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Soviet Journal of Quantum Electronics

Stimulated resonant hyper-Raman scattering of light by polaritons in alkali metal vapors

Yu A Galaĭchuk, Yu. N. Yashkir

Published Dec 31, 1989• 1 citation
Publisher

Abstract

A theory is developed for the calculation of the gain g due to stimulated resonant hyper-Raman scattering of light by polaritons in gaseous media. It is shown that throughout the tuning range of the pump frequency (including one- and two-photon resonances) a maximum of g corresponds to a dispersion curve of polaritons plotted ignoring attenuation. Theoretical results are used to analyze characteristics of hyper-Raman scattering in sodium vapor. It is shown that under normal experimental conditions the splitting of polariton branches is considerable (amounting to tens of reciprocal centimeters on the frequency scale and several angular degrees). The value of g is estimated for two-photon resonances in the case when the pump frequency is tunable in a wide range. The optimal conditions for stimulated hyper-Raman scattering are identified.

DOI
10.1070/qe1989v019n12abeh010180

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A theory is developed for the calculation of the gain g due to stimulated resonant hyper-Raman scattering of light by polaritons in gaseous media. It is shown that throughout the tuning range of the pump frequency (including one- and two-photon resonances) a maximum of g corresponds to a dispersion curve of polaritons plotted ignoring attenuation. Theoretical results are used to analyze characteristics of hyper-Raman scattering in sodium vapor. It is shown that under normal experimental conditions the splitting of polariton branches is considerable (amounting to tens of reciprocal centimeters on the frequency scale and several angular degrees). The value of g is estimated for two-photon resonances in the case when the pump frequency is tunable in a wide range. The optimal conditions for stimulated hyper-Raman scattering are identified.
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.
Investigations are made of hyper-Raman scattering and four-photon parametric processes in two-photon excitation of metal vapor. The laws of propagation of infrared and ultraviolet radiation generated in a metal vapor medium by these processes are found for the steady-state interaction. The nonlinear polarization of the medium is obtained in terms of elements of the atomic density matrix allowing for saturation by the pump field and for the influence of collisions. The spectral and tuning characteristics of the converted radiation are studied and a comparison is made with experimental data. A dip observed in the infrared radiation spectrum for hyper-Raman scattering and its broadening are explained. A detailed discussion is given of the role of collisions that substantially narrow the tuning range of the infrared radiation in hyper-Raman scattering.
A report is given of the first quantitative study of the spontaneous and stimulated electronic Raman scattering by a resonance doublet of the sodium atom excited resonantly at the D 1 and D 2 lines by a tunable dye laser. Theoretical and experimental analyses of the differential scattering cross section and polarization properties at the Stokes and anti-Stokes frequencies show that the observed scattering is due to a nearly resonant process involving the ground state 3 S 1/2 as the dominant intermediate state. The stimulated Stokes and anti-Stokes scattering lines, which are shifted from the D 1 and D 2 lines by an amount corresponding to the frequency separation between lowest-lying excited doublets 3 P 1/2 and 3 P 3/2 , are observed by exciting a sodium vapor cell with a passively mode-locked dye laser.
Experimental and theoretical investigations were made of four-wave frequency mixing of the ?4? = ?1 ? ?2 ? ?3 type in cesium vapor enhanced by a Raman resonance (the field at the frequency ?2 is formed as a result of electronic stimulated Raman scattering of the pump field ?1). A strong dependence of the mixing characteristics on the conditions for excitation of electronic stimulated Raman scattering was identified and analyzed. Recommendations are given on the choice of optimal conditions for efficient frequency mixing in Raman resonance systems.
Stimulated two-photon induced Raman scattering (hyper-Raman scattering) in an amplifier consisting of four-level atoms is analyzed semiclassically, via the coupled density matrix and Maxwell equations. We consider conditions typically encountered in the optical regime and in vapors. We show that even in the linear regime, it is characterized by a significant depletion of the atomic ground-state population, thus invalidating perturbative analyses based, for instance, on the nonlinear susceptibility tensor. Two major regimes of operation are found, one in which the population is completely consumed by the interaction ("linear regime"), and one in which the pump laser is depleted ("nonlinear regime"). Both regimes are, however, characterized by small photon conversion efficiencies. The tuning range is also briefly discussed.
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.