Non-collinear magnetism in the post-perovskite thiocyanate frameworks CsM(NCS)(3)

AMX(3) compounds are structurally diverse, a notable example being the post-perovskite structure which adopts a two-dimensional framework with corner- and edge-sharing octahedra. Few molecular post-perovskites are known and of these, none have reported magnetic structures. Here we report the synthesis, structure and magnetic properties of molecular post-perovskites: CsNi(NCS)(3), a thiocyanate framework, and two new isostructural analogues CsCo(NCS)(3) and CsMn(NCS)(3). Magnetisation measurements show that all three compounds undergo magnetic order. CsNi(NCS)(3) (Curie temperature, T(C) = 8.5(1) K) and CsCo(NCS)(3) (T(C) = 6.7(1) K) order as weak ferromagnets. On the other hand, CsMn(NCS)(3) orders as an antiferromagnet (Néel temperature, T(N) = 16.8(8) K). Neutron diffraction data of CsNi(NCS)(3) and CsMn(NCS)(3), show that both are non-collinear magnets. These results suggest molecular frameworks are fruitful ground for realising the spin textures required for the next generation of information technology.