Atomistic study of an ideal metal/thermoelectric contact: the full-Heusler/half-Heusler interface

Half-Heusler alloys such as the (Zr,Hf)NiSn intermetallic compounds are important thermoelectric materials for converting waste heat into electricity. Reduced electrical resistivity at the hot interface between the half-Heusler material and a metal contact is critical for device performance, however this has yet to be achieved in practice. Recent experimental work suggests that a coherent interface between half-Heusler and full-Heusler compounds can form due to diffusion of transition metal atoms into the vacant sublattice of the half-Heusler lattice. We study theoretically the structural and electronic properties of such an interface using a first-principles based approach that combines {\it ab initio} calculations with macroscopic modeling. We find that the prototypical interface HfNi$_2$Sn/HfNiSn provides very low contact resistivity and almost ohmic behavior over a wide range of temperatures and doping levels. Given the potential of these interfaces to remain stable over a wide range of temperatures, our study suggests that full-Heuslers might provide nearly ideal electrical contacts to half-Heuslers that can be harnessed for efficient thermoelectric generator devices.