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Journal of Quantitative Spectroscopy and Radiative Transfer

Resonance fluorescence and Raman line shapes produced by monochromatic laser fields: Effects of branching ratio and homogeneous broadening

Frederick H. Mies

Published Mar 1, 1983• 6 citations
Publisher
DOI
10.1016/0022-4073(83)90042-0

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Journal of Raman Spectroscopy•Dec 1, 1975•3 citations
A method is introduced to calculate for a model set of molecular levels the spectral line shapes expected for a variety of conventional laser experiments including absorption, hole burning, fluorescence line narrowing, and Raman scattering. The method allows the incident laser field to have arbitrary intensity. Furthermore, the effects of model Gaussian or Lorenzian inhomogeneous distributions are readily incorporated. Earlier results for a two-level system are easily obtained and new results are presented for inhomogeneously broadened two and three level systems, and for the effects of pure dephasing on the strong field spectra. In particular we have described the differences between fluorescence and Raman in strong fields, and the effect of strong fields on the spontaneous emission of inhomogeneously broadened transitions. Some predictions are made regarding line narrowing experiments in the strong-field limit.
The resonant Raman scattering in a three level system produces an optical pumping of molecules from the initial to the final states which are radiatively coupled to the intermediate resonant state. We consider the pumping that is produced by an intense, pulsed, monochromatic radiation field that is near-resonant with the initial resonance frequency. The Heitler–Ma damping theory is solved exactly for the case when the resonance fluorescence is weak compared to the Raman scattering, or any other processes which might cause irreversible decay of the resonant state. In particular, we examine the usefulness of dressed states to describe the intense field limit. The spectral line shape for the Raman scattering is obtained. The transient behavior following the onset of the laser pulse is examined and a careful analysis of the pumping rate and its relationship to both weak and strong field theories is presented.
Abstract Presupposing exponentially decaying states (with phenomenological lifetimes) of the particle system interacting with the radiation field, the shape and width of Raman lines is discussed on a quantum‐mechanical basis for the most important types of excitation: non‐resonance, pre‐resonance, rigorous resonance with a continuum level and with a discrete, non‐degenerate, and isolated level; monochromatic and non‐monochromatic irradiation. Attention is called to peculiar intensity distributions of the secondary radiation obtainable by sufficiently monochromatic excitation in near resonance to an isolated state (resonance fluorescence case) which deviate characteristically from those customary in traditional fluorescence and scattering spectra.