Room-Temperature, Strong Emission of Momentum-Forbidden Interlayer Excitons in Nanocavity-Coupled Twisted van der Waals Heterostructures

Nano Lett. 2025 Jan 8. doi: 10.1021/acs.nanolett.4c05647. Online ahead of print.

Abstract

The emission efficiency of interlayer excitons (IEs) in twisted 2D heterostructures has long suffered from momentum mismatch, limiting their applications in ultracompact excitonic devices. Here, we report strong room-temperature emission of the momentum-forbidden IEs in a 30°-twisted MoS2/WS2 heterobilayer. Utilizing the Purcell effect of a compact plasmonic nanocavity boosts the IE emission intensity in the cavity by over 2 orders of magnitude. We further study the interplay of this Purcell enhancement and phonon assistance in 30°- and 0°-twisted heterostructures. Temperature-dependent and time-resolved spectroscopic measurements reveal that the IE enhancement in the 30°-twisted case involves competition between IE and intralayer-exciton emissions, which is remarkably distinct from the 0°-twisted case. We propose an exciton decay model capturing the features of phonon-assisted momentum compensation and Purcell enhancement in the IE emission, showing consistency with the experimental measurements. Our results enrich the understanding of the nanocavity-assisted light-matter interaction for momentum-indirect excitonic transitions.

Keywords: Purcell effect; heterostructure; interlayer exciton; momentum mismatch; twist angle.