Experimental and modeling study of the impact of vertical transport processes from the boundary-layer on the variability and the budget of tropospheric ozone

Closing the tropospheric ozone budget requires a better understanding of the role of transport processes from the major reservoirs: the planetary boundary layer and the stratosphere. Case studies lead to the identification of mechanisms involved as well as their efficiency. However, their global impact on the budget must be addressed on a climatological basis. This manuscript is thus divided in two parts. First, we present case studies based on ozone LIDAR measurements performed during the ESCOMPTE campaign. This work consists in a data analysis investigation by means of a hybrid - Lagrangian study involving: global meteorological analyses, Lagrangian particle dispersion computation, and mesoscale, chemistry - transport, and Lagrangian photochemistry modeling. Our aim is to document the amount of observed ozone variability related to transport processes and, when appropriate, to infer the role of tropospheric photochemical production. Second, we propose a climatological analysis of the respective impact of transport from the boundary-layer and from the tropopause region on the tropospheric ozone budget. A multivariate analysis is presented and compared to a trajectography approach. Once validated, this algorithm is applied to the whole database of ozone profiles collected above Europe during the past 30 years in order to discuss the seasonal, geographical and temporal variability of transport processes as well as their impact on the tropospheric ozone budget. The variability of turbulent mixing and its impact on the persistence of tropospheric layers will also be discussed. (author)