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The Journal of Chemical Physics

Cooperative radiationless relaxation

Marvin M. Miller, Francis K. Fong

Published Aug 1, 1973• 7 citations
Publisher

Abstract

The theory of cooperative nonradiative multiphonon relaxation by a multiatom system is developed in the framework of the adiabatic approximation in analogy with the Dicke theory of superradiance. As a concrete example, the nonradiative decay of impurity centers doped in a crystal lattice is considered. The assumptions underlying the theoretical development and the possibility of the experimental realization of this effect are discussed.

DOI
10.1063/1.1680211

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The theory of cooperative nonradiative multiphonon relaxation by a multiatom system is developed in the framework of the adiabatic approximation in analogy with the Dicke theory of superradiance. As a concrete example, the nonradiative decay of impurity centers doped in a crystal lattice is considered. The assumptions underlying the theoretical development and the possibility of the experimental realization of this effect are discussed.
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The Dicke theory of coherent spontaneous emission is generalized by means of group-theoretical methods. Effects of superradiation and the structure of coherent responses of an equilibrium medium to pulsed excitation are considered. A method of calculating cooperative effects in second-order perturbation theory is developed. The role of collective properties of a system of radiators in experiments with high power exciting radiation is discussed. Some "anomalous" features of stimulated Raman scattering are accounted for.
We study effects of direct interatomic interaction on cooperative processes in atom-photon dynamics. Using a model of two-level atoms with Ising-type interaction as an example, it is demonstrated that interparticle interaction can promote cooperative radiative relaxation. For small number of atoms this results in inhibition of incoherent spontaneous decay leading to the regime of collective pulse relaxation. Above superradiance threshold increase in delay time and enhancement of superradiance is occurred. In the case of strong interaction (as compared to excitation energy of an atom) transition to the regime of multiphoton relaxation occurs, which we discuss using a simple model of two atoms in a high-Q single mode cavity. It is shown that such transition is accompanied by Rabi oscillations involving many-atom multiphoton states. Dephasing effect of dipole-dipole interaction and solitonic mechanism of relaxation are discussed as well.
The Dicke superradiance on vibronic transitions of impurity crystals is considered. It is shown that parameters of the superradiance (duration and intensity of the superradiance pulse and delay times) on each vibronic transition depend on the strength of coupling of electronic states with the intramolecular impurity vibration (responsible for the vibronic structure of the optical spectrum in the form of vibrational replicas of the pure electronic line) and on the crystal temperature through the Debye-Waller factor of the lattice vibrations. Theoretical estimates of the ratios of the time delays, as well as of the superradiance pulse intensities for different vibronic transitions well agree with the results of experimental observations of two-color superradiance in the polar dielectric KCl:O 2 − . In addition, the theory describes qualitatively correctly the critical temperature dependence of the superradiance effect.
We study effects of direct interatomic interaction on cooperative processes in atom-photon dynamics. Using a model of two-level atoms with Ising-type interaction as an example, it is demonstrated that interparticle interaction combined with atom-field coupling can introduce additional interatomic correlations acting as a phase synchronizing factor. For the case of weakly interacting atoms with $J<\ensuremath{\hbar}{\ensuremath{\omega}}_{0}$, where JJJ is the interparticle coupling constant and ${\ensuremath{\omega}}_{0}$ is the atomic frequency, dynamical regimes of cooperative relaxation of atoms are analyzed in the Born-Markov approximation both numerically and using the mean field approximation. We show that interparticle correlations induced by the direct interaction result in inhibition of incoherent spontaneous decay leading to the regime of collective pulse relaxation which differs from superradiance in nature. For superradiant transition, the synchronizing effect of interatomic interaction is found to manifest itself in enhancement of superradiance. When the interaction is strong and $J>\ensuremath{\hbar}{\ensuremath{\omega}}_{0}$, one-particle one-photon transitions are excluded and transition to the regime of multiphoton relaxation occurs. Using a simple model of two atoms in a high-QQQ single mode cavity we show that such transition is accompanied by Rabi oscillations involving many-atom multiphoton states. Dephasing effects of dipole-dipole interaction and solitonic mechanism of relaxation are discussed.