Bounding the role of black carbon in the climate system: A scientific assessment

Journal of Geophysical Research Atmospheres, Journal Year: 2013, Volume and Issue: 118(11), P. 5380 - 5552

Published: April 22, 2013

Abstract Black carbon aerosol plays a unique and important role in Earth's climate system. is type of carbonaceous material with combination physical properties. This assessment provides an evaluation black‐carbon forcing that comprehensive its inclusion all known relevant processes quantitative providing best estimates uncertainties the main terms: direct solar absorption; influence on liquid, mixed phase, ice clouds; deposition snow ice. These effects are calculated models, but when possible, they evaluated both microphysical measurements field observations. Predominant sources combustion related, namely, fossil fuels for transportation, solid industrial residential uses, open burning biomass. Total global emissions black using bottom‐up inventory methods 7500 Gg yr −1 year 2000 uncertainty range to 29000. However, atmospheric absorption attributable too low many models should be increased by factor almost 3. After this scaling, estimate industrial‐era (1750 2005) radiative +0.71 W m −2 90% bounds (+0.08, +1.27) . sources, without subtracting preindustrial background, estimated as +0.88 (+0.17, +1.48) Direct alone does not capture rapid adjustment mechanisms. A framework described used quantifying forcings, including adjustments. The through mechanisms, clouds cryosphere forcing, +1.1 +0.17 +2.1 Thus, there very high probability emissions, independent co‐emitted species, have positive warm climate. We carbon, total , second most human emission terms present‐day atmosphere; only dioxide greater forcing. Sources emit also other short‐lived species may either cool or Climate forcings from herein. When principal co‐emissions, cooling agents such sulfur dioxide, included net energy‐related (fossil fuel biofuel) +0.22 (−0.50 +1.08) during first after emission. For few these diesel engines possibly biofuels, warming strong enough eliminating would reduce (i.e., produce cooling). which levels organic matter, total, black‐carbon‐rich becomes slightly negative (−0.06 −1.45 +1.29 ). substantial, largely due lack knowledge about cloud interactions carbon. In prioritizing potential mitigation actions, non‐science factors, technical feasibility, costs, policy design, implementation feasibility play roles. major presently different stages regard near‐term mitigation. assessment, evaluating large number complexity associated sets baseline improve future estimates.

Language: Английский

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Understanding atmospheric organic aerosols via factor analysis of aerosol mass spectrometry: a review

Analytical and Bioanalytical Chemistry, Journal Year: 2011, Volume and Issue: 401(10), P. 3045 - 3067

Published: Oct. 4, 2011

Organic species are an important but poorly characterized constituent of airborne particulate matter. A quantitative understanding the organic fraction particles (organic aerosol, OA) is necessary to reduce some largest uncertainties that confound assessment radiative forcing climate and air quality management policies. In recent years, aerosol mass spectrometry has been increasingly relied upon for highly time-resolved characterization OA chemistry elucidation sources lifecycle processes. Aerodyne spectrometers (AMS) particularly widely used, because their ability quantitatively characterize size-resolved composition submicron (PM1). AMS report bulk temporal variations in form ensemble spectra (MS) acquired over short time intervals. Because each MS represents linear superposition individual components weighed by concentrations, multivariate factor analysis matrix proved effective at retrieving factors offer a simplified description thousands species. The sum accounts nearly 100% typically corresponds large group constituents with similar chemical behavior characteristic different and/or atmospheric application this technique grown rapidly last six years. Here we review techniques applied other spectrometers, summarize key findings from field observations. Results provide valuable information about and, particular, secondary evolution on regional global scales highlighted. Advanced methods, example a-priori constraints combined gas phase data discussed. Integrated worldwide used present holistic OA. Finally, ways which can constrain models

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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Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere

Physical Chemistry Chemical Physics, Journal Year: 2011, Volume and Issue: 13(43), P. 19238 - 19238

Published: Jan. 1, 2011

Recently, it has been proposed that organic aerosol particles in the atmosphere can exist an amorphous semi-solid or solid (i.e. glassy) state. In this perspective, we analyse and discuss formation properties of semi-solids glasses from liquids. Based on a systematic survey wide range compounds, present estimates for glass forming atmospheric secondary (SOA). particular investigate dependence transition temperature Tg upon various molecular such as compounds' melting temperature, their molar mass, atomic oxygen-to-carbon ratios (O : C ratios). Also effects mixing different compounds hygroscopic water uptake depending ambient relative humidity are investigated. addition to suggest mass content much more important than O ratio characterizing whether particle is liquid, semi-solid, glassy Moreover, show how viscosity states affect diffusivity those molecules constituting matrix well guest oxidants, implications multi-phase processes. Finally, assess current state knowledge level scientific understanding, propose avenues future studies resolve existing uncertainties.

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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Kinetics, products, and mechanisms of secondary organic aerosol formation

Chemical Society Reviews, Journal Year: 2012, Volume and Issue: 41(19), P. 6582 - 6582

Published: Jan. 1, 2012

Secondary organic aerosol (SOA) is formed in the atmosphere when volatile compounds (VOCs) emitted from anthropogenic and biogenic sources are oxidized by reactions with OH radicals, O3, NO3 or Cl atoms to form less products that subsequently partition into particles. Once particles, these can undergo heterogenous/multiphase more highly oligomeric products. SOA comprises a large fraction of atmospheric mass have significant effects on chemistry, visibility, human health, climate. Previous articles reviewed kinetics, products, mechanisms VOC general chemistry physics involved formation. In this article we present detailed review heterogeneous/multiphase as they apply formation, focus molecular structure kinetics initial major oxidants, subsequent alkyl, alkyl peroxy, alkoxy radical intermediates, composition resulting Structural features reactants discussed include compound carbon number; linear, branched, cyclic configurations; presence CC bonds aromatic rings; functional groups such carbonyl, hydroxyl, ester, hydroxperoxy, carboxyl, peroxycarboxyl, nitrate, peroxynitrate. The intention provide chemists sufficient information understand dominant pathways which classes VOCs react further This will allow reasonable predictions be made, based structure, about reactions, including important variables VOC, oxidant, NOx concentrations well temperature, humidity, particle acidity. Such knowledge should useful for interpreting results laboratory field studies developing models. A number recommendations future research also presented.

Language: Английский

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Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) – Part 1: Fine particle composition and organic source apportionment

Atmospheric chemistry and physics, Journal Year: 2009, Volume and Issue: 9(17), P. 6633 - 6653

Published: Sept. 11, 2009

Abstract. Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at T0 urban supersite Mexico City with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and complementary instrumentation. concentrations, diurnal cycles, size distributions of inorganic organic species are similar to results from CENICA April 2003 (OA) comprising about half fine PM mass. Positive Matrix Factorization (PMF) analysis high resolution OA spectra identified three major components: chemically-reduced primary emissions (hydrocarbon-like OA, HOA), oxygenated (OOA, mostly secondary or SOA), biomass burning (BBOA) that correlates levoglucosan acetonitrile. BBOA includes several very large plumes regional fires likely also some refuse burning. A fourth component is small local nitrogen-containing reduced (LOA) which accounts for 9% mass but one third nitrogen, as amines. OOA almost on average, consistent previous observations. apportionment PMF-AMS compared PM2.5 chemical balance molecular markers (CMB-OMM, GC/MS filters). Results both methods overall consistent. Both assign components urban, burning/woodsmoke, sources magnitudes. The inventory underestimates by factor ~4, it ~16 times lower than afternoon concentrations when included. Additionally, forest fire contribution least an order-of-magnitude larger inventory.

Language: Английский

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Multiphase Chemistry at the Atmosphere–Biosphere Interface Influencing Climate and Public Health in the Anthropocene

Chemical Reviews, Journal Year: 2015, Volume and Issue: 115(10), P. 4440 - 4475

Published: April 9, 2015

ADVERTISEMENT RETURN TO ISSUEPREVReviewNEXTMultiphase Chemistry at the Atmosphere–Biosphere Interface Influencing Climate and Public Health in AnthropoceneUlrich Pöschl* Manabu Shiraiwa*View Author Information Multiphase Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany*E-mail: [email protected] (U.P.).*E-mail: (M.S.).Cite this: Chem. Rev. 2015, 115, 10, 4440–4475Publication Date (Web):April 9, 2015Publication History Received1 September 2014Published online9 April 2015Published inissue 27 May 2015https://doi.org/10.1021/cr500487sCopyright © 2015 American Chemical SocietyRIGHTS & PERMISSIONSACS AuthorChoicewith CC-BYlicenseArticle Views17935Altmetric-Citations359LEARN ABOUT THESE METRICSArticle Views are COUNTER-compliant sum of 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 InReddit (7 MB) Get e-AlertsSUBJECTS:Aerosols,Atmospheric chemistry,Free radicals,Nanoparticles,Particulate matter e-Alerts

Language: Английский

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Elucidating secondary organic aerosol from diesel and gasoline vehicles through detailed characterization of organic carbon emissions

Proceedings of the National Academy of Sciences, Journal Year: 2012, Volume and Issue: 109(45), P. 18318 - 18323

Published: Sept. 27, 2012

Emissions from gasoline and diesel vehicles are predominant anthropogenic sources of reactive gas-phase organic carbon key precursors to secondary aerosol (SOA) in urban areas. Their relative importance for formation is a controversial issue with implications air quality control policy public health. We characterize the chemical composition, mass distribution, potential emissions vehicles, find exhaust seven times more efficient at forming than exhaust. However, both important quality; depending on region’s fuel use, responsible 65% 90% vehicular-derived SOA, substantial contributions aromatic aliphatic hydrocarbons. Including these insights source characterization SOA will improve regional pollution policies, regulations, methodologies future measurement, laboratory, modeling studies.

Language: Английский

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Aerosol mass spectrometer constraint on the global secondary organic aerosol budget

Atmospheric chemistry and physics, Journal Year: 2011, Volume and Issue: 11(23), P. 12109 - 12136

Published: Dec. 7, 2011

Abstract. The budget of atmospheric secondary organic aerosol (SOA) is very uncertain, with recent estimates suggesting a global source between 12 and 1820 Tg a−1. We used dataset mass spectrometer (AMS) observations from 34 different surface locations to evaluate the GLOMAP chemical transport model. standard model simulation (which included SOA monoterpenes only) underpredicted (OA) observed by AMS had little skill reproducing variability in dataset. simulated formation biogenic (monoterpenes isoprene), lumped anthropogenic biomass burning volatile compounds (VOCs) varied yield each precursor produce best overall match observations. assumed that essentially non-volatile condenses irreversibly onto existing aerosol. Our estimate 140 a−1 but large uncertainty range which we be 50–380 found minimum normalised mean error (NME) when (100 a−1) sources spatially matched pollution term antropogenically controlled SOA). carbon compiled Bahadur et al. (2009) our estimated sources. was most consistent these observations, however improvement over (250 small. 14C rural maximum 10 (10 %) anthropogenically could fossil (urban/industrial) suggest an additional likely due enhancement VOCs. Such would result substantial climate forcing. direct effect −0.26 ± 0.15 Wm−2 indirect (cloud albedo) −0.6+0.24−0.14 SOA. are not well constrained this analysis limited number OA regions periods strongly impacted To further improve constraints method, needed tropics Southern Hemisphere.

Language: Английский

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