Trends in GeTe Thermoelectrics: From Fundamentals to Applications

Abstract Germanium telluride (GeTe) with ultrafast ferroelectric transition, Rashba‐like electronic transport, and anomalous phonon anharmonicity are historically studied for potential memorizing and thermoelectric applications. Due to recent breakthroughs in spintronics, valleytronics, orbitronics, pre‐eminent GeTe thermoelectrics have re‐attracted enormous interest from both academia and industries, with increasing reports of significant figure‐of‐merit over 2.7 and the maximum efficiency of up to 17.0%. Here, the emerging trends in advancing GeTe thermoelectrics, starting from fundamentals of phase transformation, crystal structure, bonding mechanisms, and transport characteristics, with a highlight on the roles of Ge_4s² lone pairs, are timely overviewed. Technical insights in synthesis, characterization, property measurement, and computation are then summarized. After that, several innovative strategies for increasing the figure‐of‐merit, including entropy engineering, nanostructuring, and hybridization, which will further benefit near‐room‐temperature and n‐type performance, are examined. Moreover, high‐density and high‐efficiency devices with broad working temperatures are discussed as a result of rational configurational and interfacial design. In the end, perspective remarks on the challenges and outlook envisaging for next‐generation GeTe thermoelectrics, which will play a prominent role in future energy and environmental landscapes, are provided.