ISSN 1017-2548(Print)
ISSN 2234-8530(Online)
Volume 20, Number 2
JKCSEZ 20(2)
April 20, 1976 

Effects of direct multiple quantum excitations in vibrational energy transfer were investigated. Vibrational transition probabilities for 0→2, 0→3, and 0→4 excitations were explicitly formulated including both direct 0→n excitations and stepwise single quantum processes. For the formulation the perturbing force was derived from the exponential potential including terms up to fourth order in the vibrational amplitude. The head-on collinear collision model between a harmonic oscillator and an incident particle was employed, and the formulation was based on the semiclassical approximation. Numerical results were obtained for five different collision systems (Ar…O-N, He…H-H, He…H-Cl, 5…1-2, 2…12-12). Comparison between the present results and those obtained using the linearized interaction potential showed that the overall effect of including the direct multiple quantum transition is to decrease the probabilities at low collision energies and to increase them at high energies. The present results were found to be significantly different from those obtained using the linearized potential for collision systems He…H-H, He…H-Cl, and 5…1-2. For systems Ar…O-N and 2…12-12 the differences were negligible.