Dopant induced band convergence leading to high thermoelectric power factor in Mg2Sn

Abstract

Band convergence is a common technique for enhancing the power factor of thermoelectric (TE) materials. This is usually achieved by solid solution formation in compounds having specific electronic band features. In this work, we show that a similar band convergence effect can be achieved in Mg2Sn by doping with small amounts of Bi. To identify this effect and the possible reason behind it, a detailed investigation of the electronic band structure (EBS) has been carried out using a recently developed multi-band refinement technique (MBRT). Nominal compositions of Mg2.2Sn1-xBix (x = 0,0.005, 0.01, 0.0125, 0.015, 0.02) have been synthesized by induction melting followed by compaction using uniaxial hot-pressing. Measurement of Seebeck coefficient (S), electrical conductivity (σ) and Hall Coefficient (RH) have been performed between 300K–700K and the data used for multi-band refinement. Results indicate changes in the inter-band separation of conduction bands with doping content and temperature. Significantly lower inter-band separation compared to reported undoped data is found even for the lowest doped composition, resulting in both conduction bands contributing to the power factor (S2σ). Further, for the heavily doped compositions (x = 0.0125, 0.015, 0.02) band-flipping between the conduction bands has been observed. Thus, the light conduction band is found to constitute the conduction band edge in the heavily doped compositions. This is contrary to the reported EBS of undoped Mg2Sn in which the heavy conduction band has a lower energy. Also, increasing temperature results in band convergence in the heavily doped compositions. A plausible cause for the band-flipping behaviour is provided based on merging of the impurity band with the light conduction band in heavily doped Mg2Sn. The band-flipping and the subsequent band convergence results in an even higher S2σ in the heavily doped compositions. The work highlights the beneficial influence of Bi doping on the TE properties of Mg2Sn and opens the possibility of utilizing dopants for achieving band convergence in TE materials.