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Soviet Journal of Quantum Electronics

Stimulated Raman scattering under resonance illumination conditions

Vladimir D Taranukhin

Published Oct 31, 1979• 0 citations
Publisher

Abstract

A new variant of active Raman spectroscopy is proposed. Instead of two-frequency pumping, radiation in resonance with the scattering transition is used and a static electric field is applied simultaneously. This variant may have an advantage over the conventional method in the case of a large Stokes shift which is found, for example, in the Raman scattering due to electronic transitions. An analysis is made of the dynamics of the interacting waves and the optimal length of nonlinear medium to which a static electric field should be applied is determined.

DOI
10.1070/qe1979v009n10abeh009545

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A new variant of active Raman spectroscopy is proposed. Instead of two-frequency pumping, radiation in resonance with the scattering transition is used and a static electric field is applied simultaneously. This variant may have an advantage over the conventional method in the case of a large Stokes shift which is found, for example, in the Raman scattering due to electronic transitions. An analysis is made of the dynamics of the interacting waves and the optimal length of nonlinear medium to which a static electric field should be applied is determined.
A model is developed for the description of stimulated Raman scattering. This model allows for changes in the level populations due to radiative transitions and it can be used also for an arbitrary detuning of the pump radiation from the center of a line of an atom in the active medium. A study is made of the conversion of wide-band laser radiation into a Stokes signal. It is shown that this conversion is quite efficient and the Stokes signal gain corresponds to coherent scattering. This result is related to the matching of the phases of the pump and Stokes signals. Numerical investigations carried out using this model under the experimental conditions described elsewhere give results in agreement with the experimental data.
The stimulated Raman scattering (SRS), arising from the interaction between molecules of a medium and two strong light fields - a resonant field and a pumping field - is studied theoretically. The transitions of molecules between a given pair of levels is assumed to be both Raman active and infrared active. A semiclassical approach, in which the density matrix method is used for the quantum mechanical description for the medium, is employed. We expand the density matrix in various orders within which the zeroth-order is referred to as the solution of the equation of motion of the density matrix when only the resonant field is applied. -- We obtain a set of equations in second order of the density matrix element p₁₀⑵ (ω) from which the gain function can be derived. This set of equations in the special case of steady state is accidentally similar to those obtained by Mollow in his study of the power spectrum of a strong driven two-level system. We have shown that the SRS in the steady state under the resonant field interaction, is drastically reduced in general. When the flopping frequency is larger than the relaxation constants (Ω > r), we find there appears both weak positive and weak negative gains on both sides of the ordinary SRS components. Since we retain our second-order equations in a general form rather than the form for steady state, we are able to take account of the dependence on the transient zeroth solution. By employing the Laplace transform technique with the help of convolution products, we are able to solve for ρ₁₀⑵(ω) in the stationary flopping state. When the intensity of the resonant field is high, we have found theoretically that both the Stokes and anti-Stokes component become doublets and equally displaced by the amount of the flopping frequency, Ω, on the opposite sides of ordinary Stokes and anti-Stokes components, respectively. The gain maxima are approximately the order of Ω/4r times the ordinary gain of the Stokes component, where Ω/r >> 1 if the flopping exists. The gains are therefore large in comparison with the ordinary gain for SRS in the steady state.
An analysis is made of the propagation of a short coherent optical pulse in a three-level resonant medium with an essentially nonequidistant spectrum as a function of the degree of preexcitation of the medium. It is found that in addition to self-induced transparency and resonance scattering, stimulated Raman scattering (Stokes or anti-Stokes) should be observed under certain spatial phase-matching conditions. The area theorem is formulated for all radiation components. An analysis is made of the case of propagation of a resonant electromagnetic pulse of frequency ω in a system of three-level atoms having an equidistant spectrum. Under conditions of preexcitation of the medium at the frequency 2ω by longitudinal acoustic pulses, a scattered transverse acoustic wave at the frequency ω may be observed.
An analysis is made of some features of spontaneous resonance Raman scattering representing a noise signal which is amplified by a strong field in a nonlinear medium. A detailed review is made of the experimental results obtained in investigations of the spectra of stimulated preresonance and resonance Raman scattering in nonlasing and lasing systems. It is shown that, depending on the experimental conditions, these spectra may be due to transitions between vibrational levels of molecules which are in the ground or first excited electronic states. The example of several compounds is used to demonstrate the information which can be derived from such spectra. Possible practical applications of studies of such spectra are indicated. The physical basis of the theory of stimulated resonance Raman scattering is discussed and conclusions are drawn on the nature and mechanism of this Raman effect.
Stimulated Raman scattering (SRS) from a system that is both Raman active and infrared active has been investigated theoretically when a strong coherent resonant infrared light field, in addition to a pumping field, is applied. In the density matrix formulation, it is found that the gain function in steady state is redistributed as a result of the modulation on the populations and transition probabilities by the presence of the strong resonant field. The redistribution curve shows Rabi frequency splitting for the Stokes component and a new origin of anti-Stokes components of SRS that is anticipated in the present mechanism.