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Universal A-Cation Splitting in LiNbO-Type Structure Driven by Intrapositional Multivalent Coupling. | LitMetric

AI Article Synopsis

  • Understanding electric dipole switching in multiferroic materials, particularly in LiNbO-type polar magnets, requires examining atomic-scale structural changes, which remains poorly defined in high-pressure synthesized samples.
  • The discovery of Zn-ion splitting in the ZnFeNbO compound, validated through various diffraction techniques, highlights the presence of a paraelectric-like phase within its lattice and prompts a reevaluation of A-site atomic splitting in other similar compounds.
  • The study concludes that A-site splitting is common in LiNbO-type structures with mixed B-site or anionic configurations, with the extent of displacement being influenced by magnetic interactions and bonding dynamics between cations.

Article Abstract

Understanding the electric dipole switching in multiferroic materials requires deep insight of the atomic-scale local structure evolution to reveal the ferroelectric mechanism, which remains unclear and lacks a solid experimental indicator in high-pressure prepared LiNbO-type polar magnets. Here, we report the discovery of Zn-ion splitting in LiNbO-type ZnFeNbO established by multiple diffraction techniques. The coexistence of a high-temperature paraelectric-like phase in the polar ZnFeNbO lattice motivated us to revisit other high-pressure prepared LiNbO-type ABB'O compounds. The A-site atomic splitting (∼1.0-1.2 Å between the split-atom pair) in B/B'-mixed ZnFeTaO and O/N-mixed ZnTaON is verified by both powder X-ray diffraction structural refinements and high angle annular dark field scanning transmission electron microscopy images, but is absent in single-B-site ZnSnO. Theoretical calculations are in good agreement with experimental results and suggest that this kind of A-site splitting also exists in the B-site mixed Mn-analogues, MnFeMO (M = Nb, Ta) and anion-mixed MnTaON, where the smaller A-site splitting (∼0.2 Å atomic displacement) is attributed to magnetic interactions and bonding between A and B cations. These findings reveal universal A-site splitting in LiNbO-type structures with mixed multivalent B/B', or anionic sites, and the splitting-atomic displacement can be strongly suppressed by magnetic interactions and/or hybridization of valence bands between d electrons of the A- and B-site cations.

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Source
http://dx.doi.org/10.1021/jacs.0c01814DOI Listing

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