Lead-free and lead-based ABO(3) perovskite relaxors with mixed-valence A-site and B-site disorder: comparative neutron scattering structural study of (Na1/2Bi1/2) TiO3 and Pb(Mg1/3Nb2/3)O-3

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dc.contributorVirginia Techen
dc.contributor.authorGe, Wenweien
dc.contributor.authorDevreugd, Christopher P.en
dc.contributor.authorPhelan, Danielen
dc.contributor.authorZhang, Qinhuien
dc.contributor.authorAhart, Muhtaren
dc.contributor.authorLi, Jiefangen
dc.contributor.authorLuo, Haosuen
dc.contributor.authorBoatner, Lynn A.en
dc.contributor.authorViehland, Dwight D.en
dc.contributor.authorGehring, Peter M.en
dc.contributor.departmentMaterials Science and Engineering (MSE)en
dc.date.accessed2014-04-23en
dc.date.accessioned2014-05-07T15:37:00Zen
dc.date.available2014-05-07T15:37:00Zen
dc.date.issued2013-11-01en
dc.description.abstractWe report the results of neutron elastic-scattering measurements made between -250 degrees C and 620 degrees C on the lead-free relaxor (Na1/2Bi1/2)TiO3 (NBT). Strong, anisotropic, elastic diffuse scattering intensity decorates the (100), (110), (111), (200), (210), and (220) Bragg peaks at room temperature. The wave-vector dependence of this diffuse scattering is compared to that in the lead-based relaxor Pb(Mg1/3Nb2/3)O-3 (PMN) to determine if any features might be common to relaxors. Prominent ridges in the elastic diffuse scattering intensity contours that extend along < 110 > are seen that exhibit the same zone dependence as those observed in PMN and other lead-based relaxors. These ridges disappear gradually on heating above the cubic-to-tetragonal phase transition temperature T-CT = 523 degrees C, which is also near the temperature at which the dielectric permittivity begins to deviate from Curie-Weiss behavior. We thus identify the < 110 >-oriented ridges as a relaxor-specific property. The diffuse scattering contours also display narrower ridges oriented along < 100 > that are consistent with the x-ray results of Kreisel et al. [Phys. Rev. B 68, 014113 (2003)]; these vanish near 320 degrees C, indicating that they have a different physical origin. The < 100 >-oriented ridges are not observed in PMN. We observe no equivalent relaxor-specific elastic diffuse scattering from the homovalent relaxor analogues K0.95Li0.05TiO3 (A-site disordered) and KTa0.95Nb0.05O3 (B-site disordered). This suggests that the < 110 >-oriented diffuse scattering ridges are correlated with the presence of strong random electric fields and invites a reassessment of what defines the relaxor phase. We find that doping NBT with 5.6% BaTiO3, a composition close to the morphotropic phase boundary with enhanced piezoelectric properties, increases the room-temperature correlation length along [1 (1) over bar0] from 40 to 60 angstrom while doubling the associated integrated diffuse scattering. Similar behavior was reported by Matsuura et al. [Phys. Rev. B 74, 144107 (2006)] for morphotropic compositions of PMN doped with PbTiO3. Finally, we comment on the recent observation of monoclinicity in NBT at room temperature by placing a strict bound on the strength of the (1/2 1/2 1/2) superlattice reflection associated with the Cc space group based on the atomic coordinates published in the x-ray study by Aksel et al. [Appl. Phys. Lett. 98, 152901 (2011)] for NBT. We show that a skin effect, analogous to that reported in the relaxors PZN-xPT and PMN-xPT, can reconcile our neutron single-crystal data with the x-ray powder data of Aksel et al. [Appl. Phys. Lett. 98, 152901 (2011)]. Our finding of a skin effect in a lead-free, A-site disordered, heterovalent relaxor supports the idea that it arises in the presence of strong random electric fields.en
dc.description.sponsorshipUS Department of Energy DE-FG02-07ER46480en
dc.description.sponsorshipUS Office of Naval Research N00014-13-1-0049en
dc.description.sponsorshipNatural Science Foundation of China 51332009en
dc.description.sponsorshipShanghai Rising-Star Program 11QA1407500en
dc.description.sponsorshipU.S. Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Divisionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationGe, W. W.; Devreugd, C. P.; Phelan, D.; Zhang, Q. H.; Ahart, M.; Li, J. F.; Luo, H. S.; Boatner, L. A.; Viehland, D.; Gehring, P. M., "Lead-free and lead-based ABO(3) perovskite relaxors with mixed-valence A-site and B-site disorder: comparative neutron scattering structural study of (Na1/2Bi1/2) TiO3 and Pb(Mg1/3Nb2/3)O-3," Phys. Rev. B 88, 174115 DOI: http://dx.doi.org/10.1103/PhysRevB.88.174115en
dc.identifier.doihttps://doi.org/10.1103/PhysRevB.88.174115en
dc.identifier.issn1098-0121en
dc.identifier.urihttp://hdl.handle.net/10919/47859en
dc.identifier.urlhttp://journals.aps.org/prb/abstract/10.1103/PhysRevB.88.174115en
dc.language.isoen_USen
dc.publisherAmerican Physical Societyen
dc.rightsIn Copyrighten
dc.rights.urihttp://rightsstatements.org/vocab/InC/1.0/en
dc.subjectSingle-crystalen
dc.subjectDiffuse-scatteringen
dc.subjectPhase transitionsen
dc.subjectAverageen
dc.subjectStructureen
dc.subjectBismuth-titanateen
dc.subjectFerroelectricsen
dc.subjectBehavioren
dc.subjectTemperatureen
dc.subjectAnomaliesen
dc.subjectPhysicsen
dc.subjectCondensed matteren
dc.titleLead-free and lead-based ABO(3) perovskite relaxors with mixed-valence A-site and B-site disorder: comparative neutron scattering structural study of (Na1/2Bi1/2) TiO3 and Pb(Mg1/3Nb2/3)O-3en
dc.title.serialPhysical Review Ben
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten

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