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Giant room-temperature nonlinearities in a monolayer Janus topological semiconductor

Author

Listed:
  • Jiaojian Shi

    (Stanford University
    SLAC National Accelerator Laboratory)

  • Haowei Xu

    (Massachusetts Institute of Technology)

  • Christian Heide

    (Stanford University
    Stanford PULSE Institute, SLAC National Accelerator Laboratory)

  • Changan HuangFu

    (Tsinghua University)

  • Chenyi Xia

    (Stanford University
    SLAC National Accelerator Laboratory)

  • Felipe Quesada

    (Stanford University
    SLAC National Accelerator Laboratory)

  • Hongzhi Shen

    (Westlake University)

  • Tianyi Zhang

    (Massachusetts Institute of Technology)

  • Leo Yu

    (Stanford University)

  • Amalya Johnson

    (Stanford University)

  • Fang Liu

    (Stanford PULSE Institute, SLAC National Accelerator Laboratory
    Stanford University)

  • Enzheng Shi

    (Westlake University)

  • Liying Jiao

    (Tsinghua University)

  • Tony Heinz

    (Stanford PULSE Institute, SLAC National Accelerator Laboratory
    Stanford University)

  • Shambhu Ghimire

    (Stanford PULSE Institute, SLAC National Accelerator Laboratory)

  • Ju Li

    (Massachusetts Institute of Technology
    Massachusetts Institute of Technology)

  • Jing Kong

    (Massachusetts Institute of Technology)

  • Yunfan Guo

    (Zhejiang University)

  • Aaron M. Lindenberg

    (Stanford University
    SLAC National Accelerator Laboratory
    Stanford PULSE Institute, SLAC National Accelerator Laboratory)

Abstract

Nonlinear optical materials possess wide applications, ranging from terahertz and mid-infrared detection to energy harvesting. Recently, the correlations between nonlinear optical responses and certain topological properties, such as the Berry curvature and the quantum metric tensor, have attracted considerable interest. Here, we report giant room-temperature nonlinearities in non-centrosymmetric two-dimensional topological materials—the Janus transition metal dichalcogenides in the 1 T’ phase, synthesized by an advanced atomic-layer substitution method. High harmonic generation, terahertz emission spectroscopy, and second harmonic generation measurements consistently show orders-of-the-magnitude enhancement in terahertz-frequency nonlinearities in 1 T’ MoSSe (e.g., > 50 times higher than 2H MoS2 for 18th order harmonic generation; > 20 times higher than 2H MoS2 for terahertz emission). We link this giant nonlinear optical response to topological band mixing and strong inversion symmetry breaking due to the Janus structure. Our work defines general protocols for designing materials with large nonlinearities and heralds the applications of topological materials in optoelectronics down to the monolayer limit.

Suggested Citation

  • Jiaojian Shi & Haowei Xu & Christian Heide & Changan HuangFu & Chenyi Xia & Felipe Quesada & Hongzhi Shen & Tianyi Zhang & Leo Yu & Amalya Johnson & Fang Liu & Enzheng Shi & Liying Jiao & Tony Heinz &, 2023. "Giant room-temperature nonlinearities in a monolayer Janus topological semiconductor," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-40373-z
    DOI: 10.1038/s41467-023-40373-z
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