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

Chen, Yi-Hsun; Lo, Ping-Yuan; Boschen, Kyle W; Hsu, Chih-En; Hsu, Yung-Ning; Holtzman, Luke N; Peng, Guan-Hao; Huang, Chun-Jui et al. · Nat Commun · 2025

basic_science · Level V

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Abstract

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 on 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 MoS<sub>2</sub>, MoSe<sub>2</sub>, WS<sub>2</sub>, and WSe<sub>2</sub>, showing a high tuneability 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.