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Enhanced interactions of interlayer excitons in free-standing heterobilayers

Author

Listed:
  • Xueqian Sun

    (the Australian National University)

  • Yi Zhu

    (the Australian National University)

  • Hao Qin

    (the Australian National University)

  • Boqing Liu

    (the Australian National University)

  • Yilin Tang

    (the Australian National University)

  • Tieyu Lü

    (Xiamen University)

  • Sharidya Rahman

    (the Australian National University)

  • Tanju Yildirim

    (National Institute for Materials Science (NIMS))

  • Yuerui Lu

    (the Australian National University
    the Australian National University)

Abstract

Strong, long-range dipole–dipole interactions between interlayer excitons (IXs) can lead to new multiparticle correlation regimes1,2, which drive the system into distinct quantum and classical phases2–5, including dipolar liquids, crystals and superfluids. Both repulsive and attractive dipole–dipole interactions have been theoretically predicted between IXs in a semiconductor bilayer2,6–8, but only repulsive interactions have been reported experimentally so far3,9–16. This study investigated free-standing, twisted (51°, 53°, 45°) tungsten diselenide/tungsten disulfide (WSe2/WS2) heterobilayers, in which we observed a transition in the nature of dipolar interactions among IXs, from repulsive to attractive. This was caused by quantum-exchange-correlation effects, leading to the appearance of a robust interlayer biexciton phase (formed by two IXs), which has been theoretically predicted6–8 but never observed before in experiments. The reduced dielectric screening in a free-standing heterobilayer not only resulted in a much higher formation efficiency of IXs, but also led to strongly enhanced dipole–dipole interactions, which enabled us to observe the many-body correlations of pristine IXs at the two-dimensional quantum limit. In addition, we firstly observed several emission peaks from moiré-trapped IXs at room temperature in a well-aligned, free-standing WSe2/WS2 heterobilayer. Our findings open avenues for exploring new quantum phases with potential for applications in non-linear optics.

Suggested Citation

  • Xueqian Sun & Yi Zhu & Hao Qin & Boqing Liu & Yilin Tang & Tieyu Lü & Sharidya Rahman & Tanju Yildirim & Yuerui Lu, 2022. "Enhanced interactions of interlayer excitons in free-standing heterobilayers," Nature, Nature, vol. 610(7932), pages 478-484, October.
    • Handle: RePEc:nat:nature:v:610:y:2022:i:7932:d:10.1038_s41586-022-05193-z
    DOI: 10.1038/s41586-022-05193-z
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    Cited by:

    1. Suman Chatterjee & Medha Dandu & Pushkar Dasika & Rabindra Biswas & Sarthak Das & Kenji Watanabe & Takashi Taniguchi & Varun Raghunathan & Kausik Majumdar, 2023. "Harmonic to anharmonic tuning of moiré potential leading to unconventional Stark effect and giant dipolar repulsion in WS2/WSe2 heterobilayer," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    2. 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.
    3. N. Fang & Y. R. Chang & S. Fujii & D. Yamashita & M. Maruyama & Y. Gao & C. F. Fong & D. Kozawa & K. Otsuka & K. Nagashio & S. Okada & Y. K. Kato, 2024. "Room-temperature quantum emission from interface excitons in mixed-dimensional heterostructures," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    4. Riya Sebait & Roberto Rosati & Seok Joon Yun & Krishna P. Dhakal & Samuel Brem & Chandan Biswas & Alexander Puretzky & Ermin Malic & Young Hee Lee, 2023. "Sequential order dependent dark-exciton modulation in bi-layered TMD heterostructure," Nature Communications, Nature, vol. 14(1), pages 1-9, December.

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