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Determination of rate constants for the uptake process involving SO2 and an aerosol particle. A quantum mechanics/molecular mechanics and quantum statistical investigation

Sloth Madsen, Marianne; Gross, Allan; Falsig, Hanne; Kongsted, Jacob LU ; Osted, Anders; Mikkelsen, Kurt V and Christiansen, Ove (2008) In Chemical Physics 348(1-3). p.21-30
Abstract
We present a combined quantum mechanics/molecular mechanics and quantum statistical investigation of the interactions between a Molecule (SO2) and an aerosol particle including rate constants for the uptake process. A coupled cluster/molecular mechanics method including explicit polarization is used along with a quantum statistical method for calculating sticking coefficients. The importance of the polarization of the classical subsystem (the aerosol particle), the size of the classical subsystem and the size of one-electron basis sets are studied. The interaction energy is divided into van der Waals, electrostatic and polarization contributions. Relevant binding sites for the evaluation of the sticking coefficient are identified. These... (More)
We present a combined quantum mechanics/molecular mechanics and quantum statistical investigation of the interactions between a Molecule (SO2) and an aerosol particle including rate constants for the uptake process. A coupled cluster/molecular mechanics method including explicit polarization is used along with a quantum statistical method for calculating sticking coefficients. The importance of the polarization of the classical subsystem (the aerosol particle), the size of the classical subsystem and the size of one-electron basis sets are studied. The interaction energy is divided into van der Waals, electrostatic and polarization contributions. Relevant binding sites for the evaluation of the sticking coefficient are identified. These are classified into three groups according to the strength of the molecule-aerosol particle interaction energy. The identification of binding sites provides relevant information used in the quantum statistical method and thereby knowledge of the magnitude of the sticking coefficients for the different binding sites along with the total rates for the uptake processes between the aerosol particle and the SO2 molecule. (Less)
Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
SO2, quantum mechanics/molecular mechanics, uptake coefficient
in
Chemical Physics
volume
348
issue
1-3
pages
21 - 30
publisher
Elsevier
external identifiers
  • wos:000256737200003
  • scopus:43849095967
ISSN
0301-0104
DOI
10.1016/j.chemphys.2008.02.008
language
English
LU publication?
yes
id
7f97c7d6-05cd-4534-aa96-0024d311a192 (old id 1191121)
date added to LUP
2008-09-08 11:35:26
date last changed
2017-01-01 06:19:19
@article{7f97c7d6-05cd-4534-aa96-0024d311a192,
  abstract     = {We present a combined quantum mechanics/molecular mechanics and quantum statistical investigation of the interactions between a Molecule (SO2) and an aerosol particle including rate constants for the uptake process. A coupled cluster/molecular mechanics method including explicit polarization is used along with a quantum statistical method for calculating sticking coefficients. The importance of the polarization of the classical subsystem (the aerosol particle), the size of the classical subsystem and the size of one-electron basis sets are studied. The interaction energy is divided into van der Waals, electrostatic and polarization contributions. Relevant binding sites for the evaluation of the sticking coefficient are identified. These are classified into three groups according to the strength of the molecule-aerosol particle interaction energy. The identification of binding sites provides relevant information used in the quantum statistical method and thereby knowledge of the magnitude of the sticking coefficients for the different binding sites along with the total rates for the uptake processes between the aerosol particle and the SO2 molecule.},
  author       = {Sloth Madsen, Marianne and Gross, Allan and Falsig, Hanne and Kongsted, Jacob and Osted, Anders and Mikkelsen, Kurt V and Christiansen, Ove},
  issn         = {0301-0104},
  keyword      = {SO2,quantum mechanics/molecular mechanics,uptake coefficient},
  language     = {eng},
  number       = {1-3},
  pages        = {21--30},
  publisher    = {Elsevier},
  series       = {Chemical Physics},
  title        = {Determination of rate constants for the uptake process involving SO2 and an aerosol particle. A quantum mechanics/molecular mechanics and quantum statistical investigation},
  url          = {http://dx.doi.org/10.1016/j.chemphys.2008.02.008},
  volume       = {348},
  year         = {2008},
}