Ultrathin quantum light source with van der Waals NbOCl2 crystal

Qiangbing Guo (), Xiao-Zhuo Qi, Lishu Zhang, Meng Gao, Sanlue Hu, Wenju Zhou, Wenjie Zang, Xiaoxu Zhao, Junyong Wang, Bingmin Yan, Mingquan Xu, Yun-Kun Wu, Goki Eda, Zewen Xiao, Shengyuan A. Yang, Huiyang Gou, Yuan Ping Feng, Guang-Can Guo, Wu Zhou, Xi-Feng Ren (), Cheng-Wei Qiu (), Stephen J. Pennycook () and Andrew T. S. Wee ()
Additional contact information
Qiangbing Guo: National University of Singapore
Xiao-Zhuo Qi: University of Science and Technology of China
Lishu Zhang: National University of Singapore
Meng Gao: University of Chinese Academy of Sciences
Sanlue Hu: Huazhong University of Science and Technology
Wenju Zhou: Center for High Pressure Science and Technology Advanced Research
Wenjie Zang: National University of Singapore
Xiaoxu Zhao: Peking University
Junyong Wang: National University of Singapore
Bingmin Yan: Center for High Pressure Science and Technology Advanced Research
Mingquan Xu: University of Chinese Academy of Sciences
Yun-Kun Wu: University of Science and Technology of China
Goki Eda: National University of Singapore
Zewen Xiao: Huazhong University of Science and Technology
Shengyuan A. Yang: Singapore University of Technology and Design
Huiyang Gou: Center for High Pressure Science and Technology Advanced Research
Yuan Ping Feng: National University of Singapore
Guang-Can Guo: University of Science and Technology of China
Wu Zhou: University of Chinese Academy of Sciences
Xi-Feng Ren: University of Science and Technology of China
Cheng-Wei Qiu: National University of Singapore
Stephen J. Pennycook: National University of Singapore
Andrew T. S. Wee: National University of Singapore

Nature, 2023, vol. 613, issue 7942, 53-59

Abstract: Abstract Interlayer electronic coupling in two-dimensional materials enables tunable and emergent properties by stacking engineering. However, it also results in significant evolution of electronic structures and attenuation of excitonic effects in two-dimensional semiconductors as exemplified by quickly degrading excitonic photoluminescence and optical nonlinearities in transition metal dichalcogenides when monolayers are stacked into van der Waals structures. Here we report a van der Waals crystal, niobium oxide dichloride (NbOCl2), featuring vanishing interlayer electronic coupling and monolayer-like excitonic behaviour in the bulk form, along with a scalable second-harmonic generation intensity of up to three orders higher than that in monolayer WS2. Notably, the strong second-order nonlinearity enables correlated parametric photon pair generation, through a spontaneous parametric down-conversion (SPDC) process, in flakes as thin as about 46 nm. To our knowledge, this is the first SPDC source unambiguously demonstrated in two-dimensional layered materials, and the thinnest SPDC source ever reported. Our work opens an avenue towards developing van der Waals material-based ultracompact on-chip SPDC sources as well as high-performance photon modulators in both classical and quantum optical technologies1–4.

Date: 2023
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DOI: 10.1038/s41586-022-05393-7

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