Dimensionality reduction induced synergetic optimization of the thermoelectric properties in Bi2Si2X6 (X=Se, Te) monolayers

Different from three-dimensional bulk compounds, two-dimensional monolayer compounds exhibit much better thermoelectric performance on account of the quantum confinement and interface effect. Here, we present a systematic study on the electronic and thermal transport properties of bulk and monolayer Bi2Si2X6 (X = Se, Te) through theoretical calculations using density functional theory based on first-principles and Boltzmann transport theory. Monolayer Bi2Si2X6 are chemically, mechanically and thermodynamically stable semiconductors with suitable band gaps, and they have lower lattice thermal conductivity (κL) in the a/b direction than their bulk counterparts. The calculated κL of monolayer Bi2Si2Se6 (Bi2Si2Te6) is as low as 0.72 (0.95) W m-1 K-1 at 700 K. Moreover, monolayer Bi2Si2X6 exhibit a higher Seebeck coefficient compared with bulk Bi2Si2X6 owing to the sharper peaks in the electronic density of states (DOS). This results in a significant increase in power factor by dimensionality reduction. Combined with the synergetically suppressed thermal conductivity, the maximum ZT values for monolayer Bi2Si2Se6 and Bi2Si2Te6 are significantly enhanced up to 5.03 and 2.87 with p-type doping at 700 K, which are more than 2 times that of the corresponding bulk compounds. These results demonstrate the superb thermoelectric performance of monolayer Bi2Si2X6 for promising thermoelectric conversion applications.