Enhanced Thermoelectric Transport and Stability in Atomic Layer Deposited-HfO₂/ZnO and TiO₂/ZnO-Sandwiched Multilayer Thin Films

Abstract

Herein, enhancements in thermoelectric (TE) performance, both the power factor (PF) and thermal stability, are exhibited by sandwiching HfO2 and TiO2 layers onto atomic layer deposited-ZnO thin films. High-temperature TE measurements from 300 to 450 K revealed an almost two-fold improvement in electrical conductivity for TiO2/ZnO (TZO) samples, primarily owing to an increase in carrier concentration by Ti doping. On the other hand, HfO2/ZnO (HZO) achieved the highest PF values owing to maintaining Seebeck coefficients comparable to pure ZnO. HZO also exhibited excellent stability after multiple thermal cycles, which has not been previously observed for pure or doped ZnO thin films. Such improvement in both TE properties and thermal stability of HZO can be attributed to a shift in crystalline orientation from the a axis to c axis, as well as the high bond dissociation energy of Hf–O, stabilizing the ZnO structure. These unique properties exhibited by HZO and TZO thin films synthesized by atomic layer deposition pave the way for next-generation transparent TE devices.