Looking for new semiconductors among the TMX intermetallic using high-throughput calculations
Résumé
Novel high-performance materials are needed for developing thermoelectric devices. One
way to answer this need is to screen a large number of compounds by first-principles
calculations and to synthesize the most promising compounds.
We focus our investigation on the ternary intermetallic compounds T-M-X, with T a transition
metal, a rare earth or an alkaline earth metal, M an element from the first line of the
transition metal and X, a metalloid. For each prototype, all the possible T-M-X combinations
are investigated by DFT calculations. Among all these candidates, those which are
predicted as thermodynamically unstable and metallic are dismissed. For the most
promising compounds, predicted as stable and semiconductor, complementary calculations
as the phonon band structure and additional BoltzTrap electronic transport calculations are
carried out to better assess their thermoelectric properties. After those theoretical steps,
experimental investigations are performed to confirm calculations.
The study of the equimolar TMX in four different prototypes lead to the investigation of 2280
possible configurations. Then our screening process allowed us to highlight more than 45
possible new semiconductors. Among these, new compositions such as HfCoP, SrCuSb or
TaFeSb were predicted to be stable and non-metallic. Complementary calculations allowed
to estimate their lattice thermal conductivity and Seebeck coefficient.
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