Molecular coherence effects in stimulated raman scattering

Abstract

A semi-classical calculation of the three-level system consisting of the ground state, the vibrationally excited state and the electronic excited state under the laser and the Stokes perturbation is given. The induced molecular polarization produces gain modulation of the Stokes and loss modulation of the laser at a frequency that is dependent on the optical intensity. With the optical intensity in self-trapped filaments in nonlinear liquids such as CS₂, the period of modulation becomes of the order 10⁻¹¹ s and a large amplitude modulation of the laser and the Stokes waves will result.

The amplitude modulation is not much reduced, if the molecular relaxation time of the order 10⁻¹¹ s is taken into account. Effects of non-uniform field distribution and the width and shape of the incident laser pulse are discussed. The frequency broadening caused by the three-level effect is shown to be larger than, or at least as large as, the broadening caused by the optical Kerr effect.