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Physical Review Letters

Superradiance of High Density Frenkel Excitons at Room Temperature

H. Z. Wang, Xiuyuan Zheng, F. L. Zhao, Zhen Liang Gao, Z. X. Yu

Published May 15, 1995• 26 citations
Publisher

Abstract

Superradiance of high density Frenkel excitons in an $R$-phycoerythrin single crystal is observed at room temperature for the first time. No fluorescence is observed except the emission at the sharp exciton band when the superradiance of excitons occurs, and the higher the pump density, the sharper the emission bandwidth. A redshift and a blueshift are observed at the rise time and the fall time of the emission pulse, respectively. The experimental results also imply deformed-boson properties of high density Frenkel excitons.

DOI
10.1103/physrevlett.74.4079

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Superradiance of high density Frenkel excitons in an RRR-phycoerythrin single crystal is observed at room temperature for the first time. No fluorescence is observed except the emission at the sharp exciton band when the superradiance of excitons occurs, and the higher the pump density, the sharper the emission bandwidth. A redshift and a blueshift are observed at the rise time and the fall time of the emission pulse, respectively. The experimental results also imply deformed-boson properties of high density Frenkel excitons.
We systematically study the fluorescence of low-density Frenkel excitons in a crystal slab containing NT{N}_{T}NT​ V-type three-level atoms. Based on symmetric quasispin realization of SU(3) in large N limit, the two-mode exciton operators are invoked to depict various collective excitations of the collection of these V-type atoms starting from their ground state. By making use of the rotating-wave approximation, the light intensity of radiation for the single-lattice layer is investigated in detail. As a quantum coherence effect, the quantum beat phenomenon is discussed in detail for different initial excitonic states. We also test the above results analytically without the consideration of the rotating-wave approximation and the self-interaction of radiance field is also included.
The fluorescence of Frenkel excitons in low density regime is studied without the aid of rotating wave approximation and Markov approximation. The evolution of the emitted field is derived in terms of its initial conditions. It is found that the usual interaction Hamiltonian of $(e/mc)\mathbf{P}\ensuremath{\cdot}\mathbf{A}$ type leads to unreasonable characteristic equation for decay rates. Only when the term (e2/2mc2)A2{(e}^{2}{/2\mathrm{mc}}^{2}){\mathbf{A}}^{2}(e2/2mc2)A2 is added to the $(e/mc)\mathbf{P}\ensuremath{\cdot}\mathbf{A},$ the result becomes reasonable. The case of single lattice layer is studied in detail. Different features of statistical properties of the superfluorescence are shown as compared with that of atom aggregate. Double and triple lattice-layer cases are also studied to show the effect of coupling between the excitons of different wave vectors.
Collective spontaneous emission from a one-dimensional mesoscopic exciton system interacting via static dipole moments is investigated by virtue of the analogy to the quantum XXZ spin chain. The rigorous expression for the initial state is obtained at any degree of excitation from the ground state by a short intense laser pulse. The emission profile from the initial state with partial population inversion exhibits oscillations and very rapid decay in comparison with that from the completely inverted state. The time-resolved emission spectra are also discussed.
The effect of the nonstationary condensation of electron-hole pairs in GaAs/AlGaAs p-i-n heterostructures at room temperature under the conditions of generation of superradiance pulses was demonstrated in an explicit form. It was found that a dramatic decrease in spontaneous emission from the entire conduction band and a rapid electron transition to the very bottom of the band occurred at the earliest stages of the development of a superradiance pulse. The condensation of electrons at the band bottom resulted in the formation of a nonequilibrium coherent cooperative state, the recombination of which was observed previously as high-power femtosecond superradiance pulses.
Dicke's superradiance from a gas system of atoms and molecules was described in terms of two-level atoms, i.e., as an assembly of half-spin operators. In this system the magnitude of the total spin, which is called a cooperation number, is conserved at the maximum for the whole radiative process. We will answer in this paper how this superradiance is modified in the crystal in which an excitation can propagate from atom to atom through dipolar interactions. As a prototype of a crystal, we choose a linear chain of two-level atoms. The superradiance master equation of this system can be solved in terms of the exact solution of Lieb, Shultz, and Mattis for the spin system. The first effect is that the emitted frequency shows opposite shifts red and blue, respectively, for the first and second halves of the superradiance pulse, or vice versa, depending upon the sign of the transfer-matrix element of the excitation. The second effect is the appearance of a slow component in the emission tail, which originates from mixture of the states with smaller cooperation numbers or smaller oscillator strength under the transfer of the excitations. These results are demonstrated for a mesoscopic system of linear chains.