Weak Distance Dependence of Hot-Electron-Transfer Rates at the Interface between Monolayer MoS2 and Gold

Electron transport across the transition-metal dichalcogenide (TMD)/metal interface plays an important role in determining the performance of TMD-based optoelectronic devices. However, the robustness of this process against structural heterogeneities remains unexplored, to the best of our knowledge. Here, we employ a combination of time-resolved photoemission electron microscopy (TR-PEEM) and atomic force microscopy to investigate the spatially resolved hot-electron-transfer dynamics at the monolayer (1L) MoS2/Au interface. A spatially heterogeneous distribution of 1L-MoS2/Au gap distances, along with the sub-80 nm spatial- and sub-60 fs temporal resolution of TR-PEEM, permits the simultaneous measurement of electron-transfer rates across a range of 1L-MoS2/Au distances. These decay exponentially as a function of distance, with an attenuation coefficient beta similar to 0.06 +/- 0.01 angstrom(-1), comparable to molecular wires. Ab initio simulations suggest that surface plasmon-like states mediate hot-electron-transfer, hence accounting for its weak distance dependence. The weak distance dependence of the interfacial hot-electron-transfer rate indicates that this process is insensitive to distance fluctuations at the TMD/metal interface, thus motivating further exploration of optoelectronic devices based on hot carriers.

Automated summary

The study investigates the hot-electron transfer dynamics at the 1L MoS2/Au interface using TR-PEEM and atomic force microscopy, revealing an exponential decay of electron transfer rates with a decay coefficient of about 0.06 angstrom(-1). Ab initio simulations suggest that surface plasmon-like states mediate hot-electron transfer and explain its weak distance dependence.