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Layer dependence of stacking order in nonencapsulated few-layer CrI3

本征铁磁二维材料CrI3层间堆叠结构层数依赖性研究

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Abstract

Long-range magnetic orders in atomically thin ferromagnetic CrI3 trigger new fascinating physics and application perspectives. The physical properties of two-dimensional (2D) ferromagnetism CrI3 are significantly influenced by interlayer spacing and stacking order, which are sensitive to the hydrostatic pressure and external environments. However, there remains debate on the stacking order at low temperature. Here, we study the interlayer coupling and stacking order of non-encapsulated 2–5 layer and bulk CrI3 at 10 K by Raman spectroscopy; demonstrate a rhombohedral stacking in both antiferromagnetic and ferromagnetic CrI3. The opposite helicity dependence of Ag and Eg modes arising from phonon symmetry further validates the rhombohedral stacking. An anomalous temperature-dependent behavior is observed due to spin-phonon coupling below 60 K. Our study provides insights into the interlayer coupling and stacking orders of 2D ferromagnetic materials.

摘要

二维体系中的长程铁磁序现象再次打破了Mermin-Wagner理论. 铁磁二维材料的铁磁性与层层堆叠的顺序、 结构、 层间距息息相关. 目前对铁磁二维材料CrI3在低温下的堆叠顺序和结构仍不确定, 且未见报道. 针对该科学问题, 本工作深入研究了2–5层及块体CrI3的拉曼特征, 详细研究了拉曼特征峰与层数、 偏振、 旋光和温度之间的依赖关系; 揭示了2–5层及块体CrI3在低温下(10 K)为菱方堆叠结构, 解决了领域内关于CrI3低温结构的争议, 填补了该领域的研究空白, 并发现了自旋声子耦合现象. 本工作开创了独特的磁光电原位传输测量系统, 从样品制备到表征完全与空气隔绝, 避免样品污染和损坏, 因此, 本工作更准确地表征出了CrI3最本征的结构特性.

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Acknowledgements

We acknowledge the financial support from the National Natural Science Foundation of China (51602040 and 51872039), the Science and Technology Program of Sichuan (M112018JY0025) and the Scientific Research Foundation for New Teachers of UESTC (A03013023601007).

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Authors and Affiliations

  1. National Engineering Research Center of Electromagnetic Radiation Control Materials, School of Electronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu, 611731, China

    Kai Guo  (郭锴), Zhen Liu  (刘镇), Zhongtai Shi  (石钟太), Lei Bi  (毕磊), Li Zhang  (张丽), Haipeng Lu  (陆海鹏), Peiheng Zhou  (周佩珩), Linbo Zhang  (张林博) & Bo Peng  (彭波)

  2. Key Laboratory of Flexible Electronics & Institute of Advanced Materials, Jiangsu National Synergetic Innovation Center for Advanced Materials, Nanjing Tech University, Nanjing, 211816, China

    Chaofeng Gao  (高超峰) & Yingchun Cheng  (程迎春)

  3. Department of Physics, Broida Hall, University of California, Santa Barbara, CA, 93106-9530, USA

    Bowen Deng  (邓博文)

  4. Key Laboratory of Multi-spectral Absorbing Materials and Structures of Ministry of Education, University of Electronic Science and Technology of China, Chengdu, 611731, China

    Kai Guo  (郭锴), Zhen Liu  (刘镇), Zhongtai Shi  (石钟太), Lei Bi  (毕磊), Li Zhang  (张丽), Haipeng Lu  (陆海鹏), Peiheng Zhou  (周佩珩), Linbo Zhang  (张林博) & Bo Peng  (彭波)

Authors
  1. Kai Guo  (郭锴)
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  2. Bowen Deng  (邓博文)
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  3. Zhen Liu  (刘镇)
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  4. Chaofeng Gao  (高超峰)
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  5. Zhongtai Shi  (石钟太)
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  6. Lei Bi  (毕磊)
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  7. Li Zhang  (张丽)
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  8. Haipeng Lu  (陆海鹏)
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  9. Peiheng Zhou  (周佩珩)
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  10. Linbo Zhang  (张林博)
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  11. Yingchun Cheng  (程迎春)
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  12. Bo Peng  (彭波)
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Contributions

Author contributions Peng B developed the concept, designed the experiment and prepared the manuscript. Cheng Y synthesized the CrI3 crystal. Deng B, Guo K, Liu Z, Gao C and Shi Z prepared the CrI3 samples and performed the Raman measurements. Bi L, Zhou P, Zhang L, Lu H and Zhang L contributed to mechanism of Raman scattering.

Corresponding authors

Correspondence to Linbo Zhang  (张林博) or Bo Peng  (彭波).

Ethics declarations

Conflict of interest The authors declare no competing financial interests.

Additional information

Bo Peng received his BSc (Honors) from Lanzhou University in 2005, and obtained his PhD degree from the Technical Institute of Physics and Chemistry, Chinese Academy of Sciences in 2010. He did his postdoctoral research in Singapore between 2010 and 2015. He is currently the Head of the Magneto-optical 2D Materials Group in the University of Electronic Science and Technology of China. His research is focused on the 2D ferromagnetic materials toward spintronics and valleytronics.

Kai Guo received his BSc from the University of Electronic Science and Technology of China in 2017. He focuses his research on the Raman studies of 2D ferromagnetic CrI3.

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Guo, K., Deng, B., Liu, Z. et al. Layer dependence of stacking order in nonencapsulated few-layer CrI3. Sci. China Mater. 63, 413–420 (2020). https://doi.org/10.1007/s40843-019-1214-y

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  • DOI: https://doi.org/10.1007/s40843-019-1214-y

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