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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

Degauillaume, L.; Tilgner, Andreas; Schrödner, Roland LU ; Wolke, Ralf; Chaumerliac, Nadine and Herrmann, H. (2009) In Journal of Atmospheric Chemistry 64(1). p.1-35
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... (More)
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. (Less)
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author
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Multiphase cloud chemistry, CAPRAM, Mechanism reduction, Regional modeling, MUSCAT
in
Journal of Atmospheric Chemistry
volume
64
issue
1
pages
1 - 35
publisher
Springer
external identifiers
  • scopus:78649323235
ISSN
0167-7764
DOI
10.1007/s10874-010-9168-8
language
English
LU publication?
no
id
c63296f2-1549-48c9-b8ae-79496189c4ed
date added to LUP
2017-07-05 15:34:43
date last changed
2017-09-17 09:50:30
@article{c63296f2-1549-48c9-b8ae-79496189c4ed,
  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.},
  author       = {Degauillaume, L. and Tilgner, Andreas and Schrödner, Roland and Wolke, Ralf and Chaumerliac, Nadine and Herrmann, H.},
  issn         = {0167-7764},
  keyword      = {Multiphase cloud chemistry,CAPRAM,Mechanism reduction,Regional modeling,MUSCAT},
  language     = {eng},
  number       = {1},
  pages        = {1--35},
  publisher    = {Springer},
  series       = {Journal of Atmospheric Chemistry},
  title        = {Towards an operational aqueous phase chemistry mechanism for regional chemistry-transport models: CAPRAM-RED and its application to the COSMO-MUSCAT model},
  url          = {http://dx.doi.org/10.1007/s10874-010-9168-8},
  volume       = {64},
  year         = {2009},
}