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Chemical Physics

Theory of time- and frequency-resolved resonance Raman and resonance fluorescence induced by realistic coherent pulses of arbitrary strength

A D Wilson, Harry Friedmann

Published Jul 1, 1977• 20 citations
Publisher
DOI
10.1016/0301-0104(77)89048-4

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Soviet Journal of Quantum Electronics•Jan 31, 1984•1 citation
Based on the time-dependent theory, an analysis of the distinction between resonance Raman (RR) and resonance fluorescence (RF) with pulse excitation was presented. The real population of the intermediate state gives two optical components-the independent time evolution of intermediate ket and bra states generates RR while RF originates from the phase coherent between ket and bra states. In cw limit, the transition probability of spontaneous emission with pulse excitation can be reduced to the classical theory.
Light scattering by isolated small and intermediate-size molecules is studied theoretically. A quantum-mechanical model is developed that treats the molecule and the radiation field on equal terms and allows a nonperturbative solution for arbitrary wave forms and field strengths. The molecular states are described in terms of a basis set of zeroth-order states chosen so as to minimize the number of excited molecular states in the laser frequency range that combines radiatively with the initial (ground) state, i.e., that act as doorways for the field. Detailed calculations are restricted to the case of a single doorway. Closed-form expressions are obtained for the frequency-resolved scattering rates and time-resolved scattering spectra, including fluorescence and Rayleigh–Raman components, for a variety of conditions, including δ(t) excitation, excitation by a Lorentzian light pulse, by a coherent train of pulses and stationary excitation. The case of nonlinear scattering by very intense pulses is also investigated. Model calculations are reported for systems of 1–3 molecular levels. It is found that in general phase relations are maintained so that the coherence survives as long as the signal.
The approximation of nonoverlapping lines is used to calculate spectra of resonance fluorescence and Raman scattering when two- and three-level atoms are pumped by a smooth pulse of duration comparable with the excited-state lifetime. The difference between the quasienergy terms, that determines the satellite frequency, depends on time and has the same value twice, at the pulse leading and trailing edges, so that interference may occur between the radiation produced in the appropriate parts of the pulse. However, the interference pattern is blurred since radiative broadening destroys the coherence. Relationships are obtained between the parameters for which interference may be observed. An analysis is made of the change to short pulses when allowance can be made for the scattered field using the first order of perturbation theory.