High-angular momentum excitations in collinear antiferromagnet FePS$_3$

Abstract

We report on magneto-optical studies of the quasi-two-dimensional van der Waals antiferromagnet FePS$_3$. 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 $|S_z|=4$ multipolar magnon -- a single-ion 4-magnon bound state -- that corresponds to a full reversal of a single magnetic moment of the Fe$^{2+}$ ion. We argue that condensation of multipolar magnons in large-spin materials with a strong magnetic anisotropy can produce new exotic states.