Recent observations of long-ranged magnetic ordering in van der Waals bonded, layered magnetic materials down to the single layer limit has led to a plethora of research dedicated to the study of two-dimensional (2D) magnets, with plenty of opportunities to investigate fundamental physics and potential quantum applications. With these materials, the properties are typically strongly correlated to the number of layers, with new physics occurring in the few-layer (~few nm) regime. In this sense, common techniques used to measure magnetic behaviors such as neutron scattering and SQUID are at a disadvantage due to sample size requirements. On the other hand, Raman spectroscopy, which has diffraction-limited spatial resolution, is a powerful, non-destructive optical method to probe magnetism in 2D layered materials through inelastic scattering as a function of temperature, laser energy, polarization, and magnetic field. One material of particular interest is chromium tri-iodide (CrI3), a ferromagnet at bulk thicknesses below the Curie temperature but with the remarkable property of layered antiferromagnetism in thin multilayers. Here, we will report on a magneto-Raman spectroscopy study on multi-layered CrI3 [1], 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 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. In addition, through DFT-calculations and symmetry arguments, we conclude that the new modes are not magnons as previously believed, but instead are zone-folded phonons.References: [1] A. McCreary et al. arXiv:1910.01237.

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

O1: 2D Magnetic Materials

technical paper

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Amber McCreary

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

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