Interfacial-Water-Modulated Photoluminescence of Single-Layer WS₂ on Mica

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 their surrounding environment because of their 2D nature. In this work, we report that the photoluminescence (PL) of single-layer WS₂ is substantially affected by interfacial water that is inevitably present between it and the 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 could be attributed to the more efficient annihilation between excitons than between trions. By gas-controlled PL imaging, we also prove that the interfacial water converted the trions into excitons by depleting native negative charges through an oxygen reduction reaction, which rendered the excited WS₂ more susceptible to nonradiative decay via exciton-exciton annihilation. Understanding the role of nanoscopic water in complex low-dimensional materials will eventually contribute to devising their novel functions and related devices.