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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Suppression and shifting of odd-photon resonant excitations and stimulated hyper-Raman emissions

W. R. Garrett, M. G. Payne

Published Apr 1, 1992• 0 citations
Publisher

Abstract

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.

DOI
10.1117/12.58107

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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.
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.
Discriptions are given of recent theoretical and experimental results of dramatic effects, during the interval of the excitation pulse, in optically pumped stimulated emissions (OPSE). Forward-directed OPSE from a two-photon resonantly excited state to a lower state which is also coupled to the ground state is strongly suppressed and backward emissions are frequency shifted. Surprisingly, the effects are caused by an interference from a wave-mixing field. Several other implications of this effect are given and, on the basis of this phenomenon, several puzzling ASE observations mentioned in other published work are noted and clarified.
We present a theory for two- and three-photon excitation, optical shifting, and four-wave mixing when a first laser is tuned onto, or near, a two-photon resonance and a second much more intense laser is tuned near or on resonance between the two-photon resonance and a second excited state. When the second excited state has a dipole-allowed transition back to the ground state and the concentration is sufficiently high, a destructive interference is produced between three-photon coupling of the ground state and the second excited state and one-photon coupling between the same states by the internally generated four-wave mixing field. This interference leads to several striking effects. For instance, as the onset of the interference occurs, the optical shifts in the two-photon resonance excitation line shape become smaller in copropagating geometry so that the line shapes for multiphoton ionization enhanced by the two-photon resonance eventually become unaffected by the second laser. In the same range of concentrations the four-wave mixing field evolves to a concentration-independent intensity. With counterpropagating laser beams the line shape exhibits normal optical shifts like those observed for both copropagating and counterpropagating laser beams at very low concentrations. The theoretical work presented here extends our earlier works by including the effect of laser bandwidth and by removing the restriction of having the second laser be tuned far from three-photon resonance. In this way we have now included, as a special case, the effect of both laser bandwidth and interference on laser-induced transparency. Unlike other effects related to odd-photon destructive interference, the effect of a broad bandwidth is to bring about the predicted effects at much lower concentrations. Studies in rubidium show good agreement between theory and experiment for both ionization line shapes and four-wave mixing intensity as a function of concentration.
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.