Semiclassical Dynamics in Phase Space; Time-Dependent Self-Consistent Field Approximation

Abstract

Gaussian wavepackets in phase space, which are constructed to have the exact first and second moments with respect to the coordinates and momenta, are used to develop self-consistent equations of motion for the semiclassical time evolution of interacting anharmonic systems. The equations apply to pure as well as to mixed states and may, therefore, be particularly useful for molecular dynamics in condensed phases. Numerical calculations of Raman excitation profiles, using a Morse oscillator, demonstrate the accuracy of the present equations.