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Reconciling Local Structure Disorder and the Relaxor State in (Bi1/2Na1/2)TiO3-BaTiO3

Groszewicz, Pedro B. ; Gröting, Melanie ; Breitzke, Hergen ; Jo, Wook ; Albe, Karsten ; Buntkowsky, Gerd ; Rödel, Jürgen (2023)
Reconciling Local Structure Disorder and the Relaxor State in (Bi1/2Na1/2)TiO3-BaTiO3.
In: Scientific Reports, 2016, 6 (1)
doi: 10.26083/tuprints-00018896
Article, Secondary publication, Publisher's Version

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Item Type: Article
Type of entry: Secondary publication
Title: Reconciling Local Structure Disorder and the Relaxor State in (Bi1/2Na1/2)TiO3-BaTiO3
Language: English
Date: 11 July 2023
Place of Publication: Darmstadt
Year of primary publication: 2016
Publisher: Springer Nature
Journal or Publication Title: Scientific Reports
Volume of the journal: 6
Issue Number: 1
Collation: 11 Seiten
DOI: 10.26083/tuprints-00018896
Corresponding Links:
Origin: Secondary publication service
Abstract:

Lead-based relaxor ferroelectrics are key functional materials indispensable for the production of multilayer ceramic capacitors and piezoelectric transducers. Currently there are strong efforts to develop novel environmentally benign lead-free relaxor materials. The structural origins of the relaxor state and the role of composition modifications in these lead-free materials are still not well understood. In the present contribution, the solid-solution (100-x)(Bi1/2Na1/2)TiO3-xBaTiO3 (BNT-xBT), a prototypic lead-free relaxor is studied by the combination of solid-state nuclear magnetic resonance (NMR) spectroscopy, dielectric measurements and ab-initio density functional theory (DFT). For the first time it is shown that the peculiar composition dependence of the EFG distribution width (ΔQISwidth) correlates strongly to the dispersion in dielectric permittivity, a fingerprint of the relaxor state. Significant disorder is found in the local structure of BNT-xBT, as indicated by the analysis of the electric field gradient (EFG) in 23Na 3QMAS NMR spectra. Aided by DFT calculations, this disorder is attributed to a continuous unimodal distribution of octahedral tilting. These results contrast strongly to the previously proposed coexistence of two octahedral tilt systems in BNT-xBT. Based on these results, we propose that considerable octahedral tilt disorder may be a general feature of these oxides and essential for their relaxor properties.

Identification Number: 31739
Status: Publisher's Version
URN: urn:nbn:de:tuda-tuprints-188967
Classification DDC: 500 Science and mathematics > 530 Physics
500 Science and mathematics > 540 Chemistry
Divisions: 11 Department of Materials and Earth Sciences > Material Science > Nonmetallic-Inorganic Materials
07 Department of Chemistry > Eduard Zintl-Institut > Physical Chemistry
DFG-Collaborative Research Centres (incl. Transregio) > Collaborative Research Centres > CRC 595: Electrical fatigue > B - Characterisation > Subproject B9: Characterization of Structure-Property-Relationships of electrical Functional Materials with Solid State-NMR
Date Deposited: 11 Jul 2023 11:37
Last Modified: 27 Sep 2023 10:24
URI: https://tuprints.ulb.tu-darmstadt.de/id/eprint/18896
PPN: 510717675
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