Stacking‐Controlled Growth of rBN Crystalline Films with High Nonlinear Optical Conversion Efficiency up to 1%

Author:

Qi Jiajie1ORCID,Ma Chenjun1,Guo Quanlin1,Ma Chaojie1,Zhang Zhibin1,Liu Fang1,Shi Xuping1,Wang Li2,Xue Mingshan3,Wu Muhong4,Gao Peng4,Hong Hao1,Wang Xinqiang1,Wang Enge245,Liu Can6ORCID,Liu Kaihui145ORCID

Affiliation:

1. State Key Laboratory for Mesoscopic Physics Frontiers Science Center for Nano‐Optoelectronics School of Physics Peking University Beijing 100871 China

2. Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China

3. School of Materials Science and Engineering Nanchang Hangkong University Nanchang 330063 China

4. International Center for Quantum Materials Collaborative Innovation Center of Quantum Matter Peking University Beijing 100871 China

5. Songshan Lake Materials Lab Institute of Physics Chinese Academy of Sciences Dongguan 523808 China

6. Key Laboratory of Quantum State Construction and Manipulation (Ministry of Education) Department of Physics Renmin University of China Beijing 100872 China

Abstract

AbstractNonlinear optical crystals lie at the core of ultrafast laser science and quantum communication technology. The emergence of 2D materials provides a revolutionary potential for nonlinear optical crystals due to their exceptionally high nonlinear coefficients. However, uncontrolled stacking orders generally induce the destructive nonlinear response due to the optical phase deviation in different 2D layers. Therefore, conversion efficiency of 2D nonlinear crystals is typically limited to less than 0.01% (far below the practical criterion of >1%). Here, crystalline films of rhombohedral boron nitride (rBN) with parallel stacked layers are controllably synthesized. This success is realized by the utilization of vicinal FeNi (111) single crystal, where both the unidirectional arrangement of BN grains into a single‐crystal monolayer and the continuous precipitation of (B,N) source for thick layers are guaranteed. The preserved in‐plane inversion asymmetry in rBN films keeps the in‐phase second‐harmonic generation field in every layer and leads to a record‐high conversion efficiency of 1% in the whole family of 2D materials within the coherence thickness of only 1.6 µm. The work provides a route for designing ultrathin nonlinear optical crystals from 2D materials, and will promote the on‐demand fabrication of integrated photonic and compact quantum optical devices.

Funder

National Key Research and Development Program of China

National Natural Science Foundation of China

Publisher

Wiley

Subject

Mechanical Engineering,Mechanics of Materials,General Materials Science

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