Achieving Ultralow Lattice Thermal Conductivity and High Thermoelectric Performance in GeTe Alloys via Introducing Cu2Te Nanocrystals and Resonant Level Doping

The binary compound of GeTe emerging as a potential medium-temperature thermoelectric material has drawn a great deal of attention. Here, we achieve ultralow lattice thermal conductivity and high thermoelectric performance in In and a heavy content of Cu codoped GeTe thermoelectrics. In dopants improve the density of state near the surface of Femi of GeTe by introducing resonant levels, producing a sharp increase of the Seebeck coefficient. In and Cu codoping not only optimizes carrier concentration but also substantially increases carrier mobility to a high value of 87 cm(2) V-1 s(-1 )due to the diminution of Ge vacancies. The enhanced Seebeck coefficient coupled with dramatically enhanced carrier mobility results in significant enhancement of PF in Ge1.04-x-yInxCuyTe series. Moreover, we introduce Cu2Te nanocrystals' secondary phase into GeTe by alloying a heavy content of Cu. Cu2Te nanocrystals and a high density of dislocations cause strong phonon scattering, significantly diminishing lattice thermal conductivity. The lattice thermal conductivity reduced as low as 0.31 W m(-1) K-1 at 823 K, which is not only lower than the amorphous limit of GeTe but also competitive with those of thermoelectric materials with strong lattice anharmonicity or complex crystal structures. Consequently, a high ZT of 2.0 was achieved for Ge0.9In0.015Cu0.125Te by decoupling electron and phonon transport of GeTe. This work highlights the importance of phonon engineering in advancing high-performance GeTe thermoelectrics.

Automated summary

The codoping of In and Cu in GeTe results in ultralow lattice thermal conductivity and high thermoelectric performance due to the increased Seebeck coefficient and carrier mobility. The introduction of Cu2Te nanocrystals and a high density of dislocations lead to strong phonon scattering, significantly reducing lattice thermal conductivity. This phonon engineering approach results in a ZT of 2.0 for Ge0.9In0.015Cu0.125Te by decoupling electron and phonon transport in GeTe.