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article
Role of phonon scattering by elastic strain field in thermoelectric Sr1−xYxTiO3−δ
Abstract
Perovskite-type SrTiO3-δ ceramics are multifunctional materials with significant potential as n-type thermoelectric (TE) materials. The electronic and thermal transport properties of spark plasma sintered polycrystalline Sr1-xYxTiO3-δ (x=0.05, 0.075, 0.1) ceramics are systematically investigated from (15-800) K. The Sr0.9Y0.1TiO3-δ simultaneously exhibits a large Seebeck coefficient, α>-80μV/K and moderately high electrical resistivity, ρ∼0.8mΩ-cm at a carrier concentration of ∼1021cm-3 at 300K resulting in a high TE power factor defined herein as (α2σT)∼0.84W/m-K at 760K. Despite the similar atomic masses of Sr (87.6g/mol) and Y (88.9g/mol), the lattice thermal conductivity (κL) of Sr1-xY xTiO3-δ is significantly reduced with increased Y-doping, owing to the smaller ionic radii of Y3+ (∼1.23Å, coordination number 12) compared to Sr2+ (∼1.44Å, coordination number 12) ions. In order to understand the thermal conductivity reduction mechanism, the κL in the Sr1-xY xTiO3-δ series are phenomenologically modeled with a modified Callaway's equation from 30-600K. Phonon scattering by elastic strain field due to ionic radii mismatch is found to be the prominent scattering mechanism in reducing κL of these materials. In addition, the effect of Y-doping on the elastic moduli of Sr1-xY xTiO3-δ (x=0, 0.1) is investigated using resonant ultrasound spectroscopy, which exhibits an anomaly in x=0.1 in the temperature range 300-600K. As a result, the phonon mean free path is found to be further reduced in the Sr0.9Y0.1TiO3-δ compared to that of SrTiO3-δ, resulting in a considerably low thermal conductivity κ∼2.7W/m-K at 760K. Finally, we report a thermoelectric figure of merit (ZT)∼0.3 at 760K in the Sr0.9Y 0.1TiO3-δ, the highest ZT value reported in the Y-doped SrTiO3 ceramics thus far. © 2014 AIP Publishing LLC.