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International Conference on Ultrafast Phenomena

Femtosecond Four-Wave Mixing for Molecule Based Computation

Vadim V. Lozovoy, Igor Pastirk, Matthew Comstock, Katherine A. Walowicz, Marcos M. Dantus

Published Jan 1, 2002• 0 citations
Publisher

Abstract

Three shaped non-degenerate pulses can initialize a manifold of rovibronic states, store information, and perform a computation. Results from experiments carried out on molecular iodine will be presented.
DOI
10.1364/up.2002.tue16

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The object of this study is to quantitatively elucidate the laser-power dependence in transient degenerate four-wave mixing (DFWM) with an emphasis on the high laser-pump intensity region. We discuss our investigation on the power dependence of transient DFWM by taking gas-phase iodine (I2{\mathrm{I}}_{2}I2​) molecules as a testing example. The distinct physical feature is that in the high-power laser pump, where both laser-pulse duration and the inverse of pump rate are much shorter than the molecular population relaxation time, the steady-state DFWM theory of Abrams and Lind [Optical Phase Conjugation, edited by R. A. Fisher (Academic, New York, 1983), Chap. 8, pp. 211--284; Opt. Lett. 2, 94 (1978); 3, 205 (1978)] is not appropriate. The prediction by the steady-state theory has shown the DFWM to decrease with increasing laser-pump intensity as a function of 1/Ilaser{\mathrm{I}}_{\mathrm{laser}}Ilaser​, which disagrees with the saturation behavior observed in the experiment. To elucidate the dependence of DFWM on the laser pump intensity, a non-steady-state extension of the nonperturbative theory of Abrams and Lind is required. The non-steady-state theoretical result will be shown to be in good agreement with the experimental power dependence at resonance transient DFWM especially in the high-power pump region.