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Correcting model biases of CO in East Asia: impact on oxidant distributions during KORUS-AQ Public Deposited

https://scholar.colorado.edu/concern/articles/q237ht184
Abstract
  • Global coupled chemistry–climate models underestimate carbon monoxide (CO) in the Northern Hemisphere, exhibiting a pervasive negative bias against measurements peaking in late winter and early spring. While this bias has been commonly attributed to underestimation of direct anthropogenic and biomass burning emissions, chemical production and loss via OH reaction from emissions of anthropogenic and biogenic volatile organic compounds (VOCs) play an important role. Here we investigate the reasons for this underestimation using aircraft measurements taken in May and June 2016 from the Korea–United States Air Quality (KORUS-AQ) experiment in South Korea and the Air Chemistry Research in Asia (ARIAs) in the North China Plain (NCP). For reference, multispectral CO retrievals (V8J) from the Measurements of Pollution in the Troposphere (MOPITT) are jointly assimilated with meteorological observations using an ensemble adjustment Kalman filter (EAKF) within the global Community Atmosphere Model with Chemistry (CAM-Chem) and the Data Assimilation Research Testbed (DART). With regard to KORUS-AQ data, CO is underestimated by 42 % in the control run and by 12 % with the MOPITT assimilation run. The inversion suggests an underestimation of anthropogenic CO sources in many regions, by up to 80 % for northern China, with large increments over the Liaoning Province and the North China Plain (NCP). Yet, an often-overlooked aspect of these inversions is that correcting the underestimation in anthropogenic CO emissions also improves the comparison with observational O 3 datasets and observationally constrained box model simulations of OH and HO 2 . Running a CAM-Chem simulation with the updated emissions of anthropogenic CO reduces the bias by 29 % for CO, 18 % for ozone, 11 % for HO 2 , and 27 % for OH. Longer-lived anthropogenic VOCs whose model errors are correlated with CO are also improved, while short-lived VOCs, including formaldehyde, are difficult to constrain solely by assimilating satellite retrievals of CO. During an anticyclonic episode, better simulation of O 3 , with an average underestimation of 5.5 ppbv, and a reduction in the bias of surface formaldehyde and oxygenated VOCs can be achieved by separately increasing by a factor of 2 the modeled biogenic emissions for the plant functional types found in Korea. Results also suggest that controlling VOC and CO emissions, in addition to widespread NO x controls, can improve ozone pollution over East Asia.

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  • Full list of author: Benjamin Gaubert1, Louisa K. Emmons1, Kevin Raeder2, Simone Tilmes1, Kazuyuki Miyazaki3, Avelino F. Arellano Jr.4, Nellie Elguindi5, Claire Granier5,6, Wenfu Tang7, Jérôme Barré8, Helen M. Worden1, Rebecca R. Buchholz1, David P. Edwards1, Philipp Franke9, Jeffrey L. Anderson2, Marielle Saunois10, Jason Schroeder11, Jung-Hun Woo12, Isobel J. Simpson13, Donald R. Blake13, Simone Meinardi13, Paul O. Wennberg14, John Crounse14, Alex Teng14, Michelle Kim14, Russell R. Dickerson15,16, Hao He15,16, Xinrong Ren15,17, Sally E. Pusede18, and Glenn S. Diskin19 1Atmospheric Chemistry Observations and Modeling, National Center for Atmospheric Research, Boulder, CO, USA 2Computational and Information Systems Laboratory, National Center for Atmospheric Research, Boulder, CO, USA 3Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA, USA 4Dept. of Hydrology and Atmospheric Sciences, University of Arizona, Tucson, AZ, USA 5Laboratoire d’Aérologie, CNRS, Université de Toulouse, Toulouse, France 6NOAA Chemical Sciences Laboratory-CIRES/University of Colorado, Boulder, CO, USA 7Advanced Study Program, National Center for Atmospheric Research, Boulder, CO, USA 8European Centre for Medium-Range Weather Forecasts, Shinfield Park, Reading, RG2 9AX, UK 9Forschungszentrum Jülich GmbH, Institut für Energie und Klimaforschung IEK-8, 52425 Jülich, Germany 10Laboratoire des Sciences du Climat et de l’Environnement, LSCE-IPSL (CEA-CNRS-UVSQ), Université Paris-Saclay, 91191 Gif-sur-Yvette, France 11California Air Resources Board, Sacramento, CA, USA 12Department of Advanced Technology Fusion, Konkuk University, Seoul, South Korea 13Department of Chemistry, University of California, Irvine, Irvine, CA 92697, USA 14California Institute of Technology, Pasadena, CA, USA 15Department of Atmospheric and Oceanic Science, University of Maryland, College Park, MD, USA 16Earth System Science Interdisciplinary Center, University of Maryland, College Park, MD, USA 17Air Resources Laboratory, National Oceanic and Atmospheric Administration, College Park, MD, USA 18Department of Environmental Sciences, University of Virginia, Charlottesville, VA, USA 19NASA Langley Research Center, Hampton, VA, USA
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Journal Issue/Number
  • 23
Journal Volume
  • 20
Last Modified
  • 2022-01-19
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DOI
ISSN
  • 1680-7324
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