journal article·2021-06-22Open access

Structural Monoclinicity and Its Coupling to Layered Magnetism in Few-Layer CrI3

Xiaoyu Guo, Wencan Jin, Zhipeng Ye, Gaihua Ye, Hongchao Xie, Bowen Yang, Hyun Ho Kim, Shaohua Yan, Yang Fu, Shangjie Tian, Hechang Lei, Adam W. Tsen, Kai Sun, Jia-An Yan, Rui He, Liuyan Zhao

ACS Nano· Volume 15· Issue 6

Abstract

Using polarization-resolved Raman spectroscopy, we investigate layer number, temperature, and magnetic field dependence of Raman spectra in one- to four-layer CrI3. Layer-number-dependent Raman spectra show that in the paramagnetic phase a doubly degenerated Eg mode of monolayer CrI3 splits into one Ag and one Bg mode in N-layer (N > 1) CrI3 due to the monoclinic stacking. Their energy separation increases in thicker samples until an eventual saturation. Temperature-dependent measurements further show that the split modes tend to merge upon cooling but remain separated until 10 K, indicating a failed attempt of the monoclinic-to-rhombohedral structural phase transition that is present in the bulk crystal. Magnetic-field-dependent measurements reveal an additional monoclinic distortion across the magnetic-field-induced layered antiferromagnetism-to-ferromagnetism phase transition. We propose a structural change that consists of both a lateral sliding toward the rhombohedral stacking and a decrease in the interlayer distance to explain our experimental observations.
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Research context

OpenAlex topics: 2D Materials and Applications · Heusler alloys: electronic and magnetic properties · MXene and MAX Phase Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Physics, University of Michigan, 450 Church Street, Ann Arbor, Michigan 48109, United States

Department of Physics, Auburn University, 380 Duncan Drive, Auburn, Alabama 36849, United States

Department of Electrical and Computer Engineering, Texas Tech University, 910 Boston Avenue, Lubbock, Texas 79409, United States

Institute for Quantum Computing, Department of Physics and Astronomy, and Department of Chemistry, University of Waterloo, Waterloo, ON N2L 3G1, Canada

School of Materials Science and Engineering, Kumoh National Institute of Technology, Gumi 39177, Korea

Department of Physics and Beijing Key Laboratory of Optoelectronic Functional Materials & Micro-nano Devices, Renmin University of China, 100872 Beijing, China

Department of Physics, Astronomy & Geosciences, Towson University, Towson, Maryland 21252, United States

Funding

Division of Emerging Frontiers in Research and Innovation · Army Research Office · Air Force Office of Scientific Research · Canada First Research Excellence Fund · National Natural Science Foundation of China · Division of Materials Research · Fundamental Research Funds for the Central Universities and Research Funds of Renmin University of China · National Key R&D Program of China · National Science and Engineering Research Council of Canada · Ontario Early Researcher Award · Beijing Natural Science Foundation

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