Anticollinear order and degeneracy lifting in square lattice antiferromagnet LaSrCrO4

We report the static and dynamic magnetic properties of LaSrCrO4, a seemingly canonical spin-3/2 square-lattice antiferromagnet that exhibits frustration between magnetic layers - owing to their AB stacking - and offers a rare testbed to investigate accidental-degeneracy lifting in magnetism. Neutron diffraction experiments on single-crystal samples uncover a remarkable anticollinear magnetic order below TN = 170 K characterized by a Néel arrangement of the spins within each layer and an orthogonal arrangement between adjacent layers. To understand the origin of this unusual magnetic structure, we analyze the spin-wave excitation spectrum by means of inelastic neutron scattering and bulk measurements. A spectral gap of 0.5 meV, along with a spin-flop transition at 3.2 T, reflect the energy scale associated with the degeneracy-lifting. A minimal model to explain these observations requires both a positive biquadratic interlayer exchange and dipolar interactions, both of which are on the order of 10-4 meV, only a few parts per million of the dominant exchange interaction J1≈11 meV. These results provide direct evidence for the selection of a noncollinear magnetic structure by the combined effect of two distinct degeneracy lifting interactions.