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physica status solidi (b)

Redistribution of Resonance Bonds and Dynamics of Two‐Center Self‐Trapping in Rare‐Gas Crystals

I. Ya. Fugol’, A. M. Ratner, Е. Ю. Тарасова

Published Mar 1, 1992• 6 citations
Publisher

Abstract

Abstract It is shown that in the process of the exciton two‐center self‐trapping the resonance bonds generating a free exciton state are redistributed so that the total resonance contribution to the energy increases. 50% of the electronic excitation is concentrated inside a two‐center quasimolecule close to the self‐trapping threshold. The rest is distributed in neighbouring atoms, resulting in a generation of weaker extrinsic bonds along with the intermolecular resonance one. The attendant deformation of the molecular term produces a decrease in the self‐trapping barrier and an appreciable increase in its transparency.

DOI
10.1002/pssb.2221700116

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Abstract It is shown that in the process of the exciton two‐center self‐trapping the resonance bonds generating a free exciton state are redistributed so that the total resonance contribution to the energy increases. 50% of the electronic excitation is concentrated inside a two‐center quasimolecule close to the self‐trapping threshold. The rest is distributed in neighbouring atoms, resulting in a generation of weaker extrinsic bonds along with the intermolecular resonance one. The attendant deformation of the molecular term produces a decrease in the self‐trapping barrier and an appreciable increase in its transparency.
This paper presents the first results on a correlation between the luminescence of excitons self-trapped at the surface of solid argon and desorption. Recently, Jennison and Emin showed that localisation of electronic excitation at the surface of the crystal is an essential condition, and that especially self-trapping of excitons can lead to desorption of neutral atoms1. In the case of solid argon, self-trapping of excitons at the surface has been proved to exist2. It leads to characteristic luninescence bands which were also measured with electron excitation techniques3. Two of them exactly coincide with the 3P1 and 1P1 emission of isolated argon atoms and were not understood up to now. In the course of this work it turned out that they are emitted by desorbing neutral atoms.
We have examined the luminescence from highly excited self-trapped one-center states, the relaxation processes of the band excitations, and the mechanisms of formation of highly excited quasiatomic centers in low-temperature crystals of the light rare gases and their solid solutions. The fundamental channel of population of highly excited emitting centers involves hole self-trapping with formation of two-center R2+ states; dissociative recombination of these forms one-center np5(n + 1)p excitations. We discuss the effect of self-trapping of highly excited states on the population of the lowest emitting centers in neon and argon crystals.
Abstract The luminescence of Ne* centers in solid Ne is investigated. The samples are excited with synchrotron radiation in the excitonic range. By an appropriate selection of the excitation energy and by time correlated measurement of the emission spectra, overlapping luminescence bands are separated and assigned to Ne* centers in different electronic states (1P1, 3P1, 3P2) and different environments in the bulk and at the surface of the solid. Lifetime measurements and excitation spectra of spectrally selected luminescence bands support the assignments, Electronic relaxation from n ≧ 2 free excitons to the n = 1 state is found to be less effective than exciton trapping into Ne* centers. Resonance fluorescence of free Ne* atoms indicates a close connection between exciton trapping and desorption.
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.