The Hidden Cost of Alloying: Disorder-Driven Transport Collapse in TMDs
Alloying in two dimensional semiconductors is widely used to tune bandgaps, yet its implications for charge and energy transport remain poorly understood. Here, we investigate MoS2xSe2(1-x) alloys as a model system to study the interplay between composition, thickness, and disorder. Optical transitions and valence band dispersions evolve continuously with both stoichiometry and number of layers, with negligible bandgap bowing and a composition dependent attenuation of thickness driven renormalization. In contrast, time resolved spatial mapping of photoexcited carriers reveals a pronounced and asymmetric collapse of carrier diffusivity at intermediate compositions, which cannot be accounted for by changes in effective mass or band alignment, and instead emerges from strong real space fluctuations in the local energetic landscape generated by random chalcogen substitution. Microscopic simulations reproduce the experimental trends and show that the character of disorder depends critically on the direction of alloying, producing either scattering barriers or deep trapping sites. Together, these results demonstrate that transport in TMD alloys is governed by disorder physics, overlooked by conventional optical and photoemission probes at equilibrium. Our findings establish transport as a stringent metric of electronic quality and high-light intrinsic limitations in the usage of TMD alloys for layered semiconductor devices.