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Physical Review Letters

Resonant Raman Scattering or Resonance Fluorescence in I2 Vapor?

R. L. St. Peters, Seth D. Silverstein, M. Lapp, Carl M. Penney

Published Feb 5, 1973• 37 citations
Publisher

Abstract

An examination of the foreign-gas pressure dependence of the intensity and spectrum of the signal from ${\mathrm{I}}_{2}$ vapor under off-resonance monochromatic excitation indicates that the re-emission process is not resonance Raman scattering as recently reported by Fouche and Chang.

DOI
10.1103/physrevlett.30.191

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•Jan 26, 2020•0 citations
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.
We demonstrate that at all pressures, the resonant scattering emission in I2{\mathrm{I}}_{2}I2​ vapor as excited by a 501.7-nm Ar-ion laser line is dominated by the combined effects of discrete-state resonant fluorescence and dissociative-state continuum resonant Raman scattering (RRS). The changes in the emission upon increased pressures, such as relative and absolute intensities of Stokes overtones, and the variation in depolarization ratios are demonstrated to be due to the gradual quenching of the resonance fluorescence at high pressure, while the dissociative-state RRS contribution remains unaltered.
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.