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Chemical Physics Letters

Effects of collective emission on multiphoton excitation and ionization near a three-photon resonance

M. G. Payne, W. R. Garrett, Howard C. Baker

Published Nov 1, 1980• 82 citations
Publisher
DOI
10.1016/0009-2614(80)80557-4

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Three-photon resonance enhancement of third-harmonic generation and multiphoton ionization is treated for a slab geometry configuration. Striking pressure effects which become important at concentrations $n\ensuremath{\gtrsim}{10}^{12}$ /cm3{/\mathrm{c}\mathrm{m}}^{3}/cm3 for narrow-bandwidth short-pulse lasers are predicted for both the third-harmonic signal and the multiphoton ionization. For example, part of the third-harmonic signal exists the slab simultaneously with the laser pulse while another part is time delayed for small detunings from resonance. At intermediate detuning from the three-photon resonance the two parts can interfere. Multiphoton ionization yields near three-photon resonance are strongly suppressed under certain conditions, and peaks may occur for proper detunings on both sides of the three-photon resonance. A detailed experimental verification is suggested for Xe.
In connection with a recent experiment of vacuum-ultraviolet generation in multiphoton resonant ionization of xenon at increasing pressure, a model is elaborated to account for the simultaneous effect of a laser excitation tuned near a three-photon resonance and a pressure-induced emission from the resonant state to the ground state. Under certain assumptions usual in various super-radiance treatments, a system of Bloch equations is derived and numerically solved. The dependence of the ionization probability and third-harmonic production versus the interaction time, gas pressure, dynamical detuning, and laser intensity is extensively studied. A transition between a high and low ionization rate is observed when the pressure increases simultaneously with the disappearance of Rabi oscillations and a saturation of third-harmonic generation. An order-of-magnitude calculation reveals that such phenomena are accessible to experiment and a qualitative comparison with the above-mentioned results in xenon is found to be satisfactory.