Interfacial control of hot-carrier extraction and photostability in two-dimensional materials

TL;DR

This study investigates how interface morphology affects charge carrier dynamics and stability in monolayer WS2 on different substrates, revealing that optimized interfaces enhance photocurrent and photostability without encapsulation.

Contribution

It demonstrates that interface morphology controls charge transfer efficiency and stability in 2D TMDCs, highlighting interfacial design as key for device performance.

Findings

Discontinuous WS2 contacts on rough Au produce larger photocurrents.

Ultrafast charge extraction suppresses recombination and prevents degradation.

Interface morphology influences charge transfer and device stability.

Abstract

Two-dimensional transition metal dichalcogenides (TMDCs) are promising materials for next-generation optoelectronic devices, yet their implementation is hindered by limited sample stability and challenges in forming reliable electrical contacts. Here, by utilizing time-domain THz emission spectroscopy we directly probe charge carrier dynamics in monolayer WS2 on gold (Au) and fused silica (SiO2) as a function of interface morphology. For laser excitation above the band gap of WS2, we independently extract effective transport times for both electrons and holes and find that discontinuous WS2 contacts on rough Au generate larger net photocurrents than uniform, strongly coupled interfaces - a counterintuitive observation attributed to imbalanced electron and hole transfer from WS2 to Au. Crucially, we demonstrate that ultrafast charge extraction and separation suppress recombination-driven energy release and thereby prevent photo-induced degradation under ambient conditions, eliminating the need for encapsulation. These findings redefine interfacial design as a central control parameter for both performance and stability in 2D optoelectronic devices.