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Journal of the Optical Society of America A

Spectral and temporal investigations of transient coherent Raman scattering (A)

Wolfgang Zinth, A. Laubereau, W. Kaiser

Published Jun 1, 1980• 0 citations
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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.
By use of a streak camera, the temporal variations of light pulses generated by stimulated Raman scattering have been observed when the pulse duration is of the order of the inverse Raman linewidth. In this regime, which is intermediate between transient and steady state, the pulse shapes undergo large shot-to-shot variations due to the effects of quantum moise. It is found that some of the pulses bear a strong resemblance to the temporal coherence modes, i.e., the eigenfunctions of the two-time field autocorrelation function.1 Probability distributions for the energy content of each of these modes are negative-exponential functions of energy. This explains why isolated modes are sometimes seen on a single shot.
A theory is developed for transient hyper-Raman scattering and four-wave parametric processes in a gaseous medium subjected to an ultrashort pump pulse field. Investigations are made of the intensity and spectrum of the infrared and ultraviolet radiation generated in a medium as a result of these processes, bearing in mind the transient properties of the pump (phase modulation, pulse profile). It is shown that the initial nonlinearity of the pump field and the parametric processes result in new effects not observed in transient stimulated Raman scattering. For a large two-photon detuning, the hyper-Raman forward scattering is suppressed because of destructive interference with stimulated parametric generation of ultraviolet radiation. The gain of the infrared and ultraviolet radiation depends on the pump pulse profile. Under exact two-photon resonance conditions in the absence of any phase modulation of the pump, infrared and ultraviolet pulses are coherently split into various subpulses and a time-dependent Autler–Townes doublet is observed in their spectrum.