Thermally-induced mimicry of quantum cluster excitations and implications for the magnetic transition in FePX₃

In two dimensional magnets, the interplay of thermal fluctuations and spin anisotropy control the existence of long-range magnetic order. In the van der Waals antiferromagnets FePX₃, orbital degeneracy in the t2g levels of the Fe²⁺ ions in octahedral coordination yields strong uniaxial anisotropy, which stabilizes magnetic order up to T ≈ 100 K. Recent inelastic neutron scattering measurements around the magnetic ordering transition have shown the existence of a broad spectrum of magnetic fluctuations with nontrivial momentum dependence, what has been interpreted as evidence for localized entangled cluster excitations. In this paper, we offer an alternative interpretation using classical non-linear spin dynamics simulations. We present stochastic Landau Lifshitz dynamics simulations that reproduce the neutron scattering measurements of Chen et al. [1] on FePX₃. These calculations faithfully explain the dynamical structure factor's momentum and energy dependence and point to a classical origin for the excitations observed in neutron spectroscopy and that the order-disorder transition can be understood in terms of thermal fluctuations overcoming the anisotropy energy.