2022Unpublished venueOpen access

Comment on gmd-2021-388

Cyril Caram, Sophie Szopa, Anne Cozic, Slimane Bekki, Carlos A. Cuevas, Alfonso Saiz‐Lopez

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Abstract

Abstract. The atmospheric chemistry of halogenated species (Cl, Br, I) participates in the global chemical sink of tropospheric ozone and perturbs the oxidizing capacity of the troposphere, notably influencing the atmospheric lifetime of methane. Global chemistry-climate models are commonly used to assess the global budget of ozone, its sensitivity to emissions of its precursors, and to project its long-term evolution. Here, we report on the implementation of tropospheric halogens chemistry in the chemistry-climate model LMDZ-INCA and its effects on the tropospheric ozone budget. Overall, the results show that the model simulates satisfactorily the impact of halogens on the photooxidizing system in the troposphere, in particular in the marine boundary layer. To elucidate the mechanisms and quantify the effects, standard metrics representative of the behavior of the tropospheric chemical system (Ox, HOx, NOx, CH4, and NMVOCs) are computed with and without halogen chemistry. Tropospheric halogens in the LMDZ-INCA model lead to a decrease of 22 % in the ozone burden, 8 % in OH, and 33 % in NOx. Additional sensitivity simulations show that the inclusion of halogens chemistry makes ozone more sensitive to perturbations in CH4, NOx, and NMVOCs. Consistent with other global model studies, the sensitivity of the tropospheric ozone burden to changes from pre-industrial to present-day emissions is found to be ~20 % lower when tropospheric halogens are taken into account.

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Abstract. The atmospheric chemistry of halogenated species (Cl, Br, I) participates in the global chemical sink of tropospheric ozone and perturbs the oxidizing capacity of the troposphere, notably influencing the atmospheric lifetime of methane. Global chemistry-climate models are commonly used to assess the global budget of ozone, its sensitivity to emissions of its precursors, and to project its long-term evolution. Here, we report on the implementation of tropospheric halogens chemistry in the chemistry-climate model LMDZ-INCA and its effects on the tropospheric ozone budget. Overall, the results show that the model simulates satisfactorily the impact of halogens on the photooxidizing system in the troposphere, in particular in the marine boundary layer. To elucidate the mechanisms and quantify the effects, standard metrics representative of the behavior of the tropospheric chemical system (Ox, HOx, NOx, CH4, and NMVOCs) are computed with and without halogen chemistry. Tropospheric halogens in the LMDZ-INCA model lead to a decrease of 22 % in the ozone burden, 8 % in OH, and 33 % in NOx. Additional sensitivity simulations show that the inclusion of halogens chemistry makes ozone more sensitive to perturbations in CH4, NOx, and NMVOCs. Consistent with other global model studies, the sensitivity of the tropospheric ozone burden to changes from pre-industrial to present-day emissions is found to be ~20 % lower when tropospheric halogens are taken into account.

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Available abstract

Abstract. The atmospheric chemistry of halogenated species (Cl, Br, I) participates in the global chemical sink of tropospheric ozone and perturbs the oxidizing capacity of the troposphere, notably influencing the atmospheric lifetime of methane. Global chemistry-climate models are commonly used to assess the global budget of ozone, its sensitivity to emissions of its precursors, and to project its long-term evolution. Here, we report on the implementation of tropospheric halogens chemistry in the chemistry-climate model LMDZ-INCA and its effects on the tropospheric ozone budget. Overall, the results show that the model simulates satisfactorily the impact of halogens on the photooxidizing system in the troposphere, in particular in the marine boundary layer. To elucidate the mechanisms and quantify the effects, standard metrics representative of the behavior of the tropospheric chemical system (Ox, HOx, NOx, CH4, and NMVOCs) are computed with and without halogen chemistry. Tropospheric halogens in the LMDZ-INCA model lead to a decrease of 22 % in the ozone burden, 8 % in OH, and 33 % in NOx. Additional sensitivity simulations show that the inclusion of halogens chemistry makes ozone more sensitive to perturbations in CH4, NOx, and NMVOCs. Consistent with other global model studies, the sensitivity of the tropospheric ozone burden to changes from pre-industrial to present-day emissions is found to be ~20 % lower when tropospheric halogens are taken into account.

Key concepts: Tropospheric ozone, Troposphere, Ozone, Atmospheric chemistry, Halogen, Bromine, Atmospheric sciences, Chemistry

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