Articles | Volume 15, issue 23
Atmos. Chem. Phys., 15, 13487–13506, 2015
Atmos. Chem. Phys., 15, 13487–13506, 2015

Research article 08 Dec 2015

Research article | 08 Dec 2015

Limited effect of anthropogenic nitrogen oxides on secondary organic aerosol formation

Y. Zheng1, N. Unger1,2, A. Hodzic3, L. Emmons3, C. Knote3,a, S. Tilmes3, J.-F. Lamarque3, and P. Yu4,5,b Y. Zheng et al.
  • 1Department of Geology and Geophysics, Yale University, New Haven, CT, USA
  • 2School of Forestry and Environmental Studies, Yale University, New Haven, CT, USA
  • 3Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA
  • 4Department of Atmospheric and Oceanic Sciences, University of Colorado, Boulder, CO, USA
  • 5Laboratory for Atmospheric and Space Physics, University of Colorado, Boulder, CO, USA
  • anow at: Meteorologisches Institut, Ludwig-Maximilians-Universitaet, Munich, Germany
  • bnow at: Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA

Abstract. 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. 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.

Short summary
Nitrogen oxides (NOx) play an important but complex role in secondary organic aerosol (SOA) formation. In this study we update the SOA scheme in a global 3-D chemistry-climate model by implementing a 4-product volatility basis set (VBS) framework with NOx-dependent yields and simplified aging parameterizations. We find that the SOA decrease in response to a 50% reduction in anthropogenic NOx emissions is limited due to the buffering in different chemical pathways.
Final-revised paper