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Soviet Journal of Quantum Electronics

Coherent interaction between high-power light pulses and exciton–impurity centers in molecular crystals

Leonas Valkūnas, É Gaĭzhauskas, I A Poluéktov, Yurii M Popov

Published Sep 30, 1979• 0 citations
Publisher

Abstract

A theoretical investigation is made of the coherent interaction between high-power optical radiation and excitons in impurity-doped molecular crystals. A self-consistent system of equations is obtained for the medium and the optical field. It is shown that, under certain conditions, the distances over which coherence effects are observed, decrease sharply. An analysis is made of the specific conditions for the experimental observation of these effects.

DOI
10.1070/qe1979v009n09abeh009468

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A theoretical investigation is made of the coherent interaction between high-power optical radiation and excitons in impurity-doped molecular crystals. A self-consistent system of equations is obtained for the medium and the optical field. It is shown that, under certain conditions, the distances over which coherence effects are observed, decrease sharply. An analysis is made of the specific conditions for the experimental observation of these effects.
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The phenomenon of self-induced transparency (SIT) in the exciton range of the spectrum consists of the propagation through the crystal of solitary wave packets of coherent excitons and photons with anomalous small losses. In the running frame of reference at the site occupied by the soliton a single aperiodic transformation of photons into excitons and a reverse motion of the energy into the field takes place. The solutions of the SIT equations have been received in the slowly-varying amplitude approximation. Taking into account the phase modulation, the authors have shown the appearance of the branch of the carrier wave frequency with anomalous dispersion not only at the given pulse width but at the given pulse amplitude. They have also found the exact solution of the above mentioned equations taking into account the effect of saturation of the dipole momentum transition from the crystal ground state to the exciton state. It leads to the increasing of the soliton time width, to the decreasing of its amplitude and worsens the SIT observation.
Exciton self-trapping in a molecular medium is considered within a self-consistent model taking into account the change in the dipole moment as a result of a displacement of molecules and the resonance interaction with an electromagnetic field. New mechanisms and specific features of the formation of localized structures in quasi-one-dimensional molecular structures are investigated. It is shown that the dependence of the dipole moment on molecular vibrations leads to new conditions for exciton self-trapping and intrinsic optical bistability, as well as for the formation of electromagnetically induced transparency. The theory proposed is used to explain the specific features of exciton self-trapping in a conjugated polymer and J aggregates of dyes under the action of an external laser field.