Dielectric Relaxation, Local Structure and Lattice Dynamics in Mn-Doped Potassium Tantalate Ceramics
authors Tkach, A; Almeida, A; Levin, I; Woicik, JC; Vilarinho, PM
nationality International
author keywords electroceramics; perovskites; polar dielectrics; X-ray absorption; Raman spectroscopy
abstract Alkaline niobate and tantalate perovskites have attracted attention as polar dielectrics for electronics and telecommunications. Here, we studied the polar behaviour, lattice dynamics, and local structure in conventionally processed K0.985Mn0.015TaO3 +/-delta ceramics using a combination of variable-temperature dielectric and Raman spectroscopies, and X-ray absorption fine structure (XAFS) measurements, respectively. Mn doping induces a low-frequency dielectric relaxation in KTaO3 (KT), which follows the Arrhenius law with an activation energy U approximate to 105 meV and the characteristic relaxation time tau(0) approximate to 4.6 x 10(-14) s. Our XAFS results support preferential Mn occupancy of the cuboctahedral sites as Mn2+, with these cations strongly off-centred in the oversized oxygen cages. Such disordered Mn displacements generate electric dipoles, which are proposed as the source of the observed dielectric relaxation. We show that in Mn-doped ceramics, the low-frequency polar TO1 mode softens on cooling and, at low temperatures, exhibits a higher frequency than in undoped KT. This mode displays no detectable splitting, which contrasts with Li-doped KT that also contains off-centred Li+ species on the cuboctahedral sites. Therefore, we conclude that the coupling between the Mn displacements and the lattice is weaker than in the Li case, and Mn-doped KT therefore exhibits a dielectric relaxation but no ferroelectric transition.
publisher MDPI
isbn 1996-1944
year published 2021
volume 14
issue 16
digital object identifier (doi) 10.3390/ma14164632
web of science category 11
subject category Chemistry, Physical; Materials Science, Multidisciplinary; Metallurgy & Metallurgical Engineering; Physics, Applied; Physics, Condensed Matter
unique article identifier WOS:000689568200001
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journal impact factor 3.057
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