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Study of the diurnal variability of atmospheric chemistry with respect to boundary layer dynamics during DOMINO

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Author(s): B. J. H. van Stratum | J. Vilà-Guerau de Arellano | H. G. Ouwersloot | K. van den Dries | T. W. van Laar | M. Martinez | J. Lelieveld | J.-M. Diesch | F. Drewnick | H. Fischer | Z. Hosaynali Beygi | H. Harder | E. Regelin | V. Sinha | J. A. Adame | M. Sörgel | R. Sander | H. Bozem | W. Song | J. Williams | N. Yassaa

Journal: Atmospheric Chemistry and Physics Discussions
ISSN 1680-7367

Volume: 12;
Issue: 3;
Start page: 6519;
Date: 2012;
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ABSTRACT
We study the interactions between atmospheric boundary layer (ABL) dynamics and atmospheric chemistry using a mixed-layer model (MXLCH) coupled to chemical reaction schemes. Guided by both atmospheric and chemical measurements obtained during the DOMINO campaign (2008), numerical experiments are performed to study the role of ABL dynamics and the accuracy of chemical schemes with different complexity: MOZART-4 and a reduced mechanism of this chemical system. Both schemes produce satisfactory results, indicating that the reduced scheme is capable of reproducing the O3-NOx-VOC-HOx diurnal cycle during conditions characterised by a low NOx regime and small O3 tendencies (less than 1 ppb per hour). By focussing on the budget equations of chemical species in the mixed-layer model, we show that for species like O3, NO and NO2, the influence of entrainment and boundary layer growth is of the same order as chemical production/loss. This indicates that an accurate representation of ABL processes is crucial in understanding the daily cycle of chemical species. By comparing the time scales of chemical reactive species with the mixing time scale of turbulence, we propose a classification based on the Damköhler number to further determine the importance of dynamics on chemistry during field campaigns. Our findings advocate an integrated approach, simultaneously solving the ABL dynamics and chemical reactions, in order to obtain a better understanding of chemical pathways and processes and the interpretation of the results obtained during measurement campaigns.
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