Distinct magneto-Raman signatures of spin-flip phase transitions in CrI(3)

The discovery of 2-dimensional (2D) materials, such as CrI(3), 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 CrI(3), 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 CrI(3).