Lifetimes for resonance fluorescence and near resonance Raman scattering

Abstract

In this paper we present a quantum mechanical treatment of time resolved resonant and near resonant light scattering from a molecular system. The time resolved decay pattern is characterized by just two types of lifetimes, those specifying the molecular system and those characterizing the light pulse, while the off resonance energy parameter affects the total intensity and, in some cases, the relative intensities of the different decay components. The theoretical results for the ’’isolated’’ molecule are confronted with the recent experimental data of Williams, Rousseau, and Dworetzky [Phys. Rev. Lett. 32, 196 (1974)] for resonance and near resonance photon scattering from I₂. Finally, we present a general scheme for handling photon scattering from a multilevel molecular system.