Phase‐Controlled Synthesis of Large‐Area Trigonal 2D Cr2S3 Thin Films via Ultralow Gas‐Flow Governed Dynamic Transport

Author:

Fan Xiulian1,Chen Zhihui1ORCID,Xu Defeng1,Zou Luwei1,Ouyang Fangping123,Deng Shibin45,Wang Xiao6,Zhao Jiong7,Zhou Yu12ORCID

Affiliation:

1. School of Physics Hunan Key Laboratory of Nanophotonics and Devices Central South University 932 South Lushan Road Changsha Hunan 410083 P. R. China

2. State Key Laboratory of Powder Metallurgy Central South University Changsha Hunan 410083 P. R. China

3. School of Physical Science and Technology Xinjiang University Urumqi 830046 P. R. China

4. Ultrafast Electron Microscopy Laboratory School of Physics Nankai University Tianjin 300071 P. R. China

5. The MOE Key Laboratory of Weak‐Light Nonlinear Photonics School of Physics Nankai University Tianjin 300071 P. R. China

6. Key Laboratory for Micro‐Nano Physics and Technology of Hunan Province College of Materials Science and Engineering Hunan University Changsha 410082 P. R. China

7. Department of Applied Physics The Hong Kong Polytechnic University Kowloon Hong Kong 999077 P. R. China

Abstract

AbstractAs for nonlayered 2D polymorphic materials, especially for Cr‐based chalcogenides, large‐area thin film growth with phase control is considered the most important synthesis challenge for magnetic, electronic, and optoelectronic devices. However, the synthesis methods of large continuous thin films for nonlayered 2D materials are still limited and rarely reported, also for the phase control growth, which is inhibited by isotropic 3D growth and similar Gibbs free energy for different phases. Herein, enhanced mass transport chemical vapor deposition is established to achieve the control synthesis of trigonal Cr2S3 thin films, in which the stable boundary layer supplies the continuous reaction species and tunes the reaction kinetics. The trigonal phase formation is confirmed by atomic structure characterization, optical absorption and piezoelectric measurements, demonstrating unique physical properties different from rhombohedral phase. The trigonal Cr2S3 thin films show obvious layer independent and dissimilar angle‐resolved harmonic generation, indicating the surface broken symmetry that can be understood by the combination of negligible piezoelectric response for bulk. The work presents the large‐area synthesized strategy by the modification of mass transport for nonlayered 2D materials with new phase formation and establishes the surface symmetry breaking dominated SHG mechanism for future nonlinear optical materials.

Funder

Natural Science Foundation of Hunan Province

National Natural Science Foundation of China

Publisher

Wiley

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