Single-ion anisotropy driven chiral magnetic order in a spin-1 antiferromagnetic chain

Chirality in magnetic systems gives rise to a wide range of exotic phenomena, yet its influence in S = 1 chains remains largely unexplored. Herein, we present a comprehensive experimental study of a chiral antiferromagnetic S = 1 chain, [ Ni ( pym ) ( H 2 O ) 4 ] SO 4 · H 2 O (pym = pyrimidine), where the Ni(II) octahedral orientation exhibits a fourfold chiral periodicity. Muon-spin rotation measurements indicate the onset of long-range magnetic order below T N = 1.82 ( 1 ) K . Neutron diffraction measurements reveal a chiral antiferromagnetic order driven by a chiral modulation of the easy-axis anisotropy direction, rather than the typical scenario of Dzyaloshinskii-Moriya interactions, geometrical frustration, or higher-order interactions. Inelastic neutron scattering measurements reveal dispersive spin-wave excitations well described by linear spin-wave theory, with Hamiltonian parameters J 0 = 6.81 ( 1 ) K (intrachain exchange), J 1 a ′ = − 0.09 ( 1 ) K (interchain exchange), and D = − 3.02 ( 1 ) K (easy-axis single-ion anisotropy). These parameters are further validated by Monte Carlo simulations of the magnetization. Additionally, the inelastic neutron scattering data reveal multiple dispersionless bands, suggesting the presence of further excitations beyond the scope of our linear spin-wave theory.