Dynamic Lattice Disorder and Collective Dipole Coupling Give Rise to Dicke Physics in Perovskite Quantum Dots

TL;DR

This paper develops a microscopic theory explaining how lattice disorder and dipole interactions in perovskite quantum dots lead to collective optical phenomena like superradiance, with control via material parameters and temperature.

Contribution

It introduces a theory linking lattice dynamics and dipole coupling to Dicke effects, enabling control of cooperative emission in perovskite quantum dots.

Findings

Cooperative emission depends on the balance between collective coupling and lattice disorder.

Cooling induces a transition to coherent emission as lattice fluctuations freeze.

The theory explains size, composition, and temperature effects on radiative properties.

Abstract

Halide perovskite quantum dots exhibit cooperative optical phenomena that are absent in conventional semiconductor nanocrystals, including exciton superradiance, superabsorption, and biexciton superradiance within individual dots. Here we develop a microscopic theory that identifies the physical origin of these Dicke effects and establishes how they can be controlled by materials parameters. The central result is that cooperative emission emerges from a competition between collective coupling of optical transition dipoles and lattice-induced disorder, with the balance governed by the Raman-derived phonon spectral density and the excitonic oscillator strength. At elevated temperature, strong Fr\"ohlich coupling and glassy lattice dynamics produce dynamic disorder that suppresses dipole synchronization and yields incoherent emission. Upon cooling, lattice fluctuations freeze and cooperative coherence emerges when the collective coupling exceeds residual static disorder, defining size- and composition-dependent crossover temperatures that we map as phase diagrams. Extending the framework to biexcitons, we show that a confined biexciton constitutes a single correlated charge distribution dressed by a shared lattice configuration, enabling pathway-indistinguishable decay and cooperative radiative enhancement. The theory quantitatively accounts for observed size, composition, and temperature trends in radiative-rate constant ratios and biexciton binding energies, while explaining why full Dicke saturation is not universal. More broadly, the results establish Raman spectral weight and oscillator strength as design parameters for engineering cooperative quantum-optical behavior in quantum materials.