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Near-ideal molecule-based Haldane spin chain
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(2020) Near-ideal molecule-based Haldane spin chain. Physical Review Research, 2 (1). 013082 . doi:10.1103/PhysRevResearch.2.013082 ISSN 2643-1564.
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Official URL: https://doi.org/10.1103/PhysRevResearch.2.013082
Abstract
The molecular coordination complex NiI2(3,5-lut)4 [where (3,5-lut) = (3,5-lutidine) = (C7H9N)] has been synthesized and characterized by several techniques including synchrotron X-ray diffraction, ESR, SQUID magnetometry, pulsed-field magnetization, inelastic neutron scattering and muon spin relaxation. Templated by the configuration of 3,5-lut ligands the molecules pack in-registry with the Ni–I· · · I–Ni chains aligned along the c–axis. This arrangement leads to through-space I· · · I magnetic coupling which is directly measured for the first time in this work. The net result is a near-ideal realization of the S = 1 Haldane chain with J = 17.5 K and energy gaps of ∆∥ = 5.3 K ∆⊥ = 7.7 K, split by the easy-axis single-ion anisotropy D = −1.2 K. The ratio D/J = −0.07 affords one of the most isotropic Haldane systems yet discovered, while the ratio ∆0/J = 0.40(1) (where ∆0 is the average gap size) is close to its ideal theoretical value, suggesting a very high degree of magnetic isolation of the spin chains in this material. The Haldane gap is closed by orientation-dependent critical fields μ0Hc∥ = 5.3 T and μ0Hc⊥ = 4.3 T, which are readily accessible experimentally and permit investigations across the entirety of the Haldane phase, with the fully polarized state occurring at μ0Hs∥ = 46.0 T and μ0Hs⊥ = 50.7 T. The results are explicable within the so-called fermion model, in contrast to other reported easy-axis Haldane systems. Zero-field magnetic order is absent down to 20 mK and emergent end-chain effects are observed in the gapped state, as evidenced by detailed low-temperature measurements.
| Item Type: | Journal Article | ||||||||||||||||||||||||||||||||||||||||||||||||
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| Subjects: | Q Science > QD Chemistry | ||||||||||||||||||||||||||||||||||||||||||||||||
| Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | ||||||||||||||||||||||||||||||||||||||||||||||||
| Library of Congress Subject Headings (LCSH): | Molecules -- Magnetic properties, Magnetochemistry, Condensed matter -- Magnetic properties | ||||||||||||||||||||||||||||||||||||||||||||||||
| Journal or Publication Title: | Physical Review Research | ||||||||||||||||||||||||||||||||||||||||||||||||
| Publisher: | American Physical Society | ||||||||||||||||||||||||||||||||||||||||||||||||
| ISSN: | 2643-1564 | ||||||||||||||||||||||||||||||||||||||||||||||||
| Official Date: | 27 January 2020 | ||||||||||||||||||||||||||||||||||||||||||||||||
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| Volume: | 2 | ||||||||||||||||||||||||||||||||||||||||||||||||
| Number: | 1 | ||||||||||||||||||||||||||||||||||||||||||||||||
| Article Number: | 013082 | ||||||||||||||||||||||||||||||||||||||||||||||||
| DOI: | 10.1103/PhysRevResearch.2.013082 | ||||||||||||||||||||||||||||||||||||||||||||||||
| Status: | Peer Reviewed | ||||||||||||||||||||||||||||||||||||||||||||||||
| Publication Status: | Published | ||||||||||||||||||||||||||||||||||||||||||||||||
| Access rights to Published version: | Open Access (Creative Commons) | ||||||||||||||||||||||||||||||||||||||||||||||||
| Date of first compliant deposit: | 21 November 2019 | ||||||||||||||||||||||||||||||||||||||||||||||||
| Date of first compliant Open Access: | 28 January 2020 | ||||||||||||||||||||||||||||||||||||||||||||||||
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