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Physical Review A

Soliton dynamics, anti-Stokes generation, and diffraction in stimulated Raman scattering

Michael Scalora, C. M. Bowden, Joseph W. Haus

Published Nov 1, 1993• 2 citations
Publisher

Abstract

We have studied the diffractive coupling of Stokes, anti-Stokes, and pump fields in stimulated Raman scattering. We find that, depending on the strength of the anti-Stokes field relative to that of the Stokes, both soliton dynamics and beam-pointing fluctuations are affected for finite Fresnel numbers. The generation of the anti-Stokes waves can inhibit a gain-focusing mechanism that we predicted for the Stokes field, when a soliton propagates in the medium. Although no qualitative differences arise in the beam-pointing fluctuations of the Stokes field, we predict that the anti-Stokes beam may be much more stable than the Stokes counterpart. Our analysis shows that for a Fresnel number of 5, the difference can be as large as 70%, while for Fresnel numbers of order unity, it is nearly 10%.

DOI
10.1103/physreva.48.3916

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We have studied the diffractive coupling of Stokes, anti-Stokes, and pump fields in stimulated Raman scattering. We find that, depending on the strength of the anti-Stokes field relative to that of the Stokes, both soliton dynamics and beam-pointing fluctuations are affected for finite Fresnel numbers. The generation of the anti-Stokes waves can inhibit a gain-focusing mechanism that we predicted for the Stokes field, when a soliton propagates in the medium. Although no qualitative differences arise in the beam-pointing fluctuations of the Stokes field, we predict that the anti-Stokes beam may be much more stable than the Stokes counterpart. Our analysis shows that for a Fresnel number of 5, the difference can be as large as 70%, while for Fresnel numbers of order unity, it is nearly 10%.
We have observed fluctuations in the direction of propagation of light pulses generated by stimulated Raman scattering (SRS). This fluctuation is analogous to the pointing fluctuation of laser beams,1 and is due to quantum mechanical uncertainties in the occupation numbers of different spatial modes. When SRS is generated in an interaction region with Fresnel number less than unity, the lowest order spatial mode dominates the generation process, but higher order spatial modes are also weakly and randomly excited. This results in small fluctuations in the wavefront of the light field. The direction of propagation is characterized by the transverse component of an average wave-vector determined by the gradient of the wave-front. We report experimental results by measuring the "center of mass" of the far-field intensity pattern of a single Stokes beam, and the fringe separation of an interference pattern formed by superposing two independently generated Stokes pulses. The experimental results are compared to theory.2
The far field direction of propagation of light pulses generated by transient, single pass stimulated Raman scattering (SRS) is observed to fluctuate front pulse to pulse due to quantum mechanical uncertainties in the occupation numbers of different coherent spatial modes. When SRS is generated on the Q(l) vibrational transition in hydrogen with an interaction region Fresnel number near unity, the lowest-order coherent spatial mode dominates the generation process, leading to near-diffraction-limited Stokes light.
A three-dimensional analysis of stimulated Raman emission is presented for a medium through which a cylindrical laser beam passes. The buildup of the Stokes radiation from the spontaneous fluctuations in the Raman medium is considered. A generalization of the fluctuation-dissipation theorem is derived relating the current-current fluctuations at the Stokes frequency to the laser-induced (negative) conductance at this frequency. The anti-Stokes radiation is treated as arising from the interaction of the laser field and the molecular vibrations accompanying the Stokes radiation. The anti-Stokes radiation emerges in a narrow cone around the familiar phase-matching direction given by ${\mathbf{\ensuremath{\beta}}}_{\ensuremath{-}}=2{\mathbf{k}}_{L}\ensuremath{-}{\mathbf{\ensuremath{\beta}}}_{+}$, where ${\mathbf{\ensuremath{\beta}}}_{\ensuremath{-}}$ and ${\mathbf{\ensuremath{\beta}}}_{+}$ are the (real parts of the) propagation constants of Stokes and anti-Stokes waves in the medium, and kL{\mathbf{k}}_{L}kL​ is the laser propagation vector. The angular width of the anti-Stokes radiation cone is evaluated.
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.
In the coherent anti-Stokes Raman scattering process, the spectrum of the generated optical phonon depends on the degree of temporal correlation between the pump laser field and the Stokes field. When the two fields are strongly correlated, such as when the Stokes field is generated with stimulated Raman scattering (SRS), the spectral shape of the optical phonon is found experimentally and theoretically to be the same as the gain-narrowed Raman line shape because the laser phase fluctuations cancel out totally, leaving only the collisional noise in the SRS process. When the two fields are uncorrelated, the shape of the optical-phonon spectrum is found to be the same as the Raman line shape without gain narrowing. When two fields are partially correlated, then the two spectral components appear together. We provide a method to measure the degree of correlation between two optical fields that have different central frequencies. The theory developed to interpret the experimental results is an extension of the quantum theory of SRS to include anti-Stokes scattering. We show that only in the high-gain limit can the quantum fluctuations be thought of as arising from a classical noise process.