Synergetic optimization of the electrical and thermal
transport
performance of GeTe has been achieved through Sb doping in this work,
resulting in a high thermoelectric figure of merit ZT of 2.2 at 723 K. Positron annihilation measurements provided clear
evidence that Sb doping in GeTe can effectively suppress the Ge vacancies,
and the decrease of vacancy concentration coincides well with the
change of hole carrier concentration after Sb doping. The decreased
scattering by hole carriers and vacancies causes notable increase
in carrier mobility. Despite this, the density of states effective
mass is not enhanced by Sb doping, a maximum power factor of 4562
μW m–1 K–2 at 723 K is obtained
for Ge0.94Sb0.06Te with an optimized carrier
concentration of ∼3.65 × 1020 cm–3. Meanwhile, the electronic thermal conductivity κe is reduced because of the decreased electrical conductivity σ
with the increase of the Sb doping amount. In addition, the lattice
thermal conductivity κL is also suppressed due to
multiple phonon scattering mechanism, such as the large mass and strain
fluctuations by the substitution of Sb for Ge atoms, and also the
unique microstructure including grain boundary, nano-pore, and dislocation
in the samples. In conclusion, a maximum ZT of 2.2
is gained at 723 K, which contributes to preferable TE property for
GeTe-based materials.