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arXiv:physics/0302059 · Optics and Spectroscopy

On the theory of vibronic superradiance

A. P. Saǐko

Published Aug 1, 2002• 2 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1134/1.1503754

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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.
Abstract For the first time peculiarities of the formation of Dicke optical superradiance are studied experimentally and theoretically in a pyrene‐doped biphenyl crystal under active phonon effect (the energy level is 1Ag−1B2u; wavelength 373.93 nm; pyrene concentration 0.25 mol%; temperature 1.5 to 4.2 K). The possibilities of this phenomenon to obtain spectroscopic data are demonstrated. The pseudolocalized phonon lifetime τphon and the activation energy ΔE are estimated to ΔE = (7 ± 3) cm−1 and τphon = 2 to 20 ps by the temperature dependence of the superradiance intensity.
The problem of resonant interaction between an electromagnetic radiation field and a vibronic system, such as a molecule or a localized electronphonon system, is considered. The vibronic coupling is assumed to result from displaced and distorted potential energy surfaces for the vibrational motion in the electronic quantum states involved in the resonant interaction with the radiation field. Furthermore, the vibrational energy relaxation is taken into account without assumptions about Markovian-type relaxation. In order to study correlation properties of higher than second order in the electric field strength of the light emitted a method of calculation of the expectation value of an arbitrary product combination of effective time evolution operators of the vibronic system is developed. The calculations are performed by utilizing Feynman's disentangling and operator ordering techniques and yield closed solutions in the low-temperature limit. The theory is used for studying the intensity and the normally ordered intensity correlation function of the resonance fluorescence light from a two-atom molecule excited by a relatively weak laser field, which undergoes phase fluctuations. It is shown that the vibronic coupling can give rise to an anticorrelation effect which is substantially stronger than in the case of resonance fluorescence from an atom. For the case of small vibrational damping a general formula which directly connects the asymptotic long-time behaviour of the normalized intensity correlation function with the vibrational relaxation in the molecule is deduced. It should be convenient for the determination of very small vibrational decay rates.
The paper describes experimental investigations of two-color optical super-radiance (SR) in LaF3:Pr3+ crystal. Optical excitation was made on the transition 3P0- 3H4(0) at liquid helium temperature. When the power of the pumping 10ns-pulse was higher than a certain threshold, the resonant medium emitted an optical SR pulse on 3P0-3H4(0) transition with a duration of 8-10 ns in the direction of the pumping pulse delayed in time by 12-15 ns with respect to the pumping pulse. When the peak power of the pumping pulse increases up to 40 kW, an SR pulse was also observed for the 3P0-3H6(1) transition. The delay time of this pulse was about 30 ns. Thus, the two-color SR in the employed crystal was observed.
A simple theoretical description of vibrational coherence decay in isotopically mixed molecular crystals at low temperatures is presented. Dephasing due to impurity scattering is shown to be a slower than exponential decay process for optically excited vibrons lying near band singularities, by analogy with the theory of coherence loss in weakly disordered crystals [I. I. Abram and R. M. Hochstrasser, J. Chem. Phys. 72, 3617 (1970)]. When the nature of the initially excited state is properly taken into account, the rate constant for population decay displays an unexpected interplay between trapping and self-relaxation which can, in principle, lead to a nonmonotonic dependence of the relaxation rate with impurity concentration. Our results are related to recent time resolved CARS measurements in low temperature molecular crystals.