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Physical Review A

Simultaneous observation of excited-state Raman scattering and resonance-enhanced three-photon scattering

Yaakov Shevy, M. Rosenbluh, Harry Friedmann

Published Feb 1, 1985• 13 citations
Publisher

Abstract

New resonances have been observed in the fluorescence spectrum of atomic sodium, near the D lines, for both resonant and nonresonant laser excitation. The resonances are interpreted as arising from the interaction of the strong driving laser field and the three-level atom. Specifically, two simultaneously acting mechanisms are identified: resonantly enhanced three-photon scattering and excited-state Raman scattering.

DOI
10.1103/physreva.31.1209

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New resonances have been observed in the fluorescence spectrum of atomic sodium, near the D lines, for both resonant and nonresonant laser excitation. The resonances are interpreted as arising from the interaction of the strong driving laser field and the three-level atom. Specifically, two simultaneously acting mechanisms are identified: resonantly enhanced three-photon scattering and excited-state Raman scattering.
Two types of parametric four-wave mixing are observed when a single intense laser beam propagates through Na vapor near the D(1) and D(2) resonance lines. The first is related to three-photon scattering, while the second results from the coherent parametric interaction of the laser with excited-state Raman scattering. Identification of the two processes was greatly facilitated by the use of an optical multichannel detector system to observe the total emission spectrum for each individual laser pulse. The experimental conditions that determine whether stimulated emission or one or both of the four-wave mixing processes dominates the emission spectrum are described.
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.
We consider the possible physical processes that may arise in a three-level atom when only two of its levels interact with a strong electromagnetic field and when the atomic transition frequency is nearly equal to once and twice the frequency of the laser field, respectively. There have been found pronounced cooperative effects in the spectrum of the two-level system, which is in resonance with the laser field, arising from the presence of the third level. The excitation spectra describing the transitions from the first excited state into the second excited state and from that to the ground state consist, apart from the two central peaks, of two pairs of sidebands which are induced by the laser field of the neighbouring system. Detailed expressions of the spectral functions for the physical processes of one- and two-photon resonance fluorescence have been derived and discussed in the limit of high photon densities. The excitation spectrum of the low frequency modes has been considered and discussed in detail. It is found that quantum beats in spontaneous emission may appear in the spectra of the one- and two-photon resonance fluorescence arising from the interference between the two atomic transition frequencies and the frequency of the laser field. The importance of the low frequency modes that occur in the processes in question has been pointed out.