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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Multiphoton processes in molecules with excited vibrational squeezed states in a strong electromagnetic field

V.A. Kovarsky, Alexandr V. Belousov, O. B. Prepelitsa, S. A. Baranov

Published Mar 5, 1999• 0 citations
Publisher

Abstract

The preparation of the squeezed vibrational states in molecules may be realized due to excitation by short intensive electromagnetic pulses or by means of hot proton impact. New types of multiphoton processes have appeared: the combined multiphoton-multivibron processes, the intensity of such type transitions are apparently depended on parameters of squeezed vibrational states. The multiphoton excitation, high harmonic generation and light scattering processes in molecules are analyzed.

DOI
10.1117/12.341460

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The preparation of the squeezed vibrational states in molecules may be realized due to excitation by short intensive electromagnetic pulses or by means of hot proton impact. New types of multiphoton processes have appeared: the combined multiphoton-multivibron processes, the intensity of such type transitions are apparently depended on parameters of squeezed vibrational states. The multiphoton excitation, high harmonic generation and light scattering processes in molecules are analyzed.
Specific features of optical and nonradiative transitions in molecular systems in the field of an intense electromagnetic wave are studied with account of squeezed vibrational states. It is shown that a field of laser radiation considerably enhances the tunneling processes in electronic vibrational systems and makes it possible to obtain the generation of higher harmonics. Conditions are found under which squeezed vibrational states can lead to some stabilization of excited electronic states with respect to the processes of luminescence.
The dynamics of high-intense laser fields at coherent Raman self-scattering are investigated by the use of numerical simulation. The processes under investigation take place at the Raman scattering on electronic states in atoms with transition to be forbidden in electro-dipole approximation, on vibrational or rotational states in molecules, on states connected with the spin flip and other. It is found that the threshold intensities exist provided that the pulse duration is smaller than dephasing time of the Raman transition in the medium. Under this, the following processes occur: an effective generation of the high-order harmonics comes up; the plateau forms in the harmonic spectrum. The maximum which arises on this plateau shifts to the higher-harmonic numbers in case of the higher threshold intensities of the pulse. It is shown how the transformation of the initial pulse intensity into high-order harmonics intensity can be considerably increased with the different initial parameters of the pulse and the medium.
A review is given of experimental and theoretical achievements in studies of multiphoton spontaneous scattering processes in atomic and molecular media. An analysis is made of integral multiphoton scattering, particularly of scattering in statistically inhomogeneous media with short-range quasiorder. A study of the intensity of the noncoherent multiphoton scattering component provides direct information on the nonlinear polarizability of atoms and molecules whilst the coherent component is associated with various atomic and molecular correlation mechanisms. An analysis of the spectra of elastic and inelastic multiphoton scattering processes yields information on the translational and rotational motion of the molecules. In particular, it is possible to measure the higher-order rotational relaxation times and to verify the adequacy of the various stochastic models of molecular motion. Observations of the spectral lines of three- or more-photon scattering, which obeys new selection rules, yield detail on the fine structure of the molecules and their linear and nonlinear vibrations. Examples are given of the most interesting spectra of three- or more-photon scattering in gases, liquids, and crystals obtained in singleand multichannel systems. The stochastic theory of multiphoton scattering in liquids is discussed, using the spherical tensor concept. The derived general expression reduces to known results for certain cases.