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Geoscientific Model Development An interactive open-access journal of the European Geosciences Union
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https://doi.org/10.5194/gmd-2020-335
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/gmd-2020-335
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: development and technical paper 05 Nov 2020

Submitted as: development and technical paper | 05 Nov 2020

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This preprint is currently under review for the journal GMD.

Effects of heterogeneous reactions on global tropospheric chemistry

Phuc T. M. Ha1, Fumikazu Taketani2, Yugo Kanaya2, Ryoki Matsuda1, and Kengo Sudo1,2 Phuc T. M. Ha et al.
  • 1Graduate School of Environmental Studies, Nagoya University, Nagoya, 464-8601, Japan
  • 2Research Institute for Global Change, JAMSTEC, Yokohama, 236-0001, Japan

Abstract. This study uses a chemistry-climate model CHASER (MIROC) to explore the roles of heterogeneous reactions (HRs) in global tropospheric chemistry. Three distinct HRs of N2O5, HO2, and RO2 are considered for surfaces of aerosols and cloud particles. The model simulation is verified with EANET and EMEP stationary observations, R/V MIRAI ship-based data, ATOM1 aircraft measurements, satellite observations by OMI, ISCCP, and CALIPSO-GOCCP, and reanalysis data JRA55. The heterogeneous chemistry facilitates improvement of model performance with respect to observations for NO2, OH, CO, and O3, especially in the lower troposphere. The calculated effects of heterogeneous reactions cause marked changes in global abundances of O3 (−3 %), NOx (−2.2 %), CO (+3.3 %), and global mean CH4 lifetime (+5.9 %). These global effects were contributed mostly by N2O5 uptake onto aerosols in the middle troposphere. At the surface, HO2 uptake gives the largest contributions, with a particularly significant effect in the North Pacific region (−24% O3, +68 % NOx, +8 % CO, and −70 % OH), mainly attributable to its uptake onto clouds. The RO2 reaction has a small contribution, but its global-mean negative effect on O3 is not negligible. In general, the uptakes onto ice crystals and cloud droplets that occur mainly by HO2 and RO2 radicals cause smaller global effects than the aerosol-uptake effects by N2O5 radicals (+1.34 % CH4 lifetime, +1.71 % NOx, −0.56 % O3, +0.63 % CO abundances). Nonlinear responses of tropospheric O3, NOx, and OH to the N2O5 and HO2 uptakes are found in the same modelling framework of this study (R > 0.93). Although all HRs showed negative tendencies for OH and O3 levels, the effects of HR(HO2) on the tropospheric abundance of O3 showed a small increment with an increasing loss rate. However, this positive tendency turns to reduction at higher rates (> 5 times). Our results demonstrate that the HRs affect not only polluted areas but also remote areas such as the mid-latitude sea boundary layer and upper troposphere. Furthermore, HR(HO2) can bring challenges to pollution reduction efforts because it causes opposite effects between NOx (increase) and surface O3 (decrease).

Phuc T. M. Ha et al.

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Phuc T. M. Ha et al.

Model code and software

Effects of heterogeneous reactions on global tropospheric chemistry (Version CHASER-V4.0) Ha, T. M. Phuc, Taketani, Fumikazu, Kanaya, Yugo, Matsuda, Ryoki, and Sudo, Kengo https://doi.org/10.5281/zenodo.4153452

Phuc T. M. Ha et al.

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Short summary
Policies to mitigate air pollution acquire understanding of tropospheric oxidizing capacity, which is controlled by several mechanisms includes heterogeneous processes on aerosols and clouds. This study uses a chemistry-climate model CHASER (MIROC) to explore the heterogeneous effects in troposphere for −3 % O3, −2.2 % NOx, +3.3 % CO, and +5.9 % CH4 lifetime. Besides, these processes affect not only polluted areas but also remote areas and can bring challenges to pollution reduction efforts.
Policies to mitigate air pollution acquire understanding of tropospheric oxidizing capacity,...
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