Reducing Lattice Thermal Conductivity of the Thermoelectric Compound AgSbTe2 (P4/mmm) by Lanthanum Substitution: Computational and Experimental Approaches

In this study we performed lattice dynamics first-principles calculations for the promising thermoelectric (TE) compound AgSbTe₂, and estimated the stability of its three polymorphs over a wide temperature range from 0 to 600 K. We calculated the vibrational density of states of the AgSbTe₂ (P4/mmm) phase. The results suggested that formation of substitutional defects at Ag-sublattice sites impedes lattice vibrations, thereby reducing lattice thermal conductivity. We focused on calculations based on the Debye approximation for the compound La_0.125Ag_0.875SbTe₂, and predicted reduction of the average sound velocity from 1684 to 1563 m s^?1 as a result of La doping. This is manifested as a ca. 14% reduction in thermal conductivity. To confirm the results from computation we produced two Ag–Sb–Te-based alloys, a ternary alloy without La addition and a quaternary alloy containing La. We measured the thermal conductivity of both alloys by use of the laser flash analysis method, and, as a result of La alloying, observed a reduction in thermal conductivity from 0.92 to 0.71 W m^?1 K^?1 at 573 K, as calculated from first principles.