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

Amber McCreary, et al.

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Oct 30, 2019

Received Date: 14th October 19

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

The discovery of 2-dimensional (2D) materials, such as CrI3, that retain magnetic ordering at monolayer thickness has resulted in a surge of research in 2D magnetism from both pure and applied perspectives. Here, we report a magneto-Raman spectroscopy study on multilayered CrI3, focusing on two new features in the spectra which appear at temperatures below the magnetic ordering temperature and were previously assigned to high frequency magnons. We observe a striking evolution of the Raman spectra with increasing magnetic field 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. In addition, we theoretically examine potential origins for the new modes, which we deduce are unlikely single magnons.

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This is an abstract of a preprint hosted on an independent third party site. It has not been peer reviewed but is currently under consideration at Nature Communications.

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