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      Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol

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          Abstract

          Highly oxygenated organic molecules (HOM) are formed in the atmosphere via autoxidation involving peroxy radicals arising from volatile organic compounds (VOC). HOM condense on pre-existing particles and can be involved in new particle formation. HOM thus contribute to the formation of secondary organic aerosol (SOA), a significant and ubiquitous component of atmospheric aerosol known to affect the Earth’s radiation balance. HOM were discovered only very recently, but the interest in these compounds has grown rapidly. In this Review, we define HOM and describe the currently available techniques for their identification/quantification, followed by a summary of the current knowledge on their formation mechanisms and physicochemical properties. A main aim is to provide a common frame for the currently quite fragmented literature on HOM studies. Finally, we highlight the existing gaps in our understanding and suggest directions for future HOM research.

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          Evolution of organic aerosols in the atmosphere.

          Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present 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. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.
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            Chemistry of secondary organic aerosol: Formation and evolution of low-volatility organics in the atmosphere

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              Direct observations of atmospheric aerosol nucleation.

              Atmospheric nucleation is the dominant source of aerosol particles in the global atmosphere and an important player in aerosol climatic effects. The key steps of this process occur in the sub-2-nanometer (nm) size range, in which direct size-segregated observations have not been possible until very recently. Here, we present detailed observations of atmospheric nanoparticles and clusters down to 1-nm mobility diameter. We identified three separate size regimes below 2-nm diameter that build up a physically, chemically, and dynamically consistent framework on atmospheric nucleation--more specifically, aerosol formation via neutral pathways. Our findings emphasize the important role of organic compounds in atmospheric aerosol formation, subsequent aerosol growth, radiative forcing and associated feedbacks between biogenic emissions, clouds, and climate.
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                Author and article information

                Journal
                Chem Rev
                Chem. Rev
                cr
                chreay
                Chemical Reviews
                American Chemical Society
                0009-2665
                1520-6890
                25 February 2019
                27 March 2019
                : 119
                : 6
                : 3472-3509
                Affiliations
                []Institute for Atmospheric and Earth System Research, Faculty of Science, University of Helsinki , Helsinki 00014, Finland
                []Aerosol and Haze Laboratory, University of Chemical Technology , Beijing 100029, P.R. China
                [§ ]IRCELYON, CNRSUniversity of Lyon , Villeurbanne 69626, France
                []Department of Environmental Science and Analytical Chemistry, Stockholm University , Stockholm 11418, Sweden
                []Division of Nuclear Physics, Department of Physics, Lund University , Lund 22100, Sweden
                [# ]Leibniz Institute for Tropospheric Research , Leipzig 04318, Germany
                []Division of Geological and Planetary Sciences, California Institute of Technology , Pasadena, California 91125, United States
                []Institut für Energie und Klimaforschung, IEK-8, Forschungszentrum Jülich GmbH , Jülich 52425, Germany
                []Institute of Physics, University of Tartu , Tartu 50090, Estonia
                []Aerodyne Research Inc. , Billerica, Massachusetts 01821, United States
                [+ ]Department of Atmospheric Sciences, University of Washington , Seattle, Washington 98195, United States
                []Center for Atmospheric Particle Studies, Carnegie Mellon University , Pittsburgh, Pennsylvania 15213, United States
                []Department of Chemistry, University of Cøpenhagen , Cøpenhagen 2100, Denmark
                Author notes
                Article
                10.1021/acs.chemrev.8b00395
                6439441
                30799608
                d7463814-baf9-4f07-99df-5aa0f818c167
                Copyright © 2019 American Chemical Society

                This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.

                History
                : 25 June 2018
                Categories
                Review
                Custom metadata
                cr8b00395
                cr-2018-00395m

                Chemistry
                Chemistry

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