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Optics Letters

Stimulated excited-state Raman scattering and three-photon scattering in sodium

Yaakov Shevy, Harry Friedmann, M. Rosenbluh

Published Feb 1, 1986• 12 citations
Publisher

Abstract

We have observed stimulated emission from Na vapor excited by a laser tuned near the Na D lines. The stimulated-emission processes have been identified as Rayleigh scattering, excited-state Raman scattering, and ordinary as well as resonance-enhanced three-photon scattering. The observations indicate that at least part of the conical emission observed in many systems has its origin in these processes.

DOI
10.1364/ol.11.000085

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Acta Optica Sinica•Jan 1, 1984•0 citations
We have observed stimulated emission from Na vapor excited by a laser tuned near the Na D lines. The stimulated-emission processes have been identified as Rayleigh scattering, excited-state Raman scattering, and ordinary as well as resonance-enhanced three-photon scattering. The observations indicate that at least part of the conical emission observed in many systems has its origin in these processes.
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.
Laser excitation and ionization processes in dense (1–10 Torr) sodium vapor have been studied for laser wavelengths near the two-photon allowed nd 2D(n=3, 4, 5) and ns 2S(n=4, 5, 6) states. In particular, the 1 3Σ+g→1 3Σ+u excimer emission in Na2, predicted in 1980 by Konowalow and Julienne and observed recently by Dinev et al, was studied here in greater detail. Strong excimer emission (∼830 nm) was observed for two-photon pumping to both sides of the unresolved 4D states, and weak excimer emission was seen when pumping near the 5D levels. The excimer emission exhibits a complicated pump laser profile with a pronounced ‘‘dip’’ at the 4d 2D two-photon resonance. Similarly, [2+1] photon ionization via the 3d 2D and 4d 2D states shows a dramatic decrease as the sodium density increases. These results can be attributed either to depleted 3d 2D or 4d 2D population due to stimulated electronic Raman scattering (SERS) or to the interference effects recently reported by Malcuit et al. and Krasnikov et al. and treated theoretically by Manykin and Afanas’ev and by Agarwal. It is argued that both mechanisms are operative. Strong ionization and SERS signals were observed at the hybrid resonances corresponding to 3p 2P3/2, 1/2 →4d 2D transitions; however, no excimer lasing at 830 nm was detected. No excimer emission was detected upon two-photon pumping near or at the 3d 2D or ns 2S(n=4, 5, 6) states. Based on these and other observations, the 1 3Σ+g→1 3Σ+u excimer emission is attributed to a molecular Raman process involving stimulated emission or six-wave mixing via a pathway of the type 1 3Σ+u→2hν 3Δu→ j 3Πg→(k 3Πu, l 3Σ +u)→1 3Σ+g→1 3Σ +u .
The polarization properties of stimulated three-photon scattering in a three-level atomic system are presented. In our investigation of the stimulated emission spectrum of Na, we find that interference between the amplitudes of the resonant contributions of the Na doublet states results in interesting polarization phenomena. Particularly striking is the behavior when the laser is tuned near the dispersion-free point. With the laser linearly polarized the stimulated three-photon scattering is polarized perpendicular to the laser polarization. For circularly polarized excitation, total extinction of three-photon scattering is observed.
Using linearly polarized dye laser beam which is tuned between the doublet on Na to excite Na vapor, a conical emission with polarization perpendicular to that of the incident laser in the forward direction has been observed. Its spectrum and the time evolution are measured. The relation between this emission and the density of Na, the parameters of laser and the pressure of the buff re gas have been studied. This phenomena may be explained by considering the coupling of Rayleigh scattering and transient field of Na atom.