Energy transfer driven brightening of MoS2 by ultrafast polariton relaxation in microcavity MoS2/hBN/WS2 heterostructures

Zehua Hu; Tanjung Krisnanda; Antonio Fieramosca; Jiaxin Zhao; Qianlu Sun; Yuzhong Chen; Haiyun Liu; Yuan Luo; Rui Su; Junyong Wang; Kenji Watanabe; Takashi Taniguchi; Goki Eda; Xiao Renshaw Wang; Sanjib Ghosh; Kevin Dini; Daniele Sanvitto; Timothy C. H. Liew; Qihua Xiong

doi:10.1038/s41467-024-45554-y

Journal article Energy transfer driven brightening of MoS2 by ultrafast polariton relaxation in microcavity MoS2/hBN/WS2 heterostructures

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Zehua Hu, Tanjung Krisnanda, Antonio Fieramosca, Jiaxin Zhao, Qianlu Sun, Yuzhong Chen, Haiyun Liu, Yuan Luo, Rui Su, Junyong Wang, Kenji Watanabe, Takashi Taniguchi, Goki Eda, Xiao Renshaw Wang, Sanjib Ghosh, Kevin Dini, Daniele Sanvitto, Timothy C. H. Liew, Qihua Xiong. Energy transfer driven brightening of MoS2 by ultrafast polariton relaxation in microcavity MoS2/hBN/WS2 heterostructures. Nature Communications. 2024, 15 (1), 1747. https://doi.org/10.1038/s41467-024-45554-y

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Energy transfer is a ubiquitous phenomenon that delivers energy from a blue-shifted emitter to a red-shifted absorber, which has enabled plentiful photonic applications of light-emitting diodes (LEDs), lasers, solar cells, and display devices1-5. The fast-emerging two-dimensional (2D) semiconductors offer unique opportunities for exploring new energy transfer mechanism in the atomic-scale limit enabled by confined geometry and van der Waals architectures, which transcend the conventional Förster and Dexter types. Herein, we have successfully designed and constructed a planar optical microcavity-confined MoS2/hBN/WS2 heterojunction, which realizes the strong coupling among donor exciton, acceptor exciton and cavity photon mode for the first time. Such a configuration demonstrates the unconventional energy transfer via ultrafast polariton relaxation, leading to the brightening of MoS2 neutral exciton with a record-high enhancement factor of ~440, i.e., two-order-of-magnitude higher than the data reported to date. A short characteristic time of ~1.3 ps is extracted by setting up a high-resolution k-space transient-reflectivity spectroscopy. This ultrafast polariton relaxation is attributed to the significantly enhanced intra- and inter-branch exciton-exciton scattering to overcome the hot phonon bottleneck effect, as revealed by theoretical calculation with the coupled rate equations. Our study not only opens a new direction of microcavity 2D semiconductor heterojunctions for high-brightness ultrafast polaritonic light sources, but also provides a new paradigm to study the ultrafast polariton carrier dynamics.

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