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

Autor: Gaubert B; Atmospheric Chemistry Observations and Modeling, National Center for Atmospheric Research, Boulder, CO, USA., Emmons LK; Atmospheric Chemistry Observations and Modeling, National Center for Atmospheric Research, Boulder, CO, USA., Raeder K; Computational and Information Systems Laboratory, National Center for Atmospheric Research, Boulder, CO, USA., Tilmes S; Atmospheric Chemistry Observations and Modeling, National Center for Atmospheric Research, Boulder, CO, USA., Miyazaki K; Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA, USA., Arellano AF Jr; Dept. of Hydrology and Atmospheric Sciences, University of Arizona, Tucson, AZ, USA., Elguindi N; Laboratoire d'Aérologie, CNRS, Université de Toulouse, Toulouse, France., Granier C; Laboratoire d'Aérologie, CNRS, Université de Toulouse, Toulouse, France.; NOAA Chemical Sciences Laboratory-CIRES/University of Colorado, Boulder, CO, USA., Tang W; Advanced Study Program, National Center for Atmospheric Research, Boulder, CO, USA., Barré J; European Centre for Medium-Range Weather Forecasts, Shinfield Park, Reading, RG2 9AX, UK., Worden HM; Atmospheric Chemistry Observations and Modeling, National Center for Atmospheric Research, Boulder, CO, USA., Buchholz RR; Atmospheric Chemistry Observations and Modeling, National Center for Atmospheric Research, Boulder, CO, USA., Edwards DP; Atmospheric Chemistry Observations and Modeling, National Center for Atmospheric Research, Boulder, CO, USA., Franke P; Forschungszentrum Jülich GmbH, Institut für Energie und Klimaforschung IEK-8, 52425 Jülich, Germany., Anderson JL; Computational and Information Systems Laboratory, National Center for Atmospheric Research, Boulder, CO, USA., Saunois M; Laboratoire des Sciences du Climat et de l'Environnement, LSCE-IPSL (CEA-CNRS-UVSQ), Université Paris-Saclay, 91191 Gif-sur-Yvette, France., Schroeder J; California Air Resources Board, Sacramento, CA, USA., Woo JH; Department of Advanced Technology Fusion, Konkuk University, Seoul, South Korea., Simpson IJ; Department of Chemistry, University of California, Irvine, Irvine, CA 92697, USA., Blake DR; Department of Chemistry, University of California, Irvine, Irvine, CA 92697, USA., Meinardi S; Department of Chemistry, University of California, Irvine, Irvine, CA 92697, USA., Wennberg PO; California Institute of Technology, Pasadena, CA, USA., Crounse J; California Institute of Technology, Pasadena, CA, USA., Teng A; California Institute of Technology, Pasadena, CA, USA., Kim M; California Institute of Technology, Pasadena, CA, USA., Dickerson RR; Department of Atmospheric and Oceanic Science, University of Maryland, College Park, MD, USA.; Earth System Science Interdisciplinary Center, University of Maryland, College Park, MD, USA., He H; Department of Atmospheric and Oceanic Science, University of Maryland, College Park, MD, USA.; Earth System Science Interdisciplinary Center, University of Maryland, College Park, MD, USA., Ren X; Department of Atmospheric and Oceanic Science, University of Maryland, College Park, MD, USA.; Air Resources Laboratory, National Oceanic and Atmospheric Administration, College Park, MD, USA., Pusede SE; Department of Environmental Sciences, University of Virginia, Charlottesville, VA, USA., Diskin GS; NASA Langley Research Center, Hampton, VA, USA.
Jazyk: angličtina
Zdroj: Atmospheric chemistry and physics [Atmos Chem Phys] 2020 Dec 01; Vol. 20 (23), pp. 14617-14647.
DOI: 10.5194/acp-20-14617-2020
Abstrakt: 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.
Competing Interests: Competing interests. The authors declare that they have no conflict of interest.
Databáze: MEDLINE
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