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  1. 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 ϕ6.5 , 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 Society2025 
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