Roberto; Lee, Bang-Yong; Shin, Kyung-Hoon

    2017-08-01

    The connection between marine biogenic dimethyl sulfide (DMS) and the formation of aerosol particles in the Arctic atmosphere was evaluated by analyzing atmospheric DMS mixing ratio, aerosol particle size distribution and aerosol chemical composition data that were concurrently collected at Ny-Ålesund, Svalbard (78.5° N, 11.8° E), during April and May 2015. Measurements of aerosol sulfur (S) compounds showed distinct patterns during periods of Arctic haze (April) and phytoplankton blooms (May). Specifically, during the phytoplankton bloom period the contribution of DMS-derived SO42- to the total aerosol SO42- increased by 7-fold compared with that during the proceeding Arctic haze period, and accounted for up to 70 % of fine SO42- particles (< 2.5 µm in diameter). The results also showed that the formation of submicron SO42- aerosols was significantly associated with an increase in the atmospheric DMS mixing ratio. More importantly, two independent estimates of the formation of DMS-derived SO42- aerosols, calculated using the stable S-isotope ratio and the non-sea-salt SO42- / methanesulfonic acid ratio, respectively, were in close agreement, providing compelling evidence that the contribution of biogenic DMS to the formation of aerosol particles was substantial during the Arctic phytoplankton bloom period.

  10. Towards retrievals of aerosol chemical composition from satellite observations by POLDER/PARASOL polarimeter

    Science.gov (United States)

    Li, L.; Dubovik, O.; Derimian, Y.; Lapyonok, T.; Schuster, G. L.; Ducos, F.

    2016-12-01

    The information about composition of aerosols has a great importance for monitoring and understanding of climate and environment dynamics. Such information can be obtained using situ measurements or chemical transport models. However, in situ sampling has limited spatial and temporal coverage, while estimations have large uncertainties. The present work enables the monitoring of aerosol chemical species from space-borne observations, providing observationally-based results with spatial and temporal coverage. Following the ideas of Schuster et al.(2005, 2009, 2016), we retrieve chemical composition directly from remote sensing measurements without intermediate retrieval of the refractive index (in contrast with Schuster's approach). This approach is expected to reduce the influence of modeling uncertainties, and to provide additional constraints in situations where remote sensing observations do not have enough spectral sensitivity to refractive index. One of principal difficulties is the identification of an adequate model for linking refractive index to chemical composition. Therefore, the initial effort of this work has focused on identifying an optimal "chemical composition to refractive index" conversion model. With that purpose, we first tested the retrieval approach using a simplified volume-weighting model and updated by the Maxwell Garnett mixing model. This concept was incorporated into the GRASP algorithm designed to retrieve an extended set of atmospheric parameters from remote sensing observations. Then a series of sensitivity tests using synthetic data of POLDER/PARASOL were conducted, and followed by inversion of real PARASOL observations. The sensitivity tests showed that these two models allow the retrieval to distinguish amongst the assumed chemical species. Results obtained from real PARASOL data demonstrated good agreement with the optical characteristics provided by AERONET (e.g., r2 of AOT 0.9). The obtained patterns of chemical component

  11. Evaluation of anthropogenic influence on thermodynamics, gas and aerosol composition of city air

    Science.gov (United States)

    Uzhegova, Nina; Belan, Boris; Antokhin, Pavel; Zhidovkhin, Evgenii; Ivlev, Georgii; Kozlov, Artem; Fofonov, Aleksandr

    2010-05-01

    In the last 40-50 years there is a global tendency of urbanisation, which is a consequence of most countries' economical development. Concurrently, the issue of environment's ecological state has become critical. Urban air pollution is among the most important ecological problems nowadays. World Health Organization (WHO) points out certain "classical" polluting agents: carbon monoxide (CO), nitric oxide (NO), nitrogen dioxide (NO2), sulphur dioxide (SO2), troposphere ozone (O3) (studied here), as well as lead, carbon dioxide (CO2), aldehydes, soot, benzpyrene and dredges (including dust, haze and smoke) [1]. An evaluation of antropogenic component's weight in the thermodynamical conditions and gas and aerosol composition of a city's atmosphere (by the example of Tomsk) is given in this paper. Tomsk is located at the South of West Siberia and is the administrative center of Tomsk region. The city's area is equal to 294,6 km2. Its population is 512.6 thousands of people. The overall number of registered motor vehicles in the city in 2008 was 131 700. That is, every fourth city inhabitant has a personal car. From 2002 to 2008 the number of motor vehicles in Tomsk has increased by 25 thousands units [2]. This increase consists mostly of passenger cars. There is also a positive trend in fuel consumtion by the city's industries and motor vehicles - from 2004 to 2007 it has increased by 10%. Such a quick rate of transport quantity's increase in the city provides reason to suggest an unfavorable ecological situation in Tomsk. For this study we have used the AKV-2 mobile station designed by the SB RAS Institute of Atmospheric Optics. The station's equipment provides the following measurements [3]: air temperature and humidity; aerosol disperse composition in 15 channels with a particle size range of 0.3-20 µm by use of the Grimm-1.108 aerosol spectrometer; NO, NO2, O3, SO2, CO, CO2 concentration. This paper describes a single experiment conducted in Tomsk. Date of

  12. Laboratory studies of the chemical composition and cloud condensation nuclei (CCN activity of secondary organic aerosol (SOA and oxidized primary organic aerosol (OPOA

    Directory of Open Access Journals (Sweden)

    A. T. Lambe

    2011-09-01

    Full Text Available Secondary organic aerosol (SOA and oxidized primary organic aerosol (OPOA were produced in laboratory experiments from the oxidation of fourteen precursors representing atmospherically relevant biogenic and anthropogenic sources. The SOA and OPOA particles were generated via controlled exposure of precursors to OH radicals and/or O3 in a Potential Aerosol Mass (PAM flow reactor over timescales equivalent to 1–20 days of atmospheric aging. Aerosol mass spectra of SOA and OPOA were measured with an Aerodyne aerosol mass spectrometer (AMS. The fraction of AMS signal at m/z = 43 and m/z = 44 (f43, f44, the hydrogen-to-carbon (H/C ratio, and the oxygen-to-carbon (O/C ratio of the SOA and OPOA were obtained, which are commonly used to characterize the level of oxidation of oxygenated organic aerosol (OOA. The results show that PAM-generated SOA and OPOA can reproduce and extend the observed f44f43 composition beyond that of ambient OOA as measured by an AMS. Van Krevelen diagrams showing H/C ratio as a function of O/C ratio suggest an oxidation mechanism involving formation of carboxylic acids concurrent with fragmentation of carbon-carbon bonds. Cloud condensation nuclei (CCN activity of PAM-generated SOA and OPOA was measured as a function of OH exposure and characterized as a function of O/C ratio. CCN activity of the SOA and OPOA, which was characterized in the form of the hygroscopicity parameter κorg, ranged from 8.4×10−4 to 0.28 over measured O/C ratios ranging from 0.05 to 1.42. This range of κorg and O/C ratio is significantly wider than has been previously obtained. To first order, the κorg-to-O/C relationship is well represented by a linear function of the form κorg = (0.18±0.04 ×O/C + 0.03, suggesting that a simple, semi-empirical parameterization of OOA hygroscopicity and

  13. Can 'extrafine' dry powder aerosols improve lung deposition?

    NARCIS (Netherlands)

    De Boer, Anne H.; Gjaltema, Doetie; Hagedoorn, Paul; Frijlink, Henderik W.

    2015-01-01

    There is increasing interest in the use of so-called 'extrafine' aerosols to target the small airways in the management of asthma and COPD. Using previously presented deposition data, we assessed whether submicron (

  14. Temporal variability in aerosol composition at an urban site, Varanasi in the eastern Indo-Gangetic Plain

    Science.gov (United States)

    Ram, Kirpa; Norra, Stefan; Yuan, Chen; Venkata Satish, Rangu; Rastogi, Neeraj

    2017-04-01

    PM2.5 aerosol samples (n=31) were collected from an urban site, Varanasi (25° 28'N, 83°0' E) in the eastern Indo-Gangetic Plain during May 2015 to March 2016 using a mini-volume sampler (Leckel GmbH, Germany) at a flow rate of 200 l/hr. The PM2.5 samples were integrated for 7 days and were analyzed for organic and elemental carbon (OC & EC), water-soluble OC (WSOC), organic and inorganic nitrogen (ON & IN) and water-soluble inorganic species (WSIS) to study the geochemical behavior of aerosols. The mass concentration of OC and EC varies from 4.2 to 105.2 (average: 32.8) μg m-3 and 1.2 to 7.0 (average: 4.6) μg m-3 during the study period with total carbonaceous aerosols (TCA=1.6*OC+EC), on an average, accounting for ˜59% of PM2.5 mass. Relatively high WSOC/OC ratio (average: 0.55±0.18; range 0.18-0.86) indicate a significant contribution from the secondary organic aerosols at Varanasi. The concentration of ON varies from less than detection limit to 5.3 (average: 2.4) μg m-3 which contribute to ˜12% of WSOC highlighting the presence of nitro-organic compounds in aerosols at Varanasi. The average WSIS contribution to PM2.5 is only 17% with a strong seasonal variability (range: 4-36%). Generally, carbonaceous and inorganic aerosol concentration is higher during winter, fall and post-monsoon that those in the summer when dust aerosol contribution is significant (as high as 75% of PM2.5 mass). This study highlights the role of nitro-organic compounds in secondary organic aerosols which is lacking in Indian aerosols. Furthermore, these aerosol samples could be very important for the study of particle morphology and composition using scanning-electron Microscope-Energy Dispersive X-ray due to lower impaction in the mini-volume sampler.

  15. Elemental composition of Arctic soils and aerosols in Ny-Ålesund measured using laser-induced breakdown spectroscopy

    Science.gov (United States)

    Kim, Gibaek; Yoon, Young-Jun; Kim, Hyun-A.; Cho, Hee-joo; Park, Kihong

    2017-08-01

    Two laser-induced breakdown spectroscopy (LIBS) systems (soil LIBS and aerosol LIBS) were used to determine the elemental composition of soils and ambient aerosols less than 2.5 μm in Ny-Ålesund, Svalbard (the world's most northerly human settlement). For soil LIBS measurements, matrix effects such as moisture content, soil grain size, and surrounding gas on the LIBS response were minimized. When Ar gas was supplied onto the soil sample surfaces, a significant enhancement in LIBS emission lines was observed. Arctic soil samples were collected at 10 locations, and various elements (Al, Ba, C, Ca, Cu, Fe, H, K, Mg, Mn, N, Na, O, Pb, and Si) were detected in soils. The elemental distribution in arctic soils was clearly distinguishable from those in urban and abandoned mining soils in Korea. Moreover, the concentrations of most of anthropogenic metals were fairly low, and localized sources in extremely close proximity affected the elevated level of Cu in the soil samples derived from Ny-Ålesund. The number of elements detected in aerosols (C, Ca, H, K, Mg, Na, and O) was lower than those determined in soils. The elements in aerosols can mainly originate from minerals and sea salts. The elemental distribution in aerosols was also clearly distinguishable from that in soils, suggesting that the resuspension of local soil particles by wind erosion into aerosols was minimal. The daily variation of particle number concentration (RSD = 71%) and the elements in aerosols (RSD = 25%) varied substantially, possibly due to fluctuating air masses and meteorological conditions.

  16. Predicting the Mineral Composition of Dust Aerosols. Part 2; Model Evaluation and Identification of Key Processes with Observations

    Science.gov (United States)

    Perlwitz, J. P.; Garcia-Pando, C. Perez; Miller, R. L.

    2015-01-01

    A global compilation of nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT) that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF) method assumes that the aerosol mineral fractions match the fractions of the soil. The MMT is based upon soil measurements after wet sieving, a process that destroys aggregates of soil particles that would have been emitted from the original, undisturbed soil. The second method approximately reconstructs the emitted aggregates. This model is referred to as the Aerosol Mineral Fraction (AMF) method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observations. Only the AMF method exhibits phyllosilicate mass at silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in better agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at distinct clay and silt particle sizes are shown to be more useful for evaluation of the models, in contrast to the sum over all particles sizes that is susceptible to compensating errors, as illustrated by the SMF experiment. Model errors suggest that allocation of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining source of uncertainty. Evaluation of both models and the MMT is hindered by the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. The importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.

  17. Predicting the mineral composition of dust aerosols – Part 2: Model evaluation and identification of key processes with observations

    Directory of Open Access Journals (Sweden)

    J. P. Perlwitz

    2015-10-01

    Full Text Available A global compilation of nearly sixty measurement studies is used to evaluate two methods of simulating the mineral composition of dust aerosols in an Earth system model. Both methods are based upon a Mean Mineralogical Table (MMT that relates the soil mineral fractions to a global atlas of arid soil type. The Soil Mineral Fraction (SMF method assumes that the aerosol mineral fractions match the fractions of the soil. The MMT is based upon soil measurements after wet sieving, a process that destroys aggregates of soil particles that would have been emitted from the original, undisturbed soil. The second method approximately reconstructs the emitted aggregates. This model is referred to as the Aerosol Mineral Fraction (AMF method because the mineral fractions of the aerosols differ from those of the wet-sieved parent soil, partly due to reaggregation. The AMF method remedies some of the deficiencies of the SMF method in comparison to observations. Only the AMF method exhibits phyllosilicate mass at silt sizes, where they are abundant according to observations. In addition, the AMF quartz fraction of silt particles is in better agreement with measured values, in contrast to the overestimated SMF fraction. Measurements at distinct clay and silt particle sizes are shown to be more useful for evaluation of the models, in contrast to the sum over all particles sizes that is susceptible to compensating errors, as illustrated by the SMF experiment. Model errors suggest that allocation of the emitted silt fraction of each mineral into the corresponding transported size categories is an important remaining source of uncertainty. Evaluation of both models and the MMT is hindered by the limited number of size-resolved measurements of mineral content that sparsely sample aerosols from the major dust sources. The importance of climate processes dependent upon aerosol mineral composition shows the need for global and routine mineral measurements.

  18. Chemical Composition, Seasonal Variation and Size distribution of Atmospheric Aerosols at an Alpine Site in Guanzhong Plain, China

    Science.gov (United States)

    Li, J.

    2015-12-01

    PM10 and size-segregated aerosol samples were collected at Mt. Hua (2065 a.s.m) in central China, and determined for carbonaceous fraction, ions and organic composition. The concentration of most chemical compositions in summer are lower than those in winter, due to decreased emissions of biomass and coal burning for house heating. High temperature and relative humidity (RH) conditions are favorable for secondary aerosol formation, resulting in higher concentrations of SO42- and NH4+ in summer. Non-dehydrated sugars are increased in summer because of the enhanced metabolism. Carbon preference index results indicate that n-alkanes at Mt. Hua are derived mostly by plant wax. Low Benzo(a)pyrene/Benzo(a)pyrene ratios indicate that mountain aerosols are more aged. Concentrations of biogenic (BSOA, the isoprene/pinene/caryophyllene oxidation products) and anthropogenic (ASOA, mainly aromatic acids) SOA positively correlated with temperature . However, a decreasing trend of BSOA concentration with an increase in RH was observed during the sampling period, although a clear trend between ASOA and RH was not found. Based on the AIM Model calculation, we found that during the sampling period an increase in RH resulted in a decrease in the aerosol acidity and thus reduced the effect of acid-catalysis on BSOA formation. Size distributions of K+ and NH4+ present as an accumulation mode, in contrast to Ca2+ and Mg2+, which are mainly existed in coarse particles. SO42- and NO3- show a bimodal pattern. Dehydrated sugars, fossil fuel derived n-alkanes and PAHs presented unimode size distribution, whereas non-dehydrated sugars and plant wax derived n-alkanes showed bimodal pattern. Most of the determined BSOA are formed in the aerosol phase and enriched in the fine mode except for cis-pinonic acid, which is formed in the gas phase and subsequently partitioned into aerosol phase and thus presents a bimodal pattern with a major peak in the coarse mode.

  19. Seasonality of the mass concentration and chemical composition of aerosols around an urbanized basin in East Asia

    Science.gov (United States)

    Chou, C. C.-K.; Hsu, W.-C.; Chang, S.-Y.; Chen, W.-N.; Chen, M.-J.; Huang, W.-R.; Huang, S.-H.; Tsai, C.-Y.; Chang, S.-C.; Lee, C.-T.; Liu, S.-C.

    2017-02-01

    This study investigated seasonal variations in the mass concentration and chemical composition of ambient aerosols observed at three stations (coastal, mountainous, and downtown sites) in northern Taiwan from March 2009 to February 2012. The results show that the major aerosol components include ammonium, sulfate, nitrate, sea salt, dust, organic carbon, and elemental carbon, whereas the mass fraction of each species depends on the sampling location and season. A significant correlation (r = 0.7-0.8) was observed in aerosol concentrations measured at the respective stations, indicating that aerosol concentrations were dominated by regional-scale factors. Ammonium, sulfate, and nitrate consistently reached respective peak values in the spring in conjunction with dust particle levels. This shows that the transport of dust and particulate air pollutants from the Asian continent has affected the atmospheric environment in this area. Distinct seasonality was observed for sea salt and secondary organic carbon (SOC): sea salt levels peaked in the autumn, whereas SOC levels peaked in the summer, implying that their sources were regulated by independent seasonal factors. Correlation between sea salt concentration and surface wind speed was derived from coastal measurements and showed a high value for the wind speed sensitivity parameter of around 0.37 for our location. In addition, it was revealed that the SOC concentration in aerosols was positively correlated with oxidant photolysis index (Ox × UVB), suggesting that the SOC seasonality was dominated by hydroxyl radical production.

  20. Chemical Composition of Aerosol from an E-Cigarette: A Quantitative Comparison with Cigarette Smoke.

    Science.gov (United States)

    Margham, Jennifer; McAdam, Kevin; Forster, Mark; Liu, Chuan; Wright, Christopher; Mariner, Derek; Proctor, Christopher

    2016-10-17

    There is interest in the relative toxicities of emissions from electronic cigarettes and tobacco cigarettes. Lists of cigarette smoke priority toxicants have been developed to focus regulatory initiatives. However, a comprehensive assessment of e-cigarette chemical emissions including all tobacco smoke Harmful and Potentially Harmful Constituents, and additional toxic species reportedly present in e-cigarette emissions, is lacking. We examined 150 chemical emissions from an e-cigarette (Vype ePen), a reference tobacco cigarette (Ky3R4F), and laboratory air/method blanks. All measurements were conducted by a contract research laboratory using ISO 17025 accredited methods. The data show that it is essential to conduct laboratory air/method measurements when measuring e-cigarette emissions, owing to the combination of low emissions and the associated impact of laboratory background that can lead to false-positive results and overestimates. Of the 150 measurands examined in the e-cigarette aerosol, 104 were not detected and 21 were present due to laboratory background. Of the 25 detected aerosol constituents, 9 were present at levels too low to be quantified and 16 were generated in whole or in part by the e-cigarette. These comprised major e-liquid constituents (nicotine, propylene glycol, and glycerol), recognized impurities in Pharmacopoeia-quality nicotine, and eight thermal decomposition products of propylene glycol or glycerol. By contrast, approximately 100 measurands were detected in mainstream cigarette smoke. Depending on the regulatory list considered and the puffing regime used, the emissions of toxicants identified for regulation were from 82 to >99% lower on a per-puff basis from the e-cigarette compared with those from Ky3R4F. Thus, the aerosol from the e-cigarette is compositionally less complex than cigarette smoke and contains significantly lower levels of toxicants. These data demonstrate that e-cigarettes can be developed that offer the potential

  1. Composition of Secondary Organic Aerosol from the Photolysis of 1-Nitronaphthalene

    Science.gov (United States)

    Wenger, J.; Healy, R.; Chen, Y.; Kalberer, M.; Kourtchev, I.

    2012-12-01

    Nitro-substituted polycyclic aromatic hydrocarbons are of interest due to their associated mutagenic and carcinogenic effects. 1-Nitronaphthalene is emitted directly from combustion processes such as vehicle exhaust, but is also formed through the reaction of naphthalene with the hydroxyl or nitrate radical in the presence of NOx. Photolysis has previously been demonstrated to be the major degradation pathway for 1-nitronaphthalene in the troposphere. In this study, a series of simulation chamber experiments has been performed to investigate the chemical composition of secondary organic aerosol (SOA) formed through the direct photolysis of 1-nitronaphthalene using an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS, TSI). SOA forms rapidly with a yield of up to 50% depending on precursor concentration and photolysis rate. Along with expected products such as naphthoquinone and nitronaphthol, condensed species exhibiting mass spectra consistent with the presence of four aromatic rings were also observed. It is proposed that these species may be formed through dimerization of naphthoxy radicals generated during the photolysis process. Further evidence to support this mechanism was obtained when 1-nitronaphthalene was photolyzed in the presence of excess nitrobenzene. Dimers were then formed containing three aromatic rings, consistent with the reaction of phenoxy and naphthoxy radicals. The molecular formulae of the dimers were also confirmed by collecting SOA on filters and analysing the extracts off-line using an LTQ Orbitrap Velos mass spectrometer (Thermo-Fisher Scientific), fitted with a TriVersa NanoMate chip-based electrospray ionization source (Advion Biosystems). The rapid formation of condensable dimers through the self-reaction of naphthoxy radicals represents a previously unreported potential pathway to SOA formation. Analogous mechanisms may also be important for other nitrated polycyclic aromatic hydrocarbons.

  2. Inferring the effects of compositional boundary layers on crystal nucleation, growth textures, and mineral chemistry in natural volcanic tephras through submicron-resolution imaging

    Directory of Open Access Journals (Sweden)

    Georg F. Zellmer

    2016-09-01

    Full Text Available Crystal nucleation and growth are first order processes captured in volcanic rocks and record important information about the rates of magmatic processes and chemical evolution of magmas during their ascent and eruption. We have studied glass-rich andesitic tephras from the Central Plateau of the Southern Taupo Volcanic Zone by electron- and ion-microbeam imaging techniques to investigate down to sub-micrometre scale the potential effects of compositional boundary layers (CBLs of melt around crystals on the nucleation and growth of mineral phases and the chemistry of crystal growth zones. We find that CBLs may influence the types of mineral phases nucleating and growing, and growth textures such as the development of swallowtails. The chemistry of the CBLs also has the capacity to trigger intermittent overgrowths of nanometre-scale bands of different phases in rapidly growing crystals, resulting in what we refer to as cryptic phase zoning. The existence of cryptic phase zoning has implications for the interpretation of microprobe compositional data, and the resulting inferences made on the conditions of magmatic evolution. Identification of cryptic phase zoning may in future lead to more accurate thermobarometric estimates and thus geospeedometric constraints. In future, a more quantitative characterization of CBL formation and its effects on crystal nucleation and growth may contribute to a better understanding of melt rheology and magma ascent processes at the onset of explosive volcanic eruptions, and will likely be of benefit to hazard mitigation efforts.

  3. Combustion Aerosols from Full-Scale Suspension-Firing of Wood Pellets

    DEFF Research Database (Denmark)

    Damø, Anne Juul; Wu, Hao; Frandsen, Flemming

    2012-01-01

    combustion (without coal ash addition) consisted primarily of irregularly shaped aggregates rich in K, Cl and S (probably KCl and K2SO4). The addition of coal fly ash mainly affected the submicron aerosols in two ways: the relative amount of spherical particles originated from molten minerals was increased.......03 – 12.7 μm) was used to sample aerosols in the flue gas, in the top of the boiler before the SCR (Tfluegas ~350 oC). The collected aerosols were subsequently characterized with respect to particle size distribution, morphology, and chemical composition. The mass-based size distribution of the aerosols...... revealed that the formation of submicron particles was increased significantly when no coal ash was injected, as compared to the reference experiments with addition of coal fly ash. PM1 for the experiments without coal ash addition was in the range 44 – 47 mg/Nm3, while it was only 11 – 19 mg/Nm3...

  4. Comparison of aerosol properties over Beijing and Kanpur: Optical, physical properties and aerosol component composition retrieved from 12 years ground-based Sun-sky radiometer remote sensing data

    Science.gov (United States)

    Li, Zhengqiang; Li, Lei; Zhang, Fengxia; Li, Donghui; Xie, Yisong; Xu, Hua

    2015-02-01

    Aerosol mixtures composed of coarse and fine particles occur frequently in metropolitan areas in the world, especially in developing countries. Beijing, China, and Kanpur, India, are both in Asian monsoon regions and experience strong aerosol loading because of increased economic activities, vehicles, and urbanization. Observations originating from the Aerosol Robotic Network (AERONET) have played a vital role in the field of aerosol study. In order to understand the variations of aerosol optical, physical properties and component composition over Beijing and Kanpur, we focus on AERONET measurements collected at these two sites from 2002 to 2013 and employ a five-component (including black carbon, BC; mineral dust, DU; brown carbon, BrC; ammonium sulfate like, AS; and aerosol water content, AW) aerosol mixture model to retrieve the aerosol component composition. Particle size distribution, spectral characteristics of single-scattering albedo, and refractive indices of the aerosols over Beijing and Kanpur are found to be distinct and with regular seasonal variations. Correspondingly, aerosol components show distinct temporal characteristics at both sites. In Beijing, BC shows a significant decrease from 2002 to 2013 (especially after 2007) with an average declining rate of 0.69 mg m-2 yr-1. Among the five components, BC and BrC are higher during winter and autumn especially at Beijing, while DU and AS are higher during spring and summer at the two sites. With respect to site differences, BC and BrC are usually higher in Beijing in most of the year, while DU and AS are higher in Kanpur especially from April to June. Moreover, AW is similar and quite comparable at two sites.

  5. Wintertime aerosol chemical composition, volatility, and spatial variability in the greater London area

    Directory of Open Access Journals (Sweden)

    L. Xu

    2016-02-01

    Full Text Available The composition of PM1 (particulate matter with diameter less than 1 µm in the greater London area was characterized during the Clean Air for London (ClearfLo project in winter 2012. Two high-resolution time-of-flight aerosol mass spectrometers (HR-ToF-AMS were deployed at a rural site (Detling, Kent and an urban site (North Kensington, London. The simultaneous and high-temporal resolution measurements at the two sites provide a unique opportunity to investigate the spatial distribution of PM1. We find that the organic aerosol (OA concentration is comparable between the rural and urban sites, but the contribution from different sources is distinctly different between the two sites. The concentration of solid fuel OA at the urban site is about twice as high as at the rural site, due to elevated domestic heating in the urban area. While the concentrations of oxygenated OA (OOA are well-correlated between the two sites, the OOA concentration at the rural site is almost twice that of the urban site. At the rural site, more than 70 % of the carbon in OOA is estimated to be non-fossil, which suggests that OOA is likely related to aged biomass burning considering the small amount of biogenic SOA in winter. Thus, it is possible that the biomass burning OA contributes a larger fraction of ambient OA in wintertime than what previous field studies have suggested. A suite of instruments was deployed downstream of a thermal denuder (TD to investigate the volatility of PM1 species at the rural Detling site. After heating at 250 °C in the TD, 40 % of the residual mass is OA, indicating the presence of non-volatile organics in the aerosol. Although the OA associated with refractory black carbon (rBC; measured by a soot-particle aerosol mass spectrometer only accounts for < 10 % of the total OA (measured by a HR-ToF-AMS at 250 °C, the two measurements are well-correlated, suggesting that the non-volatile organics have similar sources or have

  6. Compositional evolution of particle-phase reaction products and water in the heterogeneous OH oxidation of model aqueous organic aerosols

    Science.gov (United States)

    Chim, Man Mei; Cheng, Chiu Tung; Davies, James F.; Berkemeier, Thomas; Shiraiwa, Manabu; Zuend, Andreas; Nin Chan, Man

    2017-12-01

    Organic compounds present at or near the surface of aqueous droplets can be efficiently oxidized by gas-phase OH radicals, which alter the molecular distribution of the reaction products within the droplet. A change in aerosol composition affects the hygroscopicity and leads to a concomitant response in the equilibrium amount of particle-phase water. The variation in the aerosol water content affects the aerosol size and physicochemical properties, which in turn governs the oxidation kinetics and chemistry. To attain better knowledge of the compositional evolution of aqueous organic droplets during oxidation, this work investigates the heterogeneous OH-radical-initiated oxidation of aqueous methylsuccinic acid (C5H8O4) droplets, a model compound for small branched dicarboxylic acids found in atmospheric aerosols, at a high relative humidity of 85 % through experimental and modeling approaches. Aerosol mass spectra measured by a soft atmospheric pressure ionization source (Direct Analysis in Real Time, DART) coupled with a high-resolution mass spectrometer reveal two major products: a five carbon atom (C5) hydroxyl functionalization product (C5H8O5) and a C4 fragmentation product (C4H6O3). These two products likely originate from the formation and subsequent reactions (intermolecular hydrogen abstraction and carbon-carbon bond scission) of tertiary alkoxy radicals resulting from the OH abstraction occurring at the methyl-substituted carbon site. Based on the identification of the reaction products, a kinetic model of oxidation (a two-product model) coupled with the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model is built to simulate the size and compositional changes of aqueous methylsuccinic acid droplets during oxidation. Model results show that at the maximum OH exposure, the droplets become slightly more hygroscopic after oxidation, as the mass fraction of water is predicted to increase from 0.362 to 0.424; however, the

  7. Compositional evolution of particle-phase reaction products and water in the heterogeneous OH oxidation of model aqueous organic aerosols

    Directory of Open Access Journals (Sweden)

    M. M. Chim

    2017-12-01

    Full Text Available Organic compounds present at or near the surface of aqueous droplets can be efficiently oxidized by gas-phase OH radicals, which alter the molecular distribution of the reaction products within the droplet. A change in aerosol composition affects the hygroscopicity and leads to a concomitant response in the equilibrium amount of particle-phase water. The variation in the aerosol water content affects the aerosol size and physicochemical properties, which in turn governs the oxidation kinetics and chemistry. To attain better knowledge of the compositional evolution of aqueous organic droplets during oxidation, this work investigates the heterogeneous OH-radical-initiated oxidation of aqueous methylsuccinic acid (C5H8O4 droplets, a model compound for small branched dicarboxylic acids found in atmospheric aerosols, at a high relative humidity of 85 % through experimental and modeling approaches. Aerosol mass spectra measured by a soft atmospheric pressure ionization source (Direct Analysis in Real Time, DART coupled with a high-resolution mass spectrometer reveal two major products: a five carbon atom (C5 hydroxyl functionalization product (C5H8O5 and a C4 fragmentation product (C4H6O3. These two products likely originate from the formation and subsequent reactions (intermolecular hydrogen abstraction and carbon–carbon bond scission of tertiary alkoxy radicals resulting from the OH abstraction occurring at the methyl-substituted carbon site. Based on the identification of the reaction products, a kinetic model of oxidation (a two-product model coupled with the Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients (AIOMFAC model is built to simulate the size and compositional changes of aqueous methylsuccinic acid droplets during oxidation. Model results show that at the maximum OH exposure, the droplets become slightly more hygroscopic after oxidation, as the mass fraction of water is predicted to increase from

  8. Towards High Capacity Li-ion Batteries Based on Silicon-Graphene Composite Anodes and Sub-micron V-doped LiFePO4 Cathodes

    Science.gov (United States)

    Loveridge, M. J.; Lain, M. J.; Johnson, I. D.; Roberts, A.; Beattie, S. D.; Dashwood, R.; Darr, J. A.; Bhagat, R.

    2016-11-01

    Lithium iron phosphate, LiFePO4 (LFP) has demonstrated promising performance as a cathode material in lithium ion batteries (LIBs), by overcoming the rate performance issues from limited electronic conductivity. Nano-sized vanadium-doped LFP (V-LFP) was synthesized using a continuous hydrothermal process using supercritical water as a reagent. The atomic % of dopant determined the particle shape. 5 at. % gave mixed plate and rod-like morphology, showing optimal electrochemical performance and good rate properties vs. Li. Specific capacities of >160 mAh g-1 were achieved. In order to increase the capacity of a full cell, V-LFP was cycled against an inexpensive micron-sized metallurgical grade Si-containing anode. This electrode was capable of reversible capacities of approximately 2000 mAh g-1 for over 150 cycles vs. Li, with improved performance resulting from the incorporation of few layer graphene (FLG) to enhance conductivity, tensile behaviour and thus, the composite stability. The cathode material synthesis and electrode formulation are scalable, inexpensive and are suitable for the fabrication of larger format cells suited to grid and transport applications.

  9. Chemical composition of ambient aerosol, ice residues and cloud droplet residues in mixed-phase clouds: single particle analysis during the Cloud and Aerosol Characterization Experiment (CLACE 6

    Directory of Open Access Journals (Sweden)

    M. Kamphus

    2010-08-01

    Full Text Available Two different single particle mass spectrometers were operated in parallel at the Swiss High Alpine Research Station Jungfraujoch (JFJ, 3580 m a.s.l. during the Cloud and Aerosol Characterization Experiment (CLACE 6 in February and March 2007. During mixed phase cloud events ice crystals from 5–20 μm were separated from larger ice aggregates, non-activated, interstitial aerosol particles and supercooled droplets using an Ice-Counterflow Virtual Impactor (Ice-CVI. During one cloud period supercooled droplets were additionally sampled and analyzed by changing the Ice-CVI setup. The small ice particles and droplets were evaporated by injection into dry air inside the Ice-CVI. The resulting ice and droplet residues (IR and DR were analyzed for size and composition by the two single particle mass spectrometers: a custom-built Single Particle Laser-Ablation Time-of-Flight Mass Spectrometer (SPLAT and a commercial Aerosol Time-of-Flight Mass Spectrometer (ATOFMS, TSI Model 3800. During CLACE 6 the SPLAT instrument characterized 355 individual IR that produced a mass spectrum for at least one polarity and the ATOFMS measured 152 IR. The mass spectra were binned in classes, based on the combination of dominating substances, such as mineral dust, sulfate, potassium and elemental carbon or organic material. The derived chemical information from the ice residues is compared to the JFJ ambient aerosol that was sampled while the measurement station was out of clouds (several thousand particles analyzed by SPLAT and ATOFMS and to the composition of the residues of supercooled cloud droplets (SPLAT: 162 cloud droplet residues analyzed, ATOFMS: 1094. The measurements showed that mineral dust was strongly enhanced in the ice particle residues. Close to all of the SPLAT spectra from ice residues did contain signatures from mineral compounds, albeit connected with varying amounts of soluble compounds. Similarly, close to all of the ATOFMS IR spectra show a

  10. Single-particle Analyses of Compositions, Morphology, and Viscosity of Aerosol Particles Collected During GoAmazon2014

    Science.gov (United States)

    Adachi, K.; Gong, Z.; Bateman, A. P.; Martin, S. T.; Cirino, G. G.; Artaxo, P.; Sedlacek, A. J., III; Buseck, P. R.

    2014-12-01

    Single-particle analysis using transmission electron microscopy (TEM) shows composition and morphology of individual aerosol particles collected during the GoAmazon2014 campaign. These TEM results indicate aerosol types and mixing states, both of which are important for evaluating particle optical properties and cloud condensation nuclei activity. The samples were collected at the T3 site, which is located in the Amazon forest with influences from the urban pollution plume from Manaus. Samples were also collected from the T0 site, which is in the middle of the jungle with minimal to no influences of anthropogenic sources. The aerosol particles mainly originated from 1) anthropogenic pollution (e.g., nanosphere soot, sulfate), 2) biogenic emissions (e.g., primary biogenic particles, organic aerosols), and 3) long-range transport (e.g., sea salts). We found that the biogenic organic aerosol particles contain homogeneously distributed potassium. Particle viscosity is important for evaluating gas-particle interactions and atmospheric chemistry for the particles. Viscosity can be estimated from the rebounding behavior at controlled relative humidities, i.e., highly viscous particles display less rebound on a plate than low-viscosity particles. We collected 1) aerosol particles from a plate (non-rebounded), 2) those that had rebounded from the plate and were then captured onto an adjacent sampling plate, and 3) particles from ambient air using a separate impactor sampler. Preliminary results show that more than 90% of non-rebounded particles consisted of nanosphere soot with or without coatings. The coatings mostly consisted of organic matter. Although rebounded particles also contain nanosphere soot (number fraction 64-69%), they were mostly internally mixed with sulfate, organic matter, or their mixtures. TEM tilted images suggested that the rebounded particles were less deformed on the substrate, whereas the non-rebounded particles were more deformed, which could

  11. Laboratory Studies of Planetary Hazes: composition of cool exoplanet atmospheric aerosols with very high resolution mass spectrometry

    Science.gov (United States)

    Moran, Sarah E.; Horst, Sarah; He, Chao; Flandinet, Laurene; Moses, Julianne I.; Orthous-Daunay, Francois-Regis; Vuitton, Veronique; Wolters, Cedric; Lewis, Nikole

    2017-10-01

    We present first results of the composition of laboratory-produced exoplanet haze analogues. With the Planetary HAZE Research (PHAZER) Laboratory, we simulated nine exoplanet atmospheres of varying initial gas phase compositions representing increasing metallicities (100x, 1000x, and 10000x solar) and exposed them to three different temperature regimes (600, 400, and 300 K) with two different “instellation” sources (a plasma source and a UV lamp). The PHAZER exoplanet experiments simulate a temperature and atmospheric composition phase space relevant to the expected planetary yield of the Transiting Exoplanet Survey Satellite (TESS) mission as well as recently discovered potentially habitable zone exoplanets in the TRAPPIST-1, LHS-1140, and Proxima Centauri systems. Upon exposure to the energy sources, all of these experiments produced aerosol particles, which were collected in a dry nitrogen glove box and then analyzed with an LTQ Orbitrap XL™ Hybrid Ion Trap-Orbitrap Mass Spectrometer utilizing m/z ranging from 50 to 1000. The collected aerosol samples were found to contain complex organics. Constraining the composition of these aerosols allows us to better understand the photochemical and dynamical processes ongoing in exoplanet atmospheres. Moreover, these data can inform our telescope observations of exoplanets, which is of critical importance as we enter a new era of exoplanet atmosphere observation science with the upcoming launch of the James Webb Space Telescope. The molecular makeup of these haze particles provides key information for understanding exoplanet atmospheric spectra, and constraining the structure and behavior of clouds, hazes, and other aerosols is at the forefront of exoplanet atmosphere science.

  12. Sea spray aerosol chemical composition: elemental and molecular mimics for laboratory studies of heterogeneous and multiphase reactions.

    Science.gov (United States)

    Bertram, Timothy H; Cochran, Richard E; Grassian, Vicki H; Stone, Elizabeth A

    2018-02-16

    Sea spray aerosol particles (SSA), formed through wave breaking at the ocean surface, contribute to natural aerosol particle concentrations in remote regions of Earth's atmosphere, and alter the direct and indirect effects of aerosol particles on Earth's radiation budget. In addition, sea spray aerosol serves as suspended surface area that can catalyze trace gas reactions. It has been shown repeatedly that sea spray aerosol is heavily enriched in organic material compared to the surface ocean. The selective enrichment of organic material complicates the selection of representative molecular mimics of SSA for laboratory or computational studies. In this review, we first provide a short introduction to SSA formation processes and discuss chemical transformations of SSA that occur in polluted coastal regions and remote pristine air. We then focus on existing literature of the chemical composition of nascent SSA generated in controlled laboratory experiments and field investigations. We combine the evidence on the chemical properties of nascent SSA with literature measurements of SSA water uptake to assess SSA molecular composition and liquid water content. Efforts to speciate SSA organic material into molecular classes and specific molecules have led to the identification of saccharides, alkanes, free fatty acids, anionic surfactants, dicarboxylic acids, amino acids, proteinaceous matter, and other large macromolecules. However to date, less than 25% of the organic mass of nascent SSA has been quantified at a molecular level. As discussed here, quantitative measurements of size resolved elemental ratios, combined with determinations of water uptake properties, provides unique insight on the concentration of ions within SSA as a function of particle size, pointing to a controlling role for relative humidity and the hygroscopicity of SSA organic material at small particle diameters.

  13. An Electronic Cigarette Vaping Machine for the Characterization of Aerosol Delivery and Composition.

    Science.gov (United States)

    Havel, Christopher M; Benowitz, Neal L; Jacob, Peyton; St Helen, Gideon

    2017-10-01

    Characterization of aerosols generated by electronic cigarettes (e-cigarettes) is one method used to evaluate the safety of e-cigarettes. While some researchers have modified smoking machines for e-cigarette aerosol generation, these machines are either not readily available, not automated for e-cigarette testing or have not been adequately described. The objective of this study was to build an e-cigarette vaping machine that can be used to test, under standard conditions, e-liquid aerosolization and nicotine and toxicant delivery. The vaping machine was assembled from commercially available parts, including a puff controller, vacuum pump, power supply, switch to control current flow to the atomizer, three-way value to direct air flow to the atomizer, and three gas dispersion tubes for aerosol trapping. To validate and illustrate its use, the variation in aerosol generation was assessed within and between KangerTech Mini ProTank 3 clearomizers, and the effect of voltage on aerosolization and toxic aldehyde generation were assessed. When using one ProTank 3 clearomizer and different e-liquid flavors, the coefficient of variation (CV) of aerosol generated ranged between 11.5% and 19.3%. The variation in aerosol generated between ProTank 3 clearomizers with different e-liquid flavors and voltage settings ranged between 8.3% and 16.3% CV. Aerosol generation increased linearly at 3-6V across e-liquids and clearomizer brands. Acetaldehyde, acrolein, and formaldehyde generation increased markedly at voltages at or above 5V. The vaping machine that we describe reproducibly aerosolizes e-liquids from e-cigarette atomizers under controlled conditions and is useful for testing of nicotine and toxicant delivery. This study describes an electronic cigarette vaping machine that was assembled from commercially available parts. The vaping machine can be replicated by researchers and used under standard conditions to generate e-cigarette aerosols and characterize nicotine and

  14. Investigating organic aerosol loading in the remote marine environment

    Directory of Open Access Journals (Sweden)

    K. Lapina

    2011-09-01

    Full Text Available Aerosol loading in the marine environment is investigated using aerosol composition measurements from several research ship campaigns (ICEALOT, MAP, RHaMBLe, VOCALS and OOMPH, observations of total AOD column from satellite (MODIS and ship-based instruments (Maritime Aerosol Network, MAN, and a global chemical transport model (GEOS-Chem. This work represents the most comprehensive evaluation of oceanic OM emission inventories to date, by employing aerosol composition measurements obtained from campaigns with wide spatial and temporal coverage. The model underestimates AOD over the remote ocean on average by 0.02 (21 %, compared to satellite observations, but provides an unbiased simulation of ground-based Maritime Aerosol Network (MAN observations. Comparison with cruise data demonstrates that the GEOS-Chem simulation of marine sulfate, with the mean observed values ranging between 0.22 μg m−3 and 1.34 μg m−3, is generally unbiased, however surface organic matter (OM concentrations, with the mean observed concentrations between 0.07 μg m−3 and 0.77 μg m−3, are underestimated by a factor of 2–5 for the standard model run. Addition of a sub-micron marine OM source of approximately 9 TgC yr−1 brings the model into agreement with the ship-based measurements, however this additional OM source does not explain the model underestimate of marine AOD. The model underestimate of marine AOD is therefore likely the result of a combination of satellite retrieval bias and a missing marine aerosol source (which exhibits a different spatial pattern than existing aerosol in the model.

  15. Evolution of Asian aerosols during transpacific transport in INTEX-B

    Energy Technology Data Exchange (ETDEWEB)

    Dunlea, E. J.; DeCarlo, Peter; Aiken, Allison; Kimmel, Joel; Peltier, R. E.; Weber, R. J.; Tomlinson, Jason M.; Collins, Donald R.; Shinozuka, Yohei; McNaughton, C. S.; Howell, S. G.; Clarke, A. D.; Emmons, L.; Apel, Eric; Pfister, G. G.; van Donkelaar, A.; Martin, R. V.; Millet, D. B.; Heald, C. L.; Jimenez, J. L.

    2009-10-01

    Measurements of aerosol composition were made with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) on board the NSF/NCAR C-130 aircraft as part of the Intercontinental Chemical Transport Experiment Phase B 5 (INTEX-B) field campaign over the Eastern Pacific Ocean. The HR-ToF-AMS measurements of non-refractory submicron aerosol mass are shown to compare well with other aerosol instrumentation in the INTEX-B field study. Two case studies are described for pollution layers transported across the Pacific from the Asian continent, intercepted 3–4 days and 7–10 days downwind of Asia, respectively. Aerosol chemistry is shown to 10 be a robust tracer for air masses originating in Asia, specifically the presence of sulfate dominated aerosol is a distinguishing feature of Asian pollution layers that have been transported to the Eastern Pacific. We examine the time scales of processing for sulfate and organic aerosol in the atmosphere and show that our observations confirm a conceptual model for transpacific transport from Asia proposed by Brock et al. (2004). 15 Our observations of both sulfate and organic aerosol in aged Asian pollution layers are consistent with fast formation near the Asian continent, followed by washout during lofting and subsequent transformation during transport across the Pacific. Our observations are the first atmospheric measurements to indicate that although secondary organic aerosol (SOA) formation from pollution happens on the timescale of one day, 20 the oxidation of organic aerosol continues at longer timescales in the atmosphere. Comparisons with chemical transport models of data from the entire campaign reveal an under-prediction of SOA mass in the MOZART model, but much smaller discrepancies with the GEOS-Chem model than found in previous studies over the Western Pacific. No evidence is found to support a previous hypothesis for significant secondary 25 organic aerosol formation in the free troposphere.

  16. A Kitchen Degreaser Containing Monoethanolamine Can Alter Indoor Aerosol Composition for Days.

    OpenAIRE

    Schwarz, Jaroslav

    2017-01-01

    Using of such degreaser and consequences related to indoor aerosol are described in this study. Monoethanolamine, a part of a commercial degreaser being used in kitchens, was able to replace ammonium in its sulfate and nitrate salts in the indoor environment, while those salts usually form up to half of PM2.5 aerosol mass indoors.

  17. Chemical and isotopic composition of secondary organic aerosol generated by α-pinene ozonolysis

    NARCIS (Netherlands)

    Meusinger, Carl; Dusek, Ulrike|info:eu-repo/dai/nl/314134166; King, Stephanie M.; Holzinger, Rupert|info:eu-repo/dai/nl/337989338; Rosenørn, Thomas; Sperlich, Peter; Julien, Maxime; Remaud, Gerald S.; Bilde, Merete; Röckmann, Thomas|info:eu-repo/dai/nl/304838233; Johnson, Matthew S.

    2017-01-01

    Secondary organic aerosol (SOA) plays a central role in air pollution and climate. However, the description of the sources and mechanisms leading to SOA is elusive despite decades of research. While stable isotope analysis is increasingly used to constrain sources of ambient aerosol, in many cases

  18. Chemical composition and sources of organic aerosols over London from the ClearfLo 2012 campaigns

    Science.gov (United States)

    Finessi, Emanuela; Holmes, Rachel; Hopkins, James; Lee, James; Harrison, Roy; Hamilton, Jacqueline

    2014-05-01

    Air quality in urban areas represents a major public health issue with around one third of the European population concentrated in cities and numbers expected to increase at global scale, particularly in developing countries. Particulate matter (PM) represents a primary threat for human health as numerous studies have confirmed the association between increased levels of cardiovascular and respiratory diseases with the exposure to PM. Despite considerable efforts made in improving air quality and progressively stricter emissions regulations, the PM concentrations have not changed much over the past decades for reasons that remain unclear, and highlight that studies on PM source apportionment are required for the formulation of effective policy. We investigated the chemical composition of organic aerosol (OA) collected during two intensive field campaigns held in winter and summer 2012 in the frame of the project Clean air for London (http://www.clearflo.ac.uk/). PM samples were collected both at a city background site (North Kensington) and at a rural site 50 km southeast of London (Detling) with 8 to 24 hours sampling schedule and analysed using off-line methods. Thermal-optical analysis was used to quantify OC-EC components while a suite of soft ionization mass spectrometric techniques was deployed for detailed chemical characterization. Liquid chromatography mass Spectrometry (LC-MSn) was mostly used for the simultaneous detection and quantification of various tracers for both primary and secondary OA sources. Well-established markers for wood burning primary OA like levoglucosan and azelaic acid were quantified together with various classes of nitroaromatics including methyl-nitrocatechols that are potential tracers for wood burning secondary OA. In addition, oxidation products of biogenic VOCs such as isoprene and monoterpenes were also quantified for both seasons and sites. A non-negligible contribution from biogenic SOA to urban OA was found in summertime

  19. Comparison of organic compositions in dust storm and normal aerosol samples collected at Gosan, Jeju Island, during spring 2005

    Science.gov (United States)

    Wang, Gehui; Kawamura, Kimitaka; Lee, Meehye

    To better understand the current physical and chemical properties of East Asian aerosols, an intensive observation of atmospheric particles was conducted at Gosan site, Jeju Island, South Korea during 2005 spring. Total suspended particle (TSP) samples were collected using pre-combusted quartz filters and a high-volume air sampler with the time intervals ranging from 3 h to 48 h. The kinds and amount of various organic compounds were measured in the samples using gas chromatography-mass spectrometry. Among the 99 target compounds detected, saccharides (average, 130 ± 14 ng m -3), fatty acids (73 ± 7 ng m -3), alcohols (41 ± 4 ng m -3), n-alkanes (32 ± 3 ng m -3), and phthalates (21 ± 2 ng m -3) were found to be major compound classes with polyols/polyacids, lignin and resin products, PAHs, sterols and aromatic acids being minor. Compared to the previous results reported for 2001 late spring samples, no significant changes were found in the levels of their concentrations and compositions for 4 years, although the economy in East Asia, especially in China, has sharply expanded from 2001 to 2005. During the campaign at Gosan site, we encountered two distinct dust storm episodes with high TSP concentrations. The first dust event occurred on March 28, which was characterized by a predominance of secondary organic aerosols. The second event that occurred on the next day (March 29) was found to be characterized by primary organic aerosols associated with forest fires in Siberia/northeastern China. A significant variation in the molecular compositions, which was found within a day, suggests that the compositions of East Asian aerosols are heterogeneous due to multi-contributions from different source regions together with different pathways of long-range atmospheric transport of particles.

  20. Impact of wildfires on size-resolved aerosol composition at a coastal California site

    Science.gov (United States)

    Maudlin, L. C.; Wang, Z.; Jonsson, H. H.; Sorooshian, A.

    2015-10-01

    Size-resolved aerosol composition measurements were conducted at a coastal site in central California during the Nucleation in California Experiment (NiCE) between July and August of 2013. The site is just east of ship and marine emission sources and is also influenced by continental pollution and wildfires, such as those near the California-Oregon border which occurred near the end of NiCE. Two micro-orifice uniform deposit impactors (MOUDIs) were used, and water-soluble and elemental compositions were measured. The five most abundant water-soluble species (in decreasing order) were chloride, sodium, non-sea salt (nss) sulfate, ammonium, and nitrate. During wildfire periods, nss K mass concentrations were not enhanced as strongly as other species in the sub-micrometer stages and even decreased in the super-micrometer stages; species other than nss K are more reliable tracers for biomass burning in this region. Chloride levels were reduced in the fire sets likely due to chloride depletion by inorganic and organic acids that exhibited elevated levels in transported plumes. During wildfire periods, the mass size distribution of most dicarboxylic acids changed from unimodal to bimodal with peaks in the 0.32 μm and 1.0-1.8 μm stages. Furthermore, sulfate's peak concentration shifted from the 0.32 μm to 0.56 μm stage, and nitrate also shifted to larger sizes (1.0 μm to 1.8-3.2 μm stages). Mass concentrations of numerous soil tracer species (e.g., Si, Fe) were strongly enhanced in samples influenced by wildfires, especially in the sub-micrometer range. Airborne cloud water data confirm that soil species were associated with fire plumes transported south along the coast. In the absence of biomass burning, cloud condensation nuclei (CCN) composition is dominated by nss sulfate and ammonium, and the water-soluble organic fraction is dominated by methanesulfonate, whereas for the samples influenced by wildfires, ammonium becomes the dominant overall species, and

  1. Optimal eigenanalysis for the treatment of aerosols in the retrieval of atmospheric composition from transmission measurements.

    Science.gov (United States)

    Timofeyev, Yuriy M; Polyakov, Alexander V; Steele, Helen M; Newchurch, Michael J

    2003-05-20

    The separation of the individual contributions of aerosol and gases to the total attenuation of radiation through the atmosphere has been the subject of much scientific investigation since remote sensing experiments first began. We describe a new scheme to account for the spectral variation of the aerosol extinction in the inversion of transmission data from occultation measurements. Because the spectral variation of the aerosol extinction is generally unknown,the inversion problem is underdetermined and cannot be solved without a reduction in the number of unknowns in the set of equations used to describe the attenuation at each wavelength. This reduction can be accomplished by a variety of methods, including use of a priori information, the parameterization of the aerosol spectral attenuation, and the specification of the form of the aerosol size distribution. We have developed and implemented a parameterization scheme based on existing empirical and modeled information about the microphysical properties of aerosols. This scheme employs the eigenvectors from an extensive set of simulations to parameterize the aerosol extinction coefficient for incorporation into the inversion algorithm. We examine the accuracy of our method using data sets containing over 24,000 extinction spectra and compare it with that of another scheme that is currently implemented in the Polar Ozone and Aerosol Measurement (POAM) satellite experiment. In simulations using 80 wavelengths in the UV-visible-near-IR spectral range of the Stratospheric Aerosol and Gas Experiment III (SAGE) instrument, we show that, for our optimal parameterization, errors below 1% are observed in 80% of cases, whereas only approximately 20% of all cases are as accurate as this in a quadratic parameterization employing the logarithm of the wavelength.

  2. Chemical composition of Titan's aerosols analogues characterized with a systematic pyrolysis-gas chromatography-mass spectrometry characterization

    Science.gov (United States)

    Szopa, Cyril; Raulin, Francois; Coll, Patrice; Cabane, Michel; GCMS Team

    2014-05-01

    The in situ chemical characterization of Titan's atmosphere was achieved in 2005 with two instruments present onboard the Huygens atmospheric probe : the Aerosol Collector and Pyrolyzer (ACP) devoted to collect and pyrolyse Titan's aerosols ; the Gas Chromatograph-Mass Spectrometer (GCMS) experiment devoted to analyze gases collected in the atmosphere or coming from the aerosols pyrolysis. The GCMS was developed by Hasso Niemann in the filiation of the quadrupole mass spectrometers he built for several former space missions. The main objectives were to : determine the concentration profile of the most abundant chemical species; seek for minor atmospheric organic species not detected with remote observations ; give a first view of the organic aerosols structure; characterize the condensed volatiles present at the surface (e.g. lakes) in case of survival of the probe to the landing impact. Taking into account for the potential complexity of the gaseous samples to be analyzed, it was decided to couple to the MS analyzer a gas chromatograph capable to separate volatile species from light inorganic molecules and noble gases, to organic compounds including aromatics. This was the first GCMS analyzer that worked in an extraterrestrial environment since the Viking missions on Mars. Even if the GCMS coupling mode did not provide any result of interest, it has been demonstrated to be functional during the Huygens descent. But, the direct MS analysis of the atmosphere, and the pyrolysis-MS analysis of aerosols allowed to make great discoveries which are still of primary importance to describe the Titan's lower atmosphere composition. This contribution aims at presenting this instrument that worked in the Titan's atmosphere, and summarizing the most important discoveries it allowed.

  3. Insights into the molecular level composition, sources, and formation mechanisms of dissolved organic matter in aerosols and precipitation

    Science.gov (United States)

    Altieri, Katye Elisabeth

    Atmospheric aerosols scatter and absorb light influencing the global radiation budget and climate, and are associated with adverse effects on human health. Precipitation is an important removal mechanism for atmospheric dissolved organic matter (DOM), and a potentially important input for receiving ecosystems. However, the sources, formation, and composition of atmospheric DOM in aerosols and precipitation are not well understood. This dissertation investigates the composition and formation mechanisms of secondary organic aerosol (SOA) formed through cloud processing reactions, elucidates the composition and sources of DOM in rainwater, and provides links connecting the two. Photochemical batch aqueous-phase reactions of organics with both biogenic and anthropogenic sources (i.e., methylglyoxal, pyruvic acid) and OH radical were performed to simulate cloud processing. The composition of products formed through cloud processing experiments and rainwater collected in New Jersey, USA was investigated using a combination of electrospray ionization mass spectrometry techniques, including ultra-high resolution Fourier transform ion cyclotron resonance mass spectrometry. This dissertation has resulted in the first evidence that oligomers form through cloud processing reactions, the first detailed chemical mechanism of aqueous phase oligomerization, the first identification of oligomers, organosulfates, and nitrooxy organosulfates in precipitation, and the first molecular level chemical characterization of organic nitrogen in precipitation. The formation of oligomers in SOA helps to explain the presence of large multifunctional compounds and humic like substances (HULIS) that dominate particulate organic mass. Oligomers have low vapor pressures and remain in the particle phase after cloud evaporation, enhancing SOA. The chemical properties of the oligomers suggest that they are less hygroscopic than the monomeric reaction products (i.e., organic acids). Their elemental

  4. Pb isotope composition in lichens and aerosols from eastern Sicily: Insights into the regional impact of volcanoes on the environment

    Energy Technology Data Exchange (ETDEWEB)

    Monna, F. (Institut FA Forel (Switzerland)); Aiuppa, A.; Varrica, D. (Dipt. C.F.T.A., Palermo (Italy)); Dongarra, G. (Dipt. C.F.T.A., Palermo (Italy) CNR, Palermo (Italy). Istituto Geochimica dei Fluidi)

    1999-08-01

    A total of 25 lichen thalli of Parmelia conspersa (Ehrh), collected at Vulcano island and at Mt. Etna, during a one-year biogeochemical survey, were analyzed for Pb, br, Al, Sc,[sup 206]Pb/[sup 207]Pb, and [sup 208]Pb/[sup 206]Pb ratios. Lead isotope ratios were also measured on aerosol samples from urban areas and industrial sites of Sicily. The observed [sup 206]Pb/[sup 207]Pb range for urban and industrial aerosols matches the anthropogenic signature. Lichens instead, are closer to the compositional field of [sup 206]Pb rich geogenic sources. This natural input is more evident at Vulcano island than at Mt. Etna, where the anthropogenic activities are considerably more effective. On the basis of lead isotope data, Pb/Br ratios and calculated lead enrichment factors, a natural lead pollution from volcanoes is suggested. Volcanic lead contribution ranges from 10 to 30% at Mt. Etna to 10--80% at Vulcano island.

  5. Contrasting organic aerosol particles from boreal and tropical forests during HUMPPA-COPEC-2010 and AMAZE-08 using coherent vibrational spectroscopy

    Directory of Open Access Journals (Sweden)

    C. J. Ebben

    2011-10-01

    Full Text Available We present the vibrational sum frequency generation spectra of organic particles collected in a boreal forest in Finland and a tropical forest in Brazil. These spectra are compared to those of secondary organic material produced in the Harvard Environmental Chamber. By comparing coherent vibrational spectra of a variety of terpene and olefin reference compounds, along with the secondary organic material synthesized in the environmental chamber, we show that submicron aerosol particles sampled in Southern Finland during HUMPPA-COPEC-2010 are composed to a large degree of material similar in chemical composition to synthetic α-pinene-derived material. For material collected in Brazil as part of AMAZE-08, the organic component is found to be chemically complex in the coarse mode but highly uniform in the fine mode. When combined with histogram analyses of the isoprene and monoterpene abundance recorded during the HUMPPA-COPEC-2010 and AMAZE-08 campaigns, the findings presented here indicate that if air is rich in monoterpenes, submicron-sized secondary aerosol particles that form under normal OH and O3 concentration levels can be described in terms of their hydrocarbon content as being similar to α-pinene-derived model secondary organic aerosol particles. If the isoprene concentration dominates the chemical composition of organic compounds in forest air, then the hydrocarbon component of secondary organic material in the submicron size range is not simply well-represented by that of isoprene-derived model secondary organic aerosol particles but is more complex. Throughout the climate-relevant size range of the fine mode, however, we find that the chemical composition of the secondary organic particle material from such air is invariant with size, suggesting that the particle growth does not change the chemical composition of the hydrocarbon component of the particles in a significant way.

  6. PM2.5 Chemical Compositions and Aerosol Optical Properties in Beijing during the Late Fall

    Directory of Open Access Journals (Sweden)

    Huanbo Wang

    2015-01-01

    Full Text Available Daily PM2.5 mass concentrations and chemical compositions together with the aerosol optical properties were measured from 8–28 November 2011 in Beijing. PM2.5 mass concentration varied from 15.6–237.5 μg∙m−3 and showed a mean value of 111.2 ± 73.4 μg∙m−3. Organic matter, NH4NO3 and (NH42SO4 were the major constituents of PM2.5, accounting for 39.4%, 15.4%, and 14.9% of the total mass, respectively, while fine soil, chloride salt, and elemental carbon together accounted for 27.7%. Daily scattering and absorption coefficients (σsc and σap were in the range of 31.1–667 Mm−1 and 8.24–158.0 Mm−1, with mean values of 270 ± 200 Mm−1 and 74.3 ± 43.4 Mm−1. Significant increases in σsc and σap were observed during the pollution accumulation episodes. The revised IMPROVE algorithm was applied to estimate the extinction coefficient (bext. On average, organic matter was the largest contributor, accounting for 44.6% of bext, while (NH42SO4, NH4NO3, elemental carbon, and fine soil accounted for 16.3% 18.0%, 18.6%, and 2.34% of bext, respectively. Nevertheless, the contributions of (NH42SO4 and NH4NO3 were significantly higher during the heavy pollution periods than those on clean days. Typical pollution episodes were also explored, and it has been characterized that secondary formation of inorganic compounds is more important than carbonaceous pollution for visibility impairment in Beijing.

  7. Near Real-Time, Microchip Assay of Aerosol Chemical Composition Project

    Data.gov (United States)

    National Aeronautics and Space Administration — A compact, autonomous and rugged instrument to measure the concentration of inorganic ions, and possibly organic acids, in atmospheric aerosols is proposed. This...

  8. Technical note: Relating functional group measurements to carbon types for improved model-measurement comparisons of organic aerosol composition

    Science.gov (United States)

    Takahama, Satoshi; Ruggeri, Giulia

    2017-04-01

    Functional group (FG) analysis provides a means by which functionalization in organic aerosol can be attributed to the abundances of its underlying molecular structures. However, performing this attribution requires additional, unobserved details about the molecular mixture to provide constraints in the estimation process. We present an approach for conceptualizing FG measurements of organic aerosol in terms of its functionalized carbon atoms. This reformulation facilitates estimation of mass recovery and biases in popular carbon-centric metrics that describe the extent of functionalization (such as oxygen to carbon ratio, organic mass to organic carbon mass ratio, and mean carbon oxidation state) for any given set of molecules and FGs analyzed. Furthermore, this approach allows development of parameterizations to more precisely estimate the organic carbon content from measured FG abundance. We use simulated photooxidation products of α-pinene secondary organic aerosol previously reported by Ruggeri et al. (2016) and FG measurements by Fourier transform infrared (FT-IR) spectroscopy in chamber experiments by Sax et al. (2005) to infer the relationships among molecular composition, FG composition, and metrics of organic aerosol functionalization. We find that for this simulated system, ˜ 80 % of the carbon atoms should be detected by FGs for which calibration models are commonly developed, and ˜ 7 % of the carbon atoms are undetectable by FT-IR analysis because they are not associated with vibrational modes in the infrared. Estimated biases due to undetected carbon fraction for these simulations are used to make adjustments in these carbon-centric metrics such that model-measurement differences are framed in terms of unmeasured heteroatoms (e.g., in hydroperoxide and nitrate groups for the case studied in this demonstration). The formality of this method provides framework for extending FG analysis to not only model-measurement but also instrument

  9. IMPACT OF AEROSOL LIQUID WATER ON SECONDARY ORGANIC AEROSOL YIELDS OF IRRADIATED TOLUENE/PROPYLENE/NOX/(NH4)2SO4/AIR MIXUTRES

    Science.gov (United States)

    Laboratory experiments were conducted to assess whether the presence of liquid water on pre-existing submicron ammonium sulfate aerosols affects yields of condensible organic compounds. Toluene/propylene/NOX/air mixtures were irradiated in the presence of submicron ammonium su...

  10. Aerosol Observability and Data Assimilation Investigations in Support of Atmospheric Composition Forecasts

    Science.gov (United States)

    2013-09-30

    elevated Aqua MODIS aerosol optical depth retrievals over the mid-latitude Southern Oceans through intercomparison with co-located CALIOP, MAN, and...AERONET datasets, J. Geophys. Res, in press Eck, T. F., B. N. Holben, J. S. Reid, et al., (2013), A seasonal trend of single scattering albedo in...Hsu, N. C., (2013), Critical evaluation of the MODIS Deep Blue aerosol optical depth product for data assimilation over North Africa, Atmos. Meas

  11. AIP1OGREN: Aerosol Observing Station Intensive Properties Value-Added Product

    Energy Technology Data Exchange (ETDEWEB)

    Koontz, Annette [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Flynn, Connor [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

    2017-09-15

    The aip1ogren value-added product (VAP) computes several aerosol intensive properties. It requires as input calibrated, corrected, aerosol extensive properties (scattering and absorption coefficients, primarily) from the Aerosol Observing Station (AOS). Aerosol extensive properties depend on both the nature of the aerosol and the amount of the aerosol. We compute several properties as relationships between the various extensive properties. These intensive properties are independent of aerosol amount and instead relate to intrinsic properties of the aerosol itself. Along with the original extensive properties we report aerosol single-scattering albedo, hemispheric backscatter fraction, asymmetry parameter, and Ångström exponent for scattering and absorption with one-minute averaging. An hourly averaged file is produced from the 1-minute files that includes all extensive and intensive properties as well as submicron scattering and submicron absorption fractions. Finally, in both the minutely and hourly files the aerosol radiative forcing efficiency is provided.

  12. Enhancement of the aerosol direct radiative effect by semi-volatile aerosol components: airborne measurements in North-Western Europe

    Directory of Open Access Journals (Sweden)

    W. T. Morgan

    2010-09-01

    Full Text Available A case study of atmospheric aerosol measurements exploring the impact of the vertical distribution of aerosol chemical composition upon the radiative budget in North-Western Europe is presented. Sub-micron aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS on both an airborne platform and a ground-based site at Cabauw in the Netherlands. The examined period in May 2008 was characterised by enhanced pollution loadings in North-Western Europe and was dominated by ammonium nitrate and Organic Matter (OM. Both ammonium nitrate and OM were observed to increase with altitude in the atmospheric boundary layer. This is primarily attributed to partitioning of semi-volatile gas phase species to the particle phase at reduced temperature and enhanced relative humidity. Increased ammonium nitrate concentrations in particular were found to strongly increase the ambient scattering potential of the aerosol burden, which was a consequence of the large amount of associated water as well as the enhanced mass. During particularly polluted conditions, increases in aerosol optical depth of 50–100% were estimated to occur due to the observed increase in secondary aerosol mass and associated water uptake. Furthermore, the single scattering albedo was also shown to increase with height in the boundary layer. These enhancements combined to increase the negative direct aerosol radiative forcing by close to a factor of two at the median percentile level. Such increases have major ramifications for regional climate predictions as semi-volatile components are often not included in aerosol models.

    The results presented here provide an ideal opportunity to test regional and global representations of both the aerosol vertical distribution and subsequent impacts in North-Western Europe. North-Western Europe can be viewed as an analogue for the possible future air quality over other polluted regions of the Northern Hemisphere, where

  13. A review of current knowledge concerning PM2. 5 chemical composition, aerosol optical properties and their relationships across China

    Science.gov (United States)

    Tao, Jun; Zhang, Leiming; Cao, Junji; Zhang, Renjian

    2017-08-01

    To obtain a thorough knowledge of PM2. 5 chemical composition and its impact on aerosol optical properties across China, existing field studies conducted after the year 2000 are reviewed and summarized in terms of geographical, interannual and seasonal distributions. Annual PM2. 5 was up to 6 times the National Ambient Air Quality Standards (NAAQS) in some megacities in northern China. Annual PM2. 5 was higher in northern than southern cities, and higher in inland than coastal cities. In a few cities with data longer than a decade, PM2. 5 showed a slight decrease only in the second half of the past decade, while carbonaceous aerosols decreased, sulfate (SO42-) and ammonium (NH4+) remained at high levels, and nitrate (NO3-) increased. The highest seasonal averages of PM2. 5 and its major chemical components were typically observed in the cold seasons. Annual average contributions of secondary inorganic aerosols to PM2. 5 ranged from 25 to 48 %, and those of carbonaceous aerosols ranged from 23 to 47 %, both with higher contributions in southern regions due to the frequent dust events in northern China. Source apportionment analysis identified secondary inorganic aerosols, coal combustion and traffic emission as the top three source factors contributing to PM2. 5 mass in most Chinese cities, and the sum of these three source factors explained 44 to 82 % of PM2. 5 mass on annual average across China. Biomass emission in most cities, industrial emission in industrial cities, dust emission in northern cities and ship emission in coastal cities are other major source factors, each of which contributed 7-27 % to PM2. 5 mass in applicable cities. The geographical pattern of scattering coefficient (bsp) was similar to that of PM2. 5, and that of aerosol absorption coefficient (bap) was determined by elemental carbon (EC) mass concentration and its coating. bsp in ambient condition of relative humidity (RH) = 80 % can be amplified by about 1.8 times that under dry conditions

  14. Global distribution and climate forcing of marine organic aerosol: 1. Model improvements and evaluation

    Science.gov (United States)

    Meskhidze, N.; Xu, J.; Gantt, B.; Zhang, Y.; Nenes, A.; Ghan, S. J.; Liu, X.; Easter, R.; Zaveri, R.

    2011-11-01

    Marine organic aerosol emissions have been implemented and evaluated within the National Center of Atmospheric Research (NCAR)'s Community Atmosphere Model (CAM5) with the Pacific Northwest National Laboratory's 7-mode Modal Aerosol Module (MAM-7). Emissions of marine primary organic aerosols (POA), phytoplankton-produced isoprene- and monoterpenes-derived secondary organic aerosols (SOA) and methane sulfonate (MS-) are shown to affect surface concentrations of organic aerosols in remote marine regions. Global emissions of submicron marine POA is estimated to be 7.9 and 9.4 Tg yr-1, for the Gantt et al. (2011) and Vignati et al. (2010) emission parameterizations, respectively. Marine sources of SOA and particulate MS- (containing both sulfur and carbon atoms) contribute an additional 0.2 and 5.1 Tg yr-1, respectively. Widespread areas over productive waters of the Northern Atlantic, Northern Pacific, and the Southern Ocean show marine-source submicron organic aerosol surface concentrations of 100 ng m-3, with values up to 400 ng m-3 over biologically productive areas. Comparison of long-term surface observations of water insoluble organic matter (WIOM) with POA concentrations from the two emission parameterizations shows that despite revealed discrepancies (often more than a factor of 2), both Gantt et al. (2011) and Vignati et al. (2010) formulations are able to capture the magnitude of marine organic aerosol concentrations, with the Gantt et al. (2011) parameterization attaining better seasonality. Model simulations show that the mixing state of the marine POA can impact the surface number concentration of cloud condensation nuclei (CCN). The largest increases (up to 20%) in CCN (at a supersaturation (S) of 0.2%) number concentration are obtained over biologically productive ocean waters when marine organic aerosol is assumed to be externally mixed with sea-salt. Assuming marine organics are internally-mixed with sea-salt provides diverse results with increases

  15. Global distribution and climate forcing of marine organic aerosol - Part 1: Model improvements and evaluation

    Science.gov (United States)

    Meskhidze, N.; Xu, J.; Gantt, B.; Zhang, Y.; Nenes, A.; Ghan, S. J.; Liu, X.; Easter, R.; Zaveri, R.

    2011-07-01

    Marine organic aerosol emissions have been implemented and evaluated within the National Center of Atmospheric Research (NCAR)'s Community Atmosphere Model (CAM5) with the Pacific Northwest National Laboratory's 7-mode Modal Aerosol Module (MAM-7). Emissions of marine primary organic aerosols (POA), phytoplankton-produced isoprene- and monoterpenes-derived secondary organic aerosols (SOA) and methane sulfonate (MS-) are shown to affect surface concentrations of organic aerosols in remote marine regions. Global emissions of submicron marine POA is estimated to be 7.9 and 9.4 Tg yr-1, for the Gantt et al. (2011) and Vignati et al. (2010) emission parameterizations, respectively. Marine sources of SOA and particulate MS- (containing both sulfur and carbon atoms) contribute an additional 0.2 and 5.1 Tg yr-1, respectively. Widespread areas over productive waters of the Northern Atlantic, Northern Pacific, and the Southern Ocean show marine-source submicron organic aerosol surface concentrations of 100 ng m-3, with values up to 400 ng m-3 over biologically productive areas. Comparison of long-term surface observations of water insoluble organic matter (WIOM) with POA concentrations from the two emission parameterizations shows that both Gantt et al. (2011) and Vignati et al. (2010) formulations are able to capture the magnitude of marine organic aerosol concentrations, with the Gantt et al. (2011) parameterization attaining better seasonality. Model simulations show that the mixing state of the marine POA can impact the surface number concentration of cloud condensation nuclei (CCN). The largest increases (up to 20 %) in CCN (at a supersaturation (S) of 0.2 %) number concentration are obtained over biologically productive ocean waters when marine organic aerosol is assumed to be externally mixed with sea-salt. Assuming marine organics are internally-mixed with sea-salt provides diverse results with increase and decrease in the concentration of CCN over different parts of

  16. Combined use of optical and electron microscopic techniques for the measurement of hygroscopic property, chemical composition, and morphology of individual aerosol particles.

    Science.gov (United States)

    Ahn, Kang-Ho; Kim, Sun-Man; Jung, Hae-Jin; Lee, Mi-Jung; Eom, Hyo-Jin; Maskey, Shila; Ro, Chul-Un

    2010-10-01

    In this work, an analytical method for the characterization of the hygroscopic property, chemical composition, and morphology of individual aerosol particles is introduced. The method, which is based on the combined use of optical and electron microscopic techniques, is simple and easy to apply. An optical microscopic technique was used to perform the visual observation of the phase transformation and hygroscopic growth of aerosol particles on a single particle level. A quantitative energy-dispersive electron probe X-ray microanalysis, named low-Z particle EPMA, was used to perform a quantitative chemical speciation of the same individual particles after the measurement of the hygroscopic property. To validate the analytical methodology, the hygroscopic properties of artificially generated NaCl, KCl, (NH(4))(2)SO(4), and Na(2)SO(4) aerosol particles of micrometer size were investigated. The practical applicability of the analytical method for studying the hygroscopic property, chemical composition, and morphology of ambient aerosol particles is demonstrated.

  17. Fe-Si-Cr/PTFE magnetic composite thick films on polyethylene terephthalate sheets for near field communications by aerosol deposition.

    Science.gov (United States)

    Kim, Hyung-Jun; Nam, Song-Min; Koh, Jung-Hyuk

    2014-10-01

    Thick film growth of Fe-Si-Cr/poly-tetra-fluoro-ethylene (PTFE) composite films on polyethylene terephthalate (PET) sheets was investigated by aerosol deposition (AD) as a magnetic absorber for near field communication. The Fe-Si-Cr flakes were crushed to micro flakes smaller than 1 μm after the deposition, and formed dense microstructure on the PET sheets. The Fe-Si-Cr/PTFE composite thick films using 0.2 wt.% PTFE starting powder showed dense and uniform microstructure compared to the 0.5 wt.% film. The real relative permeability /' and the imaginary permeability μ" of Fe-Si-Cr/PTFE composite thick films using the 0.2 wt.% PTFE starting powder were 13.1 and 2.9 at 13.56 MHz, respectively. In the case of 0.5 wt.%, μ' and μ" respectively decreased to 7.4 and 1.0 at 13.56 MHz caused by adding PTFE.

  18. Ambient Aerosol in Southeast Asia: High Resolution Aerosol Mass Spectrometer Measurements Over Oil Palm (Elaeis guineensis)

    Science.gov (United States)

    Phillips, G.; Dimarco, C.; Misztal, P.; Nemitz, E.; Farmer, D.; Kimmel, J.; Jimenez, J.

    2008-12-01

    The emission of organic compounds in the troposphere is important factor in the formation of secondary organic aerosol (SOA). A very large proportion of organic material emitted globally is estimated to arise from biogenic sources, with almost half coming from tropical and sub-tropical forests. Preliminary analyses of leave cuvette emission studies suggest that oil palm (Elaeis guineensis) is a significantly larger source of isoprene than tropical forest. Much larger sources of isoprene over oil palm allied with a larger anthropogenic component of local emissions contrast greatly with the remote tropical forest environment and therefore the character of SOA formed may differ significantly. These issues, allied with the high price of palm oil on international markets leading to increased use of land for oil palm production, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions and composition of organic aerosol over all important land-uses in the tropical environment. This in turn will lead to a greater understanding of the present, and to an improvement in predictive capacity for the future system. To help address these issues, a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as part of the field component of the Aerosol Coupling in the Earth System (ACES) project, part of the UK NERC APPRAISE program. This project was allied closely with measurements made of similar chemical species and aerosol components at a forest site in the Danum Valley as part of the UK Oxidant and Particle Photochemical Processes above a Southeast Asian tropical rainforest (OP3) project. Measurements of submicron non- refractory aerosol composition are presented along with some preliminary analysis of chemically resolved aerosol fluxes made with a new eddy covariance system, based on the

  19. Molecular Distributions and Compound-specific Stable Carbon Isotopic Compositions of Lipids in Wintertime Aerosols from Beijing

    Science.gov (United States)

    Ren, L.; Fu, P.; He, Y.; Hou, J.; Chen, J.; Chandra Mouli, P.; Yele, S.; Wang, Z.

    2016-12-01

    Molecular distributions and stable carbon isotopic compositions (δ13C) of n-alkanes, fatty acids and n-alcohols were investigated in urban aerosols from Beijing, northern China to better understand the sources and long-range atmospheric transport of terrestrial organic matter during polluted and clear days in winter. n-Alkanes (C19-C36), fatty acids (C8-C32) and n-alcohols (C16-C32) detected in Beijing aerosols are characterized by the predominance of C23, C16 and C28, respectively. Carbon preference index (CPI) values of n-alkanes, the ratios of the sum of odd-numbered n-alkanes to the sum of even-numbered n-alkanes, are close to 1, indicating a heavy influence of fossil fuel combustion. Relatively higher ratios of C(18:0+16:0)/C(18:n+16:1) (fatty acids) on clear days than polluted days indicate that long-distance transport and/or photochemical aging are more significant during clear days. δ13C values of n-alkanes and low molecular weight fatty acids (C16:0, C18:0) ranged from -34.1 to -24.7‰ and -26.9 to -24.6‰, respectively, which are generally heavier on polluted days than those on clear days. Such a wide range suggests that atmospheric lipids in Beijing aerosols originate from multiple sources and encounter complicated atmospheric processes during long-range transport in North China.

  20. Investigating the composition of organic aerosol resulting from cyclohexene ozonolysis: low molecular weight and heterogeneous reaction products

    Directory of Open Access Journals (Sweden)

    J. F. Hamilton

    2006-01-01

    Full Text Available The composition of organic aerosol formed from the gas phase ozonolysis of cyclohexene has been investigated in a smog chamber experiment. Comprehensive gas chromatography with time of flight mass spectrometric detection was used to determine that dicarboxylic acids and corresponding cyclic anhydrides dominated the small gas phase reaction products found in aerosol sampled during the first hour after initial aerosol formation. Structural analysis of larger more polar molecules was performed using liquid chromatography with ion trap tandem mass spectrometry. This indicated that the majority of identified organic mass was in dimer form, built up from combinations of the most abundant small acid molecules, with frequent indication of the inclusion of adipic acid. Trimers and tetramers potentially formed via similar acid combinations were also observed in lower abundances. Tandem mass spectral data indicated dimers with either acid anhydride or ester functionalities as the linkage between monomers. High-resolution mass spectrometry identified the molecular formulae of the most abundant dimer species to be C10H16O6, C11H18O6, C10H14O8 and C11H16O8 and could be used in some cases to reduce uncertainty in exact chemical structure determination by tandem MS.

  1. Molecular composition of rainwater and aerosol during rain events in León, Spain, using high resolution mass spectrometry.

    Science.gov (United States)

    Fee, Anna

    2017-04-01

    Anna Fee (1), Markus Kalberer (1), Roberto Fraile (2), Amaya Castro (2), Ana. I. Calvo (2), Carlos Blanco-Alegre (2), Fernanda Oduber (2) and Mário Cerqueira (3). 1 Department of Chemistry, University of Cambridge, UK. 2 Department of Applied Chemistry and Physics, IMARENAB, University of León, Spain. 3 Department of Environmental Planning, University of Aveiro, Portugal. A wide range of atmospheric compounds which are present in rainwater are often also present in aerosol. They can be taken up during cloud droplet formation (in-cloud scavenging) or washed out during precipitation (below-cloud scavenging). Such compounds including aromatic hydrocarbons and organic nitrogen containing compounds are hazardous to health. In this study, the organic chemical composition of rainwater and aerosol from rain events in León, Spain, is being analysed using high resolution mass spectrometry. Collected rainwater along with high volume and low volume filters from rain events which occurred during spring, summer and winter of 2016 have been selected for analysis. Rainwater samples were prepared using Polymeric Reversed Phase Solid Phase Extraction (SPE) and filters have been extracted in water with and without SPE. Three different SPE polymer based sorbents were tested; one for extracting neutral compounds and two which are more suitable for extracting organic compounds containing sulphate and other polar functional groups. The sorbent for extracting neutral compounds was found to yield a higher number of compounds from the sample extraction than the other two varieties. Kendrick masses, Van Krevelen plots and carbon oxidation states have been investigated to identify compounds and patterns. Preliminary results show a predominance in peaks with O/C ratios between 0.2 and 0.7 and H/C ratios between 1 and 2 in both rain and aerosol samples which indicates substituted aromatic compounds. Cellulose material and fatty acids may also be present. The rain samples also have a

  2. Long term measurements of the elemental composition and optical properties of aerosols in Amazonia

    Directory of Open Access Journals (Sweden)

    Arana A. A.

    2013-04-01

    Full Text Available Aerosols are being collected and analyzed for trace elements in two sites in Amazonia since January 2008. On eof the site, Manaus is located in a very pristine area in Central Amazonia. The site is nt affected directly by any urban plume for thousands of kilometers. A second site is located in Porto Velho, in a region with heavy land use change and deforestation. Optical properties (light scattering ad absorption are also being measured in order to study the climatic impact of aerosols. It was observed a clear seasonal pattern for both sites, with higher concentrations in the dry season. But the difference in seasonal concentrations observed for Porto Velho is much larger due to stronger anthropogenic influences. In Manaus during the wet season, very low concentrations of heavy metals, maybe the smallest measured in continental regions are reported. Positive Matrix Factorization (PMF was used to separate the different aerosol components. In general, for fine and coarse mode and wet and dry season, 3 aerosol components could be observed: 1 Natural biogenic aerosol; 2 biomass burning component; 3 Soil dust both locally and long range transported Sahara dust

  3. Composition and chirality of amino acids in aerosol/dust from laboratory and residential enclosures.

    Science.gov (United States)

    Armstrong, D W; Kullman, J P; Chen, X; Rowe, M

    2001-01-01

    Initial results from the analyses of geological and anthropological samples for amino acids were difficult to accept because of the high enantiomeric purities of the analytes (i.e., predominantly L-amino acids). Consequently, sources of contamination had to be considered. All sources were eliminated except for direct atmospheric contamination. Essentially invisible, microscopic, aerosol/dust was found to rapidly contaminate the surface of samples and sample containers even after brief exposure times in clean laboratories. Contamination increased with exposure time. The aerosol/dust amino acids were contained predominantly in a proteinaceous material. Aerosol/dust from different locations can contain different percentages of proteinoid/amino acid material. However, the relative concentrations of the amino acids were similar for both laboratory and residential samples. The enantiomeric purity of the L-amino acids studied in aerosol/dust appears to be 99% or greater for the samples examined. Thus, even slight contamination of any sample with microscopic dust or aerosol particles can skew the results of trace amino acid analyses and amino acid e.e. determinations.

  4. New Approach for Near-Real-Time Measurement of Elemental Composition of Aerosol Using Laser-Induced Breakdown Spectroscopy.

    Science.gov (United States)

    Diwakar, Prasoon; Kulkarni, Pramod; Birch, M Eileen

    A new approach has been developed for making near-real-time measurement of elemental composition of aerosols using plasma spectroscopy. The method allows preconcentration of miniscule particle mass (pg to ng) directly from the sampled aerosol stream through electrostatic deposition of charged particles (30-900 nm) onto a flat-tip microneedle electrode. The collected material is subsequently ablated from the electrode and monitored by laser-induced breakdown spectroscopy. Atomic emission spectra were collected using a broadband spectrometer with a wavelength range of 200-980 nm. A single-sensor delay time of 1.3 μs was used in the spectrometer for all elements to allow simultaneous measurement of multiple elements. The system was calibrated for various elements including Cd, Cr, Cu, Mn, Na, and Ti. The absolute mass detection limits for these elements were experimentally determined and found to be in the range of 0.018-5 ng. The electrostatic collection technique has many advantages over other substrate-based methods involving aerosol collection on a filter or its focused deposition using an aerodynamic lens. Because the particle mass is collected over a very small area that is smaller than the spatial extent of the laser-induced plasma, the entire mass is available for analysis. This considerably improves reliability of the calibration and enhances measurement accuracy and precision. Further, the aerosol collection technique involves very low pressure drop, thereby allowing higher sample flow rates with much smaller pumps-a desirable feature for portable instrumentation. Higher flow rates also make it feasible to measure trace element concentrations at part per trillion levels. Detection limits in the range of 18-670 ng m-3 can be achieved for most of the elements studied at a flow rate of 1.5 L min-1 with sampling times of 5 min.

  5. Insights into a dust event transported through Beijing in spring 2012: Morphology, chemical composition and impact on surface aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Hu, Wei [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China); Faculty of Environmental and Symbiotic Sciences, Prefectural University of Kumamoto, Kumamoto 862-8502 (Japan); Niu, Hongya [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China); Key Laboratory of Resource Exploration Research of Hebei Province, Hebei University of Engineering, Handan, Hebei 056038 (China); Zhang, Daizhou [Faculty of Environmental and Symbiotic Sciences, Prefectural University of Kumamoto, Kumamoto 862-8502 (Japan); Wu, Zhijun [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China); Chen, Chen [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China); Beijing Municipal Environmental Monitoring Center, Beijing 100044 (China); Wu, Yusheng; Shang, Dongjie [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China); Hu, Min, E-mail: minhu@pku.edu.cn [State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871 (China)

    2016-09-15

    Multiple approaches were used to investigate the evolution of surface aerosols in Beijing during the passage of a dust event at high altitude, which was from the Gobi areas of southern Mongolia and covered a wide range of North China. Single particle analysis with electron microscope showed that the majority of coarse particles were mineral ones, and most of them were in the size range of 1–7 μm with a peak of number concentration at about 3.5 μm. Based on elemental composition and morphology, the mineral particles could be classified into several groups, including Si-rich (71%), Ca-rich (15%), Fe-rich (6%), and halite-rich (2%), etc., and they were the main contributors to the aerosol optical depth as the dust occurred. The size distributions of surface aerosols were significantly affected by the dust intrusion. The average number concentration of accumulation mode particles during the event was about 400 cm{sup −3}, which was much lower than that in heavily polluted days (6300 cm{sup −3}). At the stage of floating dust, the number concentration of accumulation mode particles decreased, and coarse particles contributed to total volume concentration of particulate matter as much as 90%. The accumulation mode particles collected in this stage were mostly in the size range of 0.2–0.5 μm, and were rectangular or spherical. They were considered to be particles consisting of ammonium sulfate. New particle formation (NPF) was observed around noon in the three days during the dust event, indicating that the passage of the dust was probably favorable for NPF. - Highlights: • A dust event transported at high altitude through Beijing was investigated. • The dust event caused high variation in surface aerosol number concentrations. • Fine particles in the floating dust period probably consisted of ammonium sulfate. • Passage of the dust induced a favorable condition for new particle formation.

  6. Submicron Features in Higher Manganese Silicide

    Directory of Open Access Journals (Sweden)

    Yatir Sadia

    2013-01-01

    Full Text Available The world energy crisis had increased the demand for alternative energy sources and as such is one of the topics at the forefront of research. One way for reducing energy consumption is by thermoelectricity. Thermoelectric effects enable direct conversion of thermal into electrical energy. Higher manganese silicide (HMS, MnSi1.75 is one of the promising materials for applications in the field of thermoelectricity. The abundance and low cost of the elements, combined with good thermoelectric properties and high mechanical and chemical stability at high temperatures, make it very attractive for thermoelectric applications. Recent studies have shown that Si-rich HMS has improved thermoelectric properties. The most interesting of which is the unusual reduction in thermal conductivity. In the current research, transmission (TEM and scanning (SEM electron microscopy as well as X-ray diffraction methods were applied for investigation of the govern mechanisms resulting in very low thermal conductivity values of an Si-rich HMS composition, following arc melting and hot-pressing procedures. In this paper, it is shown that there is a presence of sub-micron dislocations walls, stacking faults, and silicon and HMS precipitates inside each other apparent in the matrix, following a high temperature (0.9 Tm hot pressing for an hour. These are not just responsible for the low thermal conductivity values observed but also indicate the ability to create complicate nano-structures that will last during the production process and possibly during the application.

  7. On the dry deposition of submicron particles

    Energy Technology Data Exchange (ETDEWEB)

    Wesely, M. L.

    1999-10-08

    The air-surface exchange of particles can have a strong role in determining the amount, size, and chemical composition of particles in the troposphere. Here the authors consider only dry processes (deposition processes not directly aided by precipitation) and mostly address particles less than about 2 {micro}m in diameter (often referred to as submicron particles because most of such particles are less than 1 {micro}m in diameter). The processes that control the dry exchange of particulate material between the atmosphere and the surface of the Earth are numerous, highly varied, and sometimes poorly understood. As a result, determining which of the surface processes to parameterize or simulate in modeling the tropospheric mass budget of a particulate substance can be a significant challenge. Dry deposition, for example, can be controlled by a combination of Brownian diffusion, impaction, interception, and gravitational settling, depending on the size of the particles, the roughness of the surface on both micrometeorological and microscopic scales, the geometrical structure of vegetative canopies, and other surface characteristics such as wetness. Particles can be added to the lower atmosphere by resuspension from land surfaces and sea spray. The roles of rapid gas-to-particle conversion and growth or shrinkage of particles as a result of water condensation or evaporation in the lower few meters of the atmosphere can also have a significant impact on particle concentrations in the lower atmosphere. Here, a few micrometeorological observations and inferences on particle air-surface exchange are briefly addressed.

  8. Organic composition and source apportionment of fine aerosol at Monterrey, Mexico, based on organic markers

    Science.gov (United States)

    Mancilla, Y.; Mendoza, A.; Fraser, M. P.; Herckes, P.

    2016-01-01

    attribution results obtained using the CMB (chemical mass balance) model indicate that emissions from motor vehicle exhausts are the most important, accounting for the 64 % of the PM2.5, followed by meat-cooking operations with 31 % The vegetative detritus and biomass burning had the smallest contribution (2.2 % of the PM2.5). To our knowledge, this is only the second study to explore the organic composition and source apportionment of fine organic aerosol based on molecular markers in Mexico and the first for the MMA. Particularly molecular marker were quantified by solvent extraction with dichloromethane, derivatization, and gas chromatography with mass spectrometry (GC/MS).

  9. Organic molecular compositions and temporal variations of summertime mountain aerosols over Mt. Tai, North China Plain

    Science.gov (United States)

    Fu, Pingqing; Kawamura, Kimitaka; Okuzawa, Kazuhiro; Aggarwal, Shankar Gopala; Wang, Gehui; Kanaya, Yugo; Wang, Zifa

    2008-10-01

    Total suspended particles (TSP) were collected at the summit of Mt. Tai (1534 m above sea level) on a daytime and nighttime basis during a summertime campaign (May-June 2006) and were characterized for organic molecular compositions using solvent extraction/derivatization and gas chromatography/mass spectrometry technique. The n-Alkanes, fatty acids, fatty alcohols, sugars, glycerol and polyacids, and phthalate esters were found as major organic compound classes, whereas lignin and resin products, sterols, aromatic acids, hopanes, and polycyclic aromatic hydrocarbons (PAHs) were detected as minor classes. Sugars (49.8-2115 ng m-3, average 640 ng m-3 in daytime; 18.1-4348 ng m-3, 799 ng m-3 in nighttime) were found to be the dominant compound class. Levoglucosan, a specific cellulose pyrolysis product, was detected as the most abundant single compound, followed by C28 fatty alcohol, diisobutyl and di-n-butyl phthalates, C29n-alkane, C16 and C28 fatty acids, and malic acid. By grouping organic compounds based on their sources, we found that emission of terrestrial plant waxes was the most significant source (30-34%) of the TSP, followed by biomass burning products (25-27%) (e.g., levoglucosan and lignin and resin products), soil resuspension (15-18%) due to agricultural activities, secondary oxidation products (8-10%), plastic emission (3-10%), marine/microbial sources (6%), and urban/industrial emissions from fossil fuel use (4%). However, low molecular weight dicarboxylic acids (such as oxalic acid) of photochemical origin were not included in this study. Malic acid was found to be much higher than those reported in the ground level, suggesting an enhanced photochemical production in the free troposphere over mountain areas. Temporal variations of biomass burning tracers (e.g., levoglucosan, galactosan, mannosan) and some higher plant wax derived compound classes suggested that there were two major (E1 and E2) and one minor (E3) biomass-burning events during this

  10. Org Areo Boreal Forest Sources, compositions and properties of newly formed and regional organic aerosol in a boreal forest during the Biogenic Aerosol: Effects on Clouds and Climate Campaign

    Energy Technology Data Exchange (ETDEWEB)

    Thornton, Joel A [Univ. of Washington, Seattle, WA (United States)

    2017-12-01

    The major goals of this project were to make unique measurements, as part of the DOE sponsored Biogenic Aerosol Effects on Clouds and Climate (BAECC) campaign, of the volatility and molecular composition of organic aerosol, as well as gas-phase concentrations of oxygenated organic compounds that interact and affect organic aerosol. In addition, we aimed to conduct a similar set of measurements as part of a collaborative set of environmental simulation chamber experiments at PNNL, the aim of which was to simulate the atmospheric oxidation of key biogenic volatile organic compounds (BVOC) and study the associated formation and evolution of secondary organic aerosol (SOA). The target BVOC were a set of monoterpenes, isoprene, and related intermediates such as IEPOX. The ultimate goal of such measurements are to develop a more detailed mechanistic understanding of the sensitivity of SOA mass formation and lifetime to precursor and environmental conditions. Molecular composition and direct volatility measurements provide robust tracers of chemical processing and properties. As such, meeting these goals will allow for stronger constraints on the types of processes and their fundamental descriptions needed to simulate aerosol particle number and size, and cloud nucleating ability in regional and global earth system models.

  11. Aerosol concentrations and composition in the North Pacific marine boundary layer

    Science.gov (United States)

    Choi, Yongjoo; Rhee, Tae Siek; Collett, Jeffrey L.; Park, Taehyun; Park, Seung-Myung; Seo, Beom-Keun; Park, Gyutae; Park, Keyhong; Lee, Taehyoung

    2017-12-01

    Ship-borne measurements of inorganic and organic aerosols, including methanesulfonic acid (MSA), were conducted over the Northern Pacific using a High Resolution Time of Flight Aerosol Mass Spectrometer (AMS). This study, conducted aboard the Korean ice breaker R/V Araon, was part of the SHIP-borne Pole-to-Pole Observations (SHIPPO) project. Based on air mass source region, the cruise track could be divided into five sections. Overall, the South Asia and Northern Japan ship transects showed higher aerosol concentrations due to continental pollution and biomass burning sources, respectively. In all five regions, the average mass concentrations of sulfate and organic aerosols (OA) were much higher than concentrations of nitrate and ammonium. Positive matrix factorization (PMF) analysis distinguished two organic aerosol factors as hydrocarbon-like and oxidized OA (HOA and OOA). HOA peaked in South Asia under the influence of anthropogenic pollution source areas, such as China and Korea, and generally decreased with increasing latitude across the full study region. OOA concentrations peaked in Northern Japan near the Tsugaru Strait and appear to reflect fine particle contributions from biomass burning. The mean HOA concentration in the clean marine area (Aleutian Island to Siberia) was 0.06 μg/m3 and comprised approximately 8% of the OA mass fraction. The highest MSA concentrations peaked in the Aleutian Islands at nearly 15 μg/m3, suggesting influence from higher dimethyl sulfide (DMS) emissions resulting from biological nutrient uptake during summer. The MSA/sulfate ratio, an indicator of the relative fine particle contributions of DMS and anthropogenic sources, revealed a sharp gradient as the ship approached the clean marine areas where the dominance of DMS increased. The patterns in OOA, HOA, and MSA concentrations found in this study provide a better understanding of the characteristics of inorganic and organic aerosols in the Northern Pacific Ocean.

  12. Modelling the formation and composition of secondary organic aerosol from α- and β-pinene ozonolysis using MCM v3

    Directory of Open Access Journals (Sweden)

    M. E. Jenkin

    2004-01-01

    Full Text Available The formation and detailed composition of secondary organic aerosol (SOA from the gas phase ozonolysis of α- and β-pinene has been simulated using the Master Chemical Mechanism version 3 (MCM v3, coupled with a representation of gas-to-aerosol transfer of semivolatile and involatile oxygenated products. A kinetics representation, based on equilibrium absorptive partitioning of ca. 200 semivolatile products, was found to provide an acceptable description of the final mass concentrations observed in a number of reported laboratory and chamber experiments, provided partitioning coefficients were increased by about two orders of magnitude over those defined on the basis of estimated vapour pressures. This adjustment is believed to be due, at least partially, to the effect of condensed phase association reactions of the partitioning products. Even with this adjustment, the simulated initial formation of SOA was delayed relative to that observed, implying the requirement for the formation of species of much lower volatility to initiate SOA formation. The inclusion of a simplified representation of the formation and gas-to-aerosol transfer of involatile dimers of 22 bi- and multifunctional carboxylic acids (in addition to the absorptive partitioning mechanism allowed a much improved description of SOA formation for a wide range of conditions. The simulated SOA composition recreates certain features of the product distributions observed in a number of experimental studies, but implies an important role for multifunctional products containing hydroperoxy groups (i.e. hydroperoxides. This is particularly the case for experiments in which 2-butanol is used to scavenge OH radicals, because [HO2]/[RO2] ratios are elevated in such systems. The optimized mechanism is used to calculate SOA yields from α- and β-pinene ozonolysis in the presence and absence of OH scavengers, and as a function of temperature.

  13. Organic Aerosol Composition and Sources in Pasadena, California during the 2010 CalNex Campaign

    Science.gov (United States)

    Organic aerosols (OA) in Pasadena are characterized using multiple measurements from the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign. Five OA components are identified using positive matrix factorization including hydrocarbon-like OA (HOA) ...

  14. Aerosol assisted synthesis of hierarchical tin–carbon composites and their application as lithium battery anode materials

    KAUST Repository

    Guo, Juchen

    2013-01-01

    We report a method for synthesizing hierarchically structured tin-carbon (Sn-C) composites via aerosol spray pyrolysis. In this method, an aqueous precursor solution containing tin(ii) chloride and sucrose is atomized, and the resultant aerosol droplets carried by an inert gas are pyrolyzed in a high-temperature tubular furnace. Owing to the unique combination of high reaction temperature and short reaction time, this method is able to achieve a hetero-structure in which small Sn particles (15 nm) are uniformly embedded in a secondary carbon particle. This procedure allows the size and size distribution of the primary Sn particles to be tuned, as well as control over the size of the secondary carbon particles by addition of polymeric surfactant in the precursor solution. When evaluated as anode materials for lithium-ion batteries, the resultant Sn-C composites demonstrate attractive electrochemical performance in terms of overall capacity, electrochemical stability, and coulombic efficiency. © 2013 The Royal Society of Chemistry.

  15. Evaluation of the performance of four chemical transport models in predicting the aerosol chemical composition in Europe in 2005

    Directory of Open Access Journals (Sweden)

    M. Prank

    2016-05-01

    Full Text Available Four regional chemistry transport models were applied to simulate the concentration and composition of particulate matter (PM in Europe for 2005 with horizontal resolution  ∼  20 km. The modelled concentrations were compared with the measurements of PM chemical composition by the European Monitoring and Evaluation Programme (EMEP monitoring network. All models systematically underestimated PM10 and PM2.5 by 10–60 %, depending on the model and the season of the year, when the calculated dry PM mass was compared with the measurements. The average water content at laboratory conditions was estimated between 5 and 20 % for PM2.5 and between 10 and 25 % for PM10. For majority of the PM chemical components, the relative underestimation was smaller than it was for total PM, exceptions being the carbonaceous particles and mineral dust. Some species, such as sea salt and NO3−, were overpredicted by the models. There were notable differences between the models' predictions of the seasonal variations of PM, mainly attributable to different treatments or omission of some source categories and aerosol processes. Benzo(apyrene concentrations were overestimated by all the models over the whole year. The study stresses the importance of improving the models' skill in simulating mineral dust and carbonaceous compounds, necessity for high-quality emissions from wildland fires, as well as the need for an explicit consideration of aerosol water content in model–measurement comparison.

  16. Clouds and aerosols in Puerto Rico ─ a new evaluation

    Directory of Open Access Journals (Sweden)

    U. Dusek

    2008-03-01

    Full Text Available The influence of aerosols, both natural and anthropogenic, remains a major area of uncertainty when predicting the properties and behaviour of clouds and their influence on climate. In an attempt to better understand warm cloud formation in a tropical marine environment, a period of intensive measurements took place in December 2004 in Puerto Rico, using some of the latest developments in online instrumentation such as aerosol mass spectrometers, cloud condensation nuclei counters and a hygroscopicity tandem differential mobility analyser. Simultaneous online measurements of aerosol size distributions, composition, hygroscopicity and optical properties were made near the lighthouse of Cape San Juan in the north-eastern corner of the island and at the top of East Peak mountain (1040 m a.s.l., the two sites separated by 17 km. Additional measurements of the cloud droplet residual and interstitial aerosol properties were made at the mountain site, accompanied by measurements of cloud droplet size distributions, liquid water content and the chemical composition of cloud and rain water samples. Both aerosol composition and cloud properties were found to be sensitive to wind sector. Air from the east-northeast (ENE was mostly free of anthropogenic influences, the submicron fraction being mainly composed of non-sea salt sulphate, while that from the east-southeast (ESE was found to be moderately influenced by populated islands upwind, adding smaller (<100 nm, externally mixed, carbonaceous particles to the aerosol that increased the number concentrations by over a factor of 3. This change in composition was also accompanied with a reduction in the measured hygroscopicity and fractional cloud activation potential of the aerosol. At the mountain site, the average cloud droplet concentrations increased from 193 to 519 cm−3, median volume diameter decreased from 20 to 14 μm and the liquid water content increased from 0.24 to 0.31 g m−3 when the winds

  17. Size-segregated aerosol in a hot-spot pollution urban area: Chemical composition and three-way source apportionment.

    Science.gov (United States)

    Bernardoni, V; Elser, M; Valli, G; Valentini, S; Bigi, A; Fermo, P; Piazzalunga, A; Vecchi, R

    2017-08-24

    In this work, a comprehensive characterisation and source apportionment of size-segregated aerosol collected using a multistage cascade impactor was performed. The samples were collected during wintertime in Milan (Italy), which is located in the Po Valley, one of the main pollution hot-spot areas in Europe. For every sampling, size-segregated mass concentration, elemental and ionic composition, and levoglucosan concentration were determined. Size-segregated data were inverted using the program MICRON to identify and quantify modal contributions of all the measured components. The detailed chemical characterisation allowed the application of a three-way (3-D) receptor model (implemented using Multilinear Engine) for size-segregated source apportionment and chemical profiles identification. It is noteworthy that - as far as we know - this is the first time that three-way source apportionment is attempted using data of aerosol collected by traditional cascade impactors. Seven factors were identified: wood burning, industry, resuspended dust, regional aerosol, construction works, traffic 1, and traffic 2. Further insights into size-segregated factor profiles suggested that the traffic 1 factor can be associated to diesel vehicles and traffic 2 to gasoline vehicles. The regional aerosol factor resulted to be the main contributor (nearly 50%) to the droplet mode (accumulation sub-mode with modal diameter in the range 0.5-1 μm), whereas the overall contribution from the two factors related to traffic was the most important one in the other size modes (34-41%). The results showed that applying a 3-D receptor model to size-segregated samples allows identifying factors of local and regional origin while receptor modelling on integrated PM fractions usually singles out factors characterised by primary (e.g. industry, traffic, soil dust) and secondary (e.g. ammonium sulphate and nitrate) origin. Furthermore, the results suggested that the information on size

  18. Real-Time Investigation of Chemical Compositions and Hygroscopic Properties of Aerosols Generated from NaCl and Malonic Acid Mixture Solutions Using in Situ Raman Microspectrometry.

    Science.gov (United States)

    Li, Xue; Gupta, Dhrubajyoti; Lee, Jisoo; Park, Geonhee; Ro, Chul-Un

    2017-01-03

    Recently, ambient sea spray aerosols (SSAs) have been reported to undergo reactions with dicarboxylic acids (DCAs). Several studies have examined the hygroscopic behavior and chemical reactivity of aerosols generated from NaCl-DCA mixture solutions, but the results have varied, especially for the NaCl-malonic acid (NaCl-MA) mixture system. In this work, in situ Raman microspectrometry (RMS) was used to simultaneously monitor the change in chemical composition, size, and phase as a function of the relative humidity, for individual aerosols generated from NaCl-MA solutions, during two hygroscopic measurement cycles, which were performed first through the dehydration process, followed by a humidification process, in each cycle. In situ RMS analysis for the aerosols showed that the chemical reaction between NaCl and MA occurred rapidly in the time scale of 1 h and considerably in the aqueous phase, mostly during the first dehydration process, and the chemical reaction occurs more rapidly when MA is more enriched in the aerosols. For example, the reaction between NaCl and MA for aerosols generated from solutions of NaCl:MA = 2:1 and 1:2 occurred by 81% and 100% at RH = 42% and 45%, respectively, during the first dehydration process. The aerosols generated from the solution of NaCl:MA = 2:1 revealed single efflorescence and deliquescence transitions repeatedly during two hygroscopic cycles. The aerosols from NaCl:MA = 1:1 and 1:2 solutions showed just an efflorescence transition during the first dehydration process and no efflorescence and deliquescence transition during the hygroscopic cycles, respectively. The observed different hygroscopic behavior was due to the different contents of NaCl, MA, and monosodium malonate in the aerosols, which were monitored real-time by in situ RMS.

  19. Complementary online aerosol mass spectrometry and offline FT-IR spectroscopy measurements: Prospects and challenges for the analysis of anthropogenic aerosol particle emissions

    Science.gov (United States)

    Faber, Peter; Drewnick, Frank; Bierl, Reinhard; Borrmann, Stephan

    2017-10-01

    The aerosol mass spectrometer (AMS) is well established in investigating highly time-resolved dynamics of submicron aerosol chemical composition including organic aerosol (OA). However, interpretation of mass spectra on molecular level is limited due to strong fragmentation of organic substances and potential reactions inside the AMS ion chamber. Results from complementary filter-based FT-IR absorption measurements were used to explain features in high-resolution AMS mass spectra of different types of OA (e.g. cooking OA, cigarette smoking OA, wood burning OA). Using this approach some AMS fragment ions were validated in this study as appropriate and rather specific markers for a certain class of organic compounds for all particle types under investigation. These markers can therefore be used to get deeper insights in the chemical composition of OA based on AMS mass spectra in upcoming studies. However, the specificity of other fragment ions such as C2H4O2+ (m/z 60.02114) remains ambiguous. In such cases, complementary FT-IR measurements allow the interpretation of highly time-resolved AMS mass spectra at the level of molecular functional groups. Furthermore, this study discusses the challenges in reducing inorganic interferences (e.g. from water and ammonium salts) in FT-IR spectra of atmospheric aerosols to decrease spectral uncertainties for better comparisons and, thus, to get more robust results.

  20. Tropospheric Aerosols

    Science.gov (United States)

    Buseck, P. R.; Schwartz, S. E.

    2003-12-01

    It is widely believed that "On a clear day you can see forever," as proclaimed in the 1965 Broadway musical of the same name. While an admittedly beautiful thought, we all know that this concept is only figurative. Aside from Earth's curvature and Rayleigh scattering by air molecules, aerosols - colloidal suspensions of solid or liquid particles in a gas - limit our vision. Even on the clearest day, there are billions of aerosol particles per cubic meter of air.Atmospheric aerosols are commonly referred to as smoke, dust, haze, and smog, terms that are loosely reflective of their origin and composition. Aerosol particles have arisen naturally for eons from sea spray, volcanic emissions, wind entrainment of mineral dust, wildfires, and gas-to-particle conversion of hydrocarbons from plants and dimethylsulfide from the oceans. However, over the industrial period, the natural background aerosol has been greatly augmented by anthropogenic contributions, i.e., those produced by human activities. One manifestation of this impact is reduced visibility (Figure 1). Thus, perhaps more than in other realms of geochemistry, when considering the composition of the troposphere one must consider the effects of these activities. The atmosphere has become a reservoir for vast quantities of anthropogenic emissions that exert important perturbations on it and on the planetary ecosystem in general. Consequently, much recent research focuses on the effects of human activities on the atmosphere and, through them, on the environment and Earth's climate. For these reasons consideration of the geochemistry of the atmosphere, and of atmospheric aerosols in particular, must include the effects of human activities. (201K)Figure 1. Impairment of visibility by aerosols. Photographs at Yosemite National Park, California, USA. (a) Low aerosol concentration (particulate matter of aerodynamic diameter less than 2.5 μm, PM2.5=0.3 μg m-3; particulate matter of aerodynamic diameter less than 10

  1. Origins and composition of fine atmospheric carbonaceous aerosol in the Sierra Nevada Mountains, California

    Directory of Open Access Journals (Sweden)

    D. R. Worton

    2011-10-01

    Full Text Available In this paper we report chemically resolved measurements of organic aerosol (OA and related tracers during the Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX at the Blodgett Forest Research Station, California from 15 August–10 October 2007. OA contributed the majority of the mass to the fine atmospheric particles and was predominately oxygenated (OOA. The highest concentrations of OA were during sporadic wildfire influence when aged plumes were impacting the site. In situ measurements of particle phase molecular markers were dominated by secondary compounds and along with gas phase compounds could be categorized into six factors or sources: (1 aged biomass burning emissions and oxidized urban emissions, (2 oxidized urban emissions (3 oxidation products of monoterpene emissions, (4 monoterpene emissions, (5 anthropogenic emissions and (6 local methyl chavicol emissions and oxidation products. There were multiple biogenic components that contributed to OA at this site whose contributions varied diurnally, seasonally and in response to changing meteorological conditions, e.g. temperature and precipitation events. Concentrations of isoprene oxidation products were larger when temperatures were higher during the first half of the campaign (15 August–12 September due to more substantial emissions of isoprene and enhanced photochemistry. The oxidation of methyl chavicol, an oxygenated terpene emitted by ponderosa pine trees, contributed similarly to OA throughout the campaign. In contrast, the abundances of monoterpene oxidation products in the particle phase were greater during the cooler conditions in the latter half of the campaign (13 September–10 October, even though emissions of the precursors were lower, although the mechanism is not known. OA was correlated with the anthropogenic tracers 2-propyl nitrate and carbon monoxide (CO, consistent with previous observations, while being comprised of mostly non-fossil carbon

  2. Organic Aerosol Volatility Parameterizations and Their Impact on Atmospheric Composition and Climate

    Science.gov (United States)

    Tsigaridis, Konsta; Bauer, Susanne E.

    2015-01-01

    Despite their importance and ubiquity in the atmosphere, organic aerosols are still very poorly parameterized in global models. This can be explained by two reasons: first, a very large number of unconstrained parameters are involved in accurate parameterizations, and second, a detailed description of semi-volatile organics is computationally very expensive. Even organic aerosol properties that are known to play a major role in the atmosphere, namely volatility and aging, are poorly resolved in global models, if at all. Studies with different models and different parameterizations have not been conclusive on whether the additional complexity improves model simulations, but the added diversity of the different host models used adds an unnecessary degree of variability in the evaluation of results that obscures solid conclusions.

  3. Composition and sources of organic tracers in aerosol particles of industrial central India

    Science.gov (United States)

    Giri, Basant; Patel, Khageshwar S.; Jaiswal, Nitin K.; Sharma, Saroj; Ambade, Balram; Wang, Wentao; Simonich, Staci L. Massey; Simoneit, Bernd R. T.

    2013-02-01

    Organic aerosols are important atmospheric components, and their formation and sources represent important aspects of urban air quality and health effects. Asia, including India, is the largest global source of aerosol particles due to regional natural advection (e.g. desert and soil dust) and anthropogenic activities (e.g. emissions from traffic, industry and burning of coal, biomass and agricultural waste) that generate vast amounts of particulate matter (PM) significantly contributing to climate change. This article reports on the distributions, concentrations, and sources of organic compounds (i.e., alkanes, carboxylic acids, carbonyl compounds, alcohols, plasticizers, PAHs, biomarkers) of PM in the ambient atmosphere of an extensively industrialized area of central India (Raipur, Chhattisgarh, a coal mega-burning region). The dominant components are emissions from fossil fuel utilization, burning of biomass and plastics, and fugitive sources. Speciation and variations of potential new tracer compounds identified are also described.

  4. Number size distributions and seasonality of submicron particles in Europe 2008-2009

    Science.gov (United States)

    Asmi, A.; Wiedensohler, A.; Laj, P.; Fjaeraa, A.-M.; Sellegri, K.; Birmili, W.; Weingartner, E.; Baltensperger, U.; Zdimal, V.; Zikova, N.; Putaud, J.-P.; Marinoni, A.; Tunved, P.; Hansson, H.-C.; Fiebig, M.; Kivekäs, N.; Lihavainen, H.; Asmi, E.; Ulevicius, V.; Aalto, P. P.; Swietlicki, E.; Kristensson, A.; Mihalopoulos, N.; Kalivitis, N.; Kalapov, I.; Kiss, G.; de Leeuw, G.; Henzing, B.; Harrison, R. M.; Beddows, D.; O'Dowd, C.; Jennings, S. G.; Flentje, H.; Weinhold, K.; Meinhardt, F.; Ries, L.; Kulmala, M.

    2011-06-01

    Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the

  5. Production Mechanisms, Number Concentration, Size Distribution. Chemical Composition, and Optical Properties of Sea Spray Aerosols

    Science.gov (United States)

    Meskhidze, Nicholas; Petters, Markus; Tsigaridis, Kostas; Bates. Tim; O'Dowd, Colin; Reid, Jeff; Lewis, Ernie R.; Gantt, Brett; Anguelova, Magdalena D.; Bhave, Prakash V.; hide

    2013-01-01

    Over forty scientists from six countries convened in Raleigh, NC on June 4-6 2012 to review the status and prospects of sea spray aerosol research. Participants were researchers from the oceanography and atmospheric science communities, including academia, private industry, and government agencies. The recommendations from the working groups are summarized in a science prioritization matrix that is meant to prioritize the research agenda and identify areas of investigation by the magnitude of their impact on proposed science questions. Str

  6. Global and Regional Impacts of HONO on the Chemical Composition of Clouds and Aerosols

    Science.gov (United States)

    Elshorbany, Y. F.; Crutzen, P. J.; Steil, B.; Pozzer, A.; Tost, H.; Lelieveld, J.

    2014-01-01

    Recently, realistic simulation of nitrous acid (HONO) based on the HONO / NOx ratio of 0.02 was found to have a significant impact on the global budgets of HOx (OH + HO2) and gas phase oxidation products in polluted regions, especially in winter when other photolytic sources are of minor importance. It has been reported that chemistry-transport models underestimate sulphate concentrations, mostly during winter. Here we show that simulating realistic HONO levels can significantly enhance aerosol sulphate (S(VI)) due to the increased formation of H2SO4. Even though in-cloud aqueous phase oxidation of dissolved SO2 (S(IV)) is the main source of S(VI), it appears that HONO related enhancement of H2O2 does not significantly affect sulphate because of the predominantly S(IV) limited conditions, except over eastern Asia. Nitrate is also increased via enhanced gaseous HNO3 formation and N2O5 hydrolysis on aerosol particles. Ammonium nitrate is enhanced in ammonia-rich regions but not under ammonia-limited conditions. Furthermore, particle number concentrations are also higher, accompanied by the transfer from hydrophobic to hydrophilic aerosol modes. This implies a significant impact on the particle lifetime and cloud nucleating properties. The HONO induced enhancements of all species studied are relatively strong in winter though negligible in summer. Simulating realistic HONO levels is found to improve the model measurement agreement of sulphate aerosols, most apparent over the US. Our results underscore the importance of HONO for the atmospheric oxidizing capacity and corroborate the central role of cloud chemical processing in S(IV) formation

  7. Single Usage of a Kitchen Degreaser Can Alter Indoor Aerosol Composition for Days.

    Science.gov (United States)

    Schwarz, Jaroslav; Makeš, Otakar; Ondráček, Jakub; Cusack, Michael; Talbot, Nicholas; Vodička, Petr; Kubelová, Lucie; Ždímal, Vladimír

    2017-06-06

    To the best of our knowledge, this study represents the first observation of multiday persistence of an indoor aerosol transformation linked to a kitchen degreaser containing monoethanol amine (MEA). MEA remaining on the cleaned surfaces and on a wiping paper towel in a trash can was able to transform ammonium sulfate and ammonium nitrate into (MEA) 2 SO 4 and (MEA)NO 3 . This influence persisted for at least 60 h despite a high average ventilation rate. The influence was observed using both offline (filters, impactors, and ion chromatography analysis) and online (compact time-of-flight aerosol mass spectrometer) techniques. Substitution of ammonia in ammonium salts was observed not only in aerosol but also in particles deposited on a filter before the release of MEA. The similar influence of other amines is expected based on literature data. This influence represents a new pathway for MEA exposure of people in an indoor environment. The stabilizing effect on indoor nitrate also causes higher indoor exposure to fine nitrates.

  8. Formation of Oxidized Organic Aerosol (OOA) through Fog Processing in the Po Valley

    Science.gov (United States)

    Gilardoni, S.; Paglione, M.; Rinaldi, M.; Giulianelli, L.; Massoli, P.; Hillamo, R. E.; Carbone, S.; Lanconelli, C.; Laaksonen, A. J.; Russell, L. M.; Poluzzi, V.; Fuzzi, S.; Facchini, C.

    2014-12-01

    Aqueous phase chemistry might be responsible for the formation of a significant fraction of the organic aerosol (OA) observed in the atmosphere, and could explain some of the discrepancies between OA concentration and properties predicted by models and observed in the environment. Aerosol - fog interaction and its effect on submicron aerosol properties were investigated in the Po Valley (northern Italy) during fall 2011, in the framework of the Supersite project (ARPA Emilia Romagna). Composition and physical properties of submicron aerosol were measured online by a High Resolution- Time of Flight - Aerosol Mass Spectrometer (HR-TOF-AMS), a Soot Photometer - Aerosol Mass Spectrometer (SP-AMS), and a Tandem Differential Mobility Particle Sizer (TDMPS). Organic functional group analysis was performed off-line by Hydrogen - Nuclear Magnetic Resonance (H-NMR) spectrometry and by Fourier Transform Infrared (FTIR) spectrometry. Aerosol absorption, scattering, and total extinction were measured simultaneously with a Particle Soot Absorption Photometer (PSAP), a Nephelometer, and a Cavity Attenuated Phase Shift Spectrometer particle extinction monitor (CAPS PMex), respectively. Water-soluble organic carbon in fog-water was characterized off-line by HR-TOF-AMS. Fourteen distinct fog events were observed. Fog dissipation left behind an aerosol enriched in particles larger than 400 nm, typical of fog and cloud processing, and dominated by secondary species, including ammonium nitrate, ammonium sulfate and oxidized OA (OOA). Source apportionment of OA allowed us to identify OOA as the difference between total OA and primary OA (hydrocarbon like OA and biomass burning OA). The formation of OOA through fog processing is proved by the correlation of OOA concentration with hydroxyl methyl sulfonate signal and by the similarity of OOA spectra with organic mass spectra obtained by re-aerosolization of fog water samples. The oxygen to carbon ratio and the hydrogen to carbon ratio of

  9. Aerosol composition and source apportionment in the Mexico City Metropolitan Area with PIXE/PESA/STIM and multivariate analysis

    Directory of Open Access Journals (Sweden)

    K. S. Johnson

    2006-01-01

    Full Text Available Aerosols play an important role in the atmosphere but are poorly characterized, particularly in urban areas like the Mexico City Metropolitan Area (MCMA. The chemical composition of urban particles must be known to assess their effects on the environment, and specific particulate emissions sources should be identified to establish effective pollution control standards. For these reasons, samples of particulate matter ≤2.5 μm (PM2.5 were collected during the MCMA-2003 Field Campaign for elemental and multivariate analyses. Proton-Induced X-ray Emission (PIXE, Proton-Elastic Scattering Analysis (PESA and Scanning Transmission Ion Microscopy (STIM measurements were done to determine concentrations of 19 elements from Na to Pb, hydrogen, and total mass, respectively. The most abundant elements from PIXE analysis were S, Si, K, Fe, Ca, and Al, while the major emissions sources associated with these elements were industry, wind-blown soil, and biomass burning. Wind trajectories suggest that metals associated with industrial emissions came from northern areas of the city whereas soil aerosols came from the southwest and increased in concentration during dry conditions. Elemental markers for fuel oil combustion, V and Ni, correlated with a large SO2 plume to suggest an anthropogenic, rather than volcanic, emissions source. By subtracting major components of soil and sulfates determined by PIXE analysis from STIM total mass measurements, we estimate that approximately 50% of non-volatile PM2.5 consisted of carbonaceous material.

  10. Wind speed dependent size-resolved parameterization for the organic mass fraction of sea spray aerosol

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    B. Gantt

    2011-08-01

    Full Text Available For oceans to be a significant source of primary organic aerosol (POA, sea spray aerosol (SSA must be highly enriched with organics relative to the bulk seawater. We propose that organic enrichment at the air-sea interface, chemical composition of seawater, and the aerosol size are three main parameters controlling the organic mass fraction of sea spray aerosol (OMSSA. To test this hypothesis, we developed a new marine POA emission function based on a conceptual relationship between the organic enrichment at the air-sea interface and surface wind speed. The resulting parameterization is explored using aerosol chemical composition and surface wind speed from Atlantic and Pacific coastal stations, and satellite-derived ocean concentrations of chlorophyll-a, dissolved organic carbon, and particulate organic carbon. Of all the parameters examined, a multi-variable logistic regression revealed that the combination of 10 m wind speed and surface chlorophyll-a concentration ([Chl-a] are the most consistent predictors of OMSSA. This relationship, combined with the published aerosol size dependence of OMSSA, resulted in a new parameterization for the organic mass fraction of SSA. Global emissions of marine POA are investigated here by applying this newly-developed relationship to existing sea spray emission functions, satellite-derived [Chl-a], and modeled 10 m winds. Analysis of model simulations shows that global annual submicron marine organic emission associated with sea spray is estimated to be from 2.8 to 5.6 Tg C yr−1. This study provides additional evidence that marine primary organic aerosols are a globally significant source of organics in the atmosphere.

  11. Aerosol particle measurements at three stationary sites in the megacity of Paris during summer 2009: meteorology and air mass origin dominate aerosol particle composition and size distribution

    National Research Council Canada - National Science Library

    Freutel, F; Schneider, J; Drewnick, F; von der Weiden-Reinmüller, S.-L; Crippa, M; Prévôt, A. S. H; Baltensperger, U; Poulain, L; Wiedensohler, A; Sciare, J; Sarda-Estève, R; Burkhart, J. F; Eckhardt, S; Stohl, A; Gros, V; Colomb, A; Michoud, V; Doussin, J. F; Borbon, A; Haeffelin, M; Morille, Y; Beekmann, M; Borrmann, S

    2013-01-01

    .... It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol...

  12. Composition and sources of carbonaceous aerosols in Northern Europe during winter

    Science.gov (United States)

    Glasius, M.; Hansen, A. M. K.; Claeys, M.; Henzing, J. S.; Jedynska, A. D.; Kasper-Giebl, A.; Kistler, M.; Kristensen, K.; Martinsson, J.; Maenhaut, W.; Nøjgaard, J. K.; Spindler, G.; Stenström, K. E.; Swietlicki, E.; Szidat, S.; Simpson, D.; Yttri, K. E.

    2018-01-01

    Sources of elemental carbon (EC) and organic carbon (OC) in atmospheric aerosols (carbonaceous aerosols) were investigated by collection of weekly aerosol filter samples at six background sites in Northern Europe (Birkenes, Norway; Vavihill, Sweden; Risoe, Denmark; Cabauw and Rotterdam in The Netherlands; Melpitz, Germany) during winter 2013. Analysis of 14C and a set of molecular tracers were used to constrain the sources of EC and OC. During the four-week campaign, most sites (in particular those in Germany and The Netherlands) were affected by an episode during the first two weeks with high concentrations of aerosol, as continental air masses were transported westward. The analysis results showed a clear, increasing north to south gradient for most molecular tracers. Total carbon (TC = OC + EC) at Birkenes showed an average concentration of 0.5 ± 0.3 μg C m-3, whereas the average concentration at Melpitz was 6.0 ± 4.3 μg C m-3. One weekly mean TC concentration as high as 11 μg C m-3 was observed at Melpitz. Average levoglucosan concentrations varied by an order of magnitude from 25 ± 13 ng m-3 (Birkenes) to 249 ± 13 ng m-3 (Melpitz), while concentrations of tracers of fungal spores (arabitol and mannitol) and vegetative debris (cellulose) were very low, showing a minor influence of primary biological aerosol particles during the North European winter. The fraction of modern carbon generally varied from 0.57 (Melpitz) to 0.91 (Birkenes), showing an opposite trend compared to the molecular tracers and TC. Total concentrations of 10 biogenic and anthropogenic carboxylic acids, mainly of secondary origin, were 4-53 ng m-3, with the lowest concentrations observed at Birkenes and the highest at Melpitz. However, the highest relative concentrations of carboxylic acids (normalized to TC) were observed at the most northern sites. Levels of organosulphates and nitrooxy organosulphates varied more than two orders of magnitude, from 2 to 414 ng m-3, between

  13. Chemical composition, source, and process of urban aerosols during winter haze formation in Northeast China.

    Science.gov (United States)

    Zhang, Jian; Liu, Lei; Wang, Yuanyuan; Ren, Yong; Wang, Xin; Shi, Zongbo; Zhang, Daizhou; Che, Huizheng; Zhao, Hujia; Liu, Yanfei; Niu, Hongya; Chen, Jianmin; Zhang, Xiaoye; Lingaswamy, A P; Wang, Zifa; Li, Weijun

    2017-12-01

    The characteristics of aerosol particles have been poorly evaluated even though haze episodes frequently occur in winter in Northeast China. OC/EC analysis, ion chromatography, and transmission electron microscopy (TEM) were used to investigate the organic carbon (OC) and elemental carbon (EC), and soluble ions in PM 2.5 and the mixing state of individual particles during a severe wintertime haze episode in Northeast China. The organic matter (OM), NH 4 + , SO 4 2- , and NO 3 - concentrations in PM 2.5 were 89.5 μg/m 3 , 24.2 μg/m 3 , 28.1 μg/m 3 , and 32.8 μg/m 3 on the haze days, respectively. TEM observations further showed that over 80% of the haze particles contained primary organic aerosols (POAs). Based on a comparison of the data obtained during the haze formation, we generate the following synthetic model of the process: (1) Stable synoptic meteorological conditions drove the haze formation. (2) The early stage of haze formation (light or moderate haze) was mainly caused by the enrichment of POAs from coal burning for household heating and cooking. (3) High levels of secondary organic aerosols (SOAs), sulfates, and nitrates formation via heterogeneous reactions together with POAs accumulation promoted to the evolution from light or moderate to severe haze. Compared to the severe haze episodes over the North China Plain, the PM 2.5 in Northeast China analyzed in the present study contained similar sulfate, higher SOA, and lower nitrate contents. Our results suggest that most of the POAs and secondary particles were likely related to emissions from coal-burning residential stoves in rural outskirts and small boilers in urban areas. The inefficient burning of coal for household heating and cooking should be monitored during wintertime in Northeast China. Copyright © 2017 Elsevier Ltd. All rights reserved.

  14. Year-round records of bulk and size-segregated aerosol composition in central Antarctica (Concordia site – Part 1: Fractionation of sea-salt particles

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    M. Legrand

    2017-11-01

    Full Text Available Multiple year-round records of bulk and size-segregated composition of aerosol were obtained at the inland site of Concordia located at Dome C in East Antarctica. In parallel, sampling of acidic gases on denuder tubes was carried out to quantify the concentrations of HCl and HNO3 present in the gas phase. These time series are used to examine aerosol present over central Antarctica in terms of chloride depletion relative to sodium with respect to freshly emitted sea-salt aerosol as well as depletion of sulfate relative to sodium with respect to the composition of seawater. A depletion of chloride relative to sodium is observed over most of the year, reaching a maximum of  ∼ 20 ng m−3 in spring when there are still large sea-salt amounts and acidic components start to recover. The role of acidic sulfur aerosol and nitric acid in replacing chloride from sea-salt particles is here discussed. HCl is found to be around twice more abundant than the amount of chloride lost by sea-salt aerosol, suggesting that either HCl is more efficiently transported to Concordia than sea-salt aerosol or re-emission from the snow pack over the Antarctic plateau represents an additional significant HCl source. The size-segregated composition of aerosol collected in winter (from 2006 to 2011 indicates a mean sulfate to sodium ratio of sea-salt aerosol present over central Antarctica of 0.16 ± 0.05, suggesting that, on average, the sea-ice and open-ocean emissions equally contribute to sea-salt aerosol load of the inland Antarctic atmosphere. The temporal variability of the sulfate depletion relative to sodium was examined at the light of air mass backward trajectories, showing an overall decreasing trend of the ratio (i.e., a stronger sulfate depletion relative to sodium when air masses arriving at Dome C had traveled a longer time over sea ice than over open ocean. The findings are shown to be useful to discuss sea-salt ice records extracted at deep

  15. Aerosol microphysics simulations of the Mt.~Pinatubo eruption with the UM-UKCA composition-climate model

    National Research Council Canada - National Science Library

    Dhomse, S. S; Emmerson, K. M; Mann, G. W; Bellouin, N; Carslaw, K. S; Chipperfield, M. P; Hommel, R; Abraham, N. L; Telford, P; Braesicke, P; Dalvi, M; Johnson, C. E; O'Connor, F; Morgenstern, O; Pyle, J. A; Deshler, T; Zawodny, J. M; Thomason, L. W

    2014-01-01

    We use a stratosphere–troposphere composition–climate model with interactive sulfur chemistry and aerosol microphysics, to investigate the effect of the 1991 Mount Pinatubo eruption on stratospheric aerosol properties...

  16. Changes in background aerosol composition in Finland during polluted and clean periods studied by TEM/EDX individual particle analysis

    Directory of Open Access Journals (Sweden)

    J. V. Niemi

    2006-01-01

    Full Text Available Aerosol samples were collected at a rural background site in southern Finland in May 2004 during pollution episode (PM1~16 µg m−3, backward air mass trajectories from south-east, intermediate period (PM1~5 µg m−3, backtrajectories from north-east and clean period (PM1~2 µg m−3, backtrajectories from north-west/north. The elemental composition, morphology and mixing state of individual aerosol particles in three size fractions were studied using transmission electron microscopy (TEM coupled with energy dispersive X-ray (EDX microanalyses. The TEM/EDX results were complemented with the size-segregated bulk chemical measurements of selected ions and organic and elemental carbon. Many of the particles in PM0.2–1 and PM1–3.3 size fractions were strongly internally mixed with S, C and/or N. The major particle types in PM0.2–1 samples were 1 soot and 2 (ammoniumsulphates and their mixtures with variable amounts of C, K, soot and/or other inclusions. Number proportions of those two particle groups in PM0.2–1 samples were 0–12% and 83–97%, respectively. During the pollution episode, the proportion of Ca-rich particles was very high (26–48% in the PM1–3.3 and PM3.3–11 samples, while the PM0.2–1 and PM1–3.3 samples contained elevated proportions of silicates (22–33%, metal oxides/hydroxides (1–9% and tar balls (1–4%. These aerosols originated mainly from polluted areas of Eastern Europe, and some open biomass burning smoke was also brought by long-range transport. During the clean period, when air masses arrived from the Arctic Ocean, PM1–3.3 samples contained mainly sea salt particles (67–89% with a variable rate of Cl substitution (mainly by NO3−. During the intermediate period, the PM1–3.3 sample contained porous (sponge-like Na-rich particles (35% with abundant S, K and O. They might originate from the burning of wood pulp wastes of paper industry. The proportion of biological particles and C-rich fragments

  17. Fatty acid composition analysis in polysorbate 80 with high performance liquid chromatography coupled to charged aerosol detection.

    Science.gov (United States)

    Ilko, David; Braun, Alexandra; Germershaus, Oliver; Meinel, Lorenz; Holzgrabe, Ulrike

    2015-08-01

    The fatty acid (FA) composition of polysorbate 80 (PS80), a sorbitan oleic acid ester copolymerized with about 20mole of ethylene oxide, is typically characterized by gas chromatography. Here, an alternative method was developed. After saponification with potassium hydroxide the FA fraction was collected with liquid-liquid extraction using methyl-tert-butyl ether. HPLC in combination with a Corona® charged aerosol detector (CAD) was applied for the separation and detection. The method was fully validated in terms of specificity, repeatability, limits of quantification, linearity, range, accuracy and robustness. The characterization of 16 different PS80 batches demonstrated variability regarding their FA composition, with e.g. the amount of oleic acid ranging from 67.8±0.7% to 96.6±1.4%. Furthermore, we identified petroselinic acid, a double-bond positional isomer to oleic acid in all batches, an FA not known to pharmacopoeias at present. In addition, 11-hydroxy-9-octadecenoic acid, an oxidation product of oleic acid was identified. Structure elucidation was performed by means of HPLC-MS/MS. In addition, the method was expanded to the evaluation of the free FAs. Having determined the entire FA composition, the acid value according to EP and USP can be calculated. Copyright © 2014 Elsevier B.V. All rights reserved.

  18. The physical and chemical characteristics of marine primary organic aerosol: a review

    Directory of Open Access Journals (Sweden)

    B. Gantt

    2013-04-01

    Full Text Available Knowledge of the physical characteristics and chemical composition of marine organic aerosols is needed for the quantification of their effects on solar radiation transfer and cloud processes. This review examines research pertinent to the chemical composition, size distribution, mixing state, emission mechanism, photochemical oxidation and climatic impact of marine primary organic aerosol (POA associated with sea-spray. Numerous measurements have shown that both the ambient mass concentration of marine POA and size-resolved organic mass fraction of sea-spray aerosol are related to surface ocean biological activity. Recent studies have also indicated that fine mode (smaller than 200 nm in diameter marine POA can have a size distribution independent from sea-salt, while coarse mode aerosols (larger than 1000 nm in diameter are more likely to be internally mixed with sea-salt. Modelling studies have estimated global submicron marine POA emission rates of ~10 ± 5 Tg yr−1, with a considerable fraction of these emissions occurring over regions most susceptible to aerosol perturbations. Climate studies have found that marine POA can cause large local increases in the cloud condensation nuclei concentration and have a non-negligible influence on model assessments of the anthropogenic aerosol forcing of climate. Despite these signs of climate-relevance, the source strength, chemical composition, mixing state, hygroscopicity, cloud droplet activation potential, atmospheric aging and removal of marine POA remain poorly quantified. Additional laboratory, field, and modelling studies focused on the chemistry, size distribution and mixing state of marine POA are needed to better understand and quantify their importance.

  19. Water soluble organic aerosols in the Colorado Rocky Mountains, USA: composition, sources and optical properties

    Science.gov (United States)

    Xie, Mingjie; Mladenov, Natalie; Williams, Mark W.; Neff, Jason C.; Wasswa, Joseph; Hannigan, Michael P.

    2016-12-01

    Atmospheric aerosols have been shown to be an important input of organic carbon and nutrients to alpine watersheds and influence biogeochemical processes in these remote settings. For many remote, high elevation watersheds, direct evidence of the sources of water soluble organic aerosols and their chemical and optical characteristics is lacking. Here, we show that the concentration of water soluble organic carbon (WSOC) in the total suspended particulate (TSP) load at a high elevation site in the Colorado Rocky Mountains was strongly correlated with UV absorbance at 254 nm (Abs254, r = 0.88 p 90% of OC on average. According to source apportionment analysis, biomass burning had the highest contribution (50.3%) to average WSOC concentration; SOA formation and motor vehicle emissions dominated the contribution to WSOC in the summer. The source apportionment and backward trajectory analysis results supported the notion that both wildfire and Colorado Front Range pollution sources contribute to the summertime OC peaks observed in wet deposition at high elevation sites in the Colorado Rocky Mountains. These findings have important implications for water quality in remote, high-elevation, mountain catchments considered to be our pristine reference sites.

  20. Investigating types and sources of organic aerosol in Rocky Mountain National Park using aerosol mass spectrometry

    Science.gov (United States)

    Schurman, M. I.; Lee, T.; Sun, Y.; Schichtel, B. A.; Kreidenweis, S. M.; Collett, J. L., Jr.

    2015-01-01

    The environmental impacts of atmospheric particles are highlighted in remote areas where visibility and ecosystem health can be degraded by even relatively low particle concentrations. Submicron particle size, composition, and source apportionment were explored at Rocky Mountain National Park using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer. This summer campaign found low average, but variable, particulate mass (PM) concentrations (max = 93.1 μg m-3, avg. = 5.13 ± 2.72 μg m-3) of which 75.2 ± 11.1% is organic. Low-volatility oxidized organic aerosol (LV-OOA, 39.3% of PM1 on average) identified using Positive Matrix Factorization appears to be mixed with ammonium sulfate (3.9% and 16.6% of mass, respectively), while semi-volatile OOA (27.6%) is correlated with ammonium nitrate (nitrate: 4.3%); concentrations of these mixtures are enhanced with upslope (SE) surface winds from the densely populated Front Range area, indicating the importance of transport. A local biomass burning organic aerosol (BBOA, 8.4%) source is suggested by mass spectral cellulose combustion markers (m/z 60 and 73) limited to brief, high-concentration, polydisperse events (suggesting fresh combustion), a diurnal maximum at 22:00 local standard time when campfires were set at adjacent summer camps, and association with surface winds consistent with local campfire locations. The particle characteristics determined here represent typical summertime conditions at the Rocky Mountain site based on comparison to ~10 years of meteorological, particle composition, and fire data.

  1. Instrument development and characterization of atmospheric aerosol physical properties through airborne measurement

    Science.gov (United States)

    Wang, Jian

    To increase the speed of submicron aerosol size distribution measurements, a mixing condensation nucleus counter (MCNC) has been developed. By carefully designing the mixing chamber and condenser, the response time of the MCNC was significantly reduced. Our experiments demonstrate that a differential mobility analyzer (DMA) coupled with the developed MCNC can measure complete aerosol size distributions in as little as 2 seconds. The effects of bends and elbows on the diffusional losses of particle in nanometer range were studied. The results show that the effect of bends and elbows on particle diffusion loss is significant, and for Reynolds number smaller than 250, the enhancement of diffusion losses due to bends and elbows is sensitive to both the relative orientations of the bends and elbows and the lengths of straight tubing between them. When the Reynolds number exceeds 250, the enhancement is insensitive to the actual flow configurations. Experimental results are presented, which can be used for design of aerosol flow systems at Reynolds number larger than 250. To minimize the airborne sampling bias, an advanced differential mobility analyzer (DMA) system for measuring submicron aerosol size distribution at ambient relative humidity, with special attention to implementation on aircraft, has been developed. The system includes an active RH controller, a cylindrical differential mobility analyzer (CDMA), and a condensation nucleus counter. A cascade controller maintains the RH inside the CDMA at ambient RH by actively adding or removing water vapor from the air stream. The flows are controlled with feedback PID controllers, which compensate for the variation of pressure as the aircraft changes altitude. During the ACE-Asia experiment, the above DMA system, together with an aerodynamic particle sizer (APS), was used to characterize aerosol size distributions in East Asia on board of CIRPAS Twin Otter aircraft. Besides providing the aerosol size characteristics

  2. Primary and secondary aerosols in Beijing in winter: sources, variations and processes

    Directory of Open Access Journals (Sweden)

    Y. Sun

    2016-07-01

    Full Text Available Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %, sulfate (15 % and nitrate (11 %. Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA factors from traffic, cooking, biomass burning (BBOA and coal combustion (CCOA emissions as well as two secondary OA (SOA factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %. Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 % and biomass burning emissions (18 %. BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93, and made a considerable contribution to OA in winter (9 %. An aqueous-phase-processed SOA (aq-OOA that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+ was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %. Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on

  3. Chemical and geochemical composition of spring-summer Arctic aerosol collected at Ny Alesund, Svalbard Islands.

    Science.gov (United States)

    Udisti, Roberto; Becagli, Silvia; Caiazzo, Laura; Cappelletti, David; Giardi, Fabio; Grotti, Marco; Lucarelli, Franco; Moroni, Beatrice; Nava, Silvia; Severi, Mirko; Traversi, Rita

    2017-04-01

    Since March 2010, spring-summer (usually March - September) campaigns were continuously carried out at the Italian Gruvebadet Observatory, Ny Alesund, Svalbard Island. Aerosol was sampled by PM10 (daily) and 4-stage (4-day resolution) collector devices and size distribution was evaluated at 10 min resolution in the range 10 nm - 20 um (106 size classes by a TSI SMPS-APS integrated system). Six-year (2010-2015) PM10 and size-segregated (>10, 10-2.5, 2.5-1, 10.1016/j.atmosenv.2016.04.002. A. Bazzano et al., "Long-range transport of atmospheric lead reaching Ny Alesund: inter-annual and seasonal variations of potential source areas". Atmos. Environ., 2016, 139, 11-19. http://dx.doi.org/10.1016/j.atmosenv.2016.05.026.

  4. Organic composition of carbonaceous aerosols in an aged prescribed fire plume

    Directory of Open Access Journals (Sweden)

    B. Yan

    2008-11-01

    Full Text Available Aged smoke from a prescribed fire (dominated by conifers impacted Atlanta, GA on 28 February 2007 and dramatically increased hourly ambient concentrations of PM2.5 and organic carbon (OC up to 140 and 72 μg m−3, respectively. It was estimated that over 1 million residents were exposed to the smoky air lasting from the late afternoon to midnight. To better understand the processes impacting the aging of fire plumes, a detailed chemical speciation of carbonaceous aerosols was conducted by gas chromatography/mass spectrometry (GC/MS analysis. Ambient concentrations of many organic species (levoglucosan, resin acids, retene, n-alkanes and n-alkanoic acids associated with wood burning emission were significantly elevated on the event day. Levoglucosan increased by a factor of 10, while hopanes, steranes, cholesterol and major polycyclic aromatic hydrocarbons (PAHs did not show obvious increases. Strong odd over even carbon number predominance was found for n-alkanes versus even over odd predominance for n-alkanoic acids. Alteration of resin acids during transport from burning sites to monitors is suggested by the observations. Our study also suggests that large quantities of biogenic volatile organic compounds (VOCs and semivolatile organic compounds (SVOCs were released both as products of combustion and unburned vegetation heated by the fire. Higher leaf temperature can stimulate biogenic VOC and SVOC emissions, which enhanced formation of secondary organic aerosols (SOA in the atmosphere. This is supported by elevated ambient concentrations of secondary organic tracers (dicarboxylic acids, 2-methyltetrols, pinonic acid and pinic acid. An approximate source profile was built for the aged fire plume to help better understand evolution of wood smoke emission and for use in source impact assessment.

  5. Phase, composition, and growth mechanism for secondary organic aerosol from the ozonolysis of α-cedrene

    Directory of Open Access Journals (Sweden)

    Y. Zhao

    2016-03-01

    Full Text Available Sesquiterpenes are an important class of biogenic volatile organic compounds (BVOCs and have a high secondary organic aerosol (SOA forming potential. However, SOA formation from sesquiterpene oxidation has received less attention compared to other BVOCs such as monoterpenes, and the underlying mechanisms remain poorly understood. In this work, we present a comprehensive experimental investigation of the ozonolysis of α-cedrene both in a glass flow reactor (27–44 s reaction times and in static Teflon chambers (30–60 min reaction times. The SOA was collected by impaction or filters, followed by analysis using attenuated total reflectance Fourier transform infrared (ATR-FTIR spectroscopy and electrospray ionization mass spectrometry (ESI-MS, or measured online using direct analysis in real-time mass spectrometry (DART-MS and aerosol mass spectrometry (AMS. The slow evaporation of 2-ethylhexyl nitrate that was incorporated into the SOA during its formation and growth gives an estimated diffusion coefficient of 3  ×  10−15 cm2 s−1 and shows that SOA is a highly viscous semisolid. Possible structures of four newly observed low molecular weight (MW  ≤  300 Da reaction products with higher oxygen content than those previously reported were identified. High molecular weight (HMW products formed in the early stages of the oxidation have structures consistent with aldol condensation products, peroxyhemiacetals, and esters. The size-dependent distributions of HMW products in the SOA, as well as the effects of stabilized Criegee intermediate (SCI scavengers on HMW products and particle formation, confirm that HMW products and reactions of SCI play a crucial role in early stages of particle formation. Our studies provide new insights into mechanisms of SOA formation and growth in α-cedrene ozonolysis and the important role of sesquiterpenes in new particle formation as suggested by field measurements.

  6. Stable carbon isotopic compositions of low-molecular-weight dicarboxylic acids, glyoxylic acid and glyoxal in tropical aerosols: implications for photochemical processes of organic aerosols

    Directory of Open Access Journals (Sweden)

    Stelyus L. Mkoma

    2014-10-01

    Full Text Available Tropical aerosols of PM2.5 and PM10 were collected at a rural site in Morogoro, Tanzania (East Africa, and analysed for stable carbon isotopic composition (δ13C of dicarboxylic acids (C2–C9, glyoxylic acid (ωC2 and glyoxal (Gly using gas chromatography/isotope ratio mass spectrometer. PM2.5 samples showed that δ13C of oxalic (C2 acid are largest (mean, −18.3±1.7‰ followed by malonic (C3, −19.6±1.0‰ and succinic (C4, −21.8±2.2‰ acids, whereas those in PM10 are a little smaller: −19.9±3.1‰ (C2, −20.2±2.7‰ (C3 and −23.3±3.2‰ (C4. The δ13C of C2–C4 diacids showed a decreasing trend with an increase in carbon numbers. The higher δ13C values of oxalic acid can be explained by isotopic enrichment of 13C in the remaining C2 due to the atmospheric decomposition of oxalic acid or its precursors. δ13C of ωC2 and Gly that are precursors of oxalic acid also showed larger values (mean, −22.5‰ and −20.2‰, respectively in PM2.5 than those (−26.7‰ and −23.7‰ in PM10. The δ13C values of ωC2 and Gly are smaller than those of C2 in both PM2.5 and PM10. On the other hand, azelaic acid (C9; mean, −28.5‰ is more depleted in 13C, which is consistent with the previous knowledge; that is, C9 is produced by the oxidation of unsaturated fatty acids emitted from terrestrial higher plants. A significant enrichment of 13C in oxalic acid together with its negative correlations with relative abundance of C2 in total diacids and ratios of water-soluble organic carbon and organic carbon further support that a photochemical degradation of oxalic acid occurs during long-range transport from source regions.

  7. Composition of microbial communities in aerosol, snow and ice samples from remote glaciated areas (Antarctica, Alps, Andes)

    Science.gov (United States)

    Elster, J.; Delmas, R. J.; Petit, J.-R.; Řeháková, K.

    2007-06-01

    Taxonomical and ecological analyses were performed on micro-autotrophs (cyanobacteria and algae together with remnants of diatom valves), micro-fungi (hyphae and spores), bacteria (rod, cocci and red clusters), yeast, and plant pollen extracted from various samples: Alps snow (Mt. Blank area), Andean snow (Illimani, Bolivia), Antarctic aerosol filters (Dumont d'Urville, Terre Adélie), and Antarctic inland ice (Terre Adélie). Three methods for ice and snow sample's pre-concentration were tested (filtration, centrifugation and lyophilisation). Afterwards, cultivation methods for terrestrial, freshwater and marine microorganisms (micro-autotrophs and micro-fungi) were used in combination with liquid and solid media. The main goal of the study was to find out if micro-autotrophs are commonly transported by air masses, and later stored in snow and icecaps around the world. The most striking result of this study was the absence of culturable micro-autotrophs in all studied samples. However, an unusual culturable pigmented prokaryote was found in both alpine snow and aerosol samples. Analyses of many samples and proper statistical analyses (PCA, RDA- Monte Carlo permutation tests) showed that studied treatments highly significantly differ in both microbial community and biotic remnants composition F=9.33, p=0.001. In addition, GLM showed that studied treatments highly significantly differ in numbers of categories of microorganisms and remnants of biological material F=11.45, p=0.00005. The Antarctic aerosol samples were characterised by having red clusters of bacteria, the unusual prokaryote and yeasts. The high mountain snow from the Alps and Andes contained much more culturable heterotrophs. The unusual prokaryote was very abundant, as were coccoid bacteria, red clusters of bacteria, as well as yeasts. The Antarctic ice samples were quite different. These samples had higher numbers of rod bacteria and fungal hyphae. The microbial communities and biological remnants of

  8. Stable lead isotope compositions in selected coals from around the world and implications for present day aerosol source tracing.

    Science.gov (United States)

    Díaz-Somoano, M; Kylander, M E; López-Antón, M A; Suárez-Ruiz, I; Martínez-Tarazona, M R; Ferrat, M; Kober, B; Weiss, D J

    2009-02-15

    The phasing out of leaded gasoline in many countries around the world at the end of the last millennium has resulted in a complex mixture of lead sources in the atmosphere. Recent studies suggest that coal combustion has become an important source of Pb in aerosols in urban and remote areas. Here, we report lead concentration and isotopic composition for 59 coal samples representing major coal deposits worldwide in an attempt to characterize this potential source. The average concentration in these coals is 35 microg Pb g(-1), with the highest values in coals from Spain and Peru and the lowest in coals from Australia and North America. The 206Pb/207Pb isotope ratios range between 1.15 and 1.24, with less radiogenic Pb in coals from Europe and Asia compared to South and North America. Comparing the Pb isotopic signatures of coals from this and previous studies with those published for Northern and Southern Hemisphere aerosols, we hypothesize that coal combustion might now be an important Pb source in China, the eastern U.S., and to some extent, in Europe but not as yet in other regions including South Africa, South America, and western U.S. This supports the notion that "old Pb pollution" from leaded gasoline reemitted into the atmosphere or long-range transport (i.e., from China to the western U.S.) is important. Comparing the isotope ratios of the coals, the age of the deposits, and Pb isotope evolution models for the major geochemical reservoirs suggests that the PbIC in coals is strongly influenced by the depositional coal forming environment.

  9. Submicron magnetic core conducting polypyrrole polymer shell: Preparation and characterization.

    Science.gov (United States)

    Tenório-Neto, Ernandes Taveira; Baraket, Abdoullatif; Kabbaj, Dounia; Zine, Nadia; Errachid, Abdelhamid; Fessi, Hatem; Kunita, Marcos Hiroiuqui; Elaissari, Abdelhamid

    2016-04-01

    Magnetic particles are of great interest in various biomedical applications, such as, sample preparation, in vitro biomedical diagnosis, and both in vivo diagnosis and therapy. For in vitro applications and especially in labs-on-a-chip, microfluidics, microsystems, or biosensors, the needed magnetic dispersion should answer various criteria, for instance, submicron size in order to avoid a rapid sedimentation rate, fast separations under an applied magnetic field, and appreciable colloidal stability (stable dispersion under shearing process). Then, the aim of this work was to prepare highly magnetic particles with a magnetic core and conducting polymer shell particles in order to be used not only as a carrier, but also for the in vitro detection step. The prepared magnetic seed dispersions were functionalized using pyrrole and pyrrole-2-carboxylic acid. The obtained core-shell particles were characterized in terms of particle size, size distribution, magnetization properties, FTIR analysis, surface morphology, chemical composition, and finally, the conducting property of those particles were evaluated by cyclic voltammetry. The obtained functional submicron highly magnetic particles are found to be conducting material bearing function carboxylic group on the surface. These promising conducting magnetic particles can be used for both transport and lab-on-a-chip detection. Copyright © 2015. Published by Elsevier B.V.

  10. Day-night differences in the composition and sources of carbonaceous aerosol at a polluted regional background site in the Netherlands

    Science.gov (United States)

    Dusek, Ulrike; Broekema, Elise; Holzinger, Rupert; Röckmann, Thomas; Meijer, Harro

    2017-04-01

    The origin of carbonaceous aerosol differs during day- and night-time, because emissions from major sources such as traffic, biomass combustion, and secondary organic aerosol formation show a distinct diurnal pattern. Moreover, photochemical processing and evaporation of semi-volatile organic compounds are enhanced during day-time, due to the availability of sunlight and higher temperatures. Assessing day-night differences in sources and chemical composition can give an indication of the importance of local/regional carbon sources and processing, since day-night differences should be averaged out during long-range transport. If local sources dominate, one could expect a strong diurnal variation in the source profile, but if long-range transport dominates the diurnal variation would be much weaker. In this study we measure the isotopic (14C and 13C) and detailed chemical composition of the organic fraction of the aerosol on high volume PM2.5 filter samples that were collected separately during day and night time. Radiocarbon (14C) measurements are used to estimate three main aerosol sources of organic and elemental carbon (OC and EC): Fossil fuel combustion (ff), biomass combustion (bb), and biogenic sources (bio). The detailed chemical and stable isotopic composition are measured at different desorption temperatures from the filter, which separates the more and less refractory organic compounds. The composition of the organic aerosol is measured using an thermal-desporption Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS) method (Holzinger et al, 2010) and the stable isotopic composition is measured using a thermal desorption IRMS method (Dusek et al., 2013). Source apportionment results using 14C show that the contribution of fossil fuel combustion to EC and OC is higher during day-time than during night-time. This is valid for all seasons. During night-time biomass combustion plays a bigger role as a source of carbonaceous aerosol. Even in

  11. Aerosol source apportionment from 1-year measurements at the CESAR tower in Cabauw, the Netherlands

    Directory of Open Access Journals (Sweden)

    P. Schlag

    2016-07-01

    Full Text Available Intensive measurements of submicron aerosol particles and their chemical composition were performed with an Aerosol Chemical Speciation Monitor (ACSM at the Cabauw Experimental Site for Atmospheric Research (CESAR in Cabauw, the Netherlands, sampling at 5 m height above ground. The campaign lasted nearly 1 year from July 2012 to June 2013 as part of the EU-FP7-ACTRIS project (Q-ACSM Network. Including equivalent black carbon an average particulate mass concentration of 9.50 µg m−3 was obtained during the whole campaign with dominant contributions from ammonium nitrate (45 %, organic aerosol (OA, 29 %, and ammonium sulfate (19 %. There were 12 exceedances of the World Health Organization (WHO PM2.5 daily mean limit (25 µg m−3 observed at this rural site using PM1 instrumentation only. Ammonium nitrate and OA represented the largest contributors to total particulate matter during periods of exceedance. Source apportionment of OA was performed season-wise by positive matrix factorization (PMF using the multilinear engine 2 (ME-2 controlled via the source finder (SoFi. Primary organic aerosols were attributed mainly to traffic (8–16 % contribution to total OA, averaged season-wise and biomass burning (0–23 %. Secondary organic aerosols (SOAs, 61–84 % dominated the organic fraction during the whole campaign, particularly on days with high mass loadings. A SOA factor which is attributed to humic-like substances (HULIS was identified as a highly oxidized background aerosol in Cabauw. This shows the importance of atmospheric aging processes for aerosol concentration at this rural site. Due to the large secondary fraction, the reduction of particulate mass at this rural site is challenging on a local scale.

  12. Single particle analysis of eastern Mediterranean aerosol particles: Influence of the source region on the chemical composition

    Science.gov (United States)

    Clemen, Hans-Christian; Schneider, Johannes; Köllner, Franziska; Klimach, Thomas; Pikridas, Michael; Stavroulas, Iasonas; Sciare, Jean; Borrmann, Stephan

    2017-04-01

    The Mediterranean region is one of the most climatically sensitive areas and is influenced by air masses of different origin. Aerosol particles are one important factor contributing to the Earth's radiative forcing, but knowledge about their composition and sources is still limited. Here, we report on results from the INUIT-BACCHUS-ACTRIS campaign, which was conducted at the Cyprus Atmospheric Observatory (CAO, Agia Marina Xyliatou) in Cyprus in April 2016. Our results show that the chemical composition of the aerosol particles in the eastern Mediterranean is strongly dependent on their source region. The composition of particles in a size range between 150 nm and 3 μm was measured using the Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA), which is a single particle laser ablation instrument using a bipolar time-of-flight mass spectrometer. The mass spectral information on cations and anions allow for the analysis of different molecular fragments. The information about the source regions results from backward trajectories using HYSPLIT Trajectory Model (Trajectory Ensemble) on hourly basis. To assess the influence of certain source regions on the air masses arriving at CAO, we consider the number of trajectories that crossed the respective source region within defined time steps. For a more detailed picture also the height and the velocity of the air masses during their overpass above the source regions will be considered. During the campaign at CAO in April 2016 three main air mass source regions were observed: 1) Northern Central Europe, likely with an enhanced anthropogenic influence (e.g. sulfate and black carbon from combustion processes, fly ash particles from power plants, characterized by Sr and Ba), 2) Southwest Europe, with a higher influence of the Mediterranean Sea including sea salt particles (characterized by, e.g., NaxCly, NaClxNOy), 3) Northern Africa/Sahara, with air masses that are expected to have a higher load of mineral dust

  13. Analysis of cloud condensation nuclei composition and growth kinetics using a pumped counterflow virtual impactor and aerosol mass spectrometer

    Directory of Open Access Journals (Sweden)

    J. G. Slowik

    2011-08-01

    Full Text Available We present a new method of determining the size and composition of CCN-active aerosol particles. Method utility is illustrated through a series of ambient measurements. A continuous-flow thermal-gradient diffusion chamber (TGDC, pumped counterflow virtual impactor (PCVI, and Aerodyne time-of-flight mass spectrometer (AMS are operated in series. Ambient particles are sampled into the TGDC, where a constant supersaturation is maintained, and CCN-active particles grow to ~2.5 ± 0.5 μm. The output flow from the TGDC is directed into the PCVI, where a counterflow of dry N2 gas opposes the particle-laden flow, creating a region of zero axial velocity. This stagnation plane can only be traversed by particles with sufficient momentum, which depends on their size. Particles that have activated in the TGDC cross the stagnation plane and are entrained in the PCVI output flow, while the unactivated particles are diverted to a pump. Because the input gas is replaced by the counterflow gas with better than 99 % efficiency at the stagnation plane, the output flow consists almost entirely of dry N2 and water evaporates from the activated particles. In this way, the system yields an ensemble of CCN-active particles whose chemical composition and size are analyzed using the AMS. Measurements of urban aerosol in downtown Toronto identified an external mixture of CCN-active particles consisting almost entirely of ammonium nitrate and ammonium sulfate, with CCN-inactive particles of the same size consisting of a mixture of ammonium nitrate, ammonium sulfate, and organics. We also discuss results from the first field deployment of the TGDC-PCVI-AMS system, conducted from mid-May to mid-June 2007 in Egbert, Ontario, a semirural site ~80 km north of Toronto influenced both by clean air masses from the north and emissions from the city. Organic-dominated particles sampled during a major biogenic event exhibited higher CCN activity and/or faster

  14. Characterization of flue gas, fly ash, aerosol and deposit compositions as a function of waste composition and grate operation

    DEFF Research Database (Denmark)

    Pedersen, Anne Juul; Zeuthen, Frederik Jacob; Frandsen, Flemming

    2007-01-01

    The Danish strategy for waste management is still to increase recycling and on the same time to reduce the volume of land-filled waste, in order to avoid loss of resources, and waste incineration is an important part of this strategy. In 2004, 26 % of the total reported Danish waste production...... metals, was then mixed with the reference fuel in the individual test runs. The dedicated waste fractions comprised NaCl (road salt), batteries, automotive shredder waste, CCA (Copper-Chromate-Arsenate)-impregnated wood, PVC plastics, and (leather) shoes. Test runs with varying operational parameters, e...... elements Pb, Zn, Cd and Cu was found in the fly ash fractions sampled at app. 175oC, but not in the deposits sampled at 400oC. This indicated condensation of metal chlorides at lower temperatures. It was concluded that the composition of the input waste affected the composition of the fly ash and deposits...

  15. In-Flight Chemical Composition Observations of Aircraft Emissions using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer

    Science.gov (United States)

    Ziemba, L. D.; Martin, R.; Moore, R.; Shook, M.; Thornhill, K. L., II; Winstead, E.; Anderson, B. E.

    2015-12-01

    Commercial aircraft are an important source of aerosols to the upper troposphere. The microphysical and chemical properties of these emitted aerosols govern their ability to act as ice nuclei, both in near-field contrails and for cirrus formation downstream. During the ACCESS-II (Alternative Fuel Effects on Contrails and Cruise Emissions) campaign, NASA DC-8 CFM56-2-C1 engine emissions were sampled systematically at a range of cruise-relevant thrust levels and at several altitudes. Sampling was done aboard the NASA HU-25 Falcon aircraft, which was equipped with a suite of aerosol and gas-phase instruments focused on assessing the effects of burning different fuel mixtures on aerosol properties and their associated contrails. Here we present in-flight measurements of particle chemical composition made by a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). The AMS was able to sufficiently resolve near-field (within 100m) aircraft emissions plumes. Low-sulfur HEFA (hydro-processed esters and fatty-acids) and JetA fuels yielded particles that contained 11 and 8% sulfate, respectively, compared to 30% sulfate contribution for traditional JetA fuel. Each of the fuels produced organic aerosol with similarly low oxygen content. Lubrication oils, which are not a combustion product but result from leaks in the engine, were likely a dominant fraction of the measured organic mass based on mass-spectral marker analysis. These results are compared to similar engine conditions from ground-based testing.

  16. Chemical composition and hygroscopic properties of aerosol particles over the Aegean Sea

    NARCIS (Netherlands)

    Bezantakos, S.; Barmpounis, K.; Giamarelou, M.; Bossioli, E.; Tombrou, M.; Mihalopoulos, N.; Eleftheriadis, K.; Kalogiros, J.; Allan, J.D.; Bacak, A.; Percival, C.J.; Coe, H.; Biskos, G.

    2013-01-01

    The chemical composition and water uptake characteristics of sub-micrometre atmospheric particles over the region of the Aegean Sea were measured between 25 August and 11 September 2011 within the framework of the Aegean-Game campaign. High temporal-resolution measurements of the chemical

  17. Elemental composition of ambient aerosols measured with high temporal resolution using an online XRF spectrometer

    Directory of Open Access Journals (Sweden)

    M. Furger

    2017-06-01

    Full Text Available The Xact 625 Ambient Metals Monitor was tested during a 3-week field campaign at the rural, traffic-influenced site Härkingen in Switzerland during the summer of 2015. The field campaign encompassed the Swiss National Day fireworks event, providing increased concentrations and unique chemical signatures compared to non-fireworks (or background periods. The objective was to evaluate the data quality by intercomparison with other independent measurements and test its applicability for aerosol source quantification. The Xact was configured to measure 24 elements in PM10 with 1 h time resolution. Data quality was evaluated for 10 24 h averages of Xact data by intercomparison with 24 h PM10 filter data analysed with ICP-OES for major elements, ICP-MS for trace elements, and gold amalgamation atomic absorption spectrometry for Hg. Ten elements (S, K, Ca, Ti, Mn, Fe, Cu, Zn, Ba, Pb showed excellent correlation between the compared methods, with r2 values  ≥  0.95. However, the slopes of the regressions between Xact 625 and ICP data varied from 0.97 to 1.8 (average 1.28 and thus indicated generally higher Xact elemental concentrations than ICP for these elements. Possible reasons for these differences are discussed, but further investigations are needed. For the remaining elements no conclusions could be drawn about their quantification for various reasons, mainly detection limit issues. An indirect intercomparison of hourly values was performed for the fireworks peak, which brought good agreement of total masses when the Xact data were corrected with the regressions from the 24 h value intercomparison. The results demonstrate that multi-metal characterization at high-time-resolution capability of Xact is a valuable and practical tool for ambient monitoring.

  18. Elemental composition of ambient aerosols measured with high temporal resolution using an online XRF spectrometer

    Science.gov (United States)

    Furger, Markus; Cruz Minguillón, María; Yadav, Varun; Slowik, Jay G.; Hüglin, Christoph; Fröhlich, Roman; Petterson, Krag; Baltensperger, Urs; Prévôt, André S. H.

    2017-06-01

    The Xact 625 Ambient Metals Monitor was tested during a 3-week field campaign at the rural, traffic-influenced site Härkingen in Switzerland during the summer of 2015. The field campaign encompassed the Swiss National Day fireworks event, providing increased concentrations and unique chemical signatures compared to non-fireworks (or background) periods. The objective was to evaluate the data quality by intercomparison with other independent measurements and test its applicability for aerosol source quantification. The Xact was configured to measure 24 elements in PM10 with 1 h time resolution. Data quality was evaluated for 10 24 h averages of Xact data by intercomparison with 24 h PM10 filter data analysed with ICP-OES for major elements, ICP-MS for trace elements, and gold amalgamation atomic absorption spectrometry for Hg. Ten elements (S, K, Ca, Ti, Mn, Fe, Cu, Zn, Ba, Pb) showed excellent correlation between the compared methods, with r2 values ≥ 0.95. However, the slopes of the regressions between Xact 625 and ICP data varied from 0.97 to 1.8 (average 1.28) and thus indicated generally higher Xact elemental concentrations than ICP for these elements. Possible reasons for these differences are discussed, but further investigations are needed. For the remaining elements no conclusions could be drawn about their quantification for various reasons, mainly detection limit issues. An indirect intercomparison of hourly values was performed for the fireworks peak, which brought good agreement of total masses when the Xact data were corrected with the regressions from the 24 h value intercomparison. The results demonstrate that multi-metal characterization at high-time-resolution capability of Xact is a valuable and practical tool for ambient monitoring.

  19. Micromagnetic Simulations of Submicron Cobalt Dots

    Energy Technology Data Exchange (ETDEWEB)

    Parker, G.J.; Cerjan, C.

    1999-08-30

    Numerical simulations of submicron Co extruded elliptical dots were performed to illustrate the relative importance of different physical parameters on the switching behavior in the easy direction. Shape, size, magnetic moment magnitude and crystalline anisotropy, both magnitude and distribution, were varied. The simulation includes calculation of the magnetostatic, exchange and crystalline anisotropy fields on a structured mesh using finite difference techniques. The smooth boundary of the dots are accurately represented by use of the Embedded Curve Boundary method.

  20. Submicron Surface-Patterned Fibers and Textiles

    Science.gov (United States)

    2016-11-04

    The patterned fiber surface behaves as an optical diffraction grating when the feature size is comparable with visible light wavelengths. A red laser...the optical fiber gratings For the first diffraction order of the micron and submicron patterned fiber , we utilize the formula α tanh (where s...e) SEM images of patterned PMMA fiber are depicted. The inset shows the cross- section of this fiber . Submitted to 20 Figure S3

  1. Phase transformation and intense 2.7 μm emission from Er3+ doped YF3/YOF submicron-crystals.

    Science.gov (United States)

    Chai, Guanqi; Dong, Guoping; Qiu, Jianrong; Zhang, Qinyuan; Yang, Zhongmin

    2013-01-01

    Yttrium fluoride YF3:Er(3+) and yttrium oxyfluoride YOF:Er(3+) submicron-crystals with mid-infrared fluorescent emissions were synthesized for the first time. The rhombohedral phase YOF submicron-crystals were synthesized by the crystalline phase transformation from pure orthorhombic YF3 submicron-crystals, which were prepared by co-precipitation method. The composition and morphology were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM) and transmission electron microscopy (TEM), which showed that submicron-crystals were quasi-spherical with the particle size of ~400 nm. A novel formation mechanism of YOF submicron-crystals was proposed. Photoluminescence (PL) spectra indicated the 2.7 μm emission of Er(3+) has remarkably enhanced with the increase of Er(3+) doping concentration, and a novel dynamic circulatory energy transfer mechanism was proposed. Fourier transform infrared spectra (FTIR) were used to demonstrate the change of hydroxyl content. These oxyfluoride submicron-crystals provide a new material for nano/submicron-crystals-glass composites, and open a brand new field for the realization of mid-infrared micro/nano-lasers.

  2. Sources, Composition, and Properties of Newly Formed and Regional Organic Aerosol in a Boreal Forest during the Biogenic Aerosol: Effects on Clouds and Climate Field Campaign Report

    Energy Technology Data Exchange (ETDEWEB)

    Thornton, Joel [Univ. of Washington, Seattle, WA (United States)

    2016-05-01

    The Thornton Laboratory participated in the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility’s Biogenic Aerosol Effects on Clouds and Climate (BAECC) campaign in Finland by deploying our mass spectrometer. We then participated in environmental simulation chamber studies at Pacific Northwest National Laboratory (PNNL). Thereafter, we analyzed the results as demonstrated in the several presentations and publications. The field campaign and initial environmental chamber studies are described below.

  3. Chemical and Physical Properties of Aerosols in Regional Background Air masses and Free Troposphere in the Western U.S.

    Science.gov (United States)

    Zhou, S.; Collier, S.; Jaffe, D. A.; Hee, J.; Zhang, Q.

    2016-12-01

    Understanding the sources, evolution, and physicochemical properties of aerosols in regional background air masses and from the free troposphere (FT) is crucial for constraining the climate impacts that aerosols have on a global scale. In summer 2013, we conducted a field study at a remote high elevation site (2.8 km a.s.l.) in Central Oregon - the Mt. Bachelor Observatory (MBO) - to characterize non-refractory submicron aerosols (NR-PM1) using a High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-AMS) coupled with a thermodenuder (TD) system. During this study, MBO was frequently impacted by transported wildfire plumes but there were two periods (July 25 - 30 and August 17 - 21) when concentrations of air pollutants were very low (e.g., average NR-PM1 = 3.7 ± 4.2 μg m-3; CO = 87.8 ± 17.9 ppb). Here we focus on examining the chemical and physical properties of aerosol particles during these clean periods in order to understand the characteristics of aerosols in regional background air masses and their evolution in association with boundary layer (BL) dynamics. Major aerosol components showed clear diurnal variations with higher concentrations occurring during daytime driven by the evolution of the BL, consistent with previous studies at MBO. Conversely, lower concentrations of aerosol were observed at night when MBO resided in the FT and the aerosols appeared to be acidic with high mass fraction of ammonium sulfate (up to 90% of NR-PM1) and organonitrate. Nevertheless, organic aerosol (OA), which tend to be highly oxidized (O/C = 0.84), on average accounted for 85% of NR-PM1 during the clean periods. Positive Matrix Factorization (PMF) analysis of the HR-AMS data determined a BL-OOA (O/C = 0.69; 70% of OA mass) representing oxygenated OA (OOA) influenced by BL dynamics and a FT-OOA (30% of OA) comprised of highly oxidized low-volatility organics (O/C = 1.09). These results highlight the significant compositional differences between FT and BL aerosols in

  4. Aerosol properties associated with air masses arriving into the North East Atlantic during the 2008 Mace Head EUCAARI intensive observing period: an overview

    Directory of Open Access Journals (Sweden)

    M. Dall'Osto

    2010-09-01

    Full Text Available As part of the EUCAARI Intensive Observing Period, a 4-week campaign to measure aerosol physical, chemical and optical properties, atmospheric structure, and cloud microphysics was conducted from mid-May to mid-June, 2008 at the Mace Head Atmospheric Research Station, located at the interface of Western Europe and the N. E. Atlantic and centered on the west Irish coastline. During the campaign, continental air masses comprising both young and aged continental plumes were encountered, along with polar, Arctic and tropical air masses. Polluted-continental aerosol concentrations were of the order of 3000 cm−3, while background marine air aerosol concentrations were between 400–600 cm−3. The highest marine air concentrations occurred in polar air masses in which a 15 nm nucleation mode, with concentration of 1100 cm−3, was observed and attributed to open ocean particle formation. Continental air submicron chemical composition (excluding refractory sea salt was dominated by organic matter, closely followed by sulphate mass. Although the concentrations and size distribution spectral shape were almost identical for the young and aged continental cases, hygroscopic growth factors (GF and cloud condensation nuclei (CCN to total condensation nuclei (CN concentration ratios were significantly less in the younger pollution plume, indicating a more oxidized organic component to the aged continental plume. The difference in chemical composition and hygroscopic growth factor appear to result in a 40–50% impact on aerosol scattering coefficients and Aerosol Optical Depth, despite almost identical aerosol microphysical properties in both cases, with the higher values been recorded for the more aged case. For the CCN/CN ratio, the highest ratios were seen in the more age plume. In marine air, sulphate mass dominated the sub-micron component, followed by water soluble organic carbon, which, in turn, was dominated by

  5. Chemical and isotopic composition of secondary organic aerosol generated by α-pinene ozonolysis

    DEFF Research Database (Denmark)

    Meusinger, Carl; Dusek, Ulrike; King, Stephanie M.

    2017-01-01

    of the specific carbon atom sites was determined using positionspecific isotope analysis (PSIA). The PSIA analysis showed variations at individual positions from -6.9 to +10:5% relative to the bulk composition. SOA was formed from α-pinene and ozone in a constant-flow chamber under dark, dry, and low......-NOx conditions, with OH scavengers and in the absence of seed particles. The excess of ozone and long residence time in the flow chamber ensured that virtually all α-pinene had reacted. Product SOA was collected on two sequential quartz filters. The filters were analysed offline by heating them stepwise from 100....... The observation of a number of components that occurred across the full range of desorption temperatures suggests that they are generated by thermal decomposition of oligomers. The isotopic composition of SOA was more or less independent of desorption temperature above 100 °C. TC analysis showed that SOA...

  6. Composition of carbonaceous smoke particles from prescribed burning of a Canadian boreal forest: 1. Organic aerosol characterization by gas chromatography

    Energy Technology Data Exchange (ETDEWEB)

    Mazurek, M.A.; Laterza, C.; Newman, L.; Daum, P. [Brookhaven National Lab., Upton, NY (United States); Cofer, W.R. III; Levine, J.S. [National Aeronautics and Space Administration, Hampton, VA (United States). Langley Research Center; Winstead, E.L. [Science Applications International Corporation, Hampton, VA (United States)

    1995-06-01

    In this study we examine the molecular organic constituents (C8 to C40 lipid compounds) collected as smoke particles from a Canadian boreal forest prescribed burn. Of special interest are (1) the molecular identity of polar organic aerosols, and (2) the amount of polar organic matter relative to the total mass of aerosol particulate carbon. Organic extracts of smoke aerosol particles show complex distributions of the lipid compounds when analyzed by capillary gas chromatography/mass spectrometry. The molecular constituents present as smoke aerosol are grouped into non-polar (hydrocarbons) and polar {minus}2 oxygen atoms) subtractions. The dominant chemical species found in the boreal forest smoke aerosol are unaltered resin compounds (C20 terpenes) which are abundant in unburned conifer wood, plus thermally altered wood lignins and other polar aromatic hydrocarbons. Our results show that smoke aerosols contain molecular tracers which are related to the biofuel consumed. These smoke tracers can be related structurally back to the consumed softwood and hardwood vegetation. In addition, combustion of boreal forest materials produces smoke aerosol particles that are both oxygen-rich and chemically complex, yielding a carbonaceous aerosol matrix that is enriched in polar substances. As a consequence, emissions of carbonaceous smoke particles from large-scale combustion of boreal forest land may have a disproportionate effect on regional atmospheric chemistry and on cloud microphysical processes.

  7. Complex chemical composition of colored surface films formed from reactions of propanal in sulfuric acid at upper troposphere/lower stratosphere aerosol acidities.

    Science.gov (United States)

    Van Wyngarden, A L; Pérez-Montaño, S; Bui, J V H; Li, E S W; Nelson, T E; Ha, K T; Leong, L; Iraci, L T

    Particles in the upper troposphere and lower stratosphere (UT/LS) consist mostly of concentrated sulfuric acid (40-80 wt %) in water. However, airborne measurements have shown that these particles also contain a significant fraction of organic compounds of unknown chemical composition. Acid-catalyzed reactions of carbonyl species are believed to be responsible for significant transfer of gas phase organic species into tropospheric aerosols and are potentially more important at the high acidities characteristic of UT/LS particles. In this study, experiments combining sulfuric acid (H2SO4) with propanal and with mixtures of propanal with glyoxal and/or methylglyoxal at acidities typical of UT/LS aerosols produced highly colored surface films (and solutions) that may have implications for aerosol properties. In order to identify the chemical processes responsible for the formation of the surface films, attenuated total reflectance-Fourier transform infrared (ATR-FTIR) and 1H nuclear magnetic resonance (NMR) spectroscopies were used to analyze the chemical composition of the films. Films formed from propanal were a complex mixture of aldol condensation products, acetals and propanal itself. The major aldol condensation products were the dimer (2-methyl-2-pentenal) and 1,3,5-trimethylbenzene that was formed by cyclization of the linear aldol condensation trimer. Additionally, the strong visible absorption of the films indicates that higher-order aldol condensation products must also be present as minor species. The major acetal species were 2,4,6-triethyl-1,3,5-trioxane and longer-chain linear polyacetals which are likely to separate from the aqueous phase. Films formed on mixtures of propanal with glyoxal and/or methylglyoxal also showed evidence of products of cross-reactions. Since cross-reactions would be more likely than self-reactions under atmospheric conditions, similar reactions of aldehydes like propanal with common aerosol organic species like glyoxal and

  8. Complex chemical composition of colored surface films formed from reactions of propanal in sulfuric acid at upper troposphere/lower stratosphere aerosol acidities

    Science.gov (United States)

    Van Wyngarden, A. L.; Pérez-Montaño, S.; Bui, J. V. H.; Li, E. S. W.; Nelson, T. E.; Ha, K. T.; Leong, L.; Iraci, L. T.

    2016-01-01

    Particles in the upper troposphere and lower stratosphere (UT/LS) consist mostly of concentrated sulfuric acid (40–80 wt %) in water. However, airborne measurements have shown that these particles also contain a significant fraction of organic compounds of unknown chemical composition. Acid-catalyzed reactions of carbonyl species are believed to be responsible for significant transfer of gas phase organic species into tropospheric aerosols and are potentially more important at the high acidities characteristic of UT/LS particles. In this study, experiments combining sulfuric acid (H2SO4) with propanal and with mixtures of propanal with glyoxal and/or methylglyoxal at acidities typical of UT/LS aerosols produced highly colored surface films (and solutions) that may have implications for aerosol properties. In order to identify the chemical processes responsible for the formation of the surface films, attenuated total reflectance–Fourier transform infrared (ATR-FTIR) and 1H nuclear magnetic resonance (NMR) spectroscopies were used to analyze the chemical composition of the films. Films formed from propanal were a complex mixture of aldol condensation products, acetals and propanal itself. The major aldol condensation products were the dimer (2-methyl-2-pentenal) and 1,3,5-trimethylbenzene that was formed by cyclization of the linear aldol condensation trimer. Additionally, the strong visible absorption of the films indicates that higher-order aldol condensation products must also be present as minor species. The major acetal species were 2,4,6-triethyl-1,3,5-trioxane and longer-chain linear polyacetals which are likely to separate from the aqueous phase. Films formed on mixtures of propanal with glyoxal and/or methylglyoxal also showed evidence of products of cross-reactions. Since cross-reactions would be more likely than self-reactions under atmospheric conditions, similar reactions of aldehydes like propanal with common aerosol organic species like glyoxal and

  9. Global distribution of secondary organic aerosol particle phase state

    Science.gov (United States)

    Shiraiwa, M.; Li, Y., Sr.; Tsimpidi, A.; Karydis, V.; Berkemeier, T.; Pandis, S. N.; Lelieveld, J.; Koop, T.; Poeschl, U.

    2016-12-01

    Secondary organic aerosols (SOA) account for a large fraction of submicron particles in the atmosphere and play a key role in aerosol effects on climate, air quality and public health. The formation and aging of SOA proceed through multiple steps of chemical reaction and mass transport in the gas and particle phases, which is challenging for the interpretation of field measurements and laboratory experiments as well as accurate representation of SOA evolution in atmospheric aerosol models. SOA particles can adopt liquid, semi-solid and amorphous solid (glassy) phase states depending on chemical composition, relative humidity and temperature. The particle phase state is crucial for various atmospheric gas-particle interactions, including SOA formation, heterogeneous and multiphase reactions and ice nucleation. We found that organic compounds with a wide variety of functional groups fall into molecular corridors, characterized by a tight inverse correlation between molar mass and volatility. Based on the concept of molecular corridors, we develop a method to estimate glass transition temperatures based on the molar mass and molecular O:C ratio of SOA components, which is a key property for determination of particle phase state. We use the global chemistry climate model EMAC with the organic aerosol module ORACLE to predict the atmospheric SOA phase state. For the planetary boundary layer, global simulations indicate that SOA is mostly liquid in tropical and polar air with high relative humidity, semi-solid in the mid-latitudes, and solid over dry lands. We find that in the middle and upper troposphere (>500 hPa) SOA should be mostly in a glassy solid phase state. Thus, slow diffusion of water, oxidants, and organic molecules could kinetically limit gas-particle interactions of SOA in the free and upper troposphere, promote ice nucleation and facilitate long-range transport of reactive and toxic organic pollutants embedded within SOA.

  10. On-Line Chemical Composition Analysis of Refillable Electronic Cigarette Aerosol-Measurement of Nicotine and Nicotyrine.

    Science.gov (United States)

    Martinez, Raul E; Dhawan, Steven; Sumner, Walton; Williams, Brent J

    2015-10-01

    Electronic cigarettes (e-cigs) generate aerosols that users inhale. Analyses of e-liquids inconsistently report nicotyrine, a nicotine analog that could impede nicotine metabolism, raising questions about nicotyrine formation. E-cig aerosols were analyzed on-line using a Thermal Desorption Aerosol Gas Chromatograph. Three e-liquids were tested: an unflavored solution in propylene glycol (PG); an unflavored solution in PG and vegetable glycerin (VG), and a flavored solution in PG and VG. A heating duration experiment determined the nicotyrine to nicotine ratio (NNR) in particle phase as a function of the duration of e-cig activation. An aging experiment determined the NNR in e-liquids and aerosols as a function of time since initial exposure to air and storage condition. Nicotine and nicotyrine were quantified in all 3 e-liquids and aerosols. Duration of e-cig activation was inversely related to NNR (NNR = 0.04 with 3-s activation, 0.26 with 0.5 s). Aging influenced both e-liquid NNR and aerosol NNR. On average, the e-liquid NNR increased from 0.03 at 11 days after opening to 0.08 after 60 days. For similar heating durations, aerosol NNR increased from 0.05 at 11 days to 0.23 after 60 days. Storage conditions had little effect on NNR. E-cig aerosols have variable nicotyrine quantities. Aerosol NNR depends on vaping technique and time elapsed since the e-liquid was exposed to air. It is hypothesized that aerosolized nicotyrine could facilitate nicotine absorption, inhibit the metabolism of nicotine, and reduce a user's urge to smoke. © The Author 2014. Published by Oxford University Press on behalf of the Society for Research on Nicotine and Tobacco. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.

  11. Hygroscopic behavior and chemical composition evolution of internally mixed aerosols composed of oxalic acid and ammonium sulfate

    Directory of Open Access Journals (Sweden)

    X. Wang

    2017-10-01

    Full Text Available Although water uptake of aerosol particles plays an important role in the atmospheric environment, the effects of interactions between components on chemical composition and hygroscopicity of particles are still not well constrained. The hygroscopic properties and phase transformation of oxalic acid (OA and mixed particles composed of ammonium sulfate (AS and OA with different organic to inorganic molar ratios (OIRs have been investigated by using confocal Raman spectroscopy. It is found that OA droplets first crystallize to form OA dihydrate at 71 % relative humidity (RH, and further lose crystalline water to convert into anhydrous OA around 5 % RH during the dehydration process. The deliquescence and efflorescence point for AS is determined to be 80.1 ± 1.5 % RH and 44.3 ± 2.5 % RH, respectively. The observed efflorescence relative humidity (ERH for mixed OA ∕ AS droplets with OIRs of 1 : 3, 1 : 1 and 3 : 1 is 34.4 ± 2.0, 44.3 ± 2.5 and 64.4 ± 3.0 % RH, respectively, indicating the elevated OA content appears to favor the crystallization of mixed systems at higher RH. However, the deliquescence relative humidity (DRH of AS in mixed OA ∕ AS particles with OIRs of 1 : 3 and 1 : 1 is observed to occur at 81.1 ± 1.5 and 77 ± 1.0 % RH, respectively. The Raman spectra of mixed OA ∕ AS droplets indicate the formation of ammonium hydrogen oxalate (NH4HC2O4 and ammonium hydrogen sulfate (NH4HSO4 from interactions between OA and AS in aerosols during the dehydration process on the time scale of hours, which considerably influence the subsequent deliquescence behavior of internally mixed particles with different OIRs. The mixed OA ∕ AS particles with an OIR of 3 : 1 exhibit no deliquescence transition over the RH range studied due to the considerable transformation of (NH42SO4 into NH4HC2O4 with a high DRH. Although the hygroscopic growth of mixed OA

  12. Influence of sample composition on aerosol organic and black carbon determinations

    Energy Technology Data Exchange (ETDEWEB)

    Novakov, T.; Corrigan, C.E.

    1995-07-01

    In this paper we present results on characterization of filter-collected redwood (Sequoia sempevirens)-needle and eucalyptus smoke particles by thermal, optical, and solvent extraction methods. Our results demonstrate that organic and black carbon concentrations determined by thermal and optical methods are not only method dependent, but also critically influenced by the overall chemical composition of the samples. These conclusions are supported by the following: (1) the organic fraction of biomass smoke particles analyzed includes a component, ranging in concentration from about 6-20% of total carbon or from 16-30% of organic carbon, that is relatively non-volatile and has a combustion temperature close to that of black carbon; (2) presence of K or Na in biomass smoke samples lowers the combustion temperatures of this organic component and of black carbon, making their combustion properties indistinguishable; (3) about 20% of total organic material is nonvolatile when heated to 550{degrees}C in an inert atmosphere. Consequently, thermal methods that rely on a specific temperature to separate organic from black carbon may either underestimate or overestimate the black and organic carbon concentrations, depending on the amounts of Na and K and on the composition and concentration of organic material present in a sample. These analytical uncertainties and, under some conditions, absorption by organic material may contribute to the variability of empirically derived proportionality between light transmission through filter deposits and black carbon concentrations.

  13. Photothermal spectroscopy of aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Campillo, A.J.; Lin, H.B.

    1981-04-01

    In situ aerosol absorption spectroscopy was performed using two novel photothermal detection schemes. The first, based on a photorefractive effect and coherent detection, called phase fluctuation optical heterodyne (PFLOH) spectroscopy, could, depending on the geometry employed, yield particle specific or particle and gas absorption data. Single particles of graphite as small as 1 ..mu..m were detected in the particle specific mode. In another geometrical configuration, the total absorption (both gas and particle) of submicron sized aerosols of ammonium sulfate particles in equilibrium with gaseous ammonia and water vapor were measured at varying CO/sub 2/ laser frequencies. The specific absorption coefficient for the sulfate ion was measured to be 0.5 m/sup 2//g at 1087 cm/sup -1/. The absorption coefficient sensitivity of this scheme was less than or equal to 10/sup -8/ cm/sup -1/. The second scheme is a hybrid visible Mie scattering scheme incorporating photothermal modulation. Particle specific data on ammonium sulfate droplets were obtained. For chemically identical species, the relative absorption spectrum versus laser frequency can be obtained for polydisperse aerosol distributions directly from the data without the need for complex inverse scattering calculations.

  14. Imaging aerosol viscosity

    Science.gov (United States)

    Pope, Francis; Athanasiadis, Thanos; Botchway, Stan; Davdison, Nicholas; Fitzgerald, Clare; Gallimore, Peter; Hosny, Neveen; Kalberer, Markus; Kuimova, Marina; Vysniauskas, Aurimas; Ward, Andy

    2017-04-01

    Organic aerosol particles play major roles in atmospheric chemistry, climate, and public health. Aerosol particle viscosity is important since it can determine the ability of chemical species such as oxidants, organics or water to diffuse into the particle bulk. Recent measurements indicate that OA may be present in highly viscous states; however, diffusion rates of small molecules such as water appear not to be limited by these high viscosities. We have developed a technique for measuring viscosity that allows for the imaging of aerosol viscosity in micron sized aerosols through use of fluorescence lifetime imaging of viscosity sensitive dyes which are also known as 'molecular rotors'. These rotors can be introduced into laboratory generated aerosol by adding minute quantities of the rotor to aerosol precursor prior to aerosolization. Real world aerosols can also be studied by doping them in situ with the rotors. The doping is achieved through generation of ultrafine aerosol particles that contain the rotors; the ultrafine aerosol particles deliver the rotors to the aerosol of interest via impaction and coagulation. This work has been conducted both on aerosols deposited on microscope coverslips and on particles that are levitated in their true aerosol phase through the use of a bespoke optical trap developed at the Central Laser Facility. The technique allows for the direct observation of kinetic barriers caused by high viscosity and low diffusivity in aerosol particles. The technique is non-destructive thereby allowing for multiple experiments to be carried out on the same sample. It can dynamically quantify and track viscosity changes during atmospherically relevant processes such oxidation and hygroscopic growth (1). This presentation will focus on the oxidation of aerosol particles composed of unsaturated and saturated organic species. It will discuss how the type of oxidant, oxidation rate and the composition of the oxidized products affect the time

  15. Laser direct writing using submicron-diameter fibers.

    Science.gov (United States)

    Tian, Feng; Yang, Guoguang; Bai, Jian; Xu, Jianfeng; Hou, Changlun; Liang, Yiyong; Wang, Kaiwei

    2009-10-26

    In this paper, a novel direct writing technique using submicron-diameter fibers is presented. The submicron-diameter fiber probe serves as a tightly confined point source and it adopts micro touch mode in the process of writing. The energy distribution of direct writing model is analyzed by Three-Dimension Finite-Difference Time-Domain method. Experiments demonstrate that submicron-diameter fiber direct writing has some advantages: simple process, 350-nm-resolution (lower than 442-nm-wavelength), large writing area, and controllable width of lines. In addition, by altering writing direction of lines, complex submicron patterns can be fabricated.

  16. Seasonal variations of stable carbon isotopic composition and biogenic tracer compounds of water-soluble organic aerosols in a deciduous forest

    Directory of Open Access Journals (Sweden)

    Y. Miyazaki

    2012-02-01

    Full Text Available To investigate the seasonal changes in biogenic water-soluble organic carbon (WSOC aerosols in a boreal forest, aerosol samples were collected continuously in the canopy of a deciduous forest in northern Japan during 2009–2010. Stable carbon isotopic composition of WSOC (δ13CWSOC in total suspended particulate matter (TSP exhibited a distinct seasonal cycle, with lower values from June through September (−25.5±0.5 ‰. This cycle follows the net CO2 exchange between the forest ecosystem and the atmosphere, indicating that δ13CWSOC likely reflects the biological activity at the forest site. WSOC concentrations showed the highest values in early summer and autumn. Positive matrix factorization (PMF analysis indicated that the factor in which biogenic secondary organic aerosols (BSOAs dominated accounted for ~40 % of the highest concentrations of WSOC, where BSOAs mostly consisted of α-/β-pinene SOA. In addition, primary biological aerosol particles (PBAPs made similar contributions (~57 % to the WSOC near the forest floor in early summer. This finding indicates that the production of both primary and secondary WSOC aerosols is important during the growing season in a deciduous forest. The methanesulfonic acid (MSA maximum was also found in early summer and had a distinct vertical gradient with larger concentrations near the forest floor. Together with the similar vertical gradients found for WSOC and δ13CWSOC as well as the α-/β-pinene SOA tracers, our results indicate that the forest floor, including ground vegetation and soil, acts as a significant source of WSOC in TSP within a forest canopy at the study site.

  17. Global measurements of coarse-mode aerosol size distributions - first results from the Atmospheric Tomography Mission (ATom)

    Science.gov (United States)

    Weinzierl, B.; Dollner, M.; Schuh, H.; Brock, C. A.; Bui, T. V.; Gasteiger, J.; Froyd, K. D.; Schwarz, J. P.; Spanu, A.; Murphy, D. M.; Katich, J. M.; Kupc, A.; Williamson, C.

    2016-12-01

    Although coarse-mode aerosol (>1 µm diameter), composed mainly of mineral dust and sea-salt, is highly abundant over large regions of the world, these particles form a particularly poorly understood and characterized subset of atmospheric aerosol constituents. The NASA-sponsored Atmospheric Tomography Mission (ATom) is an unprecedented field program that investigates how human emissions affect air quality and climate change. ATom provides a singular opportunity to characterize the global coarse-mode size distribution by continuously profiling between 0.2 and 13 km with the NASA DC-8 research aircraft while traveling from the high Arctic down south the middle of the Pacific Ocean, to the Southern Ocean and back north over the Atlantic Ocean basin in four seasons. For ATom, the DC-8 aircraft has been equipped with multiple instruments to observe the composition of the air. The coarse mode and cloud particle size distribution is measured in-situ with a Cloud, Aerosol, and Precipitation Spectrometer (CAPS) mounted under the wing of the DC-8 research aircraft. The CAPS consists of an optical spectrometer providing size distributions in the size range between 0.5 and 50 µm and an imager detecting number concentration, size and shape of particles between 15 and 930 µm diameter. Early ATom flights indicated complicated vertical layering: over the sea, we regularly observed sea salt aerosol which extended from the ground up to 0.6-1 km altitude. In addition - depending on the location of the measurements - we frequently found layers with coarse mode aerosol originating from deserts and biomass burning aerosol aloft. In this study, we will present first results of coarse mode aerosol observations from the entire first ATom deployment in summer 2016. We will show vertical profiles of coarse mode aerosol number concentration, discuss their interhemispheric differences, and look into the question how frequently coarse-mode aerosol is externally mixed with submicron black

  18. Organic composition of aerosol particulate matter during a haze episode in Kuala Lumpur, Malaysia

    Science.gov (United States)

    Radzi Bin Abas, M.; Rahman, Noorsaadah A.; Omar, Nasr Yousef M. J.; Maah, M. Jamil; Abu Samah, Azizan; Oros, Daniel R.; Otto, Angelika; Simoneit, Bernd R. T.

    The solvent-extractable compounds of urban airborne particulate matter were analyzed to determine the distributions of homologous and biomarker tracers. Samples were collected by high-volume air filtration during the haze episode of 1997 around the University of Malaya campus near Petaling Jaya, a suburb of Kuala Lumpur, Malaysia. These results show that the samples contain n-alkanes, n-alkan-2-ones, n-alkanols, methyl n-alkanoates, n-alkyl nitriles, n-alkanals, n-alkanoic acids, levoglucosan, PAHs, and UCM as the dominant components, with minor amounts of terpenoids, glyceryl esters and sterols, all derived from natural biogenic sources (vascular plant wax), from burning of biomass, and from anthropogenic utilization of fossil fuel products (lubricating oil, vehicle emissions, etc.). Some compositional differences are observed in the samples and greater atmospheric concentrations were found for almost all organic components in the samples collected near a roadway. The results interpreted in terms of major sources are due to local build-up of organic contaminants from vehicular emissions, smoke from biomass burning, and natural background as a result of the atmospheric stability during the haze episodes. The organic components transported in from areas outside the region, assuming all smoke components are external to the city, amount to about 30% of the total organic particle burden.

  19. Sulfur Isotopic Compositions of Individual Aerosol Particles from Below and Within Stratocumulus Clouds over the Southeast Pacific Ocean During VOCALS

    Science.gov (United States)

    Bose, M.; Anderson, J. R.; Twohy, C. H.; Williams, P.

    2012-12-01

    The VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-Rex) was a large multi-national field experiment that collected data and samples from a region of the southeast Pacific with the world's largest stratocumulus cloud systems. Samples examined here are residues of cloud droplets and ambient particles from below the clouds collected during flights of the NCAR C-130 off the coast of Chile. Selected samples were studied using scanning electron microscopy (SEM) and secondary ion mass spectrometry (SIMS) in order to contribute to the understanding of the source of non-sea-salt sulfate in this region. Particles in the size range from 0.2 to 1μm diameter on holey and lacey carbon were characterized by SEM combined with energy dispersive spectrometry (EDS), thus identifying sulfur-containing particles. Subsequently, sulfur ion imaging of identified sea salt, ammonium sulfate and sodium sulfate particles was done with the Cameca Ametek NanoSIMS 50L at Arizona State University. A electrons were collected simultaneously at high mass resolution (m/Δm>10000). Each measurement typically consists of 5 to 8 frames (~5.4 min/frame). NIST barium sulfate and ammonium sulfate particles were used as isotopic standards. Preliminary analyses on a small pool of VOCALS individual particles show a wide range in sulfur isotopic compositions (δ34S = -56 to +41‰). In addition, the in-cloud particles are enriched in 32S, while the ambient particles exhibit 34S excesses. Isotopic data on a large inventory of particles is being currently acquired, which will be presented at the meeting. Data will be used to investigate sulfur sources (marine vs. continental) and the processing of aerosols through sulfate formation.

  20. Contributions of transported Prudhoe Bay oil field emissions to the aerosol population in Utqiaġvik, Alaska

    Science.gov (United States)

    Gunsch, Matthew J.; Kirpes, Rachel M.; Kolesar, Katheryn R.; Barrett, Tate E.; China, Swarup; Sheesley, Rebecca J.; Laskin, Alexander; Wiedensohler, Alfred; Tuch, Thomas; Pratt, Kerri A.

    2017-09-01

    Loss of sea ice is opening the Arctic to increasing development involving oil and gas extraction and shipping. Given the significant impacts of absorbing aerosol and secondary aerosol precursors emitted within the rapidly warming Arctic region, it is necessary to characterize local anthropogenic aerosol sources and compare to natural conditions. From August to September 2015 in Utqiaġvik (Barrow), AK, the chemical composition of individual atmospheric particles was measured by computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy (0.13-4 µm projected area diameter) and real-time single-particle mass spectrometry (0.2-1.5 µm vacuum aerodynamic diameter). During periods influenced by the Arctic Ocean (70 % of the study), our results show that fresh sea spray aerosol contributed ˜ 20 %, by number, of particles between 0.13 and 0.4 µm, 40-70 % between 0.4 and 1 µm, and 80-100 % between 1 and 4 µm particles. In contrast, for periods influenced by emissions from Prudhoe Bay (10 % of the study), the third largest oil field in North America, there was a strong influence from submicron (0.13-1 µm) combustion-derived particles (20-50 % organic carbon, by number; 5-10 % soot by number). While sea spray aerosol still comprised a large fraction of particles (90 % by number from 1 to 4 µm) detected under Prudhoe Bay influence, these particles were internally mixed with sulfate and nitrate indicative of aging processes during transport. In addition, the overall mode of the particle size number distribution shifted from 76 nm during Arctic Ocean influence to 27 nm during Prudhoe Bay influence, with particle concentrations increasing from 130 to 920 cm-3 due to transported particle emissions from the oil fields. The increased contributions of carbonaceous combustion products and partially aged sea spray aerosol should be considered in future Arctic atmospheric composition and climate simulations.

  1. A First Assessment of the Elemental Composition of Atmospheric Aerosols in the Canadian Oil Sands Region

    Directory of Open Access Journals (Sweden)

    Dabek-Zlotorzynska E.

    2013-04-01

    Full Text Available Canadian Oil Sands, which comprise 97% of Canada’s 176 billion barrels of proven oil reserves, are located beneath 140,200 km2 of boreal forests, prairies and wetlands, and are the second largest known deposit of crude oil in the world. As such, this region has experienced rapid industrial development, which resulted also in increasing industrial air emissions, primarily from bitumen upgrading and mine vehicle fleet operations. This rapid development has led to concerns regarding health risk to humans, and other terrestrial and aquatic wildlife associated with exposure to toxic contaminants, especially metals and polycyclic aromatic compounds (PACs particularly along the Athabasca River and its watershed. Canada’s Minister of the Environment announced that Environment Canada (EC will jointly lead, in collaboration with Government of Alberta and relevant stakeholders, the development and implementation of an enhanced monitoring system in the Oil Sands region to provide information on the state of the air, water, land andbiodiversity. This work presents preliminary data on the first assessment of elemental composition of fine particulate matter (particles<2.5 mm in diameter; PM2.5 at 3 air quality sites in close proximity to Oil Sands processing activities. Since December 2010, integrated 24 hour air samples were collected every sixth day on a 47-mm Teflon filters using Thermo Fisher Partisol 2000-FRM samplers operated by the National Air Pollution Surveillance (NAPS network that involves EC and the Canadian provinces and territories. All samples including laboratory, travel and field blanks were subjected to gravimetric determination of PM2.5 mass and energy dispersive X-ray fluorescence (ED-XRF analysis for 46 elements. Since ED-XRF is a non-destructive technique, PM2.5 samples were subsequently analyzed for 37 trace elements including rare earth elements using inductively-coupled plasma mass spectrometry (ICP-MS combined with microwave

  2. Formation of secondary aerosols from biomass burning plumes: chamber simulation study

    Science.gov (United States)

    Wang, X.; Hu, Q.; Fang, Z.; Deng, W.

    2015-12-01

    Biomass burning contributed substantially to carbonaceous aerosols in China's ambient air, even in its highly industrialized megacities, based on recent source attributions by receptor modeling or by molecular and isotopic tracers. Although chemical evolution of biomass burning plumes in the ambient is a vital issue for the study of climatic and health effects, the understanding of secondary pollutants formation during the aging of biomass burning plumes is far from complete. Here we collected typical agriculture residues and forest plant branches in the Pearl River Delta in south China, and got them burned in laboratory-controlled conditions and introduced the plumes from burning these biomass directly into the GIGCAS indoor smog chamber with a reactor of 30 m3 to investigate the photochemical aging of the plumes. The inorganic trace gases, including SO2, NOx, NH3 and O3, were monitored online with chemiluminescence gas analyzers, precursor volatile organic compounds (VOCs) were monitor online with a PTR-ToF-MS and offline by a preconcentrator coupled with a gas chromatography-mass selective detector/flame ionization detector/electron capture detector (GC-MSD/FID/ECD), particle number concentrations and size distributions were obtained using a scanning mobility particle sizer (SMPS), and a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) was used to measure the chemical compositions and evolutions of submicron aerosols and to trace the change in the average element ratios of organics, like H/C, O/C, and N/C. The results from the study were summarized in the following aspects: 1) primary emission factors of gaseous and particulate pollutants from burning of typical biomass including agricultural remains and forest wood plants; 2) yields of secondary pollutants, including secondary inorganic and organic aerosols and gaseous products (like O3) during photochemical aging of biomass burning plumes; 3) relationship between the formed secondary

  3. Stable hydrogen isotope composition of n-alkanes in urban atmospheric aerosols in Taiyuan, China

    Science.gov (United States)

    Bai, Huiling; Li, Yinghui; Peng, Lin; Liu, Xiangkai; Liu, Xiaofeng; Song, Chongfang; Mu, Ling

    2017-03-01

    The hydrogen isotope compositions (δD) of n-alkanes associated with particulate matter with a diameter of ≤10 μm from Taiyuan, China, during heating and non-heating periods were measured via gas chromatography-isotope ratio mass spectrometry to reveal the spatial and temporal characteristics of five functional zones and to provide another constraint on atmospheric pollutants. The δD values of n-C16 to n-C31 during the heating and non-heating periods ranged from -235.9‰ to -119.8‰ and from -231.3‰ to -129.2‰, respectively, but these similar spans had different distribution features. During the heating period, the δD distributions between non-central heating and commercial districts were consistent, as were those between residential and industrial districts; the n-alkanes came from two or more types of emission sources. Coal soot might be the primary local emission source, but not the only source. During the non-heating period, the n-alkanes of n-C16 to n-C20 were more depleted in D with the increasing carbon number in all functional zones, but there was no rule for n-C21 to n-C31. Specifically, coal soot and vehicle exhaust might be the primary sources of n-alkanes for non-central heating districts in the heating and non-heating periods, respectively, according to the δD distribution of n-C18 to n-C22; gasoline vehicle exhaust might be an n-alkane source, and the hydrogen isotope fractionation effect during the condensation process should be a pollution mechanism for the commercial district during the heating period; the δD distribution difference of n-C16 to n-C18 between the two periods in the residential and industrial districts was consistent, which indicates a similar source of fossil fuel combustion and a similar isotope fractionation effect during the non-heating period.

  4. Analysis of aerosol composition data for western United States wildfires between 2005 and 2015: Dust emissions, chloride depletion, and most enhanced aerosol constituents.

    Science.gov (United States)

    Schlosser, Joseph S; Braun, Rachel A; Bradley, Trevor; Dadashazar, Hossein; MacDonald, Alexander B; Aldhaif, Abdulmonam A; Aghdam, Mojtaba Azadi; Mardi, Ali Hossein; Xian, Peng; Sorooshian, Armin

    2017-08-27

    This study examines major wildfires in the western United States between 2005 and 2015 to determine which species exhibit the highest percent change in mass concentration on day of peak fire influence relative to preceding nonfire days. Forty-one fires were examined using the Environmental Protection Agency (EPA) Interagency Monitoring of Protected Visual Environments (IMPROVE) data set. Organic carbon (OC) and elemental carbon (EC) constituents exhibited the highest percent change increase. The sharpest enhancements were for the volatile (OC1) and semivolatile (OC2) OC fractions, suggestive of secondary organic aerosol formation during plume transport. Of the noncarbonaceous constituents, Cl, P, K, NO3-, and Zn levels exhibited the highest percent change. Dust was significantly enhanced in wildfire plumes, based on significant enhancements in fine soil components (i.e., Si, Ca, Al, Fe, and Ti) and PMcoarse (i.e., PM10-PM2.5). A case study emphasized how transport of wildfire plumes significantly impacted downwind states, with higher levels of fine soil and PMcoarse at the downwind state (Arizona) as compared to the source of the fires (California). A global model (Navy Aerosol Analysis and Prediction System, NAAPS) did not capture the dust influence over California or Arizona during this case event because it is not designed to resolve dust dynamics in fires, which motivates improved treatment of such processes. Significant chloride depletion was observed on the peak EC day for almost a half of the fires examined. Size-resolved measurements during two specific fires at a coastal California site revealed significant chloride reductions for particle aerodynamic diameters between 1 and 10 μm.

  5. Nicotine delivery from the refill liquid to the aerosol via high-power e-cigarette device.

    Science.gov (United States)

    Prévôt, Nathalie; de Oliveira, Fabien; Perinel-Ragey, Sophie; Basset, Thierry; Vergnon, Jean-Michel; Pourchez, Jérémie

    2017-06-01

    To offer an enhanced and well-controlled nicotine delivery from the refill liquid to the aerosol is a key point to adequately satisfy nicotine cravings using electronic nicotine delivery systems (ENDS). A recent high-power ENDS, exhibiting higher aerosol nicotine delivery than older technologies, was used. The particle size distribution was measured using a cascade impactor. The effects of the refill liquid composition on the nicotine content of each size-fraction in the submicron range were investigated. Nicotine was quantified by liquid chromatography coupled with tandem mass spectrometry. Particle size distribution of the airborne refill liquid and the aerosol nicotine demonstrated that the nicotine is equally distributed in droplets regardless of their size. Results also proved that the nicotine concentration in aerosol was significantly lower compared to un-puffed refill liquid. A part of the nicotine may be left in the ENDS upon depletion, and consequently a portion of the nicotine may not be transferred to the user. Thus, new generation high-power ENDS associated with propylene glycol/vegetable glycerin (PG/VG) based solvent were very efficient to generate carrier-droplets containing nicotine molecules with a constant concentration. Findings highlighted that a portion of the nicotine in the refill liquid may not be transferred to the user.

  6. Microscopic imaging ellipsometry of submicron-scale bacterial cells ...

    African Journals Online (AJOL)

    Microscopic imaging ellipsometry of submicron-scale bacterial cells. ... Conclusion: MIE is a sensitive non-optical technique that can be used to image biological systems without the need for labeling of molecules. Keywords: Objective plane, Imaging ellipsometry, Submicron-scale bacterial cells, Streptococcus mutans, ...

  7. Influence of marine aerosols and aerotechnogenic load on chemical composition of rainwaters on small islands (ludas) of the White Sea

    Science.gov (United States)

    Gorbacheva, Tamara; Mazukhina, Svetlana; Isaeva, Ludmila; Shumilov, Oleg

    2013-04-01

    In June 2001 intensive monitoring plots were established on the island part of Kandalaksha Bay of the White Sea (the island Tonnaya Luda; 67o06'60"N; 32o24'12"E) with the installation of stationary rainwater collectors. The purpose was studying the chemical composition of rain waters in the zone of cumulative influence of marine aerosols and aerotechnogenic load. Water sampling was carried out monthly during the vegetative season of 2001 and 2002. pH of rain water was determined by potentiometric method without preliminary filtration. The samples were passed through the paper filter with the pore diameter of 1-2.5 microns, the analysis of filtrate carried out by methods of atomic emission spectrometry (K, Na) and atomic absorption spectrometry (Ca, Mg, Zn, Mn, Cu, Ni, Al, Fe), total P and P of phosphates, Si and NH4+ - by photocolorimetry, total carbon - by bichromate method, NO3-, SO42-, Cl--by ion exchange chromatography method. Balance method was chosen as a research basis to determine the interrelation of rain water organic matter and dynamics of its redistribution under the influence of natural and technogenic factors. The difference between the cations sum (including NH4+and H+) and mineral acids anions sum (SO42-, Cl-, NO3-) was identified as organic acids anions concentration (μeq l-1). The level of Na, Cl-, K, Ca, Mg, SO42-, Sr in rainwaters on the island and the remote areas is indicative of the possible influence of marine aerosols on the island part of the White Sea. The increase of Al, Cu, Ni, Cd, Co concentrations in rainwaters up to one order against the background values points to the cumulative influence of the emissions of industrial enterprises located in the region. The relative stability of pH values of rain waters during all seasons indicates to the buffer action of weak organic acids anions. The correlation analysis of ionic structure in normal concentrations has allowed us to estimate the distribution of the cationic part from the

  8. Theoretical studies on aerosol agglomeration processes

    Energy Technology Data Exchange (ETDEWEB)

    Lehtinen, K.E.J. [VTT Energy, Espoo (Finland). Energy Use

    1997-12-31

    In this thesis, theoretical modeling of certain aerosol systems has been presented. At first, the aerosol general dynamic equation is introduced, along with a discretization routine for its numerical solution. Of the various possible phenomena affecting aerosol behaviour, this work is mostly focused on aerosol agglomeration. The fundamentals of aerosol agglomeration theory are thus briefly reviewed. The two practical applications of agglomeration studied in this thesis are flue gas cleaning using an electrical agglomerator and nanomaterial synthesis with a free jet reactor. In an electrical agglomerator the aerosol particles are charged and brought into an alternating electric field. The aim is to remove submicron particles from flue gases by collisions with larger particles before conventional gas cleaning devices that have a clear penetration window in the problematic 0.1-1{mu}m size range. A mathematical model was constructed to find out the effects of the different system parameters on the agglomerator`s performance. A crucial part of this task was finding out the collision efficiencies of particles of varying size and charge. The original idea was to use unipolar charging of the particles, and a laboratory scale apparatus was constructed for this purpose. Both theory and experiments clearly show that significant removal of submicron particles can not be achieved by such an arrangement. The theoretical analysis further shows that if the submicron particles and the large collector particles were charged with opposite polarity, significant removal of the submicron particles could be obtained. The second application of agglomeration considered in this thesis is predicting/controlling nanoparticle size in the gas-to-particle aerosol route to material synthesis. In a typical material reactor, a precursor vapor reacts to form molecules of the desired material. In a cooling environment, a particulate phase forms, the dynamics of which are determined by the rates of

  9. Combining Mass Spectrometry and ATR-FTIR Spectroscopy to Study Phase, Diffusion and Composition of Secondary Organic Aerosol from the Ozonolysis of α-pinene

    Science.gov (United States)

    Perraud, V. M.; Finlayson-Pitts, B. J.; Waring-Kidd, C.

    2014-12-01

    Secondary organic aerosol (SOA) is ubiquitous in the atmosphere and composes a large fraction of the total aerosol budget. Recent reports from field measurements and laboratory studies show that some SOA particles are better represented by a semi-solid low viscosity tar-like material rather than a ideal liquid often assumed in regional and global models. Characterizing the phase of SOA is crucial to understanding how particles interact with trace gases and how it ultimately impacts their growth and evolution in the atmosphere. We report here laboratory studies carried out in the unique UCI large-volume, slow-flow, aerosol flow reactor. Particles from the ozonolysis of a-pinene were formed at various relative humidities (RH from < 3% to 90%) and collected onto a custom ATR-FTIR impactor. The observed impaction pattern provided insights into changes in phase/viscosity of the SOA as a function of relative humidity. In addition, attenuated total reflectance FTIR and mass spectrometry measurements provided information on simultaneous changes on composition. Application of ATR-FTIR combined with PTR-MS provided additional data on the volatility of the SOA at room temperature and diffusion coefficients of two key components pinonaldehyde and acetic acid present in the SOA. Implication for modeling the growth and ultimately the lifetime of SOA in the atmosphere will be discussed.

  10. Ball Lightning Aerosol Electrochemical Power Source or A Cloud of Batteries

    Science.gov (United States)

    Meshcheryakov, Oleg

    2007-07-01

    Despite numerous attempts, an adequate theoretical and experimental simulation of ball lightning still remains incomplete. According to the model proposed here, the processes of electrochemical oxidation within separate aerosol particles are the basis for this phenomenon, and ball lightning is a cloud of composite nano or submicron particles, where each particle is a spontaneously formed nanobattery which is short-circuited by the surface discharge because it is of such a small size. As free discharge-shorted current loops, aerosol nanobatteries are exposed to a powerful mutual magnetic dipole dipole attraction. The gaseous products and thermal energy produced by each nanobattery as a result of the intra-particle self-sustaining electrochemical reactions, cause a mutual repulsion of these particles over short distances and prevent their aggregation, while a collectivization of the current loops of separate particles, due to the electric arc overlapping between adjacent particles, weakens their mutual magnetic attraction over short distances. Discharge currents in the range of several amperes to several thousand amperes as well as the pre-explosive mega ampere currents, generated in the reduction oxidation reactions and distributed between all the aerosol particles, explain both the magnetic attraction between the elements of the ball lightning substance and the impressive electromagnetic effects of ball lightning.

  11. Ball Lightning–Aerosol Electrochemical Power Source or A Cloud of Batteries

    Science.gov (United States)

    2007-01-01

    Despite numerous attempts, an adequate theoretical and experimental simulation of ball lightning still remains incomplete. According to the model proposed here, the processes of electrochemical oxidation within separate aerosol particles are the basis for this phenomenon, and ball lightning is a cloud of composite nano or submicron particles, where each particle is a spontaneously formed nanobattery which is short-circuited by the surface discharge because it is of such a small size. As free discharge-shorted current loops, aerosol nanobatteries are exposed to a powerful mutual magnetic dipole–dipole attraction. The gaseous products and thermal energy produced by each nanobattery as a result of the intra-particle self-sustaining electrochemical reactions, cause a mutual repulsion of these particles over short distances and prevent their aggregation, while a collectivization of the current loops of separate particles, due to the electric arc overlapping between adjacent particles, weakens their mutual magnetic attraction over short distances. Discharge currents in the range of several amperes to several thousand amperes as well as the pre-explosive mega ampere currents, generated in the reduction–oxidation reactions and distributed between all the aerosol particles, explain both the magnetic attraction between the elements of the ball lightning substance and the impressive electromagnetic effects of ball lightning.

  12. Ball Lightning–Aerosol Electrochemical Power Source or A Cloud of Batteries

    Directory of Open Access Journals (Sweden)

    Meshcheryakov Oleg

    2007-01-01

    Full Text Available AbstractDespite numerous attempts, an adequate theoretical and experimental simulation of ball lightning still remains incomplete. According to the model proposed here, the processes of electrochemical oxidation within separate aerosol particles are the basis for this phenomenon, and ball lightning is a cloud of composite nano or submicron particles, where each particle is a spontaneously formed nanobattery which is short-circuited by the surface discharge because it is of such a small size. As free discharge-shorted current loops, aerosol nanobatteries are exposed to a powerful mutual magnetic dipole–dipole attraction. The gaseous products and thermal energy produced by each nanobattery as a result of the intra-particle self-sustaining electrochemical reactions, cause a mutual repulsion of these particles over short distances and prevent their aggregation, while a collectivization of the current loops of separate particles, due to the electric arc overlapping between adjacent particles, weakens their mutual magnetic attraction over short distances. Discharge currents in the range of several amperes to several thousand amperes as well as the pre-explosive mega ampere currents, generated in the reduction–oxidation reactions and distributed between all the aerosol particles, explain both the magnetic attraction between the elements of the ball lightning substance and the impressive electromagnetic effects of ball lightning.

  13. Aerosol optical properties relevant to regional remote sensing of CCN activity and links to their organic mass fraction: airborne observations over Central Mexico and the US West Coast during MILAGRO/INTEX-B

    Directory of Open Access Journals (Sweden)

    Y. Shinozuka

    2009-09-01

    Full Text Available Remote sensing of cloud condensation nuclei (CCN would help evaluate the indirect effects of tropospheric aerosols on clouds and climate. To assess its feasibility, we examined relationships of submicron aerosol composition to CCN activity and optical properties observed during the MILAGRO/INTEX-B aircraft campaigns. An indicator of CCN activity, κ, was calculated from hygroscopicity measured under saturation. κ for dry 100 nm particles decreased with increasing organic fraction of non-refractory mass of submicron particles (OMF as 0.34–0.20×OMF over Central Mexico and 0.47–0.43×OMF over the US West Coast. These fits represent the critical dry diameter, centered near 100 nm for 0.2% supersaturation but varied as κ(−1/3, within measurement uncertainty (~20%. The decreasing trends of CCN activity with the organic content, evident also in our direct CCN counts, were consistent with previous ground and laboratory observations of highly organic particles. The wider range of OMF, 0–0.8, for our research areas means that aerosol composition will be more critical for estimation of CCN concentration than at the fixed sites previously studied. Furthermore, the wavelength dependence of extinction was anti-correlated with OMF as −0.70×OMF+2.0 for Central Mexico's urban and industrial pollution air masses, for unclear reasons. The Angstrom exponent of absorption increased with OMF, more rapidly under higher single scattering albedo, as expected for the interplay between soot and colored weak absorbers (some organic species and dust. Because remote sensing products currently use the wavelength dependence of extinction albeit in the column integral form and may potentially include that of absorption, these regional spectral dependencies are expected to facilitate retrievals of aerosol bulk chemical composition and CCN activity over Central Mexico.

  14. Diurnal variations of organic molecular tracers and stable carbon isotopic composition in atmospheric aerosols over Mt. Tai in the North China Plain: an influence of biomass burning

    Directory of Open Access Journals (Sweden)

    P. Q. Fu

    2012-09-01

    organic carbon (SOC, we estimate that an average of 24% (up to 64% of the OC in the Mt. Tai aerosols was due to biomass burning in early June, followed by the contribution of isoprene SOC (mean 4.3%. In contrast, isoprene SOC was the main contributor (6.6% to OC, and only 3.0% of the OC was due to biomass burning in late June. In early June, δ13C of TC (−26.6 to −23.2‰, mean −25.0‰ were lower than those (−23.9 to −21.9‰, mean −22.9‰ in late June. In addition, a strong anti-correlation was found between levoglucosan and δ13C values. This study demonstrates that crop-residue burning activities can significantly enhance the organic aerosol loading and alter the organic composition and stable carbon isotopic composition of aerosol particles in the troposphere over the North China Plain.

  15. Spectroscopic characterization of Antarctic marine aerosol

    Science.gov (United States)

    Paglione, Marco; Zanca, Nicola; Rinaldi, Matteo; Dall'osto, Manuel; Simo, Rafel; Facchini, Maria Cristina; Decesari, Stefano

    2017-04-01

    Marine aerosol constitutes an important and not thoroughly investigated natural aerosol system. In particular, the poor knowledge of the physical-chemical properties of primary (sea-spray) and secondary particles, especially over biologically active seawaters, affects the current capability of modeling the effect of marine aerosol on climate (O'Dowd et al., 2004). In polar regions, surface seawater composition and its exchanges with the atmosphere is complicated also by the presence of sea-ice and of the variety of micro-organisms (viruses, prokaryotes and microalgae) living within it (Levasseur,2013). In the framework of the Spanish project PEGASO (Plankton-derived Emission of Gases and Aerosols in the Southern Ocean) submicron aerosol samples were collected during a 6 weeks long oceanographic cruise (2nd January 2015 - 11th February 2015) conducted in the regions of Antarctic Peninsula, South Orkney and South Georgia Islands, an area of the Southern Ocean characterized every summer by both large patches of productive waters (phytoplankton blooms) and sea-ice cover. The collected samples were analyzed by means of proton-Nuclear Magnetic Resonance (H-NMR) spectroscopy with aim of organic compounds characterization in terms of functional groups and specific molecular tracers identification (Decesari et al., 2011). H-NMR spectral features resulted quite variable among the different samples both in terms of relative abundance of main functional groups and in terms of presence of specific compounds. In all the samples were found biogenic markers, like low-molecular-weight alkyl-amines and methanesulphonate (MSA), of secondary origin (formed by the condensation of vapors onto particles). Resonance signals of other aliphatic compounds of possible primary origin, like lipids, aminoacids (e.g. alanine) and sugars (e.g. sucrose) are present in variable concentrations in the samples. A hierarchical cluster analysis applied on the NMR spectra allowed to identify similarities

  16. Aerosol mixing state, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    Directory of Open Access Journals (Sweden)

    S. Lance

    2013-05-01

    Full Text Available Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. κ-Köhler theory is used to evaluate the characteristic hygroscopicity parameter, κ*, for the CCN active aerosol population using both size-resolved HTMDA and size-resolved CCNc measurements. Organic mass fractions (forg are evaluated from size-resolved aerosol mass spectrometer (AMS measurements, from which predictions of the hygroscopicity parameter are compared against κ*. Strong diurnal changes in aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF events are correlated with an increased κ* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN at 0.51% ± 0.06% supersaturation can surpass by more than a factor of two the corresponding concentrations of 100 nm particles. We also find that at 06:00–08:00 LT throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally mixed fraction for 40 nm particles and 30% externally mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as "internally mixed". Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events, the early morning "rush hour" and the entire campaign. We show that κ* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for κ* versus particle size, which can be attributed to unresolved mixing state and the presence of refractory

  17. Organic composition of PM 2.5 and size-segregated aerosols and their sources during the 2002 Bay Regional Atmospheric Chemistry Experiment (BRACE), Florida, USA

    Science.gov (United States)

    Tremblay, Raphaël T.; Riemer, Daniel D.; Zika, Rod G.

    PM 2.5 and size-segregated aerosols were collected in May 2002 as part of the Bay Regional Atmospheric Chemistry Experiment (BRACE), Florida, USA. Aerosol organic composition was used to estimate sources of a series of alkanes and polycyclic aromatic hydrocarbons (PAHs) using chemical indices, hierarchical cluster analysis (HCA) and a chemical mass balance receptor model (CMB). Aerosols were collected on quartz fiber filters (QFF) using a PM 2.5 high volume sampler and on aluminum foil discs using a Micro-Orifice Uniform Deposit Impactor (MOUDI, 50% aerodynamic cut diameters were 18, 10, 5.6, 3.2, 1.8, 1.0, 0.56, 0.315 and 0.171 μm). Target compounds included alkanes and PAHs and were solvent extracted using a mixture of dichloromethane, acetone and hexane, concentrated and then analyzed using a gas chromatograph/mass spectrometer (GC/MS). The target compounds in PM 2.5 were dominated by six sources during the study period: mobile sources (39±5%), coal burning (33±5%), biogenic primary emission (20±2%), oil combustion (5±2%), biomass burning (1.0±0.3%) and an unidentified source (3±2%). Results obtained from the chemical indices, HCA and CMB were in very good agreement with each other. PAH size distributions are presented for days dominated by a same source. Seventy-five percent and 50% of the PAH were found below 1.8 and 0.56 μm, respectively (monthly PAH geometric diameters averaged 0.43 μm). Coarse size PAHs were observed on 1 day (15 May) and were correlated with nitrate and sodium size distribution. It is hypothesized that the PAHs, sodium and nitrate were internally mixed and that the PAHs deposited onto a pre-existing marine aerosol. This transfer process has significant implications for PAH deposition and lifetime and warrants further study.

  18. Towards a better understanding of the origins, chemical composition and aging of oxygenated organic aerosols: case study of a Mediterranean industrialized environment, Marseille

    Directory of Open Access Journals (Sweden)

    I. El Haddad

    2013-08-01

    Full Text Available As part of the FORMES summer 2008 experiment, an Aerodyne compact time-of-flight aerosol mass spectrometer (cToF-AMS was deployed at an urban background site in Marseille to investigate the sources and aging of organic aerosols (OA. France's second largest city and the largest port in the Mediterranean, Marseille, provides a locale that is influenced by significant urban industrialized emissions and an active photochemistry with very high ozone concentrations. Particle mass spectra were analyzed by positive matrix factorization (PMF2 and the results were in very good agreement with previous apportionments obtained using a chemical mass balance (CMB approach coupled to organic markers and metals (El Haddad et al., 2011a. AMS/PMF2 was able to identify for the first time, to the best of our knowledge, the organic aerosol emitted by industrial processes. Even with significant industries in the region, industrial OA was estimated to contribute only ~ 5% of the total OA mass. Both source apportionment techniques suggest that oxygenated OA (OOA constitutes the major fraction, contributing ~ 80% of OA mass. A novel approach combining AMS/PMF2 data with 14C measurements was applied to identify and quantify the fossil and non-fossil precursors of this fraction and to explicitly assess the related uncertainties. Results show with high statistical confidence that, despite extensive urban and industrial emissions, OOA is overwhelmingly non-fossil, formed via the oxidation of biogenic precursors, including monoterpenes. AMS/PMF2 results strongly suggest that the variability observed in the OOA chemical composition is mainly driven in our case by the aerosol photochemical age. This paper presents the impact of photochemistry on the increase of OOA oxygenation levels, formation of humic-like substances (HULIS and the evolution of α-pinene SOA (secondary OA components.

  19. Sub-Antarctic marine aerosol: dominant contributions from biogenic sources

    Directory of Open Access Journals (Sweden)

    J. Schmale

    2013-09-01

    Full Text Available Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS, was 21% non-sea-salt sulfate, 2% nitrate, 8% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea spray signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA profiles could be isolated: an amino acid/amine factor (AA-OA, 18% of OA mass, a methanesulfonic acid OA factor (MSA-OA, 25%, a marine oxygenated OA factor (M-OOA, 41%, a sea spray OA fraction (SS-OA, 7% and locally produced hydrocarbon-like OA (HOA, 9%. The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (N : C ratio = 0.13, has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea spray aerosol was identified (SS-OA. However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not

  20. Global distribution and climate forcing of marine organic aerosol: 1. Model improvements and evaluation

    Directory of Open Access Journals (Sweden)

    N. Meskhidze

    2011-11-01

    Full Text Available Marine organic aerosol emissions have been implemented and evaluated within the National Center of Atmospheric Research (NCAR's Community Atmosphere Model (CAM5 with the Pacific Northwest National Laboratory's 7-mode Modal Aerosol Module (MAM-7. Emissions of marine primary organic aerosols (POA, phytoplankton-produced isoprene- and monoterpenes-derived secondary organic aerosols (SOA and methane sulfonate (MS are shown to affect surface concentrations of organic aerosols in remote marine regions. Global emissions of submicron marine POA is estimated to be 7.9 and 9.4 Tg yr−1, for the Gantt et al. (2011 and Vignati et al. (2010 emission parameterizations, respectively. Marine sources of SOA and particulate MS (containing both sulfur and carbon atoms contribute an additional 0.2 and 5.1 Tg yr−1, respectively. Widespread areas over productive waters of the Northern Atlantic, Northern Pacific, and the Southern Ocean show marine-source submicron organic aerosol surface concentrations of 100 ng m−3, with values up to 400 ng m−3 over biologically productive areas. Comparison of long-term surface observations of water insoluble organic matter (WIOM with POA concentrations from the two emission parameterizations shows that despite revealed discrepancies (often more than a factor of 2, both Gantt et al. (2011 and Vignati et al. (2010 formulations are able to capture the magnitude of marine organic aerosol concentrations, with the Gantt et al. (2011 parameterization attaining better seasonality. Model simulations show that the mixing state of the marine POA can impact the surface number concentration of cloud condensation nuclei (CCN. The largest increases (up to 20% in CCN (at a supersaturation (S of 0.2% number concentration are obtained over biologically productive ocean waters when marine organic aerosol is assumed to be externally mixed with sea-salt. Assuming

  1. Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model

    Directory of Open Access Journals (Sweden)

    G. W. Mann

    2010-10-01

    Full Text Available A new version of the Global Model of Aerosol Processes (GLOMAP is described, which uses a two-moment pseudo-modal aerosol dynamics approach rather than the original two-moment bin scheme. GLOMAP-mode simulates the multi-component global aerosol, resolving sulfate, sea-salt, dust, black carbon (BC and particulate organic matter (POM, the latter including primary and biogenic secondary POM. Aerosol processes are simulated in a size-resolved manner including primary emissions, secondary particle formation by binary homogeneous nucleation of sulfuric acid and water, particle growth by coagulation, condensation and cloud-processing and removal by dry deposition, in-cloud and below-cloud scavenging. A series of benchmark observational datasets are assembled against which the skill of the model is assessed in terms of normalised mean bias (b and correlation coefficient (R. Overall, the model performs well against the datasets in simulating concentrations of aerosol precursor gases, chemically speciated particle mass, condensation nuclei (CN and cloud condensation nuclei (CCN. Surface sulfate, sea-salt and dust mass concentrations are all captured well, while BC and POM are biased low (but correlate well. Surface CN concentrations compare reasonably well in free troposphere and marine sites, but are underestimated at continental and coastal sites related to underestimation of either primary particle emissions or new particle formation. The model compares well against a compilation of CCN observations covering a range of environments and against vertical profiles of size-resolved particle concentrations over Europe. The simulated global burden, lifetime and wet removal of each of the simulated aerosol components is also examined and each lies close to multi-model medians from the AEROCOM model intercomparison exercise.

  2. Zirconia nanocrystals as submicron level biological label

    Science.gov (United States)

    Smits, K.; Liepins, J.; Gavare, M.; Patmalnieks, A.; Gruduls, A.; Jankovica, D.

    2012-08-01

    Inorganic nanocrystals are of increasing interest for their usage in biology and pharmacology research. Our interest was to justify ZrO2 nanocrystal usage as submicron level biological label in baker's yeast Saccharomyces cerevisia culture. For the first time (to our knowledge) images with sub micro up-conversion luminescent particles in biologic media were made. A set of undoped as well as Er and Yb doped ZrO2 samples at different concentrations were prepared by sol-gel method. The up-conversion luminescence for free standing and for nanocrystals with baker's yeast cells was studied and the differences in up-conversion luminescence spectra were analyzed. In vivo toxic effects of ZrO2 nanocrystals were tested by co-cultivation with baker's yeast.

  3. Aerosol gels

    Science.gov (United States)

    Sorensen, Christopher M. (Inventor); Chakrabarti, Amitabha (Inventor); Dhaubhadel, Rajan (Inventor); Gerving, Corey (Inventor)

    2010-01-01

    An improved process for the production of ultralow density, high specific surface area gel products is provided which comprises providing, in an enclosed chamber, a mixture made up of small particles of material suspended in gas; the particles are then caused to aggregate in the chamber to form ramified fractal aggregate gels. The particles should have a radius (a) of up to about 50 nm and the aerosol should have a volume fraction (f.sub.v) of at least 10.sup.-4. In preferred practice, the mixture is created by a spark-induced explosion of a precursor material (e.g., a hydrocarbon) and oxygen within the chamber. New compositions of matter are disclosed having densities below 3.0 mg/cc.

  4. A novel inlet system for online chemical analysis of semi-volatile submicron particulate matter

    Science.gov (United States)

    Eichler, P.; Müller, M.; D'Anna, B.; Wisthaler, A.

    2015-03-01

    We herein present a novel modular inlet system designed to be coupled to low-pressure gas analyzers for online chemical characterization of semi-volatile submicron particles. The "chemical analysis of aerosol online" (CHARON) inlet consists of a gas-phase denuder for stripping off gas-phase analytes, an aerodynamic lens for particle collimation combined with an inertial sampler for the particle-enriched flow and a thermodesorption unit for particle volatilization prior to chemical analysis. The denuder was measured to remove gas-phase organics with an efficiency > 99.999% and to transmit particles in the 100-750 nm size range with a 75-90% efficiency. The measured average particle enrichment factor in the subsampling flow from the aerodynamic lens was 25.6, which is a factor of 3 lower than the calculated theoretical optimum. We coupled the CHARON inlet to a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS) which quantitatively detects most organic analytes and ammonia. The combined CHARON-PTR-ToF-MS setup is thus capable of measuring both the organic and the ammonium fraction in submicron particles in real time. Individual organic compounds can be detected down to levels of 10-20 ng m-3. Two proof-of-principle studies were carried out for demonstrating the analytical power of this new instrumental setup: (i) oxygenated organics and their partitioning between the gas and the particulate phase were observed from the reaction of limonene with ozone and (ii) nicotine was measured in cigarette smoke particles demonstrating that selected organic target compounds can be detected in submicron particles in real time.

  5. One year online chemical speciation of submicron particulate matter (PM1) sampled at a French industrial and coastal site

    Science.gov (United States)

    Zhang, Shouwen; Riffault, Véronique; Dusanter, Sébastien; Augustin, Patrick; Fourmentin, Marc; Delbarre, Hervé

    2015-04-01

    The harbor of Dunkirk (Northern France) is surrounded by different industrial plants (metallurgy, petrochemistry, food processing, power plant, etc.), which emit gaseous and particulate pollutants such as Volatile Organic Compounds (VOCs), oxides of nitrogen (NOx) and sulfur (SO2), and submicron particles (PM1). These emissions are poorly characterized and their impact on neighboring urban areas has yet to be assessed. Studies are particularly needed in this type of complex environments to get a better understanding of PM1sources, especially from the industrial sector, their temporal variability, and their transformation. Several instruments, capable of real-time measurements (temporal resolution ≤ 30 min), were deployed at a site located downwind from the industrial area of Dunkirk for a one-year duration (July 2013-September 2014). An Aerosol Chemical Speciation Monitor (ACSM) and an Aethalometer monitored the main chemical species in the non-refractory submicron particles and black carbon, respectively. Concomitant measurements of trace gases and wind speed and direction were also performed. This dataset was analyzed considering four wind sectors, characteristics of marine, industrial, industrial-urban, and urban influences, and the different seasons. We will present a descriptive analysis of PM1, showing strong variations of ambient concentrations, as well as evidences of SO2 to SO4 gas-particle conversion when industrial plumes reached the monitoring site. The organic fraction measured by ACSM (37% of the total mass on average) was analyzed using a source-receptor model based on Positive Matrix Factorization (PMF) to identify chemical signatures of main emission sources and to quantify the contribution of each source to the PM1 budget given the wind sector. Four main factors were identified: hydrocarbon organic aerosol (HOA), oxygenated organic aerosol (OOA), biomass burning organic aerosol (BBOA) and cooking-like organic aerosol (COA). Overall, the total PM

  6. Analysis of Fine and Coarse mode Aerosol Distributions from AERONET's mini-DRAGON Set-up at Singapore 2012

    Science.gov (United States)

    Salinas Cortijo, S. V.; Chew, B. N.; Muller, A.; Liew, S.

    2013-12-01

    Aerosol optical depth combined with the Angstrom exponent and its derivative, are often used as a qualitative indicator of aerosol type and particle size regime. In Singapore, the sources of aerosols are mostly from fossil fuel burning (energy stations, incinerators, urban transport etc.) and from industrial and urban areas. However, depending on the time of the year (July-October), there can be a strong bio-mass component originated from uncontrolled forest/plantation fires from the neighboring land masses of Sumatra and Borneo. Unlike urban/fossil fuel aerosols, smoke or bio-mass related aerosol particles are typically characterized by showing a large optical depth and small, sub-micron particle size distributions. Trans-boundary smoke episodes has become an annual phenomenon in this region. Severe episodes were recorded in 1997 and 2006 and other minor episodes happened during 2002, 2004, 2010 and more recently on 2013. On August-September 2012, as part of CRISP participation on the August-September ground campaign of the Southeast Asia Composition, Cloud Climate Coupling Regional Study (SEAC4RS), a Distributed Regional Aerosol Gridded Observation Networks (DRAGON) set of six CIMEL CE-318A automatic Sun-tracking photometers have been deployed at sites located at North (Yishun ITE), East (Temasek Poly), West (NUS and Pandan Reservoir), Central (NEA) and South (St. John's island) of Singapore. In order to fully discriminate bio-mass burning events over other local sources, we perform a spectral discrimination of fine/coarse mode particle regime to all DRAGON sites; subsequently, the fine mode parameters such as optical depth, optical ratio and fine mode Angstrom exponent are used to identify possible bio-mass related events within the data set. Spatio-temporal relationship between sites are also investigated.

  7. Direct shortwave forcing of climate by anthropogenic sulfate aerosol: Sensitivity to particle size, composition, and relative humidity

    Energy Technology Data Exchange (ETDEWEB)

    Nemesure, S.; Wagener, R.; Schwartz, S.E. [Brookhaven National Lab., Upton, New York (United States)

    1996-04-01

    Recent estimates of global or hemispheric average forcing of climate by anthropogenic sulfate aerosol due to scattering of shortwave radiation are uncertain by more than a factor of 2. This paper examines the sensitivity of forcing to these microphysical properties for the purposes of obtaining a better understanding of the properties required to reduce the uncertainty in the forcing.

  8. Aerosol time-series measurements over the tropical Northeast Atlantic Ocean: Dust sources, elemental composition and mineralogy

    NARCIS (Netherlands)

    Patey, M.D.; Achterberg, E.P.; Rijkenberg, M.J.; Pearce, R.

    2015-01-01

    The North Atlantic receives the largest dust loading of any of the world's oceans due to its proximity to North African deserts and prevailing wind patterns. The supply of biologically important trace elements and nutrients via aerosols has an important influence on biogeochemical processes and

  9. Classifying aerosol type using in situ surface spectral aerosol optical properties

    Science.gov (United States)

    Schmeisser, Lauren; Andrews, Elisabeth; Ogren, John A.; Sheridan, Patrick; Jefferson, Anne; Sharma, Sangeeta; Kim, Jeong Eun; Sherman, James P.; Sorribas, Mar; Kalapov, Ivo; Arsov, Todor; Angelov, Christo; Mayol-Bracero, Olga L.; Labuschagne, Casper; Kim, Sang-Woo; Hoffer, András; Lin, Neng-Huei; Chia, Hao-Ping; Bergin, Michael; Sun, Junying; Liu, Peng; Wu, Hao

    2017-10-01

    Knowledge of aerosol size and composition is important for determining radiative forcing effects of aerosols, identifying aerosol sources and improving aerosol satellite retrieval algorithms. The ability to extrapolate aerosol size and composition, or type, from intensive aerosol optical properties can help expand the current knowledge of spatiotemporal variability in aerosol type globally, particularly where chemical composition measurements do not exist concurrently with optical property measurements. This study uses medians of the scattering Ångström exponent (SAE), absorption Ångström exponent (AAE) and single scattering albedo (SSA) from 24 stations within the NOAA/ESRL Federated Aerosol Monitoring Network to infer aerosol type using previously published aerosol classification schemes.Three methods are implemented to obtain a best estimate of dominant aerosol type at each station using aerosol optical properties. The first method plots station medians into an AAE vs. SAE plot space, so that a unique combination of intensive properties corresponds with an aerosol type. The second typing method expands on the first by introducing a multivariate cluster analysis, which aims to group stations with similar optical characteristics and thus similar dominant aerosol type. The third and final classification method pairs 3-day backward air mass trajectories with median aerosol optical properties to explore the relationship between trajectory origin (proxy for likely aerosol type) and aerosol intensive parameters, while allowing for multiple dominant aerosol types at each station.The three aerosol classification methods have some common, and thus robust, results. In general, estimating dominant aerosol type using optical properties is best suited for site locations with a stable and homogenous aerosol population, particularly continental polluted (carbonaceous aerosol), marine polluted (carbonaceous aerosol mixed with sea salt) and continental dust/biomass sites

  10. Classifying aerosol type using in situ surface spectral aerosol optical properties

    Directory of Open Access Journals (Sweden)

    L. Schmeisser

    2017-10-01

    Full Text Available Knowledge of aerosol size and composition is important for determining radiative forcing effects of aerosols, identifying aerosol sources and improving aerosol satellite retrieval algorithms. The ability to extrapolate aerosol size and composition, or type, from intensive aerosol optical properties can help expand the current knowledge of spatiotemporal variability in aerosol type globally, particularly where chemical composition measurements do not exist concurrently with optical property measurements. This study uses medians of the scattering Ångström exponent (SAE, absorption Ångström exponent (AAE and single scattering albedo (SSA from 24 stations within the NOAA/ESRL Federated Aerosol Monitoring Network to infer aerosol type using previously published aerosol classification schemes.Three methods are implemented to obtain a best estimate of dominant aerosol type at each station using aerosol optical properties. The first method plots station medians into an AAE vs. SAE plot space, so that a unique combination of intensive properties corresponds with an aerosol type. The second typing method expands on the first by introducing a multivariate cluster analysis, which aims to group stations with similar optical characteristics and thus similar dominant aerosol type. The third and final classification method pairs 3-day backward air mass trajectories with median aerosol optical properties to explore the relationship between trajectory origin (proxy for likely aerosol type and aerosol intensive parameters, while allowing for multiple dominant aerosol types at each station.The three aerosol classification methods have some common, and thus robust, results. In general, estimating dominant aerosol type using optical properties is best suited for site locations with a stable and homogenous aerosol population, particularly continental polluted (carbonaceous aerosol, marine polluted (carbonaceous aerosol mixed with sea salt and continental dust

  11. Impact of sea-salt emissions on the model performance and aerosol chemical composition and deposition in the East Mediterranean coastal regions

    Science.gov (United States)

    Im, Ulas

    2013-08-01

    East Mediterranean region is often exposed to significant levels of particulate matter (PM), partly due to the natural emission sources surrounding the area. The complex coastal geography together with the high water coverage of the area implies important contribution of sea-salt aerosols (SSA) to the PM levels and composition. WRF-CMAQ air quality modeling system has been employed to simulate and quantify the impacts of SSA emissions on the model performance in the region. The results show up to one order of magnitude higher SSA emissions when surf-zone emissions are added. 10-20% improvements are calculated in terms of model discrepancies of PM10 mass with regards to the observations. SSA related particles (sodium (Na+) and chloride (Cl-)) are more realistically represented. The total nitrate (NO3-) partitioning ratio increases substantially up to 0.5 on average when SSA emissions are inserted to the model, leading to nitric acid (HNO3) levels decrease by more than 40% and total NO3- aerosols increase by more than an order of magnitude over the source areas. Adding surf-zone emissions over those from open-ocean increase PM10 deposition by up to 11% and wet deposition by around 1%. The results suggest that coastal areas are important sources of SSA emissions and can significantly alter the PM levels and composition in their vicinities.

  12. Organic aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Penner, J.E.

    1994-01-01

    Organic aerosols scatter solar radiation. They may also either enhance or decrease concentrations of cloud condensation nuclei. This paper summarizes observed concentrations of aerosols in remote continental and marine locations and provides estimates for the sources of organic aerosol matter. The anthropogenic sources of organic aerosols may be as large as the anthropogenic sources of sulfate aerosols, implying a similar magnitude of direct forcing of climate. The source estimates are highly uncertain and subject to revision in the future. A slow secondary source of organic aerosols of unknown origin may contribute to the observed oceanic concentrations. The role of organic aerosols acting as cloud condensation nuclei (CCN) is described and it is concluded that they may either enhance or decrease the ability of anthropogenic sulfate aerosols to act as CCN.

  13. The ToF-ACSM: a portable aerosol chemical speciation monitor with TOFMS detection

    Science.gov (United States)

    Fröhlich, R.; Cubison, M. J.; Slowik, J. G.; Bukowiecki, N.; Prévôt, A. S. H.; Baltensperger, U.; Schneider, J.; Kimmel, J. R.; Gonin, M.; Rohner, U.; Worsnop, D. R.; Jayne, J. T.

    2013-11-01

    We present a new instrument for monitoring aerosol composition, the time-of-flight aerosol chemical speciation monitor (ToF-ACSM), combining precision state-of-the-art time-of-flight mass spectrometry with stability, reliability, and easy handling, which are necessities for long-term monitoring operations on the scale of months to years. Based on Aerodyne aerosol mass spectrometer (AMS) technology, the ToF-ACSM provides continuous online measurements of chemical composition and mass of non-refractory submicron aerosol particles. In contrast to the larger AMS, the compact-sized and lower-priced ToF-ACSM does not feature particle sizing, similar to the widely-used quadrupole-ACSM (Q-ACSM). Compared to the Q-ACSM, the ToF-ACSM features a better mass resolution of M/ΔM = 600 and better detection limits on the order of trained personnel on site. Intercomparisons with Q-ACSM, C-ToF-AMS, nephelometer and scanning mobility particle sizer (SMPS) measurements, performed during a first long-term deployment (> 10 months) on the Jungfraujoch mountain ridge (3580 m a.s.l.) in the Swiss Alps, agree quantitatively. Additionally, the mass resolution of the ToF-ACSM is sufficient for basic mass defect resolved peak fitting of the recorded spectra, providing a data stream not accessible to the Q-ACSM. This allows for quantification of certain hydrocarbon and oxygenated fragments (e.g. C3H7+ and C2H3O+, both occurring at m/Q = 43 Th), as well as improving inorganic/organic separation.

  14. Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation

    Directory of Open Access Journals (Sweden)

    E. Asmi

    2010-05-01

    Full Text Available The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.

  15. Inferring the composition and concentration of aerosols by combining the AERONET, MPLNET and CALIOP data: comparison with in-situ measurements and utilization to evaluate and improve GCM results

    Science.gov (United States)

    Ganguly, D.; Ginoux, P. A.; Ramaswamy, V.

    2009-12-01

    We present a method to derive the concentration of aerosol components using the spectral measurements of AOD (aerosol optical depth) and single scattering albedo along with their size distribution and extinction profile available from AERONET (Aerosol Robotic Network) and MPLNET (Micro-pulse Lidar Network) stations as well as the space borne CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) lidar [Ganguly et al., 2009a; 2009b]. The technique involves finding the best combination of aerosol concentration by minimizing differences between measured and calculated spectral variation in AOD and single scattering albedo along with the size distribution of aerosols over specific locations. Lidar data on extinction profile provides the vertical constraint on the distribution of aerosols in the atmosphere. Relative humidity from NCEP reanalysis is used to compute the hygroscopic growth factors and associated changes in the optical properties of aerosol components at all vertical levels. The technique has been successfully applied over different regions around the world such as North America, Southern Africa and South Asia. The results have been validated using in-situ measurements of aerosol composition available from the first two regions. Finally, we show how these results are being used to evaluate and improve the GFDL-AM2/AM3 climate model simulations. We believe our technique could also be used for the retrieval of air quality by calculating PM2.5 and PM10 concentrations. This could improve the existing methods by providing a better relation between surface measurements of PM2.5 concentration and satellite data. References: Ganguly, D., P. Ginoux, V. Ramaswamy, O. Dubovik, J. Welton, E. A. Reid and B. N. Holben (2009a), Inferring the composition and concentration of aerosols by combining AERONET and MPLNET data: comparison with other measurements and utilization to evaluate GCM output, J. Geophys. Res., 114, D16203, doi:10.1029/2009JD011895. Ganguly, D., P

  16. Optical-microphysical properties of Saharan dust aerosols and composition relationship using a multi-wavelength Raman lidar, in situ sensors and modelling: a case study analysis

    Science.gov (United States)

    Papayannis, A.; Mamouri, R. E.; Amiridis, V.; Remoundaki, E.; Tsaknakis, G.; Kokkalis, P.; Veselovskii, I.; Kolgotin, A.; Nenes, A.; Fountoukis, C.

    2012-05-01

    A strong Saharan dust event that occurred over the city of Athens, Greece (37.9° N, 23.6° E) between 27 March and 3 April 2009 was followed by a synergy of three instruments: a 6-wavelength Raman lidar, a CIMEL sun-sky radiometer and the MODIS sensor. The BSC-DREAM model was used to forecast the dust event and to simulate the vertical profiles of the aerosol concentration. Due to mixture of dust particles with low clouds during most of the reported period, the dust event could be followed by the lidar only during the cloud-free day of 2 April 2009. The lidar data obtained were used to retrieve the vertical profile of the optical (extinction and backscatter coefficients) properties of aerosols in the troposphere. The aerosol optical depth (AOD) values derived from the CIMEL ranged from 0.33-0.91 (355 nm) to 0.18-0.60 (532 nm), while the lidar ratio (LR) values retrieved from the Raman lidar ranged within 75-100 sr (355 nm) and 45-75 sr (532 nm). Inside a selected dust layer region, between 1.8 and 3.5 km height, mean LR values were 83 ± 7 and 54 ± 7 sr, at 355 and 532 nm, respectively, while the Ångström-backscatter-related (ABR355/532) and Ångström-extinction-related (AER355/532) were found larger than 1 (1.17 ± 0.08 and 1.11 ± 0.02, respectively), indicating mixing of dust with other particles. Additionally, a retrieval technique representing dust as a mixture of spheres and spheroids was used to derive the mean aerosol microphysical properties (mean and effective radius, number, surface and volume density, and mean refractive index) inside the selected atmospheric layers. Thus, the mean value of the retrieved refractive index was found to be 1.49( ± 0.10) + 0.007( ± 0.007)i, and that of the effective radiuses was 0.30 ± 0.18 μm. The final data set of the aerosol optical and microphysical properties along with the water vapor profiles obtained by Raman lidar were incorporated into the ISORROPIA II model to provide a possible aerosol composition

  17. Environmental Snapshots for Satellite Multi-Angle Aerosol Retrieval Validation During the ACE-Asia Field Campaign

    Science.gov (United States)

    Kahn, Ralph; Anderson, Jim; Anderson, Theodore L.; Bates, Tim; Brechtel, Fred; Clarke, Antony; Dutton, Ellsworth; Flagan, Richard; Fouin, Robert; Fukushima, Hajime

    2003-01-01

    On five occasions spanning the ACE-Asia field experiment in spring 2001, the multi-angle imaging MISR instrument, flying aboard the NASA Earth Observing System s Terra satellite, took quarter-kilometer data over a 400-km-wide swath, coincident with high-quality observations by multiple instruments on two or more participating surface and airborne platforms. The cases capture a range of clean, polluted, and dusty aerosol conditions. They represent some of the best opportunities during ACE- Asia for comparative studies among intensive and extensive aerosol observations in their environmental context. We inter-compare related measurements and discuss the implications of apparent discrepancies for each case, at a level of detail appropriate to the analysis of satellite observations. With a three-stage optical modeling process, we synthesize data from multiple sources into layer-by-layer snapshots that summarize what we know about the state of the atmosphere and surface at key locations during each event, to be used for satellite vicarious calibration and aerosol retrieval validation. Aerosols within a few kilometers of the surface were composed primarily of pollution and Asian dust mixtures, as expected. Accumulation and coarse-mode particle size distributions varied little among the events studied, but column aerosol optical depth changed by more than a factor of four, and the near-surface proportion of dust ranged from about 25% to 50%. The amount of absorbing material in the sub-micron fraction was highest when near-surface winds crossed Beijing and the Korean Peninsula, and was considerably lower for all other cases. Ambiguities remain in segregating size distributions by composition; having simultaneous single scattering albedo measurements at more than a single wavelength would significantly reduce the resulting optical model uncertainties, as would integral constraints from surface and atmospheric radiative flux observations. The consistency of component

  18. Hygroscopic Behavior of Multicomponent Aerosols Involving NaCl and Dicarboxylic Acids.

    Science.gov (United States)

    Peng, Chao; Jing, Bo; Guo, Yu-Cong; Zhang, Yun-Hong; Ge, Mao-Fa

    2016-02-25

    Atmospheric aerosols are usually complex mixtures of inorganic and organic compounds. The hygroscopicity of mixed particles is closely related to their chemical composition and interactions between components, which is still poorly understood. In this study, the hygroscopic properties of submicron particles composed of NaCl and dicarboxylic acids including oxalic acid (OA), malonic acid (MA), and succinic acid (SA) with various mass ratios are investigated with a hygroscopicity tandem differential mobility analyzer (HTDMA) system. Both the Zdanovskii-Stokes-Robinson (ZSR) method and extended aerosol inorganics model (E-AIM) are applied to predict the water uptake behaviors of sodium chloride/dicarboxylic acid mixtures. For NaCl/OA mixed particles, the measured growth factors were significantly lower than predictions from the model methods, indicating a change in particle composition caused by chloride depletion. The hygroscopic growth of NaCl/MA particles was well described by E-AIM, and that of NaCl/SA particles was dependent upon mixing ratio. Compared with model predictions, it was determined that water uptake of the NaCl/OA mixture could be enhanced and could be closer to the predictions by addition of levoglucosan or malonic acid, which retained water even at low relative humidity (RH), leading to inhibition of HCl evaporation during dehydration. These results demonstrate that the coexisting hygroscopic species have a strong influence on the phase state of particles, thus affecting chemical interactions between inorganic and organic compounds as well as the overall hygroscopicity of mixed particles.

  19. Submicron particle mass concentrations and sources in the Amazonian wet season (AMAZE-08)

    Science.gov (United States)

    Chen, Q.; Farmer, D. K.; Rizzo, L. V.; Pauliquevis, T.; Kuwata, M.; Karl, T. G.; Guenther, A.; Allan, J. D.; Coe, H.; Andreae, M. O.; Pöschl, U.; Jimenez, J. L.; Artaxo, P.; Martin, S. T.

    2015-04-01

    Real-time mass spectra of the non-refractory species in submicron aerosol particles were recorded in a tropical rainforest in the central Amazon Basin during the wet season from February to March 2008, as a part of the Amazonian Aerosol Characterization Experiment (AMAZE-08). Organic material accounted on average for more than 80% of the non-refractory submicron particle mass concentrations during the period of measurements. There was insufficient ammonium to neutralize sulfate. In this acidic, isoprene-rich, HO2-dominant environment, positive-matrix factorization of the time series of particle mass spectra identified four statistical factors to account for the 99% of the variance in the signal intensities of the organic constituents. The first factor was identified as associated with regional and local pollution and labeled "HOA" for its hydrocarbon-like characteristics. A second factor was associated with long-range transport and labeled "OOA-1" for its oxygenated characteristics. A third factor, labeled "OOA-2," was implicated as associated with the reactive uptake of isoprene oxidation products, especially of epoxydiols to acidic haze, fog, or cloud droplets. A fourth factor, labeled "OOA-3," was consistent with an association with the fresh production of secondary organic material (SOM) by the mechanism of gas-phase oxidation of biogenic volatile organic precursors followed by gas-to-particle conversion of the oxidation products. The suffixes 1, 2, and 3 on the OOA labels signify ordinal ranking with respect to the extent of oxidation represented by the factor. The process of aqueous-phase oxidation of water-soluble products of gas-phase photochemistry might also have been associated to some extent with the OOA-2 factor. The campaign-average factor loadings had a ratio of 1.4:1 for OOA-2 : OOA-3, suggesting the comparable importance of particle-phase compared to gas-phase pathways for the production of SOM during the study period.

  20. Submicron particle mass concentrations and sources in the Amazonian wet season (AMAZE-08)

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Q.; Farmer, D. K.; Rizzo, L. V.; Pauliqueivis, T.; Kuwata, Mikinori; Karl, Thomas G.; Guenther, Alex B.; Allan, James D.; Coe, H.; Andreae, M. O.; Poeschl, U.; Jiminez, J. L.; Artaxo, Paulo; Martin, Scot T.

    2015-01-01

    Real-time mass spectra of non-refractory component of submicron aerosol particles were recorded in a tropical rainforest in the central Amazon basin during the wet season of 2008, as a part of the Amazonian Aerosol Characterization Experiment (AMAZE-08). Organic components accounted on average for more than 80% of the non-refractory submicron particle mass concentrations during the period of measurements. Ammonium was present in sufficient quantities to halfway neutralize sulfate. In this acidic, isoprene-dominated, low-NOx environment the high-resolution mass spectra as well as mass closures with ion chromatography measurements did not provide evidence for significant contributions of organosulfate species, at least at concentrations above uncertainty levels. Positive-matrix factorization of the time series of particle mass spectra identified four statistical factors to account for the variance of the signal intensities of the organic constituents: a factor HOA having a hydro