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Decadal changes in summertime reactive oxidized nitrogen and surface ozone over the Southeast United States

Li, Jingyi and Mao, Jingqiu and Fiore, Arlene M. and Cohen, Ronald C. and Crounse, John D. and Teng, Alex P. and Wennberg, Paul O. and Lee, Ben H. and Lopez-Hilfiker, Felipe D. and Thornton, Joel A. and Peischl, Jeff and Pollack, Ilana B. and Ryerson, Thomas B. and Veres, Patrick and Roberts, James M. and Neuman, J. Andrew and Nowak, John B. and Wolfe, Glenn M. and Hanisco, Thomas F. and Fried, Alan and Singh, Hanwant B. and Dibb, Jack and Paulot, Fabien and Horowitz, Larry W. (2018) Decadal changes in summertime reactive oxidized nitrogen and surface ozone over the Southeast United States. Atmospheric Chemistry and Physics, 18 (3). pp. 2341-2361. ISSN 1680-7324. https://resolver.caltech.edu/CaltechAUTHORS:20180307-130604960

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Abstract

Widespread efforts to abate ozone (O_3) smog have significantly reduced emissions of nitrogen oxides (NO_x) over the past 2 decades in the Southeast US, a place heavily influenced by both anthropogenic and biogenic emissions. How reactive nitrogen speciation responds to the reduction in NO_x emissions in this region remains to be elucidated. Here we exploit aircraft measurements from ICARTT (July–August 2004), SENEX (June–July 2013), and SEAC4RS (August–September 2013) and long-term ground measurement networks alongside a global chemistry–climate model to examine decadal changes in summertime reactive oxidized nitrogen (RON) and ozone over the Southeast US. We show that our model can reproduce the mean vertical profiles of major RON species and the total (NO_y) in both 2004 and 2013. Among the major RON species, nitric acid (HNO_3) is dominant (∼ 42–45 %), followed by NO_x (31 %), total peroxy nitrates (ΣPNs; 14 %), and total alkyl nitrates (ΣANs; 9–12 %) on a regional scale. We find that most RON species, including NO_x, ΣPNs, and HNO_3, decline proportionally with decreasing NO_x emissions in this region, leading to a similar decline in NO_y. This linear response might be in part due to the nearly constant summertime supply of biogenic VOC emissions in this region. Our model captures the observed relative change in RON and surface ozone from 2004 to 2013. Model sensitivity tests indicate that further reductions of NO_x emissions will lead to a continued decline in surface ozone and less frequent high-ozone events.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.5194/acp-18-2341-2018DOIArticle
https://www.atmos-chem-phys.net/18/2341/2018/PublisherArticle
https://www.atmos-chem-phys.net/18/2341/2018/acp-18-2341-2018-supplement.pdfPublisherSupplement
ORCID:
AuthorORCID
Crounse, John D.0000-0001-5443-729X
Wennberg, Paul O.0000-0002-6126-3854
Thornton, Joel A.0000-0002-5098-4867
Additional Information:© Author(s) 2018. This work is distributed under the Creative Commons Attribution 4.0 License. Received: 29 Jun 2017 – Discussion started: 13 Jul 2017. Revised: 23 Dec 2017 – Accepted: 03 Jan 2018 – Published: 16 Feb 2018. The authors thank Vaishali Naik (NOAA GFDL) for providing emission inventories in the GFDL AM3 model and Leo Donner (NOAA GFDL) and William Cooke (UCAR/NOAA) for help with the convection scheme of AM3. Jingyi Li, Jingqiu Mao, and Larry W. Horowitz acknowledge support from the NOAA Climate Program Office under grant no. NA13OAR431007. Jingqiu Mao, Larry W. Horowitz, and Arlene M. Fiore acknowledge support from the NOAA Climate Program Office under grant no. NA14OAR4310133. John D. Crounse and Paul O. Wennberg acknowledge support from NASA grants (NNX12AC06G and NNX14AP46G). Jingyi Li acknowledges support from the Startup Foundation for Introducing Talent of NUIST grant no. 2243141701014 and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD). Data availability. Observational datasets and modeling results are available upon request to the corresponding author (jmao2@alaska.edu). The authors declare that they have no conflict of interest. Edited by: Nga Lee Ng Reviewed by: three anonymous referees
Funders:
Funding AgencyGrant Number
National Oceanic and Atmospheric Administration (NOAA)NA13OAR431007
National Oceanic and Atmospheric Administration (NOAA)NA14OAR4310133
NASANNX12AC06G
NASANNX14AP46G
Nanjing University of Information Science and Technology2243141701014
Priority Academic Program Development of Jiangsu Higher Education InstitutionsUNSPECIFIED
Issue or Number:3
Record Number:CaltechAUTHORS:20180307-130604960
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20180307-130604960
Official Citation:Li, J., Mao, J., Fiore, A. M., Cohen, R. C., Crounse, J. D., Teng, A. P., Wennberg, P. O., Lee, B. H., Lopez-Hilfiker, F. D., Thornton, J. A., Peischl, J., Pollack, I. B., Ryerson, T. B., Veres, P., Roberts, J. M., Neuman, J. A., Nowak, J. B., Wolfe, G. M., Hanisco, T. F., Fried, A., Singh, H. B., Dibb, J., Paulot, F., and Horowitz, L. W.: Decadal changes in summertime reactive oxidized nitrogen and surface ozone over the Southeast United States, Atmos. Chem. Phys., 18, 2341-2361, https://doi.org/10.5194/acp-18-2341-2018, 2018.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:85183
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:07 Mar 2018 21:48
Last Modified:03 Oct 2019 19:27

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