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

Bassey, Euan N.; Paddison, Joe A.M.; Keyzer, Evan N.; Lee, Jeongjae; Manuel, Pascal; da Silva, Ivan; Dutton, Siân E.; Grey, Clare P.; Cliffe, Matthew J.

doi:10.1021/acs.inorgchem.0c01478

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

Journal Article · Mon Jul 27 00:00:00 EDT 2020 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.0c01478· OSTI ID:1657972

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Univ. of Cambridge (United Kingdom)
Univ. of Cambridge (United Kingdom). Cavendish Lab.; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Cambridge (United Kingdom); Seoul National Univ., Seoul (Korea)
Science and Technology Facilities Council (STFC), Oxford (United Kingdom). Rutherford Appleton Lab., ISIS Neutron Source
Univ. of Cambridge (United Kingdom). Cavendish Lab.
Univ. of Cambridge (United Kingdom); Univ. of Nottingham (United Kingdom). School of Chemistry

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, θ, 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 $$t_{2_g}$$ 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, while Ni(NCS)₂ adopts a ground state structure consisting of ferromagnetically ordered layers stacked antiferromagnetically. We show that significantly stronger exchange interactions can be realized in these thiocyanate frameworks by using earlier TMs.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); University of Cambridge, United Kingdom; University of Nottingham, United Kingdom; Engineering and Physical Sciences Research Council (EPSRC)

Grant/Contract Number:: AC05-00OR22725; EP/M000524/1

OSTI ID:: 1657972

Journal Information:: Inorganic Chemistry, Vol. 59, Issue 16; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 9 works

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CSD 2006184: Experimental Crystal Structure Determination N., Bassey, Euan; M., Paddison, Joseph A.; N., Keyzer, Evan https://doi.org/10.5517/ccdc.csd.cc25blmr The current record is supplemented by this dataset	dataset	January 2020
CCDC 2006185: Experimental Crystal Structure Determination N., Bassey, Euan; M., Paddison, Joseph A.; N., Keyzer, Evan https://doi.org/10.5517/ccdc.csd.cc25blns The current record is supplemented by this dataset	dataset	January 2020
CCDC 2006186: Experimental Crystal Structure Determination N., Bassey, Euan; M., Paddison, Joseph A.; N., Keyzer, Evan https://doi.org/10.5517/ccdc.csd.cc25blpt The current record is supplemented by this dataset	dataset	January 2020
CCDC 2006187: Experimental Crystal Structure Determination N., Bassey, Euan; M., Paddison, Joseph A.; N., Keyzer, Evan https://doi.org/10.5517/ccdc.csd.cc25blqv The current record is supplemented by this dataset	dataset	January 2020

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

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