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Theoretical and Mathematical Physics

Kinetics of two-photon superradiance in the case of damped polarization

A. A. Bakasov, N. N. Bogolyubov, A. S. Shumovskiǐ, Vyacheslav I. Yukalov

Published Sep 1, 1987• 2 citations
Publisher
DOI
10.1007/bf01018306

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The Journal of Chemical Physics•Jun 1, 1989•7 citations
A theoretical model for superradiant damping effect in inhomogeneously broadened media and its application to photon-echo problems are discussed. Only optically thin systems are considered, and all nonradiative relaxation mechanisms are neglected. Numerical calculations are performed for a very wide square inhomogeneous line shape and square applied pulses. It is shown that excitation of the system becomes increasingly difficult as the superradiant lifetime ${\ensuremath{\tau}}_{s}$ becomes comparable with T2∗{T}_{2}^{*}T2∗​. The energy reradiated after the end of the exciting pulse is considerable for ${\ensuremath{\tau}}_{s}\ensuremath{\approx}{T}_{2}^{*}$ and for some applied pulse areas. Two-pulse sequences produce multiple echoes as the microscopic polarizations spontaneously rephase. The first-echo amplitude maximum is found to occur for first-applied-pulse areas increasingly above $\frac{1}{2}\ensuremath{\pi}$ as ${\ensuremath{\tau}}_{s}$ decreases. For a given first-pulse area, the echo intensities increase initially as ${\ensuremath{\tau}}_{s}$ decreases (negligible damping) and finally decrease and vanish (important damping). The ratio of the second- to first-echo amplitudes is found to be proportional to $\frac{{T}_{2}^{*}}{{\ensuremath{\tau}}_{s}}$ for small superradiance levels and to decrease when ${\ensuremath{\tau}}_{s}$ approaches T2∗{T}_{2}^{*}T2∗​. An approximate estimate of this ratio is derived for the region of linearity in $\frac{{T}_{2}^{*}}{{\ensuremath{\tau}}_{s}}$.
We numerically investigate optical dephasing from as many as 500 interacting two-level absorbers by making the semiclassical approximation on the radiation–matter interaction which includes retarded dipole–dipole coupling and superradiant coupling. We calculate the superradiant decay rate following single pulse optical excitation, the photon echo decay and the fluorescence. By carrying out an expansion to the second order in time we demonstrate a fundamental difference between the homogeneous free-induction decay and photon echo decay which is due to radiation damping. We show that an echo sequence is capable of reversing superradiant damping in some cases. Specific computations for pentacene doped mixed molecular crystals, where ‘‘domains’’ of resonant impurities are likely to exist, are presented and compared with experimental results.