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Recently it was discovered that van der Waals-bonded magnetic materialsretain long range magnetic ordering down to a single layer, opening manyavenues in fundamental physics and potential applications of these fascinatingmaterials. One such material is FePS3, a large spin (S=2) Mott insulator wherethe Fe atoms form a honeycomb lattice. In the bulk, FePS3 has been shown to bea quasi-two-dimensional-Ising antiferromagnet, with additional features in theRaman spectra emerging below the Neel temperature of approximately 120 K. Usingmagneto-Raman spectroscopy as an optical probe of magnetic structure, we showthat one of these Raman-active modes in the magnetically ordered state isactually a magnon with a frequency of of approximately 3.7 THz (122 cm-1).Contrary to previous work, which interpreted this feature as a phonon, ourRaman data shows the expected frequency shifting and splitting of the magnon asa function of temperature and magnetic field, respectively, where we determinethe g-factor to be approximately 2. In addition, the symmetry behavior of themagnon is studied by polarization-dependent Raman spectroscopy and explainedusing the magnetic point group of FePS3.

Quasi-Two-Dimensional Magnon Identification in Antiferromagnetic FePS3 via Magneto-Raman Spectroscopy