Simulating Aerosol Size Distribution and Mass Concentration with Simultaneous Nucleation, Condensation/Coagulation, and Deposition with the GRAPES-CUACE

Science.gov (United States)

Zhou, Chunhong; Shen, Xiaojing; Liu, Zirui; Zhang, Yangmei; Xin, Jinyuan

2018-04-01

A coupled aerosol-cloud model is essential for investigating the formation of haze and fog and the interaction of aerosols with clouds and precipitation. One of the key tasks of such a model is to produce correct mass and number size distributions of aerosols. In this paper, a parameterization scheme for aerosol size distribution in initial emission, which took into account the measured mass and number size distributions of aerosols, was developed in the GRAPES-CUACE [Global/Regional Assimilation and PrEdiction System-China Meteorological Administration (CMA) Unified Atmospheric Chemistry Environment model]—an online chemical weather forecast system that contains microphysical processes and emission, transport, and chemical conversion of sectional multi-component aerosols. In addition, the competitive mechanism between nucleation and condensation for secondary aerosol formation was improved, and the dry deposition was also modified to be in consistent with the real depositing length. Based on the above improvements, the GRAPES-CUACE simulations were verified against observational data during 1-31 January 2013, when a series of heavy regional haze-fog events occurred in eastern China. The results show that the aerosol number size distribution from the improved experiment was much closer to the observation, whereas in the old experiment the number concentration was higher in the nucleation mode and lower in the accumulation mode. Meanwhile, the errors in aerosol number size distribution as diagnosed by its sectional mass size distribution were also reduced. Moreover, simulations of organic carbon, sulfate, and other aerosol components were improved and the overestimation as well as underestimation of PM2.5 concentration in eastern China was significantly reduced, leading to increased correlation coefficient between simulated and observed PM2.5 by more than 70%. In the remote areas where bad simulation results were produced previously, the correlation coefficient

Miniature Sensor for Aerosol Mass Measurements, Phase I

Data.gov (United States)

National Aeronautics and Space Administration — This SBIR project seeks to develop a miniature sensor for mass measurement of size-classified aerosols. A cascade impactor will be used to classify aerosol sample...

Testing of an automated online EA-IRMS method for fast and simultaneous carbon content and stable isotope measurement of aerosol samples

Science.gov (United States)

Major, István; Gyökös, Brigitta; Túri, Marianna; Futó, István; Filep, Ágnes; Hoffer, András; Molnár, Mihály

2016-04-01

Comprehensive atmospheric studies have demonstrated that carbonaceous aerosol is one of the main components of atmospheric particulate matter over Europe. Various methods, considering optical or thermal properties, have been developed for quantification of the accurate amount of both organic and elemental carbon constituents of atmospheric aerosol. The aim of our work was to develop an alternative fast and easy method for determination of the total carbon content of individual aerosol samples collected on prebaked quartz filters whereby the mass and surface concentration becomes simply computable. We applied the conventional "elemental analyzer (EA) coupled online with an isotope ratio mass spectrometer (IRMS)" technique which is ubiquitously used in mass spectrometry. Using this technique we are able to measure simultaneously the carbon stable isotope ratio of the samples, as well. During the developing process, we compared the EA-IRMS technique with an off-line catalytic combustion method worked out previously at Hertelendi Laboratory of Environmental Studies (HEKAL). We tested the combined online total carbon content and stable isotope ratio measurement both on standard materials and real aerosol samples. Regarding the test results the novel method assures, on the one hand, at least 95% of carbon recovery yield in a broad total carbon mass range (between 100 and 3000 ug) and, on the other hand, a good reproducibility of stable isotope measurements with an uncertainty of ± 0.2 per mill. Comparing the total carbon results obtained by the EA-IRMS and the off-line catalytic combustion method we found a very good correlation (R2=0.94) that proves the applicability of both preparation method. Advantages of the novel method are the fast and simplified sample preparation steps and the fully automated, simultaneous carbon stable isotope ratio measurement processes. Furthermore stable isotope ratio results can effectively be applied in the source apportionment

Characterisation of organic compounds in aerosol particles from a finnish forest by on-line coupled supercritical fluid extraction-liquid chromatography-gas chromatography-mass spectrometry

Energy Technology Data Exchange (ETDEWEB)

Shimmo, Masahiko; Jaentti, Jaana; Hartonen, Kari; Hyoetylaeinen, Tuulia; Riekkola, Marja-Liisa [Laboratory of Analytical Chemistry, Department of Chemistry, University of Helsinki, P.O. Box 55, 00014, Helsinki (Finland); Aalto, Pasi; Kulmala, Markku [Division of Atmospheric Sciences, Department of Physical Sciences, University of Helsinki, P.O. Box 64, 00014, Helsinki (Finland)

2004-04-01

During the European Union project Quantification of Aerosol Nucleation in the European Boundary Layer (QUEST), which began in spring 2003, atmospheric aerosol particles were collected in a Finnish Scots pine forest using a high-volume sampler. The organic compounds in the filter samples were then analysed by on-line coupled supercritical fluid extraction-liquid chromatography-gas chromatography-mass spectrometry (SFE-LC-GC-MS). The sample was first extracted by SFE. During LC the extracts were fractionated into three fractions according to polarity. The final separation was carried out by GC-MS. A fraction volume as high as 840 {mu}L was transferred to the GC, using the partial concurrent eluent evaporation technique. The same instrumentation, with an in-situ SFE derivatisation method, was used to analyse organic acids. Major compounds such as n-alkanes and PAH were analysed quantitatively. Their concentrations were lower than those usually observed in urban areas or in other forest areas in Europe. The wind direction was one of the most important factors affecting changes in the daily concentrations of these compounds. Scots pine needles were analysed with the same system to obtain reference data for identification of biogenic compounds in aerosol particles. Other organic compounds found in this study included hopanes, steranes, n-alkanals, n-alkan-2-ones, oxy-PAH, and alkyl-PAH; some biogenic products, including oxidation products of monoterpenes, were also identified. (orig.)

Precision and accuracy of β gauge for aerosol mass determinations

International Nuclear Information System (INIS)

Courtney, W.J.; Shaw, R.W.; Dzabay, T.G.

1982-01-01

Results of an experimental determination of the precision and the accuracy of a β-ray attenuation method for measurement of aerosol mass are presented. The instrumental precision for a short-term experiment was 25 μg for a 6.5-cm 2 deposit collected on approximately 1 mg/cm 2 Teflon filters; for a longer-term experiment the precision was 27 μg. The precision of the gravimetric determinations of aerosol deposits was 22 μg for Teflon filters weighed to 1 μg. Filter reorientation and air density changes that were able adversely to affect the β-ray attenuation results are discussed. β-ray attenuation results are in good agreement with gravimetric measurements on the same filter-collected aerosols. Using dichotomous samplers in Durham, NC, we collected 136 aerosol samples on Teflon filters in two size ranges. A regression line was calculated implicitly assuming errors in both measurements of mass. The 90% confidence intervals lay within 21 μg of the regression line for mean fine fraction aerosol mass loadings of 536 μg and within 19 μg of the regression line for mean coarse fraction aerosol mass loadings of 349 μg. Any bias between gravimetric and β-gauge mass measurements was found to be less than 5%

Aerosol quantification with the Aerodyne Aerosol Mass Spectrometer: detection limits and ionizer background effects

Directory of Open Access Journals (Sweden)

S. Borrmann

2009-02-01

Full Text Available Systematic laboratory experiments were performed to investigate quantification of various species with two versions of the Aerodyne Aerosol Mass Spectrometer, a Quadrupole Aerosol Mass Spectrometer (Q-AMS and a compact Time-of-Flight Aerosol Mass Spectrometer (c-ToF-AMS. Here we present a new method to continuously determine the detection limits of the AMS analyzers during regular measurements, yielding detection limit (DL information under various measurement conditions. Minimum detection limits range from 0.03 μg m⁻³ (nitrate, sulfate, and chloride up to 0.5 μg m⁻³ (organics for the Q-AMS. Those of the c-ToF-AMS are found between 0.003 μg m⁻³ (nitrate, sulfate and 0.03 μg m⁻³ (ammonium, organics. The DL values found for the c-ToF-AMS were ~10 times lower than those of the Q-AMS, mainly due to differences in ion duty cycle. Effects causing an increase of the detection limits include long-term instrument contamination, measurement of high aerosol mass concentrations and short-term instrument history. The self-cleaning processes which reduce the instrument background after measurement of large aerosol concentrations as well as the influences of increased instrument background on mass concentration measurements are discussed. Finally, improvement of detection limits by extension of averaging time intervals, selected or reduced ion monitoring, and variation of particle-to-background measurement ratio are investigated.

Development and first application of an Aerosol Collection Module (ACM) for quasi online compound specific aerosol measurements

Science.gov (United States)

Hohaus, Thorsten; Kiendler-Scharr, Astrid; Trimborn, Dagmar; Jayne, John; Wahner, Andreas; Worsnop, Doug

2010-05-01

Atmospheric aerosols influence climate and human health on regional and global scales (IPCC, 2007). In many environments organics are a major fraction of the aerosol influencing its properties. Due to the huge variety of organic compounds present in atmospheric aerosol current measurement techniques are far from providing a full speciation of organic aerosol (Hallquist et al., 2009). The development of new techniques for compound specific measurements with high time resolution is a timely issue in organic aerosol research. Here we present first laboratory characterisations of an aerosol collection module (ACM) which was developed to allow for the sampling and transfer of atmospheric PM1 aerosol. The system consists of an aerodynamic lens system focussing particles on a beam. This beam is directed to a 3.4 mm in diameter surface which is cooled to -30 °C with liquid nitrogen. After collection the aerosol sample can be evaporated from the surface by heating it to up to 270 °C. The sample is transferred through a 60cm long line with a carrier gas. In order to test the ACM for linearity and sensitivity we combined it with a GC-MS system. The tests were performed with octadecane aerosol. The octadecane mass as measured with the ACM-GC-MS was compared versus the mass as calculated from SMPS derived total volume. The data correlate well (R2 0.99, slope of linear fit 1.1) indicating 100 % collection efficiency. From 150 °C to 270 °C no effect of desorption temperature on transfer efficiency could be observed. The ACM-GC-MS system was proven to be linear over the mass range 2-100 ng and has a detection limit of ~ 2 ng. First experiments applying the ACM-GC-MS system were conducted at the Jülich Aerosol Chamber. Secondary organic aerosol (SOA) was formed from ozonolysis of 600 ppbv of b-pinene. The major oxidation product nopinone was detected in the aerosol and could be shown to decrease from 2 % of the total aerosol to 0.5 % of the aerosol over the 48 hours of

Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry

Directory of Open Access Journals (Sweden)

J. Wang

2016-07-01

Full Text Available In this work, the Aerodyne soot particle – aerosol mass spectrometer (SP-AMS was deployed for the first time during the spring of 2015 in urban Nanjing, a megacity in the Yangtze River Delta (YRD of China, for online characterization of the submicron aerosols (PM1. The SP-AMS enables real-time and fast quantification of refractory black carbon (rBC simultaneously with other non-refractory species (ammonium, sulfate, nitrate, chloride, and organics. The average PM1 concentration was found to be 28.2 µg m−3, with organics (45 % as the most abundant component, following by sulfate (19.3 %, nitrate (13.6 %, ammonium (11.1 %, rBC (9.7 %, and chloride (1.3 %. These PM1 species together can reconstruct ∼ 44 % of the light extinction during this campaign based on the IMPROVE method. Chemically resolved mass-based size distributions revealed that small particles especially ultrafine ones (< 100 nm vacuum aerodynamic diameter were dominated by organics and rBC, while large particles had significant contributions from secondary inorganic species. Source apportionment of organic aerosols (OA yielded four OA subcomponents, including hydrocarbon-like OA (HOA, cooking-related OA (COA, semi-volatile oxygenated OA (SV-OOA, and low-volatility oxygenated OA (LV-OOA. Overall, secondary organic aerosol (SOA, equal to the sum of SV-OOA and LV-OOA dominated the total OA mass (55.5 %, but primary organic aerosol (POA, equal to the sum of HOA and COA can outweigh SOA in the early morning and evening due to enhanced human activities. High OA concentrations were often associated with high mass fractions of POA and rBC, indicating the important role of anthropogenic emissions during heavy pollution events. The diurnal cycles of nitrate, chloride, and SV-OOA both showed good anti-correlations with air temperatures, suggesting their variations were likely driven by thermodynamic equilibria and gas-to-particle partitioning. On the other hand

Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry

Science.gov (United States)

Wang, Junfeng; Ge, Xinlei; Chen, Yanfang; Shen, Yafei; Zhang, Qi; Sun, Yele; Xu, Jianzhong; Ge, Shun; Yu, Huan; Chen, Mindong

2016-07-01

In this work, the Aerodyne soot particle - aerosol mass spectrometer (SP-AMS) was deployed for the first time during the spring of 2015 in urban Nanjing, a megacity in the Yangtze River Delta (YRD) of China, for online characterization of the submicron aerosols (PM1). The SP-AMS enables real-time and fast quantification of refractory black carbon (rBC) simultaneously with other non-refractory species (ammonium, sulfate, nitrate, chloride, and organics). The average PM1 concentration was found to be 28.2 µg m-3, with organics (45 %) as the most abundant component, following by sulfate (19.3 %), nitrate (13.6 %), ammonium (11.1 %), rBC (9.7 %), and chloride (1.3 %). These PM1 species together can reconstruct ˜ 44 % of the light extinction during this campaign based on the IMPROVE method. Chemically resolved mass-based size distributions revealed that small particles especially ultrafine ones (cooking-related OA (COA), semi-volatile oxygenated OA (SV-OOA), and low-volatility oxygenated OA (LV-OOA). Overall, secondary organic aerosol (SOA, equal to the sum of SV-OOA and LV-OOA) dominated the total OA mass (55.5 %), but primary organic aerosol (POA, equal to the sum of HOA and COA) can outweigh SOA in the early morning and evening due to enhanced human activities. High OA concentrations were often associated with high mass fractions of POA and rBC, indicating the important role of anthropogenic emissions during heavy pollution events. The diurnal cycles of nitrate, chloride, and SV-OOA both showed good anti-correlations with air temperatures, suggesting their variations were likely driven by thermodynamic equilibria and gas-to-particle partitioning. On the other hand, in contrast to other species, sulfate, and LV-OOA concentrations increased in the afternoon, and showed no positive correlations with relative humidity (RH), likely indicating the contribution from photochemical oxidation is dominant over that of aqueous-phase processing for their formations. The

Characterization of urban aerosol using aerosol mass spectrometry and proton nuclear magnetic resonance spectroscopy

Science.gov (United States)

Cleveland, M. J.; Ziemba, L. D.; Griffin, R. J.; Dibb, J. E.; Anderson, C. H.; Lefer, B.; Rappenglück, B.

2012-07-01

Particulate matter was measured during August and September of 2006 in Houston as part of the Texas Air Quality Study II Radical and Aerosol Measurement Project. Aerosol size and composition were determined using an Aerodyne quadrupole aerosol mass spectrometer. Aerosol was dominated by sulfate (4.1 ± 2.6 μg m-3) and organic material (5.5 ± 4.0 μg m-3), with contributions of organic material from both primary (˜32%) and secondary (˜68%) sources. Secondary organic aerosol appears to be formed locally. In addition, 29 aerosol filter samples were analyzed using proton nuclear magnetic resonance (1H NMR) spectroscopy to determine relative concentrations of organic functional groups. Houston aerosols are less oxidized than those observed elsewhere, with smaller relative contributions of carbon-oxygen double bonds. These particles do not fit 1H NMR source apportionment fingerprints for identification of secondary, marine, and biomass burning organic aerosol, suggesting that a new fingerprint for highly urbanized and industrially influenced locations be established.

Characterization of aerosol particles from grass mowing by joint deployment of ToF-AMS and ATOFMS instruments

Science.gov (United States)

Drewnick, Frank; Dall'Osto, Manuel; Harrison, Roy

During a measurement campaign at a semi-urban/industrial site a grass-cutting event was observed, when the lawn in the immediate surrounding of the measurement site was mowed. Using a wide variety of state-of-the-art aerosol measurement technology allowed a broad characterization of the aerosol generated by the lawn mowing. The instrumentation included two on-line aerosol mass spectrometers: an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS) and a TSI Aerosol Time-of-Flight Mass Spectrometer (ATOFMS); in addition, a selection of on-line aerosol concentration and size distribution instruments (OPC, APS, SMPS, CPC, FDMS-TEOM, MAAP) was deployed. From comparison of background aerosol measurements during most of the day with the aerosol measured during the lawn mowing, the grass cutting was found to generate mainly two different types of aerosol particles: an intense ultrafine particle mode (1 h average: 4 μg m -3) of almost pure hydrocarbon-like organics and a distinct particle mode in the upper sub-micrometer size range containing particles with potassium and nitrogen-organic compounds. The ultrafine particles are probably lubricating oil particles from the lawn mower exhaust; the larger particles are swirled-up plant debris particles from the mowing process. While these particle types were identified in the data from the two mass spectrometers, the on-line aerosol concentration and size distribution data support these findings. The results presented here show that the combination of quantitative aerosol particle ensemble mass spectrometry (ToF-AMS) and single particle mass spectrometry (ATOFMS) provides much deeper insights into the nature of the aerosol properties than each of the instruments could do alone. Therefore a combined deployment of both types of instruments is strongly recommended.

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modeling of complete high time-resolution aerosol mass spectra

Science.gov (United States)

McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2014-08-01

Receptor modeling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's Canadian Regional and Urban Investigation System for Environmental Research (CRUISER) mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach compared to the more common method of analyzing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulfate- and oxygenated organic aerosol-containing factor (Sulfate-OA); an ammonium nitrate- and oxygenated organic aerosol-containing factor (Nitrate-OA); an ammonium chloride-containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analyzing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case the Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this

Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modelling of complete high time-resolution aerosol mass spectra

Science.gov (United States)

McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

2014-02-01

Receptor modelling was performed on quadrupole unit mass resolution aerosol mass spectrometer (Q-AMS) sub-micron particulate matter (PM) chemical speciation measurements from Windsor, Ontario, an industrial city situated across the Detroit River from Detroit, Michigan. Aerosol and trace gas measurements were collected on board Environment Canada's CRUISER mobile laboratory. Positive matrix factorization (PMF) was performed on the AMS full particle-phase mass spectrum (PMFFull MS) encompassing both organic and inorganic components. This approach was compared to the more common method of analysing only the organic mass spectra (PMFOrg MS). PMF of the full mass spectrum revealed that variability in the non-refractory sub-micron aerosol concentration and composition was best explained by six factors: an amine-containing factor (Amine); an ammonium sulphate and oxygenated organic aerosol containing factor (Sulphate-OA); an ammonium nitrate and oxygenated organic aerosol containing factor (Nitrate-OA); an ammonium chloride containing factor (Chloride); a hydrocarbon-like organic aerosol (HOA) factor; and a moderately oxygenated organic aerosol factor (OOA). PMF of the organic mass spectrum revealed three factors of similar composition to some of those revealed through PMFFull MS: Amine, HOA and OOA. Including both the inorganic and organic mass proved to be a beneficial approach to analysing the unit mass resolution AMS data for several reasons. First, it provided a method for potentially calculating more accurate sub-micron PM mass concentrations, particularly when unusual factors are present, in this case, an Amine factor. As this method does not rely on a priori knowledge of chemical species, it circumvents the need for any adjustments to the traditional AMS species fragmentation patterns to account for atypical species, and can thus lead to more complete factor profiles. It is expected that this method would be even more useful for HR-ToF-AMS data, due to the ability

Pollutants identification of ambient aerosols by two types of aerosol mass spectrometers over southeast coastal area, China.

Science.gov (United States)

Yan, Jinpei; Chen, Liqi; Lin, Qi; Zhao, Shuhui; Li, Lei

2018-02-01

Two different aerosol mass spectrometers, Aerodyne Aerosol Mass Spectrometer (AMS) and Single Particle Aerosol Mass Spectrometer (SPAMS) were deployed to identify the aerosol pollutants over Xiamen, representing the coastal urban area. Five obvious processes were classified during the whole observation period. Organics and sulfate were the dominant components in ambient aerosols over Xiamen. Most of the particles were in the size range of 0.2-1.0μm, accounting for over 97% of the total particles measured by both instruments. Organics, as well as sulfate, measured by AMS were in good correlation with measured by SPAMS. However, high concentration of NH 4 + was obtained by AMS, while extremely low value of NH 4 + was detected by SPAMS. Contrarily, high particle number counts of NO 3 - and Cl - were given by SPAMS while low concentrations of NO 3 - and Cl - were measured by AMS. The variations of POA and SOA obtained from SPAMS during event 1 and event 2 were in accordance with the analysis of HOA and OOA given by AMS, suggesting that both of AMS and SPAMS can well identify the organic clusters of aerosol particles. Overestimate or underestimate of the aerosol sources and acidity would be present in some circumstances when the measurement results were used to analyze the aerosol properties, because of the detection loss of some species for both instruments. Copyright © 2017. Published by Elsevier B.V.

Aerosol detection efficiency in inductively coupled plasma mass spectrometry

Science.gov (United States)

Hubbard, Joshua A.; Zigmond, Joseph A.

2016-05-01

An electrostatic size classification technique was used to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Size-segregated particles were counted with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized by the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10- 5 to 10- 11. Free molecular heat and mass transfer theory was applied, but

Secondary organic aerosol formation from in-use motor vehicle emissions using a potential aerosol mass reactor.

Science.gov (United States)

Tkacik, Daniel S; Lambe, Andrew T; Jathar, Shantanu; Li, Xiang; Presto, Albert A; Zhao, Yunliang; Blake, Donald; Meinardi, Simone; Jayne, John T; Croteau, Philip L; Robinson, Allen L

2014-10-07

Secondary organic aerosol (SOA) formation from in-use vehicle emissions was investigated using a potential aerosol mass (PAM) flow reactor deployed in a highway tunnel in Pittsburgh, Pennsylvania. Experiments consisted of passing exhaust-dominated tunnel air through a PAM reactor over integrated hydroxyl radical (OH) exposures ranging from ∼ 0.3 to 9.3 days of equivalent atmospheric oxidation. Experiments were performed during heavy traffic periods when the fleet was at least 80% light-duty gasoline vehicles on a fuel-consumption basis. The peak SOA production occurred after 2-3 days of equivalent atmospheric oxidation. Additional OH exposure decreased the SOA production presumably due to a shift from functionalization to fragmentation dominated reaction mechanisms. Photo-oxidation also produced substantial ammonium nitrate, often exceeding the mass of SOA. Analysis with an SOA model highlight that unspeciated organics (i.e., unresolved complex mixture) are a very important class of precursors and that multigenerational processing of both gases and particles is important at longer time scales. The chemical evolution of the organic aerosol inside the PAM reactor appears to be similar to that observed in the atmosphere. The mass spectrum of the unoxidized primary organic aerosol closely resembles ambient hydrocarbon-like organic aerosol (HOA). After aging the exhaust equivalent to a few hours of atmospheric oxidation, the organic aerosol most closely resembles semivolatile oxygenated organic aerosol (SV-OOA) and then low-volatility organic aerosol (LV-OOA) at higher OH exposures. Scaling the data suggests that mobile sources contribute ∼ 2.9 ± 1.6 Tg SOA yr(-1) in the United States, which is a factor of 6 greater than all mobile source particulate matter emissions reported by the National Emissions Inventory. This highlights the important contribution of SOA formation from vehicle exhaust to ambient particulate matter concentrations in urban areas.

Apportionment of urban aerosol sources in Cork (Ireland) by synergistic measurement techniques.

Science.gov (United States)

Dall'Osto, Manuel; Hellebust, Stig; Healy, Robert M; O'Connor, Ian P; Kourtchev, Ivan; Sodeau, John R; Ovadnevaite, Jurgita; Ceburnis, Darius; O'Dowd, Colin D; Wenger, John C

2014-09-15

The sources of ambient fine particulate matter (PM2.5) during wintertime at a background urban location in Cork city (Ireland) have been determined. Aerosol chemical analyses were performed by multiple techniques including on-line high resolution aerosol time-of-flight mass spectrometry (Aerodyne HR-ToF-AMS), on-line single particle aerosol time-of-flight mass spectrometry (TSI ATOFMS), on-line elemental carbon-organic carbon analysis (Sunset_EC-OC), and off-line gas chromatography/mass spectrometry and ion chromatography analysis of filter samples collected at 6-h resolution. Positive matrix factorization (PMF) has been carried out to better elucidate aerosol sources not clearly identified when analyzing results from individual aerosol techniques on their own. Two datasets have been considered: on-line measurements averaged over 2-h periods, and both on-line and off-line measurements averaged over 6-h periods. Five aerosol sources were identified by PMF in both datasets, with excellent agreement between the two solutions: (1) regional domestic solid fuel burning--"DSF_Regional," 24-27%; (2) local urban domestic solid fuel burning--"DSF_Urban," 22-23%; (3) road vehicle emissions--"Traffic," 15-20%; (4) secondary aerosols from regional anthropogenic sources--"SA_Regional" 9-13%; and (5) secondary aged/processed aerosols related to urban anthropogenic sources--"SA_Urban," 21-26%. The results indicate that, despite regulations for restricting the use of smoky fuels, solid fuel burning is the major source (46-50%) of PM2.5 in wintertime in Cork, and also likely other areas of Ireland. Whilst wood combustion is strongly associated with OC and EC, it was found that peat and coal combustion is linked mainly with OC and the aerosol from these latter sources appears to be more volatile than that produced by wood combustion. Ship emissions from the nearby port were found to be mixed with the SA_Regional factor. The PMF analysis allowed us to link the AMS cooking organic

Direct gravimetric determination of aerosol mass concentration in central antarctica.

Science.gov (United States)

Annibaldi, Anna; Truzzi, Cristina; Illuminati, Silvia; Scarponi, Giuseppe

2011-01-01

In Antarctica, experimental difficulties due to extreme conditions have meant that aerosol mass has rarely been measured directly by gravimetry, and only in coastal areas where concentrations were in the range of 1-7 μg m(-3). The present work reports on a careful differential weighing methodology carried out for the first time on the plateau of central Antarctica (Dome C, East Antarctica). To solve problems of accurate aerosol mass measurements, a climatic room was used for conditioning and weighing filters. Measurements were carried out in long stages of several hours of readings with automatic recording of temperature/humidity and mass. This experimental scheme allowed us to sample from all the measurements (up to 2000) carried out before and after exposure, those which were recorded under the most stable humidity conditions and, even more importantly, as close to each other as possible. The automatic reading of the mass allowed us in any case to obtain hundreds of measurements from which to calculate average values with uncertainties sufficiently low to meet the requirements of the differential weighing procedure (±0.2 mg in filter weighing, between ±7% and ±16% both in aerosol mass and concentration measurements). The results show that the average summer aerosol mass concentration (aerodynamic size ≤10 μm) in central Antarctica is about 0.1 μg m(-3), i.e., about 1/10 of that of coastal Antarctic areas. The concentration increases by about 4-5 times at a site very close to the station.

Online Simulations of Global Aerosol Distributions in the NASA GEOS-4 Model and Comparisons to Satellite and Ground-Based Aerosol Optical Depth

Science.gov (United States)

Colarco, Peter; daSilva, Arlindo; Chin, Mian; Diehl, Thomas

2010-01-01

We have implemented a module for tropospheric aerosols (GO CART) online in the NASA Goddard Earth Observing System version 4 model and simulated global aerosol distributions for the period 2000-2006. The new online system offers several advantages over the previous offline version, providing a platform for aerosol data assimilation, aerosol-chemistry-climate interaction studies, and short-range chemical weather forecasting and climate prediction. We introduce as well a methodology for sampling model output consistently with satellite aerosol optical thickness (AOT) retrievals to facilitate model-satellite comparison. Our results are similar to the offline GOCART model and to the models participating in the AeroCom intercomparison. The simulated AOT has similar seasonal and regional variability and magnitude to Aerosol Robotic Network (AERONET), Moderate Resolution Imaging Spectroradiometer, and Multiangle Imaging Spectroradiometer observations. The model AOT and Angstrom parameter are consistently low relative to AERONET in biomass-burning-dominated regions, where emissions appear to be underestimated, consistent with the results of the offline GOCART model. In contrast, the model AOT is biased high in sulfate-dominated regions of North America and Europe. Our model-satellite comparison methodology shows that diurnal variability in aerosol loading is unimportant compared to sampling the model where the satellite has cloud-free observations, particularly in sulfate-dominated regions. Simulated sea salt burden and optical thickness are high by a factor of 2-3 relative to other models, and agreement between model and satellite over-ocean AOT is improved by reducing the model sea salt burden by a factor of 2. The best agreement in both AOT magnitude and variability occurs immediately downwind of the Saharan dust plume.

Development of a method for fast and automatic radiocarbon measurement of aerosol samples by online coupling of an elemental analyzer with a MICADAS AMS

Energy Technology Data Exchange (ETDEWEB)

Salazar, G., E-mail: gary.salazar@dcb.unibe.ch [Department of Chemistry and Biochemistry & Oeschger Centre for Climate Change Research, University of Bern, 3012 Bern (Switzerland); Zhang, Y.L.; Agrios, K. [Department of Chemistry and Biochemistry & Oeschger Centre for Climate Change Research, University of Bern, 3012 Bern (Switzerland); Paul Scherrer Institut (PSI), 5232 Villigen (Switzerland); Szidat, S. [Department of Chemistry and Biochemistry & Oeschger Centre for Climate Change Research, University of Bern, 3012 Bern (Switzerland)

2015-10-15

A fast and automatic method for radiocarbon analysis of aerosol samples is presented. This type of analysis requires high number of sample measurements of low carbon masses, but accepts precisions lower than for carbon dating analysis. The method is based on online Trapping CO{sub 2} and coupling an elemental analyzer with a MICADAS AMS by means of a gas interface. It gives similar results to a previously validated reference method for the same set of samples. This method is fast and automatic and typically provides uncertainties of 1.5–5% for representative aerosol samples. It proves to be robust and reliable and allows for overnight and unattended measurements. A constant and cross contamination correction is included, which indicates a constant contamination of 1.4 ± 0.2 μg C with 70 ± 7 pMC and a cross contamination of (0.2 ± 0.1)% from the previous sample. A Real-time online coupling version of the method was also investigated. It shows promising results for standard materials with slightly higher uncertainties than the Trapping online approach.

Geochemical perspectives from a new aerosol chemical mass closure

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B. Guinot

2007-01-01

Full Text Available The aerosol chemical mass closure is revisited and a simple and inexpensive methodology is proposed. This methodology relies on data obtained for aerosol mass, and concentration of the major ions and the two main carbon components, the organic carbon (OC and the black carbon (BC. Atmospheric particles are separated into coarse (AD>2 μm and fine (AD<2 μm fractions and are treated separately. For the coarse fraction the carbonaceous component is minor and assumption is made for the conversion factor k of OC-to-POM (Particulate Organic Matter which is fixed to the value of 1.8 accounting for secondary species. The coarse soluble calcium is shown to display a correlation (regression coefficient f, y axis intercept b with the missing mass. Conversely, the fine fraction is dominated by organic species and assumption is made for dust which is assumed to have the same f factor as the coarse mode dust. The fine mode mass obtained from chemical analyses is then adjusted to the actual weighed mass by tuning the k conversion factor. The k coefficient is kept different in the two modes due to the expected different origins of the organic particles. Using the f and k coefficient obtained from the data set, the mass closure is reached for each individual sample with an undetermined fraction less than 10%. The procedure has been applied to different urban and peri-urban environments in Europe and in Beijing and its efficiency and uncertainties on f and k values are discussed. The f and k coefficients are shown to offer consistent geochemical indications on aerosol origin and transformations. f allows to retrieve dust mass and its value accounting for Ca abundance in dust at the site of investigation may serve as an indicator of dust origin and aerosol interactions with anthropogenic acids. f values were found to vary in the 0.08–0.12 range in European urban areas, and a broader range in Beijing (0.01–0.16. As expected, k appears to be a relevant proxy for

Aerosol concentration measurements and correlations with air mass trajectories at the Pierre Auger Observatory

Science.gov (United States)

Micheletti, M. I.; Louedec, K.; Freire, M.; Vitale, P.; Piacentini, R. D.

2017-06-01

Aerosols play an important role in radiative transfer processes involved in different fields of study. In particular, their influence is crucial in the attenuation of light at astronomical and astrophysical observatories, and has to be taken into account in light transfer models employed to reconstruct the signals. The Andean Argentinean region is increasingly being considered as a good candidate to host such facilities, as well as the ones for solar-energy resources, and an adequate knowledge of aerosols characteristics there is needed, but it is not always possible due to the vast area involved and the scarce atmospheric data at ground. The aim of this work is to find correlations between aerosol data and particle trajectories that can give an insight into the origin and behaviour of aerosols in this zone and can be employed in situations in which one does not have local aerosol measurements. For this purpose, an aerosol spectrometer and dust monitor (Grimm 1.109) was installed at the Pierre Auger Observatory of ultra-high-energy cosmic rays, to record aerosol concentrations in different size intervals, at surface level. These measurements are analysed and correlated with air mass trajectories obtained from HYSPLIT (NOAA) model calculations. High aerosol concentrations are registered predominantly when air masses have travelled mostly over continental areas, mainly from the NE direction, while low aerosol concentrations are found in correspondence with air masses coming from the Pacific Ocean, from the NW direction. Different size distribution patterns were found for the aerosols depending on their origin: marine or continental. This work shows for the first time the size distribution of aerosols registered at the Pierre Auger Observatory. The correlations found between mass and particle concentrations (total and for different size ranges) and HYSPLIT air mass trajectories, confirm that the latter can be employed as a useful tool to infer the sources, evolution

Measurement of particle size distribution and mass concentration of nuclear fuel aerosols

International Nuclear Information System (INIS)

Pickering, S.

1982-01-01

The particle size distribution and particle mass concentration of a nuclear fuel aerosol is measured by admitting the aerosol into a vertically-extending container, positioning an alpha particle detector within the container so that its window is horizontal and directed vertically, stopping the admission of aerosol into the container, detecting the alpha-activity of the particles of the aerosol sedimenting onto the detector window (for example in a series of equal time intervals until a constant level is reached), and converting the alpha-activity measurements into particle size distribution and/or particle mass concentration measurements. The detector is attached to a pivotted arm and by raising a counterweight can be lowered from the container for cleaning. (author)

Derivation of Aerosol Columnar Mass from MODIS Optical Depth

Science.gov (United States)

Gasso, Santiago; Hegg, Dean A.

2003-01-01

In order to verify performance, aerosol transport models (ATM) compare aerosol columnar mass (ACM) with those derived from satellite measurements. The comparison is inherently indirect since satellites derive optical depths and they use a proportionality constant to derive the ACM. Analogously, ATMs output a four dimensional ACM distribution and the optical depth is linearly derived. In both cases, the proportionality constant requires a direct intervention of the user by prescribing the aerosol composition and size distribution. This study introduces a method that minimizes the direct user intervention by making use of the new aerosol products of MODIS. A parameterization is introduced for the derivation of columnar aerosol mass (AMC) and CCN concentration (CCNC) and comparisons between sunphotometer, MODIS Airborne Simulator (MAS) and in-measurements are shown. The method still relies on the scaling between AMC and optical depth but the proportionality constant is dependent on the MODIS derived r$_{eff}$,\\eta (contribution of the accumulation mode radiance to the total radiance), ambient RH and an assumed constant aerosol composition. The CCNC is derived fkom a recent parameterization of CCNC as a function of the retrieved aerosol volume. By comparing with in-situ data (ACE-2 and TARFOX campaigns), it is shown that retrievals in dry ambient conditions (dust) are improved when using a proportionality constant dependent on r$ {eff}$ and \\eta derived in the same pixel. In high humidity environments, the improvement inthe new method is inconclusive because of the difficulty in accounting for the uneven vertical distribution of relative humidity. Additionally, two detailed comparisons of AMC and CCNC retrieved by the MAS algorithm and the new method are shown. The new method and MAS retrievals of AMC are within the same order of magnitude with respect to the in-situ measurements of aerosol mass. However, the proposed method is closer to the in-situ measurements than

Sources and atmospheric processing of organic aerosol in the Mediterranean: insights from aerosol mass spectrometer factor analysis

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L. Hildebrandt

2011-12-01

Full Text Available Atmospheric particles were measured in the late winter (25 February–26 March 2009 at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2009. A quadrupole aerosol mass spectrometer (Q-AMS was employed to quantify the size-resolved chemical composition of non-refractory submicron aerosol, and a thermodenuder was used to analyze the organic aerosol (OA volatility. Complementary measurements included particle size distributions from a scanning mobility particle sizer, inorganic and organic particle composition from filter analysis, air ion concentrations, O₃, NO_x and NO_y concentrations, and meteorological measurements. Factor analysis was performed on the OA mass spectra, and the variability in OA composition could best be explained with three OA components. The oxygenated organic aerosol (OOA was similar in composition and volatility to the summertime OA previously measured at this site and may represent an effective endpoint in particle-phase oxidation of organics. The two other OA components, one associated with amines (Amine-OA and the other probably associated with the burning of olive branches (OB-OA, had very low volatility but were less oxygenated. Hydrocarbon-like organic aerosol (HOA was not detected. The absence of OB-OA and Amine-OA in the summer data may be due to lower emissions and/or photochemical conversion of these components to OOA.

Photochemical aging of aerosol particles in different air masses arriving at Baengnyeong Island, Korea

Science.gov (United States)

Kang, Eunha; Lee, Meehye; Brune, William H.; Lee, Taehyoung; Park, Taehyun; Ahn, Joonyoung; Shang, Xiaona

2018-05-01

Atmospheric aerosol particles are a serious health risk, especially in regions like East Asia. We investigated the photochemical aging of ambient aerosols using a potential aerosol mass (PAM) reactor at Baengnyeong Island in the Yellow Sea during 4-12 August 2011. The size distributions and chemical compositions of aerosol particles were measured alternately every 6 min from the ambient air or through the highly oxidizing environment of a potential aerosol mass (PAM) reactor. Particle size and chemical composition were measured by using the combination of a scanning mobility particle sizer (SMPS) and a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Inside the PAM reactor, O3 and OH levels were equivalent to 4.6 days of integrated OH exposure at typical atmospheric conditions. Two types of air masses were distinguished on the basis of the chemical composition and the degree of aging: air transported from China, which was more aged with a higher sulfate concentration and O : C ratio, and the air transported across the Korean Peninsula, which was less aged with more organics than sulfate and a lower O : C ratio. For both episodes, the particulate sulfate mass concentration increased in the 200-400 nm size range when sampled through the PAM reactor. A decrease in organics was responsible for the loss of mass concentration in 100-200 nm particles when sampled through the PAM reactor for the organics-dominated episode. This loss was especially evident for the m/z 43 component, which represents less oxidized organics. The m/z 44 component, which represents further oxidized organics, increased with a shift toward larger sizes for both episodes. It is not possible to quantify the maximum possible organic mass concentration for either episode because only one OH exposure of 4.6 days was used, but it is clear that SO2 was a primary precursor of secondary aerosol in northeast Asia, especially during long-range transport from China. In addition

Aerosol formation from heat and mass transfer in vapour-gas mixtures

International Nuclear Information System (INIS)

Clement, C.F.

1985-01-01

Heat and mass transfer equations and their coupling to the equation for the aerosol size distribution are examined for mixtures in which pressure changes are slow. Specific results in terms of Cn (the condensation number) and Le (the Lewis number - the ratio of the relative rates of evaporation and condensation) are obtained for the proportion of vapour condensing as a aerosol during the cooling and heating of a mixture in a well-mixed cavity. The assumption of allowing no supersaturations, the validity of which is examined, is shown to lead to maximum aerosol formation. For water vapour-air mixtures predictions are made as to temperature regions in which aerosols will evaporate or not form in cooling processes. The results are also qualitatively applied to some atmospheric effects as well as to water aerosols formed in the containment of a pressurized water reactor following a possible accident. In this context, the present conclusion that the whereabouts of vapour condensation is controlled by heat and mass transfer, contrasts with previous assumptions that the controlling factor is relative surface areas. (U.K.)

Effect of variable power levels on the yield of total aerosol mass and formation of aldehydes in e-cigarette aerosols.

Science.gov (United States)

Gillman, I G; Kistler, K A; Stewart, E W; Paolantonio, A R

2016-03-01

The study objective was to determine the effect of variable power applied to the atomizer of refillable tank based e-cigarette (EC) devices. Five different devices were evaluated, each at four power levels. Aerosol yield results are reported for each set of 25 EC puffs, as mass/puff, and normalized for the power applied to the coil, in mass/watt. The range of aerosol produced on a per puff basis ranged from 1.5 to 28 mg, and, normalized for power applied to the coil, ranged from 0.27 to 1.1 mg/watt. Aerosol samples were also analyzed for the production of formaldehyde, acetaldehyde, and acrolein, as DNPH derivatives, at each power level. When reported on mass basis, three of the devices showed an increase in total aldehyde yield with increasing power applied to the coil, while two of the devices showed the opposite trend. The mass of formaldehyde, acetaldehyde, and acrolein produced per gram of total aerosol produced ranged from 0.01 to 7.3 mg/g, 0.006 to 5.8 mg/g, and acrolein from EC aerosols from specific devices, and were compared to estimated exposure from consumption of cigarettes, to occupational and workplace limits, and to previously reported results from other researchers. Copyright © 2015 The Authors. Published by Elsevier Inc. All rights reserved.

Ion mobility spectrometry-mass spectrometry (IMS-MS) for on- and offline analysis of atmospheric gas and aerosol species

Science.gov (United States)

Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan; Junninen, Heikki; Massoli, Paola; Lambe, Andrew T.; Kimmel, Joel R.; Cubison, Michael J.; Graf, Stephan; Lin, Ying-Hsuan; Budisulistiorini, Sri H.; Zhang, Haofei; Surratt, Jason D.; Knochenmuss, Richard; Jayne, John T.; Worsnop, Douglas R.; Jimenez, Jose-Luis; Canagaratna, Manjula R.

2016-07-01

Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS-MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS-MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI-IMS-MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS) ambient field campaign in the forested SE US. The ambient IMS-MS signals are consistent with laboratory IMS-MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS-MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS-MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. Controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of oligomers, and confirm the

Elemental mass size distribution of the Debrecen urban aerosol

International Nuclear Information System (INIS)

Kertesz, Zs.; Szoboszlai, Z.; Dobos, E.; Borbely-Kiss, I.

2007-01-01

Complete text of publication follows. Size distribution is one of the basic properties of atmospheric aerosol. It is closely related to the origin, chemical composition and age of the aerosol particles, and it influences the optical properties, environmental effects and health impact of aerosol. As part of the ongoing aerosol research in the Group of Ion Beam Applications of the Atomki, elemental mass size distribution of urban aerosol were determined using particle induced X-ray emission (PIXE) analytical technique. Aerosol sampling campaigns were carried out with 9-stage PIXE International cascade impactors, which separates the aerosol into 10 size fractions in the 0.05-30 ?m range. Five 48-hours long samplings were done in the garden of the Atomki, in April and in October, 2007. Both campaigns included weekend and working day samplings. Basically two different kinds of particles could be identified according to the size distribution. In the size distribution of Al, Si, Ca, Fe, Ba, Ti, Mn and Co one dominant peak can be found around the 3 m aerodynamic diameter size range, as it is shown on Figure 1. These are the elements of predominantly natural origin. Elements like S, Cl, K, Zn, Pb and Br appears with high frequency in the 0.25-0.5 mm size range as presented in Figure 2. These elements are originated mainly from anthropogenic sources. However sometimes in the size distribution of these elements a 2 nd , smaller peak appears at the 2-4 μm size ranges, indicating different sources. Differences were found between the size distribution of the spring and autumn samples. In the case of elements of soil origin the size distribution was shifted towards smaller diameters during October, and a 2 nd peak appeared around 0.5 μm. A possible explanation to this phenomenon can be the different meteorological conditions. No differences were found between the weekend and working days in the size distribution, however the concentration values were smaller during the weekend

Progress Toward a Global, EOS-Era Aerosol Air Mass Type Climatology

Science.gov (United States)

Kahn, Ralph A.

2012-01-01

The MISR and MODIS instruments aboard the NASA Earth Observing System's Terra Satellite have been collecting data containing information about the state of Earth's atmosphere and surface for over eleven years. Data from these instruments have been used to develop a global, monthly climatology of aerosol amount that is widely used as a constraint on climate models, including those used for the 2007 IPCC assessment report. The next frontier in assessing aerosol radiative forcing of climate is aerosol type, and in particular, the absorption properties of major aerosol air masses. This presentation will focus on the prospects for constraining aerosol type globally, and the steps we are taking to apply a combination of satellite and suborbital data to this challenge.

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

Prospects of real-time single-particle biological aerosol analysis: A comparison between laser-induced breakdown spectroscopy and aerosol time-of-flight mass spectrometry

International Nuclear Information System (INIS)

Beddows, D.C.S.; Telle, H.H.

2005-01-01

In this paper we discuss the prospects of real-time, in situ laser-induced breakdown spectroscopy applied for the identification and classification of bio-aerosols (including species of potential bio-hazard) within common urban aerosol mixtures. In particular, we address the issues associated with the picking out of bio-aerosols against common background aerosol particles, comparing laser-induced breakdown spectroscopy measurements with data from a mobile single-particle aerosol mass spectrometer (ATOFMS). The data from the latter provide statistical data over an extended period of time, highlighting the variation of the background composition. While single-particle bio-aerosols are detectable in principle, potential problems with small (∼ 1 μm size) bio-aerosols have been identified; constituents of the air mass other than background aerosols, e.g. gaseous CO 2 in conjunction with common background aerosols, may prevent unique recognition of the bio-particles. We discuss whether it is likely that laser-induced breakdown spectroscopy on its own can provide reliable, real-time identification of bio-aerosol in an urban environment, and it is suggested that more than one technique should be or would have to be used. A case for using a combination of laser-induced breakdown spectroscopy and Raman (and/or) laser-induced fluorescence spectroscopy is made

Satellite measurements of aerosol mass and transport

Energy Technology Data Exchange (ETDEWEB)

Fraser, R.S.; Kaufman, Y.J.; Mahoney, R.L.

1984-01-01

The aerosol optical thickness over land is derived from satellite measurements of the radiance of scattered sunlight. These data are used to estimate the columnar mass density of particulate sulfur on a day with a large amount of sulfur. The horizontal transport of the particulate sulfur is calculated using wing vectors measured with rawins. 33 references, 7 figures, 1 table.

Quantitative determination of carbonaceous particle mixing state in Paris using single particle mass spectrometer and aerosol mass spectrometer measurements

Science.gov (United States)

Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

2013-04-01

Single particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been estimated using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulphate and potassium were compared with concurrent measurements from an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal/optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and ten discrete mixing states for carbonaceous particles were identified and quantified. Potassium content was used to identify particles associated with biomass combustion. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorization, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulphate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA/EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidized OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the heterogeneity of primary and

Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements

Directory of Open Access Journals (Sweden)

R. M. Healy

2013-09-01

Full Text Available Single-particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single-particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been determined using an aerosol time-of-flight mass spectrometer (ATOFMS as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC, organic aerosol (OA, ammonium, nitrate, sulfate and potassium were compared with concurrent measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS, a thermal–optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC. ATOFMS-derived estimated mass concentrations reproduced the variability of these species well (R2 = 0.67–0.78, and 10 discrete mixing states for carbonaceous particles were identified and quantified. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorisation, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA detected in Paris is associated with two EC-rich mixing states which differ in their relative sulfate content, while fresh biomass burning OA (BBOA is associated with two mixing states which differ significantly in their OA / EC ratios. Aged biomass burning OA (OOA2-BBOA was found to be significantly internally mixed with nitrate, while secondary, oxidised OA (OOA was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the range of primary and secondary organic aerosol mixing states in Paris. Examination of the

Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements

Science.gov (United States)

Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

2013-09-01

Single-particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single-particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been determined using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulfate and potassium were compared with concurrent measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal-optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived estimated mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and 10 discrete mixing states for carbonaceous particles were identified and quantified. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorisation, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulfate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA / EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidised OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the range of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal

Reactions and mass spectra of complex particles using Aerosol CIMS

Science.gov (United States)

Hearn, John D.; Smith, Geoffrey D.

2006-12-01

Aerosol chemical ionization mass spectrometry (CIMS) is used both on- and off-line for the analysis of complex laboratory-generated and ambient particles. One of the primary advantages of Aerosol CIMS is the low degree of ion fragmentation, making this technique well suited for investigating the reactivity of complex particles. To demonstrate the usefulness of this "soft" ionization, particles generated from meat cooking were reacted with ozone and the composition was monitored as a function of reaction time. Two distinct kinetic regimes were observed with most of the oleic acid in these particles reacting quickly but with 30% appearing to be trapped in the complex mixture. Additionally, detection limits are measured to be sufficiently low (100-200 ng/m3) to detect some of the more abundant constituents in ambient particles, including sulfate, which is measured in real-time at 1.2 [mu]g/m3. To better characterize complex aerosols from a variety of sources, a novel off-line collection method was also developed in which non-volatile and semi-volatile organics are desorbed from particles and concentrated in a cold U-tube. Desorption from the U-tube followed by analysis with Aerosol CIMS revealed significant amounts of nicotine in cigarette smoke and levoglucosan in oak and pine smoke, suggesting that this may be a useful technique for monitoring particle tracer species. Additionally, secondary organic aerosol formed from the reaction of ozone with R-limonene and volatile organics from orange peel were analyzed off-line showing large molecular weight products (m/z > 300 amu) that may indicate the formation of oligomers. Finally, mass spectra of ambient aerosol collected offline reveal a complex mixture of what appears to be highly processed organics, some of which may contain nitrogen.

Mass and chemically speciated size distribution of Prague aerosol using an aerosol dryer - The influence of air mass origin

Czech Academy of Sciences Publication Activity Database

Schwarz, Jaroslav; Štefancová, Lucia; Maenhaut, W.; Smolík, Jiří; Ždímal, Vladimír

2012-01-01

Roč. 437, OCT 15 (2012), s. 348-362 ISSN 0048-9697 R&D Projects: GA ČR GA205/09/2055; GA ČR GAP209/11/1342; GA MŠk ME 941 Grant - others:SRF GU(BE) 01S01306 Institutional support: RVO:67985858 Keywords : atmospheric aerosols * mass size distribution * chemical composition Subject RIV: DI - Air Pollution ; Quality Impact factor: 3.258, year: 2012

PHEBUS on-line aerosol monitor development test program

International Nuclear Information System (INIS)

Sprenger, M.H.; Pentecost, C.G.

1992-03-01

EG ampersand G Idaho, Inc. developed an on-line aerosol monitor (OLAM) for the French PHEBUS Fission Product Project. Part of the development was to manufacture and test an OLAM prototype. This report presents the results of the testing which determined the mechanical integrity of the monitor at operating temperature and pressure and performed a preliminary test of the optical system. A series of twenty different tests was conducted during the prototype testing sequence. Since no leaks were detected, the OLAM demonstrated that it could provide a pressure boundary at required test conditions. The optical and electrical system also proved its integrity by exceeding the design requirement of less than 105 optical signal drift during an actual two-hour test sequence

Mass analysis of charged aerosol particles in NLC and PMSE during the ECOMA/MASS campaign

Directory of Open Access Journals (Sweden)

S. Robertson

2009-03-01

Full Text Available MASS (Mesospheric Aerosol Sampling Spectrometer is a multichannel mass spectrometer for charged aerosol particles, which was flown from the Andøya Rocket Range, Norway, through NLC and PMSE on 3 August 2007 and through PMSE on 6 August 2007. The eight-channel analyzers provided for the first time simultaneous measurements of the charge density residing on aerosol particles in four mass ranges, corresponding to ice particles with radii <0.5 nm (including ions, 0.5–1 nm, 1–2 nm, and >3 nm (approximately. Positive and negative particles were recorded on separate channels. Faraday rotation measurements provided electron density and a means of checking charge density measurements made by the spectrometer. Additional complementary measurements were made by rocket-borne dust impact detectors, electric field booms, a photometer and ground-based radar and lidar. The MASS data from the first flight showed negative charge number densities of 1500–3000 cm⁻³ for particles with radii >3 nm from 83–88 km approximately coincident with PMSE observed by the ALWIN radar and NLC observed by the ALOMAR lidar. For particles in the 1–2 nm range, number densities of positive and negative charge were similar in magnitude (~2000 cm⁻³ and for smaller particles, 0.5–1 nm in radius, positive charge was dominant. The occurrence of positive charge on the aerosol particles of the smallest size and predominately negative charge on the particles of largest size suggests that nucleation occurs on positive condensation nuclei and is followed by collection of negative charge during subsequent growth to larger size. Faraday rotation measurements show a bite-out in electron density that increases the time for positive aerosol particles to be neutralized and charged negatively. The larger particles (>3 nm are observed throughout the NLC region, 83–88 km, and the smaller particles are observed primarily at the high end of the range, 86–88 km

Mass analysis of charged aerosol particles in NLC and PMSE during the ECOMA/MASS campaign

Directory of Open Access Journals (Sweden)

S. Robertson

2009-03-01

Full Text Available MASS (Mesospheric Aerosol Sampling Spectrometer is a multichannel mass spectrometer for charged aerosol particles, which was flown from the Andøya Rocket Range, Norway, through NLC and PMSE on 3 August 2007 and through PMSE on 6 August 2007. The eight-channel analyzers provided for the first time simultaneous measurements of the charge density residing on aerosol particles in four mass ranges, corresponding to ice particles with radii <0.5 nm (including ions, 0.5–1 nm, 1–2 nm, and >3 nm (approximately. Positive and negative particles were recorded on separate channels. Faraday rotation measurements provided electron density and a means of checking charge density measurements made by the spectrometer. Additional complementary measurements were made by rocket-borne dust impact detectors, electric field booms, a photometer and ground-based radar and lidar. The MASS data from the first flight showed negative charge number densities of 1500–3000 cm−3 for particles with radii >3 nm from 83–88 km approximately coincident with PMSE observed by the ALWIN radar and NLC observed by the ALOMAR lidar. For particles in the 1–2 nm range, number densities of positive and negative charge were similar in magnitude (~2000 cm−3 and for smaller particles, 0.5–1 nm in radius, positive charge was dominant. The occurrence of positive charge on the aerosol particles of the smallest size and predominately negative charge on the particles of largest size suggests that nucleation occurs on positive condensation nuclei and is followed by collection of negative charge during subsequent growth to larger size. Faraday rotation measurements show a bite-out in electron density that increases the time for positive aerosol particles to be neutralized and charged negatively. The larger particles (>3 nm are observed throughout the NLC region, 83–88 km, and the smaller particles are observed primarily at the high end of the range, 86–88 km. The second flight into

Single particle composition measurements of artificial Calcium Carbonate aerosols

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Zorn, S. R.; Mentel, T. F.; Schwinger, T.; Croteau, P. L.; Jayne, J.; Worsnop, D. R.; Trimborn, A.

2012-12-01

Mineral dust, with an estimated total source from natural and anthropogenic emissions of up to 2800 Tg/yr, is one of the two largest contributors to total aerosol mass, with only Sea salt having a similar source strength (up to 2600 Tg/yr). The composition of dust particles varies strongly depending on the production process and, most importantly, the source location. Therefore, the composition of single dust particles can be used both to trace source regions of air masses as well as to identify chemical aging processes. Here we present results of laboratory studies on generating artificial calcium carbonate (CaCO3) particles, a model compound for carbonaceous mineral dust particles. Particles were generated by atomizing an aqueous hydrogen carbonate solution. Water was removed using a silica diffusion dryer., then the particles were processed in an oven at temperatures up to 900°C, converting the hydrogen carbonate to its anhydrous form. The resulting aerosol was analyzed using an on-line single particle laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF). The results confirm the conversion to calcium carbonate, and validate that the produced particles indeed can be used as a model compound for carbonaceous dust aerosols.

Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior

Energy Technology Data Exchange (ETDEWEB)

UC Davis; Cappa, Christopher D.; Wilson, Kevin R.

2010-10-28

Vacuum Ultraviolet (VUV) photoionization mass spectrometry has been used to measure the evolution of chemical composition for two distinct organic aerosol types as they are passed through a thermodenuder at different temperatures. The two organic aerosol types considered are primary lubricating oil (LO) aerosol and secondary aerosol from the alpha-pinene + O3 reaction (alphaP). The evolution of the VUV mass spectra for the two aerosol types with temperature are observed to differ dramatically. For LO particles, the spectra exhibit distinct changes with temperature in which the lower m/z peaks, corresponding to compounds with higher vapor pressures, disappear more rapidly than the high m/z peaks. In contrast, the alphaP aerosol spectrum is essentially unchanged by temperature even though the particles experience significant mass loss due to evaporation. The variations in the LO spectra are found to be quantitatively in agreement with expectations from absorptive partitioning theory whereas the alphaP spectra suggest that the evaporation of alphaP derived aerosol appears to not be governed by partitioning theory. We postulate that this difference arises from the alphaP particles existing as in a glassy state instead of having the expected liquid-like behavior. To reconcile these observations with decades of aerosol growth measurements, which indicate that OA formation is described by equilibrium partitioning, we present a conceptual model wherein the secondary OA is formed and then rapidly converted from an absorbing form to a non-absorbing form. The results suggest that although OA growth may be describable by equilibrium partitioning theory, the properties of organic aerosol once formed may differ significantly from the properties determined in the equilibrium framework.

Online characterization of nano-aerosols released by commercial spray products using SMPS–ICPMS coupling

Energy Technology Data Exchange (ETDEWEB)

Losert, Sabrina; Hess, Adrian [Empa Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Analytical Chemistry (Switzerland); Ilari, Gabriele [Empa Swiss Federal Laboratories for Materials Science and Technology, Electron Microscopy Center (Switzerland); Goetz, Natalie von, E-mail: natalie.von.goetz@chem.ethz.ch; Hungerbuehler, Konrad [ETH Zürich Swiss Federal Institute of Technology Zürich, Institute for Chemical and Bioengineering (Switzerland)

2015-07-15

Nanoparticle-containing sprays are a critical class of consumer products, since human exposure may occur by inhalation of nanoparticles (NP) in the generated aerosols. In this work, the suspension and the released aerosol of six different commercially available consumer spray products were analyzed. Next to a broad spectrum of analytical methods for the characterization of the suspension, a standardized setup for the analysis of aerosol has been used. In addition, a new online coupling technique (SMPS–ICPMS) for the simultaneous analysis of particle size and elemental composition of aerosol particles has been applied. Results obtained with this new method were confirmed by other well-established techniques. Comparison of particles in the original suspensions and in the generated aerosol showed that during spraying single particles of size less than 20 nm had been formed, even though in none of the suspensions particles of size less than 280 nm were present (Aerosol size range scanned: 7–300 nm). Both pump sprays and propellant gas sprays were analyzed and both released particles in the nm size range. Also, both water-based and organic solvent-based sprays released NP. However, a trend was observed that spraying an aqueous suspension contained in a pump spray dispenser after drying resulted in bigger agglomerates than spraying organic suspensions in propellant gas dispensers.

Laboratory and field measurements of organic aerosols with the photoionization aerosol mass spectrometer

Science.gov (United States)

Dreyfus, Matthew A.

Analytical methods developed to sample and characterize ambient organic aerosols often face the trade-off between long sampling times and the loss of detailed information regarding specific chemical species present. The soft, universal ionization scheme of the Photoionization Aerosol Mass Spectrometer (PIAMS) allows for identification of various chemical compounds by a signature ion, often the molecular ion. The goal of this thesis work is to apply PIAMS to both laboratory and field experiments to answer questions regarding the formation, composition, and behavior of organic aerosols. To achieve this goal, a variety of hardware and software upgrades were administered to PIAMS to optimize the instrument. Data collection and processing software were either refined or built from the ground up to simplify difficult or monotonous tasks. Additional components were added to PIAMS with the intent to automate the instrument, enhance the results, and make the instrument more rugged and user-friendly. These changes, combined with the application of an external particle concentration system (mini-Versatile Aerosol Concentration Enrichment System, m-VACES), allowed PIAMS to be suitable for field measurements of organic aerosols. Two such field campaigns were completed, both at the State of Delaware Air Quality Monitoring Site in Wilmington, Delaware: a one week period in June, 2006, and an 18 day period in October and November of 2007. A sampling method developed was capable of collecting sufficient ambient organic aerosol and analyzing it with a time resolution of 3.5 minutes. Because of this method, short term concentration changes of individual species can be tracked. Combined with meteorological data, the behavior of these species can be analyzed as a function of time or wind direction. Many compounds are found at enhanced levels during the evening/night-time hours; potentially due to the combined effects of temperature inversion, and fresh emissions in a cooler environment

Sources and atmospheric processing of winter aerosols in Seoul, Korea: insights from real-time measurements using a high-resolution aerosol mass spectrometer

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Kim, Hwajin; Zhang, Qi; Bae, Gwi-Nam; Kim, Jin Young; Bok Lee, Seung

2017-02-01

Highly time-resolved chemical characterization of nonrefractory submicrometer particulate matter (NR-PM1) was conducted in Seoul, the capital and largest metropolis of Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The measurements were performed during winter, when elevated particulate matter (PM) pollution events are often observed. This is the first time that detailed real-time aerosol measurement results have been reported from Seoul, Korea, and they reveal valuable insights into the sources and atmospheric processes that contribute to PM pollution in this region. The average concentration of submicron aerosol (PM1 = NR-PM1+ black carbon (BC)) was 27.5 µg m-3, and the total mass was dominated by organics (44 %), followed by nitrate (24 %) and sulfate (10 %). The average atomic ratios of oxygen to carbon (O / C), hydrogen to carbon (H / C), and nitrogen to carbon (N / C) of organic aerosols (OA) were 0.37, 1.79, and 0.018, respectively, which result in an average organic mass-to-carbon (OM / OC) ratio of 1.67. The concentrations (2.6-90.7 µg m-3) and composition of PM1 varied dynamically during the measurement period due to the influences of different meteorological conditions, emission sources, and air mass origins. Five distinct sources of OA were identified via positive matrix factorization (PMF) analysis of the HR-ToF-AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA, O / C = 0.06), cooking activities represented by a cooking OA factor (COA, O / C = 0.14), wood combustion represented by a biomass burning OA factor (BBOA, O / C = 0.34), and secondary organic aerosol (SOA) represented by a semivolatile oxygenated OA factor (SV-OOA, O / C = 0.56) and a low-volatility oxygenated OA factor (LV-OOA, O / C = 0.68). On average, primary OA (POA = HOA + COA + BBOA) accounted for 59 % the OA mass, whereas SV-OOA and LV-OOA contributed 15 and 26 %, respectively. Our results indicate that air

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the UK

Science.gov (United States)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-05-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the UK. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in

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

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

Long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometer

Science.gov (United States)

Xu, J.; Zhang, X.; Liu, Y.; Shichang, K.; Ma, Y.

2017-12-01

An intensive measurement was conducted at a remote, background, and high-altitude site (Qomolangma station, QOMS, 4276 m a.s.l.) in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) along with other collocated instruments. The field measurement was performed from April 12 to May 12, 2016 to chemically characterize high time-resolved submicron particulate matter (PM1) and obtain the influence of biomass burning emissions to the Himalayas, frequently transported from south Asia during pre-monsoon season. Two high aerosol loading periods were observed during the study. Overall, the average (± 1σ) PM1 mass concentration was 4.44 (± 4.54) µg m-3 for the entire study, comparable with those observed at other remote sites worldwide. Organic aerosols (OA) was the dominant PM1 species (accounting for 54.3% of total PM1 mass on average) and its contribution increased with the increase of total PM1 mass loading. The average size distributions of PM1 species all peaked at an overlapping accumulation mode ( 500 nm), suggesting that aerosol particles were internally well-mixed and aged during long-range transportations. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a biomass burning related OA (BBOA, 43.7%) and two oxygenated OA (Local-OOA and LRT-OOA; 13.9% and 42.4%) represented sources from local emissions and long-range transportations, respectively. Two polluted air mass origins (generally from the west and southwest of QOMS) and two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions were observed, respectively, suggesting the important sources of wildfires from south Asia. One of polluted aerosol plumes was investigated in detail to illustrate the evolution of aerosol characteristics at QOMS driving by different impacts of wildfires, air mass origins, meteorological conditions and

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

Science.gov (United States)

McMeeking, G. R.; Morgan, W. T.; Flynn, M.; Highwood, E. J.; Turnbull, K.; Haywood, J.; Coe, H.

2011-09-01

Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA

Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

Directory of Open Access Journals (Sweden)

G. R. McMeeking

2011-09-01

Full Text Available Black carbon (BC aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2 measurements of refractory BC (rBC mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA operated by the Facility for Airborne Atmospheric Measurements (FAAM. We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS and used positive matrix factorization to separate hydrocarbon-like (HOA and oxygenated organic aerosols (OOA. We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NO_x ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NO_x and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA did change for

Identification of aerosol types over an urban site based on air-mass trajectory classification

Science.gov (United States)

Pawar, G. V.; Devara, P. C. S.; Aher, G. R.

2015-10-01

Columnar aerosol properties retrieved from MICROTOPS II Sun Photometer measurements during 2010-2013 over Pune (18°32‧N; 73°49‧E, 559 m amsl), a tropical urban station in India, are analyzed to identify aerosol types in the atmospheric column. Identification/classification is carried out on the basis of dominant airflow patterns, and the method of discrimination of aerosol types on the basis of relation between aerosol optical depth (AOD500 nm) and Ångström exponent (AE, α). Five potential advection pathways viz., NW/N, SW/S, N, SE/E and L have been identified over the observing site by employing the NOAA-HYSPLIT air mass back trajectory analysis. Based on AE against AOD500 nm scatter plot and advection pathways followed five major aerosol types viz., continental average (CA), marine continental average (MCA), urban/industrial and biomass burning (UB), desert dust (DD) and indeterminate or mixed type (MT) have been identified. In winter, sector SE/E, a representative of air masses traversed over Bay of Bengal and Eastern continental Indian region has relatively small AOD (τpλ = 0.43 ± 0.13) and high AE (α = 1.19 ± 0.15). These values imply the presence of accumulation/sub-micron size anthropogenic aerosols. During pre-monsoon, aerosols from the NW/N sector have high AOD (τpλ = 0.61 ± 0.21), and low AE (α = 0.54 ± 0.14) indicating an increase in the loading of coarse-mode particles over Pune. Dominance of UB type in winter season for all the years (i.e. 2010-2013) may be attributed to both local/transported aerosols. During pre-monsoon seasons, MT is the dominant aerosol type followed by UB and DD, while the background aerosols are insignificant.

Determination of the biogenic secondary organic aerosol fraction in the boreal forest by NMR spectroscopy

Directory of Open Access Journals (Sweden)

E. Finessi

2012-01-01

Full Text Available The study investigates the sources of fine organic aerosol (OA in the boreal forest, based on measurements including both filter sampling (PM₁ and online methods and carried out during a one-month campaign held in Hyytiälä, Finland, in spring 2007. Two aerosol mass spectrometers (Q-AMS, ToF-AMS were employed to measure on-line concentrations of major non-refractory aerosol species, while the water extracts of the filter samples were analyzed by nuclear magnetic resonance (NMR spectroscopy for organic functional group characterization of the polar organic fraction of the aerosol. AMS and NMR spectra were processed separately by non-negative factorization algorithms, in order to apportion the main components underlying the submicrometer organic aerosol composition and depict them in terms of both mass fragmentation patterns and functional group compositions.

The NMR results supported the AMS speciation of oxidized organic aerosol (OOA into two main fractions, which could be generally labelled as more and less oxidized organics. The more oxidized component was characterized by a mass spectrum dominated by the m/z 44 peak, and in parallel by a NMR spectrum showing aromatic and aliphatic backbones highly substituted with oxygenated functional groups (carbonyls/carboxyls and hydroxyls. Such component, contributing on average 50% of the OA mass throughout the observing period, was associated with pollution outbreaks from the Central Europe. The less oxidized component was enhanced in concomitance with air masses originating from the North-to-West sector, in agreement with previous investigations conducted at this site. NMR factor analysis was able to separate two distinct components under the less oxidized fraction of OA. One of these NMR-factors was associated with the formation of terrestrial biogenic secondary organic aerosol (BSOA, based on the comparison with spectral profiles obtained from laboratory experiments of

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

Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry

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N. L. Ng

2010-05-01

Full Text Available In this study we compile and present results from the factor analysis of 43 Aerosol Mass Spectrometer (AMS datasets (27 of the datasets are reanalyzed in this work. The components from all sites, when taken together, provide a holistic overview of Northern Hemisphere organic aerosol (OA and its evolution in the atmosphere. At most sites, the OA can be separated into oxygenated OA (OOA, hydrocarbon-like OA (HOA, and sometimes other components such as biomass burning OA (BBOA. We focus on the OOA components in this work. In many analyses, the OOA can be further deconvolved into low-volatility OOA (LV-OOA and semi-volatile OOA (SV-OOA. Differences in the mass spectra of these components are characterized in terms of the two main ions m/z 44 (CO₂⁺ and m/z 43 (mostly C₂H₃O⁺, which are used to develop a new mass spectral diagnostic for following the aging of OA components in the atmosphere. The LV-OOA component spectra have higher f₄₄ (ratio of m/z 44 to total signal in the component mass spectrum and lower f₄₃ (ratio of m/z 43 to total signal in the component mass spectrum than SV-OOA. A wide range of f₄₄ and O:C ratios are observed for both LV-OOA (0.17±0.04, 0.73±0.14 and SV-OOA (0.07±0.04, 0.35±0.14 components, reflecting the fact that there is a continuum of OOA properties in ambient aerosol. The OOA components (OOA, LV-OOA, and SV-OOA from all sites cluster within a well-defined triangular region in the f₄₄ vs. f₄₃ space, which can be used as a standardized means for comparing and characterizing any OOA components (laboratory or ambient observed with the AMS. Examination of the OOA components in this triangular space indicates that OOA component spectra become increasingly similar to each other and to fulvic acid and HULIS sample spectra as f₄₄ (a

Expanding Single Particle Mass Spectrometer Analyses for the Identification of Microbe Signatures in Sea Spray Aerosol.

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Sultana, Camille M; Al-Mashat, Hashim; Prather, Kimberly A

2017-10-03

Ocean-derived microbes in sea spray aersosol (SSA) have the potential to influence climate and weather by acting as ice nucleating particles in clouds. Single particle mass spectrometers (SPMSs), which generate in situ single particle composition data, are excellent tools for characterizing aerosols under changing environmental conditions as they can provide high temporal resolution and require no sample preparation. While SPMSs have proven capable of detecting microbes, these instruments have never been utilized to definitively identify aerosolized microbes in ambient sea spray aersosol. In this study, an aerosol time-of-flight mass spectrometer was used to analyze laboratory generated SSA produced from natural seawater in a marine aerosol reference tank. We present the first description of a population of biological SSA mass spectra (BioSS), which closely match the ion signatures observed in previous terrestrial microbe studies. The fraction of BioSS dramatically increased in the largest supermicron particles, consistent with field and laboratory measurements of microbes ejected by bubble bursting, further supporting the assignment of BioSS mass spectra as microbes. Finally, as supported by analysis of inorganic ion signals, we propose that dry BioSS particles have heterogeneous structures, with microbes adhered to sodium chloride nodules surrounded by magnesium-enriched coatings. Consistent with this structure, chlorine-containing ion markers were ubiquitous in BioSS spectra and identified as possible tracers for distinguishing recently aerosolized marine from terrestrial microbes.

Evaluation of Aerosol Mixing State Classes in the GISS Modele-matrix Climate Model Using Single-particle Mass Spectrometry Measurements

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Bauer, Susanne E.; Ault, Andrew; Prather, Kimberly A.

2013-01-01

Aerosol particles in the atmosphere are composed of multiple chemical species. The aerosol mixing state, which describes how chemical species are mixed at the single-particle level, provides critical information on microphysical characteristics that determine the interaction of aerosols with the climate system. The evaluation of mixing state has become the next challenge. This study uses aerosol time-of-flight mass spectrometry (ATOFMS) data and compares the results to those of the Goddard Institute for Space Studies modelE-MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) model, a global climate model that includes a detailed aerosol microphysical scheme. We use data from field campaigns that examine a variety of air mass regimens (urban, rural, and maritime). At all locations, polluted areas in California (Riverside, La Jolla, and Long Beach), a remote location in the Sierra Nevada Mountains (Sugar Pine) and observations from Jeju (South Korea), the majority of aerosol species are internally mixed. Coarse aerosol particles, those above 1 micron, are typically aged, such as coated dust or reacted sea-salt particles. Particles below 1 micron contain large fractions of organic material, internally-mixed with sulfate and black carbon, and few external mixtures. We conclude that observations taken over multiple weeks characterize typical air mass types at a given location well; however, due to the instrumentation, we could not evaluate mass budgets. These results represent the first detailed comparison of single-particle mixing states in a global climate model with real-time single-particle mass spectrometry data, an important step in improving the representation of mixing state in global climate models.

Ozonolysis of α-pinene: parameterization of secondary organic aerosol mass fraction

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R. K. Pathak

2007-07-01

Full Text Available Existing parameterizations tend to underpredict the α-pinene aerosol mass fraction (AMF or yield by a factor of 2–5 at low organic aerosol concentrations (<5 µg m⁻³. A wide range of smog chamber results obtained at various conditions (low/high NO_x, presence/absence of UV radiation, dry/humid conditions, and temperatures ranging from 15–40°C collected by various research teams during the last decade are used to derive new parameterizations of the SOA formation from α-pinene ozonolysis. Parameterizations are developed by fitting experimental data to a basis set of saturation concentrations (from 10⁻² to 10⁴ µg m⁻³ using an absorptive equilibrium partitioning model. Separate parameterizations for α-pinene SOA mass fractions are developed for: 1 Low NO_x, dark, and dry conditions, 2 Low NO_x, UV, and dry conditions, 3 Low NO_x, dark, and high RH conditions, 4 High NO_x, dark, and dry conditions, 5 High NO_x, UV, and dry conditions. According to the proposed parameterizations the α-pinene SOA mass fractions in an atmosphere with 5 µg m⁻³ of organic aerosol range from 0.032 to 0.1 for reacted α-pinene concentrations in the 1 ppt to 5 ppb range.

Characterization of ambient aerosols in Mexico City during the MCMA-2003 campaign with Aerosol Mass Spectrometry: results from the CENICA Supersite

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D. Salcedo

2006-01-01

Full Text Available An Aerodyne Aerosol Mass Spectrometer (AMS was deployed at the CENICA Supersite, during the Mexico City Metropolitan Area field study (MCMA-2003 from 31 March-4 May 2003 to investigate particle concentrations, sources, and processes. The AMS provides real time information on mass concentration and composition of the non-refractory species in particulate matter less than 1 µm (NR-PM1 with high time and size-resolution. In order to account for the refractory material in the aerosol, we also present estimates of Black Carbon (BC using an aethalometer and an estimate of the aerosol soil component obtained from Proton-Induced X-ray Emission Spectrometry (PIXE analysis of impactor substrates. Comparisons of AMS + BC + soil mass concentration with other collocated particle instruments (a LASAIR Optical Particle Counter, a PM2.5 Tapered Element Oscillating Microbalance (TEOM, and a PM2.5 DustTrak Aerosol Monitor show that the AMS + BC + soil mass concentration is consistent with the total PM2.5 mass concentration during MCMA-2003 within the combined uncertainties. In Mexico City, the organic fraction of the estimated PM2.5 at CENICA represents, on average, 54.6% (standard deviation σ=10% of the mass, with the rest consisting of inorganic compounds (mainly ammonium nitrate and sulfate/ammonium salts, BC, and soil. Inorganic compounds represent 27.5% of PM2.5 (σ=10%; BC mass concentration is about 11% (σ=4%; while soil represents about 6.9% (σ=4%. Size distributions are presented for the AMS species; they show an accumulation mode that contains mainly oxygenated organic and secondary inorganic compounds. The organic size distributions also contain a small organic particle mode that is likely indicative of fresh traffic emissions; small particle modes exist for the inorganic species as well. Evidence suggests that the organic and inorganic species are not always internally mixed, especially in the small modes. The aerosol seems to be neutralized most

Aerosol mass loading over the marine environment of Arabian Sea ...

Indian Academy of Sciences (India)

The decrease in mass loading from the coast of India towards west is estimated to ... ment of the role of aerosols in radiative forcing ... Oceans are the single largest sources of natural ... While island stations provide informa- ... (Pacific Exploratory Mission), INDOEX (Indian ... very close (150–200km away) to the west Asian.

Modeling organic aerosol from the oxidation of α-pinene in a Potential Aerosol Mass (PAM chamber

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S. Chen

2013-05-01

Full Text Available A model has been developed to simulate the formation and evolution of secondary organic aerosol (SOA and was tested against data produced in a Potential Aerosol Mass (PAM flow reactor and a large environmental chamber. The model framework is based on the two-dimensional volatility basis set approach (2D-VBS, in which SOA oxidation products in the model are distributed on the 2-D space of effective saturation concentration (Ci* and oxygen-to-carbon ratio (O : C. The modeled organic aerosol mass concentrations (COA and O : C agree with laboratory measurements within estimated uncertainties. However, while both measured and modeled O : C increase with increasing OH exposure as expected, the increase of modeled O : C is rapid at low OH exposure and then slows as OH exposure increases while the increase of measured O : C is initially slow and then accelerates as OH exposure increases. A global sensitivity analysis indicates that modeled COA values are most sensitive to the assumed values for the number of Ci* bins, the heterogeneous OH reaction rate coefficient, and the yield of first-generation products. Modeled SOA O : C values are most sensitive to the assumed O : C of first-generation oxidation products, the number of Ci* bins, the heterogeneous OH reaction rate coefficient, and the number of O : C bins. All these sensitivities vary as a function of OH exposure. The sensitivity analysis indicates that the 2D-VBS model framework may require modifications to resolve discrepancies between modeled and measured O : C as a function of OH exposure.

Analysis of Marine Aerosol Polysaccharides by Pyrolysis Time-of-Flight Mass Spectrometry

Science.gov (United States)

Lawler, M. J.; Grieman, M. M.; Sengur, I.; Saltzman, E. S.

2017-12-01

The relationship between surface ocean biological productivity and marine cloud formation and properties has been explored for decades, but the impacts of marine biogenic emissions on cloudiness and climate remain highly uncertain. This is in part due to the challenge of directly linking biogenic materials in the surface ocean with cloud-forming aerosol. It has been shown that polysaccharide gel-forming materials, also known as transparent exopolymers, may be mechanically ejected from the sea surface during air bubble bursting (Leck and Bigg, 2005). Existing analysis methods for such aerosols require considerable sample mass and sample preparation. As part of the multi-year seasonal North Atlantic Aerosols and Marine Ecosystems Study (NAAMES), ambient submicron marine aerosol was collected in November 2015 and May 2016 from the R/V Atlantis at using a Particle into Liquid Sampler (PILS). These samples of roughly 15 minute time resolution were frozen and returned to UC Irvine for analysis. A new technique has been developed to attempt to quantify polysaccharide material in these ambient samples. A small subsample (1- 5 µL) is taken from the PILS vial samples and allowed to dry on a Pt ribbon filament in the chemical ionization source region of a time-of-flight mass spectrometer. The sample then undergoes a two-step heating process, in which volatilizable molecules are first desorbed and then non-volatilizable large molecules such as polysaccharides are pyrolyzed. These desorbed molecules and decomposition products are ionized using either O2- or H3O+ reagent ion and are directly sampled into the mass spectrometer. The resulting spectra can then be compared to standards of known polysaccharide materials for quantification and potentially structural and/or compositional information.

Characterizing aerosol transport into the Canadian High Arctic using aerosol mass spectrometry and Lagrangian modelling

Science.gov (United States)

Kuhn, T.; Damoah, R.; Bacak, A.; Sloan, J. J.

2010-05-01

We report the analysis of measurements made using an aerosol mass spectrometer (AMS; Aerodyne Research Inc.) that was installed in the Polar Environment Atmospheric Research Laboratory (PEARL) in summer 2006. PEARL is located in the Canadian high Arctic at 610 m above sea level on Ellesmere Island (80° N 86° W). PEARL is unique for its remote location in the Arctic and because most of the time it is situated within the free troposphere. It is therefore well suited as a receptor site to study the long range tropospheric transport of pollutants into the Arctic. Some information about the successful year-round operation of an AMS at a high Arctic site such as PEARL will be reported here, together with design considerations for reliable sampling under harsh low-temperature conditions. Computational fluid dynamics calculations were made to ensure that sample integrity was maintained while sampling air at temperatures that average -40 °C in the winter and can be as low as -55 °C. Selected AMS measurements of aerosol mass concentration, size, and chemical composition recorded during the months of August, September and October 2006 will be reported. During this period, sulfate was at most times the predominant aerosol component with on average 0.115 μg m-3 (detection limit 0.003 μg m-3). The second most abundant component was undifferentiated organic aerosol, with on average 0.11 μg m-3 detection limit (0.04 μg m-3). The nitrate component, which averaged 0.007 μg m-3, was above its detection limit (0.002 μg m-3), whereas the ammonium ion had an apparent average concentration of 0.02 μg m-3, which was approximately equal to its detection limit. A few episodes having increased mass concentrations and lasting from several hours to several days are apparent in the data. These were investigated further using a statistical analysis to determine their common characteristics. High correlations among some of the components arriving during the short term episodes provide

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

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F. Freutel

2013-01-01

Full Text Available During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. 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 measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m⁻³, 2 μg m⁻³, 2 μg m⁻³, and 7 μg m⁻³, respectively were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m⁻³, 0.2 μg m⁻³, 0.4 μg m⁻³, and 1–3 μg m⁻³, respectively. For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NO_x it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be

A parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models: improvement of particulate nitrate prediction

Science.gov (United States)

Chen, Ying; Wolke, Ralf; Ran, Liang; Birmili, Wolfram; Spindler, Gerald; Schröder, Wolfram; Su, Hang; Cheng, Yafang; Tegen, Ina; Wiedensohler, Alfred

2018-01-01

The heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T), relative humidity (RH), aerosol particle composition, and the surface area concentration (S). However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5) of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R = 0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMO-MUSCAT, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10-25 September 2013) to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3-]) were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz). The modelled [NO3-] was significantly overestimated for this period by a factor of 5-19, with the corrected NH3 emissions (reduced by 50 %) and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3-] by ˜ 35 %. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17-18 and 25 September 2013) when [NO3-] was dominated by local chemical formations. In our case, the suppression of organic coating was negligible over western and central Europe

Two-Column Aerosol Project (TCAP) Field Campaign Report

Energy Technology Data Exchange (ETDEWEB)

Berg, Larry K [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

2016-05-01

This study included the deployment of the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility’s Mobile Facility (AMF), ARM Mobile Aerosol Observing System (MAOS) and the ARM Aerial Facility (AAF). The study was a collaborative effort involving scientists from DOE national laboratories, NOAA, NASA, and universities. The AAF and MAOS were deployed for two approximately month-long Intensive Operational Periods (IOPs) conducted in June 2012 and February 2013. Seasonal differences in the aerosol chemical and optical properties observed using the AMF, AAF, and MAOS are presented in this report. The total mass loading of aerosol is found to be much greater in the summer than in the winter, with the difference associated with greater amounts of organic aerosol. The mass fraction of organic aerosol is much reduced in the winter, when sulfate is the dominant aerosol type. Surprisingly, very little sea-salt aerosol was observed in the summer. In contrast, much more sea salt aerosol was observed in the winter. The mass loading of black carbon is nearly the same in both seasons. These differences lead to a relative increase in the aerosol light absorption in the winter and an associated decrease in observed single-scattering albedo. Measurements of aerosol mixing state were made using a single-particle mass spectrometer, which showed that the majority of the summertime aerosol consisted of organic compounds mixed with various amounts of sulfate. A number of other findings are also summarized in the report, including: impact of aerosol layers aloft on the column aerosol optical depth; documentation of the aerosol properties at the AMF; differences in the aerosol properties associated with both columns, which are not systematic but reflect the complicated meteorological and chemical processes that impact aerosol as it is advected away from North America; and new instruments and data-processing techniques for measuring both aerosol and

Development and calibration of an on-line aerosol monitor for PHEBUS test FPT1

International Nuclear Information System (INIS)

O'Brien, J.E.; Carmack, W.J.; Sprenger, M.H.; Thurston, G.C.; Hunt, J.L.

1994-10-01

An on-line aerosol monitor (OLAM2) has been developed and tested for PHEBUS test FPT1. OLAM2 utilizes new detachable fiber optic cables and sapphire light pipes for light transmission between the OLAM and the electronics. This light transmission system was tested and found to provide better signal-to-noise performance than was achieved with the continuous fibers used for test FPT0. An additional advantage of the detachable fiber/light pipe system is ease of installation. Aerosol testing (OLAM calibration) was performed in order to verify adequate signal-to-noise performance of the new fiber optic system over the specified operating conditions and to check the quantitative light attenuation measurements against theoretical predictions. Results of the testing indicated that light extinction measurements obtained during Phebus tests could be used to estimate aerosol volume concentrations, if diamond window fouling can be avoided. OLAM2 was also subjected to a proof pressure test and a long-term thermal stability test. These tests verified the mechanical and thermal integrity of the OLAM within design specifications. Long-term output signal stability was also verified with the system maintained at design temperature and half-design pressure

Overview of aerosol properties associated with air masses sampled by the ATR-42 during the EUCAARI campaign (2008

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S. Crumeyrolle

2013-05-01

Full Text Available Within the frame of the European Aerosol Cloud Climate and Air Quality Interactions (EUCAARI project, the Météo-France aircraft ATR-42 performed 22 research flights over central Europe and the North Sea during the intensive observation period in May 2008. For the campaign, the ATR-42 was equipped to study the aerosol physical, chemical, hygroscopic and optical properties, as well as cloud microphysics. For the 22 research flights, retroplume analyses along the flight tracks were performed with FLEXPART in order to classify air masses into five sectors of origin, allowing for a qualitative evaluation of emission influence on the respective air parcel. This study shows that the extensive aerosol parameters (aerosol mass and number concentrations show vertical decreasing gradients and in some air masses maximum mass concentrations (mainly organics in an intermediate layer (1–3 km. The observed mass concentrations (in the boundary layer (BL: between 10 and 30 μg m−3; lower free troposphere (LFT: 0.8 and 14 μg m−3 are high especially in comparison with the 2015 European norms for PM2.5 (25 μg m−3 and with previous airborne studies performed over England (Morgan et al., 2009; McMeeking et al., 2012. Particle number size distributions show a larger fraction of particles in the accumulation size range in the LFT compared to BL. The chemical composition of submicron aerosol particles is dominated by organics in the BL, while ammonium sulphate dominates the submicron aerosols in the LFT, especially in the aerosol particles originated from north-eastern Europe (~ 80%, also experiencing nucleation events along the transport. As a consequence, first the particle CCN acting ability, shown by the CCN/CN ratio, and second the average values of the scattering cross sections of optically active particles (i.e. scattering coefficient divided by the optical active particle concentration are increased in the LFT compared to BL.

Elemental analysis of chamber organic aerosol using an aerodyne high-resolution aerosol mass spectrometer

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P. S. Chhabra

2010-05-01

Full Text Available The elemental composition of laboratory chamber secondary organic aerosol (SOA from glyoxal uptake, α-pinene ozonolysis, isoprene photooxidation, single-ring aromatic photooxidation, and naphthalene photooxidation is evaluated using Aerodyne high-resolution time-of-flight mass spectrometer data. SOA O/C ratios range from 1.13 for glyoxal uptake experiments to 0.30–0.43 for α-pinene ozonolysis. The elemental composition of α-pinene and naphthalene SOA is also confirmed by offline mass spectrometry. The fraction of organic signal at m/z 44 is generally a good measure of SOA oxygenation for α-pinene/O₃, isoprene/high-NO_x, and naphthalene SOA systems. The agreement between measured and estimated O/C ratios tends to get closer as the fraction of organic signal at m/z 44 increases. This is in contrast to the glyoxal uptake system, in which m/z 44 substantially underpredicts O/C. Although chamber SOA has generally been considered less oxygenated than ambient SOA, single-ring aromatic- and naphthalene-derived SOA can reach O/C ratios upward of 0.7, well within the range of ambient PMF component OOA, though still not as high as some ambient measurements. The spectra of aromatic and isoprene-high-NO_x SOA resemble that of OOA, but the spectrum of glyoxal uptake does not resemble that of any ambient organic aerosol PMF component.

Constraining Aerosol Optical Models Using Ground-Based, Collocated Particle Size and Mass Measurements in Variable Air Mass Regimes During the 7-SEAS/Dongsha Experiment

Science.gov (United States)

Bell, Shaun W.; Hansell, Richard A.; Chow, Judith C.; Tsay, Si-Chee; Wang, Sheng-Hsiang; Ji, Qiang; Li, Can; Watson, John G.; Khlystov, Andrey

2012-01-01

During the spring of 2010, NASA Goddard's COMMIT ground-based mobile laboratory was stationed on Dongsha Island off the southwest coast of Taiwan, in preparation for the upcoming 2012 7-SEAS field campaign. The measurement period offered a unique opportunity for conducting detailed investigations of the optical properties of aerosols associated with different air mass regimes including background maritime and those contaminated by anthropogenic air pollution and mineral dust. What appears to be the first time for this region, a shortwave optical closure experiment for both scattering and absorption was attempted over a 12-day period during which aerosols exhibited the most change. Constraints to the optical model included combined SMPS and APS number concentration data for a continuum of fine and coarse-mode particle sizes up to PM2.5. We also take advantage of an IMPROVE chemical sampler to help constrain aerosol composition and mass partitioning of key elemental species including sea-salt, particulate organic matter, soil, non sea-salt sulphate, nitrate, and elemental carbon. Our results demonstrate that the observed aerosol scattering and absorption for these diverse air masses are reasonably captured by the model, where peak aerosol events and transitions between key aerosols types are evident. Signatures of heavy polluted aerosol composed mostly of ammonium and non sea-salt sulphate mixed with some dust with transitions to background sea-salt conditions are apparent in the absorption data, which is particularly reassuring owing to the large variability in the imaginary component of the refractive indices. Extinctive features at significantly smaller time scales than the one-day sample period of IMPROVE are more difficult to reproduce, as this requires further knowledge concerning the source apportionment of major chemical components in the model. Consistency between the measured and modeled optical parameters serves as an important link for advancing remote

Laboratory investigation of photochemical oxidation of organic aerosol from wood fires 2: analysis of aerosol mass spectrometer data

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A. P. Grieshop

2009-03-01

Full Text Available Experiments were conducted to investigate the effects of photo-oxidation on organic aerosol (OA in dilute wood smoke by exposing emissions from soft- and hard-wood fires to UV light in a smog chamber. This paper focuses on changes in OA composition measured using a unit-mass-resolution quadrupole Aerosol Mass Spectrometer (AMS. The results highlight how photochemical processing can lead to considerable evolution of the mass, volatility and level of oxygenation of biomass-burning OA. Photochemical oxidation produced substantial new OA, more than doubling the OA mass after a few hours of aging under typical summertime conditions. Aging also decreased the volatility of the OA and made it progressively more oxygenated. The results also illustrate strengths of, and challenges with, using AMS data for source apportionment analysis. For example, the mass spectra of fresh and aged BBOA are distinct from fresh motor-vehicle emissions. The mass spectra of the secondary OA produced from aging wood smoke are very similar to those of the oxygenated OA (OOA that dominates ambient AMS datasets, further reinforcing the connection between OOA and OA formed from photo-chemistry. In addition, aged wood smoke spectra are similar to those from OA created by photo-oxidizing dilute diesel exhaust. This demonstrates that the OOA observed in the atmosphere can be produced by photochemical aging of dilute emissions from different types of combustion systems operating on fuels with modern or fossil carbon. Since OOA is frequently the dominant component of ambient OA, the similarity of spectra of aged emissions from different sources represents an important challenge for AMS-based source apportionment studies.

Detection of biological particles in ambient air using Bio-Aerosol Mass Spectrometry

International Nuclear Information System (INIS)

McJimpsey, E L; Steele, P T; Coffee, K R; Fergenson, D P; Riot, V J; Woods, B W; Gard, E E; Frank, M; Tobias, H J; Lebrilla, C

2006-01-01

The Bio-Aerosol Mass Spectrometry (BAMS) system is an instrument used for the real time detection and identification of biological aerosols. Particles are drawn from the atmosphere directly into vacuum and tracked as they scatter light from several continuous wave lasers. After tracking, the fluorescence of individual particles is excited by a pulsed 266nm or 355nm laser. Molecules from those particles with appropriate fluorescence properties are subsequently desorbed and ionized using a pulsed 266nm laser. Resulting ions are analyzed in a dual polarity mass spectrometer. During two field deployments at the San Francisco International Airport, millions of ambient particles were analyzed and a small but significant fraction were found to have fluorescent properties similar to Bacillus spores and vegetative cells. Further separation of non-biological background particles from potential biological particles was accomplished using laser desorption/ionization mass spectrometry. This has been shown to enable some level of species differentiation in specific cases, but the creation and observation of higher mass ions is needed to enable a higher level of specificity across more species. A soft ionization technique, matrix-assisted laser desorption/ionization (MALDI) is being investigated for this purpose. MALDI is particularly well suited for mass analysis of biomolecules since it allows for the generation of molecular ions from large mass compounds that would fragment under normal irradiation. Some of the initial results from a modified BAMS system utilizing this technique are described

New characteristics of submicron aerosols and factor analysis of combined organic and inorganic aerosol mass spectra during winter in Beijing

Science.gov (United States)

Zhang, J. K.; Ji, D. S.; Liu, Z. R.; Hu, B.; Wang, L. L.; Huang, X. J.; Wang, Y. S.

2015-07-01

In recent years, an increasing amount of attention has been paid to heavy haze pollution in Beijing, China. In addition to Beijing's population of approximately 20 million and its 5 million vehicles, nearby cities and provinces are host to hundreds of heavily polluting industries. In this study, a comparison between observations in January 2013 and January 2014 showed that non-refractory PM1 (NR-PM1) pollution was weaker in January 2014, which was primarily caused by variations in meteorological conditions. For the first time, positive matrix factorization (PMF) was applied to the merged high-resolution mass spectra of organic and inorganic aerosols from aerosol mass spectrometer measurements in Beijing, and the sources and evolution of NR-PM1 in January 2014 were investigated. The two factors, NO3-OA1 and NO3-OA2, were primarily composed of ammonium nitrate, and each showed a different degree of oxidation and diurnal variation. The organic fraction of SO4-OA showed the highest degree of oxidation of all PMF factors. The hydrocarbon-like organic aerosol (OA) and cooking OA factors contained negligible amounts of inorganic species. The coal combustion OA factor contained a high contribution from chloride in its mass spectrum. The NR-PM1 composition showed significant variations in January 2014, in which the contribution of nitrate clearly increased during heavy pollution events. The most effective way to control fine particle pollution in Beijing is through joint prevention and control measures at the regional level, rather than a focus on an individual city, especially for severe haze events.

Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically resolved aerosol fluxes

Directory of Open Access Journals (Sweden)

D. K. Farmer

2011-06-01

Full Text Available Although laboratory studies show that biogenic volatile organic compounds (VOCs yield substantial secondary organic aerosol (SOA, production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR PM₁ fluxes. Average deposition velocities for total NR-PM₁ aerosol at noon were 2.05 ± 0.04 mm s⁻¹. Using a high resolution measurement of the NH₂⁺ and NH₃⁺ fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm s⁻¹ and are dominated by deposition of ammonium sulphate.

Chemical composition and characteristics of ambient aerosols and rainwater residues during Indian summer monsoon: Insight from aerosol mass spectrometry

Science.gov (United States)

Chakraborty, Abhishek; Gupta, Tarun; Tripathi, Sachchida N.

2016-07-01

Real time composition of non-refractory submicron aerosol (NR-PM1) is measured via Aerosol mass spectrometer (AMS) for the first time during Indian summer monsoon at Kanpur, a polluted urban location located at the heart of Indo Gangetic Plain (IGP). Submicron aerosols are found to be dominated by organics followed by nitrate. Source apportionment of organic aerosols (OA) via positive matrix factorization (PMF) revealed several types of secondary/oxidized and primary organic aerosols. On average, OA are completely dominated by oxidized OA with a very little contribution from biomass burning OA. During rain events, PM1 concentration is decreased almost by 60%, but its composition remains nearly the same. Oxidized OA showed slightly more decrease than primary OAs, probably due to their higher hygroscopicity. The presence of organo nitrates (ON) is also detected in ambient aerosols. Apart from real-time sampling, collected fog and rainwater samples were also analyzed via AMS in offline mode and in the ICP-OES (Inductively coupled plasma - Optical emission spectrometry) for elements. The presence of sea salt, organo nitrates and sulfates has been observed. Rainwater residues are also dominated by organics but their O/C ratios are 15-20% lower than the observed values for ambient OA. Alkali metals such as Ca, Na, K are found to be most abundant in the rainwater followed by Zn. Rainwater residues are also found to be much less oxidized than the aerosols present inside the fog water, indicating presence of less oxidized organics. These findings indicate that rain can act as an effective scavenger of different types of pollutants even for submicron particle range. Rainwater residues also contain organo sulfates which indicate that some portion of the dissolved aerosols has undergone aqueous processing, possibly inside the cloud. Highly oxidized and possibly hygroscopic OA during monsoon period compared to other seasons (winter, post monsoon), indicates that they can act

Estimation of Uncertainty in Aerosol Concentration Measured by Aerosol Sampling System

Energy Technology Data Exchange (ETDEWEB)

Lee, Jong Chan; Song, Yong Jae; Jung, Woo Young; Lee, Hyun Chul; Kim, Gyu Tae; Lee, Doo Yong [FNC Technology Co., Yongin (Korea, Republic of)

2016-10-15

FNC Technology Co., Ltd has been developed test facilities for the aerosol generation, mixing, sampling and measurement under high pressure and high temperature conditions. The aerosol generation system is connected to the aerosol mixing system which injects SiO{sub 2}/ethanol mixture. In the sampling system, glass fiber membrane filter has been used to measure average mass concentration. Based on the experimental results using main carrier gas of steam and air mixture, the uncertainty estimation of the sampled aerosol concentration was performed by applying Gaussian error propagation law. FNC Technology Co., Ltd. has been developed the experimental facilities for the aerosol measurement under high pressure and high temperature. The purpose of the tests is to develop commercial test module for aerosol generation, mixing and sampling system applicable to environmental industry and safety related system in nuclear power plant. For the uncertainty calculation of aerosol concentration, the value of the sampled aerosol concentration is not measured directly, but must be calculated from other quantities. The uncertainty of the sampled aerosol concentration is a function of flow rates of air and steam, sampled mass, sampling time, condensed steam mass and its absolute errors. These variables propagate to the combination of variables in the function. Using operating parameters and its single errors from the aerosol test cases performed at FNC, the uncertainty of aerosol concentration evaluated by Gaussian error propagation law is less than 1%. The results of uncertainty estimation in the aerosol sampling system will be utilized for the system performance data.

Characterization of primary organic aerosol emissions from meat cooking, trash burning, and motor vehicles with high-resolution aerosol mass spectrometry and comparison with ambient and chamber observations.

Science.gov (United States)

Mohr, Claudia; Huffman, Alex; Cubison, Michael J; Aiken, Allison C; Docherty, Kenneth S; Kimmel, Joel R; Ulbrich, Ingrid M; Hannigan, Michael; Jimenez, Jose L

2009-04-01

Organic aerosol (OA) emissions from motor vehicles, meat-cooking and trash burning are analyzed here using a high-resolution aerosol mass spectrometer (AMS). High resolution data show that aerosols emitted by combustion engines and plastic burning are dominated by hydrocarbon-like organic compounds. Meat cooking and especially paper burning emissions contain significant fractions of oxygenated organic compounds; however, their unit-resolution mass spectral signatures are very similar to those from ambient hydrocarbon-like OA, and very different from the mass spectra of ambient secondary or oxygenated OA (OOA). Thus, primary OA from these sources is unlikelyto be a significant direct source of ambient OOA. There are significant differences in high-resolution tracer m/zs that may be useful for differentiating some of these sources. Unlike in most ambient spectra, all of these sources have low total m/z 44 and this signal is not dominated by the CO2+ ion. All sources have high m/z 57, which is low during high OOA ambient periods. Spectra from paper burning are similar to some types of biomass burning OA, with elevated m/z 60. Meat cooking aerosols also have slightly elevated m/z 60, whereas motor vehicle emissions have very low signal at this m/z.

Gasoline emissions dominate over diesel in formation of secondary organic aerosol mass

Science.gov (United States)

Bahreini, R.; Middlebrook, A. M.; de Gouw, J. A.; Warneke, C.; Trainer, M.; Brock, C. A.; Stark, H.; Brown, S. S.; Dube, W. P.; Gilman, J. B.; Hall, K.; Holloway, J. S.; Kuster, W. C.; Perring, A. E.; Prevot, A. S. H.; Schwarz, J. P.; Spackman, J. R.; Szidat, S.; Wagner, N. L.; Weber, R. J.; Zotter, P.; Parrish, D. D.

2012-03-01

Although laboratory experiments have shown that organic compounds in both gasoline fuel and diesel engine exhaust can form secondary organic aerosol (SOA), the fractional contribution from gasoline and diesel exhaust emissions to ambient SOA in urban environments is poorly known. Here we use airborne and ground-based measurements of organic aerosol (OA) in the Los Angeles (LA) Basin, California made during May and June 2010 to assess the amount of SOA formed from diesel emissions. Diesel emissions in the LA Basin vary between weekdays and weekends, with 54% lower diesel emissions on weekends. Despite this difference in source contributions, in air masses with similar degrees of photochemical processing, formation of OA is the same on weekends and weekdays, within the measurement uncertainties. This result indicates that the contribution from diesel emissions to SOA formation is zero within our uncertainties. Therefore, substantial reductions of SOA mass on local to global scales will be achieved by reducing gasoline vehicle emissions.

Preliminary observations of organic gas-particle partitioning from biomass combustion smoke using an aerosol mass spectrometer

Science.gov (United States)

T. Lee; S. M. Kreidenweis; J. L. Collett; A. P. Sullivan; C. M. Carrico; J. L. Jimenez; M. Cubison; S. Saarikoski; D. R. Worsnop; T. B. Onasch; E. Fortner; W. C. Malm; E. Lincoln; Cyle Wold; WeiMin Hao

2010-01-01

Aerosols play important roles in adverse health effects, indirect and direct forcing of Earth’s climate, and visibility degradation. Biomass burning emissions from wild and prescribed fires can make a significant contribution to ambient aerosol mass in many locations and seasons. In order to better understand the chemical properties of particles produced by combustion...

Real-time analysis of organic compounds in ship engine aerosol emissions using resonance-enhanced multiphoton ionisation and proton transfer mass spectrometry.

Science.gov (United States)

Radischat, Christian; Sippula, Olli; Stengel, Benjamin; Klingbeil, Sophie; Sklorz, Martin; Rabe, Rom; Streibel, Thorsten; Harndorf, Horst; Zimmermann, Ralf

2015-08-01

Organic combustion aerosols from a marine medium-speed diesel engine, capable to run on distillate (diesel fuel) and residual fuels (heavy fuel oil), were investigated under various operating conditions and engine parameters. The online chemical characterisation of the organic components was conducted using a resonance-enhanced multiphoton ionisation time-of-flight mass spectrometer (REMPI TOF MS) and a proton transfer reaction-quadrupole mass spectrometer (PTR-QMS). Oxygenated species, alkenes and aromatic hydrocarbons were characterised. Especially the aromatic hydrocarbons and their alkylated derivatives were very prominent in the exhaust of both fuels. Emission factors of known health-hazardous compounds (e.g. mono- and poly-aromatic hydrocarbons) were calculated and found in higher amounts for heavy fuel oil (HFO) at typical engine loadings. Lower engine loads lead in general to increasing emissions for both fuels for almost every compound, e.g. naphthalene emissions varied for diesel fuel exhaust between 0.7 mg/kWh (75 % engine load, late start of injection (SOI)) and 11.8 mg/kWh (10 % engine load, late SOI) and for HFO exhaust between 3.3 and 60.5 mg/kWh, respectively. Both used mass spectrometric techniques showed that they are particularly suitable methods for online monitoring of combustion compounds and very helpful for the characterisation of health-relevant substances. Graphical abstract Three-dimensional REMPI data of organic species in diesel fuel and heavy fuel oil exhaust.

Physical metrology of aerosols; Metrologie physique des aerosols

Energy Technology Data Exchange (ETDEWEB)

Boulaud, D.; Vendel, J. [CEA Saclay, 91 - Gif-sur-Yvette (France). Inst. de Protection et de Surete Nucleaire

1996-12-31

The various detection and measuring methods for aerosols are presented, and their selection is related to aerosol characteristics (size range, concentration or mass range), thermo-hydraulic conditions (carrier fluid temperature, pressure and flow rate) and to the measuring system conditions (measuring frequency, data collection speed, cost...). Methods based on aerosol dynamic properties (inertial, diffusional and electrical methods) and aerosol optical properties (localized and integral methods) are described and their performances and applications are compared

A study of photochemical againg of ambient air using Potential Aerosol Mass (PAM) chamber under the different sources and types of emissions

Science.gov (United States)

Lee, T.; Son, J.; Kim, J.; Kim, S.; Sung, K.; Park, G.; Link, M.; Park, T.; Kim, K.; Kang, S.; Ban, J.; Kim, D. S.

2016-12-01

Recent research proposed that Secondary Aerosol (SA) is important class of predicting future climate change scenarios, health effect, and a general air quality. However, there has been lack of studies to investigate SA formation all over the world. This study tried to focus on understanding potential secondary aerosol formation and its local impact by the photochemical aging of inorganic and organic aerosols in the ambient air using the Potential Aerosol Mass (PAM) chamber under the different sources and types of emissions. PAM chamber manufactured by Aerodyne make an oxidizing environment that simulates oxidation processes on timescales of 12-15 hrs in the atmosphere. Chemical compositions of ambient aerosol and aerosol that was aged in the PAM chamber were alternately measured every 2-minutes using the High Resolution-Time of Flight-Aerosol Mass Spectrometer (HR-ToF-AMS). HR-ToF-AMS provides non-refractory aerosol mass concentrations including nitrate, sulfate, hydrocarbon-like and oxygenated organic aerosol in real time. This study includes a residence area of mixture of sources, a forest site of dominant source of biogenic VOCs, an underground parking lot of dominant vehicle emission, and laboratory experiment of vehicle emissions under different fuels and speeds using the chassis dynamometer. As a result, it was revealed that gasoline and LPG vehicle relatively made more potential SA than diesel vehicle.

A parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models: improvement of particulate nitrate prediction

Directory of Open Access Journals (Sweden)

Y. Chen

2018-01-01

Full Text Available The heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T, relative humidity (RH, aerosol particle composition, and the surface area concentration (S. However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5 of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R =  0.91 between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMO–MUSCAT, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10–25 September 2013 to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3−] were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz. The modelled [NO3−] was significantly overestimated for this period by a factor of 5–19, with the corrected NH3 emissions (reduced by 50 % and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3−] by  ∼  35 %. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17–18 and 25 September 2013 when [NO3−] was dominated by local chemical formations. In our case, the suppression of organic coating

A reference aerosol for a radon reference chamber

Science.gov (United States)

Paul, Annette; Keyser, Uwe

1996-02-01

The measurement of radon and radon progenies and the calibration of their detection systems require the production and measurement of aerosols well-defined in size and concentration. In the German radon reference chamber, because of its unique chemical and physical properties, carnauba wax is used to produce standard aerosols. The aerosol size spectra are measured on-line by an aerosol measurement system in the range of 10 nm to 1 μm aerodynamic diameter. The experimental set-ups for the study of adsorption of radioactive ions on aerosols as function of their size and concentration will be described, the results presented and further adaptations for an aerosol jet introduced (for example, for the measurement of short-lived neutron-rich isotopes). Data on the dependence of aerosol radius, ion concentration and element selectivity is collected by using a 252Cf-sf source. The fission products of this source range widely in elements, isotopes and charges. Adsorption and the transport of radioactive ions on aerosols have therefore been studied for various ions for the first time, simultaneously with the aerosol size on-line spectrometry.

A reference aerosol for a radon reference chamber

Energy Technology Data Exchange (ETDEWEB)

Paul, A. [Physikalisch-Technische Bundesanstalt, Braunschweig (Germany); Keyser, U. [Physikalisch-Technische Bundesanstalt, Braunschweig (Germany)

1996-01-11

The measurement of radon and radon progenies and the calibration of their detection systems require the production and measurement of aerosols well-defined in size and concentration. In the German radon reference chamber, because of its unique chemical and physical properties, carnauba wax is used to produce standard aerosols. The aerosol size spectra are measured on-line by an aerosol measurement system in the range of 10 nm to 1 {mu}m aerodynamic diameter. The experimental set-ups for the study of adsorption of radioactive ions on aerosols as function of their size and concentration are described, the results presented and further adaptations for an aerosol jet introduced (for example, for the measurement of short-lived neutron-rich isotopes). Data on the dependence of aerosol radius, ion concentration and element selectivity is collected by using a {sup 252}Cf-sf source. The fission products of this source range widely in elements, isotopes and charges. Adsorption and the transport of radioactive ions on aerosols have therefore been studied for various ions for the first time, simultaneously with the aerosol size on-line spectrometry. (orig.).

Separating refractory and non-refractory particulate chloride and estimating chloride depletion by aerosol mass spectrometry in a marine environment

OpenAIRE

I. Nuaaman; S.-M. Li; K. L. Hayden; T. B. Onasch; P. Massoli; D. Sueper; D. R. Worsnop; T. S. Bates; P. K. Quinn; R. McLaren

2015-01-01

Aerosol composition and concentration measurements along the coast of California were obtained using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) onboard the research vessel Atlantis during the CalNex study in 2010. This paper focuses on the measurement of aerosol chloride using the HR-AMS that can be ambiguous in regions with significant quantities of sea salt aerosols. This ambiguity arises due to large differences in the sensitivity of the HR...

Aerosol formation from high-velocity uranium drops: Comparison of number and mass distributions. Final report

Energy Technology Data Exchange (ETDEWEB)

Rader, D.J.; Benson, D.A.

1995-05-01

This report presents the results of an experimental study of the aerosol produced by the combustion of high-velocity molten-uranium droplets produced by the simultaneous heating and electromagnetic launch of uranium wires. These tests are intended to simulate the reduction of high-velocity fragments into aerosol in high-explosive detonations or reactor accidents involving nuclear materials. As reported earlier, the resulting aerosol consists mainly of web-like chain agglomerates. A condensation nucleus counter was used to investigate the decay of the total particle concentration due to coagulation and losses. Number size distributions based on mobility equivalent diameter obtained soon after launch with a Differential Mobility Particle Sizer showed lognormal distributions with an initial count median diameter (CMD) of 0.3 {mu}m and a geometric standard deviation, {sigma}{sub g} of about 2; the CMD was found to increase and {sigma}{sub g} decrease with time due to coagulation. Mass size distributions based on aerodynamic diameter were obtained for the first time with a Microorifice Uniform Deposit Impactor, which showed lognormal distributions with mass median aerodynamic diameters of about 0.5 {mu}m and an aerodynamic geometric standard deviation of about 2. Approximate methods for converting between number and mass distributions and between mobility and aerodynamic equivalent diameters are presented.

Aerosol formation from high-velocity uranium drops: Comparison of number and mass distributions. Final report

International Nuclear Information System (INIS)

Rader, D.J.; Benson, D.A.

1995-05-01

This report presents the results of an experimental study of the aerosol produced by the combustion of high-velocity molten-uranium droplets produced by the simultaneous heating and electromagnetic launch of uranium wires. These tests are intended to simulate the reduction of high-velocity fragments into aerosol in high-explosive detonations or reactor accidents involving nuclear materials. As reported earlier, the resulting aerosol consists mainly of web-like chain agglomerates. A condensation nucleus counter was used to investigate the decay of the total particle concentration due to coagulation and losses. Number size distributions based on mobility equivalent diameter obtained soon after launch with a Differential Mobility Particle Sizer showed lognormal distributions with an initial count median diameter (CMD) of 0.3 μm and a geometric standard deviation, σ g of about 2; the CMD was found to increase and σ g decrease with time due to coagulation. Mass size distributions based on aerodynamic diameter were obtained for the first time with a Microorifice Uniform Deposit Impactor, which showed lognormal distributions with mass median aerodynamic diameters of about 0.5 μm and an aerodynamic geometric standard deviation of about 2. Approximate methods for converting between number and mass distributions and between mobility and aerodynamic equivalent diameters are presented

Molecular composition of organic aerosols in central Amazonia: an ultra-high-resolution mass spectrometry study

OpenAIRE

Kourtchev, I; Godoi, RHM; Connors, S; Levine, JG; Archibald, AT; Godoi, AFL; Paralovo, SL; Barbosa, CGG; Souza, RAF; Manzi, AO; Seco, R; Sjostedt, S; Park, J-H; Guenther, A; Kim, S

2016-01-01

The Amazon Basin plays key role in atmospheric chemistry, biodiversity and climate change. In this study we applied nanoelectrospray (nanoESI) ultra-high-resolution mass spectrometry (UHRMS) for the analysis of the organic fraction of PM$_{2.5}$ aerosol samples collected during dry and wet seasons at a site in central Amazonia receiving background air masses, biomass burning and urban pollution. Comprehensive mass spectral data evaluation methods (e.g. Kendrick mass defect, Van Krevelen diagr...

A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

Directory of Open Access Journals (Sweden)

M. F. Heringa

2012-02-01

Full Text Available Organic aerosol (OA represents a significant and often major fraction of the non-refractory PM₁ (particulate matter with an aerodynamic diameter d_a < 1 μm mass. Secondary organic aerosol (SOA is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS and compared to SOA from α-pinene.

The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production.

Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra showing Pearson's r values >0.94 for the correlations between the four different SOA types after five hours of aging. High-resolution mass spectra (HR-MS showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C₂H₃O⁺ and CO₂⁺, respectively, similarly to the relatively fresh semi-volatile oxygenated OA (SV-OOA observed in the ambient aerosol. The atomic O:C ratios were found to be in the range of 0.25–0.55 with no major increase during the first five hours of aging. On average, the diesel SOA showed the lowest O:C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions revealed that the SOA source with the highest O:C ratio had the largest fraction of small ions.

The HR data of the four sources could be clustered and separated using

Improved identification of primary biological aerosol particles using single-particle mass spectrometry

Directory of Open Access Journals (Sweden)

M. A. Zawadowicz

2017-06-01

Full Text Available Measurements of primary biological aerosol particles (PBAP, especially at altitudes relevant to cloud formation, are scarce. Single-particle mass spectrometry (SPMS has been used to probe aerosol chemical composition from ground and aircraft for over 20 years. Here we develop a method for identifying bioaerosols (PBAP and particles containing fragments of PBAP as part of an internal mixture using SPMS. We show that identification of bioaerosol using SPMS is complicated because phosphorus-bearing mineral dust and phosphorus-rich combustion by-products such as fly ash produce mass spectra with peaks similar to those typically used as markers for bioaerosol. We have developed a methodology to differentiate and identify bioaerosol using machine learning statistical techniques applied to mass spectra of known particle types. This improved method provides far fewer false positives compared to approaches reported in the literature. The new method was then applied to two sets of ambient data collected at Storm Peak Laboratory and a forested site in Central Valley, California to show that 0.04–2 % of particles in the 200–3000 nm aerodynamic diameter range were identified as bioaerosol. In addition, 36–56 % of particles identified as biological also contained spectral features consistent with mineral dust, suggesting internal dust–biological mixtures.

Variability of aerosol, gaseous pollutants and meteorological characteristics associated with changes in air mass origin at the SW Atlantic coast of Iberia

Directory of Open Access Journals (Sweden)

J.-M. Diesch

2012-04-01

Full Text Available Measurements of the ambient aerosol were performed at the Southern coast of Spain, within the framework of the DOMINO (Diel Oxidant Mechanisms In relation to Nitrogen Oxides project. The field campaign took place from 20 November until 9 December 2008 at the atmospheric research station "El Arenosillo" (37°5'47.76" N, 6°44'6.94" W. As the monitoring station is located at the interface between a natural park, industrial cities (Huelva, Seville and the Atlantic Ocean, a variety of physical and chemical parameters of aerosols and gas phase could be characterized in dependency on the origin of air masses. Backwards trajectories were examined and compared with local meteorology to classify characteristic air mass types for several source regions. Aerosol number and mass as well as polycyclic aromatic hydrocarbons and black carbon concentrations were measured in PM₁ and size distributions were registered covering a size range from 7 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol (NR-PM₁ was measured by means of an Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS. Gas phase analyzers monitored various trace gases (O₃, SO₂, NO, NO₂, CO₂ and a weather station provided meteorological parameters.

Lowest average submicron particle mass and number concentrations were found in air masses arriving from the Atlantic Ocean with values around 2 μg m⁻³ and 1000 cm⁻³. These mass concentrations were about two to four times lower than the values recorded in air masses of continental and urban origins. For some species PM₁-fractions in marine air were significantly larger than in air masses originating from Huelva, a closely located city with extensive industrial activities. The largest fraction of sulfate (54% was detected in marine air masses and was to a high degree not neutralized. In addition, small concentrations of

Variability of aerosol, gaseous pollutants and meteorological characteristics associated with changes in air mass origin at the SW Atlantic coast of Iberia

Science.gov (United States)

Diesch, J.-M.; Drewnick, F.; Zorn, S. R.; von der Weiden-Reinmüller, S.-L.; Martinez, M.; Borrmann, S.

2012-04-01

Measurements of the ambient aerosol were performed at the Southern coast of Spain, within the framework of the DOMINO (Diel Oxidant Mechanisms In relation to Nitrogen Oxides) project. The field campaign took place from 20 November until 9 December 2008 at the atmospheric research station "El Arenosillo" (37°5'47.76" N, 6°44'6.94" W). As the monitoring station is located at the interface between a natural park, industrial cities (Huelva, Seville) and the Atlantic Ocean, a variety of physical and chemical parameters of aerosols and gas phase could be characterized in dependency on the origin of air masses. Backwards trajectories were examined and compared with local meteorology to classify characteristic air mass types for several source regions. Aerosol number and mass as well as polycyclic aromatic hydrocarbons and black carbon concentrations were measured in PM1 and size distributions were registered covering a size range from 7 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol (NR-PM1) was measured by means of an Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS). Gas phase analyzers monitored various trace gases (O3, SO2, NO, NO2, CO2) and a weather station provided meteorological parameters. Lowest average submicron particle mass and number concentrations were found in air masses arriving from the Atlantic Ocean with values around 2 μg m-3 and 1000 cm-3. These mass concentrations were about two to four times lower than the values recorded in air masses of continental and urban origins. For some species PM1-fractions in marine air were significantly larger than in air masses originating from Huelva, a closely located city with extensive industrial activities. The largest fraction of sulfate (54%) was detected in marine air masses and was to a high degree not neutralized. In addition, small concentrations of methanesulfonic acid (MSA), a product of biogenic dimethyl sulfate (DMS) emissions, could be identified in the particle phase

Effect of relative humidity on soot - secondary organic aerosol mixing: A case study from the Soot Aerosol Aging Study (PNNL-SAAS)

Science.gov (United States)

Sharma, N.; China, S.; Zaveri, R. A.; Shilling, J. E.; Pekour, M. S.; Liu, S.; Aiken, A. C.; Dubey, M. K.; Wilson, J. M.; Zelenyuk, A.; OBrien, R. E.; Moffet, R.; Gilles, M. K.; Gourihar, K.; Chand, D.; Sedlacek, A. J., III; Subramanian, R.; Onasch, T. B.; Laskin, A.; Mazzoleni, C.

2014-12-01

Atmospheric processing of fresh soot particles emitted by anthropogenic as well as natural sources alters their physical and chemical properties. For example, fresh and aged soot particles interact differently with incident solar radiation, resulting in different overall radiation budgets. Varying atmospheric chemical and meteorological conditions can result in complex soot mixing states. The Soot Aerosol Aging Study (SAAS) was conducted at the Pacific Northwest National Laboratory in November 2013 and January 2014 as a step towards understanding the evolution of mixing state of soot and its impact on climate-relevant properties. Aging experiments on diesel soot were carried out in a controlled laboratory chamber, and the effects of condensation and coagulation processes were systematically explored in separate sets of experiments. In addition to online measurement of aerosol properties, aerosol samples were collected for offline single particle analysis to investigate the evolution of the morphology, elemental composition and fine structure of sample particles from different experiments. Condensation experiments focused on the formation of α-pinene secondary organic aerosol on diesel soot aerosol seeds. Experiments were conducted to study the aging of soot under dry (RH < 2%) and humid conditions (RH ~ 80%). We present an analysis of the morphology of soot, its evolution, and its correlation with optical properties, as the condensation of α-pinene SOA is carried out for the two different RH conditions. The analysis was performed by using scanning electron microscopy, transmission electron microscopy, scanning transmission x-ray microscopy and atomic force microscopy for single particle characterization. In addition, particle size, mass, composition, shape, and density were characterized in-situ, as a function of organics condensed on soot seeds, using single particle mass spectrometer.

Investigation of Simultaneous Effects of Aerosol Properties and Aerosol Peak Height on the Air Mass Factors for Space-Borne NO2 Retrievals

Directory of Open Access Journals (Sweden)

Hyunkee Hong

2017-02-01

Full Text Available We investigate the simultaneous effects of aerosol peak height (APH, aerosol properties, measurement geometry, and other factors on the air mass factor for NO2 retrieval at sites with high NO2 concentration. A comparison of the effects of high and low surface reflectance reveals that NO2 air mass factor (AMF values over a snowy surface (surface reflectance 0.8 are generally higher than those over a deciduous forest surface (surface reflectance 0.05. Under high aerosol optical depth (AOD conditions, the aerosol shielding effect over a high-albedo surface is revealed to reduce the path-length of light at the surface, whereas high single scattering albedo (SSA conditions (e.g., SSA = 0.95 lead to an increase in the aerosol albedo effect, which results in an increased AMF over areas with low surface reflectance. We also conducted an in-depth study of the APH effect on AMF. For an AOD of 0.1 and half width (HW of 5 km, NO2 AMF decreases by 29% from 1.36 to 0.96 as APH changes from 0 to 2 km. In the case of high-AOD conditions (0.9 and HW of 5 km, the NO2 AMF decreases by 240% from 1.85 to 0.54 as APH changes from 0 to 2 km. The AMF variation due to error in the model input parameters (e.g., AOD, SSA, aerosol shape, and APH is also examined. When APH is 0 km with an AOD of 0.4, SSA of 0.88, and surface reflectance of 0.05, a 30% error in AOD induces an AMF error of between 4.85% and −3.67%, an SSA error of 0.04 leads to NO2 VCD errors of between 4.46% and −4.77%, and a 30% error in AOD induces an AMF error of between −9.53% and 8.35% with an APH of 3 km. In addition to AOD and SSA, APH is an important factor in calculating AMF, due to the 2 km error in APH under high-SZA conditions, which leads to an NO2 VCD error of over 60%. Aerosol shape is also found to have a measureable effect on AMF under high-AOD and small relative azimuth angle (RAA conditions. The diurnal effect of the NO2 profile is also examined and discussed.

Trace metal analysis in arctic aerosols by an inductively coupled plasma-time of flight-mass spectrometer combined with an inductively heated vaporizer

International Nuclear Information System (INIS)

Luedke, Christian; Skole, Jochen; Taubner, Kerstin; Kriews, Michael

2005-01-01

Two newly developed instruments were combined to analyze the trace metal content in size separated arctic aerosols during the measurement campaign ASTAR 2004 (Arctic Study of Tropospheric Aerosols, Clouds and Radiation 2004) at Spitsbergen in May-June 2004. The aim of this extensive aerosol measurement campaign was to obtain a database for model-calculations of arctic aerosol, which play an important role in the global climate change. The ASTAR project was centered on two aircraft measurement campaigns, scheduled from 2004 to 2005, addressing both aerosol and cloud measurements, combined with ground-based and satellite observations. In the present paper one example for the analysis of ground-based aerosol particles is described. The sampling of aerosol particles was performed in a well-known manner by impaction of the particles on cleaned graphite targets. By means of a cascade impactor eight size classes between 0.35 and 16.6 μm aerodynamic diameters were separated. To analyze the metal content in the aerosol particles the targets were rapidly heated up to 2700 deg. C in an inductively heated vaporizer system (IHVS). An argon flow transports the vaporized sample material into the inductively coupled plasma (ICP) used as ionization source for the time of flight-mass spectrometer (TOF-MS). The simultaneous extraction of the ions from the plasma, as realized in the TOF instrument, allows to obtain the full mass spectrum of the sample during the vaporization pulse without any limitation in the number of elements detected. With optimized experimental parameters the element content in arctic aerosol particles was determined in a mass range between 7 Li and 209 Bi. Comparing the size distribution of the elemental content of the aerosol particles, two different meteorological situations were verified. For calibration acidified reference solutions were placed on the cleaned target inside the IHVS. The limits of detection (LOD) for the element mass on the target range

Stratospheric aerosols

International Nuclear Information System (INIS)

Rosen, J.; Ivanov, V.A.

1993-01-01

Stratospheric aerosol measurements can provide both spatial and temporal data of sufficient resolution to be of use in climate models. Relatively recent results from a wide range of instrument techniques for measuring stratospheric aerosol parameters are described. Such techniques include impactor sampling, lidar system sensing, filter sampling, photoelectric particle counting, satellite extinction-sensing using the sun as a source, and optical depth probing, at sites mainly removed from tropospheric aerosol sources. Some of these techniques have also had correlative and intercomparison studies. The main methods for determining the vertical profiles of stratospheric aerosols are outlined: lidar extinction measurements from satellites; impactor measurements from balloons and aircraft; and photoelectric particle counter measurements from balloons, aircraft, and rockets. The conversion of the lidar backscatter to stratospheric aerosol mass loading is referred to. Absolute measurements of total solar extinction from satellite orbits can be used to extract the aerosol extinction, and several examples of vertical profiles of extinction obtained with the SAGE satellite are given. Stratospheric mass loading can be inferred from extinction using approximate linear relationships but under restrictive conditions. Impactor sampling is essentially the only method in which the physical nature of the stratospheric aerosol is observed visually. Vertical profiles of stratospheric aerosol number concentration using impactor data are presented. Typical profiles using a dual-size-range photoelectric dustsonde particle counter are given for volcanically disturbed and inactive periods. Some measurements of the global distribution of stratospheric aerosols are also presented. Volatility measurements are described, indicating that stratospheric aerosols are composed primarily of about 75% sulfuric acid and 25% water

Is there an aerosol signature of aqueous processing?

Science.gov (United States)

Ervens, B.; Sorooshian, A.

2017-12-01

The formation of aerosol mass in cloud water has been recognized as a substantial source of atmospheric aerosol mass. While sulfate formation can be relatively well constrained, the formation of secondary organic aerosol mass in the aqueous phase (aqSOA) is much more complex due to the multitude of precursors and variety in chemical processes. Aqueous phase processing adds aerosol mass to the droplet mode, which is formed due to mass addition to activated particles in clouds. In addition, it has been shown that aqSOA mass has specific characteristics in terms of oxidation state and hygroscopicity that might help to distinguish it from other SOA sources. Many models do not include detailed chemical mechanisms of sulfate and aqSOA formation and also lack details on the mass distribution of newly formed mass. Mass addition inside and outside clouds modifies different parts of an aerosol population and consequently affects predictions of properties and lifetime of particles. Using a combination of field data analysis and model studies for a variety of air masses, we will show which chemical and physical aerosol properties can be used, in order to identify an `aqueous phase signature' in processed aerosol populations. We will discuss differences in this signature in clean (e.g., background), moderately polluted (e.g., urban) and highly polluted (e.g., biomass burning) air masses and suggest air-mass-specific chemical and/or physical properties that will help to quantify the aqueous-phase derived aerosol mass.

Antarctic aerosols - A review

Science.gov (United States)

Shaw, Glenn E.

1988-02-01

Tropospheric aerosols with the diameter range of half a micron reside in the atmosphere for tens of days and teleconnect Antarctica with other regions by transport that reaches planetary scales of distances; thus, the aerosol on the Antarctic ice represents 'memory modules' of events that took place at regions separated from Antarctica by tens of thousands of kilometers. In terms of aerosol mass, the aerosol species include insoluble crustal products (less than 5 percent), transported sea-salt residues (highly variable but averaging about 10 percent), Ni-rich meteoric material, and anomalously enriched material with an unknown origin. Most (70-90 percent by mass) of the aerosol over the Antarctic ice shield, however, is the 'natural acid sulfate aerosol', apparently deriving from biological processes taking place in the surrounding oceans.

Variability of aerosol, gaseous pollutants and meteorological characteristics associated with continental, urban and marine air masses at the SW Atlantic coast of Iberia

Science.gov (United States)

Diesch, J.-M.; Drewnick, F.; Zorn, S. R.; von der Weiden-Reinmüller, S.-L.; Martinez, M.; Borrmann, S.

2011-12-01

Measurements of the ambient aerosol were performed at the Southern coast of Spain, within the framework of the DOMINO (Diel Oxidant Mechanisms In relation to Nitrogen Oxides) project. The field campaign took place from 20 November until 9 December 2008 at the atmospheric research station "El Arenosillo" (37°5'47.76" N, 6°44'6.94" W). As the monitoring station is located at the interface between a natural park, industrial cities (Huelva, Seville) and the Atlantic Ocean a variety of physical and chemical parameters of aerosols and gas phase could be characterized in dependency on the origin of air masses. Backwards trajectories were examined and compared with local meteorology to classify characteristic air mass types for several source regions. Aerosol number and mass as well as polycyclic aromatic hydrocarbons and black carbon concentrations were measured in PM1 and size distributions were registered covering a size range from 7 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol was measured by means of an Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS). Gas phase analyzers monitored various trace gases (O3, SO2, NO, NO2, CO2) and a weather station provided meteorological parameters. Lowest average submicron particle mass and number concentrations were found in air masses arriving from the Atlantic Ocean with values around 2 μg m-3 and 1000 cm-3. These mass concentrations were about two to four times lower than the values recorded in air masses of continental and urban origins. For some species PM1-fractions in marine air were significantly larger than in air masses originating from Huelva, a closely located city with extensive industrial activities. The largest fraction of sulfate (54%) was detected in marine air masses and was to a high degree not neutralized. In addition small concentrations of methanesulfonic acid (MSA), a product of biogenic dimethyl sulfate (DMS) emissions could be identified in the particle phase. In all

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

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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

Seasonal and spatial variability of the organic matter-to-organic carbon mass ratios in Chinese urban organic aerosols and a first report of high correlations between aerosol oxalic acid and zinc

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Xing, L.; Fu, T.-M.; Cao, J. J.; Lee, S. C.; Wang, G. H.; Ho, K. F.; Cheng, M.-C.; You, C.-F.; Wang, T. J.

2013-01-01

We calculated the organic matter to organic carbon mass ratios (OM/OC mass ratios) in PM2.5 collected from 14 Chinese cities during summer and winter of 2003 and analyzed the causes for their seasonal and spatial variability. The OM/OC mass ratios were calculated two ways. Using a mass balance method, the calculated OM/OC mass ratios averaged 1.92 ± 0.39 yr-round, with no significant seasonal or spatial variation. The second calculation was based on chemical species analyses of the organic compounds extracted from the PM2.5 samples using dichloromethane/methanol and water. The calculated OM/OC mass ratio in summer was relatively high (1.75 ± 0.13) and spatially-invariant, due to vigorous photochemistry and secondary OA production throughout the country. The calculated OM/OC mass ratio in winter (1.59 ± 0.18) was significantly lower than that in summer, with lower values in northern cities (1.51 ± 0.07) than in southern cities (1.65 ± 0.15). This likely reflects the wider usage of coal for heating purposes in northern China in winter, in contrast to the larger contributions from biofuel and biomass burning in southern China in winter. On average, organic matters constituted 36% and 34% of Chinese urban PM2.5 mass in summer and winter, respectively. We reported, for the first time, high correlations between Zn and oxalic acid in Chinese urban aerosols in summer. This is consistent with the formation of stable Zn oxalate complex in the aerosol phase previously proposed by Furukawa and Takahashi (2011). We found that many other dicarboxylic acids were also highly correlated with Zn in the summer Chinese urban aerosol samples, suggesting that they may also form stable organic complexes with Zn. Such formation may have profound implications for the atmospheric abundance and hygroscopic property of aerosol dicarboxylic acids.

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

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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

Radioactive aerosols

International Nuclear Information System (INIS)

Chamberlain, A.C.

1991-01-01

Radon. Fission product aerosols. Radioiodine. Tritium. Plutonium. Mass transfer of radioactive vapours and aerosols. Studies with radioactive particles and human subjects. Index. This paper explores the environmental and health aspects of radioactive aerosols. Covers radioactive nuclides of potential concern to public health and applications to the study of boundary layer transport. Contains bibliographic references. Suitable for environmental chemistry collections in academic and research libraries

Response of an aerosol mass spectrometer to organonitrates and organosulfates and implications for atmospheric chemistry.

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Farmer, D K; Matsunaga, A; Docherty, K S; Surratt, J D; Seinfeld, J H; Ziemann, P J; Jimenez, J L

2010-04-13

Organonitrates (ON) are important products of gas-phase oxidation of volatile organic compounds in the troposphere; some models predict, and laboratory studies show, the formation of large, multifunctional ON with vapor pressures low enough to partition to the particle phase. Organosulfates (OS) have also been recently detected in secondary organic aerosol. Despite their potential importance, ON and OS remain a nearly unexplored aspect of atmospheric chemistry because few studies have quantified particulate ON or OS in ambient air. We report the response of a high-resolution time-of-flight aerosol mass spectrometer (AMS) to aerosol ON and OS standards and mixtures. We quantify the potentially substantial underestimation of organic aerosol O/C, commonly used as a metric for aging, and N/C. Most of the ON-nitrogen appears as NO(x)+ ions in the AMS, which are typically dominated by inorganic nitrate. Minor organonitrogen ions are observed although their identity and intensity vary between standards. We evaluate the potential for using NO(x)+ fragment ratios, organonitrogen ions, HNO(3)+ ions, the ammonium balance of the nominally inorganic ions, and comparison to ion-chromatography instruments to constrain the concentrations of ON for ambient datasets, and apply these techniques to a field study in Riverside, CA. OS manifests as separate organic and sulfate components in the AMS with minimal organosulfur fragments and little difference in fragmentation from inorganic sulfate. The low thermal stability of ON and OS likely causes similar detection difficulties for other aerosol mass spectrometers using vaporization and/or ionization techniques with similar or larger energy, which has likely led to an underappreciation of these species.

Absorbing Aerosols: Field and Laboratory Studies of Black Carbon and Dust

Science.gov (United States)

Aiken, A. C.; Flowers, B. A.; Dubey, M. K.

2011-12-01

Currently, absorbing aerosols are thought to be the most uncertain factor in atmospheric climate models (~0.4-1.2 W/m2), and the 2nd most important factor after CO2 in global warming (1.6 W/m2; Ramanathan and Carmichael, Nature Geoscience, 2008; Myhre, Science, 2009). While most well-recognized atmospheric aerosols, e.g., sulfate from power-plants, have a cooling effect on the atmosphere by scattering solar radiation, black carbon (BC or soot) absorbs sunlight strongly which results in a warming of the atmosphere. Dust particles are also present globally and can absorb radiation, contributing to a warmer and drier atmosphere. Direct on-line measurements of BC and hematite, an absorbing dust aerosol, can be made with the Single Particle Soot Photometer (SP2), which measures the mass of the particles by incandescence on an individual particle basis. Measurements from the SP2 are combined with absorption measurements from the three-wavelength photoacoustic soot spectrometer (PASS-3) at 405, 532, and 781 nm and the ultraviolet photoacoustic soot spectrometer (PASS-UV) at 375 nm to determine wavelength-dependent mass absorption coefficients (MACs). Laboratory aerosol samples include flame-generated soot, fullerene soot, Aquadag, hematite, and hematite-containing dusts. Measured BC MAC's compare well with published values, and hematite MAC's are an order of magnitude less than BC. Absorbing aerosols measured in the laboratory are compared with those from ambient aerosols measured during the Las Conchas fire and BEACHON-RoMBAS. The Las Conchas fire was a wildfire in the Jemez Mountains of New Mexico that burned over 100,000 acres during the Summer of 2011, and BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen - Rocky Mountain Biogenic Aerosol Study) is a field campaign focusing on biogenic aerosols at the Manitou Forest Observatory near Colorado Springs, CO in Summer 2011. Optical properties and size

GEM-AQ/EC, an on-line global multi-scale chemical weather modelling system: model development and evaluation of global aerosol climatology

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S. L. Gong

2012-09-01

Full Text Available A global air quality modeling system GEM-AQ/EC was developed by implementing tropospheric chemistry and aerosol processes on-line into the Global Environmental Multiscale weather prediction model – GEM. Due to the multi-scale features of the GEM, the integrated model, GEM-AQ/EC, is able to investigate chemical weather at scales from global to urban domains. The current chemical mechanism is comprised of 50 gas-phase species, 116 chemical and 19 photolysis reactions, and is complemented by a sectional aerosol module CAM (The Canadian Aerosol Module with 5 aerosols types: sulphate, black carbon, organic carbon, sea-salt and soil dust. Monthly emission inventories of black carbon and organic carbon from boreal and temperate vegetation fires were assembled using the most reliable areas burned datasets by countries, from statistical databases and derived from remote sensing products of 1995–2004. The model was run for ten years from from 1995–2004 with re-analyzed meteorology on a global uniform 1° × 1° horizontal resolution domain and 28 hybrid levels extending up to 10 hPa. The simulating results were compared with various observations including surface network around the globe and satellite data. Regional features of global aerosols are reasonably captured including emission, surface concentrations and aerosol optical depth. For various types of aerosols, satisfactory correlations were achieved between modeled and observed with some degree of systematic bias possibly due to large uncertainties in the emissions used in this study. A global distribution of natural aerosol contributions to the total aerosols is obtained and compared with observations.

Development and characterization of a single particle laser ablation mass spectrometer (SPLAM for organic aerosol studies

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F. Gaie-Levrel

2012-01-01

Full Text Available A single particle instrument was developed for real-time analysis of organic aerosol. This instrument, named Single Particle Laser Ablation Mass Spectrometry (SPLAM, samples particles using an aerodynamic lens system for which the theoretical performances were calculated. At the outlet of this system, particle detection and sizing are realized by using two continuous diode lasers operating at λ = 403 nm. Polystyrene Latex (PSL, sodium chloride (NaCl and dioctylphtalate (DOP particles were used to characterize and calibrate optical detection of SPLAM. The optical detection limit (DL and detection efficiency (DE were determined using size-selected DOP particles. The DE ranges from 0.1 to 90% for 100 and 350 nm DOP particles respectively and the SPLAM instrument is able to detect and size-resolve particles as small as 110–120 nm. During optical detection, particle scattered light from the two diode lasers, is detected by two photomultipliers and the detected signals are used to trigger UV excimer laser (λ = 248 nm used for one-step laser desorption ionization (LDI of individual aerosol particles. The formed ions are analyzed by a 1 m linear time-of-flight mass spectrometer in order to access to the chemical composition of individual particles. The TOF-MS detection limit for gaseous aromatic compounds was determined to be 0.85 × 10⁻¹⁵ kg (∼4 × 10³ molecules. DOP particles were also used to test the overall operation of the instrument. The analysis of a secondary organic aerosol, formed in a smog chamber by the ozonolysis of indene, is presented as a first application of the instrument. Single particle mass spectra were obtained with an effective hit rate of 8%. Some of these mass spectra were found to be very different from one particle to another possibly reflecting chemical differences within the investigated indene SOA particles. Our study shows that an exhaustive statistical analysis, over hundreds of particles

Molecular Characterization of Organosulfates in Urban Aerosols during the Spring Festival by FT-ICR Mass Spectrometry

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Xie, Q.; Fu, P.

2017-12-01

Aerosol particles collected at daytime and nighttime in Beijing during the spring festival, including the episodes of various gradient level pollution and short-term pollution raised by fireworks, were analyzed using 15T Fourier transform ion cyclotron resonance mass spectrometry (FT-ICRMS). Organosulfates (OSs), tracers for secondary organic aerosol formation, were identified through accurate mass measurements. Both the total number and the arbitrary abundance of OSs were consistent with the total OC concentrations of the aerosol samples. Nitrooxy-organosulfates were more abundant in the nighttime than those in the daytime due to high NOX concentrations at night. Although all subgroups OSs increased with the deterioration of air quality, especially for the relative abundance of aromatic OSs with high double bond equivalents, the percentage contributions of aliphatic OSs with low degree of unsaturation decreased. It was worth to note that aliphatic OSs with a wide range in carbon-chain length of C6-40 were identified in this study. The candidates for their potential precursors were alkanes and fatty acids. Moreover, a large number of aromatic OSs, about two thirds of OSs, were detected. The rapid formation of these compounds in New Year's Eve with plentiful aromatics from firework burning suggests that they may be derived from PAHs. The high carbon and oxygen contents of OSs may indicate the presence of dimmers, even polymers. Our results support the important contribution of anthropogenic precursors to OSs in ambient aerosols on the basis of aromatic and aliphatic OSs, which may have a significant impact on the hygroscopic properties of ambient aerosol particles.

Aerosol volatility in a boreal forest environment

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Häkkinen, S. A. K.; ńijälä, M.; Lehtipalo, K.; Junninen, H.; Virkkula, A.; Worsnop, D. R.; Kulmala, M.; Petäjä, T.; Riipinen, I.

2012-04-01

Climate and health effects of atmospheric aerosols are determined by their properties such as their chemical composition. Aerosol chemical composition can be studied indirectly by measuring volatility of aerosol particles. The volatility of submicron aerosol particles (20-500 nm) was studied in a boreal forest site at SMEAR II (Station for Measuring Ecosystem-Atmosphere Relations II) station (Vesala et al., 1998) in Hyytiälä, Finland, during 01/2008-05/2010. The instrument used for the measurements was VDMPS (Volatility Differential Mobility Particle Sizer), which consists of two separate instruments: DMPS (Differential Mobility Particle Sizer, Aalto et al., 2001) and TD (Thermodenuder, Wehner et al., 2002). Aerosol evaporation was examined by heating the aerosol and comparing the total aerosol mass before and after heating. In the VDMPS system ambient aerosol sample was heated up to temperatures ranging from 80 °C to 280 °C. The higher the heating temperature was the more aerosol material was evaporated. There was a non-volatile residual present in aerosol particles when heated up to 280 °C. This residual explained (20±8)% of the total aerosol mass. Aerosol non-volatile mass fraction was highest during winter and smallest during summer months. The role of black carbon in the observed non-volatile residual was determined. Black carbon explained 40 to 90% of the non-volatile mass. Especially during colder seasons noticeable amount of non-volatile material, something else than black carbon, was observed. According to Kalberer et al. (2004) some atmospheric organic species can form polymers that have high evaporation temperatures. Also low-volatile organic salts may contribute to the non-volatile aerosol (Smith et al., 2010). Aerosol mass composition measured directly with AMS (Aerosol Mass Spectrometer, Jayne et al., 2000) was analyzed in order to examine the properties of the non-volatile material (other than black carbon). The AMS measurements were performed

Aerosol Optical Properties Measured Onboard the Ronald H. Brown During ACE Asia as a Function of Aerosol Chemical Composition and Source Region

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Quinn, P. K.; Coffman, D. J.; Bates, T. S.; Welton, E. J.; Covert, D. S.; Miller, T. L.; Johnson, J. E.; Maria, S.; Russell, L.; Arimoto, R.

2004-01-01

During the ACE Asia intensive field campaign conducted in the spring of 2001 aerosol properties were measured onboard the R/V Ronald H. Brown to study the effects of the Asian aerosol on atmospheric chemistry and climate in downwind regions. Aerosol properties measured in the marine boundary layer included chemical composition; number size distribution; and light scattering, hemispheric backscattering, and absorption coefficients. In addition, optical depth and vertical profiles of aerosol 180 deg backscatter were measured. Aerosol within the ACE Asia study region was found to be a complex mixture resulting from marine, pollution, volcanic, and dust sources. Presented here as a function of air mass source region are the mass fractions of the dominant aerosol chemical components, the fraction of the scattering measured at the surface due to each component, mass scattering efficiencies of the individual components, aerosol scattering and absorption coefficients, single scattering albedo, Angstrom exponents, optical depth, and vertical profiles of aerosol extinction. All results except aerosol optical depth and the vertical profiles of aerosol extinction are reported at a relative humidity of 55 +/- 5%. An over-determined data set was collected so that measured and calculated aerosol properties could be compared, internal consistency in the data set could be assessed, and sources of uncertainty could be identified. By taking into account non-sphericity of the dust aerosol, calculated and measured aerosol mass and scattering coefficients agreed within overall experimental uncertainties. Differences between measured and calculated aerosol absorption coefficients were not within reasonable uncertainty limits, however, and may indicate the inability of Mie theory and the assumption of internally mixed homogeneous spheres to predict absorption by the ACE Asia aerosol. Mass scattering efficiencies of non-sea salt sulfate aerosol, sea salt, submicron particulate organic

Contributions of Organic Sources to Atmospheric Aerosol Particle Concentrations and Growth

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Russell, L. M.

2017-12-01

Organic molecules are important contributors to aerosol particle mass and number concentrations through primary emissions as well as secondary growth in the atmosphere. New techniques for measuring organic aerosol components in atmospheric particles have improved measurements of this contribution in the last 20 years, including Scanning Transmission X-ray Microscopy Near Edge X-ray Absorption Fine Structure (STXM-NEXAFS), Fourier Transform Infrared spectroscopy (FTIR), and High-Resolution Aerosol Mass Spectrometry (AMS). STXM-NEXAFS individual aerosol particle composition illustrated the variety of morphology of organic components in marine aerosols, the inherent relationships between organic composition and shape, and the links between atmospheric aerosol composition and particles produced in smog chambers. This type of single particle microscopy has also added to size distribution measurements by providing evidence of how surface-controlled and bulk-controlled processes contribute to the growth of particles in the atmosphere. FTIR analysis of organic functional groups are sufficient to distinguish combustion, marine, and terrestrial organic particle sources and to show that each of those types of sources has a surprisingly similar organic functional group composition over four different oceans and four different continents. Augmenting the limited sampling of these off-line techniques with side-by-side inter-comparisons to online AMS provides complementary composition information and consistent quantitative attribution to sources (despite some clear method differences). Single-particle AMS techniques using light scattering and event trigger modes have now also characterized the types of particles found in urban, marine, and ship emission aerosols. Most recently, by combining with off-line techniques, single particle composition measurements have separated and quantified the contributions of organic, sulfate and salt components from ocean biogenic and sea spray

Evaluating the Sensitivity of the Mass-Based Particle Removal Calculations for HVAC Filters in ISO 16890 to Assumptions for Aerosol Distributions

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Brent Stephens

2018-02-01

Full Text Available High efficiency particle air filters are increasingly being recommended for use in heating, ventilating, and air-conditioning (HVAC systems to improve indoor air quality (IAQ. ISO Standard 16890-2016 provides a methodology for approximating mass-based particle removal efficiencies for PM1, PM2.5, and PM10 using size-resolved removal efficiency measurements for 0.3 µm to 10 µm particles. Two historical volume distribution functions for ambient aerosol distributions are assumed to represent ambient air in urban and rural areas globally. The goals of this work are to: (i review the ambient aerosol distributions used in ISO 16890, (ii evaluate the sensitivity of the mass-based removal efficiency calculation procedures described in ISO 16890 to various assumptions that are related to indoor and outdoor aerosol distributions, and (iii recommend several modifications to the standard that can yield more realistic estimates of mass-based removal efficiencies for HVAC filters, and thus provide a more realistic representation of a greater number of building scenarios. The results demonstrate that knowing the PM mass removal efficiency estimated using ISO 16890 is not sufficient to predict the PM mass removal efficiency in all of the environments in which the filter might be used. The main reason for this insufficiency is that the assumptions for aerosol number and volume distributions can substantially impact the results, albeit with some exceptions.

Fullerene Soot in Eastern China Air: Results from Soot Particle-Aerosol Mass Spectrometer

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Wang, J.; Ge, X.; Chen, M.; Zhang, Q.; Yu, H.; Sun, Y.; Worsnop, D. R.; Collier, S.

2015-12-01

In this work, we present for the first time, the observation and quantification of fullerenes in ambient airborne particulate using an Aerodyne Soot Particle - Aerosol Mass Spectrometer (SP-AMS) deployed during 2015 winter in suburban Nanjing, a megacity in eastern China. The laser desorption and electron impact ionization techniques employed by the SP-AMS allow us to differentiate various fullerenes from other aerosol components. Mass spectrum of the identified fullerene soot is consisted by a series of high molecular weight carbon clusters (up to m/z of 2000 in this study), almost identical to the spectral features of commercially available fullerene soot, both with C70 and C60 clusters as the first and second most abundant species. This type of soot was observed throughout the entire study period, with an average mass loading of 0.18 μg/m3, accounting for 6.4% of the black carbon mass, 1.2% of the total organic mass. Temporal variation and diurnal pattern of fullerene soot are overall similar to those of black carbon, but are clearly different in some periods. Combining the positive matrix factorization, back-trajectory and analyses of the meteorological parameters, we identified the petrochemical industrial plants situating upwind from the sampling site, as the major source of fullerene soot. In this regard, our findings imply the ubiquitous presence of fullerene soot in ambient air of industry-influenced area, especially the oil and gas production regions. This study also offers new insights into the characterization of fullerenes from other environmental samples via the advanced SP-AMS technique.

Mass yields of secondary organic aerosols from the oxidation of α-pinene and real plant emissions

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J. N. Smith

2011-02-01

Full Text Available Biogenic volatile organic compounds (VOCs are a significant source of global secondary organic aerosol (SOA; however, quantifying their aerosol forming potential remains a challenge. This study presents smog chamber laboratory work, focusing on SOA formation via oxidation of the emissions of two dominant tree species from boreal forest area, Scots pine (Pinus sylvestris L. and Norway spruce (Picea abies, by hydroxyl radical (OH and ozone (O3. Oxidation of α-pinene was also studied as a reference system. Tetramethylethylene (TME and 2-butanol were added to control OH and O3 levels, thereby allowing SOA formation events to be categorized as resulting from either OH-dominated or O3-initiated chemistry. SOA mass yields from α-pinene are consistent with previous studies while the yields from the real plant emissions are generally lower than that from α-pinene, varying from 1.9% at an aerosol mass loading of 0.69 μg m−3 to 17.7% at 26.0 μg m−3. Mass yields from oxidation of real plant emissions are subject to the interactive effects of the molecular structures of plant emissions and their reaction chemistry with OH and O3, which lead to variations in condensable product volatility. SOA formation can be reproduced with a two-product gas-phase partitioning absorption model in spite of differences in the source of oxidant species and product volatility in the real plant emission experiments. Condensable products from OH-dominated chemistry showed a higher volatility than those from O3-initiated systems during aerosol growth stage. Particulate phase products became less volatile via aging process which continued after input gas-phase oxidants had been completely consumed.

Microphysical processing of aerosol particles in orographic clouds

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Pousse-Nottelmann, S.; Zubler, E. M.; Lohmann, U.

2015-08-01

An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO). The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen (WBF) process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases

Microphysical processing of aerosol particles in orographic clouds

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S. Pousse-Nottelmann

2015-08-01

aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener–Bergeron–Findeisen (WBF process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice crystal number

Characterization of the sources and processes of organic and inorganic aerosols in New York city with a high-resolution time-of-flight aerosol mass apectrometer

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Y.-L. Sun

2011-02-01

Full Text Available Submicron aerosol particles (PM₁ were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer during the summer 2009 Field Intensive Study at Queens College in New York, NY. Organic aerosol (OA and sulfate are the two dominant species, accounting for 54% and 24%, respectively, of the total PM₁ mass. The average mass-based size distribution of OA presents a small mode peaking at ~150 nm (D_va and an accumulation mode (~550 nm that is internally mixed with sulfate, nitrate, and ammonium. The diurnal cycles of both sulfate and OA peak between 01:00–02:00 p.m. EST due to photochemical production. The average (±σ oxygen-to-carbon (O/C, hydrogen-to-carbon (H/C, and nitrogen-to-carbon (N/C ratios of OA in NYC are 0.36 (±0.09, 1.49 (±0.08, and 0.012 (±0.005, respectively, corresponding to an average organic mass-to-carbon (OM/OC ratio of 1.62 (±0.11. Positive matrix factorization (PMF of the high resolution mass spectra identified two primary OA (POA sources, traffic and cooking, and three secondary OA (SOA components including a highly oxidized, regional low-volatility oxygenated OA (LV-OOA; O/C = 0.63, a less oxidized, semi-volatile SV-OOA (O/C = 0.38 and a unique nitrogen-enriched OA (NOA; N/C = 0.053 characterized with prominent C_xH_{2x + 2}N⁺ peaks likely from amino compounds. Our results indicate that cooking and traffic are two distinct and mass-equivalent POA sources in NYC, together contributing ~30% of the total OA mass during this study. The OA composition is dominated by secondary species, especially during high PM events. SV-OOA and LV-OOA on average account for 34% and 30%, respectively, of the total OA mass. The chemical evolution of SOA in NYC appears to progress with a continuous oxidation from SV-OOA to LV-OOA, which is further supported by a gradual increase of O/C ratio and a simultaneous decrease of H/C ratio in total OOA. Detailed

Interpretation of organic components from Positive Matrix Factorization of aerosol mass spectrometric data

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I. M. Ulbrich

2009-05-01

Full Text Available The organic aerosol (OA dataset from an Aerodyne Aerosol Mass Spectrometer (Q-AMS collected at the Pittsburgh Air Quality Study (PAQS in September 2002 was analyzed with Positive Matrix Factorization (PMF. Three components – hydrocarbon-like organic aerosol OA (HOA, a highly-oxygenated OA (OOA-1 that correlates well with sulfate, and a less-oxygenated, semi-volatile OA (OOA-2 that correlates well with nitrate and chloride – are identified and interpreted as primary combustion emissions, aged SOA, and semivolatile, less aged SOA, respectively. The complexity of interpreting the PMF solutions of unit mass resolution (UMR AMS data is illustrated by a detailed analysis of the solutions as a function of number of components and rotational forcing. A public web-based database of AMS spectra has been created to aid this type of analysis. Realistic synthetic data is also used to characterize the behavior of PMF for choosing the best number of factors, and evaluating the rotations of non-unique solutions. The ambient and synthetic data indicate that the variation of the PMF quality of fit parameter (Q, a normalized chi-squared metric vs. number of factors in the solution is useful to identify the minimum number of factors, but more detailed analysis and interpretation are needed to choose the best number of factors. The maximum value of the rotational matrix is not useful for determining the best number of factors. In synthetic datasets, factors are "split" into two or more components when solving for more factors than were used in the input. Elements of the "splitting" behavior are observed in solutions of real datasets with several factors. Significant structure remains in the residual of the real dataset after physically-meaningful factors have been assigned and an unrealistic number of factors would be required to explain the remaining variance. This residual structure appears to be due to variability in the spectra of the components

Highly time-resolved chemical characterization of atmospheric submicron particles during 2008 Beijing Olympic Games using an Aerodyne High-Resolution Aerosol Mass Spectrometer

Directory of Open Access Journals (Sweden)

X.-F. Huang

2010-09-01

Full Text Available As part of Campaigns of Air Quality Research in Beijing and Surrounding Region-2008 (CAREBeijing-2008, an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS was deployed in urban Beijing to characterize submicron aerosol particles during the time of 2008 Beijing Olympic Games and Paralympic Games (24 July to 20 September 2008. The campaign mean PM₁ mass concentration was 63.1 ± 39.8 μg m⁻³; the mean composition consisted of organics (37.9%, sulfate (26.7%, ammonium (15.9%, nitrate (15.8%, black carbon (3.1%, and chloride (0.87%. The average size distributions of the species (except BC were all dominated by an accumulation mode peaking at about 600 nm in vacuum aerodynamic diameter, and organics was characterized by an additional smaller mode extending below 100 nm. Positive Matrix Factorization (PMF analysis of the high resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., hydrocarbon-like (HOA, cooking-related (COA, and two oxygenated organic aerosols (OOA-1 and OOA-2, which on average accounted for 18.1, 24.4, 33.7 and 23.7% of the total organic mass, respectively. The HOA was identified to be closely associated with primary combustion sources, while the COA mass spectrum and diurnal pattern showed similar characteristics to that measured for cooking emissions. The OOA components correspond to aged secondary organic aerosol. Although the two OOA components have similar elemental (O/C, H/C compositions, they display differences in mass spectra and time series which appear to correlate with the different source regions sampled during the campaign. Back trajectory clustering analysis indicated that the southerly air flows were associated with the highest PM₁ pollution during the campaign. Aerosol particles in southern airmasses were especially rich in inorganic and oxidized organic species. Aerosol particles in northern airmasses

Highly time-resolved chemical characterization of atmospheric submicron particles during 2008 Beijing Olympic Games using an Aerodyne High-Resolution Aerosol Mass Spectrometer

Science.gov (United States)

Huang, X.-F.; He, L.-Y.; Hu, M.; Canagaratna, M. R.; Sun, Y.; Zhang, Q.; Zhu, T.; Xue, L.; Zeng, L.-W.; Liu, X.-G.; Zhang, Y.-H.; Jayne, J. T.; Ng, N. L.; Worsnop, D. R.

2010-09-01

As part of Campaigns of Air Quality Research in Beijing and Surrounding Region-2008 (CAREBeijing-2008), an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed in urban Beijing to characterize submicron aerosol particles during the time of 2008 Beijing Olympic Games and Paralympic Games (24 July to 20 September 2008). The campaign mean PM1 mass concentration was 63.1 ± 39.8 μg m-3; the mean composition consisted of organics (37.9%), sulfate (26.7%), ammonium (15.9%), nitrate (15.8%), black carbon (3.1%), and chloride (0.87%). The average size distributions of the species (except BC) were all dominated by an accumulation mode peaking at about 600 nm in vacuum aerodynamic diameter, and organics was characterized by an additional smaller mode extending below 100 nm. Positive Matrix Factorization (PMF) analysis of the high resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., hydrocarbon-like (HOA), cooking-related (COA), and two oxygenated organic aerosols (OOA-1 and OOA-2), which on average accounted for 18.1, 24.4, 33.7 and 23.7% of the total organic mass, respectively. The HOA was identified to be closely associated with primary combustion sources, while the COA mass spectrum and diurnal pattern showed similar characteristics to that measured for cooking emissions. The OOA components correspond to aged secondary organic aerosol. Although the two OOA components have similar elemental (O/C, H/C) compositions, they display differences in mass spectra and time series which appear to correlate with the different source regions sampled during the campaign. Back trajectory clustering analysis indicated that the southerly air flows were associated with the highest PM1 pollution during the campaign. Aerosol particles in southern airmasses were especially rich in inorganic and oxidized organic species. Aerosol particles in northern airmasses contained a large fraction of primary HOA

FROM TRADITIONAL DISTANCE LEARNING TO MASS ONLINE OPEN COURSES

Directory of Open Access Journals (Sweden)

V. N. Vasilev

2014-01-01

Full Text Available The issue of transition for higher education institutions of Russia from traditional distance learning to mass electronic education on the basis of the online open courses is considered, its relevance is proved. Analysis of the major prerequisites for transition success is carried out (a demand for the educational Internet resources from mobile devices; existence of a large number of various electronic resources which are successfully used in practice by higher education institutions in remote educational technologies; maintaining experience for electronic magazines of students’ progress for planning and estimation of training results; essential growth of material costs in the world online training market. Key issues of transition are defined and the basic principles of electronic online courses development are formulated. A technique for electronic online course development aimed at the result is given. The technique contains the following four stages: planning of expected training results, course electronic content structuring and training scenarios creation, development of the tests plan and electronic estimated means for automatic control of the planned training results; course realization by means of game mechanics and technologies of network communication between students. Requirements to various forms of control planned in the course of learning results are defined. Two kinds of electronic online courses are assigned (knowledge-intensive and technological courses. Examples of their realization in the authors’ online courses "Wave Optics", "Theory of Graphs ", "Development of Web Interfaces on the Basis of HTML and CSS" created and practically used in NRU ITMO in 2013 are given. Finally, the actual tasks of mass open education development in the leading higher education institutions of Russia are set forth.

Determination of gaseous compounds using online mass spectrometry

International Nuclear Information System (INIS)

Praun, S.

1999-08-01

The work is divided in three major parts and describes various measurements of gaseous compounds. The first part tasks the problem of transit traffic along the motorway from Kufstein, Northern Tyrol/Austria until Ala, Trentino/Italy. During three periods measurements of the immissions of many compounds were carried out simultaneously in Northern Tyrol, Southern Tyrol and Trentino. The influence of the ban of heavy lorry traffic during the weekend and during the night on the reduction of NO 2 could be demonstrated. Furthermore certain compounds (e.g. Benzene) were monitored online for the first time along the motorway at lowest concentrations using the mass spectrometer 'Airsense 500'. In the second part online measurements of exhaled human breath after the oral application of a medicine against bronchitis was performed. In that way beside clinical and pharmacological studies the effectiveness of this pharmacon could be proved. The last part of the present work shows adsorption- and desorption measurements on four different adsorbents. During this procedure seven different gases with an increasing number of carbon atoms were monitored online by the hyphenation of these adsorbents with the mass spectrometer 'Airsense 500'. Thereby, the various properties of the adsorbents in the interaction with the gases could be demonstrated. (author)

On-line mass separator of superheavy atoms

International Nuclear Information System (INIS)

Oganesyan, Yu.Ts.

2002-01-01

The concept is presented of an on-line Mass Analyzer of SuperHeavy Atoms (MASHA) dedicated to the separation and determination of the mass and decay properties of new elements and isotopes produced in heavy-ion induced reactions. The new nuclides with half-lives T 1/2 ≥ 1 s are transported to an ECR-source working at a frequency of 2.45 GHz and are separated by mass with a mass resolution of M/ΔM ∼ 1500. In the focal plane of the magnetic analyzer a front strip detector surrounded by side detectors will be placed to determine the mass according to the signals from the detected α-particles or fission fragments with efficiency of about 90 %. In comparison to other existing in-flight recoil separators, the present setup will be characterized by higher efficiency and high selectivity relative to background reaction products. The setup MASHA may be used also in the investigation of nuclear reactions of different type induced by stable and radioactive beams

On-Line Mass Separator of Superheavy Atoms

CERN Document Server

Oganessian, Yu T

2002-01-01

The concept is presented of an on-line Mass Analyzer of SuperHeavy Atoms (MASHA) dedicated to the separation and determination of the mass and decay properties of new elements and isotopes produced in heavy-ion induced reactions. The new nuclides with half-lives T_{1/2}\\ge 1 s are transported to an ECR-source working at a frequency of 2.45 GHz and are separated by mass with a mass resolution of M/\\Delta M\\sim 1500. In the focal plane of the magnetic analyzer a front strip detector surrounded by side detectors will be placed to determine the mass according to the signals from the detected alpha-particles or fission fragments with efficiency of about 90 %. In comparison to other existing in-flight recoil separators, the present setup will be characterized by higher efficiency and high selectivity relative to background reaction products. The setup MASHA may be used also in the investigation of nuclear reactions of different type induced by stable and radioactive beams.

Characterizing Organic Aerosol Processes and Climatically Relevant Properties via Advanced and Integrated Analyses of Aerosol Mass Spectrometry Datasets from DOE Campaigns and ACRF Measurements. Final report for DE-SC0007178

Energy Technology Data Exchange (ETDEWEB)

Zhang, Qi [Univ. of California, Davis, CA (United States)

2017-05-21

Organic aerosols (OA) are an important but poorly characterized component of the earth’s climate system. Enormous complexities commonly associated with OA composition and life cycle processes have significantly complicated the simulation and quantification of aerosol effects. To unravel these complexities and improve understanding of the properties, sources, formation, evolution processes, and radiative properties of atmospheric OA, we propose to perform advanced and integrated analyses of multiple DOE aerosol mass spectrometry datasets, including two high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) datasets from intensive field campaigns on the aerosol life cycle and the Aerosol Chemical Speciation Monitor (ACSM) datasets from long-term routine measurement programs at ACRF sites. In this project, we will focus on 1) characterizing the chemical (i.e., composition, organic elemental ratios), physical (i.e., size distribution and volatility), and radiative (i.e., sub- and super-saturated growth) properties of organic aerosols, 2) examining the correlations of these properties with different source and process regimes (e.g., primary, secondary, urban, biogenic, biomass burning, marine, or mixtures), 3) quantifying the evolutions of these properties as a function of photochemical processing, 4) identifying and characterizing special cases for important processes such as SOA formation and new particle formation and growth, and 5) correlating size-resolved aerosol chemistry with measurements of radiative properties of aerosols to determine the climatically relevant properties of OA and characterize the relationship between these properties and processes of atmospheric aerosol organics. Our primary goal is to improve a process-level understanding of the life cycle of organic aerosols in the Earth’s atmosphere. We will also aim at bridging between observations and models via synthesizing and translating the results and insights generated from this

Measurement of the ambient organic aerosol volatility distribution: application during the Finokalia Aerosol Measurement Experiment (FAME-2008

Directory of Open Access Journals (Sweden)

B. H. Lee

2010-12-01

Full Text Available A variable residence time thermodenuder (TD was combined with an Aerodyne Aerosol Mass Spectrometer (AMS and a Scanning Mobility Particle Sizer (SMPS to measure the volatility distribution of aged organic aerosol in the Eastern Mediterranean during the Finokalia Aerosol Measurement Experiment in May of 2008 (FAME-2008. A new method for the quantification of the organic aerosol volatility distribution was developed combining measurements of all three instruments together with an aerosol dynamics model.

Challenges in the interpretation of ambient thermodenuder-AMS measurements include the potential resistances to mass transfer during particle evaporation, the effects of particle size on the evaporated mass fraction, the changes in the AMS collection efficiency and particle density as the particles evaporate partially in the TD, and finally potential losses inside the TD. Our proposed measurement and data analysis method accounts for all of these problems combining the AMS and SMPS measurements.

The AMS collection efficiency of the aerosol that passed through the TD was found to be approximately 10% lower than the collection efficiency of the aerosol that passed through the bypass. The organic aerosol measured at Finokalia is approximately 2 or more orders of magnitude less volatile than fresh laboratory-generated monoterpene (α-pinene, β-pinene and limonene under low NO_x conditions secondary organic aerosol. This low volatility is consistent with its highly oxygenated AMS mass spectrum. The results are found to be highly sensitive to the mass accommodation coefficient of the evaporating species. This analysis is based on the assumption that there were no significant reactions taking place inside the thermodenuder.

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

Aerosol Chemical Composition and its Effects on Cloud-Aerosol Interactions during the 2007 CHAPS Experiment

Science.gov (United States)

Lee, Y.; Alexander, L.; Newburn, M.; Jayne, J.; Hubbe, J.; Springston, S.; Senum, G.; Andrews, B.; Ogren, J.; Kleinman, L.; Daum, P.; Berg, L.; Berkowitz, C.

2007-12-01

Chemical composition of submicron aerosol particles was determined using an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (AMS) outfitted on the DOE G-1 aircraft during the Cumulus Humilis Aerosol Processing Study (CHAPS) conducted in Oklahoma City area in June 2007. The primary objective of CHAPS was to investigate the effects of urban emissions on cloud aerosol interactions as a function of processing of the emissions. Aerosol composition was typically determined at three different altitudes: below, in, and above cloud, in both upwind and downwind regions of the urban area. Aerosols were sampled from an isokinetic inlet with an upper size cut-off of ~1.5 micrometer. During cloud passages, the AMS also sampled particles that were dried from cloud droplets collected using a counter-flow virtual impactor (CVI) sampler. The aerosol mass concentrations were typically below 10 microgram per cubic meter, and were dominated by organics and sulfate. Ammonium was often less than required for complete neutralization of sulfate. Aerosol nitrate levels were very low. We noted that nitrate levels were significantly enhanced in cloud droplets compared to aerosols, most likely resulting from dissolution of gaseous nitric acid. Organic to sulfate ratios appeared to be lower in cloud droplets than in aerosols, suggesting cloud condensation nuclei properties of aerosol particles might be affected by loading and nature of the organic components in aerosols. In-cloud formation of sulfate was considered unimportant because of the very low SO2 concentration in the region. A detailed examination of the sources of the aerosol organic components (based on hydrocarbons determined using a proton transfer reaction mass spectrometer) and their effects on cloud formation as a function of atmospheric processing (based on the degree of oxidation of the organic components) will be presented.

Estimation of atmospheric columnar organic matter (OM) mass concentration from remote sensing measurements of aerosol spectral refractive indices

Science.gov (United States)

Zhang, Ying; Li, Zhengqiang; Sun, Yele; Lv, Yang; Xie, Yisong

2018-04-01

Aerosols have adverse effects on human health and air quality, changing Earth's energy balance and lead to climate change. The components of aerosol are important because of the different spectral characteristics. Based on the low hygroscopic and high scattering properties of organic matter (OM) in fine modal atmospheric aerosols, we develop an inversion algorithm using remote sensing to obtain aerosol components including black carbon (BC), organic matter (OM), ammonium nitrate-like (AN), dust-like (DU) components and aerosol water content (AW). In the algorithm, the microphysical characteristics (i.e. volume distribution and complex refractive index) of particulates are preliminarily separated to fine and coarse modes, and then aerosol components are retrieved using bimodal parameters. We execute the algorithm using remote sensing measurements of sun-sky radiometer at AERONET site (Beijing RADI) in a period from October of 2014 to January of 2015. The results show a reasonable distribution of aerosol components and a good fit for spectral feature calculations. The mean OM mass concentration in atmospheric column is account for 14.93% of the total and 56.34% of dry and fine-mode aerosol, being a fairly good correlation (R = 0.56) with the in situ observations near the surface layer.

Determination of particulate lead during MILAGRO / MCMA-2006 using Aerosol Mass Spectrometry

Science.gov (United States)

Salcedo, Dara; Onasch, T. B.; Aiken, A. C.; Williams, L. R.; de Foy, B.; Cubison, M. J.; Worsnop, D. R.; Molina, L. T.; Jimenez, J. L.

2010-05-01

We report the first measurements of particulate lead (Pb) from Aerodyne Aerosol Mass Spectrometers, which were deployed in and around Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO) / Mexico City Metropolitan Area 2006 (MCMA-2006) field campaigns. The high resolution mass spectrometer of one of the AMS instruments (HR-AMS) and the measured isotopic ratios unequivocally prove the detection of Pb in ambient particles. A substantial fraction of the lead evaporated slowly from the vaporizer of the instruments, which is indicative of species with low volatility at 600oC. A model was developed in order to estimate the ambient particulate Pb entering the AMS from the signals in the "open" and the "closed" (or "background") mass spectrum modes of the AMS. The model suggests the presence of at least two lead fractions with ~25% of the Pb signal exhibiting rapid evaporation (1/e decay constant, τ PEMEX32 site). From laboratory experiments with pure Pb(NO3)2 particles, we estimated that the Pb ionization efficiency relative to nitrate (RIEPb) is 0.5. Comparison of time series of AMS Pb with other measurements carried out at the T0 urban supersite during MILAGRO (using Proton Induced X-ray Emission (PIXE), Inductively-Coupled Plasma Mass Spectrometry (ICP-MS) and single-particle counts from an Aerosol Time-of-Fight Mass Spectrometer (ATOFMS)) shows similar levels (for PIXE and ICP-MS) and substantial correlation. During part of the campaign, sampling at T0 was alternated every 10 minutes with an Aerosol Concentrator, which enabled the detection of signals for PbCl+ and PbS+ ions. PbS+ displays the signature of a slowly evaporating species, while PbCl+ appears to arise only from fast evaporation, which is likely due to the higher vapor pressure of the compounds generating PbCl+. This is consistent with the evaporation model results. Levels of particulate Pb measured during MILAGRO at T0 were similar to previous studies in Mexico

Determination of particulate lead using aerosol mass spectrometry: MILAGRO/MCMA-2006 observations

Science.gov (United States)

Salcedo, D.; Onasch, T. B.; Aiken, A. C.; Williams, L. R.; de Foy, B.; Cubison, M. J.; Worsnop, D. R.; Molina, L. T.; Jimenez, J. L.

2010-06-01

We report the first measurements of particulate lead (Pb) from Aerodyne Aerosol Mass Spectrometers, which were deployed in and around Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO)/Mexico City Metropolitan Area 2006 (MCMA-2006) field campaigns. The high resolution mass spectrometer of one of the AMS instruments (HR-AMS) and the measured isotopic ratios unequivocally prove the detection of Pb in ambient particles. A substantial fraction of the lead evaporated slowly from the vaporizer of the instruments, which is indicative of species with low volatility at 600 °C. A model was developed in order to estimate the ambient particulate Pb entering the AMS from the signals in the "open" and the "closed" (or "background") mass spectrum modes of the AMS. The model suggests the presence of at least two lead fractions with ~25% of the Pb signal exhibiting rapid evaporation (1/e decay constant, τPEMEX site). From laboratory experiments with pure Pb(NO3)2 particles, we estimated that the Pb ionization efficiency relative to nitrate (RIEPb) is 0.5. Comparison of time series of AMS Pb with other measurements carried out at the T0 supersite during MILAGRO (using Proton Induced X-ray Emission (PIXE), Inductively-Coupled Plasma Mass Spectrometry (ICP-MS) and single-particle counts from an Aerosol Time-of-Fight Mass Spectrometer (ATOFMS)) shows similar levels (for PIXE and ICP-MS) and substantial correlation. During part of the campaign, sampling at T0 was alternated every 10 min with an Aerosol Concentrator, which enabled the detection of signals for PbCl+ and PbS+ ions. PbS+ displays the signature of a slowly evaporating species, while PbCl+ appears to arise only from fast evaporation, which is likely due to the higher vapor pressure of the compounds generating PbCl+. This is consistent with the evaporation model results. Levels of particulate Pb measured at T0 were similar to previous studies in Mexico City. Pb shows a diurnal cycle

Influences of in-cloud aerosol scavenging parameterizations on aerosol concentrations and wet deposition in ECHAM5-HAM

Directory of Open Access Journals (Sweden)

B. Croft

2010-02-01

Full Text Available A diagnostic cloud nucleation scavenging scheme, which determines stratiform cloud scavenging ratios for both aerosol mass and number distributions, based on cloud droplet, and ice crystal number concentrations, is introduced into the ECHAM5-HAM global climate model. This scheme is coupled with a size-dependent in-cloud impaction scavenging parameterization for both cloud droplet-aerosol, and ice crystal-aerosol collisions. The aerosol mass scavenged in stratiform clouds is found to be primarily (>90% scavenged by cloud nucleation processes for all aerosol species, except for dust (50%. The aerosol number scavenged is primarily (>90% attributed to impaction. 99% of this impaction scavenging occurs in clouds with temperatures less than 273 K. Sensitivity studies are presented, which compare aerosol concentrations, burdens, and deposition for a variety of in-cloud scavenging approaches: prescribed fractions, a more computationally expensive prognostic aerosol cloud processing treatment, and the new diagnostic scheme, also with modified assumptions about in-cloud impaction and nucleation scavenging. Our results show that while uncertainties in the representation of in-cloud scavenging processes can lead to differences in the range of 20–30% for the predicted annual, global mean aerosol mass burdens, and near to 50% for accumulation mode aerosol number burden, the differences in predicted aerosol mass concentrations can be up to one order of magnitude, particularly for regions of the middle troposphere with temperatures below 273 K where mixed and ice phase clouds exist. Different parameterizations for impaction scavenging changed the predicted global, annual mean number removal attributed to ice clouds by seven-fold, and the global, annual dust mass removal attributed to impaction by two orders of magnitude. Closer agreement with observations of black carbon profiles from aircraft (increases near to one order of magnitude for mixed phase clouds

Clouds and aerosols in Puerto Rico - a new evaluation

Science.gov (United States)

Allan, J. D.; Baumgardner, D.; Raga, G. B.; Mayol-Bracero, O. L.; Morales-García, F.; García-García, F.; Montero-Martínez, G.; Borrmann, S.; Schneider, J.; Mertes, S.; Walter, S.; Gysel, M.; Dusek, U.; Frank, G. P.; Krämer, M.

2008-03-01

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 (residual particles and concentrations of cloudwater nitrate, sulphate and insoluble material increased during polluted conditions. Previous studies in Puerto Rico had reported the presence of a significant non-anthropogenic organic fraction in the aerosols measured and concluded that this was a factor controlling the in situ cloud properties. However, this was not observed in our case. In contrast to the 1.00±0.14 μg m-3 of organic carbon measured in 1992 and 1995, the organic matter measured in the current study of 0

Chemical characterization of long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometry

Science.gov (United States)

Zhang, Xinghua; Xu, Jianzhong; Kang, Shichang; Liu, Yanmei; Zhang, Qi

2018-04-01

An intensive field measurement was conducted at a remote, background, high-altitude site (Qomolangma Station, QOMS, 4276 m a.s.l.) in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) along with other collocated instruments. The field measurement was performed from 12 April to 12 May 2016 to chemically characterize the high time-resolved submicron particulate matter (PM1) and obtain the dynamic processes (emissions, transport, and chemical evolution) of biomass burning (BB), frequently transported from South Asia to the Himalayas during pre-monsoon season. Overall, the average (±1σ) PM1 mass concentration was 4.44 (±4.54) µg m-3 for the entire study, which is comparable with those observed at other remote sites worldwide. Organic aerosol (OA) was the dominant PM1 species (accounting for 54.3 % of total PM1 on average) followed by black carbon (BC) (25.0 %), sulfate (9.3 %), ammonium (5.8 %), nitrate (5.1 %), and chloride (0.4 %). The average size distributions of PM1 species all peaked at an overlapping accumulation mode (˜ 500 nm), suggesting that aerosol particles were internally well-mixed and aged during long-range transport. Positive matrix factorization (PMF) analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a BB-related OA (BBOA, 43.7 %), a nitrogen-containing OA (NOA, 13.9 %) and a more-oxidized oxygenated OA (MO-OOA, 42.4 %). Two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions from the west and southwest of QOMS during the study were observed. A typical BB plume was investigated in detail to illustrate the chemical evolution of aerosol characteristics under distinct air mass origins, meteorological conditions, and atmospheric oxidation processes.

A soluble, one-dimensional problem for coupled heat conduction and mass diffusion with aerosol formation in a vapour-gas mixture

International Nuclear Information System (INIS)

Barrett, J.C.; Clement, C.F.

1986-01-01

The coupled equations for heat and mass transfer are reduced to ordinary differential equations applying to semi-infinite region bounded by a wall. Solutions are obtained in the limits of no aerosol and of negligible supersaturations, in which case the aerosol growth rate is calculated. In agreement with earlier general predictions, results for water vapour-air mixtures show very different behaviour between heating and cooling the mixtures, and that aerosol growth rates do not increase with temperature, but rather become a much smaller fraction of evaporation or condensation rates at the wall. A new feature is that, in the cooling case, an aerosol growth region is predicted to exist immediately adjacent to the wall, whereas further away any aerosol is predicted to evaporate. (author)

Enviro-HIRLAM/ HARMONIE Studies in ECMWF HPC EnviroAerosols Project

Science.gov (United States)

Hansen Sass, Bent; Mahura, Alexander; Nuterman, Roman; Baklanov, Alexander; Palamarchuk, Julia; Ivanov, Serguei; Pagh Nielsen, Kristian; Penenko, Alexey; Edvardsson, Nellie; Stysiak, Aleksander Andrzej; Bostanbekov, Kairat; Amstrup, Bjarne; Yang, Xiaohua; Ruban, Igor; Bergen Jensen, Marina; Penenko, Vladimir; Nurseitov, Daniyar; Zakarin, Edige

2017-04-01

The EnviroAerosols on ECMWF HPC project (2015-2017) "Enviro-HIRLAM/ HARMONIE model research and development for online integrated meteorology-chemistry-aerosols feedbacks and interactions in weather and atmospheric composition forecasting" is aimed at analysis of importance of the meteorology-chemistry/aerosols interactions and to provide a way for development of efficient techniques for on-line coupling of numerical weather prediction and atmospheric chemical transport via process-oriented parameterizations and feedback algorithms, which will improve both the numerical weather prediction and atmospheric composition forecasts. Two main application areas of the on-line integrated modelling are considered: (i) improved numerical weather prediction with short-term feedbacks of aerosols and chemistry on formation and development of meteorological variables, and (ii) improved atmospheric composition forecasting with on-line integrated meteorological forecast and two-way feedbacks between aerosols/chemistry and meteorology. During 2015-2016 several research projects were realized. At first, the study on "On-line Meteorology-Chemistry/Aerosols Modelling and Integration for Risk Assessment: Case Studies" focused on assessment of scenarios with accidental and continuous emissions of sulphur dioxide for case studies for Atyrau (Kazakhstan) near the northern part of the Caspian Sea and metallurgical enterprises on the Kola Peninsula (Russia), with GIS integration of modelling results into the RANDOM (Risk Assessment of Nature Detriment due to Oil spill Migration) system. At second, the studies on "The sensitivity of precipitation simulations to the soot aerosol presence" & "The precipitation forecast sensitivity to data assimilation on a very high resolution domain" focused on sensitivity and changes in precipitation life-cycle under black carbon polluted conditions over Scandinavia. At third, studies on "Aerosol effects over China investigated with a high resolution

Lung toxicity determination by in vitro exposure at the air liquid interface with an integrated online dose measurement

International Nuclear Information System (INIS)

Muelhopt, Sonja; Paur, H-R; Diabate, S; Weiss, C; Krebs, T

2009-01-01

Epidemiological studies show an association between the concentration of ultrafine particles in the atmosphere and the rate of mortality or morbidity due to respiratory and cardiovascular diseases. For the quantitative assessment of the toxicity of airborne nanoparticles the dose-response relationship is tested in in vitro test systems using bioassays of cell cultures as sensor. For the air-liquid interface exposure of cell cultures towards aerosols the Karlsruhe exposure system was developed. The human lung cell cultures are exposed in VITROCELL (registered) system modules with a constant flow of the conditioned aerosol. After exposure the cells are analyzed to measure the biological responses such as viability, inflammatory or oxidative stress. For the determination of the dose response relationship the accurate knowledge of the deposited particle mass is essential. A new online method is developed in the Karlsruhe exposure system: the sensor of a quartz crystal microbalance is placed in an exposure chamber instead of the membrane insert and exposed to the aerosol in the same way as the cell cultures. The deposited mass per area unit is monitored as a function of exposure time showing a linear relationship for a constant aerosol flow with defined particle concentration. A comparison of this new dose signal to a dosimetry method using fluorescein sodium particles shows a very good correlation between the sensor signal of the quartz crystal microbalance and the deposited mass on the membranes shown by spectroscopy. This system for the first time provides an online dose measurement for in vitro experiments with nanoparticles.

A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

Science.gov (United States)

Heringa, M. F.; Decarlo, P. F.; Chirico, R.; Tritscher, T.; Clairotte, M.; Mohr, C.; Crippa, M.; Slowik, J. G.; Pfaffenberger, L.; Dommen, J.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.

2012-02-01

Organic aerosol (OA) represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and compared to SOA from α-pinene. The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production. Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra showing Pearson's r values >0.94 for the correlations between the four different SOA types after five hours of aging. High-resolution mass spectra (HR-MS) showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxygenated OA (SV-OOA) observed in the ambient aerosol. The atomic O:C ratios were found to be in the range of 0.25-0.55 with no major increase during the first five hours of aging. On average, the diesel SOA showed the lowest O:C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions revealed that the SOA source with the highest O:C ratio had the largest fraction of small ions. The HR data of the four sources could be clustered and separated using principal component analysis (PCA). The model showed a significant separation of the four SOA types and clustering of the duplicate experiments on the first two principal components (PCs), which explained 79% of the total variance. Projection of ambient SV-OOA spectra resolved by positive matrix factorization (PMF) showed that this approach could be useful to identify large contributions of the tested SOA sources to SV-OOA. The first results from this

Organic Aerosol Component (OACOMP) Value-Added Product

Energy Technology Data Exchange (ETDEWEB)

Fast, J [Pacific Northwest National Laboratory; Zhang, Q; tilp, A [Brookhaven National Laboratory; Shippert, T [Pacific Northwest National Laboratory; Parworth, C; Mei, F [Pacific Northwest National Laboratory

2013-08-23

Organic aerosol (OA, i.e., the organic fraction of particles) accounts for 10–90% of the fine aerosol mass globally and is a key determinant of aerosol radiative forcing. But atmospheric OA is poorly characterized and its life cycle insufficiently represented in models. As a result, current models are unable to simulate OA concentrations and properties accurately. This deficiency represents a large source of uncertainty in quantification of aerosol effects and prediction of future climate change. Evaluation and development of aerosol models require data products generated from field observations. Real-time, quantitative data acquired with aerosol mass spectrometers (AMS) (Canagaratna et al. 2007) are critical to this need. The AMS determines size-resolved concentrations of non-refractory (NR) species in submicrometer particles (PM1) with fast time resolution suitable for both ground-based and aircraft deployments. The high-resolution AMS (HR-AMS), which is equipped with a high mass resolution time-of-flight mass spectrometer, can be used to determine the elemental composition and oxidation degrees of OA (DeCarlo et al. 2006).

Technical Note: Molecular characterization of aerosol-derived water soluble organic carbon using ultrahigh resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry

Directory of Open Access Journals (Sweden)

R. M. Dickhut

2008-09-01

Full Text Available Despite the acknowledged relevance of aerosol-derived water-soluble organic carbon (WSOC to climate and biogeochemical cycling, characterization of aerosol WSOC has been limited. Electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI FT-ICR MS was utilized in this study to provide detailed molecular level characterization of the high molecular weight (HMW; m/z>223 component of aerosol-derived WSOC collected from rural sites in Virginia and New York, USA. More than 3000 peaks were detected by ESI FT-ICR MS within a m/z range of 223–600 for each sample. Approximately 86% (Virginia and 78% (New York of these peaks were assigned molecular formulas using only carbon (C, hydrogen (H, oxygen (O, nitrogen (N, and sulfur (S as elemental constituents. H/C and O/C molar ratios were plotted on van Krevelen diagrams and indicated a strong contribution of lignin-like and lipid-like compounds to the aerosol-derived WSOC samples. Approximately 1–4% of the peaks in the aerosol-derived WSOC mass spectra were classified as black carbon (BC on the basis of double bond equivalents calculated from the assigned molecular formulas. In addition, several high-magnitude peaks in the mass spectra of samples from both sites corresponded to molecular formulas proposed in previous secondary organic aerosol (SOA laboratory investigations indicating that SOAs are important constituents of the WSOC. Overall, ESI FT-ICR MS provides a level of resolution adequate for detailed compositional and source information of the HMW constituents of aerosol-derived WSOC.

ACTRIS ACSM intercomparison - Part 2: Intercomparison of ME-2 organic source apportionment results from 15 individual, co-located aerosol mass spectrometers

Science.gov (United States)

Fröhlich, R.; Crenn, V.; Setyan, A.; Belis, C. A.; Canonaco, F.; Favez, O.; Riffault, V.; Slowik, J. G.; Aas, W.; Aijälä, M.; Alastuey, A.; Artiñano, B.; Bonnaire, N.; Bozzetti, C.; Bressi, M.; Carbone, C.; Coz, E.; Croteau, P. L.; Cubison, M. J.; Esser-Gietl, J. K.; Green, D. C.; Gros, V.; Heikkinen, L.; Herrmann, H.; Jayne, J. T.; Lunder, C. R.; Minguillón, M. C.; Močnik, G.; O'Dowd, C. D.; Ovadnevaite, J.; Petralia, E.; Poulain, L.; Priestman, M.; Ripoll, A.; Sarda-Estève, R.; Wiedensohler, A.; Baltensperger, U.; Sciare, J.; Prévôt, A. S. H.

2015-06-01

Chemically resolved atmospheric aerosol data sets from the largest intercomparison of the Aerodyne aerosol chemical speciation monitors (ACSMs) performed to date were collected at the French atmospheric supersite SIRTA. In total 13 quadrupole ACSMs (Q-ACSM) from the European ACTRIS ACSM network, one time-of-flight ACSM (ToF-ACSM), and one high-resolution ToF aerosol mass spectrometer (AMS) were operated in parallel for about 3 weeks in November and December~2013. Part 1 of this study reports on the accuracy and precision of the instruments for all the measured species. In this work we report on the intercomparison of organic components and the results from factor analysis source apportionment by positive matrix factorisation (PMF) utilising the multilinear engine 2 (ME-2). Except for the organic contribution of mass-to-charge ratio m/z 44 to the total organics (f44), which varied by factors between 0.6 and 1.3 compared to the mean, the peaks in the organic mass spectra were similar among instruments. The m/z 44 differences in the spectra resulted in a variable f44 in the source profiles extracted by ME-2, but had only a minor influence on the extracted mass contributions of the sources. The presented source apportionment yielded four factors for all 15 instruments: hydrocarbon-like organic aerosol (HOA), cooking-related organic aerosol (COA), biomass burning-related organic aerosol (BBOA) and secondary oxygenated organic aerosol (OOA). ME-2 boundary conditions (profile constraints) were optimised individually by means of correlation to external data in order to achieve equivalent / comparable solutions for all ACSM instruments and the results are discussed together with the investigation of the influence of alternative anchors (reference profiles). A comparison of the ME-2 source apportionment output of all 15 instruments resulted in relative standard deviations (SD) from the mean between 13.7 and 22.7 % of the source's average mass contribution depending on the

Online coupling of pure O_2 thermo-optical methods – "1"4C AMS for source apportionment of carbonaceous aerosols

International Nuclear Information System (INIS)

Agrios, Konstantinos; Salazar, Gary; Zhang, Yan-Lin; Uglietti, Chiara; Battaglia, Michael; Luginbühl, Marc; Ciobanu, Viorela Gabriela; Vonwiller, Matthias; Szidat, Sönke

2015-01-01

This paper reports on novel separation methods developed for the direct determination of "1"4C in organic carbon (OC) and elemental carbon (EC), two sub-fractions of total carbon (TC) of atmospheric air particulate matter. Until recently, separation of OC and EC has been performed off-line by manual and time-consuming techniques that relied on the collection of massive CO_2 fractions. We present here two on-line hyphenated techniques between a Sunset OC/EC analyzer and a MICADAS (MIni radioCArbon DAting System) accelerator mass spectrometer (AMS) equipped with a gas ion source. The first implementation facilitates the direct measurement in the low sample size range (<10 μg C) with high throughput on a routine basis, while the second explores the potential for a continuous-flow real-time CO_2 gas feed into the ion source. The performance achieved with reference materials and real atmospheric samples will be discussed to draw conclusions on the improvement offered in the field of "1"4C aerosol source apportionment.

Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

Science.gov (United States)

Lewis, K. A.; Arnott, W. P.; Moosmüller, H.; Chakrabarty, R. K.; Carrico, C. M.; Kreidenweis, S. M.; Day, D. E.; Malm, W. C.; Laskin, A.; Jimenez, J. L.; Ulbrich, I. M.; Huffman, J. A.; Onasch, T. B.; Trimborn, A.; Liu, L.; Mishchenko, M. I.

2009-11-01

Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used were Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients revealed a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: (1) shielding of inner monomers after particle consolidation or collapse with water uptake; (2) the lower case contribution of mass transfer through evaporation and condensation at high relative humidity (RH) to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

Reduction in biomass burning aerosol light absorption upon humidification: Roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

Energy Technology Data Exchange (ETDEWEB)

lewis, Kristen A.; Arnott, W. P.; Moosmuller, H.; Chakrabarti, Raj; Carrico, Christian M.; Kreidenweis, Sonia M.; Day, Derek E.; Malm, William C.; Laskin, Alexander; Jimenez, Jose L.; Ulbrich, Ingrid M.; Huffman, John A.; Onasch, Timothy B.; Trimborn, Achim; Liu, Li; Mishchenko, M.

2009-11-27

Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used are Montana ponderosa pine (Pinus ponderosa), southern California chamise (Adenostoma fasciculatum), and Florida saw palmetto (Serenoa repens). Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients reveal a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: 1. Shielding of inner monomers after particle consolidation or collapse with water uptake; 2. The contribution of mass transfer through evaporation and condensation at high relative humidity to the usual heat transfer pathway for energy release by laser heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

A new application of hierarchical cluster analysis to investigate organic peaks in bulk mass spectra obtained with an Aerodyne Aerosol Mass Spectrometer

Science.gov (United States)

Middlebrook, A. M.; Marcolli, C.; Canagaratna, M. R.; Worsnop, D. R.; Bahreini, R.; de Gouw, J. A.; Warneke, C.; Goldan, P. D.; Kuster, W. C.; Williams, E. J.; Lerner, B. M.; Roberts, J. M.; Meagher, J. F.; Fehsenfeld, F. C.; Marchewka, M. L.; Bertman, S. B.

2006-12-01

We applied hierarchical cluster analysis to an Aerodyne aerosol mass spectrometer (AMS) bulk mass spectral dataset collected aboard the NOAA research vessel Ronald H. Brown during the 2002 New England Air Quality Study off the east coast of the United States. Emphasizing the organic peaks, the cluster analysis yielded a series of categories that are distinguishable with respect to their mass spectra and their occurrence as a function of time. The differences between the categories mainly arise from relative intensity changes rather than from the presence or absence of specific peaks. The most frequent category exhibits a strong signal at m/z 44 and represents oxidized organic matter probably originating from both anthropogenic as well as biogenic sources. On the basis of spectral and trace gas correlations, the second most common category with strong signals at m/z 29, 43, and 44 contains contributions from isoprene oxidation products. The third through the fifth most common categories have peak patterns characteristic of monoterpene oxidation products and were most frequently observed when air masses from monoterpene rich regions were sampled. Taken together, the second through the fifth most common categories represent on average 17% of the total organic mass that stems likely from biogenic sources during the ship's cruise. These numbers have to be viewed as lower limits since the most common category was attributed to anthropogenic sources for this calculation. The cluster analysis was also very effective in identifying a few contaminated mass spectra that were not removed during pre-processing. This study demonstrates that hierarchical clustering is a useful tool to analyze the complex patterns of the organic peaks in bulk aerosol mass spectra from a field study.

Use of the NASA GEOS-5 SEAC4RS Meteorological and Aerosol Reanalysis for assessing simulated aerosol optical properties as a function of smoke age

Science.gov (United States)

Randles, C. A.; da Silva, A. M., Jr.; Colarco, P. R.; Darmenov, A.; Buchard, V.; Govindaraju, R.; Chen, G.; Hair, J. W.; Russell, P. B.; Shinozuka, Y.; Wagner, N.; Lack, D.

2014-12-01

The NASA Goddard Earth Observing System version 5 (GEOS-5) Earth system model, which includes an online aerosol module, provided chemical and weather forecasts during the SEAC4RS field campaign. For post-mission analysis, we have produced a high resolution (25 km) meteorological and aerosol reanalysis for the entire campaign period. In addition to the full meteorological observing system used for routine NWP, we assimilate 550 nm aerosol optical depth (AOD) derived from MODIS (both Aqua and Terra satellites), ground-based AERONET sun photometers, and the MISR instrument (over bright surfaces only). Daily biomass burning emissions of CO, CO2, SO2, and aerosols are derived from MODIS fire radiative power retrievals. We have also introduced novel smoke "age" tracers, which provide, for a given time, a snapshot histogram of the age of simulated smoke aerosol. Because GEOS-5 assimilates remotely sensed AOD data, it generally reproduces observed (column) AOD compared to, for example, the airborne 4-STAR instrument. Constraining AOD, however, does not imply a good representation of either the vertical profile or the aerosol microphysical properties (e.g., composition, absorption). We do find a reasonable vertical structure for aerosols is attained in the model, provided actual smoke injection heights are not much above the planetary boundary layer, as verified with observations from DIAL/HRSL aboard the DC8. The translation of the simulated aerosol microphysical properties to total column AOD, needed in the aerosol assimilation step, is based on prescribed mass extinction efficiencies that depend on wavelength, composition, and relative humidity. Here we also evaluate the performance of the simulated aerosol speciation by examining in situ retrievals of aerosol absorption/single scattering albedo and scattering growth factor (f(RH)) from the LARGE and AOP suite of instruments. Putting these comparisons in the context of smoke age as diagnosed by the model helps us to

The Pasadena Aerosol Characterization Observatory (PACO: chemical and physical analysis of the Western Los Angeles basin aerosol

Directory of Open Access Journals (Sweden)

S. P. Hersey

2011-08-01

Full Text Available The Pasadena Aerosol Characterization Observatory (PACO represents the first major aerosol characterization experiment centered in the Western/Central Los Angeles Basin. The sampling site, located on the campus of the California Institute of Technology in Pasadena, was positioned to sample a continuous afternoon influx of transported urban aerosol with a photochemical age of 1–2 h and generally free from major local contributions. Sampling spanned 5 months during the summer of 2009, which were broken into 3 regimes on the basis of distinct meteorological conditions. Regime I was characterized by a series of low pressure systems, resulting in high humidity and rainy periods with clean conditions. Regime II typified early summer meteorology, with significant morning marine layers and warm, sunny afternoons. Regime III was characterized by hot, dry conditions with little marine layer influence. Regardless of regime, organic aerosol (OA is the most significant constituent of nonrefractory submicron Los Angeles aerosol (42, 43, and 55 % of total submicron mass in regimes I, II, and III, respectively. The overall oxidation state remains relatively constant on timescales of days to weeks (O:C = 0.44 ± 0.08, 0.55 ± 0.05, and 0.48 ± 0.08 during regimes I, II, and III, respectively, with no difference in O:C between morning and afternoon periods. Periods characterized by significant morning marine layer influence followed by photochemically favorable afternoons displayed significantly higher aerosol mass and O:C ratio, suggesting that aqueous processes may be important in the generation of secondary aerosol and oxidized organic aerosol (OOA in Los Angeles. Online analysis of water soluble organic carbon (WSOC indicates that water soluble organic mass (WSOM reaches maxima near 14:00–15:00 local time (LT, but the percentage of AMS organic mass contributed by WSOM remains relatively constant throughout the day. Sulfate and nitrate reside predominantly

Whole-body nanoparticle aerosol inhalation exposures.

Science.gov (United States)

Yi, Jinghai; Chen, Bean T; Schwegler-Berry, Diane; Frazer, Dave; Castranova, Vince; McBride, Carroll; Knuckles, Travis L; Stapleton, Phoebe A; Minarchick, Valerie C; Nurkiewicz, Timothy R

2013-05-07

Inhalation is the most likely exposure route for individuals working with aerosolizable engineered nano-materials (ENM). To properly perform nanoparticle inhalation toxicology studies, the aerosols in a chamber housing the experimental animals must have: 1) a steady concentration maintained at a desired level for the entire exposure period; 2) a homogenous composition free of contaminants; and 3) a stable size distribution with a geometric mean diameter generation of aerosols containing nanoparticles is quite challenging because nanoparticles easily agglomerate. This is largely due to very strong inter-particle forces and the formation of large fractal structures in tens or hundreds of microns in size (6), which are difficult to be broken up. Several common aerosol generators, including nebulizers, fluidized beds, Venturi aspirators and the Wright dust feed, were tested; however, none were able to produce nanoparticle aerosols which satisfy all criteria (5). A whole-body nanoparticle aerosol inhalation exposure system was fabricated, validated and utilized for nano-TiO2 inhalation toxicology studies. Critical components: 1) novel nano-TiO2 aerosol generator; 2) 0.5 m(3) whole-body inhalation exposure chamber; and 3) monitor and control system. Nano-TiO2 aerosols generated from bulk dry nano-TiO2 powders (primary diameter of 21 nm, bulk density of 3.8 g/cm(3)) were delivered into the exposure chamber at a flow rate of 90 LPM (10.8 air changes/hr). Particle size distribution and mass concentration profiles were measured continuously with a scanning mobility particle sizer (SMPS), and an electric low pressure impactor (ELPI). The aerosol mass concentration (C) was verified gravimetrically (mg/m(3)). The mass (M) of the collected particles was determined as M = (Mpost-Mpre), where Mpre and Mpost are masses of the filter before and after sampling (mg). The mass concentration was calculated as C = M/(Q*t), where Q is sampling flowrate (m(3)/min), and t is the sampling

The ToF-ACSM: a portable aerosol chemical speciation monitor with TOFMS detection

Directory of Open Access Journals (Sweden)

R. Fröhlich

2013-11-01

Full Text Available 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 −3 for a time resolution of 30 min. With simple upgrades these limits can be brought down by another factor of ~ 8. This allows for operation at higher time resolutions and in low concentration environments. The associated software packages (single packages for integrated operation and calibration and analysis provide a high degree of automation and remote access, minimising the need for 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.

On-Line Synthesis and Analysis by Mass Spectrometry

Science.gov (United States)

Bain, Ryan M.; Pulliam, Christopher J.; Raab, Shannon A.; Cooks, R. Graham

2015-01-01

In this laboratory experiment, students learn how to use ESI to accelerate chemical synthesis and to couple it with on-line mass spectrometry for structural analysis. The Hantzsch synthesis of symmetric 1,4-dihydropyridines is a classic example of a one-pot reaction in which multiple intermediates can serve to indicate the progress of the reaction…

Reduction in biomass burning aerosol light absorption upon humidification: roles of inorganically-induced hygroscopicity, particle collapse, and photoacoustic heat and mass transfer

Directory of Open Access Journals (Sweden)

L. Liu

2009-11-01

Full Text Available Smoke particle emissions from the combustion of biomass fuels typical for the western and southeastern United States were studied and compared under high humidity and ambient conditions in the laboratory. The fuels used were Montana ponderosa pine (Pinus ponderosa, southern California chamise (Adenostoma fasciculatum, and Florida saw palmetto (Serenoa repens. Information on the non-refractory chemical composition of biomass burning aerosol from each fuel was obtained with an aerosol mass spectrometer and through estimation of the black carbon concentration from light absorption measurements at 870 nm. Changes in the optical and physical particle properties under high humidity conditions were observed for hygroscopic smoke particles containing substantial inorganic mass fractions that were emitted from combustion of chamise and palmetto fuels. Light scattering cross sections increased under high humidity for these particles, consistent with the hygroscopic growth measured for 100 nm particles in HTDMA measurements. Photoacoustic measurements of aerosol light absorption coefficients revealed a 20% reduction with increasing relative humidity, contrary to the expectation of light absorption enhancement by the liquid coating taken up by hygroscopic particles. This reduction is hypothesized to arise from two mechanisms: (1 shielding of inner monomers after particle consolidation or collapse with water uptake; (2 the lower case contribution of mass transfer through evaporation and condensation at high relative humidity (RH to the usual heat transfer pathway for energy release by laser-heated particles in the photoacoustic measurement of aerosol light absorption. The mass transfer contribution is used to evaluate the fraction of aerosol surface covered with liquid water solution as a function of RH.

The performance and the characterization of laser ablation aerosol particle time-of-flight mass spectrometry (LAAP-ToF-MS)

Science.gov (United States)

Gemayel, Rachel; Hellebust, Stig; Temime-Roussel, Brice; Hayeck, Nathalie; Van Elteren, Johannes T.; Wortham, Henri; Gligorovski, Sasho

2016-05-01

Hyphenated laser ablation-mass spectrometry instruments have been recognized as useful analytical tools for the detection and chemical characterization of aerosol particles. Here we describe the performances of a laser ablation aerosol particle time-of-flight mass spectrometer (LAAP-ToF-MS) which was designed for aerodynamic particle sizing using two 405 nm scattering lasers and characterization of the chemical composition of single aerosol particle via ablation/ionization by a 193 nm excimer laser and detection in a bipolar time-of-flight mass spectrometer with a mass resolving power of m/Δm > 600.We describe a laboratory based optimization strategy for the development of an analytical methodology for characterization of atmospheric particles using the LAAP-ToF-MS instrument in combination with a particle generator, a differential mobility analyzer and an optical particle counter. We investigated the influence of particle number concentration, particle size and particle composition on the detection efficiency. The detection efficiency is a product of the scattering efficiency of the laser diodes and the ionization efficiency or hit rate of the excimer laser. The scattering efficiency was found to vary between 0.6 and 1.9 % with an average of 1.1 %; the relative standard deviation (RSD) was 17.0 %. The hit rate exhibited good repeatability with an average value of 63 % and an RSD of 18 %. In addition to laboratory tests, the LAAP-ToF-MS was used to sample ambient air during a period of 6 days at the campus of Aix-Marseille University, situated in the city center of Marseille, France. The optimized LAAP-ToF-MS methodology enables high temporal resolution measurements of the chemical composition of ambient particles, provides new insights into environmental science, and a new investigative tool for atmospheric chemistry and physics, aerosol science and health impact studies.

ACTRIS ACSM intercomparison – Part 2: Intercomparison of ME-2 organic source apportionment results from 15 individual, co-located aerosol mass spectrometers

Directory of Open Access Journals (Sweden)

R. Fröhlich

2015-06-01

Full Text Available Chemically resolved atmospheric aerosol data sets from the largest intercomparison of the Aerodyne aerosol chemical speciation monitors (ACSMs performed to date were collected at the French atmospheric supersite SIRTA. In total 13 quadrupole ACSMs (Q-ACSM from the European ACTRIS ACSM network, one time-of-flight ACSM (ToF-ACSM, and one high-resolution ToF aerosol mass spectrometer (AMS were operated in parallel for about 3 weeks in November and December~2013. Part 1 of this study reports on the accuracy and precision of the instruments for all the measured species. In this work we report on the intercomparison of organic components and the results from factor analysis source apportionment by positive matrix factorisation (PMF utilising the multilinear engine 2 (ME-2. Except for the organic contribution of mass-to-charge ratio m/z 44 to the total organics (f44, which varied by factors between 0.6 and 1.3 compared to the mean, the peaks in the organic mass spectra were similar among instruments. The m/z 44 differences in the spectra resulted in a variable f44 in the source profiles extracted by ME-2, but had only a minor influence on the extracted mass contributions of the sources. The presented source apportionment yielded four factors for all 15 instruments: hydrocarbon-like organic aerosol (HOA, cooking-related organic aerosol (COA, biomass burning-related organic aerosol (BBOA and secondary oxygenated organic aerosol (OOA. ME-2 boundary conditions (profile constraints were optimised individually by means of correlation to external data in order to achieve equivalent / comparable solutions for all ACSM instruments and the results are discussed together with the investigation of the influence of alternative anchors (reference profiles. A comparison of the ME-2 source apportionment output of all 15 instruments resulted in relative standard deviations (SD from the mean between 13.7 and 22.7 % of the source's average mass contribution depending on

Seasonal and spatial variability of the OM/OC mass ratios and high regional correlation between oxalic acid and zinc in Chinese urban organic aerosols

Directory of Open Access Journals (Sweden)

L. Xing

2013-04-01

Full Text Available We calculated the organic matter to organic carbon mass ratios (OM/OC mass ratios in PM2.5 collected from 14 Chinese cities during summer and winter of 2003 and analyzed the causes for their seasonal and spatial variability. The OM/OC mass ratios were calculated two ways. Using a mass balance method, the calculated OM/OC mass ratios averaged 1.92 ± 0.39 year-round, with no significant seasonal or spatial variation. The second calculation was based on chemical species analyses of the organic compounds extracted from the PM2.5 samples using dichloromethane/methanol and water. The calculated OM/OC mass ratio in summer was relatively high (1.75 ± 0.13 and spatially-invariant due to vigorous photochemistry and secondary organic aerosol (OA production throughout the country. The calculated OM/OC mass ratio in winter (1.59 ± 0.18 was significantly lower than that in summer, with lower values in northern cities (1.51 ± 0.07 than in southern cities (1.65 ± 0.15. This likely reflects the wider usage of coal for heating purposes in northern China in winter, in contrast to the larger contributions from biofuel and biomass burning in southern China in winter. On average, organic matter constituted 36% and 34% of Chinese urban PM2.5 mass in summer and winter, respectively. We report, for the first time, a high regional correlation between Zn and oxalic acid in Chinese urban aerosols in summer. This is consistent with the formation of stable Zn oxalate complex in the aerosol phase previously proposed by Furukawa and Takahashi (2011. We found that many other dicarboxylic acids were also highly correlated with Zn in the summer Chinese urban aerosol samples, suggesting that they may also form stable organic complexes with Zn. Such formation may have profound implications for the atmospheric abundance and hygroscopic properties of aerosol dicarboxylic acids.

Seasonal and spatial variability of the OM/OC mass ratios and high regional correlation between oxalic acid and zinc in Chinese urban organic aerosols

Science.gov (United States)

Xing, L.; Fu, T.-M.; Cao, J. J.; Lee, S. C.; Wang, G. H.; Ho, K. F.; Cheng, M.-C.; You, C.-F.; Wang, T. J.

2013-04-01

We calculated the organic matter to organic carbon mass ratios (OM/OC mass ratios) in PM2.5 collected from 14 Chinese cities during summer and winter of 2003 and analyzed the causes for their seasonal and spatial variability. The OM/OC mass ratios were calculated two ways. Using a mass balance method, the calculated OM/OC mass ratios averaged 1.92 ± 0.39 year-round, with no significant seasonal or spatial variation. The second calculation was based on chemical species analyses of the organic compounds extracted from the PM2.5 samples using dichloromethane/methanol and water. The calculated OM/OC mass ratio in summer was relatively high (1.75 ± 0.13) and spatially-invariant due to vigorous photochemistry and secondary organic aerosol (OA) production throughout the country. The calculated OM/OC mass ratio in winter (1.59 ± 0.18) was significantly lower than that in summer, with lower values in northern cities (1.51 ± 0.07) than in southern cities (1.65 ± 0.15). This likely reflects the wider usage of coal for heating purposes in northern China in winter, in contrast to the larger contributions from biofuel and biomass burning in southern China in winter. On average, organic matter constituted 36% and 34% of Chinese urban PM2.5 mass in summer and winter, respectively. We report, for the first time, a high regional correlation between Zn and oxalic acid in Chinese urban aerosols in summer. This is consistent with the formation of stable Zn oxalate complex in the aerosol phase previously proposed by Furukawa and Takahashi (2011). We found that many other dicarboxylic acids were also highly correlated with Zn in the summer Chinese urban aerosol samples, suggesting that they may also form stable organic complexes with Zn. Such formation may have profound implications for the atmospheric abundance and hygroscopic properties of aerosol dicarboxylic acids.

Chemical characterization of long-range transport biomass burning emissions to the Himalayas: insights from high-resolution aerosol mass spectrometry

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X. Zhang

2018-04-01

Full Text Available An intensive field measurement was conducted at a remote, background, high-altitude site (Qomolangma Station, QOMS, 4276 m a.s.l. in the northern Himalayas, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS along with other collocated instruments. The field measurement was performed from 12 April to 12 May 2016 to chemically characterize the high time-resolved submicron particulate matter (PM1 and obtain the dynamic processes (emissions, transport, and chemical evolution of biomass burning (BB, frequently transported from South Asia to the Himalayas during pre-monsoon season. Overall, the average (±1σ PM1 mass concentration was 4.44 (±4.54 µg m−3 for the entire study, which is comparable with those observed at other remote sites worldwide. Organic aerosol (OA was the dominant PM1 species (accounting for 54.3 % of total PM1 on average followed by black carbon (BC (25.0 %, sulfate (9.3 %, ammonium (5.8 %, nitrate (5.1 %, and chloride (0.4 %. The average size distributions of PM1 species all peaked at an overlapping accumulation mode (∼ 500 nm, suggesting that aerosol particles were internally well-mixed and aged during long-range transport. Positive matrix factorization (PMF analysis on the high-resolution organic mass spectra identified three distinct OA factors, including a BB-related OA (BBOA, 43.7 %, a nitrogen-containing OA (NOA, 13.9 % and a more-oxidized oxygenated OA (MO-OOA, 42.4 %. Two polluted episodes with enhanced PM1 mass loadings and elevated BBOA contributions from the west and southwest of QOMS during the study were observed. A typical BB plume was investigated in detail to illustrate the chemical evolution of aerosol characteristics under distinct air mass origins, meteorological conditions, and atmospheric oxidation processes.

Online coupling of pure O{sub 2} thermo-optical methods – {sup 14}C AMS for source apportionment of carbonaceous aerosols

Energy Technology Data Exchange (ETDEWEB)

Agrios, Konstantinos [Department of Chemistry and Biochemistry, University of Bern, Bern (Switzerland); Oeschger Centre for Climate Change Research, University of Bern, Bern (Switzerland); Paul Scherrer Institute, Villigen (Switzerland); Salazar, Gary [Department of Chemistry and Biochemistry, University of Bern, Bern (Switzerland); Oeschger Centre for Climate Change Research, University of Bern, Bern (Switzerland); Zhang, Yan-Lin; Uglietti, Chiara [Department of Chemistry and Biochemistry, University of Bern, Bern (Switzerland); Oeschger Centre for Climate Change Research, University of Bern, Bern (Switzerland); Paul Scherrer Institute, Villigen (Switzerland); Battaglia, Michael [Department of Chemistry and Biochemistry, University of Bern, Bern (Switzerland); Oeschger Centre for Climate Change Research, University of Bern, Bern (Switzerland); Luginbühl, Marc [Department of Chemistry and Biochemistry, University of Bern, Bern (Switzerland); Ciobanu, Viorela Gabriela [Paul Scherrer Institute, Villigen (Switzerland); Vonwiller, Matthias [Department of Chemistry and Biochemistry, University of Bern, Bern (Switzerland); Oeschger Centre for Climate Change Research, University of Bern, Bern (Switzerland); Paul Scherrer Institute, Villigen (Switzerland); Szidat, Sönke, E-mail: szidat@dcb.unibe.ch [Department of Chemistry and Biochemistry, University of Bern, Bern (Switzerland); Oeschger Centre for Climate Change Research, University of Bern, Bern (Switzerland)

2015-10-15

This paper reports on novel separation methods developed for the direct determination of {sup 14}C in organic carbon (OC) and elemental carbon (EC), two sub-fractions of total carbon (TC) of atmospheric air particulate matter. Until recently, separation of OC and EC has been performed off-line by manual and time-consuming techniques that relied on the collection of massive CO{sub 2} fractions. We present here two on-line hyphenated techniques between a Sunset OC/EC analyzer and a MICADAS (MIni radioCArbon DAting System) accelerator mass spectrometer (AMS) equipped with a gas ion source. The first implementation facilitates the direct measurement in the low sample size range (<10 μg C) with high throughput on a routine basis, while the second explores the potential for a continuous-flow real-time CO{sub 2} gas feed into the ion source. The performance achieved with reference materials and real atmospheric samples will be discussed to draw conclusions on the improvement offered in the field of {sup 14}C aerosol source apportionment.

Single particle characterization, source apportionment, and aging effects of ambient aerosols in Southern California

Science.gov (United States)

Shields, Laura Grace

Composed of a mixture of chemical species and phases and existing in a variety of shapes and sizes, atmospheric aerosols are complex and can have serious influence on human health, the environment, and climate. In order to better understand the impact of aerosols on local to global scales, detailed measurements on the physical and chemical properties of ambient particles are essential. In addition, knowing the origin or the source of the aerosols is important for policymakers to implement targeted regulations and effective control strategies to reduce air pollution in their region. One of the most ground breaking techniques in aerosol instrumentation is single particle mass spectrometry (SPMS), which can provide online chemical composition and size information on the individual particle level. The primary focus of this work is to further improve the ability of one specific SPMS technique, aerosol time-of-flight mass spectrometry (ATOFMS), for the use of identifying the specific origin of ambient aerosols, which is known as source apportionment. The ATOFMS source apportionment method utilizes a library of distinct source mass spectral signatures to match the chemical information of the single ambient particles. The unique signatures are obtained in controlled source characterization studies, such as with the exhaust emissions of heavy duty diesel vehicles (HDDV) operating on a dynamometer. The apportionment of ambient aerosols is complicated by the chemical and physical processes an individual particle can undergo as it spends time in the atmosphere, which is referred to as "aging" of the aerosol. Therefore, the performance of the source signature library technique was investigated on the ambient dataset of the highly aged environment of Riverside, California. Additionally, two specific subsets of the Riverside dataset (ultrafine particles and particles containing trace metals), which are known to cause adverse health effects, were probed in greater detail. Finally

Sources of carbonaceous aerosol in the Amazon basin

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S. Gilardoni

2011-03-01

Full Text Available The quantification of sources of carbonaceous aerosol is important to understand their atmospheric concentrations and regulating processes and to study possible effects on climate and air quality, in addition to develop mitigation strategies.

In the framework of the European Integrated Project on Aerosol Cloud Climate Interactions (EUCAARI fine (D_p < 2.5 μm and coarse (2.5 μm < D_p <10 μm aerosol particles were sampled from February to June (wet season and from August to September (dry season 2008 in the central Amazon basin. The mass of fine particles averaged 2.4 μg m⁻³ during the wet season and 4.2 μg m⁻³ during the dry season. The average coarse aerosol mass concentration during wet and dry periods was 7.9 and 7.6 μg m⁻³, respectively. The overall chemical composition of fine and coarse mass did not show any seasonality with the largest fraction of fine and coarse aerosol mass explained by organic carbon (OC; the average OC to mass ratio was 0.4 and 0.6 in fine and coarse aerosol modes, respectively. The mass absorbing cross section of soot was determined by comparison of elemental carbon and light absorption coefficient measurements and it was equal to 4.7 m² g⁻¹ at 637 nm. Carbon aerosol sources were identified by Positive Matrix Factorization (PMF analysis of thermograms: 44% of fine total carbon mass was assigned to biomass burning, 43% to secondary organic aerosol (SOA, and 13% to volatile species that are difficult to apportion. In the coarse mode, primary biogenic aerosol particles (PBAP dominated the carbonaceous aerosol mass. The results confirmed the importance of PBAP in forested areas.

The source apportionment results were employed to evaluate the ability of global chemistry transport models to simulate carbonaceous aerosol sources in a regional tropical background site. The comparison showed an overestimation

Size-resolved mass concentrations of iron oxide aerosols and size-resolved number concentrations of iron oxide aerosols collected from King Air aircraft in Yellow Sea and East China Sea from 2013-02-14 to 2013-03-10 (NCEI Accession 0162201)

Data.gov (United States)

National Oceanic and Atmospheric Administration, Department of Commerce — This dataset contains size-resolved mass concentrations of iron oxide aerosols and size-resolved number concentrations of iron oxide aerosols, measured using the...

Physical aerosol properties and their relation to air mass origin at Monte Cimone (Italy during the first MINATROC campaign

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R. Van Dingenen

2005-01-01

Full Text Available Aerosol physical properties were measured at the Monte Cimone Observatory (Italy from 1 June till 6 July 2000. The measurement site is located in the transition zone between the continental boundary layer and the free troposphere (FT, at the border between the Mediterranean area and Central Europe, and is exposed to a variety of air masses. Sub-μm number size distributions, aerosol hygroscopicity near 90% RH, refractory size distribution at 270°C and equivalent black carbon mass were continuously measured. Number size distributions and hygroscopic properties indicate that the site is exposed to aged continental air masses, however during daytime it is also affected by upslope winds. The mixing of this transported polluted boundary layer air masses with relatively clean FT air leads to frequent nucleation events around local noon. Night-time size distributions, including fine and coarse fractions for each air mass episode, have been parameterized by a 3-modal lognormal distribution. Number and volume concentrations in the sub-μm modes are strongly affected by the air mass origin, with highest levels in NW-European air masses, versus very clean, free tropospheric air coming from the N-European sector. During a brief but distinct dust episode, the coarse mode is clearly enhanced. The observed hygroscopic behavior of the aerosol is consistent with the chemical composition described by Putaud et al. (2004, but no closure between known chemical composition and measured hygroscopicity could be made because the hygroscopic properties of the water-soluble organic matter (WSOM are not known. The data suggest that WSOM is slightly-to-moderately hygroscopic (hygroscopic growth factor GF at 90% relative humidity between 1.05 and 1.51, and that this property may well depend on the air mass origin and history. External mixing of aerosol particles is observed in all air masses through the occurrence of two hygroscopicity modes (average GF of 1.22 and 1

Laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF): performance, reference spectra and classification of atmospheric samples

Science.gov (United States)

Shen, Xiaoli; Ramisetty, Ramakrishna; Mohr, Claudia; Huang, Wei; Leisner, Thomas; Saathoff, Harald

2018-04-01

The laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF, AeroMegt GmbH) is able to identify the chemical composition and mixing state of individual aerosol particles, and thus is a tool for elucidating their impacts on human health, visibility, ecosystem, and climate. The overall detection efficiency (ODE) of the instrument we use was determined to range from ˜ (0.01 ± 0.01) to ˜ (4.23 ± 2.36) % for polystyrene latex (PSL) in the size range of 200 to 2000 nm, ˜ (0.44 ± 0.19) to ˜ (6.57 ± 2.38) % for ammonium nitrate (NH4NO3), and ˜ (0.14 ± 0.02) to ˜ (1.46 ± 0.08) % for sodium chloride (NaCl) particles in the size range of 300 to 1000 nm. Reference mass spectra of 32 different particle types relevant for atmospheric aerosol (e.g. pure compounds NH4NO3, K2SO4, NaCl, oxalic acid, pinic acid, and pinonic acid; internal mixtures of e.g. salts, secondary organic aerosol, and metallic core-organic shell particles; more complex particles such as soot and dust particles) were determined. Our results show that internally mixed aerosol particles can result in spectra with new clusters of ions, rather than simply a combination of the spectra from the single components. An exemplary 1-day ambient data set was analysed by both classical fuzzy clustering and a reference-spectra-based classification method. Resulting identified particle types were generally well correlated. We show how a combination of both methods can greatly improve the interpretation of single-particle data in field measurements.

The influence of continental air masses on the aerosols and nutrients deposition over the western North Pacific

Science.gov (United States)

Fu, Jiangping; Wang, Bo; Chen, Ying; Ma, Qingwei

2018-01-01

The air masses transported from East Asia have a strong impact on the aerosol properties and deposition in the marine boundary layer of the western North Pacific (WNP) during winter and spring. We joined a cruise between 17 Mar. and 22 Apr. 2014 and investigated the changes of aerosol composition and size distribution over the remote WNP and marginal seas. Although the secondary aerosol species (SO42-, NO3- and NH4+) in remote WNP were influenced significantly by the continental transport, NH4+ concentrations were lower than 2.7 μg m-3 in most sampling days and not correlated with non-sea-salt (nss)-SO42- suggesting that the ocean could be a primary source of NH4+. Moderate Cl- depletion (23%) was observed in remote WNP, and the inverse relationship between Cl- depletion percentages and nss-K+ in aerosols suggested that the transport of biomass burning smoke from East Asia might be a vital extra source of Cl-. Both Asian dust and haze events were encountered during the cruise. Asian dust carried large amounts of crustal elements such as Al and Ti to the WNP, and the dusty Fe deposition may double its background concentration in seawater. Differently, a dramatic increase of dry deposition flux of dissolved particulate inorganic nitrogen was observed during the haze event. Our study reveals that the transport of different continental air masses may have distinct biogeochemical impacts on the WNP by increasing the fluxes of different nutrient elements and potentially changing the nutrient stoichiometry.

Physicochemical characterization of Capstone depleted uranium aerosols I: uranium concentration in aerosols as a function of time and particle size.

Science.gov (United States)

Parkhurst, Mary Ann; Cheng, Yung Sung; Kenoyer, Judson L; Traub, Richard J

2009-03-01

During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing DU were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols were evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time, particularly within the first minute after a shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s after perforation, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% after 30 min. The initial and maximum uranium concentrations were lower in the Bradley vehicle than those observed in the Abrams tank, and the concentration levels decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in a cyclone sampler, which collected aerosol continuously for 2 h after perforation. The percentages of uranium mass in the cyclone separator stages ranged from 38 to 72% for the Abrams tank with conventional armor. In most cases, it varied with particle size, typically with less uranium associated with the smaller particle sizes. Neither the Abrams tank with DU armor nor the Bradley vehicle results were specifically correlated with particle size and can best be represented by their average uranium mass concentrations of 65

Aerosol Mass Scattering Efficiency: Generalized Treatment of the Organic Fraction

Science.gov (United States)

Garland, R. M.; Ravishankara, A. R.; Lovejoy, E. R.; Tolbert, M. A.; Baynard, T.

2005-12-01

Atmospheric aerosols are complex mixtures of organic and inorganic compounds. Current efforts to provide a simplified parameterization to describe the RH dependence of water uptake and associated optical properties lack the capability to include any dependence on the composition of the organic fraction. Using laboratory generated aerosol we have investigated the validity of such simplified treatment of organic fraction and estimated potential biases. In this study, we use cavity ring-down aerosol extinction photometry (CRD-AEP) to study the relative humidity (RH) dependence of the light extinction of aerosols, σep, simultaneously considering the influence of particle size, chemical composition, and mixing state (internal and external mixtures). We have produced internally mixed aerosol systems including; ammonium sulfate, ammonium nitrate, sodium chloride, dicarboxylic acids, sugars, amino acids and humic acid. These aerosols are produced with an atomizer and size-selected with a Differential Mobility Analyzer (DMA). The particles then enter into a CRD-AEP to measure dry extinction, σep(Dry), after which they travel into a RH conditioner and another CRD-AEP to measure the humidified aerosol extinction, fσ(ep)RH. The ratio of the humidified extinction to the dry extinction is fσ(ep)RH. Representative organic compounds were found to have fσ(ep)RH values that are much smaller than pure salts; though the fσ(ep)RH values vary little within the organic compounds studied. In addition, we have found that treating the inorganic/organic aerosols as external mixtures is generally correct to within ~10%, indicating appropriate simplified treatment of the RH dependence of atmospheric aerosol according to inorganic/organic fraction. In this presentation, we include recommendations for the generalized treatment of the organic fraction, exceptions to this generalized behavior, and estimates of the potential bias caused by generalized treatment.

Characterization of particulate matter emissions from on-road gasoline and diesel vehicles using a soot particle aerosol mass spectrometer

OpenAIRE

Dallmann, T. R.; Onasch, T. B.; Kirchstetter, T. W.; Worton, D. R.; Fortner, E. C.; Herndon, S. C.; Wood, E. C.; Franklin, J. P.; Worsnop, D. R.; Goldstein, A. H.; Harley, R. A.

2014-01-01

Particulate matter (PM) emissions were measured in July 2010 from on-road motor vehicles driving through a highway tunnel in the San Francisco Bay area. A soot particle aerosol mass spectrometer (SP-AMS) was used to measure the chemical composition of PM emitted by gasoline and diesel vehicles at high time resolution. Organic aerosol (OA) and black carbon (BC) concentrations were measured during various time periods that had different levels of diesel influence, as well as d...

Comparison of the impact of volcanic eruptions and aircraft emissions on the aerosol mass loading and sulfur budget in the stratosphere

Science.gov (United States)

Yue, Glenn K.; Poole, Lamont R.

1992-01-01

Data obtained by the Stratospheric Aerosol and Gas Experiment (SAGE) 1 and 2 were used to study the temporal variation of aerosol optical properties and to assess the mass loading of stratospheric aerosols from the eruption of volcanos Ruiz and Kelut. It was found that the yearly global average of optical depth at 1.0 micron for stratospheric background aerosols in 1979 was 1.16 x 10(exp -3) and in 1989 was 1.66 x 10(exp -3). The eruptions of volcanos Ruiz and Kelut ejected at least 5.6 x 10(exp 5) and 1.8 x 10(exp 5) tons of materials into the stratosphere, respectively. The amount of sulfur emitted per year from the projected subsonic and supersonic fleet is comparable to that contained in the background aerosol particles in midlatitudes from 35 deg N to 55 deg N.

Aerosol optical properties in the southeastern United States in summer – Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters

Directory of Open Access Journals (Sweden)

C. A. Brock

2016-04-01

Full Text Available Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US. Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015. We use these 0–4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH. For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry–climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of  ∼  25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1–0.5 µm diameter dominates

Ubiquitous influence of wildfire emissions and secondary organic aerosol on summertime atmospheric aerosol in the forested Great Lakes region

Science.gov (United States)

Gunsch, Matthew J.; May, Nathaniel W.; Wen, Miao; Bottenus, Courtney L. H.; Gardner, Daniel J.; VanReken, Timothy M.; Bertman, Steven B.; Hopke, Philip K.; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Long-range aerosol transport affects locations hundreds of kilometers from the point of emission, leading to distant particle sources influencing rural environments that have few major local sources. Source apportionment was conducted using real-time aerosol chemistry measurements made in July 2014 at the forested University of Michigan Biological Station near Pellston, Michigan, a site representative of the remote forested Great Lakes region. Size-resolved chemical composition of individual 0.5-2.0 µm particles was measured using an aerosol time-of-flight mass spectrometer (ATOFMS), and non-refractory aerosol mass less than 1 µm (PM1) was measured with a high-resolution aerosol mass spectrometer (HR-AMS). The field site was influenced by air masses transporting Canadian wildfire emissions and urban pollution from Milwaukee and Chicago. During wildfire-influenced periods, 0.5-2.0 µm particles were primarily aged biomass burning particles (88 % by number). These particles were heavily coated with secondary organic aerosol (SOA) formed during transport, with organics (average O/C ratio of 0.8) contributing 89 % of the PM1 mass. During urban-influenced periods, organic carbon, elemental carbon-organic carbon, and aged biomass burning particles were identified, with inorganic secondary species (ammonium, sulfate, and nitrate) contributing 41 % of the PM1 mass, indicative of atmospheric processing. With current models underpredicting organic carbon in this region and biomass burning being the largest combustion contributor to SOA by mass, these results highlight the importance for regional chemical transport models to accurately predict the impact of long-range transported particles on air quality in the upper Midwest, United States, particularly considering increasing intensity and frequency of Canadian wildfires.

Online mass storage system detailed requirements document

Science.gov (United States)

1976-01-01

The requirements for an online high density magnetic tape data storage system that can be implemented in a multipurpose, multihost environment is set forth. The objective of the mass storage system is to provide a facility for the compact storage of large quantities of data and to make this data accessible to computer systems with minimum operator handling. The results of a market survey and analysis of candidate vendor who presently market high density tape data storage systems are included.

Retrieval of Aerosol Components Using Multi-Wavelength Mie-Raman Lidar and Comparison with Ground Aerosol Sampling

Directory of Open Access Journals (Sweden)

Yukari Hara

2018-06-01

Full Text Available We verified an algorithm using multi-wavelength Mie-Raman lidar (MMRL observations to retrieve four aerosol components (black carbon (BC, sea salt (SS, air pollution (AP, and mineral dust (DS with in-situ aerosol measurements, and determined the seasonal variation of aerosol components in Fukuoka, in the western region of Japan. PM2.5, PM10, and mass concentrations of BC and SS components are derived from in-situ measurements. MMRL provides the aerosol extinction coefficient (α, particle linear depolarization ratio (δ, backscatter coefficient (β, and lidar ratio (S at 355 and 532 nm, and the attenuated backscatter coefficient (βatt at 1064 nm. We retrieved vertical distributions of extinction coefficients at 532 nm for four aerosol components (BC, SS, AP, and DS using 1α532 + 1β532 + 1βatt,1064 + 1δ532 data of MMRL. The retrieved extinction coefficients of the four aerosol components at 532 nm were converted to mass concentrations using the theoretical computed conversion factor assuming the prescribed size distribution, particle shape, and refractive index for each aerosol component. MMRL and in-situ measurements confirmed that seasonal variation of aerosol optical properties was affected by internal/external mixing of various aerosol components, in addition to hygroscopic growth of water-soluble aerosols. MMRL overestimates BC mass concentration compared to in-situ observation using the pure BC model. This overestimation was reduced drastically by introducing the internal mixture model of BC and water-soluble substances (Core-Gray Shell (CGS model. This result suggests that considering the internal mixture of BC and water-soluble substances is essential for evaluating BC mass concentration in this area. Systematic overestimation of BC mass concentration was found during summer, even when we applied the CGS model. The observational facts based on in-situ and MMRL measurements suggested that misclassification of AP as CGS particles was

Characterization of biogenic secondary organic aerosols using statistical methods; Charakterisierung Biogener Sekundaerer Organischer Aerosole mit Statistischen Methoden

Energy Technology Data Exchange (ETDEWEB)

Spindler, Christian

2010-07-01

Atmospheric aerosols have important influence on the radiation balance of the Earth, on visibility and human health. Secondary organic aerosol is formed from gas-to-particle conversion of oxidized volatile organic compounds. A dominant fraction of the gases originates from plant emissions, making biogenic secondary organic aerosol (BSOA) an especially important constituent of the atmosphere. Knowing the chemical composition of BSOA particles is crucial for a thorough understanding of aerosol processes in the environment. In this work, the chemical composition of BSOA particles was measured with aerosol mass spectrometry and analyzed with statistical methods. The experimental part of the work comprises process studies of the formation and aging of biogenic aerosols in simulation chambers. Using a plant chamber, real tree emissions were used to produce particles in a way close to conditions in forest environments. In the outdoor chamber SAPHIR, OH-radicals were produced from the photooxidation of ozone under illumination with natural sunlight. Here, BSOA was produced from defined mixtures of mono- and sesquiterpenes that represent boreal forest emissions. A third kind of experiments was performed in the indoor chamber AIDA. Here, particles were produced from ozonolysis of single monoterpenes and aged by condensing OH-oxidation products. Two aerosol mass spectrometers (AMS) were used to measure the chemical composition of the particles. One of the instruments is equipped with a quadrupole mass spectrometer providing unit mass resolution. The second instrument contains a time-of-flight mass spectrometer and provides mass resolution sufficient to distinguish different fragments with the same nominal mass. Aerosol mass spectra obtained with these instruments are strongly fragmented due to electron impact ionization of the evaporated molecules. In addition, typical BSOA mass spectra are very similar to each other. In order to get a more detailed knowledge about the mass

Preliminary study of elemental mass size distribution of urban aerosol collected in Debrecen

International Nuclear Information System (INIS)

Kertesz, Zs.; Borbely-Kiss, I.; Kiss, A.Z.; Koltay, E.; Szabo, Gy.

2000-01-01

Complete text of publication follows. Aerosol sampling campaigns were performed during January-February 1998 and August 1998 at an urban location (in the yard of the Institute of Nuclear Research), where aerosol sampling has been carried out continuously since 1991 with single stage Nuclepore filter holders, and since 1994 with 2-stage Gent stacked filter units (SFU). In the winter period in four weekdays 24-hours samplings were performed with a 7-stage PIXE International Cascade Impactor (PCI) and simultaneously with a SFU. On 19-25 August 1998, a week-long aerosol sampling campaign was carried out with the PCI (24-hour samplings), a SFU (24-hour samplings), and a streaker sampler (168-hour continuous sampling). For this period meteorological data were also obtained by a micro-meteorological station installed at the same location by the Radon Group. Elemental concentrations for Al, Si, P, S, Cl, K, Ca, Ti, V, Mn, Fe, Ni, Cu, Zn, Ba and Pb of the aerosol samples were determined by PIXE using the 2 MeV energy proton beam of the 5 MeV Van de Graaff accelerator of the Institute. The obtained average elemental concentrations and the seasonal variation in the elemental concentrations show good correlation with the results obtained from the analysis of the samples collected in previous years. In winter the elemental concentrations are usually lower than in summer, except Cl. The Cl concentration in the coarse fraction is higher with a factor of 10 than in summer due to the salting of the roads and pavements. The summer period included a long weekend with a national holiday. During the weekend the elemental concentrations and also the total mass decreased, and in the beginning of the following week it started to increase. Size distribution: the impactor we have used separate the aerosol within the size range of 0.25 μm and 30 μm into 7 fractions. The mass size distribution for elements of natural origin, like Si, Ca, Ti, Fe, and Mn has one mode: the coarse mode. The

Determination of particulate lead using aerosol mass spectrometry: MILAGRO/MCMA-2006 observations

Directory of Open Access Journals (Sweden)

D. Salcedo

2010-06-01

Full Text Available We report the first measurements of particulate lead (Pb from Aerodyne Aerosol Mass Spectrometers, which were deployed in and around Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO/Mexico City Metropolitan Area 2006 (MCMA-2006 field campaigns. The high resolution mass spectrometer of one of the AMS instruments (HR-AMS and the measured isotopic ratios unequivocally prove the detection of Pb in ambient particles. A substantial fraction of the lead evaporated slowly from the vaporizer of the instruments, which is indicative of species with low volatility at 600 °C. A model was developed in order to estimate the ambient particulate Pb entering the AMS from the signals in the "open" and the "closed" (or "background" mass spectrum modes of the AMS. The model suggests the presence of at least two lead fractions with ~25% of the Pb signal exhibiting rapid evaporation (1/e decay constant, τ<0.1 s and ~75% exhibiting slow evaporation (τ~2.4 min at the T0 urban supersite and a different fraction (70% prompt and 30% slow evaporation at a site northwest from the metropolitan area (PEMEX site. From laboratory experiments with pure Pb(NO₃₂ particles, we estimated that the Pb ionization efficiency relative to nitrate (RIE_Pb is 0.5. Comparison of time series of AMS Pb with other measurements carried out at the T0 supersite during MILAGRO (using Proton Induced X-ray Emission (PIXE, Inductively-Coupled Plasma Mass Spectrometry (ICP-MS and single-particle counts from an Aerosol Time-of-Fight Mass Spectrometer (ATOFMS shows similar levels (for PIXE and ICP-MS and substantial correlation. During part of the campaign, sampling at T0 was alternated every 10 min with an Aerosol Concentrator, which enabled the detection of signals for PbCl⁺ and PbS⁺ ions. PbS⁺ displays the signature of a slowly evaporating species, while PbCl⁺ appears to arise only

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.

Towards the improvements of simulating the chemical and optical properties of Chinese aerosols using an online coupled model – CUACE/Aero

Directory of Open Access Journals (Sweden)

Chun-Hong Zhou

2012-07-01

Full Text Available CUACE/Aero, the China Meteorological Administration (CMA Unified Atmospheric Chemistry Environment for aerosols, is a comprehensive numerical aerosol module incorporating emissions, gaseous chemistry and size-segregated multi-component aerosol algorithm. On-line coupled into a meso-scale weather forecast model (MM5, its performance and improvements for aerosol chemical and optical simulations have been evaluated using the observations data of aerosols/gases from the intensive observations and from the CMA Atmosphere Watch network, plus aerosol optical depth (AOD data from CMA Aerosol Remote Sensing network (CARSNET and from Moderate Resolution Imaging Spectroradiometer (MODIS. Targeting Beijing and North China region from July 13 to 31, 2008, when a heavy hazy weather system occurred, the model captured the general variations of PM10 with most of the data within a factor of 2 from the observations and a combined correlation coefficient (r of 0.38 (significance level=0.05. The correlation coefficients are better at rural than at urban sites, and better at daytime than at nighttime. Chemically, the correlation coefficients between the daily-averaged modelled and observed concentrations range from 0.34 for black carbon (BC to 0.09 for nitrates with sulphate, ammonium and organic carbon (OC in between. Like the PM10, the values of chemical species are higher for the daytime than those for the nighttime. On average, the sulphate, ammonium, nitrate and OC are underestimated by about 60, 70, 96.0 and 10.8%, respectively. Black carbon is overestimated by about 120%. A new size distribution for the primary particle emissions was constructed for most of the anthropogenic aerosols such as BC, OC, sulphate, nitrate and ammonium from the observed size distribution of atmospheric aerosols in Beijing. This not only improves the correlation between the modelled and observed AOD, but also reduces the overestimation of AOD simulated by the original model size

Aerosol Chemical Mass Closure during the EUROTRAC-2 AEROSOL Intercomparison 2000

Czech Academy of Sciences Publication Activity Database

Maenhaut, W.; Schwarz, Jaroslav; Cafmeyer, J.; Chi, X.

2002-01-01

Roč. 186, - (2002), s. 233-237 ISSN 0168-583X Institutional research plan: CEZ:AV0Z4072921 Keywords : ion chromatography * chemical composition * atmospheric aerosols Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 1.158, year: 2002

Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem

International Nuclear Information System (INIS)

Mazurek, M.A.; Cofer, W.R. III; Levine, J.S.

1991-01-01

Smoke aerosol and background aerosol particles were collected from the controlled burning of boreal forest where vegetation species and relative mass distributions are known. Chemical mass balances were constructed for the total mass of carbonaceous aerosol particles emitted during the prescribed burn. In addition, a carbonaceous species inventory was developed for aerosol particles presnt under background, smoldering, and full-fire conditions; the production of organic carbon and elemental carbon particles is noted for these two fire regimes. Distributions of the solvent-soluble organic components of the sampled aerosols were generated to identify molecular properties that can be traced to unburned and pyrolyzed materials present in the boreal forest fuels

Interacting effects of uniform flow, plane shear, and near-wall proximity on the heat and mass transfer of respiratory aerosols

Energy Technology Data Exchange (ETDEWEB)

Worth Longest, P. [Virginia Commonwealth University, Richmond, VA (United States). Dept. of Mechanical Engineering; Kleinstreuer, C. [North Carolina State University, Raleigh, NC (United States). Dept. of Mechanical and Aerospace Engineering

2004-10-01

Individual and interacting effects of uniform flow, plane shear, and near-wall proximity on spherical droplet heat and mass transfer have been assessed for low Reynolds number conditions beyond the creeping flow regime. Validated resolved volume simulations were used to compute heat and mass transfer surface gradients of two-dimensional axisymmetric droplets and three-dimensional spherical droplets near planar wall boundaries for conditions consistent with inhalable aerosols (5 {<=} d {<=} 300 {mu}m) in the upper respiratory tract. Results indicate that planar shear significantly impacts droplet heat and mass transfer for shear-based Reynolds numbers greater than 1, which occur for near-wall respiratory aerosols with diameters in excess of 50 {mu}m. Wall proximity is shown to significantly enhance heat and mass transfer due to conduction and diffusion at separation distances less than five particle diameters and for small Reynolds numbers. For the Reynolds number conditions of interest, significant non-linear effects arise due to the concurrent interaction of uniform flow and shear such that linear superposition of Sherwood or Nusselt number terms is not allowable. Based on the validated numeric simulations, multivariable Sherwood and Nusselt number correlations are provided to account for individual flow characteristics and concurrent non-linear interactions of uniform flow, planar shear, and near-wall proximity. These heat and mass transfer correlations can be applied to effectively compute condensation and evaporation rates of potentially toxic or therapeutic aerosols in the upper respiratory tract, where non-uniform flow and wall proximity are expected to significantly affect droplet transport, deposition, and vapor formation. (author)

Analyses of CsI aerosol deposition in aerosol behavior tests in WIND project

International Nuclear Information System (INIS)

Kudo, Tamotsu; Shibazaki, Hiroaki; Hidaka, Akihide

1999-01-01

The aerosol deposition tests have been performed in WIND project at JAERI to characterize the aerosol behavior. The aerosol deposition tests named WAV1-D and WAV2-D were analyzed by aerosol behavior analysis codes, JAERI's ART and SNL's VICTORIA. The comparison calculation was performed for the confirmation of the analytical capabilities of the both codes and improvement of the models in ART. The deposition mass calculated by ART was larger than that by VICTORIA. This discrepancy is caused by differences in model for FP vapor condensation onto the wall surface. In the WAV2-D test, in which boric acid was placed on the floor area of the test section prior to the deposition phase to simulate the PWR primary coolant, there was a discrepancy in deposition mass between analytical results in both codes and experimental results. The discrepancy may be caused by existence of boric acid which is not considered in the codes. (author)

Evaluation of chemical transport model predictions of primary organic aerosol for air masses classified by particle-component-based factor analysis

OpenAIRE

C. A. Stroud; M. D. Moran; P. A. Makar; S. Gong; W. Gong; J. Zhang; J. G. Slowik; J. P. D. Abbatt; G. Lu; J. R. Brook; C. Mihele; Q. Li; D. Sills; K. B. Strawbridge; M. L. McGuire

2012-01-01

Observations from the 2007 Border Air Quality and Meteorology Study (BAQS-Met 2007) in Southern Ontario, Canada, were used to evaluate predictions of primary organic aerosol (POA) and two other carbonaceous species, black carbon (BC) and carbon monoxide (CO), made for this summertime period by Environment Canada's AURAMS regional chemical transport model. Particle component-based factor analysis was applied to aerosol mass spectrometer measurements made at one urban site (Windsor, ON) and two...

Laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF: performance, reference spectra and classification of atmospheric samples

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X. Shen

2018-04-01

Full Text Available The laser ablation aerosol particle time-of-flight mass spectrometer (LAAPTOF, AeroMegt GmbH is able to identify the chemical composition and mixing state of individual aerosol particles, and thus is a tool for elucidating their impacts on human health, visibility, ecosystem, and climate. The overall detection efficiency (ODE of the instrument we use was determined to range from  ∼  (0.01 ± 0.01 to  ∼  (4.23 ± 2.36 % for polystyrene latex (PSL in the size range of 200 to 2000 nm,  ∼  (0.44 ± 0.19 to  ∼  (6.57 ± 2.38 % for ammonium nitrate (NH4NO3, and  ∼  (0.14 ± 0.02 to  ∼  (1.46 ± 0.08 % for sodium chloride (NaCl particles in the size range of 300 to 1000 nm. Reference mass spectra of 32 different particle types relevant for atmospheric aerosol (e.g. pure compounds NH4NO3, K2SO4, NaCl, oxalic acid, pinic acid, and pinonic acid; internal mixtures of e.g. salts, secondary organic aerosol, and metallic core–organic shell particles; more complex particles such as soot and dust particles were determined. Our results show that internally mixed aerosol particles can result in spectra with new clusters of ions, rather than simply a combination of the spectra from the single components. An exemplary 1-day ambient data set was analysed by both classical fuzzy clustering and a reference-spectra-based classification method. Resulting identified particle types were generally well correlated. We show how a combination of both methods can greatly improve the interpretation of single-particle data in field measurements.

Aerosol counterflow two-jets unit for continuous measurement of the soluble fraction of atmospheric aerosols.

Science.gov (United States)

Mikuska, Pavel; Vecera, Zbynek

2005-09-01

A new type of aerosol collector employing a liquid at laboratory temperature for continuous sampling of atmospheric particles is described. The collector operates on the principle of a Venturi scrubber. Sampled air flows at high linear velocity through two Venturi nozzles "atomizing" the liquid to form two jets of a polydisperse aerosol of fine droplets situated against each other. Counterflow jets of droplets collide, and within this process, the aerosol particles are captured into dispersed liquid. Under optimum conditions (air flow rate of 5 L/min and water flow rate of 2 mL/min), aerosol particles down to 0.3 microm in diameter are quantitatively collected in the collector into deionized water while the collection efficiency of smaller particles decreases. There is very little loss of fine aerosol within the aerosol counterflow two-jets unit (ACTJU). Coupling of the aerosol collector with an annular diffusion denuder located upstream of the collector ensures an artifact-free sampling of atmospheric aerosols. Operation of the ACTJU in combination with on-line detection devices allows in situ automated analysis of water-soluble aerosol species (e.g., NO2-, NO3-)with high time resolution (as high as 1 s). Under the optimum conditions, the limit of detection for particulate nitrite and nitrate is 28 and 77 ng/m(3), respectively. The instrument is sufficiently rugged for its application at routine monitoring of aerosol composition in the real time.

Method for characterization of low molecular weight organic acids in atmospheric aerosols using ion chromatography mass spectrometry.

Science.gov (United States)

Brent, Lacey C; Reiner, Jessica L; Dickerson, Russell R; Sander, Lane C

2014-08-05

The structural composition of PM2.5 monitored in the atmosphere is usually divided by the analysis of organic carbon, black (also called elemental) carbon, and inorganic salts. The characterization of the chemical composition of aerosols represents a significant challenge to analysts, and studies are frequently limited to determination of aerosol bulk properties. To better understand the potential health effects and combined interactions of components in aerosols, a variety of measurement techniques for individual analytes in PM2.5 need to be implemented. The method developed here for the measurement of organic acids achieves class separation of aliphatic monoacids, aliphatic diacids, aromatic acids, and polyacids. The selective ion monitoring capability of a triple quadropole mass analyzer was frequently capable of overcoming instances of incomplete separations. Standard Reference Material (SRM) 1649b Urban Dust was characterized; 34 organic acids were qualitatively identified, and 6 organic acids were quantified.

Aerosol composition and sources during the Chinese Spring Festival: fireworks, secondary aerosol, and holiday effects

Science.gov (United States)

Jiang, Q.; Sun, Y. L.; Wang, Z.; Yin, Y.

2015-06-01

Aerosol particles were characterized by an Aerodyne aerosol chemical speciation monitor along with various collocated instruments in Beijing, China, to investigate the role of fireworks (FW) and secondary aerosol in particulate pollution during the Chinese Spring Festival of 2013. Three FW events, exerting significant and short-term impacts on fine particles (PM2.5), were observed on the days of Lunar New Year, Lunar Fifth Day, and Lantern Festival. The FW were shown to have a large impact on non-refractory potassium, chloride, sulfate, and organics in submicron aerosol (PM1), of which FW organics appeared to be emitted mainly in secondary, with its mass spectrum resembling that of secondary organic aerosol (SOA). Pollution events (PEs) and clean periods (CPs) alternated routinely throughout the study. Secondary particulate matter (SPM = SOA + sulfate + nitrate + ammonium) dominated the total PM1 mass on average, accounting for 63-82% during nine PEs in this study. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM1 (6.4 m2 g-1) than during CPs (4.4 m2 g-1). The Chinese Spring Festival also provides a unique opportunity to study the impact of reduced anthropogenic emissions on aerosol chemistry in the city. Primary species showed ubiquitous reductions during the holiday period with the largest reduction being in cooking organic aerosol (OA; 69%), in nitrogen monoxide (54%), and in coal combustion OA (28%). Secondary sulfate, however, remained only slightly changed, and the SOA and the total PM2.5 even slightly increased. Our results have significant implications for controlling local primary source emissions during PEs, e.g., cooking and traffic activities. Controlling these factors might have a limited effect on improving air quality in the megacity of Beijing, due to the dominance of SPM from regional transport in aerosol particle composition.

Columnar aerosol optical and radiative properties according to season and air mass transport pattern over East Asia.

Science.gov (United States)

Noh, Young M; Müller, Detlef; Lee, Hanlim; Lee, Kwonho; Kim, Young Joon

2012-08-01

The column-integrated optical and radiative properties of aerosols in the downwind area of East Asia were investigated based on sun/sky radiometer measurements performed from February 2004 to June 2005 at Gwangju (35.23° N, 126.84° E) and Anmyeon (36.54° N, 126.33° E), Korea. The observed aerosol data were analyzed for differences among three seasons: spring (March-May), summer (June-August), and autumn/winter (September-February). The data were also categorized into five types depending on the air mass origin in arriving in the measurement sites: (a) from a northerly direction in spring (S(N)), (b) from a westerly direction in spring (S(W)), (c) cases with a low Ångström exponent (air mass origin. The forcing efficiency in summer was -131.7 and -125.6 W m(-2) at the surface in Gwangju and Anmyeon, respectively. These values are lower than those under the atmospheric conditions of spring and autumn/winter. The highest forcing efficiencies in autumn/winter were -214.3 and -255.9 W m(-2) at the surface in Gwangju and Anmyeon, respectively, when the air mass was transported from westerly directions.

Initial results with the Berkeley on-line mass separator-RAMA

International Nuclear Information System (INIS)

Cerny, J.; Moltz, D.M.; Evans, H.C.; Vieira, D.J.; Parry, R.F.; Wouters, J.M.; Gough, R.A.; Zisman, M.S.

1977-11-01

Initial performance is described for a reasonably fast and universal (having little or no chemical selectivity) on-line mass analysis system used to expand capabilities in studying nuclei far from stability. The system is termed RAMA, an acronym for Recoil Atom Mass Analyzer. Basically, this system utilizes the helium-jet method to transport activity to a Sidenius hollow-cathode ion source which is coupled to a mass spectrometer. Initial experiments and planned improvements are discussed. Transport efficiencies of between 10 and 60 percent have routinely been achieved, though the latter is much more typical when conditions are optimized

Evolution of size-segregated aerosol mass concentration during the Antarctic summer at Northern Foothills, Victoria Land

Science.gov (United States)

Illuminati, Silvia; Bau, Sébastien; Annibaldi, Anna; Mantini, Caterina; Libani, Giulia; Truzzi, Cristina; Scarponi, Giuseppe

2016-01-01

Within the framework of the Italian National Programm for Antarctic Research (PNRA), the first direct gravimetric measurements of size-segregated aerosol fractions were carried out at Faraglione Camp, ˜3-km far from the Italian station "M. Zucchelli" (Terra Nova Bay, Ross Sea), during the 2014-2015 austral summer. A six-stage high-volume cascade impactor with size classes between 10 μm and 0.49 μm, and, in parallel, for comparison purposes, a PM10 high-volume sampler (50% cut-off aerodynamic diameter of 10 μm) were used. A 10-day sampling strategy was adopted. Aerosol mass measurements were carried out before and after exposure by using a microbalance specifically designed for the filter weight and placed inside a glove bag in order to maintain stable temperature and humidity conditions during weighing sessions. Measured atmospheric concentrations (referred to the "actual air conditions" of mean temperature of 268 K and mean pressure of 975 hPa) of size-segregated aerosol fractions showed the following values, given as size range, means (interquartile range): Dp range 0.1-1.0 μm) and two coarse modes (CM1 in the range 1.0-3.0 μm, and CM2 in the range 3.0-10 μm). From 50% to 90% of the PM10 mass comes from particles of a size smaller than 1.0 μm. The two coarse modes represented from ˜5% to ˜35% of the PM10, showing opposite seasonal trends (CM1 decreased while CM2 increased). During summer, PM10 mass concentration increased to a maximum of ˜1.6 μg m-3 at mid-December, while in January it decreased to values that are typical of November. Both accumulation and upper super-micron fractions showed a maximum in the same period contributing to the PM10 peak of mid-summer.

Glyoxal contribution to aerosols over Los Angeles

Science.gov (United States)

Balcerak, Ernie

2012-01-01

Laboratory and field studies have indicated that glyoxal (chemical formula OCHCHO), an atmospheric oxidation product of isoprene and aromatic compounds, may contribute to secondary organic aerosols in the atmosphere, which can block sunlight and affect atmospheric chemistry. Some aerosols are primary aerosols, emitted directly into the atmosphere, while others are secondary, formed through chemical reactions in the atmosphere. Washenfelder et al. describe in situ glyoxal measurements from Pasadena, Calif., near Los Angeles, made during summer 2010. They used three different methods to calculate the contribution of glyoxal to secondary atmospheric aerosol and found that it is responsible for 0-0.2 microgram per cubic meter, or 0-4%, of the secondary organic aerosol mass. The researchers also compared their results to those of a previous study that calculated the glyoxal contribution to aerosol for Mexico City. Mexico City had higher levels of organic aerosol mass from glyoxal. They suggest that the lower contribution of glyoxal to aerosol concentrations for Los Angeles may be due to differences in the composition or water content of the aerosols above the two cities. (Journal of Geophysical Research-Atmospheres, doi:10.1029/2011JD016314, 2011)

Aerosol Observing System (AOS) Handbook

Energy Technology Data Exchange (ETDEWEB)

Jefferson, A

2011-01-17

The Aerosol Observing System (AOS) is a suite of in situ surface measurements of aerosol optical and cloud-forming properties. The instruments measure aerosol properties that influence the earth’s radiative balance. The primary optical measurements are those of the aerosol scattering and absorption coefficients as a function of particle size and radiation wavelength and cloud condensation nuclei (CCN) measurements as a function of percent supersaturation. Additional measurements include those of the particle number concentration and scattering hygroscopic growth. Aerosol optical measurements are useful for calculating parameters used in radiative forcing calculations such as the aerosol single-scattering albedo, asymmetry parameter, mass scattering efficiency, and hygroscopic growth. CCN measurements are important in cloud microphysical models to predict droplet formation.

Variability of Atmospheric Radon-222 and Secondary Aerosol Components in Accordance with Air Mass Transport Pathways at Jeju Island, Korea, during 2011-2014

International Nuclear Information System (INIS)

Bu, Jun-Oh; Song, Jung-Min; Kim, Won-Hyung; Kang, Chang-Hee; Chambers, Scott D.; Williams, Alastair G.; Lee, Chulkyu

2016-01-01

Real-time monitoring of hourly atmospheric Radon-222 concentration and three daily monitoring of the secondary aerosol components of PM_1_0 were performed throughout 2011-2014 at Gosan station, Jeju Island, in order to characterize their background levels and temporal variation. The annual mean radon and PM_1_0 mass concentrations were 2326 ± 1198 mBq/m"3 and 37.1 ± 19.5 μg/m"3, respectively. Based on cluster analyses of air mass back trajectories, the frequencies of air masses originating from continental China, the Korean Peninsula, and North Pacific Ocean routes were 53, 28, and 19%, respectively. When the air masses were transported to Jeju Island from continental China, the concentrations of radon and secondary aerosol components (nss-SO_4"2"-, NO_3"-, NH_4"+) were relatively high: 2577 mBq/m"3 and 14.4 μg/m"3, respectively. In cases when the air masses have moved from the Korean Peninsula, the corresponding concentrations were 2247 mBq/m"3 and 11.4 μg/m"3, respectively. On the other hand, when the air masses came from the North Pacific Ocean, their radon and secondary aerosol concentrations decreased much further, 1372 mBq/m"3 and 10.5 μg/m"3, respectively. Consequently, the variability of atmospheric radon concentrations at Gosan station might be characterized by synoptic changes in air mass fetch as well as diurnal changes in atmospheric mixing depth.

Applicability of a two-step laser desorption-ionization aerosol time-of-flight mass spectrometer for determination of chemical composition of ultrafine aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Laitinen, T.

2013-11-01

This thesis is based on the construction of a two-step laser desorption-ionization aerosol time-of-flight mass spectrometer (laser AMS), which is capable of measuring 10 to 50 nm aerosol particles collected from urban and rural air at-site and in near real time. The operation and applicability of the instrument was tested with various laboratory measurements, including parallel measurements with filter collection/chromatographic analysis, and then in field experiments in urban environment and boreal forest. Ambient ultrafine aerosol particles are collected on a metal surface by electrostatic precipitation and introduced to the time-of-flight mass spectrometer (TOF-MS) with a sampling valve. Before MS analysis particles are desorbed from the sampling surface with an infrared laser and ionized with a UV laser. The formed ions are guided to the TOF-MS by ion transfer optics, separated according to their m/z ratios, and detected with a micro channel plate detector. The laser AMS was used in urban air studies to quantify the carbon cluster content in 50 nm aerosol particles. Standards for the study were produced from 50 nm graphite particles, suspended in toluene, with 72 hours of high power sonication. The results showed the average amount of carbon clusters (winter 2012, Helsinki, Finland) in 50 nm particles to be 7.2% per sample. Several fullerenes/fullerene fragments were detected during the measurements. In boreal forest measurements, the laser AMS was capable of detecting several different organic species in 10 to 50 nm particles. These included nitrogen-containing compounds, carbon clusters, aromatics, aliphatic hydrocarbons, and oxygenated hydrocarbons. A most interesting event occurred during the boreal forest measurements in spring 2011 when the chemistry of the atmosphere clearly changed during snow melt. On that time concentrations of laser AMS ions m/z 143 and 185 (10 nm particles) increased dramatically. Exactly at the same time, quinoline concentrations

Can Condensing Organic Aerosols Lead to Less Cloud Particles?

Science.gov (United States)

Gao, C. Y.; Tsigaridis, K.; Bauer, S.

2017-12-01

We examined the impact of condensing organic aerosols on activated cloud number concentration in a new aerosol microphysics box model, MATRIX-VBS. The model includes the volatility-basis set (VBS) framework in an aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) that resolves aerosol mass and number concentrations and aerosol mixing state. Preliminary results show that by including the condensation of organic aerosols, the new model (MATRIX-VBS) has less activated particles compared to the original model (MATRIX), which treats organic aerosols as non-volatile. Parameters such as aerosol chemical composition, mass and number concentrations, and particle sizes which affect activated cloud number concentration are thoroughly evaluated via a suite of Monte-Carlo simulations. The Monte-Carlo simulations also provide information on which climate-relevant parameters play a critical role in the aerosol evolution in the atmosphere. This study also helps simplifying the newly developed box model which will soon be implemented in the global model GISS ModelE as a module.

A new broadly tunable (7.4-10.2 eV) laser based VUV light source and its first application to aerosol mass spectrometry

Science.gov (United States)

Hanna, S. J.; Campuzano-Jost, P.; Simpson, E. A.; Robb, D. B.; Burak, I.; Blades, M. W.; Hepburn, J. W.; Bertram, A. K.

2009-01-01

A laser based vacuum ultraviolet (VUV) light source using resonance enhanced four wave difference mixing in xenon gas was developed for near threshold ionization of organics in atmospheric aerosol particles. The source delivers high intensity pulses of VUV light (in the range of 1010 to 1013 photons/pulse depending on wavelength, 5 ns FWHM) with a continuously tunable wavelength from 122 nm (10.2 eV) to 168 nm (7.4 eV)E The setup allows for tight (caffeine aerosols vaporized by a pulsed CO2 laser in an ion trap mass spectrometer. Mass spectra from single particles down to 300 nm in diameter were collected. Excellent signal to noise characteristics for these small particles give a caffeine detection limit of 8 × 105 molecules which is equivalent to a single 75 nm aerosol, or approximately 1.5% of a 300 nm particleE The appearance energy of caffeine originating from the aerosol was also measured and found to be 7.91 ± 0.05 eV, in good agreement with literature values.

Anthropogenic contribution to cloud condensation nuclei and the first aerosol indirect climate effect

International Nuclear Information System (INIS)

Yu Fangqun; Ma Xiaoyan; Luo Gan

2013-01-01

Atmospheric particles influence the climate indirectly by acting as cloud condensation nuclei (CCN). The first aerosol indirect radiative forcing (FAIRF) constitutes the largest uncertainty among the radiative forcings quantified by the latest IPCC report (IPCC2007) and is a major source of uncertainty in predicting climate change. Here, we investigate the anthropogenic contribution to CCN and associated FAIRF using a state-of-the-art global chemical transport and aerosol model (GEOS-Chem/APM) that contains a number of advanced features (including sectional particle microphysics, online comprehensive chemistry, consideration of all major aerosol species, online aerosol–cloud–radiation calculation, and usage of more accurate assimilated meteorology). The model captures the absolute values and spatial distributions of CCN concentrations measured in situ around the globe. We show that anthropogenic emissions increase the global mean CCN in the lower troposphere by ∼60–80% and cloud droplet number concentration by ∼40%. The global mean FAIRF based on GEOS-Chem/APM is −0.75 W m −2 , close to the median values of both IPCC2007 and post-IPCC2007 studies. To the best of our knowledge, this is the first time that a global sectional aerosol model with full online chemistry and considering all major aerosol species (including nitrate, ammonium, and second organic aerosols) has been used used to calculate FAIRF. (letter)

Rural continental aerosol properties and processes observed during the Hohenpeissenberg Aerosol Characterization Experiment (HAZE2002

Directory of Open Access Journals (Sweden)

N. Hock

2008-02-01

Full Text Available Detailed investigations of the chemical and microphysical properties of rural continental aerosols were performed during the HAZE2002 experiment, which was conducted in May 2002 at the Meteorological Observatory Hohenpeissenberg (DWD in Southern Germany.

Online measurements included: Size-resolved chemical composition of submicron particles; total particle number concentrations and size distributions over the diameter range of 3 nm to 9 μm; gas-phase concentration of monoterpenes, CO, O₃, OH, and H₂SO₄. Filter sampling and offline analytical techniques were used to determine: Fine particle mass (PM2.5, organic, elemental and total carbon in PM2.5 (OC2.5, EC2.5, TC2.5, and selected organic compounds (dicarboxylic acids, polycyclic aromatic hydrocarbons, proteins.

Overall, the non-refractory components of submicron particles detected by aerosol mass spectrometry (PM1, 6.6±5.4 μg m⁻³, arithmetic mean and standard deviation accounted for ~62% of PM2.5 determined by filter gravimetry (10.6±4.7 μg m⁻³. The relative proportions of non-refractory submicron particle components were: (23±39% ammonium nitrate, (27±23% ammonium sulfate, and (50±40% organics (OM1. OM1 was closely correlated with PM1 (r²=0.9 indicating a near-constant ratio of non-refractory organics and inorganics.

The average ratio of OM1 to OC2.5 was 2.1±1.4, indicating a high proportion of heteroelements in the organic fraction of the sampled rural aerosol. This is consistent with the high ratio of oxygenated organic aerosol (OOA over hydrocarbon-like organic aerosol (HOA inferred from the AMS results (4:1, and also with the high abundance of proteins (~3% indicating a high proportion of primary biological material (~30% in PM2.5. This finding was confirmed by low abundance of PAHs (<1 ng m⁻³ and EC (<1 μg m⁻³ in PM2.5 and detection of several

Fourteen months of on-line measurements of the non-refractory submicron aerosol at the Jungfraujoch (3580 m a.s.l.) - chemical composition, origins and organic aerosol sources

Science.gov (United States)

Fröhlich, R.; Cubison, M. J.; Slowik, J. G.; Bukowiecki, N.; Canonaco, F.; Croteau, P. L.; Gysel, M.; Henne, S.; Herrmann, E.; Jayne, J. T.; Steinbacher, M.; Worsnop, D. R.; Baltensperger, U.; Prévôt, A. S. H.

2015-10-01

Chemically resolved (organic, nitrate, sulfate, ammonium) data of non-refractory submicron (NR-PM1) aerosol from the first long-term deployment (27 July 2012 to 02 October 2013) of a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) at the Swiss high-altitude site Jungfraujoch (JFJ; 3580 m a.s.l.) are presented. Besides total mass loadings, diurnal variations and relative species contributions during the different meteorological seasons, geographical origin and sources of organic aerosol (OA) are discussed. Backward transport simulations show that the highest (especially sulfate) concentrations of NR-PM1 were measured in air masses advected to the station from regions south of the JFJ, while lowest concentrations were seen from western regions. OA source apportionment for each season was performed using the Source Finder (SoFi) interface for the multilinear engine (ME-2). OA was dominated in all seasons by oxygenated OA (OOA, 71-88 %), with lesser contributions from local tourism-related activities (7-12 %) and hydrocarbon-like OA related to regional vertical transport (3-9 %). In summer the OOA can be separated into a background low-volatility OA (LV-OOA I, possibly associated with long-range transport) and a slightly less oxidised low-volatility OA (LV-OOA II) associated with regional vertical transport. Wood burning-related OA associated with regional transport was detected during the whole winter 2012/2013 and during rare events in summer 2013, in the latter case attributed to small-scale transport for the surrounding valleys. Additionally, the data were divided into periods with free tropospheric (FT) conditions and periods with planetary boundary layer (PBL) influence, enabling the assessment of the composition for each. Most nitrate and part of the OA are injected from the regional PBL, while sulfate is mainly produced in the FT. The south/north gradient of sulfate is also pronounced in FT air masses (sulfate mass fraction from the south: 45

The Potential of The Synergy of Sunphotometer and Lidar Data to Validate Vertical Profiles of The Aerosol Mass Concentration Estimated by An Air Quality Model

Directory of Open Access Journals (Sweden)

Siomos N.

2016-01-01

Full Text Available Vertical profiles of the aerosol mass concentration derived by the Lidar/Radiometer Inversion Code (LIRIC, that uses combined sunphotometer and lidar data, were used in order to validate the aerosol mass concentration profiles estimated by the air quality model CAMx. Lidar and CIMEL measurements performed at the Laboratory of Atmospheric Physics of the Aristotle University of Thessaloniki, Greece (40.5N, 22.9E from the period 2013-2014 were used in this study.

Influence of moisture on the behavior of aerosols

International Nuclear Information System (INIS)

Adams, R.E.; Longest, A.W.; Tobias, M.L.

1987-01-01

The behavior of aerosols assumed to be characteristic of those generated during light water reactor accident sequences and released into containment has been studied in the Nuclear Safety Pilot Plant located at the Oak Ridge National Laboratory. It has been observed that in a saturated steam-air environment a change occurs in the shape of aerosol agglomerates of U 3 O 8 aerosol, Fe 2 O 3 aerosol, and mixed U 3 O 8 -Fe 2 O 3 aerosol from branched-chain to spherical, and that the rate of reduction in the airborne aerosol mass concentration is increased relative to the rate observed in a dry atmosphere. The effect of a steam-air environment on the behavior of concrete aerosol is different. The shape of the agglomerated concrete aerosol is intermediate between branched-chain and spherical and the effect on the rate of reduction in airborne mass concentration appears to be slight. In a related project the shape of an agglomerated Fe 2 O 3 aerosol was observed to change from branched-chain to spherical at, or near, 100% relative humidity

Steps Toward an EOS-Era Aerosol Air Mass Type Climatology

Science.gov (United States)

Kahn, Ralph A.

2012-01-01

We still have a way to go to develop a global climatology of aerosol type from the EOS-era satellite data record that currently spans more than 12 years of observations. We have demonstrated the ability to retrieve aerosol type regionally, providing a classification based on the combined constraints on particle size, shape, and single-scattering albedo (SSA) from the MISR instrument. Under good but not necessarily ideal conditions, the MISR data can distinguish three-to-five size bins, two-to-four bins in SSA, and spherical vs. non-spherical particles. However, retrieval sensitivity varies enormously with scene conditions. So, for example, there is less information about aerosol type when the mid-visible aerosol optical depth (AOD) is less that about 0.15 or 0.2.

Resolving the Aerosol Piece of the Global Climate Picture

Science.gov (United States)

Kahn, R. A.

2017-12-01

Factors affecting our ability to calculate climate forcing and estimate model predictive skill include direct radiative effects of aerosols and their indirect effects on clouds. Several decades of Earth-observing satellite observations have produced a global aerosol column-amount (AOD) record, but an aerosol microphysical property record required for climate and many air quality applications is lacking. Surface-based photometers offer qualitative aerosol-type classification, and several space-based instruments map aerosol air-mass types under favorable conditions. However, aerosol hygroscopicity, mass extinction efficiency (MEE), and quantitative light absorption, must be obtained from in situ measurements. Completing the aerosol piece of the climate picture requires three elements: (1) continuing global AOD and qualitative type mapping from space-based, multi-angle imagers and aerosol vertical distribution from near-source stereo imaging and downwind lidar, (2) systematic, quantitative in situ observations of particle properties unobtainable from space, and (3) continuing transport modeling to connect observations to sources, and extrapolate limited sampling in space and time. At present, the biggest challenges to producing the needed aerosol data record are: filling gaps in particle property observations, maintaining global observing capabilities, and putting the pieces together. Obtaining the PDFs of key particle properties, adequately sampled, is now the leading observational deficiency. One simplifying factor is that, for a given aerosol source and season, aerosol amounts often vary, but particle properties tend to be repeatable. SAM-CAAM (Systematic Aircraft Measurements to Characterize Aerosol Air Masses), a modest aircraft payload deployed frequently could fill this gap, adding value to the entire satellite data record, improving aerosol property assumptions in retrieval algorithms, and providing MEEs to translate between remote-sensing optical constraints

Cluster Analysis of the Organic Peaks in Bulk Mass Spectra Obtained During the 2002 New England Air Quality Study with an Aerodyne Aerosol Mass Spectrometer

Science.gov (United States)

Marcolli, C.; Canagaratna, M. R.; Worsnop, D. R.; Bahreini, R.; de Gouw, J. A.; Warneke, C.; Goldan, P. D.; Kuster, W. C.; Williams, E. J.; Lerner, B. M.; Roberts, J. M.; Meagher, J. F.; Fehsenfeld, F. C.; Marchewka, M.; Bertman, S. B.; Middlebrook, A. M.

2006-12-01

We applied hierarchical cluster analysis to an Aerodyne aerosol mass spectrometer (AMS) bulk mass spectral dataset collected aboard the NOAA research vessel R. H. Brown during the 2002 New England Air Quality Study off the east coast of the United States. Emphasizing the organic peaks, the cluster analysis yielded a series of categories that are distinguishable with respect to their mass spectra and their occurrence as a function of time. The differences between the categories mainly arise from relative intensity changes rather than from the presence or absence of specific peaks. The most frequent category exhibits a strong signal at m/z 44 and represents oxidized organic matter probably originating from both anthropogenic as well as biogenic sources. On the basis of spectral and trace gas correlations, the second most common category with strong signals at m/z 29, 43, and 44 contains contributions from isoprene oxidation products. The third through the fifth most common categories have peak patterns characteristic of monoterpene oxidation products and were most frequently observed when air masses from monoterpene rich regions were sampled. Taken together, the second through the fifth most common categories represent on average 17% of the total organic mass that stems likely from biogenic sources during the ship's cruise. These numbers have to be viewed as lower limits since the most common category was attributed to anthropogenic sources for this calculation. The cluster analysis was also very effective in identifying a few contaminated mass spectra that were not removed during pre-processing. This study demonstrates that hierarchical clustering is a useful tool to analyze the complex patterns of the organic peaks in bulk aerosol mass spectra from a field study.

Online-coupled meteorology and chemistry models: history, current status, and outlook

Directory of Open Access Journals (Sweden)

Y. Zhang

2008-06-01

Full Text Available The climate-chemistry-aerosol-cloud-radiation feedbacks are important processes occurring in the atmosphere. Accurately simulating those feedbacks requires fully-coupled meteorology, climate, and chemistry models and presents significant challenges in terms of both scientific understanding and computational demand. This paper reviews the history and current status of the development and application of online-coupled meteorology and chemistry models, with a focus on five representative models developed in the US including GATOR-GCMOM, WRF/Chem, CAM3, MIRAGE, and Caltech unified GCM. These models represent the current status and/or the state-of-the science treatments of online-coupled models worldwide. Their major model features, typical applications, and physical/chemical treatments are compared with a focus on model treatments of aerosol and cloud microphysics and aerosol-cloud interactions. Aerosol feedbacks to planetary boundary layer meteorology and aerosol indirect effects are illustrated with case studies for some of these models. Future research needs for model development, improvement, application, as well as major challenges for online-coupled models are discussed.

Aerodynamics, heat and mass transfer in steam-aerosol turbulent flows in containment

Energy Technology Data Exchange (ETDEWEB)

Nigmatulin, B.I.; Pershukov, V.A.; Ris, V.V. [Research & Engineering Centre of Nuclear Plants Safety, Moscow (Russian Federation)] [and others

1995-09-01

In this report an analysis of aerodynamic and heat transfer processes at the blowdown of gas-dispersed mixture into the containment volume is presented. A few models for description of the volume averaged and local characteristics are analyzed. The mathematical model for description of the local characteristics of the turbulent gas-dispersed flows was developed. The calculation of aerodynamic, heat and mass transfer characteristics was based on the Navier-Stokes, energy and gas mass fractions conservation equations. For calculation of dynamics and deposition of the aerosols the original diffusion-inertia model is developed. The pulsating characteristics of the gaseous phase were calculated on the base (k-{xi}) model of turbulence with modification to account thermogravitational force action and influence of particle mass loading. The appropriate boundary conditions using the {open_quotes}near-wall function{close_quotes} approach was obtained. Testing of the mathematical models and boundary conditions has shown a good agreement between computation and data of comparison. The described mathematical models were applied to two- and three dimensional calculations of the turbulent flow in containment at the various stages of the accident.

Two-Step Single Particle Mass Spectrometry for On-Line Monitoring of Polycyclic Aromatic Hydrocarbons Bound to Ambient Fine Particulate Matter

Science.gov (United States)

Zimmermann, R.; Bente, M.; Sklorz, M.

2007-12-01

Polycyclic aromatic hydrocarbons (PAH) are formed as trace products in combustion processes and are emitted to the atmosphere. Larger PAH have low vapour pressure and are predominantly bound to the ambient fine particulate matter (PM). Upon inhalation, PAH show both, chronic human toxicity (i.e. many PAH are potent carcinogens) as well as acute human toxicity (i.e. inflammatory effects due to oxi-dative stress) and are discussed to be relevant for the observed health effect of ambient PM. Therefore a better understanding of the occurrence, dynamics and particle size dependence of particle bound-PAH is of great interest. On-line aerosol mass spectrometry in principle is the method of choice to investigate the size resolved changes in the chemical speciation of particles as well the status of internal vs. external mixing of chemical constituents. However the present available aerosol mass spectrometers (ATOFMS and AMS) do not allow detection of PAH from ambient air PM. In order to allow a single particle based monitoring of PAH from ambient PM a new single particle laser ionisation mass spectrometer was built and applied. The system is based on ATOFMS principle but uses a two- step photo-ionization. A tracked and sized particle firstly is laser desorbed (LD) by a IR-laser pulse (CO2-laser, λ=10.2 μm) and subsequently the released PAH are selectively ionized by an intense UV-laser pulse (ArF excimer, λ=248 nm) in a resonance enhanced multiphoton ionisation process (REMPI). The PAH-ions are detected in a time of flight mass spectrometer (TOFMS). A virtual impactor enrichment unit is used to increase the detection frequency of the ambient particles. With the current inlet system particles from about 400 nm to 10 μm are accessible. Single particle based temporal profiles of PAH containing particles ion (size distribution and PAH speciation) have been recorded in Oberschleissheim, Germany from ambient air. Furthermore profiles of relevant emission sources (e

Single particle characterization using a light scattering module coupled to a time-of-flight aerosol mass spectrometer

Science.gov (United States)

Cross, E. S.; Onasch, T. B.; Canagaratna, M.; Jayne, J. T.; Kimmel, J.; Yu, X.-Y.; Alexander, M. L.; Worsnop, D. R.; Davidovits, P.

2008-12-01

We present the first single particle results obtained using an Aerodyne time-of-flight aerosol mass spectrometer coupled with a light scattering module (LS-ToF-AMS). The instrument was deployed at the T1 ground site approximately 40 km northeast of the Mexico City Metropolitan Area (MCMA) as part of the MILAGRO field study in March of 2006. The instrument was operated as a standard AMS from 12-30 March, acquiring average chemical composition and size distributions for the ambient aerosol, and in single particle mode from 27-30 March. Over a 75-h sampling period, 12 853 single particle mass spectra were optically triggered, saved, and analyzed. The correlated optical and chemical detection allowed detailed examination of single particle collection and quantification within the LS-ToF-AMS. The single particle data enabled the mixing states of the ambient aerosol to be characterized within the context of the size-resolved ensemble chemical information. The particulate mixing states were examined as a function of sampling time and most of the particles were found to be internal mixtures containing many of the organic and inorganic species identified in the ensemble analysis. The single particle mass spectra were deconvolved, using techniques developed for ensemble AMS data analysis, into HOA, OOA, NH4NO3, (NH4)2SO4, and NH4Cl fractions. Average single particle mass and chemistry measurements are shown to be in agreement with ensemble MS and PTOF measurements. While a significant fraction of ambient particles were internal mixtures of varying degrees, single particle measurements of chemical composition allowed the identification of time periods during which the ambient ensemble was externally mixed. In some cases the chemical composition of the particles suggested a likely source. Throughout the full sampling period, the ambient ensemble was an external mixture of combustion-generated HOA particles from local sources (e.g. traffic), with number concentrations peaking

On-line mass spectometry of nuclear reactions induced by heavy ions

International Nuclear Information System (INIS)

Saint Simon, M. de.

1977-01-01

The adaptation of the on-line mass-spectrometric technique to the special conditions of heavy ion induced reactions is described. The method is very selective about A and Z, even for the very heavy reaction products in counterpart of the limitation of its applications to the alkaline elements only. This method is used in order to study the effects of angular momentum brought by the projectile in the complete fusion process and in the following neutron evaporation. The analysis of excitation functions shows that the increase in mass of the projectile has not always the effect of increasing the rotation energy of the compound nucleus. The on-line mass spectrometry has allowed to study heavy ion induced fission. Measurements of complementary isotopic distributions of fission products make it possible to explain that the total number of neutrons emitted per fission can be always deduced from the fragment excitation energy. The study of the isotope distribution variance shows that the statistical model for fission is in good agreement with experimental results after taking into account the non-fusion processes [fr

Characterization of biomass burning aerosols produced in the laboratory with a light-scattering aerosol mass spectrometer

Science.gov (United States)

Middlebrook, A. M.; Adler, G. A.; Coggon, M.; De Gouw, J. A.; Franchin, A.; Gilman, J.; Koss, A.; Krechmer, J. E.; Lamb, K.; Manfred, K.; Roberts, J. M.; Schwarz, J. P.; Sekimoto, K.; Selimovic, V.; Stockwell, C.; Wagner, N.; Warneke, C.; Washenfelder, R. A.; Womack, C.; Yokelson, R. J.; Yuan, B.

2017-12-01

During the 2016 NOAA FIREX project at the Missoula Fire Sciences Laboratory, small fires of known fuel type and properties were ignited to characterize their direct emissions with a large variety of new sampling methods. Two types of experiments were employed: sampling smoke directly from the exhaust stack throughout the lifecycle of the fires (stack burns) or sampling when the exhaust vent was closed to fill the room with smoke (room burns). For both types of burns, photo-oxidation chambers were at times used to mimic aging in the atmosphere. During all these experiments, we measured the non-refractory components of the smoke particles using an Aerodyne compact time-of-flight aerosol mass spectrometer (AMS) with a light scattering module and diluted the sample line as little as possible (usually by a factor of 10) without overwhelming our instrument. For the stack burns, our AMS was placed near the top of the exhaust stack to capture the composition and size distribution during the rapidly changing stages of the fires. We found that the chemical composition of the aerosols varied with fuel type and combustion conditions on time scales of a few minutes as the fuels went through different stages of heating and combustion. For the room burns, we obtained additional measurements with the light-scattering module aimed at understanding how well smoke particles are measured with the AMS, along with characterization of their physical properties. We will present a summary of our results, with connections to their relevance for constraining model treatments of fire emissions on the atmosphere.

Desorption atmospheric pressure photoionization high-resolution mass spectrometry: a complementary approach for the chemical analysis of atmospheric aerosols

Czech Academy of Sciences Publication Activity Database

Parshintsev, J.; Vaikkinen, A.; Lipponen, K.; Vrkoslav, Vladimír; Cvačka, Josef; Kostiainen, R.; Kotiaho, T.; Hartonen, K.; Riekkola, M. L.; Kauppila, T. J.

2015-01-01

Roč. 29, č. 13 (2015), s. 1233-1241 ISSN 0951-4198 Grant - others:GA AV ČR(CZ) M200551204 Institutional support: RVO:61388963 Keywords : atmospheric aerosols * mass spectrometry * ambient ionization Subject RIV: CB - Analytical Chemistry , Separation Impact factor: 2.226, year: 2015

Simultaneous aerosol mass spectrometry and chemical ionisation mass spectrometry measurements during a biomass burning event in the UK: insights into nitrate chemistry

Directory of Open Access Journals (Sweden)

E. Reyes-Villegas

2018-03-01

Full Text Available Over the past decade, there has been an increasing interest in short-term events that negatively affect air quality such as bonfires and fireworks. High aerosol and gas concentrations generated from public bonfires or fireworks were measured in order to understand the night-time chemical processes and their atmospheric implications. Nitrogen chemistry was observed during Bonfire Night with nitrogen containing compounds in both gas and aerosol phases and further N2O5 and ClNO2 concentrations, which depleted early next morning due to photolysis of NO3 radicals and ceasing production. Particulate organic oxides of nitrogen (PONs concentrations of 2.8 µg m−3 were estimated using the m ∕ z 46 : 30 ratios from aerosol mass spectrometer (AMS measurements, according to previously published methods. Multilinear engine 2 (ME-2 source apportionment was performed to determine organic aerosol (OA concentrations from different sources after modifying the fragmentation table and it was possible to identify two PON factors representing primary (pPON_ME2 and secondary (sPON_ME2 contributions. A slight improvement in the agreement between the source apportionment of the AMS and a collocated AE-31 Aethalometer was observed after modifying the prescribed fragmentation in the AMS organic spectrum (the fragmentation table to determine PON sources, which resulted in an r2 =  0.894 between biomass burning organic aerosol (BBOA and babs_470wb compared to an r2 =  0.861 obtained without the modification. Correlations between OA sources and measurements made using time-of-flight chemical ionisation mass spectrometry with an iodide adduct ion were performed in order to determine possible gas tracers to be used in future ME-2 analyses to constrain solutions. During Bonfire Night, strong correlations (r2 were observed between BBOA and methacrylic acid (0.92, acrylic acid (0.90, nitrous acid (0.86, propionic acid, (0.85 and hydrogen cyanide (0

Simultaneous aerosol mass spectrometry and chemical ionisation mass spectrometry measurements during a biomass burning event in the UK: insights into nitrate chemistry

Science.gov (United States)

Reyes-Villegas, Ernesto; Priestley, Michael; Ting, Yu-Chieh; Haslett, Sophie; Bannan, Thomas; Le Breton, Michael; Williams, Paul I.; Bacak, Asan; Flynn, Michael J.; Coe, Hugh; Percival, Carl; Allan, James D.

2018-03-01

Over the past decade, there has been an increasing interest in short-term events that negatively affect air quality such as bonfires and fireworks. High aerosol and gas concentrations generated from public bonfires or fireworks were measured in order to understand the night-time chemical processes and their atmospheric implications. Nitrogen chemistry was observed during Bonfire Night with nitrogen containing compounds in both gas and aerosol phases and further N2O5 and ClNO2 concentrations, which depleted early next morning due to photolysis of NO3 radicals and ceasing production. Particulate organic oxides of nitrogen (PONs) concentrations of 2.8 µg m-3 were estimated using the m / z 46 : 30 ratios from aerosol mass spectrometer (AMS) measurements, according to previously published methods. Multilinear engine 2 (ME-2) source apportionment was performed to determine organic aerosol (OA) concentrations from different sources after modifying the fragmentation table and it was possible to identify two PON factors representing primary (pPON_ME2) and secondary (sPON_ME2) contributions. A slight improvement in the agreement between the source apportionment of the AMS and a collocated AE-31 Aethalometer was observed after modifying the prescribed fragmentation in the AMS organic spectrum (the fragmentation table) to determine PON sources, which resulted in an r2 = 0.894 between biomass burning organic aerosol (BBOA) and babs_470wb compared to an r2 = 0.861 obtained without the modification. Correlations between OA sources and measurements made using time-of-flight chemical ionisation mass spectrometry with an iodide adduct ion were performed in order to determine possible gas tracers to be used in future ME-2 analyses to constrain solutions. During Bonfire Night, strong correlations (r2) were observed between BBOA and methacrylic acid (0.92), acrylic acid (0.90), nitrous acid (0.86), propionic acid, (0.85) and hydrogen cyanide (0.76). A series of oxygenated species

Determination of low-molecular-weight dicarboxylic acids in atmospheric aerosols by injection-port derivatization and gas chromatography-mass spectrometry

Science.gov (United States)

Ding, W.; Hsu, C.

2008-12-01

Currently, the investigations on aerosol water-soluble organic compounds (WSOCs) formed by burning biomass have become increasingly concerned with the role of these compounds in atmospheric chemistry and their effect on climate, because they have great potential to influence cloud formation, precipitation, and climate on both global and regional scales. Of these compounds, low-molecular weight (LMW) dicarboxylic acids (from C2 to C10) have attracted the most interest because of their properties as specific tracers for the burning of biomass. In this study, a modified injection-port derivatization and gas chromatography - mass spectrometry method was developed and evaluated for rapid determination of LMW dicarboxylic acids in atmospheric aerosol samples. The parameters related to the derivatization process (i.e., type of ion-pair reagent, injection-port temperature and concentration of ion-pair reagent) were optimized. Tetrabutylammonium hydroxide (TBA-OH) dissolved in methanol used as the ion-pair solution gave excellent yield for di-butyl ester low-molecular weight derivatives. Solid-phase extraction method instead of rotary evaporation was used to concentrate analytes from filter extracts. The recovery from filter extracts ranged from 67 to 86% with relative standard deviation (RSD) less than 13%. The concentrations of dicarboxylated C2, C3, C4, C5 and C6-C10 in atmospheric aerosols ranged from 91-240 ng/m3, 11-56 ng/m3, 12-49 ng/m3, 8-35 ng/m3 and n.d. to 17 ng/m3, respectively. Oxalic (C2) acid was the dominant dicarboxylic acids detected in aerosol samples. The total concentrations of the LMW dicarboxylic acids (from C2 to C10) correspond to 2.2 to 2.6% of the total aerosol mass.

Study of total column atmospheric aerosol optical depth, ozone and ...

Indian Academy of Sciences (India)

Extensive observations of the columnar aerosol optical depth (AOD), total column ozone (TCO) and precipitable water content (PWC) have been carried out using the on-line, multi-band solar radiometers onboard ORV Sagar Kanya (Cruise#SK 147B) over Bay of Bengal during 11th-28th August 1999. Aerosol optical and ...

Adsorption of radioactive ions on carnauba-wax aerosols

Energy Technology Data Exchange (ETDEWEB)

Paul, A.; Keyser, U. [Physikalisch-Technische Bundesanstalt, Braunschweig (Germany)

1998-08-01

A new method based on parallel aerosol size spectrometry and {gamma}-spectrometry is introduced for the measurement of short-lived radioactive ions, fission products or super-heavy elements produced at accelerators. Furthermore a new aerosol generator is presented.The possibility of controlling and changing the aerosol size distribution in the helium aerosol jet produced by the aerosol generator allows the process of the adsorption and transport of radioactive ions on aerosols to be examined for the first time. This is due to the fact that the distribution is surveyed on-line using a negligible part of its total volume and parallel to the transporting flow. The radioactivity of the transported ions is measured by a germanium detector in offline position. In principle, both an on- or offline position with narrow multi-detector geometry (e.g. {beta}{gamma}{gamma}) is possible. (orig.) With 8 figs., 14 refs.

Flight-based chemical characterization of biomass burning aerosols within two prescribed burn smoke plumes

Directory of Open Access Journals (Sweden)

K. A. Pratt

2011-12-01

Full Text Available Biomass burning represents a major global source of aerosols impacting direct radiative forcing and cloud properties. Thus, the goal of a number of current studies involves developing a better understanding of how the chemical composition and mixing state of biomass burning aerosols evolve during atmospheric aging processes. During the Ice in Clouds Experiment-Layer Clouds (ICE-L in the fall of 2007, smoke plumes from two small Wyoming Bureau of Land Management prescribed burns were measured by on-line aerosol instrumentation aboard a C-130 aircraft, providing a detailed chemical characterization of the particles. After ~2–4 min of aging, submicron smoke particles, produced primarily from sagebrush combustion, consisted predominantly of organics by mass, but were comprised primarily of internal mixtures of organic carbon, elemental carbon, potassium chloride, and potassium sulfate. Significantly, the fresh biomass burning particles contained minor mass fractions of nitrate and sulfate, suggesting that hygroscopic material is incorporated very near or at the point of emission. The mass fractions of ammonium, sulfate, and nitrate increased with aging up to ~81–88 min and resulted in acidic particles. Decreasing black carbon mass concentrations occurred due to dilution of the plume. Increases in the fraction of oxygenated organic carbon and the presence of dicarboxylic acids, in particular, were observed with aging. Cloud condensation nuclei measurements suggested all particles >100 nm were active at 0.5% water supersaturation in the smoke plumes, confirming the relatively high hygroscopicity of the freshly emitted particles. For immersion/condensation freezing, ice nuclei measurements at −32 °C suggested activation of ~0.03–0.07% of the particles with diameters greater than 500 nm.

Submicron aerosol source apportionment of wintertime pollution in Paris, France by double positive matrix factorization (PMF2) using an aerosol chemical speciation monitor (ACSM) and a multi-wavelength Aethalometer

International Nuclear Information System (INIS)

Petit, J.E.; Favez, O.; Leoz-Garziandia, E.; Sciare, J.

2014-01-01

Online non-refractory submicron aerosol mass spectrometer (AMS) measurements in urban areas have successfully allowed the apportionment of specific sources and/or physical and chemical properties of the organic fraction. However, in order to be fully representative of PM pollution, a comprehensive source apportionment analysis is needed by taking into account all major components of submicron aerosols, creating strengthened bonds between the organic components and pollution sources. We present here a novel two-step methodology to perform such an analysis, by taking advantage of high time resolution of monitoring instruments: the aerosol chemical speciation monitor (ACSM) and the multi-wavelength absorption measurements (Aethalometer AE31) in Paris, France. As a first step, organic aerosols (OA) were de-convolved to hydrocarbon-like OA (HOA), biomass burning OA (BBOA) and oxygenated OA (OOA) with positive matrix factorization (PMF), and black carbon was de-convolved into its wood burning and fossil fuel combustion fractions. A second PMF analysis was then carried out with organic factors, BC fractions and inorganic species (nitrate, sulfate, ammonium, chloride), leading to a four-factor solution allowing highly time-resolved characterization of the major sources of PM1. Outputs of this PMF2 include two dominant combustion sources (wood burning and traffic) as well as semi-volatile and low-volatile secondary aerosols. While HOA is found to be emitted by both wood burning and traffic, the latter sources occurred to significantly contribute also to OOA. (authors)

Variability of Atmospheric Radon-222 and Secondary Aerosol Components in Accordance with Air Mass Transport Pathways at Jeju Island, Korea, during 2011-2014

Energy Technology Data Exchange (ETDEWEB)

Bu, Jun-Oh; Song, Jung-Min; Kim, Won-Hyung; Kang, Chang-Hee [Jeju National University, Jeju (Korea, Republic of); Chambers, Scott D.; Williams, Alastair G. [Australian Nuclear Science and Technology Organisation, Kirrawee DC (Australia); Lee, Chulkyu [Korea Meteorological Administration, Seoul (Korea, Republic of)

2016-06-15

Real-time monitoring of hourly atmospheric Radon-222 concentration and three daily monitoring of the secondary aerosol components of PM{sub 10} were performed throughout 2011-2014 at Gosan station, Jeju Island, in order to characterize their background levels and temporal variation. The annual mean radon and PM{sub 10} mass concentrations were 2326 ± 1198 mBq/m{sup 3} and 37.1 ± 19.5 μg/m{sup 3}, respectively. Based on cluster analyses of air mass back trajectories, the frequencies of air masses originating from continental China, the Korean Peninsula, and North Pacific Ocean routes were 53, 28, and 19%, respectively. When the air masses were transported to Jeju Island from continental China, the concentrations of radon and secondary aerosol components (nss-SO{sub 4}{sup 2-}, NO{sub 3}{sup -}, NH{sub 4}{sup +}) were relatively high: 2577 mBq/m{sup 3} and 14.4 μg/m{sup 3}, respectively. In cases when the air masses have moved from the Korean Peninsula, the corresponding concentrations were 2247 mBq/m{sup 3} and 11.4 μg/m{sup 3}, respectively. On the other hand, when the air masses came from the North Pacific Ocean, their radon and secondary aerosol concentrations decreased much further, 1372 mBq/m{sup 3} and 10.5 μg/m{sup 3}, respectively. Consequently, the variability of atmospheric radon concentrations at Gosan station might be characterized by synoptic changes in air mass fetch as well as diurnal changes in atmospheric mixing depth.

Characterization of key aerosol, trace gas and meteorological properties and particle formation and growth processes dependent on air mass origins in coastal Southern Spain

Science.gov (United States)

Diesch, J.; Drewnick, F.; Sinha, V.; Williams, J.; Borrmann, S.

2011-12-01

The chemical composition and concentration of aerosols at a certain site can vary depending on season, the air mass source region and distance from sources. Regardless of the environment, new particle formation (NPF) events are one of the major sources for ultrafine particles which are potentially hazardous to human health. Grown particles are optically active and efficient CCN resulting in important implications for visibility and climate (Zhang et al., 2004). The study presented here is intended to provide information about various aspects of continental, urban and marine air masses reflected by wind patterns of the air arriving at the measurement site. Additionally we will be focusing on NPF events associated with different types of air masses affecting their emergence and temporal evolution. Measurements of the ambient aerosol, various trace gases and meteorological parameters were performed within the framework of the DOMINO (Diel Oxidant Mechanisms In relation to Nitrogen Oxides) project. The field campaign took place from mid-November to mid-December 2008 at the atmospheric research station "El Arenosillo" located at the interface between a natural park, industrial cities (Huelva, Seville) and the Atlantic Ocean. Number and mass as well as PAH and black carbon concentrations were measured in PM1 and size distribution instruments covered the size range 6 nm up to 32 μm. The chemical composition of the non-refractory submicron aerosol was measured by means of an Aerosol Mass Spectrometer (AMS). In order to evaluate the characteristics of different air masses linking local and regional sources as well as NPF processes, characteristic air mass types were classified dependent on backwards trajectory pathways and local meteorology. Large nuclei mode concentrations in the number size distribution were found within continental and urban influenced air mass types due to frequently occurring NPF events. Exploring individual production and sink variables, sulfuric

Carbonaceous aerosols and pollutants over Delhi urban environment: Temporal evolution, source apportionment and radiative forcing

Energy Technology Data Exchange (ETDEWEB)

Bisht, D.S. [Indian Institute of Tropical Meteorology, New Delhi (India); Dumka, U.C., E-mail: dumka@aries.res.in [Aryabhatta Research Institute of Observational Sciences, Nainital (India); Kaskaoutis, D.G. [School of Natural Sciences, Shiv Nadar University, Tehsil Dadri (India); Pipal, A.S. [Department of Chemistry, Savitribai Phule Pune University, Pune (India); Srivastava, A.K. [Indian Institute of Tropical Meteorology, New Delhi (India); Soni, V.K.; Attri, S.D.; Sateesh, M. [India Meteorology Department, Lodhi Road, New Delhi (India); Tiwari, S. [Indian Institute of Tropical Meteorology, New Delhi (India)

2015-07-15

Particulate matter (PM{sub 2.5}) samples were collected over Delhi, India during January to December 2012 and analysed for carbonaceous aerosols and inorganic ions (SO{sub 4}{sup 2−} and NO{sub 3}{sup −}) in order to examine variations in atmospheric chemistry, combustion sources and influence of long-range transport. The PM{sub 2.5} samples are measured (offline) via medium volume air samplers and analysed gravimetrically for carbonaceous (organic carbon, OC; elemental carbon, EC) aerosols and inorganic ions (SO{sub 4}{sup 2−} and NO{sub 3}{sup −}). Furthermore, continuous (online) measurements of PM{sub 2.5} (via Beta-attenuation analyser), black carbon (BC) mass concentration (via Magee scientific Aethalometer) and carbon monoxide (via CO-analyser) are carried out. PM{sub 2.5} (online) range from 18.2 to 500.6 μg m{sup −3} (annual mean of 124.6 ± 87.9 μg m{sup −3}) exhibiting higher night-time (129.4 μg m{sup −3}) than daytime (103.8 μg m{sup −3}) concentrations. The online concentrations are 38% and 28% lower than the offline during night and day, respectively. In general, larger night-time concentrations are found for the BC, OC, NO{sub 3}{sup −}and SO{sub 4}{sup 2−}, which are seasonally dependent with larger differences during late post-monsoon and winter. The high correlation (R{sup 2} = 0.74) between OC and EC along with the OC/EC of 7.09 (day time) and 4.55 (night-time), suggest significant influence of biomass-burning emissions (burning of wood and agricultural waste) as well as secondary organic aerosol formation during daytime. Concentrated weighted trajectory (CWT) analysis reveals that the potential sources for the carbonaceous aerosols and pollutants are local emissions within the urban environment and transported smoke from agricultural burning in northwest India during post-monsoon. BC radiative forcing estimates result in very high atmospheric heating rates (~ 1.8–2.0 K day{sup −1}) due to agricultural burning effects

Carbonaceous aerosols and pollutants over Delhi urban environment: Temporal evolution, source apportionment and radiative forcing

International Nuclear Information System (INIS)

Bisht, D.S.; Dumka, U.C.; Kaskaoutis, D.G.; Pipal, A.S.; Srivastava, A.K.; Soni, V.K.; Attri, S.D.; Sateesh, M.; Tiwari, S.

2015-01-01

Particulate matter (PM 2.5 ) samples were collected over Delhi, India during January to December 2012 and analysed for carbonaceous aerosols and inorganic ions (SO 4 2− and NO 3 − ) in order to examine variations in atmospheric chemistry, combustion sources and influence of long-range transport. The PM 2.5 samples are measured (offline) via medium volume air samplers and analysed gravimetrically for carbonaceous (organic carbon, OC; elemental carbon, EC) aerosols and inorganic ions (SO 4 2− and NO 3 − ). Furthermore, continuous (online) measurements of PM 2.5 (via Beta-attenuation analyser), black carbon (BC) mass concentration (via Magee scientific Aethalometer) and carbon monoxide (via CO-analyser) are carried out. PM 2.5 (online) range from 18.2 to 500.6 μg m −3 (annual mean of 124.6 ± 87.9 μg m −3 ) exhibiting higher night-time (129.4 μg m −3 ) than daytime (103.8 μg m −3 ) concentrations. The online concentrations are 38% and 28% lower than the offline during night and day, respectively. In general, larger night-time concentrations are found for the BC, OC, NO 3 − and SO 4 2− , which are seasonally dependent with larger differences during late post-monsoon and winter. The high correlation (R 2 = 0.74) between OC and EC along with the OC/EC of 7.09 (day time) and 4.55 (night-time), suggest significant influence of biomass-burning emissions (burning of wood and agricultural waste) as well as secondary organic aerosol formation during daytime. Concentrated weighted trajectory (CWT) analysis reveals that the potential sources for the carbonaceous aerosols and pollutants are local emissions within the urban environment and transported smoke from agricultural burning in northwest India during post-monsoon. BC radiative forcing estimates result in very high atmospheric heating rates (~ 1.8–2.0 K day −1 ) due to agricultural burning effects during the 2012 post-monsoon season. - Highlights: • Very high PM 2.5 (> 200 µg m −3 ) levels

Intercomparison and closure calculations using measurements of aerosol species and optical properties during the Yosemite Aerosol Characterization Study

Science.gov (United States)

Malm, William C.; Day, Derek E.; Carrico, Christian; Kreidenweis, Sonia M.; Collett, Jeffrey L.; McMeeking, Gavin; Lee, Taehyoung; Carrillo, Jacqueline; Schichtel, Bret

2005-07-01

Physical and optical properties of inorganic aerosols have been extensively studied, but less is known about carbonaceous aerosols, especially as they relate to the non-urban settings such as our nation's national parks and wilderness areas. Therefore an aerosol characterization study was conceived and implemented at one national park that is highly impacted by carbonaceous aerosols, Yosemite. The primary objective of the study was to characterize the physical, chemical, and optical properties of a carbon-dominated aerosol, including the ratio of total organic matter weight to organic carbon, organic mass scattering efficiencies, and the hygroscopic characteristics of a carbon-laden ambient aerosol, while a secondary objective was to evaluate a variety of semi-continuous monitoring systems. Inorganic ions were characterized using 24-hour samples that were collected using the URG and Interagency Monitoring of Protected Visual Environments (IMPROVE) monitoring systems, the micro-orifice uniform deposit impactor (MOUDI) cascade impactor, as well as the semi-continuous particle-into-liquid sampler (PILS) technology. Likewise, carbonaceous material was collected over 24-hour periods using IMPROVE technology along with the thermal optical reflectance (TOR) analysis, while semi-continuous total carbon concentrations were measured using the Rupprecht and Patashnick (R&P) instrument. Dry aerosol number size distributions were measured using a differential mobility analyzer (DMA) and optical particle counter, scattering coefficients at near-ambient conditions were measured with nephelometers fitted with PM10 and PM2.5 inlets, and "dry" PM2.5 scattering was measured after passing ambient air through Perma Pure Nafion® dryers. In general, the 24-hour "bulk" measurements of various aerosol species compared more favorably with each other than with the semi-continuous data. Semi-continuous sulfate measurements correlated well with the 24-hour measurements, but were biased low by

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.

Emissions of biogenic volatile organic compounds and subsequent photochemical production of secondary organic aerosol in mesocosm studies of temperate and tropical plant species

Science.gov (United States)

Wyche, K. P.; Ryan, A. C.; Hewitt, C. N.; Alfarra, M. R.; McFiggans, G.; Carr, T.; Monks, P. S.; Smallbone, K. L.; Capes, G.; Hamilton, J. F.; Pugh, T. A. M.; MacKenzie, A. R.

2014-12-01

Silver birch (Betula pendula) and three Southeast Asian tropical plant species (Ficus cyathistipula, Ficus benjamina and Caryota millis) from the pantropical fig and palm genera were grown in a purpose-built and environment-controlled whole-tree chamber. The volatile organic compounds emitted from these trees were characterised and fed into a linked photochemical reaction chamber where they underwent photo-oxidation under a range of controlled conditions (relative humidity or RH ~65-89%, volatile organic compound-to-NOx or VOC / NOx ~3-9 and NOx ~2 ppbV). Both the gas phase and the aerosol phase of the reaction chamber were monitored in detail using a comprehensive suite of on-line and off-line chemical and physical measurement techniques. Silver birch was found to be a high monoterpene and sesquiterpene but low isoprene emitter, and its emissions were observed to produce measurable amounts of secondary organic aerosol (SOA) via both nucleation and condensation onto pre-existing seed aerosol (YSOA 26-39%). In contrast, all three tropical species were found to be high isoprene emitters with trace emissions of monoterpenes and sesquiterpenes. In tropical plant experiments without seed aerosol there was no measurable SOA nucleation, but aerosol mass was shown to increase when seed aerosol was present. Although principally isoprene emitting, the aerosol mass produced from tropical fig was mostly consistent (i.e. in 78 out of 120 aerosol mass calculations using plausible parameter sets of various precursor specific yields) with condensation of photo-oxidation products of the minor volatile organic compounds (VOCs) co-emitted; no significant aerosol yield from condensation of isoprene oxidation products was required in the interpretations of the experimental results. This finding is in line with previous reports of organic aerosol loadings consistent with production from minor biogenic VOCs co-emitted with isoprene in principally isoprene-emitting landscapes in Southeast

Influence of moisture on the behavior of aerosols

International Nuclear Information System (INIS)

Adams, R.E.; Longest, A.W.; Tobias, M.L.

1986-01-01

The behavior of aerosols assumed to be characteristic of those generated during light water reactor (LWR) accident sequences and released into containment has been studied in the Nuclear Safety Pilot Plant (NSPP) located at the Oak Ridge National Laboratory (ORNL). It has been observed that in a saturated steam-air environment a change occurs in the shape of aerosol agglomerates of U 3 O 8 aerosol, Fe 2 O 3 aerosol, and mixed U 3 O 8 -Fe 2 O 3 aerosol from branched-chain to spherical, and that the rate of reduction in the airborne aerosol mass concentration is increased relative to the rate observed in a dry atmosphere. The effect of a steam-air environment on the behavior of concrete aerosol is different. The shape of the agglomerated concrete aerosol is intermediate between branched-chain and spherical and the effect on the rate of reduction in airborne mass concentration appears to be slight. In a related project the shape of an agglomerated Fe 2 O 3 aerosol was observed to change from branched-chain to spherical at, or near, 100% relative humidity

Optical properties of the urban aerosol and their relation to chemical composition

International Nuclear Information System (INIS)

Leaderer, B.P.; Stolwijk, J.A.J.

1980-01-01

Light extinction and resulting visibility degradation in an unsaturated precipitation-free atmosphere are determined by light absorption and scattering and are caused by a complex mix of natural components and anthropogenic pollutants. The paper reviews correlation studies relating light scattering and light extinction (visibility) to concentrations of sulfate mass, nitrate mass, the remainder of the mass, and in some cases organic aerosol mass, while accounting for variations in relative humidity. It is found that sulfate aerosol mass is the dominant chemical aerosol species affecting light scattering and extinction. The dominant effect of sulfate mass on light scattering and extinction, even when sulfates account for a relatively small fraction of the total mass, results from the fact that sulfates are secondary aerosols and are mostly found in the 0.1-1.0 micron size range

MATRIX-VBS (v1.0): Implementing an Evolving Organic Aerosol Volatility in an Aerosol Microphysics Model

Science.gov (United States)

Gao, Chloe Y.; Tsigaridis, Kostas; Bauer, Susanne E.

2017-01-01

The gas-particle partitioning and chemical aging of semi-volatile organic aerosol are presented in a newly developed box model scheme, where its effect on the growth, composition, and mixing state of particles is examined. The volatility-basis set (VBS) framework is implemented into the aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state), which resolves mass and number aerosol concentrations and in multiple mixing-state classes. The new scheme, MATRIX-VBS, has the potential to significantly advance the representation of organic aerosols in Earth system models by improving upon the conventional representation as non-volatile particulate organic matter, often also with an assumed fixed size distribution. We present results from idealized cases representing Beijing, Mexico City, a Finnish forest, and a southeastern US forest, and investigate the evolution of mass concentrations and volatility distributions for organic species across the gas and particle phases, as well as assessing their mixing state among aerosol populations. Emitted semi-volatile primary organic aerosols evaporate almost completely in the intermediate-volatility range, while they remain in the particle phase in the low-volatility range. Their volatility distribution at any point in time depends on the applied emission factors, oxidation by OH radicals, and temperature. We also compare against parallel simulations with the original scheme, which represented only the particulate and non-volatile component of the organic aerosol, examining how differently the condensed-phase organic matter is distributed across the mixing states in the model. The results demonstrate the importance of representing organic aerosol as a semi-volatile aerosol, and explicitly calculating the partitioning of organic species between the gas and particulate phases.

Cluster Analysis of the Organic Peaks in Bulk Mass Spectra Obtained During the 2002 New England Air Quality Study with an Aerodyne Aerosol Mass Spectrometer

Directory of Open Access Journals (Sweden)

C. Marcolli

2006-01-01

Full Text Available We applied hierarchical cluster analysis to an Aerodyne aerosol mass spectrometer (AMS bulk mass spectral dataset collected aboard the NOAA research vessel R. H. Brown during the 2002 New England Air Quality Study off the east coast of the United States. Emphasizing the organic peaks, the cluster analysis yielded a series of categories that are distinguishable with respect to their mass spectra and their occurrence as a function of time. The differences between the categories mainly arise from relative intensity changes rather than from the presence or absence of specific peaks. The most frequent category exhibits a strong signal at m/z 44 and represents oxidized organic matter probably originating from both anthropogenic as well as biogenic sources. On the basis of spectral and trace gas correlations, the second most common category with strong signals at m/z 29, 43, and 44 contains contributions from isoprene oxidation products. The third through the fifth most common categories have peak patterns characteristic of monoterpene oxidation products and were most frequently observed when air masses from monoterpene rich regions were sampled. Taken together, the second through the fifth most common categories represent on average 17% of the total organic mass that stems likely from biogenic sources during the ship's cruise. These numbers have to be viewed as lower limits since the most common category was attributed to anthropogenic sources for this calculation. The cluster analysis was also very effective in identifying a few contaminated mass spectra that were not removed during pre-processing. This study demonstrates that hierarchical clustering is a useful tool to analyze the complex patterns of the organic peaks in bulk aerosol mass spectra from a field study.

The physico-chemical evolution of atmospheric aerosols and the gas-particle partitioning of inorganic aerosol during KORUS-AQ

Science.gov (United States)

Lee, T.; Park, T.; Lee, J. B.; Lim, Y. J.; Ahn, J.; Park, J. S.; Soo, C. J.; Desyaterik, Y.; Collett, J. L., Jr.

2017-12-01

Aerosols influence climate change directly by scattering and absorption and indirectly by acting as cloud condensation nuclei and some of the effects of aerosols are reduction in visibility, deterioration of human health, and deposition of pollutants to ecosystems. Urban area is large source of aerosols and aerosol precursors. Aerosol sources are both local and from long-range transport. Long-range transport processed aerosol are often dominant sources of aerosol pollution in Korea. To improve our knowledge of aerosol chemistry, Korea and U.S-Air Quality (KORUS-AQ) of Aircraft-based aerosol measurement took place in and around Seoul, Korea during May and June 2016. KORUS-AQ campaigns were conducted to study the chemical characterization and processes of pollutants in the Seoul Metropolitan area to regional scales of Korean peninsula. Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed on aircraft platforms on-board DC-8 (NASA) aircraft. We characterized aerosol chemical properties and mass concentrations of sulfate, nitrate, ammonium and organics in polluted air plumes and investigate the spatial and vertical distribution of the species. The results of studies show that organics is predominant in Aerosol and a significant fraction of the organics is oxygenated organic aerosol (OOA) at the high altitude. Both Nitrate and sulfate can partition between the gas and particle phases. The ratios for HNO3/(N(V) (=gaseous HNO3 + particulate Nitrate) and SO2/(SO2+Sulfate) were found to exhibit quite different distributions between the particles and gas phase for the locations during KORUS-AQ campaign, representing potential for formation of additional particulate nitrate and sulfate. The results of those studies can provide highly resolved temporal and spatial air pollutant, which are valuable for air quality model input parameters for aerosol behaviour.

Comparison of three aerosol chemical characterization techniques utilizing PTR-ToF-MS: a study on freshly formed and aged biogenic SOA

Science.gov (United States)

Gkatzelis, Georgios I.; Tillmann, Ralf; Hohaus, Thorsten; Müller, Markus; Eichler, Philipp; Xu, Kang-Ming; Schlag, Patrick; Schmitt, Sebastian H.; Wegener, Robert; Kaminski, Martin; Holzinger, Rupert; Wisthaler, Armin; Kiendler-Scharr, Astrid

2018-03-01

An intercomparison of different aerosol chemical characterization techniques has been performed as part of a chamber study of biogenic secondary organic aerosol (BSOA) formation and aging at the atmosphere simulation chamber SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction chamber). Three different aerosol sampling techniques - the aerosol collection module (ACM), the chemical analysis of aerosol online (CHARON) and the collection thermal-desorption unit (TD) were connected to proton transfer reaction time-of-flight mass spectrometers (PTR-ToF-MSs) to provide chemical characterization of the SOA. The techniques were compared among each other and to results from an aerosol mass spectrometer (AMS) and a scanning mobility particle sizer (SMPS). The experiments investigated SOA formation from the ozonolysis of β-pinene, limonene, a β-pinene-limonene mix and real plant emissions from Pinus sylvestris L. (Scots pine). The SOA was subsequently aged by photo-oxidation, except for limonene SOA, which was aged by NO3 oxidation. Despite significant differences in the aerosol collection and desorption methods of the PTR-based techniques, the determined chemical composition, i.e. the same major contributing signals, was found by all instruments for the different chemical systems studied. These signals could be attributed to known products expected from the oxidation of the examined monoterpenes. The sampling and desorption method of ACM and TD provided additional information on the volatility of individual compounds and showed relatively good agreement. Averaged over all experiments, the total aerosol mass recovery compared to an SMPS varied within 80 ± 10, 51 ± 5 and 27 ± 3 % for CHARON, ACM and TD, respectively. Comparison to the oxygen-to-carbon ratios (O : C) obtained by AMS showed that all PTR-based techniques observed lower O : C ratios, indicating a loss of molecular oxygen either during aerosol sampling or detection. The differences in total

The online measured black carbon aerosol and source orientations in the Nam Co region, Tibet.

Science.gov (United States)

Zhang, Xin; Ming, Jing; Li, Zhongqin; Wang, Feiteng; Zhang, Guoshuai

2017-11-01

Equivalent black carbon (eBC) mass concentrations were measured by an aethalometer (AE-31) in the Nam Co, central Tibet from 2010 to 2014. Different from previous filter-sampling studies (Ming et al., J Environ Sci 22(11):1748-1756, 2010; Zhao et al., Environ Sci Pollut Res 20:5827-5838, 2013), the first high-resolution online eBC measurement conducted in central Tibet is reported here, allowing to discuss the diurnal variations as well as seasonal variabilities of eBC. Average daily eBC concentration was 74 ± 50 ng/m 3 , reflecting a global background level. Meteorological conditions influenced eBC concentrations largely at seasonal scale, which are higher in February-May but lower in June-January. The highest eBC concentrations (greater than 210 ng/m 3 ) were more associated with the W and WSW winds smaller than 6 m/s. The diurnal variations of eBC showed plateaus from 10:00 to 15:00 with seasonal variations, associated with local anthropogenic activities, such as indigenous Tibetan burning animal waste and tourism traffic. The PBLHs showed a co-variance with eBC concentrations, implicating close sources. The aerosol optical depths derived from the MODIS data over the Nam Co Observatory Station (NCOS)-included sub-area (30° N-40° N, 90° E-100° E) showed significant relationship with eBC concentrations. This suggests that nearby or short-distance sources other than long-distance transported pollutants could be important contributors to eBC concentrations at the NCOS, different from the conclusions suggested by previous studies.

Aerosols in Northern Morocco: Input pathways and their chemical fingerprint

Science.gov (United States)

Benchrif, A.; Guinot, B.; Bounakhla, M.; Cachier, H.; Damnati, B.; Baghdad, B.

2018-02-01

The Mediterranean basin is one of the most sensitive regions in the world regarding climate change and air quality. Deserts and marine aerosols combine with combustion aerosols from maritime traffic, large urban centers, and at a larger scale from populated industrialized regions in Europe. From Tetouan city located in the North of Morocco, we attempted to better figure out the main aerosol transport pathways and their respective aerosol load and chemical profile by examining air mass back trajectory patterns and aerosol chemical compositions from May 2011 to April 2012. The back trajectory analysis throughout the sampling period led to four clusters, for which meteorological conditions and aerosol chemical characteristics have been investigated. The most frequent cluster (CL3: 39%) corresponds to polluted air masses coming from the Mediterranean Basin, characterized by urban and marine vessels emissions out of Spain and of Northern Africa. Two other polluted clusters were characterized. One is of local origin (CL1: 22%), with a marked contribution from urban aerosols (Rabat, Casablanca) and from biomass burning aerosols. The second (CL2: 32%) defines air masses from the near Atlantic Ocean, affected by pollutants emitted from the Iberian coast. A fourth cluster (CL4: 7%) is characterized by rather clean, fast and rainy oceanic air masses, influenced during their last 24 h before reaching Tetouan by similar sources with those affecting CL2, but to a lesser extent. The chemical data show that carbonaceous species are found in the fine aerosols fraction and are generally from local primary sources (low OC/EC) rather than long-range transported. In addition to fresh traffic and maritime vessel aerosols, our results suggest the contribution of local biomass burning.

Particle mass yield in secondary organic aerosol formed by the dark ozonolysis of α-pinene

Directory of Open Access Journals (Sweden)

J. E. Shilling

2008-04-01

Full Text Available The yield of particle mass in secondary organic aerosol (SOA formed by dark ozonolysis was measured for 0.3–22.8 ppbv of reacted α-pinene. Most experiments were conducted using a continuous-flow chamber, allowing nearly constant SOA concentration and chemical composition for several days. For comparison, some experiments were also conducted in batch mode. Reaction conditions were 25°C, 40% RH, dry (NH₄SO₄ seed particles, and excess 1-butanol. The organic particle loading was independently measured by an aerosol mass spectrometer and a scanning mobility particle sizer, and the two measurements agreed well. The observations showed that SOA formation occurred for even the lowest reacted α-pinene concentration of 0.3 ppbv. The particle mass yield was 0.09 at 0.15 μg m⁻³, increasing to 0.27 at 40 μg m⁻³. Compared to some results reported in the literature, the yields were 80 to 100% larger for loadings above 2 μg m⁻³. At lower loadings, the yields had an offset of approximately +0.07 from those reported in the literature. To as low as 0.15 μm⁻³, the yield curve had no inflection point toward null yield, implying the formation of one or several products having vapor pressures below this value. These observations of increased yields, especially for low loadings, are potentially important for accurate prediction by chemical transport models of organic particle concentrations in the ambient atmosphere.

Instrumentation for tropospheric aerosol characterization

Energy Technology Data Exchange (ETDEWEB)

Shi, Z.; Young, S.E.; Becker, C.H.; Coggiola, M.J. [SRI International, Menlo Park, CA (United States); Wollnik, H. [Giessen Univ. (Germany)

1997-12-31

A new instrument has been developed that determines the abundance, size distribution, and chemical composition of tropospheric and lower stratospheric aerosols with diameters down to 0.2 {mu}m. In addition to aerosol characterization, the instrument also monitors the chemical composition of the ambient gas. More than 25.000 aerosol particle mass spectra were recorded during the NASA-sponsored Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) field program using NASA`s DC-8 research aircraft. (author) 7 refs.

Instrumentation for tropospheric aerosol characterization

Energy Technology Data Exchange (ETDEWEB)

Shi, Z; Young, S E; Becker, C H; Coggiola, M J [SRI International, Menlo Park, CA (United States); Wollnik, H [Giessen Univ. (Germany)

1998-12-31

A new instrument has been developed that determines the abundance, size distribution, and chemical composition of tropospheric and lower stratospheric aerosols with diameters down to 0.2 {mu}m. In addition to aerosol characterization, the instrument also monitors the chemical composition of the ambient gas. More than 25.000 aerosol particle mass spectra were recorded during the NASA-sponsored Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) field program using NASA`s DC-8 research aircraft. (author) 7 refs.

Aerosol composition and source apportionment in Santiago de Chile

International Nuclear Information System (INIS)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-01-01

Santiago de Chile, Sao Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp 10 mass of particles smaller than 10 μm) and black carbon concentration were also measured. Particle-Induced X-ray Emission (PIXE) was used to measure the concentration of 22 trace elements at levels below 0.5 ng m -3 . Quantitative aerosol source apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10 ). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2 . In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of

MATRIX (Multiconfiguration Aerosol TRacker of mIXing state): an aerosol microphysical module for global atmospheric models

OpenAIRE

Bauer , S. E.; Wright , D.; Koch , D.; Lewis , E. R.; Mcgraw , R.; Chang , L.-S.; Schwartz , S. E.; Ruedy , R.

2008-01-01

A new aerosol microphysical module MATRIX, the Multiconfiguration Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS) climate model (ModelE) are described. This module, which is based on the quadrature method of moments (QMOM), represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mod...

Aerosols on the surface of needles in the vicinity of Winterthur

International Nuclear Information System (INIS)

Wyttenbach, A.; Tobler, L.; Bajo, S.

1991-01-01

The composition and the mass of aerosols residing on the surface of one-year-old needles of Norway spruce are described. The composition of aerosols on spruce needles is compared with that of aerosols collected by air filters and the composition of the local soil. A comparison of the years 1982 and 1985 shows virtually identical conditions. Finally, possible connections between aerosol mass and inherent needle content are discussed. (author) 5 figs., 2 tabs., 13 refs

MATRIX (Multiconfiguration Aerosol TRacker of mIXing state: an aerosol microphysical module for global atmospheric models

Directory of Open Access Journals (Sweden)

S. E. Bauer

2008-10-01

Full Text Available A new aerosol microphysical module MATRIX, the Multiconfiguration Aerosol TRacker of mIXing state, and its application in the Goddard Institute for Space Studies (GISS climate model (ModelE are described. This module, which is based on the quadrature method of moments (QMOM, represents nucleation, condensation, coagulation, internal and external mixing, and cloud-drop activation and provides aerosol particle mass and number concentration and particle size information for up to 16 mixed-mode aerosol populations. Internal and external mixing among aerosol components sulfate, nitrate, ammonium, carbonaceous aerosols, dust and sea-salt particles are represented. The solubility of each aerosol population, which is explicitly calculated based on its soluble and insoluble components, enables calculation of the dependence of cloud drop activation on the microphysical characterization of multiple soluble aerosol populations.

A detailed model description and results of box-model simulations of various aerosol population configurations are presented. The box model experiments demonstrate the dependence of cloud activating aerosol number concentration on the aerosol population configuration; comparisons to sectional models are quite favorable. MATRIX is incorporated into the GISS climate model and simulations are carried out primarily to assess its performance/efficiency for global-scale atmospheric model application. Simulation results were compared with aircraft and station measurements of aerosol mass and number concentration and particle size to assess the ability of the new method to yield data suitable for such comparison. The model accurately captures the observed size distributions in the Aitken and accumulation modes up to particle diameter 1 μm, in which sulfate, nitrate, black and organic carbon are predominantly located; however the model underestimates coarse-mode number concentration and size, especially in the marine environment

Estimating marine aerosol particle volume and number from Maritime Aerosol Network data

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A. M. Sayer

2012-09-01

Full Text Available As well as spectral aerosol optical depth (AOD, aerosol composition and concentration (number, volume, or mass are of interest for a variety of applications. However, remote sensing of these quantities is more difficult than for AOD, as it is more sensitive to assumptions relating to aerosol composition. This study uses spectral AOD measured on Maritime Aerosol Network (MAN cruises, with the additional constraint of a microphysical model for unpolluted maritime aerosol based on analysis of Aerosol Robotic Network (AERONET inversions, to estimate these quantities over open ocean. When the MAN data are subset to those likely to be comprised of maritime aerosol, number and volume concentrations obtained are physically reasonable. Attempts to estimate surface concentration from columnar abundance, however, are shown to be limited by uncertainties in vertical distribution. Columnar AOD at 550 nm and aerosol number for unpolluted maritime cases are also compared with Moderate Resolution Imaging Spectroradiometer (MODIS data, for both the present Collection 5.1 and forthcoming Collection 6. MODIS provides a best-fitting retrieval solution, as well as the average for several different solutions, with different aerosol microphysical models. The "average solution" MODIS dataset agrees more closely with MAN than the "best solution" dataset. Terra tends to retrieve lower aerosol number than MAN, and Aqua higher, linked with differences in the aerosol models commonly chosen. Collection 6 AOD is likely to agree more closely with MAN over open ocean than Collection 5.1. In situations where spectral AOD is measured accurately, and aerosol microphysical properties are reasonably well-constrained, estimates of aerosol number and volume using MAN or similar data would provide for a greater variety of potential comparisons with aerosol properties derived from satellite or chemistry transport model data. However, without accurate AOD data and prior knowledge of

Identification of secondary aerosol precursors emitted by an aircraft turbofan

Science.gov (United States)

Kılıç, Doğuşhan; El Haddad, Imad; Brem, Benjamin T.; Bruns, Emily; Bozetti, Carlo; Corbin, Joel; Durdina, Lukas; Huang, Ru-Jin; Jiang, Jianhui; Klein, Felix; Lavi, Avi; Pieber, Simone M.; Rindlisbacher, Theo; Rudich, Yinon; Slowik, Jay G.; Wang, Jing; Baltensperger, Urs; Prévôt, Andre S. H.

2018-05-01

Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM) chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs) and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS) for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS) for nonrefractory particulate matter (NR-PM1) were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5-7 %), more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

Receptor modeling of near-roadway aerosol mass spectrometer data in Las Vegas, Nevada, with EPA PMF

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S. G. Brown

2012-01-01

Full Text Available Ambient non-refractory PM₁ aerosol particles were measured with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-AMS at an elementary school 18 m from the US 95 freeway soundwall in Las Vegas, Nevada, during January 2008. Additional collocated continuous measurements of black carbon (BC, carbon monoxide (CO, nitrogen oxides (NO_x, and meteorological data were collected. The US~Environmental Protection Agency's (EPA positive matrix factorization (PMF data analysis tool was used to apportion organic matter (OM as measured by HR-AMS, and rotational tools in EPA PMF were used to better characterize the solution space and pull resolved factors toward known source profiles. Three- to six-factor solutions were resolved. The four-factor solution was the most interpretable, with the typical AMS PMF factors of hydrocarbon-like organic aerosol (HOA, low-volatility oxygenated organic aerosol (LV-OOA, biomass burning organic aerosol (BBOA, and semi-volatile oxygenated organic aerosol (SV-OOA. When the measurement site was downwind of the freeway, HOA composed about half the OM, with SV-OOA and LV-OOA accounting for the rest. Attempts to pull the PMF factor profiles toward source profiles were successful but did not qualitatively change the results, indicating that these factors are very stable. Oblique edges were present in G-space plots, suggesting that the obtained rotation may not be the most plausible one. Since solutions found by pulling the profiles or using F_peak retained these oblique edges, there appears to be little rotational freedom in the base solution. On average, HOA made up 26% of the OM, while LV-OOA was highest in the afternoon and accounted for 26% of the OM. BBOA occurred in the evening hours, was predominantly from the residential area to the north, and on average constituted 12% of the OM; SV-OOA accounted for the remaining third of the OM. Use of the pulling techniques

Aerosol composition and source apportionment in Santiago de Chile

Science.gov (United States)

Artaxo, Paulo; Oyola, Pedro; Martinez, Roberto

1999-04-01

Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dpsource apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m 3 PM 10). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM 10 aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO 2. In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of several heavy metals such as Zn, Cu and others. A factor with molybdenum, arsenic, copper and sulfur was observed frequently, and it results from emissions of copper smelters.

Quantitative characterization of colloidal assembly of graphene oxide-silver nanoparticle hybrids using aerosol differential mobility-coupled mass analyses.

Science.gov (United States)

Nguyen, Thai Phuong; Chang, Wei-Chang; Lai, Yen-Chih; Hsiao, Ta-Chih; Tsai, De-Hao

2017-10-01

In this work, we develop an aerosol-based, time-resolved ion mobility-coupled mass characterization method to investigate colloidal assembly of graphene oxide (GO)-silver nanoparticle (AgNP) hybrid nanostructure on a quantitative basis. Transmission electron microscopy (TEM) and zeta potential (ZP) analysis were used to provide visual information and elemental-based particle size distributions, respectively. Results clearly show a successful controlled assembly of GO-AgNP by electrostatic-directed heterogeneous aggregation between GO and bovine serum albumin (BSA)-functionalized AgNP under an acidic environment. Additionally, physical size, mass, and conformation (i.e., number of AgNP per nanohybrid) of GO-AgNP were shown to be proportional to the number concentration ratio of AgNP to GO (R) and the selected electrical mobility diameter. An analysis of colloidal stability of GO-AgNP indicates that the stability increased with its absolute ZP, which was dependent on R and environmental pH. The work presented here provides a proof of concept for systematically synthesizing hybrid colloidal nanomaterials through the tuning of surface chemistry in aqueous phase with the ability in quantitative characterization. Graphical Abstract Colloidal assembly of graphene oxide-silver nanoparticle hybrids characterized by aerosol differential mobility-coupled mass analyses.

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.

A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG

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Y. Zhang

2016-11-01

Full Text Available We present a rapid method for apportioning the sources of atmospheric organic aerosol composition measured by gas chromatography–mass spectrometry methods. Here, we specifically apply this new analysis method to data acquired on a thermal desorption aerosol gas chromatograph (TAG system. Gas chromatograms are divided by retention time into evenly spaced bins, within which the mass spectra are summed. A previous chromatogram binning method was introduced for the purpose of chromatogram structure deconvolution (e.g., major compound classes (Zhang et al., 2014. Here we extend the method development for the specific purpose of determining aerosol samples' sources. Chromatogram bins are arranged into an input data matrix for positive matrix factorization (PMF, where the sample number is the row dimension and the mass-spectra-resolved eluting time intervals (bins are the column dimension. Then two-dimensional PMF can effectively do three-dimensional factorization on the three-dimensional TAG mass spectra data. The retention time shift of the chromatogram is corrected by applying the median values of the different peaks' shifts. Bin width affects chemical resolution but does not affect PMF retrieval of the sources' time variations for low-factor solutions. A bin width smaller than the maximum retention shift among all samples requires retention time shift correction. A six-factor PMF comparison among aerosol mass spectrometry (AMS, TAG binning, and conventional TAG compound integration methods shows that the TAG binning method performs similarly to the integration method. However, the new binning method incorporates the entirety of the data set and requires significantly less pre-processing of the data than conventional single compound identification and integration. In addition, while a fraction of the most oxygenated aerosol does not elute through an underivatized TAG analysis, the TAG binning method does have the ability to achieve molecular level

On-line Field Measurements of Speciated PM1 Emission Factors from Common South Asian Combustion Sources

Science.gov (United States)

DeCarlo, P. F.; Goetz, J. D.; Giordano, M.; Stockwell, C.; Maharjan, R.; Adhikari, S.; Bhave, P.; Praveen, P. S.; Panday, A. K.; Jayarathne, T. S.; Stone, E. A.; Yokelson, R. J.

2017-12-01

Characterization of aerosol emissions from prevalent but under sampled combustion sources in South Asia was performed as part of the Nepal Ambient Monitoring and Source Testing Experiment (NAMaSTE) in April 2015. Targeted emission sources included cooking stoves with a variety of solid fuels, brick kilns, garbage burning, crop-residue burning, diesel irrigation pumps, and motorcycles. Real-time measurements of submicron non-refractory particulate mass concentration and composition were obtained using an Aerodyne mini Aerosol Mass Spectrometer (mAMS). Speciated PM1 mass emission factors were calculated for all particulate species (e.g. organics, sulfates, nitrates, chlorides, ammonium) and for each source type using the carbon mass balance approach. Size resolved emission factors were also acquired using a novel high duty cycle particle time-of-flight technique (ePTOF). Black carbon and brown carbon absorption emission factors and absorption Angström exponents were measured using filter loading and scattering corrected attenuation at 370 nm and 880 nm with a dual spot aethalometer (Magee Scientific AE-33). The results indicate that open garbage burning is a strong emitter of organic aerosol, black carbon, and internally mixed particle phase hydrogen chloride (HCl). Emissions of HCl were attributed to the presence chlorinated plastics. The primarily coal fired brick kilns were found to be large emitters of sulfate but large differences in the organic and light absorbing component of emissions were observed between the two kiln types investigated (technologically advanced vs. traditional). These results, among others, bring on-line and field-tested aerosol emission measurements to an area of atmoshperic research dominated by off-line or laboratory based measurements.

[Size distributions of aerosol during the Spring Festival in Nanjing].

Science.gov (United States)

Wang, Hong-Lei; Zhu, Bin; Shen, Li-Juan; Liu, Xiao-Hui; Zhang, Ze-Feng; Yang, Yang

2014-02-01

In order to investigate the firework burning impacts on spectrum distribution of atmospheric aerosol during the Spring Festival in Nanjing, number concentration and mass concentration of aerosol as well as mass concentration of gas pollutants were measured during January 19-31, 2012. The results indicated that the concentration of aerosol between 10-20 nm decreased, aerosol concentration in the range of 50-100 nm, 100-200 nm and 200-500 nm increased during the firework burning period comparing to those during the non-burning period. However, there was no obvious variation for aerosol between 20-50 nm and 0.5-10 microm. The spectrum distribution of number concentration was bimodal during the non-burning period and unimodal during the burning period, with the peak value shifting to large diameter section. The mass concentration presented a bimodal distribution, the value of PM2.5/PM10 and PM10/PM10 increased by 10% during the burning period. The firework burning events had big influence on the density of aerosol between 1.0-2.1 microm.

Polar and non-polar organic aerosols from large-scale agricultural-waste burning emissions in Northern India: Implications to organic mass-to-organic carbon ratio.

Science.gov (United States)

Rajput, Prashant; Sarin, M M

2014-05-01

This study focuses on characteristics of organic aerosols (polar and non-polar) and total organic mass-to-organic carbon ratio (OM/OC) from post-harvest agricultural-waste (paddy- and wheat-residue) burning emissions in Northern India. Aerosol samples from an upwind location (Patiala: 30.2°N, 76.3°E) in the Indo-Gangetic Plain were analyzed for non-polar and polar fractions of organic carbon (OC1 and OC2) and their respective mass (OM1 and OM2). On average, polar organic aerosols (OM2) contribute nearly 85% of the total organic mass (OM) from the paddy- and wheat-residue burning emissions. The water-soluble-OC (WSOC) to OC2 ratio, within the analytical uncertainty, is close to 1 from both paddy- and wheat-residue burning emissions. However, temporal variability and relatively low WSOC/OC2 ratio (Av: 0.67±0.06) is attributed to high moisture content and poor combustion efficiency during paddy-residue burning, indicating significant contribution (∼30%) of aromatic carbon to OC2. The OM/OC ratio for non-polar (OM1/OC1∼1.2) and polar organic aerosols (OM2/OC2∼2.2), hitherto unknown for open agricultural-waste burning emissions, is documented in this study. The total OM/OC ratio is nearly identical, 1.9±0.2 and 1.8±0.2, from paddy- and wheat-residue burning emissions. Copyright © 2013 Elsevier Ltd. All rights reserved.

Clouds and aerosols in Puerto Rico ─ a new evaluation

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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

Direct Radiative Impacts of Central American Biomass Burning Smoke Aerosols: Analysis from a Coupled Aerosol-Radiation-Meteorology Model RAMS-AROMA

Science.gov (United States)

Wang, J.; Christopher, S. A.; Nair, U. S.; Reid, J. S.; Prins, E. M.

2005-12-01

Considerable efforts including various field experiments have been carried out in the last decade for studying the regional climatic impact of smoke aerosols produced by biomass burning activities in Africa and South America. In contrast, only few investigations have been conducted for Central American Biomass Burning (CABB) region. Using a coupled aerosol-radiation-meteorology model called RAMS-AROMA together with various ground-based observations, we present a comprehensive analysis of the smoke direct radiative impacts on the surface energy budget, boundary layer evolution, and e precipitation process during the CABB events in Spring 2003. Quantitative estimates are also made regarding the transboundary carbon mass to the U.S. in the form of smoke particles. Buult upon the Regional Atmospheric Modeling System (RAMS) mesoscale model, the RAMS AROMA has several features including Assimilation and Radiation Online Modeling of Aerosols (AROMA) algorithms. The model simulates smoke transport by using hourly smoke emission inventory from the Fire Locating and Modeling of Burning Emissions (FLAMBE) geostationary satellite database. It explicitly considers the smoke effects on the radiative transfer at each model time step and model grid, thereby coupling the dynamical processes and aerosol transport. Comparison with ground-based observation show that the simulation realistically captured the smoke transport timeline and distribution from daily to hourly scales. The effects of smoke radiative extinction on the decrease of 2m air temperature (2mT), diurnal temperature range (DTR), and boundary layer height over the land surface are also quantified. Warming due to smoke absorption of solar radiation can be found in the lower troposphere over the ocean, but not near the underlying land surface. The increase of boundary layer stability produces a positive feedback where more smoke particles are trapped in the lower boundary layer. These changes in temperature, surface

A soluble one-dimensional problem for coupled heat conduction and mass diffusion with aerosol formation in a vapour-gas mixture

International Nuclear Information System (INIS)

Barrett, J.C.; Clement, C.F.

1986-01-01

The coupled equations for heat and mass transfer are reduced to ordinary differential equations applying to a semi-infinite region bounded by a wall. Solutions are obtained in the limits of no aerosol and of negligible supersaturations in which case the aerosol growth rate is calculated. In agreement with earlier general predictions, results for water vapour-air mixtures show very different behaviour between heating and cooling the mixtures, and that aerosol growth rates do not increase with temperature, but rather become a much smaller fraction of evaporation or condensation rates at the wall. A new feature is that, in the cooling case, an aerosol growth region is predicted to exist immediately adjacent to the wall, whereas further away any aerosol is predicted to evaporate. The general features of the results are expected to apply to many situations of steady or quasi-steady flow. For example, similar results to ours would be obtained for the laminar flow of a saturated water vapour-air mixture past a wall through which it is being cooled. General characteristics of such flows should include a widening mist-filled layer next to the wall and separation by a sharp spatial division from an unsaturated layer. (author)

Impact of cloud-borne aerosol representation on aerosol direct and indirect effects

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S. J. Ghan

2006-01-01

Full Text Available Aerosol particles attached to cloud droplets are much more likely to be removed from the atmosphere and are much less efficient at scattering sunlight than if unattached. Models used to estimate direct and indirect effects of aerosols employ a variety of representations of such cloud-borne particles. Here we use a global aerosol model with a relatively complete treatment of cloud-borne particles to estimate the sensitivity of simulated aerosol, cloud and radiation fields to various approximations to the representation of cloud-borne particles. We find that neglecting transport of cloud-borne particles introduces little error, but that diagnosing cloud-borne particles produces global mean biases of 20% and local errors of up to 40% for aerosol, droplet number, and direct and indirect radiative forcing. Aerosol number, aerosol optical depth and droplet number are significantly underestimated in regions and seasons where and when wet removal is primarily by stratiform rather than convective clouds (polar regions during winter, but direct and indirect effects are less biased because of the limited sunlight there and then. A treatment that predicts the total mass concentration of cloud-borne particles for each mode yields smaller errors and runs 20% faster than the complete treatment. The errors are much smaller than current estimates of uncertainty in direct and indirect effects of aerosols, which suggests that the treatment of cloud-borne aerosol is not a significant source of uncertainty in estimates of direct and indirect effects.

Changes in ground-level PM mass concentration and column aerosol optical depth over East Asia during 2004-2014

Science.gov (United States)

Nam, J.; Kim, S. W.; Park, R.; Yoon, S. C.; Sugimoto, N.; Park, J. S.; Hong, J.

2015-12-01

Multi-year records of moderate resolution imaging spectroradiometer (MODIS), ground-level particulate matter (PM) mass concentration, cloud-aerosol lidar with orthogonal polarization (CALIOP), and ground-level lidar were analyzed to investigate seasonal and annual changes of aerosol optical depth (AOD) and PM mass concentration over East Asia. Least mean square fit method is applied to detect the trends and their magnitudes for each selected regions and stations. Eleven-year MODIS measurements show generally increasing trends in both AOD (1.18 % yr-1) and Ångström exponent (0.98 % yr-1), especially over the east coastal industrialized region in China. Monthly variation of AOD show maximum value at April-July, which were related to the progress of summer monsoon rain band and stationary continental air mass on the northeast of Asia. Increasing trends of AOD were found for eight cites in China (0.80 % yr-1) and Seoul site, Korea (0.40 % yr-1), whereas no significant change were shown in Gosan background site (0.04 % yr-1) and decreasing trend at five background sites in Japan (-0.42 % yr-1). Contrasting to AOD trend, all fifteen sites in China (-1.28 % yr-1), Korea (-2.77 % yr-1), and Japan (-2.03 % yr-1) showed decreasing trend of PM10 mass concentration. Also, PM2.5 mass concentration at Beijing, Seoul, Rishiri, and Oki show significant decreasing trend of -1.16 % yr-1. To further discuss the opposite trend of surface PM mass concentration and column AOD, we investigate vertical aerosol profile from lidar measurements. AOD estimated for planetary boundary layer (surface~1.5 km altitude; AODPBL) from CALIOP measurements over East China show decreasing trend of -1.71 % yr-1 over the period of 2007-2014, wherever AOD estimated for free troposphere (1.5 km~5 km altitude; AODFT) show increasing trend of 2.92 % yr-1. In addition, ground-level lidar measurements in Seoul show decreasing AODPBL trend of -2.57 % yr-1, whereas, AODFT show no significant change (-0.44 % yr

Studies on aerosol properties during ICARB–2006 campaign period ...

Indian Academy of Sciences (India)

Continuous and campaign-based aerosol field measurements are essential in understanding funda- ... aerosol mass concentration and aerosol particle size distribution were carried out during the cam- .... the details provided by the supplier, the calibration ..... solar flux at the surface, derived from principal-plane sky.

Rapid characterization of agglomerate aerosols by in situ mass-mobility measurements.

Science.gov (United States)

Scheckman, Jacob H; McMurry, Peter H; Pratsinis, Sotiris E

2009-07-21

Transport and physical/chemical properties of nanoparticle agglomerates depend on primary particle size and agglomerate structure (size, fractal dimension, and dynamic shape factor). This research reports on in situ techniques for measuring such properties. Nanoparticle agglomerates of silica were generated by oxidizing hexamethyldisiloxane in a methane/oxygen diffusion flame. Upon leaving the flame, agglomerates of known electrical mobility size were selected with a differential mobility analyzer (DMA), and their mass was measured with an aerosol particle mass analyzer (APM), resulting in their mass fractal dimension, D(f), and dynamic shape factor, chi. Scanning and transmission electron microscopy (SEM/TEM) images were used to determine primary particle diameter and to qualitatively investigate agglomerate morphology. The DMA-APM measurements were reproducible within 5%, as determined by multiple measurements on different days under the same flame conditions. The effects of flame process variables (oxygen flow rate and mass production rate) on particle characteristics (D(f), and chi) were determined. All generated particles were fractal-like agglomerates with average primary particle diameters of 12-93 nm and D(f) = 1.7-2.4. Increasing the oxygen flow rate decreased primary particle size and D(f), while it increased chi. Increasing the production rate increased the agglomerate and primary particle sizes, and decreased chi without affecting D(f). The effects of oxygen flow rate and particle production rate on primary particle size reported here are in agreement with ex situ measurements in the literature, while the effect of process variables on agglomerate shape (chi) is demonstrated for the first time to our knowledge.

Real-time, controlled OH-initiated oxidation of biogenic secondary organic aerosol

Directory of Open Access Journals (Sweden)

J. G. Slowik

2012-10-01

Full Text Available The chemical complexity of atmospheric organic aerosol (OA requires novel methods for characterization of its components and description of its atmospheric processing-induced transformations. We present the first field deployment of the Toronto Photooxidation Tube (TPOT, a field-deployable flow reactor for the controlled exposure of ambient aerosol to OH radicals. The system alternates between sampling of (1 (unreacted ambient aerosol, (2 aerosol exposed to UV light and subjected to a ~4 to 10 °C temperature increase, and (3 aerosol that is oxidized by OH (in addition to the aforementioned UV exposure/temperature increase. This allows both characterization of the aging process and classification of aerosol in terms of its volatility and reaction-based properties. Summertime measurements by an aerosol mass spectrometer coupled to the TPOT were performed in the remote forest of western Canada, resulting in aerosol dominated by biogenic secondary organic aerosol. Volatilization/UV exposure resulted in an approximately 10 to 25% decrease in organic mass and resulted in a slight increase in oxygenation. OH oxidation resulted in a further organic mass decrease (additional ~25% and yielded an aerosol with O:C values comparable to those characteristic of low volatility, highly oxygenated OA. Most OH-induced changes occurred within ~3 day-equivalents of atmospheric processing, with further reactions generally proceeding at a greatly reduced rate. Positive matrix factorization (PMF analysis of the TPOT data yielded five factors. One factor is related to primary biomass burning organic aerosol, while the others describe oxygenated organic aerosol (OOA components in terms of reactivity and volatility: (1 volatile and reactive; (2 non-volatile and reactive; (3 non-volatile and reactive early-generation product; (4 non-volatile and non-reactive product. This PMF classification of aerosol components directly in terms of reactivity and volatility is enabled by

Steam condensation modelling in aerosol codes

International Nuclear Information System (INIS)

Dunbar, I.H.

1986-01-01

The principal subject of this study is the modelling of the condensation of steam into and evaporation of water from aerosol particles. These processes introduce a new type of term into the equation for the development of the aerosol particle size distribution. This new term faces the code developer with three major problems: the physical modelling of the condensation/evaporation process, the discretisation of the new term and the separate accounting for the masses of the water and of the other components. This study has considered four codes which model the condensation of steam into and its evaporation from aerosol particles: AEROSYM-M (UK), AEROSOLS/B1 (France), NAUA (Federal Republic of Germany) and CONTAIN (USA). The modelling in the codes has been addressed under three headings. These are the physical modelling of condensation, the mathematics of the discretisation of the equations, and the methods for modelling the separate behaviour of different chemical components of the aerosol. The codes are least advanced in area of solute effect modelling. At present only AEROSOLS/B1 includes the effect. The effect is greater for more concentrated solutions. Codes without the effect will be more in error (underestimating the total airborne mass) the less condensation they predict. Data are needed on the water vapour pressure above concentrated solutions of the substances of interest (especially CsOH and CsI) if the extent to which aerosols retain water under superheated conditions is to be modelled. 15 refs

Source identification and airborne chemical characterisation of aerosol pollution from long-range transport over Greenland during POLARCAT summer campaign 2008

Science.gov (United States)

Schmale, J.; Schneider, J.; Ancellet, G.; Quennehen, B.; Stohl, A.; Sodemann, H.; Burkhart, J. F.; Hamburger, T.; Arnold, S. R.; Schwarzenboeck, A.; Borrmann, S.; Law, K. S.

2011-10-01

We deployed an aerosol mass spectrometer during the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols, and Transport) summer campaign in Greenland in June/July 2008 on the research aircraft ATR-42. Online size resolved chemical composition data of submicron aerosol were collected up to 7.6 km altitude in the region 60 to 71° N and 40 to 60° W. Biomass burning (BB) and fossil fuel combustion (FF) plumes originating from North America, Asia, Siberia and Europe were sampled. Transport pathways of detected plumes included advection below 700 hPa, air mass uplifting in warm conveyor belts, and high altitude transport in the upper troposphere. By means of the Lagrangian particle dispersion model FLEXPART, trace gas analysis of O3 and CO, particle size distributions and aerosol chemical composition 48 pollution events were identified and classified into five chemically distinct categories. Aerosol from North American BB consisted of 22% particulate sulphate, while with increasing anthropogenic and Asian influence aerosol in Asian FF dominated plumes was composed of up to 37% sulphate category mean value. Overall, it was found that the organic matter fraction was larger (85%) in pollution plumes than for background conditions (71%). Despite different source regions and emission types the particle oxygen to carbon ratio of all plume classes was around 1 indicating low-volatility highly oxygenated aerosol. The volume size distribution of out-of-plume aerosol showed markedly smaller modes than all other distributions with two Aitken mode diameters of 24 and 43 nm and a geometric standard deviation σg of 1.12 and 1.22, respectively, while another very broad mode was found at 490 nm (σg = 2.35). Nearly pure BB particles from North America exhibited an Aitken mode at 66 nm (σg = 1.46) and an accumulation mode diameter of 392 nm (σg = 1.76). An aerosol lifetime, including all processes from emission to

Filter-based Aerosol Measurement Experiments using Spherical Aerosol Particles under High Temperature and High Pressure

Energy Technology Data Exchange (ETDEWEB)

Lee, Jong Chan; Jung, Woo Young; Lee, Hyun Chul; Lee, Doo Young [FNC TECH., Yongin (Korea, Republic of)

2016-05-15

Optical Particle Counter (OPC) is used to provide real-time measurement of aerosol concentration and size distribution. Glass fiber membrane filter also be used to measure average mass concentration. Three tests (MTA-1, 2 and 3) have been conducted to study thermal-hydraulic effect, a filtering tendency at given SiO{sub 2} particles. Based on the experimental results, the experiment will be carried out further with a main carrier gas of steam and different aerosol size. The test results will provide representative behavior of the aerosols under various conditions. The aim of the tests, MTA 1, 2 and 3, are to be able to 1) establish the test manuals for aerosol generation, mixing, sampling and measurement system, which defines aerosol preparation, calibration, operating and evaluation method under high pressure and high temperature 2) develop commercial aerosol test modules applicable to the thermal power plant, environmental industry, automobile exhaust gas, chemical plant, HVAC system including nuclear power plant. Based on the test results, sampled aerosol particles in the filter indicate that important parameters affecting aerosol behavior aerosols are 1) system temperature to keep above a evaporation temperature of ethanol and 2) aerosol losses due to the settling by ethanol liquid droplet.

Influence of particle size and chemistry on the cloud nucleating properties of aerosols

Directory of Open Access Journals (Sweden)

P. K. Quinn

2008-02-01

Full Text Available The ability of an aerosol particle to act as a cloud condensation nuclei (CCN is a function of the size of the particle, its composition and mixing state, and the supersaturation of the cloud. In-situ data from field studies provide a means to assess the relative importance of these parameters. During the 2006 Texas Air Quality – Gulf of Mexico Atmospheric Composition and Climate Study (TexAQS-GoMACCS, the NOAA RV Ronald H. Brown encountered a wide variety of aerosol types ranging from marine near the Florida panhandle to urban and industrial in the Houston-Galveston area. These varied sources provided an opportunity to investigate the role of aerosol sources and chemistry in the potential activation of particles to form cloud droplets. Measurements were made of CCN concentrations, aerosol chemical composition in the size range relevant for particle activation in warm clouds, and aerosol size distributions. Variability in aerosol composition was parameterized by the mass fraction of Hydrocarbon-like Organic Aerosol (HOA for particle diameters less than 200 nm (vacuum aerodynamic. The HOA mass fraction in this size range was lowest for marine aerosol and highest for aerosol sampled close to anthropogenic sources. Combining all data from the experiment reveals that composition (defined by HOA mass fraction explains 40% of the variance in the critical diameter for particle activation at the instrumental supersaturation (S of 0.44%. Correlations between HOA mass fraction and aerosol mean diameter show that these two parameters are essentially independent of one another for this data set. We conclude that, based on the variability of the HOA mass fraction observed during TexAQS-GoMACCS, variability in particle composition played a significant role in determining the fraction of particles that could activate to form cloud droplets. Using a simple model based on Köhler theory and the assumption that HOA is insoluble, we estimate the

Identification of secondary aerosol precursors emitted by an aircraft turbofan

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D. Kılıç

2018-05-01

Full Text Available Oxidative processing of aircraft turbine-engine exhausts was studied using a potential aerosol mass (PAM chamber at different engine loads corresponding to typical flight operations. Measurements were conducted at an engine test cell. Organic gases (OGs and particle emissions pre- and post-PAM were measured. A suite of instruments, including a proton-transfer-reaction mass spectrometer (PTR-MS for OGs, a multigas analyzer for CO, CO2, NOx, and an aerosol mass spectrometer (AMS for nonrefractory particulate matter (NR-PM1 were used. Total aerosol mass was dominated by secondary aerosol formation, which was approximately 2 orders of magnitude higher than the primary aerosol. The chemical composition of both gaseous and particle emissions were also monitored at different engine loads and were thrust-dependent. At idling load (thrust 2.5–7 %, more than 90 % of the secondary particle mass was organic and could mostly be explained by the oxidation of gaseous aromatic species, e.g., benzene; toluene; xylenes; tri-, tetra-, and pentamethyl-benzene; and naphthalene. The oxygenated-aromatics, e.g., phenol, furans, were also included in this aromatic fraction and their oxidation could alone explain up to 25 % of the secondary organic particle mass at idling loads. The organic fraction decreased with thrust level, while the inorganic fraction increased. At an approximated cruise load sulfates comprised 85 % of the total secondary particle mass.

Vertical profiles of aerosol mass concentration derived by unmanned airborne in situ and remote sensing instruments during dust events

Science.gov (United States)

Mamali, Dimitra; Marinou, Eleni; Sciare, Jean; Pikridas, Michael; Kokkalis, Panagiotis; Kottas, Michael; Binietoglou, Ioannis; Tsekeri, Alexandra; Keleshis, Christos; Engelmann, Ronny; Baars, Holger; Ansmann, Albert; Amiridis, Vassilis; Russchenberg, Herman; Biskos, George

2018-05-01

In situ measurements using unmanned aerial vehicles (UAVs) and remote sensing observations can independently provide dense vertically resolved measurements of atmospheric aerosols, information which is strongly required in climate models. In both cases, inverting the recorded signals to useful information requires assumptions and constraints, and this can make the comparison of the results difficult. Here we compare, for the first time, vertical profiles of the aerosol mass concentration derived from light detection and ranging (lidar) observations and in situ measurements using an optical particle counter on board a UAV during moderate and weak Saharan dust episodes. Agreement between the two measurement methods was within experimental uncertainty for the coarse mode (i.e. particles having radii > 0.5 µm), where the properties of dust particles can be assumed with good accuracy. This result proves that the two techniques can be used interchangeably for determining the vertical profiles of aerosol concentrations, bringing them a step closer towards their systematic exploitation in climate models.

Investigation of the CCN Activity, BC and UVBC Mass Concentrations of Biomass Burning Aerosols during the 2013 BASELInE Campaign

Science.gov (United States)

Hsiao, Ta-Chih; Ye, Wei-Cheng; Wang, Sheng-Hsiang; Tsay, Si-Chee; Chen, Wei-Nai; Lin, Neng-Huei; Lee, Chung-Te; Hung, Hui-Ming; Chuang, Ming-Tung; Chantara, Somporn

2015-01-01

Biomass-burning (BB) aerosols, acting as cloud condensation nuclei (CCN), can influence cloud microphysical and radiative properties. In this study, we present CCN measured near the BB source regions over northern Southeast Asia (Doi Ang Khang, Thailand) and at downwind receptor areas (Lulin Atmospheric Background Station, Taiwan), focusing exclusively on 13-20 March 2013 as part of 2013 spring campaign of the Seven SouthEast Asian Studies (7-SEAS) intensive observation. One of the campaigns objectives is to characterize BB aerosols serving as CCN in SouthEast Asia (SEA). CCN concentrations were measured by a CCN counter at 5 supersaturation (SS) levels: 0.15%, 0.30%, 0.45%, 0.60%, and 0.75%. In addition, PM2.5 and black carbon mass concentrations were analyzed by using a tapered element oscillating microbalance and an aethalometer. It was found the number-size distributions and the characteristics of hygroscopicity (e.g., activation ratio and k) of BB aerosols in SEA have a strong diurnal pattern, and different behaviors of patterns were characterized under two distinct weather systems. The overall average value was low (0.05-0.1) but comparable with previous CCN studies in other BB source regions. Furthermore, a large fraction of UV-absorbing organic material (UVBC) and high Delta-C among BB aerosols were also observed, which suggest the existence of substantial particulate organic matter in fresh BB aerosols. These data provide the most extensive characterization of BB aerosols in SEA until now.

A model of aerosol evaporation kinetics in a thermodenuder

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C. D. Cappa

2010-05-01

Full Text Available Aerosol thermodenuders provide a measure of particle volatility. The information provided by a thermodenuder is fundamentally related to the kinetics of evaporation and condensation within the device. Here, a time-dependent, multi-component model of particle and gas-phase mass transfer in a thermodenuder is described. This model empirically accounts for the temperature profile along the length of a typical thermodenuder and distinguishes between the influence of the heating section and of the adsorbent denuder section. It is shown that "semi-volatile" aerosol is particularly sensitive to the inclusion of an adsorbent denuder in the model. As expected, the mass loss from evaporation of particles as they pass through the thermodenuder is directly related to the compound vapor pressure, although the assumptions regarding the enthalpy of vaporization are shown to also have a large influence on the overall calculated mass thermograms. The model has been validated by comparison with previously measured mass thermograms for single-component aerosols and is shown to provide reasonable semi-quantitative agreement. The model that has been developed here can be used to provide quantitative understanding of aerosol volatility measurements of single and multi-component aerosol made using thermodenuders that include adsorbent denuder sections.

Speciation Analysis of ¹²⁹I and ¹²⁷I in Aerosols Using Sequential Extraction and Mass Spectrometry Detection

DEFF Research Database (Denmark)

Zhang, Luyuan; Hou, Xiaolin; Xu, Sheng

2015-01-01

A new analytical method has been developed for speciation analysis of 127I and 129I in aerosols collected on polypropylene (PP) filter paper. Iodide, iodate, NaOH soluble iodine, and insoluble iodine were separated from aerosols using sequential extraction, chromatography separation, and alkaline...... ashing and measured using inductive coupled plasma mass spectrometry (ICP-MS) for 127I and accelerator mass spectrometry (AMS) for 129I. Parameters affecting the leaching efficiency and stability of iodine species, such as leaching time and temperature, amount of alkaline reagent for ashing, ashing...... temperature and time, and iodine protective agent, were investigated and optimized. It was observed that long time water leaching would change inorganic iodine species due to photochemical oxidation of iodide on the PP filter surface. NaOH leaching can only extract less than 60% of iodine from the studied...

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.

Studies on aerosol properties during ICARB–2006 campaign period ...

Indian Academy of Sciences (India)

Synchronous measurements of Aerosol Optical Depth (AOD), Black Carbon (BC) aerosol mass concentration and aerosol particle size distribution were carried out during the campaign period at tropical urban regions of Hyderabad, India. Daily satellite datasets of DMSP-OLS were processed for night-time forest fires over ...

Comparison of three aerosol chemical characterization techniques utilizing PTR-ToF-MS: a study on freshly formed and aged biogenic SOA

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G. I. Gkatzelis

2018-03-01

Full Text Available An intercomparison of different aerosol chemical characterization techniques has been performed as part of a chamber study of biogenic secondary organic aerosol (BSOA formation and aging at the atmosphere simulation chamber SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction chamber. Three different aerosol sampling techniques – the aerosol collection module (ACM, the chemical analysis of aerosol online (CHARON and the collection thermal-desorption unit (TD were connected to proton transfer reaction time-of-flight mass spectrometers (PTR-ToF-MSs to provide chemical characterization of the SOA. The techniques were compared among each other and to results from an aerosol mass spectrometer (AMS and a scanning mobility particle sizer (SMPS. The experiments investigated SOA formation from the ozonolysis of β-pinene, limonene, a β-pinene–limonene mix and real plant emissions from Pinus sylvestris L. (Scots pine. The SOA was subsequently aged by photo-oxidation, except for limonene SOA, which was aged by NO3 oxidation. Despite significant differences in the aerosol collection and desorption methods of the PTR-based techniques, the determined chemical composition, i.e. the same major contributing signals, was found by all instruments for the different chemical systems studied. These signals could be attributed to known products expected from the oxidation of the examined monoterpenes. The sampling and desorption method of ACM and TD provided additional information on the volatility of individual compounds and showed relatively good agreement. Averaged over all experiments, the total aerosol mass recovery compared to an SMPS varied within 80 ± 10, 51 ± 5 and 27 ± 3 % for CHARON, ACM and TD, respectively. Comparison to the oxygen-to-carbon ratios (O : C obtained by AMS showed that all PTR-based techniques observed lower O : C ratios, indicating a loss of molecular oxygen either during aerosol sampling or

Multi-compartment Aerosol Transport Model

Energy Technology Data Exchange (ETDEWEB)

Hubbard, Joshua Allen; Santarpia, Joshua; Brotherton, Christopher M.; Omana, Michael Alexis; Rivera, Danielle; Lucero, Gabriel Anthony

2017-06-01

A simple aerosol transport model was developed for a multi-compartmented cleanroom. Each compartment was treated as a well-mixed volume with ventilating supply and return air. Gravitational settling, intercompartment transport, and leakage of exterior air into the system were included in the model. A set of first order, coupled, ordinary differential equations was derived from the conservation equations of aerosol mass and air mass. The system of ODEs was then solved in MATLAB using pre-existing numerical methods. The model was verified against cases of (1) constant inlet-duct concentration, and (2) exponentially decaying inlet-duct concentration. Numerical methods resulted in normalized error of less than 10 -9 when model solutions were compared to analytical solutions. The model was validated against experimental measurements from a single field test and showed good agreement in the shape and magnitude of the aerosol concentration profile with time.

Pulmonary deposition of urban atmospheric aerosol. Assessments of the mass, number and surface of the deposited particles; Deposizione polmonare dell'aerosol atmosferico urbano in termini di massa, numero e superficie delle particelle

Energy Technology Data Exchange (ETDEWEB)

Luciani, A.; Berico, M.; Castellani, C.M. [ENEA, Centro Ricerche Ezio Clementel, Bologna (Italy). Dipt. Ambiente

1998-07-01

Pulmonary deposition of urban atmospheric aerosol has been calculated by means of the data derived from March 1995 measurement campaign of urban aerosol. The human respiratory tract model of the International Commission on Radiological Protection (n. 66) developed for radiation protection purposes has been used. The number and surface of the deposited particles, as well as the mass, have been also evaluated. [Italian] I dati relativi alla campagna di misure effettuata nel marzo 1995 sono stati rielaborati al fine di valutare la deposizione polmonare dell'aerosol atmosferico in area urbana. Le valutazioni di deposizione nel tratto respiratorio umano sono state condotte mediante l'utilizzo del modello del tratto respiratorio umano presentato per fini radioprotezionistici dalla International Commission on Radiological Protection (n. 66). Sono state effettuate valutazioni di deposizione in massa e in termini di numero e superficie delle particelle.

Optical, physical and chemical properties of aerosols transported to a coastal site in the western Mediterranean: a focus on primary marine aerosols

Directory of Open Access Journals (Sweden)

M. Claeys

2017-06-01

Full Text Available As part of the ChArMEx-ADRIMED campaign (summer 2013, ground-based in situ observations were conducted at the Ersa site (northern tip of Corsica; 533 m a.s.l. to characterise the optical, physical and chemical properties of aerosols. During the observation period, a major influence of primary marine aerosols was detected (22–26 June, with a mass concentration reaching up to 6.5 µg m−3 and representing more than 40 % of the total PM10 mass concentration. Its relatively low ratio of chloride to sodium (average of 0.57 indicates a fairly aged sea salt aerosol at Ersa. In this work, an original data set, obtained from online real-time instruments (ATOFMS, PILS-IC has been used to characterise the ageing of primary marine aerosols (PMAs. During this PMA period, the mixing of fresh and aged PMAs was found to originate from both local and regional (Gulf of Lion emissions, according to local wind measurements and FLEXPART back trajectories. Two different aerosol regimes have been identified: a dust outbreak (dust originating from Algeria/Tunisia, and a pollution period with aerosols originating from eastern Europe, which includes anthropogenic and biomass burning sources (BBP. The optical, physical and chemical properties of the observed aerosols, as well as their local shortwave (SW direct radiative effect (DRE in clear-sky conditions, are compared for these three periods in order to assess the importance of the direct radiative impact of PMAs compared to other sources above the western Mediterranean Basin. As expected, AERONET retrievals indicate a relatively low local SW DRF during the PMA period with mean values of −11 ± 4 at the surface and −8 ± 3 W m−2 at the top of the atmosphere (TOA. In comparison, our results indicate that the dust outbreak observed at our site during the campaign, although of moderate intensity (AOD of 0.3–0.4 at 440 nm and column-integrated SSA of 0.90–0.95, induced a local

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

PM 2.5 mass concentrations in comparison with aerosol optical depths over the Arabian Sea and Indian Ocean during winter monsoon

Science.gov (United States)

Ramachandran, S.

An analysis of PM 2.5 mass concentrations and 0.5 μm aerosol optical depths (AODs) during the Northeast winter monsoon seasons of 1996-2000 is performed and intercompared. AODs are found to show diurnal variations over Coastal India (CI) (west coast) while they are relatively smooth over the Arabian Sea (AS) (5-20°N) and tropical Indian Ocean (TIO) (5°N-20°S). PM 2.5, PM 10 and total mass concentrations show less variations in a day over these oceanic regions. Columnar AODs are found to increase with an increase in the marine boundary layer aerosol concentrations over CI and AS while an opposite trend is seen over TIO. The yearly-mean AODs and mass concentrations are found to increase over CI and AS, over TIO the mass concentrations increased while the AODs decreased during 1996-2000. It is found from the 7-days air back trajectory analyses that at different altitudes air masses can originate from different source regions leading to changes in chemical, physical and optical characteristics of the aerosol between the surface and column. The differences in the surface and columnar measurements could also occur due to changes in the meteorological conditions, wind patterns, in addition to changes in production and subsequently the transport of aerosols. Least-squares fits to the above intercomparison resulted in intercepts of 0.24 and 0.22 over CI and AS indicating that the background AODs over these oceanic regions are higher. An examination of the daily-mean wind speeds and PM 2.5 mass concentrations yielded an index of wind dependence of 0.04 for AS and 0.07 for TIO. The background PM 2.5 mass concentrations are also found to be high at 36 and 25 μg m -3 over AS and TIO, respectively, indicating a stronger influence from the continent. Frequency distribution figures show that 28% of the PM 2.5 values over CI lie in the 60-80 μg m -3 range. Over AS the dominant mode of distribution is 40-60 μg m -3 with a peak value of 42%. Over TIO PM 2.5 values are found to

Mass spectra features of biomass burning boiler and coal burning boiler emitted particles by single particle aerosol mass spectrometer.

Science.gov (United States)

Xu, Jiao; Li, Mei; Shi, Guoliang; Wang, Haiting; Ma, Xian; Wu, Jianhui; Shi, Xurong; Feng, Yinchang

2017-11-15

In this study, single particle mass spectra signatures of both coal burning boiler and biomass burning boiler emitted particles were studied. Particle samples were suspended in clean Resuspension Chamber, and analyzed by ELPI and SPAMS simultaneously. The size distribution of BBB (biomass burning boiler sample) and CBB (coal burning boiler sample) are different, as BBB peaks at smaller size, and CBB peaks at larger size. Mass spectra signatures of two samples were studied by analyzing the average mass spectrum of each particle cluster extracted by ART-2a in different size ranges. In conclusion, BBB sample mostly consists of OC and EC containing particles, and a small fraction of K-rich particles in the size range of 0.2-0.5μm. In 0.5-1.0μm, BBB sample consists of EC, OC, K-rich and Al_Silicate containing particles; CBB sample consists of EC, ECOC containing particles, while Al_Silicate (including Al_Ca_Ti_Silicate, Al_Ti_Silicate, Al_Silicate) containing particles got higher fractions as size increase. The similarity of single particle mass spectrum signatures between two samples were studied by analyzing the dot product, results indicated that part of the single particle mass spectra of two samples in the same size range are similar, which bring challenge to the future source apportionment activity by using single particle aerosol mass spectrometer. Results of this study will provide physicochemical information of important sources which contribute to particle pollution, and will support source apportionment activities. Copyright © 2017. Published by Elsevier B.V.

ORILAM, a three-moment lognormal aerosol scheme for mesoscale atmospheric model: Online coupling into the Meso-NH-C model and validation on the Escompte campaign

Science.gov (United States)

Tulet, Pierre; Crassier, Vincent; Cousin, Frederic; Suhre, Karsten; Rosset, Robert

2005-09-01

Classical aerosol schemes use either a sectional (bin) or lognormal approach. Both approaches have particular capabilities and interests: the sectional approach is able to describe every kind of distribution, whereas the lognormal one makes assumption of the distribution form with a fewer number of explicit variables. For this last reason we developed a three-moment lognormal aerosol scheme named ORILAM to be coupled in three-dimensional mesoscale or CTM models. This paper presents the concept and hypothesis of a range of aerosol processes such as nucleation, coagulation, condensation, sedimentation, and dry deposition. One particular interest of ORILAM is to keep explicit the aerosol composition and distribution (mass of each constituent, mean radius, and standard deviation of the distribution are explicit) using the prediction of three-moment (m0, m3, and m6). The new model was evaluated by comparing simulations to measurements from the Escompte campaign and to a previously published aerosol model. The numerical cost of the lognormal mode is lower than two bins of the sectional one.

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

Influence of aerosol acidity on the chemical composition of secondary organic aerosol from β-caryophyllene

Directory of Open Access Journals (Sweden)

E. M. Knipping

2011-02-01

Full Text Available The secondary organic aerosol (SOA yield of β-caryophyllene photooxidation is enhanced by aerosol acidity. In the present study, the influence of aerosol acidity on the chemical composition of β-caryophyllene SOA is investigated using ultra performance liquid chromatography/electrospray ionization-time-of-flight mass spectrometry (UPLC/ESI-TOFMS. A number of first-, second- and higher-generation gas-phase products having carbonyl and carboxylic acid functional groups are detected in the particle phase. Particle-phase reaction products formed via hydration and organosulfate formation processes are also detected. Increased acidity leads to different effects on the abundance of individual products; significantly, abundances of organosulfates are correlated with aerosol acidity. To our knowledge, this is the first detection of organosulfates and nitrated organosulfates derived from a sesquiterpene. The increase of certain particle-phase reaction products with increased acidity provides chemical evidence to support the acid-enhanced SOA yields. Based on the agreement between the chromatographic retention times and accurate mass measurements of chamber and field samples, three β-caryophyllene products (i.e., β-nocaryophyllon aldehyde, β-hydroxynocaryophyllon aldehyde, and β-dihydroxynocaryophyllon aldehyde are suggested as chemical tracers for β-caryophyllene SOA. These compounds are detected in both day and night ambient samples collected in downtown Atlanta, GA and rural Yorkville, GA during the 2008 August Mini-Intensive Gas and Aerosol Study (AMIGAS.

Seasonal dependence of aerosol processing in urban Philadelphia

Science.gov (United States)

Avery, A. M.; Waring, M. S.; DeCarlo, P. F.

2017-12-01

Urban aerosols pose an important threat to human health due to the conflation of emissions and concentrated population exposed. Winter and summer aerosol and trace gas measurements were taken in downtown Philadelphia in 2016. Measurements included aerosol composition and size with an Aerodyne Aerosol Mass Spectrometer (AMS), particle size distributions with an SMPS, and an aethalometer. Trace gas measurements of O3, NO, CH4, CO, and CO2 were taken concurrently. Sampling in seasonal extremes provided contrast in aerosol and trace gas composition, aerosol processing, and emission factors. Inorganic aerosol components contributed approximately 60% of the submicron aerosol mass, while summertime aerosol composition was roughly 70% organic matter. Positive Matrix Factorization (PMF) on the organic aerosol (OA) matrix revealed three factors in common in each season, including an oxygenated organic aerosol (OOA) factor with different temporal behavior in each season. In summertime, OOA varied diurnally with ozone and daytime temperature, but in the wintertime, it was anti-correlated with ozone and temperature, and instead trended with calculated liquid water, indicating a seasonally-dependent processing of organic aerosol in Philadelphia's urban environment. Due to the inorganic dominant winter aerosol, liquid water much higher (2.65 μg/m3) in winter than in summer (1.54 μg/m3). Diurnally varying concentrations of background gas phase species (CH4, CO2) were higher in winter and varied less as a result of boundary layer conditions; ozone was also higher in background in winter than summer. Winter stagnation events with low windspeed showed large buildup of trace gases CH4, CO, CO2, and NO. Traffic related aerosol was also elevated with black carbon and hydrocarbon-like OA (HOA) plumes of each at 3-5 times higher than the winter the average value for each. Winter ratios of HOA to black carbon were significantly higher in the winter than the summer due to lower

Detailed Source-Specific Molecular Composition of Ambient Aerosol Organic Matter Using Ultrahigh Resolution Mass Spectrometry and 1H NMR

Directory of Open Access Journals (Sweden)

Amanda S. Willoughby

2016-06-01

Full Text Available Organic aerosols (OA are universally regarded as an important component of the atmosphere that have far-ranging impacts on climate forcing and human health. Many of these impacts are related to OA molecular characteristics. Despite the acknowledged importance, current uncertainties related to the source apportionment of molecular properties and environmental impacts make it difficult to confidently predict the net impacts of OA. Here we evaluate the specific molecular compounds as well as bulk structural properties of total suspended particulates in ambient OA collected from key emission sources (marine, biomass burning, and urban using ultrahigh resolution mass spectrometry (UHR-MS and proton nuclear magnetic resonance spectroscopy (1H NMR. UHR-MS and 1H NMR show that OA within each source is structurally diverse, and the molecular characteristics are described in detail. Principal component analysis (PCA revealed that (1 aromatic nitrogen species are distinguishing components for these biomass burning aerosols; (2 these urban aerosols are distinguished by having formulas with high O/C ratios and lesser aromatic and condensed aromatic formulas; and (3 these marine aerosols are distinguished by lipid-like compounds of likely marine biological origin. This study provides a unique qualitative approach for enhancing the chemical characterization of OA necessary for molecular source apportionment.

Production of Highly Charged Pharmaceutical Aerosols Using a New Aerosol Induction Charger.

Science.gov (United States)

Golshahi, Laleh; Longest, P Worth; Holbrook, Landon; Snead, Jessica; Hindle, Michael

2015-09-01

Properly charged particles can be used for effective lung targeting of pharmaceutical aerosols. The objective of this study was to characterize the performance of a new induction charger that operates with a mesh nebulizer for the production of highly charged submicrometer aerosols to bypass the mouth-throat and deliver clinically relevant doses of medications to the lungs. Variables of interest included combinations of model drug (albuterol sulfate) and charging excipient (NaCl) as well as strength of the charging field (1-5 kV/cm). Aerosol charge and size were measured using a modified electrical low pressure impactor system combined with high performance liquid chromatography. At the approximate mass median aerodynamic diameter (MMAD) of the aerosol (~0.4 μm), the induction charge on the particles was an order of magnitude above the field and diffusion charge limit. The nebulization rate was 439.3 ± 42.9 μl/min, which with a 0.1% w/v solution delivered 419.5 ± 34.2 μg of medication per minute. A new correlation was developed to predict particle charge produced by the induction charger. The combination of the aerosol induction charger and predictive correlations will allow for the practical generation and control of charged submicrometer aerosols for targeting deposition within the lungs.

Sources and composition of submicron organic mass in marine aerosol particles

Science.gov (United States)

Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

2014-11-01

The sources and composition of atmospheric marine aerosol particles (aMA) have been investigated with a range of physical and chemical measurements from open-ocean research cruises. This study uses the characteristic functional group composition (from Fourier transform infrared spectroscopy) of aMA from five ocean regions to show the following: (i) The organic functional group composition of aMA that can be identified as mainly atmospheric primary marine (ocean derived) aerosol particles (aPMA) is 65 ± 12% hydroxyl, 21 ± 9% alkane, 6 ± 6% amine, and 7 ± 8% carboxylic acid functional groups. Contributions from photochemical reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal or continental emissions mix in alkane and carboxylic acid groups. (ii) The organic composition of aPMA is nearly identical to model-generated primary marine aerosol particles from bubbled seawater (gPMA, which has 55 ± 14% hydroxyl, 32 ± 14% alkane, and 13 ± 3% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied and the ratio of organic carbon to sodium (OC/Na+) in the gPMA remained nearly constant over a broad range of chlorophyll a concentrations, the gPMA alkane group fraction appeared to increase with chlorophyll a concentrations (r = 0.66). gPMA from productive seawater had a larger fraction of alkane functional groups (42 ± 9%) compared to gPMA from nonproductive seawater (22 ± 10%), perhaps due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of

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�

Heterogeneous formation of HONO on carbonaceous aerosol

Energy Technology Data Exchange (ETDEWEB)

Ammann, M.; Kalberer, M.; Tabor, K. [Paul Scherrer Inst. (PSI), Villigen (Switzerland)] [and others

1997-09-01

Based on an on-line and in situ experimental approach, for the first time heterogeneous production of nitrous acid (HONO) on carbon aerosol at ambient pressure and low NO{sub 2} concentration has been quantified by use of a {sup 13}N tracer technique. (author) 1 fig., 4 refs.

Organic Aerosol Component (OACOMP) Value-Added Product Report

Energy Technology Data Exchange (ETDEWEB)

Fast, J; Zhang, Q; Tilp, A; Shippert, T; Parworth, C; Mei, F

2013-08-23

Significantly improved returns in their aerosol chemistry data can be achieved via the development of a value-added product (VAP) of deriving OA components, called Organic Aerosol Components (OACOMP). OACOMP is primarily based on multivariate analysis of the measured organic mass spectral matrix. The key outputs of OACOMP are the concentration time series and the mass spectra of OA factors that are associated with distinct sources, formation and evolution processes, and physicochemical properties.

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

Directory of Open Access Journals (Sweden)

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

Operation manual for the INEL on-line mass-separator facility

International Nuclear Information System (INIS)

Anderl, R.A.

1984-06-01

This report is an operation manual for an on-line mass-separator facility which is located in Building 661 at the Test Reactor Area of the Idaho National Engineering Laboratory. The facility provides mass-separated sources of short-lived fission-product radionuclides whose decay properties can be studied using a variety of nuclear spectroscopic techniques. This facility is unique in that it utilizes the gas-jet technique to transport fission products from a 252 Cf source located in a hot cell to the ion source of the mass separator. This document includes the following: (a) a detailed description of the facility, (b) identification of equipment hazards and safety controls, (c) detailed operating procedures for startup, continuous operation and shutdown, (d) operating procedures for the californium hot cell, and (e) an operator's manual for the automated moving tape collector/data acquisition system. 7 references, 16 figures, 8 tables

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.

Structure sensitivity of methanol electrooxidation pathways on platinum : an on-line electrochemical mass spectrometry study

NARCIS (Netherlands)

Housmans, T.H.M.; Wonders, A.H.; Koper, M.T.M.

2006-01-01

By monitoring the mass fractions of CO2 (m/z 44) and methylformate (m/z 60, formed from CH3OH + HCOOH) with on-line electrochemical mass spectrometry (OLEMS), the selectivity and structure sensitivity of the methanol oxidation pathways were investigated on the basal planesPt(111), Pt(110), and

Future aerosols of the southwest - Implications for fundamental aerosol research

International Nuclear Information System (INIS)

Friedlander, S.K.

1980-01-01

It is shown that substantial increases in the use of coal in the U.S. will lead to substantial increases in emissions of particulate matter, SO/sub x/, and NO/sub x/ in the part of the U.S. west of the Mississippi. A shift in the primary particulate emissions from coarse to submicron particles is predicted. Attention is given to the nature of the submicron aerosol in the southwest, the distribution of sulfur with respect to particle size, the formation of new particles in the atmosphere, and the ammonium nitrate equilibrium. It is concluded that increased coal use will result in a 50% increase in SO/sub x/ emissions and a doubling of NO/sub x/ emissions in the western U.S. by the year 2000, that ambient levels of aerosol sulfates and nitrates will increase, and that a large increase in submicron aerosol mass is likely

Aerosols behavior inside a PWR during an accident

International Nuclear Information System (INIS)

Hervouet, C.

1983-01-01

During very hypothetical accidents occurring in a pressurized water ractor, radioactive aerosols can be released, during core-melt, inside the reactor containment building. A good knowledge of their behavior in the humid containment atmosphere (mass concentration and size distribution) is essential in order to evaluate their harmfulness in case of environment contamination and to design possible filtration devices. Accordingly the Safety Analysis Department of the Atomic Energy Commission uses several computer models, describing the particle formation (BOIL/MARCH), then behavior in the primary circuits (TRAP-MELT), and in the reactor containment building (AEROSOLS-PARFDISEKO-III B). On the one hand, these models have been improved, in particular the one related to the aerosol formation (nature and mass of released particles) using recent experimental results. On the other hand, sensitivity analyses have been performed with the AEROSOLS code which emphasize the particle coagulation parameters: agglomerate shape factors and collision efficiency. Finally, the different computer models have been applied to the study of aerosol behavior during a 900 MWe PWR accident: loss-of-coolant-accident (small break with failure of all safety systems) [fr

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

Science.gov (United States)

Adler, G.; Flores, J. M.; Abo Riziq, A.; Borrmann, S.; Rudich, Y.

2011-02-01

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.

Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea ice

Directory of Open Access Journals (Sweden)

R. S. Humphries

2016-02-01

Full Text Available Better characterisation of aerosol processes in pristine, natural environments, such as Antarctica, have recently been shown to lead to the largest reduction in uncertainties in our understanding of radiative forcing. Our understanding of aerosols in the Antarctic region is currently based on measurements that are often limited to boundary layer air masses at spatially sparse coastal and continental research stations, with only a handful of studies in the vast sea-ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the icebreaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3 concentrations exhibited a five-fold increase moving across the polar front, with mean polar cell concentrations of 1130 cm−3 – higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low-pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air masses quickly from the free troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea-ice boundary layer air masses travelled equatorward into the low-albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei which, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and their transport pathways described here, could help reduce the discrepancy currently present between

Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea ice

Science.gov (United States)

Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Keywood, M.; Ward, J.; Wilson, S. R.

2016-02-01

Better characterisation of aerosol processes in pristine, natural environments, such as Antarctica, have recently been shown to lead to the largest reduction in uncertainties in our understanding of radiative forcing. Our understanding of aerosols in the Antarctic region is currently based on measurements that are often limited to boundary layer air masses at spatially sparse coastal and continental research stations, with only a handful of studies in the vast sea-ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the icebreaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the polar front, with mean polar cell concentrations of 1130 cm-3 - higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low-pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air masses quickly from the free troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea-ice boundary layer air masses travelled equatorward into the low-albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei which, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and their transport pathways described here, could help reduce the discrepancy currently present between simulations and observations of

Aerosol characterization in smoke plumes from a wetlands fire

International Nuclear Information System (INIS)

Woods, D.C.; Cofer, W.R. III; Levine, J.S.; Chuan, R.L.

1991-01-01

In this chapter, the authors present results from airborne measurements of aerosol mass loading, size distribution, and elemental composition obtained in a smoke plume from the burning of vegetation at a Florida wildlife refuge. These are important parameters in assessing the impact of biomass burning on the atmosphere. The results show that there was a high concentration of carbon-containing aerosols and salt crystals in the 0.1 μm to 0.2 μm size range, giving rise to a relatively strong fine particle size mode, during the hot flaming phase of the burning, compared to that during the smoldering phase, when a higher concentration of coarse particles were produced. They also found that the composition and morphology of the aerosols differed with size. They used the aerosol mass concentration along with CO 2 concentrations to calculate ratios or aerosol and CO 2 , which we found to be higher for the smoldering phase than for the flaming phase of combustion

Experience with Aerosol Generation During Rotary Mode Core Sampling in the Hanford Single Shell Waste Tanks

International Nuclear Information System (INIS)

SCHOFIELD, J.S.

1999-01-01

This document provides data on aerosol concentrations in tank head spaces, total mass of aerosols in the tank head space and mass of aerosols sent to the exhauster during Rotary Mode Core Sampling from November 1994 through April 1999

Aerosol-ozone correlations during dust transport episodes

Directory of Open Access Journals (Sweden)

P. Bonasoni

2004-01-01

Full Text Available Its location in the Mediterranean region and its physical characteristics render Mt. Cimone (44°11′ N, 10°42′ E, the highest peak of the Italian northern Apennines (2165 m asl, particularly suitable to study the transport of air masses from the north African desert area to Europe. During these northward transports 12 dust events were registered in measurements of the aerosol concentration at the station during the period June–December 2000, allowing the study of the impact of mineral dust transports on free tropospheric ozone concentrations, which were also measured at Mt. Cimone. Three-dimensional backward trajectories were used to determine the air mass origin, while TOMS Aerosol Index data for the Mt. Cimone area were used to confirm the presence of absorbing aerosol over the measurement site. A trajectory statistical analysis allowed identifying the main source areas of ozone and aerosols. The analysis of these back trajectories showed that central Europe and north and central Italy are the major pollution source areas for ozone and fine aerosol, whereas the north African desert regions were the most important source areas for coarse aerosol and low ozone concentrations. During dust events, the Mt. Cimone mean volume concentration for coarse particles was 6.18 µm3/cm3 compared to 0.63 µm3/cm3 in dust-free conditions, while the ozone concentrations were 4% to 21% lower than the monthly mean background values. Our observations show that surface ozone concentrations were lower than the background values in air masses coming from north Africa, and when these air masses were also rich in coarse particles, the lowest ozone values were registered. Moreover, preliminary results on the possible impact of the dust events on PM10 and ozone values measured in Italian urban and rural areas showed that during the greater number of the considered dust events, significant PM10 increases and ozone decreases have occurred in the Po valley.

Modeling aerosol suspension from soils and oceans as sources of micropollutants to air.

Science.gov (United States)

Qureshi, Asif; MacLeod, Matthew; Hungerbühler, Konrad

2009-10-01

Soil and marine aerosol suspension are two physical mass transfer processes that are not usually included in models describing fate and transport of environmental pollutants. Here, we review the literature on soil and marine aerosol suspension and estimate aerosol suspension mass transfer velocities for inclusion in multimedia models, as a global average and on a 1 x 1 scale. The yearly, global average mass transfer velocity for soil aerosol suspension is estimated to be 6 x 10(-10)mh(-1), approximately an order of magnitude smaller than marine aerosol suspension, which is estimated to be 8 x 10(-9)mh(-1). Monthly averages of these velocities can be as high as 10(-7)mh(-1) and 10(-5)mh(-1) for soil and marine aerosol suspension, respectively, depending on location. We use a unit-world multimedia model to analyze the relevance of these two suspension processes as a mechanism that enhances long-range atmospheric transport of pollutants. This is done by monitoring a metric of long-range transport potential, phi-one thousand (phi1000), that denotes the fraction of modeled emissions to air, water or soil in a source region that reaches a distance of 1000 km in air. We find that when the yearly, globally averaged mass transfer velocity is used, marine aerosol suspension increases phi1000 only fractionally for both emissions to air and water. However, enrichment of substances in marine aerosols, or speciation between ionic and neutral forms in ocean water may increase the influence of this surface-to-air transfer process. Soil aerosol suspension can be the dominant process for soil-to-air transfer in an emission-to-soil scenario for certain substances that have a high affinity to soil. When a suspension mass transfer velocity near the maximum limit is used, soil suspension remains important if the emissions are made to soil, and marine aerosol suspension becomes important regardless of if emissions are made to air or water compartments. We recommend that multimedia models

Factors Affecting Aerosol Radiative Forcing

Science.gov (United States)

Wang, J.; Lin, J.; Ni, R.

2016-12-01

Rapid industrial and economic growth has meant large amount of aerosols in the atmosphere with strong radiative forcing (RF) upon the climate system. Over parts of the globe, the negative forcing of aerosols has overcompensated for the positive forcing of greenhouse gases. Aerosol RF is determined by emissions and various chemical-transport-radiative processes in the atmosphere, a multi-factor problem whose individual contributors have not been well quantified. In this study, we analyze the major factors affecting RF of secondary inorganic aerosols (SIOAs, including sulfate, nitrate and ammonium), primary organic aerosol (POA), and black carbon (BC). We analyze the RFof aerosols produced by 11 major regions across the globe, including but not limited to East Asia, Southeast Asia, South Asia, North America, and Western Europe. Factors analyzed include population size, per capita gross domestic production (GDP), emission intensity (i.e., emissionsper unit GDP), chemical efficiency (i.e., mass per unit emissions) and radiative efficiency (i.e., RF per unit mass). We find that among the 11 regions, East Asia produces the largest emissions and aerosol RF, due to relatively high emission intensity and a tremendous population size.South Asia produce the second largest RF of SIOA and BC and the highest RF of POA, in part due to its highest chemical efficiency among all regions. Although Southeast Asia also has large emissions,its aerosol RF is alleviated by its lowest chemical efficiency.The chemical efficiency and radiative efficiency of BC produced by the Middle East-North Africa are the highest across the regions, whereas its RF is loweredbyasmall per capita GDP.Both North America and Western Europe have low emission intensity, compensating for the effects on RF of large population sizes and per capita GDP. There has been a momentum to transfer industries to Southeast Asia and South Asia, and such transition is expected to continue in the coming years. The resulting

Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea-ice

Science.gov (United States)

Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Keywood, M.; Ward, J.; Wilson, S. R.

2015-10-01

The effect of aerosols on clouds and their radiative properties is one of the largest uncertainties in our understanding of radiative forcing. A recent study has concluded that better characterisation of pristine, natural aerosol processes leads to the largest reduction in these uncertainties. Antarctica, being far from anthropogenic activities, is an ideal location for the study of natural aerosol processes. Aerosol measurements in Antarctica are often limited to boundary layer air-masses at spatially sparse coastal and continental research stations, with only a handful of studies in the sea ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the ice-breaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the Polar Front, with mean Polar Cell concentrations of 1130 cm-3 - higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air-masses quickly from the free-troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea ice boundary layer air-masses travelled equator-ward into the low albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei where, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and

Measurements of the aerosol chemical composition and mixing state in the Po Valley using multiple spectroscopic techniques

Science.gov (United States)

Decesari, S.; Allan, J.; Plass-Duelmer, C.; Williams, B. J.; Paglione, M.; Facchini, M. C.; O'Dowd, C.; Harrison, R. M.; Gietl, J. K.; Coe, H.; Giulianelli, L.; Gobbi, G. P.; Lanconelli, C.; Carbone, C.; Worsnop, D.; Lambe, A. T.; Ahern, A. T.; Moretti, F.; Tagliavini, E.; Elste, T.; Gilge, S.; Zhang, Y.; Dall'Osto, M.

2014-11-01

The use of co-located multiple spectroscopic techniques can provide detailed information on the atmospheric processes regulating aerosol chemical composition and mixing state. So far, field campaigns heavily equipped with aerosol mass spectrometers have been carried out mainly in large conurbations and in areas directly affected by their outflow, whereas lesser efforts have been dedicated to continental areas characterised by a less dense urbanisation. We present here the results obtained at a background site in the Po Valley, Italy, in summer 2009. For the first time in Europe, six state-of-the-art spectrometric techniques were used in parallel: aerosol time-of-flight mass spectrometer (ATOFMS), two aerosol mass spectrometers (high-resolution time-of-flight aerosol mass spectrometer - HR-ToF-AMS and soot particle aerosol mass spectrometer - SP-AMS), thermal desorption aerosol gas chromatography (TAG), chemical ionisation mass spectrometry (CIMS) and (offline) proton nuclear magnetic resonance (1H-NMR) spectroscopy. The results indicate that, under high-pressure conditions, atmospheric stratification at night and early morning hours led to the accumulation of aerosols produced by anthropogenic sources distributed over the Po Valley plain. Such aerosols include primary components such as black carbon (BC), secondary semivolatile compounds such as ammonium nitrate and amines and a class of monocarboxylic acids which correspond to the AMS cooking organic aerosol (COA) already identified in urban areas. In daytime, the entrainment of aged air masses in the mixing layer is responsible for the accumulation of low-volatility oxygenated organic aerosol (LV-OOA) and also for the recycling of non-volatile primary species such as black carbon. According to organic aerosol source apportionment, anthropogenic aerosols accumulating in the lower layers overnight accounted for 38% of organic aerosol mass on average, another 21% was accounted for by aerosols recirculated in

Variability of aerosol vertical distribution in the Sahel

Directory of Open Access Journals (Sweden)

O. Cavalieri

2010-12-01

Full Text Available In this work, we have studied the seasonal and inter-annual variability of the aerosol vertical distribution over Sahelian Africa for the years 2006, 2007 and 2008, characterizing the different kind of aerosols present in the atmosphere in terms of their optical properties observed by ground-based and satellite instruments, and their sources searched for by using trajectory analysis. This study combines data acquired by three ground-based micro lidar systems located in Banizoumbou (Niger, Cinzana (Mali and M'Bour (Senegal in the framework of the African Monsoon Multidisciplinary Analysis (AMMA, by the AEROsol RObotic NETwork (AERONET sun-photometers and by the space-based Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP onboard the CALIPSO satellite (Cloud-Aerosol Lidar and Infrared Pathfinder Observations.

During winter, the lower levels air masses arriving in the Sahelian region come mainly from North, North-West and from the Atlantic area, while in the upper troposphere air flow generally originates from West Africa, crossing a region characterized by the presence of large biomass burning sources. The sites of Cinzana, Banizoumbou and M'Bour, along a transect of aerosol transport from East to West, are in fact under the influence of tropical biomass burning aerosol emission during the dry season, as revealed by the seasonal pattern of the aerosol optical properties, and by back-trajectory studies.

Aerosol produced by biomass burning are observed mainly during the dry season and are confined in the upper layers of the atmosphere. This is particularly evident for 2006, which was characterized by a large presence of biomass burning aerosols in all the three sites.

Biomass burning aerosol is also observed during spring when air masses originating from North and East Africa pass over sparse biomass burning sources, and during summer when biomass burning aerosol is transported from the southern part of the

Enviro-HIRLAM online integrated meteorology–chemistry modelling system: strategy, methodology, developments and applications (v7.2

Directory of Open Access Journals (Sweden)

A. Baklanov

2017-08-01

Full Text Available The Environment – High Resolution Limited Area Model (Enviro-HIRLAM is developed as a fully online integrated numerical weather prediction (NWP and atmospheric chemical transport (ACT model for research and forecasting of joint meteorological, chemical and biological weather. The integrated modelling system is developed by the Danish Meteorological Institute (DMI in collaboration with several European universities. It is the baseline system in the HIRLAM Chemical Branch and used in several countries and different applications. The development was initiated at DMI more than 15 years ago. The model is based on the HIRLAM NWP model with online integrated pollutant transport and dispersion, chemistry, aerosol dynamics, deposition and atmospheric composition feedbacks. To make the model suitable for chemical weather forecasting in urban areas, the meteorological part was improved by implementation of urban parameterisations. The dynamical core was improved by implementing a locally mass-conserving semi-Lagrangian numerical advection scheme, which improves forecast accuracy and model performance. The current version (7.2, in comparison with previous versions, has a more advanced and cost-efficient chemistry, aerosol multi-compound approach, aerosol feedbacks (direct and semi-direct on radiation and (first and second indirect effects on cloud microphysics. Since 2004, the Enviro-HIRLAM has been used for different studies, including operational pollen forecasting for Denmark since 2009 and operational forecasting atmospheric composition with downscaling for China since 2017. Following the main research and development strategy, further model developments will be extended towards the new NWP platform – HARMONIE. Different aspects of online coupling methodology, research strategy and possible applications of the modelling system, and fit-for-purpose model configurations for the meteorological and air quality communities are discussed.

Behavior of aerosols in a steam-air environment

International Nuclear Information System (INIS)

Adams, R.E.; Tobias, M.L.; Longest, A.W.

1985-01-01

The behavior of aerosols assumed to be characteristic of those generated during light water reactor (LWR) accident sequences and released into containment is being studied in the Nuclear Safety Pilot Plant (NSPP) which is located at the Oak Ridge National Laboratory (ORNL). The program plan for the NSPP aerosol project provides for the study of the behavior, within containment, of simulated LWR accident aerosols emanating from fuel, reactor core structural materials, and from concrete-molten core materials interactions. The aerodynamic behavior of each of these aerosols was studied individually to establish its characteristics; current experiments involve mixtures of these aerosols to establish their interaction and collective behavior within containment. Tests have been conducted with U 3 O 8 aerosols, Fe 2 O 3 aerosols, and concrete aerosols in an environment of either dry air [relative humidity (RH) less than 20%] or steam-air [relative humidity (RH) approximately 100%] with aerosol mass concentration being the primary experimental variable

Evaluation of the new capture vapourizer for aerosol mass spectrometers (AMS) through laboratory studies of inorganic species

Science.gov (United States)

Hu, Weiwei; Campuzano-Jost, Pedro; Day, Douglas A.; Croteau, Philip; Canagaratna, Manjula R.; Jayne, John T.; Worsnop, Douglas R.; Jimenez, Jose L.

2017-08-01

Aerosol mass spectrometers (AMSs) and Aerosol Chemical Speciation Monitors (ACSMs) commercialized by Aerodyne are widely used to measure the non-refractory species in submicron particles. With the standard vapourizer (SV) that is installed in all commercial instruments to date, the quantification of ambient aerosol mass concentration requires the use of the collection efficiency (CE) to correct for the loss of particles due to bounce. A new capture vapourizer (CV) has been designed to reduce the need for a bounce-related CE correction. Two high-resolution AMS instruments, one with a SV and one with a CV, were operated side by side in the laboratory. Four standard species, NH4NO3, NaNO3, (NH4)2SO4 and NH4Cl, which typically constitute the majority of the mass of ambient submicron inorganic species, are studied. The effect of vapourizer temperature (Tv ˜ 200-800 °C) on the detected fragments, CE and size distributions are investigated. A Tv of 500-550 °C for the CV is recommended. In the CV, CE was identical (around unity) for more volatile species (e.g. NH4NO3) and comparable to or higher than the SV for less-volatile species (e.g. (NH4)2SO4), demonstrating an improvement in CE for laboratory inorganic species in the CV. The detected relative intensities of fragments of NO3 and SO4 species observed with the CV are different from those observed with the SV, and are consistent with additional thermal decomposition arising from the increased residence time and multiple collisions. Increased residence times with the CV also lead to broader particle size distribution measurements than with the SV. A method for estimating whether pure species will be detected in AMS sizing mode is proposed. Production of CO2(g) from sampled nitrate on the vapourizer surface, which has been reported for the SV, is negligible for the CV for NH4NO3 and comparable to the SV for NaNO3. . We observe an extremely consistent fragmentation for ammonium compared to very large changes for the

Seasonal variability of aerosol concentration and size distribution in Cape Verde using a continuous aerosol optical spectrometer

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Casimiro Adrião Pio

2014-05-01

Full Text Available One year of, almost continuous, measurements of aerosol optical properties and chemical composition were performed at the outskirts of Praia, Santiago Island, Cape Verde, within the framework of CV-DUST (Atmospheric aerosol in Cape Verde region: seasonal evaluation of composition, sources and transport research project, during 2011. This article reports the aerosol number and mass concentration measurements using a GRIMM Optical Aerosol Spectrometer that provides number size discrimination into 31 size ranges from 0.25 to 32 µm. Time series of 5 min average PM10 concentrations revealed peak values higher than 1000 µg.m-3 during winter dust storm events originating over Northern Africa. The 24 hours average concentrations exceeded the World Health Organization (WHO guidelines for PM2.5 and PM10 in 20% and 30% of the 2001 days, respectively. Annual average mass concentrations (±standard deviation for PM1, PM2.5 and PM10 were 5±5, 19±21 and 48±64 µg.m-3, respectively. The annual PM2.5 and PM10 values were also above the limits prescribed by the WHO (10 and 20 µg.m-3, respectively. The aerosol mass size distribution revealed two main modes for particles smaller than 10 µm: a fine mode (0.7-0.8 µm, which possibly results of gas to particle conversion processes; and a coarse mode with maxima at 3-4 µm, which is associated with desert dust and sea salt sources. Within the coarse mode two sub-modes with maxima at 5-6 µm and 10-12 µm were frequently present.

Reduction of photosynthetically active radiation under extreme stratospheric-aerosol loads

International Nuclear Information System (INIS)

Gerstl, S.A.W.; Zardecki, A.

1981-01-01

The recently published hypothesis that the Cretaceous-Tertiary extinctions might be caused by an obstruction of sunlight is tested by model calculations. First we compute the total mass of stratospheric aerosols under normal atmospheric conditions for four different (measured) aerosol size distributions and vertical profiles. For comparison, the stratospheric dust masses after four volcanic eruptions are also evaluated. Detailed solar radiative transfer calculations are then performed for artificially increased aerosol amounts until the postulated darkness scenario is obtained. Thus we find that a total stratospheric aerosol mass between 1 and 4 times 10 16 g is sufficient to reduce photosynthesis to 10 3 of normal. We also infer from this result that the impact of a 0.4- to 3-km-diameter asteroid or a close encounter with a Halley-size comet may deposit that amount of particulates into the stratosphere. The darkness scenario of Alvarez et al., is thus shown to be a possible extinction mechanism, even with smaller size asteroids or comets than previously estimated

Reduction of photosynthetically active radiation under extreme stratospheric aerosol loads

International Nuclear Information System (INIS)

Gerstl, S.A.W.; Zardecki, A.

1981-08-01

The recently published hypothesis that the Cretaceous-Tertiary extinctions might be caused by an obstruction of sunlight is tested by model calculations. First we compute the total mass of stratospheric aerosols under normal atmospheric conditions for four different (measured) aerosol size distributions and vertical profiles. For comparison, the stratospheric dust masses after four volcanic eruptions are also evaluated. Detailed solar radiative transfer calculations are then performed for artificially increased aerosol amounts until the postulated darkness scenario is obtained. Thus we find that a total stratospheric aerosol mass between 1 and 4 times 10 1 g is sufficient to reduce photosynthesis to 10 -3 of normal. We also infer from this result tha the impact of a 0.4- to 3-km-diameter asteroid or a close encounter with a Halley-size comet may deposit that amount of particulates into the stratosphere. The darkness scenario of Alvarez et al. is thus shown to be a possible extinction mechanism, even with smaller size asteroids of comets than previously estimated

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

The regional aerosol-climate model REMO-HAM

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J.-P. Pietikäinen

2012-11-01

Full Text Available REMO-HAM is a new regional aerosol-climate model. It is based on the REMO regional climate model and includes most of the major aerosol processes. The structure for aerosol is similar to the global aerosol-climate model ECHAM5-HAM, for example the aerosol module HAM is coupled with a two-moment stratiform cloud scheme. On the other hand, REMO-HAM does not include an online coupled aerosol-radiation nor a secondary organic aerosol module. In this work, we evaluate the model and compare the results against ECHAM5-HAM and measurements. Four different measurement sites were chosen for the comparison of total number concentrations, size distributions and gas phase sulfur dioxide concentrations: Hyytiälä in Finland, Melpitz in Germany, Mace Head in Ireland and Jungfraujoch in Switzerland. REMO-HAM is run with two different resolutions: 50 × 50 km² and 10 × 10 km². Based on our simulations, REMO-HAM is in reasonable agreement with the measured values. The differences in the total number concentrations between REMO-HAM and ECHAM5-HAM can be mainly explained by the difference in the nucleation mode. Since we did not use activation nor kinetic nucleation for the boundary layer, the total number concentrations are somewhat underestimated. From the meteorological point of view, REMO-HAM represents the precipitation fields and 2 m temperature profile very well compared to measurement. Overall, we show that REMO-HAM is a functional aerosol-climate model, which will be used in further studies.

Field and Laboratory Studies of Atmospheric Organic Aerosol

Science.gov (United States)

Coggon, Matthew Mitchell

This thesis is the culmination of field and laboratory studies aimed at assessing processes that affect the composition and distribution of atmospheric organic aerosol. An emphasis is placed on measurements conducted using compact and high-resolution Aerodyne Aerosol Mass Spectrometers (AMS). The first three chapters summarize results from aircraft campaigns designed to evaluate anthropogenic and biogenic impacts on marine aerosol and clouds off the coast of California. Subsequent chapters describe laboratory studies intended to evaluate gas and particle-phase mechanisms of organic aerosol oxidation. The 2013 Nucleation in California Experiment (NiCE) was a campaign designed to study environments impacted by nucleated and/or freshly formed aerosol particles. Terrestrial biogenic aerosol with > 85% organic mass was observed to reside in the free troposphere above marine stratocumulus. This biogenic organic aerosol (BOA) originated from the Northwestern United States and was transported to the marine atmosphere during periodic cloud-clearing events. Spectra recorded by a cloud condensation nuclei counter demonstrated that BOA is CCN active. BOA enhancements at latitudes north of San Francisco, CA coincided with enhanced cloud water concentrations of organic species such as acetate and formate. Airborne measurements conducted during the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) were aimed at evaluating the contribution of ship emissions to the properties of marine aerosol and clouds off the coast of central California. In one study, analysis of organic aerosol mass spectra during periods of enhanced shipping activity yielded unique tracers indicative of cloud-processed ship emissions (m/z 42 and 99). The variation of their organic fraction (f42 and f 99) was found to coincide with periods of heavy (f 42 > 0.15; f99 > 0.04), moderate (0.05 controlled organic plume emitted from the R/V Point Sur. Under sunny conditions, nucleated particles composed

Source identification and airborne chemical characterisation of aerosol pollution from long-range transport over Greenland during POLARCAT summer campaign 2008

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J. Schmale

2011-10-01

Full Text Available We deployed an aerosol mass spectrometer during the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols, and Transport summer campaign in Greenland in June/July 2008 on the research aircraft ATR-42. Online size resolved chemical composition data of submicron aerosol were collected up to 7.6 km altitude in the region 60 to 71° N and 40 to 60° W. Biomass burning (BB and fossil fuel combustion (FF plumes originating from North America, Asia, Siberia and Europe were sampled. Transport pathways of detected plumes included advection below 700 hPa, air mass uplifting in warm conveyor belts, and high altitude transport in the upper troposphere. By means of the Lagrangian particle dispersion model FLEXPART, trace gas analysis of O₃ and CO, particle size distributions and aerosol chemical composition 48 pollution events were identified and classified into five chemically distinct categories. Aerosol from North American BB consisted of 22% particulate sulphate, while with increasing anthropogenic and Asian influence aerosol in Asian FF dominated plumes was composed of up to 37% sulphate category mean value. Overall, it was found that the organic matter fraction was larger (85% in pollution plumes than for background conditions (71%. Despite different source regions and emission types the particle oxygen to carbon ratio of all plume classes was around 1 indicating low-volatility highly oxygenated aerosol. The volume size distribution of out-of-plume aerosol showed markedly smaller modes than all other distributions with two Aitken mode diameters of 24 and 43 nm and a geometric standard deviation σ_g of 1.12 and 1.22, respectively, while another very broad mode was found at 490 nm (σ_g = 2.35. Nearly pure BB particles from North America exhibited an Aitken mode at 66 nm (σ_g = 1.46 and an accumulation mode diameter of 392 nm (σ_g = 1

Development of a supercritical fluid extraction-gas chromatography-mass spectrometry method for the identification of highly polar compounds in secondary organic aerosols formed from biogenic hydrocarbons in smog chamber experiments.

Science.gov (United States)

Chiappini, L; Perraudin, E; Durand-Jolibois, R; Doussin, J F

2006-11-01

A new one-step method for the analysis of highly polar components of secondary organic aerosols (SOA) has been developed. This method should lead to a better understanding of SOA formation and evolution since it enables the compounds responsible for SOA formation to be identified. Since it is based on supercritical fluid extraction coupled to gas chromatography-mass spectrometry, it minimizes the analysis time and significantly enhances sensitivity, which makes it suitable for trace-level compounds, which are constituents of SOA. One of the key features of this method is the in situ derivatisation step: an online silylation allowing the measurement of highly polar, polyfunctional compounds, which is a prerequisite for the elucidation of chemical mechanisms. This paper presents the development of this analytical method and highlights its ability to address this major atmospheric issue through the analysis of SOA formed from the ozonolysis of a biogenic hydrocarbon (sabinene). Ozonolysis of sabinene was performed in a 6 m3 Teflon chamber. The aerosol components were derivatised in situ. More than thirty products, such as sabinaketone, sabinic acid and other multifunctional compounds including dicarboxylic acids and oxoacids, were measured. Nine of them were identified and quantified. The sensitivity and the linearity (0.91

Development of a supercritical fluid extraction-gas chromatography-mass spectrometry method for the identification of highly polar compounds in secondary organic aerosols formed from biogenic hydrocarbons in smog chamber experiments

Energy Technology Data Exchange (ETDEWEB)

Chiappini, L.; Perraudin, E.; Durand-Jolibois, R.; Doussin, J.F. [Universites Paris, Laboratoire Interuniversitaire des Systemes Atmospheriques, UMR CNRS 7583, Creteil (France)

2006-11-15

A new one-step method for the analysis of highly polar components of secondary organic aerosols (SOA) has been developed. This method should lead to a better understanding of SOA formation and evolution since it enables the compounds responsible for SOA formation to be identified. Since it is based on supercritical fluid extraction coupled to gas chromatography-mass spectrometry, it minimizes the analysis time and significantly enhances sensitivity, which makes it suitable for trace-level compounds, which are constituents of SOA. One of the key features of this method is the in situ derivatisation step: an online silylation allowing the measurement of highly polar, polyfunctional compounds, which is a prerequisite for the elucidation of chemical mechanisms. This paper presents the development of this analytical method and highlights its ability to address this major atmospheric issue through the analysis of SOA formed from the ozonolysis of a biogenic hydrocarbon (sabinene). Ozonolysis of sabinene was performed in a 6 m{sup 3} Teflon chamber. The aerosol components were derivatised in situ. More than thirty products, such as sabinaketone, sabinic acid and other multifunctional compounds including dicarboxylic acids and oxoacids, were measured. Nine of them were identified and quantified. The sensitivity and the linearity (0.91 < R < 0.98) of the method were both good and detection limits ranged from 1.2 to 6.4 ng for the investigated compounds. (orig.)

Laboratory Measurements of Mass Specific Absorption Spectra for Suites of Black Carbon-like, Biomass Burning and Mineral Dust Aerosols

Science.gov (United States)

Radney, J.; Zangmeister, C.

2017-12-01

Light-absorbing atmospheric aerosols can be grouped into three categories: black carbon (BC), brown carbon (BrC) or mineral dust (MD). In many cases, the absorption of these species is best quantified using a mass-specific absorption cross section (MAC) since the particles are in the Rayleigh regime (BC) or optically thin (BrC and MD); notably, MAC values are both traceable to the SI and transferrable between photoacoustic spectroscopy and filter-based absorption measurements. Here, we present laboratory measurements of MAC for all three light-absorbing aerosol classes. Particles were size- and mass-selected using a differential mobility analyzer and aerosol particle mass analyzer, respectively, with absorption coefficients (αabs) and number concentrations (N) being measured by a broadband photoacoustic spectrometer and condensation particle counter, respectively. This suite of instrumentation allows for direct quantification of MAC from the measured parameters (MAC = αabs/Nmp). Further, the measurements contained > 8 data points spanning λ = 405 nm to 840 nm allowing for spectral curvatures (i.e. the Absorption Angstrom Exponent or AAE) to be fit from many data points versus the more common 2-point interpolations. For the carbonaceous, BC-like aerosols - five samples generated from flames, spark discharge soot (i.e. fullerene soot), graphene, reduced graphene oxide (rGO), and fullerene (C60) - we found: 1) measured MAC ranged between 2.4 m2 g-1 and 8.6 m2 g-1 at λ = 550 nm, 2) most AAEs ranged between 0.5 and 1.3; C60 AAE was 7.5 ± 0.9 and 3) MAC spectra were dependent on fuel type and formation conditions. For BrC particles generated from smoldering combustion of 3 hardwood (Oak, Hickory and Mesquite) and 3 softwood species (Western redcedar, Blue spruce and Baldcypress), we found: 1) median MAC values ranged from 1.4 x 10-2 m2 g-1 to 7.9 x 10-2 m2 g-1 at λ = 550 nm, 2) AAE values ranged between 3.5 and 6.2, and 3) Oak, Western redcedar and Blue spruce

Optical properties and source analysis of aerosols over a desert area in Dunhuang, Northwest china

Science.gov (United States)

Ma, Yongjing; Xin, Jinyuan; Ma, Yining; Kong, Lingbin; Zhang, Kequan; Zhang, Wenyu; Wang, Yuesi; Wang, Xiuqin; Zhu, Yongfeng

2017-08-01

Aerosol observational data for 2012 obtained from Dunhuang Station of CARE-China (Campaign on Atmospheric Aerosol Research Network of China) were analyzed to achieve in-depth knowledge of aerosol optical properties over Dunhuang region. The results showed that the annual average aerosol optical depth (AOD) at 500 nm was 0.32±0.06, and the Ångström exponent ( α) was 0.73 ± 0.27. Aerosol optical properties revealed significant seasonal characteristics. Frequent sandstorms in MAM (March-April-May) resulted in the seasonal maximum AOD, 0.41 ± 0.04, and a relatively smaller α value, 0.44±0.04. The tourism seasons, JJA (June-July-August) and SON (September-October-November) coincide with serious emissions of small anthropogenic aerosols. While in DJF (December-January-February), the composition of the atmosphere was a mixture of dust particles and polluted aerosols released by domestic heating; the average AOD and α were 0.29 ± 0.02 and 0.66 ± 0.17, respectively. Different air masses exhibited different degrees of influence on the aerosol concentration over Dunhuang in different seasons. During MAM, ranges of AOD (0.11-1.18) and α (0.06-0.82) were the largest under the dust influence of northwest-short-distance air mass in the four trajectories. Urban aerosols transported by northwest-short-distance air mass accounted for a very large proportion in JJA and the mixed aerosols observed in SON were mainly conveyed by air masses from the west. In DJF, the similar ranges of AOD and α under the three air mass demonstrated the analogous diffusion effects on regional pollutants over Dunhuang.

Determination of Aerosol Particle Diameter Using Cascade Impactor Procedure

International Nuclear Information System (INIS)

Bunawas; Ruslanto, P. O

1998-01-01

Determination of aerosol particle size distribution has been done using a low pressure Andersen's cascade impactor with 13 stages. The aerosol has been sampled with flow rate of aerosol sampling of 28.3 Ipm. Preliminary study result shows that aerosol in the simulation chamber was spread in monomodal distribution with Mass Median Aerodynamic Diameter of 4.9 μm. The aerosol measurement in Japan Power Demonstration Reactor has been spread in trimodal distribution with Activity Median Aerodynamic Diameter equal to 13.3 μm. The use of mylar as impaction plate instead of aluminum foil gives good result

The Finokalia Aerosol Measurement Experiment – 2008 (FAME-08: an overview

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M. Pikridas

2010-07-01

Full Text Available A month (4 May to 8 June 2008 of ambient aerosol, air ion and gas phase sampling (Finokalia Aerosol Measurement Experiment 2008, FAME-08 was conducted at Finokalia, on the island of Crete, Greece. The purpose of the study was to characterize the physical and chemical properties of aged aerosol and to investigate new particle formation. Measurements included aerosol and air ion size distributions, size-resolved chemical composition, organic aerosol thermal volatility, water uptake and particle optical properties (light scattering and absorption. Statistical analysis of the aerosol mass concentration variations revealed the absence of diurnal patterns suggesting the lack of strong local sources. Sulfates accounted for approximately half of the particulate matter less than 1 micrometer in diameter (PM₁ and organics for 28%. The PM₁ organic aerosol fraction was highly oxidized with 80% water soluble. The supermicrometer particles were dominated by crustal components (50%, sea salt (24% and nitrates (16%. The organic carbon to elemental carbon (OC/EC ratio correlated with ozone measurements but with a one-day lag. The average OC/EC ratio for the study period was equal to 5.4. For three days air masses from North Africa resulted in a 6-fold increase of particulate matter less than 10 micrometers in diameter (PM₁₀ and a decrease of the OC/EC ratio by a factor of 2. Back trajectory analysis, based on FLEXPART footprint plots, identified five source regions (Athens, Greece, Africa, other continental and marine, each of which influenced the PM₁ aerosol composition and properties. Marine air masses had the lowest PM₁ concentrations and air masses from the Balkans, Turkey and Eastern Europe the highest.

Carbonaceous aerosol particles from common vegetation in the Grand Canyon

International Nuclear Information System (INIS)

Hallock, K.A.; Mazurek, M.A.; Cass, G.R.

1992-05-01

The problem of visibility reduction in the Grand Canyon due to fine organic aerosol particles in the atmosphere has become an area of increased environmental concern. Aerosol particles can be derived from many emission sources. In this report, we focus on identifying organic aerosols derived from common vegetation in the Grand Canyon. These aerosols are expected to be significant contributors to the total atmospheric organic aerosol content. Aerosol samples from living vegetation were collected by resuspension of surface wax and resin components liberated from the leaves of vegetation common to areas of the Grand Canyon. The samples were analyzed using high-resolution gas chromatography/mass spectrometry (GC/MS). Probable identification of compounds was made by comparison of sample spectra with National Institute of Standards and Technology (NIST) mass spectral references and positive identification of compounds was made when possible by comparison with authentic standards as well as NIST references. Using these references, we have been able to positively identify the presence of n-alkane and n-alkanoic acid homolog series in the surface waxes of the vegetation sampled. Several monoterpenes, sesquiterpenes, and diterpenes were identified also as possible biogenic aerosols which may contribute to the total organic aerosol abundance leading to visibility reduction in the Grand Canyon

Effect of acidic seed on biogenic secondary organic aerosol growth

Science.gov (United States)

Czoschke, Nadine M.; Jang, Myoseon; Kamens, Richard M.

Secondary organic aerosol (SOA) growth in the presence of acid aerosols was studied in twin 500 l Teflon bags and in a 4 m flow reactor. In Teflon bags, isoprene, acrolein and α-pinene were all made to react individually with ozone and exposed to either acid or non-acid inorganic seed aerosols to determine the effect of acid-catalyzed heterogeneous reactions on SOA growth. α-Pinene and ozone were made to react in a flow reactor to assess the immediate effect of mixing an acid aerosol with SOA at high and low relative humidity levels. In all cases, exposure to acid seed aerosol increased the amount of SOA mass produced. Fourier transform infrared spectra of the SOA in acid systems confirmed the transformation of carbonyl functional groups through acid-catalyzed heterogeneous reactions when SOAs formed in acidic environments or were exposed to acidic aerosols. Organic products initially produced from ozonation in the gas phase partition onto the inorganic seed aerosol and react heterogeneously with an acid catalyst forming low vapor pressure products. These acid-catalyzed heterogeneous reactions are implicated in generating the increased SOA mass observed in acidic aerosol systems as they transform predominantly gas phase compounds of high volatility into low vapor pressure predominantly particle phase products.

Modification of Local Urban Aerosol Properties by Long-Range Transport of Biomass Burning Aerosol

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Iwona S. Stachlewska

2018-03-01

Full Text Available During August 2016, a quasi-stationary high-pressure system spreading over Central and North-Eastern Europe, caused weather conditions that allowed for 24/7 observations of aerosol optical properties by using a complex multi-wavelength PollyXT lidar system with Raman, polarization and water vapour capabilities, based at the European Aerosol Research Lidar Network (EARLINET network urban site in Warsaw, Poland. During 24–30 August 2016, the lidar-derived products (boundary layer height, aerosol optical depth, Ångström exponent, lidar ratio, depolarization ratio were analysed in terms of air mass transport (HYSPLIT model, aerosol load (CAMS data and type (NAAPS model and confronted with active and passive remote sensing at the ground level (PolandAOD, AERONET, WIOS-AQ networks and aboard satellites (SEVIRI, MODIS, CATS sensors. Optical properties for less than a day-old fresh biomass burning aerosol, advected into Warsaw’s boundary layer from over Ukraine, were compared with the properties of long-range transported 3–5 day-old aged biomass burning aerosol detected in the free troposphere over Warsaw. Analyses of temporal changes of aerosol properties within the boundary layer, revealed an increase of aerosol optical depth and Ångström exponent accompanied by an increase of surface PM10 and PM2.5. Intrusions of advected biomass burning particles into the urban boundary layer seem to affect not only the optical properties observed but also the top height of the boundary layer, by moderating its increase.

STRAPS v1.0: evaluating a methodology for predicting electron impact ionisation mass spectra for the aerosol mass spectrometer

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D. O. Topping

2017-06-01

Full Text Available Our ability to model the chemical and thermodynamic processes that lead to secondary organic aerosol (SOA formation is thought to be hampered by the complexity of the system. While there are fundamental models now available that can simulate the tens of thousands of reactions thought to take place, validation against experiments is highly challenging. Techniques capable of identifying individual molecules such as chromatography are generally only capable of quantifying a subset of the material present, making it unsuitable for a carbon budget analysis. Integrative analytical methods such as the Aerosol Mass Spectrometer (AMS are capable of quantifying all mass, but because of their inability to isolate individual molecules, comparisons have been limited to simple data products such as total organic mass and the O : C ratio. More detailed comparisons could be made if more of the mass spectral information could be used, but because a discrete inversion of AMS data is not possible, this activity requires a system of predicting mass spectra based on molecular composition. In this proof-of-concept study, the ability to train supervised methods to predict electron impact ionisation (EI mass spectra for the AMS is evaluated. Supervised Training Regression for the Arbitrary Prediction of Spectra (STRAPS is not built from first principles. A methodology is constructed whereby the presence of specific mass-to-charge ratio (m∕z channels is fitted as a function of molecular structure before the relative peak height for each channel is similarly fitted using a range of regression methods. The widely used AMS mass spectral database is used as a basis for this, using unit mass resolution spectra of laboratory standards. Key to the fitting process is choice of structural information, or molecular fingerprint. Our approach relies on using supervised methods to automatically optimise the relationship between spectral characteristics and these molecular

STRAPS v1.0: evaluating a methodology for predicting electron impact ionisation mass spectra for the aerosol mass spectrometer

Science.gov (United States)

Topping, David O.; Allan, James; Rami Alfarra, M.; Aumont, Bernard

2017-06-01

Our ability to model the chemical and thermodynamic processes that lead to secondary organic aerosol (SOA) formation is thought to be hampered by the complexity of the system. While there are fundamental models now available that can simulate the tens of thousands of reactions thought to take place, validation against experiments is highly challenging. Techniques capable of identifying individual molecules such as chromatography are generally only capable of quantifying a subset of the material present, making it unsuitable for a carbon budget analysis. Integrative analytical methods such as the Aerosol Mass Spectrometer (AMS) are capable of quantifying all mass, but because of their inability to isolate individual molecules, comparisons have been limited to simple data products such as total organic mass and the O : C ratio. More detailed comparisons could be made if more of the mass spectral information could be used, but because a discrete inversion of AMS data is not possible, this activity requires a system of predicting mass spectra based on molecular composition. In this proof-of-concept study, the ability to train supervised methods to predict electron impact ionisation (EI) mass spectra for the AMS is evaluated. Supervised Training Regression for the Arbitrary Prediction of Spectra (STRAPS) is not built from first principles. A methodology is constructed whereby the presence of specific mass-to-charge ratio (m/z) channels is fitted as a function of molecular structure before the relative peak height for each channel is similarly fitted using a range of regression methods. The widely used AMS mass spectral database is used as a basis for this, using unit mass resolution spectra of laboratory standards. Key to the fitting process is choice of structural information, or molecular fingerprint. Our approach relies on using supervised methods to automatically optimise the relationship between spectral characteristics and these molecular fingerprints. Therefore

Black carbon in aerosol during BIBLE B

Science.gov (United States)

Liley, J. Ben; Baumgardner, D.; Kondo, Y.; Kita, K.; Blake, D. R.; Koike, M.; Machida, T.; Takegawa, N.; Kawakami, S.; Shirai, T.; Ogawa, T.

2003-02-01

The Biomass Burning and Lightning Experiment (BIBLE) A and B campaigns over the tropical western Pacific during springtime deployed a Gulfstream-II aircraft with systems to measure ozone and numerous precursor species. Aerosol measuring systems included a MASP optical particle counter, a condensation nucleus (CN) counter, and an absorption spectrometer for black carbon. Aerosol volume was very low in the middle and upper troposphere during both campaigns, and during BIBLE A, there was little aerosol enhancement in the boundary layer away from urban areas. In BIBLE B, there was marked aerosol enhancement in the lowest 3 km of the atmosphere. Mixing ratios of CN in cloud-free conditions in the upper troposphere were in general higher than in the boundary layer, indicating new particle formation from gaseous precursors. High concentrations of black carbon were observed during BIBLE B, with mass loadings up to 40 μg m-3 representing as much as one quarter of total aerosol mass. Strong correlations with hydrocarbon enhancement allow the determination of a black carbon emission ratio for the fires at that time. Expressed as elemental carbon, it is about 0.5% of carbon dioxide and 6% of carbon monoxide emissions from the same fires, comparable to methane production, and greater than that of other hydrocarbons.

Elemental Composition Analysis to Investigate NOx Effects on Secondary Organic Aerosol from α-Pinene Using Ultrahigh Resolution Mass Spectrometry

Science.gov (United States)

Lim, H. J.; Park, J. H.; Babar, Z.

2015-12-01

Secondary organic aerosol (SOA) accounts for 20-70% of atmospheric fine aerosol. NOx plays crucial roles in SOA formation and consequently affects the composition and yield of SOA. SOA component speciation is incomplete due to its complex composition of polar oxygenated and multifunctional species. In this study, ultrahigh resolution mass spectrometry (UHR MS) was applied to improve the understanding of NOx effects on biogenic SOA formation by identifying the elemental composition of SOA. Additional research aim was to investigate oligomer components that are considered as a driving force for SOA formation and growth. In this study α-pinene SOA from photochemical reaction was examined. SOA formation was performed in the absence and presence of NOx at dry condition (grant funded by the Korea government (MEST) (No. 2011-01350000).

VUV photoionization aerosol mass spectrometric study on the iodine oxide particles formed from O3-initiated photooxidation of diiodomethane (CH2I2)

Czech Academy of Sciences Publication Activity Database

Wei, N.; Hu, Ch.; Zhou, S.; Ma, Q.; Mikuška, Pavel; Večeřa, Zbyněk; Gai, Y.; Lin, X.; Gu, X.; Zhao, W.; Fang, B.; Zhang, W.; Chen, J.; Liu, F.; Shan, X.; Sheng, L.

2017-01-01

Roč. 7, č. 89 (2017), s. 56779-56787 ISSN 2046-2069 Institutional support: RVO:68081715 Keywords : iodine oxide particles * photooxidation * aerosol mass spectrometer Subject RIV: CB - Analytical Chemistry, Separation OBOR OECD: Analytical chemistry Impact factor: 3.108, year: 2016

Cloud condensation nuclei closure study on summer arctic aerosol

Science.gov (United States)

Martin, M.; Chang, R. Y.-W.; Sierau, B.; Sjogren, S.; Swietlicki, E.; Abbatt, J. P. D.; Leck, C.; Lohmann, U.

2011-11-01

We present an aerosol - cloud condensation nuclei (CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration was then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer (AMS) and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory, surface tension of water and an internally mixed aerosol. The last assumption was supported by measurements made with a hygroscopic tandem differential mobility analyzer (HTDMA) for particles >70 nm. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one for those two supersaturations. This might be caused by a relative larger insoluble organic mass fraction of the smaller particles that activate at these supersaturations, which are thus less good CCN than the larger particles. On average, 36% of the mass measured with the AMS was organic mass. At 0.20, 0.15 and 0.10% supersaturation, closure could be achieved with different combinations of hygroscopic parameters and densities within the uncertainty range of the fit. The best agreement of the calculated CCN number concentration with the observed one was achieved when the organic fraction of the aerosol was treated as nearly water insoluble

Highly-controlled, reproducible measurements of aerosol emissions from African biomass combustion

Science.gov (United States)

Haslett, Sophie; Thomas, J. Chris; Morgan, William; Hadden, Rory; Liu, Dantong; Allan, James; Williams, Paul; Sekou, Keïta; Liousse, Catherine; Coe, Hugh

2017-04-01

Particulate emissions from biomass burning can alter the atmosphere's radiative balance and cause significant harm to human health. However, the relationship between these emissions and fundamental combustion processes is, to date, poorly characterised. In atmospheric models, aerosol emissions are represented by emission factors based on mass loss, which are averaged over an entire combustion event for each particulate species. This approach, however, masks huge variability in emissions during different phases of the combustion period. Laboratory tests have shown that even small changes to the burning environment can lead to huge variation in observed aerosol emission factors (Akagi et al., 2011). In order to address this gap in understanding, in this study, small wood samples sourced from Côte D'Ivoire were burned in a highly-controlled laboratory environment. The shape and mass of samples, available airflow and surrounding heat were carefully regulated. Organic aerosol and refractory black carbon emissions were measured in real-time using an Aerosol Mass Spectrometer and a Single Particle Soot Photometer, respectively. Both of these instruments are used regularly to measure aerosol concentrations in the field. This methodology produced remarkably repeatable results, allowing three different phases of combustion to be identified by their emissions. Black carbon was emitted predominantly during flaming combustion; organic aerosols were emitted during pyrolysis before ignition and from smouldering-dominated behaviour near the end of combustion. During the flaming period, there was a strong correlation between the emission of black carbon and the rate of mass loss, which suggests there is value in employing a mass-based emission factor for this species. However, very little correlation was seen between organic aerosol and mass loss throughout the tests. As such, results here suggest that emission factors averaged over an entire combustion event are unlikely to be

Comprehensive two-dimensional liquid chromatography–time-of-flight mass spectrometry in the analysis of acidic compounds in atmospheric aerosols

Czech Academy of Sciences Publication Activity Database

Pól, Jaroslav; Hohnová, B.; Jussila, M.; Hyötyläinen, T.

2006-01-01

Roč. 1130, č. 1 (2006), s. 64-71 ISSN 0021-9673. [International Symposium on Hyphenated Techniques in Chromatography and Hyphenated Chromatographic Analyzers /9./. York, 08.02.2006-10.02.2006] Institutional research plan: CEZ:AV0Z40310501 Keywords : comprehensive two-dimensional liquid chromatography * time-of-flight mass spectrometry * atmospheric aerosol analysis Subject RIV: CB - Analytical Chemistry, Separation Impact factor: 3.554, year: 2006