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

Curley, S. 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.

doi:10.1103/physrevmaterials.5.034401

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

Journal Article · Wed Mar 03 00:00:00 EST 2021 · Physical Review Materials

DOI:https://doi.org/10.1103/physrevmaterials.5.034401· OSTI ID:1783532

^[1];

^[2]; Williams, R. C. ^[1];

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^[3];

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^[4]; Xiao, F. ^[5];

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^[7]; Eckert, J. C. ^[8]; Krenkel, E. H. ^[8]; Villa, J. A. ^[9]; Rhodehouse, M. L. ^[9]; Manson, J. L. ^[9]

Univ. of Warwick, Coventry (United Kingdom)
Univ. of Oxford (United Kingdom). Clarendon Lab.; Univ. of Bern (Switzerland)
Polytechnic of Milan (Italy); Istituto Italiano di Tecnologia, Milan (Italy). Center for Nano Science and Technology (CNST); Univ. of Bern (Switzerland)
Durham Univ. (United Kingdom)
Paul Scherrer Inst., Villigen (Switzerland). Lab. for Neutron Scattering and Imaging
Univ. of Oxford (United Kingdom). Clarendon Lab.
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). National High Magnetic Field Lab. (MagLab)
Harvey Mudd College, Claremont, CA (United States)
Eastern Washington Univ., Cheney, WA (United States)

The magnetic properties of the two isostructural molecule-based magnets— $Ni {(NCS)}_{2} {(thiourea)}_{2}, S = 1 [thiourea = SC {({NH}_{2})}_{2}]$ 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 ( $D_{Co} ~ - 100$ K, $D_{Ni} ~ - 10$ K). Crystal and electronic structure, combined with dc-field magnetometry, affirm highly quasi-one-dimensional behavior, with ferromagnetic intrachain exchange interactions $J_{Co} \approx + 4$ K and $J_{Ni} ~ + 100$ K and weak antiferromagnetic interchain exchange, on the order of $J^{'} ~ - 0.1$ K. Furthermore, 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 $M {Cl}_{2} {(thiourea)}_{4}, M$ = 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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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE; National Science Foundation (NSF); Engineering and Physical Sciences Research Council (EPSRC)

Grant/Contract Number:: 89233218CNA000001; 681260; DMR-1703003; CHE-1834750; EP/N023803/1; EP/N024028/1; DMR-1157490

OSTI ID:: 1783532

Alternate ID(s):: OSTI ID: 1830587

Report Number(s):: LA-UR-20-29089; LA-UR-20-29511; TRN: US2210335

Journal Information:: Physical Review Materials, Vol. 5, Issue 3; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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