Pseudo-easy-axis anisotropy in antiferromagnetic S=1 diamond-lattice systems NiX₂(pym)₂

We investigate the magnetic properties of $S=1$ antiferromagnetic diamond lattice, Ni$X_{2}$(pyrimidine)$_{2}$ ($X$ = Cl, Br), hosting a single-ion anisotropy (SIA) orientation which alternates between neighbouring sites. Through neutron diffraction measurements of the $X$ = Cl compound, the ordered state spins are found to align collinearly along a pseudo-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 pseudo-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 pseudo-easy-axis. Contrary to conventional easy-axis systems, there exist field directions perpendicular to the pseudo-easy-axis for which the magnetic saturation is approached asymptotically and no symmetry-breaking phase transition is observed at finite fields.