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Journal of Physics B Atomic and Molecular Physics

Stimulated collision-induced resonance Raman scattering

V.M. Arutunyan, N. Sh. Badanyan, N. V. Shakhnazaryan

Published Oct 14, 1985• 0 citations
Publisher

Abstract

The passage of strong monochromatic laser radiation through a resonance medium consisting of three-level atoms is investigated. It is shown that if collisions are taken into account in the scattered waves the resonances at combination frequencies occur to first order in the laser field intensity. A numerical analysis of the dependence of the stimulated electronic Raman scattering (SERS) components' gain factors on the pump frequency is carried out. The dispersion curves of the SERS components' gain (absorption) factors for fixed values of pump frequency and intensity are plotted.

DOI
10.1088/0022-3700/18/19/020

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The passage of strong monochromatic laser radiation through a resonance medium consisting of three-level atoms is investigated. It is shown that if collisions are taken into account in the scattered waves the resonances at combination frequencies occur to first order in the laser field intensity. A numerical analysis of the dependence of the stimulated electronic Raman scattering (SERS) components' gain factors on the pump frequency is carried out. The dispersion curves of the SERS components' gain (absorption) factors for fixed values of pump frequency and intensity are plotted.
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.
We have observed collisional redistribution of laser light scattered by a three-level atom, thallium, in the presence of argon. The two observed spectral components correspond to Raman scattering and collision-induced fluorescence. We have seen the growth of both components from spontaneous to stimulated scattering as the laser intensity is increased. While the gain for the Raman component agrees with theory, the observed gain of the collision-induced fluorescence is over an order of magnitude lower than predicted.
The main properties of infrared stimulated electronic Raman scattering (SERS) at the 6 2 S 1/2 -7 2 S 1/2, 3/2 transitions in cesium atoms are studied theoretically and experimentally as functions of the atomic concentration, which was varied from 10 11 to 10 16 cm −3 . It is found that the efficiency of generation of Stokes radiation strongly depends on one-photon absorption of the pump radiation tuned near frequencies of the 6 2 S 1/2 -7 2 P 1/2, 3/2 transitions. By using the equation for the density matrix, which describes the evolution of a three-level system, the theory of resonance excitation of IR radiation upon one-photon absorption at an adjacent transition is developed. The theory describes well the main features of IR SERS in alkali-metal vapors.
The influence of phase memory effects on the spectrum of resonance Raman scattering by three-level atoms with the Λ configuration of levels experiencing collisions with buffer gas atoms in a strong monochromatic radiation field is studied theoretically. Systems with a small Doppler broadening compared to the collision frequency (large buffer gas pressures) are analysed in the general case of an arbitrary change (from complete change to complete preservation) in the phase memory at any of three transitions in the Λ system. It is shown that in the absence of the collision relaxation of the low-frequency coherence at the transitions between two lower levels of the Λ system, the radiation scattering spectrum has a spectrally narrow component at the Raman frequency, which, despite the homogeneous broadening of the absorption line, exhibits a strongly pronounced anisotropy. In the direction, close to the propagation direction of exciting radiation, this line maximally narrows down. It is significant that upon optical pumping to the level unaffected by a strong field the resonance Raman spectrum noticeably differs from the spectrum in the case of the probe field. A simple expression is proposed for calculating the degree of the phase memory preservation in collisions from the relative amplitude of the Raman resonance.
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.
We have studied the stimulated hyper-Raman scattering process in the presence of two strong electromagnetic fields whose frequency modes are initially populated and are near resonance with the two atomic transition frequencies. Using the Green's-function formalism, the excitation spectra are calculated in the limit of high photon densities of both laser fields. Expressions are derived for the relative intensities describing the following processes when (i) both pump fields are at resonance, (ii) the detunings take opposite values corresponding to the cooperative two-photon resonance, and (iii) both laser fields are off resonance. In processes (i) and (ii), the spectra consist of a single peak describing the stimulated hyper-Raman scattering and two pairs of sidebands induced by the laser fields. A new peak appears in process (iii) in addition to those appearing in processes (i) and (ii). The induced spectra are symmetric at resonance but asymmetric in the off-resonance processes, and the extent of the asymmetry depends strongly on the numerical values of the detunings. It is shown that when the two laser fields are treated classically, the derived results are identical to those obtained when the fields are quantized only when photon-photon correlations arising from each laser field are discarded. Numerical calculations for selected values of Rabi frequencies and detunings are graphically presented and discussed.