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

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

;R. M. Doherty;D. S. Stevenson;W. J. Collins;M. G. Sanderson
Journal of agricultural and food chemistry 2005 Vol. 5 pp. 3205-3218
160
doherty2005atmosphericinfluence

Abstract

The impact of convection on tropospheric O3 and its precursors has been examined in a coupled chemistry-climate model. There are two ways that convection affects O3. First, convection affects O3 by vertical mixing of O3 itself. Convection lifts lower tropospheric air to regions where the O3 lifetime is longer, whilst mass-balance subsidence mixes O3-rich upper tropospheric (UT) air downwards to regions where the O3 lifetime is shorter. This tends to decrease UT O3 and the overall tropospheric column of O3. Secondly, convection affects O3 by vertical mixing of O3 precursors. This affects O3 chemical production and destruction. Convection transports isoprene and its degradation products to the UT where they interact with lightning NOx to produce PAN, at the expense of NOx. In our model, we find that convection reduces UT NOx through this mechanism; convective down-mixing also flattens our imposed profile of lightning emissions, further reducing UT NOx. Over tropical land, which has large lightning NOx emissions in the UT, we find convective lofting of NOx from surface sources appears relatively unimportant. Despite UT NOx decreases, UT O3 production increases as a result of UT HOx increases driven by isoprene oxidation chemistry. However, UT O3 tends to decrease, as the effect of convective overturning of O3 itself dominates over changes in O3 chemistry. Convective transport also reduces UT O3 in the mid-latitudes resulting in a 13% decrease in the global tropospheric O3 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 – 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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