Theory of high-temperature superfluorescence in hybrid perovskite thin films.

Abstract

The recent discovery of high-temperature superfluorescence in hybrid perovskite thin films has opened new possibilities for harnessing macroscopic quantum phenomena in nanotechnology. This study aimed to elucidate the mechanism that enables high-temperature superfluorescence in these systems. The proposed model describes a quasi-2D Wannier exciton in a thin film that interacts with phonons via the longitudinal optical phonon-exciton Fröhlich interaction. We show that the super-radiant properties of the coherent state in hybrid perovskites are stable against perturbations caused by the longitudinal optical phonon-exciton Fröhlich interaction. Using the multiconfiguration Hartree approach, we derive semiclassical equations of motion for a single-exciton wavefunction, where the vibrational degrees of freedom interact with the Wannier exciton through a mean-field Hartree term. Super-radiance is effectively described by a non-Hermitian term in the Hamiltonian. The analysis was then extended to multiple excited states using the semiclassical Hamiltonian as the basic model. We demonstrate that the ground state of the model exciton Hamiltonian with long-range interactions is a symmetric Dicke super-radiant state, where the Fröhlich interaction is nullified. The additional density matrix-based consideration draws an analogy between this system and stable systems, where the conservation laws determine the nullification of the constant (momentum-independent) decay rate part. In the exciton-phonon system, nullification is associated with the absence of a momentum-independent component in the Wannier exciton-phonon interaction coupling function.