FEMTOSECOND QUANTUM STRUCTURE, EQUILIBRATION AND TIME-REVERSAL FOR THE CH-CHROMOPHORE DYNAMICS IN CHD2F

We present a new numerical scheme to compute femtosecond quantum molec ular dynamics involving several strongly coupled degrees of freedom. T his method is based on a combination of contracted grid basis eigensta te calculations with time-dependent propagation under coherent infrare d multiphoton excitation with transformation to the quasi-resonant bas is. Using data from our previous high-resolution spectroscopic investi gation of CHD2F, we present quantum wavepacket results for the CH-chro mophore dynamics, including coherent time evolution of CH stretching e xcitation in terms of explicit probability densities for the correspon ding normal coordinate, relaxation towards approximate, partial quasi- equilibrium on the 100 fs time scale and a discussion of symmetry unde r time reversal in the ps time range.