Chemical Physics Letters, Vol.420, No.4-6, 296-303, 2006
Semiclassical IVR approach to rotational excitation of non-polar diatomic molecules by non-resonant laser pulses
We apply the 'classic' semiclassical initial value representation (SC-IVR) approach to describe rotational excitation of non-polar diatomic molecules by intense short non-resonant laser pulses. We also investigate the applicability of the quantum mechanical sudden approximation. It is found that the SC-IVR approach gives accurate rotational excitation probabilities in regimes where the sudden approximation fails. Primitive semiclassical wavefunction propagation is used to illustrate the phenomenon of angular focussing of rotation states by strong pulses. (c) 2006 Elsevier B.V. All rights reserved.