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<p>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.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年3月26日

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  • Yi-Hsun Chen,
  • Ping-Yuan Lo,
  • Kyle W. Boschen,
  • Chih-En Hsu,
  • Yung-Ning Hsu,
  • Luke N. Holtzman,
  • Guan-Hao Peng,
  • Chun-Jui Huang,
  • Madisen Holbrook,
  • Wei-Hua Wang,
  • Katayun Barmak,
  • James Hone,
  • Pawel Hawrylak,
  • Hung-Chung Hsueh,
  • Jeffrey A. Davis,
  • Shun-Jen Cheng,
  • Michael S. Fuhrer,
  • Shao-Yu Chen

摘要

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 MoS2, MoSe2, WS2, and WSe2, 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.