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Quantum Electronics

Determination of the third-order correlation function by noncollinear two-beam third-harmonic generation

Grigorii G Grigoryan, A. O. Melikyan, David G. Sarkisyan, A. S. Sarkisyan

Published Mar 31, 1995• 2 citations
Publisher

Abstract

A method was developed for determination of the third-order correlation function G (3) (0, τ) on the basis of noncollinear two-beam generation of the third harmonic in a cell containing an atomic metal vapour. The advantages of the proposed method are its simplicity, validity in a wide range of wavelengths, and ability to reveal the asymmetry of an ultrashort pulse in one laser shot. A criterion of the reproducibility of the laser output pulses from one shot to the next was established. In the case of smooth laser pulses it is possible to select a convenient analytic model for the function G (3) (0, τ). The capabilities of the method are demonstrated by the application to a picosecond YAIO 3 : Nd 3+ laser.

DOI
10.1070/qe1995v025n03abeh000340

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A method was developed for determination of the third-order correlation function G (3) (0, τ) on the basis of noncollinear two-beam generation of the third harmonic in a cell containing an atomic metal vapour. The advantages of the proposed method are its simplicity, validity in a wide range of wavelengths, and ability to reveal the asymmetry of an ultrashort pulse in one laser shot. A criterion of the reproducibility of the laser output pulses from one shot to the next was established. In the case of smooth laser pulses it is possible to select a convenient analytic model for the function G (3) (0, τ). The capabilities of the method are demonstrated by the application to a picosecond YAIO 3 : Nd 3+ laser.
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 simple method of measuring atomic level populations was implemented by comparing the energies of the third harmonic generated by two identical ultrashort pulses. When the first ultrashort pulse induces a process that removes some of the atoms from the ground (initial) level for third harmonic generation, the energy of the second third-harmonic pulse Wth2 becomes lower than Wth1 as a result of a reduction in the number of atoms. In the experiments K = Wth1 / Wth2 increased as the ultrashort pulse intensity increased. Experimental investigations and theoretical estimates showed that the most probable process causing a reduction in the population of the 62S1/2 level of cesium atoms was multiphoton ionization. It was found that the degree of multiphoton ionization could be estimated from K.
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.
Three-photon resonance enhancement of third-harmonic generation and multiphoton ionization have been studied in xenon under excitation by the Bessel and the focused annular laser beams. It has been shown that the transformation of a Gaussian beam into a Bessel or an annular one leads to significant changes of third-harmonic excitation profiles and ionization spectra. These changes result from a principal difference of the beams, where either collinear (Gaussian beams) or noncollinear (Bessel and focused annular beams) excitation geometries are realized. It has been shown that the noncollinear ring-type phase matching shifts the maximum of the generated third harmonic to the longer wavelength toward the atomic resonance. Numerical calculations of third-harmonic excitation spectra have been carried out and compared with experimental results. The efficiency of frequency tripling in collinear and noncollinear excitation geometries have been compared. Cancellation of the three-photon 6s6s6s resonance and the influence of harmonic photons on the excitation of the four-photon 4f4f4f resonance in the Bessel beams are discussed.
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.