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THEORY OF THE TIME-DEPENDENCE OF NEAR-RESONANT RAMAN SCATTERING

Robert C. Hilborn

Published Jan 1, 1974• 0 citations
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Abstract

$^{1}$A. Corney and G. w. Series, Proc. Phys. Soc. 83, 207 (1964) $^{2}$P, Schenck, R. C. Hilborn, and H. Metcalf, Phys. Rev. Letters 31, 189 (1973) $^{3}$P. F. Williams, D. L. Rousseau, and S. H. Dworetsky, Phys. Rev. Letters 32, 196 (1974)

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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)
1^{1}1 G. Placzek, Handbuch der Radiologie, ed. by E. Marx (Academische Verlag., Leipzig, 1934) Vol. VI, Part 2, pp. 205. 2^{2}2 C. H. Ting, the following paper. 3^{3}3 H A. Kramers and W.C. Heisenberg, Z. Physik 31, 681 (1925).
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.
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.