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Soviet Journal of Quantum Electronics

Influence of the polarization of radiation on the energy characteristics and threshold of stimulated Raman scattering due to rotational transitions

G V Venkin, Yu A Il'inskiĭ, G. M. Mikheev

Published Mar 31, 1985• 34 citations
Publisher

Abstract

It is shown experimentally and theoretically that the threshold intensity for stimulated Raman scattering (STRS) due to rotational transitions depends strongly on the polarization of the pump radiation. The threshold for rotational STRS is lowest for circularly polarized radiation and increases sharply for linearly polarized radiation. The results of investigations of the energy characteristics of rotational STRS on the degree of ellipticity of the pump radiation are presented.

DOI
10.1070/qe1985v015n03abeh006349

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It is shown experimentally and theoretically that the threshold intensity for stimulated Raman scattering (STRS) due to rotational transitions depends strongly on the polarization of the pump radiation. The threshold for rotational STRS is lowest for circularly polarized radiation and increases sharply for linearly polarized radiation. The results of investigations of the energy characteristics of rotational STRS on the degree of ellipticity of the pump radiation are presented.
A theoretical analysis is made of the stimulated Raman scattering in gases in the presence of spatial degeneracy of the energy levels. Saturation of the population difference and influence of anti-Stokes radiation are allowed for. Various polarizations of the pump fields and of the Stokes and anti-Stokes radiation are considered. It is shown that the profile of the stimulated Raman line is generally a sum of three Lorentzian lines and the scattering includes scalar, symmetric, and antisymmetric components. The use of circularly polarized pump radiation suppresses the influence of anti-Stokes radiation on the gain of the Stokes wave.
An investigation was made of the influence of the geometric excitation conditions on the energy dependences of the stimulated scattering of focused laser pulses of ~ 10 −8 sec duration when the sharpness and depth of focusing were varied. The experimental results obtained in this study were interpreted theoretically on the basis of a quantum analysis of stimulated Raman scattering in a two-level system. The experimental relationships could be explained only if an allowance was made for the changes in the populations of the levels participating in the Raman transition. It was possible to select the experimental conditions so that reconstruction of the wavefront of the pump radiation was observed under stimulated scattering conditions in a wide energy range.
Polarization effects in stimulated Raman and stimulated Rayleigh scattering and self focusing are investigated from the viewpoint of the scattering of polarized photons by molecules. Both stimulated vibrational Raman scattering in liquids and stimulated rotational Raman scattering in gases are considered, and it is demonstrated that the polarization changes and relative power thresholds for different laser polarizations should be somewhat different to those predicted in other theories. For example, the ellipticity eta 0 of the stimulated rotational Raman photons in the forward direction from Delta J=+or-2 transitions in gaseous symmetric top molecules is given in terms of the initial ellipticity eta 1 by sin 2 eta 0 = - 5 / 7 sin 2 eta 1 , whereas conventional theories predict that eta 0 and eta 1 are equal in magnitude and opposite in sign. Furthermore it is shown that deviations from this relation could provide a measure of the degree of optical orientation of the molecules.
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.
Abstract The theory of multifrequency stimulated Raman scattering (SRS) of light on rotational transitions of molecules, which are simulated by a three-level quantum system, is developed. It is shown that the application of bichromatic pumping increases the scattered radiation spectrum width. The exact algebraic solution for the wave amplitudes is obtained in the simplest version of synchronous SRS on transitions with a negligibly low eigenfrequency. It is found that an increase in the ratio of the Raman transition frequency to the pump radiation frequency leads to predominance of the anti-Stokes scattering branch. The effect of wave asynchronism emerging due to linear and nonlinear dispersion of the medium as well as the phase difference of the pump waves on SRS is considered. All types of asynchronism narrow generated frequency spectrum and suppress the anti-Stokes scattering branch. Nonlinear dispersion ensures positive values of wave amplitudes due to phase jumps by π during the propagation of waves in a medium.