Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3

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 Yao, Xiaodong Xu () and Shiwei Wu ()
Additional contact information
Zeyuan Sun: Fudan University
Yangfan Yi: Fudan University
Tiancheng Song: University of Washington
Genevieve Clark: University of Washington
Bevin Huang: University of Washington
Yuwei Shan: Fudan University
Shuang Wu: Fudan University
Di Huang: Fudan University
Chunlei Gao: Fudan University
Zhanghai Chen: Fudan University
Michael McGuire: Oak Ridge National Laboratory
Ting Cao: University of Washington
Di Xiao: Carnegie Mellon University
Wei-Tao Liu: Fudan University
Wang Yao: University of Hong Kong
Xiaodong Xu: University of Washington
Shiwei Wu: Fudan University

Nature, 2019, vol. 572, issue 7770, 497-501

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41586-019-1445-3

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