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Optics Letters

Correlated third-harmonic generation in I_2 using photon-echo process

C. Tai, Henry J. Simon

Published Mar 1, 1981• 5 citations
Publisher

Abstract

We report the application of third-harmonic generation (THG) to study photon-echo-associated coherent molecular states. Two temporally separated circularly polarized laser pulses are focused into a cell containing I(2) vapor to create the coherent dipole moments. A delayed oppositely circularly polarized pulse is then focused into the same region to generate the third harmonic. Since no THG can be produced by any individual pulse, correlated THG may easily be measured without using any fast detection scheme.

DOI
10.1364/ol.6.000133

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Journal of the Optical Society of America B•Mar 1, 2004•2 citations
We report the application of third-harmonic generation (THG) to study photon-echo-associated coherent molecular states. Two temporally separated circularly polarized laser pulses are focused into a cell containing I(2) vapor to create the coherent dipole moments. A delayed oppositely circularly polarized pulse is then focused into the same region to generate the third harmonic. Since no THG can be produced by any individual pulse, correlated THG may easily be measured without using any fast detection scheme.
A technique of third-harmonic generation (THG) with nonsynchronous pulses is applied to study the dynamics of resonant wave mixing. A circularly polarized laser pulse is focused into a cell containing I2{\mathrm{I}}_{2}I2​ vapor to create the coherent dipole moments. An oppositely circularly polarized pulse is then focused into the same region to generate the third harmonic. Since no THG is produced by any individual pulse, correlated THG can be easily measured without using any fast detection scheme. A theory is presented to explain the measured coherent lifetime of approximately 1 ns. The technique of wave mixing with two linearly polarized pulse is applied to study saturation in resonant THG and to measure the homogeneous relaxation rate of the molecular states. This technique is also applied to study the photon echo generating process.
Magnetic-field-induced resonant third-harmonic generation in I2{\mathrm{I}}_{2}I2​ with circularly polarized light is studied. With a magnetic field perpendicular to the propagating direction of the light, the axial symmetry is broken and the angular momentum is no longer conserved in such a system, and the third harmonic may be generated under such conditions. Quantum beats in photon-echo-like third-harmonic generation with nonsynchronous laser pulses are also studied. The intensity of the harmonic generated may be interpreted in terms of the interference between a molecule and itself as well as the interference between different molecules. The gyromagnetic ratio of the resonant states is measured.
A numerical investigation is made of third harmonic generation (THG) under conditions of two-photon resonance between the fundamental frequency and a selected transition in the atoms of a medium. It is shown that under conditions of coherent interaction between the pump pulse and the medium, a THG efficiency of ∼20% or higher may be achieved. In this case, THG in the form of high-power ultrashort pulses may be obtained. It is shown that experimental observation of similar effects in specific media should not present particular difficulties.
This work examines the use of higher order multiphoton resonances in higher harmonic generation together with judicious exploitation of coherent interaction properties to achieve efficient harmonic generation. A detailed experimental study on third harmonic generation in two photon resonant coherent interaction and a theoretical study on four photon resonant coherent interaction have been conducted. Two photon resonant coheren propagation in lithium vapor (2S-4S and 2S-3D interaction) has been studied in detail as a function of phase and delay of the interacting pulse sequence. Under coherent lossless propagation of 90 phase shifted pulse pair, third harmonic generation is enhanced. A maximum energy conversion efficiency of 1% was measured experimentally. This experiment shows that phase correlated pulse sequence can be used to control multiphoton coherent resonant effects. A larger two photon resonant enhancement does not result in more efficient harmonic generation, in agreement with the theoretical prediction. An accurate (to at least 0.5 A°) measurement of intensity dependent Stark shift has been done with the newly developed "interferometric wavemeter." Stark shifts as big as several pulse bandwidths (of picosecond pulses) result in a poor tuning of multiphoton resonance and become a limiting factor of resonant harmonic generation. A complete theory has been developed for harmonic generation in a four photon resonant coherent interaction. A numerical application of the theory to the Hg atom successfully interprets the experimental observations in terms of the phase dependent stimulated Raman scattering. With the intensity required for four photon resonant transition, the calculation predicts a dramatic Stark shift effect which completely destroys the resonance condition. This model provides a basis for the development of future schemes for efficient higher order coherent upconversion.
The work of this dissertation has been to prove that the coherence of multiphoton excitation can be studied by an appropriately phased and time delayed sequence of pulses. An application of this fundamental study of coherence has been made for the enhancement of third harmonic generation. The coherent recovery of the energy lost to the two photon absorption process enalled a larger propagation distance for the fundamental than in an interaction which is incoherent or coherent, but not using a 90 degree phase shifted pulse pair. Phase matching over this longer propagation distance gave an enhancement of third harmonic generation.
The effect of temporal coherent control on the two-photon resonant third-harmonic generation in the continuum of ionization of an atomic system is experimentally investigated by means of a pair of partially incoherent, identical laser pulses. The evidence of quantum interference in the third-harmonic generation, as a function of delay between pulses, is reported. The transition from a resonant to a nonresonant case is also shown. The results agree with the predictions of a recently published theoretical model showing that the onset of quantum interference appears to be related to the coherence time of the laser radiation that is much shorter than the pulse duration.