Excitonic Thermalization Bottleneck in Twisted TMD Heterostructures.

Abstract

Twisted van der Waals heterostructures show intriguing interface exciton physics, including hybridization effects and emergence of moiré potentials. Recent experiments have revealed that moiré-trapped excitons exhibit remarkable dynamics, where excited states show lifetimes that are several orders of magnitude longer than in monolayers. The origin of this behavior is still under debate. Based on a microscopic many-particle approach, we investigate the phonon-driven relaxation cascade of nonequilibrium moiré excitons in the exemplary MoSe2-WSe2 heterostructure. We track exciton relaxation pathways across different moiré mini-bands and identify the phonon-scattering channels assisting the spatial redistribution of excitons into low-energy pockets of the moiré potential. We unravel a phonon bottleneck in the flat band structure at low twist angles preventing excitons from fully thermalizing into the lowest state, explaining the measured enhanced emission intensity and lifetime of excited moiré excitons. Overall, our work provides important insights into exciton relaxation dynamics in flat-band exciton materials.