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

We present a new numerical scheme to compute femtosecond quantum molecular dynamics involving several strongly coupled degrees of freedom. This method is based on a combination of contracted grid basis eigenstate calculations with time-dependent propagation under coherent infrared multiphoton excitation with transformation to the quasi-resonant basis. Using data from our previous high-resolution spectroscopic investigation of CHD2F, we present quantum wavepacket results for the CH-chromophore dynamics, including coherent time evolution of CH stretching excitation in terms of explicit probability densities for the corresponding normal coordinate, relaxation towards approximate, partial quasi-equilibrium on the 100 fs time scale and a discussion of symmetry under time reversal in the ps time range.