p-type to n-type conductivity transition in thermoelectric CoSbS

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Abstract

We demonstrate a p-type to n-type conductivity transition for thermoelectric CoSbS achieved by precisely controlling the sulfur vapor pressure during the sample synthesis. The p-n transition is experimentally confirmed by both the Seebeck coefficient and the Hall effect measurements. From the crystal structure refinements, the increase in the sulfur vapor pressure in the synthesis is weakly but steadily reflected in the occupancy factor of sulfur in the CoSbS lattice, while the p-n transition is seen as a peak in all the three lattice parameters, a, b, and c. Computationally, the situation could be simulated with first principle DFT calculations on compressed CoSbS. Without compression, DFT presents CoSbS as a p-type semiconductor with an indirect bandgap of 0.38 eV, while the pressure application results in an n-type semiconductor with decreased lattice parameters but the same indirect bandgap as in the uncompressed case. Experimentally, the thermal conductivity is strongly enhanced for sulfur-deficient samples, which could be due to larger phonon mean free paths. The sulfur loading significantly enhances the electrical conductivity while moderately decreasing the Seebeck coefficient such that the overall power factor is improved by a factor of 9 for the n-type sample and by a factor of 6 for the p-type sample, owing to the increased charge carrier density, although the performance is still relatively low. Thus, this study highlights CoSbS as a promising building block for thermoelectric devices based on its bipolar semiconductor nature with the possibility for both p-type and n-type doping with enhanced power factor.

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Kousar, H. S., Srivastava, D., Karttunen, A. J., Karppinen, M., & Tewari, G. C. (2022). p-type to n-type conductivity transition in thermoelectric CoSbS. APL Materials, 10(9). https://doi.org/10.1063/5.0107277

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