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Physical Review A

Suppression of forward-propagating stimulated hyper-Raman emission in cesium vapor due to four-wave-mixing interference

Mary Anne Moore, D.M. Boye, Girish Gvalani

Published Apr 1, 1993• 1 citation
Publisher

Abstract

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.

DOI
10.1103/physreva.47.3210

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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 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.
When a principal atomic transition (dipole allowed from the ground state) is driven by odd- multi-photon excitation or by stimulated hyper-Raman scattering, a nonlinear multi-wave mixing field is generated at the transition frequency. A number of dramatic effects on such odd-photon mediated processes can ensue as a result of the internally generated wave-mixing fields. Excellent agreement between theory and experimental studies in Xe and in metal vapors is illustrated for a number of predicted effects including: suppression and strong shifting of resonance lines and hyper-Raman emissions under single and multi-laser excitation. We illustrate the dependence of the interference-related effects on pressure, oscillator strength, wavelength combination and relative propagation directions of pump laser beams. Contrary to most other nonlinear effects, we show that none of the features (in the semi-classical regime) depends on the intensity of the driving laser field.
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.
Two-photon-resonant excitation of the sodium 3d3d3d level can lead to the generation of new frequencies either by amplified spontaneous emission at the $3d\ensuremath{\rightarrow}3p$ transition frequency or by a resonantly enhanced four-wave mixing process. Competition between these two processes has been observed. The four-wave mixing process can suppress amplified spontaneous emission by preventing the excitation of the 3d3d3d level due to an interference between two different pathways connecting the ground (3s3s3s) and 3d3d3d states.