1Laboratoire de Physique et Chimie de l’Environnement/CNRS and Universitè d’Orléans, 3A Avenue de la Recherche Scientifique, 45071 Orléans cedex 2, France
2Instituto de Pesquisas Meteorológicas, Universidade Estadual Paulista, CX Postal 281 17033-360 Bauru, SP, Brazil
3Laboratoire de Météorologie Physique/CNRS-OPGC/Université Blaise Pascal, 24 Avenue des Landais, 63177 Aubière cedex, France
4Centro de Previsão de Tempo e Estudos Climàticos, Rodovia Presidente Dutra, km 40 SPRJ 12630-000, Cachoeira Paulista, SP, Brazil
Abstract. The aim of this work is to study the local impact of deep convection on the upper troposphere/lower stratosphere air composition. For this purpose, we performed a 42-h simulation of a severe convective event near Bauru, in the central State of São Paulo (Brazil), with the 3-D mesoscale model RAMS coupled on-line with a chemistry model. The meteorological results of the simulation are evaluated using comparisons with near surface measurements of wind and temperature and with surface rainfall rates derived from radar observations. These comparisons show that the model produces meteorological fields consistent with the observations.
This present paper (Part I) is devoted to the analysis of the ozone precursors in the upper troposphere/lower stratosphere: CO, NOx (=NO+NO2) and non-methane volatile organic compounds. The simulation results show that the distribution of CO with altitude is closely related to the upward convective motions and consecutive outflow at the top of the convective cells leading to a bulge of CO between 7 km altitude and the cold point tropopause (around 17km altitude). The model results for CO are consistent with satellite-borne measurements in the 700–500 hPa layer. The simulation also indicates enhanced amounts of NOx up to 2 ppbv in the 7–17 km altitude layer. These NOx concentrations are mainly produced by the lightning associated with the intense convective activity. Stratospheric NOx are not affected by the tropospheric NOx since there is, on average, no significant upward NOx flux through the tropopause. For non-methane volatile organic compounds, the convective activity tends to significantly increase the amount of ozone precursors in the 7–17 km layer by dynamical effects as for CO. During daytime, this bulge is largely reduced in the upper part of the layer for reactive species, such as isoprene, ethene and propene, since they undergo chemical loss. This loss is mainly due to their reactions with OH, OH mixing ratio being significantly increased during the daytime by the production of NOx by lightning. The bulges of ozone precursors in the upper troposphere are likely to be of importance in the ozone budget in the upper troposphere and lower stratosphere. This issue is discussed in Part II of this series of papers.