Hole-doping effect on the thermoelectric properties and electronic structure of CoSi

We report the effect of Al substitution on the temperature-dependent electrical resistivity, Seebeck coefficient, as well as thermal conductivity in the binary compound cobalt monosilicide. It is found that the substitution of Al onto the Si sites causes a dramatic decrease in the electrical resistivity and lattice thermal conductivity. A theoretical analysis indicated that the reduction of lattice thermal conductivity arises mainly from point-defect scattering of the phonons. For $x>~0.05$ in the CoSi_1-xAlₓ system, the Seebeck coefficient changes sign from negative to positive, accompanied by the appearance of a broad maximum. These features are associated with the change in the electronic band structure, where the Fermi level shifts downwards from the center of the pseudogap due to hole-doping effect. While the thermoelectric performance improves with increasing Al substitution, the largest figure-of-merit ZT value among these alloys is still an order of magnitude lower than the conventional thermoelectric materials.