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Physical Review A

Comment on "Resonant fluorescence and Raman scattering"

Stephen E. Schwartz

Published Mar 1, 1975• 14 citations
Publisher

Abstract

The uncertainty-principle implications of the recent study of Williams, Rousseau, and Dworetsky are considered. The incompatible requirements of excitation pulse duration and bandwidth rule out a test of their proposed relation between excitation frequency and scattering time in the transition from resonance fluorescence to Raman scattering.

DOI
10.1103/physreva.11.1121

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Chinese Physics Letters•Apr 1, 2000•0 citations
The uncertainty-principle implications of the recent study of Williams, Rousseau, and Dworetsky are considered. The incompatible requirements of excitation pulse duration and bandwidth rule out a test of their proposed relation between excitation frequency and scattering time in the transition from resonance fluorescence to Raman scattering.
Pulses of laser light which undergo Raman scattering by a molecule at a resonance are observed to consist of two components: a short pulse which lasts as long as the driving pulse, and a long tail which falls off with the lifetime of the excited state. It is shown that the recent observations of Williams, Rousseau, and Dworetsky on I2{\mathrm{I}}_{2}I2​ can be fitted by theory; one has to suppose that the frequency spectrum of the driving pulses is broadened to an extent equivalent to a reduction of the stated rise and fall times by a factor of 10.
Abstract If and only if spontaneous resonance Raman scattering is excited by irradiation upon a single, discrete and non‐degenerate energy level sufficiently distant from other levels can it be interpreted as resonance fiuorescence, i.e. a sequence of two independent one‐photon processes, an absorption and an emission in definte order of succession. This decomposition of the resonance scattering process is independent of the bandwidth of the exciting radiation relative to the widths of the combining levels. These widths however determine quantitatively the temporal decay of the resonance scattering (= resonance fluorescence) probability given explicitly in the paper.
1^{1}1A. Corney and G. w. Series, Proc. Phys. Soc. 83, 207 (1964) 2^{2}2P, Schenck, R. C. Hilborn, and H. Metcalf, Phys. Rev. Letters 31, 189 (1973) 3^{3}3P. F. Williams, D. L. Rousseau, and S. H. Dworetsky, Phys. Rev. Letters 32, 196 (1974)
The theory of resonance Raman effect, resonantly enhanced two-photon absorption, and resonance fluorescence---valid also for strong fields---is treated in a unified and simplified way. Dressed states, Bloch equations, and perturbation theory are used to calculate line positions, and integrated intensities both for steady state and transient excitation. The case of adiabatic following is solved explicitly; it occurs when an off-resonance incident pulse is turned on and off slowly. It leads to the identification of Raman scattering, two-photon absorption, and Rayleigh scattering with an adiabatic process while fluorescence and consecutive two-photon absorption with nonadiabaticity. Time-dependent spectra are defined in a rigorous way. Our formulas agree in the various limits with those that appear in the literature.
An examination of the foreign-gas pressure dependence of the intensity and spectrum of the signal from I2{\mathrm{I}}_{2}I2​ vapor under off-resonance monochromatic excitation indicates that the re-emission process is not resonance Raman scattering as recently reported by Fouche and Chang.
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.