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Optics and Spectroscopy

Effect of squeezed vibrational states on the optical properties of molecular systems in a field of laser radiation

É. P. Sineavsky, E.Yu. Kanarovsky, A. M. Rusanov

Published Jan 1, 2003• 0 citations
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Abstract

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.

DOI
10.1134/1.1540198

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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.
Squeezing of radiation is a purely quantum mechanical phenomenon which has no classical counterpart. This quantum effect is expected to manifest itself in optical processes in which the nonlinear response of the system to the radiation field plays an important role. The concept of squeezing started in mid 1980s. Since then there has been an enormous upsurge of interest in this field owing to its low noise property. In the present paper various aspects of squeezing of radiation are studied and possible means of generation of squeezed light in which the quantum fluctuations are reduced below shot noise limit are investigated. The amplitude of the electric field of a mode of an electromagnetic field is always associated with quantum mechanical fluctuations. Squeezing states are characterised by reduced quantum fluctuations in one quadrature component of the field at the expense of increased fluctuations in the other noncommuting component. A fully quantum mechanical approach is followed. In the present paper we intend to review different aspects of squeezing and higher order squeezing in higher order Raman processes as well as in multiwave mixing processes. A comparative study between different processes are made which will pave a way for easier generation of squeezed light.
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.