Efficient light upconversion via resonant exciton-exciton annihilation of dark excitons in few-layer transition metal dichalcogenides

Materials capable of light upconversion—transforming low-energy photons into higher-energy ones—are pivotal in advancing optoelectronics, energy solutions, and photocatalysis. However, the discovery in various materials pays little attention to few-layer transition metal dichalcogenides, primarily due to their indirect bandgaps and weaker light-matter interactions. Here, we report a pronounced light upconversion in few-layer transition metal dichalcogenides through upconversion photoluminescence spectroscopy. Our joint theory-experiment study attributes the upconversion photoluminescence to a resonant exciton-exciton annihilation involving a pair of dark excitons with opposite momenta, followed by the spontaneous emission of upconverted bright excitons, which can have a high upconversion efficiency. Additionally, the upconversion photoluminescence is generic in MoS2, MoSe2, WS2, and WSe2, showing a high tunability from green to ultraviolet light (2.34–3.1 eV). The findings pave the way for further exploration of light upconversion regarding fundamental properties and device applications in two-dimensional semiconductors.