Journal of Chemical Physics, Vol.110, No.3, 1711-1725, 1999
Semiclassical simulations of multidimensional Raman echoes
A high-temperature and a weak-nonlinearity (low-temperature) semiclassical expansion are developed for computing two-dimensional vibrational Raman spectroscopies, and applied to an exactly solvable Brownian-oscillator model. The origin of photon echoes is discussed using phase-space-wave-packets. Impulsive and semi-impulsive echoes are shown to satisfy different phase-matching conditions, and are generated in different directions.
Keywords:CLASSICAL S-MATRIX;5TH-ORDER NONLINEAR SPECTROSCOPY;TIME-RESOLVED 4-WAVE;VIBRATIONAL SPECTROSCOPY;LIQUID CS2;CONDENSED-PHASE;PATH APPROACH;5TH ORDER;DYNAMICS;MODES