Effects of anthropogenic emissions on aerosol formation from isoprene and monoterpenes in the southeastern United States

Author:

Xu Lu,Guo Hongyu,Boyd Christopher M.,Klein Mitchel,Bougiatioti Aikaterini,Cerully Kate M.,Hite James R.,Isaacman-VanWertz GabrielORCID,Kreisberg Nathan M.,Knote Christoph,Olson Kevin,Koss Abigail,Goldstein Allen H.,Hering Susanne V.,de Gouw Joost,Baumann Karsten,Lee Shan-Hu,Nenes Athanasios,Weber Rodney J.,Ng Nga Lee

Abstract

Secondary organic aerosol (SOA) constitutes a substantial fraction of fine particulate matter and has important impacts on climate and human health. The extent to which human activities alter SOA formation from biogenic emissions in the atmosphere is largely undetermined. Here, we present direct observational evidence on the magnitude of anthropogenic influence on biogenic SOA formation based on comprehensive ambient measurements in the southeastern United States (US). Multiple high-time-resolution mass spectrometry organic aerosol measurements were made during different seasons at various locations, including urban and rural sites in the greater Atlanta area and Centreville in rural Alabama. Our results provide a quantitative understanding of the roles of anthropogenic SO2 and NOx in ambient SOA formation. We show that isoprene-derived SOA is directly mediated by the abundance of sulfate, instead of the particle water content and/or particle acidity as suggested by prior laboratory studies. Anthropogenic NOx is shown to enhance nighttime SOA formation via nitrate radical oxidation of monoterpenes, resulting in the formation of condensable organic nitrates. Together, anthropogenic sulfate and NOx can mediate 43–70% of total measured organic aerosol (29–49% of submicron particulate matter, PM1) in the southeastern US during summer. These measurements imply that future reduction in SO2 and NOx emissions can considerably reduce the SOA burden in the southeastern US. Updating current modeling frameworks with these observational constraints will also lead to more accurate treatment of aerosol formation for regions with substantial anthropogenic−biogenic interactions and consequently improve air quality and climate simulations.

Funder

National Science Foundation

U.S. Environmental Protection Agency

DOC | National Oceanic and Atmospheric Administration

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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