Optical properties and aging of light-absorbing secondary organic aerosol

The light-absorbing organic aerosol (OA) commonly referred to as “brown carbon” (BrC) has attracted considerable attention in recent years because of its potential to affect atmospheric radiation balance, especially in the ultraviolet region and thus impact photochemical processes. A growing amoun...

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Main Authors: J. Liu, P. Lin, A. Laskin, J. Laskin, S. M. Kathmann, M. Wise, R. Caylor, F. Imholt, V. Selimovic, J. E. Shilling
Format: Article
Language:English
Published: Copernicus Publications 2016-10-01
Series:Atmospheric Chemistry and Physics
Online Access:https://www.atmos-chem-phys.net/16/12815/2016/acp-16-12815-2016.pdf
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author J. Liu
P. Lin
A. Laskin
J. Laskin
S. M. Kathmann
M. Wise
R. Caylor
F. Imholt
V. Selimovic
V. Selimovic
J. E. Shilling
author_facet J. Liu
P. Lin
A. Laskin
J. Laskin
S. M. Kathmann
M. Wise
R. Caylor
F. Imholt
V. Selimovic
V. Selimovic
J. E. Shilling
author_sort J. Liu
collection DOAJ
description The light-absorbing organic aerosol (OA) commonly referred to as “brown carbon” (BrC) has attracted considerable attention in recent years because of its potential to affect atmospheric radiation balance, especially in the ultraviolet region and thus impact photochemical processes. A growing amount of data has indicated that BrC is prevalent in the atmosphere, which has motivated numerous laboratory and field studies; however, our understanding of the relationship between the chemical composition and optical properties of BrC remains limited. We conducted chamber experiments to investigate the effect of various volatile organic carbon (VOC) precursors, NO<sub><i>x</i></sub> concentrations, photolysis time, and relative humidity (RH) on the light absorption of selected secondary organic aerosols (SOA). Light absorption of chamber-generated SOA samples, especially aromatic SOA, was found to increase with NO<sub><i>x</i></sub> concentration, at moderate RH, and for the shortest photolysis aging times. The highest mass absorption coefficient (MAC) value is observed from toluene SOA products formed under high-NO<sub><i>x</i></sub> conditions at moderate RH, in which nitro-aromatics were previously identified as the major light-absorbing compounds. BrC light absorption is observed to decrease with photolysis time, correlated with a decline of the organic nitrate fraction of SOA. SOA formed from mixtures of aromatics and isoprene absorb less visible (Vis) and ultraviolet (UV) light than SOA formed from aromatic precursors alone on a mass basis. However, the mixed SOA absorption was underestimated when optical properties were predicted using a two-product SOA formation model, as done in many current climate models. Further investigation, including analysis on detailed mechanisms, are required to explain the discrepancy.
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spelling doaj.art-558bb4e40f0c4d4e8e01b287b30e07d82022-12-21T20:16:36ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242016-10-0116128151282710.5194/acp-16-12815-2016Optical properties and aging of light-absorbing secondary organic aerosolJ. Liu0P. Lin1A. Laskin2J. Laskin3S. M. Kathmann4M. Wise5R. Caylor6F. Imholt7V. Selimovic8V. Selimovic9J. E. Shilling10Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA, USAEnvironmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA, USAEnvironmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA, USAPhysical Sciences Division, Pacific Northwest National Laboratory, Richland, WA, USAPhysical Sciences Division, Pacific Northwest National Laboratory, Richland, WA, USAMath and Science Department, Concordia University, Portland, OR, USAMath and Science Department, Concordia University, Portland, OR, USAMath and Science Department, Concordia University, Portland, OR, USAMath and Science Department, Concordia University, Portland, OR, USAnow at: Department of Chemistry, University of Montana, Missoula, MT 59812, USAAtmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA, USAThe light-absorbing organic aerosol (OA) commonly referred to as “brown carbon” (BrC) has attracted considerable attention in recent years because of its potential to affect atmospheric radiation balance, especially in the ultraviolet region and thus impact photochemical processes. A growing amount of data has indicated that BrC is prevalent in the atmosphere, which has motivated numerous laboratory and field studies; however, our understanding of the relationship between the chemical composition and optical properties of BrC remains limited. We conducted chamber experiments to investigate the effect of various volatile organic carbon (VOC) precursors, NO<sub><i>x</i></sub> concentrations, photolysis time, and relative humidity (RH) on the light absorption of selected secondary organic aerosols (SOA). Light absorption of chamber-generated SOA samples, especially aromatic SOA, was found to increase with NO<sub><i>x</i></sub> concentration, at moderate RH, and for the shortest photolysis aging times. The highest mass absorption coefficient (MAC) value is observed from toluene SOA products formed under high-NO<sub><i>x</i></sub> conditions at moderate RH, in which nitro-aromatics were previously identified as the major light-absorbing compounds. BrC light absorption is observed to decrease with photolysis time, correlated with a decline of the organic nitrate fraction of SOA. SOA formed from mixtures of aromatics and isoprene absorb less visible (Vis) and ultraviolet (UV) light than SOA formed from aromatic precursors alone on a mass basis. However, the mixed SOA absorption was underestimated when optical properties were predicted using a two-product SOA formation model, as done in many current climate models. Further investigation, including analysis on detailed mechanisms, are required to explain the discrepancy.https://www.atmos-chem-phys.net/16/12815/2016/acp-16-12815-2016.pdf
spellingShingle J. Liu
P. Lin
A. Laskin
J. Laskin
S. M. Kathmann
M. Wise
R. Caylor
F. Imholt
V. Selimovic
V. Selimovic
J. E. Shilling
Optical properties and aging of light-absorbing secondary organic aerosol
Atmospheric Chemistry and Physics
title Optical properties and aging of light-absorbing secondary organic aerosol
title_full Optical properties and aging of light-absorbing secondary organic aerosol
title_fullStr Optical properties and aging of light-absorbing secondary organic aerosol
title_full_unstemmed Optical properties and aging of light-absorbing secondary organic aerosol
title_short Optical properties and aging of light-absorbing secondary organic aerosol
title_sort optical properties and aging of light absorbing secondary organic aerosol
url https://www.atmos-chem-phys.net/16/12815/2016/acp-16-12815-2016.pdf
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