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Physical Review A

Stimulated Kerr scattering and reorientation work of molecules in liquid CS2

Guang S. He, Paras N. Prasad

Published Mar 1, 1990• 55 citations
Publisher

Abstract

A Stokes shifted superbroadening stimulated scattering has been studied in a ${\mathrm{CS}}_{2}$ liquid-core hollow fiber system with a long gain length (2.5 m) by using \ensuremath{\approxeq}10-ns laser pulses with a pump intensity range of (${10}^{6}$--5\ifmmode\times\else\texttimes\fi{}${10}^{8}$ W/${\mathrm{cm}}^{2}$). The salient features of this stimulated scattering are that the spectral broadening range is very large (\ensuremath{\ge}700 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$) and no detectable shift of the spectral maximum or periodical modulation structure is observed. In order to interpret our experimental results, various possible mechanisms and processes are discussed. A model based on stimulated Kerr scattering of anisotropic molecules in liquid is suggested to explain the observation. This model assumes a single-step reorientation of anisotropic molecules induced by an intense optical field.

DOI
10.1103/physreva.41.2687

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A Stokes shifted superbroadening stimulated scattering has been studied in a CS2{\mathrm{CS}}_{2}CS2​ liquid-core hollow fiber system with a long gain length (2.5 m) by using \ensuremath{\approxeq}10-ns laser pulses with a pump intensity range of (106{10}^{6}106--5\ifmmode\times\else\texttimes\fi{}108{10}^{8}108 W/cm2{\mathrm{cm}}^{2}cm2). The salient features of this stimulated scattering are that the spectral broadening range is very large (\ensuremath{\ge}700 cm\ensuremath−1{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}cm\ensuremath−1) and no detectable shift of the spectral maximum or periodical modulation structure is observed. In order to interpret our experimental results, various possible mechanisms and processes are discussed. A model based on stimulated Kerr scattering of anisotropic molecules in liquid is suggested to explain the observation. This model assumes a single-step reorientation of anisotropic molecules induced by an intense optical field.
By using a liquid-core multimode hollow fiber system with a long gain-length (2.5 or 7 m), a superbroadening stimulated scattering added to the pump line and/or the several orders of Stokes-stimulated Raman scattering lines of the core medium can be observed. This kind of stimulated scattering is related to the optical Kerr (reorientation) effect and Raman-induced Kerr effect in a liquid consisting of anisotropic molecules. Experimental studies of hollow fiber filled with different liquid samples (carbon disulfide, benzene, carbon tetrachloride) are reported. A theoretical approach based on a photon scattering model of optical Kerr effect and Raman-induced Kerr effect is proposed to explain the principal features of our experimental results. The significance of stimulated Kerr scattering studies and their potential applications are discussed.
The theory of transient stimulated Raman scattering has been extended to include an arbitrary shape of the laser pump pulse. It is shown that the maximum Stokes gain depends on the total energy content per unit area of the pump pulse, and not on the instanteous intensity for an exciting pulse of short duration. The Stokes pulse has a leading edge which rises sharply to a maximum, where the maximum occurs with some delay with respect to the maximum of the pump pulse. The trailing edge follows the decay of the pump. In a nondispersive medium, the gain is not reduced by frequency broadening of the laser output, while in a dispersive medium, considerable gain reduction is expected. Numerical results for various laser-pulse shapes and spectral distributions are presented.
The nonlinear theory of stimulated Raman scattering of high-energy long laser pulses in two-level media is constructed and provides a unified global interpretation of the experiments of Dr\"uhl, Wenzel, and Carlsten [Phys. Rev. Lett. 51, 1171 (1983)]. It is proved that the model, resulting from the slowly varying envelope approximation and including phase mismatch and detuning from Raman resonance, is integrable by the spectral transform method for arbitrary boundary values. The essential variable in the theory is the phase of the Stokes pulse relative to the pump. For long duration input pump pulses and when pump and Stokes pulses experience a rapid \ensuremath{\pi} phase shift, an anomalous spike of pump radiation is created in the pump depletion zone. It is shown in particular that the decay of Raman spikes is related to the velocity of this \ensuremath{\pi} phase shift. For fast flips, the possibility of observing spike overflow is established and, with multiple phase flips, a multiple-spike phenomenon is produced, suggesting new experiments. Lastly, the number of optical phonons participating to the interaction is explicitly calculated.
A theoretical study of the polarization dependence of stimulated Rayleigh-wing scattering and the optical-frequency Kerr effect has been undertaken. When the incident light is circularly polarized, a striking difference in gain is found for the co- and counter-rotating senses of polarization of the scattered light---the former being suppressed and the latter being exceptionally favored. The analysis begins with a model for the Kerr effect, which involves the alignment of anisotropic molecules in an electric field, but the results can be immediately generalized to any light scattering process of tensor symmetry. The nonlinear problem of the propagation of an intense elliptically polarized light wave in a Kerr-active medium is shown to have a solution in which the vibrational ellipse undergoes self-precession and self-retardation. The stimulated scatterings or instabilities of such a self-precessing and self-retarding light wave are obtained for the backward and forward directions. Birefringence, optical activity, and linear and circular dichroisms are some of the phenomena which result, but the forward direction yields substantially different results from the backward direction because of Stokes-anti-Stokes coupling.
Stimulated Rayleigh-wing scattering is studied here in various liquids excited with a Bessel beam that allows a complete spatial separation between the transmitted exciting light and the scattered light. The results show that a large Stokes spectral band displaying substructures is obtained in the absence of self-focusing, cross-focusing, self-phase modulation, and cross-phase modulation. An interpretation is proposed based on the role of cascade Stokes–anti-Stokes coupled scattering processes.