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Origin of Relaxor Behavior in Barium-Titanate-Based Lead-Free Perovskites

Journal Article (2021)
Author(s)

Vignaswaran Veerapandiyan (Materials Center Leoben GmbH)

Maxim N. Popov (Materials Center Leoben GmbH)

Florian Mayer (Materials Center Leoben GmbH)

Jürgen Spitaler (Materials Center Leoben GmbH)

Sarunas Svirskas (Vilnius University)

Vidmantas Kalendra (Vilnius University)

Jonas Lins (Technische Universität Darmstadt)

Giovanna Canu (Institute of Condensed Matter Chemistry and Technologies for Energy National Research Council of Italy)

P. Braga Groszewicz (Technische Universität Darmstadt, TU Delft - Applied Sciences)

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Research Group
RST/Storage of Electrochemical Energy
DOI related publication
https://doi.org/10.1002/aelm.202100812 Final published version
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Publication Year
2021
Language
English
Research Group
RST/Storage of Electrochemical Energy
Issue number
2
Volume number
8
Downloads counter
369
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Abstract

It is well known that disordered relaxor ferroelectrics exhibit local polar correlations. The origin of localized fields that disrupt long-range polar order for different substitution types, however, is unclear. Currently, it is known that substituents of the same valence as Ti4+ at the B-site of barium titanate lattice produce random disruption of Ti-O-Ti chains that induces relaxor behavior. On the other hand, investigating lattice disruption and relaxor behavior resulting from substituents of different valence at the B-site is more complex due to the simultaneous occurrence of charge imbalances and displacements of the substituent cation. The existence of an effective charge mediated mechanism for relaxor behavior appearing at low (<10%) substituent contents in heterovalent modified barium titanate ceramics is presented in this work. These results will add credits to the current understanding of relaxor behavior in chemically modified ferroelectric materials and also acknowledge the critical role of defects (such as cation vacancies) in lattice disruption, paving the way for chemistry-based materials design in the field of dielectric and energy storage applications.