Shedding light on exciton's nature in monolayer quantum material by optical dispersion measurements.

Abstract

Strong light-matter interactions based on two-dimensional excitons formed in quantum materials such as monolayer transition-metal dichalcogenides have become a major subject of research in recent years. Particularly attractive is the extraordinarily large oscillator strength as well as binding energy of the excitonic quasiparticles in these atomically-thin crystal lattices. Numerous theoretical studies and experiments have been devoted to the exploration of the excitonic systems that could be exploited in future nano-scaled optoelectronic devices. To obtain unique insight into the exciton's characteristics in an archetype monolayer quantum material, we directly measure the quasiparticle energy-momentum dispersion for the first time optically. Our results for h-BN encapsulated single-layer WSe2 clearly indicate an emission regime with a dispersion in the meV range in within the light cone at cryogenic temperatures. The amount of dispersion agrees well with calculations for an exciton-polariton based on the material's monolayer exciton, or energetic modifications caused by exciton exchange interactions predicted for this material family. The measurable dispersion slightly weakens for elevated excitation densities, whereas at elevated temperatures, it even becomes immeasurable. The obtained reduction in dispersion is attributed to an enhanced role of uncorrelated charge carriers as well as the formation of phonon sidebands above 100 K.