One site, two cations, three environments: s2 and s0 electronic configurations generate Pb-free relaxor behaviour in a perovskite oxide

Autor: Marco Zanella, William J. Thomas, Jonathan Alaria, Luke M. Daniels, Jacinthe Gamon, Thomas A. Whittle, Philippa M. Shepley, Matthew J. Rosseinsky, Anton Goetzee-Barral, Quinn Gibson, T. Wesley Surta, Matthew A. Wright, Yang Li, John B. Claridge, Andrew J. Bell, Hongjun Niu
Přispěvatelé: Department of Chemistry University of Liverpool, University of Liverpool, School of Physics and Astronomy [Leeds], University of Leeds, School of Chemical and Process Engineering, Department of Physics - University of Liverpool, We thank the EPSRC (EP/R011753 and EP/R010293) for funding this research. J.G. and Q.D.G. acknowledge support through EP/N004884. We thank the STFC for access to Polaris (Xpress proposal 1890309) and Dr. Ron Smith for collecting the data and performing absorption corrections. We thank Argonne National Laboratory for access to the 11BM beamline (Rapid Access proposal 65125) and to Dr. Saul Lapidus and Dr. Lynn Ribaud for collecting the data
Jazyk: angličtina
Rok vydání: 2021
Předmět:
Zdroj: Journal of the American Chemical Society
Journal of the American Chemical Society, American Chemical Society, 2021, 143 (3), pp.1386-1398. ⟨10.1021/jacs.0c10572⟩
ISSN: 0002-7863
1520-5126
Popis: The piezoelectric devices widespread in society use noncentrosymmetric Pb-based oxides because of their outstanding functional properties. The highest figures of merit reported are for perovskites based on the parent Pb(Mg1/3Nb2/3)O3 (PMN), which is a relaxor: a centrosymmetric material with local symmetry breaking that enables functional properties, which resemble those of a noncentrosymmetric material. We present the Pb-free relaxor (K1/2Bi1/2)(Mg1/3Nb2/3)O3 (KBMN), where the thermal and (di)electric behavior emerges from the discrete structural roles of the s0 K+ and s2 Bi3+ cations occupying the same A site in the perovskite structure, as revealed by diffraction methods. This opens a distinctive route to Pb-free piezoelectrics based on relaxor parents, which we demonstrate in a solid solution of KBMN with the Pb-free ferroelectric (K1/2Bi1/2)TiO3, where the structure and function evolve together, revealing a morphotropic phase boundary, as seen in PMN-derived systems. The detailed multiple-length-scale understanding of the functional behavior of KBMN suggests that precise chemical manipulation of the more diverse local displacements in the Pb-free relaxor will enhance performance.
Databáze: OpenAIRE