Boosting Thermoelectric Performance in Epitaxial GeTe Film/Si by Domain Engineering and Point Defect Control

This study demonstrates a simultaneous realization of ultralow thermal conductivity and high thermoelectric power factor in epitaxial GeTe thin films/Si substrates by a combination of the interface introduction by domain engineering and the suppression of Ge vacancy generation by point defect control. We formed epitaxial Te-poor GeTe thin films having low-angle grain boundaries with a misorientation angle close to 0° or twin interfaces with a misorientation angle close to 180°. The control of interfaces and point defects gave rise to ultralow lattice thermal conductivity of ∼0.7 ± 0.2 W m^-1 K^-1. This value was the same in the order of magnitude as the theoretical minimum lattice thermal conductivity of ∼0.5 W m^-1 K^-1 calculated by the Cahill-Pohl model. At the same time, the GeTe thin films exhibited a high thermoelectric power factor because of the suppression of Ge vacancy generation and a small contribution of grain boundary carrier scattering. The outstanding combined technique of domain engineering and point defect control can be a great approach for developing high-performance thermoelectric films.