Observation of 4- and 6-Magnon Bound States in the Spin-Anisotropic Frustrated Antiferromagnet FeI2

Abstract

Spin-waves e.g. magnons are the conventional elementary excitations of ordered magnets. However, other possibilities exist. For instance, magnon bound-states can arise due to attractive magnon-magnon interactions and drastically impact the static and dynamic properties of materials. Here, we demonstrate a zoo of distinct multi-magnon quasiparticles in the frustrated spin-1 triangular antiferromagnet FeI$_2$ using time-domain terahertz spectroscopy. The energy-magnetic field excitation spectrum contains signatures of one-, two-, four- and six-magnon bound-states, which we analyze using an exact diagonalization approach for a dilute gas of interacting magnons. The two-magnon single-ion bound states occur due to strong anisotropy and the preponderance of even higher order excitations arises from the tendency of the single-ion bound states to themselves form bound states due to their very flat dispersion. This menagerie of tunable interacting quasiparticles provides a unique platform in a condensed matter setting that is reminiscent of the few-body quantum phenomena central to cold-atom, nuclear, and particle physics experiments.