Interfacial-Water-Modulated Photoluminescence of Single-Layer WS$_2$ on Mica

Abstract

Because of their bandgap tunability and strong light-matter interactions, two-dimensional (2D) semiconductors are considered promising candidates for next-generation optoelectronic devices. However, their photophysical properties are greatly affected by environments because of their 2D nature. In this work, we report that the photoluminescence (PL) of single-layer WS$_2$ is substantially affected by interfacial water that is inevitably present between itself and supporting mica substrates. Using PL spectroscopy and wide-field imaging, we show that the emission signals from A excitons and their negative trions decreased at distinctively different rates with increasing excitation power, which can be attributed to the more efficient annihilation between excitons than trions. By gas-controlled PL imaging, we also prove that interfacial water converts trions into excitons by depleting native negative charges through an oxygen reduction reaction, which renders excited WS$_2$ more susceptible to nonradiative decay via exciton-exciton annihilation. Understanding the roles of nanoscopic water in complex low-dimensional materials will eventually contribute to devising their novel functions and devices.