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Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3

Author

Listed:
  • Zeyuan Sun

    (Fudan University
    Fudan University)

  • Yangfan Yi

    (Fudan University
    Fudan University)

  • Tiancheng Song

    (University of Washington)

  • Genevieve Clark

    (University of Washington)

  • Bevin Huang

    (University of Washington)

  • Yuwei Shan

    (Fudan University
    Fudan University)

  • Shuang Wu

    (Fudan University
    Fudan University)

  • Di Huang

    (Fudan University
    Fudan University)

  • Chunlei Gao

    (Fudan University
    Fudan University
    Collaborative Innovation Center of Advanced Microstructures)

  • Zhanghai Chen

    (Fudan University
    Fudan University
    Collaborative Innovation Center of Advanced Microstructures)

  • Michael McGuire

    (Oak Ridge National Laboratory)

  • Ting Cao

    (University of Washington
    Stanford University)

  • Di Xiao

    (Carnegie Mellon University)

  • Wei-Tao Liu

    (Fudan University
    Fudan University
    Collaborative Innovation Center of Advanced Microstructures)

  • Wang Yao

    (University of Hong Kong)

  • Xiaodong Xu

    (University of Washington
    University of Washington)

  • Shiwei Wu

    (Fudan University
    Fudan University
    Collaborative Innovation Center of Advanced Microstructures)

Abstract

Layered antiferromagnetism is the spatial arrangement of ferromagnetic layers with antiferromagnetic interlayer coupling. The van der Waals magnet chromium triiodide (CrI3) has been shown to be a layered antiferromagnetic insulator in its few-layer form1, opening up opportunities for various functionalities2–7 in electronic and optical devices. Here we report an emergent nonreciprocal second-order nonlinear optical effect in bilayer CrI3. The observed second-harmonic generation (SHG; a nonlinear optical process that converts two photons of the same frequency into one photon of twice the fundamental frequency) is several orders of magnitude larger than known magnetization-induced SHG8–11 and comparable to the SHG of the best (in terms of nonlinear susceptibility) two-dimensional nonlinear optical materials studied so far12,13 (for example, molybdenum disulfide). We show that although the parent lattice of bilayer CrI3 is centrosymmetric, and thus does not contribute to the SHG signal, the observed giant nonreciprocal SHG originates only from the layered antiferromagnetic order, which breaks both the spatial-inversion symmetry and the time-reversal symmetry. Furthermore, polarization-resolved measurements reveal underlying C2h crystallographic symmetry—and thus monoclinic stacking order—in bilayer CrI3, providing key structural information for the microscopic origin of layered antiferromagnetism14–18. Our results indicate that SHG is a highly sensitive probe of subtle magnetic orders and open up possibilities for the use of two-dimensional magnets in nonlinear and nonreciprocal optical devices.

Suggested Citation

  • Zeyuan Sun & Yangfan Yi & Tiancheng Song & Genevieve Clark & Bevin Huang & Yuwei Shan & Shuang Wu & Di Huang & Chunlei Gao & Zhanghai Chen & Michael McGuire & Ting Cao & Di Xiao & Wei-Tao Liu & Wang Y, 2019. "Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3," Nature, Nature, vol. 572(7770), pages 497-501, August.
  • Handle: RePEc:nat:nature:v:572:y:2019:i:7770:d:10.1038_s41586-019-1445-3
    DOI: 10.1038/s41586-019-1445-3
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    1. Fengrui Yao & Volodymyr Multian & Zhe Wang & Nicolas Ubrig & Jérémie Teyssier & Fan Wu & Enrico Giannini & Marco Gibertini & Ignacio Gutiérrez-Lezama & Alberto F. Morpurgo, 2023. "Multiple antiferromagnetic phases and magnetic anisotropy in exfoliated CrBr3 multilayers," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. ZhuangEn Fu & Piumi I. Samarawickrama & John Ackerman & Yanglin Zhu & Zhiqiang Mao & Kenji Watanabe & Takashi Taniguchi & Wenyong Wang & Yuri Dahnovsky & Mingzhong Wu & TeYu Chien & Jinke Tang & Allan, 2024. "Tunneling current-controlled spin states in few-layer van der Waals magnets," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Shuai Xu & Jiesu Wang & Pan Chen & Kuijuan Jin & Cheng Ma & Shiyao Wu & Erjia Guo & Chen Ge & Can Wang & Xiulai Xu & Hongbao Yao & Jingyi Wang & Donggang Xie & Xinyan Wang & Kai Chang & Xuedong Bai & , 2023. "Magnetoelectric coupling in multiferroics probed by optical second harmonic generation," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    4. Xingzhi Wang & Qishuo Tan & Tie Li & Zhengguang Lu & Jun Cao & Yanan Ge & Lili Zhao & Jing Tang & Hikari Kitadai & Mingda Guo & Yun-Mei Li & Weigao Xu & Ran Cheng & Dmitry Smirnov & Xi Ling, 2024. "Unveiling the spin evolution in van der Waals antiferromagnets via magneto-exciton effects," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    5. Faran Zhou & Kyle Hwangbo & Qi Zhang & Chong Wang & Lingnan Shen & Jiawei Zhang & Qianni Jiang & Alfred Zong & Yifan Su & Marc Zajac & Youngjun Ahn & Donald A. Walko & Richard D. Schaller & Jiun-Haw C, 2022. "Dynamical criticality of spin-shear coupling in van der Waals antiferromagnets," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    6. Sahar Pakdel & Asbjørn Rasmussen & Alireza Taghizadeh & Mads Kruse & Thomas Olsen & Kristian S. Thygesen, 2024. "High-throughput computational stacking reveals emergent properties in natural van der Waals bilayers," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    7. Shivangi Shree & Delphine Lagarde & Laurent Lombez & Cedric Robert & Andrea Balocchi & Kenji Watanabe & Takashi Taniguchi & Xavier Marie & Iann C. Gerber & Mikhail M. Glazov & Leonid E. Golub & Bernha, 2021. "Interlayer exciton mediated second harmonic generation in bilayer MoS2," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    8. 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.
    9. P. Padmanabhan & F. L. Buessen & R. Tutchton & K. W. C. Kwock & S. Gilinsky & M. C. Lee & M. A. McGuire & S. R. Singamaneni & D. A. Yarotski & A. Paramekanti & J.-X. Zhu & R. P. Prasankumar, 2022. "Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    10. Xiaoyu Guo & Wenhao Liu & Jonathan Schwartz & Suk Hyun Sung & Dechen Zhang & Makoto Shimizu & Aswin L. N. Kondusamy & Lu Li & Kai Sun & Hui Deng & Harald O. Jeschke & Igor I. Mazin & Robert Hovden & B, 2024. "Extraordinary phase transition revealed in a van der Waals antiferromagnet," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    11. Liangting Ye & Wenju Zhou & Dajian Huang & Xiao Jiang & Qiangbing Guo & Xinyu Cao & Shaohua Yan & Xinyu Wang & Donghan Jia & Dequan Jiang & Yonggang Wang & Xiaoqiang Wu & Xiao Zhang & Yang Li & Hechan, 2023. "Manipulation of nonlinear optical responses in layered ferroelectric niobium oxide dihalides," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    12. Ziqian Wang & Meng Wang & Jannis Lehmann & Yuki Shiomi & Taka-hisa Arima & Naoto Nagaosa & Yoshinori Tokura & Naoki Ogawa, 2024. "Electric-field-enhanced second-harmonic domain contrast and nonreciprocity in a van der Waals antiferromagnet," Nature Communications, Nature, vol. 15(1), pages 1-7, December.
    13. Myeongjin Jang & Sol Lee & Fernando Cantos-Prieto & Ivona Košić & Yue Li & Arthur R. C. McCray & Min-Hyoung Jung & Jun-Yeong Yoon & Loukya Boddapati & Francis Leonard Deepak & Hu Young Jeong & Charuda, 2024. "Direct observation of twisted stacking domains in the van der Waals magnet CrI3," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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