Giant room-temperature nonlinearities in a monolayer Janus topological semiconductor

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, Shambhu Ghimire, Ju Li, Jing Kong, Yunfan Guo () and Aaron M. Lindenberg ()
Additional contact information
Jiaojian Shi: Stanford University
Haowei Xu: Massachusetts Institute of Technology
Christian Heide: Stanford University
Changan HuangFu: Tsinghua University
Chenyi Xia: Stanford University
Felipe Quesada: Stanford University
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
Enzheng Shi: Westlake University
Liying Jiao: Tsinghua University
Tony Heinz: Stanford PULSE Institute, SLAC National Accelerator Laboratory
Shambhu Ghimire: Stanford PULSE Institute, SLAC National Accelerator Laboratory
Ju Li: Massachusetts Institute of Technology
Jing Kong: Massachusetts Institute of Technology
Yunfan Guo: Zhejiang University
Aaron M. Lindenberg: Stanford University

Nature Communications, 2023, vol. 14, issue 1, 1-8

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-40373-z

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