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 () and Angela R. Hight Walker ()
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Amber McCreary: National Institute of Standards and Technology
Thuc T. Mai: National Institute of Standards and Technology
Franz G. Utermohlen: The Ohio State University
Jeffrey R. Simpson: National Institute of Standards and Technology
Kevin F. Garrity: National Institute of Standards and Technology
Xiaozhou Feng: The Ohio State University
Dmitry Shcherbakov: The Ohio State University
Yanglin Zhu: The Pennsylvania State University
Jin Hu: University of Arkansas
Daniel Weber: The Ohio State University
Kenji Watanabe: National Institute for Materials Science
Takashi Taniguchi: National Institute for Materials Science
Joshua E. Goldberger: The Ohio State University
Zhiqiang Mao: The Pennsylvania State University
Chun Ning Lau: The Ohio State University
Yuanming Lu: The Ohio State University
Nandini Trivedi: The Ohio State University
Rolando Valdés Aguilar: The Ohio State University
Angela R. Hight Walker: National Institute of Standards and Technology

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41467-020-17320-3

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