Theoretical investigations of electrical transport properties in CoSb3 skutterudites under hydrostatic loadings

CoSb-based skutterudites have been a benchmark mid-temperature thermoelectric material under intensive experimental and theoretical studies for decades.Doping and filling, to the first order, alter the crystal lattice constant of CoSb3 in the context of "chemical pressure." In this work, we employed ab initio density functional theory in conjunction with semiclassical Boltzmann transport theory to investigate the mechanical properties and especially how hydrostatic loadings, i.e., "physical pressure," impact the electronic band structure, Seebeck coefficient,and power factor of pristine CoSb. It is found that hydrostatic pressure enlarges the band gap, suppresses the density of states(DOS) near the valence band edge, and fosters the band convergence between the valley bands and the conduction band minimum(CBM). By contrast,hydrostatic tensile reduces the band gap, increases the DOS near the valence band edge, and diminishes the valley bands near the CBM. Therefore, applying hydrostatic pressure provides an alternative avenue for achieving band convergence to improve thermoelectric properties of N-type CoSb3, which is further supported by our carrier concentration studies. These results provide valuable insight into the further improvement of thermoelectric performance of CoSb3-based skutterudites via a synergy of physical and chemical pressures.