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Covalency is Frustrating: La2Sn2O7 and the Nature of Bonding in Pyrochlores under High Pressure-Temperature Conditions.

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cam.issuedOnline2018-07-02
dc.contributor.authorChilds, Christian
dc.contributor.authorLawler, Keith V
dc.contributor.authorHector, Andrew L
dc.contributor.authorPetitgirard, Sylvain
dc.contributor.authorNoked, Ori
dc.contributor.authorSmith, Jesse S
dc.contributor.authorDaisenberger, Dominik
dc.contributor.authorBezacier, Lucile
dc.contributor.authorJura, Marek
dc.contributor.authorPickard, Chris J
dc.contributor.authorSalamat, Ashkan
dc.contributor.orcidLawler, Keith V [0000-0003-1087-5815]
dc.contributor.orcidHector, Andrew L [0000-0002-9964-2163]
dc.date.accessioned2018-10-10T05:19:10Z
dc.date.available2018-10-10T05:19:10Z
dc.date.issued2018-12-17
dc.description.abstractNatural specimens of the pyrochlore (A2B2O7) compounds have been found to retain foreign actinide impurities within their parent framework, undergoing metamictization to a fully amorphous state. The response to radionuclide decay identifies pyrochlore systems with having high radiation tolerance and tailored use in radioactive waste applications and radionuclide sequestration. High pressure is a powerful pathway to high density states and amorphization with parallels to radiation-induced processes. Here, La2Sn2O7 is evaluated under extreme conditions via the combination of laser heating in a diamond anvil cell with X-ray diffraction and Raman spectroscopy. The measurements are supported by ab initio random structure searching and molecular dynamics calculations. A new ground state at 70 GPa is revealed, and high temperature annealing is fundamental to access its crystalline ground state and fully determine the structure. This crystalline phase ( P21/ c) retains its structural integrity during decompression and is fully recoverable to ambient conditions. The final state of the system is shown to be highly pathway dependent due to the covalent nature of the Sn-O bonding. The Tc pyrochlore, La2Tc2O7, is analyzed for similarities in the bonding to determine the likelihood of an analogous pathway dependency to a final state.
dc.description.sponsorshipRoyal Society
dc.format.mediumPrint-Electronic
dc.identifier.doi10.17863/CAM.30805
dc.identifier.eissn1520-510X
dc.identifier.issn0020-1669
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/283438
dc.languageeng
dc.language.isoeng
dc.publisherAmerican Chemical Society (ACS)
dc.publisher.urlhttp://dx.doi.org/10.1021/acs.inorgchem.8b01419
dc.rightsAttribution 4.0 International
dc.rights.urihttps://creativecommons.org/licenses/by/4.0/
dc.subject34 Chemical Sciences
dc.subject3406 Physical Chemistry
dc.titleCovalency is Frustrating: La2Sn2O7 and the Nature of Bonding in Pyrochlores under High Pressure-Temperature Conditions.
dc.typeArticle
dcterms.dateAccepted2018-06-08
prism.endingPage15061
prism.issueIdentifier24
prism.publicationDate2018
prism.publicationNameInorg Chem
prism.startingPage15051
prism.volume57
pubs.funder-project-idRoyal Society (WM150023)
pubs.funder-project-idEngineering and Physical Sciences Research Council (EP/P022596/1)
rioxxterms.licenseref.startdate2018-12
rioxxterms.licenseref.urihttp://www.rioxx.net/licenses/all-rights-reserved
rioxxterms.typeJournal Article/Review
rioxxterms.versionVoR
rioxxterms.versionofrecord10.1021/acs.inorgchem.8b01419

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