Theory of High-Temperature Superfluorescence in Hybrid Perovskite Thin Films

TL;DR

This paper develops a theoretical model explaining high-temperature superfluorescence in hybrid perovskite thin films, highlighting the stability of superradiant states against phonon interactions and identifying conditions for superradiance.

Contribution

It introduces a comprehensive theoretical framework for superfluorescence in hybrid perovskites, emphasizing the role of exciton-phonon interactions and the symmetry of the exciton states.

Findings

Superradiant states are stable against phonon interactions.

The ground state is a symmetric Dicke superradiant state.

Nullification of decay rates is linked to interaction symmetry.

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 Frohlich interaction. We show that the superradiant properties of the coherent state in hybrid perovskites are stable against perturbations caused by the longitudinal optical phonon-exciton Frohlich 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. Superradiance 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 superradiant state, where the Frohlich 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.