Modification of electronic structure and thermoelectric properties of hole-doped tungsten dichalcogenides

We present a study on the modification of the electronic structure and hole-doping effect for the layered dichalcogenide WSe_2 with a multi-valley band structure, where Ta is doped on the W site along with a partial substitution of Te for its lighter counterpart Se. By means of band-structure calculations and specific-heat measurements, the introduction of Te is theoretically and experimentally found to change the electronic states in WSe_2. While in WSe_2 the valence-band maximum is located at the Gamma point, the introduction of Te raises the bands at the K point with respect to the Gamma point. In addition, thermal-transport measurements reveal a smaller thermal conductivity at room temperature of W_1-xTa_xSe_1.6Te_0.4 than reported for W_1-xTa_xSe_2. However, when approaching 900 K, the thermal conductivities of both systems converge while the resistivity in W_1-xTa_xSe_1.6Te_0.4 is larger than in W_1-xTa_xSe_2, leading to comparable but slightly smaller values of the figure of merit in W_1-xTa_xSe_1.6Te_0.4.