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dc.contributor.authorKoskelo, EliseAnne C
dc.contributor.authorLiu, Cheng
dc.contributor.authorMukherjee, Paromita
dc.contributor.authorKelly, Nicola
dc.contributor.authorDutton, Sian
dc.date.accessioned2022-06-17T01:21:23Z
dc.date.available2022-06-17T01:21:23Z
dc.date.issued2022-04-12
dc.identifier.issn0897-4756
dc.identifier.other35572784
dc.identifier.otherPMC9098179
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/338187
dc.descriptionFunder: Winston Churchill Foundation of the United States
dc.descriptionFunder: University of Cambridge
dc.description.abstractFrustrated lanthanide oxides with dense magnetic lattices are of fundamental interest for their potential in cryogenic refrigeration due to a large ground state entropy and suppressed ordering temperatures but can often be limited by short-range correlations. Here, we present examples of frustrated fcc oxides, Ba2GdSbO6 and Sr2GdSbO6, and the new site-disordered analogue Ca2GdSbO6 ([CaGd] A [CaSb] B O6), in which the magnetocaloric effect is influenced by minimal superexchange (J 1 ∼ 10 mK). We report on the crystal structures using powder X-ray diffraction and the bulk magnetic properties through low-field susceptibility and isothermal magnetization measurements. The Gd compounds exhibit a magnetic entropy change of up to -15.8 J/K/molGd in a field of 7 T at 2 K, a 20% excess compared to the value of -13.0 J/K/molGd for a standard in magnetic refrigeration, Gd3Ga5O12. Heat capacity measurements indicate a lack of magnetic ordering down to 0.4 K for Ba2GdSbO6 and Sr2GdSbO6, suggesting cooling down through the liquid 4-He regime. A mean-field model is used to elucidate the role of primarily free-spin behavior in the magnetocaloric performance of these compounds in comparison to other top-performing Gd-based oxides. The chemical flexibility of the double perovskites raises the possibility of further enhancement of the magnetocaloric effect in the Gd3+ fcc lattices.
dc.description.sponsorshipWinton Programme for the Physics of Sustainability Churchill Scholarship from the Winston Churchill Foundation of the United States Diamond Light Source
dc.languageeng
dc.publisherAmerican Chemical Society (ACS)
dc.rightsAttribution 4.0 International
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/
dc.sourceessn: 1520-5002
dc.sourcenlmid: 9884133
dc.titleFree-Spin Dominated Magnetocaloric Effect in Dense Gd3+ Double Perovskites.
dc.typeArticle
dc.date.updated2022-06-17T01:21:23Z
prism.endingPage3450
prism.issueIdentifier7
prism.publicationNameChem Mater
prism.startingPage3440
prism.volume34
dc.identifier.doi10.17863/CAM.85598
dcterms.dateAccepted2022-03-15
rioxxterms.versionofrecord10.1021/acs.chemmater.2c00261
rioxxterms.versionVoR
rioxxterms.licenseref.urihttps://creativecommons.org/licenses/by/4.0/
dc.contributor.orcidKoskelo, EliseAnne C [0000-0002-0440-565X]
dc.contributor.orcidLiu, Cheng [0000-0002-3509-951X]
dc.contributor.orcidMukherjee, Paromita [0000-0001-5121-6280]
dc.contributor.orcidKelly, Nicola [0000-0003-2861-1623]
dc.contributor.orcidDutton, Sian [0000-0003-0984-5504]
dc.identifier.eissn1520-5002
pubs.funder-project-idEPSRC (EP/T028580/1)
pubs.funder-project-idEPSRC (2124516)
cam.issuedOnline2022-03-29


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Attribution 4.0 International
Except where otherwise noted, this item's licence is described as Attribution 4.0 International