First principles study of heavily doped full Heusler Fe2YZ for high thermoelectric power factor

Using a combination of first-principles calculations based on density functional theory and Boltzmann semi-classical transport theory, we investigate the properties of heavily $n$-type doped full Heusler Fe2YZ1-xAx compounds. Using a supercell approach and including explicitly the dopant impurities, we recover in some cases giant thermoelectric power factors as previously predicted under doping within the rigid band approximations [Phys. Rev. Lett. 114, 136601 (2015)]. In other cases, however, we highlight that the system evolves toward a ferromagnetic half-metallic ground state so that the power factor is strongly modified. We rationalize the appearance of this magnetic instability, showing that it consistent with the Stoner model. The uncovered properties of the heavily doped phases of the studied Fe2YZ1-xAx compounds appear promising for Seebeck and spin-Seebeck applications.