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Physical Review A

Rotationally invariant theory of stimulated Raman scattering

Richard B. Holmes, Allen M. Flusberg

Published Mar 1, 1988• 33 citations
Publisher

Abstract

We present a detailed derivation of a new, rotationally invariant formalism for the theory of stimulated Raman scattering. The formalism is applied to Raman transitions of well-defined rotational symmetry, e.g., rotational Raman (S) transitions, yielding the explicit dependence of gain on light polarization, phase mismatch, and frequency offset. For a linearly polarized laser, the Stokes fields parallel and perpendicular to the laser field are decoupled. Far from Stokes--anti-Stokes phase matching, their gain coefficients are in the ratio of 4:3; at phase matching, both are suppressed and have zero exponential gain. For a circularly polarized laser, the circularly polarized Stokes fields circulating in the same and opposite senses as the laser field are decoupled. The gain of the opposite-sense field, which is decoupled from the anti-Stokes field, is independent of phase mismatch. Far from phase matching, the gain of the same-sense Stokes field is (1/6 that of the opposite-sense field; at phase matching, the same-sense field has zero exponential gain. An unpolarized laser is shown to have the lowest Raman gain; far from phase matching, its Stokes fields decouple into two incoherent, oppositely circularly polarized fields, but at phase matching all Stokes polarizations have zero exponential gain. The gradual transition away from phase matching is also treated explicitly, and it is shown that when the gain is suppressed the maximum Stokes growth occurs when the Stokes-laser beat is a fraction of a Raman linewidth off resonance.

DOI
10.1103/physreva.37.1588

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Physical Review A•Oct 1, 1981•358 citations
We present a detailed derivation of a new, rotationally invariant formalism for the theory of stimulated Raman scattering. The formalism is applied to Raman transitions of well-defined rotational symmetry, e.g., rotational Raman (S) transitions, yielding the explicit dependence of gain on light polarization, phase mismatch, and frequency offset. For a linearly polarized laser, the Stokes fields parallel and perpendicular to the laser field are decoupled. Far from Stokes--anti-Stokes phase matching, their gain coefficients are in the ratio of 4:3; at phase matching, both are suppressed and have zero exponential gain. For a circularly polarized laser, the circularly polarized Stokes fields circulating in the same and opposite senses as the laser field are decoupled. The gain of the opposite-sense field, which is decoupled from the anti-Stokes field, is independent of phase mismatch. Far from phase matching, the gain of the same-sense Stokes field is (1/6 that of the opposite-sense field; at phase matching, the same-sense field has zero exponential gain. An unpolarized laser is shown to have the lowest Raman gain; far from phase matching, its Stokes fields decouple into two incoherent, oppositely circularly polarized fields, but at phase matching all Stokes polarizations have zero exponential gain. The gradual transition away from phase matching is also treated explicitly, and it is shown that when the gain is suppressed the maximum Stokes growth occurs when the Stokes-laser beat is a fraction of a Raman linewidth off resonance.
The authors have extended the theory of stimulated Raman scattering to include the effects of laser bandwidths, in both the transient and steady-state regimes. The case of two interacting laser beams, a pump laser and a probe (Stokes) laser, is treated. Using the phase-diffusion model for laser bandwidth, the authors demonstrate that in the absence of dispersion, the forward Raman gain is essentially independent of the laser bandwidths in the high-gain limit, while in the low-gain limit the gain coefficient is inversely proportional to the sum of the bandwidths. It is further shown that when the pump-laser bandwidth is much larger than the linewidth of the Raman medium, the stimulated Stokes output assumes the same spectrum as the pump laser in the high-gain limit. A possible interpretation of these results is discussed assuming a "phase-locking" of the Stokes phase to the fluctuations in the pump-laser phase, due to the nonlinear interaction of the two beams through the Raman medium.
A theory of nonstationary stimulated Raman scattering is developed, allowing for the coupling between the Stokes and anti-Stokes waves. The main equations are solved in the asymptotic approximation, which is valid for large values of the gain. The dependences of the gain on the phase mismatch Δ k , pulse duration τ p , and cell length l are discussed and the optimal angle for the observation of the anti-Stokes rings is calculated. Moreover, the spectral distributions of the Stokes and anti-Stokes waves are considered.
A theoretical study of the polarization dependence of stimulated Rayleigh-wing scattering and the optical-frequency Kerr effect has been undertaken. When the incident light is circularly polarized, a striking difference in gain is found for the co- and counter-rotating senses of polarization of the scattered light---the former being suppressed and the latter being exceptionally favored. The analysis begins with a model for the Kerr effect, which involves the alignment of anisotropic molecules in an electric field, but the results can be immediately generalized to any light scattering process of tensor symmetry. The nonlinear problem of the propagation of an intense elliptically polarized light wave in a Kerr-active medium is shown to have a solution in which the vibrational ellipse undergoes self-precession and self-retardation. The stimulated scatterings or instabilities of such a self-precessing and self-retarding light wave are obtained for the backward and forward directions. Birefringence, optical activity, and linear and circular dichroisms are some of the phenomena which result, but the forward direction yields substantially different results from the backward direction because of Stokes-anti-Stokes coupling.
A theory of stimulated Raman scattering (SRS) is presented which treats in a unified manner the buildup of SRS from spontaneous Raman scattering and the spatial propagation which leads to gain. Maxwell-Bloch equations describe the coupling between the Stokes field operator and the collective atomic operators, which are driven by a classical laser field under low-signal-gain conditions, where the atomic ground states and laser field remain undepleted. An analytic expression is derived for the forward-propagating Stokes field operator in a one-dimensional spatial approximation when the Fresnel number of the excited medium is unity. Steady-state and transient Stokes intensities are evaluated under low-gain (spontaneous) and high-gain (stimulated) conditions. The Stokes intensity is found to be exactly independent of a laser bandwidth arising solely from phase fluctuations. The power spectrum of steady-state SRS is evaluated, giving a gain-narrowed spectral profile when the laser is narrow band, and a spectrum identical to the laser spectrum when the laser is broad band. A strong analogy between SRS and two-level superfluorescence is found; in both cases the macroscopic, collective dipole moment is initiated by quantum fluctuations.