Budget Amount *help 
¥1,900,000 (Direct Cost : ¥1,900,000)
Fiscal Year 1997 : ¥200,000 (Direct Cost : ¥200,000)
Fiscal Year 1996 : ¥1,700,000 (Direct Cost : ¥1,700,000)

Research Abstract 
In this Scientific Research Program (C), notifying arbitrary nonlinearity of the solutesolvent interaction in the hamiltonian for chemical reacting systems in condensed phase, the final research purposes were to formulate the reaction rate for the charge transfer reactions and to compare the numerical results with the experimental ones. In the term of project, in order to estimate the vibrational nonadiabaticity in the classicalquantum coupled systems, we proposed a new quantization method based on an equation of motion and have executed numerical treatment for the concentration and dissipative transfer of the reactive energy due to nonequilibrium induced by the vibrational nonadiabaticity in the present systems. 1. A dividing surface is newly proposed in a manybody phase space, over which the system trajectories do not recross if the saddle crossing motions are regarded as quasiperiodic. The recrossing dynamics of a four degreesoffreedom Hamiltonian, a model of proton transfer reac
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tion of malonaldehyde, is investigated. It is shown that the apparent barrier recrossing motions observed over a naive dividing surface in the configurational space are 'rotated away' by a nonlinear canonical transformation, to noreturn single crossing motions over the new dividing surface defined in the phase space. 2. A stochastic Pathintegral (SPI) technique is explored. It is shown that this technique enables the direct computation of the transition amplitude with a finite spacetime range, by generating a set of classical paths subject to simultaneous stochastic differential equations.The numerical values of the Boltzmann matrix elements for a harmonic potential are in good agreement with the analytical ones. Within the quantum TS theory, the fluxflux autocorrelation function is also evaluated at 630K for the H+H_2 exchange reaction and is found to give a satisfactory agreement with the previous studies. To appraise the influence of the dimensionality, both 1dimensional Eckart potential and a full 3D LSTH potential calculations have been perfomed. The calculated values of the Boltzmann matrix elements for the collinear and the full 3D cases are found to deviate slightly each other in the lower temperature range. The 3D thermal rate constant becomes in very good agreement with the previous one. Less
