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Journal of Raman Spectroscopy

Review and interpretation of experiments on coherent four-photon Raman scattering

M. M. Sushchinskiǐ

Published Jan 1, 2000• 2 citations
Publisher

Abstract

The general theory of stimulated radiation is applied to four-photon coherent Raman scattering. A comparison with the theory of the two-photon scattering is presented. Some peculiarities of the stimulated Raman scattering such as radiation asymmetry, replication effects, rings of the Raman components are considered based on the theory for coherent processes. Copyright © 2000 John Wiley & Sons, Ltd.

DOI
10.1002/1097-4555(200008/09)31:8/9<669::aid-jrs592>3.0.co;2-s

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The general theory of stimulated radiation is applied to four-photon coherent Raman scattering. A comparison with the theory of the two-photon scattering is presented. Some peculiarities of the stimulated Raman scattering such as radiation asymmetry, replication effects, rings of the Raman components are considered based on the theory for coherent processes. Copyright © 2000 John Wiley & Sons, Ltd.
The quantum theory of the statistical properties and the photocount statistics of intense radiation in Raman scattering are presented making use of the coherent-state techniques. Both the Heisenberg-Langevin and Fokker-Planck equations approaches are developed. The existence of the conditional Glauber-Sudarshan quasi-distribution is also discussed. The time dependences of the photocount distribution and its factorial moments are demonstrated in the case of stimulated scattering and anticorrelation and antibunching of scattered photons are found.
The basis of this dissertation is a review of the quantum mechanical formulation of damping and stimulation, particularly in non-linear optical processes. The basic problems of the quantum theory of damping are discussed, and the formalism for the quantum theory is introduced. The study of a particular example, that of a damped simple harmonic oscillator, provides an introduction to the handling of the basic tool, the master equation. The physical aspects of the non-linear processes are contained in the systems' photon statistics, and the master equation provides several approaches for obtaining these. This theory is then used to formulate a quantum mechanical model of Raman scattering by phonons, and to thus obtain the photon statistics of the scattered radiation.
We present a three-dimensional theory of stimulated Raman scattering (SRS) or super-radiance. In particular we address how the spatial and temporal properties of the generated SRS beam or Stokes beam of radiation depends on the spatial properties of the gain medium. Maxwell equations for the Stokes field operators and of the atomic operators are solved analytically and a correlation function for the Stokes field is derived. In the analysis we identify a super-radiating part of the Stokes radiation that exhibit beam characteristics. We show how the intensity in this beam builds up in time and at some point largely dominates the total Stokes radiation of the gain medium. We show how the SRS depends on the Fresnel number and the optical depth and that in fact these two factors are the only factors describing the coherent radiation.
The Dicke theory of coherent spontaneous emission is generalized by means of group-theoretical methods. Effects of superradiation and the structure of coherent responses of an equilibrium medium to pulsed excitation are considered. A method of calculating cooperative effects in second-order perturbation theory is developed. The role of collective properties of a system of radiators in experiments with high power exciting radiation is discussed. Some "anomalous" features of stimulated Raman scattering are accounted for.
An experimental investigation was made of the resonant stimulated electronic Raman scattering near the principal doublet of potassium. A study was made of the dispersion, interaction of two- and three-photon scattering, and influence of four-photon processes. Possible mechanisms of the population of the 4 2 P 1/2 and 4 2 P 3/2 potassium levels were considered. The possibility of phase-matched four-photon parametric interactions in the investigated part of the spectrum was confirmed theoretically.