Groszewicz, Pedro B. ; Gröting, Melanie ; Breitzke, Hergen ; Jo, Wook ; Albe, Karsten ; Buntkowsky, Gerd ; Rödel, Jürgen (2016)
Reconciling Local Structure Disorder and the Relaxor State in (Bi1/2Na1/2)TiO3-BaTiO3.
In: Scientific Reports, 6
doi: 10.1038/srep31739
Artikel, Bibliographie
Kurzbeschreibung (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.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2016 |
| Autor(en): | Groszewicz, Pedro B. ; Gröting, Melanie ; Breitzke, Hergen ; Jo, Wook ; Albe, Karsten ; Buntkowsky, Gerd ; Rödel, Jürgen |
| Art des Eintrags: | Bibliographie |
| Titel: | Reconciling Local Structure Disorder and the Relaxor State in (Bi1/2Na1/2)TiO3-BaTiO3 |
| Sprache: | Englisch |
| Publikationsjahr: | 22 August 2016 |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Scientific Reports |
| Jahrgang/Volume einer Zeitschrift: | 6 |
| Kollation: | 11 Seiten |
| DOI: | 10.1038/srep31739 |
| Zugehörige Links: | |
| Kurzbeschreibung (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. |
| Zusätzliche Informationen: | SFB 595 Cooperation B9 ; Artikel-ID: 31739 |
| Fachbereich(e)/-gebiet(e): | 11 Fachbereich Material- und Geowissenschaften 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Materialmodellierung 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Nichtmetallisch-Anorganische Werkstoffe DFG-Sonderforschungsbereiche (inkl. Transregio) DFG-Sonderforschungsbereiche (inkl. Transregio) > Sonderforschungsbereiche 07 Fachbereich Chemie 07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Physikalische Chemie Zentrale Einrichtungen Zentrale Einrichtungen > Hochschulrechenzentrum (HRZ) Zentrale Einrichtungen > Hochschulrechenzentrum (HRZ) > Hochleistungsrechner DFG-Sonderforschungsbereiche (inkl. Transregio) > Sonderforschungsbereiche > SFB 595: Elektrische Ermüdung DFG-Sonderforschungsbereiche (inkl. Transregio) > Sonderforschungsbereiche > SFB 595: Elektrische Ermüdung > B - Charakterisierung DFG-Sonderforschungsbereiche (inkl. Transregio) > Sonderforschungsbereiche > SFB 595: Elektrische Ermüdung > B - Charakterisierung > Teilprojekt B9: Charakterisierung der Struktur-Eigenschaftsbeziehungen elektrischer Funktionsmaterialien mit Festkörper-NMR-Verfahren |
| Hinterlegungsdatum: | 20 Sep 2016 10:17 |
| Letzte Änderung: | 12 Jul 2023 05:58 |
| PPN: | 509440428 |
| Zugehörige Links: | |
| Sponsoren: | The authors would like to thank Prof. George Rossetti and Prof. Ian Reaney for very fruitful discussions. This work has been financially supported by the Collaborative Research Center SFB 595 “Electrical Fatigue in Functional Materials” of, the Deutsche Forschungsgemeinschaft (DFG). WJ wishes to acknowledge also the financial support by the Basic Science Research Program through the National Research Foundation of Korea (NRF), funded by the Ministry of Science, ICT and future Planning (No. 2014R1A2A1A11053597). We acknowledge grants for computing time on the “Lichtenberg” high-performance computer at TU Darmstadt. |
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