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Research Article

Room-temperature ferromagnetism and piezoelectricity in metal-free 2D semiconductor crystalline carbon nitride

Yong Wang1,2,§, Dingyi Yang1,3,§, Wei Xu4,§, Yongjie Xu5, Yu Zhang6, Zixuan Cheng1, Yizhang Wu7, Xuetao Gan8( ), Wei Zhong4, Yan Liu1,2( ), Genquan Han1,2, Yue Hao1,2
Wide Bandgap Semiconductor Technology Disciplines State Key Laboratory, School of Microelectronics, Academy of Advanced Interdisciplinary Research, Xidian University, Xi’an 710071, China
Emerging Device and Chip Laboratory, Hangzhou Institute of Technology, Xidian University, Hangzhou 311200, China
INRS Centre for Energy, Materials and Telecommunications, 1650 Boul. Lionel Boulet, Varennes, QC J3X 1P7, Canada
National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures and Jiangsu Provincial Key Laboratory for Nanotechnology, Nanjing University, Nanjing 210093, China
School of Education, Jiangsu Open University, Nanjing 210036, China
Department of Physics, Shaanxi University of Science and Technology, Xi’an 710021, China
Department of Applied Physical Sciences, The University of North Carolina at Chapel Hill, Chapel Hill, NC 27514, USA
Key Laboratory of Light Field Manipulation and Information Acquisition, Ministry of Industry and Information Technology, and Shaanxi Key Laboratory of Optical Information Technology, School of Physical Science and Technology, Northwestern Polytechnical University, Xi'an 710129 China

§ Yong Wang, Dingyi Yang, and Wei Xu contributed equally to this work.

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Graphical Abstract

In this study, we successfully synthesized highly crystalline two-dimensional carbon nitride using carbodiimide as a precursor. Structural characterization and theoretical calculations confirmed that the introduction of C–O–C bonds into the highly ordered heptazine structure leads to localized spins and magnetic ordering, resulting in strong room-temperature ferromagnetism. Furthermore, stress can effectively modulate magnetic behavior and piezoelectric potential at room temperature.

Abstract

Two-dimensional (2D) materials that combine ferromagnetic, semiconductor, and piezoelectric properties hold significant potential for both fundamental research and spin electronic devices. However, the majority of reported 2D ferromagnetic-semiconductor-piezoelectric materials rely on d-electron systems, which limits their practical applications due to a Curie temperature lower than room temperature (RT). Here, we report a high-crystallinity carbon nitride (CCN) material based on sp-electrons using a chemical vapor deposition strategy. CCN exhibits a band gap of 1.8 eV and has been confirmed to possess substantial in-plane and out-of-plane piezoelectricity. Moreover, we acquired clear evidences of ferromagnetic behavior at room temperature. Extensive structural characterizations combined with theoretical calculations reveal that incorporating structural oxygen into the highly ordered heptazine structure causes partial substitution of nitrogen sites, which is primarily responsible for generating room-temperature ferromagnetism and piezoelectricity. As a result, the strain in wrinkles can effectively modulate the domain behavior and piezoelectric potential at room temperature. The addition of RT ferromagnetic-semiconductor-piezoelectric material based on sp-electrons to the family of two-dimensional materials opens up numerous possibilities for novel applications in fundamental research and spin electronic devices.

Keywords

crystallinity carbon nitrideroom-temperature ferromagnetismpiezoelectricitymagnetic force microscopydensity functional theory (DFT) calculations

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Nano Research
Volume 17 Issue 6,
June 2024
Pages 5670-5679
DOI: 10.1007/s12274-024-6491-y
Cite this article:
Wang Y, Yang D, Xu W, et al. Room-temperature ferromagnetism and piezoelectricity in metal-free 2D semiconductor crystalline carbon nitride. Nano Research, 2024, 17(6): 5670-5679. https://doi.org/10.1007/s12274-024-6491-y
Topics:
CarbonFerromagnetic materials Wide band gap semiconductors

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Received: 12 October 2023
Revised: 30 December 2023
Accepted: 15 January 2024
Published: 22 February 2024
© Tsinghua University Press 2024
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