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Magnetic ground state of the one-dimensional ferromagnetic chain compounds M(NCS)2(thiourea)2 (M=Ni,Co)

Curley, S.P.M.; Scatena, R.; Williams, R.C.; Goddard, P.A.; Macchi, P.; Hicken, T.J.; Lancaster, T.; Xiao, F.; Blundell, S.J.; Zapf, V.; Eckert, J.C.; Krenkel, E.H.; Villa, J.A.; Rhodehouse, M.L.; Manson, J.L.

Magnetic ground state of the one-dimensional ferromagnetic chain compounds M(NCS)2(thiourea)2 (M=Ni,Co) Thumbnail


Authors

S.P.M. Curley

R. Scatena

R.C. Williams

P.A. Goddard

P. Macchi

T.J. Hicken

F. Xiao

S.J. Blundell

V. Zapf

J.C. Eckert

E.H. Krenkel

J.A. Villa

M.L. Rhodehouse

J.L. Manson



Abstract

The magnetic properties of the two isostructural molecule-based magnets—Ni(NCS)2(thiourea)2, S = 1 [thiourea = SC(NH2 )2] and Co(NCS)2 (thiourea)2, S = 3/2—are characterized using several techniques in order to rationalize their relationship with structural parameters and to ascertain magnetic changes caused by substitution of the spin. Zero-field heat capacity and muon-spin relaxation measurements reveal low-temperature long-range ordering in both compounds, in addition to Ising-like (D < 0) single-ion anisotropy (DCo ∼ −100 K, DNi ∼ −10 K). Crystal and electronic structure, combined with dc-field magnetometry, affirm highly quasi-onedimensional behavior, with ferromagnetic intrachain exchange interactions JCo ≈ +4 K and JNi ∼ +100 K and weak antiferromagnetic interchain exchange, on the order of J ∼ −0.1 K. Electron charge- and spin-density mapping reveals through-space exchange as a mechanism to explain the large discrepancy in J-values despite, from a structural perspective, the highly similar exchange pathways in both materials. Both species can be compared to the similar compounds MCl2(thiourea)4, M = Ni(II) (DTN) and Co(II) (DTC), where DTN is known to harbor two magnetic-field-induced quantum critical points. Direct comparison of DTN and DTC with the compounds studied here shows that substituting the halide Cl− ion for the NCS− ion results in a dramatic change in both the structural and magnetic properties.

Citation

Curley, S., Scatena, R., Williams, R., Goddard, P., Macchi, P., Hicken, T., …Manson, J. (2021). Magnetic ground state of the one-dimensional ferromagnetic chain compounds M(NCS)2(thiourea)2 (M=Ni,Co). Physical Review Materials, 5(3), Article 034401. https://doi.org/10.1103/physrevmaterials.5.034401

Journal Article Type Article
Acceptance Date Feb 3, 2021
Online Publication Date Mar 3, 2021
Publication Date 2021
Deposit Date Mar 3, 2021
Publicly Available Date Sep 30, 2021
Journal Physical Review Materials
Publisher American Physical Society
Peer Reviewed Peer Reviewed
Volume 5
Issue 3
Article Number 034401
DOI https://doi.org/10.1103/physrevmaterials.5.034401
Public URL https://durham-repository.worktribe.com/output/1251770

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Copyright Statement
Reprinted with permission from the American Physical Society: Curley, S. P. M., Scatena, R., Williams, R. C., Goddard, P. A., Macchi, P., Hicken, T. J., Lancaster, T., Xiao, F., Blundell, S. J., Zapf, V., Eckert, J. C., Krenkel, E. H., Villa, J. A., Rhodehouse, M. L. & Manson, J. L. (2021). Magnetic ground state of the one-dimensional ferromagnetic chain compounds M(NCS)2(thiourea)2 (M=Ni,Co). Physical Review Materials 5(3): 034401.
© 2021 by the American Physical Society. Readers may view, browse, and/or download material for temporary copying purposes only, provided these uses are for noncommercial personal purposes. Except as provided by law, this material may not be further reproduced, distributed, transmitted, modified, adapted, performed, displayed, published, or sold in whole or part, without prior written permission from the American Physical Society.






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