Ultrasensitive Anti-Stokes Luminescence Thermometry in Transition Metal Dichalcogenide Monolayers

Abstract

Accurate temperature mapping at the nanoscale is a critical challenge in modern science and technology, as conventional methods fail at these dimensions. To address this challenge, we demonstrate a highly sensitive nanothermometer using anti-Stokes photoluminescence, also known as photoluminescence upconversion (UPL), in monolayer tungsten disulfide ($\mathrm{WS_2}$). Leveraging the direct band gap and strong exciton-phonon coupling in the two-dimensional monolayers, we achieve an exceptional relative sensitivity above $4\%\,\mathrm{K}^{-1}$ across the 300 K to 425 K range, ranking it among the best-performing materials reported. A strong resonantly enhanced UPL is observed, confirming the central role of optical phonons in the upconversion mechanism. Furthermore, we introduce a new analytical model to quantitatively describe the UPL process, taking into account the interplay of phonon populations, bandgap narrowing, and substrate effects, which predicts resonant temperatures and provides a framework with broad applicability to any material exhibiting an anti-Stokes photoluminescence response. To demonstrate its use as a high-resolution optical thermometer, we map a $20\,^{\circ}\mathrm{C}$ thermal gradient across a $20\,\mu\mathrm{m}$ long monolayer with a spatial resolution of $1\,\mu\mathrm{m}$. With its high sensitivity, strong signal, and excellent reproducibility, our work establishes monolayer transition metal dichalcogenide as a leading platform for non-invasive thermal sensing in advanced microelectronic and biological systems.