title: Formation of Carbonic Acid in Impact of CO2 on Ice and Water.
abstract: A new mode of formation is proposed for carbonic acid in the atmosphere. It involves impact of vibrationally excited gas-phase CO2 molecules on water or ice particles. This is a first mechanism that supports formation on ice as well as on liquid water surfaces. Results of ab initio molecular dynamics simulations are presented on collisions of CO2 with (H2O)n clusters (n = 1, 4, 8, 12). Efficient formation of carbonic acid is seen with product lifetimes exceeding 100 ps. The reaction is feasible even for collision of CO2 with a single water molecule but in a different mechanism than for larger clusters. For clusters, the transition state shows charge separation into H3O(+)···HCO3(-), which transforms into neutral carbonic acid as the product, hydrated by the remaining waters. Possible atmospheric implications of the results are discussed.
authors.affiliation: Institute of Chemistry and the Fritz-Haber center for Molecular Dynamics, The Hebrew University , Jerusalem 9190401, Israel.
authors.forename: Barak
authors.initials: B
authors.lastname: Hirshberg
authors.affiliation: Institute of Chemistry and the Fritz-Haber center for Molecular Dynamics, The Hebrew University , Jerusalem 9190401, Israel.|Department of Chemistry, University of California , Irvine, California 92697, United States.
authors.forename: R Benny
authors.initials: RB
authors.lastname: Gerber