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Title: 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 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 x 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 x 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 x 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) lightmore » 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.« less
Authors:
; ; ; ; ; ; ; ; ;
Publication Date:
Grant/Contract Number:
Laboratory Directed Research and Development
Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 16 Journal Issue: 19; Journal ID: ISSN 1680-7324
Publisher:
Copernicus GmbH
Sponsoring Org:
USDOE
Country of Publication:
Germany
Language:
English
OSTI Identifier:
1328969

Liu, Jiumeng, Lin, Peng, Laskin, Alexander, Laskin, Julia, Kathmann, Shawn M., Wise, Matthew, Caylor, Ryan, Imholt, Felisha, Selimovic, Vanessa, and Shilling, John E.. Optical properties and aging of light-absorbing secondary organic aerosol. Germany: N. p., Web. doi:10.5194/acp-16-12815-2016.
Liu, Jiumeng, Lin, Peng, Laskin, Alexander, Laskin, Julia, Kathmann, Shawn M., Wise, Matthew, Caylor, Ryan, Imholt, Felisha, Selimovic, Vanessa, & Shilling, John E.. Optical properties and aging of light-absorbing secondary organic aerosol. Germany. doi:10.5194/acp-16-12815-2016.
Liu, Jiumeng, Lin, Peng, Laskin, Alexander, Laskin, Julia, Kathmann, Shawn M., Wise, Matthew, Caylor, Ryan, Imholt, Felisha, Selimovic, Vanessa, and Shilling, John E.. 2016. "Optical properties and aging of light-absorbing secondary organic aerosol". Germany. doi:10.5194/acp-16-12815-2016.
@article{osti_1328969,
title = {Optical properties and aging of light-absorbing secondary organic aerosol},
author = {Liu, Jiumeng and Lin, Peng and Laskin, Alexander and Laskin, Julia and Kathmann, Shawn M. and Wise, Matthew and Caylor, Ryan and Imholt, Felisha and Selimovic, Vanessa and Shilling, John E.},
abstractNote = {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, NOx 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 NOx 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-NOx 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.},
doi = {10.5194/acp-16-12815-2016},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 19,
volume = 16,
place = {Germany},
year = {2016},
month = {10}
}