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Soviet Journal of Low Temperature Physics

Peculiarities of Dicke optical superradiance in pyrene-doped biphenyl crystal under narrow-band and wide-band excitation

P. V. Zinov’ev, Yu. V. Malyukin, Yu. V. Naboĭkin, E. N. Rudenko, В. В. Самарцев, Nataliya B. Silaeva

Published Feb 1, 1986• 0 citations
Publisher

Abstract

The effect of coherence and the exciting radiation linewidth on the formation of superradiance has been investigated, using a pyrene-doped molecular biphenyl crystal as an example. Three types of lasers with various degrees of coherence and substantially different emission linewidths provided the excitation. The formation of superradiance is shown to be independent of the degree of pumping coherence and its spectral composition is shown to depend on the exciting radiation bandwidth. The investigations demonstrate that optical superradiance holds out promise in high-resolution spectroscopy.

DOI
10.1063/10.0031448

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The effect of coherence and the exciting radiation linewidth on the formation of superradiance has been investigated, using a pyrene-doped molecular biphenyl crystal as an example. Three types of lasers with various degrees of coherence and substantially different emission linewidths provided the excitation. The formation of superradiance is shown to be independent of the degree of pumping coherence and its spectral composition is shown to depend on the exciting radiation bandwidth. The investigations demonstrate that optical superradiance holds out promise in high-resolution spectroscopy.
The results of theoretical and experimental superradiance studies in a pyrene-doped biphenyl crystal are presented. The superradiance nature of photon emission under certain conditions is experimentally proved for this crystal system. Experimental data fit the theory. The influence of induced radiation and of electron-phonon coupling on optical superradiance is theoretically investigated using the nonequilibrium statistical operator method. Possible superradiance applications are discussed, including coherent nonlinear spectroscopy, coherent electromagnetic pulse generation, and superradiant echo.
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.
Coherent excitation of a molecular ensemble coupled to a common radiation mode can lead to the collective emission of radiation known as superradiance. This collective emission only occurs if there is an entanglement between the molecules in their ground and excited state and can, therefore, serve as a macroscopic measure of coherence in the ensemble. Reported here are wave packet propagations for various pyrazine models of increasing complexity and molecular ensembles thereof. We show that ensemble coherence upon photoexcitation can prevail up to relatively long time scales although the effect can diminish quickly with increasing ensemble size. Coherence can also build up over time and even reemerge after the molecules have passed through a conical intersection. The effect of the pump pulse characteristics on the collective response of the molecular ensemble is also studied. A broadband pulse imprints a large amount of initial coherence to the system, as compared to a longer pulse with a smaller spread in the frequency domain. However, the differential effects arising from a different pulse duration and coherent bandwidth become less prominent if the emission of light from the ensemble takes place after a non-adiabatic decay process.