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Towards an operational aqueous phase chemistry mechanism for regional chemistry-transport models: CAPRAM-RED and its application to the COSMO-MUSCAT model

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Abstract

Mechanism reductions of the detailed aqueous phase chemistry mechanism CAPRAM 3.0i are performed. Manual methods and automatic techniques are both applied in order to provide a less computationally intensive mechanism which is operational in regional chemistry transport models (CTMs). The finally reduced mechanism contains less than 200 reactions (4 times smaller than the detailed CAPRAM 3.0i) and describes the main characteristics of inorganic and organic aqueous phase processes occurring in tropospheric warm clouds. Most of the chemical reduction potential is realized in the CAPRAM 3.0i organic chemistry. The number of aqueous phase species decreases from 380 in the full mechanism to 130 in the final reduced version. The calculated percentage deviations between the full and reduced mechanism are on average below 5% for the most important organic and inorganic target compounds such as oxidants, inorganic and organic acids, carbonyls and alcohols. Comparisons of the required CPU times between the full and reduced mechanisms show reductions of approximately 40%. 2-D test simulations with the CTM MUSCAT were performed using prescribed meteorological conditions in order to examine the applicability of the reduced mechanism at regional scale. Simulations with the reduced CAPRAM 3.0i mechanism and a much less complex mechanism with only limited inorganic chemistry (INORG) were compared to evaluate the effects of more detailed chemistry. The model results show large differences in the level of oxidants and the inorganic and organic mass processing. Prospectively, the reduced mechanism represents the basis for studying aerosol cloud processing effects at regional scale with future CTMs and will allow more adequate interpretation of field data.

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Abbreviations

C2.4:

CAPRAM2.4: Inorganic chemistry mechanism + C1-C2 organic chemistry

C2.4cond:

Manually condensed CAPRAM2.4 mechanism

C2.4ISSA:

Automatically reduced CAPRAM2.4 mechanism (ISSA method)

C3.0:

Full CAPRAM mechanism: CAPRAM3.0i (C2.4 + C2-C5 organic chemistry)

C3.0cond:

C2.4cond + C2-C5 organic chemistry

C3.0ISSA:

C2.4ISSA + C2-C5 organic chemistry

C3.0condRED(Man):

Manually reduced version of C3.0cond

C3.0ISSARED(Man):

Manually reduced version of C3.0ISSA

C3.0ISSARED(Aut):

Automatically reduced version of C3.0

C3.0RED:

Final reduced mechanism

SPACCIM:

Spectral Aerosol Cloud Chemistry Interaction Model

MUSCAT model:

MUltiScale Chemistry Aerosol Transport Model

RTOL:

Relative integration error tolerance

ATOL:

Absolute integration error tolerance

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Authors and Affiliations

  1. Leibniz-Institut für Troposphärenforschung (IfT), Permoserstr. 15, 04318, Leipzig, Germany

    Laurent Deguillaume, Andreas Tilgner, Roland Schrödner, Ralf Wolke & Hartmut Herrmann

  2. Clermont Université, Université Blaise Pascal, OPGC, Laboratoire de Météorologie Physique, 63000, Clermont-Ferrand, France

    Laurent Deguillaume & Nadine Chaumerliac

  3. CNRS, UMR 6016, LaMP, 63177, Clermont-Ferrand, France

    Laurent Deguillaume & Nadine Chaumerliac

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  1. Laurent Deguillaume
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  2. Andreas Tilgner
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Correspondence to Hartmut Herrmann.

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Deguillaume, L., Tilgner, A., Schrödner, R. et al. Towards an operational aqueous phase chemistry mechanism for regional chemistry-transport models: CAPRAM-RED and its application to the COSMO-MUSCAT model. J Atmos Chem 64, 1–35 (2009). https://doi.org/10.1007/s10874-010-9168-8

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