Neutron study of the magnetism in NiCl2⋅4SC(NH2)2

We study the strongly anisotropic quasi-one-dimensional S = 1 quantum magnet NiCl2⋅4SC(NH2)2 using elastic and inelastic neutron scattering. We demonstrate that a magnetic field splits the excited doublet state and drives the lower doublet state to zero energy at a critical field Hc1. For Hc1 <H <Hc2, where Hc2 indicates the transition to a fully magnetized state, three-dimensional magnetic order is established with the AF moment perpendicular to the magnetic field. We mapped the temperature/magnetic field phase diagram, and we find that the total ordered magnetic moment reaches mtot = 2.1 μB at the field μH = 6 T and is thus close to the saturation value of the fully ordered moment. We study the magnetic spin dynamics in the fully magnetized state for H > Hc2, and we demonstrate the presence of an AF interaction between Ni2+ on the two interpenetrating sublattices. In the antiferromagnetically ordered phase, the spin-waves that develop from the lower-energy doublet are split into two modes. This is most likely the result of the presence of the AF interaction between the interpenetrating lattices.