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The discovery of 2-dimensional (2D) materials, such as CrI3, that retainmagnetic ordering at monolayer thickness has resulted in a surge of research in2D magnetism from both pure and applied perspectives. Here, we report amagneto-Raman spectroscopy study on multilayered CrI3, focusing on two newfeatures in the spectra which appear at temperatures below the magneticordering temperature and were previously assigned to high frequency magnons. Weobserve a striking evolution of the Raman spectra with increasing magneticfield in which clear, sudden changes in intensities of the modes are attributedto the interlayer ordering changing from antiferromagnetic to ferromagnetic ata critical magnetic field. Our work highlights the sensitivity of the Ramanmodes to weak interlayer spin ordering in CrI3. In addition, we theoreticallyexamine potential origins for the new modes, which we deduce are unlikelysingle magnons.

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