The AeroCom evaluation and intercomparison of organic aerosol in global models

Atmospheric chemistry and physics, Journal Year: 2014, Volume and Issue: 14(19), P. 10845 - 10895

Published: Oct. 15, 2014

Abstract. This paper evaluates the current status of global modeling organic aerosol (OA) in troposphere and analyzes differences between models as well observations. Thirty-one chemistry transport (CTMs) general circulation (GCMs) have participated this intercomparison, framework AeroCom phase II. The simulation OA varies greatly terms magnitude primary emissions, secondary (SOA) formation, number species used (2 to 62), complexity parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, microphysics), physical, optical properties. diversity results has increased since earlier experiments, mainly due increasing SOA parameterization models, implementation new, highly uncertain, sources. Diversity over one order exists modeled vertical distribution concentrations that deserves a dedicated future study. Furthermore, although / OC ratio depends on sources atmospheric processing, is important for model evaluation against observations, it resolved only by few models.

median (POA) source strength 56 Tg a⁻¹ (range 34–144 a⁻¹) (natural anthropogenic) 19 13–121 a⁻¹). Among take into account semi-volatile nature, calculated be 51 16–121 a⁻¹), much larger than value calculate more simplistic way (19 a⁻¹; range 13–20 a⁻¹, with at 37 burden 1.4 (24 0.6–2.0 4 2.0 3.8 Tg), lifetime 5.4 days 3.8–9.6 days). In reported both sulfate burdens, OA/sulfate 0.77; 13 lower 1, 9 higher 1. For 26 deposition fluxes, wet removal 70 28–209 which average 85% total deposition. Fine carbon (OC) observations from continuous monitoring networks individual field campaigns been evaluation. At urban locations, model–observation comparison indicates missing knowledge anthropogenic sources, seasonality. combined model–measurements analysis suggests existence levels during summer biogenic formation large areas USA can same POA, even contribute measured seasonal pattern. Global are able simulate high character observed atmosphere result POA amount present remains largely underestimated, mean normalized bias (MNB) equal −0.62 (−0.51) based data all surface, −0.15 (+0.51) when compared remote measurements, −0.30 marine locations data. temporal correlations across stations low measurements: 0.47 (0.52) stations, 0.39 (0.37) 0.25 combination (negative) MNB correlation sites about processes govern removal, top their stations. There no clear change skill regard or mass concentration. However, needed distinguish natural climate mitigation, impact accurately.

Language: Английский

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Chemistry and the Linkages between Air Quality and Climate Change

Chemical Reviews, Journal Year: 2015, Volume and Issue: 115(10), P. 3856 - 3897

Published: April 30, 2015

ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTChemistry and the Linkages between Air Quality Climate ChangeErika von Schneidemesser*†, Paul S. Monks*‡, James D. Allan§∥, Lori Bruhwiler⊥, Piers Forster#, David Fowler∇, Axel Lauer†, William T. Morgan§, Pauli Paasonen○, Mattia Righi◆, Katerina Sindelarova¶□, Mark A. Sutton∇View Author Information† Institute for Advanced Sustainability Studies, 14467 Potsdam, Germany‡ Department of Chemistry, University Leicester, Leicester LE1 7RH, United Kingdom§ §School Earth, Atmospheric Environmental Sciences, ∥National Centre Science, Manchester, Manchester M13 9PL, Kingdom⊥ National Oceanic & Administration, Boulder, Colorado 80303, States# Leeds, Leeds LS2 9JT, Kingdom∇ Ecology Hydrology, Natural Environment Research Council, Edinburgh EH26 0QB, Kingdom○ Physics, Helsinki, 00100 Finland◆ Deutsches Zentrum für Luft- und Raumfahrt, Institut Physik der Atmosphäre, 82234 Oberpfaffenhofen, Germany¶ UPMC Univ. Paris 06, Université Versailles St-Quentin; CNRS/INSU; LATMOS-IPSL, UMR 8190 Paris, France□ Faculty Mathematics Charles University, 116 36 Prague, Czech Republic*E-mail: [email protected]*E-mail: protected]Cite this: Chem. Rev. 2015, 115, 10, 3856–3897Publication Date (Web):April 30, 2015Publication History Received10 February 2015Published online30 April inissue 27 May 2015https://doi.org/10.1021/acs.chemrev.5b00089Copyright © 2015 American Chemical SocietyRIGHTS PERMISSIONSACS AuthorChoicewith CC-BYlicenseArticle Views28841Altmetric-Citations260LEARN ABOUT THESE METRICSArticle Views are COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated to reflect usage leading up last few days.Citations number other articles citing this article, calculated by Crossref daily. Find more information about citation counts.The Altmetric Attention Score is a quantitative measure attention that research has received online. Clicking on donut icon will load page at altmetric.com with additional details score social media presence given article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InReddit (22 MB) Get e-AlertscloseSUBJECTS:Aerosols,Atmospheric chemistry,Climate,Particulate matter,Redox reactions e-Alerts

Language: Английский

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Emissions of trace gases and aerosols during the open combustion of biomass in the laboratory

Journal of Geophysical Research Atmospheres, Journal Year: 2009, Volume and Issue: 114(D19)

Published: Oct. 13, 2009

We characterized the gas‐ and speciated aerosol‐phase emissions from open combustion of 33 different plant species during a series 255 controlled laboratory burns Fire Laboratory at Missoula Experiments (FLAME). The we tested were chosen to improve existing database for U.S. domestic fuels: laboratory‐based emission factors have not previously been reported many commonly burned that are frequently consumed by fires near populated regions protected scenic areas. plants included chaparral chamise, manzanita, ceanothus, common southeastern United States (common reed, hickory, kudzu, needlegrass rush, rhododendron, cord grass, sawgrass, titi, wax myrtle). Fire‐integrated gas‐phase CO 2 , CO, CH 4 C 2–4 hydrocarbons, NH 3 SO NO, NO HNO particle‐phase organic carbon (OC), elemental (EC), 2− − Cl Na + K generally varied with both fuel type fire‐integrated modified efficiency (MCE), measure relative importance flaming‐ smoldering‐phase total burn. Chaparral fuels tended emit less particulate OC per unit mass dry than did other types, whereas had some largest observed fine matter. Our measurements spanned larger range MCE prior studies, thus help estimates variation conditions individual fuels.

Language: Английский

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Model Representation of Secondary Organic Aerosol in CMAQv4.7

Environmental Science & Technology, Journal Year: 2010, Volume and Issue: 44(22), P. 8553 - 8560

Published: Sept. 30, 2010

Numerous scientific upgrades to the representation of secondary organic aerosol (SOA) are incorporated into Community Multiscale Air Quality (CMAQ) modeling system. Additions include several recently identified SOA precursors: benzene, isoprene, and sesquiterpenes; pathways: in-cloud oxidation glyoxal methylglyoxal, particle-phase oligomerization, acid enhancement isoprene SOA. NOx-dependent aromatic yields also added along with new empirical measurements enthalpies vaporization mass-to-carbon ratios. For first time, these precursors, pathways parameters included simultaneously in an air quality model for annual simulation spanning continental U.S. Comparisons CMAQ-modeled carbon (OCsec) semiempirical estimates screened from 165 routine monitoring sites across indicate module substantially improves performance. The most notable improvement occurs central southeastern where regionally averaged temporal correlations (r) between modeled OCsec increase −0.5 0.8 −0.3 0.8, respectively, when is employed. Wintertime results improve all regions seasonal regional patterns biogenic better represented.

Language: Английский

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Heterogeneous oxidation of atmospheric aerosol particles by gas-phase radicals

Nature Chemistry, Journal Year: 2010, Volume and Issue: 2(9), P. 713 - 722

Published: Aug. 23, 2010

Language: Английский

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Optical Properties of Secondary Organic Aerosols and Their Changes by Chemical Processes

Chemical Reviews, Journal Year: 2015, Volume and Issue: 115(10), P. 4400 - 4439

Published: April 15, 2015

ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTOptical Properties of Secondary Organic Aerosols and Their Changes by Chemical ProcessesTamar Moise, J. Michel Flores, Yinon Rudich*View Author Information Department Earth Planetary Sciences, Weizmann Institute, Rehovot 76100, Israel*E-mail [email protected]Cite this: Chem. Rev. 2015, 115, 10, 4400–4439Publication Date (Web):April 15, 2015Publication History Received16 September 2014Published online15 April 2015Published inissue 27 May 2015https://pubs.acs.org/doi/10.1021/cr5005259https://doi.org/10.1021/cr5005259review-articleACS PublicationsCopyright © 2015 American SocietyRequest reuse permissionsArticle Views6013Altmetric-Citations291LEARN ABOUT THESE METRICSArticle Views are the COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated to reflect usage leading up last few days.Citations number other articles citing this article, calculated Crossref daily. Find more information about citation counts.The Altmetric Attention Score is a quantitative measure attention that research has received online. Clicking on donut icon will load page at altmetric.com with additional details score social media presence for given article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Absorption,Aerosols,Optical properties,Quantum mechanics,Redox reactions Get e-Alerts

Language: Английский

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Evaporation kinetics and phase of laboratory and ambient secondary organic aerosol

Proceedings of the National Academy of Sciences, Journal Year: 2011, Volume and Issue: 108(6), P. 2190 - 2195

Published: Jan. 24, 2011

Field measurements of secondary organic aerosol (SOA) find significantly higher mass loads than predicted by models, sparking intense effort focused on finding additional SOA sources but leaving the fundamental assumptions used models unchallenged. Current air-quality use absorptive partitioning theory assuming particles are liquid droplets, forming instantaneous reversible equilibrium with gas phase. Further, they ignore effects adsorption spectator species during formation properties and fate. Using accurate highly sensitive experimental approach for studying evaporation kinetics size-selected single particles, we characterized room-temperature laboratory-generated α-pinene ambient atmospheric SOA. We found that even when phase organics removed, it takes ∼24 h pure to evaporate 75% their mass, which is in sharp contrast ∼10 min time scale current kinetic models. Adsorption “spectator” vapors formation, aging these coated dramatically reduced rate, some cases nearly stopped it. Ambient was exhibit behavior very similar aged For all studied this work, size-independent does not follow model assumptions. The findings about phase, rates, importance gases indicate there need reformulate way treated

Language: Английский

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An overview of the MILAGRO 2006 Campaign: Mexico City emissions and their transport and transformation

Atmospheric chemistry and physics, Journal Year: 2010, Volume and Issue: 10(18), P. 8697 - 8760

Published: Sept. 16, 2010

Abstract. MILAGRO (Megacity Initiative: Local And Global Research Observations) is an international collaborative project to examine the behavior and export of atmospheric emissions from a megacity. The Mexico City Metropolitan Area (MCMA) – one world's largest megacities North America's most populous city was selected as case study characterize sources, concentrations, transport, transformation processes gases fine particles emitted MCMA atmosphere evaluate regional global impacts these emissions. findings this are relevant evolution pollution many other megacities. measurement phase consisted month-long series carefully coordinated observations chemistry physics in near during March 2006, using wide range instruments at ground sites, on aircraft satellites, enlisting over 450 scientists 150 institutions 30 countries. Three supersites were set up primary particles. Additional platforms or included mobile vans containing scientific laboratories stationary upward-looking lidars. Seven instrumented research provided information about large region various altitudes. Satellite-based peered down into atmosphere, providing even larger geographical coverage. overall campaign complemented by meteorological forecasting numerical simulations, satellite surface networks. Together, have comprehensive characterization MCMA's urban composition that will take years analyze fully. In paper we review 120 papers resulting MILAGRO/INTEX-B Campaign been published submitted, well earlier MCMA-2003 Campaign, with aim road map for community interested understanding megacity such their air quality climate. This describes measurements performed results obtained meteorology dynamics, particles, sources concentrations volatile organic compounds, photochemistry, ambient particulate matter, aerosol radiative properties, plume characterization, health studies. A summary key field presented.

Language: Английский

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Chemical composition, sources, and aging process of submicron aerosols in Beijing: Contrast between summer and winter

Journal of Geophysical Research Atmospheres, Journal Year: 2016, Volume and Issue: 121(4), P. 1955 - 1977

Published: Jan. 23, 2016

Abstract To investigate the seasonal characteristics of submicron aerosol (PM 1 ) in Beijing urban areas, a high‐resolution time‐of‐flight aerosol‐mass‐spectrometer (HR‐ToF‐AMS) was utilized at an site summer (August to September 2011) and winter (November December 2010), coupled with multiple state art online instruments. The average mass concentrations PM (60–84 µg m −3 its chemical compositions different campaigns were relatively consistent recent years. In summer, daily variations stable repeatable. Eighty‐two percent concentration on composed secondary species, where 62% is inorganic 20% organic (SOA). winter, changed dramatically because meteorological conditions. high fraction (58%) primary species including (POA), black carbon, chloride indicates emissions usually played more important role winter. However, aqueous chemistry resulting efficient formation during occasional periods relative humidity may also contribute substantially haze Results past OA source apportionment studies show 45–67% 22–50% can be SOA. Based results, we found 45% POA 61% are from nonfossil sources, contributed by cooking both seasons biomass burning (BBOA) Cooking OA, accounting for 13–24% carbon all years should not neglected. fossil sources include hydrocarbon‐like vehicle coal combustion (CCOA) CCOA BBOA two main contributors (57% OA) highest (>100 POA/ΔCO ratios 11 16 ppm −1 , respectively, similar western cities. Higher OOA/O x (= NO 2 + O 3 ratio (0.49 ppb study than these cities (0.03–0.16 observed, which due reaction or extra SOA semivolatile compounds various (e.g., CCOA) Beijing. evolution oxygen (O/C) photochemical age allows estimate equivalent rate constant aging as k OH ~ 4.1 × 10 −12 cm molecule s same order obtained other anthropogenic influenced areas useful modeling.

Language: Английский

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Organic aerosol components derived from 25 AMS data sets across Europe using a consistent ME-2 based source apportionment approach

Atmospheric chemistry and physics, Journal Year: 2014, Volume and Issue: 14(12), P. 6159 - 6176

Published: June 23, 2014

Abstract. Organic aerosols (OA) represent one of the major constituents submicron particulate matter (PM1) and comprise a huge variety compounds emitted by different sources. Three intensive measurement field campaigns to investigate aerosol chemical composition all over Europe were carried out within framework European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI) Monitoring Evaluation Programme (EMEP) during 2008 (May–June September–October) 2009 (February–March). In this paper we focus identification main organic sources define standardized methodology perform source apportionment using positive matrix factorization (PMF) with multilinear engine (ME-2) Aerodyne mass spectrometer (AMS) data. Our procedure is tested applied 25 data sets accounting for two urban, several rural remote high altitude sites; therefore it likely suitable treatment AMS-related ambient sets. For most sites, four components are retrieved, improving significantly previous results where only separation in primary secondary OA was possible. Generally, our solutions include sources, i.e. hydrocarbon-like (HOA) biomass burning (BBOA) components, semi-volatile oxygenated (SV-OOA) low-volatility (LV-OOA). specific sites cooking-related (COA) marine-related (MSA) also separated. Finally, work provides large overview an interesting set highly time resolved modeling purposes.

Language: Английский

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