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

06 December 2022, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


AMX3 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, TC = 8.5(1) K) and CsCo(NCS)3 (TC = 6.7(1) K) order as weak ferromagnets. On the other hand, CsMn(NCS)3 orders as an antiferromagnet (Néel temperature, TN = 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.


Molecular magnetism
neutron diffraction
coordination polymers

Supplementary materials

Supplementary information
Experimental details for synthesis, physical property measurements and computational calculations. Additional figures and crystallographic tables with refinement statistics.


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