We have synthesized n- and p-type clathrates Ba8−d Au x Si46−x−y with various Au contents (4.6 < x < 6.0) by arc-melting, annealing at 1173 K, and spark plasma sintering at 1073 K. The Au compositions found by wavelength-dispersive x-ray spectrometry for the synthesized samples were slightly lower than the nominal compositions. Ba7.8Au4.6Si41.4 and Ba7.7Au4.9Si41.1 samples showed n- and p-type conduction, respectively. According to the electron count (Ba2+)8Au(3−)5.33Si40.67, the clathrate composition with x = 5.33 is expected to be an intrinsic semiconductor. Our experimental results show that increase of the Au composition causes a transition from n-type to p-type conduction between x = 4.6 and 4.9. We have also calculated the band structures of the Ba8Au x Si46−x clathrate including a vacancy by ab initio calculation based on density functional theory with structure optimization. It was found that the vacancy behaves like an electron acceptor and the numbers of vacancies at 24k sites for the synthesized Ba8Au x Si46−x−y clathrates can be estimated as ∼0.4 in a unit cell.
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Munetoh, S., Saisho, M., Oka, T. et al. Reinvestigation of Thermoelectric Properties of n- and p-Type Ba8−d Au x Si46−x−y Clathrate. Journal of Elec Materi 43, 2430–2434 (2014). https://doi.org/10.1007/s11664-014-3118-1
- Thermoelectric properties
- Ba-Au-Si clathrate
- spark plasma sintering
- ab initio calculation