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AIP conference proceedings

New features of strong suppression and shifting phenomena in resonant excitations and stimulated emissions

W. R. Garrett

Published Jan 1, 1993• 0 citations
Publisher

Abstract

Descriptions are given of recent theoretical and experimental results of dramatic effects, during the interval of the excitation pulse, in optically pumped stimulated emissions (OPSE). [W. R. Garrett, Phys. Rev. Lett. (in press).] 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.

DOI
10.1063/1.45056

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Optics Letters•Nov 1, 1987•6 citations
Descriptions are given of recent theoretical and experimental results of dramatic effects, during the interval of the excitation pulse, in optically pumped stimulated emissions (OPSE). [W. R. Garrett, Phys. Rev. Lett. (in press).] 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.
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.
Theoretical and experimental presentations are given of a drastic suppression, during the interval of the excitation pulse, of forward-directed optically pumped stimulated emission from a two-photon resonantly excited state to a lower state which is also coupled to the ground state. The effect is caused by a self-induced interference from the difference-frequency mixing field that is generated during the time that the excitation fields are present. Several other implications of this effect are given and some puzzling observations in other studies are noted and clarified.
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.
A semiclassical dynamic theory of the nonlinear propagation of a few interacting intense light pulses is applied to study the nonlinear counterpropagation of amplified spontaneous emission (ASE) induced by three-photon absorption of short intense laser pulses in a chromophore solution. Several important results from the modeling are reached for the ASE process developing in the regime of strong saturation. Accounting for ASE in both forward and backward directions with respect to the pump pulse results in a smaller efficiency of nonlinear conversion for the forward ASE compared with the case in which forward emission is considered alone, something that results from the partial repump of the absorbed energy to the backward ASE component; the overall efficiency is nevertheless higher than for the forward emission considered alone. The efficiency of nonlinear conversion of the pump energy to the counterpropagating ASE pulses is strongly dependent on the concentration of active molecules so that a particular combination of concentration versus cell length optimizes the conversion coefficient. Under certain specified conditions, the ASE effect is found to be oscillatory; the origin of oscillations is dynamical competition between stimulated emission and off-resonant absorption. This result can be considered one of the possible explanations of the temporal fluctuations of the forward ASE pulse [Nature 415, 767 (2002)].
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.
We have observed, for the first time to our knowledge, stimulated emission in atomic-copper vapor that is excited by a resonant tunable laser beam. One of the important and interesting results obtained in this experiment is that excitation of the (2)P(1/2) level of the copper atoms generates strong amplified spontaneous emission (ASE) for both(2)P(1/2)-(2)D(3/2) and (2)P(3/2)-(2)D(5/2) transitions. This is the first reported direct experimental evidence observed for collisional mixing between the (2)P(1/2) and (2)P(3/2) levels in a copper-vapor laser. Excitation of the (2)P(3/2) level induces substantially weaker ASE for the (2)P(1/2)-(2)D(3/2) transition. In addition, we observed collision-induced ASE for both transitions over a wide range of detuning of the pump frequency. The preliminary results of the experiment are presented, and the implications of the results for high-pressure copper-vapor lasers are discussed.