Thermal stability and thermoelectric properties of p-type Ba_8Ga_(16)Ge_(30) clathrates

Abstract

The thermal stability of p-type Ba_8Ga_(16)Ge_(30) clathrates grown from gallium flux has been tested by heat treatment in low pressure Ar atmosphere at 400, 600, and 800 °C. Significant gallium loss was observed for all samples during heat treatment. The treatment at 400 °C does not significantly change the sample properties, and the samples remain p-type and comparable to the untreated, as-prepared, sample. At 600 °C the sample switches from extrinsic p-type to extrinsic n-type, presumably due to significant loss of Ga, and shows a high thermopower but a reduced electrical conductivity compared to as-made n-type samples. Surprisingly, after a thermal treatment at 800 °C, the crystal structure seemingly loses less Ga, only reducing the hole concentration to near intrinsic levels and thus has a negative impact on ZT. Regardless of the heat treatment temperature of the p-type samples the thermal conductivity remained exceptionally low, for some samples 0.9 W/m K. Heat treatment can thus greatly affect the thermoelectric properties of p-type Ba_8Ga_(16)Ge_(30), but the crystal structure remains intact.

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