Effects of (Al,Ge) Double Doping on the Thermoelectric Properties of Higher Manganese Silicides


X. Chen, Weathers, A., Salta, D., Zhang, L. B., Zhou, J. S., Goodenough, J. B., and Shi, L., “Effects of (Al,Ge) Double Doping on the Thermoelectric Properties of Higher Manganese Silicides,” Journal of Applied Physics, vol. 114, pp. 173705, 2013.


Experiments and analysis have been carried out to investigate the effects of Al and (Al,Ge) doping on the microstructure and thermoelectric properties of polycrystalline higher manganese silicide (HMS) samples, which were prepared by solid-state reaction, ball milling, and followed by spark plasma sintering. It has been found that Al doping effectively increases the hole concentration, which leads to an increase in the electrical conductivity and power factor. By introducing the second dopant Ge into Al-doped HMS, the electrical conductivity is increased, and the Seebeck coefficient is decreased as a result of further increased hole concentration. The peak power factor is found to occur at a hole concentration between 1.8 × 1021 and 2.2 × 1021 cm−3 measured at room temperature. The (Al,Ge)-doped HMS samples show lower power factors owing to their higher hole concentrations. The mobility of Mn(Al0.0035 Ge ySi0.9965-y)1.8 with y = 0.035 varies approximately as T−3/2 above 200 K, suggesting acoustic phonon scattering is the dominant scattering mechanism. The thermal conductivity of HMS does not change appreciably by Al or (Al,Ge) doping. The maximum ZT of (Al,Ge)-doped HMS is 0.57 at 823 K, which is similar to the highest value found in the Al-doped HMS samples. The ZT values were reduced in the Mn(Al0.0035 Ge ySi0.9965-y)1.8 samples with high Ge concentration of y = 0.025 and 0.035, because of reduced power factor. In addition, a two-band model was employed to show that the hole contribution to the thermal conductivity dominates the bipolar and electron contributions for all samples from 300 to 823 K and accounts for about 12% of the total thermal conductivity at about 800 K.