Materials composed of spin-1 antiferromagnetic (AFM) chains are known to adopt complex ground states that are sensitive to the single-ion-anisotropy (SIA) energy (
D), and intrachain (
J0) and interchain (
J1,2′) exchange energy scales. While theoretical and experimental studies have extended this model to include various other energy scales, the effect of the lack of a common SIA axis is not well explored. Here we investigate the magnetic properties of
Ni(pyrimidine)(H2O)2(NO3)2, a chain compound where the tilting of Ni octahedra leads to a twofold alternation of the easy-axis directions along the chain. Muon-spin relaxation measurements indicate a transition to long-range order at
TN=2.3K and the magnetic structure is initially determined to be antiferromagnetic and collinear using elastic neutron diffraction experiments. Inelastic neutron scattering measurements were used to find
J0=5.107(7)K, D=2.79(1)K,J1′=0.00(5)K, J2′=0.18(3)K, and a rhombic anisotropy energy
E=0.19(9)K. Mean-field modeling reveals that the ground state structure hosts spin canting of
ϕ≈6.5∘, which is not detectable above the noise floor of the elastic neutron diffraction data. Monte Carlo simulation of the powder-averaged magnetization,
M(H), is then used to confirm these Hamiltonian parameters, while single-crystal
M(H) simulations provide insight into features observed in the data. Published by the American Physical Society 2025