Experimental verification of band convergence in Sr and Na codoped PbTe

Abstract

Scanning tunneling microscopy and transport measurements have been performed to investigate the electronic structure and its temperature dependence in heavily Sr and Na codoped PbTe, which is recognized as one of the most promising thermoelectric materials. Our main findings are as follows: (i) Below T=4.5 K, all carriers are distributed in the first valence band at the L point (L band), which forms tube-shaped Fermi surfaces with concave curvature. With Sr and Na doping, the dispersion of the L band changes, and the band gap increases from 200 meV to 300 meV. (ii) At T=4.5 K, the Fermi energy is located ~100 meV below the edge of the L band for the Sr/Na codoped PbTe. The second valence band at the Sigma point (Sigma band) is lower than the L band by 150 meV, which is significantly smaller than that of pristine PbTe (200 meV). The decrease in the band offset, leading to band convergence, provides a desirable condition for thermoelectric materials.(iii) With increasing temperature, the carrier distribution to the Sigma band starts at T=100 K and we estimate that about 50 percent of the total carriers are redistributed in the Sigma band at T=300 K.Our work demonstrates that scanning tunneling microscopy and angular dependent magnetoresistance measurements are particularly powerful tools to determine the electronic structure and carrier distribution. We believe that they will provide a bird's eye view of the doping strategy towards realizing high-efficiency thermoelectric materials.