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

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