Abstract
We investigate the magnetic properties of S=1 antiferromagnetic diamond-lattice, NiX2(pyrimidine)2 (X=Cl, Br), hosting a single-ion anisotropy (SIA) orientation which alternates between neighboring sites. Through neutron diffraction measurements of the X=Cl compound, the ordered state spins are found to align collinearly along a pseduo-easy axis, a unique direction created by the intersection of two easy planes. Similarities in the magnetization, exhibiting spin-flop transitions, and the magnetic susceptibility in the two compounds imply that the same magnetic structure and a pseduo-easy axis is also present for X=Br. We estimate the Hamiltonian parameters by combining analytical calculations and Monte Carlo (MC) simulations of the spin-flop and saturation field. The MC simulations also reveal that the spin-flop transition occurs when the applied field is parallel to the pseduo-easy axis. Contrary to conventional easy-axis systems, there exist field directions perpendicular to the pseduo-easy axis for which the magnetic saturation is approached asymptotically and no symmetry-breaking phase transition is observed at finite fields. Published by the American Physical Society 2024
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