MODEL-CALCULATIONS OF RESONANT VIBRATION TO VIBRATION TRANSITION-PROBABILITIES IN CLUSTERS

Authors
Citation
Mf. Herman, MODEL-CALCULATIONS OF RESONANT VIBRATION TO VIBRATION TRANSITION-PROBABILITIES IN CLUSTERS, The Journal of chemical physics, 109(12), 1998, pp. 4726-4733
Citations number
24
Categorie Soggetti
Physics, Atomic, Molecular & Chemical
ISSN journal
00219606
Volume
109
Issue
12
Year of publication
1998
Pages
4726 - 4733
Database
ISI
SICI code
0021-9606(1998)109:12<4726:MORVTV>2.0.ZU;2-Q
Abstract
Results are presented for the calculated probability for resonant tran sfer of vibrational excitation energy in clusters of identical molecul es. The calculations are performed for two-dimensional clusters in ord er to allow for calculations on larger clusters. Clusters of 5, 10, an d 20 molecules are considered. The probability of resonant transfer is calculated by quantum mechanically propagating the wave function for the vibrational degrees of freedom of the molecules in the cluster, wh ile the rotational and translational degrees of freedom evolve along c lassical trajectories. The transition probabilities are averaged over a canonical distribution of initial phase space points for the traject ories. If the probability for the transition of a vibrational quantum of energy from one molecule to some other molecule in an N molecule cl uster is evaluated as N-1 independent two molecule vibrational problem s, the results are found to be in excellent agreement with those obtai ned from the propagation of the full N molecule vibrational problem. T he results also show that quantum coherence effects result in an early time nonlinear behavior in the transition probabilities that persists for several picoseconds in these systems. (C) 1998 American Institute of Physics.