High-resolution x-ray diffraction (XRD), Raman spectroscopy and total scattering XRD coupled to atomic pair distribution function (PDF) analysis studies of the atomic-scale structure of archetypal BaZrxTi1-xO3 (x = 0.10, 0.20, 0.40) ceramics are presented over a wide temperature range (100-450 K). For x = 0.1 and 0.2 the results reveal, well above the Curie temperature, the presence of Ti-rich polar clusters which are precursors of a long-range ferroelectric order observed below TC. Polar nanoregions (PNRs) and relaxor behaviour are observed over the whole temperature range for x = 0.4. Irrespective of ceramic composition, the polar clusters are due to locally correlated off-centre displacement of Zr/Ti cations compatible with local rhombohedral symmetry. Formation of Zr-rich clusters is indicated by Raman spectroscopy for all compositions. Considering the isovalent substitution of Ti with Zr in BaZrxTi1-xO3, the mechanism of formation and growth of the PNRs is not due to charge ordering and random fields, but rather to a reduction of the local strain promoted by the large difference in ion size between Zr4+ and Ti4+. As a result, non-polar or weakly polar Zr-rich clusters and polar Ti-rich clusters are randomly distributed in a paraelectric lattice and the long-range ferroelectric order is disrupted with increasing Zr concentration.
Average and local atomic-scale structure in BaZrxTi1-xO3 (x = 0. 10, 0.20, 0.40) ceramics by high-energy x-ray diffraction and Raman spectroscopy / V. Buscaglia, S. Tripathi, V. Petkov, M. Dapiaggi, M. Deluca, A. Gajović, Y. Ren. - In: JOURNAL OF PHYSICS. CONDENSED MATTER. - ISSN 0953-8984. - 26:6(2014 Jan 17).
|Titolo:||Average and local atomic-scale structure in BaZrxTi1-xO3 (x = 0. 10, 0.20, 0.40) ceramics by high-energy x-ray diffraction and Raman spectroscopy|
|Parole Chiave:||BaTiO3; highenergy; Raman spectroscopy; relaxors|
|Settore Scientifico Disciplinare:||Settore GEO/06 - Mineralogia|
|Data di pubblicazione:||17-gen-2014|
|Digital Object Identifier (DOI):||http://dx.doi.org/10.1088/0953-8984/26/6/065901|
|Appare nelle tipologie:||01 - Articolo su periodico|