Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation.

Science.gov (United States)

Gordon, Hamish; Sengupta, Kamalika; Rap, Alexandru; Duplissy, Jonathan; Frege, Carla; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K; Wagner, Robert; Dunne, Eimear M; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill S; Dias, Antonio; Ehrhart, Sebastian; Fischer, Lukas; Flagan, Richard C; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Kirkby, Jasper; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Monks, Sarah A; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P; Pringle, Kirsty J; Richards, Nigel A D; Rissanen, Matti P; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E; Seinfeld, John H; Sharma, Sangeeta; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander Lucas; Wagner, Andrea C; Wagner, Paul E; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M; Worsnop, Douglas R; Baltensperger, Urs; Kulmala, Markku; Curtius, Joachim; Carslaw, Kenneth S

2016-10-25

The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by [Formula: see text] (27%) to [Formula: see text] Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

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.

Laser filament-induced aerosol formation

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H. Saathoff

2013-05-01

Full Text Available Using the aerosol and cloud simulation chamber AIDA, we investigated the laser filament induced particle formation in ambient air, humid synthetic air, humid nitrogen, argon–oxygen mixture, and pure argon in order to simulate the particle formation under realistic atmospheric conditions as well as to investigate the influence of typical gas-phase atmospheric constituents on the particle formation. Terawatt laser plasma filaments generated new particles in the size range 3 to 130 nm with particle production rates ranging from 1 × 107 to 5 × 109 cm−3 plasma s−1 for the given experimental conditions. In all cases the particle formation rates increased exponentially with the water content of the gas mixture. Furthermore, the presence of a few ppb of trace gases like SO2 and α-pinene clearly enhanced the particle yield by number, the latter also by mass. Our findings suggest that new particle formation is efficiently supported by oxidized species like acids generated by the photoionization of both major and minor components of the air, including N2, NH3, SO2 and organics.

Mechanisms of Formation of Secondary Organic Aerosols and Implications for Global Radiative Forcing

Energy Technology Data Exchange (ETDEWEB)

Seinfeld, John H. [California Inst. of Technology (CalTech), Pasadena, CA (United States)

2011-12-02

Organic material constitutes about 50% of global atmospheric aerosol mass, and the dominant source of organic aerosol is the oxidation of volatile hydrocarbons, to produce secondary organic aerosol (SOA). Understanding the formation of SOA is crucial to predicting present and future climate effects of atmospheric aerosols. The goal of this program is to significantly increase our understanding of secondary organic aerosol (SOA) formation in the atmosphere. Ambient measurements indicate that the amount of SOA in the atmosphere exceeds that predicted in current models based on existing laboratory chamber data. This would suggest that either the SOA yields measured in laboratory chambers are understated or that all major organic precursors have not been identified. In this research program we are systematically exploring these possibilities.

Organic aerosol formation in citronella candle plumes.

Science.gov (United States)

Bothe, Melanie; Donahue, Neil McPherson

2010-09-01

Citronella candles are widely used as insect repellants, especially outdoors in the evening. Because these essential oils are unsaturated, they have a unique potential to form secondary organic aerosol (SOA) via reaction with ozone, which is also commonly elevated on summer evenings when the candles are often in use. We investigated this process, along with primary aerosol emissions, by briefly placing a citronella tealight candle in a smog chamber and then adding ozone to the chamber. In repeated experiments, we observed rapid and substantial SOA formation after ozone addition; this process must therefore be considered when assessing the risks and benefits of using citronella candle to repel insects.

A look at aerosol formation using data mining techniques

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S. Hyvönen

2005-01-01

Full Text Available Atmospheric aerosol particle formation is frequently observed throughout the atmosphere, but despite various attempts of explanation, the processes behind it remain unclear. In this study data mining techniques were used to find the key parameters needed for atmospheric aerosol particle formation to occur. A dataset of 8 years of 80 variables collected at the boreal forest station (SMEAR II in Southern Finland was used, incorporating variables such as radiation, humidity, SO2, ozone and present aerosol surface area. This data was analyzed using clustering and classification methods. The aim of this approach was to gain new parameters independent of any subjective interpretation. This resulted in two key parameters, relative humidity and preexisting aerosol particle surface (condensation sink, capable in explaining 88% of the nucleation events. The inclusion of any further parameters did not improve the results notably. Using these two variables it was possible to derive a nucleation probability function. Interestingly, the two most important variables are related to mechanisms that prevent the nucleation from starting and particles from growing, while parameters related to initiation of particle formation seemed to be less important. Nucleation occurs only with low relative humidity and condensation sink values. One possible explanation for the effect of high water content is that it prevents biogenic hydrocarbon ozonolysis reactions from producing sufficient amounts of low volatility compounds, which might be able to nucleate. Unfortunately the most important biogenic hydrocarbon compound emissions were not available for this study. Another effect of water vapour may be due to its linkage to cloudiness which may prevent the formation of nucleating and/or condensing vapours. A high number of preexisting particles will act as a sink for condensable vapours that otherwise would have been able to form sufficient supersaturation and initiate the

Direct Observations of Isoprene Secondary Organic Aerosol Formation in Ambient Cloud Droplets

Science.gov (United States)

Zelenyuk, A.; Bell, D.; Thornton, J. A.; Fast, J. D.; Shrivastava, M. B.; Berg, L. K.; Imre, D. G.; Mei, F.; Shilling, J.; Suski, K. J.; Liu, J.; Tomlinson, J. M.; Wang, J.

2017-12-01

Multiphase chemistry of isoprene photooxidation products has been shown to be one of the major sources of secondary organic aerosol (SOA) in the atmosphere. A number of recent studies indicate that aqueous aerosol phase provides a medium for reactive uptake of isoprene photooxidation products, and in particular, isomeric isoprene epoxydiols (IEPOX), with reaction rates and yields being dependent on aerosol acidity, water content, sulfate concentration, and organic coatings. However, very few studies focused on chemistry occurring within actual cloud droplets. We will present data acquired during recent Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) Campaign, which provide direct evidence for IEPOX-SOA formation in cloud droplets. Single particle mass spectrometer, miniSPLAT, and a high-resolution, time-of-flight aerosol mass spectrometer were used to characterize the composition of aerosol particles and cloud droplet residuals, while a high-resolution, time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) was used to characterize gas-phase compounds. We find that the composition of cloud droplet residuals was markedly different than that of aerosol particles sampled outside the cloud. Cloud droplet residuals were comprised of individual particles with high relative fractions of sulfate and nitrate and significant fraction of particles with mass spectra that are nearly identical to those of laboratory-generated IEPOX-SOA particles. The observed cloud-induced formation of IEPOX-SOA was accompanied by simultaneous decrease in measured concentrations of IEPOX and other gas-phase isoprene photooxidation products. Ultimately, the combined cloud, aerosol, and gas-phase measurements conducted during HI-SCALE will be used to develop and evaluate model treatments of aqueous-phase isoprene SOA formation.

The formation of aerosol particles during combustion of biomass and waste. Final report

Energy Technology Data Exchange (ETDEWEB)

Hjerrild Zeuthen, J

2007-05-15

This thesis describes the formation of aerosol particles during combustion of biomass and waste. The formation of aerosol particles is investigated by studying condensation of alkali salts from synthetic flue gasses in a laboratory tubular furnace. In this so-called laminar flow aerosol condenser-furnace gaseous alkali chlorides are mixed with sulphur dioxide, water vapour and oxygen. At high temperatures the alkali chloride reacts with sulphur dioxide to form alkali sulphate. During subsequent cooling of the synthetic flue gas the chlorides and sulphates condense either as deposits on walls or on other particles or directly from the gas phase by homogenous nucleation. A previously developed computer code for simulation of one-component nucleation of particles in a cylindrical laminar flow is extended to include a homogeneous gas phase reaction to produce gaseous alkali sulphate. The formation of aerosol particles during full-scale combustion of wheat straw is investigated in a 100 MW grate-fired boiler. Finally, aerosols from incineration of waste are investigated during full-scale combustion of municipal waste in a 22 MW grate-fired unit. (BA)

Missing ozone-induced potential aerosol formation in a suburban deciduous forest

Science.gov (United States)

Nakayama, T.; Kuruma, Y.; Matsumi, Y.; Morino, Y.; Sato, K.; Tsurumaru, H.; Ramasamy, S.; Sakamoto, Y.; Kato, S.; Miyazaki, Y.; Mochizuki, T.; Kawamura, K.; Sadanaga, Y.; Nakashima, Y.; Matsuda, K.; Kajii, Y.

2017-12-01

As a new approach to investigating formation processes of secondary organic aerosol (SOA) in the atmosphere, ozone-induced potential aerosol formation was measured in summer at a suburban forest site surrounded by deciduous trees, near Tokyo, Japan. After passage through a reactor containing high concentrations of ozone, increases in total particle volume (average of 1.4 × 109 nm3/cm3, which corresponds to 17% that of pre-existing particles) were observed, especially during daytime. The observed aerosol formations were compared with the results of box model simulations using simultaneously measured concentrations of gaseous and particulate species. According to the model, the relative contributions of isoprene, monoterpene, and aromatic hydrocarbon oxidation to SOA formation in the reactor were 24, 21, and 55%, respectively. However, the model could explain, on average, only ∼40% of the observed particle formation, and large discrepancies between the observations and model were found, especially around noon and in the afternoon when the concentrations of isoprene and oxygenated volatile organic compounds were high. The results suggest a significant contribution of missing (unaccounted-for) SOA formation processes from identified and/or unidentified volatile organic compounds, especially those emitted during daytime. Further efforts should be made to explore and parameterize this missing SOA formation to assist in the improvement of atmospheric chemistry and climate models.

Technical committee meeting on aerosol formation, vapour deposits and sodium vapour trapping. Summary report

Energy Technology Data Exchange (ETDEWEB)

NONE

1977-01-01

The papers presented at the LMFBR meeting on aerosol formation covered the following four main topics: theoretical studies on aerosol behaviour and comparison with experimental results; techniques for measurement of aerosols; techniques for trapping sodium vapour and aerosols in gas circuits; design of components having to cope with aerosol deposits. The resulting summaries, conclusions and recommendations which were were agreed upon are presented.

Technical committee meeting on aerosol formation, vapour deposits and sodium vapour trapping. Summary report

International Nuclear Information System (INIS)

1977-01-01

The papers presented at the LMFBR meeting on aerosol formation covered the following four main topics: theoretical studies on aerosol behaviour and comparison with experimental results; techniques for measurement of aerosols; techniques for trapping sodium vapour and aerosols in gas circuits; design of components having to cope with aerosol deposits. The resulting summaries, conclusions and recommendations which were were agreed upon are presented

Formation and dynamic change of aerosol particles

International Nuclear Information System (INIS)

Kasahara, Mikio

1986-01-01

Processes of aerosol particle nucleation are roughly grouped into two types. In one, aerosol is produced as a result of dispersion of solid or liquid by mechanical force while in the other it is formed through phase transition from gas to solid or liquid due to cohesion caused by cooling, expansion or chemical reaction. This article reviews various aspects of aerosol particle nucleation through the latter type of processes and behaviors of the particles formed. Gas-to-particle conversion processes are divided into those of homogeneous and heterogeneous nucleation, and the former include homogeneous homomolecular and homogeneous heteromolecular nucleation processes. Here, homoneneous homomolecular nucleation is described centering on the theories proposed by Backer and Doring-Zeldovich-Volmer-Frenkel while homogeneous heteromolecular systems are outlined citing the theory developed by Kiang and Stauffer. Heterogeneous nucleation (or heterogeneous condensation) is discussed on the basis of the relationship between the mean free path of air molecules and the particle size. Various theories for particle formation and growth are listed and briefly outlined. Some of them are compared with experimental results. Models are cited to explain behaviors of aerosol particles after being formed. Also described is simulation of particle nucleation and growth in relation to atmospheric pollution and possible accidents of liquid-metal fast breeder reactors. (Nogami, K.)

Properties of aerosols and formation mechanisms over southern China during the monsoon season

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W. Chen

2016-10-01

Full Text Available Measurements of size-resolved aerosols from 0.25 to 18 µm were conducted at three sites (urban, suburban and background sites and used in tandem with an atmospheric transport model to study the size distribution and formation of atmospheric aerosols in southern China during the monsoon season (May–June in 2010. The mass distribution showed the majority of chemical components were found in the smaller size bins (< 2.5 µm. Sulfate was found to be strongly correlated with aerosol water and anticorrelated with atmospheric SO2, hinting at aqueous-phase reactions being the main formation pathway. Nitrate was the only major species that showed a bimodal distribution at the urban site and was dominated by the coarse mode in the other two sites, suggesting that an important component of nitrate formation is chloride depletion of sea salt transported from the South China Sea. In addition to these aqueous-phase reactions and interactions with sea salt aerosols, new particle formation, chemical aging, and long-range transport from upwind urban or biomass burning regions was also found to be important in at least some of the sites on some of the days. This work therefore summarizes the different mechanisms that significantly impact the aerosol chemical composition during the monsoon over southern China.

Secondary aerosol formation from stress-induced biogenic emissions and possible climate feedbacks

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Th. F. Mentel

2013-09-01

Full Text Available Atmospheric aerosols impact climate by scattering and absorbing solar radiation and by acting as ice and cloud condensation nuclei. Biogenic secondary organic aerosols (BSOAs comprise an important component of atmospheric aerosols. Biogenic volatile organic compounds (BVOCs emitted by vegetation are the source of BSOAs. Pathogens and insect attacks, heat waves and droughts can induce stress to plants that may impact their BVOC emissions, and hence the yield and type of formed BSOAs, and possibly their climatic effects. This raises questions of whether stress-induced changes in BSOA formation may attenuate or amplify effects of climate change. In this study we assess the potential impact of stress-induced BVOC emissions on BSOA formation for tree species typical for mixed deciduous and Boreal Eurasian forests. We studied the photochemical BSOA formation for plants infested by aphids in a laboratory setup under well-controlled conditions and applied in addition heat and drought stress. The results indicate that stress conditions substantially modify BSOA formation and yield. Stress-induced emissions of sesquiterpenes, methyl salicylate, and C17-BVOCs increase BSOA yields. Mixtures including these compounds exhibit BSOA yields between 17 and 33%, significantly higher than mixtures containing mainly monoterpenes (4–6% yield. Green leaf volatiles suppress SOA formation, presumably by scavenging OH, similar to isoprene. By classifying emission types, stressors and BSOA formation potential, we discuss possible climatic feedbacks regarding aerosol effects. We conclude that stress situations for plants due to climate change should be considered in climate–vegetation feedback mechanisms.

Modeling Secondary Organic Aerosol Formation From Emissions of Combustion Sources

Science.gov (United States)

Jathar, Shantanu Hemant

Atmospheric aerosols exert a large influence on the Earth's climate and cause adverse public health effects, reduced visibility and material degradation. Secondary organic aerosol (SOA), defined as the aerosol mass arising from the oxidation products of gas-phase organic species, accounts for a significant fraction of the submicron atmospheric aerosol mass. Yet, there are large uncertainties surrounding the sources, atmospheric evolution and properties of SOA. This thesis combines laboratory experiments, extensive data analysis and global modeling to investigate the contribution of semi-volatile and intermediate volatility organic compounds (SVOC and IVOC) from combustion sources to SOA formation. The goals are to quantify the contribution of these emissions to ambient PM and to evaluate and improve models to simulate its formation. To create a database for model development and evaluation, a series of smog chamber experiments were conducted on evaporated fuel, which served as surrogates for real-world combustion emissions. Diesel formed the most SOA followed by conventional jet fuel / jet fuel derived from natural gas, gasoline and jet fuel derived from coal. The variability in SOA formation from actual combustion emissions can be partially explained by the composition of the fuel. Several models were developed and tested along with existing models using SOA data from smog chamber experiments conducted using evaporated fuel (this work, gasoline, fischertropschs, jet fuel, diesels) and published data on dilute combustion emissions (aircraft, on- and off-road gasoline, on- and off-road diesel, wood burning, biomass burning). For all of the SOA data, existing models under-predicted SOA formation if SVOC/IVOC were not included. For the evaporated fuel experiments, when SVOC/IVOC were included predictions using the existing SOA model were brought to within a factor of two of measurements with minor adjustments to model parameterizations. Further, a volatility

Properties of aerosols and formation mechanisms over southern China during the monsoon season

Science.gov (United States)

Chen, Weihua; Wang, Xuemei; Blake Cohen, Jason; Zhou, Shengzhen; Zhang, Zhisheng; Chang, Ming; Chan, Chuen-Yu

2016-10-01

Measurements of size-resolved aerosols from 0.25 to 18 µm were conducted at three sites (urban, suburban and background sites) and used in tandem with an atmospheric transport model to study the size distribution and formation of atmospheric aerosols in southern China during the monsoon season (May-June) in 2010. The mass distribution showed the majority of chemical components were found in the smaller size bins (water and anticorrelated with atmospheric SO2, hinting at aqueous-phase reactions being the main formation pathway. Nitrate was the only major species that showed a bimodal distribution at the urban site and was dominated by the coarse mode in the other two sites, suggesting that an important component of nitrate formation is chloride depletion of sea salt transported from the South China Sea. In addition to these aqueous-phase reactions and interactions with sea salt aerosols, new particle formation, chemical aging, and long-range transport from upwind urban or biomass burning regions was also found to be important in at least some of the sites on some of the days. This work therefore summarizes the different mechanisms that significantly impact the aerosol chemical composition during the monsoon over southern China.

Modeling biogenic secondary organic aerosol (BSOA) formation from monoterpene reactions with NO3: A case study of the SOAS campaign using CMAQ

Science.gov (United States)

Qin, Momei; Hu, Yongtao; Wang, Xuesong; Vasilakos, Petros; Boyd, Christopher M.; Xu, Lu; Song, Yu; Ng, Nga Lee; Nenes, Athanasios; Russell, Armistead G.

2018-07-01

Monoterpenes react with nitrate radicals (NO3), contributing substantially to nighttime organic aerosol (OA) production. In this study, the role of reactions of monoterpenes + NO3 in forming biogenic secondary organic aerosol (BSOA) was examined using the Community Multiscale Air Quality (CMAQ) model, with extended emission profiles of biogenic volatile organic compounds (BVOCs), species-specific representations of BSOA production from individual monoterpenes and updated aerosol yields for monoterpene + NO3. The model results were compared to detailed measurements from the Southern Oxidants and Aerosol Study (SOAS) at Centreville, Alabama. With the more detailed model, monoterpene-derived BSOA increased by ∼1 μg m-3 at night, accounting for one-third of observed less-oxidized oxygenated OA (LO-OOA), more closely agreeing with observations (lower error, stronger correlation). Implementation of a multigenerational oxidation approach resulted in the model capturing elevated OA episodes. With the aging model, aged semi-volatile organic compounds (ASVOCs) contributed over 60% of the monoterpene-derived BSOA, followed by SOA formation via nitrate radical chemistry, making up to 34% of that formed at night. Among individual monoterpenes, β-pinene and limonene contributed most to the monoterpene-derived BSOA from nighttime reactions.

Substantial secondary organic aerosol formation in a coniferous forest: observations of both day- and nighttime chemistry

OpenAIRE

A. K. Y. Lee; J. P. D. Abbatt; W. R. Leaitch; S.-M. Li; S. J. Sjostedt; S. J. Sjostedt; J. J. B. Wentzell; J. Liggio; A. M. Macdonald

2016-01-01

Substantial biogenic secondary organic aerosol (BSOA) formation was investigated in a coniferous forest mountain region at Whistler, British Columbia. A largely biogenic aerosol growth episode was observed, providing a unique opportunity to investigate BSOA formation chemistry in a forested environment with limited influence from anthropogenic emissions. Positive matrix factorization of aerosol mass spectrometry (AMS) measurement identifie...

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation

Science.gov (United States)

Shiraiwa, Manabu; Yee, Lindsay D.; Schilling, Katherine A.; Loza, Christine L.; Craven, Jill S.; Zuend, Andreas; Ziemann, Paul J.; Seinfeld, John H.

2013-01-01

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process. PMID:23818634

Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation.

Science.gov (United States)

Shiraiwa, Manabu; Yee, Lindsay D; Schilling, Katherine A; Loza, Christine L; Craven, Jill S; Zuend, Andreas; Ziemann, Paul J; Seinfeld, John H

2013-07-16

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process.

Secondary organic aerosol formation from primary aliphatic amines with NO3 radical

Science.gov (United States)

Malloy, Q. G. J.; Qi, Li; Warren, B.; Cocker, D. R., III; Erupe, M. E.; Silva, P. J.

2009-03-01

Primary aliphatic amines are an important class of nitrogen containing compounds emitted from automobiles, waste treatment facilities and agricultural animal operations. A series of experiments conducted at the UC-Riverside/CE-CERT Environmental Chamber is presented in which oxidation of methylamine, ethylamine, propylamine, and butylamine with O3 and NO3 have been investigated. Very little aerosol formation is observed in the presence of O3 only. However, after addition of NO, and by extension NO3, large aerosol mass yields (~44% for butylamine) are seen. Aerosol generated was determined to be organic in nature due to the small fraction of NO and NO2 in the total signal (tested) as detected by an aerosol mass spectrometer (AMS). We propose a reaction mechanism between carbonyl containing species and the parent amine leading to formation of particulate imine products. These findings can have significant impacts on rural communities with elevated nighttime PM loadings, when significant levels of NO3 exist.

Secondary organic aerosol formation from primary aliphatic amines with NO3 radical

Directory of Open Access Journals (Sweden)

P. J. Silva

2009-03-01

Full Text Available Primary aliphatic amines are an important class of nitrogen containing compounds emitted from automobiles, waste treatment facilities and agricultural animal operations. A series of experiments conducted at the UC-Riverside/CE-CERT Environmental Chamber is presented in which oxidation of methylamine, ethylamine, propylamine, and butylamine with O3 and NO3 have been investigated. Very little aerosol formation is observed in the presence of O3 only. However, after addition of NO, and by extension NO3, large aerosol mass yields (~44% for butylamine are seen. Aerosol generated was determined to be organic in nature due to the small fraction of NO and NO2 in the total signal (<1% for all amines tested as detected by an aerosol mass spectrometer (AMS. We propose a reaction mechanism between carbonyl containing species and the parent amine leading to formation of particulate imine products. These findings can have significant impacts on rural communities with elevated nighttime PM loadings, when significant levels of NO3 exist.

Satellite remote sensing of dust aerosol indirect effects on ice cloud formation.

Science.gov (United States)

Ou, Steve Szu-Cheng; Liou, Kuo-Nan; Wang, Xingjuan; Hansell, Richard; Lefevre, Randy; Cocks, Stephen

2009-01-20

We undertook a new approach to investigate the aerosol indirect effect of the first kind on ice cloud formation by using available data products from the Moderate-Resolution Imaging Spectrometer (MODIS) and obtained physical understanding about the interaction between aerosols and ice clouds. Our analysis focused on the examination of the variability in the correlation between ice cloud parameters (optical depth, effective particle size, cloud water path, and cloud particle number concentration) and aerosol optical depth and number concentration that were inferred from available satellite cloud and aerosol data products. Correlation results for a number of selected scenes containing dust and ice clouds are presented, and dust aerosol indirect effects on ice clouds are directly demonstrated from satellite observations.

An interfacial mechanism for cloud droplet formation on organic aerosols.

Science.gov (United States)

Ruehl, Christopher R; Davies, James F; Wilson, Kevin R

2016-03-25

Accurate predictions of aerosol/cloud interactions require simple, physically accurate parameterizations of the cloud condensation nuclei (CCN) activity of aerosols. Current models assume that organic aerosol species contribute to CCN activity by lowering water activity. We measured droplet diameters at the point of CCN activation for particles composed of dicarboxylic acids or secondary organic aerosol and ammonium sulfate. Droplet activation diameters were 40 to 60% larger than predicted if the organic was assumed to be dissolved within the bulk droplet, suggesting that a new mechanism is needed to explain cloud droplet formation. A compressed film model explains how surface tension depression by interfacial organic molecules can alter the relationship between water vapor supersaturation and droplet size (i.e., the Köhler curve), leading to the larger diameters observed at activation. Copyright © 2016, American Association for the Advancement of Science.

Formation of charged particles in condensation aerosol generators used for inhalation studies

International Nuclear Information System (INIS)

Ramu, M.C.R.; Vohra, K.G.

1976-01-01

Formation of charged particles in a condensation aerosol generator has been studied using a charge collector and a mobility analyzer. Measurements carried out using the charge collector show that the number of charged particles increases with an increase in the particle diameter. The number of charged particles measured also depends on the thickness of the sodium chloride coating on the platinum wire used in the aerosol generator for the production of condensation nuclei. It was found that the charged particle concentration increases with decreasing coating thickness. Mobility measurements have shown that the particles are singly and doubly charged. It has been estimated that about 10% of the particles produced in the generator are charged. The mechanism of formation of charged particles in the aerosol generator has been briefly discussed. (author)

Modelling of primary aerosols in the chemical transport model MOCAGE: development and evaluation of aerosol physical parameterizations

Directory of Open Access Journals (Sweden)

B. Sič

2015-02-01

Full Text Available This paper deals with recent improvements to the global chemical transport model of Météo-France MOCAGE (Modèle de Chimie Atmosphérique à Grande Echelle that consists of updates to different aerosol parameterizations. MOCAGE only contains primary aerosol species: desert dust, sea salt, black carbon, organic carbon, and also volcanic ash in the case of large volcanic eruptions. We introduced important changes to the aerosol parameterization concerning emissions, wet deposition and sedimentation. For the emissions, size distribution and wind calculations are modified for desert dust aerosols, and a surface sea temperature dependant source function is introduced for sea salt aerosols. Wet deposition is modified toward a more physically realistic representation by introducing re-evaporation of falling rain and snowfall scavenging and by changing the in-cloud scavenging scheme along with calculations of precipitation cloud cover and rain properties. The sedimentation scheme update includes changes regarding the stability and viscosity calculations. Independent data from satellites (MODIS, SEVIRI, the ground (AERONET, EMEP, and a model inter-comparison project (AeroCom are compared with MOCAGE simulations and show that the introduced changes brought a significant improvement on aerosol representation, properties and global distribution. Emitted quantities of desert dust and sea salt, as well their lifetimes, moved closer towards values of AeroCom estimates and the multi-model average. When comparing the model simulations with MODIS aerosol optical depth (AOD observations over the oceans, the updated model configuration shows a decrease in the modified normalized mean bias (MNMB; from 0.42 to 0.10 and a better correlation (from 0.06 to 0.32 in terms of the geographical distribution and the temporal variability. The updates corrected a strong positive MNMB in the sea salt representation at high latitudes (from 0.65 to 0.16, and a negative MNMB in

High formation of secondary organic aerosol from the photo-oxidation of toluene

Directory of Open Access Journals (Sweden)

L. Hildebrandt

2009-05-01

Full Text Available Toluene and other aromatics have long been viewed as the dominant anthropogenic secondary organic aerosol (SOA precursors, but the SOA mass yields from toluene reported in previous studies vary widely. Experiments conducted in the Carnegie Mellon University environmental chamber to study SOA formation from the photo-oxidation of toluene show significantly larger SOA production than parameterizations employed in current air-quality models. Aerosol mass yields depend on experimental conditions: yields are higher under higher UV intensity, under low-NO_x conditions and at lower temperatures. The extent of oxidation of the aerosol also varies with experimental conditions, consistent with ongoing, progressive photochemical aging of the toluene SOA. Measurements using a thermodenuder system suggest that the aerosol formed under high- and low-NO_x conditions is semi-volatile. These results suggest that SOA formation from toluene depends strongly on ambient conditions. An approximate parameterization is proposed for use in air-quality models until a more thorough treatment accounting for the dynamic nature of this system becomes available.

Numerical analysis of the formation process of aerosols in the alveoli

Science.gov (United States)

Haslbeck, Karsten; Seume, Jörg R.

2008-11-01

For a successful diagnosis of lung diseases through an analysis of non-volatile molecules in the exhaled breath, an exact understanding of the aerosol formation process is required. This process is modeled using Computational Fluid Dynamics (CFD). The model shows the interaction of the boundary surface between the streamed airway and the local epithelial liquid layer. A 2-D volume mesh of an alveolus is generated by taking into account the connection of the alveoli with the sacculi alveolares (SA). The Volume of Fluid (VOF) Method is used to model the interface between the gas and the liquid film. The non-Newtonian flow is modeled by the implementation of the Ostwald de Waele model. Surface tension is a function of the surfactant concentration. The VOF-Method allows the distribution of the concentration of the epithelial liquid layer at the surface to be traced in a transient manner. The simulations show the rupturing of the liquid film through the drop formation. Aerosol particles are ejected into the SA and do not collide with the walls. The quantity, the geometrical size as well as the velocity distributions of the generated aerosols are determined. The data presented in the paper provide the boundary conditions for future CFD analysis of the aerosol transport through the airways up to exhalation.

Aircraft exhaust aerosol formation and growth

Energy Technology Data Exchange (ETDEWEB)

Brown, R C; Miake-Lye, R C; Anderson, M R; Kolb, C E [Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics

1998-12-31

Aerosol formation and growth in the exhaust plume of the ATTAS aircraft at an altitude of approximately 9 km, burning fuels with 2 ppmm sulfur (`low`) and 266 ppmm (`high`) sulfur has been modeled using an aerosol dynamics model for nucleation, vapor condensation and coagulation, coupled to a 2-dimensional, axisymmetric flow code to treat plume dilution and turbulent mixing. For both the `low` and `high` sulfur fuels, approximately 60% of the available water had condensed within the first 200 m downstream of the exhaust exit. The contrail particle diameters ranged between 0.4 to 1.6 {mu}m. However, the size distributions as a function of radial position for the `low` sulfur plume were broader than the corresponding distributions for the `high` sulfur plume. The model results indicate for a fuel sulfur mass loading of 2 ppmm, sulfuric acid remains a viable activating agent and that the differences in the contrail particle size distributions for sulfur mass loadings between 2 ppmm and 260 ppmm would be difficult to detect. (author) 12 refs.

Aircraft exhaust aerosol formation and growth

Energy Technology Data Exchange (ETDEWEB)

Brown, R.C.; Miake-Lye, R.C.; Anderson, M.R.; Kolb, C.E. [Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics

1997-12-31

Aerosol formation and growth in the exhaust plume of the ATTAS aircraft at an altitude of approximately 9 km, burning fuels with 2 ppmm sulfur (`low`) and 266 ppmm (`high`) sulfur has been modeled using an aerosol dynamics model for nucleation, vapor condensation and coagulation, coupled to a 2-dimensional, axisymmetric flow code to treat plume dilution and turbulent mixing. For both the `low` and `high` sulfur fuels, approximately 60% of the available water had condensed within the first 200 m downstream of the exhaust exit. The contrail particle diameters ranged between 0.4 to 1.6 {mu}m. However, the size distributions as a function of radial position for the `low` sulfur plume were broader than the corresponding distributions for the `high` sulfur plume. The model results indicate for a fuel sulfur mass loading of 2 ppmm, sulfuric acid remains a viable activating agent and that the differences in the contrail particle size distributions for sulfur mass loadings between 2 ppmm and 260 ppmm would be difficult to detect. (author) 12 refs.

A new oxidation flow reactor for measuring secondary aerosol formation of rapidly changing emission sources

Science.gov (United States)

Simonen, Pauli; Saukko, Erkka; Karjalainen, Panu; Timonen, Hilkka; Bloss, Matthew; Aakko-Saksa, Päivi; Rönkkö, Topi; Keskinen, Jorma; Dal Maso, Miikka

2017-04-01

Oxidation flow reactors (OFRs) or environmental chambers can be used to estimate secondary aerosol formation potential of different emission sources. Emissions from anthropogenic sources, such as vehicles, often vary on short timescales. For example, to identify the vehicle driving conditions that lead to high potential secondary aerosol emissions, rapid oxidation of exhaust is needed. However, the residence times in environmental chambers and in most oxidation flow reactors are too long to study these transient effects ( ˜ 100 s in flow reactors and several hours in environmental chambers). Here, we present a new oxidation flow reactor, TSAR (TUT Secondary Aerosol Reactor), which has a short residence time ( ˜ 40 s) and near-laminar flow conditions. These improvements are achieved by reducing the reactor radius and volume. This allows studying, for example, the effect of vehicle driving conditions on the secondary aerosol formation potential of the exhaust. We show that the flow pattern in TSAR is nearly laminar and particle losses are negligible. The secondary organic aerosol (SOA) produced in TSAR has a similar mass spectrum to the SOA produced in the state-of-the-art reactor, PAM (potential aerosol mass). Both reactors produce the same amount of mass, but TSAR has a higher time resolution. We also show that TSAR is capable of measuring the secondary aerosol formation potential of a vehicle during a transient driving cycle and that the fast response of TSAR reveals how different driving conditions affect the amount of formed secondary aerosol. Thus, TSAR can be used to study rapidly changing emission sources, especially the vehicular emissions during transient driving.

Glyoxal processing by aerosol multiphase chemistry: towards a kinetic modeling framework of secondary organic aerosol formation in aqueous particles

Directory of Open Access Journals (Sweden)

B. Ervens

2010-09-01

Full Text Available This study presents a modeling framework based on laboratory data to describe the kinetics of glyoxal reactions that form secondary organic aerosol (SOA in aqueous aerosol particles. Recent laboratory results on glyoxal reactions are reviewed and a consistent set of empirical reaction rate constants is derived that captures the kinetics of glyoxal hydration and subsequent reversible and irreversible reactions in aqueous inorganic and water-soluble organic aerosol seeds. Products of these processes include (a oligomers, (b nitrogen-containing products, (c photochemical oxidation products with high molecular weight. These additional aqueous phase processes enhance the SOA formation rate in particles and yield two to three orders of magnitude more SOA than predicted based on reaction schemes for dilute aqueous phase (cloud chemistry for the same conditions (liquid water content, particle size.

The application of the new module including detailed chemical processes in a box model demonstrates that both the time scale to reach aqueous phase equilibria and the choice of rate constants of irreversible reactions have a pronounced effect on the predicted atmospheric relevance of SOA formation from glyoxal. During day time, a photochemical (most likely radical-initiated process is the major SOA formation pathway forming ∼5 μg m⁻³ SOA over 12 h (assuming a constant glyoxal mixing ratio of 300 ppt. During night time, reactions of nitrogen-containing compounds (ammonium, amines, amino acids contribute most to the predicted SOA mass; however, the absolute predicted SOA masses are reduced by an order of magnitude as compared to day time production. The contribution of the ammonium reaction significantly increases in moderately acidic or neutral particles (5 < pH < 7.

Glyoxal uptake into ammonium sulfate seed under dark conditions can be represented with a single reaction parameter k_effupt that does not depend

Effect of NOx level on secondary organic aerosol (SOA formation from the photooxidation of terpenes

Directory of Open Access Journals (Sweden)

R. C. Flagan

2007-10-01

Full Text Available Secondary organic aerosol (SOA formation from the photooxidation of one monoterpene (α-pinene and two sesquiterpenes (longifolene and aromadendrene is investigated in the Caltech environmental chambers. The effect of NOx on SOA formation for these biogenic hydrocarbons is evaluated by performing photooxidation experiments under varying NOx conditions. The NOx dependence of α-pinene SOA formation follows the same trend as that observed previously for a number of SOA precursors, including isoprene, in which SOA yield (defined as the ratio of the mass of organic aerosol formed to the mass of parent hydrocarbon reacted decreases as NOx level increases. The NOx dependence of SOA yield for the sesquiterpenes, longifolene and aromadendrene, however, differs from that determined for isoprene and α-pinene; the aerosol yield under high-NOx conditions substantially exceeds that under low-NOx conditions. The reversal of the NOx dependence of SOA formation for the sesquiterpenes is consistent with formation of relatively low-volatility organic nitrates, and/or the isomerization of large alkoxy radicals leading to less volatile products. Analysis of the aerosol chemical composition for longifolene confirms the presence of organic nitrates under high-NOx conditions. Consequently the formation of SOA from certain biogenic hydrocarbons such as sesquiterpenes (and possibly large anthropogenic hydrocarbons as well may be more efficient in polluted air.

Formation of secondary organic aerosol from isoprene oxidation over Europe

Directory of Open Access Journals (Sweden)

M. Karl

2009-09-01

Full Text Available The role of isoprene as a precursor to secondary organic aerosol (SOA over Europe is studied with the two-way nested global chemistry transport model TM5. The inclusion of the formation of SOA from isoprene oxidation in our model almost doubles the atmospheric burden of SOA over Europe compared to SOA formation from terpenes and aromatics. The reference simulation, which considers SOA formation from isoprene, terpenes and aromatics, predicts a yearly European production rate of 1.0 Tg SOA yr⁻¹ and an annual averaged atmospheric burden of about 50 Gg SOA over Europe. A fraction of 35% of the SOA produced in the boundary layer over Europe is transported to higher altitudes or to other world regions. Summertime measurements of organic matter (OM during the extensive EMEP OC/EC campaign 2002/2003 are better reproduced when SOA formation from isoprene is taken into account, reflecting also the strong seasonality of isoprene and other biogenic volatile organic compounds (BVOC emissions from vegetation. However, during winter, our model strongly underestimates OM, likely caused by missing wood burning in the emission inventories. Uncertainties in the parameterisation of isoprene SOA formation have been investigated. Maximum SOA production is found for irreversible sticking (non-equilibrium partitioning of condensable vapours on particles, with tropospheric SOA production over Europe increased by a factor of 4 in summer compared to the reference case. Completely neglecting SOA formation from isoprene results in the lowest estimate (0.51 Tg SOA yr⁻¹. The amount and the nature of the absorbing matter are shown to be another key uncertainty when predicting SOA levels. Consequently, smog chamber experiments on SOA formation should be performed with different types of seed aerosols and without seed aerosols in order to derive an improved treatment of the absorption of SOA in the models. Consideration of a number of recent insights

Mechanism and Kinetics of the Formation and Transport of Aerosol Particles in the Lower Stratosphere

Science.gov (United States)

Aloyan, A. E.; Ermakov, A. N.; Arutyunyan, V. O.

2018-03-01

Field and laboratory observation data on aerosol particles in the lower stratosphere are considered. The microphysics of their formation, mechanisms of heterogeneous chemical reactions involving reservoir gases (e.g., HCl, ClONO2, etc.) and their kinetic characteristics are analyzed. A new model of global transport of gaseous and aerosol admixtures in the lower stratosphere is described. The preliminary results from a numerical simulation of the formation of sulfate particles of the Junge layer and particles of polar stratospheric clouds (PSCs, types Ia, Ib, and II) are presented, and their effect on the gas and aerosol composition is analyzed.

Molecular structure impacts on secondary organic aerosol formation from glycol ethers

Science.gov (United States)

Li, Lijie; Cocker, David R.

2018-05-01

Glycol ethers, a class of widely used solvents in consumer products, are often considered exempt as volatile organic compounds based on their vapor pressure or boiling points by regulatory agencies. However, recent studies found that glycol ethers volatilize at ambient conditions nearly as rapidly as the traditional high-volatility solvents indicating the potential of glycol ethers to form secondary organic aerosol (SOA). This is the first work on SOA formation from glycol ethers. The impact of molecular structure, specifically -OH, on SOA formation from glycol ethers and related ethers are investigated in the work. Ethers with and without -OH, with methyl group hindrance on -OH and with -OH at different location are studied in the presence of NOX and under "NOX free" conditions. Photooxidation experiments under different oxidation conditions confirm that the processing of ethers is a combination of carbonyl formation, cyclization and fragmentation. Bulk SOA chemical composition analysis and oxidation products identified in both gas and particle phase suggests that the presence and location of -OH in the carbon bond of ethers determine the occurrence of cyclization mechanism during ether oxidation. The cyclization is proposed as a critical SOA formation mechanism to prevent the formation of volatile compounds from fragmentation during the oxidation of ethers. Glycol ethers with -CH2-O-CH2CH2OH structure is found to readily form cyclization products, especially with the presence of NOx, which is more relevant to urban atmospheric conditions than without NOx. Glycol ethers are evaluated as dominating SOA precursors among all ethers studied. It is estimated that the contribution of glycol ethers to anthropogenic SOA is roughly 1% of the current organic aerosol from mobile sources. The contribution of glycol ethers to anthropogenic SOA is roughly 1% of the current organic aerosol from mobile sources and will play a more important role in future anthropogenic SOA

Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO2

Directory of Open Access Journals (Sweden)

T. Liu

2016-01-01

Full Text Available Sulfur dioxide (SO2 can enhance the formation of secondary aerosols from biogenic volatile organic compounds (VOCs, but its influence on secondary aerosol formation from anthropogenic VOCs, particularly complex mixtures like vehicle exhaust, remains uncertain. Gasoline vehicle exhaust (GVE and SO2, a typical pollutant from coal burning, are directly co-introduced into a smog chamber, in this study, to investigate the formation of secondary organic aerosols (SOA and sulfate aerosols through photooxidation. New particle formation was enhanced, while substantial sulfate was formed through the oxidation of SO2 in the presence of high concentration of SO2. Homogenous oxidation by OH radicals contributed a negligible fraction to the conversion of SO2 to sulfate, and instead the oxidation by stabilized Criegee intermediates (sCIs, formed from alkenes in the exhaust reacting with ozone, dominated the conversion of SO2. After 5 h of photochemical aging, GVE's SOA production factor revealed an increase by 60–200 % in the presence of high concentration of SO2. The increase could principally be attributed to acid-catalyzed SOA formation as evidenced by the strong positive linear correlation (R2 = 0.97 between the SOA production factor and in situ particle acidity calculated by the AIM-II model. A high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS resolved OA's relatively lower oxygen-to-carbon (O : C (0.44 ± 0.02 and higher hydrogen-to-carbon (H : C (1.40 ± 0.03 molar ratios for the GVE / SO2 mixture, with a significantly lower estimated average carbon oxidation state (OSc of −0.51 ± 0.06 than −0.19 ± 0.08 for GVE alone. The relative higher mass loading of OA in the experiments with SO2 might be a significant explanation for the lower SOA oxidation degree.

Formation of secondary organic aerosol coating on black carbon particles near vehicular emissions

Science.gov (United States)

Lee, Alex K. Y.; Chen, Chia-Li; Liu, Jun; Price, Derek J.; Betha, Raghu; Russell, Lynn M.; Zhang, Xiaolu; Cappa, Christopher D.

2017-12-01

Black carbon (BC) emitted from incomplete combustion can result in significant impacts on air quality and climate. Understanding the mixing state of ambient BC and the chemical characteristics of its associated coatings is particularly important to evaluate BC fate and environmental impacts. In this study, we investigate the formation of organic coatings on BC particles in an urban environment (Fontana, California) under hot and dry conditions using a soot-particle aerosol mass spectrometer (SP-AMS). The SP-AMS was operated in a configuration that can exclusively detect refractory BC (rBC) particles and their coatings. Using the -log(NOx / NOy) ratio as a proxy for photochemical age of air masses, substantial formation of secondary organic aerosol (SOA) coatings on rBC particles was observed due to active photochemistry in the afternoon, whereas primary organic aerosol (POA) components were strongly associated with rBC from fresh vehicular emissions in the morning rush hours. There is also evidence that cooking-related organic aerosols were externally mixed from rBC. Positive matrix factorization and elemental analysis illustrate that most of the observed SOA coatings were freshly formed, providing an opportunity to examine SOA coating formation on rBCs near vehicular emissions. Approximately 7-20 wt % of secondary organic and inorganic species were estimated to be internally mixed with rBC on average, implying that rBC is unlikely the major condensation sink of SOA in this study. Comparison of our results to a co-located standard high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurement suggests that at least a portion of SOA materials condensed on rBC surfaces were chemically different from oxygenated organic aerosol (OOA) particles that were externally mixed with rBC, although they could both be generated from local photochemistry.

Silver-indium-cadmium control rod behavior and aerosol formation in severe reactor accidents

International Nuclear Information System (INIS)

Petti, D.A.

1987-04-01

Silver-indium-cadmium (Ag-In-Cd) control rod behavior and aerosol formation in severe reactor accidents are examined in an attempt to improve the methodology used to estimate reactor accident source terms. Control rod behavior in both in-pile and out-of-pile experiments is reviewed. A mechanistic model named VAPOR is developed that calculates the downward relocation and simultaneous vaporization behavior of the Ag-In-Cd alloy expected after control rod failure in a severe reactor accident. VAPOR is used to predict the release of silver, indium, and cadmium vapors expected in the Power Burst Facility (PBF) Severe Fuel Damage (SFD) 1-4 experiment. In addition, a sensitivity study is performed. Although cadmium is found to be the most volatile constituent of the alloy, all of the calculations predict that the rapid relocation of the alloy down to cooler portions of the core results in a small release for all three control rod alloy vapors. Potential aerosol formation mechanisms in a severe reactor accident are reviewed. Specifically, models for homogeneous, ion-induced, and heterogeneous nucleation are investigated. These models are applied to silver, cadmium, and CsI to examine the nucleation behavior of these three potential aerosol sources in a severe reactor accident and to illustrate the competition among these mechanisms for vapor depletion. The results indicate that aerosol formation in a severe reactor accident occurs in three stages. In the first stage, ion-induced nucleation causes aerosol generation. During the second stage, ion-induced and heterogeneous nucleation operates as competing pathways for gas-to-particle conversion until sufficient aerosol surface area is generated. In the third stage, ion-induced nucleation ceases; and heterogeneous nucleation becomes the dominant mechanism of gas-to-particle conversion until equilibrium is reached

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.)

Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

Science.gov (United States)

Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.

2013-12-01

The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles cloud formation and potential

High formation of secondary organic aerosol from the photo-oxidation of toluene

OpenAIRE

L. Hildebrandt; N. M. Donahue; S. N. Pandis

2009-01-01

Toluene and other aromatics have long been viewed as the dominant anthropogenic secondary organic aerosol (SOA) precursors, but the SOA mass yields from toluene reported in previous studies vary widely. Experiments conducted in the Carnegie Mellon University environmental chamber to study SOA formation from the photo-oxidation of toluene show significantly larger SOA production than parameterizations employed in current air-quality models. Aerosol mass yields depend on experimental co...

Cloud processing of organic compounds: Secondary organic aerosol and nitrosamine formation

Science.gov (United States)

Hutchings, James W., III

Cloud processing of atmospheric organic compounds has been investigated through field studies, laboratory experiments, and numerical modeling. Observational cloud chemistry studies were performed in northern Arizona and fog studies in central Pennsylvania. At both locations, the cloud and fogs showed low acidity due to neutralization by soil dust components (Arizona) and ammonia (Pennsylvania). The field observations showed substantial concentrations (20-5500 ng•L -1) of volatile organic compounds (VOC) in the cloud droplets. The potential generation of secondary organic aerosol mass through the processing of these anthropogenic VOCs was investigated through laboratory and modeling studies. Under simulated atmospheric conditions, in idealized solutions, benzene, toluene, ethylbenzene, and xylene (BTEX) degraded quickly in the aqueous phase with half lives of approximately three hours. The degradation process yielded less volatile products which would contribute to new aerosol mass upon cloud evaporation. However, when realistic cloud solutions containing natural organic matter were used in the experiments, the reaction kinetics decreased with increasing organic carbon content, resulting in half lives of approximately 7 hours. The secondary organic aerosol (SUA) mass formation potential of cloud processing of BTEX was evaluated. SOA mass formation by cloud processing of BTEX, while strongly dependent on the atmospheric conditions, could contribute up to 9% of the ambient atmospheric aerosol mass, although typically ˜1% appears realistic. Field observations also showed the occurrence of N-nitrosodimethylamine (NDMA), a potent carcinogen, in fogs and clouds (100-340 ng•L -1). Laboratory studies were conducted to investigate the formation of NDMA from nitrous acid and dimethylamine in the homogeneous aqueous phase within cloud droplets. While NDMA was produced in the cloud droplets, the low yields (NDMA with partitioning to droplet must be the source of aqueous

Ice nucleation in sulfuric acid/organic aerosols: implications for cirrus cloud formation

Directory of Open Access Journals (Sweden)

M. R. Beaver

2006-01-01

Full Text Available Using an aerosol flow tube apparatus, we have studied the effects of aliphatic aldehydes (C3 to C10 and ketones (C3 and C9 on ice nucleation in sulfuric acid aerosols. Mixed aerosols were prepared by combining an organic vapor flow with a flow of sulfuric acid aerosols over a small mixing time (~60 s at room temperature. No acid-catalyzed reactions were observed under these conditions, and physical uptake was responsible for the organic content of the sulfuric acid aerosols. In these experiments, aerosol organic content, determined by a Mie scattering analysis, was found to vary with the partial pressure of organic, the flow tube temperature, and the identity of the organic compound. The physical properties of the organic compounds (primarily the solubility and melting point were found to play a dominant role in determining the inferred mode of nucleation (homogenous or heterogeneous and the specific freezing temperatures observed. Overall, very soluble, low-melting organics, such as acetone and propanal, caused a decrease in aerosol ice nucleation temperatures when compared with aqueous sulfuric acid aerosol. In contrast, sulfuric acid particles exposed to organic compounds of eight carbons and greater, of much lower solubility and higher melting temperatures, nucleate ice at temperatures above aqueous sulfuric acid aerosols. Organic compounds of intermediate carbon chain length, C4-C7, (of intermediate solubility and melting temperatures nucleated ice at the same temperature as aqueous sulfuric acid aerosols. Interpretations and implications of these results for cirrus cloud formation are discussed.

Evidence for the role of organics in aerosol particle formation under atmospheric conditions

International Nuclear Information System (INIS)

Metzger, A.; Dommen, J.; Duplissy, J.; Prevot, A.S.H.; Weingartner, E.; Baltensperger, U.; Verheggen, B.; Riipinen, I.; Kulmala, M.; Spracklen, D.V.; Carslaw, K.S.

2010-01-01

New particle formation in the atmosphere is an important parameter in governing the radiative forcing of atmospheric aerosols. However, detailed nucleation mechanisms remain ambiguous, as laboratory data have so far not been successful in explaining atmospheric nucleation. We investigated the formation of new particles in a smog chamber simulating the photochemical formation of H2SO4 and organic condensable species. Nucleation occurs at H2SO4 concentrations similar to those found in the ambient atmosphere during nucleation events. The measured particle formation rates are proportional to the product of the concentrations of H2SO4 and an organic molecule. This suggests that only one H2SO4 molecule and one organic molecule are involved in the rate-limiting step of the observed nucleation process. Parameterizing this process in a global aerosol model results in substantially better agreement with ambient observations compared to control runs.

Uptake of Alkylamines on Dicarboxylic Acids Relevant to Secondary Organic Aerosol Formation

Science.gov (United States)

Marrero-Ortiz, W.; Secrest, J.; Zhang, R.

2017-12-01

Aerosols play a critical role in climate directly by scattering and absorbing solar radiation, and indirectly by functioning as cloud condensation nuclei (CCN); both represent the largest uncertainties in climate predictions. New particle formation contributes significantly to CCN production; however, the mechanisms related to particle nucleation and growth processes are not well understood. Organic acids are atmospherically abundant, and their neutralization by low molecular weight amines may result in the formation of stable low volatility aminium salt products contributing to the growth of secondary organic aerosols and even the alteration of the aerosol properties. The acid-base neutralization of particle phase succinic acid and tartaric acid by low molecular weight aliphatic amines, i.e. methylamine, dimethylamine, and trimethylamine, has been investigated by employing a low-pressure fast flow reactor at 298K with an ion drift - chemical ionization mass spectrometer (ID-CIMS). The heterogeneous uptake is time dependent and influenced by organic acids functionality, alkylamines basicity, and steric effect. The implications of our results to atmospheric nanoparticle growth will be discussed.

An exploratory study of alkali sulfate aerosol formation during biomass combustion

DEFF Research Database (Denmark)

Løj, Lusi Hindiyarti; Frandsen, Flemming; Livbjerg, Hans

2008-01-01

mechanism. The modeling predictions are compared to data from laboratory experiments and entrained flow reactor experiments available in the literature. The analysis support that alkali sulfate aerosols are formed from homogeneous nucleation following a series of steps occurring in the gas phase. The rate......It is still in discussion to what extent alkali sulfate aerosols in biomass combustion are formed in the gas phase by a homogeneous mechanism or involve heterogeneous or catalyzed reactions. The present study investigates sulfate aerosol formation based on calculations with a detailed gas phase......-limiting step may be the oxidation of sulfite to sulfate, rather than the oxidation of SO2 to SO3 proposed previously. Even though the proposed model is consistent with experimental observations, experiments in a rigorously homogeneous system are called for to test its validity....

Simulating SAL formation and aerosol size distribution during SAMUM-I

KAUST Repository

Khan, Basit Ali

2015-04-01

To understand the formation mechanisms of Saharan Air Layer (SAL), we combine model simulations and dust observations collected during the first stage of the Saharan Mineral Dust Experiment (SAMUM-I), which sampled dust events that extended from Morocco to Portugal, and investigated the spatial distribution and the microphysical, optical, chemical, and radiative properties of Saharan mineral dust. We employed the Weather Research Forecast model coupled with the Chemistry/Aerosol module (WRF-Chem) to reproduce the meteorological environment and spatial and size distributions of dust. The experimental domain covers northwest Africa including the southern Sahara, Morocco and part of the Atlantic Ocean with 5 km horizontal grid spacing and 51 vertical layers. The experiments were run from 20 May to 9 June 2006, covering the period of most intensive dust outbreaks. Comparisons of model results with available airborne and ground-based observations show that WRF-Chem reproduces observed meteorological fields as well as aerosol spatial distribution across the entire region and along the airplane\\'s tracks. We evaluated several aerosol uplift processes and found that orographic lifting, aerosol transport through the land/sea interface with steep gradients of meteorological characteristics, and interaction of sea breezes with the continental outflow are key mechanisms that form a surface-detached aerosol plume over the ocean. Comparisons of simulated dust size distributions with airplane and ground-based observations are generally good, but suggest that more detailed treatment of microphysics in the model is required to capture the full-scale effect of large aerosol particles.

Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2

OpenAIRE

Gantt, B.; Kelly, J. T.; Bash, J. O.

2015-01-01

Sea spray aerosols (SSAs) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. Model evaluations of SSA emissions have mainly focused on the global scale, but regional-scale evaluations are also important due to the localized impact of SSAs on atmospheric chemistry near the coast. In this study, SSA emissions in the Community Multiscale Air Quality (CMAQ) model were updated to enhance the...

Identifying precursors and aqueous organic aerosol formation pathways during the SOAS campaign

Directory of Open Access Journals (Sweden)

N. Sareen

2016-11-01

Full Text Available Aqueous multiphase chemistry in the atmosphere can lead to rapid transformation of organic compounds, forming highly oxidized, low-volatility organic aerosol and, in some cases, light-absorbing (brown carbon. Because liquid water is globally abundant, this chemistry could substantially impact climate, air quality, and health. Gas-phase precursors released from biogenic and anthropogenic sources are oxidized and fragmented, forming water-soluble gases that can undergo reactions in the aqueous phase (in clouds, fogs, and wet aerosols, leading to the formation of secondary organic aerosol (SOAAQ. Recent studies have highlighted the role of certain precursors like glyoxal, methylglyoxal, glycolaldehyde, acetic acid, acetone, and epoxides in the formation of SOAAQ. The goal of this work is to identify additional precursors and products that may be atmospherically important. In this study, ambient mixtures of water-soluble gases were scrubbed from the atmosphere into water at Brent, Alabama, during the 2013 Southern Oxidant and Aerosol Study (SOAS. Hydroxyl (OH⚫ radical oxidation experiments were conducted with the aqueous mixtures collected from SOAS to better understand the formation of SOA through gas-phase followed by aqueous-phase chemistry. Total aqueous-phase organic carbon concentrations for these mixtures ranged from 92 to 179 µM-C, relevant for cloud and fog waters. Aqueous OH-reactive compounds were primarily observed as odd ions in the positive ion mode by electrospray ionization mass spectrometry (ESI-MS. Ultra high-resolution Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR-MS spectra and tandem MS (MS–MS fragmentation of these ions were consistent with the presence of carbonyls and tetrols. Products were observed in the negative ion mode and included pyruvate and oxalate, which were confirmed by ion chromatography. Pyruvate and oxalate have been found in the particle phase in many locations (as salts and

Laboratory experiments on the formation and recoil jet transport of aerosol by laser ablation

Science.gov (United States)

Hirooka, Yoshi; Tanaka, Kazuo A.; Imamura, Keisuke; Okazaki, Katsuya

2016-05-01

In a high-repetition rate inertial fusion reactor, the first wall will be subjected to repeated ablation along with pellet implosions, which then leads to the formation of aerosol to scatter and/or deflect laser beams for the subsequent implosion, affecting the overall reactor performance. Proposed in the present work is a method of in-situ directed transport of aerosol particles by the use of laser ablation-induced jet recoil momenta. Lithium and carbon are used as the primary ablation targets, the former of which is known to form aerosol in the form of droplet, and the latter of which tends to form carbon nanotubes. Laboratory-scale experiments have been conducted to irradiate airborne aerosol particles with high-intensity laser to produce ablation-induced jet. Data have indicated a change in aerosol flow direction, but only in the case of lithium.

Aerosol Formation during the Combustion of Straw with Addition of Sorbents

DEFF Research Database (Denmark)

Zeuthen, Frederik Jacob; Jensen, Peter Arendt; Jensen, Jørgen P.

2007-01-01

, calcium phosphate, Bentonite, ICA5000, and clay. The addition of chalk increased the aerosol mass concentration by 24%. Experiments in a laminar flow aerosol condenser with the six sorbents were carried out in the laboratory using a synthetic flue gas to avoid fluctuations in the alkali feeding......The influence of six sorbents on aerosol formation during the combustion of straw in a 100 MW boiler on a Danish power plant has been studied in full-scale. The following sorbents were studied: ammonium sulfate, monocalcium phosphate, Bentonite, ICA5000, clay, and chalk. Bentonite and ICA5000...... are mixtures of clay minerals and consist mainly of the oxides from Fe, Al, and Si. The straw used was Danish wheat and seed grass. Measurements were also made with increased flow of primary air. The experiments showed between 46% and 70% reduction in particle mass concentrations when adding ammonium sulfate...

Heterogeneous photochemistry of imidazole-2-carboxaldehyde: HO2 radical formation and aerosol growth

Directory of Open Access Journals (Sweden)

L. González Palacios

2016-09-01

Full Text Available The multiphase chemistry of glyoxal is a source of secondary organic aerosol (SOA, including its light-absorbing product imidazole-2-carboxaldehyde (IC. IC is a photosensitizer that can contribute to additional aerosol ageing and growth when its excited triplet state oxidizes hydrocarbons (reactive uptake via H-transfer chemistry. We have conducted a series of photochemical coated-wall flow tube (CWFT experiments using films of IC and citric acid (CA, an organic proxy and H donor in the condensed phase. The formation rate of gas-phase HO2 radicals (PHO2 was measured indirectly by converting gas-phase NO into NO2. We report on experiments that relied on measurements of NO2 formation, NO loss and HONO formation. PHO2 was found to be a linear function of (1 the [IC]  ×  [CA] concentration product and (2 the photon actinic flux. Additionally, (3 a more complex function of relative humidity (25 %  <  RH  <  63 % and of (4 the O2 ∕ N2 ratio (15 %  <  O2 ∕ N2  <  56 % was observed, most likely indicating competing effects of dilution, HO2 mobility and losses in the film. The maximum PHO2 was observed at 25–55 % RH and at ambient O2 ∕ N2. The HO2 radicals form in the condensed phase when excited IC triplet states are reduced by H transfer from a donor, CA in our system, and subsequently react with O2 to regenerate IC, leading to a catalytic cycle. OH does not appear to be formed as a primary product but is produced from the reaction of NO with HO2 in the gas phase. Further, seed aerosols containing IC and ammonium sulfate were exposed to gas-phase limonene and NOx in aerosol flow tube experiments, confirming significant PHO2 from aerosol surfaces. Our results indicate a potentially relevant contribution of triplet state photochemistry for gas-phase HO2 production, aerosol growth and ageing in the atmosphere.

[Estimate of the formation potential of secondary organic aerosol in Beijing summertime].

Science.gov (United States)

Lü, Zi-Feng; Hao, Ji-Ming; Duan, Jing-Chun; Li, Jun-Hua

2009-04-15

Fractional aerosol coefficients (FAC) are used in conjunction with measurements of volatile organic compounds (VOC) during ozone episodes to estimate the formation potential of secondary organic aerosols (SOA) in the summertime of Beijing. The estimation is based on the actual atmospheric conditions of Beijing, and benzene and isoprene are considered as the precursors of SOA. The results show that 31 out of 70 measured VOC species are SOA precursors, and the total potential SOA formation is predicted to be 8.48 microg/m3, which accounts for 30% of fine organic particle matter. Toluene, xylene, pinene, ethylbenzene and n-undecane are the 5 largest contributors to SOA production and account for 20%, 22%, 14%, 9% and 4% of total SOA production, respectively. The anthropogenic aromatic compounds, which yield 76% of the calculated SOA, are the major source of SOA. The biogenic alkenes, alkanes and carbonyls produce 16%, 7% and 1% of SOA formation, respectively. The major components of produced SOA are expected to be aromatic compounds, aliphatic acids, carbonyls and aliphatic nitrates, which contribute to 72%, 14%, 11% and 3% of SOA mass, respectively. The SOA precursors have relatively low atmospheric concentrations and low ozone formation potential. Hence, SOA formation potential of VOC species, in addition to their atmospheric concentrations and ozone formation potential, should be considered in policy making process of VOCs control.

Reactive oxidation products promote secondary organic aerosol formation from green leaf volatiles

Directory of Open Access Journals (Sweden)

J. F. Hamilton

2009-06-01

Full Text Available Green leaf volatiles (GLVs are an important group of chemicals released by vegetation which have emission fluxes that can be significantly increased when plants are damaged or stressed. A series of simulation chamber experiments has been conducted at the European Photoreactor in Valencia, Spain, to investigate secondary organic aerosol (SOA formation from the atmospheric oxidation of the major GLVs cis-3-hexenylacetate and cis-3-hexen-1-ol. Liquid chromatography-ion trap mass spectrometry was used to identify chemical species present in the SOA. Cis-3-hexen-1-ol proved to be a more efficient SOA precursor due to the high reactivity of its first generation oxidation product, 3-hydroxypropanal, which can hydrate and undergo further reactions with other aldehydes resulting in SOA dominated by higher molecular weight oligomers. The lower SOA yields produced from cis-3-hexenylacetate are attributed to the acetate functionality, which inhibits oligomer formation in the particle phase. Based on observed SOA yields and best estimates of global emissions, these compounds may be calculated to be a substantial unidentified global source of SOA, contributing 1–5 TgC yr⁻¹, equivalent to around a third of that predicted from isoprene. Molecular characterization of the SOA, combined with organic mechanistic information, has provided evidence that the formation of organic aerosols from GLVs is closely related to the reactivity of their first generation atmospheric oxidation products, and indicates that this may be a simple parameter that could be used in assessing the aerosol formation potential for other unstudied organic compounds in the atmosphere.

Secondary organic aerosol formation and composition from the photo-oxidation of methyl chavicol (estragole)

Science.gov (United States)

Pereira, K. L.; Hamilton, J. F.; Rickard, A. R.; Bloss, W. J.; Alam, M. S.; Camredon, M.; Muñoz, A.; Vázquez, M.; Borrás, E.; Ródenas, M.

2014-06-01

The increasing demand for palm oil for uses in biofuel and food products is leading to rapid expansion of oil palm agriculture. Methyl chavicol (also known as estragole and 1-allyl-4-methoxybenzene) is an oxygenated biogenic volatile organic compound (VOC) that was recently identified as the main floral emission from an oil palm plantation in Malaysian Borneo. The emissions of methyl chavicol observed may impact regional atmospheric chemistry, but little is known of its ability to form secondary organic aerosol (SOA). The photo-oxidation of methyl chavicol was investigated at the European Photoreactor chamber as a part of the atmospheric chemistry of methyl chavicol (ATMECH) project. Aerosol samples were collected using a particle into liquid sampler (PILS) and analysed offline using an extensive range of instruments including; high-performance liquid chromatography mass spectrometry (HPLC-ITMS), high-performance liquid chromatography quadrupole time-of-flight mass spectrometry (HPLC-QTOFMS) and Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS). The SOA yield was determined as 18 and 29% for an initial VOC mixing ratio of 212 and 460 ppbv (parts per billion by volume) respectively; using a VOC:NOx ratio of ~5:1. In total, 59 SOA compounds were observed and the structures of 10 compounds have been identified using high-resolution tandem mass spectrometry. The addition of hydroxyl and/or nitro-functional groups to the aromatic ring appears to be an important mechanistic pathway for aerosol formation. This results in the formation of compounds with both low volatility and high O:C ratios, where functionalisation rather than fragmentation is mainly observed as a result of the stability of the ring. The SOA species observed can be characterised as semi-volatile to low-volatility oxygenated organic aerosol (SVOOA and LVOOA) components and therefore may be important in aerosol formation and growth.

Evaluation of the atmospheric significance of multiphase reactions in atmospheric secondary organic aerosol formation

Directory of Open Access Journals (Sweden)

Gelencsér

2005-01-01

Full Text Available In a simple conceptual cloud-aerosol model the mass of secondary organic aerosol (SOA that may be formed in multiphase reaction in an idealized scenario involving two cloud cycles separated with a cloud-free period is evaluated. The conditions are set to those typical of continental clouds, and each parameter used in the model calculations is selected as a mean of available observational data of individual species for which the multiphase SOA formation route has been established. In the idealized setting gas and aqueous-phase reactions are both considered, but only the latter is expected to yield products of sufficiently low volatility to be retained by aerosol particles after the cloud dissipates. The key variable of the model is the Henry-constant which primarily determines how important multiphase reactions are relative to gas-phase photooxidation processes. The precursor considered in the model is assumed to already have some affinity to water, i.e. it is a compound having oxygen-containing functional group(s. As a principal model output an aerosol yield parameter is calculated for the multiphase SOA formation route as a function of the Henry-constant, and has been found to be significant already above H~103 M atm-1. Among the potential precursors that may be eligible for this mechanism based on their Henry constants, there are a suite of oxygenated compounds such as primary oxidation products of biogenic and anthropogenic hydrocarbons, including, for example, pinonaldehyde. Finally, the analogy of multiphase SOA formation to in-cloud sulfate production is exploited.

Modeling organic aerosols in a megacity: potential contribution of semi-volatile and intermediate volatility primary organic compounds to secondary organic aerosol formation

Directory of Open Access Journals (Sweden)

A. Hodzic

2010-06-01

Full Text Available It has been established that observed local and regional levels of secondary organic aerosols (SOA in polluted areas cannot be explained by the oxidation and partitioning of anthropogenic and biogenic VOC precursors, at least using current mechanisms and parameterizations. In this study, the 3-D regional air quality model CHIMERE is applied to estimate the potential contribution to SOA formation of recently identified semi-volatile and intermediate volatility organic precursors (S/IVOC in and around Mexico City for the MILAGRO field experiment during March 2006. The model has been updated to include explicitly the volatility distribution of primary organic aerosols (POA, their gas-particle partitioning and the gas-phase oxidation of the vapors. Two recently proposed parameterizations, those of Robinson et al. (2007 ("ROB" and Grieshop et al. (2009 ("GRI" are compared and evaluated against surface and aircraft measurements. The 3-D model results are assessed by comparing with the concentrations of OA components from Positive Matrix Factorization of Aerosol Mass Spectrometer (AMS data, and for the first time also with oxygen-to-carbon ratios derived from high-resolution AMS measurements. The results show a substantial enhancement in predicted SOA concentrations (2–4 times with respect to the previously published base case without S/IVOCs (Hodzic et al., 2009, both within and downwind of the city leading to much reduced discrepancies with the total OA measurements. Model improvements in OA predictions are associated with the better-captured SOA magnitude and diurnal variability. The predicted production from anthropogenic and biomass burning S/IVOC represents 40–60% of the total measured SOA at the surface during the day and is somewhat larger than that from commonly measured aromatic VOCs, especially at the T1 site at the edge of the city. The SOA production from the continued multi-generation S/IVOC oxidation products continues actively

Secondary organic aerosol formation through cloud processing of aromatic VOCs

Science.gov (United States)

Herckes, P.; Hutchings, J. W.; Ervens, B.

2010-12-01

Field observations have shown substantial concentrations (20-5,500 ng L-1) of aromatic volatile organic compounds (VOC) in cloud droplets. The potential generation of secondary organic aerosol mass through the processing of these anthropogenic VOCs was investigated through laboratory and modeling studies. Under simulated atmospheric laboratory conditions, in idealized solutions, benzene, toluene, ethylbenzene, and xylene (BTEX) degraded quickly in the aqueous phase. The degradation process yielded less volatile products which would contribute to new aerosol mass upon cloud evaporation. However, when realistic cloud solutions containing natural organic matter were used in the experiments, the reaction rates decreased with increasing organic carbon content. Kinetic data derived from these experiments were used as input to a multiphase box model in order to evaluate the secondary organic aerosol (SOA) mass formation potential of cloud processing of BTEX. Model results will be presented that quantify the SOA amounts from these aqueous phase pathways. The efficiency of this multiphase SOA source will be compared to SOA yields from the same aromatics as treated in traditional SOA models that are restricted to gas phase oxidation and subsequent condensation on particles.

Photochemical Formation of Aerosol in Planetary Atmospheres: Photon and Water Mediated Chemistry of SO_2

Science.gov (United States)

Kroll, Jay A.; Donaldson, D. J.; Vaida, Veronica

2016-06-01

Sulfur compounds have been observed in a number of planetary atmospheres throughout our solar system. Our current understanding of sulfur chemistry explains much of what we observe in Earth's atmosphere. However, several discrepancies between modeling and observations of the Venusian atmosphere show there are still problems in our fundamental understanding of sulfur chemistry. This is of particular concern due to the important role sulfur compounds play in the formation of aerosols, which have a direct impact on planetary climates, including Earth's. We investigate the role of water complexes in the hydration of sulfur oxides and dehydration of sulfur acids and will present spectroscopic studies to document such effects. I will present recent work investigating mixtures of SO_2 and water that generate large quantities of aerosol when irradiated with solar UV light, even in the absence of traditional OH chemistry. I will discuss a proposed mechanism for the formation of sulfurous acid (H_2SO_3) and present recent experimental work that supports this proposed mechanism. Additionally, the implications that photon-induced hydration of SO_2 has for aerosol formation in the atmosphere of earth as well as other planetary atmospheres will be discussed.

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.

Effect of flavoring chemicals on free radical formation in electronic cigarette aerosols.

Science.gov (United States)

Bitzer, Zachary T; Goel, Reema; Reilly, Samantha M; Elias, Ryan J; Silakov, Alexey; Foulds, Jonathan; Muscat, Joshua; Richie, John P

2018-05-20

Flavoring chemicals, or flavorants, have been used in electronic cigarettes (e-cigarettes) since their inception; however, little is known about their toxicological effects. Free radicals present in e-cigarette aerosols have been shown to induce oxidative stress resulting in damage to proliferation, survival, and inflammation pathways in the cell. Aerosols generated from e-liquid solvents alone contain high levels of free radicals but few studies have looked at how these toxins are modulated by flavorants. We investigated the effects of different flavorants on free radical production in e-cigarette aerosols. Free radicals generated from 49 commercially available e-liquid flavors were captured and analyzed using electron paramagnetic resonance (EPR). The flavorant composition of each e-liquid was analyzed by gas chromatography mass spectroscopy (GCMS). Radical production was correlated with flavorant abundance. Ten compounds were identified and analyzed for their impact on free radical generation. Nearly half of the flavors modulated free radical generation. Flavorants with strong correlations included β-damascone, δ-tetradecalactone, γ-decalactone, citral, dipentene, ethyl maltol, ethyl vanillin, ethyl vanillin PG acetal, linalool, and piperonal. Dipentene, ethyl maltol, citral, linalool, and piperonal promoted radical formation in a concentration-dependent manner. Ethyl vanillin inhibited the radical formation in a concentration dependent manner. Free radical production was closely linked with the capacity to oxidize biologically-relevant lipids. Our results suggest that flavoring agents play an important role in either enhancing or inhibiting the production of free radicals in flavored e-cigarette aerosols. This information is important for developing regulatory strategies aimed at reducing potential harm from e-cigarettes. Copyright © 2018 Elsevier Inc. All rights reserved.

Global two-channel AVHRR aerosol climatology: effects of stratospheric aerosols and preliminary comparisons with MODIS and MISR retrievals

International Nuclear Information System (INIS)

Geogdzhayev, Igor V.; Mishchenko, Michael I.; Liu Li; Remer, Lorraine

2004-01-01

We present an update on the status of the global climatology of the aerosol column optical thickness and Angstrom exponent derived from channel-1 and -2 radiances of the Advanced Very High Resolution Radiometer (AVHRR) in the framework of the Global Aerosol Climatology Project (GACP). The latest version of the climatology covers the period from July 1983 to September 2001 and is based on an adjusted value of the diffuse component of the ocean reflectance as derived from extensive comparisons with ship sun-photometer data. We use the updated GACP climatology and Stratospheric Aerosol and Gas Experiment (SAGE) data to analyze how stratospheric aerosols from major volcanic eruptions can affect the GACP aerosol product. One possible retrieval strategy based on the AVHRR channel-1 and -2 data alone is to infer both the stratospheric and the tropospheric aerosol optical thickness while assuming fixed microphysical models for both aerosol components. The second approach is to use the SAGE stratospheric aerosol data in order to constrain the AVHRR retrieval algorithm. We demonstrate that the second approach yields a consistent long-term record of the tropospheric aerosol optical thickness and Angstrom exponent. Preliminary comparisons of the GACP aerosol product with MODerate resolution Imaging Spectrometer (MODIS) and Multiangle Imaging Spectro-Radiometer aerosol retrievals show reasonable agreement, the GACP global monthly optical thickness being lower than the MODIS one by approximately 0.03. Larger differences are observed on a regional scale. Comparisons of the GACP and MODIS Angstrom exponent records are less conclusive and require further analysis

Secondary organic aerosol formation from a large number of reactive man-made organic compounds

Energy Technology Data Exchange (ETDEWEB)

Derwent, Richard G., E-mail: r.derwent@btopenworld.com [rdscientific, Newbury, Berkshire (United Kingdom); Jenkin, Michael E. [Atmospheric Chemistry Services, Okehampton, Devon (United Kingdom); Utembe, Steven R.; Shallcross, Dudley E. [School of Chemistry, University of Bristol, Bristol (United Kingdom); Murrells, Tim P.; Passant, Neil R. [AEA Environment and Energy, Harwell International Business Centre, Oxon (United Kingdom)

2010-07-15

A photochemical trajectory model has been used to examine the relative propensities of a wide variety of volatile organic compounds (VOCs) emitted by human activities to form secondary organic aerosol (SOA) under one set of highly idealised conditions representing northwest Europe. This study applied a detailed speciated VOC emission inventory and the Master Chemical Mechanism version 3.1 (MCM v3.1) gas phase chemistry, coupled with an optimised representation of gas-aerosol absorptive partitioning of 365 oxygenated chemical reaction product species. In all, SOA formation was estimated from the atmospheric oxidation of 113 emitted VOCs. A number of aromatic compounds, together with some alkanes and terpenes, showed significant propensities to form SOA. When these propensities were folded into a detailed speciated emission inventory, 15 organic compounds together accounted for 97% of the SOA formation potential of UK man made VOC emissions and 30 emission source categories accounted for 87% of this potential. After road transport and the chemical industry, SOA formation was dominated by the solvents sector which accounted for 28% of the SOA formation potential.

Substantial secondary organic aerosol formation in a coniferous forest: observations of both day- and nighttime chemistry

Directory of Open Access Journals (Sweden)

A. K. Y. Lee

2016-06-01

Full Text Available Substantial biogenic secondary organic aerosol (BSOA formation was investigated in a coniferous forest mountain region in Whistler, British Columbia. A largely biogenic aerosol growth episode was observed, providing a unique opportunity to investigate BSOA formation chemistry in a forested environment with limited influence from anthropogenic emissions. Positive matrix factorization of aerosol mass spectrometry (AMS measurement identified two types of BSOA (BSOA-1 and BSOA-2, which were primarily generated by gas-phase oxidation of monoterpenes and perhaps sesquiterpenes. The temporal variations of BSOA-1 and BSOA-2 can be explained by gas–particle partitioning in response to ambient temperature and the relative importance of different oxidation mechanisms between day and night. While BSOA-1 arises from gas-phase ozonolysis and nitrate radical chemistry at night, BSOA-2 is likely less volatile than BSOA-1 and consists of products formed via gas-phase oxidation by OH radical and ozone during the day. Organic nitrates produced through nitrate radical chemistry can account for 22–33 % of BSOA-1 mass at night. The mass spectra of BSOA-1 and BSOA-2 have higher values of the mass fraction of m/z 91 (f91 compared to the background organic aerosol. Using f91 to evaluate BSOA formation pathways in this unpolluted, forested region, heterogeneous oxidation of BSOA-1 is a minor production pathway of BSOA-2.

Update to the R33 cross section file format

International Nuclear Information System (INIS)

Vickridge, I.C.

2003-01-01

In September 1991, in response to the workshop on cross sections for Ion Beam Analysis (IBA) held in Namur (July 1991, Nuclear Instruments and Methods B66(1992)), a simple ascii format was proposed to facilitate transfer and collation of nuclear reaction cross section data for Ion Beam Analysis (IBA) and especially for Nuclear Reaction Analysis (NRA). Although intended only as a discussion document, the ascii format - referred to as the R33 (Report 33) format - has become a de facto standard. In the decade since this first proposal there have been spectacular advances in computing power and in software usability, however the cross-platform compatibility of the ascii character set has ensured that the need for an ascii format remains. Nuclear reaction cross section data for Nuclear Reaction analysis has been collected and archived on internet web sites over the last decade. This data has largely been entered in the R33 format, although there is a series of elastic cross sections that are expressed as the ratio to the corresponding Rutherford cross sections that have been entered in a format referred to as RTR (ratio to Rutherford). During this time the R33 format has been modified and added to - firstly to take into account angular distributions, which were not catered for in the first proposal, and more recently to cater for elastic cross sections expressed as the ratio-to- Rutherford, which it is useful to have for some elastic scattering programs. It is thus timely to formally update the R33 format. There also exists the large nuclear cross section data collections of the Nuclear Data Network - of which the core centres are the OECD NEA Nuclear Data Bank, the IAEA Nuclear Data Section, the Brookhaven National Laboratory National Nuclear Data Centre and CJD IPPE Obninsk, Russia. The R33 format is now proposed to become a legal computational format for the NDN. It is thus also necessary to provide an updated formal definition of the R33 format in order to provide

Rapid Formation of Molecular Bromine from Deliquesced NaBr Aerosol in the Presence of Ozone and UV Light

Science.gov (United States)

The formation of gas-phase bromine from aqueous sodium bromide aerosols is investigated through a combination of chamber experiments and chemical kinetics modeling. Experiments show that Br2(g) is produced rapidly from deliquesced NaBr aerosols in the presence of OH radicals prod...

Study of particle size distribution and formation mechanism of radioactive aerosols generated in high-energy neutron fields

CERN Document Server

Endo, A; Noguchi, H; Tanaka, S; Iida, T; Furuichi, S; Kanda, Y; Oki, Y

2003-01-01

The size distributions of sup 3 sup 8 Cl, sup 3 sup 9 Cl, sup 8 sup 2 Br and sup 8 sup 4 Br aerosols generated by irradiations of argon and krypton gases containing di-octyl phthalate (DOP) aerosols with 45 MeV and 65 MeV quasi-monoenergetic neutrons were measured in order to study the formation mechanism of radioactive particles in high energy radiation fields. The effects of the size distribution of the radioactive aerosols on the size of the added DOP aerosols, the energy of the neutrons and the kinds of nuclides were studied. The observed size distributions of the radioactive particles were explained by attachment of the radioactive atoms generated by the neutron-induced reactions to the DOP aerosols. (author)

Coastal new particle formation: environmental conditions and aerosol physicochemical characteristics during nucleation bursts

NARCIS (Netherlands)

O'Dowd, C.D.; Haemeri, K.; Maekelae, J.M.; Vaekeva, M.; Aalto, P.; Leeuw, G. de; Kunz, G.J.; Becker, E.; Hansson, H-C.; Allen, A.G.; Harrison, R.M.; Berresheim, H.; Kleefeld, C.; Geever, M.; Jennings, S.G.; Kulmala, M.

2002-01-01

Nucleation mode aerosol was characterized during coastal nucleation events at Mace Head during intensive New Particle Formation and Fate in the Coastal Environment (PARFORCE) field campaigns in September 1998 and June 1999. Nucleation events were observed almost on a daily basis during the

Exchanges in boundary layer and low troposphere and consequences on pollution of Fos-Berre-Marseille area (ESCOMPTE experiment); Les aerosols: emissions, formation d'aerosols organiques secondaires, transport longue distance. Zoom sur les aerosols carbones en Europe

Energy Technology Data Exchange (ETDEWEB)

Guillaume, B

2006-01-15

There are two types of 'carbonaceous aerosols': 'black carbon' (BC) and 'organic carbon'(OC). BC is directly emitted in the atmosphere while OC is either directly emitted (primary OC, OCp) or secondarily formed through oxidation processes in the atmosphere (secondary organic aerosols, SOA). Complexity of carbonaceous aerosols is still poorly represented in existing aerosol models and uncertainties appear mainly both in their emission inventories and in their complex atmospheric evolution (transport, gas-particle interactions, dry/wet deposition), making difficult the estimation of their radiative impact. In this framework, I developed during my PhD at Laboratoire d'Aerologie, a new approach to deal with this complexity, with implementation of both a new carbonaceous aerosol emission inventory and a new aerosol modelling tool at global scale. My work is divided in 5 different tasks: - better characterisation of BC and OCp emissions, achieved through the development of a new emission inventory from fossil fuel and biofuel combustion sources (industrial, domestic and mobile sources). This inventory provides BC and OCp emissions for Europe at 25 km * 25 km resolution for the years 1990, 1995, 2000, 2005 and 2010, with two additional regional zooms: on France, at 10 km * 10 km resolution for the years 2000 and 2010 with improved road traffic, and in Marseille region (Escompte campaign, 1999,-2001) at 1 km * 1 km resolution for the year 1999; - better modelling of carbonaceous aerosol complex atmospheric evolution, through coupling of a global scale gas transport/chemistry model (TM4) with an aerosol module (ORISAM) featuring size-distributed aerosols (on 8 diameter sections from 40 nm to 10 {mu}m) organic/inorganic chemical composition and explicit treatment of SOA formation; - simulations with this new aerosol model ORISAM-TM4 and model/measurements comparisons to study BC and OC long-range transport; - sensitivity tests on SOA

The critical assessment of vapour pressure estimation methods for use in modelling the formation of atmospheric organic aerosol

Directory of Open Access Journals (Sweden)

M. H. Barley

2010-01-01

Full Text Available A selection of models for estimating vapour pressures have been tested against experimental data for a set of compounds selected for their particular relevance to the formation of atmospheric aerosol by gas-liquid partitioning. The experimental vapour pressure data (all <100 Pa of 45 multifunctional compounds provide a stringent test of the estimation techniques, with a recent complex group contribution method providing the best overall results. The effect of errors in vapour pressures upon the formation of organic aerosol by gas-liquid partitioning in an atmospherically relevant example is also investigated. The mass of organic aerosol formed under typical atmospheric conditions was found to be very sensitive to the variation in vapour pressure values typically present when comparing estimation methods.

Role of aldehyde chemistry and NOx concentrations in secondary organic aerosol formation

Directory of Open Access Journals (Sweden)

P. O. Wennberg

2010-08-01

Full Text Available Aldehydes are an important class of products from atmospheric oxidation of hydrocarbons. Isoprene (2-methyl-1,3-butadiene, the most abundantly emitted atmospheric non-methane hydrocarbon, produces a significant amount of secondary organic aerosol (SOA via methacrolein (a C4-unsaturated aldehyde under urban high-NOx conditions. Previously, we have identified peroxy methacryloyl nitrate (MPAN as the important intermediate to isoprene and methacrolein SOA in this NOx regime. Here we show that as a result of this chemistry, NO2 enhances SOA formation from methacrolein and two other α, β-unsaturated aldehydes, specifically acrolein and crotonaldehyde, a NOx effect on SOA formation previously unrecognized. Oligoesters of dihydroxycarboxylic acids and hydroxynitrooxycarboxylic acids are observed to increase with increasing NO2/NO ratio, and previous characterizations are confirmed by both online and offline high-resolution mass spectrometry techniques. Molecular structure also determines the amount of SOA formation, as the SOA mass yields are the highest for aldehydes that are α, β-unsaturated and contain an additional methyl group on the α-carbon. Aerosol formation from 2-methyl-3-buten-2-ol (MBO232 is insignificant, even under high-NO2 conditions, as PAN (peroxy acyl nitrate, RC(OOONO2 formation is structurally unfavorable. At atmospherically relevant NO2/NO ratios (3–8, the SOA yields from isoprene high-NOx photooxidation are 3 times greater than previously measured at lower NO2/NO ratios. At sufficiently high NO2 concentrations, in systems of α, β-unsaturated aldehydes, SOA formation from subsequent oxidation of products from acyl peroxyl radicals+NO2 can exceed that from RO2+HO2 reactions under the same inorganic seed conditions, making RO2+NO2 an important channel for SOA formation.

Role of aldehyde chemistry and NOx concentrations in secondary organic aerosol formation

Science.gov (United States)

Chan, A. W. H.; Chan, M. N.; Surratt, J. D.; Chhabra, P. S.; Loza, C. L.; Crounse, J. D.; Yee, L. D.; Flagan, R. C.; Wennberg, P. O.; Seinfeld, J. H.

2010-08-01

Aldehydes are an important class of products from atmospheric oxidation of hydrocarbons. Isoprene (2-methyl-1,3-butadiene), the most abundantly emitted atmospheric non-methane hydrocarbon, produces a significant amount of secondary organic aerosol (SOA) via methacrolein (a C4-unsaturated aldehyde) under urban high-NOx conditions. Previously, we have identified peroxy methacryloyl nitrate (MPAN) as the important intermediate to isoprene and methacrolein SOA in this NOx regime. Here we show that as a result of this chemistry, NO2 enhances SOA formation from methacrolein and two other α, β-unsaturated aldehydes, specifically acrolein and crotonaldehyde, a NOx effect on SOA formation previously unrecognized. Oligoesters of dihydroxycarboxylic acids and hydroxynitrooxycarboxylic acids are observed to increase with increasing NO2/NO ratio, and previous characterizations are confirmed by both online and offline high-resolution mass spectrometry techniques. Molecular structure also determines the amount of SOA formation, as the SOA mass yields are the highest for aldehydes that are α, β-unsaturated and contain an additional methyl group on the α-carbon. Aerosol formation from 2-methyl-3-buten-2-ol (MBO232) is insignificant, even under high-NO2 conditions, as PAN (peroxy acyl nitrate, RC(O)OONO2) formation is structurally unfavorable. At atmospherically relevant NO2/NO ratios (3-8), the SOA yields from isoprene high-NOx photooxidation are 3 times greater than previously measured at lower NO2/NO ratios. At sufficiently high NO2 concentrations, in systems of α, β-unsaturated aldehydes, SOA formation from subsequent oxidation of products from acyl peroxyl radicals+NO2 can exceed that from RO2+HO2 reactions under the same inorganic seed conditions, making RO2+NO2 an important channel for SOA formation.

Formation and evolution of aerosols in filtered air and in natural air. Effect of radioactivity; Formation et evolution des aerosols dans l'air filtre et dans l'air naturel action de la radioactivite

Energy Technology Data Exchange (ETDEWEB)

Madelaine, G J [Commissariat a l' Energie Atomique, 92 - Fontenay-aux-Roses (France). Centre d' Etudes Nucleaires

1968-06-01

Results are presented concerning the formation, the evolution, the coagulation and the electrical charge of aerosols which form in natural filtered air containing only gaseous impurities, under the influence of solar light (photolysis) and of radioactive disintegrations (radiolysis). The modifications brought about in the aerosol by an increase in the sulphur dioxide content and in the natural radioactive gas content are studied. The work is then repeated with non-filtered natural atmospheric air. A comparison is also made of the behaviour of non-radioactive and radioactive particles (active thoron deposit). In conclusion, the possible consequences of these phenomena on the origin and the size distribution of particles occurring in the atmosphere is considered. (author) [French] On expose les resultats obtenus sur la formation, l'evolution, la coagulation et la charge electrique des aerosols qui se forment dans l'air naturel filtre, ne contenant que des impuretes gazeuses, sous l'influence de la lumiere solaire (photolyse) et des desintegrations radioactives (radiolyse). On examine les modifications apportees a l'aerosol forme par l'augmentation de la teneur de l'air en anhydride sulfureux et en gaz radioactif naturel. Cette etude est ensuite reprise mais avec de l'air naturel atmospherique non filtre. On compare egalement le comportement des particules non radioactives et radioactives (depot actif du thoron). En conclusion, on examine les consequences que peuvent avoir ces phenomenes sur l'origine et la granulometrie des particules contenues dans l'atmosphere. (auteur)

Secondary organic aerosol formation from ozone-initiated reactions with nicotine and secondhand tobacco smoke

Science.gov (United States)

Sleiman, Mohamad; Destaillats, Hugo; Smith, Jared D.; Liu, Chen-Lin; Ahmed, Musahid; Wilson, Kevin R.; Gundel, Lara A.

2010-11-01

We used controlled laboratory experiments to evaluate the aerosol-forming potential of ozone reactions with nicotine and secondhand smoke. Special attention was devoted to real-time monitoring of the particle size distribution and chemical composition of SOA as they are believed to be key factors determining the toxicity of SOA. The experimental approach was based on using a vacuum ultraviolet photon ionization time-of-flight aerosol mass spectrometer (VUV-AMS), a scanning mobility particle sizer (SMPS) and off-line thermal desorption coupled to mass spectrometry (TD-GC-MS) for gas-phase byproducts analysis. Results showed that exposure of SHS to ozone induced the formation of ultrafine particles (smoke that is associated with the formation of ultrafine particles (UFP) through oxidative aging of secondhand smoke. The significance of this chemistry for indoor exposure and health effects is highlighted.

Updating sea spray aerosol emissions in the Community Multiscale Air Quality (CMAQ) model version 5.0.2

Science.gov (United States)

Gantt, B.; Kelly, J. T.; Bash, J. O.

2015-11-01

Sea spray aerosols (SSAs) impact the particle mass concentration and gas-particle partitioning in coastal environments, with implications for human and ecosystem health. Model evaluations of SSA emissions have mainly focused on the global scale, but regional-scale evaluations are also important due to the localized impact of SSAs on atmospheric chemistry near the coast. In this study, SSA emissions in the Community Multiscale Air Quality (CMAQ) model were updated to enhance the fine-mode size distribution, include sea surface temperature (SST) dependency, and reduce surf-enhanced emissions. Predictions from the updated CMAQ model and those of the previous release version, CMAQv5.0.2, were evaluated using several coastal and national observational data sets in the continental US. The updated emissions generally reduced model underestimates of sodium, chloride, and nitrate surface concentrations for coastal sites in the Bay Regional Atmospheric Chemistry Experiment (BRACE) near Tampa, Florida. Including SST dependency to the SSA emission parameterization led to increased sodium concentrations in the southeastern US and decreased concentrations along parts of the Pacific coast and northeastern US. The influence of sodium on the gas-particle partitioning of nitrate resulted in higher nitrate particle concentrations in many coastal urban areas due to increased condensation of nitric acid in the updated simulations, potentially affecting the predicted nitrogen deposition in sensitive ecosystems. Application of the updated SSA emissions to the California Research at the Nexus of Air Quality and Climate Change (CalNex) study period resulted in a modest improvement in the predicted surface concentration of sodium and nitrate at several central and southern California coastal sites. This update of SSA emissions enabled a more realistic simulation of the atmospheric chemistry in coastal environments where marine air mixes with urban pollution.

Secondary Organic Aerosol Formation from Acetylene (C2H2: seed effect on SOA yields due to organic photochemistry in the aerosol aqueous phase

Directory of Open Access Journals (Sweden)

P. J. Ziemann

2009-03-01

Full Text Available The lightest Non Methane HydroCarbon (NMHC, i.e., acetylene (C2H2 is found to form secondary organic aerosol (SOA. Contrary to current belief, the number of carbon atoms, n, for a NMHC to act as SOA precursor is lowered to n=2 here. The OH-radical initiated oxidation of C2H2 forms glyoxal (CHOCHO as the highest yield product, and >99% of the SOA from C2H2 is attributed to CHOCHO. SOA formation from C2H2 and CHOCHO was studied in a photochemical and a dark simulation chamber. Further, the experimental conditions were varied with respect to the chemical composition of the seed aerosols, mild acidification with sulphuric acid (SA, 3aerosols is found responsible for this seed effect. WSOC photochemistry enhances the SOA source from CHOCHO, while seeds containing amino acids (AA and/or SA showed among the lowest of all YSOA values, and largely suppress the photochemical enhancement on the rate of CHOCHO uptake. Our results give first evidence for the importance of heterogeneous photochemistry of CHOCHO in SOA formation, and identify a potential bias in the currently available YSOA data for other SOA precursor NMHCs. We demonstrate that SOA formation via the aqueous phase is not limited to cloud droplets, but proceeds also in the absence of clouds, i.e., does not stop once a cloud droplet evaporates. Atmospheric models need to be expanded to include SOA formation from WSOC photochemistry of CHOCHO, and possibly other α-dicarbonyls, in aqueous aerosols.

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

CERN Document Server

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

2015-01-01

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

Formation of high-molecular-weight compounds via the heterogeneous reactions of gaseous C8-C10 n-aldehydes in the presence of atmospheric aerosol components

Science.gov (United States)

Han, Yuemei; Kawamura, Kimitaka; Chen, Qingcai; Mochida, Michihiro

2016-02-01

A laboratory study on the heterogeneous reactions of straight-chain aldehydes was performed by exposing n-octanal, nonanal, and decanal vapors to ambient aerosol particles. The aerosol and blank filters were extracted using methanol. The extracts were nebulized and the resulting compositions were examined using a high-resolution time-of-flight aerosol mass spectrometer. The mass spectral analysis showed that the exposures of the aldehydes to aerosol samples increased the peak intensities in the high mass range. The peaks in the mass spectra of the aerosol samples after exposure to different aldehydes were characterized by a homologous series of peak shifts due to the addition of multiple CH2 units. This result is explained by the formation of high-molecular-weight (HMW) compounds that contain single or multiple aldehyde moieties. The HMW fragment peaks for the blank filters exposed to n-aldehydes were relatively weak, indicating an important contribution from the ambient aerosol components to the formation of the HMW compounds. Among the factors affecting the overall interaction of aldehydes with atmospheric aerosol components, gas phase diffusion possibly limited the reactions under the studied conditions; therefore, their occurrence to a similar degree in the atmosphere is not ruled out, at least for the reactions involving n-nonanal and decanal. The major formation pathways for the observed HMW products may be the self-reactions of n-aldehydes mediated by atmospheric aerosol components and the reactions of n-aldehydes with organic aerosol components. The observed formation of HMW compounds encourages further investigations into their effects on the aerosol properties as well as the organic aerosol mass in the atmosphere.

Research on aerosol formation, aerosol behaviour, aerosol filtration, aerosol measurement techniques and sodium fires at the Laboratory for Aerosol Physics and Filter Technology at the Nuclear Research Center Karlsruhe

Energy Technology Data Exchange (ETDEWEB)

Jordan, S; Schikarski, W; Schoeck, W [Gesellschaft fuer Kernforschung mbH, Karlsruhe (Germany)

1977-01-01

The behaviour of aerosols in LMFBR plant systems is of great importance for a number of problems, both normal operational and accident kind. This paper covers the following: aerosol modelling for LMFBR containment systems; aerosol size spectrometry by laser light scattering; experimental facilities and experimental results concerned with aerosol release under accident conditions; filtration of sodium oxide aerosols by multilayer sand bed filters.

Research on aerosol formation, aerosol behaviour, aerosol filtration, aerosol measurement techniques and sodium fires at the Laboratory for Aerosol Physics and Filter Technology at the Nuclear Research Center Karlsruhe

International Nuclear Information System (INIS)

Jordan, S.; Schikarski, W.; Schoeck, W.

1977-01-01

The behaviour of aerosols in LMFBR plant systems is of great importance for a number of problems, both normal operational and accident kind. This paper covers the following: aerosol modelling for LMFBR containment systems; aerosol size spectrometry by laser light scattering; experimental facilities and experimental results concerned with aerosol release under accident conditions; filtration of sodium oxide aerosols by multilayer sand bed filters

Diurnal Cycles of Aerosol Optical Properties at Pico Tres Padres, Mexico City: Evidences for Changes in Particle Morphology and Secondary Aerosol Formation

Science.gov (United States)

Mazzoleni, C.; Dubey, M.; Chakrabarty, R.; Moosmuller, H.; Onasch, T.; Zavala, M.; Herndon, S.; Kolb, C.

2007-12-01

Aerosol optical properties affect planetary radiative balance and depend on chemical composition, size distribution, and morphology. During the MILAGRO field campaign, we measured aerosol absorption and scattering in Mexico City using the Los Alamos aerosol photoacoustic (LAPA) instrument operating at 781 nm. The LAPA was mounted on-board the Aerodyne Research Inc. mobile laboratory, which hosted a variety of gaseous and aerosol instruments. During the campaign, the laboratory was moved to different sites, capturing spatial and temporal variability. Additionally, we collected ambient aerosols on Nuclepore filters for scanning electron microscopy (SEM) analysis. SEM images of selected filters were taken to study particle morphology. Between March 7th and 19th air was sampled at the top of Pico Tres Padres, a mountain on the north side of Mexico City. Aerosol absorption and scattering followed diurnal patterns related to boundary layer height and solar insulation. We report an analysis of aerosol absorption, scattering, and morphology for three days (9th, 11th and 12th of March 2006). The single scattering albedo (SSA, ratio of scattering to total extinction) showed a drop in the tens-of-minutes-to-hour time frame after the boundary layer grew above the sampling site. Later in the day the SSA rose steadily reaching a maximum in the afternoon. The SEM images showed a variety of aerosol shapes including fractal-like aggregates, spherical particles, and other shapes. The absorption correlated with the CO2 signal and qualitatively with the fraction of fractal-like particles to the total particle count. In the afternoon the SSA qualitatively correlated with a relative increase in spherical particles and total particle count. These observed changes in optical properties and morphology can be explained by the dominant contribution of freshly emitted particles in the morning and by secondary particle formation in the afternoon. SSA hourly averaged values ranged from ~0.63 in

Laboratory Investigation of Aerosol Formation in Combustion of Biomass

International Nuclear Information System (INIS)

Zeuthen, Jacob; Livbjerg, Hans

2005-01-01

In this project the formation of aerosol particles and deposits in power plants during combustion of CO 2 -neutral fuels are investigated. For the experimental work a 173 cm long tubular furnace (diam=25 mm) with laminar flow is used. It is possible to control the temperature up to ∼ 1200 deg C in nine separate axial sections along the flue gas flow direction. In the first part of the reactor an inner tube is placed. In this inner tube a flow of inert nitrogen passes pellets of inert alumina impregnated with the salt to be volatilized (e.g. NaCl or KCl). The nitrogen gets saturated and by changing the temperature of the pellets it is possible to adjust the salt concentration in the gas. Other reactive gases (SO2, H2O, NO and O2/air) enter the reactor on the outside of the salt-containing alumina pipe. The temperature is kept constant in the first part of the reactor and is then decreased in the flow direction after a given length. The results obtained so far have shown that the homogeneous nucleation rate of pure salts depends on cooling rate, salt concentration and on the vapor pressure of the salt. Examples of results are shown at figure 1a. Here, two identical experiments are performed with two different salts. Since the vapor pressure of KCl is higher than for NaCl at the same temperature, a higher mass concentration of particles is obtained for this salt. Due to a lower salt concentration the number concentration of NaCl particles is higher, but the particles are smaller. The particles are analyzed with a number of instruments, including scanning mobility particle sizer, low pressure cascade impactor and transition electron microscopy. Experiments with introduction of nucleation seeds in the inlet gas have been performed, and it has been found that a suppression of homogeneous nucleation can be observed at rather low number concentrations of seeds. Homogeneous nucleation is favored by rapid cooling and the critical seed concentration for suppression of

Heterogeneous reactions and aerosol formation in flue gas cleaning by electron beam

International Nuclear Information System (INIS)

Baumann, W.; Jordan, S.; Leichsenring, C.H.; Maetzing, H.; Paur, H.R.; Schikarski, W.

1990-08-01

The electron beam dry scrubbing process is a simultaneous method for the removal of SO 2 and NO x from flue gas. By electron irradiation radicals (OH, O 2 H, O) are formed from the main flue gas components which oxidize NO x and SO 2 into the acids HNO 3 and H 2 SO 4 . These are then neutralized by the injection of NH 3 . A submicron aerosol consisting of ammonium salts is formed which is filtered from the offgas. The main pathways of the gas phase chemistry and product formation have been elucidated by experimental and theoretical studies. Back reactions which occur in the gas and the particle phase limit the energy efficiency of the process. By recirculation of irradiated gas into the reaction vessel (multiple irradiation) a significant improvement of removal yields was obtained. This enhancement of the energy efficiency requires the removal of products between the irradiation steps. Studies show that the material balance is complete. Deficits in the N and S balance of the process are due to the additional formation of molecular nitrogen and the deposition of ammonium sulfate in the ducts. Aerosol formation participates only with 30% in the material balance. The remaining 70% of the product are formed by surface reactions in the filter cake (40%) and in the ducts (30%). (orig.) With 38 figs., 29 tabs [de

Model analysis of secondary organic aerosol formation by glyoxal in laboratory studies: the case for photoenhanced chemistry.

Science.gov (United States)

Sumner, Andrew J; Woo, Joseph L; McNeill, V Faye

2014-10-21

The reactive uptake of glyoxal by atmospheric aerosols is believed to be a significant source of secondary organic aerosol (SOA). Several recent laboratory studies have been performed with the goal of characterizing this process, but questions remain regarding the effects of photochemistry on SOA growth. We applied GAMMA (McNeill et al. Environ. Sci. Technol. 2012, 46, 8075-8081), a photochemical box model with coupled gas-phase and detailed aqueous aerosol-phase chemistry, to simulate aerosol chamber studies of SOA formation by the uptake of glyoxal by wet aerosol under dark and irradiated conditions (Kroll et al. J. Geophys. Res. 2005, 110 (D23), 1-10; Volkamer et al. Atmos. Chem. Phys. 2009, 9, 1907-1928; Galloway et al. Atmos. Chem. Phys. 2009, 9, 3331- 306 3345 and Geophys. Res. Lett. 2011, 38, L17811). We find close agreement between simulated SOA growth and the results of experiments conducted under dark conditions using values of the effective Henry's Law constant of 1.3-5.5 × 10(7) M atm(-1). While irradiated conditions led to the production of some organic acids, organosulfates, and other oxidation products via well-established photochemical mechanisms, these additional product species contribute negligible aerosol mass compared to the dark uptake of glyoxal. Simulated results for irradiated experiments therefore fell short of the reported SOA mass yield by up to 92%. This suggests a significant light-dependent SOA formation mechanism that is not currently accounted for by known bulk photochemistry, consistent with recent laboratory observations of SOA production via photosensitizer chemistry.

On the Role of Ammonia in Arctic Aerosol Nucleation and Cloud Formation

Science.gov (United States)

Browse, J.; Dall'Osto, M.; Geels, C.; Skov, H.; Massling, A.; Boertmann, D.; Beddows, D.; Gordon, H.; Pringle, K.

2017-12-01

This study investigates the importance of ammonia in Arctic aerosol nucleation and the formation of cloud condensation nuclei (CCN) at high-latitudes. The importance of atmospheric nucleation processes to summertime Arctic aerosol concentration has been frequently noted at ground-stations, during campaigns and within models (which typically predict that the majority of aerosol in the Arctic summertime boundary layer derives from nucleation). However, as nucleation mechanisms in global models have increased in complexity (improving model skill globally) our skill in the Arctic has generally decreased. This decrease in model skill is likely due to a lack of organic compounds (monterpenes etc.) in the modelled high Arctic which have been identified as a key component in atmospheric nucleation in the mid-latitudes and thus incorporated into many global nucleation parametrisations. Recently it has been suggested that ammonia (also identified as a potentially important component in atmospheric nucleation) may control nucleation processes in the Arctic. However, the source (or sources) of Arctic ammonia remain unclear. Here, we use modelling, long-term aerosol in-situ observations, high resolution sea-ice satellite observations and new emission inventories to investigate the link between ammonia sources (including bird colonies, sea-ice melt and open ocean in the marginal ice zones) and nucleation events in the mid-to-high Arctic, and thus quantify the importance of individual ammonia sources to Arctic-wide CCN and cloud droplet populations.

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

Czech Academy of Sciences Publication Activity Database

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

2015-01-01

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

Aerosol formation of Sea-Urchin-like nanostructures of carbon nanotubes on bimetallic nanocomposite particles

International Nuclear Information System (INIS)

Kim, S. H.; Wang, C.; Zachariah, M. R.

2011-01-01

With the advantage of continuous production of pure carbon nanotubes (CNTs), a new simple aerosol process for the formation of CNTs was developed. A combination of conventional spray pyrolysis and thermal chemical vapor deposition enabled the formation unusual sea-urchin-like carbon nanostructures composed of multi-walled CNTs and metal composite nanoparticles. The CNTs formed were relatively untangled and uniform with a diameter of less than∼10 nm. The key to the formation of CNTs in this way was to create a substrate particle containing both a catalytic and non-catalytic component, which prevented coking. The density of the CNTs grown on the spherical metal nanoparticles could be controlled by perturbing the density of the metal catalysts (Fe) in the host non-catalytic metal particle matrix (Al). Mobility size measurement was identified as a useful technique to real-time characterization of either the catalytic formation of thin carbon layer or CNTs on the surface of the metal aerosol. These materials have shown unique properties in enhancing the thermal conductivity of fluids. Other potential advantages are that the as-produced material can be manipulated easily without the concern of high mobility of conventional nanowires, and then subsequently released at the desired time in an unagglomerated state.

Modeling of aerosol formation during biomass combustion in grate furnaces and comparison with measurements

NARCIS (Netherlands)

Joeller, M.; Brunner, T.; Obernberger, I.

2005-01-01

Results from mathematical modeling of aerosol formation during combustion of woody biomass fuels were compared with results from particle size distribution (PSD) measurements at a pilot-scale biomass combustion unit with moving grate and flame tube boiler. The mathematical model is a plug flow model

Measurements of organic gases during aerosol formation events in the boreal forest atmosphere during QUEST

Directory of Open Access Journals (Sweden)

K. Sellegri

2005-01-01

Full Text Available Biogenic VOCs are important in the growth and possibly also in the early stages of formation of atmospheric aerosol particles. In this work, we present 10 min-time resolution measurements of organic trace gases at Hyytiälä, Finland during March 2002. The measurements were part of the project QUEST (Quantification of Aerosol Nucleation in the European Boundary Layer and took place during a two-week period when nucleation events occurred with various intensities nearly every day. Using a ground-based Chemical Ionization Mass Spectrometer (CIMS instrument, the following trace gases were detected: acetone, TMA, DMA, mass 68amu (candidate=isoprene, monoterpenes, methyl vinyl ketone (MVK and methacrolein (MaCR and monoterpene oxidation products (MTOP. For all of them except for the amines, we present daily variations during different classes of nucleation events, and non-event days. BVOC oxidation products (MVK, MaCR and MTOP show a higher ratio to the CS on event days compared to non-event days, indicating that their abundance relative to the surface of aerosol available is higher on nucleation days. Moreover, BVOC oxidation products are found to show significant correlations with the condensational sink (CS on nucleation event days, which indicates that they are representative of less volatile organic compounds that contribute to the growth of the nucleated particles and generally secondary organic aerosol formation. Behaviors of BVOC on event and non event days are compared to the behavior of CO.

Formation of secondary organic aerosols from gas-phase emissions of heated cooking oils

Directory of Open Access Journals (Sweden)

T. Liu

2017-06-01

Full Text Available Cooking emissions can potentially contribute to secondary organic aerosol (SOA but remain poorly understood. In this study, formation of SOA from gas-phase emissions of five heated vegetable oils (i.e., corn, canola, sunflower, peanut and olive oils was investigated in a potential aerosol mass (PAM chamber. Experiments were conducted at 19–20 °C and 65–70 % relative humidity (RH. The characterization instruments included a scanning mobility particle sizer (SMPS and a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS. The efficiency of SOA production, in ascending order, was peanut oil, olive oil, canola oil, corn oil and sunflower oil. The major SOA precursors from heated cooking oils were related to the content of monounsaturated fat and omega-6 fatty acids in cooking oils. The average production rate of SOA, after aging at an OH exposure of 1. 7 × 1011 molecules cm−3 s, was 1. 35 ± 0. 30 µg min−1, 3 orders of magnitude lower compared with emission rates of fine particulate matter (PM2. 5 from heated cooking oils in previous studies. The mass spectra of cooking SOA highly resemble field-derived COA (cooking-related organic aerosol in ambient air, with R2 ranging from 0.74 to 0.88. The average carbon oxidation state (OSc of SOA was −1.51 to −0.81, falling in the range between ambient hydrocarbon-like organic aerosol (HOA and semi-volatile oxygenated organic aerosol (SV-OOA, indicating that SOA in these experiments was lightly oxidized.

Aerosol vertical distribution, new particle formation, and jet aircraft particle emissions in the free troposhere and tropopause region; Vertikalverteilung und Neubildungsprozesse des Aerosols und partikelfoermige Flugzeugemissionen in der freien Troposphaere und Tropopausenregion

Energy Technology Data Exchange (ETDEWEB)

Schroeder, F P

2000-07-01

A contribution to the understanding of natural and anthropogenously induced particle formation as well as aerosol physical transformation processes within the free troposphere (FT) is introduced. Documentation and interpretation of empirical data relevant with respect to possible climatologic impact of anthropogenous aerosol emissions into the atmosphere is presented. The first section describes new technique for high spatial resolution measurements of ultrafine aerosol particles by condensation nucleus counters (CNCs), a necessary prerequisite for the observation of natural particle formation and jet aircraft emissions. The second section illustrates vertical distribution and variability ranges of the aerosol in the FT and the tropopause region (TP). Typical microphysical states of the atmospheric aerosol within the Northern Hemisphere are documented by means of systematic measurements during more than 60 flight missions. Simple mathematical parameterizations of the aerosol vertical distribution and aerosol size distributions are developed. Important aerosol sources within the FT are localized and possible aerosol formation processes are discussed. The third section is focussed on jet-engine particle emissions within the FT and TP. A unique inflight experiment for detection of extremely high concentrations (>10{sup 6} cm{sup -3}) of extremely small (donw to <3 nm) aerosols inside the exhaust plumes of several jet aircraft is described. Particle emission indices and emission-controlling parameters are deduced. Most important topic is the impact of fuel sulfur content of kerosine on number, size and chemical composition of jet particle emissions. Generalized results are parameterized in form of lognormal aerosol particle size distributions. (orig.) [German] Ein Beitrag zum Verstaendnis natuerlicher und anthropogen induzierter Aerosolneubildung sowie physikalischer Aerosolumwandlung in der freien Troposphaere wird vorgestellt. Empirisch gewonnenes Datenmaterial wird

Characterization of Halyomorpha halys (brown marmorated stink bug) biogenic volatile organic compound emissions and their role in secondary organic aerosol formation.

Science.gov (United States)

Solomon, Danielle; Dutcher, Dabrina; Raymond, Timothy

2013-11-01

The formation of aerosols is a key component in understanding cloud formation in the context of radiative forcings and global climate modeling. Biogenic volatile organic compounds (BVOCs) are a significant source of aerosols, yet there is still much to be learned about their structures, sources, and interactions. The aims of this project were to identify the BVOCs found in the defense chemicals of the brown marmorated stink bug Halymorpha halys and quantify them using gas chromatography-mass spectrometry (GC/MS) and test whether oxidation of these compounds by ozone-promoted aerosol and cloud seed formation. The bugs were tested under two conditions: agitation by asphyxiation and direct glandular exposure. Tridecane, 2(5H)-furanone 5-ethyl, and (E)-2-decenal were identified as the three most abundant compounds. H. halys were also tested in the agitated condition in a smog chamber. It was found that in the presence of 100-180 ppm ozone, secondary aerosols do form. A scanning mobility particle sizer (SMPS) and a cloud condensation nuclei counter (CCNC) were used to characterize the secondary aerosols that formed. This reaction resulted in 0.23 microg/ bug of particulate mass. It was also found that these secondary organic aerosol particles could act as cloud condensation nuclei. At a supersaturation of 1%, we found a kappa value of 0.09. Once regional populations of these stink bugs stablilize and the populations estimates can be made, the additional impacts of their contribution to regional air quality can be calculated.

Secondary organic aerosol formation from road vehicle emissions

Science.gov (United States)

Pieber, Simone M.; Platt, Stephen M.; El Haddad, Imad; Zardini, Alessandro A.; Suarez-Bertoa, Ricardo; Slowik, Jay G.; Huang, Ru-Jin; Hellebust, Stig; Temime-Roussel, Brice; Marchand, Nicolas; Drinovec, Luca; Mocnik, Grisa; Baltensperger, Urs; Astorga, Covadogna; Prévôt, André S. H.

2014-05-01

Organic aerosol particles (OA) are a major fraction of the submicron particulate matter. OA consists of directly emitted primary (POA) and secondary OA (SOA). SOA is formed in-situ in the atmosphere via the reaction of volatile organic precursors. The partitioning of SOA species depends not only on the exposure to oxidants, but for instance also on temperature, relative humidity (RH), and the absorptive mass chemical composition (presence of inorganics) and concentration. Vehicle exhaust is a known source of POA and likely contributes to SOA formation in urban areas [1;2]. This has recently been estimated by (i) analyzing ambient data from urban areas combined with fuel consumption data [3], (ii) by examining the chemical composition of raw fuels [4], or (iii) smog chamber studies [5, 6]. Contradictory and thus somewhat controversial results in the relative quantity of SOA from diesel vs. gasoline vehicle exhaust were observed. In order to elucidate the impact of variable ambient conditions on the potential SOA formation of vehicle exhaust, and its relation to the emitted gas phase species, we studied SOA formed from the exhaust of passenger cars and trucks as a function of fuel and engine type (gasoline, diesel) at different temperatures (T 22 vs. -7oC) and RH (40 vs. 90%), as well as with different levels of inorganic salt concentrations. The exhaust was sampled at the tailpipe during regulatory driving cycles on chassis dynamometers, diluted (200 - 400x) and introduced into the PSI mobile smog chamber [6], where the emissions were subjected to simulated atmospheric ageing. Particle phase instruments (HR-ToF-AMS, aethalometers, CPC, SMPS) and gas phase instruments (PTR-TOF-MS, CO, CO2, CH4, THC, NH3 and other gases) were used online during the experiments. We found that gasoline emissions, because of cold starts, were generally larger than diesel, especially during cold temperatures driving cycles. Gasoline vehicles also showed the highest SOA formation

Communication: Quantitative Fourier-transform infrared data for competitive loading of small cages during all-vapor instantaneous formation of gas-hydrate aerosols

Science.gov (United States)

Uras-Aytemiz, Nevin; Abrrey Monreal, I.; Devlin, J. Paul

2011-10-01

A simple method has been developed for the measurement of high quality FTIR spectra of aerosols of gas-hydrate nanoparticles. The application of this method enables quantitative observation of gas hydrates that form on subsecond timescales using our all-vapor approach that includes an ether catalyst rather than high pressures to promote hydrate formation. The sampling method is versatile allowing routine studies at temperatures ranging from 120 to 210 K of either a single gas or the competitive uptake of different gas molecules in small cages of the hydrates. The present study emphasizes hydrate aerosols formed by pulsing vapor mixtures into a cold chamber held at 160 or 180 K. We emphasize aerosol spectra from 6 scans recorded an average of 8 s after "instantaneous" hydrate formation as well as of the gas hydrates as they evolve with time. Quantitative aerosol data are reported and analyzed for single small-cage guests and for mixed hydrates of CO2, CH4, C2H2, N2O, N2, and air. The approach, combined with the instant formation of gas hydrates from vapors only, offers promise with respect to optimization of methods for the formation and control of gas hydrates.

Hydration of the sulfuric acid-methylamine complex and implications for aerosol formation.

Science.gov (United States)

Bustos, Danielle J; Temelso, Berhane; Shields, George C

2014-09-04

The binary H2SO4-H2O nucleation is one of the most important pathways by which aerosols form in the atmosphere, and the presence of ternary species like amines increases aerosol formation rates. In this study, we focus on the hydration of a ternary system of sulfuric acid (H2SO4), methylamine (NH2CH3), and up to six waters to evaluate its implications for aerosol formation. By combining molecular dynamics (MD) sampling with high-level ab initio calculations, we determine the thermodynamics of forming H2SO4(NH2CH3)(H2O)n, where n = 0-6. Because it is a strong acid-base system, H2SO4-NH2CH3 quickly forms a tightly bound HSO4(-)-NH3CH3(+) complex that condenses water more readily than H2SO4 alone. The electronic binding energy of H2SO4-NH2CH3 is -21.8 kcal mol(-1) compared with -16.8 kcal mol(-1) for H2SO4-NH3 and -12.8 kcal mol(-1) for H2SO4-H2O. Adding one to two water molecules to the H2SO4-NH2CH3 complex is more favorable than adding to H2SO4 alone, yet there is no systematic difference for n ≥ 3. However, the average number of water molecules around H2SO4-NH2CH3 is consistently higher than that of H2SO4, and it is fairly independent of temperature and relative humidity.

Accessing the Impact of Sea-Salt Emissions on Aerosol Chemical Formation and Deposition Over Pearl River Delta, China

Science.gov (United States)

Fan, Q.; Wang, X.; Liu, Y.; Wu, D.; Chan, P. W.; Fan, S.; Feng, Y.

2015-12-01

Sea-salt aerosol (SSA) emissions have a significant impact on aerosol pollution and haze formation in the coastal areas. In this study, Models-3/CMAQ modeling system was utilized to access the impact of SSA emissions on aerosol chemical formation and deposition over Pearl River Delta (PRD), China in July 2006. More SSAs were transported inland from the open-ocean under the southeast wind in summertime. Two experiments (with and without SSA emissions in the CMAQ model) were set up to compare the modeling results with each other. The results showed that the increase of sulfate concentrations were more attributable to the primary emissions of coarse SO42- particles in SSA, while the increase of nitrate concentrations were more attributable to secondary chemical formations, known as the mechanisms of chloride depletion in SSA. In the coastal areas, 17.62 % of SO42-, 26.6% of NO3- and 38.2% of PM10 were attributed to SSA emissions, while those portions were less than 1% in the inland areas. The increases of PM10 and its components due to SSA emissions resulted in higher deposition fluxes over PRD, particularly in the coastal areas, except for the wet deposition of nitrate. Nitrate was more sensitive to SSA emissions in chemical formations than sulfate and dry deposition of aerosol was also more sensitive than that for wet deposition. Process analysis of sulfate and nitrate was applied to find out the difference of physical and chemical mechanisms between Guangzhou (the inland areas) and Zhuhai (the coastal areas). The negative contributions of dry deposition process to both sulfate and nitrate concentrations increased if SSA emissions were taken into account in the model, especially for Zhuhai. The negative contributions of cloud process also increased due to cloud scavenging and wet deposition process. In the coastal area, the gas-to-particle conversions became more active with high contributions of aerosol process to nitrate concentrations.

Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology

Science.gov (United States)

Stevens, R. G.; Pierce, J. R.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.

2012-01-01

New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM). The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

Chemical composition, source, and process of urban aerosols during winter haze formation in Northeast China.

Science.gov (United States)

Zhang, Jian; Liu, Lei; Wang, Yuanyuan; Ren, Yong; Wang, Xin; Shi, Zongbo; Zhang, Daizhou; Che, Huizheng; Zhao, Hujia; Liu, Yanfei; Niu, Hongya; Chen, Jianmin; Zhang, Xiaoye; Lingaswamy, A P; Wang, Zifa; Li, Weijun

2017-12-01

The characteristics of aerosol particles have been poorly evaluated even though haze episodes frequently occur in winter in Northeast China. OC/EC analysis, ion chromatography, and transmission electron microscopy (TEM) were used to investigate the organic carbon (OC) and elemental carbon (EC), and soluble ions in PM 2.5 and the mixing state of individual particles during a severe wintertime haze episode in Northeast China. The organic matter (OM), NH 4 + , SO 4 2- , and NO 3 - concentrations in PM 2.5 were 89.5 μg/m 3 , 24.2 μg/m 3 , 28.1 μg/m 3 , and 32.8 μg/m 3 on the haze days, respectively. TEM observations further showed that over 80% of the haze particles contained primary organic aerosols (POAs). Based on a comparison of the data obtained during the haze formation, we generate the following synthetic model of the process: (1) Stable synoptic meteorological conditions drove the haze formation. (2) The early stage of haze formation (light or moderate haze) was mainly caused by the enrichment of POAs from coal burning for household heating and cooking. (3) High levels of secondary organic aerosols (SOAs), sulfates, and nitrates formation via heterogeneous reactions together with POAs accumulation promoted to the evolution from light or moderate to severe haze. Compared to the severe haze episodes over the North China Plain, the PM 2.5 in Northeast China analyzed in the present study contained similar sulfate, higher SOA, and lower nitrate contents. Our results suggest that most of the POAs and secondary particles were likely related to emissions from coal-burning residential stoves in rural outskirts and small boilers in urban areas. The inefficient burning of coal for household heating and cooking should be monitored during wintertime in Northeast China. Copyright © 2017 Elsevier Ltd. All rights reserved.

Effect of Pellet Boiler Exhaust on Secondary Organic Aerosol Formation from α-Pinene.

Science.gov (United States)

Kari, Eetu; Hao, Liqing; Yli-Pirilä, Pasi; Leskinen, Ari; Kortelainen, Miika; Grigonyte, Julija; Worsnop, Douglas R; Jokiniemi, Jorma; Sippula, Olli; Faiola, Celia L; Virtanen, Annele

2017-02-07

Interactions between anthropogenic and biogenic emissions, and implications for aerosol production, have raised particular scientific interest. Despite active research in this area, real anthropogenic emission sources have not been exploited for anthropogenic-biogenic interaction studies until now. This work examines these interactions using α-pinene and pellet boiler emissions as a model test system. The impact of pellet boiler emissions on secondary organic aerosol (SOA) formation from α-pinene photo-oxidation was studied under atmospherically relevant conditions in an environmental chamber. The aim of this study was to identify which of the major pellet exhaust components (including high nitrogen oxide (NO x ), primary particles, or a combination of the two) affected SOA formation from α-pinene. Results demonstrated that high NO x concentrations emitted by the pellet boiler reduced SOA yields from α-pinene, whereas the chemical properties of the primary particles emitted by the pellet boiler had no effect on observed SOA yields. The maximum SOA yield of α-pinene in the presence of pellet boiler exhaust (under high-NO x conditions) was 18.7% and in the absence of pellet boiler exhaust (under low-NO x conditions) was 34.1%. The reduced SOA yield under high-NO x conditions was caused by changes in gas-phase chemistry that led to the formation of organonitrate compounds.

New 4.4 km-resolution aerosol product from NASA's Multi-angle Imaging SpectroRadiometer: A user's guide

Science.gov (United States)

Nastan, A.; Garay, M. J.; Witek, M. L.; Seidel, F.; Bull, M. A.; Kahn, R. A.; Diner, D. J.

2017-12-01

The NASA Multi-angle Imaging SpectroRadiometer (MISR) instrument on NASA's Terra satellite has provided an 18-year-and-growing aerosol data record. MISR's V22 aerosol product has been used extensively in studies of regional and global climate and the health effects of particulate air pollution. The MISR team recently released a new version of this product (V23), which increases the spatial resolution from 17.6 km to 4.4 km, improves performance versus AERONET, and provides better spatial coverage, more accurate cloud screening, and improved radiometric conditioning relative to V22. The product formatting was also completely revamped to improve clarity and usability. Established and prospective users of the MISR aerosol product are invited to learn about the features and performance of the new product and to participate in one-on-one demonstrations of how to obtain, visualize, and analyze the new product. Because the aerosol product is used in generating atmospherically-corrected surface bidirectional reflectance factors, improvements in MISR's 1.1 km resolution land surface product are a by-product of the updated aerosol retrievals. Illustrative comparisons of the V22 and V23 aerosol and surface products will be shown.

Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology

Directory of Open Access Journals (Sweden)

R. G. Stevens

2012-01-01

Full Text Available New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO₂ with condensation of H₂SO₄ onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM, a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM. The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H₂SO₄ condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NO_x since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation

Directory of Open Access Journals (Sweden)

E. Asmi

2010-05-01

Full Text Available The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.

Formation of secondary aerosols from the ozonolysis of styrene: Effect of SO2 and H2O

Science.gov (United States)

Díaz-de-Mera, Yolanda; Aranda, Alfonso; Martínez, Ernesto; Rodríguez, Ana Angustias; Rodríguez, Diana; Rodríguez, Ana

2017-12-01

In this work we report the study of the ozonolysis of styrene and the reaction conditions leading to the formation of secondary aerosols. The reactions have been carried out in a Teflon chamber filled with synthetic air mixtures at atmospheric pressure and room temperature. We have found that the ozonolysis of styrene in the presence of low concentrations of SO2 readily produces new particles under concentrations of reactants lower than those required in experiments in the absence of SO2. Thus, nucleation events occur at concentrations around (5.6 ± 1.7) × 108molecule cm-3 (errors are 2σ±20%) and SO2 is consumed during the experiments. The reaction of the Criegee intermediates with SO2 to produce SO3 and then H2SO4 may explain (together with OH reactions' contribution) the high capacity of styrene to produce particulate matter in polluted atmospheres. The formation of secondary aerosols in the smog chamber is inhibited under high H2O concentrations. So, the potential formation of secondary aerosols under atmospheric conditions depends on the concentration of SO2 and relative humidity, with a water to SO2 rate constants ratio kH2O/kSO2 = (2.8 ± 0.7) × 10-5 (errors are 2σ±20%).

Influence of intense secondary aerosol formation and long-range transport on aerosol chemistry and properties in the Seoul Metropolitan Area during spring time: results from KORUS-AQ

Science.gov (United States)

Kim, Hwajin; Zhang, Qi; Heo, Jongbae

2018-05-01

Non-refractory submicrometer particulate matter (NR-PM1) was measured in the Seoul Metropolitan Area (SMA), Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) from 14 April to 15 June 2016, as a part of the Korea-US Air Quality Study (KORUS-AQ) campaign. This was the first highly time-resolved, real-time measurement study of springtime aerosol in SMA and the results reveal valuable insights into the sources and atmospheric processes that contribute to PM pollution in this region. The average concentration of submicrometer aerosol (PM1 = NR-PM1 + black carbon (BC)) was 22.1 µg m-3, which was composed of 44 % organics, 20 % sulfate, 17 % nitrate, 12 % ammonium, and 7 % BC. Organics had an average atomic oxygen-to-carbon (O / C) ratio of 0.49 and an average organic mass-to-carbon (OM/OC) ratio of 1.82. Four 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 = 0.15; 17 % of OA mass), food cooking activities represented by a cooking-influenced OA factor (COA; O / C = 0.19; 22 % of OA mass), and secondary organic aerosol (SOA) represented by a semi-volatile oxygenated OA factor (SV-OOA; O / C = 0.44; 27 % of OA mass) and a low-volatility oxygenated OA factor (LV-OOA; O / C = 0.91; 34 % of OA mass). Our results indicate that air quality in SMA during KORUS-AQ was influenced strongly by secondary aerosol formation, with sulfate, nitrate, ammonium, SV-OOA, and LV-OOA together accounting for 76 % of the PM1 mass. In particular, the formation of LV-OOA and sulfate was mainly promoted by elevated ozone concentrations and photochemical reactions during daytime, whereas SV-OOA and nitrate formation was contributed by both nocturnal processing of VOC and nitrogen oxides, respectively, and daytime photochemical reactions. In addition, lower nighttime temperature promoted gas-to-particle partitioning of

Anthropogenic Influence on Secondary Aerosol Formation and Total Water-Soluble Carbon on Atmospheric Particles

Science.gov (United States)

Gioda, Adriana; Mateus, Vinicius; Monteiro, Isabela; Taira, Fabio; Esteves, Veronica; Saint'Pierre, Tatiana

2013-04-01

On a global scale, the atmosphere is an important source of nutrients, as well as pollutants, because of its interfaces with soil and water. Important compounds in the gaseous phase are in both organic and inorganic forms, such as organic acids, nitrogen, sulfur and chloride. In spite of the species in gas form, a huge number of process, anthropogenic and natural, are able to form aerosols, which may be transported over long distances. Sulfates e nitrates are responsible for rain acidity; they may also increase the solubility of organic compounds and metals making them more bioavailable, and also can act as cloud condensation nuclei (CCN). Aerosol samples (PM2.5) were collected in a rural and industrial area in Rio de Janeiro, Brazil, in order to quantify chemical species and evaluate anthropogenic influences in secondary aerosol formation and organic compounds. Samples were collected during 24 h every six days using a high-volume sampler from August 2010 to July 2011. The aerosol mass was determined by Gravimetry. The water-soluble ionic composition (WSIC) was obtained by Ion Chromatography in order to determine the major anions (NO3-, SO4= and Cl-); total water-soluble carbon (TWSC) was determined by a TOC analyzer. The average aerosol (PM2.5) concentrations ranged from 1 to 43 ug/m3 in the industrial site and from 4 to 35 ug/m3 in the rural area. Regarding anions, the highest concentrations were measured for SO42- (10.6 μg/m3-12.6 μg/m3); where the lowest value was found in the rural site and the highest in the industrial. The concentrations for NO3- and Cl- ranged from 4.2 μg/m3 to 9.3 μg/m3 and 3.1 μg/m3 to 6.4 μg /m3, respectively. Sulfate was the major species and, like nitrate, it is related to photooxidation in the atmosphere. Interestingly sulfate concentrations were higher during the dry period and could be related to photochemistry activity. The correlations between nitrate and non-sea-salt sulfate were weak, suggesting different sources for these

Assessing the impact of anthropogenic pollution on isoprene-derived secondary organic aerosol formation in PM2.5 collected from the Birmingham, Alabama, ground site during the 2013 Southern Oxidant and Aerosol Study

Directory of Open Access Journals (Sweden)

W. Rattanavaraha

2016-04-01

Full Text Available In the southeastern US, substantial emissions of isoprene from deciduous trees undergo atmospheric oxidation to form secondary organic aerosol (SOA that contributes to fine particulate matter (PM2.5. Laboratory studies have revealed that anthropogenic pollutants, such as sulfur dioxide (SO2, oxides of nitrogen (NOx, and aerosol acidity, can enhance SOA formation from the hydroxyl radical (OH-initiated oxidation of isoprene; however, the mechanisms by which specific pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected at the Birmingham, Alabama (BHM, ground site during the 2013 Southern Oxidant and Aerosol Study (SOAS. Sample extracts were analyzed by gas chromatography–electron ionization-mass spectrometry (GC/EI-MS with prior trimethylsilylation and ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS to identify known isoprene SOA tracers. Tracers quantified using both surrogate and authentic standards were compared with collocated gas- and particle-phase data as well as meteorological data provided by the Southeastern Aerosol Research and Characterization (SEARCH network to assess the impact of anthropogenic pollution on isoprene-derived SOA formation. Results of this study reveal that isoprene-derived SOA tracers contribute a substantial mass fraction of organic matter (OM ( ∼  7 to  ∼  20 %. Isoprene-derived SOA tracers correlated with sulfate (SO42− (r2 = 0.34, n = 117 but not with NOx. Moderate correlations between methacrylic acid epoxide and hydroxymethyl-methyl-α-lactone (together abbreviated MAE/HMML-derived SOA tracers with nitrate radical production (P[NO3] (r2 = 0.57, n = 40 were observed during nighttime, suggesting a

Organic aerosol formation in citronella candle plumes

OpenAIRE

Bothe, Melanie; Donahue, Neil McPherson

2010-01-01

Citronella candles are widely used as insect repellants, especially outdoors in the evening. Because these essential oils are unsaturated, they have a unique potential to form secondary organic aerosol (SOA) via reaction with ozone, which is also commonly elevated on summer evenings when the candles are often in use. We investigated this process, along with primary aerosol emissions, by briefly placing a citronella tealight candle in a smog chamber and then adding ozone to the chamber. In rep...

Effects of Large Polycyclic Aromatic Hydrocarbons on the Soot Formation in Ethylene-Air Nonpremixed Flames

KAUST Repository

Prabhu, S.; Arias, P.G.; Wang, Y.; Gao, Y.; Park, S.; Im, Hong G.; Sarathy, Mani; Chung, Suk-Ho; Lu, T.

2015-01-01

This study presents updated comprehensive gas-phase kinetic mechanism and aerosol models to predict soot formation characteristics in ethylene-air nonpremixed flames. A main objective is to investigate the sensitivity of the soot formation rate to various chemical pathways for large polycyclic aromatic hydrocarbons (PAH). In this study, the detailed chemical mechanism was reduced from 397 to 99 species using directed relation graph (DRG) and sensitivity analysis. The method of moments with interpolative closure (MOMIC) was employed for the soot aerosol model. Counterflow nonpremixed flames of pure ethylene at low strain rate sooting conditions are considered, for which the sensitivity of soot formation characteristics with respect to hetrogeneous nucleation is investigated. Results show that higher PAH concentrations result in higher soot nucleation rate, and that the average size of the particles are in good agreement with experimental results. It is found that the nucleation processes (i.e., soot inception) from higher PAH precursors, coronene in particular, is critical for accurate prediction of the overall soot formation.

Effects of Large Polycyclic Aromatic Hydrocarbons on the Soot Formation in Ethylene-Air Nonpremixed Flames

KAUST Repository

Prabhu, S.

2015-03-30

This study presents updated comprehensive gas-phase kinetic mechanism and aerosol models to predict soot formation characteristics in ethylene-air nonpremixed flames. A main objective is to investigate the sensitivity of the soot formation rate to various chemical pathways for large polycyclic aromatic hydrocarbons (PAH). In this study, the detailed chemical mechanism was reduced from 397 to 99 species using directed relation graph (DRG) and sensitivity analysis. The method of moments with interpolative closure (MOMIC) was employed for the soot aerosol model. Counterflow nonpremixed flames of pure ethylene at low strain rate sooting conditions are considered, for which the sensitivity of soot formation characteristics with respect to hetrogeneous nucleation is investigated. Results show that higher PAH concentrations result in higher soot nucleation rate, and that the average size of the particles are in good agreement with experimental results. It is found that the nucleation processes (i.e., soot inception) from higher PAH precursors, coronene in particular, is critical for accurate prediction of the overall soot formation.

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

Science.gov (United States)

Palm, Brett B.; de Sá, Suzane S.; Day, Douglas A.; Campuzano-Jost, Pedro; Hu, Weiwei; Seco, Roger; Sjostedt, Steven J.; Park, Jeong-Hoo; Guenther, Alex B.; Kim, Saewung; Brito, Joel; Wurm, Florian; Artaxo, Paulo; Thalman, Ryan; Wang, Jian; Yee, Lindsay D.; Wernis, Rebecca; Isaacman-VanWertz, Gabriel; Goldstein, Allen H.; Liu, Yingjun; Springston, Stephen R.; Souza, Rodrigo; Newburn, Matt K.; Lizabeth Alexander, M.; Martin, Scot T.; Jimenez, Jose L.

2018-01-01

Secondary organic aerosol (SOA) formation from ambient air was studied using an oxidation flow reactor (OFR) coupled to an aerosol mass spectrometer (AMS) during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O3, over ranges from hours to days (O3) or weeks (OH) of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to as much as 10 µg m-3, depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air and were confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA) after OH oxidation showed formation of typical oxidized OA factors and a loss of primary OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased with increasing elemental O : C up to O : C ˜ 1.0, and then decreased as O : C increased further. Possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. While measured ambient precursors were sufficient to explain the amount of SOA formed from O3, they could only explain 10-50 % of the SOA formed from OH. This is consistent with previous OFR studies, which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C = C bonds) are present in ambient air and can explain such additional SOA formation. To investigate the sources of the unmeasured SOA-forming gases during this campaign

New aerosol particles formation in the Sao Paulo Metropolitan Area

Science.gov (United States)

Vela, Angel; Andrade, Maria de Fatima; Ynoue, Rita

2016-04-01

performance. For secondary aerosols, a simulation scenario (Case_1) with only emission of primary gases (biogenic and anthropogenic) is performed to evaluate its formation potential. The study period from 7th August to 6th September 2012 has been selected due to the avaliability of experimental data from the Narrowing the Uncertainties on Aerosol and Climate Changes in Sao Paulo State (NUANCE) project. Aerosol measurements consist basically on PM2.5 and PM10 concentration. OC, EC, ion, and aerosol mass size distribution measurements were also carried out in one of the measurement sites (IAG-USP). Results show that overall the emissions of primary gases coming mainly from vehicles have a potential to form new particles between 20 and 30% in relation to the baseline PM2.5 mass concentration found in the downtown SPMA. In addition, both the observed and predicted OC and EC at the IAG-USP measurement site make up the largest fraction of PM2.5 mass with contributions around 55 and 40%, respectively.

Code Development on Fission Product Behavior under Severe Accident-Validation of Aerosol Sedimentation

International Nuclear Information System (INIS)

Ha, Kwang Soon; Kim, Sung Il; Jang, Jin Sung; Kim, Dong Ha

2016-01-01

The gas and aerosol phases of the radioactive materials move through the reactor coolant systems and containments as loaded on the carrier gas or liquid, such as steam or water. Most radioactive materials might escape in the form of aerosols from a nuclear power plant during a severe reactor accident, and it is very important to predict the behavior of these radioactive aerosols in the reactor cooling system and in the containment building under severe accident conditions. Aerosols are designated as very small solid particles or liquid droplets suspended in a gas phase. The suspended solid or liquid particles typically have a range of sizes of 0.01 m to 20 m. Aerosol concentrations in reactor accident analyses are typically less than 100 g/m3 and usually less than 1 g/m3. When there are continuing sources of aerosol to the gas phase or when there are complicated processes involving engineered safety features, much more complicated size distributions develop. It is not uncommon for aerosols in reactor containments to have bimodal size distributions for at least some significant periods of time early during an accident. Salient features of aerosol physics under reactor accident conditions that will affect the nature of the aerosols are (1) the formation of aerosol particles, (2) growth of aerosol particles, (3) shape of aerosol particles. At KAERI, a fission product module has been developed to predict the behaviors of the radioactive materials in the reactor coolant system under severe accident conditions. The fission product module consists of an estimation of the initial inventories, species release from the core, aerosol generation, gas transport, and aerosol transport. The final outcomes of the fission product module designate the radioactive gas and aerosol distribution in the reactor coolant system. The aerosol sedimentation models in the fission product module were validated using ABCOVE and LACE experiments. There were some discrepancies on the predicted

Code Development on Fission Product Behavior under Severe Accident-Validation of Aerosol Sedimentation

Energy Technology Data Exchange (ETDEWEB)

Ha, Kwang Soon; Kim, Sung Il; Jang, Jin Sung; Kim, Dong Ha [KAERI, Daejeon (Korea, Republic of)

2016-05-15

The gas and aerosol phases of the radioactive materials move through the reactor coolant systems and containments as loaded on the carrier gas or liquid, such as steam or water. Most radioactive materials might escape in the form of aerosols from a nuclear power plant during a severe reactor accident, and it is very important to predict the behavior of these radioactive aerosols in the reactor cooling system and in the containment building under severe accident conditions. Aerosols are designated as very small solid particles or liquid droplets suspended in a gas phase. The suspended solid or liquid particles typically have a range of sizes of 0.01 m to 20 m. Aerosol concentrations in reactor accident analyses are typically less than 100 g/m3 and usually less than 1 g/m3. When there are continuing sources of aerosol to the gas phase or when there are complicated processes involving engineered safety features, much more complicated size distributions develop. It is not uncommon for aerosols in reactor containments to have bimodal size distributions for at least some significant periods of time early during an accident. Salient features of aerosol physics under reactor accident conditions that will affect the nature of the aerosols are (1) the formation of aerosol particles, (2) growth of aerosol particles, (3) shape of aerosol particles. At KAERI, a fission product module has been developed to predict the behaviors of the radioactive materials in the reactor coolant system under severe accident conditions. The fission product module consists of an estimation of the initial inventories, species release from the core, aerosol generation, gas transport, and aerosol transport. The final outcomes of the fission product module designate the radioactive gas and aerosol distribution in the reactor coolant system. The aerosol sedimentation models in the fission product module were validated using ABCOVE and LACE experiments. There were some discrepancies on the predicted

Volcanic Plume Impact on the Atmosphere and Climate: O- and S-Isotope Insight into Sulfate Aerosol Formation

Directory of Open Access Journals (Sweden)

Erwan Martin

2018-05-01

Full Text Available The impact of volcanic eruptions on the climate has been studied over the last decades and the role played by sulfate aerosols appears to be major. S-bearing volcanic gases are oxidized in the atmosphere into sulfate aerosols that disturb the radiative balance on earth at regional to global scales. This paper discusses the use of the oxygen and sulfur multi-isotope systematics on volcanic sulfates to understand their formation and fate in more or less diluted volcanic plumes. The study of volcanic aerosols collected from air sampling and ash deposits at different distances from the volcanic systems (from volcanic vents to the Earth poles is discussed. It appears possible to distinguish between the different S-bearing oxidation pathways to generate volcanic sulfate aerosols whether the oxidation occurs in magmatic, tropospheric, or stratospheric conditions. This multi-isotopic approach represents an additional constraint on atmospheric and climatic models and it shows how sulfates from volcanic deposits could represent a large and under-exploited archive that, over time, have recorded atmospheric conditions on human to geological timescales.

Lithium vapor/aerosol studies. Interim summary report

International Nuclear Information System (INIS)

Whitlow, G.A.; Bauerle, J.E.; Down, M.G.; Wilson, W.L.

1979-04-01

The temperature/cover gas pressure regime, in which detectable lithium aerosol is formed in a static system has been mapped for argon and helium cover gases using a portable He--Ne laser device. At 538 0 C (1000 0 F), lithium aerosol particles were observed over the range 0.5 to 20 torr and 2 to 10 torr for argon and helium respectively. The experimental conditions in this study were more conducive to aerosol formation than in a fusion reactor. In the real reactor system, very high intensity mechanical and thermal disturbances will be made to the liquid lithium. These disturbances, particularly transient increases in lithium vapor pressure appear to be capable of producing high concentrations of optically-dense aerosol. A more detailed study is, therefore, proposed using the basic information generated in these preliminary experiments, as a starting point. Areas recommended include the kinetics of aerosol formation and the occurrence of supersaturated vapor during rapid vapor pressure transients, and also the effect of lithium agitation (falls, jets, splashing, etc.) on aerosol formation

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

Directory of Open Access Journals (Sweden)

M. E. Jenkin

2004-01-01

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

Impacts of controlling biomass burning emissions on wintertime carbonaceous aerosol in Europe

NARCIS (Netherlands)

Fountoukis, C.; Butler, T.; Lawrence, M.G.; Denier van der Gon, H.A.C.; Visschedijk, A.J.H.; Charalampidis, P.; Pilinis, C.; Pandis, S.N.

2014-01-01

We use a 3-D regional chemical transport model, with the latest advancements in the organic aerosol (OA) treatment, and an updated emission inventory for wood combustion to study the organic aerosol change in response to the replacement of current residential wood combustion technologies with pellet

Characterization of new particle and secondary aerosol formation during summertime in Beijing, China

Energy Technology Data Exchange (ETDEWEB)

Zhang, Y. M. (Key Laboratory for Atmospheric Chemistry, Centre for Atmosphere Watch and Services, Chinese Academy of Meteorological Sciences, China Meteorological Administration, Beijing (China); Graduate Univ. of Chinese Academy of Sciences, Beijing (China)); Zhang, X. Y.; Sun, J. Y.; Lin, W. L.; Shen, X. J. (Key Laboratory for Atmospheric Chemistry, Centre for Atmosphere Watch and Services, Chinese Academy of Meteorological Sciences, China Meteorological Administration, Beijing (China)), e-mail: xiaoye@cams.cma.gov.cn; Gong, S. L. (Air Quality Research Div., Science and Technology Branch, Environment Canada, Toronto (Canada)); Yang, S. (State Key Laboratory of Numerical Modeling for Atmospheric Sciences and Geophysical Fluid Dynamics, Inst. of Atmospheric Physics, CAS, Beijing (China))

2011-07-15

Size-resolved aerosol number and mass concentrations and the mixing ratios of O{sub 3} and various trace gases were continuously measured at an urban station before and during the Beijing Olympic and Paralympic Games (5 June to 22 September, 2008). 23 new particle formation (NPF) events were identified; these usually were associated with changes in wind direction and/or rising concentrations of gas-phase precursors or after precipitation events. Most of the NPF events started in the morning and continued to noon as particles in the nucleation mode grew into the Aitken mode. From noon to midnight, the aerosols grew into the accumulation mode through condensation and coagulation. Ozone showed a gradual rise starting around 10:00 local time, reached its peak around 15:00 and then declined as the organics increased. The dominant new particle species were organics (40-75% of PM{sub 1}) and sulphate; nitrate and ammonium were more minor contributors

Characterization of new particle and secondary aerosol formation during summertime in Beijing, China

Science.gov (United States)

Zhang, Y. M.; Zhang, X. Y.; Sun, J. Y.; Lin, W. L.; Gong, S. L.; Shen, X. J.; Yang, S.

2011-07-01

Size-resolved aerosol number and mass concentrations and the mixing ratios of O3 and various trace gases were continuously measured at an urban station before and during the Beijing Olympic and Paralympic Games (5 June to 22 September, 2008). 23 new particle formation (NPF) events were identified; these usually were associated with changes in wind direction and/or rising concentrations of gas-phase precursors or after precipitation events. Most of the NPF events started in the morning and continued to noon as particles in the nucleation mode grew into the Aitken mode. From noon to midnight, the aerosols grew into the accumulation mode through condensation and coagulation. Ozone showed a gradual rise starting around 10:00 local time, reached its peak around 15:00 and then declined as the organics increased. The dominant new particle species were organics (40-75% of PM1) and sulphate; nitrate and ammonium were more minor contributors.

Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic

Science.gov (United States)

Marelle, Louis; Raut, Jean-Christophe; Law, Kathy S.; Berg, Larry K.; Fast, Jerome D.; Easter, Richard C.; Shrivastava, Manish; Thomas, Jennie L.

2017-10-01

In this study, the WRF-Chem regional model is updated to improve simulated short-lived pollutants (e.g., aerosols, ozone) in the Arctic. Specifically, we include in WRF-Chem 3.5.1 (with SAPRC-99 gas-phase chemistry and MOSAIC aerosols) (1) a correction to the sedimentation of aerosols, (2) dimethyl sulfide (DMS) oceanic emissions and gas-phase chemistry, (3) an improved representation of the dry deposition of trace gases over seasonal snow, and (4) an UV-albedo dependence on snow and ice cover for photolysis calculations. We also (5) correct the representation of surface temperatures over melting ice in the Noah Land Surface Model and (6) couple and further test the recent KF-CuP (Kain-Fritsch + Cumulus Potential) cumulus parameterization that includes the effect of cumulus clouds on aerosols and trace gases. The updated model is used to perform quasi-hemispheric simulations of aerosols and ozone, which are evaluated against surface measurements of black carbon (BC), sulfate, and ozone as well as airborne measurements of BC in the Arctic. The updated model shows significant improvements in terms of seasonal aerosol cycles at the surface and root mean square errors (RMSEs) for surface ozone, aerosols, and BC aloft, compared to the base version of the model and to previous large-scale evaluations of WRF-Chem in the Arctic. These improvements are mostly due to the inclusion of cumulus effects on aerosols and trace gases in KF-CuP (improved RMSE for surface BC and BC profiles, surface sulfate, and surface ozone), the improved surface temperatures over sea ice (surface ozone, BC, and sulfate), and the updated trace gas deposition and UV albedo over snow and ice (improved RMSE and correlation for surface ozone). DMS emissions and chemistry improve surface sulfate at all Arctic sites except Zeppelin, and correcting aerosol sedimentation has little influence on aerosols except in the upper troposphere.

Primary emissions and secondary organic aerosol formation from the exhaust of a flex-fuel (ethanol) vehicle

Science.gov (United States)

Suarez-Bertoa, R.; Zardini, A. A.; Platt, S. M.; Hellebust, S.; Pieber, S. M.; El Haddad, I.; Temime-Roussel, B.; Baltensperger, U.; Marchand, N.; Prévôt, A. S. H.; Astorga, C.

2015-09-01

Incentives to use biofuels may result in increasing vehicular emissions of compounds detrimental to air quality. Therefore, regulated and unregulated emissions from a Euro 5a flex-fuel vehicle, tested using E85 and E75 blends (gasoline containing 85% and 75% of ethanol (vol/vol), respectively), were investigated at 22 and -7 °C over the New European Driving Cycle, at the Vehicle Emission Laboratory at the European Commission Joint Research Centre Ispra, Italy. Vehicle exhaust was comprehensively analyzed at the tailpipe and in a dilution tunnel. A fraction of the exhaust was injected into a mobile smog chamber to study the photochemical aging of the mixture. We found that emissions from a flex-fuel vehicle, fueled by E85 and E75, led to secondary organic aerosol (SOA) formation, despite the low aromatic content of these fuel blends. Emissions of regulated and unregulated compounds, as well as emissions of black carbon (BC) and primary organic aerosol (POA) and SOA formation were higher at -7 °C. The flex-fuel unregulated emissions, mainly composed of ethanol and acetaldehyde, resulted in very high ozone formation potential and SOA, especially at low temperature (860 mg O3 km-1 and up to 38 mg C kg-1). After an OH exposure of 10 × 106 cm-3 h, SOA mass was, on average, 3 times larger than total primary particle mass emissions (BC + POA) with a high O:C ratio (up to 0.7 and 0.5 at 22 and -7 °C, respectively) typical of highly oxidized mixtures. Furthermore, high resolution organic mass spectra showed high 44/43 ratios (ratio of the ions m/z 44 and m/z 43) characteristic of low-volatility oxygenated organic aerosol. We also hypothesize that SOA formation from vehicular emissions could be due to oxidation products of ethanol and acetaldehyde, both short-chain oxygenated VOCs, e.g. methylglyoxal and acetic acid, and not only from aromatic compounds.

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.

American Association for Aerosol Research (AAAR) `95

Energy Technology Data Exchange (ETDEWEB)

NONE

1995-12-31

The Fourteenth annual meeting of the American Association for Aerosol Research was held October 9-13, 1995 at Westin William Penn Hotel in Pittsburgh, PA. This volume contains the abstracts of the papers and poster sessions presented at this meeting, grouped by the session in which they were presented as follows: Radiation Effects; Aerosol Deposition; Collision Simulations and Microphysical Behavior; Filtration Theory and Measurements; Materials Synthesis; Radioactive and Nuclear Aerosols; Aerosol Formation, Thermodynamic Properties, and Behavior; Particle Contamination Issues in the Computer Industry; Pharmaceutical Aerosol Technology; Modeling Global/Regional Aerosols; Visibility; Respiratory Deposition; Biomass and Biogenic Aerosols; Aerosol Dynamics; Atmospheric Aerosols.

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.

The Effect of Aerosol Hygroscopicity and Volatility on Aerosol Optical Properties During Southern Oxidant and Aerosol Study

Science.gov (United States)

Khlystov, A.; Grieshop, A. P.; Saha, P.; Subramanian, R.

2014-12-01

Secondary organic aerosol (SOA) from biogenic sources can influence optical properties of ambient aerosol by altering its hygroscopicity and contributing to light absorption directly via formation of brown carbon and indirectly by enhancing light absorption by black carbon ("lensing effect"). The magnitude of these effects remains highly uncertain. A set of state-of-the-art instruments was deployed at the SEARCH site near Centerville, AL during the Southern Oxidant and Aerosol Study (SOAS) campaign in summer 2013 to measure the effect of relative humidity and temperature on aerosol size distribution, composition and optical properties. Light scattering and absorption by temperature- and humidity-conditioned aerosols was measured using three photo-acoustic extinctiometers (PAX) at three wavelengths (405 nm, 532 nm, and 870 nm). The sample-conditioning system provided measurements at ambient RH, 10%RH ("dry"), 85%RH ("wet"), and 200 C ("TD"). In parallel to these measurements, a long residence time temperature-stepping thermodenuder (TD) and a variable residence time constant temperature TD in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. We will present results of the on-going analysis of the collected data set. We will show that both temperature and relative humidity have a strong effect on aerosol optical properties. SOA appears to increase aerosol light absorption by about 10%. TD measurements suggest that aerosol equilibrated fairly quickly, within 2 s. Evaporation varied substantially with ambient aerosol loading and composition and meteorology.

Aqueous-Phase Reactions of Isoprene with Sulfoxy Radical Anions as a way of Wet Aerosol Formation in the Atmosphere

Science.gov (United States)

Kuznietsova, I.; Rudzinski, K. J.; Szmigielski, R.; Laboratory of the Environmental Chemistry

2011-12-01

Atmospheric aerosols exhibit an important role in the environment. They have implications on human health and life, and - in the larger scale - on climate, the Earth's radiative balance and the cloud's formation. Organic matter makes up a significant fraction of atmospheric aerosols (~35% to ~90%) and may originate from direct emissions (primary organic aerosol, POA) or result from complex physico-chemical processes of volatile organic compounds (secondary organic aerosol, SOA). Isoprene (2-methyl-buta-1,3-diene) is one of the relevant volatile precursor of ambient SOA in the atmosphere. It is the most abundant non-methane hydrocarbon emitted to the atmosphere as a result of living vegetation. According to the recent data, the isoprene emission rate is estimated to be at the level of 500 TgC per year. While heterogeneous transformations of isoprene have been well documented, aqueous-phase reactions of this hydrocarbon with radical species that lead to the production of new class of wet SOA components such as polyols and their sulfate esters (organosulfates), are still poorly recognized. The chain reactions of isoprene with sulfoxy radical-anions (SRA) are one of the recently researched route leading to the formation of organosulfates in the aqueous phase. The letter radical species originate from the auto-oxidation of sulfur dioxide in the aqueous phase and are behind the phenomenon of atmospheric acid rain formation. This is a complicated chain reaction that is catalyzed by transition metal ions, such as manganese(II), iron(III) and propagated by sulfoxy radical anions . The presented work addresses the chemical interaction of isoprene with sulfoxy radical-anions in the water solution in the presence of nitrite ions and nitrous acid, which are important trace components of the atmosphere. We showed that nitrite ions and nitrous acid significantly altered the kinetics of the auto-oxidation of SO2 in the presence of isoprene at different solution acidity from 2 to 8

Secondary organic aerosol (trans)formation through aqueous phase guaiacol photonitration: a kinetic study

Science.gov (United States)

Kroflič, Ana; Grgić, Irena

2014-05-01

It is well known that atmospheric aerosols play a crucial role in the Earth's climate and public health (Pöschl 2005). Despite a great effort invested in the studies of secondary organic aerosol (SOA) budget, composition, and its formation mechanisms, there is still a gap between field observations and atmospheric model predictions (Heald et al. 2005, Hallquist et al. 2009, and Lim et al. 2010). The insisting uncertainties surrounding SOA formation and aging thus gained an increasing interest in atmospheric aqueous phase chemistry; they call for more complex and time consuming studies at the environmentally relevant conditions allowing confident extrapolation to desired ambient conditions. In addition to the adverse health effects of atmospheric particulate matter (PM) as such, toxicity is also attributed to nitro-aromatic and other organic compounds which have already been detected in real aerosol samples (Traversi et al. 2009). Moreover, low-volatility aromatic derivatives are believed to form at least partly in the aerosol aqueous phase and not only in the gas phase from where they partition into water droplets (Ervens et al. 2011). Two nitro derivatives of biomass burning tracer guaiacol have recently been found in winter PM10 samples from the city of Ljubljana, Slovenia, and aqueous photonitration reaction was proposed as their possible production pathway (Kitanovski et al. 2012). In this study the kinetics of guaiacol nitration in aqueous solution was investigated in the presence of H2O2 and NO2¯ upon simulated solar irradiation (Xenon lamp, 300 W). During the experiment the DURAN® flask with the reaction mixture was held in the thermostated bath and thoroughly mixed. The reaction was monitored for 44 hours at different temperatures. Guaiacol and its main nitro-products (4-nitroguaiacol, 4-NG; 6-nitroguaiacol, 6-NG; and 4,6-dinitroguaiacol, 4,6-DNG) were quantified in every aliquot, taken from the reaction mixture, by use of high pressure liquid

Secondary organic aerosol formation from ambient air in an oxidation flow reactor in central Amazonia

Directory of Open Access Journals (Sweden)

B. B. Palm

2018-01-01

Full Text Available Secondary organic aerosol (SOA formation from ambient air was studied using an oxidation flow reactor (OFR coupled to an aerosol mass spectrometer (AMS during both the wet and dry seasons at the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5 field campaign. Measurements were made at two sites downwind of the city of Manaus, Brazil. Ambient air was oxidized in the OFR using variable concentrations of either OH or O3, over ranges from hours to days (O3 or weeks (OH of equivalent atmospheric aging. The amount of SOA formed in the OFR ranged from 0 to as much as 10 µg m−3, depending on the amount of SOA precursor gases in ambient air. Typically, more SOA was formed during nighttime than daytime, and more from OH than from O3 oxidation. SOA yields of individual organic precursors under OFR conditions were measured by standard addition into ambient air and were confirmed to be consistent with published environmental chamber-derived SOA yields. Positive matrix factorization of organic aerosol (OA after OH oxidation showed formation of typical oxidized OA factors and a loss of primary OA factors as OH aging increased. After OH oxidation in the OFR, the hygroscopicity of the OA increased with increasing elemental O : C up to O : C ∼ 1.0, and then decreased as O : C increased further. Possible reasons for this decrease are discussed. The measured SOA formation was compared to the amount predicted from the concentrations of measured ambient SOA precursors and their SOA yields. While measured ambient precursors were sufficient to explain the amount of SOA formed from O3, they could only explain 10–50 % of the SOA formed from OH. This is consistent with previous OFR studies, which showed that typically unmeasured semivolatile and intermediate volatility gases (that tend to lack C = C bonds are present in ambient air and can explain such additional SOA formation. To investigate the sources of the

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.

Combustion aerosols from potassium-containing fuels

Energy Technology Data Exchange (ETDEWEB)

Balzer Nielsen, Lars

1999-12-31

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

Combustion aerosols from potassium-containing fuels

International Nuclear Information System (INIS)

Balzer Nielsen, Lars

1998-01-01

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

Combustion aerosols from potassium-containing fuels

Energy Technology Data Exchange (ETDEWEB)

Balzer Nielsen, Lars

1998-12-31

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

Natural and Anthropogenic Influences on Atmospheric Aerosol Variability

Energy Technology Data Exchange (ETDEWEB)

Asmi, A.

2012-07-01

Aerosol particles are everywhere in the atmosphere. They are a key factor in many important processes in the atmosphere, including cloud formation, scattering of incoming solar radiation and air chemistry. The aerosol particles have relatively short lifetimes in lower atmosphere, typically from days to weeks, and thus they have a high spatial and temporal variability. This thesis concentrates on the extent and reasons of sub-micron aerosol particle variability in the lower atmosphere, using both global atmospheric models and analysis of observational data. Aerosol number size distributions in the lower atmosphere are affected strongly by the new particle formation. Perhaps more importantly, a strong influence new particle formation is also evident in the cloud condensation nuclei (CCN) concentrations, suggesting a major role of the sulphuric acid driven new particle formation in the climate system. In this thesis, the sub-micron aerosol number size distributions in the European regional background air were characterized for the first time from consistent, homogenized and comparable datasets. Some recent studies have suggested that differences in aerosol emissions between weekdays could also affect the weather via aerosol-cloud interactions. In this thesis, the weekday-to-weekday variation of CCN sized aerosol number concentrations in Europe were found to be much smaller than expected from earlier studies, based on particle mass measurements. This result suggests that a lack of week-day variability in meteorology is not necessarily a sign of weak aerosol-cloud interactions. An analysis of statistically significant trends in past decades of measured aerosol number concentrations from Europe, North America, Pacific islands and Antarctica generally show decreases in concentrations. The analysis of these changes show that a potential explanation for the decreasing trends is the general reduction of anthropogenic emissions, especially SO{sub 2}, although a combination of

Atmospheric oxidation of isoprene and 1,3-Butadiene: influence of aerosol acidity and Relative humidity on secondary organic aerosol

Science.gov (United States)

The effects of acidic seed aerosols on the formation of secondary organic aerosol (SOA)have been examined in a number of previous studies, several of which have observed strong linear correlations between the aerosol acidity (measured as nmol H+ per m3 air s...

Topics in current aerosol research

CERN Document Server

Hidy, G M

1971-01-01

Topics in Current Aerosol Research deals with the fundamental aspects of aerosol science, with emphasis on experiment and theory describing highly dispersed aerosols (HDAs) as well as the dynamics of charged suspensions. Topics covered range from the basic properties of HDAs to their formation and methods of generation; sources of electric charges; interactions between fluid and aerosol particles; and one-dimensional motion of charged cloud of particles. This volume is comprised of 13 chapters and begins with an introduction to the basic properties of HDAs, followed by a discussion on the form

The SOA/VOC/NOx system: an explicit model of secondary organic aerosol formation

Directory of Open Access Journals (Sweden)

S. Madronich

2007-11-01

Full Text Available Our current understanding of secondary organic aerosol (SOA formation is limited by our knowledge of gaseous secondary organics involved in gas/particle partitioning. The objective of this study is to explore (i the potential for products of multiple oxidation steps contributing to SOA, and (ii the evolution of the SOA/VOC/NOx system. We developed an explicit model based on the coupling of detailed gas-phase oxidation schemes with a thermodynamic condensation module. Such a model allows prediction of SOA mass and speciation on the basis of first principles. The SOA/VOC/NOx system is studied for the oxidation of 1-octene under atmospherically relevant concentrations. In this study, gaseous oxidation of octene is simulated to lead to SOA formation. Contributors to SOA formation are shown to be formed via multiple oxidation steps of the parent hydrocarbon. The behaviour of the SOA/VOC/NOx system simulated using the explicit model agrees with general tendencies observed during laboratory chamber experiments. This explicit modelling of SOA formation appears as a useful exploratory tool to (i support interpretations of SOA formation observed in laboratory chamber experiments, (ii give some insights on SOA formation under atmospherically relevant conditions and (iii investigate implications for the regional/global lifetimes of the SOA.

Study of photolytic aerosols at stratospheric pressures

International Nuclear Information System (INIS)

Delattre, Patrick.

1975-07-01

An experimental study of photolytic aerosol formation at stratospheric pressure (60 Torr) and laboratory temperature, was carried out previous to the exact simulation of photolytic aerosol formation in real stratospheric conditions. An experimental simulation device, techniques of generation of known mixtures of inert gases with SO 2 and NOsub(x) traces at low concentration (below 1 ppm volume) and H 2 O traces (a few ppm), and techniques for the determination and counting of aerosol particles at low pressures were perfected. The following results were achieved: the rate of vapor condensation on nuclei was reduced when total pressure decreased. At low pressure the working of condensation nuclei counters and the formation of photolytic aerosols is influenced by this phenomenon. An explanation is proposed, as well as means to avoid this unpleasant effect on the working of nuclei counters at low pressure. No photolytic aerosol production was ascertained at 60 Torr when water concentration was below 100 ppm whatever the concentration of SO 2 or NOsub(x) traces. With water concentration below 1200ppm and SO 2 trace concentration below 1ppm, the aerosol particles produced could not consist of sulfuric acid drops but probably of nitrosyl sulfate acide crystals [fr

Aerosol-driven increase in Arctic sea ice over the middle of the twentieth century

Science.gov (United States)

Gagné, Marie-Ève; Fyfe, John C.; Gillett, Nathan P.; Polyakov, Igor V.; Flato, Gregory M.

2017-07-01

Updated observational data sets without climatological infilling show that there was an increase in sea ice concentration in the eastern Arctic between 1950 and 1975, contrary to earlier climatology infilled observational data sets that show weak interannual variations during that time period. We here present climate model simulations showing that this observed sea ice concentration increase was primarily a consequence of cooling induced by increasing anthropogenic aerosols and natural forcing. Indeed, sulphur dioxide emissions, which lead to the formation of sulphate aerosols, peaked around 1980 causing a sharp increase in the burden of sulphate between the 1950s and 1970s; but since 1980, the burden has dropped. Our climate model simulations show that the cooling contribution of aerosols offset the warming effect of increasing greenhouse gases over the midtwentieth century resulting in the expansion of the Arctic sea ice cover. These results challenge the perception that Arctic sea ice extent was unperturbed by human influence until the 1970s, suggesting instead that it exhibited earlier forced multidecadal variations, with implications for our understanding of impacts and adaptation in human and natural Arctic systems.

Improvements to the WRF-Chem 3.5.1 model for quasi-hemispheric simulations of aerosols and ozone in the Arctic

Directory of Open Access Journals (Sweden)

L. Marelle

2017-10-01

Full Text Available In this study, the WRF-Chem regional model is updated to improve simulated short-lived pollutants (e.g., aerosols, ozone in the Arctic. Specifically, we include in WRF-Chem 3.5.1 (with SAPRC-99 gas-phase chemistry and MOSAIC aerosols (1 a correction to the sedimentation of aerosols, (2 dimethyl sulfide (DMS oceanic emissions and gas-phase chemistry, (3 an improved representation of the dry deposition of trace gases over seasonal snow, and (4 an UV-albedo dependence on snow and ice cover for photolysis calculations. We also (5 correct the representation of surface temperatures over melting ice in the Noah Land Surface Model and (6 couple and further test the recent KF-CuP (Kain–Fritsch + Cumulus Potential cumulus parameterization that includes the effect of cumulus clouds on aerosols and trace gases. The updated model is used to perform quasi-hemispheric simulations of aerosols and ozone, which are evaluated against surface measurements of black carbon (BC, sulfate, and ozone as well as airborne measurements of BC in the Arctic. The updated model shows significant improvements in terms of seasonal aerosol cycles at the surface and root mean square errors (RMSEs for surface ozone, aerosols, and BC aloft, compared to the base version of the model and to previous large-scale evaluations of WRF-Chem in the Arctic. These improvements are mostly due to the inclusion of cumulus effects on aerosols and trace gases in KF-CuP (improved RMSE for surface BC and BC profiles, surface sulfate, and surface ozone, the improved surface temperatures over sea ice (surface ozone, BC, and sulfate, and the updated trace gas deposition and UV albedo over snow and ice (improved RMSE and correlation for surface ozone. DMS emissions and chemistry improve surface sulfate at all Arctic sites except Zeppelin, and correcting aerosol sedimentation has little influence on aerosols except in the upper troposphere.

Organic condensation: A vital link connecting aerosol formation to climate forcing (Invited)

Science.gov (United States)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petdjd, T. T.; Slowik, J. G.; Chang, R. Y.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M. T.

2010-12-01

Aerosol-cloud interactions represent the largest uncertainty in calculations of Earth’s radiative forcing. Number concentrations of atmospheric aerosol particles are in the core of this uncertainty, as they govern the numbers of cloud condensation nuclei (CCN) and influence the albedo and lifetime of clouds. Aerosols also impair air quality through their adverse effects on atmospheric visibility and human health. The ultrafine fraction ( 100 nm) and enhance the loss of ultrafine particles. Primary organic aerosol (POA) contributes to the large end of the aerosol size distribution, enhancing the scavenging of the ultrafine particles.

Present role of PIXE in atmospheric aerosol research

Energy Technology Data Exchange (ETDEWEB)

Maenhaut, Willy, E-mail: Willy.Maenhaut@UGent.be

2015-11-15

In the 1980s and 1990s nearly half of the elemental analyses of atmospheric aerosol samples were performed by PIXE. Since then, other techniques for elemental analysis became available and there has been a steady increase in studies on organic aerosol constituents and other aspects of aerosols, especially in the areas of nucleation (new particle formation), optical properties, and the role of aerosol particles in cloud formation and properties. First, a brief overview and discussion is given of the developments and trends in atmospheric aerosol analysis and research of the past three decades. Subsequently, it is indicated that there is still invaluable work to be done by PIXE in atmospheric aerosol research, especially if one teams up with other aerosol researchers and performs complementary measurements, e.g., on small aerosol samples that are taken with high-time resolution. Fine examples of such research are the work done by the Lund group in the CARIBIC aircraft studies and the analysis of circular streaker samples by the Florence PIXE group. These and other examples are presented and other possibilities of PIXE are indicated.

Simulating the formation of carbonaceous aerosol in a European Megacity (Paris during the MEGAPOLI summer and winter campaigns

Directory of Open Access Journals (Sweden)

C. Fountoukis

2016-03-01

Full Text Available We use a three-dimensional regional chemical transport model (PMCAMx with high grid resolution and high-resolution emissions (4 × 4 km2 over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009 and a winter (January/February 2010 period as part of the MEGAPOLI (megacities: emissions, urban, regional, and global atmospheric pollution and climate effects, and Integrated tools for assessment and mitigation campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 % of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA concentrations is also encouraging (mean bias = 0.1 µg m−3 during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 µg m−3 mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d−1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00–14:00 LT and 20 % during dinner time (20:00–22:00 LT. Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias =  −2.3 µg m−3 pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.

Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the MEGAPOLI summer and winter campaigns

Science.gov (United States)

Fountoukis, Christos; Megaritis, Athanasios G.; Skyllakou, Ksakousti; Charalampidis, Panagiotis E.; Denier van der Gon, Hugo A. C.; Crippa, Monica; Prévôt, André S. H.; Fachinger, Friederike; Wiedensohler, Alfred; Pilinis, Christodoulos; Pandis, Spyros N.

2016-03-01

We use a three-dimensional regional chemical transport model (PMCAMx) with high grid resolution and high-resolution emissions (4 × 4 km2) over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009) and a winter (January/February 2010) period as part of the MEGAPOLI (megacities: emissions, urban, regional, and global atmospheric pollution and climate effects, and Integrated tools for assessment and mitigation) campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC) high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 %) of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA) concentrations is also encouraging (mean bias = 0.1 µg m-3) during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 µg m-3) mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d-1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00-14:00 LT) and 20 % during dinner time (20:00-22:00 LT). Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias = -2.3 µg m-3) pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.

Secondary Aerosol Formation over the ESCOMPTE Area: Results from airborne Aerosol and Trace Gas Measurements

Science.gov (United States)

van Dingenen, R.; Martins-Dos Santos, S.; Putaud, J. P.; Allet, C.; Bretton, E.; Perros, P.

2003-04-01

From June 10th to July 14th 2001, the ESCOMPTE campaign took place in the Marseille-Berre area in Southern France. The goal of the campaign was to produce a high quality 3-D data base from emissions, transport and air composition measurements during urban photochemical pollution episodes at the meso-scale. The CAATER AEROPLUM project was embedded within this international field campaign. AEROPLUM aimed at mapping size distributions of aerosols and photo-oxidants in the mixed layer over the ESCOMPTE domain, using the ARAT Fokker 27 as measurement platform. Aircraft sub-micrometer aerosol measurements are validated during overpasses against ground-based measurements, carried out with similar instrumentation. We will present and discuss data during periods of seabreeze, transporting coastal industrial and urban pollution land-inwards. This leads to intense photochemical activity, evidenced by elevated O_3 concentrations and aerosol levels.

Aerosols from biomass combustion

Energy Technology Data Exchange (ETDEWEB)

Nussbaumer, T

2001-07-01

This report is the proceedings of a seminar on biomass combustion and aerosol production organised jointly by the International Energy Agency's (IEA) Task 32 on bio energy and the Swiss Federal Office of Energy (SFOE). This collection of 16 papers discusses the production of aerosols and fine particles by the burning of biomass and their effects. Expert knowledge on the environmental impact of aerosols, formation mechanisms, measurement technologies, methods of analysis and measures to be taken to reduce such emissions is presented. The seminar, visited by 50 participants from 11 countries, shows, according to the authors, that the reduction of aerosol emissions resulting from biomass combustion will remain a challenge for the future.

Aerosols from biomass combustion

Energy Technology Data Exchange (ETDEWEB)

Nussbaumer, T.

2001-07-01

This report is the proceedings of a seminar on biomass combustion and aerosol production organised jointly by the International Energy Agency's (IEA) Task 32 on bio energy and the Swiss Federal Office of Energy (SFOE). This collection of 16 papers discusses the production of aerosols and fine particles by the burning of biomass and their effects. Expert knowledge on the environmental impact of aerosols, formation mechanisms, measurement technologies, methods of analysis and measures to be taken to reduce such emissions is presented. The seminar, visited by 50 participants from 11 countries, shows, according to the authors, that the reduction of aerosol emissions resulting from biomass combustion will remain a challenge for the future.

Removal of sulfur dioxide and formation of sulfate aerosol in Tokyo

Science.gov (United States)

Miyakawa, T.; Takegawa, N.; Kondo, Y.

2007-07-01

Ground-based in situ measurements of sulfur dioxide (SO2) and submicron sulfate aerosol (SO42-) together with carbon monoxide (CO) were conducted at an urban site in Tokyo, Japan from spring 2003 to winter 2004. The observed concentrations of SO2 were affected dominantly by anthropogenic emissions (for example, manufacturing industries) in source areas, while small fraction of the data (sulfur compounds (SOx = SO2 + SO42-) and the remaining fraction of SOx, which is derived as the ratio of the linear regression slope of the SOx-CO correlation, is used as measures for the formation of SO42- and removal of SOx, respectively. Using these parameters, the average formation efficiency of SO42- (i.e., amount of SO42- produced per SO2 emitted from emission sources) are estimated to be 0.18 and 0.03 in the summer and winter periods, respectively. A simple box model was developed to estimate the lifetime of SOx. The lifetime of SOx for the summer period (26 h) is estimated to be about two times longer than that for the winter period (14 h). The seasonal variations of the remaining fraction of SOx, estimated formation efficiency of SO42-, and lifetime of SOx are likely due to those of the boundary layer height and photochemical activity (i.e., hydroxyl radical). These results provide useful insights into the formation and removal processes of sulfur compounds exported from an urban area.

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

Science.gov (United States)

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

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

Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the Megapoli summer and winter campaigns

NARCIS (Netherlands)

Fountoukis, C.; Megaritis, A.G.; Skyllakou, K.; Charalampidis, P.E.; Denier van der Gon, H.A.C.; Crippa, M.; Prevot, A.S.H.; Fachinger, F.; Wiedensohler, A.; Pilinis, C.; Pandis, S.N.

2016-01-01

We use a three-dimensional regional chemical transport model (PMCAMx) with high grid resolution and high-resolution emissions (4 x 4 km2) over the Paris greater area to simulate the formation of carbonaceous aerosol dur-ing a summer (July 2009) and a winter (January/February 2010) period as part of

Modeled aerosol nitrate formation pathways during wintertime in the Great Lakes region of North America

Science.gov (United States)

Kim, Yoo Jung; Spak, Scott N.; Carmichael, Gregory R.; Riemer, Nicole; Stanier, Charles O.

2014-11-01

Episodic wintertime particle pollution by ammonium nitrate is an important air quality concern across the Midwest U.S. Understanding and accurately forecasting PM2.5 episodes are complicated by multiple pathways for aerosol nitrate formation, each with uncertain rate parameters. Here, the Community Multiscale Air Quality model (CMAQ) simulated regional atmospheric nitrate budgets during the 2009 LADCO Winter Nitrate Study, using integrated process rate (IPR) and integrated reaction rate (IRR) tools to quantify relevant processes. Total nitrate production contributing to PM2.5 episodes is a regional phenomenon, with peak production over the Ohio River Valley and southern Great Lakes. Total nitrate production in the lower troposphere is attributed to three pathways, with 57% from heterogeneous conversion of N2O5, 28% from the reaction of OH and NO2, and 15% from homogeneous conversion of N2O5. TNO3 formation rates varied day-to-day and on synoptic timescales. Rate-limited production does not follow urban-rural gradients and NOx emissions due, to counterbalancing of urban enhancement in daytime HNO3 production with nocturnal reductions. Concentrations of HNO3 and N2O5 and nighttime TNO3 formation rates have maxima aloft (100-500 m), leading to net total nitrate vertical flux during episodes, with substantial vertical gradients in nitrate partitioning. Uncertainties in all three pathways are relevant to wintertime aerosol modeling and highlight the importance of interacting transport and chemistry processes during ammonium nitrate episodes, as well as the need for additional constraint on the system through field and laboratory experiments.

Aerosol single-scattering albedo and asymmetry parameter from MFRSR observations during the ARM Aerosol IOP 2003

Directory of Open Access Journals (Sweden)

E. I. Kassianov

2007-06-01

Full Text Available Multi-filter Rotating Shadowband Radiometers (MFRSRs provide routine measurements of the aerosol optical depth (τ at six wavelengths (0.415, 0.5, 0.615, 0.673, 0.870 and 0.94 μm. The single-scattering albedo (π₀ is typically estimated from the MFRSR measurements by assuming the asymmetry parameter (g. In most instances, however, it is not easy to set an appropriate value of g due to its strong temporal and spatial variability. Here, we introduce and validate an updated version of our retrieval technique that allows one to estimate simultaneously π₀ and g for different types of aerosol. We use the aerosol and radiative properties obtained during the Atmospheric Radiation Measurement (ARM Program's Aerosol Intensive Operational Period (IOP to validate our retrieval in two ways. First, the MFRSR-retrieved optical properties are compared with those obtained from independent surface, Aerosol Robotic Network (AERONET, and aircraft measurements. The MFRSR-retrieved optical properties are in reasonable agreement with these independent measurements. Second, we perform radiative closure experiments using the MFRSR-retrieved optical properties. The calculated broadband values of the direct and diffuse fluxes are comparable (~5 W/m² to those obtained from measurements.

Quantifying dust plume formation and aerosol size distribution during the Saharan Mineral Dust Experiment in North Africa

KAUST Repository

Khan, Basit Ali

2015-01-01

Dust particles mixed in the free troposphere have longer lifetimes than airborne particles near the surface. Their cumulative radiative impact on earth’s meteorological processes and climate might be significant despite their relatively small contribution to total dust abundance. One example is the elevated dust--laden Saharan Air Layer (SAL) over the equatorial North Atlantic, which cools the sea surface and likely suppresses hurricane activity. To understand the formation mechanisms of SAL, we combine model simulations and dust observations collected during the first stage of the Saharan Mineral Dust Experiment (SAMUM--I), which sampled dust events that extended from Morocco to Portugal, and investigated the spatial distribution and the microphysical, optical, chemical, and radiative properties of Saharan mineral dust. We employed the Weather Research Forecast model coupled with the Chemistry/Aerosol module (WRF--Chem) to reproduce the meteorological environment and spatial and size distributions of dust. The experimental domain covers northwest Africa including the southern Sahara, Morocco and part of the Atlantic Ocean with 5 km horizontal grid spacing and 51 vertical layers. The experiments were run from 20 May to 9 June 2006, covering the period of most intensive dust outbreaks. Comparisons of model results with available airborne and ground--based observations show that WRF--Chem reproduces observed meteorological fields as well as aerosol distribution across the entire region and along the airplane’s tracks. We evaluated several aerosol uplift processes and found that orographic lifting, aerosol transport through the land/sea interface with steep gradients of meteorological characteristics, and interaction of sea breezes with the continental outflow are key mechanisms that form a surface--detached aerosol plume over the ocean. Comparisons of simulated dust size distributions with airplane and ground--based observations are generally good, but suggest

Different roles of water in secondary organic aerosol formation from toluene and isoprene

Science.gov (United States)

Jia, Long; Xu, YongFu

2018-06-01

Roles of water in the formation of secondary organic aerosol (SOA) from the irradiations of toluene-NO2 and isoprene-NO2 were investigated in a smog chamber. Experimental results show that the yield of SOA from toluene almost doubled as relative humidity increased from 5 to 85 %, whereas the yield of SOA from isoprene under humid conditions decreased by 2.6 times as compared to that under dry conditions. The distinct difference of RH effects on SOA formation from toluene and isoprene is well explained with our experiments and model simulations. The increased SOA from humid toluene-NO2 irradiations is mainly contributed by O-H-containing products such as polyalcohols formed from aqueous reactions. The major chemical components of SOA in isoprene-NO2 irradiations are oligomers formed from the gas phase. SOA formation from isoprene-NO2 irradiations is controlled by stable Criegee intermediates (SCIs) that are greatly influenced by water. As a result, high RH can obstruct the oligomerization reaction of SCIs to form SOA.

Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol

Energy Technology Data Exchange (ETDEWEB)

Shrivastava, Manish [Pacific Northwest National Laboratory, Richland Washington USA; Cappa, Christopher D. [Department of Civil and Environmental Engineering, University of California, Davis California USA; Fan, Jiwen [Pacific Northwest National Laboratory, Richland Washington USA; Goldstein, Allen H. [Department of Environmental Science, Policy and Management and Department of Civil and Environmental Engineering, University of California, Berkeley California USA; Guenther, Alex B. [Department of Earth System Science, University of California, Irvine California USA; Jimenez, Jose L. [Cooperative Institute for Research in Environmental Sciences and Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder Colorado USA; Kuang, Chongai [Brookhaven National Laboratory, Upton New York USA; Laskin, Alexander [Pacific Northwest National Laboratory, Richland Washington USA; Martin, Scot T. [School of Engineering and Applied Sciences and Department of Earth and Planetary Sciences, Harvard University, Cambridge Massachusetts USA; Ng, Nga Lee [School of Chemical and Biomolecular Engineering and School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta Georgia USA; Petaja, Tuukka [Department of Physics, University of Helsinki, Helsinki Finland; Pierce, Jeffrey R. [Department of Atmospheric Science, Colorado State University, Fort Collins Colorado USA; Rasch, Philip J. [Pacific Northwest National Laboratory, Richland Washington USA; Roldin, Pontus [Department of Physics, Lund University, Lund Sweden; Seinfeld, John H. [Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena California USA; Shilling, John [Pacific Northwest National Laboratory, Richland Washington USA; Smith, James N. [Department of Earth System Science, University of California, Irvine California USA; Thornton, Joel A. [Department of Atmospheric Sciences, University of Washington, Seattle Washington USA; Volkamer, Rainer [Cooperative Institute for Research in Environmental Sciences and Department of Chemistry and Biochemistry, University of Colorado Boulder, Boulder Colorado USA; Wang, Jian [Brookhaven National Laboratory, Upton New York USA; Worsnop, Douglas R. [Aerodyne Research, Inc., Billerica Massachusetts USA; Zaveri, Rahul A. [Pacific Northwest National Laboratory, Richland Washington USA; Zelenyuk, Alla [Pacific Northwest National Laboratory, Richland Washington USA; Zhang, Qi [Department of Environmental Toxicology, University of California, Davis California USA

2017-06-01

Anthropogenic emissions and land-use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding pre-industrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features 1) influence estimates of aerosol radiative forcing and 2) can confound estimates of the historical response of climate to increases in greenhouse gases (e.g. the ‘climate sensitivity’). Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through a combination of laboratory and field measurements, yet current climate models typically do not comprehensively include all important SOA-relevant processes. Therefore, major gaps exist at present between current measurement-based knowledge on the one hand and model implementation of organic aerosols on the other. The critical review herein summarizes some of the important developments in understanding SOA formation that could potentially have large impacts on our understanding of aerosol radiative forcing and climate. We highlight the importance of some recently discovered processes and properties that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including: formation of extremely low-volatility organics in the gas-phase; isoprene epoxydiols (IEPOX) multi-phase chemistry; particle-phase oligomerization; and physical properties such as viscosity. In addition, this review also highlights some of the important processes that involve interactions between natural biogenic emissions and anthropogenic emissions, such as the role of sulfate and oxides of nitrogen (NOx) on SOA formation from biogenic volatile organic compounds. Studies that relate the observed evolution of organic aerosol

Cloud-Resolving Model Simulations of Aerosol-Cloud Interactions Triggered by Strong Aerosol Emissions in the Arctic

Science.gov (United States)

Wang, H.; Kravitz, B.; Rasch, P. J.; Morrison, H.; Solomon, A.

2014-12-01

Previous process-oriented modeling studies have highlighted the dependence of effectiveness of cloud brightening by aerosols on cloud regimes in warm marine boundary layer. Cloud microphysical processes in clouds that contain ice, and hence the mechanisms that drive aerosol-cloud interactions, are more complicated than in warm clouds. Interactions between ice particles and liquid drops add additional levels of complexity to aerosol effects. A cloud-resolving model is used to study aerosol-cloud interactions in the Arctic triggered by strong aerosol emissions, through either geoengineering injection or concentrated sources such as shipping and fires. An updated cloud microphysical scheme with prognostic aerosol and cloud particle numbers is employed. Model simulations are performed in pure super-cooled liquid and mixed-phase clouds, separately, with or without an injection of aerosols into either a clean or a more polluted Arctic boundary layer. Vertical mixing and cloud scavenging of particles injected from the surface is still quite efficient in the less turbulent cold environment. Overall, the injection of aerosols into the Arctic boundary layer can delay the collapse of the boundary layer and increase low-cloud albedo. The pure liquid clouds are more susceptible to the increase in aerosol number concentration than the mixed-phase clouds. Rain production processes are more effectively suppressed by aerosol injection, whereas ice precipitation (snow) is affected less; thus the effectiveness of brightening mixed-phase clouds is lower than for liquid-only clouds. Aerosol injection into a clean boundary layer results in a greater cloud albedo increase than injection into a polluted one, consistent with current knowledge about aerosol-cloud interactions. Unlike previous studies investigating warm clouds, the impact of dynamical feedback due to precipitation changes is small. According to these results, which are dependent upon the representation of ice nucleation

Gas-phase products and secondary organic aerosol formation from the ozonolysis and photooxidation of myrcene

Science.gov (United States)

Böge, Olaf; Mutzel, Anke; Iinuma, Yoshiteru; Yli-Pirilä, Pasi; Kahnt, Ariane; Joutsensaari, Jorma; Herrmann, Hartmut

2013-11-01

In this study, the ozone and OH-radical reactions of myrcene were investigated in an aerosol chamber (at 292-295 K and 50% relative humidity) to examine the gas-phase oxidation products and secondary organic aerosol (SOA) formation. The ozone reaction studies were performed in the presence and absence of CO, which serves as an OH radical scavenger. In the photooxidation experiments OH radicals were generated by photolysis of methyl nitrite. The ozonolysis of myrcene in the presence of CO resulted in a substantial yield of 4-vinyl-4-pentenal (55.3%), measured as m/z 111 plus m/z 93 using proton transfer reaction-mass spectrometry (PTR-MS) and confirmed unambiguously as C7H10O by denuder measurements and HPLC/ESI-TOFMS analysis of its 2,4-dinitrophenylhydrazine (DNPH) derivative. Additionally, the formation of two different organic dicarbonyls with m/z 113 and a molecular formula of C6H8O2 were observed (2.1%). The yields of these dicarbonyls were higher in the ozonolysis experiments without an OH scavenger (5.4%) and even higher (13.8%) in the myrcene OH radical reaction. The formation of hydroxyacetone as a direct product of the myrcene reaction with ozone with a molar yield of 17.6% was also observed. The particle size distribution and volume concentrations were monitored and facilitated the calculation of SOA yields, which ranged from 0 to 0.01 (ozonolysis in the presence of CO) to 0.39 (myrcene OH radical reaction). Terpenylic acid was found in the SOA samples collected from the ozonolysis of myrcene in the absence of an OH scavenger and the OH radical-initiated reaction of myrcene but not in samples collected from the ozonolysis in the presence of CO as an OH radical scavenger, suggesting that terpenylic acid formation involves the reaction of myrcene with an OH radical. A reaction mechanism describing the formation of terpenylic acid is proposed.

Science Plan Biogenic Aerosols – Effects on Clouds and Climate (BAECC)

Energy Technology Data Exchange (ETDEWEB)

Petäjä, T

2013-12-01

Atmospheric aerosol particles impact human health in urban environments, while on regional and global scales they can affect climate patterns, the hydrological cycle, and the intensity of radiation that reaches the Earth’s surface. In spite of recent advances in the understanding of aerosol formation processes and the links between aerosol dynamics and biosphere-atmosphere-climate interactions, great challenges remain in the analysis of related processes on a global scale. Boreal forests, situated in a circumpolar belt in the northern latitudes throughout the United States, Canada, Russia and Scandinavia, are among the most active areas of atmospheric aerosol formation among all biomes. The formation of aerosol particles and their growth to the sizes of cloud condensation nuclei in these areas are associated with biogenic volatile organic emissions from vegetation and soil.

The Valence of Self-Generated (Status Updates) and Other-Generated (Wall-Posts) Information Determines Impression Formation on Facebook

Science.gov (United States)

Rosenthal-Stott, Harriet E. S.; Dicks, Rea E.; Fielding, Lois S.

2015-01-01

We examined whether self-generated (status updates) or other-generated (wall-posts) information on Facebook influenced the impression formed of the target individual. Along with examining reliance on particular types of information, we explored the valence (positive/ neutral/ negative) of the information, as reliance on self-generated or other-generated information may depend on whether self-presentation is perceived (i.e., presenting oneself positively / not negatively). Self-presentation may be perceived if the targets have positive/ neutral statuses, while negative statuses would indicate a lack of self-presentation. In line with previous research, participants should rely on other-generated information (wall-posts) to form an impression when participants are viewed to have self-presented (positive / neutral status updates), as this information could be viewed as unreliable. Forty participants rated nine Facebook profiles where statuses and wall-posts portrayed personality traits varying in valence. Each profile consisted of a neutral profile photo, three status updates (all positive, negative, or neutral) and three wall-posts (all positive, negative, or neutral). Materials were established in two pilots. Impression formation was measured as perceived social, task, and physical attractiveness of the target individual. Participants also ranked the profiles for likeability. Supporting our expectations, other-generated information (wall-posts) dominated impression formation for social attractiveness when self-generated information (status updates) was positive/ neutral. Task attractiveness was affected by information valence, regardless of source (self or other). Despite the inclusion of neutral photos, physical attractiveness was affected by self-generated information, with negative statuses lowering physical attractiveness. We suggest that these findings have implications for impression formation beyond the Facebook setting. The 557 traits analyzed in Pilot 1 are

NOAA's National Air Quality Prediction and Development of Aerosol and Atmospheric Composition Prediction Components for NGGPS

Science.gov (United States)

Stajner, I.; McQueen, J.; Lee, P.; Stein, A. F.; Wilczak, J. M.; Upadhayay, S.; daSilva, A.; Lu, C. H.; Grell, G. A.; Pierce, R. B.

2017-12-01

NOAA's operational air quality predictions of ozone, fine particulate matter (PM2.5) and wildfire smoke over the United States and airborne dust over the contiguous 48 states are distributed at http://airquality.weather.gov. The National Air Quality Forecast Capability (NAQFC) providing these predictions was updated in June 2017. Ozone and PM2.5 predictions are now produced using the system linking the Community Multiscale Air Quality model (CMAQ) version 5.0.2 with meteorological inputs from the North American Mesoscale Forecast System (NAM) version 4. Predictions of PM2.5 include intermittent dust emissions and wildfire emissions from an updated version of BlueSky system. For the latter, the CMAQ system is initialized by rerunning it over the previous 24 hours to include wildfire emissions at the time when they were observed from the satellites. Post processing to reduce the bias in PM2.5 prediction was updated using the Kalman filter analog (KFAN) technique. Dust related aerosol species at the CMAQ domain lateral boundaries now come from the NEMS Global Aerosol Component (NGAC) v2 predictions. Further development of NAQFC includes testing of CMAQ predictions to 72 hours, Canadian fire emissions data from Environment and Climate Change Canada (ECCC) and the KFAN technique to reduce bias in ozone predictions. NOAA is developing the Next Generation Global Predictions System (NGGPS) with an aerosol and gaseous atmospheric composition component to improve and integrate aerosol and ozone predictions and evaluate their impacts on physics, data assimilation and weather prediction. Efforts are underway to improve cloud microphysics, investigate aerosol effects and include representations of atmospheric composition of varying complexity into NGGPS: from the operational ozone parameterization, GOCART aerosols, with simplified ozone chemistry, to CMAQ chemistry with aerosol modules. We will present progress on community building, planning and development of NGGPS.

Effects of NOx and SO2 on the secondary organic aerosol formation from photooxidation of α-pinene and limonene

Science.gov (United States)

Zhao, Defeng; Schmitt, Sebastian H.; Wang, Mingjin; Acir, Ismail-Hakki; Tillmann, Ralf; Tan, Zhaofeng; Novelli, Anna; Fuchs, Hendrik; Pullinen, Iida; Wegener, Robert; Rohrer, Franz; Wildt, Jürgen; Kiendler-Scharr, Astrid; Wahner, Andreas; Mentel, Thomas F.

2018-02-01

Anthropogenic emissions such as NOx and SO2 influence the biogenic secondary organic aerosol (SOA) formation, but detailed mechanisms and effects are still elusive. We studied the effects of NOx and SO2 on the SOA formation from the photooxidation of α-pinene and limonene at ambient relevant NOx and SO2 concentrations (NOx: leading to a lack of particle surface for the organics to condense on and thus a significant influence of vapor wall loss on SOA mass yield. By compensating for the suppressing effect on nucleation of NOx, SO2 also compensated for the suppressing effect on SOA yield. Aerosol mass spectrometer data show that increasing NOx enhanced nitrate formation. The majority of the nitrate was organic nitrate (57-77 %), even in low-NOx conditions (nitrate contributed 7-26 % of total organics assuming a molecular weight of 200 g mol-1. SOA from α-pinene photooxidation at high NOx had a generally lower hydrogen to carbon ratio (H / C), compared to low NOx. The NOx dependence of the chemical composition can be attributed to the NOx dependence of the branching ratio of the RO2 loss reactions, leading to a lower fraction of organic hydroperoxides and higher fractions of organic nitrates at high NOx. While NOx suppressed new particle formation and SOA mass formation, SO2 can compensate for such effects, and the combining effect of SO2 and NOx may have an important influence on SOA formation affected by interactions of biogenic volatile organic compounds (VOCs) with anthropogenic emissions.

Evidence of aqueous secondary organic aerosol formation from biogenic emissions in the North American Sonoran Desert.

Science.gov (United States)

Youn, Jong-Sang; Wang, Zhen; Wonaschütz, Anna; Arellano, Avelino; Betterton, Eric A; Sorooshian, Armin

2013-07-16

This study examines the role of aqueous secondary organic aerosol formation in the North American Sonoran Desert as a result of intense solar radiation, enhanced moisture, and biogenic volatile organic compounds (BVOCs). The ratio of water-soluble organic carbon (WSOC) to organic carbon (OC) nearly doubles during the monsoon season relative to other seasons of the year. When normalized by mixing height, the WSOC enhancement during monsoon months relative to preceding dry months (May-June) exceeds that of sulfate by nearly a factor of 10. WSOC:OC and WSOC are most strongly correlated with moisture parameters, temperature, and concentrations of O 3 and BVOCs. No positive relationship was identified between WSOC or WSOC:OC and anthropogenic tracers such as CO over a full year. This study points at the need for further work to understand the effect of BVOCs and moisture in altering aerosol properties in understudied desert regions.

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.

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

DEFF Research Database (Denmark)

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

2012-01-01

The objectives of the present work were to investigate the aerosol formation mechanisms during full-scale suspension firing of wood, and, to evaluate the effect of coal fly ash addition on the formation of aerosols under different ash load conditions. Tests with suspension firing of 100 % wood...

Formation of secondary organic aerosol in the Paris pollution plume and its impact on surrounding regions

Science.gov (United States)

Zhang, Q. J.; Beekmann, M.; Freney, E.; Sellegri, K.; Pichon, J. M.; Schwarzenboeck, A.; Colomb, A.; Bourrianne, T.; Michoud, V.; Borbon, A.

2015-12-01

Secondary pollutants such as ozone, secondary inorganic aerosol, and secondary organic aerosol formed in the plumes of megacities can affect regional air quality. In the framework of the FP7/EU MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) project, an intensive campaign was launched in the greater Paris region in July 2009. The major objective was to quantify different sources of organic aerosol (OA) within a megacity and in its plume. In this study, we use airborne measurements aboard the French ATR-42 aircraft to evaluate the regional chemistry-transport model CHIMERE within and downwind of the Paris region. Two mechanisms of secondary OA (SOA) formation are used, both including SOA formation from oxidation and chemical aging of primary semivolatile and intermediate volatility organic compounds (SI-SOA) in the volatility basis set (VBS) framework. As for SOA formed from traditional VOC (volatile organic compound) precursors (traditional SOA), one applies chemical aging in the VBS framework adopting different SOA yields for high- and low-NOx environments, while another applies a single-step oxidation scheme without chemical aging. Two emission inventories are used for discussion of emission uncertainties. The slopes of the airborne OA levels versus Ox (i.e., O3 + NO2) show SOA formation normalized with respect to photochemical activity and are used for specific evaluation of the OA scheme in the model. The simulated slopes were overestimated slightly by factors of 1.1, 1.7 and 1.3 with respect to those observed for the three airborne measurements, when the most realistic "high-NOx" yields for traditional SOA formation in the VBS scheme are used in the model. In addition, these slopes are relatively stable from one day to another, which suggests that they are characteristic for the given megacity plume environment. The configuration with increased primary

Comprehensive Measurement of Atmospheric Aerosols with a Wide Range Aerosol Spectrometer

International Nuclear Information System (INIS)

Keck, L; Pesch, M; Grimm, H

2011-01-01

A wide range aerosol spectrometer (WRAS) was used for comprehensive long term measurements of aerosol size distributions. The system combines the results of an optical aerosol spectrometer with the results of a Scanning Mobility Particle Sizer (SMPS) to record essentially the full size range (5 nm - 32 μm) of atmospheric particles in 72 channels. Measurements were carried out over one year (2009) at the Global Atmospheric Watch (GAW)-Station Hohenpeissenberg, Bavaria. Total particle number concentrations obtained from the aerosol size distributions were compared to the total number concentrations measured by a Condensation Particle Counter (CPC). The comparison showed an excellent agreement of the data. The high time resolution of 5 minutes allows the combination of the measured size distributions with meteorological data and correlations to gaseous pollutants (CO, NOx and SO2). A good correlation of particle number and CO concentrations was found for long distance transported small particles, which were probably mainly soot particles. Correlations to NOx were observed for aerosols from local sources such as traffic emissions. The formation of secondary aerosols from gaseous precursors was also observed. Episodes of relatively high concentration of particles in the range of 2-3 μm were probably caused by pollen.

Microphysical processing of aerosol particles in orographic clouds

Science.gov (United States)

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

Directory of Open Access Journals (Sweden)

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

Aerosol generation and filter behaviour in sodium fires. [LMFBR

Energy Technology Data Exchange (ETDEWEB)

Boehm, L; Jordan, S

1975-11-01

In the scope of a long-term program (a) aerosol-formation rates during Na fires, (b) the behavior of Na aerosols in a closed system, and (c) the filtration of Na aerosols were investigated. These experiments in the ABRAUS facility should simulate the behaviour of Na aerosols after an accident in the inner and outer containment of the sodium-cooled fast Reactor SNR 300. At the conditions of the inner-containment (0.7% oxygen content in the atmosphere) aerosol-concentrations by Na - 0/sub 2/ reactions of 1 - 10 g/m/sup 3/ are possible. At the conditions of the outer-containment (21% 0/sub 2/-content) aerosol-concentrations at Na fires of 10 - 50 g/m/sup 3/ have been measured. The aerosol-formation rates are proportional to the 0/sub 2/-concentration: the rate at 21% 0/sub 2/-concentration is about 10-times higher than the rate at 0.7% 0/sub 2/. The aerosol formation rate was determined to 20 kgNa/m/sup 2/h at 21% 0/sub 2/. The behaviour of sand-bed-filters was investigated. A sand-bed-filter arrangement was developed which is better than HEPA-standard of fiberglas-filters concerning efficiency (better than 99.99) and load capacity (about 500 g Na/sub 2/0/sub 2//m/sup 2/). Beyond that sand-bed-filters resist high pressure- and temperature-peaks. Liquid Na aerosols are filtered with an efficiency better than 99.9%. A physical model was evaluated to explain pressure increase at the sand-bed-filter during load and penetration of the filter. The calculated values were in good agreement with experimental results.

Secondary Inorganic Aerosols over an Urban Location in North-Western Himalayan Region: Seasonal Variation in Composition and Formation Process(es)

Science.gov (United States)

Kaushal, D.; Tandon, A.

2017-12-01

Oxidative photo-chemical transformation of precursor gases, mainly of anthropogenic origin, produces secondary aerosols. Secondary inorganic aerosols constitute a significant fraction of total aerosol load over urban locations especially high altitude in wet-temperate climatic set-up. Towns situated in North-Western Himalayan region (NWHR) with sizable population and attractive tourist destinations have been facing ever increasing problem of gaseous and particulate air pollution from exponential increase in vehicular traffic and other anthropogenic emissions. The present study has been planned to investigate the seasonal variations in atmospheric processes responsible for the formation of Secondary Inorganic Aerosols (SIA) and to estimate contribution of SIA to PM­10 load over an Urban location, Dharamshala, in Dhauladhar region of NWHR. Twenty four hourly PM10 aerosol samples were collected, on quartz micro fibre filters in Dharamshala (1350 amsl) on weekly basis for complete one year time-period (February 2015 - January 2016). These samples were analyzed for Water Soluble Inorganic Ions (WSII) using Ion-Chromatographic System. On annual basis, SO42- ions contributed maximum (52%) followed by NO3- (13%) and NH4+ (12%) to WSII. Based upon Principal Component Analysis (PCA), dominant sources contributing to PM10 associated WSII were identified as: Fossil-Fuel and Bio-mass burning, Vehicular (mainly diesel) emissions and gaseous emissions from the microbial degradation of dead bio-mass. Throughout the year, significantly high proportion of SO42- and considerable thermodynamic stability of (NH4)2SO2 at ambient temperatures, made it the major contributor to SIA over NH4NO3 and NH4Cl. On seasonal basis, maximum contribution of SIA to PM10 was observed in monsoon followed by the winter season. Low ambient temperature in winter season favoured formation of NH4NO3 with significant contribution to SIA. It could be concluded that observed variability in the composition and

Toward a combined SAGE II-HALOE aerosol climatology: an evaluation of HALOE version 19 stratospheric aerosol extinction coefficient observations

Directory of Open Access Journals (Sweden)

L. W. Thomason

2012-09-01

Full Text Available Herein, the Halogen Occultation Experiment (HALOE aerosol extinction coefficient data is evaluated in the low aerosol loading period after 1996 as the first necessary step in a process that will eventually allow the production of a combined HALOE/SAGE II (Stratospheric Aerosol and Gas Experiment aerosol climatology of derived aerosol products including surface area density. Based on these analyses, it is demonstrated that HALOE's 3.46 μm is of good quality above 19 km and suitable for scientific applications above that altitude. However, it is increasingly suspect at lower altitudes and should not be used below 17 km under any circumstances after 1996. The 3.40 μm is biased by about 10% throughout the lower stratosphere due to the failure to clear NO₂ but otherwise appears to be a high quality product down to 15 km. The 2.45 and 5.26 μm aerosol extinction coefficient measurements are clearly biased and should not be used for scientific applications after the most intense parts of the Pinatubo period. Many of the issues in the aerosol data appear to be related to either the failure to clear some interfering gas species or doing so poorly. For instance, it is clear that the 3.40 μm aerosol extinction coefficient measurements can be improved through the inclusion of an NO₂ correction and could, in fact, end up as the highest quality overall HALOE aerosol extinction coefficient measurement. It also appears that the 2.45 and 5.26 μm channels may be improved by updating the Upper Atmosphere Pilot Database which is used as a resource for the removal of gas species otherwise not available from direct HALOE measurements. Finally, a simple model to demonstrate the promise of mixed visible/infrared aerosol extinction coefficient ensembles for the retrieval of bulk aerosol properties demonstrates that a combined HALOE/SAGE II aerosol climatology is feasible and may represent a substantial improvement over independently derived

Evaluating MODIS Collection 6 Dark Target Over Water Aerosol Products for Multi-sensor Data Fusion

Science.gov (United States)

Shi, Y.; Zhang, J.; Reid, J. S.; Hyer, E. J.; McHardy, T. M.; Lee, L.

2014-12-01

The Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol products have been widely used in aerosol related climate, visibility, and air quality studies for more than a decade. Recently, the MODIS collection 6 (c6) aerosol products from MODIS-Aqua have been released. The reported changes between Collection 5 and Collection 6 include updates in the retrieving algorithms and a new cloud filtering process for the over-ocean products. Thus it is necessary to fully evaluate the collection 6 products for applications that require high quality MODIS aerosol optical depth data, such as operational aerosol data assimilation. The uncertainties in the MODIS c6 DT over ocean products are studied through both inter-comparing with the Multi-angle Imaging Spectroradiometer (MISR) aerosol products and by evaluation against ground truth. Special attention is given to the low bias in MODIS DT products due to the misclassifications of heavy aerosol plumes as clouds. Finally, a quality assured data assimilation grade aerosol optical product is constructed for aerosol data assimilation related applications.

Time-resolved analysis of primary volatile emissions and secondary aerosol formation potential from a small-scale pellet boiler

Science.gov (United States)

Czech, Hendryk; Pieber, Simone M.; Tiitta, Petri; Sippula, Olli; Kortelainen, Miika; Lamberg, Heikki; Grigonyte, Julija; Streibel, Thorsten; Prévôt, André S. H.; Jokiniemi, Jorma; Zimmermann, Ralf

2017-06-01

Small-scale pellet boilers and stoves became popular as a wood combustion appliance for domestic heating in Europe, North America and Asia due to economic and environmental aspects. Therefore, an increasing contribution of pellet boilers to air pollution is expected despite their general high combustion efficiency. As emissions of primary organic aerosol (POA) and permanent gases of pellet boilers are well investigated, the scope of this study was to investigate the volatile organic emissions and the formation potential of secondary aerosols for this type of appliance. Fresh and aged emissions were analysed by a soot-particle aerosol time-of-flight mass spectrometry (SP-AMS) and the molecular composition of the volatile precursors with single-photon ionisation time-of-flight mass spectrometry (SPI-TOFMS) at different pellet boiler operation conditions. Organic emissions in the gas phase were dominated by unsaturated hydrocarbons while wood-specific VOCs, e.g. phenolic species or substituted furans, were only detected during the starting phase. Furthermore, organic emissions in the gas phase were found to correlate with fuel grade and combustion technology in terms of secondary air supply. Secondary organic aerosols of optimised pellet boiler conditions (OPT, state-of-the-art combustion appliance) and reduced secondary air supply (RSA, used as a proxy for pellet boilers of older type) were studied by simulating atmospheric ageing in a Potential Aerosol Mass (PAM) flow reactor. Different increases in OA mass (55% for OPT, 102% for RSA), associated with higher average carbon oxidation state and O:C, could be observed in a PAM chamber experiment. Finally, it was found that derived SOA yields and emission factors were distinctly lower than reported for log wood stoves.

Diurnally resolved particulate and VOC measurements at a rural site: indication of significant biogenic secondary organic aerosol formation

Science.gov (United States)

Sjostedt, S. J.; Slowik, J. G.; Brook, J. R.; Chang, R. Y.-W.; Mihele, C.; Stroud, C. A.; Vlasenko, A.; Abbatt, J. P. D.

2011-06-01

We report simultaneous measurements of volatile organic compound (VOC) mixing ratios including C6 to C8 aromatics, isoprene, monoterpenes, acetone and organic aerosol mass loadings at a rural location in southwestern Ontario, Canada by Proton-Transfer-Reaction Mass Spectrometry (PTR-MS) and Aerosol Mass Spectrometry (AMS), respectively. During the three-week-long Border Air Quality and Meteorology Study in June-July 2007, air was sampled from a range of sources, including aged air from the polluted US Midwest, direct outflow from Detroit 50 km away, and clean air with higher biogenic input. After normalization to the diurnal profile of CO, a long-lived tracer, diurnal analyses show clear photochemical loss of reactive aromatics and production of oxygenated VOCs and secondary organic aerosol (SOA) during the daytime. Biogenic VOC mixing ratios increase during the daytime in accord with their light- and temperature-dependent sources. Long-lived species, such as hydrocarbon-like organic aerosol and benzene show little to no photochemical reactivity on this timescale. From the normalized diurnal profiles of VOCs, an estimate of OH concentrations during the daytime, measured O3 concentrations, and laboratory SOA yields, we calculate integrated local organic aerosol production amounts associated with each measured SOA precursor. Under the assumption that biogenic precursors are uniformly distributed across the southwestern Ontario location, we conclude that such precursors contribute significantly to the total amount of SOA formation, even during the period of Detroit outflow. The importance of aromatic precursors is more difficult to assess given that their sources are likely to be localized and thus of variable impact at the sampling location.

Hydrolysis of glyoxal in water-restricted environments: formation of organic aerosol precursors through formic acid catalysis.

Science.gov (United States)

Hazra, Montu K; Francisco, Joseph S; Sinha, Amitabha

2014-06-12

The hydrolysis of glyoxal involving one to three water molecules and also in the presence of a water molecule and formic acid has been investigated. Our results show that glyoxal-diol is the major product of the hydrolysis and that formic acid, through its ability to facilitate intermolecular hydrogen atom transfer, is considerably more efficient than water as a catalyst in the hydrolysis process. Additionally, once the glyoxal-diol is formed, the barrier for further hydrolysis to form the glyoxal-tetrol is effectively reduced to zero in the presence of a single water and formic acid molecule. There are two important implications arising from these findings. First, the results suggest that under the catalytic influence of formic acid, glyoxal hydrolysis can impact the growth of atmospheric aerosols. As a result of enhanced hydrogen bonding, mediated through their polar OH functional groups, the diol and tetrol products are expected to have significantly lower vapor pressure than the parent glyoxal molecule; hence they can more readily partition into the particle phase and contribute to the growth of secondary organic aerosols. In addition, our findings provide insight into how glyoxal-diol and glyoxal-tetrol might be formed under atmospheric conditions associated with water-restricted environments and strongly suggest that the formation of these precursors for secondary organic aerosol growth is not likely restricted solely to the bulk aqueous phase as is currently assumed.

Investigation of a Particle into Liquid Sampler to Study the Formation & Ageing of Secondary Organic Aerosol

Science.gov (United States)

Pereira, K. L.; Hamilton, J. F.; Rickard, A. R.; Bloss, W. J.; Alam, M. S.; Camredon, M.; Munoz, A.; Vazquez, M.; Rodenas, M.; Vera, T.; Borrás, E.

2012-12-01

The atmospheric oxidation of Volatile Organic Compounds (VOCs) in the presence of NOx results in the formation of tropospheric ozone and Secondary Organic Aerosol (SOA) [Hallquist et al., 2009]. Whilst SOA is known to affect both climate and human health, the VOC oxidation pathways leading to SOA formation are poorly understood [Solomon et al., 2007]. This is in part due to the vast number and the low concentration of SOA species present in the ambient atmosphere. It has been estimated as many as 10,000 to 100,000 VOCs have been detected in the atmosphere, all of which can undergo photo-chemical oxidation and contribute to SOA formation [Goldstein and Galbally, 2007]. Atmospheric simulation chambers such as the EUropean PHOtoREactor (EUPHORE) in Valencia, Spain, are often used to study SOA formation from a single VOC precursor under controlled conditions. SOA composition and formation can be studied using online techniques such as Aerosol Mass Spectrometry (AMS), which provide high time resolution but limited structural information [Zhang et al., 2007]. Offline techniques, such as collection onto filters, extraction and subsequent analysis, provide detailed SOA composition but only usually one or two samples per experiment. In this work we report time resolved SOA composition analysis using a Particle into Liquid Sampler (PILS) followed by Liquid Chromatography Ion-Trap Mass Spectrometry (LC-IT-MS/MS) and Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FTICR-MS/MS). Experiments were performed at EUPHORE investigating the formation and composition of Methyl Chavicol SOA. Methyl Chavicol (also known as Estragole) was identified as the highest floral emission from an oil palm plantation in Malaysian Borneo and has also been observed in US pine forests [Bouvier-Brown et al., 2009; Misztal et al., 2010]. Previous studies indicate a high SOA yield from Methyl Chavicol at around 40 % [Lee et al., 2006], however currently there have been very few literature

Modelling aerosol behavior in reactor cooling systems

International Nuclear Information System (INIS)

McDonald, B.H.

1990-01-01

This paper presents an overview of some of the areas of concern in using computer codes to model fission-product aerosol behavior in the reactor cooling system (RCS) of a water-cooled nuclear reactor during a loss-of-coolant accident. The basic physical processes that require modelling include: fission product release and aerosol formation in the reactor core, aerosol transport and deposition in the reactor core and throughout the rest of the RCS, and the interaction between aerosol transport processes and the thermalhydraulics. In addition to these basic physical processes, chemical reactions can have a large influence on the nature of the aerosol and its behavior in the RCS. The focus is on the physics and the implications of numerical methods used in the computer codes to model aerosol behavior in the RCS

Lessons Learned In Aerosol Monitoring With The RASA

International Nuclear Information System (INIS)

Forrester, Joel B.; Bowyer, Ted W.; Carty, Fitz; Comes, Laura; Eslinger, Paul W.; Greenwood, Lawrence R.; Haas, Derek A.; Hayes, James C.; Kirkham, Randy R.; Lepel, Elwood A.; Litke, Kevin E.; Miley, Harry S.; Morris, Scott J.; Schrom, Brian T.; Van Davelaar, Peter; Woods, Vincent T.

2011-01-01

The Radionuclide Aerosol Sampler/Analyzer (RASA) is an automated aerosol collection and analysis system designed by Pacific Northwest National Laboratory (PNNL) in the 1990's and is deployed in several locations around the world as part of the International Monitoring System (IMS) required under the Comprehensive Nuclear-Test-Ban Treaty (CTBT). The RASA operates unattended, save for regularly scheduled maintenance, iterating samples through a three-step process on a 24-hour interval. In its 15-year history, much has been learned from the operation and maintenance of the RASA that can benefit engineering updates or future aerosol systems. On 11 March 2011, a 9.0 magnitude earthquake and tsunami rocked the eastern coast of Japan, resulting in power loss and cooling failures at the Daiichi nuclear power plants in Fukushima Prefecture. Aerosol collections were conducted with the RASA in Richland, WA. We present a summary of the lessons learned over the history of the RASA, including lessons taken from the Fukushima incident, regarding the RASA IMS stations operated by the United States.

Variation in aerosol nucleation and growth in coal-fired power plant plumes due to background aerosol, meteorology and emissions: sensitivity analysis and parameterization.

Science.gov (United States)

Stevens, R. G.; Lonsdale, C. L.; Brock, C. A.; Reed, M. K.; Crawford, J. H.; Holloway, J. S.; Ryerson, T. B.; Huey, L. G.; Nowak, J. B.; Pierce, J. R.

2012-04-01

New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulphur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometres and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this presentation, we focus on sub-grid sulphate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. Based on the results of the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM) with online TwO Moment Aerosol Sectional (TOMAS) microphysics, we develop a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within coal-fired power plant plumes based on parameters commonly available in global and regional-scale models. Given large-scale mean meteorological parameters, emissions from the power plant, mean background condensation sink, and the desired distance from the source, the parameterization will predict the fraction of the emitted SO2 that is oxidized to H2SO4, the fraction of that H2SO4 that forms new particles instead of condensing onto preexisting particles, the median diameter of the newly-formed particles, and the number of newly-formed particles per kilogram SO2 emitted. We perform a sensitivity analysis of these characteristics of the aerosol size distribution to the meteorological parameters, the condensation sink, and the emissions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large preexisting aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the

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

Organic molecular composition of marine aerosols over the Arctic Ocean in summer: contributions of primary emission and secondary aerosol formation

Directory of Open Access Journals (Sweden)

P. Q. Fu

2013-02-01

Full Text Available Organic molecular composition of marine aerosol samples collected during the MALINA cruise in the Arctic Ocean was investigated by gas chromatography/mass spectrometry. More than 110 individual organic compounds were determined in the samples and were grouped into different compound classes based on the functionality and sources. The concentrations of total quantified organics ranged from 7.3 to 185 ng m⁻³ (mean 47.6 ng m⁻³, accounting for 1.8–11.0% (4.8% of organic carbon in the marine aerosols. Primary saccharides were found to be dominant organic compound class, followed by secondary organic aerosol (SOA tracers formed from the oxidation of biogenic volatile organic compounds (VOCs such as isoprene, α-pinene and β-caryophyllene. Mannitol, the specific tracer for airborne fungal spores, was detected as the most abundant organic species in the samples with a concentration range of 0.052–53.3 ng m⁻³ (9.2 ng m⁻³, followed by glucose, arabitol, and the isoprene oxidation products of 2-methyltetrols. Biomass burning tracers such as levoglucosan are evident in all samples with trace levels. On the basis of the tracer-based method for the estimation of fungal-spore OC and biogenic secondary organic carbon (SOC, we estimate that an average of 10.7% (up to 26.2% of the OC in the marine aerosols was due to the contribution of fungal spores, followed by the contribution of isoprene SOC (mean 3.8% and α-pinene SOC (2.9%. In contrast, only 0.19% of the OC was due to the photooxidation of β-caryophyllene. This study indicates that primary organic aerosols from biogenic emissions, both from long-range transport of mid-latitude aerosols and from sea-to-air emission of marine organics, as well as secondary organic aerosols formed from the photooxidation of biogenic VOCs are important factors controlling the organic chemical composition of marine aerosols in the Arctic Ocean.

How important is organic aerosol hygroscopicity to aerosol indirect forcing?

International Nuclear Information System (INIS)

Liu Xiaohong; Wang Jian

2010-01-01

Organics are among the most abundant aerosol components in the atmosphere. However, there are still large uncertainties with emissions of primary organic aerosol (POA) and volatile organic compounds (VOCs) (precursor gases of secondary organic aerosol, SOA), formation of SOA, and chemical and physical properties (e.g., hygroscopicity) of POA and SOA. All these may have significant impacts on aerosol direct and indirect forcing estimated from global models. In this study a modal aerosol module (MAM) in the NCAR community atmospheric model (CAM) is used to examine sensitivities of aerosol indirect forcing to hygroscopicity (represented by a single parameter 'κ' ) of POA and SOA. Our model simulation indicates that in the present-day (PD) condition changing the 'κ' value of POA from 0 to 0.1 increases the number concentration of cloud condensational nuclei (CCN) at supersaturation S = 0.1% by 40-80% over the POA source regions, while changing the 'κ' value of SOA by ± 50% (from 0.14 to 0.07 and 0.21) changes the CCN concentration within 40%. There are disproportionally larger changes in CCN concentration in the pre-industrial (PI) condition. Due to the stronger impact of organics hygroscopicity on CCN and cloud droplet number concentration at PI condition, global annual mean anthropogenic aerosol indirect forcing (AIF) between PD and PI conditions reduces with the increase of the hygroscopicity of organics. Global annual mean AIF varies by 0.4 W m -2 in the sensitivity runs with the control run of - 1.3 W m -2 , highlighting the need for improved understanding of organics hygroscopicity and its representation in global models.

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

Aerosol number size distribution and new particle formation at a rural/coastal site in Pearl River Delta (PRD) of China

Science.gov (United States)

Liu, Shang; Hu, Min; Wu, Zhijun; Wehner, Birgit; Wiedensohler, Alfred; Cheng, Yafang

Continuous measurements of aerosol number size distribution in the range of 3 nm-10 μm were performed in Pearl River Delta (PRD), China. These measurements were made during the period of 3 October to 5 November in 2004 at rural/coastal site, Xinken (22°37'N, 113°35'E, 6 m above sea level), in the south suburb of Guangzhou City (22°37'N, 113°35'E, 6 m above sea level), using a Twin Differential Mobility Particle Sizer (TDMPS) combined with an Aerodynamic Particle Sizer (APS). The aerosol particles at Xinken were divided into four groups according to the observation results: nucleation mode particles (3-30 nm), Aitken mode particles (30-130 nm), accumulation mode particles (130-1000 nm) and coarse mode particles (1-10 μm). Concentrations of nucleation mode, Aitken mode and accumulation mode particles were observed in the same order of magnitude (about 10,000 cm -3), among which the concentration of Aitken mode particle was the highest. The Aitken mode particles usually had two peaks: the morning peak may be caused by the land-sea circulation, which is proven to be important for transporting aged aerosols back to the sampling site, while the noon peak was ascribed to the condensational growth of new particles. New particle formation events were found on 7 days of 27 days, the new particle growth rates ranged from 2.2 to 19.8 nm h -1 and the formation rates ranged from 0.5 to 5.2 cm -3 s -1, both of them were in the range of typical observed formation rates (0.01-10 cm -3 s -1) and typical particle growth rates (1-20 nm h -1). The sustained growth of the new particles for several hours under steady northeast wind indicated that the new particle formation events may occur in a large homogeneous air mass.

Carbonaceous Aerosol Characterization during 2016 KOR-US 2016

Science.gov (United States)

Rodriguez, B.; Santos, G. M.; Sanchez, D.; Jeong, D.; Czimczik, C. I.; Kim, S.

2017-12-01

Atmospheric carbonaceous aerosols are a major component of fine particulate matter and assume important roles in Earth's climate and human health. Because atmospheric carbonaceous aerosols exist as a continuum ranging from small, light-scattering organic carbon (OC), to highly-condensed, light-absorbing elemental carbon (EC) they have contrasting effects on interaction with incoming and outgoing radiation, cloud formation, and snow/ice albedo. By strengthening our understanding of the relative contribution and sources of OC and EC we will be able to further describe aerosol formation and mixing at the regional level. To understand the relative anthropogenic and biogenic contributions to carbonaceous aerosol, 12 PM10 aerosols samples were collected on quartz fiber filters at the Mt. Taewha Research Forest in South Korea during the KORUS-AQ 2016 campaign over periods of 24-48 hours with a high-volume air sampler. Analysis of bulk C and N concentrations and absorption properties of filter extracts interspersed with HYSPLIT model results indicated that continental outflow across the Yellow Sea in enriched in bulk nitrogen loading and enhanced bulk absorptive properties of the aerosols. Bulk radiocarbon analysis also indicated enriched values in all samples indicating contamination from a nuclear power plant or the combustion of biomedical waste nearby. Here, we aim to investigate further the chemical characterization of VOCs adsorbed unto the aerosol through TD-GC-TOFMS. With this dataset we aim to determine the relative contribution of anthropogenic and biogenic aerosols by utilizing specific chemical tracers for source apportionment.

Comparison of secondary organic aerosol formation from toluene on initially wet and dry ammonium sulfate particles at moderate relative humidity

Science.gov (United States)

Liu, Tengyu; Huang, Dan Dan; Li, Zijun; Liu, Qianyun; Chan, ManNin; Chan, Chak K.

2018-04-01

The formation of secondary organic aerosol (SOA) has been widely studied in the presence of dry seed particles at low relative humidity (RH). At higher RH, initially dry seed particles can exist as wet particles due to water uptake by the seeds as well as the SOA. Here, we investigated the formation of SOA from the photooxidation of toluene using an oxidation flow reactor in the absence of NOx under a range of OH exposures on initially wet or dry ammonium sulfate (AS) seed particles at an RH of 68 %. The ratio of the SOA yield on wet AS seeds to that on dry AS seeds, the relative SOA yield, decreased from 1.31 ± 0.02 at an OH exposure of 4.66 × 1010 molecules cm-3 s to 1.01 ± 0.01 at an OH exposure of 5.28 × 1011 molecules cm-3 s. This decrease may be due to the early deliquescence of initially dry AS seeds after being coated by highly oxidized toluene-derived SOA. SOA formation lowered the deliquescence RH of AS and resulted in the uptake of water by both AS and SOA. Hence the initially dry AS seeds contained aerosol liquid water (ALW) soon after SOA formed, and the SOA yield and ALW approached those of the initially wet AS seeds as OH exposure and ALW increased, especially at high OH exposure. However, a higher oxidation state of the SOA on initially wet AS seeds than that on dry AS seeds was observed at all levels of OH exposure. The difference in mass fractions of m / z 29, 43 and 44 of SOA mass spectra, obtained using an aerosol mass spectrometer (AMS), indicated that SOA formed on initially wet seeds may be enriched in earlier-generation products containing carbonyl functional groups at low OH exposures and later-generation products containing acidic functional groups at high exposures. Our results suggest that inorganic dry seeds become at least partially deliquesced particles during SOA formation and hence that ALW is inevitably involved in the SOA formation at moderate RH. More laboratory experiments conducted with a wide variety of SOA precursors

Aerosol studies during the ESCOMPTE experiment: an overview

Science.gov (United States)

Cachier, Hélène; Aulagnier, Fabien; Sarda, Roland; Gautier, François; Masclet, Pierre; Besombes, Jean-Luc; Marchand, Nicolas; Despiau, Serge; Croci, Delphine; Mallet, Marc; Laj, Paolo; Marinoni, Angela; Deveau, Pierre-Alexandre; Roger, Jean-Claude; Putaud, Jean-Philippe; Van Dingenen, Rita; Dell'Acqua, Alessandro; Viidanoja, Jyrkki; Martins-Dos Santos, Sebastiao; Liousse, Cathy; Cousin, Frédéric; Rosset, Robert; Gardrat, Eric; Galy-Lacaux, Corinne

2005-03-01

The "Expérience sur Site pour COntraindre les Modèles de Pollution atmosphérique et de Transport d'Emissions" (ESCOMPTE) experiment took place in the Southern part of France in the Marseilles/Fos-Berre region during 6 weeks in June and July 2001. One task was to document the regional sources of atmospheric particles and to gain some insight into the aerosol transformations in the atmosphere. For this purpose, seven sites were chosen and equipped with the same basic instrumentation to obtain the chemical closure of the bulk aerosol phase and size-segregated samples. Some specific additional experiments were conducted for the speciation of the organic matter and the aerosol size distribution in number. Finally, four multiwavelength sun-photometers were also deployed during the experiment. Interestingly, in this region, three intense aerosol sources (urban, industrial and biogenic) are very active, and data show consistent results, enlightening an important background of particles over the whole ESCOMPTE domain. Notable is the overwhelming importance of the carbonaceous fraction (comprising primary and secondary particles), which is always more abundant than sulphates. Particle size studies show that, on average, more than 90% of the mean regional aerosol number is found on a size range smaller than 300 nm in diameter. The most original result is the evidence of the rapid formation of secondary aerosols occurring in the whole ESCOMPTE domain. This formation is much more important than that usually observed at these latitudes since two thirds of the particulate mass collected off source zones is estimated to be generated during atmospheric transport. On the other hand, the marine source has poor influence in the region, especially during the overlapping pollution events of Intensive Observation Periods (IOP). Preliminary results from the 0D and 3D versions of the MesoNH-aerosol model show that, with optimised gas and particle sources, the model accounts

Toward a Combined SAGE II-HALOE Aerosol Climatology: An Evaluation of HALOE Version 19 Stratospheric Aerosol Extinction Coefficient Observations

Science.gov (United States)

Thomason, L. W.

2012-01-01

Herein, the Halogen Occultation Experiment (HALOE) aerosol extinction coefficient data is evaluated in the low aerosol loading period after 1996 as the first necessary step in a process that will eventually allow the production of a combined HALOE/SAGE II (Stratospheric Aerosol and Gas Experiment) aerosol climatology of derived aerosol products including surface area density. Based on these analyses, it is demonstrated that HALOE's 3.46 microns is of good quality above 19 km and suitable for scientific applications above that altitude. However, it is increasingly suspect at lower altitudes and should not be used below 17 km under any circumstances after 1996. The 3.40 microns is biased by about 10% throughout the lower stratosphere due to the failure to clear NO2 but otherwise appears to be a high quality product down to 15 km. The 2.45 and 5.26 micron aerosol extinction coefficient measurements are clearly biased and should not be used for scientific applications after the most intense parts of the Pinatubo period. Many of the issues in the aerosol data appear to be related to either the failure to clear some interfering gas species or doing so poorly. For instance, it is clear that the 3.40micronaerosol extinction coefficient measurements can be improved through the inclusion of an NO2 correction and could, in fact, end up as the highest quality overall HALOE aerosol extinction coefficient measurement. It also appears that the 2.45 and 5.26 micron channels may be improved by updating the Upper Atmosphere Pilot Database which is used as a resource for the removal of gas species otherwise not available from direct HALOE measurements. Finally, a simple model to demonstrate the promise of mixed visible/infrared aerosol extinction coefficient ensembles for the retrieval of bulk aerosol properties demonstrates that a combined HALOE/SAGE II aerosol climatology is feasible and may represent a substantial improvement over independently derived data sets.

Aerosol Observability and Predictability: From Research to Operations for Chemical Weather Forecasting. Lagrangian Displacement Ensembles for Aerosol Data Assimilation

Science.gov (United States)

da Silva, Arlindo

2010-01-01

A challenge common to many constituent data assimilation applications is the fact that one observes a much smaller fraction of the phase space that one wishes to estimate. For example, remotely sensed estimates of the column average concentrations are available, while one is faced with the problem of estimating 3D concentrations for initializing a prognostic model. This problem is exacerbated in the case of aerosols because the observable Aerosol Optical Depth (AOD) is not only a column integrated quantity, but it also sums over a large number of species (dust, sea-salt, carbonaceous and sulfate aerosols. An aerosol transport model when driven by high-resolution, state-of-the-art analysis of meteorological fields and realistic emissions can produce skillful forecasts even when no aerosol data is assimilated. The main task of aerosol data assimilation is to address the bias arising from inaccurate emissions, and Lagrangian misplacement of plumes induced by errors in the driving meteorological fields. As long as one decouples the meteorological and aerosol assimilation as we do here, the classic baroclinic growth of error is no longer the main order of business. We will describe an aerosol data assimilation scheme in which the analysis update step is conducted in observation space, using an adaptive maximum-likelihood scheme for estimating background errors in AOD space. This scheme includes e explicit sequential bias estimation as in Dee and da Silva. Unlikely existing aerosol data assimilation schemes we do not obtain analysis increments of the 3D concentrations by scaling the background profiles. Instead we explore the Lagrangian characteristics of the problem for generating local displacement ensembles. These high-resolution state-dependent ensembles are then used to parameterize the background errors and generate 3D aerosol increments. The algorithm has computational complexity running at a resolution of 1/4 degree, globally. We will present the result of

Secondary Inorganic Soluble Aerosol in Hong Kong: Continuous Measurements, Formation Mechanism Discussion and Improvement of an Observation-Based Model to Study Control Strategies

Science.gov (United States)

Xue, Jian

Work in this thesis focuses on half-hourly or hourly measurements of PM2.5 secondary inorganic aerosols (SIA) in two locations in Hong Kong (HK) using a continuous system, PILS (Particle-into-Liquid System) coupled to two ion chromatographs. The high-resolution data sets allow the examination of SIA temporal dynamics in the scale of hours that the filter-based approach is incapable of providing. (1) Impacts of local emissions, regional transports and their interactions on chemical composition and concentrations of PM2.5 SIA and other ionic species were investigated at the Hong Kong University of Science and Technology (HKUST), a receptor site, under three synoptic conditions. (2) Chemical compositions and size characteristics of ionic species were investigated at Tung Chung, a new town area located in the Southwest part of HK. The sampling period was from 17 to 26 December 2009, covering both normal conditions and an aerosol episode. The three major secondary inorganic ions, SO42, NH4+ and NO 3-, accounted for 47 +/- 6% of PM2.5 mass. Further examination of size characteristics of NO3 - shows that fine mode NO3- is more likely to occur in environments when the fine particles are less acidic and the sea-salt aerosol contributions are low. (3) The ionic chemical composition of PM2.5 and meteorological parameters (e.g., temperature, RH) obtained at the HKUST site under all three different synoptic conditions are input into Aerosol Inorganic Model (AIM-III) for estimation of in situ pH through calculation of H+ amount and aerosol liquid water content (LWC). The second part of this thesis work is to improve an observation-based model (OBAMAP) for SIA, which was first developed by Dr. Zibing Yuan (2006) to evaluate the sensitivity of formation of nitrate ad sulfate to changes in the emissions of their precursors (i.e., NOx, SO2, and VOCs). The improvement work includes incorporating updated chemical mechanisms, thermodynamic equilibrium for gas-aerosol phase

Laboratory studies of monoterpene secondary organic aerosol formation and evolution

Science.gov (United States)

Thornton, J. A.; D'Ambro, E.; Zhao, Y.; Lee, B. H.; Pye, H. O. T.; Schobesberger, S.; Shilling, J.; Liu, J.

2017-12-01

We have conducted a series of chamber experiments to study the molecular composition and properties of secondary organic aerosol (SOA) formed from monoterpenes under a range of photochemical and dark conditions. We connect variations in the SOA mass yield to molecular composition and volatility, and use a detailed Master Chemical Mechanism (MCM) based chemical box model with dynamic gas-particle partitioning to examine the importance of various peroxy radical reaction mechanisms in setting the SOA yield and properties. We compare the volatility distribution predicted by the model to that inferred from isothermal room-temperature evaporation experiments using the FIGAERO-CIMS where SOA particles collected on a filter are allowed to evaporate under humidified pure nitrogen flow stream for up to 24 hours. We show that the combination of results requires prompt formation of low volatility SOA from predominantly gas-phase mechanisms, with important differences between monoterpenes (alpha-Pinene and delta-3-Carene) followed by slower non-radical particle phase chemistry that modulates both the chemical and physical properties of the SOA. Implications for the regional evolution of atmospheric monoterpene SOA are also discussed.

Fog-induced variations in aerosol optical and physical properties over the Indo-Gangetic Basin and impact to aerosol radiative forcing

Directory of Open Access Journals (Sweden)

S. K. Das

2008-06-01

Full Text Available A detailed study on the changes in aerosol physical and optical properties during fog events were made in December 2004 at Hissar (29.13° N, 75.70° E, a city located in the Indo-Gangetic basin. The visible aerosol optical depth was relatively low (0.3 during the initial days, which, however, increased (0.86 as the month progressed. The increasing aerosol amount, the decreasing surface temperature and a higher relative humidity condition were found favoring the formation of fog. The fog event is also found to alter the aerosol size distribution. An increase in the number concentration of the nucleation mode (radius<0.1 μm particles, along with a decrease in the mode radius showed the formation of freshly nucleated aerosols. In the case of accumulation mode (0.1 μmaerosol optical depth spectra are model fitted to infer the aerosol components which are further used to compute the aerosol radiative forcing. The top of the atmosphere forcing is found to increase during foggy days due to large backscattering of radiation back to space. It is also shown that during foggy days, as the day progresses the RH value decreases, which reduces the forcing value while the increasing solar elevation increases the forcing value. Thus the fog event which prolongs longer into the daytime has a stronger effect on the diurnally averaged aerosol radiative forcing than those events which are confined only to the early morning hours.

Fog-induced variations in aerosol optical and physical properties over the Indo-Gangetic Basin and impact to aerosol radiative forcing

Energy Technology Data Exchange (ETDEWEB)

Das, S.K.; Misra, A. [Physical Research Lab., Ahmedabad (India); Jayaraman, A. [National Atmospheric Research Lab., Gadanki (India)

2008-07-01

A detailed study on the changes in aerosol physical and optical properties during fog events were made in December 2004 at Hissar (29.13 N, 75.70 E), a city located in the Indo-Gangetic basin. The visible aerosol optical depth was relatively low (0.3) during the initial days, which, however, increased (0.86) as the month progressed. The increasing aerosol amount, the decreasing surface temperature and a higher relative humidity condition were found favoring the formation of fog. The fog event is also found to alter the aerosol size distribution. An increase in the number concentration of the nucleation mode (radius<0.1 {mu}m) particles, along with a decrease in the mode radius showed the formation of freshly nucleated aerosols. In the case of accumulation mode (0.1 {mu}maerosol optical depth spectra are model fitted to infer the aerosol components which are further used to compute the aerosol radiative forcing. The top of the atmosphere forcing is found to increase during foggy days due to large backscattering of radiation back to space. It is also shown that during foggy days, as the day progresses the RH value decreases, which reduces the forcing value while the increasing solar elevation increases the forcing value. Thus the fog event which prolongs longer into the daytime has a stronger effect on the diurnally averaged aerosol radiative forcing than those events which are confined only to the early morning hours. (orig.)

Constraining Aerosol-Cloud-Precipitation Interactions of Orographic Mixed-Phase Clouds with Trajectory Budgets

Science.gov (United States)

Glassmeier, F.; Lohmann, U.

2016-12-01

Orographic precipitation is prone to strong aerosol-cloud-precipitation interactions because the time for precipitation development is limited to the ascending section of mountain flow. At the same time, cloud microphysical development is constraint by the strong dynamical forcing of the orography. In this contribution, we discuss how changes in the amount and composition of droplet- and ice-forming aerosols influence precipitation in idealized simulations of stratiform orographic mixed-phase clouds. We find that aerosol perturbations trigger compensating responses of different precipitation formation pathways. The effect of aerosols is thus buffered. We explain this buffering by the requirement to fulfill aerosol-independent dynamical constraints. For our simulations, we use the regional atmospheric model COSMO-ART-M7 in a 2D setup with a bell-shaped mountain. The model is coupled to a 2-moment warm and cold cloud microphysics scheme. Activation and freezing rates are parameterized based on prescribed aerosol fields that are varied in number, size and composition. Our analysis is based on the budget of droplet water along trajectories of cloud parcels. The budget equates condensation as source term with precipitation formation from autoconversion, accretion, riming and the Wegener-Bergeron-Findeisen process as sink terms. Condensation, and consequently precipitation formation, is determined by dynamics and largely independent of the aerosol conditions. An aerosol-induced change in the number of droplets or crystals perturbs the droplet budget by affecting precipitation formation processes. We observe that this perturbation triggers adjustments in liquid and ice water content that re-equilibrate the budget. As an example, an increase in crystal number triggers a stronger glaciation of the cloud and redistributes precipitation formation from collision-coalescence to riming and from riming to vapor deposition. We theoretically confirm the dominant effect of water

Relative importance of nitrate and sulfate aerosol production mechanisms in urban atmospheres

International Nuclear Information System (INIS)

Middleton, P.; Kiang, C.S.

1979-01-01

The relative importance of the various sulfate and nitrate aerosol production mechanisms is calculated for different atmospheric conditions. The calculation scheme used to determine the rates of nitrate and sulfate production, based on the concept that vapor transfer to the aerosols and nitrate and sulfate formation within the aerosols are coupled kinetic processes, considers sulfate formation by ozone and hydrogen peroxide oxidation and catalytic oxidation in the presence of soot, iron and manganese of sulfite solutions and sulfuric acid condensation and nitrate formation by the liquid-phase oxidation of dissolved nitrogen oxides for different initial gas concentrations and particle compositions and sizes. It is found that sulfate production is higher under daytime conditions, primarily proceeding by mechanisms involving sulfuric acid and hydrogen peroxide, while at night oxidation processes on the surface of the aerosol film are more important. Nitrate tends to decrease nighttime sulfate production due to an increase in aerosol acidity and nitrate production is found to be higher under nighttime conditions and in the winter

Laboratory Experiments and Modeling for Interpreting Field Studies of Secondary Organic Aerosol Formation Using an Oxidation Flow Reactor

Energy Technology Data Exchange (ETDEWEB)

Jimenez, Jose-Luis [Univ. of Colorado, Boulder, CO (United States)

2016-02-01

This grant was originally funded for deployment of a suite of aerosol instrumentation by our group in collaboration with other research groups and DOE/ARM to the Ganges Valley in India (GVAX) to study aerosols sources and processing. Much of the first year of this grant was focused on preparations for GVAX. That campaign was cancelled due to political reasons and with the consultation with our program manager, the research of this grant was refocused to study the applications of oxidation flow reactors (OFRs) for investigating secondary organic aerosol (SOA) formation and organic aerosol (OA) processing in the field and laboratory through a series of laboratory and modeling studies. We developed a gas-phase photochemical model of an OFR which was used to 1) explore the sensitivities of key output variables (e.g., OH exposure, O₃, HO₂/OH) to controlling factors (e.g., water vapor, external reactivity, UV irradiation), 2) develop simplified OH exposure estimation equations, 3) investigate under what conditions non-OH chemistry may be important, and 4) help guide design of future experiments to avoid conditions with undesired chemistry for a wide range of conditions applicable to the ambient, laboratory, and source studies. Uncertainties in the model were quantified and modeled OH exposure was compared to tracer decay measurements of OH exposure in the lab and field. Laboratory studies using OFRs were conducted to explore aerosol yields and composition from anthropogenic and biogenic VOC as well as crude oil evaporates. Various aspects of the modeling and laboratory results and tools were applied to interpretation of ambient and source measurements using OFR. Additionally, novel measurement methods were used to study gas/particle partitioning. The research conducted was highly successful and details of the key results are summarized in this report through narrative text, figures, and a complete list of publications acknowledging this grant.

AEROSOL VARIABILITY OBSERVED WITH RPAS

Directory of Open Access Journals (Sweden)

B. Altstädter

2013-08-01

Full Text Available To observe the origin, vertical and horizontal distribution and variability of aerosol particles, and especially ultrafine particles recently formed, we plan to employ the remotely piloted aircraft system (RPAS Carolo-P360 "ALADINA" of TU Braunschweig. The goal of the presented project is to investigate the vertical and horizontal distribution, transport and small-scale variability of aerosol particles in the atmospheric boundary layer using RPAS. Two additional RPAS of type MASC of Tübingen University equipped with turbulence instrumentation add the opportunity to study the interaction of the aerosol concentration with turbulent transport and exchange processes of the surface and the atmosphere. The combination of different flight patterns of the three RPAS allows new insights in atmospheric boundary layer processes. Currently, the different aerosol sensors are miniaturized at the Leibniz Institute for Tropospheric Research, Leipzig and together with the TU Braunschweig adapted to fit into the RPAS. Moreover, an additional meteorological payload for measuring temperature, humidity and turbulence properties is constructed by Tübingen University. Two condensation particle counters determine the total aerosol number with a different lower detection threshold in order to investigate the horizontal and vertical aerosol variability and new particle formation (aerosol particles of some nm diameter. Further the aerosol size distribution in the range from about 0.300 to ~5 μm is given by an optical particle counter.

Chemical and microphysical properties of the aerosol during foggy and nonfoggy episodes: a relationship between organic and inorganic content of the aerosol

Science.gov (United States)

Kaul, D. S.; Gupta, T.; Tripathi, S. N.

2012-06-01

An extensive field measurement during winter was carried out at a site located in the Indo-Gangetic Plain (IGP) which gets heavily influenced by the fog during winter almost every year. The chemical and microphysical properties of the aerosols during foggy and nonfoggy episodes and chemical composition of the fogwater are presented. Positive matrix factorization (PMF) as a tool for the source apportionment was employed to understand the sources of pollution. Four major sources viz. biomass burning, refractory, secondary and mineral dust were identified. Aerosols properties during foggy episodes were heavily influenced by almost all the sources and they caused considerable loading of almost all the organic and inorganic species during the period. The biomass generated aerosols were removed from the atmosphere by scavenging during foggy episodes. The wet removal of almost all the species by the fog droplets was observed. The K+, water soluble organic carbon (WSOC), water soluble inorganic carbon (WSIC) and NO3- were most heavily scavenged among the species and their concentrations consequently became lower than the nonfoggy episode concentrations. The production of secondary inorganic aerosol, mainly sulfate and ammonium, during foggy episodes was considerably higher than nitrate which was rather heavily scavenged and removed by the fog droplets. The fogwater analysis showed that dissolved inorganic species play a vital role in processing of organic carbon such as the formation of organo-sulfate and organo-nitrate inside the fog droplets. The formation of organo-sulfate and organo-nitrate in aerosol and the influence of acidity on the secondary organic aerosol (SOA) formation were rather found to be negligible. The study average inorganic component of the aerosol was considerably higher than the carbonaceous component during both foggy and nonfoggy episode. The secondary production of the aerosol changed the microphysical properties of aerosol which was reflected by

Formation of secondary inorganic aerosols by power plant emissions exhausted through cooling towers in Saxony.

Science.gov (United States)

Hinneburg, Detlef; Renner, Eberhard; Wolke, Ralf

2009-01-01

The fraction of ambient PM10 that is due to the formation of secondary inorganic particulate sulfate and nitrate from the emissions of two large, brown-coal-fired power stations in Saxony (East Germany) is examined. The power stations are equipped with natural-draft cooling towers. The flue gases are directly piped into the cooling towers, thereby receiving an additionally intensified uplift. The exhausted gas-steam mixture contains the gases CO, CO2, NO, NO2, and SO2, the directly emitted primary particles, and additionally, an excess of 'free' sulfate ions in water solution, which, after the desulfurization steps, remain non-neutralized by cations. The precursor gases NO2 and SO2 are capable of forming nitric and sulfuric acid by several pathways. The acids can be neutralized by ammonia and generate secondary particulate matter by heterogeneous condensation on preexisting particles. The simulations are performed by a nested and multi-scale application of the online-coupled model system LM-MUSCAT. The Local Model (LM; recently renamed as COSMO) of the German Weather Service performs the meteorological processes, while the Multi-scale Atmospheric Transport Model (MUSCAT) includes the transport, the gas phase chemistry, as well as the aerosol chemistry (thermodynamic ammonium-sulfate-nitrate-water system). The highest horizontal resolution in the inner region of Saxony is 0.7 km. One summer and one winter episode, each realizing 5 weeks of the year 2002, are simulated twice, with the cooling tower emissions switched on and off, respectively. This procedure serves to identify the direct and indirect influences of the single plumes on the formation and distribution of the secondary inorganic aerosols. Surface traces of the individual tower plumes can be located and distinguished, especially in the well-mixed boundary layer in daytime. At night, the plumes are decoupled from the surface. In no case does the resulting contribution of the cooling tower emissions to PM10

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.

Sodium aerosol formation in an argon flow over hot sodium

International Nuclear Information System (INIS)

Clement, C.F.; Dolias, M.J.; UKAEA Atomic Energy Research Establishment, Harwell. Thermal Hydraulics Div.)

1987-01-01

Vapour evaporation, which partly forms aerosol, occurs when a cold gas flows over a hot liquid. A previous well-mixed model is extended to predict the final vapour plus aerosol content of such a flow in terms of its initial and final temperatures. The predictions are compared to results of the Copacabana II experiment in which argon passed over a sodium pool. Agreement is obtained for the final sodium density at moderate flow rates, and physical reasons are given as to why deviations occur at low and high flow rates. (author)

Improvement of Representation of the Cloud-Aerosol Interaction in Large-Scale Models

Energy Technology Data Exchange (ETDEWEB)

Khain, Alexander [Hebrew Univ. of Jerusalem (Israel); Phillips, Vaughan [Lund Univ. (Sweden); Pinsky, Mark [Hebrew Univ. of Jerusalem (Israel); Lynn, Barry [Hebrew Univ. of Jerusalem (Israel)

2016-12-20

The main achievements reached under the DOE award DE-SC0006788 are described. It is shown that the plan of the Project is completed. Unique results concerning cloud-aerosol interaction are obtained. It is shown that aerosols affect intensity of hurricanes. The effects of small aerosols on formation of ice in anvils of deep convective clouds are discovered, for the first time the mechanisms of drizzle formation are found and described quantitatively. Mechanisms of formation of warm rain are clarified and the dominating role of adiabatic processes and turbulence are stressed. Important results concerning the effects of sea spray on intensity of clouds and tropical cyclones are obtained. A novel methods of calculation of hail formation has been developed and implemented.

The Collection 6 'dark-target' MODIS Aerosol Products

Science.gov (United States)

Levy, Robert C.; Mattoo, Shana; Munchak, Leigh A.; Kleidman, Richard G.; Patadia, Falguni; Gupta, Pawan; Remer, Lorraine

2013-01-01

Aerosol retrieval algorithms are applied to Moderate resolution Imaging Spectroradiometer (MODIS) sensors on both Terra and Aqua, creating two streams of decade-plus aerosol information. Products of aerosol optical depth (AOD) and aerosol size are used for many applications, but the primary concern is that these global products are comprehensive and consistent enough for use in climate studies. One of our major customers is the international modeling comparison study known as AEROCOM, which relies on the MODIS data as a benchmark. In order to keep up with the needs of AEROCOM and other MODIS data users, while utilizing new science and tools, we have improved the algorithms and products. The code, and the associated products, will be known as Collection 6 (C6). While not a major overhaul from the previous Collection 5 (C5) version, there are enough changes that there are significant impacts to the products and their interpretation. In its entirety, the C6 algorithm is comprised of three sub-algorithms for retrieving aerosol properties over different surfaces: These include the dark-target DT algorithms to retrieve over (1) ocean and (2) vegetated-dark-soiled land, plus the (3) Deep Blue (DB) algorithm, originally developed to retrieve over desert-arid land. Focusing on the two DT algorithms, we have updated assumptions for central wavelengths, Rayleigh optical depths and gas (H2O, O3, CO2, etc.) absorption corrections, while relaxing the solar zenith angle limit (up to 84) to increase pole-ward coverage. For DT-land, we have updated the cloud mask to allow heavy smoke retrievals, fine-tuned the assignments for aerosol type as function of season location, corrected bugs in the Quality Assurance (QA) logic, and added diagnostic parameters such as topographic altitude. For DT-ocean, improvements include a revised cloud mask for thin-cirrus detection, inclusion of wind speed dependence in the retrieval, updates to logic of QA Confidence flag (QAC) assignment, and

Quantification of Release of Critical Elements, Formation of Fly Ash and Aerosols: Status on Current Understanding and Research Needs

DEFF Research Database (Denmark)

Jappe Frandsen, Flemming

2017-01-01

Deposit formation in utility boilers occurs via a number of consecutive steps; 1) release of critical elements like K, Na, Pb, Zn, S and Cl, 2) formation of gaseous species, fly ash and aerosols, 3) transport and adhesion of ash species, 4) deposit build-up and consolidation, and, finally, 5...... formation (slagging and fouling) on superheater tubes, leading to a potential reduction in heat transfer efficiency to the water/steam cycle, or, to chemical attack (corrosion) or physical wear (erosion) of superheater tubes. These problems may give rise to irregular operation, or even costly shutdowns...... of combustion units.Through several years, high quality research has been conducted on characterization of fuels, ashes and deposit formation in utility boilers fired with coal, biomass and waste fractions. Huge amounts of experimental data have been reported, from such work, but the fact...

Inhalation drug delivery devices: technology update

Directory of Open Access Journals (Sweden)

Ibrahim M

2015-02-01

Full Text Available Mariam Ibrahim, Rahul Verma, Lucila Garcia-ContrerasDepartment of Pharmaceutical Sciences, College of Pharmacy, The University of Oklahoma Health Sciences Center, Oklahoma City, OK, USAAbstract: The pulmonary route of administration has proven to be effective in local and systemic delivery of miscellaneous drugs and biopharmaceuticals to treat pulmonary and non-pulmonary diseases. A successful pulmonary administration requires a harmonic interaction between the drug formulation, the inhaler device, and the patient. However, the biggest single problem that accounts for the lack of desired effect or adverse outcomes is the incorrect use of the device due to lack of training in how to use the device or how to coordinate actuation and aerosol inhalation. This review summarizes the structural and mechanical features of aerosol delivery devices with respect to mechanisms of aerosol generation, their use with different formulations, and their advantages and limitations. A technological update of the current state-of-the-art designs proposed to overcome current challenges of existing devices is also provided.Keywords: pulmonary delivery, asthma, nebulizers, metered dose inhaler, dry powder inhaler

Secondary organic aerosol formation by limonene ozonolysis: Parameterizing multi-generational chemistry in ozone- and residence time-limited indoor environments

Science.gov (United States)

Waring, Michael S.

2016-11-01

Terpene ozonolysis reactions can be a strong source of secondary organic aerosol (SOA) indoors. SOA formation can be parameterized and predicted using the aerosol mass fraction (AMF), also known as the SOA yield, which quantifies the mass ratio of generated SOA to oxidized terpene. Limonene is a monoterpene that is at sufficient concentrations such that it reacts meaningfully with ozone indoors. It has two unsaturated bonds, and the magnitude of the limonene ozonolysis AMF varies by a factor of ∼4 depending on whether one or both of its unsaturated bonds are ozonated, which depends on whether ozone is in excess compared to limonene as well as the available time for reactions indoors. Hence, this study developed a framework to predict the limonene AMF as a function of the ozone [O3] and limonene [lim] concentrations and the air exchange rate (AER, h-1), which is the inverse of the residence time. Empirical AMF data were used to calculate a mixing coefficient, β, that would yield a 'resultant AMF' as the combination of the AMFs due to ozonolysis of one or both of limonene's unsaturated bonds, within the volatility basis set (VBS) organic aerosol framework. Then, β was regressed against predictors of log10([O3]/[lim]) and AER (R2 = 0.74). The β increased as the log10([O3]/[lim]) increased and as AER decreased, having the physical meaning of driving the resultant AMF to the upper AMF condition when both unsaturated bonds of limonene are ozonated. Modeling demonstrates that using the correct resultant AMF to simulate SOA formation owing to limonene ozonolysis is crucial for accurate indoor prediction.

Evaluation of the volatility basis-set approach for the simulation of organic aerosol formation in the Mexico City metropolitan area

Directory of Open Access Journals (Sweden)

A. P. Tsimpidi

2010-01-01

Full Text Available New primary and secondary organic aerosol modules have been added to PMCAMx, a three dimensional chemical transport model (CTM, for use with the SAPRC99 chemistry mechanism based on recent smog chamber studies. The new modelling framework is based on the volatility basis-set approach: both primary and secondary organic components are assumed to be semivolatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. This new framework with the use of the new volatility basis parameters for low-NO_x and high-NO_x conditions tends to predict 4–6 times higher anthropogenic SOA concentrations than those predicted with the older generation of models. The resulting PMCAMx-2008 was applied in Mexico City Metropolitan Area (MCMA for approximately a week during April 2003 during a period of very low regional biomass burning impact. The emission inventory, which uses as a starting point the MCMA 2004 official inventory, is modified and the primary organic aerosol (POA emissions are distributed by volatility based on dilution experiments. The predicted organic aerosol (OA concentrations peak in the center of Mexico City, reaching values above 40 μg m⁻³. The model predictions are compared with the results of the Positive Matrix Factorization (PMF analysis of the Aerosol Mass Spectrometry (AMS observations. The model reproduces both Hydrocarbon-like Organic Aerosol (HOA and Oxygenated Organic Aerosol (OOA concentrations and diurnal profiles. The small OA underprediction during the rush-hour periods and overprediction in the afternoon suggest potential improvements to the description of fresh primary organic emissions and the formation of the oxygenated organic aerosols, respectively, although they may also be due to errors in the simulation of dispersion and vertical mixing. However, the AMS OOA data are not specific enough to prove that the model reproduces the organic aerosol

Aerosol indirect effect from turbulence-induced broadening of cloud-droplet size distributions

Energy Technology Data Exchange (ETDEWEB)

Chandrakar, Kamal Kant; Cantrell, Will; Chang, Kelken; Ciochetto, David; Niedermeier, Dennis; Ovchinnikov, Mikhail; Shaw, Raymond A.; Yang, Fan

2016-11-28

The influence of aerosol concentration on cloud droplet size distribution is investigated in a laboratory chamber that enables turbulent cloud formation through moist convection. The experiments allow steady-state microphysics to be achieved, with aerosol input balanced by cloud droplet growth and fallout. As aerosol concentration is increased the cloud droplet mean diameter decreases as expected, but the width of the size distribution also decreases sharply. The aerosol input allows for cloud generation in the limiting regimes of fast microphysics (τ_c < τ_t) for high aerosol concentration, and slow microphysics (τ_c > τ_t) for low aerosol concentration; here, τ_c is the phase relaxation time and τ_t is the turbulence correlation time. The increase in the width of the droplet size distribution for the low aerosol limit is consistent with larger variability of supersaturation due to the slow microphysical response. A stochastic differential equation for supersaturation predicts that the standard deviation of the squared droplet radius should increase linearly with a system time scale defined as τ_s^-1 =τ_c^-1 + τ_t^-1, and the measurements are in excellent agreement with this finding. This finding underscores the importance of droplet size dispersion for the aerosol indirect effect: increasing aerosol concentration not only suppresses precipitation formation through reduction of the mean droplet diameter, but perhaps more importantly, through narrowing of the droplet size distribution due to reduced supersaturation fluctuations. Supersaturation fluctuations in the low aerosol / slow microphysics limit are likely of leading importance for precipitation formation.

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.

Eulerian-Lagranigan simulation of aerosol evolution in turbulent mixing layer

KAUST Repository

Zhou, Kun; Jiang, Xiao; Sun, Ke; He, Zhu

2016-01-01

The formation and evolution of aerosol in turbulent flows are ubiquitous in both industrial processes and nature. The intricate interaction of turbulent mixing and aerosol evolution in a canonical turbulent mixing layer was investigated by a direct

Influence of cosmic radiation on aerosol and cloud formation over short time periods

DEFF Research Database (Denmark)

Bondo, Torsten

in the atmosphere affect aerosol and cloud creation and whether it is realistic to observe Forbush decrease events in climate data. The thesis involves a theoretical examination of the ionization caused by Forbush decreases based on studies of hourly neutron monitor data and muon telescope data as proxies...... distribution of stable nucleated clusters, the model takes condensation and coagulation into account and includes various loss mechanisms. This model is used to investigate the growth of aerosols into cloud condensation nuclei size particles and to study the influence of nucleation rates and background vapour...... resolution satellite data and aerosol ground based measurements are presented. Here it is observed that significant decreases in the angstrom exponent from AERONET aerosols and cloud liquid water from satellites take place after the largest Forbush decreases. The timescales of this indicate...

Comparison of secondary organic aerosol formation from toluene on initially wet and dry ammonium sulfate particles at moderate relative humidity

Directory of Open Access Journals (Sweden)

T. Liu

2018-04-01

Full Text Available The formation of secondary organic aerosol (SOA has been widely studied in the presence of dry seed particles at low relative humidity (RH. At higher RH, initially dry seed particles can exist as wet particles due to water uptake by the seeds as well as the SOA. Here, we investigated the formation of SOA from the photooxidation of toluene using an oxidation flow reactor in the absence of NOx under a range of OH exposures on initially wet or dry ammonium sulfate (AS seed particles at an RH of 68 %. The ratio of the SOA yield on wet AS seeds to that on dry AS seeds, the relative SOA yield, decreased from 1.31 ± 0.02 at an OH exposure of 4.66 × 1010 molecules cm−3 s to 1.01 ± 0.01 at an OH exposure of 5.28 × 1011 molecules cm−3 s. This decrease may be due to the early deliquescence of initially dry AS seeds after being coated by highly oxidized toluene-derived SOA. SOA formation lowered the deliquescence RH of AS and resulted in the uptake of water by both AS and SOA. Hence the initially dry AS seeds contained aerosol liquid water (ALW soon after SOA formed, and the SOA yield and ALW approached those of the initially wet AS seeds as OH exposure and ALW increased, especially at high OH exposure. However, a higher oxidation state of the SOA on initially wet AS seeds than that on dry AS seeds was observed at all levels of OH exposure. The difference in mass fractions of m ∕ z 29, 43 and 44 of SOA mass spectra, obtained using an aerosol mass spectrometer (AMS, indicated that SOA formed on initially wet seeds may be enriched in earlier-generation products containing carbonyl functional groups at low OH exposures and later-generation products containing acidic functional groups at high exposures. Our results suggest that inorganic dry seeds become at least partially deliquesced particles during SOA formation and hence that ALW is inevitably involved in the SOA formation at moderate RH. More laboratory

Aerosols and fission product transport

International Nuclear Information System (INIS)

Megaw, W.J.

1987-12-01

A survey is presented of current knowledge of the possible role of aerosols in the consequences of in- and out-of-core LOCAs and of end fitting failures in CANDU reactors. An extensive literature search has been made of research on the behaviour of aerosols in possible accidents in water moderated and cooled reactors and the results of various studies compared. It is recommended that further work should be undertaken on the formation of aerosols during these possible accidents and to study their subsequent behaviour. It is also recommended that the fission products behaviour computer code FISSCON II should be re-examined to determine whether it reflects the advances incorporated in other codes developed for light water reactors which have been extensively compared. 47 refs

Secondary organic aerosol in the global aerosol – chemical transport model Oslo CTM2

Directory of Open Access Journals (Sweden)

I. S. A. Isaksen

2007-11-01

Full Text Available The global chemical transport model Oslo CTM2 has been extended to include the formation, transport and deposition of secondary organic aerosol (SOA. Precursor hydrocarbons which are oxidised to form condensible species include both biogenic species such as terpenes and isoprene, as well as species emitted predominantly by anthropogenic activities (toluene, m-xylene, methylbenzene and other aromatics. A model simulation for 2004 gives an annual global SOA production of approximately 55 Tg. Of this total, 2.5 Tg is found to consist of the oxidation products of anthropogenically emitted hydrocarbons, and about 15 Tg is formed by the oxidation products of isoprene. The global production of SOA is increased to about 69 Tg yr−1 by allowing semi-volatile species to partition to ammonium sulphate aerosol. This brings modelled organic aerosol values closer to those observed, however observations in Europe remain significantly underestimated. Allowing SOA to partition into ammonium sulphate aerosol increases the contribution of anthropogenic SOA from about 4.5% to 9.4% of the total production. Total modelled organic aerosol (OA values are found to represent a lower fraction of the measured values in winter (when primary organic aerosol (POA is the dominant OA component than in summer, which may be an indication that estimates of POA emissions are too low. Additionally, for measurement stations where the summer OA values are higher than in winter, the model generally underestimates the increase in summertime OA. In order to correctly model the observed increase in OA in summer, additional SOA sources or formation mechanisms may be necessary. The importance of NO3 as an oxidant of SOA precursors is found to vary regionally, causing up to 50%–60% of the total amount of SOA near the surface in polluted regions and less than 25% in more remote areas, if the yield of condensible oxidation products for β-pinene is used for NO3 oxidation of all terpenes

Simulating gas-aerosol-cirrus interactions: Process-oriented microphysical model and applications

Directory of Open Access Journals (Sweden)

B. Kärcher

2003-01-01

Full Text Available This work describes a process-oriented, microphysical-chemical model to simulate the formation and evolution of aerosols and ice crystals under the conditions prevailing in the upper troposphere and lower stratosphere. The model can be run as a box model or along atmospheric trajectories, and considers mixing, gas phase chemistry of aerosol precursors, binary homogeneous aerosol nucleation, homogeneous and heterogeneous ice nucleation, coagulation, condensation and dissolution, gas retention during particle freezing, gas trapping in growing ice crystals, and reverse processes. Chemical equations are solved iteratively using a second order implicit integration method. Gas-particle interactions and coagulation are treated over various size structures, with fully mass conserving and non-iterative numerical solution schemes. Particle types include quinternary aqueous solutions composed of H2SO4, HNO3, HCl, and HBr with and without insoluble components, insoluble aerosol particles, and spherical or columnar ice crystals deriving from each aerosol type separately. Three case studies are discussed in detail to demonstrate the potential of the model to simulate real atmospheric processes and to highlight current research topics concerning aerosol and cirrus formation near the tropopause. Emphasis is placed on how the formation of cirrus clouds and the scavenging of nitric acid in cirrus depends on small-scale temperature fluctuations and the presence of efficient ice nuclei in the tropopause region, corroborating and partly extending the findings of previous studies.

Key Role of Nitrate in Phase Transitions of Urban Particles: Implications of Important Reactive Surfaces for Secondary Aerosol Formation

Science.gov (United States)

Sun, Jiaxing; Liu, Lei; Xu, Liang; Wang, Yuanyuan; Wu, Zhijun; Hu, Min; Shi, Zongbo; Li, Yongjie; Zhang, Xiaoye; Chen, Jianmin; Li, Weijun

2018-01-01

Ammonium sulfate (AS) and ammonium nitrate (AN) are key components of urban fine particles. Both field and model studies showed that heterogeneous reactions of SO2, NO2, and NH3 on wet aerosols accelerated the haze formation in northern China. However, little is known on phase transitions of AS-AN containing haze particles. Here hygroscopic properties of laboratory-generated AS-AN particles and individual particles collected during haze events in an urban site were investigated using an individual particle hygroscopicity system. AS-AN particles showed a two-stage deliquescence at mutual deliquescence relative humidity (MDRH) and full deliquescence relative humidity (DRH) and three physical states: solid before MDRH, solid-aqueous between MDRH and DRH, and aqueous after DRH. During hydration, urban haze particles displayed a solid core and aqueous shell at RH = 60-80% and aqueous phase at RH > 80%. Most particles were in aqueous phase at RH > 50% during dehydration. Our results show that AS content in individual particles determines their DRH and AN content determines their MDRH. AN content increase can reduce MDRH, which indicates occurrence of aqueous shell at lower RH. The humidity-dependent phase transitions of nitrate-abundant urban particles are important to provide reactive surfaces of secondary aerosol formation in the polluted air.

Extraction and Characterization of Surfactants from Atmospheric Aerosols.

Science.gov (United States)

Nozière, Barbara; Gérard, Violaine; Baduel, Christine; Ferronato, Corinne

2017-04-21

Surface-active compounds, or surfactants, present in atmospheric aerosols are expected to play important roles in the formation of liquid water clouds in the Earth's atmosphere, a central process in meteorology, hydrology, and for the climate system. But because specific extraction and characterization of these compounds have been lacking for decades, very little is known on their identity, properties, mode of action and origins, thus preventing the full understanding of cloud formation and its potential links with the Earth's ecosystems. In this paper we present recently developed methods for 1) the targeted extraction of all the surfactants from atmospheric aerosol samples and for the determination of 2) their absolute concentrations in the aerosol phase and 3) their static surface tension curves in water, including their Critical Micelle Concentration (CMC). These methods have been validated with 9 references surfactants, including anionic, cationic and non-ionic ones. Examples of results are presented for surfactants found in fine aerosol particles (diameter <1 μm) collected at a coastal site in Croatia and suggestions for future improvements and other characterizations than those presented are discussed.

Dynamics of neutral and charged aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Leppae, J.

2012-07-01

Atmospheric aerosol particles have various climate effects and adverse health effects, which both depend on the size and number concentration of the particles. Freshly-formed particles are not large enough to impact neither health nor climate and they are most susceptible to removal by collisions with larger pre-existing particles. Consequently, the knowledge of both the formation and the growth rate of particles are crucially important when assessing the health and climate effects of atmospheric new particle formation. The purpose of this thesis is to increase our knowledge of the dynamics of neutral and charged aerosol particles with a specific interest towards the particle growth rate and processes affecting the aerosol charging state. A new model, Ion-UHMA, which simulates the dynamics of neutral and charged particles, was developed for this purpose. Simple analytical formulae that can be used to estimate the growth rate due to various processes were derived and used to study the effects of charged particles on the growth rate. It was found that the growth rate of a freshly-formed particle population due to condensation and coagulation could be significantly increased when a considerable fraction of the particles are charged. Finally, recent data-analysis methods that have been applied to the aerosol charging states obtained from the measurements were modified for a charge asymmetric framework. The methods were then tested on data obtained from aerosol dynamics simulations. The methods were found to be able to provide reasonable estimates on the growth rate and proportion of particles formed via ion-induced nucleation, provided that the growth rate is high enough and that the charged particles do not grow much more rapidly than the neutral ones. A simple procedure for estimating whether the methods are suitable for analysing data obtained in specific conditions was provided. In this thesis, the dynamics of neutral and charged aerosol particles were studied in

Some results of an experimental study of the atmospheric aerosol in Tomsk: A combined approach

Energy Technology Data Exchange (ETDEWEB)

Zuev, V.V. [Institute of Atmospheric Optics, Tomsk (Russian Federation)

1996-04-01

As widely accepted, aerosols strongly contribute to the formation of the earth`s radiation balance through the absorption and scattering of solar radiation. In addition, aerosols, being active condensation nuclei, also have a role in the cloud formation process. In this paper, results are presented of aerosol studies undertaken at the field measurement sites of the Institute of Atmospheric Optics in Tomsk and the Tomsk region.

Organic condensation - a vital link connecting aerosol formation to climate forcing

Science.gov (United States)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petäjä, T.; Slowik, J.; Chang, R.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.-M.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M.

2011-01-01

Atmospheric aerosol particles influence global climate as well as impair air quality through their effects on atmospheric visibility and human health. Ultrafine (<100 nm) particles often dominate aerosol numbers, and nucleation of atmospheric vapors is an important source of these particles. To have climatic relevance, however, the freshly-nucleated particles need to grow in size. We combine observations from two continental sites (Egbert, Canada and Hyytiälä, Finland) to show that condensation of organic vapors is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We demonstrate that state-of-the-science organic gas-particle partitioning models fail to reproduce the observations, and propose a modeling approach that is consistent with the measurements. We demonstrate the large sensitivity of climatic forcing of atmospheric aerosols to these interactions between organic vapors and the smallest atmospheric nanoparticles - highlighting the need for representing this process in global climate models.

Anthropogenic influence on the distribution of tropospheric sulphate aerosol

Energy Technology Data Exchange (ETDEWEB)

Langner, J; Rodhe, H; Crutzen, P J; Zimmermann, P [Swedish Meteorological and Hydrological Institute, Norrkoeping (Sweden)

1992-10-22

Human activities have increased global emissions of sulphur gases by about a factor of three during the past century, leading to increased sulphate aerosol concentrations, mainly in the Northern Hemisphere. Sulphate aerosols can affect the climate directly, by increasing the backscattering of solar radiation in cloud-free air, and indirectly, by providing additional cloud condensation nuclei. Here a global transport-chemistry model is used to estimate the changes in the distribution of tropospheric sulphate aerosol and deposition of non-seasalt sulphur that have occurred since pre-industrial times. The increase in sulphate aerosol concentration is small over the Southern Hemisphere oceans, but reaches a factor of 100 over northern Europe in winter. Calculations indicate, however, that at most 6% of the anthropogenic sulphur emissions is available for the formation of new aerosol particles. This is because about one-half of the sulphur dioxide is deposited on the Earth's surface, and most of the remainder is oxidized in cloud droplets so that the sulphate becomes associated with pre-existing particles. Even so, the rate of formation of new sulphate particles may have doubled since pre-industrial times. 18 refs., 3 figs.

Aerosols, cloud physics and radiation

International Nuclear Information System (INIS)

Twomey, S.

1990-01-01

Some aspects of climate physics are discussed with special attention given to cases where cloud physics is relevant for the phase and microstructure of clouds and, therefore, in the optical properties of the planet. It is argued that aerosol particles, through their strong effect on cloud microphysics, influence the shortwave energy input to earth, and that cloud microphysics strongly influence rain formation. Therefore, through their influence on microphysics, the aerosols play a central role in the atmospheric water cycle and, thus, on the planet's outgoing radiation. 20 refs

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.

Primary aerosol and secondary inorganic aerosol budget over the Mediterranean Basin during 2012 and 2013

Science.gov (United States)

Guth, Jonathan; Marécal, Virginie; Josse, Béatrice; Arteta, Joaquim; Hamer, Paul

2018-04-01

coastal areas. The formation of 23, 27 and 27 %, respectively of, ammonium, nitrate and sulfate aerosols is due to the emissions within the marine and coastal area.

Formation and characterization of fission-product aerosols under postulated HTGR accident conditions

International Nuclear Information System (INIS)

Tang, I.N.; Munkelwitz, H.R.

1982-07-01

The paper presents the results of an experimental investigation on the formation mechanism and physical characterization of simulated nuclear aerosols that could likely be released during an HTGR core heat-up accident. Experiments were carried out in a high-temperature flow system consisting essentially of an inductively heated release source, a vapor deposition tube, and a filter assembly for collecting particulate matter. Simulated fission products Sr and Ba as oxides are separately impregnated in H451 graphite wafers and released at elevated temperatures into a dry helium flow. In the presence of graphite, the oxides are quantitatively reduced to metals, which subsequently vaporize at temperatures much lower than required for the oxides alone to vaporize in the absence of graphite. A substantial fraction of the released material is associated with particulate matter, which is collected on filters located downstream at ambient temperature. The release and transport of simulated fission product Ag as metal are also investigated

Aerosol Delivery for Amendment Distribution in Contaminated Vadose Zones

Science.gov (United States)

Hall, R. J.; Murdoch, L.; Riha, B.; Looney, B.

2011-12-01

Remediation of contaminated vadose zones is often hindered by an inability to effectively distribute amendments. Many amendment-based approaches have been successful in saturated formations, however, have not been widely pursued when treating contaminated unsaturated materials due to amendment distribution limitations. Aerosol delivery is a promising new approach for distributing amendments in contaminated vadose zones. Amendments are aerosolized and injected through well screens. During injection the aerosol particles are transported with the gas and deposited on the surfaces of soil grains. Resulting distributions are radially and vertically broad, which could not be achieved by injecting pure liquid-phase solutions. The objectives of this work were A) to characterize transport and deposition behaviors of aerosols; and B) to develop capabilities for predicting results of aerosol injection scenarios. Aerosol transport and deposition processes were investigated by conducting lab-scale injection experiments. These experiments involved injection of aerosols through a 2m radius, sand-filled wedge. A particle analyzer was used to measure aerosol particle distributions with time, and sand samples were taken for amendment content analysis. Predictive capabilities were obtained by constructing a numerical model capable of simulating aerosol transport and deposition in porous media. Results from tests involving vegetable oil aerosol injection show that liquid contents appropriate for remedial applications could be readily achieved throughout the sand-filled wedge. Lab-scale tests conducted with aqueous aerosols show that liquid accumulation only occurs near the point of injection. Tests were also conducted using 200 g/L salt water as the aerosolized liquid. Liquid accumulations observed during salt water tests were minimal and similar to aqueous aerosol results. However, particles were measured, and salt deposited distal to the point of injection. Differences between

THE INFLUENCE OF AEROSOL GAS-DYNAMIC SUSPENSION CLEANING ON SURFACE OF THE AIRCRAFT PARTS

Directory of Open Access Journals (Sweden)

Vitaly D. Hizhko

2008-02-01

Full Text Available  The specificity of the surface microgeometry formation under the influence of aerosol gas-dynamic suspension flow was considered. The composition and character of metallic surface layer formation of aircraft parts was investigated. The possibility of surface material composition and properties adjustment changing aerosol gas-dynamic suspension flow parameters was determined. The hypothesis about the possibility of using aerosol gas-dynamic suspension flow to form corrosion-resistant coating on the detail metallic surfaces was set up.

Aerosol Angstrom Absorption Coefficient Comparisons during MILAGRO.

Science.gov (United States)

Marley, N. A.; Marchany-Rivera, A.; Kelley, K. L.; Mangu, A.; Gaffney, J. S.

2007-12-01

Measurements of aerosol absorption were obtained as part of the MAX-Mex component of the MILAGRO field campaign at site T0 (Instituto Mexicano de Petroleo in Mexico City) by using a 7-channel aethalometer (Thermo- Anderson) during the month of March, 2006. The absorption measurements obtained in the field at 370, 470, 520, 590, 660, 880, and 950 nm were used to determine the aerosol Angstrom absorption exponents by linear regression. Since, unlike other absorbing aerosol species (e.g. humic like substances, nitrated PAHs), black carbon absorption is relatively constant from the ultraviolet to the infrared with an Angstrom absorption exponent of -1 (1), a comparison of the Angstrom exponents can indicate the presence of aerosol components with an enhanced UV absorption over that expected from BC content alone. The Angstrom exponents determined from the aerosol absorption measurements obtained in the field varied from - 0.7 to - 1.3 during the study and was generally lower in the afternoon than the morning hours, indicating an increase in secondary aerosol formation and photochemically generated UV absorbing species in the afternoon. Twelve-hour integrated samples of fine atmospheric aerosols (Petroleo (IMP) and CENICA.

Effects of NOx and SO2 on the secondary organic aerosol formation from photooxidation of α-pinene and limonene

Directory of Open Access Journals (Sweden)

D. Zhao

2018-02-01

Full Text Available Anthropogenic emissions such as NOx and SO2 influence the biogenic secondary organic aerosol (SOA formation, but detailed mechanisms and effects are still elusive. We studied the effects of NOx and SO2 on the SOA formation from the photooxidation of α-pinene and limonene at ambient relevant NOx and SO2 concentrations (NOx: < 1to 20 ppb, SO2: < 0.05 to 15 ppb. In these experiments, monoterpene oxidation was dominated by OH oxidation. We found that SO2 induced nucleation and enhanced SOA mass formation. NOx strongly suppressed not only new particle formation but also SOA mass yield. However, in the presence of SO2 which induced a high number concentration of particles after oxidation to H2SO4, the suppression of the mass yield of SOA by NOx was completely or partly compensated for. This indicates that the suppression of SOA yield by NOx was largely due to the suppressed new particle formation, leading to a lack of particle surface for the organics to condense on and thus a significant influence of vapor wall loss on SOA mass yield. By compensating for the suppressing effect on nucleation of NOx, SO2 also compensated for the suppressing effect on SOA yield. Aerosol mass spectrometer data show that increasing NOx enhanced nitrate formation. The majority of the nitrate was organic nitrate (57–77 %, even in low-NOx conditions (<  ∼  1 ppb. Organic nitrate contributed 7–26 % of total organics assuming a molecular weight of 200 g mol−1. SOA from α-pinene photooxidation at high NOx had a generally lower hydrogen to carbon ratio (H ∕ C, compared to low NOx. The NOx dependence of the chemical composition can be attributed to the NOx dependence of the branching ratio of the RO2 loss reactions, leading to a lower fraction of organic hydroperoxides and higher fractions of organic nitrates at high NOx. While NOx suppressed new particle formation and SOA mass formation, SO2 can compensate for such effects, and the

Simulation of the Ozone Monitoring Instrument aerosol index using the NASA Goddard Earth Observing System aerosol reanalysis products

Science.gov (United States)

Colarco, Peter R.; Gassó, Santiago; Ahn, Changwoo; Buchard, Virginie; da Silva, Arlindo M.; Torres, Omar

2017-11-01

We provide an analysis of the commonly used Ozone Monitoring Instrument (OMI) aerosol index (AI) product for qualitative detection of the presence and loading of absorbing aerosols. In our analysis, simulated top-of-atmosphere (TOA) radiances are produced at the OMI footprints from a model atmosphere and aerosol profile provided by the NASA Goddard Earth Observing System (GEOS-5) Modern-Era Retrospective Analysis for Research and Applications aerosol reanalysis (MERRAero). Having established the credibility of the MERRAero simulation of the OMI AI in a previous paper we describe updates in the approach and aerosol optical property assumptions. The OMI TOA radiances are computed in cloud-free conditions from the MERRAero atmospheric state, and the AI is calculated. The simulated TOA radiances are fed to the OMI near-UV aerosol retrieval algorithms (known as OMAERUV) is compared to the MERRAero calculated AI. Two main sources of discrepancy are discussed: one pertaining to the OMI algorithm assumptions of the surface pressure, which are generally different from what the actual surface pressure of an observation is, and the other related to simplifying assumptions in the molecular atmosphere radiative transfer used in the OMI algorithms. Surface pressure assumptions lead to systematic biases in the OMAERUV AI, particularly over the oceans. Simplifications in the molecular radiative transfer lead to biases particularly in regions of topography intermediate to surface pressures of 600 and 1013.25 hPa. Generally, the errors in the OMI AI due to these considerations are less than 0.2 in magnitude, though larger errors are possible, particularly over land. We recommend that future versions of the OMI algorithms use surface pressures from readily available atmospheric analyses combined with high-spatial-resolution topographic maps and include more surface pressure nodal points in their radiative transfer lookup tables.

Development of a global aerosol model using a two-dimensional sectional method: 1. Model design

Science.gov (United States)

Matsui, H.

2017-08-01

This study develops an aerosol module, the Aerosol Two-dimensional bin module for foRmation and Aging Simulation version 2 (ATRAS2), and implements the module into a global climate model, Community Atmosphere Model. The ATRAS2 module uses a two-dimensional (2-D) sectional representation with 12 size bins for particles from 1 nm to 10 μm in dry diameter and 8 black carbon (BC) mixing state bins. The module can explicitly calculate the enhancement of absorption and cloud condensation nuclei activity of BC-containing particles by aging processes. The ATRAS2 module is an extension of a 2-D sectional aerosol module ATRAS used in our previous studies within a framework of a regional three-dimensional model. Compared with ATRAS, the computational cost of the aerosol module is reduced by more than a factor of 10 by simplifying the treatment of aerosol processes and 2-D sectional representation, while maintaining good accuracy of aerosol parameters in the simulations. Aerosol processes are simplified for condensation of sulfate, ammonium, and nitrate, organic aerosol formation, coagulation, and new particle formation processes, and box model simulations show that these simplifications do not substantially change the predicted aerosol number and mass concentrations and their mixing states. The 2-D sectional representation is simplified (the number of advected species is reduced) primarily by the treatment of chemical compositions using two interactive bin representations. The simplifications do not change the accuracy of global aerosol simulations. In part 2, comparisons with measurements and the results focused on aerosol processes such as BC aging processes are shown.

Influence of trace aromatics on the chemical growth mechanisms of Titan aerosol analogues

Science.gov (United States)

Gautier, Thomas; Sebree, Joshua A.; Li, Xiang; Pinnick, Veronica T.; Grubisic, Andrej; Loeffler, Mark J.; Getty, Stephanie A.; Trainer, Melissa G.; Brinckerhoff, William B.

2017-06-01

The chemical structure and formation pathways of Titan aerosols remain largely unknown. In this work, we studied the effect of trace aromatics on the chemical composition and formation pathways of laboratory analogues of Titan's organic aerosols. The aerosol analogues were produced using four different trace aromatic molecules, comprised of one or two aromatic rings, each with or without a nitrogen heteroatom. Samples were then analyzed by laser desorption/ionization Mass Spectrometry (LDMS), revealing a high variability in the sample composition depending on the trace aromatic used. Our work reveals that the final chemical structure of the aerosols depends strongly on the number of aromatic rings in the trace molecule, leading either to a polymeric or to a random co-polymeric growth of the sample. These different chemical structures can affect the physical properties of the aerosol. Future analysis of Titan's aerosols using better resolution could potentially determine whether either of the growth hypotheses are preferred.

Secondary organic material formed by methylglyoxal in aqueous aerosol mimics

Directory of Open Access Journals (Sweden)

N. Sareen

2010-02-01

Full Text Available We show that methylglyoxal forms light-absorbing secondary organic material in aqueous ammonium sulfate and ammonium nitrate solutions mimicking tropospheric aerosol particles. The kinetics were characterized using UV-Vis spectrophotometry. The results suggest that the bimolecular reaction of methylglyoxal with an ammonium or hydronium ion is the rate-limiting step for the formation of light-absorbing species, with k_NH4+^II=5×10⁻⁶ M⁻¹ min⁻¹ and k_H3O+^II≤10⁻³ M⁻¹ min⁻¹. Evidence of aldol condensation products and oligomeric species up to 759 amu was found using chemical ionization mass spectrometry with a volatilization flow tube inlet (Aerosol-CIMS. Tentative identifications of carbon-nitrogen species and a sulfur-containing compound were also made using Aerosol-CIMS. Aqueous solutions of methylglyoxal, with and without inorganic salts, exhibit significant surface tension depression. These observations add to the growing body of evidence that dicarbonyl compounds may form secondary organic material in the aerosol aqueous phase, and that secondary organic aerosol formation via heterogeneous processes may affect seed aerosol properties.

Primary Emission and the Potential of Secondary Aerosol Formation from Chinese Gasoline Engine Exhaust

Science.gov (United States)

Hu, Min; Peng, Jianfei; Qin, Yanhong; Du, Zhuofei; Li, Mengjin; Zheng, Rong; Zheng, Jing; Shang, Dongjie; Lu, Sihua; Wu, Yusheng; Zeng, Limin; Guo, Song; Shao, Min; Wang, Yinhui; Shuai, Shijin

2017-04-01

Along with the urbanization and economic growth, vehicle population in China reached 269 million, ranked the second in the world in 2015. Gasoline vehicle is identified to be the main source for urban PM2.5 in China, accounting for 15%-31%. In this study the impact of fuel components on PM2.5 and volatile organic compounds (VOCs) emissions from a gasoline port fuel injection (PFI) engine and a gasoline direct injection (GDI) engine are discussed. Results show that, higher proportion of aromatics, alkenes or sulfur in gasoline fuel will lead to higher PM emissions. The PM from the PFI engine mainly consists of OC and a small amount of EC and inorganic ions, while the PM discharge from the GDI engine mainly consists of EC, OM and a small amount of inorganic ions. Since the GDI engines can reduce fuel consumption and CO2 emissions, and it would become more and more popular in the near future. The characteristics of POM component, emission factors and source profile were investigated from GDI engine, particularly focused on the effect of engine speed, load and the catalyst, which will be very much helpful for source identification as source indicators. Chamber experiments were conducted to quantify the potential of secondary aerosol formation from exhaust of a PFI gasoline engine and China V gasoline fuel. During 4-5 h simulation, equivalent to10 days of atmospheric photo-oxidation in Beijing, the extreme SOA production was 426 ± 85 mg/kg fuel, with high precursors and OH exposure. 14% of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatility organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reduction of emissions of aerosol precursor gases from vehicles is essential to mediate pollution in China.

Experimental and modelling studies of iodine oxide formation and aerosol behaviour relevant to nuclear reactor accidents

International Nuclear Information System (INIS)

Dickinson, S.; Auvinen, A.; Ammar, Y.; Bosland, L.; Clément, B.; Funke, F.; Glowa, G.; Kärkelä, T.; Powers, D.A.; Tietze, S.; Weber, G.; Zhang, S.

2014-01-01

Highlights: • Radiolytic reactions can influence iodine volatility following a nuclear accident. • Kinetic models have been developed based on atmospheric chemistry studies. • Properties of iodine oxide aerosols produced by radiation have been measured. • Decomposition of iodine oxides by the action of heat or radiation has been observed. - Abstract: Plant assessments have shown that iodine contributes significantly to the source term for a range of accident scenarios. Iodine has a complex chemistry that determines its chemical form and, consequently, its volatility in the containment. If volatile iodine species are formed by reactions in the containment, they will be subject to radiolytic reactions in the atmosphere, resulting in the conversion of the gaseous species into involatile iodine oxides, which may deposit on surfaces or re-dissolve in water pools. The concentration of airborne iodine in the containment will, therefore, be determined by the balance between the reactions contributing to the formation and destruction of volatile species, as well as by the physico-chemical properties of the iodine oxide aerosols which will influence their longevity in the atmosphere. This paper summarises the work that has been done in the framework of the EC SARNET (Severe Accident Research Network) to develop a greater understanding of the reactions of gaseous iodine species in irradiated air/steam atmospheres, and the nature and behaviour of the reaction products. This work has mainly been focussed on investigating the nature and behaviour of iodine oxide aerosols, but earlier work by members of the SARNET group on gaseous reaction rates is also discussed to place the more recent work into context

Description of test facilities bound to the research on sodium aerosols - some significant results

Energy Technology Data Exchange (ETDEWEB)

Dolias, M; Lafon, A; Vidard, M; Schaller, K H [DRNR/STRS - Centre de Cadarache, Saint-Paul-lez-Durance (France)

1977-01-01

This communication is dedicated to the description of the CEA (French Atomic Energy Authority) testing located at CADARACHE and which are utilized for the study of sodium aerosols behavior. These testing loops are necessary for studying the operating of equipment such as filters, sodium vapour traps, condensers and separators. It is also possible to study the effect of characteristics parameters on formation, coagulation and carrying away of sodium aerosols in the cover gas. Sodium aerosols deposits in a vertical annular space configuration with a cold area in its upper part are also studied. Some significant results emphasize the importance of operating conditions on the formation of aerosols. (author)

Fractionation of Stable Isotopes in Atmospheric Aerosol Reactions

DEFF Research Database (Denmark)

Meusinger, Carl

-independent) fractionation processes of stable isotopes of C, N, O and S in order to investigate three different systems related to aerosols: 1. Post-depositional processes of nitrate in snow that obscure nitrate ice core records 2. Formation and aging of secondary organic aerosol generated by ozonolysis of X...... reactions and undergo complex chemical and physical changes during their lifetimes. In order to assess processes that form and alter aerosols, information provided by stable isotopes can be used to help constrain estimates on the strength of aerosol sources and sinks. This thesis studies (mass...... as required. The kndings provide important results for the studies' respective felds, including a description of the isotopic fractionation and quantum yield of nitrate photolysis in snow, equilibrium fractionation in secondary organic aerosol and fractionation constants of different oxidation pathways of SO2....

Model of optical response of marine aerosols to Forbush decreases

DEFF Research Database (Denmark)

Bondo, Torsten; Enghoff, Martin Andreas Bødker; Svensmark, Henrik

2010-01-01

In order to elucidate the effect of galactic cosmic rays on cloud formation, we investigate the optical response of marine aerosols to Forbush decreases - abrupt decreases in galactic cosmic rays - by means of modeling. We vary the nucleation rate of new aerosols, in a sectional coagulation...

In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor

Science.gov (United States)

Palm, Brett B.; Campuzano-Jost, Pedro; Ortega, Amber M.; Day, Douglas A.; Kaser, Lisa; Jud, Werner; Karl, Thomas; Hansel, Armin; Hunter, James F.; Cross, Eben S.; Kroll, Jesse H.; Peng, Zhe; Brune, William H.; Jimenez, Jose L.

2016-03-01

An oxidation flow reactor (OFR) is a vessel inside which the concentration of a chosen oxidant can be increased for the purpose of studying SOA formation and aging by that oxidant. During the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen-Rocky Mountain Biogenic Aerosol Study) field campaign, ambient pine forest air was oxidized by OH radicals in an OFR to measure the amount of SOA that could be formed from the real mix of ambient SOA precursor gases, and how that amount changed with time as precursors changed. High OH concentrations and short residence times allowed for semicontinuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq.) atmospheric aging. A simple model is derived and used to account for the relative timescales of condensation of low-volatility organic compounds (LVOCs) onto particles; condensational loss to the walls; and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 3 µg m-3 when LVOC fate corrected) compared to daytime (average 0.9 µg m-3 when LVOC fate corrected), with maximum formation observed at 0.4-1.5 eq. days of photochemical aging. SOA formation followed a similar diurnal pattern to monoterpenes, sesquiterpenes, and toluene+p-cymene concentrations, including a substantial increase just after sunrise at 07:00 local time. Higher photochemical aging (> 10 eq. days) led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254-70), similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production of small oxidized organic

In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor

Directory of Open Access Journals (Sweden)

B. B. Palm

2016-03-01

Full Text Available An oxidation flow reactor (OFR is a vessel inside which the concentration of a chosen oxidant can be increased for the purpose of studying SOA formation and aging by that oxidant. During the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen–Rocky Mountain Biogenic Aerosol Study field campaign, ambient pine forest air was oxidized by OH radicals in an OFR to measure the amount of SOA that could be formed from the real mix of ambient SOA precursor gases, and how that amount changed with time as precursors changed. High OH concentrations and short residence times allowed for semicontinuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq. atmospheric aging. A simple model is derived and used to account for the relative timescales of condensation of low-volatility organic compounds (LVOCs onto particles; condensational loss to the walls; and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 3 µg m−3 when LVOC fate corrected compared to daytime (average 0.9 µg m−3 when LVOC fate corrected, with maximum formation observed at 0.4–1.5 eq. days of photochemical aging. SOA formation followed a similar diurnal pattern to monoterpenes, sesquiterpenes, and toluene+p-cymene concentrations, including a substantial increase just after sunrise at 07:00 local time. Higher photochemical aging (> 10 eq. days led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254-70, similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production

Secondary organic aerosol formation through fog processing of VOCs

Science.gov (United States)

Herckes, P.; Hutchings, J. W.

2010-07-01

Volatile Organic Compounds (VOCs) including benzene, toluene, ethylbenzene and xylenes (BTEX) have been determined in highly concentrated amounts (>1 ug/L) in intercepted clouds in northern Arizona (USA). These VOCs are found in concentrations much higher than predicted by partitioning alone. The reactivity of BTEX in the fog/cloud aqueous phase was investigated through laboratory studies. BTEX species showed fast degradation in the aqueous phase in the presence of peroxides and light. Observed half-lives ranged from three and six hours, substantially shorter than the respective gas phase half-lives (several days). The observed reaction rates were on the order of 1 ppb/min but decreased substantially with increasing concentrations of organic matter (TOC). The products of BTEX oxidation reactions were analyzed using HPLC-UV and LCMS. The first generation of products identified included phenol and cresols which correspond to the hydroxyl-addition reaction to benzene and toluene. Upon investigating of multi-generational products, smaller, less volatile species are predominant although a large variety of products is found. Most reaction products have substantially lower vapor pressure and will remain in the particle phase upon droplet evaporation. The SOA generation potential of cloud and fog processing of BTEX was evaluated using simple calculations and showed that in ideal situations these reactions could add up to 9% of the ambient aerosol mass. In more conservative scenarios, the contribution of the processing of BTEX was around 1% of ambient aerosol concentrations. Overall, cloud processing of VOC has the potential to contribute to the atmospheric aerosol mass. However, the contribution will depend upon many factors such as the irradiation, organic matter content in the droplets and droplet lifetime.

Improving organic aerosol treatments in CESM/CAM5: Development, application, and evaluation

Science.gov (United States)

Glotfelty, Timothy; He, Jian; Zhang, Yang

2017-06-01

New treatments for organic aerosol (OA) formation have been added to a modified version of the CESM/CAM5 model (CESM-NCSU). These treatments include a volatility basis set treatment for the simulation of primary and secondary organic aerosols (SOAs), a simplified treatment for organic aerosol (OA) formation from glyoxal, and a parameterization representing the impact of new particle formation (NPF) of organic gases and sulfuric acid. With the inclusion of these new treatments, the concentration of oxygenated organic aerosol increases by 0.33 µg m-3 and that of primary organic aerosol (POA) decreases by 0.22 µg m-3 on global average. The decrease in POA leads to a reduction in the OA direct effect, while the increased OOA increases the OA indirect effects. Simulations with the new OA treatments show considerable improvement in simulated SOA, oxygenated organic aerosol (OOA), organic carbon (OC), total carbon (TC), and total organic aerosol (TOA), but degradation in the performance of HOA. In simulations of the current climate period, despite some deviations from observations, CESM-NCSU with the new OA treatments significantly improves the magnitude, spatial pattern, seasonal pattern of OC and TC, as well as, the speciation of TOA between POA and OOA. Sensitivity analysis reveals that the inclusion of the organic NPF treatment impacts the OA indirect effects by enhancing cloud properties. The simulated OA level and its impact on the climate system are most sensitive to choices in the enthalpy of vaporization and wet deposition of SVOCs, indicating that accurate representations of these parameters are critical for accurate OA-climate simulations.

Effects of Solvent and Temperature on Free Radical Formation in Electronic Cigarette Aerosols.

Science.gov (United States)

Bitzer, Zachary T; Goel, Reema; Reilly, Samantha M; Foulds, Jonathan; Muscat, Joshua; Elias, Ryan J; Richie, John P

2018-01-16

The ever-evolving market of electronic cigarettes (e-cigarettes) presents a challenge for analyzing and characterizing the harmful products they can produce. Earlier we reported that e-cigarette aerosols can deliver high levels of reactive free radicals; however, there are few data characterizing the production of these potentially harmful oxidants. Thus, we have performed a detailed analysis of the different parameters affecting the production of free radical by e-cigarettes. Using a temperature-controlled e-cigarette device and a novel mechanism for reliably simulating e-cigarette usage conditions, including coil activation and puff flow, we analyzed the effects of temperature, wattage, and e-liquid solvent composition of propylene glycol (PG) and glycerol (GLY) on radical production. Free radicals in e-cigarette aerosols were spin-trapped and analyzed using electron paramagnetic resonance. Free radical production increased in a temperature-dependent manner, showing a nearly 2-fold increase between 100 and 300 °C under constant-temperature conditions. Free radical production under constant wattage showed an even greater increase when going from 10 to 50 W due, in part, to higher coil temperatures compared to constant-temperature conditions. The e-liquid PG content also heavily influenced free radical production, showing a nearly 3-fold increase upon comparison of ratios of 0:100 (PG:GLY) and 100:0 (PG:GLY). Increases in PG content were also associated with increases in aerosol-induced oxidation of biologically relevant lipids. These results demonstrate that the production of reactive free radicals in e-cigarette aerosols is highly solvent dependent and increases with an increase in temperature. Radical production was somewhat dependent on aerosol production at higher temperatures; however, disproportionately high levels of free radicals were observed at ≥100 °C despite limited aerosol production. Overall, these findings suggest that e-cigarettes can be

Eulerian-Lagranigan simulation of aerosol evolution in turbulent mixing layer

KAUST Repository

Zhou, Kun

2016-09-23

The formation and evolution of aerosol in turbulent flows are ubiquitous in both industrial processes and nature. The intricate interaction of turbulent mixing and aerosol evolution in a canonical turbulent mixing layer was investigated by a direct numerical simulation (DNS) in a recent study (Zhou, K., Attili, A., Alshaarawi, A., and Bisetti, F. Simulation of aerosol nucleation and growth in a turbulent mixing layer. Physics of Fluids, 26, 065106 (2014)). In this work, Monte Carlo (MC) simulation of aerosol evolution is carried out along Lagrangian trajectories obtained in the previous simulation, in order to quantify the error of the moment method used in the previous simulation. Moreover, the particle size distribution (PSD), not available in the previous works, is also investigated. Along a fluid parcel moving through the turbulent flow, temperature and vapor concentration exhibit complex fluctuations, triggering complicate aerosol processes and rendering complex PSD. However, the mean PSD is found to be bi-modal in most of the mixing layer except that a tri-modal distribution is found in the turbulent transition region. The simulated PSDs agree with the experiment observations available in the literature. A different explanation on the formation of such PSDs is provided.

Characterization of Organic Nitrate Formation in Limonene Secondary Organic Aerosol using High-Resolution Chemical Ionization Mass Spectrometry

Science.gov (United States)

Faxon, Cameron; Hammes, Julia; Peng, Jianfei; Hallquist, Mattias; Pathak, Ravi

2016-04-01

Previous work has shown that organic nitrates (RONO2) are prevalent in the boundary layer, and can contribute significantly to secondary organic aerosol formation. Monoterpenes, including limonene, have been shown to be precursors for the formation of these organic nitrates. Limonene has two double bonds, either of which may be oxidized by NO3 or O3. This leads to the generation of products that can subsequently condense or partition into the particle phase, producing secondary organic aerosol. In order to further elucidate the particle and gas phase product distribution of organic nitrates forming from the reactions of limonene and the nitrate radical (NO3), a series of experiments were performed in the Gothenburg Flow Reactor for Oxidation Studies at Low Temperatures (G-FROST), described by previous work. N2O5 was used as the source for NO3 and NO2, and a characterized diffusion source was used to introduce limonene into the flow reactor. All experiments were conducted in the absence of light, and the concentration of limonene was increased step-wise throughout each experiment to modify the ratio of N2O5to limonene. The experiments were conducted such that both limonene- and N2O5-limited regimes were present. Gas and particle phase products were measured using an iodide High-Resolution Time-of-Flight Mass Spectrometer (HR-ToF-CIMS) coupled to a Filter Inlet for Gases and AEROsols (FIGAERO, and particle size and SOA mass concentrations were derived using a Scanning Mobility Particle Sizer (SMPS). CIMS measurement techniques have previously been employed for the measurement of organic nitrate products of such compounds using multiple reagent ions. The use of this instrumentation allowed for the identification of chemical formulas for gas and particle phase species. The findings from the experiments will be presented in terms of the relative gas-particle partitioning of major products and the effects of N2O5/limonene ratios on product distributions. Additionally, a

Characterization of aerosol photooxidation flow reactors: heterogeneous oxidation, secondary organic aerosol formation and cloud condensation nuclei activity measurements

Directory of Open Access Journals (Sweden)

A. T. Lambe

2011-03-01

Full Text Available Motivated by the need to develop instrumental techniques for characterizing organic aerosol aging, we report on the performance of the Toronto Photo-Oxidation Tube (TPOT and Potential Aerosol Mass (PAM flow tube reactors under a variety of experimental conditions. The PAM system was designed with lower surface-area-to-volume (SA/V ratio to minimize wall effects; the TPOT reactor was designed to study heterogeneous aerosol chemistry where wall loss can be independently measured. The following studies were performed: (1 transmission efficiency measurements for CO₂, SO₂, and bis(2-ethylhexyl sebacate (BES particles, (2 H₂SO₄ yield measurements from the oxidation of SO₂, (3 residence time distribution (RTD measurements for CO₂, SO₂, and BES particles, (4 aerosol mass spectra, O/C and H/C ratios, and cloud condensation nuclei (CCN activity measurements of BES particles exposed to OH radicals, and (5 aerosol mass spectra, O/C and H/C ratios, CCN activity, and yield measurements of secondary organic aerosol (SOA generated from gas-phase OH oxidation of m-xylene and α-pinene. OH exposures ranged from (2.0 ± 1.0 × 10¹⁰ to (1.8 ± 0.3 × 10¹² molec cm⁻³ s. Where applicable, data from the flow tube reactors are compared with published results from the Caltech smog chamber. The TPOT yielded narrower RTDs. However, its transmission efficiency for SO₂ was lower than that for the PAM. Transmission efficiency for BES and H₂SO₄ particles was size-dependent and was similar for the two flow tube designs. Oxidized BES particles had similar O/C and H/C ratios and CCN activity at OH exposures greater than 10¹¹ molec cm⁻³ s, but different CCN activity at lower OH exposures. The O/C ratio, H/C ratio, and yield of m-xylene and α-pinene SOA was strongly affected by reactor design and

Wintertime water-soluble aerosol composition and particle water content in Fresno, California

Science.gov (United States)

Parworth, Caroline L.; Young, Dominique E.; Kim, Hwajin; Zhang, Xiaolu; Cappa, Christopher D.; Collier, Sonya; Zhang, Qi

2017-03-01

The composition and concentrations of water-soluble gases and ionic aerosol components were measured from January to February 2013 in Fresno, CA, with a particle-into-liquid sampler with ion chromatography and annular denuders. The average (±1σ) ionic aerosol mass concentration was 15.0 (±9.4) µg m-3, and dominated by nitrate (61%), followed by ammonium, sulfate, chloride, potassium, nitrite, and sodium. Aerosol-phase organic acids, including formate and glycolate, and amines including methylaminium, triethanolaminium, ethanolaminium, dimethylaminium, and ethylaminium were also detected. Although the dominant species all came from secondary aerosol formation, there were primary sources of ionic aerosols as well, including biomass burning for potassium and glycolate, sea spray for sodium, chloride, and dimethylamine, and vehicles for formate. Particulate methanesulfonic acid was also detected and mainly associated with terrestrial sources. On average, the molar concentration of ammonia was 49 times greater than nitric acid, indicating that ammonium nitrate formation was limited by nitric acid availability. Particle water was calculated based on the Extended Aerosol Inorganics Model (E-AIM) thermodynamic prediction of inorganic particle water and κ-Köhler theory approximation of organic particle water. The average (±1σ) particle water concentration was 19.2 (±18.6) µg m-3, of which 90% was attributed to inorganic species. The fractional contribution of particle water to total fine particle mass averaged at 36% during this study and was greatest during early morning and night and least during the day. Based on aqueous-phase concentrations of ions calculated by using E-AIM, the average (±1σ) pH of particles in Fresno during the winter was estimated to be 4.2 (±0.2).

MAPPIX: A software package for off-line micro-pixe single particle aerosol analysis

International Nuclear Information System (INIS)

Ceccato, D.

2009-01-01

In the framework of a multiannual experiment performed at Baia Terra Nova, Antarctica, size-segregated aerosol samples were collected by using a 12-stage SDI impactor (Hillamo design). Approximately 2800 particles, belonging to the first four supermicrometric SDI stages - 8.39, 4.08, 2.68, 1.66 μm dynamic aerosol diameter cuts - were analyzed at the INFN-LNL micro-PIXE facility, a three lens Oxford Microprobe (OM) product, installed in the early nineties. Four regions on each of the 12 sub-samples were measured; 60 aerosol particles were detected on average in each of the analyzed regions. The off-line single aerosol particle (SAP) analysis of such big amount of data required software that is able to rapidly handle the acquired data, with a simple and fast area selection procedure; the subsequent automated PIXE spectra analysis with a specialized code was also needed. The MAPPIX 2.0 software was designed to make easier and faster the user jobs during the SAP analysis. The package is composed of two separate routines: the first one is devoted to data format conversion (OM-LMF file format to MAPPIX format), while the second one is devoted to micro-PIXE maps graphical presentation and aerosol particle selection procedure. The MAPPIX data format and software features will be discussed; a short report of the speed performances will be presented.

The US Nuclear Regulatory Commission aerosol release and the transport program

Energy Technology Data Exchange (ETDEWEB)

Silberberg, M; Kress, T [Office of Nuclear Regulatory Research, U.S. Nuclear Regulatory Commission, Washington, DC (United States); Gieseke, J [Batelle Memorial Institute, Columbus, OH (United States)

1977-01-01

An overview is presented of the U.S.N.R.C. research program for providing experimentally verified, quantitative methods for estimating the release and transport of sodium and radionuclide aerosols following postulated accidents. The program is directed towards radiological consequence assessment, however a number of aerosol behavior mechanisms being studied are applicable to LMFBR operational considerations. Related theoretical and experimental work on aerosol formation, agglomeration, settling and plating is noted. (author)

Natural and Anthropogenically Perturbed Biogenic Aerosol over Tropical South East Asia

Science.gov (United States)

Coe, H.; Robinson, N.; Allan, J. D.; Hewitt, C. N.

2014-12-01

Tropical forested regions are of interest as sources of atmospheric aerosol since they cover very large areas of the tropics and are a source of a large amount of volatile organic compounds which act as precursors for particle formation. Natural forest regions offer the potential to study the background state of the tropics and so potentially gain some insight into the pre-perturbed atmosphere. However, over the last decade in South East Asia, a considerable fraction of the native tropical deciduous forest has been deforested and replanted with palm oil plantations. This changes the range of volatile organic compounds that are emitted and act as sources of secondary organic aerosol. A suite of intensive ground and airborne measurements were made over both tropical forest and oil palm plantations in Sabah, Malaysia as part of the "Oxidant and Particle Photochemical Processes above a South East Asian tropical rainforest (OP3) during 2008. These data will be used together with recent improvements in our understanding of aerosol formation from biogenic compounds to discuss aerosol formation in tropical regions and the influence of human influence through widespread palm oil agriculture.

ENDF/B-5 formats manual. Revised update pages of Nov. 1983. Reprint of B.A. Magurno, BNL-NCS--50496 (ENDF-102) 2nd Edition

Energy Technology Data Exchange (ETDEWEB)

Magurno, B A

1986-09-01

The ENDF-5 Format, originally the format of the US Evaluated Nuclear Data File ENDF/B-5, was internationally recommended for the computer storage, processing and exchange of evaluated neutron nuclear data. The pages included in this document serve as an update to the original ENDF-5 Formats Manual BNL-NCS-50496 [ENDF-102] 2nd Edition, October 1979. (author)

Electrically Driven Technologies for Radioactive Aerosol Abatement

Energy Technology Data Exchange (ETDEWEB)

David W. DePaoli; Ofodike A. Ezekoye; Costas Tsouris; Valmor F. de Almeida

2003-01-28

The purpose of this research project was to develop an improved understanding of how electriexecy driven processes, including electrocoalescence, acoustic agglomeration, and electric filtration, may be employed to efficiently treat problems caused by the formation of aerosols during DOE waste treatment operations. The production of aerosols during treatment and retrieval operations in radioactive waste tanks and during thermal treatment operations such as calcination presents a significant problem of cost, worker exposure, potential for release, and increased waste volume.

The response of a simulated Mesoscale Convective System to increased aerosol pollution

Science.gov (United States)

Clavner, Michal

This work focuses on the impacts of aerosols on the total precipitation amount, rates and spatial distribution of precipitation produced by a Mesoscale Convective System (MCS), as well as the characteristics of a derecho event. Past studies have shown that the impacts on MCS-produced precipitation to changes in aerosol concentration are strongly dependent on environmental conditions, primarily humidity and environmental wind shear. Changes in aerosol concentrations were found to alter MCS-precipitation production directly by modifying precipitation processes and indirectly by affecting the efficiency of the storm's self-propagation. Observational and numerical studies have been conducted that have examined the dynamics responsible for the generation of widespread convectively-induced windstorms, primarily focusing on environmental conditions and the MCS features that generate a derecho event. While the sensitivity of the formation of bow-echoes, the radar signature associated with derecho events, to changes in microphysics has been examined, a study on a derecho-producing MCS characteristics to aerosol concentrations has not. In this study different aerosol concentrations and their effects on precipitation and a derecho produced by an MCS are examined by simulating the 8 May 2009 "Super-Derecho" MCS. The MCS was simulated using the Regional Atmospheric Modeling System (RAMS), a cloud-resolving model (CRM) with sophisticated aerosol and microphysical parameterizations. Three simulations were conducted that varied in their initial aerosol concentration, distribution and hygroscopicity as determined by their emission sources. The first simulation contained aerosols from only natural sources and the second with aerosols sourced from both natural and anthropogenic emissions The third simulation contained the same aerosol distribution as in the second simulation, however multiplied by a factor of 5 in order to represent a highly polluted scenario. In all three of the

Impact of Aerosol Processing on Orographic Clouds

Science.gov (United States)

Pousse-Nottelmann, Sara; Zubler, Elias M.; Lohmann, Ulrike

2010-05-01

Aerosol particles undergo significant modifications during their residence time in the atmosphere. Physical processes like coagulation, coating and water uptake, and aqueous surface chemistry alter the aerosol size distribution and composition. At this, clouds play a primary role as physical and chemical processing inside cloud droplets contributes considerably to the changes in aerosol particles. A previous study estimates that on global average atmospheric particles are cycled three times through a cloud before being removed from the atmosphere [1]. An explicit and detailed treatment of cloud-borne particles has been implemented in the regional weather forecast and climate model COSMO-CLM. The employed model version includes a two-moment cloud microphysical scheme [2] that has been coupled to the aerosol microphysical scheme M7 [3] as described by Muhlbauer and Lohmann, 2008 [4]. So far, the formation, transfer and removal of cloud-borne aerosol number and mass were not considered in the model. Following the parameterization for cloud-borne particles developed by Hoose et al., 2008 [5], distinction between in-droplet and in-crystal particles is made to more physically account for processes in mixed-phase clouds, such as the Wegener-Bergeron-Findeisen process and contact and immersion freezing. In our model, this approach has been extended to allow for aerosol particles in five different hydrometeors: cloud droplets, rain drops, ice crystals, snow flakes and graupel. We account for nucleation scavenging, freezing and melting processes, autoconversion, accretion, aggregation, riming and selfcollection, collisions between interstitial aerosol particles and hydrometeors, ice multiplication, sedimentation, evaporation and sublimation. The new scheme allows an evaluation of the cloud cycling of aerosol particles by tracking the particles even when scavenged into hydrometeors. Global simulations of aerosol processing in clouds have recently been conducted by Hoose et al

International Workshop on Stratospheric Aerosols: Measurements, Properties, and Effects

Science.gov (United States)

Pueschel, Rudolf F. (Editor)

1991-01-01

Following a mandate by the International Aerosol Climatology Program under the auspices of International Association of Meteorology and Atmospheric Physics International Radiation Commission, 45 scientists from five nations convened to discuss relevant issues associated with the measurement, properties, and effects of stratospheric aerosols. A summary is presented of the discussions on formation and evolution, transport and fate, effects on climate, role in heterogeneous chemistry, and validation of lidar and satellite remote sensing of stratospheric aerosols. Measurements are recommended of the natural (background) and the volcanically enhanced aerosol (sulfuric acid and silica particles), the exhaust of shuttle, civil aviation and supersonic aircraft operations (alumina, soot, and ice particles), and polar stratospheric clouds (ice, condensed nitric and hydrochloric acids).

Secondary organic aerosol formation from in situ OH, O3, and NO3 oxidation of ambient forest air in an oxidation flow reactor

Science.gov (United States)

Palm, Brett B.; Campuzano-Jost, Pedro; Day, Douglas A.; Ortega, Amber M.; Fry, Juliane L.; Brown, Steven S.; Zarzana, Kyle J.; Dube, William; Wagner, Nicholas L.; Draper, Danielle C.; Kaser, Lisa; Jud, Werner; Karl, Thomas; Hansel, Armin; Gutiérrez-Montes, Cándido; Jimenez, Jose L.

2017-04-01

Ambient pine forest air was oxidized by OH, O3, or NO3 radicals using an oxidation flow reactor (OFR) during the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics and Nitrogen - Rocky Mountain Biogenic Aerosol Study) campaign to study biogenic secondary organic aerosol (SOA) formation and organic aerosol (OA) aging. A wide range of equivalent atmospheric photochemical ages was sampled, from hours up to days (for O3 and NO3) or weeks (for OH). Ambient air processed by the OFR was typically sampled every 20-30 min, in order to determine how the availability of SOA precursor gases in ambient air changed with diurnal and synoptic conditions, for each of the three oxidants. More SOA was formed during nighttime than daytime for all three oxidants, indicating that SOA precursor concentrations were higher at night. At all times of day, OH oxidation led to approximately 4 times more SOA formation than either O3 or NO3 oxidation. This is likely because O3 and NO3 will only react with gases containing C = C bonds (e.g., terpenes) to form SOA but will not react appreciably with many of their oxidation products or any species in the gas phase that lacks a C = C bond (e.g., pinonic acid, alkanes). In contrast, OH can continue to react with compounds that lack C = C bonds to produce SOA. Closure was achieved between the amount of SOA formed from O3 and NO3 oxidation in the OFR and the SOA predicted to form from measured concentrations of ambient monoterpenes and sesquiterpenes using published chamber yields. This is in contrast to previous work at this site (Palm et al., 2016), which has shown that a source of SOA from semi- and intermediate-volatility organic compounds (S/IVOCs) 3.4 times larger than the source from measured VOCs is needed to explain the measured SOA formation from OH oxidation. This work suggests that those S/IVOCs typically do not contain C = C bonds. O3 and NO3 oxidation produced SOA with elemental O : C and H : C

Aerosol optical properties and radiative effects over Manora Peak in the Himalayan foothills: seasonal variability and role of transported aerosols

Energy Technology Data Exchange (ETDEWEB)

Srivastava, A.K. [Indian Institute of Tropical Meteorology (Branch), Prof Ramnath Vij Marg, New Delhi (India); Ram, K. [Institute of Environment and Sustainable Development, Banaras Hindu University, Varanasi (India); Singh, Sachchidanand, E-mail: ssingh@nplindia.org [Radio and Atmospheric Sciences Division, CSIR-National Physical Laboratory, New Delhi (India); Kumar, Sanjeev [Radio and Atmospheric Sciences Division, CSIR-National Physical Laboratory, New Delhi (India); Tiwari, S. [Indian Institute of Tropical Meteorology (Branch), Prof Ramnath Vij Marg, New Delhi (India)

2015-01-01

The higher altitude regions of Himalayas and Tibetan Plateau are influenced by the dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. In this study, we present impacts of advection of polluted air masses of natural and anthropogenic emissions, on aerosol optical and radiative properties at Manora Peak (∼ 2000 m amsl) in central Himalaya over a period of more than two years (February 2006–May 2008). We used the most updated and comprehensive data of chemical and optical properties available in one of the most climatically sensitive region, the Himalaya, to estimate atmospheric radiative forcing and heating rate. Aerosol optical depth (AOD) was found to vary from 0.04 to 0.45 with significantly higher values in summer mainly due to an increase in mineral dust and biomass burning aerosols due to transport. In contrast, single scattering albedo (SSA) varied from 0.74 to 0.88 with relatively lower values during summer, suggesting an increase in absorbing BC and mineral dust aerosols. As a result, a large positive atmospheric radiative forcing (about 28 ± 5 Wm{sup −2}) and high values of corresponding heating rate (0.80 ± 0.14 Kday{sup −1}) has been found during summer. During the entire observation period, radiative forcing at the top of the atmosphere varied from − 2 to + 14 Wm{sup −2} and from − 3 to − 50 Wm{sup −2} at the surface whereas atmospheric forcing was in the range of 3 to 65 Wm{sup −2} resulting in a heating rate of 0.1–1.8 Kday{sup −1}. - Highlights: • Aerosol chemical and optical properties at Manora Peak, in central Himalaya, were significantly affected by dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. • Elevated AOD and lower SSA values were observed at Manora Peak during summer. • Enhancement in absorbing aerosols was observed during summer. • Large aerosol radiative forcing and heating rate was observed

Aerosol optical properties and radiative effects over Manora Peak in the Himalayan foothills: seasonal variability and role of transported aerosols

International Nuclear Information System (INIS)

Srivastava, A.K.; Ram, K.; Singh, Sachchidanand; Kumar, Sanjeev; Tiwari, S.

2015-01-01

The higher altitude regions of Himalayas and Tibetan Plateau are influenced by the dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. In this study, we present impacts of advection of polluted air masses of natural and anthropogenic emissions, on aerosol optical and radiative properties at Manora Peak (∼ 2000 m amsl) in central Himalaya over a period of more than two years (February 2006–May 2008). We used the most updated and comprehensive data of chemical and optical properties available in one of the most climatically sensitive region, the Himalaya, to estimate atmospheric radiative forcing and heating rate. Aerosol optical depth (AOD) was found to vary from 0.04 to 0.45 with significantly higher values in summer mainly due to an increase in mineral dust and biomass burning aerosols due to transport. In contrast, single scattering albedo (SSA) varied from 0.74 to 0.88 with relatively lower values during summer, suggesting an increase in absorbing BC and mineral dust aerosols. As a result, a large positive atmospheric radiative forcing (about 28 ± 5 Wm −2 ) and high values of corresponding heating rate (0.80 ± 0.14 Kday −1 ) has been found during summer. During the entire observation period, radiative forcing at the top of the atmosphere varied from − 2 to + 14 Wm −2 and from − 3 to − 50 Wm −2 at the surface whereas atmospheric forcing was in the range of 3 to 65 Wm −2 resulting in a heating rate of 0.1–1.8 Kday −1 . - Highlights: • Aerosol chemical and optical properties at Manora Peak, in central Himalaya, were significantly affected by dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. • Elevated AOD and lower SSA values were observed at Manora Peak during summer. • Enhancement in absorbing aerosols was observed during summer. • Large aerosol radiative forcing and heating rate was observed over the station in the

Aerosol typing - key information from aerosol studies

Science.gov (United States)

Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

2016-04-01

Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

Dust plume formation in the free troposphere and aerosol size distribution during the Saharan Mineral Dust Experiment in North Africa

KAUST Repository

Khan, Basit Ali

2015-11-27

Dust particles mixed in the free troposphere have longer lifetimes than airborne particles near the surface. Their cumulative radiative impact on earth’s meteorological processes and climate might be significant despite their relatively small contribution to total dust abundance. One example is the elevated dust-laden Saharan Air Layer (SAL) over the tropical and subtropical North Atlantic, which cools the sea surface. To understand the formation mechanisms of a dust layer in the free troposphere, this study combines model simulations and dust observations collected during the first stage of the Saharan Mineral Dust Experiment (SAMUM-I), which sampled dust events that extended from Morocco to Portugal, and investigated the spatial distribution and the microphysical, optical, chemical, and radiative properties of Saharan mineral dust. The Weather Research Forecast model coupled with the Chemistry/Aerosol module (WRF-Chem) is employed to reproduce the meteorological environment and spatial and size distributions of dust. The model domain covers northwest Africa and adjacent water with 5 km horizontal grid spacing and 51 vertical layers. The experiments were run from 20 May to 9 June 2006, covering the period of the most intensive dust outbreaks. Comparisons of model results with available airborne and ground-based observations show that WRF-Chem reproduces observed meteorological fields as well as aerosol distribution across the entire region and along the airplane’s tracks. Several mechanisms that cause aerosol entrainment into the free troposphere are evaluated and it is found that orographic lifting, and interaction of sea breeze with the continental outflow are key mechanisms that form a surface-detached aerosol plume over the ocean. The model dust emission scheme is tuned to simultaneously fit the observed total optical depth and the ratio of aerosol optical depths generated by fine and coarse dust modes. Comparisons of simulated dust size distributions with

Dust plume formation in the free troposphere and aerosol size distribution during the Saharan Mineral Dust Experiment in North Africa

Directory of Open Access Journals (Sweden)

Basit Khan

2015-11-01

Full Text Available Dust particles mixed in the free troposphere have longer lifetimes than airborne particles near the surface. Their cumulative radiative impact on earth's meteorological processes and climate might be significant despite their relatively small contribution to total dust abundance. One example is the elevated dust-laden Saharan Air Layer (SAL over the tropical and subtropical North Atlantic, which cools the sea surface. To understand the formation mechanisms of a dust layer in the free troposphere, this study combines model simulations and dust observations collected during the first stage of the Saharan Mineral Dust Experiment (SAMUM-I, which sampled dust events that extended from Morocco to Portugal, and investigated the spatial distribution and the microphysical, optical, chemical, and radiative properties of Saharan mineral dust. The Weather Research Forecast model coupled with the Chemistry/Aerosol module (WRF-Chem is employed to reproduce the meteorological environment and spatial and size distributions of dust. The model domain covers northwest Africa and adjacent water with 5 km horizontal grid spacing and 51 vertical layers. The experiments were run from 20 May to 9 June 2006, covering the period of the most intensive dust outbreaks. Comparisons of model results with available airborne and ground-based observations show that WRF-Chem reproduces observed meteorological fields as well as aerosol distribution across the entire region and along the airplane's tracks. Several mechanisms that cause aerosol entrainment into the free troposphere are evaluated and it is found that orographic lifting, and interaction of sea breeze with the continental outflow are key mechanisms that form a surface-detached aerosol plume over the ocean. The model dust emission scheme is tuned to simultaneously fit the observed total optical depth and the ratio of aerosol optical depths generated by fine and coarse dust modes. Comparisons of simulated dust size

Factor analysis of combined organic and inorganic aerosol mass spectra from high resolution aerosol mass spectrometer measurements

Directory of Open Access Journals (Sweden)

Y. L. Sun

2012-09-01

Full Text Available Positive matrix factorization (PMF was applied to the merged high resolution mass spectra of organic and inorganic aerosols from aerosol mass spectrometer (AMS measurements to investigate the sources and evolution processes of submicron aerosols in New York City in summer 2009. This new approach is able to study the distribution of organic and inorganic species in different types of aerosols, the acidity of organic aerosol (OA factors, and the fragment ion patterns related to photochemical processing. In this study, PMF analysis of the unified AMS spectral matrix resolved 8 factors. The hydrocarbon-like OA (HOA and cooking OA (COA factors contain negligible amounts of inorganic species. The two factors that are primarily ammonium sulfate (SO₄-OA and ammonium nitrate (NO₃-OA, respectively, are overall neutralized. Among all OA factors the organic fraction of SO₄-OA shows the highest degree of oxidation (O/C = 0.69. Two semi-volatile oxygenated OA (OOA factors, i.e., a less oxidized (LO-OOA and a more oxidized (MO-OOA, were also identified. MO-OOA represents local photochemical products with a diurnal profile exhibiting a pronounced noon peak, consistent with those of formaldehyde (HCHO and O_x(= O₃ + NO₂. The NO⁺/NO₂⁺ ion ratio in MO-OOA is much higher than that in NO₃-OA and in pure ammonium nitrate, indicating the formation of organic nitrates. The nitrogen-enriched OA (NOA factor contains ~25% of acidic inorganic salts, suggesting the formation of secondary OA via acid-base reactions of amines. The size distributions of OA factors derived from the size-resolved mass spectra show distinct diurnal evolving behaviors but overall a progressing evolution from smaller to larger particle mode as the oxidation degree of OA increases. Our results demonstrate that PMF analysis of the unified aerosol mass spectral matrix which contains both

Aerosol numerical modelling at local scale

International Nuclear Information System (INIS)

Albriet, Bastien

2007-01-01

At local scale and in urban areas, an important part of particulate pollution is due to traffic. It contributes largely to the high number concentrations observed. Two aerosol sources are mainly linked to traffic. Primary emission of soot particles and secondary nanoparticle formation by nucleation. The emissions and mechanisms leading to the formation of such bimodal distribution are still badly understood nowadays. In this thesis, we try to provide an answer to this problematic by numerical modelling. The Modal Aerosol Model MAM is used, coupled with two 3D-codes: a CFD (Mercure Saturne) and a CTM (Polair3D). A sensitivity analysis is performed, at the border of a road but also in the first meters of an exhaust plume, to identify the role of each process involved and the sensitivity of different parameters used in the modelling. (author) [fr

Improving organic aerosol treatments in CESM/CAM5: Development, application, and evaluation

Science.gov (United States)

Glotfelty, Timothy; He, Jian

2017-01-01

Abstract New treatments for organic aerosol (OA) formation have been added to a modified version of the CESM/CAM5 model (CESM‐NCSU). These treatments include a volatility basis set treatment for the simulation of primary and secondary organic aerosols (SOAs), a simplified treatment for organic aerosol (OA) formation from glyoxal, and a parameterization representing the impact of new particle formation (NPF) of organic gases and sulfuric acid. With the inclusion of these new treatments, the concentration of oxygenated organic aerosol increases by 0.33 µg m−3 and that of primary organic aerosol (POA) decreases by 0.22 µg m−3 on global average. The decrease in POA leads to a reduction in the OA direct effect, while the increased OOA increases the OA indirect effects. Simulations with the new OA treatments show considerable improvement in simulated SOA, oxygenated organic aerosol (OOA), organic carbon (OC), total carbon (TC), and total organic aerosol (TOA), but degradation in the performance of HOA. In simulations of the current climate period, despite some deviations from observations, CESM‐NCSU with the new OA treatments significantly improves the magnitude, spatial pattern, seasonal pattern of OC and TC, as well as, the speciation of TOA between POA and OOA. Sensitivity analysis reveals that the inclusion of the organic NPF treatment impacts the OA indirect effects by enhancing cloud properties. The simulated OA level and its impact on the climate system are most sensitive to choices in the enthalpy of vaporization and wet deposition of SVOCs, indicating that accurate representations of these parameters are critical for accurate OA‐climate simulations. PMID:29104733

Updating the FORECAST formative evaluation approach and some implications for ameliorating theory failure, implementation failure, and evaluation failure

Science.gov (United States)

Katz, Jason; Wandersman, Abraham; Goodman, Robert M.; Griffin, Sarah; Wilson, Dawn K.; Schillaci, Michael

2013-01-01

Historically, there has been considerable variability in how formative evaluation has been conceptualized and practiced. FORmative Evaluation Consultation And Systems Technique (FORECAST) is a formative evaluation approach that develops a set of models and processes that can be used across settings and times, while allowing for local adaptations and innovations. FORECAST integrates specific models and tools to improve limitations in program theory, implementation, and evaluation. In the period since its initial use in a federally funded community prevention project in the early 1990s, evaluators have incorporated important formative evaluation innovations into FORECAST, including the integration of feedback loops and proximal outcome evaluation. In addition, FORECAST has been applied in a randomized community research trial. In this article, we describe updates to FORECAST and the implications of FORECAST for ameliorating failures in program theory, implementation, and evaluation. PMID:23624204

Possible influence of anthropogenic aerosols on cirrus clouds and anthropogenic forcing

Directory of Open Access Journals (Sweden)

J. E. Penner

2009-02-01

Full Text Available Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. Here, we examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning, from anthropogenic sulfate aerosols, and from aircraft that deposit their aerosols directly in the upper troposphere. We use a version of the aerosol model that predicts sulfate number and mass concentrations in 3-modes and includes the formation of sulfate aerosol through homogeneous binary nucleation as well as a version that only predicts sulfate mass. The 3-mode version best represents the Aitken aerosol nuclei number concentrations in the upper troposphere which dominated ice crystal residues in the upper troposphere. Fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of −0.3 to −0.4 Wm⁻² while anthropogenic sulfate aerosols and aircraft aerosols exert a forcing of −0.01 to 0.04 Wm⁻² and −0.16 to −0.12 Wm⁻², respectively, where the range represents the forcing from two parameterizations for ice nucleation. The sign of the forcing in the mass-only version of the model depends on which ice nucleation parameterization is used and can be either positive or negative. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds, but this forcing has not been included in past assessments of the total anthropogenic radiative forcing of climate.

Impact of aerosols on ice crystal size

Science.gov (United States)

Zhao, Bin; Liou, Kuo-Nan; Gu, Yu; Jiang, Jonathan H.; Li, Qinbin; Fu, Rong; Huang, Lei; Liu, Xiaohong; Shi, Xiangjun; Su, Hui; He, Cenlin

2018-01-01

The interactions between aerosols and ice clouds represent one of the largest uncertainties in global radiative forcing from pre-industrial time to the present. In particular, the impact of aerosols on ice crystal effective radius (Rei), which is a key parameter determining ice clouds' net radiative effect, is highly uncertain due to limited and conflicting observational evidence. Here we investigate the effects of aerosols on Rei under different meteorological conditions using 9-year satellite observations. We find that the responses of Rei to aerosol loadings are modulated by water vapor amount in conjunction with several other meteorological parameters. While there is a significant negative correlation between Rei and aerosol loading in moist conditions, consistent with the "Twomey effect" for liquid clouds, a strong positive correlation between the two occurs in dry conditions. Simulations based on a cloud parcel model suggest that water vapor modulates the relative importance of different ice nucleation modes, leading to the opposite aerosol impacts between moist and dry conditions. When ice clouds are decomposed into those generated from deep convection and formed in situ, the water vapor modulation remains in effect for both ice cloud types, although the sensitivities of Rei to aerosols differ noticeably between them due to distinct formation mechanisms. The water vapor modulation can largely explain the difference in the responses of Rei to aerosol loadings in various seasons. A proper representation of the water vapor modulation is essential for an accurate estimate of aerosol-cloud radiative forcing produced by ice clouds.

Aerosols, clouds and their climatic impacts

Energy Technology Data Exchange (ETDEWEB)

Kulmala, M; Laaksonen, A; Korhonen, P [Helsinki Univ. (Finland). Dept. of Physics

1996-12-31

The increasing atmospheric concentrations of greenhouse gases such as carbon dioxide and methane may drive a significant warming of the earth`s climate. However, a topic of more recent attention is the possibility that increased atmospheric concentrations of aerosol particles might drive a cooling of the planet. There are two distinct cooling mechanisms related to the enhanced concentrations of aerosol particles: the increase in the direct reflection of solar radiation (the direct effect), and the increase in cloud reflectivity caused by greater numbers of cloud condensation nuclei available (the indirect effect). Aerosols and clouds play a major role in the scattering and absorption of radiation in the Earth`s atmosphere. Locally the net effect can vary because of different kinds of surfaces. But according to measurements, the global net effect of clouds (and aerosols) on the atmosphere is net cooling and thus in opposition to the effect of greenhouse gases. The prediction of the future evolution of the climate involves substantial uncertainties. Clouds have a major effect on the radiation balance of the Earth and the prediction of amount and radiative properties of clouds is very difficult. Also the formation mechanisms and residence times of aerosol particles in the atmosphere involve large uncertainties. Thus the most serious difficulties arise in the area of the physics of clouds and aerosols

Aerosols, clouds and their climatic impacts

Energy Technology Data Exchange (ETDEWEB)

Kulmala, M.; Laaksonen, A.; Korhonen, P. [Helsinki Univ. (Finland). Dept. of Physics

1995-12-31

The increasing atmospheric concentrations of greenhouse gases such as carbon dioxide and methane may drive a significant warming of the earth`s climate. However, a topic of more recent attention is the possibility that increased atmospheric concentrations of aerosol particles might drive a cooling of the planet. There are two distinct cooling mechanisms related to the enhanced concentrations of aerosol particles: the increase in the direct reflection of solar radiation (the direct effect), and the increase in cloud reflectivity caused by greater numbers of cloud condensation nuclei available (the indirect effect). Aerosols and clouds play a major role in the scattering and absorption of radiation in the Earth`s atmosphere. Locally the net effect can vary because of different kinds of surfaces. But according to measurements, the global net effect of clouds (and aerosols) on the atmosphere is net cooling and thus in opposition to the effect of greenhouse gases. The prediction of the future evolution of the climate involves substantial uncertainties. Clouds have a major effect on the radiation balance of the Earth and the prediction of amount and radiative properties of clouds is very difficult. Also the formation mechanisms and residence times of aerosol particles in the atmosphere involve large uncertainties. Thus the most serious difficulties arise in the area of the physics of clouds and aerosols

Modeling organic aerosol concentrations and properties during winter 2014 in the northwestern Mediterranean region

OpenAIRE

Chrit, Mounir; Sartelet, Karine; Sciare, Jean; Majdi, Marwa; Nicolas, José; Petit, Jean-Eudes; Dulac, François

2018-01-01

Organic aerosols are measured at a remote site (Ersa) on Corsica Cape in the northwestern Mediterranean basin during the Chemistry-Aerosol Mediterranean Experiment (CharMEx) winter campaign of 2014, when high organic concentrations from anthropogenic origin are observed. This work aims at representing the observed organic aerosol concentrations and properties (oxidation state) using the air-quality model Polyphemus with a surrogate approach for secondary organic aerosol (SOA) formation. Becau...

Kinetic modeling studies of SOA formation from α-pinene ozonolysis

Science.gov (United States)

Gatzsche, Kathrin; Iinuma, Yoshiteru; Tilgner, Andreas; Mutzel, Anke; Berndt, Torsten; Wolke, Ralf

2017-11-01

This paper describes the implementation of a kinetic gas-particle partitioning approach used for the simulation of secondary organic aerosol (SOA) formation within the SPectral Aerosol Cloud Chemistry Interaction Model (SPACCIM). The kinetic partitioning considers the diffusion of organic compounds into aerosol particles and the subsequent chemical reactions in the particle phase. The basic kinetic partitioning approach is modified by the implementation of chemical backward reaction of the solute within the particle phase as well as a composition-dependent particle-phase bulk diffusion coefficient. The adapted gas-phase chemistry mechanism for α-pinene oxidation has been updated due to the recent findings related to the formation of highly oxidized multifunctional organic compounds (HOMs). Experimental results from a LEAK (Leipziger Aerosolkammer) chamber study for α-pinene ozonolysis were compared with the model results describing this reaction system.The performed model studies reveal that the particle-phase bulk diffusion coefficient and the particle-phase reactivity are key parameters for SOA formation. Using the same particle-phase reactivity for both cases, we find that liquid particles with higher particle-phase bulk diffusion coefficients have 310 times more organic material formed in the particle phase compared to higher viscous semi-solid particles with lower particle-phase bulk diffusion coefficients. The model results demonstrate that, even with a moderate particle-phase reactivity, about 61 % of the modeled organic mass consists of reaction products that are formed in the liquid particles. This finding emphasizes the potential role of SOA processing. Moreover, the initial organic aerosol mass concentration and the particle radius are of minor importance for the process of SOA formation in liquid particles. A sensitivity study shows that a 22-fold increase in particle size merely leads to a SOA increase of less than 10 %.Due to two additional

Recent advances in understanding secondary organic aerosol: Implications for global climate forcing

Science.gov (United States)

Shrivastava, Manish; Cappa, Christopher D.; Fan, Jiwen; Goldstein, Allen H.; Guenther, Alex B.; Jimenez, Jose L.; Kuang, Chongai; Laskin, Alexander; Martin, Scot T.; Ng, Nga Lee; Petaja, Tuukka; Pierce, Jeffrey R.; Rasch, Philip J.; Roldin, Pontus; Seinfeld, John H.; Shilling, John; Smith, James N.; Thornton, Joel A.; Volkamer, Rainer; Wang, Jian; Worsnop, Douglas R.; Zaveri, Rahul A.; Zelenyuk, Alla; Zhang, Qi

2017-06-01

Anthropogenic emissions and land use changes have modified atmospheric aerosol concentrations and size distributions over time. Understanding preindustrial conditions and changes in organic aerosol due to anthropogenic activities is important because these features (1) influence estimates of aerosol radiative forcing and (2) can confound estimates of the historical response of climate to increases in greenhouse gases. Secondary organic aerosol (SOA), formed in the atmosphere by oxidation of organic gases, represents a major fraction of global submicron-sized atmospheric organic aerosol. Over the past decade, significant advances in understanding SOA properties and formation mechanisms have occurred through measurements, yet current climate models typically do not comprehensively include all important processes. This review summarizes some of the important developments during the past decade in understanding SOA formation. We highlight the importance of some processes that influence the growth of SOA particles to sizes relevant for clouds and radiative forcing, including formation of extremely low volatility organics in the gas phase, acid-catalyzed multiphase chemistry of isoprene epoxydiols, particle-phase oligomerization, and physical properties such as volatility and viscosity. Several SOA processes highlighted in this review are complex and interdependent and have nonlinear effects on the properties, formation, and evolution of SOA. Current global models neglect this complexity and nonlinearity and thus are less likely to accurately predict the climate forcing of SOA and project future climate sensitivity to greenhouse gases. Efforts are also needed to rank the most influential processes and nonlinear process-related interactions, so that these processes can be accurately represented in atmospheric chemistry-climate models.

Volatile organic compounds and secondary organic aerosol in the Earth's atmosphere

International Nuclear Information System (INIS)

Galbally, Ian

2007-01-01

Full text: Recent research, when considered as a whole, suggests that a substantial fraction of both gas-phase and aerosol atmospheric organics have not been, or have very rarely been, directly measured. A review of the global budget for organic gases shows that we cannot account for the loss of approximately half the non-methane organic carbon entering the atmosphere. We suggest that this unaccounted-for loss most likely occurs through formation of secondary organic aerosols (SOAs), indicating that the source for these aerosols is an order of magnitude larger than current estimates. There is evidence that aged secondary organic aerosol can participate in both direct and indirect (cloud modifying) radiative forcing and that this influence may change with other global climate change. Even though our knowledge of the organic composition of the atmosphere is limited, these compounds clearly influence the reactive chemistry of the atmosphere and the formation, composition, and climate impact of aerosols A major challenge in the coming decade of atmospheric chemistry research will be to elucidate the sources, structure, chemistry, fate and influences of these clearly ubiquitous yet poorly constrained organic atmospheric constituents

Development and testing of an aerosol-stratus cloud parameterization scheme for middle and high latitudes

Energy Technology Data Exchange (ETDEWEB)

Olsson, P.Q.; Meyers, M.P.; Kreidenweis, S.; Cotton, W.R. [Colorado State Univ., Fort Collins, CO (United States)

1996-04-01

The aim of this new project is to develop an aerosol/cloud microphysics parameterization of mixed-phase stratus and boundary layer clouds. Our approach is to create, test, and implement a bulk-microphysics/aerosol model using data from Atmospheric Radiation Measurement (ARM) Cloud and Radiation Testbed (CART) sites and large-eddy simulation (LES) explicit bin-resolving aerosol/microphysics models. The primary objectives of this work are twofold. First, we need the prediction of number concentrations of activated aerosol which are transferred to the droplet spectrum, so that the aerosol population directly affects the cloud formation and microphysics. Second, we plan to couple the aerosol model to the gas and aqueous-chemistry module that will drive the aerosol formation and growth. We begin by exploring the feasibility of performing cloud-resolving simulations of Arctic stratus clouds over the North Slope CART site. These simulations using Colorado State University`s regional atmospheric modeling system (RAMS) will be useful in designing the structure of the cloud-resolving model and in interpreting data acquired at the North Slope site.

The relative importance of competing pathways for the formation of high-molecular-weight peroxides in the ozonolysis of organic aerosol particles

Directory of Open Access Journals (Sweden)

M. Mochida

2006-01-01

Full Text Available High-molecular-weight (HMW organic compounds are an important component of atmospheric particles, although their origins, possibly including in situ formation pathways, remain incompletely understood. This study investigates the formation of HMW organic peroxides through reactions involving stabilized Criegee intermediates (SCI's. The model system is methyl oleate (MO mixed with dioctyl adipate (DOA and myristic acid (MA in submicron aerosol particles, and Criegee intermediates are formed by the ozonolysis of the double bond in methyl oleate. An aerosol flow tube coupled to a quadrupole aerosol mass spectrometer (AMS is employed to determine the relative importance of different HMW organic peroxides following the ozonolysis of different mixing mole fractions of MO in DOA and MA. Possible peroxide products include secondary ozonides (SOZ's, α-acyloxyalkyl hydroperoxides and α-acyloxyalkyl alkyl peroxides (αAAHP-type compounds, diperoxides, and monoperoxide oligomers. Of these, the AMS data identify two SOZ's as major HMW products in the ozonolysis of pure methyl oleate as well as in an inert matrix of DOA to as low as 0.04 mole fraction MO. In comparison, in mixed particles of MO and MA, αAAHP-type compounds form in high yields for MO mole fractions of 0.5 or less, suggesting that SCI's efficiently attack the carboxylic acid group of myristic acid. The reactions of SCI's with carboxylic acid groups to form αAAHP-type compounds therefore compete with those of SCI's with aldehydes to form SOZ's, provided that both types of functionalities are present at significant concentrations. The results therefore suggest that SCI's in atmospheric particles contribute to the transformation of carboxylic acids and other protic groups into HMW organic peroxides.

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.

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

Aerosol lung inhalation scintigraphy in children with bronchial asthma

International Nuclear Information System (INIS)

Torii, Yoshikuni; Nakayama, Chikashi; Nakata, Hajime; Takahashi, Satomi; Tanaka, Masaaki; Koori, Tateo

1988-01-01

Aerosol lung inhalation scintigraphies performed on 37 children with bronchial asthma during asymptomatic periods were evaluated. The findings of their aerosol lung inhalation scintigrams were classified into 4 patterns, as type I: homogeneous distribution without hot spot formation, type II: peripheral homogeneity with central hot spot formation, type IIID (-): inhomogeneous distribution with hot spot formation, but without defect, and type IIID (+): with defect. These aerosol patterns were compared with those of previously reported adult cases and with the severity of bronchial asthma. Normal pattern of type I was found in 5 cases (12%) of our infantile asthmatics in contrast to previously reported adult cases, in which none of normal pattern was found. There were differences between type II and type III in both distribution and disappearance time of hot spot, which indicated that the two types differed from each other in radioaerosol deposition mechanism. There was no significant correlation between type I and type II in the severity of asthma and the frequency of asthmatic attack. Type II may be clinically considered to be the same type as type I. There is the statistically significant difference between type I, II and type III in the frequency of asthmatic attack, but not in the severity of asthma, although most of serious cases showed type III. Aerosol lung inhalation scintigraphy is a useful examination for children with bronchial asthma in which lung function tests may be difficult to perform. (author)

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.

Observations of gas- and aerosol-phase organic nitrates at BEACHON-RoMBAS 2011

Directory of Open Access Journals (Sweden)

J. L. Fry

2013-09-01

Full Text Available At the Rocky Mountain Biogenic Aerosol Study (BEACHON-RoMBAS field campaign in the Colorado front range, July–August 2011, measurements of gas- and aerosol-phase organic nitrates enabled a study of the role of NOx (NOx = NO + NO2 in oxidation of forest-emitted volatile organic compounds (VOCs and subsequent aerosol formation. Substantial formation of peroxy- and alkyl-nitrates is observed every morning, with an apparent 2.9% yield of alkyl nitrates from daytime RO2 + NO reactions. Aerosol-phase organic nitrates, however, peak in concentration during the night, with concentrations up to 140 ppt as measured by both optical spectroscopic and mass spectrometric instruments. The diurnal cycle in aerosol fraction of organic nitrates shows an equilibrium-like response to the diurnal temperature cycle, suggesting some reversible absorptive partitioning, but the full dynamic range cannot be reproduced by thermodynamic repartitioning alone. Nighttime aerosol organic nitrate is observed to be positively correlated with [NO2] × [O3] but not with [O3]. These observations support the role of nighttime NO3-initiated oxidation of monoterpenes as a significant source of nighttime aerosol. Nighttime production of organic nitrates is comparable in magnitude to daytime photochemical production at this site, which we postulate to be representative of the Colorado front range forests.

Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

Science.gov (United States)

Kirpes, Rachel M.; Bondy, Amy L.; Bonanno, Daniel; Moffet, Ryan C.; Wang, Bingbing; Laskin, Alexander; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Few measurements of aerosol chemical composition have been made during the winter-spring transition (following polar sunrise) to constrain Arctic aerosol-cloud-climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24 847 particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5-7.5 µm diameter particles, 65-95 % from 0.5-2.5 µm, and 50-60 % from 0.1-0.5 µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with 94 %, by number, internally mixed with secondary sulfate (39 %, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40 % of 1.0-4.0 µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay, consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40-50 %, by number, of 0.1-0.4 µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. Therefore, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud

Organic condensation: a vital link connecting aerosol formation to cloud condensation nuclei (CCN) concentrations

Science.gov (United States)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petäjä, T.; Slowik, J.; Chang, R.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.-M.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M.

2011-04-01

Atmospheric aerosol particles influence global climate as well as impair air quality through their effects on atmospheric visibility and human health. Ultrafine (<100 nm) particles often dominate aerosol numbers, and nucleation of atmospheric vapors is an important source of these particles. To have climatic relevance, however, the freshly nucleated particles need to grow in size. We combine observations from two continental sites (Egbert, Canada and Hyytiälä, Finland) to show that condensation of organic vapors is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We model the observed ultrafine aerosol growth with a simplified scheme approximating the condensing species as a mixture of effectively non-volatile and semi-volatile species, demonstrate that state-of-the-art organic gas-particle partitioning models fail to reproduce the observations, and propose a modeling approach that is consistent with the measurements. We find that roughly half of the mass of the condensing mass needs to be distributed proportional to the aerosol surface area (thus implying that the condensation is governed by gas-phase concentration rather than the equilibrium vapour pressure) to explain the observed aerosol growth. We demonstrate the large sensitivity of predicted number concentrations of cloud condensation nuclei (CCN) to these interactions between organic vapors and the smallest atmospheric nanoparticles - highlighting the need for representing this process in global climate models.

"Updates to Model Algorithms & Inputs for the Biogenic Emissions Inventory System (BEIS) Model"

Science.gov (United States)

We have developed new canopy emission algorithms and land use data for BEIS. Simulations with BEIS v3.4 and these updates in CMAQ v5.0.2 are compared these changes to the Model of Emissions of Gases and Aerosols from Nature (MEGAN) and evaluated the simulations against observatio...

A perspective on SOA generated in aerosol water from glyoxal and methylglyoxal and its impacts on climate-relevant aerosol properties

Science.gov (United States)

Sareen, N.; McNeill, V. F.

2011-12-01

In recent years, glyoxal and methylglyoxal have emerged to be potentially important SOA precursors with significant implications for climate-related aerosol properties. Here we will discuss how the chemistry of these and similar organic compounds in aerosol water can affect the aerosol optical and cloud formation properties. Aqueous-phase SOA production from glyoxal and methylglyoxal is a potential source of strongly light-absorbing organics, or "brown carbon". We characterized the kinetics of brown carbon formation from these precursors in mixtures of ammonium sulfate and water using UV-Vis spectrophotometry. This mechanism has been incorporated into a photochemical box model with coupled gas phase-aqueous aerosol chemistry. Methylglyoxal and related compounds also may impact an aerosol's ability to act as a cloud condensation nucleus. We recently showed via pendant drop tensiometry and aerosol chamber studies that uptake of methylglyoxal from the gas phase driven by aqueous-phase oligomerization chemistry is a potentially significant, previously unidentified source of surface-active organic material in aerosols. Results from pendant drop tensiometry showed significantly depressed surface tension in methylglyoxal-ammonium sulfate solutions. We further found that ammonium sulfate particles exposed to gas-phase methylglyoxal in a 3.5 m3 aerosol reaction chamber activate into cloud droplets at sizes up to 15% lower at a given supersaturation than do pure ammonium sulfate particles. The observed enhancement exceeds that predicted based on Henry's Law and our measurements of surface tension depression in bulk solutions, suggesting that surface adsorption of methylglyoxal plays a role in determining CCN activity. Methylglyoxal and similar gas-phase surfactants may be an important and overlooked source of enhanced CCN activity in the atmosphere. To characterize the SOA products formed in these solutions, an Aerosol Chemical Ionization Mass Spectrometer (CIMS) was used

Formation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: evaluation of the volatility-basis-set approach within the CHIMERE model

Directory of Open Access Journals (Sweden)

Q. J. Zhang

2013-06-01

Full Text Available Simulations with the chemistry transport model CHIMERE are compared to measurements performed during the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation summer campaign in the Greater Paris region in July 2009. The volatility-basis-set approach (VBS is implemented into this model, taking into account the volatility of primary organic aerosol (POA and the chemical aging of semi-volatile organic species. Organic aerosol is the main focus and is simulated with three different configurations with a modified treatment of POA volatility and modified secondary organic aerosol (SOA formation schemes. In addition, two types of emission inventories are used as model input in order to test the uncertainty related to the emissions. Predictions of basic meteorological parameters and primary and secondary pollutant concentrations are evaluated, and four pollution regimes are defined according to the air mass origin. Primary pollutants are generally overestimated, while ozone is consistent with observations. Sulfate is generally overestimated, while ammonium and nitrate levels are well simulated with the refined emission data set. As expected, the simulation with non-volatile POA and a single-step SOA formation mechanism largely overestimates POA and underestimates SOA. Simulation of organic aerosol with the VBS approach taking into account the aging of semi-volatile organic compounds (SVOC shows the best correlation with measurements. High-concentration events observed mostly after long-range transport are well reproduced by the model. Depending on the emission inventory used, simulated POA levels are either reasonable or underestimated, while SOA levels tend to be overestimated. Several uncertainties related to the VBS scheme (POA volatility, SOA yields, the aging parameterization, to emission input data, and to simulated OH levels can be responsible for

Improving the representation of secondary organic aerosol (SOA in the MOZART-4 global chemical transport model

Directory of Open Access Journals (Sweden)

A. Mahmud

2013-07-01

Full Text Available The secondary organic aerosol (SOA module in the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4 was updated by replacing existing two-product (2p parameters with those obtained from two-product volatility basis set (2p-VBS fits (MZ4-C1, and by treating SOA formation from the following additional volatile organic compounds (VOCs: isoprene, propene and lumped alkenes (MZ4-C2. Strong seasonal and spatial variations in global SOA distributions were demonstrated, with significant differences in the predicted concentrations between the base case and updated model simulations. Updates to the model resulted in significant increases in annual average SOA mass concentrations, particularly for the MZ4-C2 simulation in which the additional SOA precursor VOCs were treated. Annual average SOA concentrations predicted by the MZ4-C2 simulation were 1.00 ± 1.04 μg m−3 in South America, 1.57 ± 1.88 μg m−3 in Indonesia, 0.37 ± 0.27 μg m−3 in the USA, and 0.47 ± 0.29 μg m−3 in Europe with corresponding increases of 178, 406, 311 and 292% over the base-case simulation, respectively, primarily due to inclusion of isoprene. The increases in predicted SOA mass concentrations resulted in corresponding increases in SOA contributions to annual average total aerosol optical depth (AOD by ~ 1–6%. Estimated global SOA production was 5.8, 6.6 and 19.1 Tg yr−1 with corresponding burdens of 0.22, 0.24 and 0.59 Tg for the base-case, MZ4-C1 and MZ4-C2 simulations, respectively. The predicted SOA budgets fell well within reported ranges for comparable modeling studies, 6.7 to 96 Tg yr−1, but were lower than recently reported observationally constrained values, 50 to 380 Tg yr−1. For MZ4-C2, simulated SOA concentrations at the surface also were in reasonable agreement with comparable modeling studies and observations. Total organic aerosol (OA mass concentrations at the surface, however, were slightly over-predicted in Europe, Amazonian

Carbonaceous aerosols from prescribed burning of a boreal forest ecosystem

Science.gov (United States)

Mazurek, Monica A.; Cofer, Wesley R., III; Levine, Joel S.

1991-01-01

During the boreal forest burn studied, the ambient concentrations for the particle carbon smoke aerosol are highest for the full-fire burn conditions and vary significantly throughout the burn. Collection strategies must accordingly define ranges in the smoke aerosol concentrations produced. While the highest elemental C concentrations are observed during full-fire conditions, the great majority of smoke aerosol particles are in the form of organic C particles irrespective of fire temperature. The formation of organic C light-scattering particles was a significant process in the burn studied.

Aerosol Optical Properties Derived from the DRAGON-NE Asia Campaign, and Implications for a Single-Channel Algorithm to Retrieve Aerosol Optical Depth in Spring from Meteorological Imager (MI) On-Board the Communication, Ocean, and Meteorological Satellite (COMS)

Science.gov (United States)

Kim, M.; Kim, J.; Jeong, U.; Kim, W.; Hong, H.; Holben, B.; Eck, T. F.; Lim, J.; Song, C.; Lee, S.;

Regional radiative impacts of mixed dust and carbonaceous aerosols over West Africa

Science.gov (United States)

Malavelle, Florent; Pont, Véronique; Solmon, Fabien; Mallet, Marc; Léon, Jean-François; Liousse, Catherine; Johnson, Ben

2010-05-01

Africa is a major source of aerosols at global scale. Two types of aerosols dominate the regional background: biomass burning aerosols as results of combustion of the vegetation and mineral dust aerosols related to erosion of arid soils by wind. These important burdens of aerosols are known to have each one a strong impact on the regional radiative budget. Whereas recent modelling efforts show significant impacts at climatic timescale on West African Monsoon due to the radiative effects of dust aerosols (see Solmon et al 2008 in GRL and references therein), biomass burning radiative effects in this region stand still poorly documented. What about West Africa, during the dry season (december-february) when both biomass burning and dust aerosols are encountered in the atmospheric background ? In that frame, we use ICTP Regional Climate Model versions 3 in order to estimate the radiative forcing due to the external mixing of mineral dust and carbonaceous aerosols from biomass burning, BioFuel and Fossil Fuel combustion during the dry season. Emissions of biomass burning aerosols are taken from new inventories based on SPOT vegetation burnt area products. Optical properties of carboneaceous aerosols are updated thanks to chemical sampling at Djougou during AMMA SOP-0. This presentation focuses on the model efficiency to correctly reproduce the main features concerning aerosols observed during AMMA-SOP0/DABEX field campaigns. It refers to (i) a strong stratification of dust and smoke layers, and (ii) a marked seasonal cycle of aerosol mixture optical properties. Those features are key parameters for modelling the direct and semi direct effects of aerosols over West Africa. Results of simulations indicate that the particular low value of single scattering albedo (SSA) for biomass burning aerosols (~0.81 at 550nm) involves important diabatic heating in the atmosphere. Values of aerosol heating rates are estimated and compared with aircraft measurement from DABEX

A GCM study of organic matter in marine aerosol and its potential contribution to cloud drop activation

Directory of Open Access Journals (Sweden)

G. J. Roelofs

2008-02-01

Full Text Available With the global aerosol-climate model ECHAM5-HAM we investigate the potential influence of organic aerosol originating from the ocean on aerosol mass and chemical composition and the droplet concentration and size of marine clouds. We present sensitivity simulations in which the uptake of organic matter in the marine aerosol is prescribed for each aerosol mode with varying organic mass and mixing state, and with a geographical distribution and seasonality similar to the oceanic emission of dimethyl sulfide. Measurements of aerosol mass, aerosol chemical composition and cloud drop effective radius are used to assess the representativity of the model initializations. Good agreement with the measurements is obtained when organic matter is added to the Aitken, accumulation and coarse modes simultaneously. Representing marine organics in the model leads to higher cloud drop number concentrations and thus smaller cloud drop effective radii, and this improves the agreement with measurements. The mixing state of the organics and the other aerosol matter, i.e. internal or external depending on the formation process of aerosol organics, is an important factor for this. We estimate that globally about 75 Tg C yr⁻¹ of organic matter from marine origin enters the aerosol phase, with comparable contributions from primary emissions and secondary organic aerosol formation.

Radiative forcing of the desert aerosol at Ouarzazate (Morocco)

Science.gov (United States)

Tahiri, Abdelouahid; Diouri, Mohamed

2018-05-01

The atmospheric aerosol contributes to the definition of the climate with direct effect, the diffusion and absorption of solar and terrestrial radiations, and indirect, the cloud formation process where aerosols behave as condensation nuclei and alter the optical properties. Satellites and ground-based networks (solar photometers) allow the terrestrial aerosol observation and the determination of impact. Desert aerosol considered among the main types of tropospheric aerosols whose optical property uncertainties are still quite important. The analysis concerns the optical parameters recorded in 2015 at Ouarzazate solar photometric station (AERONET/PHOTONS network, http://aeronet.gsfc.nasa.gov/) close to Saharan zone. The daily average aerosol optical depthτaer at 0.5μm, are relatively high in summer and less degree in spring (from 0.01 to 1.82). Daily average of the Angstrom coefficients α vary between 0.01 and 1.55. The daily average of aerosol radiative forcing at the surface range between -150W/m2 and -10 W/m2 with peaks recorded in summer, characterized locally by large loads of desert aerosol in agreement with the advections of the Southeast of Morocco. Those recorded at the Top of the atmosphere show a variation from -74 W/m2 to +24 W/m2

Impact of aerosols on ice crystal size

Directory of Open Access Journals (Sweden)

B. Zhao

2018-01-01

Full Text Available The interactions between aerosols and ice clouds represent one of the largest uncertainties in global radiative forcing from pre-industrial time to the present. In particular, the impact of aerosols on ice crystal effective radius (Rei, which is a key parameter determining ice clouds' net radiative effect, is highly uncertain due to limited and conflicting observational evidence. Here we investigate the effects of aerosols on Rei under different meteorological conditions using 9-year satellite observations. We find that the responses of Rei to aerosol loadings are modulated by water vapor amount in conjunction with several other meteorological parameters. While there is a significant negative correlation between Rei and aerosol loading in moist conditions, consistent with the "Twomey effect" for liquid clouds, a strong positive correlation between the two occurs in dry conditions. Simulations based on a cloud parcel model suggest that water vapor modulates the relative importance of different ice nucleation modes, leading to the opposite aerosol impacts between moist and dry conditions. When ice clouds are decomposed into those generated from deep convection and formed in situ, the water vapor modulation remains in effect for both ice cloud types, although the sensitivities of Rei to aerosols differ noticeably between them due to distinct formation mechanisms. The water vapor modulation can largely explain the difference in the responses of Rei to aerosol loadings in various seasons. A proper representation of the water vapor modulation is essential for an accurate estimate of aerosol–cloud radiative forcing produced by ice clouds.

Aerosol formation on the flash photolysis of SO2/gas mixtures

International Nuclear Information System (INIS)

Fogel, L.D.; Sutherland, J.W.

1979-01-01

A long-lived transient absorption observed on the flash photolysis of SO 2 /gas mixtures at lambda> or =190 nm has been identified as resulting from light scattering by H 2 SO 4 aerosols. No detectable signals were monitored on photolysis at lambda> or =270 nm, indicating that the aerosol precursors originated from the promotion of SO 2 into its second singlet level and into its dissociation continuum. The SO 3 that was formed was hydrated immediately to yield H 2 SO 4 vapor in a highly supersaturated state and heteromolecular homogeneous nucleation to produce H 2 SO 4 aerosols ensued. This nucleation was quenched rapidly as the acid vapor was consumed by further nucleation, by condensation, and by vapor diffusion to the cell walls. A model was formulated in which the condensations of the H 2 SO 4 and the H 2 O vapors on the growing droplets were considered kinetically negligible and the particles grew by coagulation; simultaneously, they were lost by tranquil gravitational settling and by diffusion to the cell walls. Computer simulations demonstrated that the observed time dependence of the absorbance data (measured at a fixed wavelength) could be accounted for by this scheme. The effects of temperature, pressure, and wavelength (of the analyzing light) were also described satisfactorily by this model

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

experiment course. The SOA was simultaneously characterized by an aerosol mass spectrometer (AMS). The ACM-GC-MS results will be compared with PMF analysis of the AMS organic aerosol. The correlation of specific compounds with PMF factors will be discussed together with future applications of the ACM-GC-MS system for ambient aerosol measurements. Acknowledgement This work was supported by the US Environmental Protection Agency (EPA Grant No. RD-83107701-0) and the Department of Energy (DOE SBIR Grant No. DE-FG02-05ER84269). References Intergovernmental Panel on Climate Change (IPCC): Climate Change 2007, Cambridge University Press, UK, 2007 Hallquist et al., The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys, Vol.9, 5155-5236, 2009

Protection of air in premises and environment against beryllium aerosols

Energy Technology Data Exchange (ETDEWEB)

Bitkolov, N.Z.; Vishnevsky, E.P.; Krupkin, A.V. [Research Inst. of Industrial and Marine Medicine, St. Petersburg (Russian Federation)

1998-01-01

First and foremost, the danger of beryllium aerosols concerns a possibility of their inhalation. The situation is aggravated with high biological activity of the beryllium in a human lung. The small allowable beryllium aerosols` concentration in air poses a rather complex and expensive problem of the pollution prevention and clearing up of air. The delivery and transportation of beryllium aerosols from sites of their formation are defined by the circuit of ventilation, that forms aerodynamics of air flows in premises, and aerodynamic links between premises. The causes of aerosols release in air of premises from hoods, isolated and hermetically sealed vessels can be vibrations, as well as pulses of temperature and pressure. Furthermore, it is possible the redispersion of aerosols from dirty surfaces. The effective protection of air against beryllium aerosols at industrial plants is provided by a complex of hygienic measures: from individual means of breath protection up to collective means of the prevention of air pollution. (J.P.N.)

Insight into winter haze formation mechanisms based on aerosol hygroscopicity and effective density measurements

Science.gov (United States)

Xie, Yuanyuan; Ye, Xingnan; Ma, Zhen; Tao, Ye; Wang, Ruyu; Zhang, Ci; Yang, Xin; Chen, Jianmin; Chen, Hong

2017-06-01

We characterize a representative particulate matter (PM) episode that occurred in Shanghai during winter 2014. Particle size distribution, hygroscopicity, effective density, and single particle mass spectrometry were determined online, along with offline analysis of water-soluble inorganic ions. The mass ratio of SNA / PM1. 0 (sulfate, nitrate, and ammonium) fluctuated slightly around 0.28, suggesting that both secondary inorganic compounds and carbonaceous aerosols contributed substantially to the haze formation, regardless of pollution level. Nitrate was the most abundant ionic species during hazy periods, indicating that NOx contributed more to haze formation in Shanghai than did SO2. During the representative PM episode, the calculated PM was always consistent with the measured PM1. 0, indicating that the enhanced pollution level was attributable to the elevated number of larger particles. The number fraction of the near-hydrophobic group increased as the PM episode developed, indicating the accumulation of local emissions. Three banana-shaped particle evolutions were consistent with the rapid increase of PM1. 0 mass loading, indicating that the rapid size growth by the condensation of condensable materials was responsible for the severe haze formation. Both hygroscopicity and effective density of the particles increased considerably with growing particle size during the banana-shaped evolutions, indicating that the secondary transformation of NOx and SO2 was one of the most important contributors to the particle growth. Our results suggest that the accumulation of gas-phase and particulate pollutants under stagnant meteorological conditions and subsequent rapid particle growth by secondary processes were primarily responsible for the haze pollution in Shanghai during wintertime.

Open burning of rice, corn and wheat straws: primary emissions, photochemical aging, and secondary organic aerosol formation

Science.gov (United States)

Fang, Zheng; Deng, Wei; Zhang, Yanli; Ding, Xiang; Tang, Mingjin; Liu, Tengyu; Hu, Qihou; Zhu, Ming; Wang, Zhaoyi; Yang, Weiqiang; Huang, Zhonghui; Song, Wei; Bi, Xinhui; Chen, Jianmin; Sun, Yele; George, Christian; Wang, Xinming

2017-12-01

Agricultural residues are among the most abundant biomass burned globally, especially in China. However, there is little information on primary emissions and photochemical evolution of agricultural residue burning. In this study, indoor chamber experiments were conducted to investigate primary emissions from open burning of rice, corn and wheat straws and their photochemical aging as well. Emission factors of NOx, NH3, SO2, 67 non-methane hydrocarbons (NMHCs), particulate matter (PM), organic aerosol (OA) and black carbon (BC) under ambient dilution conditions were determined. Olefins accounted for > 50 % of the total speciated NMHCs emission (2.47 to 5.04 g kg-1), indicating high ozone formation potential of straw burning emissions. Emission factors of PM (3.73 to 6.36 g kg-1) and primary organic carbon (POC, 2.05 to 4.11 gC kg-1), measured at dilution ratios of 1300 to 4000, were lower than those reported in previous studies at low dilution ratios, probably due to the evaporation of semi-volatile organic compounds under high dilution conditions. After photochemical aging with an OH exposure range of (1.97-4.97) × 1010 molecule cm-3 s in the chamber, large amounts of secondary organic aerosol (SOA) were produced with OA mass enhancement ratios (the mass ratio of total OA to primary OA) of 2.4-7.6. The 20 known precursors could only explain 5.0-27.3 % of the observed SOA mass, suggesting that the major precursors of SOA formed from open straw burning remain unidentified. Aerosol mass spectrometry (AMS) signaled that the aged OA contained less hydrocarbons but more oxygen- and nitrogen-containing compounds than primary OA, and carbon oxidation state (OSc) calculated with AMS resolved O / C and H / C ratios increased linearly (p < 0.001) with OH exposure with quite similar slopes.

Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO2 emission controls

Directory of Open Access Journals (Sweden)

E. A. Marais

2016-02-01

Full Text Available Isoprene emitted by vegetation is an important precursor of secondary organic aerosol (SOA, but the mechanism and yields are uncertain. Aerosol is prevailingly aqueous under the humid conditions typical of isoprene-emitting regions. Here we develop an aqueous-phase mechanism for isoprene SOA formation coupled to a detailed gas-phase isoprene oxidation scheme. The mechanism is based on aerosol reactive uptake coefficients (γ for water-soluble isoprene oxidation products, including sensitivity to aerosol acidity and nucleophile concentrations. We apply this mechanism to simulation of aircraft (SEAC4RS and ground-based (SOAS observations over the southeast US in summer 2013 using the GEOS-Chem chemical transport model. Emissions of nitrogen oxides (NOx  ≡  NO + NO2 over the southeast US are such that the peroxy radicals produced from isoprene oxidation (ISOPO2 react significantly with both NO (high-NOx pathway and HO2 (low-NOx pathway, leading to different suites of isoprene SOA precursors. We find a mean SOA mass yield of 3.3 % from isoprene oxidation, consistent with the observed relationship of total fine organic aerosol (OA and formaldehyde (a product of isoprene oxidation. Isoprene SOA production is mainly contributed by two immediate gas-phase precursors, isoprene epoxydiols (IEPOX, 58 % of isoprene SOA from the low-NOx pathway and glyoxal (28 % from both low- and high-NOx pathways. This speciation is consistent with observations of IEPOX SOA from SOAS and SEAC4RS. Observations show a strong relationship between IEPOX SOA and sulfate aerosol that we explain as due to the effect of sulfate on aerosol acidity and volume. Isoprene SOA concentrations increase as NOx emissions decrease (favoring the low-NOx pathway for isoprene oxidation, but decrease more strongly as SO2 emissions decrease (due to the effect of sulfate on aerosol acidity and volume. The US Environmental Protection Agency (EPA projects 2013–2025 decreases in

Physical parameters effect on ozone-initiated formation of indoor secondary organic aerosols with emissions from cleaning products.

Science.gov (United States)

Huang, Yu; Ho, Kin Fai; Ho, Steven Sai Hang; Lee, Shun Cheng; Yau, P S; Cheng, Yan

2011-09-15

The effect of air exchange rate (ACH), temperature (T), and relative humidity (RH) on the formation of indoor secondary organic aerosols (SOAs) through ozonolysis of biogenic organic compounds (BVOCs) emitted from floor cleaner was investigated in this study. The total particle count (with D(p) of 6-225 nm) was up to 1.2 × 10(3)#cm(-3) with ACH of 1.08 h(-1), and it became much more significant with ACH of 0.36 h(-1) (1.1 × 10(4)#cm(-3)). This suggests that a higher ventilation rate can effectively dilute indoor BVOCs, resulting in a less ultrafine particle formation. The total particle count increased when temperature changed from 15 to 23 °C but it decreased when the temperature further increased to 30 °C. It could be explained that high temperature restrained the condensation of formed semi-volatile compounds resulting in low yields of SOAs. When the RH was at 50% and 80%, SOA formation (1.1-1.2 × 10(4)#cm(-3)) was the more efficient compared with that at RH of 30% (5.9 × 10(3)#cm(-3)), suggesting higher RH facilitating the initial nucleation processes. Oxidation generated secondary carbonyl compounds were also quantified. Acetone was the most abundant carbonyl compound. The formation mechanisms of formaldehyde and acetone were proposed. Copyright © 2011 Elsevier B.V. All rights reserved.

Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area

Science.gov (United States)

Ortega, Amber M.; Hayes, Patrick L.; Peng, Zhe; Palm, Brett B.; Hu, Weiwei; Day, Douglas A.; Li, Rui; Cubison, Michael J.; Brune, William H.; Graus, Martin; Warneke, Carsten; Gilman, Jessica B.; Kuster, William C.; de Gouw, Joost; Gutiérrez-Montes, Cándido; Jimenez, Jose L.

2016-06-01

Field studies in polluted areas over the last decade have observed large formation of secondary organic aerosol (SOA) that is often poorly captured by models. The study of SOA formation using ambient data is often confounded by the effects of advection, vertical mixing, emissions, and variable degrees of photochemical aging. An oxidation flow reactor (OFR) was deployed to study SOA formation in real-time during the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign in Pasadena, CA, in 2010. A high-resolution aerosol mass spectrometer (AMS) and a scanning mobility particle sizer (SMPS) alternated sampling ambient and reactor-aged air. The reactor produced OH concentrations up to 4 orders of magnitude higher than in ambient air. OH radical concentration was continuously stepped, achieving equivalent atmospheric aging of 0.8 days-6.4 weeks in 3 min of processing every 2 h. Enhancement of organic aerosol (OA) from aging showed a maximum net SOA production between 0.8-6 days of aging with net OA mass loss beyond 2 weeks. Reactor SOA mass peaked at night, in the absence of ambient photochemistry and correlated with trimethylbenzene concentrations. Reactor SOA formation was inversely correlated with ambient SOA and Ox, which along with the short-lived volatile organic compound correlation, indicates the importance of very reactive (τOH ˜ 0.3 day) SOA precursors (most likely semivolatile and intermediate volatility species, S/IVOCs) in the Greater Los Angeles Area. Evolution of the elemental composition in the reactor was similar to trends observed in the atmosphere (O : C vs. H : C slope ˜ -0.65). Oxidation state of carbon (OSc) in reactor SOA increased steeply with age and remained elevated (OSC ˜ 2) at the highest photochemical ages probed. The ratio of OA in the reactor output to excess CO (ΔCO, ambient CO above regional background) vs. photochemical age is similar to previous studies at low to moderate ages and also extends to

Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area

Directory of Open Access Journals (Sweden)

A. M. Ortega

2016-06-01

Full Text Available Field studies in polluted areas over the last decade have observed large formation of secondary organic aerosol (SOA that is often poorly captured by models. The study of SOA formation using ambient data is often confounded by the effects of advection, vertical mixing, emissions, and variable degrees of photochemical aging. An oxidation flow reactor (OFR was deployed to study SOA formation in real-time during the California Research at the Nexus of Air Quality and Climate Change (CalNex campaign in Pasadena, CA, in 2010. A high-resolution aerosol mass spectrometer (AMS and a scanning mobility particle sizer (SMPS alternated sampling ambient and reactor-aged air. The reactor produced OH concentrations up to 4 orders of magnitude higher than in ambient air. OH radical concentration was continuously stepped, achieving equivalent atmospheric aging of 0.8 days–6.4 weeks in 3 min of processing every 2 h. Enhancement of organic aerosol (OA from aging showed a maximum net SOA production between 0.8–6 days of aging with net OA mass loss beyond 2 weeks. Reactor SOA mass peaked at night, in the absence of ambient photochemistry and correlated with trimethylbenzene concentrations. Reactor SOA formation was inversely correlated with ambient SOA and Ox, which along with the short-lived volatile organic compound correlation, indicates the importance of very reactive (τOH  ∼  0.3 day SOA precursors (most likely semivolatile and intermediate volatility species, S/IVOCs in the Greater Los Angeles Area. Evolution of the elemental composition in the reactor was similar to trends observed in the atmosphere (O : C vs. H : C slope  ∼  −0.65. Oxidation state of carbon (OSc in reactor SOA increased steeply with age and remained elevated (OSC  ∼  2 at the highest photochemical ages probed. The ratio of OA in the reactor output to excess CO (ΔCO, ambient CO above regional background vs. photochemical age is similar to

Do atmospheric aerosols form glasses?

Directory of Open Access Journals (Sweden)

D. A. Pedernera

2008-09-01

Full Text Available A new process is presented by which water soluble organics might influence ice nucleation, ice growth, chemical reactions and water uptake of aerosols in the upper troposphere: the formation of glassy aerosol particles. Glasses are disordered amorphous (non-crystalline solids that form when a liquid is cooled without crystallization until the viscosity increases exponentially and molecular diffusion practically ceases. The glass transition temperatures, T_g, homogeneous ice nucleation temperatures, T_hom, and ice melting temperatures, T_m, of various aqueous inorganic, organic and multi-component solutions are investigated with a differential scanning calorimeter. The investigated solutes are: various polyols, glucose, raffinose, levoglucosan, an aromatic compound, sulfuric acid, ammonium bisulfate and mixtures of dicarboxylic acids (M5, of dicarboxylic acids and ammonium sulfate (M5AS, of two polyols, of glucose and ammonium nitrate, and of raffinose and M5AS. The results indicate that aqueous solutions of the investigated inorganic solutes show T_g values that are too low to be of atmospheric importance. In contrast, aqueous organic and multi-component solutions readily form glasses at low but atmospherically relevant temperatures (≤230 K. To apply the laboratory data to the atmospheric situation, the measured phase transition temperatures were transformed from a concentration to a water activity scale by extrapolating water activities determined between 252 K and 313 K to lower temperatures. The obtained state diagrams reveal that the higher the molar mass of the aqueous organic or multi-component solutes, the higher T_g of their respective solutions at a given water activity. To a lesser extent, T_g also depends on the hydrophilicity of the organic solutes. Therefore, aerosol particles containing larger (≳150 g mol⁻¹ and

New particle formation in the sulfuric acid-dimethylamine-water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model

Science.gov (United States)

Kürten, Andreas; Li, Chenxi; Bianchi, Federico; Curtius, Joachim; Dias, António; Donahue, Neil M.; Duplissy, Jonathan; Flagan, Richard C.; Hakala, Jani; Jokinen, Tuija; Kirkby, Jasper; Kulmala, Markku; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Onnela, Antti; Rissanen, Matti P.; Simon, Mario; Sipilä, Mikko; Stozhkov, Yuri; Tröstl, Jasmin; Ye, Penglin; McMurry, Peter H.

2018-01-01

A recent CLOUD (Cosmics Leaving OUtdoor Droplets) chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF) rates are reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter). In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up to ca. 30 nm). Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement for the high base-to-acid ratios (˜ 100) relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically controlled) NPF for the conditions during the CLOUD7 experiment (278 K, 38 % relative humidity, sulfuric acid concentration between 1 × 106 and 3 × 107 cm-3, and dimethylamine mixing ratio of ˜ 40 pptv, i.e., 1 × 109 cm-3).

Environmental Temperature Effect on the Far-Infrared Absorption Features of Aromatic-Based Titan's Aerosol Analogs

Science.gov (United States)

Gautier, Thomas; Trainer, Melissa G.; Loeffler, Mark J.; Sebree, Joshua A.; Anderson, Carrie M.

2016-01-01

Benzene detection has been reported in Titans atmosphere both in the stratosphere at ppb levels by remote sensing and in the thermosphere at ppm levels by the Cassini's Ion and Neutral Mass Spectrometer. This detection supports the idea that aromatic and heteroaromatic reaction pathways may play an important role in Titans atmospheric chemistry, especially in the formation of aerosols. Indeed, aromatic molecules are easily dissociated by ultraviolet radiation and can therefore contribute significantly to aerosol formation. It has been shown recently that aerosol analogs produced from a gas mixture containing a low concentration of aromatic and/or heteroaromatic molecules (benzene, naphthalene, pyridine, quinoline and isoquinoline) have spectral signatures below 500/cm, a first step towards reproducing the aerosol spectral features observed by Cassini's Composite InfraRed Spectrometer (CIRS) in the far infrared. In this work we investigate the influence of environmental temperature on the absorption spectra of such aerosol samples, simulating the temperature range to which aerosols, once formed, are exposed during their transport through Titans stratosphere. Our results show that environmental temperature does not have any major effect on the spectral shape of these aerosol analogs in the far-infrared, which is consistent with the CIRS observations.

New pathway of stratocumulus to cumulus transition via aerosol-cloud-precipitation interaction

Science.gov (United States)

Yamaguchi, T.; Feingold, G.; Kazil, J.

2017-12-01

The stratocumulus to cumulus transition (SCT) is typically considered to be a slow, multi-day process, caused primarily by dry air entrainment associated with overshooting cumulus rising under stratocumulus, with minor influence of precipitation. In this presentation, we show rapid SCT induced by a strong precipitation-induced modulation with Lagrangian SCT large eddy simulations. A large eddy model is coupled with a two-moment bulk microphysics scheme that predicts aerosol and droplet number concentrations. Moderate aerosol concentrations (100-250 cm-3) produce little to no drizzle from the stratocumulus deck. Large amounts of rain eventually form and wash out stratocumulus and much of the aerosol, and a cumulus state appears for approximately 10 hours. Initiation of strong rain formation is identified in penetrative cumulus clouds which are much deeper than stratocumulus, and they are able to condense large amounts of water. We show that prediction of cloud droplet number is necessary for this fast SCT since it is a result of a positive feedback of collision-coalescence induced aerosol depletion enhancing drizzle formation. Simulations with fixed droplet concentrations that bracket the time varying aerosol/drop concentrations are therefore not representative of the role of drizzle in the SCT.

Proceedings of the CSNI specialists meeting on nuclear aerosols in reactor safety

International Nuclear Information System (INIS)

1980-10-01

The technical program, as recorded by these proceedings, includes opening addresses, a panel discussion on 'nuclear aerosol measurement', a panel discussion on 'what remains to be done', six invited review papers, and 33 papers from six different countries grouped into the following topical areas: (1) aerosol source terms (nuclear aerosol formation and characterization, nucleation and condensation, size and composition of primary particles, aerosol source terms for postulated accidents); (2) aerosol processes (correction factors, growth and interaction rates, removal rates); (3) measurement techniques (focused on assessing limits of accuracy and implications for code validation for accident consequence analysis); (4) mathematical and computer modelling; (5) comparison of codes and experiments); and (6) applications (focused on application of aerosol technology to reactor design, sensitivity of results, and implications for radiological consequence assessment for hypothetical accidents)

Proceedings of the CSNI specialists meeting on nuclear aerosols in reactor safety

Energy Technology Data Exchange (ETDEWEB)

NONE

1980-10-15

The technical program, as recorded by these proceedings, includes opening addresses, a panel discussion on 'nuclear aerosol measurement', a panel discussion on 'what remains to be done', six invited review papers, and 33 papers from six different countries grouped into the following topical areas: (1) aerosol source terms (nuclear aerosol formation and characterization, nucleation and condensation, size and composition of primary particles, aerosol source terms for postulated accidents); (2) aerosol processes (correction factors, growth and interaction rates, removal rates); (3) measurement techniques (focused on assessing limits of accuracy and implications for code validation for accident consequence analysis); (4) mathematical and computer modelling; (5) comparison of codes and experiments); and (6) applications (focused on application of aerosol technology to reactor design, sensitivity of results, and implications for radiological consequence assessment for hypothetical accidents)

Aerosol measurements over Southern Africa using LIDAR, satellite and sun-photometer

CSIR Research Space (South Africa)

Sivakumar, V

2009-08-01

Full Text Available .csir.co.za Dust Sea Salt Giant nuclei Natural Particles Chemical chemical condensables : SOA, H2SO4, HNO3 … nucleation condensation Aerosol Formation and processes Health Aerosols Solar Radiation Clouds Slide 3 © CSIR 2008 www....csir.co.za Emissions from Industries, vechicle and urban Volatile Components SO2, NOx, NH3, VOC Transformation Humidity and deposition of particules Primary Aerosols, BC, OC, Marine Salts, Natural resources 0 - 16 k m U p t o 50 k m 26 – 29...

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

Energy Technology Data Exchange (ETDEWEB)

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

2017-12-01

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

A Statistical Review of CALIOP Version 3 and Version 4 Cloud Aerosol Discrimination

Science.gov (United States)

Zeng, S.

2016-12-01

The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) on board the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) mission has now delivered a 10-year record of high-resolution profiles of backscatter at 532 nm and 1064 nm and linear depolarization at 532 nm. These long-term active sensor measurements at global scale have led to significant advances in our understanding of the vertical distribution of clouds and aerosols in the atmosphere. In the fall of 2016, the CALIPSO science team is scheduled to release a new version of their cloud and aerosol data products. The new cloud and aerosol discrimination products are derived using updated probability density functions that account for numerous improvements to the CALIOP calibration and the use of the GMAO MERRA-2 meteorological data. Moreover, the CAD algorithm is now applied to all layers detected, thus greatly improving the identification of such features as overshooting convective clouds, stratospheric aerosol layers, and high intensity dust storms. Post-processing modules are added to the standard CAD algorithm to ensure proper identification of (for example) the tenuous edges of cirrus clouds and water clouds lying beneath optically dense smoke layers. This work presents statistical comparisons between the CALIOP version 3 and version 4 data sets. Areas of improvement are highlighted, sources of continuing uncertainty are discussed and a list of best practices for data users is provided.

Atmospheric data over a solar cycle: no connection between galactic cosmic rays and new particle formation

Directory of Open Access Journals (Sweden)

M. Kulmala

2010-02-01

Full Text Available Aerosol particles affect the Earth's radiative balance by directly scattering and absorbing solar radiation and, indirectly, through their activation into cloud droplets. Both effects are known with considerable uncertainty only, and translate into even bigger uncertainties in future climate predictions. More than a decade ago, variations in galactic cosmic rays were suggested to closely correlate with variations in atmospheric cloud cover and therefore constitute a driving force behind aerosol-cloud-climate interactions. Later, the enhancement of atmospheric aerosol particle formation by ions generated from cosmic rays was proposed as a physical mechanism explaining this correlation. Here, we report unique observations on atmospheric aerosol formation based on measurements at the SMEAR II station, Finland, over a solar cycle (years 1996–2008 that shed new light on these presumed relationships. Our analysis shows that none of the quantities related to aerosol formation correlates with the cosmic ray-induced ionisation intensity (CRII. We also examined the contribution of ions to new particle formation on the basis of novel ground-based and airborne observations. A consistent result is that ion-induced formation contributes typically significantly less than 10% to the number of new particles, which would explain the missing correlation between CRII and aerosol formation. Our main conclusion is that galactic cosmic rays appear to play a minor role for atmospheric aerosol formation events, and so for the connected aerosol-climate effects as well.

Modeling regional air quality and climate: improving organic aerosol and aerosol activation processes in WRF/Chem version 3.7.1

Science.gov (United States)

Yahya, Khairunnisa; Glotfelty, Timothy; Wang, Kai; Zhang, Yang; Nenes, Athanasios

2017-06-01

Air quality and climate influence each other through the uncertain processes of aerosol formation and cloud droplet activation. In this study, both processes are improved in the Weather, Research and Forecasting model with Chemistry (WRF/Chem) version 3.7.1. The existing Volatility Basis Set (VBS) treatments for organic aerosol (OA) formation in WRF/Chem are improved by considering the following: the secondary OA (SOA) formation from semi-volatile primary organic aerosol (POA), a semi-empirical formulation for the enthalpy of vaporization of SOA, and functionalization and fragmentation reactions for multiple generations of products from the oxidation of VOCs. Over the continental US, 2-month-long simulations (May to June 2010) are conducted and results are evaluated against surface and aircraft observations during the Nexus of Air Quality and Climate Change (CalNex) campaign. Among all the configurations considered, the best performance is found for the simulation with the 2005 Carbon Bond mechanism (CB05) and the VBS SOA module with semivolatile POA treatment, 25 % fragmentation, and the emissions of semi-volatile and intermediate volatile organic compounds being 3 times the original POA emissions. Among the three gas-phase mechanisms (CB05, CB6, and SAPRC07) used, CB05 gives the best performance for surface ozone and PM2. 5 concentrations. Differences in SOA predictions are larger for the simulations with different VBS treatments (e.g., nonvolatile POA versus semivolatile POA) compared to the simulations with different gas-phase mechanisms. Compared to the simulation with CB05 and the default SOA module, the simulations with the VBS treatment improve cloud droplet number concentration (CDNC) predictions (normalized mean biases from -40.8 % to a range of -34.6 to -27.7 %), with large differences between CB05-CB6 and SAPRC07 due to large differences in their OH and HO2 predictions. An advanced aerosol activation parameterization based on the Fountoukis and Nenes

THE INFLUENCE OF BENZENE AS A TRACE REACTANT IN TITAN AEROSOL ANALOGS

Energy Technology Data Exchange (ETDEWEB)

Trainer, Melissa G. [Planetary Environments Laboratory, Code 699, NASA Goddard Space Flight Center, Greenbelt, MD 20771 (United States); Sebree, Joshua A. [NASA Postdoctoral Program Fellow, Code 699, Goddard Space Flight Center, Greenbelt, MD 20771 (United States); Heidi Yoon, Y.; Tolbert, Margaret A., E-mail: melissa.trainer@nasa.gov [Cooperative Institute for Research in Environmental Sciences, University of Colorado at Boulder, Box 216 UCB, Boulder, CO 80309 (United States)

2013-03-20

Benzene has been detected in Titan's atmosphere by Cassini instruments, with concentrations ranging from sub-ppb in the stratosphere to ppm in the ionosphere. Sustained levels of benzene in the haze formation region could signify that it is an important reactant in the formation of Titan's organic aerosol. To date, there have not been laboratory investigations to assess the influence of benzene on aerosol properties. We report a laboratory study on the chemical composition of organic aerosol formed from C{sub 6}H{sub 6}/CH{sub 4}/N{sub 2} via far ultraviolet irradiation (120-200 nm). The compositional results are compared to those from aerosol generated by a more ''traditional Titan'' mixture of CH{sub 4}/N{sub 2}. Our results show that even a trace amount of C{sub 6}H{sub 6} (10 ppm) has significant impact on the chemical composition and production rates of organic aerosol. There are several pathways by which photolyzed benzene may react to form larger molecules, both with and without the presence of CH{sub 4}, but many of these reaction mechanisms are only beginning to be explored for the conditions at Titan. Continued work investigating the influence of benzene in aerosol growth will advance understanding of this previously unstudied reaction system.

Formation kinetics and abundance of organic nitrates in α-pinene ozonolysis

Science.gov (United States)

Berkemeier, Thomas; Ammann, Markus; Pöschl, Ulrich; Shiraiwa, Manabu

2016-04-01

Formation of organic nitrates affects the total atmospheric budget of oxidized nitrogen (NOy) and alters the total aerosol mass yield from secondary sources. We investigated the formation of organic nitrate species during ozonolysis of α-pinene and subsequent formation of secondary organic aerosols (SOA) using the short-lived radioactive tracer 13N inside an aerosol flow reactor (Ammann et al., 2001). The results represent direct measurements of the organic nitrate content of α-pinene secondary aerosol and give insight into the kinetics of organic nitrate formation. Organic nitrates constituted up to 40 % of aerosol mass with a pronounced influence during the initial period of particle growth. Kinetic modelling, as well as additional experiments using OH scavengers and UV irradiation, suggests that organic peroxy radicals (RO2) from the reaction of α-pinene with secondarily produced OH are important intermediates in the organic nitrate formation process. Direct oxidation of α-pinene by NO3 was found to be a less efficient pathway for formation of particle phase nitrate. The organic nitrate content decreased very slightly with an increase of relative humidity on the experimental time scale. The experiments show a tight correlation between organic nitrate content and SOA number concentrations, implying that organic nitrates play an important role in nucleation and growth of nanoparticles. Since present in large amounts in organic aerosol, organic nitrates deposited in the lung might have implications for human health as they release nitric acid upon hydrolysis, especially in regions influenced by urban pollution and large sources of monoterpene SOA precursors. References Ammann et al. (2001) Radiochimica Acta 89, 831.

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

Climate impact of anthropogenic aerosols on cirrus clouds

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Penner, J.; Zhou, C.

2017-12-01

Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. However, the efficacy with which particles act to form cirrus particles in a model depends on the representation of updrafts. Here, we use a representation of updrafts based on observations of gravity waves, and follow ice formation/evaporation during both updrafts and downdrafts. We examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning and from aircraft particles that have previously formed ice in contrails. Results show that fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of -0.15±0.02 Wm-2 while aircraft aerosols that have been pre-activated within contrails exert a forcing of -0.20±0.06 Wm-2, but it is possible to decrease these estimates of forcing if a larger fraction of dust particles act as heterogeneous ice nuclei. In addition aircraft aerosols may warm the climate if a large fraction of these particles act as ice nuclei. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds. This assessment could therefore support climate models with high sensitivity to greenhouse gas forcing, while still allowing the models to fit the overall historical temperature change.

Effect of phytoplackton-derived organic matter on the behavior of marine aerosols

Science.gov (United States)

Fuentes, E.; Coe, H.; McFiggans, G.; Green, D.

2009-04-01

The presence of significant concentrations of organic material in marine aerosols has been appreciated for several decades; however, only recently has significant progress been made towards demonstrating that this organic content is biogenically formed. Biogenic organics of placktonic life origin are incorporated in marine aerosol composition as a result of bubble bursting/breaking waves mechanisms that occur at the ocean surface. The presence of organic surfactants in the marine aerosol composition might have a significant impact on the properties of the generated aerosols by affecting the particles surface tension and solution balance properties. Nevertheless, it remains uncertain the role of such organics on the physical-chemical behavior of marine aerosols. In this work an experimental study was performed in order to determine the influence of biogenic marine organic compounds on the size distribution, hygroscopicity and cloud-nucleating properties of marine aerosols. For the experimental study a laboratory water recirculation system (bubble tank), designed for the simulation of bubble-burst aerosol formation, was used as marine aerosol generator. The bubble spectra produced by such system was characterized by means of an optical bubble measuring device (BMS) and it was found to be consistent with oceanic bubble spectra properties. Seawater proxy solutions were prepared from laboratory biologically-synthesized exudates produced by oceanic representative algal species and introduced in the tank for the generation of marine aerosol by bubble bursting. Two experimental methods were employed for seawater proxies preparation: the formation of surface monolayers from the biogenic surfactants extracted by a solid phase extraction technique (monolayer method) and the mixing of the exudates in the sea salt water bulk (bulk mixing method). Particle size distribution, hygroscopicity and cloud condensation nuclei experiments for different monolayers, and exudate mixtures

Experimental Characterization of Radiation Forcing due to Atmospheric Aerosols

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Sreenivas, K. R.; Singh, D. K.; Ponnulakshmi, V. K.; Subramanian, G.

2011-11-01

Micro-meteorological processes in the nocturnal atmospheric boundary layer (NBL) including the formation of radiation-fog and the development of inversion layers are controlled by heat transfer and the vertical temperature distribution close to the ground. In a recent study, it has been shown that the temperature profile close to the ground in stably-stratified, NBL is controlled by the radiative forcing due to suspended aerosols. Estimating aerosol forcing is also important in geo-engineering applications to evaluate the use of aerosols to mitigate greenhouse effects. Modeling capability in the above scenarios is limited by our knowledge of this forcing. Here, the design of an experimental setup is presented which can be used for evaluating the IR-radiation forcing on aerosols under either Rayleigh-Benard condition or under conditions corresponding to the NBL. We present results indicating the effect of surface emissivities of the top and bottom boundaries and the aerosol concentration on the temperature profiles. In order to understand the observed enhancement of the convection-threshold, we have determined the conduction-radiation time constant of an aerosol laden air layer. Our results help to explain observed temperature profiles in the NBL, the apparent stability of such profiles and indicate the need to account for the effect of aerosols in climatic/weather models.

Code Development of Radioactive Aerosol Scrubbing in Pool-Injection Zone

Energy Technology Data Exchange (ETDEWEB)

Jo, Hyun Joung; Ha, Kwang Soon [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of); Jang, Dong Soon [Chungnam National University, Daejeon (Korea, Republic of)

2015-10-15

The pool scrubbing models were reviewed and an aerosol scrubbing code has been prepared to calculate decontamination factor through the injection zone. The developed code has been verified using the experimental results and evaluated parametrically on the input variables. In injection zone, the initial steam condensation was most effective mechanism for the aerosol removal, and the steam fraction and pool temperature were highly affected on the decontamination factor by initial steam condensation. The aerosol scrubbing code will be updated to evaluate the decontamination factor at rise zone and finally whole pool scrubber phenomena. If a severe accident occurs in a nuclear power plant (NPP), the aerosol and gaseous fission products might be produced in the reactor vessel, and then released to the environment after the containment failure. FCVS (Filtered Containment Venting System) is one of the severe accident mitigation systems for retaining the containment integrity by discharging the high-temperature and high-pressure fission products to the environment after passing through the filtration system. In general, the FCVS is categorized into two types, wet and dry types. The scrubbing pool could play an important role in the wet type FCVS because a large amount of aerosol is captured in the water pool. The pool scrubbing phenomena have been modelled and embedded in several computer codes, such as SPARC (Suppression Pool Aerosol Removal Code), BUSCA (BUbble Scrubbing Algorithm) and SUPRA (Suppression Pool Retention Analysis). These codes aim at simulating the pool scrubbing process and estimating the decontamination factors (DFs) of the radioactive aerosol and iodine gas in the water pool, which is defined as the ratio of initial mass of the specific radioactive material to final massy after passing through the water pool. The pool scrubbing models were reviewed and an aerosol scrubbing code has been prepared to calculate decontamination factor through the injection

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

Update on the NASA GEOS-5 Aerosol Forecasting and Data Assimilation System

Science.gov (United States)

Colarco, Peter; da Silva, Arlindo; Aquila, Valentina; Bian, Huisheng; Buchard, Virginie; Castellanos, Patricia; Darmenov, Anton; Follette-Cook, Melanie; Govindaraju, Ravi; Keller, Christoph;

Chemical interactions between aerosols and vapors in the primary circuit of an LWR during a severe accident

International Nuclear Information System (INIS)

Wheatley, C.J.

1988-01-01

Aerosol formation, agglomeration, convection and deposition within the primary circuit of an LWR during a severe accident significantly affect the transport of fission products, even though they may compose only a small fraction of the aerosol material. Intra-particle and vapor chemical interactions are important to this through mass transfer between the aerosol and vapor. The authors will describe a model that attempts to account for these processes and of the two-way coupling that exists with the thermal hydraulics. They will discuss what agglomeration and deposition mechanisms must be included, alternatives for treating intra-particle chemical interactions, mechanisms of aerosol formation, and methods for solving the resulting equations. Results will be presented that illustrate the importance of treating the two-way coupling and the extent to which disequilibrium between the aerosol and vapor affects fission product behavior

Water-soluble Organic Components in Aerosols Associated with Savanna Fires in Southern Africa: Identification, Evolution and Distribution

Science.gov (United States)

Gao, Song; Hegg, Dean A.; Hobbs, Peter V.; Kirchstetter, Thomas W.; Magi, Brian I.; Sadilek, Martin

2003-01-01

During the SAFARI 2000 field campaign, both smoke aerosols from savanna fires and haze aerosols in the boundary layer and in the free troposphere were collected from an aircraft in southern Africa. These aerosol samples were analyzed for their water-soluble chemical components, particularly the organic species. A novel technique, electrospray ionization-ion trap mass spectrometry, was used concurrently with an ion chromatography system to analyze for carbohydrate species. Seven carbohydrates, seven organic acids, five metallic elements, and three inorganic anions were identified and quantified. On the average, these 22 species comprised 36% and 27% of the total aerosol mass in haze and smoke aerosols, respectively. For the smoke aerosols, levoglucosan was the most abundant carbohydrate species, while gluconic acid was tentatively identified as the most abundant organic acid. The mass abundance and possible source of each class of identified species are discussed, along with their possible formation pathways. The combustion phase of a fire had an impact on the chemical composition of the emitted aerosols. Secondary formation of sulfate, nitrate, levoglucosan, and several organic acids occurred during the initial aging of smoke aerosols. It is likely that under certain conditions, some carbohydrate species in smoke aerosols, such as levoglucosan, were converted to organic acids during upward transport.

Convective behaviour in vapour-gas-aerosol mixtures

International Nuclear Information System (INIS)

Clement, C.F.

1986-01-01

Unusual convective behaviour can occur in mixtures of gases and heavy vapour, including stabilization of mixtures hot at the base and 'upside-down' convection in mixtures hot at the top. Previous work produced a criterion for this behaviour which ignored the necessary presence of an aerosol. Modification arising from aerosol condensation is derived and is shown to involve the Lewis and condensation numbers of the mixture, as well as a quantity involving the temperature drop across a boundary layer. It becomes negligible at high temperatures, but can crucially affect the temperature for the onset of unusual behaviour. Aerosol formation produces an asymmetry between the convective forces in boundary layers in which the mixture is being heated and cooled, respectively, for example at the base and roof of a cavity. The convective behaviour discussed could occur in situations relevant to nuclear safety. (author)

Aerosol optical properties derived from the DRAGON-NE Asia campaign, and implications for a single-channel algorithm to retrieve aerosol optical depth in spring from Meteorological Imager (MI on-board the Communication, Ocean, and Meteorological Satellite (COMS

Directory of Open Access Journals (Sweden)

M. Kim

2016-02-01

Full Text Available An aerosol model optimized for northeast Asia is updated with the inversion data from the Distributed Regional Aerosol Gridded Observation Networks (DRAGON-northeast (NE Asia campaign which was conducted during spring from March to May 2012. This updated aerosol model was then applied to a single visible channel algorithm to retrieve aerosol optical depth (AOD from a Meteorological Imager (MI on-board the geostationary meteorological satellite, Communication, Ocean, and Meteorological Satellite (COMS. This model plays an important role in retrieving accurate AOD from a single visible channel measurement. For the single-channel retrieval, sensitivity tests showed that perturbations by 4 % (0.926 ± 0.04 in the assumed single scattering albedo (SSA can result in the retrieval error in AOD by over 20 %. Since the measured reflectance at the top of the atmosphere depends on both AOD and SSA, the overestimation of assumed SSA in the aerosol model leads to an underestimation of AOD. Based on the AErosol RObotic NETwork (AERONET inversion data sets obtained over East Asia before 2011, seasonally analyzed aerosol optical properties (AOPs were categorized by SSAs at 675 nm of 0.92 ± 0.035 for spring (March, April, and May. After the DRAGON-NE Asia campaign in 2012, the SSA during spring showed a slight increase to 0.93 ± 0.035. In terms of the volume size distribution, the mode radius of coarse particles was increased from 2.08 ± 0.40 to 2.14 ± 0.40. While the original aerosol model consists of volume size distribution and refractive indices obtained before 2011, the new model is constructed by using a total data set after the DRAGON-NE Asia campaign. The large volume of data in high spatial resolution from this intensive campaign can be used to improve the representative aerosol model for East Asia. Accordingly, the new AOD data sets retrieved from a single-channel algorithm, which uses a precalculated look-up table (LUT with the new aerosol model

Organic aerosols

International Nuclear Information System (INIS)

Penner, J.E.

1994-01-01

Organic aerosols scatter solar radiation. They may also either enhance or decrease concentrations of cloud condensation nuclei. This paper summarizes observed concentrations of aerosols in remote continental and marine locations and provides estimates for the sources of organic aerosol matter. The anthropogenic sources of organic aerosols may be as large as the anthropogenic sources of sulfate aerosols, implying a similar magnitude of direct forcing of climate. The source estimates are highly uncertain and subject to revision in the future. A slow secondary source of organic aerosols of unknown origin may contribute to the observed oceanic concentrations. The role of organic aerosols acting as cloud condensation nuclei (CCN) is described and it is concluded that they may either enhance or decrease the ability of anthropogenic sulfate aerosols to act as CCN

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.

Gas phase precursors to anthropogenic secondary organic aerosol: detailed observations of 1,3,5-trimethylbenzene photooxidation

Directory of Open Access Journals (Sweden)

K. P. Wyche

2009-01-01

Full Text Available A series of photooxidation experiments were conducted in an atmospheric simulation chamber in order to investigate the oxidation mechanism and secondary organic aerosol (SOA formation potential of the model anthropogenic gas phase precursor, 1,3,5-trimethylbenzene. Alongside specific aerosol measurements, comprehensive gas phase measurements, primarily by Chemical Ionisation Reaction Time-of-Flight Mass Spectrometry (CIR-TOF-MS, were carried out to provide detailed insight into the composition and behaviour of the organic components of the gas phase matrix during SOA formation. An array of gas phase organic compounds was measured during the oxidation process, including several previously unmeasured primary bicyclic compounds possessing various functional groups. Analysis of results obtained during this study implies that these peroxide bicyclic species along with a series of ring opening products and organic acids contribute to SOA growth. The effect of varying the VOC/NO_x ratio on SOA formation was explored, as was the effect of acid seeding. It was found that low NO_x conditions favour more rapid aerosol formation and a higher aerosol yield, a result that implies a role for organic peroxides in the nucleation process and SOA growth.

Strong impacts on aerosol indirect effects from historical oxidant changes

Science.gov (United States)

Hafsahl Karset, Inger Helene; Koren Berntsen, Terje; Storelvmo, Trude; Alterskjær, Kari; Grini, Alf; Olivié, Dirk; Kirkevåg, Alf; Seland, Øyvind; Iversen, Trond; Schulz, Michael

2018-06-01

Uncertainties in effective radiative forcings through aerosol-cloud interactions (ERFaci, also called aerosol indirect effects) contribute strongly to the uncertainty in the total preindustrial-to-present-day anthropogenic forcing. Some forcing estimates of the total aerosol indirect effect are so negative that they even offset the greenhouse gas forcing. This study highlights the role of oxidants in modeling of preindustrial-to-present-day aerosol indirect effects. We argue that the aerosol precursor gases should be exposed to oxidants of its era to get a more correct representation of secondary aerosol formation. Our model simulations show that the total aerosol indirect effect changes from -1.32 to -1.07 W m-2 when the precursor gases in the preindustrial simulation are exposed to preindustrial instead of present-day oxidants. This happens because of a brightening of the clouds in the preindustrial simulation, mainly due to large changes in the nitrate radical (NO3). The weaker oxidative power of the preindustrial atmosphere extends the lifetime of the precursor gases, enabling them to be transported higher up in the atmosphere and towards more remote areas where the susceptibility of the cloud albedo to aerosol changes is high. The oxidation changes also shift the importance of different chemical reactions and produce more condensate, thus increasing the size of the aerosols and making it easier for them to activate as cloud condensation nuclei.

Aerosol surface area concentration: a governing factor in new particle formation in Beijing

Directory of Open Access Journals (Sweden)

R. Cai

2017-10-01

Full Text Available The predominating role of aerosol Fuchs surface area, AFuchs, in determining the occurrence of new particle formation (NPF events in Beijing was elucidated in this study. The analysis was based on a field campaign from 12 March to 6 April 2016 in Beijing, during which aerosol size distributions down to  ∼  1 nm and sulfuric acid concentrations were simultaneously monitored. The 26 days were classified into 11 typical NPF days, 2 undefined days, and 13 non-event days. A dimensionless factor, LΓ, characterized by the relative ratio of the coagulation scavenging rate over the condensational growth rate (Kuang et al., 2010, was applied in this work to reveal the governing factors for NPF events in Beijing. The three parameters determining LΓ are sulfuric acid concentration, the growth enhancement factor characterized by contribution of other gaseous precursors to particle growth, Γ, and AFuchs. Different from other atmospheric environments, such as in Boulder and Hyytiälä, the daily-maximum sulfuric acid concentration and Γ in Beijing varied in a narrow range with geometric standard deviations of 1.40 and 1.31, respectively. A positive correlation between the estimated new particle formation rate, J1.5, and sulfuric acid concentration was found with a mean fitted exponent of 2.4. However, the maximum sulfuric acid concentrations on NPF days were not significantly higher (even lower, sometimes than those on non-event days, indicating that the abundance of sulfuric acid in Beijing was high enough to initiate nucleation, but may not necessarily lead to NPF events. Instead, AFuchs in Beijing varied greatly among days with a geometric standard deviation of 2.56, whereas the variabilities of AFuchs in Tecamac, Atlanta, and Boulder were reported to be much smaller. In addition, there was a good correlation between AFuchs and LΓ in Beijing (R2 = 0.88. Therefore, it was AFuchs that fundamentally determined the occurrence of NPF events

Global-scale combustion sources of organic aerosols: sensitivity to formation and removal mechanisms

Science.gov (United States)

Tsimpidi, Alexandra P.; Karydis, Vlassis A.; Pandis, Spyros N.; Lelieveld, Jos

2017-06-01

Organic compounds from combustion sources such as biomass burning and fossil fuel use are major contributors to the global atmospheric load of aerosols. We analyzed the sensitivity of model-predicted global-scale organic aerosols (OA) to parameters that control primary emissions, photochemical aging, and the scavenging efficiency of organic vapors. We used a computationally efficient module for the description of OA composition and evolution in the atmosphere (ORACLE) of the global chemistry-climate model EMAC (ECHAM/MESSy Atmospheric Chemistry). A global dataset of aerosol mass spectrometer (AMS) measurements was used to evaluate simulated primary (POA) and secondary (SOA) OA concentrations. Model results are sensitive to the emission rates of intermediate-volatility organic compounds (IVOCs) and POA. Assuming enhanced reactivity of semi-volatile organic compounds (SVOCs) and IVOCs with OH substantially improved the model performance for SOA. The use of a hybrid approach for the parameterization of the aging of IVOCs had a small effect on predicted SOA levels. The model performance improved by assuming that freshly emitted organic compounds are relatively hydrophobic and become increasingly hygroscopic due to oxidation.

Modeling ozone and aerosol formation and transport in the pacific northwest with the community Multi-Scale Air Quality (CMAQ) modeling system.

Science.gov (United States)

O'Neill, Susan M; Lamb, Brian K; Chen, Jack; Claiborn, Candis; Finn, Dennis; Otterson, Sally; Figueroa, Cristiana; Bowman, Clint; Boyer, Mike; Wilson, Rob; Arnold, Jeff; Aalbers, Steven; Stocum, Jeffrey; Swab, Christopher; Stoll, Matt; Dubois, Mike; Anderson, Mary

2006-02-15

The Community Multi-Scale Air Quality (CMAQ) modeling system was used to investigate ozone and aerosol concentrations in the Pacific Northwest (PNW) during hot summertime conditions during July 1-15, 1996. Two emission inventories (El) were developed: emissions for the first El were based upon the National Emission Trend 1996 (NET96) database and the BEIS2 biogenic emission model, and emissions for the second El were developed through a "bottom up" approach that included biogenic emissions obtained from the GLOBEIS model. The two simulations showed that elevated PM2.5 concentrations occurred near and downwind of the Interstate-5 corridor along the foothills of the Cascade Mountains and in forested areas of central Idaho. The relative contributions of organic and inorganic aerosols varied by region, but generally organic aerosols constituted the largest fraction of PM2.5. In wilderness areas near the 1-5 corridor, organic carbon from anthropogenic sources contributed approximately 50% of the total organic carbon with the remainder from biogenic precursors, while in wilderness areas in Idaho, biogenic organic carbon accounted for 80% of the total organic aerosol. Regional analysis of the secondary organic aerosol formation in the Columbia River Gorge, Central Idaho, and the Olympics/Puget Sound showed that the production rate of secondary organic carbon depends on local terpene concentrations and the local oxidizing capacity of the atmosphere, which was strongly influenced by anthropogenic emissions. Comparison with observations from 12 IMPROVE sites and 21 ozone monitoring sites showed that results from the two El simulations generally bracketed the average observed PM parameters and that errors calculated for the model results were within acceptable bounds. Analysis across all statistical parameters indicated that the NW-AIRQUEST El solution performed better at predicting PM2.5, PM1, and beta(ext) even though organic carbon PM was over-predicted, and the NET96 El

Updates on the development of Deep Blue aerosol algorithm for constructing consistent long-term data records from MODIS to VIIRS

Science.gov (United States)

Hsu, N. Y. C.; Sayer, A. M.; Lee, J.; Kim, W. V.

2017-12-01

The impacts of natural and anthropogenic sources of air pollution on climate and human health have continued to gain attention from the scientific community. In order to facilitate these effects, high quality consistent long-term global aerosol data records from satellites are essential. Several EOS-era instruments (e.g., SeaWiFS, MODIS, and MISR) are able to provide such information with a high degree of fidelity. However, with the aging MODIS sensors and the launch of the VIIRS instrument on Suomi NPP in late 2011, the continuation of long-term aerosol data records suitable for climate studies from MODIS to VIIRS is needed urgently. Recently, we have successfully modified our MODIS Deep Blue algorithm to process the VIIRS data. Extensive works were performed in refining the surface reflectance determination scheme to account for the wavelength differences between MODIS and VIIRS. Better aerosol models (including non-spherical dust) are also now implemented in our VIIRS algorithm compared to the MODIS C6 algorithm. We will show the global (land and ocean) distributions of various aerosol products from Version 1 of the VIIRS Deep Blue data set. The preliminary validation results of these new VIIRS Deep Blue aerosol products using data from AERONET sunphotometers over land and ocean will be discussed. We will also compare the monthly averaged Deep Blue aerosol optical depth (AOD) from VIIRS with the MODIS C6 products to investigate if any systematic biases may exist between MODIS C6 and VIIRS AOD. The Version 1 VIIRS Deep Blue aerosol products are currently scheduled to be released to the public in 2018.

Herbivory by an Outbreaking Moth Increases Emissions of Biogenic Volatiles and Leads to Enhanced Secondary Organic Aerosol Formation Capacity.

Science.gov (United States)

Yli-Pirilä, Pasi; Copolovici, Lucian; Kännaste, Astrid; Noe, Steffen; Blande, James D; Mikkonen, Santtu; Klemola, Tero; Pulkkinen, Juha; Virtanen, Annele; Laaksonen, Ari; Joutsensaari, Jorma; Niinemets, Ülo; Holopainen, Jarmo K

2016-11-01

In addition to climate warming, greater herbivore pressure is anticipated to enhance the emissions of climate-relevant biogenic volatile organic compounds (VOCs) from boreal and subarctic forests and promote the formation of secondary aerosols (SOA) in the atmosphere. We evaluated the effects of Epirrita autumnata, an outbreaking geometrid moth, feeding and larval density on herbivore-induced VOC emissions from mountain birch in laboratory experiments and assessed the impact of these emissions on SOA formation via ozonolysis in chamber experiments. The results show that herbivore-induced VOC emissions were strongly dependent on larval density. Compared to controls without larval feeding, clear new particle formation by nucleation in the reaction chamber was observed, and the SOA mass loadings in the insect-infested samples were significantly higher (up to 150-fold). To our knowledge, this study provides the first controlled documentation of SOA formation from direct VOC emission of deciduous trees damaged by known defoliating herbivores and suggests that chewing damage on mountain birch foliage could significantly increase reactive VOC emissions that can importantly contribute to SOA formation in subarctic forests. Additional feeding experiments on related silver birch confirmed the SOA results. Thus, herbivory-driven volatiles are likely to play a major role in future biosphere-vegetation feedbacks such as sun-screening under daily 24 h sunshine in the subarctic.

Investigation on aerosol transport in containment cracks

International Nuclear Information System (INIS)

Parozzi, F.; Chatzidakis, S.; Housiadas, C.; Gelain, T.; Nahas, G.; Plumecocq, W.; Vendel, J.; Herranz, L.E.; Hinis, E.; Journeau, C.; Piluso, P.; Malgarida, E.

2005-01-01

Under severe accident conditions, the containment leak-tightness could be threatened by energetic phenomena that could yield a release to the environment of nuclear aerosols through penetrating concrete cracks. As few data are presently available to quantify this aerosol leakage, a specific action was launched in the framework of the Santar Project of the European 6 th Framework Programme. In this context, both theoretical and experimental investigations have been managed to develop a model that can readily be applied within a code like Aster (Accident Source Term Evaluation Code). Particle diffusion, settling, turbulent deposition, diffusiophoresis and thermophoresis have been considered as deposition mechanisms inside the crack path. They have been encapsulated in numerical models set up to reproduce experiments with small tubes and capillaries and simulate the plug formation. Then, an original lagrangian approach has been used to evaluate the crack retention under typical PWR accident conditions, comparing its predictions with those given by the eulerian approach implemented in the ECART code. On the experimental side, the paper illustrates an aerosol production and measurement system developed to validate aerosol deposition models into cracks and the results that can be obtained: a series of tests were performed with monodispersed fluorescein aerosols injected into a cracked concrete sample. A key result that should be further explored refers to the high enhancement of aerosol retention that could be due to steam condensation. Recommendations concerning future experimentation are also given in the paper. (author)

Aerosol modelling and validation during ESCOMPTE 2001

Science.gov (United States)

Cousin, F.; Liousse, C.; Cachier, H.; Bessagnet, B.; Guillaume, B.; Rosset, R.

The ESCOMPTE 2001 programme (Atmospheric Research. 69(3-4) (2004) 241) has resulted in an exhaustive set of dynamical, radiative, gas and aerosol observations (surface and aircraft measurements). A previous paper (Atmospheric Research. (2004) in press) has dealt with dynamics and gas-phase chemistry. The present paper is an extension to aerosol formation, transport and evolution. To account for important loadings of primary and secondary aerosols and their transformation processes in the ESCOMPTE domain, the ORISAM aerosol module (Atmospheric Environment. 35 (2001) 4751) was implemented on-line in the air-quality Meso-NH-C model. Additional developments have been introduced in ORganic and Inorganic Spectral Aerosol Module (ORISAM) to improve the comparison between simulations and experimental surface and aircraft field data. This paper discusses this comparison for a simulation performed during one selected day, 24 June 2001, during the Intensive Observation Period IOP2b. Our work relies on BC and OCp emission inventories specifically developed for ESCOMPTE. This study confirms the need for a fine resolution aerosol inventory with spectral chemical speciation. BC levels are satisfactorily reproduced, thus validating our emission inventory and its processing through Meso-NH-C. However, comparisons for reactive species generally denote an underestimation of concentrations. Organic aerosol levels are rather well simulated though with a trend to underestimation in the afternoon. Inorganic aerosol species are underestimated for several reasons, some of them have been identified. For sulphates, primary emissions were introduced. Improvement was obtained too for modelled nitrate and ammonium levels after introducing heterogeneous chemistry. However, no modelling of terrigeneous particles is probably a major cause for nitrates and ammonium underestimations. Particle numbers and size distributions are well reproduced, but only in the submicrometer range. Our work points out

Calibration of aerosol radiometers. Special aerosol sources

International Nuclear Information System (INIS)

Belkina, S.K.; Zalmanzon, Yu.E.; Kuznetsov, Yu.V.; Fertman, D.E.

1988-01-01

Problems of calibration of artificial aerosol radiometry and information-measurement systems of radiometer radiation control, in particular, are considered. Special aerosol source is suggested, which permits to perform certification and testing of aerosol channels of the systems in situ without the dismantling

Manuel UNIMARC format bibliographique

CERN Document Server

2007-01-01

This manual is the French translation of the second edition of UNIMARC Manual: bibliographic format published in English in 1994 and completed by 5 updates published from 1996 to 2005. This 5th French edition is composite. It reproduces identically a part of the 4th edition published in 2002 and, for the fields of the format modified in the Update 5, it offers a new more structured presentation. This is a handbook dedicated to French-speaking users of the UNIMARC format for bibliographic descriptions.

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

Formation and toxicological effect of secondary organic aerosols%二次有机气溶胶的形成及其毒理效应

Institute of Scientific and Technical Information of China (English)

曹军骥; 李建军

2016-01-01

Background, aim, and scope Along with the rapid development of Chinese economy, pollutants derived from increasing usage of fossil fuels and biofuels, as well as emissions from waste incineration and dust have been causing serious air pollution problems in many areas of China. Particular matter (PM), especially anthropogenic aerosols, emitted from various sources may alter regional atmospheric stability, and are of significant impact on climate change and human health. Comparing with PM10 (aerodynamic diameter≤10 μm), ifne particle (PM2.5, aerodynamic diameter≤2.5 μm) do more damage to human health. Organic matter (OM), an important chemical composition of ifne particle, takes 20%—90% of the ifne particles, has a signiifcant impact on air pollution and haze event which is happening in China, and has become a frontier of atmospheric chemistry research area. Consisting with many toxic compounds, such as polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs), organic amines and so on, organic aerosol is harmful for human health. Many in-vitro and in-vito studies of biological toxicity were focused on the primary particulate matters emitted directly from the pollution sources, however, attention for the formation and toxicity of secondary organic aerosols (SOA) are really scarce and therefore urgent.Materials and methods Taking PAHs, amines, and biogenic terpenes as examples, in order to improve the understanding on health damage of SOA pollution, this article brielfy reviewed the formation and bio-toxicity effects of speciifc group of SOA, and focused on the rising toxicity of the products comparing with their parent compounds.Results (1) Polycyclic aromatic hydrocarbons (PAHs). Because of the mutagenic, teratogenic and carcinogenic properties, PAHs has focused a great deal of attention from scientiifc researchers and is considered as one of the most important organic pollutants in the atmosphere. Parent PAHs in the aerosols can undergo a

Using the OMI aerosol index and absorption aerosol optical depth to evaluate the NASA MERRA Aerosol Reanalysis

Science.gov (United States)

Buchard, V.; da Silva, A. M.; Colarco, P. R.; Darmenov, A.; Randles, C. A.; Govindaraju, R.; Torres, O.; Campbell, J.; Spurr, R.

2015-05-01

A radiative transfer interface has been developed to simulate the UV aerosol index (AI) from the NASA Goddard Earth Observing System version 5 (GEOS-5) aerosol assimilated fields. The purpose of this work is to use the AI and aerosol absorption optical depth (AAOD) derived from the Ozone Monitoring Instrument (OMI) measurements as independent validation for the Modern Era Retrospective analysis for Research and Applications Aerosol Reanalysis (MERRAero). MERRAero is based on a version of the GEOS-5 model that is radiatively coupled to the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) aerosol module and includes assimilation of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor. Since AI is dependent on aerosol concentration, optical properties and altitude of the aerosol layer, we make use of complementary observations to fully diagnose the model, including AOD from the Multi-angle Imaging SpectroRadiometer (MISR), aerosol retrievals from the AErosol RObotic NETwork (AERONET) and attenuated backscatter coefficients from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission to ascertain potential misplacement of plume height by the model. By sampling dust, biomass burning and pollution events in 2007 we have compared model-produced AI and AAOD with the corresponding OMI products, identifying regions where the model representation of absorbing aerosols was deficient. As a result of this study over the Saharan dust region, we have obtained a new set of dust aerosol optical properties that retains consistency with the MODIS AOD data that were assimilated, while resulting in better agreement with aerosol absorption measurements from OMI. The analysis conducted over the southern African and South American biomass burning regions indicates that revising the spectrally dependent aerosol absorption properties in the near-UV region improves the modeled-observed AI comparisons

Multi-sensor cloud and aerosol retrieval simulator and remote sensing from model parameters - Part 2: Aerosols

Science.gov (United States)

Wind, Galina; da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

2016-07-01

operational remote-sensing algorithms.Specifically, the MCARS-computed radiances are input into the processing chain used to produce the MODIS Data Collection 6 aerosol product (M{O/Y}D04). The M{O/Y}D04 product is of course normally produced from M{O/Y}D021KM MODIS Level-1B radiance product directly acquired by the MODIS instrument. MCARS matches the format and metadata of a M{O/Y}D021KM product. The resulting MCARS output can be directly provided to MODAPS (MODIS Adaptive Processing System) as input to various operational atmospheric retrieval algorithms. Thus the operational algorithms can be tested directly without needing to make any software changes to accommodate an alternative input source.We show direct application of this synthetic product in analysis of the performance of the MOD04 operational algorithm. We use biomass-burning case studies over Amazonia employed in a recent Working Group on Numerical Experimentation (WGNE)-sponsored study of aerosol impacts on numerical weather prediction (Freitas et al., 2015). We demonstrate that a known low bias in retrieved MODIS aerosol optical depth appears to be due to a disconnect between actual column relative humidity and the value assumed by the MODIS aerosol product.

Multi-Sensor Cloud and Aerosol Retrieval Simulator and Remote Sensing from Model Parameters . Part 2; Aerosols

Science.gov (United States)

Wind, Galina; Da Silva, Arlindo M.; Norris, Peter M.; Platnick, Steven; Mattoo, Shana; Levy, Robert C.

2016-01-01

operational remote-sensing algorithms. Specifically, the MCARS-computed radiances are input into the processing chain used to produce the MODIS Data Collection 6 aerosol product (MOYD04). TheMOYD04 product is of course normally produced from MOYD021KM MODIS Level-1B radiance product directly acquired by the MODIS instrument. MCARS matches the format and metadata of a MOYD021KM product. The resulting MCARS output can be directly provided to MODAPS (MODIS Adaptive Processing System) as input to various operational atmospheric retrieval algorithms. Thus the operational algorithms can be tested directly without needing to make any software changes to accommodate an alternative input source. We show direct application of this synthetic product in analysis of the performance of the MOD04 operational algorithm. We use biomass-burning case studies over Amazonia employed in a recent Working Group on Numerical Experimentation (WGNE)-sponsored study of aerosol impacts on numerical weather prediction (Freitas et al., 2015). We demonstrate that a known low bias in retrieved MODIS aerosol optical depth appears to be due to a disconnect between actual column relative humidity and the value assumed by the MODIS aerosol product.

Aerosol dynamics within and above forest in relation to turbulent transport and dry deposition

OpenAIRE

Rannik, Üllar; Zhou, Luxi; Zhou, Putian; Gierens, Rosa; Mammarella, Ivan; Sogachev, Andrey; Boy, Michael

2016-01-01

A 1-D atmospheric boundary layer (ABL) model coupled with a detailed atmospheric chemistry and aerosol dynamical model, the model SOSAA, was used to predict the ABL and detailed aerosol population (characterized by the number size distribution) time evolution. The model was applied over a period of 10 days in May 2013 to a pine forest site in southern Finland. The period was characterized by frequent new particle formation events and simultaneous intensive aerosol transforma...

Development and Application of an Oxidation Flow Reactor to Study Secondary Organic Aerosol Formation from Ambient Air

Science.gov (United States)

Palm, Brett Brian

Secondary organic aerosols (SOA) in the atmosphere play an important role in air quality, human health, and climate. However, the sources, formation pathways, and fate of SOA are poorly constrained. In this dissertation, I present development and application of the oxidation flow reactor (OFR) technique for studying SOA formation from OH, O3, and NO3 oxidation of ambient air. With a several-minute residence time and a portable design with no inlet, OFRs are particularly well-suited for this purpose. I first introduce the OFR concept, and discuss several advances I have made in performing and interpreting OFR experiments. This includes estimating oxidant exposures, modeling the fate of low-volatility gases in the OFR (wall loss, condensation, and oxidation), and comparing SOA yields of single precursors in the OFR with yields measured in environmental chambers. When these experimental details are carefully considered, SOA formation in an OFR can be more reliably compared with ambient SOA formation processes. I then present an overview of what OFR measurements have taught us about SOA formation in the atmosphere. I provide a comparison of SOA formation from OH, O3, and NO3 oxidation of ambient air in a wide variety of environments, from rural forests to urban air. In a rural forest, the SOA formation correlated with biogenic precursors (e.g., monoterpenes). In urban air, it correlated instead with reactive anthropogenic tracers (e.g., trimethylbenzene). In mixed-source regions, the SOA formation did not correlate well with any single precursor, but could be predicted by multilinear regression from several precursors. Despite these correlations, the concentrations of speciated ambient VOCs could only explain approximately 10-50% of the total SOA formed from OH oxidation. In contrast, ambient VOCs could explain all of the SOA formation observed from O3 and NO3 oxidation. Evidence suggests that lower-volatility gases (semivolatile and intermediate-volatility organic

A simple parameterization of aerosol emissions in RAMS

Science.gov (United States)

Letcher, Theodore

Throughout the past decade, a high degree of attention has been focused on determining the microphysical impact of anthropogenically enhanced concentrations of Cloud Condensation Nuclei (CCN) on orographic snowfall in the mountains of the western United States. This area has garnered a lot of attention due to the implications this effect may have on local water resource distribution within the Region. Recent advances in computing power and the development of highly advanced microphysical schemes within numerical models have provided an estimation of the sensitivity that orographic snowfall has to changes in atmospheric CCN concentrations. However, what is still lacking is a coupling between these advanced microphysical schemes and a real-world representation of CCN sources. Previously, an attempt to representation the heterogeneous evolution of aerosol was made by coupling three-dimensional aerosol output from the WRF Chemistry model to the Colorado State University (CSU) Regional Atmospheric Modeling System (RAMS) (Ward et al. 2011). The biggest problem associated with this scheme was the computational expense. In fact, the computational expense associated with this scheme was so high, that it was prohibitive for simulations with fine enough resolution to accurately represent microphysical processes. To improve upon this method, a new parameterization for aerosol emission was developed in such a way that it was fully contained within RAMS. Several assumptions went into generating a computationally efficient aerosol emissions parameterization in RAMS. The most notable assumption was the decision to neglect the chemical processes in formed in the formation of Secondary Aerosol (SA), and instead treat SA as primary aerosol via short-term WRF-CHEM simulations. While, SA makes up a substantial portion of the total aerosol burden (much of which is made up of organic material), the representation of this process is highly complex and highly expensive within a numerical

Effect of Heterogeneous Chemical Reactions on the Köhler Activation of Aqueous Organic Aerosols.

Science.gov (United States)

Djikaev, Yuri S; Ruckenstein, Eli

2018-05-03

We study some thermodynamic aspects of the activation of aqueous organic aerosols into cloud droplets considering the aerosols to consist of liquid solution of water and hydrophilic and hydrophobic organic compounds, taking into account the presence of reactive species in the air. The hydrophobic (surfactant) organic molecules on the surface of such an aerosol can be processed by chemical reactions with some atmospheric species; this affects the hygroscopicity of the aerosol and hence its ability to become a cloud droplet either via nucleation or via Köhler activation. The most probable pathway of such processing involves atmospheric hydroxyl radicals that abstract hydrogen atoms from hydrophobic organic molecules located on the aerosol surface (first step), the resulting radicals being quickly oxidized by ubiquitous atmospheric oxygen molecules to produce surface-bound peroxyl radicals (second step). These two reactions play a crucial role in the enhancement of the Köhler activation of the aerosol and its evolution into a cloud droplet. Taking them and a third reaction (next in the multistep chain of relevant heterogeneous reactions) into account, one can derive an explicit expression for the free energy of formation of a four-component aqueous droplet on a ternary aqueous organic aerosol as a function of four independent variables of state of a droplet. The results of numerical calculations suggest that the formation of cloud droplets on such (aqueous hydrophilic/hydrophobic organic) aerosols is most likely to occur as a Köhler activation-like process rather than via nucleation. The model allows one to determine the threshold parameters of the system necessary for the Köhler activation of such aerosols, which are predicted to be very sensitive to the equilibrium constant of the chain of three heterogeneous reactions involved in the chemical aging of aerosols.

Aerosol nucleation and growth and their coupling to thermal hydraulics

International Nuclear Information System (INIS)

Clement, C.F.

1985-01-01

We examine the physical processes leading to vapour condensation as an aerosol in the formation and cooling of vapour-gas mixtures. Requirements for mathematical, computer and experimental modelling are discussed in relation to nuclear aerosols. In the absence of sudden pressure drops we give a complete schematic set of equations which govern the motion of aerosol, vapour, gas and heat including radiation. The coupling to the aerosol equation is mainly through the droplet growth rate, R, and a nucleation term whose possible forms are described. Rapid equilibration between vapour and aerosol means that the likely heterogeneous nucleation term must be treated separately. General forms are given for the coupling terms in the equations for vapour concentration and temperature in terms of the local mass transfer rate to the aerosol. The properties of this quantity are shown clearly by an expression for it obtained in terms of Lewis and condensation numbers and the quantify, zeta, whose derivative gives the local total heat transfer rate. Sizes of these numbers are given for some relevant vapour-gas mixtures. Throughout the paper we give the physical requirements necessary to make the transitions to the more calculable cases of uniform or well-mixed aerosols, and finally we discuss the case of initially unsaturated vapour-gas mixtures. (orig.)

Evaluation of the MODIS Aerosol Retrievals over Ocean and Land during CLAMS.

Science.gov (United States)

Levy, R. C.; Remer, L. A.; Martins, J. V.; Kaufman, Y. J.; Plana-Fattori, A.; Redemann, J.; Wenny, B.

2005-04-01

The Chesapeake Lighthouse Aircraft Measurements for Satellites (CLAMS) experiment took place from 10 July to 2 August 2001 in a combined ocean-land region that included the Chesapeake Lighthouse [Clouds and the Earth's Radiant Energy System (CERES) Ocean Validation Experiment (COVE)] and the Wallops Flight Facility (WFF), both along coastal Virginia. This experiment was designed mainly for validating instruments and algorithms aboard the Terra satellite platform, including the Moderate Resolution Imaging Spectroradiometer (MODIS). Over the ocean, MODIS retrieved aerosol optical depths (AODs) at seven wavelengths and an estimate of the aerosol size distribution. Over the land, MODIS retrieved AOD at three wavelengths plus qualitative estimates of the aerosol size. Temporally coincident measurements of aerosol properties were made with a variety of sun photometers from ground sites and airborne sites just above the surface. The set of sun photometers provided unprecedented spectral coverage from visible (VIS) to the solar near-infrared (NIR) and infrared (IR) wavelengths. In this study, AOD and aerosol size retrieved from MODIS is compared with similar measurements from the sun photometers. Over the nearby ocean, the MODIS AOD in the VIS and NIR correlated well with sun-photometer measurements, nearly fitting a one-to-one line on a scatterplot. As one moves from ocean to land, there is a pronounced discontinuity of the MODIS AOD, where MODIS compares poorly to the sun-photometer measurements. Especially in the blue wavelength, MODIS AOD is too high in clean aerosol conditions and too low under larger aerosol loadings. Using the Second Simulation of the Satellite Signal in the Solar Spectrum (6S) radiative code to perform atmospheric correction, the authors find inconsistency in the surface albedo assumptions used by the MODIS lookup tables. It is demonstrated how the high bias at low aerosol loadings can be corrected. By using updated urban/industrial aerosol

Integrated aerosol and thermalhydraulics modelling for CANDU safety analysis

International Nuclear Information System (INIS)

McDonald, B.H.; Hanna, B.N.

1990-08-01

Analysis of postulated accidents in CANDU reactors that could result in severe fuel damage requires the ability to model the formation of aerosols containing fission product materials and the transport of these aerosols from the fuel, through containment, to any leak to the atmosphere. Best-estimate calculations require intimate coupling and simultaneous solution of all the equations describing the entire range of physical and chemical phenomena involved. The prototype CATHENA/PACE-3D has been developed for integrated calculation of thermalhydraulic and aerosol events in a CANDU reactor during postulated accidents. Examples demonstrate the ability of CATHENA/PACE-3D to produce realistic flow and circulation patterns and reasonable accuracy in solution of two simple fluid-flow test cases for which analytical solutions exist

Adjoint sensitivity of global cloud droplet number to aerosol and dynamical parameters

Directory of Open Access Journals (Sweden)

V. A. Karydis

2012-10-01

Full Text Available We present the development of the adjoint of a comprehensive cloud droplet formation parameterization for use in aerosol-cloud-climate interaction studies. The adjoint efficiently and accurately calculates the sensitivity of cloud droplet number concentration (CDNC to all parameterization inputs (e.g., updraft velocity, water uptake coefficient, aerosol number and hygroscopicity with a single execution. The adjoint is then integrated within three dimensional (3-D aerosol modeling frameworks to quantify the sensitivity of CDNC formation globally to each parameter. Sensitivities are computed for year-long executions of the NASA Global Modeling Initiative (GMI Chemical Transport Model (CTM, using wind fields computed with the Goddard Institute for Space Studies (GISS Global Circulation Model (GCM II', and the GEOS-Chem CTM, driven by meteorological input from the Goddard Earth Observing System (GEOS of the NASA Global Modeling and Assimilation Office (GMAO. We find that over polluted (pristine areas, CDNC is more sensitive to updraft velocity and uptake coefficient (aerosol number and hygroscopicity. Over the oceans of the Northern Hemisphere, addition of anthropogenic or biomass burning aerosol is predicted to increase CDNC in contrast to coarse-mode sea salt which tends to decrease CDNC. Over the Southern Oceans, CDNC is most sensitive to sea salt, which is the main aerosol component of the region. Globally, CDNC is predicted to be less sensitive to changes in the hygroscopicity of the aerosols than in their concentration with the exception of dust where CDNC is very sensitive to particle hydrophilicity over arid areas. Regionally, the sensitivities differ considerably between the two frameworks and quantitatively reveal why the models differ considerably in their indirect forcing estimates.

Aerosol chemical and optical properties over the Paris area within ESQUIF project

Directory of Open Access Journals (Sweden)

A. Hodzic

2006-01-01

mineral dust accounts for 8%. The comparison demonstrates the absence of systematic errors in the simulated sulfate, ammonium and nitrates total concentrations. However, for nitrates the observed partition between fine and coarse mode is not reproduced. In CHIMERE there is a clear lack of coarse-mode nitrates. This calls for additional parameterizations in order to account for the heterogeneous formation of nitrate onto dust particles. Larger discrepancies are obtained for the secondary organic aerosols due to both inconsistencies in the SOA formation processes in the model leading to an underestimation of their mass and large uncertainties in the determination of the measured aerosol organic fraction. The observed mass distribution of aerosols is not well reproduced, although no clear explanation can be given.

Synergistic reaction between SO2 and NO2 on mineral oxides: a potential formation pathway of sulfate aerosol.

Science.gov (United States)

Liu, Chang; Ma, Qingxin; Liu, Yongchun; Ma, Jinzhu; He, Hong

2012-02-07

Sulfate is one of the most important aerosols in the atmosphere. A new sulfate formation pathway via synergistic reactions between SO(2) and NO(2) on mineral oxides was proposed. The heterogeneous reactions of SO(2) and NO(2) on CaO, α-Fe(2)O(3), ZnO, MgO, α-Al(2)O(3), TiO(2), and SiO(2) were investigated by in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (in situ DRIFTS) at ambient temperature. Formation of sulfate from adsorbed SO(2) was promoted by the coexisting NO(2), while surface N(2)O(4) was observed as the crucial oxidant for the oxidation of surface sulfite. This process was significantly promoted by the presence of O(2). The synergistic effect between SO(2) and NO(2) was not observed on other mineral particles (such as CaCO(3) and CaSO(4)) probably due to the lack of the surface reactive oxygen sites. The synergistic reaction between SO(2) and NO(2) on mineral oxides resulted in the formation of internal mixtures of sulfate, nitrate, and mineral oxides. The change of mixture state will affect the physicochemical properties of atmospheric particles and therefore further influence their environmental and climate effects.

High-power laser radiation in atmospheric aerosols: Nonlinear optics of aerodispersed media

Science.gov (United States)

Zuev, V. E.; Zemlianov, A. A.; Kopytin, Iu. D.; Kuzikovskii, A. V.

The bulk of this book contains the results of investigations carried out at the Institute of Atmospheric Optics, Siberian Branch, USSR Academy of Science with the participation of the authors. The microphysical and optical characteristics of atmospheric aerosols are considered, taking into account light scattering by a single aerosol particle, light scattering by a system of particles, the scattering phase matrix, light scattering by clouds and fogs, light scattering by hazes, and scattering phase functions of polydispersed aerosols. Other topics studies are related to low-energy (subexplosive) effects of radiation on individual particles, the formation of clear zones in clouds and fogs due to the vaporization of droplets under regular regimes, self-action of a wave beam in a water aerosol under conditions of regular droplet vaporization, laser beam propagation through an explosively evaporating water-droplet aerosol, the propagation of high-power laser radiation through hazes, the ionization and optical breakdown in aerosol media, and laser monitoring of a turbid atmosphere using nonlinear effects.

SAGE aerosol measurements. Volume 1, February 21, 1979 to December 31, 1979

International Nuclear Information System (INIS)

Mccormick, M.P.

1985-10-01

The Stratospheric Aerosol and Gas Experiment (SAGE) satellite system, launched on February 18, 1979, provides profiles of aerosol extinction, ozone concentration, and nitrogen dioxide concentration between about 80 N and 80 S. Zonal averages, separated into sunrise and sunset events, and seasonal averages of the aerosol extinction at 1.00 microns and 0.45 microns ratios of the aerosol extinction to the molecular extinction at 1.00 microns, and ratios of the aerosol extinction at 0.45 microns to the aerosol extinction at 1.00 microns are given. The averages for 1979 are shown in tables and in profile and contour plots (as a function of altitude and latitude). In addition, temperature data provided by the National Oceanic and Atmospheric Administration (NOAA) for the time and location of each SAGE measurement are averaged and shown in a similar format. Typical values of the peak aerosol extinction were 0.0001 to 0.0002 km at 1.00 microns depth values for the 1.00 microns channel varied between 0.001 and 0.002 over all latitudes

Effects of Relative Humidity on Ozone and Secondary Organic Aerosol Formation from the Photooxidation of Benzene and Ethylbenzene

Science.gov (United States)

Jia, L.; Xu, Y.

2012-12-01

The formation of ozone and secondary organic aerosol from benzene-NOx and ethylbenzene-NOx irradiations was investigated under different levels of relative humidity (RH) in a smog chamber. The results show that the increase in RH can greatly reduce the maximum O3 by the transformation of -NO2 and -ONO2-containing products into the particle phase. In benzene irradiations, the SOA number concentration increases over 26 times as RH rises from ethylbenzene irradiations, ethylglyoxal favors the formation of monohydrate, which limits the RH effects. During evaporating processes, the lost substances have similar structures for both benzene and ethylbenzene. This demonstrates that ethyl-containing substances are very stable and difficult to evaporate. For benzene some of glyoxal hydrates are left to form C-O-C and C=O-containing species like hemiacetal and acetal after evaporation, whereas for ethylbenzene, glyoxal favors cross reactions with ethylglyoxal during the evaporating process. It is concluded that the increase in RH can irreversibly enhance the yields of SOA from both benzene and ethylbenzene.

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

New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model

Directory of Open Access Journals (Sweden)

A. Kürten

2018-01-01

Full Text Available A recent CLOUD (Cosmics Leaving OUtdoor Droplets chamber study showed that sulfuric acid and dimethylamine produce new aerosols very efficiently and yield particle formation rates that are compatible with boundary layer observations. These previously published new particle formation (NPF rates are reanalyzed in the present study with an advanced method. The results show that the NPF rates at 1.7 nm are more than a factor of 10 faster than previously published due to earlier approximations in correcting particle measurements made at a larger detection threshold. The revised NPF rates agree almost perfectly with calculated rates from a kinetic aerosol model at different sizes (1.7 and 4.3 nm mobility diameter. In addition, modeled and measured size distributions show good agreement over a wide range of sizes (up to ca. 30 nm. Furthermore, the aerosol model is modified such that evaporation rates for some clusters can be taken into account; these evaporation rates were previously published from a flow tube study. Using this model, the findings from the present study and the flow tube experiment can be brought into good agreement for the high base-to-acid ratios (∼ 100 relevant for this study. This confirms that nucleation proceeds at rates that are compatible with collision-controlled (a.k.a. kinetically controlled NPF for the conditions during the CLOUD7 experiment (278 K, 38 % relative humidity, sulfuric acid concentration between 1  ×  106 and 3  ×  107 cm−3, and dimethylamine mixing ratio of ∼  40 pptv, i.e., 1  ×  109 cm−3.

Air pollution control and decreasing new particle formation lead to strong climate warming

OpenAIRE

Makkonen, R.; Asmi, A.; Kerminen, V.-M.; Boy, M.; Arneth, A.; Hari, P.; Kulmala, M.

2012-01-01

The number concentration of cloud droplets determines several climatically relevant cloud properties. A major cause for the high uncertainty in the indirect aerosol forcing is the availability of cloud condensation nuclei (CCN), which in turn is highly sensitive to atmospheric new particle formation. Here we present the effect of new particle formation on anthropogenic aerosol forcing in present-day (year 2000) and future (year 2100) conditions. The present-day total aerosol forcing is increa...

Aerosol Properties of the Atmospheres of Extrasolar Giant Planets

Energy Technology Data Exchange (ETDEWEB)

Lavvas, P. [Groupe de Spectrométrie Moléculaire et Atmosphérique, UMR CNRS 7331, Université de Reims Champagne Ardenne, Reims (France); Koskinen, T., E-mail: panayotis.lavvas@univ-reims.fr [Lunar and Planetary Laboratory, University of Arizona, Tucson, AZ (United States)

2017-09-20

We use a model of aerosol microphysics to investigate the impact of high-altitude photochemical aerosols on the transmission spectra and atmospheric properties of close-in exoplanets, such as HD 209458 b and HD 189733 b. The results depend strongly on the temperature profiles in the middle and upper atmospheres, which are poorly understood. Nevertheless, our model of HD 189733 b, based on the most recently inferred temperature profiles, produces an aerosol distribution that matches the observed transmission spectrum. We argue that the hotter temperature of HD 209458 b inhibits the production of high-altitude aerosols and leads to the appearance of a clearer atmosphere than on HD 189733 b. The aerosol distribution also depends on the particle composition, photochemical production, and atmospheric mixing. Due to degeneracies among these inputs, current data cannot constrain the aerosol properties in detail. Instead, our work highlights the role of different factors in controlling the aerosol distribution that will prove useful in understanding different observations, including those from future missions. For the atmospheric mixing efficiency suggested by general circulation models, we find that the aerosol particles are small (∼nm) and probably spherical. We further conclude that a composition based on complex hydrocarbons (soots) is the most likely candidate to survive the high temperatures in hot-Jupiter atmospheres. Such particles would have a significant impact on the energy balance of HD 189733 b’s atmosphere and should be incorporated in future studies of atmospheric structure. We also evaluate the contribution of external sources to photochemical aerosol formation and find that their spectral signature is not consistent with observations.

Impact of anthropogenic aerosols on present and future climate

International Nuclear Information System (INIS)

Deandreis, C.

2008-03-01

Aerosols influence the Earth radiative budget both through their direct effect (scattering and absorption of solar radiation) and their indirect effect (impacts on cloud microphysics). The role of anthropogenic aerosol in climate change has been recognized to be significant when compared to the one of greenhouse gases. Despite many studies on this topic, the assessments of both anthropogenic aerosol radiative forcing and their impacts on meteorological variables are still very uncertain. Major reasons for these uncertainties stem from the insufficient knowledge of the emissions sources and of the processes of formation, transformation and deposition. Models used to study climate are often inadequate to study aerosol processes because of coarse spatial and temporal scales. Uncertainties due to the parameterization of the aerosol are added to the uncertainties in the representation of large scale dynamics and physical processes such as transport, hydrological cycle and radiative budget. To predict, the role of the anthropogenic aerosol impact in the future climate change, I have addressed some of these key uncertainties. In this study, I simulate interactively aerosols processes in a climate model in order to improve the estimation of their direct and indirect effects. I estimate a modification of the top of the atmosphere net flux of 60% for the present period. I also show that, for future projection, the representation of the emissions source is an other important source of error. I assess that aerosols radiative forcing differ by 40% between simulations performed with 2 different emissions inventories. These inventories are representative for a high and a low limit in term of carbonaceous aerosols emissions for the 2050 horizon. (author)

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

Impact of Biomass Burning Aerosols on Cloud Formation in Coastal Regions

Science.gov (United States)

Nair, U. S.; Wu, Y.; Reid, J. S.

2017-12-01

In the tropics, shallow and deep convective cloud structures organize in hierarchy of spatial scales ranging from meso-gamma (2-20 km) to planetary scales (40,000km). At the lower end of the spectrum is shallow convection over the open ocean, whose upscale growth is dependent upon mesoscale convergence triggers. In this context, cloud systems associated with land breezes that propagate long distances into open ocean areas are important. We utilized numerical model simulations to examine the impact of biomass burning on such cloud systems in the maritime continent, specifically along the coastal regions of Sarawak. Numerical model simulations conducted using the Weather Research and Forecasting Chemistry (WRF-Chem) model show spatial patterns of smoke that show good agreement to satellite observations. Analysis of model simulations show that, during daytime the horizontal convective rolls (HCRs) that form over land play an important role in organizing transport of smoke in the coastal regions. Alternating patterns of low and high smoke concentrations that are well correlated to the wavelengths of HCRs are found in both the simulations and satellite observations. During night time, smoke transport is modulated by the land breeze circulation and a band of enhanced smoke concentration is found along the land breeze front. Biomass burning aerosols are ingested by the convective clouds that form along the land breeze and leads to changes in total water path, cloud structure and precipitation formation.

Combustion and smoke formation following exposure of actinide metals to explosions

International Nuclear Information System (INIS)

Luna, R.E.; Church, H.W.; Elrick, R.M.; Parker, D.R.; Nelson, L.S.

1976-01-01

Results from the plutonium aerosol generation experiment (PAGE) program studies indicate that: (1) Significant quantities of metal-bearing aerosols are likely to be formed in an accidental high explosive detonation of a nuclear weapon. Although the explosive charge-to-metal ratio has been reduced in modern weapons, considerable inhalation hazard is still expected due to increased shrapnel formation and streamer combustion. (2) Close-in shrapnel particle sizes and velocities can be estimated by impact sampling techniques. (3) Uranium droplets are a very accurate simulant of plutonium droplets from the standpoint of combustion-related phenomena but do not seem to simulate either the total quantity of aerosol formed from plutonium droplets or its time-dependent generation pattern very well. This is due primarily to the large effect of the explosion of the burning uranium droplets on total aerosol formation which is not observed in the case of plutonium, even though more aerosol is produced per unit time during the actual combustion itself. (4) The formation of chain-like plutonium aerosols from the droplets produced during streamer combustion is expected to produce an unusually active material from the standpoint of inhalation into the lung and ultimate translocation in the body. 16 figures

Updated African biomass burning emission inventories in the framework of the AMMA-IDAF program, with an evaluation of combustion aerosols

Directory of Open Access Journals (Sweden)

C. Liousse

2010-10-01

Full Text Available African biomass burning emission inventories for gaseous and particulate species have been constructed at a resolution of 1 km by 1km with daily coverage for the 2000–2007 period. These inventories are higher than the GFED2 inventories, which are currently widely in use. Evaluation specifically focusing on combustion aerosol has been carried out with the ORISAM-TM4 global chemistry transport model which includes a detailed aerosol module. This paper compares modeled results with measurements of surface BC concentrations and scattering coefficients from the AMMA Enhanced Observations period, aerosol optical depths and single scattering albedo from AERONET sunphotometers, LIDAR vertical distributions of extinction coefficients as well as satellite data. Aerosol seasonal and interannual evolutions over the 2004–2007 period observed at regional scale and more specifically at the Djougou (Benin and Banizoumbou (Niger AMMA/IDAF sites are well reproduced by our global model, indicating that our biomass burning emission inventory appears reasonable.

Atmospheric carbonaceous aerosols from Indo-Gangetic Plain and Central Himalaya: impact of anthropogenic sources.

Science.gov (United States)

Ram, Kirpa; Sarin, M M

2015-01-15

In the present-day scenario of growing anthropogenic activities, carbonaceous aerosols contribute significantly (∼20-70%) to the total atmospheric particulate matter mass and, thus, have immense potential to influence the Earth's radiation budget and climate on a regional to global scale. In addition, formation of secondary organic aerosols is being increasingly recognized as an important process in contributing to the air-pollution and poor visibility over urban regions. It is, thus, essential to study atmospheric concentrations of carbonaceous species (EC, OC and WSOC), their mixing state and absorption properties on a regional scale. This paper presents the comprehensive data on emission sources, chemical characteristics and optical properties of carbonaceous aerosols from selected urban sites in the Indo-Gangetic Plain (IGP) and from a high-altitude location in the central Himalaya. The mass concentrations of OC, EC and WSOC exhibit large spatio-temporal variability in the IGP. This is attributed to seasonally varying emissions from post-harvest agricultural-waste burning, their source strength, boundary layer dynamics and secondary aerosol formation. The high concentrations of OC and SO4(2-), and their characteristic high mass scattering efficiency, contribute significantly to the aerosol optical depth and scattering coefficient. This has implications to the assessment of single scattering albedo and aerosol radiative forcing on a regional scale. Copyright © 2014 Elsevier Ltd. All rights reserved.

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

Energy Technology Data Exchange (ETDEWEB)

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

1997-12-31

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

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

Energy Technology Data Exchange (ETDEWEB)

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

1998-12-31

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

Multistatic Aerosol Cloud Lidar in Space: A Theoretical Perspective

Science.gov (United States)

Mishchenko, Michael I.; Alexandrov, Mikhail D.; Cairns, Brian; Travis, Larry D.

2016-01-01

Accurate aerosol and cloud retrievals from space remain quite challenging and typically involve solving a severely ill-posed inverse scattering problem. In this Perspective, we formulate in general terms an aerosol and aerosol-cloud interaction space mission concept intended to provide detailed horizontal and vertical profiles of aerosol physical characteristics as well as identify mutually induced changes in the properties of aerosols and clouds. We argue that a natural and feasible way of addressing the ill-posedness of the inverse scattering problem while having an exquisite vertical-profiling capability is to fly a multistatic (including bistatic) lidar system. We analyze theoretically the capabilities of a formation-flying constellation of a primary satellite equipped with a conventional monostatic (backscattering) lidar and one or more additional platforms each hosting a receiver of the scattered laser light. If successfully implemented, this concept would combine the measurement capabilities of a passive multi-angle multi-spectral polarimeter with the vertical profiling capability of a lidar; address the ill-posedness of the inverse problem caused by the highly limited information content of monostatic lidar measurements; address the ill-posedness of the inverse problem caused by vertical integration and surface reflection in passive photopolarimetric measurements; relax polarization accuracy requirements; eliminate the need for exquisite radiative-transfer modeling of the atmosphere-surface system in data analyses; yield the day-and-night observation capability; provide direct characterization of ground-level aerosols as atmospheric pollutants; and yield direct measurements of polarized bidirectional surface reflectance. We demonstrate, in particular, that supplementing the conventional backscattering lidar with just one additional receiver flown in formation at a scattering angle close to 170deg can dramatically increase the information content of the

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

Energy Technology Data Exchange (ETDEWEB)

Davidovits, Paul [Boston College, Chestnut Hill, MA (United States)

2015-10-20

Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign and much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a

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

BVOC-aerosol-climate interactions in the global aerosol-climate model ECHAM5.5-HAM2

Directory of Open Access Journals (Sweden)

R. Makkonen

2012-11-01

Full Text Available The biosphere emits volatile organic compounds (BVOCs which, after oxidation in the atmosphere, can partition on the existing aerosol population or even form new particles. The large quantities emitted provide means for a large potential impact on both aerosol direct and indirect effects. Biogenic responses to atmospheric temperature change can establish feedbacks even in rather short timescales. However, due to the complexity of organic aerosol partitioning, even the sign of these feedbacks is of large uncertainty. We use the global aerosol-climate model ECHAM5.5-HAM2 to explore the effect of BVOC emissions on new particle formation, clouds and climate. Two BVOC emission models, MEGAN2 and LPJ-GUESS, are used. MEGAN2 shows a 25% increase while LPJ-GUESS shows a slight decrease in global BVOC emission between years 2000 and 2100. The change of shortwave cloud forcing from year 1750 to 2000 ranges from −1.4 to −1.8 W m⁻² with 5 different nucleation mechanisms. We show that the change in shortwave cloud forcing from the year 2000 to 2100 ranges from 1.0 to 1.5 W m⁻². Although increasing future BVOC emissions provide 3–5% additional CCN, the effect on the cloud albedo change is modest. Due to simulated decreases in future cloud cover, the increased CCN concentrations from BVOCs can not provide significant additional cooling in the future.

Vacuum FTIR study on the hygroscopicity of magnesium acetate aerosols

Science.gov (United States)

Wang, Na; Cai, Chen; He, Xiang; Pang, Shu-Feng; Zhang, Yun-Hong

2018-03-01

Hygroscopicity and volatility of secondary organic aerosol (SOA) are two important properties, which determine the composition, concentration, size, phase state of SOA and thus chemical and optical properties for SOA. In this work, magnesium acetate (Mg(Ac)2) aerosol was used as a simple SOA model in order to reveal relationship between hygroscopicity and volatility. A novel approach was set up based on a combination of a vacuum FTIR spectrometer and a home-made relative humidity (RH) controlling system. The striking advantage of this approach was that the RH and the compositions of aerosols could be obtained from a same IR spectrum, which guaranteed the synchronism between RH and spectral features on a sub-second scale. At the constant RH of 90% and 80% for 3000 s, the water content within Mg(Ac)2 aerosol particles decreased about 19.0% and 9.4% while there were 13.4% and 6.0% of acetate loss. This was attributed to a cooperation between volatile of acetic acid and Mg2 + hydrolysis in Mg(Ac)2 aerosols, which greatly suppressed the hygroscopicity of Mg(Ac)2 aerosols. When the RH changed with pulsed mode between 70% and 90%, hygroscopicity relaxation was observed for Mg(Ac)2 aerosols. Diffuse coefficient of water in the relaxation process was estimated to be 5 × 10- 12 m2·s- 1 for the Mg(Ac)2 aerosols. Combining the IR spectra analysis, the decrease in the diffuse coefficient of water was due to the formation of magnesium hydroxide accompanying acetic acid evaporation in the aerosols.

Investigation of the tracers for plastic-enriched waste burning aerosols