A two-dimensional volatility basis set - Part 2: Diagnostics of organic-aerosol evolution
TLDR
In this article, the authors use a 2D-Voxidation space to describe organic-aerosol chemical evolution, based on two coordinates, volatility and the degree of oxidation, which can be constrained observationally or specified for known molecules.Abstract:
We discuss the use of a two-dimensional volatility-oxidation space (2-D-VBS) to describe organic- aerosol chemical evolution. The space is built around two coordinates, volatility and the degree of oxidation, both of which can be constrained observationally or specified for known molecules. Earlier work presented the thermodynam- ics of organics forming the foundation of this 2-D-VBS, al- lowing us to define the average composition (C, H, and O) of organics, including organic aerosol (OA) based on volatility and oxidation state. Here we discuss how we can analyze ex- perimental data, using the 2-D-VBS to gain fundamental in- sight into organic-aerosol chemistry. We first present a well- understood "traditional" secondary organic aerosol (SOA) system - SOA from -pinene + ozone, and then turn to two examples of "non-traditional" SOA formation - SOA from wood smoke and dilute diesel-engine emissions. Finally, we discuss the broader implications of this analysis.read more
Citations
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A large source of low-volatility secondary organic aerosol
Mikael Ehn,Joel A. Thornton,Einhard Kleist,Mikko Sipilä,Heikki Junninen,Iida Pullinen,Monika Springer,Florian Rubach,Ralf Tillmann,Ben H. Lee,Felipe D. Lopez-Hilfiker,S. Andres,Ismail-Hakki Acir,Matti P. Rissanen,Tuija Jokinen,Siegfried Schobesberger,Juha Kangasluoma,Jenni Kontkanen,Tuomo Nieminen,Theo Kurtén,Lasse B. Nielsen,Solvejg Jørgensen,Henrik G. Kjaergaard,Manjula R. Canagaratna,Miikka Dal Maso,Torsten Berndt,Tuukka Petäjä,Andreas Wahner,Veli-Matti Kerminen,Markku Kulmala,Douglas R. Worsnop,Juergen Wildt,Thomas F. Mentel +32 more
TL;DR: It is found that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies.
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Chemistry of atmospheric brown carbon.
TL;DR: Understanding of the climate-related properties of atmospheric OC is still incomplete and the specific ways in which OC impacts atmospheric environment and climate forcing are just beginning to be understood.
Secondary Organic Aerosol Formation from Anthropogenic Air Pollution: Rapid and Higher than Expected
Jose L. Jimenez,Rainer Volkamer,F. M. San Martini,Katja Dzepina,Qi Zhang,Ingrid M. Ulbrich,D. Salcedo,D. R. Worsnop,Luisa T. Molina +8 more
TL;DR: This paper showed that reactive anthropogenic VOCs (AVOCs) produce much larger amounts of SOA than these models predict, even shortly after sunrise, and a significant fraction of the excess SOA is formed from first-generation AVOC oxidation products.
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Formation of Urban Fine Particulate Matter
Renyi Zhang,Gehui Wang,Song Guo,Misti L. Zamora,Qi Ying,Yun Lin,Weigang Wang,Min Hu,Yuan Wang +8 more
TL;DR: Air pollutants consist of a complex combination of gases and particulate matter, which is emitted directly into the atmosphere or formed in the atmosphere through gas-to-particle conversion (secondary) (Figure 1).
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Particulate matter, air quality and climate: Lessons learned and future needs
Sandro Fuzzi,Urs Baltensperger,Kenneth S. Carslaw,Stefano Decesari,H.A.C. Denier van der Gon,Maria Cristina Facchini,David Fowler,Ilan Koren,Ben Langford,Ulrike Lohmann,Eiko Nemitz,Spyros N. Pandis,Ilona Riipinen,Yinon Rudich,Martijn Schaap,Jay G. Slowik,Dominick V. Spracklen,Elisabetta Vignati,Martin Wild,Martin L. Williams,Stefania Gilardoni +20 more
TL;DR: The literature on atmospheric particulate maffer (PM), or atmospheric aerosol, has increased enormously over the last 2 decades and amounts now to some 1500-2000 papers per year in the refereed literature.
References
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Journal ArticleDOI
The formation, properties and impact of secondary organic aerosol: current and emerging issues
Mattias Hallquist,John C. Wenger,Urs Baltensperger,Yinon Rudich,David Simpson,David Simpson,Magda Claeys,J. Dommen,Neil M. Donahue,Christian George,Christian George,Allen H. Goldstein,Jacqueline F. Hamilton,Hartmut Herrmann,Thorsten Hoffmann,Yoshiteru Iinuma,Myoseon Jang,Michael E. Jenkin,Jose L. Jimenez,Astrid Kiendler-Scharr,Willy Maenhaut,Gordon McFiggans,Th. F. Mentel,Anne Monod,André S. H. Prévôt,John H. Seinfeld,Jason D. Surratt,Rafal Szmigielski,Jürgen Wildt +28 more
TL;DR: In this article, an overview of the atmospheric degradation mechanisms for SOA precursors, gas-particle partitioning theory and analytical techniques used to determine the chemical composition of SOA is presented.
Journal ArticleDOI
Evolution of Organic Aerosols in the Atmosphere
Jose L. Jimenez,Manjula R. Canagaratna,Neil M. Donahue,André S. H. Prévôt,Qi Zhang,Jesse H. Kroll,Peter F. DeCarlo,James Allan,Hugh Coe,Nga L. Ng,Allison C. Aiken,Kenneth S. Docherty,Ingrid M. Ulbrich,Andrew P. Grieshop,Allen L. Robinson,Jonathan Duplissy,Jared D. Smith,Kevin R. Wilson,V. A. Lanz,Christoph Hueglin,Yele Sun,Yele Sun,Jian Tian,Ari Laaksonen,Tomi Raatikainen,Tomi Raatikainen,J. Rautiainen,Petri Vaattovaara,Mikael Ehn,Markku Kulmala,Markku Kulmala,Jason Tomlinson,Don R. Collins,Michael J. Cubison,Edward J. Dunlea,J. A. Huffman,Timothy B. Onasch,M. R. Alfarra,Paul I. Williams,Keith Bower,Yutaka Kondo,Johannes Schneider,Frank Drewnick,Stephan Borrmann,S. Weimer,Kenneth L. Demerjian,D. Salcedo,L. Cottrell,Robert J. Griffin,Akinori Takami,Takao Miyoshi,Shiro Hatakeyama,Akio Shimono,J. Y. Sun,Y. M. Zhang,Katja Dzepina,Joel R. Kimmel,Donna Sueper,J. T. Jayne,Scott C. Herndon,A. Trimborn,Leah R. Williams,Ezra C. Wood,Ann M. Middlebrook,Charles E. Kolb,Urs Baltensperger,Douglas R. Worsnop +66 more
TL;DR: A unifying model framework describing the atmospheric evolution of OA that is constrained by high–time-resolution measurements of its composition, volatility, and oxidation state is presented, which can serve as a basis for improving parameterizations in regional and global models.
Journal ArticleDOI
Organic aerosol and global climate modelling: a review
Maria Kanakidou,John H. Seinfeld,Spyros N. Pandis,Ian Barnes,Frank Dentener,Maria Cristina Facchini,R. Van Dingenen,Barbara Ervens,Athanasios Nenes,Claus J. Nielsen,Erik Swietlicki,J. P. Putaud,Yves Balkanski,Sandro Fuzzi,J. Horth,Geert K. Moortgat,R. Winterhalter,Cathrine Lund Myhre,Kostas Tsigaridis,Elisabetta Vignati,Euripides G. Stephanou,J. Wilson +21 more
TL;DR: In this article, the authors reviewed existing knowledge with regard to organic aerosol (OA) of importance for global climate modelling and defined critical gaps needed to reduce the involved uncertainties, and synthesized the information to provide a continuous analysis of the flow from the emitted material to the atmosphere up to the point of the climate impact of the produced organic aerosols.
Journal ArticleDOI
Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes
Qi Zhang,Jose L. Jimenez,Manjula R. Canagaratna,James Allan,Hugh Coe,Ingrid M. Ulbrich,M. R. Alfarra,Akinori Takami,Ann M. Middlebrook,Yele Sun,Katja Dzepina,Edward J. Dunlea,Kenneth S. Docherty,Peter F. DeCarlo,D. Salcedo,Timothy B. Onasch,J. T. Jayne,Takao Miyoshi,A. Shimono,Shiro Hatakeyama,Nobuyuki Takegawa,Yutaka Kondo,Johannes Schneider,Frank Drewnick,Stephan Borrmann,Silke Weimer,Kenneth L. Demerjian,Paul I. Williams,Keith Bower,Roya Bahreini,Roya Bahreini,L. Cottrell,Robert J. Griffin,J. Rautiainen,J. Y. Sun,Yaping Zhang,D. R. Worsnop +36 more
TL;DR: In this article, organic aerosol data acquired by the AMS in 37 field campaigns were deconvolved into hydrocarbon-like OA (HOA) and several types of oxygenated OA components.
Journal ArticleDOI
Rethinking Organic Aerosols: Semivolatile Emissions and Photochemical Aging
Allen L. Robinson,Neil M. Donahue,Manish Shrivastava,Emily A. Weitkamp,Amy M. Sage,Andrew P. Grieshop,Timothy E. Lane,Jeffrey R. Pierce,Spyros N. Pandis,Spyros N. Pandis +9 more
TL;DR: Accounting for partitioning and photochemical processing of primary emissions creates a more regionally distributed aerosol and brings model predictions into better agreement with observations, attribute this unexplained secondary organic-aerosol production to the oxidation of low-volatility gas-phase species.
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Ubiquity and dominance of oxygenated species in organic aerosols in anthropogenically-influenced Northern Hemisphere midlatitudes
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