High-Angular Momentum Excitations in Collinear Antiferromagnet FePS3

We report on magneto-optical studies of the quasi-two-dimensional van der Waals antiferromagnet FePS3. Our measurements reveal an excitation that closely resembles the antiferromagnetic resonance mode typical of easy-axis antiferromagnets; nevertheless, it displays an unusual, four-times larger Zeeman splitting in an applied magnetic field. We identify this excitation with an |Sz| = 4 multipolar magnon─a single-ion 4-magnon bound state─that corresponds to a full reversal of a single magnetic moment of the Fe2+ ion. We argue that condensation of multipolar magnons in large-spin materials with a strong magnetic anisotropy can produce new exotic states.