Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3

Amber McCreary; Thuc T Mai; Franz G Utermohlen; Jeffrey R Simpson; Kevin F Garrity; Xiaozhou Feng; Dmitry Shcherbakov; Yanglin Zhu; Jin Hu; Daniel Weber; Kenji Watanabe; Takashi Taniguchi; Joshua E Goldberger; Zhiqiang Mao; Chun Ning Lau; Yuanming Lu; Nandini Trivedi; Rolando Valdés Aguilar; Angela R Hight Walker

doi:10.1038/s41467-020-17320-3

Distinct magneto-Raman signatures of spin-flip phase transitions in CrI₃

Nat Commun. 2020 Aug 3;11(1):3879. doi: 10.1038/s41467-020-17320-3.

Authors

Amber McCreary¹, Thuc T Mai^{1

2}, Franz G Utermohlen², Jeffrey R Simpson^{1

3}, Kevin F Garrity⁴, Xiaozhou Feng², Dmitry Shcherbakov², Yanglin Zhu⁵, Jin Hu⁶, Daniel Weber^{7

8}, Kenji Watanabe⁹, Takashi Taniguchi⁹, Joshua E Goldberger⁷, Zhiqiang Mao⁵, Chun Ning Lau², Yuanming Lu², Nandini Trivedi², Rolando Valdés Aguilar¹⁰, Angela R Hight Walker¹¹

Affiliations

¹ Nanoscale Device Characterization Division, Physical Measurement Laboratory, National Institute of Standards and Technology, Gaithersburg, MD, 20899, USA.
² Department of Physics, The Ohio State University, Columbus, OH, 43210, USA.
³ Department of Physics, Astronomy, and Geosciences, Towson University, Towson, MD, 21252, USA.
⁴ Materials Measurement Science Division, Material Measurement Laboratory, National Institute of Standards and Technology, Gaithersburg, MD, 20899, USA.
⁵ Department of Physics, The Pennsylvania State University, University Park, PA, 16802, USA.
⁶ Department of Physics, University of Arkansas, Fayetteville, AR, 72701, USA.
⁷ Department of Chemistry and Biochemistry, The Ohio State University, Columbus, OH, 43210, USA.
⁸ Battery and Electrochemistry Laboratory, Institute of Nanotechnology, Karlsruhe Institute of Technology, 76344, Eggenstein-Leopoldshafen, Germany.
⁹ National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
¹⁰ Department of Physics, The Ohio State University, Columbus, OH, 43210, USA. valdesaguilar.1@osu.edu.
¹¹ Nanoscale Device Characterization Division, Physical Measurement Laboratory, National Institute of Standards and Technology, Gaithersburg, MD, 20899, USA. angela.hightwalker@nist.gov.

Abstract

The discovery of 2-dimensional (2D) materials, such as CrI₃, that retain magnetic ordering at monolayer thickness has resulted in a surge of both pure and applied research in 2D magnetism. Here, we report a magneto-Raman spectroscopy study on multilayered CrI₃, focusing on two additional features in the spectra that appear below the magnetic ordering temperature and were previously assigned to high frequency magnons. Instead, we conclude these modes are actually zone-folded phonons. We observe a striking evolution of the Raman spectra with increasing magnetic field applied perpendicular to the atomic layers in which clear, sudden changes in intensities of the modes are attributed to the interlayer ordering changing from antiferromagnetic to ferromagnetic at a critical magnetic field. Our work highlights the sensitivity of the Raman modes to weak interlayer spin ordering in CrI₃.