We quantified the global bromine- and iodine-mediated tropospheric ozone loss using global chemical transport model simulations. We tested three datasets of very short-lived substances (VSLS) emissions, three datasets of sea surface iodide concentrations, and an explicit representation of the effects of multi-phase reactions at the air-sea boundary on dry deposition. We then determined optimal model settings based on the evaluation using the ship-borne and aircraft-campaign observations over the ocean. Our evaluation suggested that the explicit representation of multi-phase reaction effects substantially reduced model biases of ozone in the lower troposphere (up to 11%). Moreover, the impacts of using different datasets of VSLS emissions and sea-surface iodide concentrations were relatively small. The global bromine- and iodine-mediated chemical ozone losses were estimated to account for 4% and 17% of the total chemical loss, respectively, while the global iodine-mediated dry deposition loss of ozone was estimated to account for 22% of the global total dry deposition. These bromine- and iodine-mediated ozone losses decreased surface ozone concentrations over the ocean by 10% and 23%, respectively. The observational constraint on model simulations made by this study supports that bromine and iodine substantially impact global tropospheric ozone through atmospheric chemical reactions and dry deposition processes.

我们使用全球化学迁移模型模拟对全球溴和碘介导的对流层臭氧损失进行了量化。我们测试了三个极短寿命物质（VSLS）排放数据集，三个海面碘化物浓度数据集，以及在气-海边界多相反应对干沉降的影响的明确表示。然后，我们根据评估结果，使用对海洋的舰载和飞机战役观测来确定最佳模型设置。我们的评估表明，多相反应效应的显式表示大大降低了对流层下层臭氧的模型偏差（高达11％）。而且，使用不同的VSLS排放和海面碘化物浓度数据集的影响相对较小。据估计，全球溴和碘介导的化学臭氧损失分别占总化学损失的4％和17％，而全球碘介导的臭氧干沉积损失估计占全球化学损失的22％。总干沉降。这些溴和碘介导的臭氧损失分别使海洋表面臭氧浓度分别降低了10％和23％。这项研究对模型模拟的观测约束表明，溴和碘会通过大气化学反应和干法沉积过程对全球对流层臭氧产生重大影响。这些溴和碘介导的臭氧损失分别使海洋表面臭氧浓度分别降低了10％和23％。这项研究对模型模拟的观测约束表明，溴和碘会通过大气化学反应和干法沉积过程对全球对流层臭氧产生重大影响。这些溴和碘介导的臭氧损失分别使海洋表面臭氧浓度分别降低了10％和23％。这项研究对模型模拟的观测约束表明，溴和碘会通过大气化学反应和干法沉积过程对全球对流层臭氧产生重大影响。