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

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 + NO 2) have been shown to play a critical role in the chemical formation of low volatility compounds. Here, 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 inmore » 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, O 3 versus NO 3-initiated oxidation) and to offsetting tendencies in the biogenic versus anthropogenic SOA responses.« less
Authors:
ORCiD logo [1] ;  [2] ;  [3] ; ORCiD logo [3] ; ORCiD logo [4] ;  [3] ;  [3] ;  [5]
  1. Yale Univ., New Haven, CT (United States). Dept. of Geology and Geophysics
  2. Yale Univ., New Haven, CT (United States). Dept. of Geology and Geophysics and School of Forestry and Environmental Studies
  3. National Center for Atmospheric Research, Boulder, CO (United States). Atmospheric Chemistry Observations and Modeling Lab.
  4. National Center for Atmospheric Research, Boulder, CO (United States). Atmospheric Chemistry Observations and Modeling Lab.; Ludwig Maximilian Univ., Munich (Germany). Meteorology Inst.
  5. 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.
Publication Date:
Grant/Contract Number:
SC0006711
Type:
Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online); Journal Volume: 15; Journal Issue: 23; Journal ID: ISSN 1680-7324
Publisher:
European Geosciences Union
Research Org:
Yale Univ., New Haven, CT (United States)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); National Center for Atmospheric Research, Boulder, CO (United States); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1228450
Alternate Identifier(s):
OSTI ID: 1457229

Zheng, Y., Unger, N., Hodzic, A., Emmons, L., Knote, C., Tilmes, S., Lamarque, J. -F., and Yu, P.. Limited effect of anthropogenic nitrogen oxides on secondary organic aerosol formation. United States: N. p., Web. doi:10.5194/acp-15-13487-2015.
Zheng, Y., Unger, N., Hodzic, A., Emmons, L., Knote, C., Tilmes, S., Lamarque, J. -F., & Yu, P.. Limited effect of anthropogenic nitrogen oxides on secondary organic aerosol formation. United States. doi:10.5194/acp-15-13487-2015.
Zheng, Y., Unger, N., Hodzic, A., Emmons, L., Knote, C., Tilmes, S., Lamarque, J. -F., and Yu, P.. 2015. "Limited effect of anthropogenic nitrogen oxides on secondary organic aerosol formation". United States. doi:10.5194/acp-15-13487-2015.
@article{osti_1228450,
title = {Limited effect of anthropogenic nitrogen oxides on secondary organic aerosol formation},
author = {Zheng, Y. and Unger, N. and Hodzic, A. and Emmons, L. and Knote, C. and Tilmes, S. and Lamarque, J. -F. and Yu, P.},
abstractNote = {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 (NOx = NO + NO2) have been shown to play a critical role in the chemical formation of low volatility compounds. Here, 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 NOx-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 NOx perturbations, respectively. The fact that SOA formation is almost unaffected by changes in NOx can be largely attributed to a limited shift in chemical regime, to buffering in chemical pathways (low- and high-NOx pathways, O3 versus NO3-initiated oxidation) and to offsetting tendencies in the biogenic versus anthropogenic SOA responses.},
doi = {10.5194/acp-15-13487-2015},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 23,
volume = 15,
place = {United States},
year = {2015},
month = {12}
}