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Toward a chemical reanalysis in a coupled chemistry-climate model: An evaluation of MOPITT CO assimilation and its impact on tropospheric composition

Journal Article · · Journal of Geophysical Research: Atmospheres
DOI:https://doi.org/10.1002/2016JD024863· OSTI ID:1480703
 [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1];  [3];  [3];  [3];  [1];  [1];  [1];  [4];  [1];  [5];  [6];  [7]
  1. National Center for Atmospheric Research, Boulder, CO (United States). Atmospheric Chemistry Observations and Modeling Lab.
  2. Univ. of Arizona, Tucson, AZ (United States). Dept. of Atmospheric Sciences
  3. National Center for Atmospheric Research, Boulder, CO (United States). Inst. for Mathematics Applied to Geosciences
  4. Max Planck Inst. for Chemistry, Mainz (Germany). Biogeochemistry Dept.
  5. Univ. of Bremen (Germany). Inst. of Environmental Physics (IUP)
  6. Univ. of Toronto, ON (Canada). Dept. of Physics
  7. Univ. of Wollongong, NSW (Australia)

Here, we examine in detail a 1 year global reanalysis of carbon monoxide (CO) that is based on joint assimilation of conventional meteorological observations and Measurement of Pollution in The Troposphere (MOPITT) multispectral CO retrievals in the Community Earth System Model (CESM). Our focus is to assess the impact to the chemical system when CO distribution is constrained in a coupled full chemistry-climate model like CESM. To do this, we first evaluate the joint reanalysis (MOPITT Reanalysis) against four sets of independent observations and compare its performance against a reanalysis with no MOPITT assimilation (Control Run). We then investigate the CO burden and chemical response with the aid of tagged sectoral CO tracers. We estimate the total tropospheric CO burden in 2002 (from ensemble mean and spread) to be 371 ± 12% Tg for MOPITT Reanalysis and 291 ± 9% Tg for Control Run. Our multispecies analysis of this difference suggests that (a) direct emissions of CO and hydrocarbons are too low in the inventory used in this study and (b) chemical oxidation, transport, and deposition processes are not accurately and consistently represented in the model. Increases in CO led to net reduction of OH and subsequent longer lifetime of CH4(Control Run: 8.7 years versus MOPITT Reanalysis: 9.3 years). Yet at the same time, this increase led to 5-10% enhancement of Northern Hemisphere O3 and overall photochemical activity via HOx recycling. Such nonlinear effects further complicate the attribution to uncertainties in direct emissions alone. This has implications to chemistry-climate modeling and inversion studies of longer-lived species.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); National Aeronautics and Space Administration (NASA) (United States); National Science Foundation (NSF) (United States); Australian Research Council (ARC)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1480703
Journal Information:
Journal of Geophysical Research: Atmospheres, Journal Name: Journal of Geophysical Research: Atmospheres Journal Issue: 12 Vol. 121; ISSN 2169-897X
Publisher:
American Geophysical UnionCopyright Statement
Country of Publication:
United States
Language:
English

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