Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3

Sun, Zeyuan; Yi, Yangfan; Song, Tiancheng; Clark, Genevieve; Huang, Bevin; Shan, Yuwei; Wu, Shuang; Huang, Di; Gao, Chunlei; Chen, Zhanghai; McGuire, Michael A.; Cao, Ting; Xiao, Di; Tao Liu, Wei; Yao, Wang; Xu, Xiaodong; Wu, Shiwei

doi:10.1038/s41586-019-1445-3

Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI₃

Journal Article · Wed Jul 31 04:00:00 EDT 2019 · Nature (London)

DOI:https://doi.org/10.1038/s41586-019-1445-3· OSTI ID:1649491

Sun, Zeyuan ^[1]; Yi, Yangfan ^[1]; Song, Tiancheng ^[2]; Clark, Genevieve ^[2]; Huang, Bevin ^[2]; Shan, Yuwei ^[1]; Wu, Shuang ^[1]; Huang, Di ^[1]; Gao, Chunlei ^[3]; Chen, Zhanghai ^[3]; ^[4]; Cao, Ting ^[5]; Xiao, Di ^[6]; Tao Liu, Wei ^[3]; Yao, Wang ^[7]; Xu, Xiaodong ^[2]; Wu, Shiwei ^[3]

Fudan Univ., Shanghai (China)
Univ. of Washington, Seattle, WA (United States)
Fudan Univ., Shanghai (China); Collaborative Innovation Center of Advanced Microstructures, Nanjing (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Washington, Seattle, WA (United States); Stanford Univ., CA (United States)
Carnegie Mellon Univ. (CMU), Pittsburgh, PA (United States)
Univ. of Hong Kong (China)

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 form, opening up opportunities for various functionalities 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 SHG and comparable to the SHG of the best (in terms of nonlinear susceptibility) two-dimensional nonlinear optical materials studied so far (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 C_2h crystallographic symmetry—and thus monoclinic stacking order—in bilayer CrI₃, providing key structural information for the microscopic origin of layered antiferromagnetism. Finally, 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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Natural Science Foundation of China (NNSFC); National Basic Research Program of China; National Key Research and Development Program of China; National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725; SC0012509

OSTI ID:: 1649491

Journal Information:: Nature (London), Journal Name: Nature (London) Journal Issue: 7770 Vol. 572; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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