Strong anisotropy of Sc2X2Se2 (X = Cl, Br, I) monolayers contributes to high thermoelectric performance

As a novel type of anisotropic two-dimensional material, extensive attention has been paid to the thermoelectric (TE) properties of FeOCl-type monolayers, such as Al2X2Se2 (X = Cl, Br, I), Sc2I2S2, and Ir2Cl2O2. Recently, theoretical works based on first-principles calculations have been powerful driving forces in field of TE research. In this work, we perform an investigation into the TE properties of Sc2X2Se2 (X = Cl, Br, I) monolayers based on density functional theory (DFT). A study on the stability, including AIMD simulation and phonon calculation, shows the stable structure of Sc2Cl2Se2, Sc2Br2Se2, and Sc2I2Se2 monolayers. Additionally, the electronic and thermal transport properties of Sc2X2Se2 monolayers are anisotropic along the x and y directions. Moreover, the combination of excellent Seebeck coefficient and ultralow lattice thermal conductivity contributes to outstanding ZT values, and the ZT values follow the order: Sc2I2Se2 > Sc2Br2Se2 > Sc2Cl2Se2. At 300 K, we obtained maximum ZT of 0.34, 0.77, and 1.97 for Sc2Cl2Se2, Sc2Br2Se2, and Sc2I2Se2, respectively, by n-type doping in the x direction. These results demonstrate that monolayer Sc2X2Se2 (X = Cl, Br, I) materials are promising thermoelectric materials, Sc2I2Se2 has more desirable properties along the x direction, and n-type doping can significantly enhance the ZT values. Our work lays a foundation for exploring the TE transport properties of FeOCl-type monolayers.