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, $T_\mathrm{C} = 8.5(1)\;$K) and CsCo(NCS)$_3$ ($T_\mathrm{C} = 6.7(1)\;$K) order as weak ferromagnets. On the other hand, CsMn(NCS)$_3$ orders as an antiferromagnet (N\'eel temperature, $T_\mathrm{N}=16.8(8)\;$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.