Enhancing Thermoelectric Performance of PbTe-Based Compounds by Substituting Elements: A First Principles Study

We investigate the influence of doping on the thermoelectric (TE) properties of PbTe-based compounds applying first principles calculations. Our approach combines a solution of the Boltzmann transport equation to obtain electronic properties with total energy calculations yielding lattice vibrational properties. We show that electrical conductivity increases from 2.71 × 10⁴ S m⁻¹ to 3 × 10⁵ S m⁻¹ at 700 K due to 6.3 at.% lanthanum doping, whereas the Seebeck coefficient decreases from 341.5 μV K⁻¹ to −52.9 μV K⁻¹, since La atoms act as electron donors. This trend is accompanied by monotonous reduction of thermal conductivity due to La doping at different levels, e.g., 6.3 at.% La doping significantly affects the elastic bulk properties, resulting in reduction of the average sound velocity from 1980 m s⁻¹ for the pure PbTe-lattice to 1347 m s⁻¹ for the La-doped PbTe lattice, thereby reducing lattice thermal conductivity by ca. 32% at 700 K. We compare the TE performance of different PbTe compounds doped with either La, Y, or Sc, indicating that La doping yields the highest power factor. We demonstrate how this method could be utilized for dopant selection oriented toward improving TE performance.