Very fast hot carrier diffusion in unconstrained MoS₂ on a glass substrate: discovered by picosecond ET-Raman

The currently reported optical-phonon-scattering-limited carrier mobility of MoS₂ is up to 417 cm² V^-1 s^-1 with two-side dielectric screening: one normal-κ side and one high-κ side. Herein, using picosecond energy transport state-resolved Raman (ET-Raman), we demonstrated very fast hot carrier diffusion in μm-scale (lateral) unconstrained MoS₂ (1.8-18 nm thick) on a glass substrate; this method enables only one-side normal-κ dielectric screening. The ET-Raman method directly probes the diffusion of the hot carrier and its contribution to phonon transfer without contact and additional sample preparation and provides unprecedented insight into the intrinsic D of MoS₂. The measured D values span from 0.76 to 9.7 cm² s^-1. A nonmonotonic thickness-dependent D trend is discovered, and it peaks at 3.0 nm thickness. This is explained by the competition between two physical phenomena: with an increase in sample thickness, the increased screening of the substrate results in higher mobility; moreover, thicker samples are subject to more surface contamination, loose substrate contact and weaker substrate dielectric screening. The corresponding carrier mobility varies from 31.0 to 388.5 cm² V^-1 s^-1. This mobility is surprisingly high considering the normal-κ and single side dielectric screening by the glass substrate. This is a direct result of the less-damaged structure of MoS₂ that is superior to those of MoS₂ samples reported in literature studies that are subjected to various post-processing techniques to facilitate measurement. The very high hot carrier mobility reduces the local carrier concentration and enhances the Raman signal, which is further confirmed by our Raman signal studies and comparison with theoretical studies.