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

We study the strongly anisotropic quasi-one-dimensional S = 1 quantum magnet NiCl2 center dot 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 H-c1. For H-c1 < H < H-c2, where H-c2 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 m(tot) = 2.1 mu(B) at the field mu H-0 = 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 > H-c2, 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.