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Physical Review

Theory of Stimulated Raman Effect. II

Y. Ron Shen

Published Jun 14, 1965• 36 citations
Publisher

Abstract

The theory of stimulated Raman scattering using the coupled-wave approach is extended to include the case of polar media, with and without inversion center. Mixed effects of parametric down-conversion and Raman emission may occur. The threshold of the stimulated Raman effect in these media should not be much higher than that in a nonpolar system. The mixed effects of parametric down-conversion and stimulated Raman emission are also considered in purely electronic systems. They may be observable if the Raman transitions have a narrow linewidth.

DOI
10.1103/physrev.138.a1741

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A simple description of the stimulated Raman emission of Stokes radiation, and of the induced absorption found by Stoicheff at the anti-Stokes frequency, is based on the semiclassical theory of radiation. This theory gives the well-known formulas for absorption and stimulated emission when carried to the first order in the time-dependent perturbation due to the interaction of the light beam with the molecules. If there are two light beams of frequencies ωL and ω, the second-order perturbation may be associated with stimulated emission at the Stokes frequency ω=ω−1=ωL—ωR and with induced absorption at the anti-Stokes frequency ω=ω1=ωL+ωR, where ωL is the laser frequency and ωR a Raman-active vibrational frequency; in both cases, there is a molecular transition to the excited vibrational state. The highly directional and very sharp anti-Stokes emission at ω1 arises from the conversion by molecules in intense beams at ωL and ω−1 of two ωL photons into an ω−1, ω1 pair. Like spontaneous emission from excited states, the production of this anti-Stokes radiation requires the full quantum theory of radiation for an adequate description. The emission of ω1 and the observed directional absorption of ω−1 due to the reverse conversion ω−1+ω1→2ωL are explained. The anti-Stokes emission is proportional to the Stokes intensity and to the square of that of the laser, and to the square of the molecular number density; its sharpness is due to the absence of a molecular transition. The generation of photon pairs ω−n+ωn, where ωn=ωL+nωR, can occur for all values of n, but it is most efficient for n=1, due to resonance in the appropriate molecular hyperpolarizability and to the intensity of the Stokes beam at ω−1.

The Journal of Chemical Physics•Jul 1, 1965•24 citations
The theory of stimulated Raman scattering using the coupled-wave approach is extended to include the case of polar media, with and without inversion center. Mixed effects of parametric down-conversion and Raman emission may occur. The threshold of the stimulated Raman effect in these media should not be much higher than that in a nonpolar system. The mixed effects of parametric down-conversion and stimulated Raman emission are also considered in purely electronic systems. They may be observable if the Raman transitions have a narrow linewidth.
Polarization effects in stimulated Raman and stimulated Rayleigh scattering and self focusing are investigated from the viewpoint of the scattering of polarized photons by molecules. Both stimulated vibrational Raman scattering in liquids and stimulated rotational Raman scattering in gases are considered, and it is demonstrated that the polarization changes and relative power thresholds for different laser polarizations should be somewhat different to those predicted in other theories. For example, the ellipticity eta 0 of the stimulated rotational Raman photons in the forward direction from Delta J=+or-2 transitions in gaseous symmetric top molecules is given in terms of the initial ellipticity eta 1 by sin 2 eta 0 = - 5 / 7 sin 2 eta 1 , whereas conventional theories predict that eta 0 and eta 1 are equal in magnitude and opposite in sign. Furthermore it is shown that deviations from this relation could provide a measure of the degree of optical orientation of the molecules.
Stimulated Raman scattering of linearly polarized light from degenerate and selectively populated atomic sublevels of potassium have been observed. The scattered radiation has a polarization perpendicular to that of the incident beam. Such transition can take place between substates of different or of the same atomic level. In the latter case, the frequencies of the incident and scattered beams are equal and the polarizations are perpendicular. The induced transitions are associated with parametric four-wave coupling possessing also characteristic polarization properties.
The semiclassical theory of spontaneous Raman scattering is reviewed. From the semiclassical theory we identify the parameters and dynamical variables involved in Raman scattering. A classical theory of stimulated Raman scattering is constructed. It is an extension of the theory of Shen and Bloembergen. We show that the system is a weakly coupled system. Because the driving term contains dynamical variables, the linewidth of the stimulated Stokes wave should be smaller than that of the spontaneous Stokes wave. Using Riemann's method, we obtain Kroll's solution rigorously, in a more general form. The steady-state limit is also derived rigorously. The conditions for the transient and steady-state gains are discussed. It is shown that for the transient case one may have an abrupt change of the Stokes gain versus incident laser power.
A simple description of the stimulated Raman emission of Stokes radiation, and of the induced absorption found by Stoicheff at the anti-Stokes frequency, is based on the semiclassical theory of radiation. This theory gives the well-known formulas for absorption and stimulated emission when carried to the first order in the time-dependent perturbation due to the interaction of the light beam with the molecules. If there are two light beams of frequencies ωL and ω, the second-order perturbation may be associated with stimulated emission at the Stokes frequency ω=ω−1=ωL—ωR and with induced absorption at the anti-Stokes frequency ω=ω1=ωL+ωR, where ωL is the laser frequency and ωR a Raman-active vibrational frequency; in both cases, there is a molecular transition to the excited vibrational state. The highly directional and very sharp anti-Stokes emission at ω1 arises from the conversion by molecules in intense beams at ωL and ω−1 of two ωL photons into an ω−1, ω1 pair. Like spontaneous emission from excited states, the production of this anti-Stokes radiation requires the full quantum theory of radiation for an adequate description. The emission of ω1 and the observed directional absorption of ω−1 due to the reverse conversion ω−1+ω1→2ωL are explained. The anti-Stokes emission is proportional to the Stokes intensity and to the square of that of the laser, and to the square of the molecular number density; its sharpness is due to the absence of a molecular transition. The generation of photon pairs ω−n+ωn, where ωn=ωL+nωR, can occur for all values of n, but it is most efficient for n=1, due to resonance in the appropriate molecular hyperpolarizability and to the intensity of the Stokes beam at ω−1.