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Japanese Journal of Applied Physics

Near Threshold Behavior of Stimulated Brillouin Scattering in an Off-Axis Resonator

Toshio Ito, Hiroshi Takuma

Published Jul 1, 1969• 2 citations
Publisher

Abstract

Strong interference of the first Stokes Raman radiation with the stimulated Brillouin radiation has been observed in an off-axis resonator: Brillouin gain decreases appreciably by the presence of the Raman radiation in a medium such as CS2, in which the Raman and Brillouin scatterings can be stimulated simultaneously. Such a type of interference can be explained as the Raman scattering of the Brillouin photons stimulated by the first Stokes Raman photons. A classical theory has shown a quantitative agreement with the experiment. The anti-Stokes Brillouin components have not been observed even though the laser excitation was intense enough to allow the observation of the multiple Stokes components which were excited directly in the off-axis resonator without the feed-back effect of the laser as an amplifier.

DOI
10.1143/jjap.8.941

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Strong interference of the first Stokes Raman radiation with the stimulated Brillouin radiation has been observed in an off-axis resonator: Brillouin gain decreases appreciably by the presence of the Raman radiation in a medium such as CS2, in which the Raman and Brillouin scatterings can be stimulated simultaneously. Such a type of interference can be explained as the Raman scattering of the Brillouin photons stimulated by the first Stokes Raman photons. A classical theory has shown a quantitative agreement with the experiment. The anti-Stokes Brillouin components have not been observed even though the laser excitation was intense enough to allow the observation of the multiple Stokes components which were excited directly in the off-axis resonator without the feed-back effect of the laser as an amplifier.
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 influence of a strong field resonant to the Raman transition on the behavior of the Stokes harmonic in saturated two-wave stimulated Raman scattering is theoretically considered based on the description of a gas of three-level atoms by medium density matrix equations. The vibrational mode of energy redistribution between laser and scattered radiation, threshold with respect to the resonant field intensity, is predicted. The action of optical fields on the absorption and amplification of the resonant field in a Raman medium is described.
A calculation is made of the intensity of the Stokes radiation in the stimulated Raman scattering of ultrashort light pulses in a dispersive medium employing the asymptotic approximation for arbitrary modulation of the amplitude and phase of the pump pulse. Particular attention was paid to the effect of phase modulation on the stimulated Raman scattering. Calculations were also made of the intensity of the anti-Stokes component in the scattering of an ultrashort pulse in a dispersive medium and of the optimal angle for the observation of the anti-Stokes rings.
An analysis is made of parametric excitation of anti-Stokes components of stimulated Raman scattering in an optical resonator filled with a medium whose refractive index is dispersion-free. The case of steady generation of the first Stokes component is considered. Expressions are obtained for the amplitudes of steady-state fluctuations of the anti-Stokes components in the case of a weak reaction of these components on the pump radiation and on the first Stokes component. Various cases of frequency dependences of the intrinsic resonator losses are considered. Conditions are found under which a large number of anti-Stokes components with similar intensities is excited so that the anti-Stokes radiation leaving the resonator is a periodic sequence of ultrashort (femtosecond) pulses with one pulse per period.
The passage of strong monochromatic laser radiation through a resonance medium consisting of three-level atoms is investigated. It is shown that if collisions are taken into account in the scattered waves the resonances at combination frequencies occur to first order in the laser field intensity. A numerical analysis of the dependence of the stimulated electronic Raman scattering (SERS) components' gain factors on the pump frequency is carried out. The dispersion curves of the SERS components' gain (absorption) factors for fixed values of pump frequency and intensity are plotted.
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.