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Influence of the ac Stark effect on stimulated hyper-Raman profiles in sodium vapor

Moore, W. R. Garrett, M. G. Payne

Published Aug 1, 1988• 0 citations
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Abstract

When pumping near the two-photon 3d resonance in pure sodium vapor and observing the backward hyper-Raman emission to the 3p substates, an asymmetry in ratios of 3p/sub 1/2/, 3p/sub 3/2/ associated emissions was observed dependent upon the direction of the initial laser detuning from the resonance. It has been determined that this asymmetry can be attributed to the ac Stark effect induced by the hyper-Raman emission itself. 3 refs., 3 figs.

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Two-photon excitation of dense sodium vapor near the n d 2D5/2, 3/2 (n=3, 4, 5) levels: Na2 1 3Σ+g→1 3Σ+u excimer emission

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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 Journal of Chemical Physics•Dec 15, 1988•12 citations
When pumping near the two-photon 3d resonance in pure sodium vapor and observing the backward hyper-Raman emission to the 3p substates, an asymmetry in ratios of 3p/sub 1/2/, 3p/sub 3/2/ associated emissions was observed dependent upon the direction of the initial laser detuning from the resonance. It has been determined that this asymmetry can be attributed to the ac Stark effect induced by the hyper-Raman emission itself. 3 refs., 3 figs.
Experimental investigations of two-photon enhanced stimulated hyper-Raman and parametric four-wave-mixing emissions are described for tuning unfocused laser beams near two-photon resonance with 3D and 4D states in sodium vapor. Over wide ranges of vapor pressures, path lengths, and laser power densities, the gains for stimulated hyper-Raman (SHR) scattering and for parametric four-wave mixing (PFWM) can become very greatly reduced from values expected from simple considerations. The suppression of gain can arise from interferences produced at two-photon and three-photon resonances, and from ac Stark shifts produced by internally generated near-resonant fields. Quantitative comparisons are made between observed and theoretically predicted values for SHR and PFWM production. Of 12 predicted consequences of the interferences and Stark shifting on the nonlinear behavior, ten are demonstrated through the experiments.
The stimulated hyper-Raman scattering (SHRS) emissions associated with the excitation of the 4P 3/2 state in sodium vapour have been observed in both the forward and backward directions as the pumping laser was tuned near the 3S-4D two-photon resonance. The results show that though the forward SHRS process is greatly reduced by a destructive interference between it and the four-wave mixing (FWM) process induced by itself, the forward SHRS emission has a positive gain and can still be observed under a certain condition.
We have measured the ac Stark effect in a two-zone stimulated Raman interaction in a sodium atomic beam. In addition, we have derived simple theoretical expressions for the ac Stark shift, based on a closed three-level system, in the Λ configuration, and have achieved qualitative agreement with the data. In particular, the magnitude and sense of the ac Stark shifts are found to depend on laser intensities as well as on the initial populations of the two low-lying levels of the Λ configuration. Specifically, the observed ac Stark shifts are smaller for larger laser intensities and also for smaller initial population differences between the two low-lying levels. The ac Stark effect must be considered for many potential applications of the Raman effect, such as a Raman clock. In this connection, we have identified conditions for the reduction of the ac Stark shift in our sodium Raman clock.
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 .