Pulse shaping and coherent Raman spectroscopy in condensed phases

Abstract

A microscopic theory for ultrafast coherent Raman spectroscopy of polyatomic molecules in condensed phases is developed. For off resonant excitation, an effective Hamiltonian that controls the molecular dynamics in a Raman process is derived. The limitations of the driven oscillator model are clarified, and generalized equations of motion, which hold for resonant and off resonant excitation, are derived. Spectral selectivity using pulse shaping is discussed.