Photodissociation of HF in ArnHF (n=1-14,54) van der Waals clusters: Effects of the solvent cluster size on the solute fragmentation dynamics

Thomas Schröder, Reinhard Schinke, Suyan Liu, Zlatko Bacic, Jules W. Moskowitz

Research output: Contribution to journalArticle

Abstract

A comprehensive study of the photodissociation of HF in ArnHF van der Waals clusters, with n=1-14,54, for an ultrashort δ(t)-pulse excitation, is presented. The emphasis is on the dependence of the photodissociation dynamics of the HF solute molecule on the size and geometry of the Arn solvent cluster. This cluster size range encompasses formation and closing of the first solvation shell, which occurs for n=12, the addition of the complete second solvent layer (n=54), as well as the change of the HF location in the cluster, from a surface site for n≤8 to the interior of a cage for n≥9 clusters. Evolution of the fragmentation dynamics is revealed by following how the H-atom kinetic energy and angular distributions, the survival probability, and cluster fragmentation patterns change as a function of the cluster size and structure. Classical trajectories are used to simulate the photodissociation dynamics. The probability distributions of the initial coordinates and momenta of the H and F atom are defined by accurate quantum five-dimensional eigenstates of the coupled, very anharmonic large amplitude intermolecular vibrations of HF in the cluster. All aspects of the dissociation process studied here are found to exhibit a strong dependence on the size and geometry of the ArnHF clusters.

Original languageEnglish (US)
Pages (from-to)9228-9241
Number of pages14
JournalThe Journal of chemical physics
Volume103
Issue number21
StatePublished - 1995

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Photodissociation
photodissociation
solutes
fragmentation
Atoms
Geometry
Angular distribution
Solvation
Ultrashort pulses
Kinetic energy
Probability distributions
Momentum
Trajectories
Molecules
closing
geometry
solvation
atoms
energy distribution
eigenvectors

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

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Photodissociation of HF in ArnHF (n=1-14,54) van der Waals clusters : Effects of the solvent cluster size on the solute fragmentation dynamics. / Schröder, Thomas; Schinke, Reinhard; Liu, Suyan; Bacic, Zlatko; Moskowitz, Jules W.

In: The Journal of chemical physics, Vol. 103, No. 21, 1995, p. 9228-9241.

Research output: Contribution to journalArticle

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