Brownness of Organic Aerosol over the United States: Evidence for Seasonal Biomass Burning and Photobleaching Effects.

ABSTRACT

Light-absorptivity of organic aerosol may play an important role in visibility and climate forcing, but it has not been assessed as extensively as black carbon (BC) aerosol. Based on multiwavelength thermal/optical analysis and spectral mass balance, this study quantifies BC for the U.S. Interagency Monitoring of Protected Visual Environments (IMPROVE) network while developing a brownness index (γBr) for non-BC organic carbon (OC*) to illustrate the spatiotemporal trends of light-absorbing brown carbon (BrC) content. OC* light absorption efficiencies range from 0 to 3.1 m2 gC-1 at 405 nm, corresponding to the lowest and highest BrC content of 0 and 100%, respectively. BC, OC*, and γBr explain >97% of the variability of measured spectral light absorption (405-980 nm) across 158 IMPROVE sites. Network-average OC* light absorptions at 405 nm are 50 and 28% those for BC over rural and urban areas, respectively. Larger organic fractions of light absorption occur in winter, partially due to higher organic brownness. Winter γBr exhibits a dramatic regional/urban-rural contrast consistent with anthropogenic BrC emissions from residential wood combustion. The spatial differences diminish to uniformly low γBr in summer, suggesting effective BrC photobleaching over the midlatitudes. An empirical relationship between BC, ambient temperature, and γBr is established, which can facilitate the incorporation of organic aerosol absorptivity into climate and visibility models that currently assume either zero or static organic light absorption efficiencies.