A large source of low-volatility secondary organic aerosol

Nature, Journal Year: 2014, Volume and Issue: 506(7489), P. 476 - 479

Published: Feb. 1, 2014

Language: Английский

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Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies

Atmospheric chemistry and physics, Journal Year: 2011, Volume and Issue: 11(21), P. 11069 - 11102

Published: Nov. 9, 2011

Abstract. Progress has been made over the past decade in predicting secondary organic aerosol (SOA) mass atmosphere using vapor pressure-driven partitioning, which implies that SOA compounds are formed gas phase and then partition to an (gasSOA). However, discrepancies oxidation state, size product (molecular mass) distribution, relative humidity (RH) dependence, color, vertical profile suggest additional sources aging processes may be important. The formation of cloud water (aqSOA) is not considered these models even though abundant medium for atmospheric chemistry such can form dicarboxylic acids "humic-like substances" (oligomers, high-molecular-weight compounds), i.e. do have any but comprise a significant fraction total mass. There direct evidence from field observations laboratory studies water, contributing substantial droplet mode. This review summarizes current knowledge on aqueous reactions combines points role aqSOA atmosphere. Model discussed explore importance suggestions model improvements based comprehensive set data presented here. A first comparison between gasSOA yields predictions selected conditions. These simulations might contribute almost as much budget, with highest contributions biogenic emissions volatile (VOC) presence anthropogenic pollutants (i.e. NOx) at high cloudiness. Gaps understanding further (laboratory, field, model) outlined complement sets.

Language: Английский

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Large contribution of natural aerosols to uncertainty in indirect forcing

Nature, Journal Year: 2013, Volume and Issue: 503(7474), P. 67 - 71

Published: Nov. 1, 2013

Language: Английский

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The CAMS reanalysis of atmospheric composition

Atmospheric chemistry and physics, Journal Year: 2019, Volume and Issue: 19(6), P. 3515 - 3556

Published: March 20, 2019

Abstract. The Copernicus Atmosphere Monitoring Service (CAMS) reanalysis is the latest global dataset of atmospheric composition produced by European Centre for Medium-Range Weather Forecasts (ECMWF), consisting three-dimensional time-consistent fields, including aerosols and chemical species. currently covers period 2003–2016 will be extended in future adding 1 year each year. A greenhouse gases being separately. CAMS builds on experience gained during production earlier Atmospheric Composition Climate (MACC) interim reanalysis. Satellite retrievals total column CO; tropospheric NO2; aerosol optical depth (AOD); column, partial profile ozone were assimilated with ECMWF's Integrated Forecasting System. new has an increased horizontal resolution about 80 km provides more species at a better temporal (3-hourly analysis 3-hourly forecast fields hourly surface fields) than previously smaller biases compared most independent ozone, carbon monoxide, nitrogen dioxide observations used validation this paper previous two reanalyses much improved consistent time, especially to MACC that can compute climatologies, study trends, evaluate models, benchmark other or serve as boundary conditions regional models past periods.

Language: Английский

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Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations

Atmospheric chemistry and physics, Journal Year: 2013, Volume and Issue: 13(4), P. 1853 - 1877

Published: Feb. 19, 2013

Abstract. We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global models have been used to simulate changes in distribution over industrial era. All estimated radiative forcing (RF) of anthropogenic DAE, and taken into account sulphate, black carbon (BC) organic aerosols (OA) from fossil fuel, biofuel, biomass burning emissions. In addition several simulated DAE nitrate influenced secondary (SOA). The model all-sky RF total has a range −0.58 −0.02 Wm−2, with mean −0.27 Wm−2 for models. Several did not include or SOA modifying estimate by accounting this information other reduces slightly strengthens mean. Modifying estimates missing components time period 1750 2010 results −0.35 Wm−2. Compared I (Schulz et al., 2006) we find very similar spreads both component RF. However, is stronger negative BC fuel biofuel emissions are positive present study than previous study. tendency having strong (positive) also (negative) sulphate OA This relationship leads smaller uncertainty compared sum individual components. spread substantial, can be divided diversities burden, mass extinction coefficient (MEC), normalized respect AOD. that these three factors give contributions results.

Language: Английский

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

Reviews of Geophysics, Journal Year: 2017, Volume and Issue: 55(2), P. 509 - 559

Published: May 18, 2017

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

Language: Английский

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Particulate matter, air quality and climate: lessons learned and future needs

Atmospheric chemistry and physics, Journal Year: 2015, Volume and Issue: 15(14), P. 8217 - 8299

Published: July 24, 2015

Abstract. The literature on atmospheric particulate matter (PM), or aerosol, has increased enormously over the last 2 decades and amounts now to some 1500–2000 papers per year in refereed literature. This is part due enormous advances measurement technologies, which have allowed for an increasingly accurate understanding of chemical composition physical properties particles their processes atmosphere. growing scientific interest aerosol high importance environmental policy. In fact, constitutes one most challenging problems both air quality climate change policies. this context, paper reviews recent results within sciences policy needs, driven much increase monitoring mechanistic research decades. synthesis reveals many new developments science underpinning climate–aerosol interactions effects PM human health environment. However, while airborne responsible globally important influences premature mortality, we still do not know relative different components these effects. Likewise, magnitude overall remains highly uncertain. Despite uncertainty there are things that could be done mitigate local global PM. Recent analyses shown reducing black carbon (BC) emissions, using known control measures, would reduce warming delay time when anthropogenic temperature exceed °C. cost-effective measures ammonia, agricultural precursor gas secondary inorganic aerosols (SIA), regional eutrophication concentrations large areas Europe, China USA. Thus, environment population. A prioritized list actions full range currently undeliverable shortcomings knowledge science; among shortcomings, roles sources response land use remaining century prominent. any case, evidence from strongly advocates integrated approach

Language: Английский

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Effects of aging on organic aerosol from open biomass burning smoke in aircraft and laboratory studies

Atmospheric chemistry and physics, Journal Year: 2011, Volume and Issue: 11(23), P. 12049 - 12064

Published: Dec. 5, 2011

Abstract. Biomass burning (BB) is a large source of primary and secondary organic aerosols (POA SOA). This study addresses the physical chemical evolution BB aerosols. Firstly, lifetime POA SOA signatures observed with Aerodyne Aerosol Mass Spectrometer are investigated, focusing on measurements at high-latitudes acquired during 2008 NASA ARCTAS mission, in comparison to data from other field studies laboratory aging experiments. The parameter f60, ratio integrated signal m/z 60 total component mass spectrum, used as marker rate oxidation fate POA. A background level f60~0.3% ± 0.06% for SOA-dominated ambient OA shown be an appropriate this tracer. Using also f44 tracer aged surrogate O:C, novel graphical method presented characterise plumes. Similar trends decreasing f60 increasing most lab studies. At least some very plumes retain clear signature. statistically significant difference between highly-oxygenated non-BB origin using tracer, consistent substantial contribution BBOA springtime Arctic aerosol burden 2008. Secondly, summary results net enhancement plumes, which shows variability. estimates gain range ΔOA/ΔCO(mass) = −0.01 ~0.05, mean ΔOA/POA ~19%. With these ratios global inventories CO due ~8 7 Tg yr−1 estimated, order 5 % recent estimates. Further following plume advection should focus future research better constrain potentially important burden.

Language: Английский

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Effects of anthropogenic emissions on aerosol formation from isoprene and monoterpenes in the southeastern United States

Proceedings of the National Academy of Sciences, Journal Year: 2014, Volume and Issue: 112(1), P. 37 - 42

Published: Dec. 22, 2014

Secondary organic aerosol (SOA) constitutes a substantial fraction of fine particulate matter and has important impacts on climate human health. The extent to which activities alter SOA formation from biogenic emissions in the atmosphere is largely undetermined. Here, we present direct observational evidence magnitude anthropogenic influence based comprehensive ambient measurements southeastern United States (US). Multiple high-time-resolution mass spectrometry were made during different seasons at various locations, including urban rural sites greater Atlanta area Centreville Alabama. Our results provide quantitative understanding roles SO2 NOx formation. We show that isoprene-derived directly mediated by abundance sulfate, instead particle water content and/or acidity as suggested prior laboratory studies. Anthropogenic shown enhance nighttime via nitrate radical oxidation monoterpenes, resulting condensable nitrates. Together, sulfate can mediate 43-70% total measured (29-49% submicron matter, PM1) US summer. These imply future reduction considerably reduce burden US. Updating current modeling frameworks with these constraints will also lead more accurate treatment for regions anthropogenic-biogenic interactions consequently improve air quality simulations.

Language: Английский

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The Molecular Identification of Organic Compounds in the Atmosphere: State of the Art and Challenges

Chemical Reviews, Journal Year: 2015, Volume and Issue: 115(10), P. 3919 - 3983

Published: Feb. 3, 2015

ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTThe Molecular Identification of Organic Compounds in the Atmosphere: State Art and ChallengesBarbara Nozière*†, Markus Kalberer*‡, Magda Claeys*§, James Allan∥, Barbara D'Anna†, Stefano Decesari⊥, Emanuela Finessi#, Marianne Glasius∇, Irena Grgić○, Jacqueline F. Hamilton#, Thorsten Hoffmann◆, Yoshiteru Iinuma¶, Mohammed Jaoui△, Ariane Kahnt§, Christopher J. Kampf▲, Ivan Kourtchev‡, Willy Maenhaut§□, Nicholas Marsden∥, Sanna Saarikoski■, Jürgen Schnelle-Kreis◇, Jason D. Surratt▼, Sönke Szidat☆, Rafal Szmigielski★, Armin Wisthaler⬡View Author Information† Ircelyon/CNRS Université Lyon 1, 69626 Villeurbanne Cedex, France‡ University Cambridge, Cambridge CB2 1EW, United Kingdom§ Antwerp, 2000 Belgium∥ The Manchester & National Centre for Atmospheric Science, M13 9PL, Kingdom⊥ Istituto ISAC - C.N.R., I-40129 Bologna, Italy# York, York YO10 5DD, Kingdom∇ Aarhus, 8000 Aarhus C, Denmark○ Institute Chemistry, 1000 Ljubljana, Slovenia◆ Johannes Gutenberg-Universität, 55122 Mainz, Germany¶ Leibniz-Institut für Troposphärenforschung, 04318 Leipzig, Germany△ Alion Science Technology, McLean, Virginia 22102, States▲ Max Planck 55128 Germany□ Ghent University, 9000 Gent, Belgium■ Finnish Meteorological Institute, FI-00101 Helsinki, Finland◇ Helmholtz Zentrum München, D-85764 Neuherberg, Germany▼ North Carolina at Chapel Hill, 27599, States☆ Bern, 3012 Switzerland★ Physical Chemistry PAS, Warsaw 01-224, Poland⬡ Oslo, 0316 Norway*E-mail: [email protected]*E-mail: protected]Cite this: Chem. Rev. 2015, 115, 10, 3919–3983Publication Date (Web):February 3, 2015Publication History Received1 July 2014Published online3 February 2015Published inissue 27 May 2015https://pubs.acs.org/doi/10.1021/cr5003485https://doi.org/10.1021/cr5003485review-articleACS PublicationsCopyright © 2015 American Chemical SocietyRequest reuse permissionsArticle Views12686Altmetric-Citations384LEARN 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 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 InRedditEmail Other access optionsGet e-Alertsclose SUBJECTS:Aerosols,Chromatography,Mathematical methods,Organic compounds,Redox reactions Get e-Alerts

Language: Английский

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