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Strengthening the Magnetic Interactions in Pseudobinary First-Row Transition Metal Thiocyanates, M(NCS)2


Euan N. Bassey

Joseph A.M. Paddison

Evan N. Keyzer

Jeongjae Lee

Pascal Manuel

Ivan da Silva


Clare P. Grey


Understanding the effect of chemical composition on the strength of magnetic interactions is key to the design of magnets with high operating temperatures. The magnetic divalent first-row transition metal (TM) thiocyanates are a class of chemically simple layered molecular frameworks. Here, we report two new members of the family, manganese (II) thiocyanate, Mn(NCS)2, and iron (II) thiocyanate, Fe(NCS)2. Using magnetic susceptibility measurements on these materials and on cobalt (II) thiocyanate and nickel (II) thiocyanate, Co(NCS)2 and Ni(NCS)2, respectively, we identify significantly stronger net antiferromagnetic interactions between the earlier TM ions-a decrease in the Weiss constant, ?, from 29 K for Ni(NCS)2 to ?115 K for Mn(NCS)2-a consequence of more diffuse 3d orbitals, increased orbital overlap and increasing numbers of unpaired t2g electrons. We elucidate the magnetic structures of these materials: Mn(NCS)2, Fe(NCS)2 and Co(NCS)2 order into the same antiferromagnetic commensurate ground state, whilst Ni(NCS)2 adopts a ground state structure consisting of ferromagnetically ordered layers stacked antiferromagnetically. We show that significantly stronger exchange interactions can be realised in these thiocyanate frameworks by using earlier TMs.


Bassey, E. N., Paddison, J. A., Keyzer, E. N., Lee, J., Manuel, P., da Silva, I., …Cliffe, M. J. (2020). Strengthening the Magnetic Interactions in Pseudobinary First-Row Transition Metal Thiocyanates, M(NCS)2. Inorganic Chemistry, 59(16), 11627–11639.

Journal Article Type Article
Acceptance Date Jul 8, 2020
Online Publication Date Jul 27, 2020
Publication Date Aug 17, 2020
Deposit Date Jul 15, 2020
Publicly Available Date Jul 28, 2021
Journal Inorganic Chemistry
Print ISSN 0020-1669
Electronic ISSN 1520-510X
Publisher American Chemical Society
Peer Reviewed Peer Reviewed
Volume 59
Issue 16
Pages 11627–11639
Keywords Physical and Theoretical Chemistry; Inorganic Chemistry
Public URL
Publisher URL
Additional Information This document is the Accepted Manuscript version of a Published Work that appeared in final form in Inorganic Chemistry ,copyright© American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see


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