Giant room-temperature nonlinearities in a monolayer Janus topological semiconductor

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...

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Bibliographic Details
Published in:Nature communications 2023-08, Vol.14 (1), p.4953-4953, Article 4953
Main Authors: Shi, Jiaojian, Xu, Haowei, Heide, Christian, HuangFu, Changan, Xia, Chenyi, de Quesada, Felipe, Shen, Hongzhi, Zhang, Tianyi, Yu, Leo, Johnson, Amalya, Liu, Fang, Shi, Enzheng, Jiao, Liying, Heinz, Tony, Ghimire, Shambhu, Li, Ju, Kong, Jing, Guo, Yunfan, Lindenberg, Aaron M.
Format: Article
Language:English
Subjects:
140/125
140/133
639/301/1019/385
639/624/400/3923
Broken symmetry
Chalcogenides
Emission measurements
Emission spectroscopy
Energy harvesting
ENGINEERING
High-harmonic generation
Humanities and Social Sciences
Molybdenum disulfide
Monolayers
multidisciplinary
Nonlinear optics
Nonlinear response
Nonlinear systems
Nonlinearity
Optical materials
Optical properties
Optics
Optoelectronics
Room temperature
Science
Science (multidisciplinary)
Second harmonic generation
Spectroscopy
Tensors
Terahertz frequencies
Topology
Transition metal compounds
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Summary: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 2 H MoS 2 for 18 th order harmonic generation; > 20 times higher than 2 H MoS 2 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. Electronic band topology may be leveraged to enhance nonlinear optical properties in monolayer semiconductors. Here, the authors report giant room-temperature nonlinearity enhancements in Janus transition metal dichalcogenides.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-023-40373-z