Evidence for biquadratic exchange in the quasi-two-dimensional antiferromagnet FePS₃

FePS$3$ is a van der Waals compound with a honeycomb lattice that is a good example of a two-dimensional antiferromagnet with Ising-like anisotropy. Neutron spectroscopy data from FePS$3$ were previously analyzed using a straightforward Heisenberg Hamiltonian with a single-ion anisotropy. The analysis captured most of the elements of the data; however, some significant discrepancies remained. The discrepancies were most obvious at the Brillouin zone boundaries. The data are subsequently reanalyzed, allowing for unequal exchange between nominally equivalent nearest-neighbors, which resolves the discrepancies. The source of the unequal exchange is attributed to a biquadratic exchange term in the Hamiltonian, which most probably arises from a strong magnetolattice coupling. The new parameters show that there are features consistent with Dirac magnon nodal lines along certain Brillouin zone boundaries.