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Physical Review A

Suppression effects in stimulated hyper-Raman emissions and parametric four-wave mixing in sodium vapor

W. R. Garrett, Mary Anne Moore, Roger C. Hart, M. G. Payne, Rainer Wunderlich

Published May 1, 1992• 44 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.45.6687

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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.
The nonlinear response of sodium vapor with a laser tuned near the 4D two-photon resonance is investigated over a large range of sodium concentrations and pump intensities with emphasis on the influence of coherent cancellation effects on the induced polarizations and the primary mechanism for the generation of the new frequencies. Over a wide range of circumstances, the response of the medium is dominated by parametric four-wave mixing as compared to amplified spontaneous emission or stimulated electronic hyper-Raman scattering. Secondary four-wave-mixing fields are generated by stimulated Raman scattering of one parametric four-wave-mixing field and a coupling of these fields with the driving laser field. A sharp onset of saturation of the parametric four-wave-mixing signals with sodium number density and a transition from a quadratic to a linear power dependence is observed. Both effects are explained in terms of the two-photon cancellation effect.
If an extended Na vapor column (heat pipe configuration) is subjected to strong laser pumping near two-photon resonance with 3D3/2,5/2 or 4D3/2,5/2 states at pressures above tens of millitorr, strong stimulated emissions are produced by amplified spontaneous emission (ASE) or stimulated electron in hyper-Raman scattering (SEHRS) and by phase matched parametric four-wave mixing (PFWM). These new electromagnetic fields that are generated within the near-resonant nonlinear medium can strongly influence the total atomic response and produce several saturation and total cancellation types of effect.
The suppression of forward-propagating stimulated hyper-Raman (SHR) emission is well studied in sodium vapor. Theory predicts that SHR emission to a state linked to the gound state by a one-photon transition is suppressed by an interference with a four-wave-mixing (FWM) emission that links that state to the ground state. Since FWM emission only propagates in the forward direction due to phase-matching considerations, only the forward SHR emission is suppressed. This has been previously demonstrated in sodium. An obvious corollary to this theory is that no suppression occurs if the state is not linked to the ground state by a one-photon transition. A serendipitous arrangement of energy levels in cesium allowed this corollary to be tested and confirmed here.
Experimental studies have been made of conjugate wave generation in a Na metal vapor heat pipe. Detailed measurements of gain profiles, pump beam absorption, and parametric wave generation at infrared frequencies for phase conjugation near the two-photon resonance with the Na 4d2D5/2 state, yield details of the effects of parasitic processes on degenerate four-wave mixing. Studies are conducted with an excimer-pumped dye laser system with ~4 ns pulses of < 10mJ/pulse, traversing Na vapor heat pipe. Included in the measurements are pump beam depletion, probe and conjugate beam intensities, and infrared light which is generated by the strong pump beams through stimulated Raman (SR) and amplified spontaneous emission processes. The role of ac Stark shifting in degenerate four-wave mixing near the 4d level is studied. We find a new effect involving a large contribution to the ac Stark effect from the internally generated SR photons. We observe a rapid onset with pressure of stimulated Raman emission accompanied by a dramatic increase in the ac Stark profile of the 4d level, and the sharp onset of gain saturation for the phase conjugate signal, due to the competition of these two processes. This effect results in an ac Stark coefficient which can be very nonlinear in laser power and Na pressure.