Abstract
We report an investigation of the magnetic structure and magnetic exchange pathways in MnS via neutron scattering methods, aided by density functional theory (DFT) modeling. The material has been confirmed to undergo antiferromagnetic (AFM) ordering at 152 K, with the magnetic structure representing AFM stacking of ferromagnetic (FM) (111) planes of Mn magnetic moments. Correspondingly, the magnetic structure is described by a propagation vector k = (1/2, 1/2, 1/2), with the volume of the magnetic unit cell being 8 times larger than the volume of the nuclear unit cell. Analysis of inelastic neutron scattering (INS) data collected on a powder sample of MnS revealed that the next-nearest-neighbor magnetic exchange constant (J2) exceeds the nearest-neighbor exchange constant (J1) by more than 3 times, while in the case of MnO, which exhibits the same nuclear and magnetic structures as MnS, the J2/J1 ratio was reported to be below 1.5. Although for MnO the signs of both J1 and J2 indicated AFM exchange interactions, machine-learning INS data analysis in combination with DFT calculations suggests that the INS data collected on MnS are best described with J1 < 0 and J2 > 0, corresponding to FM and AFM exchange couplings, respectively. To achieve a satisfactory fit to the experimentally observed data, the Hamiltonian used to model the INS spectra also included the next-next-nearest-neighbor magnetic exchange constant (J3). The best-fit model has been obtained with the values of the exchange constants J1 = −0.27 meV, J2 = 1.05 meV, and J3 = −0.19 meV.
