Limited effect of anthropogenic nitrogen oxides on secondary organic aerosol formation

Zheng, Y.; Unger, N.; Hodzic, A.; Emmons, L.; Knote, C.; Tilmes, S.; Lamarque, J. -F.; Yu, P.

doi:10.5194/acp-15-13487-2015

Title: Limited effect of anthropogenic nitrogen oxides on secondary organic aerosol formation

Journal Article · Tue Dec 08 00:00:00 EST 2015 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-15-13487-2015· OSTI ID:1228450

^[1]; Unger, N. ^[2]; Hodzic, A. ^[3];

^[3];

^[4]; Tilmes, S. ^[3]; Lamarque, J. -F. ^[3]; Yu, P. ^[5]

Yale Univ., New Haven, CT (United States). Dept. of Geology and Geophysics
Yale Univ., New Haven, CT (United States). Dept. of Geology and Geophysics and School of Forestry and Environmental Studies
National Center for Atmospheric Research, Boulder, CO (United States). Atmospheric Chemistry Observations and Modeling Lab
National Center for Atmospheric Research, Boulder, CO (United States). Atmospheric Chemistry Observations and Modeling Lab.; Ludwig Maximilian Univ., Munich (Germany). Meteorology Inst.
Univ. of Colorado, Boulder, CO (United States). Dept. of Atmospheric and Oceanic Sciences and Lab. for Atmospheric and Space Physics; National Oceanic and Atmospheric Administration (NOAA), Boulder, CO (United States). Earth System Research Lab.

Globally, secondary organic aerosol (SOA) is mostly formed from emissions of biogenic volatile organic compounds (VOCs) by vegetation, but it can be modified by human activities as demonstrated in recent research. Specifically, nitrogen oxides (NO_x = NO + NO₂) have been shown to play a critical role in the chemical formation of low volatility compounds. We have updated the SOA scheme in the global NCAR (National Center for Atmospheric Research) Community Atmospheric Model version 4 with chemistry (CAM4-chem) by implementing a 4-product volatility basis set (VBS) scheme, including NO_x-dependent SOA yields and aging parameterizations. Small differences are found for the no-aging VBS and 2-product schemes; large increases in SOA production and the SOA-to-OA ratio are found for the aging scheme. The predicted organic aerosol amounts capture both the magnitude and distribution of US surface annual mean measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network by 50 %, and the simulated vertical profiles are within a factor of 2 compared to aerosol mass spectrometer (AMS) measurements from 13 aircraft-based field campaigns across different regions and seasons. We then perform sensitivity experiments to examine how the SOA loading responds to a 50 % reduction in anthropogenic nitric oxide (NO) emissions in different regions. We find limited SOA reductions of 0.9–5.6, 6.4–12.0 and 0.9–2.8 % for global, southeast US and Amazon NO_x perturbations, respectively. The fact that SOA formation is almost unaffected by changes in NO_x can be largely attributed to a limited shift in chemical regime, to buffering in chemical pathways (low- and high-NO_x pathways, O₃ versus NO₃-initiated oxidation) and to offsetting tendencies in the biogenic versus anthropogenic SOA responses.

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Research Organization:: Yale Univ., New Haven, CT (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER); National Center for Atmospheric Research, Boulder, CO (United States); National Science Foundation (NSF)

Grant/Contract Number:: SC0006711

OSTI ID:: 1228450

Alternate ID(s):: OSTI ID: 1457229

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Vol. 15 Journal Issue: 23; ISSN 1680-7324

Publisher:: Copernicus Publications, EGUCopyright Statement

Country of Publication:: Germany

Language:: English

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Cited by: 15 works

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