Alloy engineering of excitonic properties in TMD monolayers

Abstract

We investigate monolayer MoS$_{2x}$Se$_{2(1-x)}$ alloys across the full composition range using optical spectroscopy. We demonstrate continuous tuning of the optical gap over $\sim$0.35 eV, accompanied by a systematic reduction of the B--A exciton splitting, in agreement with density functional theory calculations. Temperature-dependent measurements reveal a progressive increase of the average phonon energy from Se-rich to S-rich alloys that follows a simple reduced-mass scaling model. Polarization-resolved spectroscopy further shows a monotonic increase of the circular polarization from nearly zero in MoSe$_2$ to $\sim$15\% in MoS$_2$ at 78 K. The observed evolution of the polarization is attributed to alloy-induced modifications of the electronic structure that modify bright--dark exciton mixing and the associated valley depolarization. These findings establish alloy engineering as an effective strategy for controlling excitonic properties in TMD monolayers.