1Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA, USA
2Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, WA, USA
3Physical Sciences Division, Pacific Northwest National Laboratory, Richland, WA, USA
4Math and Science Department, Concordia University, Portland, OR, USA
anow at: Department of Chemistry, University of Montana, Missoula, MT 59812, USA
Received: 08 Jun 2016 – Published in Atmos. Chem. Phys. Discuss.: 13 Jun 2016
Abstract. 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.
Revised: 18 Sep 2016 – Accepted: 19 Sep 2016 – Published: 14 Oct 2016
Liu, J., Lin, P., Laskin, A., Laskin, J., Kathmann, S. M., Wise, M., Caylor, R., Imholt, F., Selimovic, V., and Shilling, J. E.: Optical properties and aging of light-absorbing secondary organic aerosol, Atmos. Chem. Phys., 16, 12815-12827, doi:10.5194/acp-16-12815-2016, 2016.