TY - JOUR
T1 - Dynamics simulations of atmospherically relevant molecular reactions
AU - Gerber, R. Benny
AU - Sebek, Jiri
PY - 2009/4
Y1 - 2009/4
N2 - This article offers an overview of the recent progress in theoretical modeling of molecular reactions of atmospheric interest. The review covers processes in isolated molecules, e.g. vibrational overtone-induced processes in HNO3 and H2SO4. Another focal topic is thermally, as well as overtone-induced processes of NOx, HNOx and other atmospherically relevant species in water clusters, the latter serving as models for water surfaces, aerosols and other water environments. Among the processes examined in water clusters are separations of NOx and HNOx into ion pairs in contact with water, and the reverse processes of anion/cation recombination to form neutral molecules. Physical insights into the mechanisms and properties of the processes, as extracted from theoretical simulations, are analysed. The methodology discussed in the review is mostly classical molecular dynamics simulations, using potentials directly from electronic structure methods. The merits and limitations of different electronic structure methods for the systems of interest are discussed. Limitations and open problems with regard to the classical dynamics approximation are also briefly examined. Concluding remarks are presented on the usefulness of classical dynamics with ab initio potentials for reactions of atmospheric chemistry. Possible directions for future progress are suggested.
AB - This article offers an overview of the recent progress in theoretical modeling of molecular reactions of atmospheric interest. The review covers processes in isolated molecules, e.g. vibrational overtone-induced processes in HNO3 and H2SO4. Another focal topic is thermally, as well as overtone-induced processes of NOx, HNOx and other atmospherically relevant species in water clusters, the latter serving as models for water surfaces, aerosols and other water environments. Among the processes examined in water clusters are separations of NOx and HNOx into ion pairs in contact with water, and the reverse processes of anion/cation recombination to form neutral molecules. Physical insights into the mechanisms and properties of the processes, as extracted from theoretical simulations, are analysed. The methodology discussed in the review is mostly classical molecular dynamics simulations, using potentials directly from electronic structure methods. The merits and limitations of different electronic structure methods for the systems of interest are discussed. Limitations and open problems with regard to the classical dynamics approximation are also briefly examined. Concluding remarks are presented on the usefulness of classical dynamics with ab initio potentials for reactions of atmospheric chemistry. Possible directions for future progress are suggested.
KW - Ab initio
KW - Ab initio molecular dynamics
KW - Atmospheric chemistry
KW - Hso
KW - Molecular dynamics
KW - No molecules
KW - Water clusters
UR - http://www.scopus.com/inward/record.url?scp=74949093834&partnerID=8YFLogxK
U2 - 10.1080/01442350903016684
DO - 10.1080/01442350903016684
M3 - ???researchoutput.researchoutputtypes.contributiontojournal.article???
AN - SCOPUS:74949093834
SN - 0144-235X
VL - 28
SP - 207
EP - 222
JO - International Reviews in Physical Chemistry
JF - International Reviews in Physical Chemistry
IS - 2
ER -