Controlling the superconductivity of Nb2PdxS5 via reversible Li intercalation

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dc.contributor.authorElgaml, Men_AU
dc.contributor.authorDey, Sen_AU
dc.contributor.authorCen, Jen_AU
dc.contributor.authorAvdeev, Men_AU
dc.contributor.authorScanlon, DOen_AU
dc.contributor.authorGrey, CPen_AU
dc.contributor.authorClarke, SJen_AU
dc.date.accessioned2024-02-23T04:48:03Zen_AU
dc.date.available2024-02-23T04:48:03Zen_AU
dc.date.issued2024-01-04en_AU
dc.date.statistics2024-02-23en_AU
dc.description.abstractThe Nb2PdxS5 (x ≈ 0.74) superconductor with a Tc of 6.5 K is reduced by the intercalation of lithium in ammonia solution or electrochemically to produce an intercalated phase with expanded lattice parameters. The structure expands by 2% in volume and maintains the C2/m symmetry and rigidity due to the PdS4 units linking the layers. Experimental and computational analysis of the chemically synthesized bulk sample shows that Li occupies triangular prismatic sites between the layers with an occupancy of 0.33(4). This level of intercalation suppresses the superconductivity, with the injection of electrons into the metallic system observed to also reduce the Pauli paramagnetism by ∼40% as the bands are filled to a Fermi level with a lower density of states than in the host material. Deintercalation using iodine partially restores the superconductivity, albeit at a lower Tc of ∼5.5 K and with a smaller volume fraction than in fresh Nb2PdxS5. Electrochemical intercalation reproduces the chemical intercalation product at low Li content (<0.4) and also enables greater reduction, but at higher Li contents (≥0.4) accessed by this route, phase separation occurs with the indication that Li occupies another site. © 2024 The Authors. Published by American Chemical Society. This publication is licensed under CC-BY 4.0.en_AU
dc.description.sponsorshipWe thank the Leverhulme Trust (RPG-2018-377) and the UK Engineering and Physical Sciences Research Council (EPSRC) (EP/T027991/1 and EP/R042594/1) for funding. We thank the Diamond Light Source Ltd (EE18786, CY25166, and CY32893) and the Australian Nuclear Science and Technology Organisation (ANSTO) for the award of beam time. We thank Dr. A. Baker and Dr. C. Murray for support on I11 at Diamond. We are also grateful to the UK Materials and Molecular Modelling Hub (MMM Hub), which is partially funded by the EPSRC (EP/P020194/1, EP/T022213/1), for computational resources on the Thomas, Young supercomputers and to UCL for access to the Myriad (Myriad@UCL) and Kathleen (Kathleen@UCL) supercomputers. This work used the ARCHER2 UK National Supercomputing Services via our membership in the UK’s HEC Materials Chemistry Consortium, funded by EPSRC (EP/L000202, EP/R029431, and EP/T022213). We thank Bonan Zhu for useful discussions around calculating the Li site energies.en_AU
dc.format.mediumPrint-Electronicen_AU
dc.identifier.citationElgaml, M., Dey, S., Cen, J., Avdeev, M., Scanlon, D. O., Grey, C. P., & Clarke, S. J. (2024). Controlling the superconductivity of Nb2PdxS5 via reversible Li intercalation. Inorganic Chemistry, 63(2), 1151-1165. doi:10.1021/acs.inorgchem.3c03524en_AU
dc.identifier.issn0020-1669en_AU
dc.identifier.issn1520-510Xen_AU
dc.identifier.issue2en_AU
dc.identifier.journaltitleInorganic Chemistryen_AU
dc.identifier.pagination1151-1165en_AU
dc.identifier.urihttp://dx.doi.org/10.1021/acs.inorgchem.3c03524en_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/15429en_AU
dc.identifier.volume63en_AU
dc.languageEnglishen_AU
dc.language.isoenen_AU
dc.publisherAmerican Chemical Societyen_AU
dc.subjectSuperconductivityen_AU
dc.subjectLithiumen_AU
dc.subjectElectronsen_AU
dc.subjectFermi levelen_AU
dc.subjectSymmetryen_AU
dc.subjectPauli Principleen_AU
dc.titleControlling the superconductivity of Nb2PdxS5 via reversible Li intercalationen_AU
dc.typeJournal Articleen_AU
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