Improving near-room-temperature thermoelectrics in SnTe–MnTe alloys.

The rich capabilities for both electronic and phonon engineering in SnTe are highly desirable for achieving high thermoelectric performance. Alloying high-solubility MnTe (∼15%) leads to substitutional defects for reducing lattice thermal conductivity and band convergence for enhancing electronic performance, and thus, an improvement of thermoelectric performance of SnTe is realized. However, there is no evidence that the electronic and phonon transport properties are fully optimized in SnTe-15%MnTe thermoelectrics, especially for the near-room-temperature (< 573 K) thermoelectric performance, which still needs a sufficient promotion. Here, the substituted 2% Bi in SnTe-15%MnTe alloys dramatically increases the near-room-temperature zT and peak zT to ∼0.72 (at 550 K) and ∼1.3 (at 850 K), respectively. Combining the experimental evidence and the first-principles calculations, we demonstrate that the prominent enhancement of electronic performance arises from the Bi-doping-driven transport valence band alignment and the carrier concentration optimization. Furthermore, the Debye–Callaway model verifies that the reduction in lattice thermal conductivity is dominated by the Bi substitutional defects. The present findings reveal the importance of transport engineering in achieving high thermoelectric performance particularly near room temperature. [ABSTRACT FROM AUTHOR]