Understanding the lattice dynamics and low thermal conductivities of IV-VI, V 2 -VI 3 and V materials is critical to the development of better thermoelectric and phase-change materials. Here we provide a link between chemical bonding and low thermal conductivity. Our first-principles calculations reveal that long-ranged interaction along the /100S direction of the rocksalt structure exist in lead chalcogenides, SnTe, Bi 2 Te 3 , Bi and Sb due to the resonant bonding that is common to all of them. This long-ranged interaction in lead chalcogenides and SnTe cause optical phonon softening, strong anharmonic scattering and large phase space for three-phonon scattering processes, which explain why rocksalt IV-VI compounds have much lower thermal conductivities than zincblende III-V compounds. The new insights on the relationship between resonant bonding and low thermal conductivity will help in the development of better thermoelectric and phase change materials.

A high thermoelectric power factor not only enables a potentially high figure of merit ZT but also leads to a large output power density, and hence it is pivotal to find an effective route to improve the power factor.

No abstract

Achieving higher carrier mobility plays a pivotal role for obtaining potentially high thermoelectric performance. In principle, the carrier mobility is governed by the band structure as well as by the carrier scattering mechanism. Here, we demonstrate that by manipulating the carrier scattering mechanism in n-type MgSb-based materials, a substantial improvement in carrier mobility, and hence the power factor, can be achieved. In this work, Fe, Co, Hf, and Ta are doped on the Mg site of MgSbBiTe, where the ionized impurity scattering crosses over to mixed ionized impurity and acoustic phonon scattering. A significant improvement in Hall mobility from ∼16 to ∼81 cm⋅V⋅s is obtained, thus leading to a notably enhanced power factor of ∼13 μW⋅cm⋅K from ∼5 μW⋅cm⋅K A simultaneous reduction in thermal conductivity is also achieved. Collectively, a figure of merit () of ∼1.7 is obtained at 773 K in MgCoSbBiTe The concept of manipulating the carrier scattering mechanism to improve the mobility should also be applicable to other material systems.

Discovery of thermoelectric materials has long been realized by the Edisonian trial and error approach. However, recent progress in theoretical calculations, including the ability to predict structures of unknown phases along with their thermodynamic stability and functional properties, has enabled the so-called inverse design approach. Compared to the traditional materials discovery, the inverse design approach has the potential to substantially reduce the experimental efforts needed to identify promising compounds with target functionalities. By adopting this approach, here we have discovered several unreported half-Heusler compounds. Among them, the p-type TaFeSb-based half-Heusler demonstrates a record high ZT of ~1.52 at 973 K. Additionally, an ultrahigh average ZT of ~0.93 between 300 and 973 K is achieved. Such an extraordinary thermoelectric performance is further verified by the heat-to-electricity conversion efficiency measurement and a high efficiency of ~11.4% is obtained. Our work demonstrates that the TaFeSb-based half-Heuslers are highly promising for thermoelectric power generation.