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

Four-Photon Resonant Third Harmonic Generation

Arlee V. Smith

Published Nov 20, 1985• 0 citations
Publisher

Abstract

The phenomenon of resonant enhancement of optical third harmonic generation near four-photon resonances is studied with the goal of understanding the nonlinear processes involved and evaluating them as a means of more efficiently generating coherent vacuum ultraviolet light.
DOI
10.1117/12.976141

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The ability to introduce additional resonances in the nonlinear optical susceptibility of a medium by the injection of an additional radiation field is an attractive possibility from the standpoint of efficient tunable frequency mixing processes in the VUV. The possibility of such processes suggest themselves in previous observations in atomic mercury where an enhancement of several orders of magnitude in the third harmonic generation efficiency has been reported when the input frequency is four-photon resonant with the 6S → 6D transition(1).
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As a succession of two pulses propagates through a medium which exhibits a resonance (single or multiphoton), the resonant parts of the susceptibility will depend on the relative phase of the two pulses, provided the delay between the pulses is shorter than the phase relaxation time of the interaction. As a result of this "coherent interaction", the reradiation of the sample (the fluorescence, the absorption and the generation of harmonics) will be a periodic function of the phase difference and delay between the two pulses of the sequence 1. The study of these coherent effects is important, because one expect to find conditions under which the maximum harmonic conversion to much shorter wavelengths can be greatly enhanced 2. The presence of the multiphoton resonance enhances the nonlinear susceptibility responsible for the harmonic generation, but reduces also the maximum achievable conversion efficiency because of resonant losses (depletion of the fundamental by multiphoton absorption). The latter effect can be eliminated by a judicious choice of the pulse sequencing and phasing. In addition to demonstrating, for the first time, coherent interaction enhancement in harmonic generation, the data of third harmonic versus relative phase of the pulse sequences enable us to measure the phase angle of the third order susceptibility (hence the contribution of the continuum relative to that of the resonance).