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Photocarrier relaxation pathway in two-dimensional semiconducting transition metal dichalcogenides

Author

Listed:
  • Daichi Kozawa

    (Institute of Advanced Energy, Kyoto University)

  • Rajeev Kumar

    (National University of Singapore, 2 Science Drive 3
    Graphene Research Centre, National University of Singapore, 6 Science Drive 2)

  • Alexandra Carvalho

    (National University of Singapore, 2 Science Drive 3
    Graphene Research Centre, National University of Singapore, 6 Science Drive 2)

  • Kiran Kumar Amara

    (National University of Singapore, 2 Science Drive 3
    National University of Singapore, 3 Science Drive 3)

  • Weijie Zhao

    (National University of Singapore, 2 Science Drive 3
    Graphene Research Centre, National University of Singapore, 6 Science Drive 2)

  • Shunfeng Wang

    (National University of Singapore, 2 Science Drive 3
    Graphene Research Centre, National University of Singapore, 6 Science Drive 2)

  • Minglin Toh

    (National University of Singapore, 2 Science Drive 3
    Graphene Research Centre, National University of Singapore, 6 Science Drive 2)

  • Ricardo M. Ribeiro

    (Graphene Research Centre, National University of Singapore, 6 Science Drive 2
    Center of Physics, University of Minho)

  • A. H. Castro Neto

    (National University of Singapore, 2 Science Drive 3
    Graphene Research Centre, National University of Singapore, 6 Science Drive 2)

  • Kazunari Matsuda

    (Institute of Advanced Energy, Kyoto University)

  • Goki Eda

    (National University of Singapore, 2 Science Drive 3
    Graphene Research Centre, National University of Singapore, 6 Science Drive 2
    National University of Singapore, 3 Science Drive 3)

Abstract

Two-dimensional crystals of semiconducting transition metal dichalcogenides absorb a large fraction of incident photons in the visible frequencies despite being atomically thin. It has been suggested that the strong absorption is due to the parallel band or ‘band nesting’ effect and corresponding divergence in the joint density of states. Here, we use photoluminescence excitation spectroscopy to show that the band nesting in mono- and bilayer MX2 (M=Mo, W and X=S, Se) results in excitation-dependent characteristic relaxation pathways of the photoexcited carriers. Our experimental and simulation results reveal that photoexcited electron–hole pairs in the nesting region spontaneously separate in k-space, relaxing towards immediate band extrema with opposite momentum. These effects imply that the loss of photocarriers due to direct exciton recombination is temporarily suppressed for excitation in resonance with band nesting. Our findings highlight the potential for efficient hot carrier collection using these materials as the absorbers in optoelectronic devices.

Suggested Citation

  • Daichi Kozawa & Rajeev Kumar & Alexandra Carvalho & Kiran Kumar Amara & Weijie Zhao & Shunfeng Wang & Minglin Toh & Ricardo M. Ribeiro & A. H. Castro Neto & Kazunari Matsuda & Goki Eda, 2014. "Photocarrier relaxation pathway in two-dimensional semiconducting transition metal dichalcogenides," Nature Communications, Nature, vol. 5(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:5:y:2014:i:1:d:10.1038_ncomms5543
    DOI: 10.1038/ncomms5543
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    Cited by:

    1. N. Fang & Y. R. Chang & D. Yamashita & S. Fujii & M. Maruyama & Y. Gao & C. F. Fong & K. Otsuka & K. Nagashio & S. Okada & Y. K. Kato, 2023. "Resonant exciton transfer in mixed-dimensional heterostructures for overcoming dimensional restrictions in optical processes," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    2. Kai-Qiang Lin & Jonas D. Ziegler & Marina A. Semina & Javid V. Mamedov & Kenji Watanabe & Takashi Taniguchi & Sebastian Bange & Alexey Chernikov & Mikhail M. Glazov & John M. Lupton, 2022. "High-lying valley-polarized trions in 2D semiconductors," Nature Communications, Nature, vol. 13(1), pages 1-8, December.

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