Cu Interstitials Enable Carriers and Dislocations for Thermoelectric Enhancements in n-PbTe0.75Se0.25

Summary Aliovalent defects are extremely effective in manipulating charge transport and atomic vibrational properties for thermoelectric enhancements. Electronic performance of thermoelectrics is optimized at a reduced Fermi level of ∼0.3, which causes the optimal carrier concentration (nopt) to be strongly temperature dependent. This motivates a dynamic doping approach for electronic enhancements through an increase with temperature of solubility of aliovalent dopants. In addition, the defects could simultaneously act as scattering sources of phonons for reducing the lattice thermal conductivity. These effects are illustrated in this work by the temperature-dependent excess Cu solubility in n-PbTe0.75Se0.25 thermoelectrics, in which both carriers and dislocations are induced for regulating the electronic and phononic transport properties for a realization of an extraordinary thermoelectric figure of merit. The resultant defect structures and temperature gradient doping effects (for aliovalent solutes) could in principle open extra possibilities for optimizing charge and phonon transport properties in thermoelectrics.