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


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.

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Publisher 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.
Date accepted:03 February 2021
Date deposited:30 September 2021
Date of first online publication:03 March 2021
Date first made open access:30 September 2021

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