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Journal of the Optical Society of America B

Spectral and temporal characteristics of spontaneous Raman scattering in the transient regime

Michael D. Duncan, Rita Mahon, Lawrence L. Tankersley, John F. Reintjes

Published Feb 1, 1991• 8 citations
Publisher

Abstract

We demonstrate explicitly that the quantum theories that predict that stimulated Raman scattering is initiated from zero-point fluctuations of either the material oscillators or the electromagnetic field are equivalent and that the process can be viewed as arising from both types of fluctuation. We further demonstrate experimentally that in the transient regime the spontaneous Stokes intensity reproduces the pump in amplitude and phase, as predicted by quantum theory, without any of the integrating effects normally associated with transient processes.

DOI
10.1364/josab.8.000300

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We demonstrate explicitly that the quantum theories that predict that stimulated Raman scattering is initiated from zero-point fluctuations of either the material oscillators or the electromagnetic field are equivalent and that the process can be viewed as arising from both types of fluctuation. We further demonstrate experimentally that in the transient regime the spontaneous Stokes intensity reproduces the pump in amplitude and phase, as predicted by quantum theory, without any of the integrating effects normally associated with transient processes.
From a classical point of view the generation of Stokes light by stimulated Raman scattering (SRS) is not possible unless a Stokes input signal is supplied. On the other hand, the gain in SRS can be so large that without input the spontaneous build-up of strong Stokes waves can be observed. A proper quantum theoretical description1 shows that this spontaneous initiation of Stokes generation is due to microscopic random fluctuations originating from quantum noise associated with the dynamical variable Q(t) which is active in the Raman process, e.g., a molecular normal mode coordinate. In highly transient SRS -when the duration of the excitation pulse is shorter than the dephasing time- the Stokes field is proportional to the initial Heisenberg operator Q(0) describing the state of the system just before the excitation pulse is turned on (t=0). In this case the statistics of the final Stokes pulse energy is determined by quantum mechanical uncertainties associated with the random Raman polarization of the initial state2. On the other hand, in a steady state situation the Stokes pulse fluctuations are substantially reduced and the Stokes pulse energy is stabilized as a result of damping processes.
Manifestations of quantum fluctuations in stimulated Raman scattering ( SRS ) have been intensively studied lately1. Quantum noise present in spontaneous scattering stimulates fluctuations both in phase and in amplitude characteristics of output Stokes emission. At present statistical properties of amplitude fluctuations are studied in detail and it is shown that in linear transient regime of SRS without pump depletion statistical scatter of Stokes energy Es has negative exponential distribution2. In saturation regime of SRS the amplitude fluctuations are almost suppressed simultaneously with pump depletion. The phase fluctuations manifest both in linear and in nonlinear SRS and produce beam pointing fluctuations3, a change in Stokes emission spectra from pulse to pulse4 and cause soliton appearance in Rayleigh component of SRS5. Phase noise is observed in saturation regime due to relation between phases of Stokes and phonon waves which is preserved in processes of stationary and quasistationary SRS amplification. Spectrum phase fluctuations manifest as fine structure of SRS spectrum4, fluctuations of average Stokes frequency and Stokes linewidth fluctuations. The evolution of phase fluctuations in time is determined by the nature of spontaneous scattering and polarization of Raman media and is of great interest as one can follow its development from vacuum modes level to saturation regime. However up to now this problem has not been studied yet.
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.
Theoretical and experimental details of initiating and amplifying a Stokes pulse using stimulated Raman scattering in H2 are presented.Statistics associated with the spectral fluctuations of a Stokes seed pulse have been measured and theoretically calculated.The spectral fluctuations are shown to result from quantum noise associated with spontaneous initiation.These spectral fluctuations are an example of an easily measurable macroscopic fluctuation of quantum origin.The effects of frequency fluctuations on the generation of solitons in the nonlinear regime of stimulated Raman scattering are calculated and measured.A detailed derivation of the fully quantum mechanical stimulated Raman scattering equations is given along with their solution for various approximations.The driven Maxwell's equation for the Raman system is derived from the system Hamiltonian.For treating the quantum initiation of stimulated Raman scattering, the radiation field is expanded in localized coherent modes.The details of calculating and using these modes to generate an ensemble of Stokes pulses are presented along with specific examples and ensemble average statistics.The use of localized modes for treating the pulsed cavityless Raman laser gives insight into the spontaneous initiation of Stokes pulses.iv ACKNOWLEDGMENTS I feel very fortunate to have had Dr. John Carlsten for my thesis adviser.I would like to thank John for making graduate school an enjoyable part of life and for the many hours o f stimulating discussions on fundamental physics.I am also greatly indebted to my wife, Susie, for filling my big lunch bag every morning and for her many hours spent typing this thesis
It is shown that transient anti-Stokes stimulated Raman scattering (SRS) acts as a vacuum field fluctuations amplifier at Stokes frequency, the fluctuations being amplified up to macroscopic values. This makes their investigation possible by studying macroscopic energy fluctuations of transient SRS anti-Stokes pulses. The proposed theory also gives a quantitative description of angular distribution of self-generated anti-Stokes emission around the exact phase-matching angle recently observed by Duncan et al. ( Opt. Lett. , 11 (1986) 803) in the transient regime.
The quantum theory of forward Stokes generation by means of stimulated Raman scattering is extended to the case of a colored (finite-bandwidth) chaotic pump, which has both amplitude and phase fluctuations. In both transient and steady-state limits the mean Stokes intensity is found to be enhanced over that resulting from a coherent pump. In the limit that the chaotic-pump bandwidth becomes large, the mean Stokes intensity becomes identical with that resulting from a coherent pump of the same total power.