Estimation of Maximum <i>zT</i> in Cu<sub>3</sub>SbSe<sub>4</sub> for Different Starting Materials Content

Abstract

Cu<sub>3</sub>SbSe<sub>4</sub> is considered a promising thermoelectric material because of its large effective mass and low thermal conductivity, originating from its unique lattice structure. However, Cu<sub>3</sub>SbSe<sub>4</sub> has intrinsically low carrier concentration and relatively high electric resistance which limit performance. Recently, a <i>zT</i> improvement in Cu<sub>3</sub>SbSe<sub>4</sub> was reported where doping/precipitation is controlled by changing the content of the starting materials. However, the effect of these changes in starting content on electronic band structures has not been studied. Here, we investigate how the change in starting materials content (<i>x</i> varying from 6 to 20) affects band parameters like density-of-states effective mass (<i>m<sub>d</sub></i> *), non-degenerate mobility (<i>μ<sub>0</sub></i>), weighted mobility (<i>μ<sub>W</sub></i>), and B-factor using the Single Parabolic Band (SPB) model. For <i>x</i> greater than 8, precipitation of the secondary phase (CuSe) was observed, and the band parameters changed differently for <i>x</i> greater than 8. The <i>m<sub>d</sub></i> * increases up to <i>x</i> = 8 and then rapidly decreases for <i>x</i> > 8. For <i>μ<sub>0</sub></i>, an overall decrease is observed for increasing <i>x</i>, but the rate of decrease is suppressed for <i>x</i> > 8. The <i>μ<sub>W</sub></i> reaches the maximum at <i>x</i> = 8. As <i>x</i> increases, the experimental lattice thermal conductivity also increases, especially for <i>x</i> > 8. Therefore, the B-factor, which is directly related to the theoretical maximum zT, becomes maximum at = 8. Hence the SPB model predicts a maximum <i>zT</i> of 0.0484 for <i>x</i> = 8 at 300 K, which is 15.5% higher than the experimental <i>zT</i> of 0.0419, which can be achieved by tuning the Hall carrier concentration to 4.44 × 10<sup>19</sup> cm<sup>-3</sup>.