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Journal of Experimental and Theoretical Physics

Higher-order nonlinear susceptibilities for generation of optical radiation harmonics in atomic gases

Nikolai L. Manakov, V. D. Ovsyannikov

Published Nov 1, 1980• 3 citations
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A method is suggested for the calculation of the nonlinear susceptibility corresponding to the generation of second and third optical harmonics in atomic gases. The method is based on the use of the Green's function of an atomic optical electron in the computation of the composite matrix elements. The results are given of a numerical calculation of χ(–3ω;ω,ω,ω) and χ(–2ω;0,ω,ω) for hydrogen, alkali atoms, and inert gases at the frequencies of ruby and neodymium laser radiations and their second harmonics. A two-photon resonance in the generation of the third harmonics is considered.
It is commonly assumed that for low-intensity short optical pulses far from resonance, the third-order optical nonlinear response is instantaneous. We solve the three-dimensional time-dependent Schrödinger equation for the hydrogen atom and show that this is not the case: the polarization is not simply proportional to the cube of the electric field even at low intensities. We analyze the fundamental-frequency and third-harmonic nonlinear susceptibilities of hydrogen, investigate their dependence on intensity, and find that the delays in the Kerr response rapidly approach the femtosecond time-scale at higher intensities, while the delays in the third harmonic generation remain much lower. We also propose an experimental scheme to detect and characterize the above effects.
A study was made of the influence of autoionization-like resonances in the continuum, induced by strong optical radiation, on the nonlinear susceptibilities governing third harmonic generation and the optical activity of sodium vapor. It was demonstrated experimentally for the first time that it should be possible to study high-lying states of atoms and molecules by the method of nonlinear polarization spectroscopy of the fifth-order optical nonlinearity. The experimental results were compared with the theory. An analysis was made of the feasibility of using this effect for spectroscopy of the states in the continuum and for generation of short-wavelength radiation in gaseous media.