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Influence of convective transport on tropospheric ozone and its precursors in a chemistry-climate model

Abstract

The impact of convection on tropospheric O<sub>3</sub> and its precursors has been examined in a coupled chemistry-climate model. There are two ways that convection affects O<sub>3</sub>. First, convection affects O<sub>3</sub> by vertical mixing of O<sub>3</sub> itself. Convection lifts lower tropospheric air to regions where the O<sub>3</sub> lifetime is longer, whilst mass-balance subsidence mixes O<sub>3</sub>-rich upper tropospheric (UT) air downwards to regions where the O<sub>3</sub> lifetime is shorter. This tends to decrease UT O<sub>3</sub> and the overall tropospheric column of O<sub>3</sub>. Secondly, convection affects O<sub>3</sub> by vertical mixing of O<sub>3</sub> precursors. This affects O<sub>3</sub> chemical production and destruction. Convection transports isoprene and its degradation products to the UT where they interact with lightning NO<sub>x</sub> to produce PAN, at the expense of NO<sub>x</sub>. In our model, we find that convection reduces UT NO<sub>x</sub> through this mechanism; convective down-mixing also flattens our imposed profile of lightning emissions, further reducing UT NO<sub>x</sub>. Over tropical land, which has large lightning NO<sub>x</sub> emissions in the UT, we find convective lofting of NO<sub>x</sub> from surface sources appears relatively unimportant. Despite UT NO<sub>x</sub> decreases, UT O<sub>3</sub> production increases as a result of UT HO<sub>x</sub> increases driven by isoprene oxidation chemistry. However, UT O<sub>3</sub> tends to decrease, as the effect of convective overturning of O<sub>3</sub> itself dominates over changes in O<sub>3</sub> chemistry. Convective transport also reduces UT O<sub>3</sub> in the mid-latitudes resulting in a 13% decrease in the global tropospheric O<sub>3</sub> burden. These results contrast with an earlier study that uses a model of similar chemical complexity. Differences in convection schemes as well as chemistry schemes &ndash; in particular isoprene-driven changes are the most likely causes of such discrepancies. Further modelling studies are needed to constrain this uncertainty range

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