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Physical Review A

Resonant wave mixing in I2 with nonsynchronous pulses

C. Tai

Published May 1, 1981• 9 citations
Publisher

Abstract

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 ${\mathrm{I}}_{2}$ 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.

DOI
10.1103/physreva.23.2462

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Analysis of THG modes for femtosecond laser pulse

Vyacheslav A. Trofimov, Pavel S. Sidorov

THG is used nowadays in many practical applications such as a substance diagnostics, and biological objects imaging, and etс. With developing of new materials and technology (for example, photonic crystal) an attention to THG process analysis grow. Therefore, THG features understanding are a modern problem. Early we have developed new analytical approach based on using the problem invariant for analytical solution construction of the THG process. It should be stressed that we did not use a basic wave non-depletion approximation. Nevertheless, a long pulse duration approximation and plane wave approximation has applied. The analytical solution demonstrates, in particular, an optical bistability property (and may other regimes of frequency tripling) for the third harmonic generation process. But, obviously, this approach does not reflect an influence of a medium dispersion on the frequency tripling. Therefore, in this paper we analyze THG efficiency of a femtosecond laser pulse taking into account a second order dispersion affect as well as self- and crossmodulation of the interacting waves affect on the frequency conversion process. Analysis is made using a computer simulation on the base of Schrödinger equations describing the process under consideration.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•May 16, 2017•1 citation
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.
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.
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.
The intensity of the resonant third-harmonic generation in I2{\mathrm{I}}_{2}I2​ vapor is found to decrease with increasing strength of an external magnetic field even when the exciting light is polarized parallel to the magnetic field. This effect is explained with a theory based on the interference between different molecules. The gyromagnetic ratio of the excited state is determined in this work. This technique may also be applied to study the mechanism of the various processes of saturation in resonant wave mixing.
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.
THG is used nowadays in many practical applications such as a substance diagnostics, and biological objects imaging, and etс. With developing of new materials and technology (for example, photonic crystal) an attention to THG process analysis grow. Therefore, THG features understanding are a modern problem. Early we have developed new analytical approach based on using the problem invariant for analytical solution construction of the THG process. It should be stressed that we did not use a basic wave non-depletion approximation. Nevertheless, a long pulse duration approximation and plane wave approximation has applied. The analytical solution demonstrates, in particular, an optical bistability property (and may other regimes of frequency tripling) for the third harmonic generation process. But, obviously, this approach does not reflect an influence of a medium dispersion on the frequency tripling. Therefore, in this paper we analyze THG efficiency of a femtosecond laser pulse taking into account a second order dispersion affect as well as self- and crossmodulation of the interacting waves affect on the frequency conversion process. Analysis is made using a computer simulation on the base of Schrodinger equations describing the process under consideration.
THG is used nowadays in many practical applications such as a substance diagnostics, and biological objects imaging, and etс. With developing of new materials and technology (for example, photonic crystal) an attention to THG process analysis grow. Therefore, THG features understanding are a modern problem. Early we have developed new analytical approach based on using the problem invariant for analytical solution construction of the THG process. It should be stressed that we did not use a basic wave non-depletion approximation. Nevertheless, a long pulse duration approximation and plane wave approximation has applied. The analytical solution demonstrates, in particular, an optical bistability property (and may other regimes of frequency tripling) for the third harmonic generation process. But, obviously, this approach does not reflect an influence of a medium dispersion on the frequency tripling. Therefore, in this paper we analyze THG efficiency of a femtosecond laser pulse taking into account a second order dispersion affect as well as self- and crossmodulation of the interacting waves affect on the frequency conversion process. Analysis is made using a computer simulation on the base of Schrödinger equations describing the process under consideration.