Monolayer 1T-Ag 6 S 2 with Excellent Thermoelectric Properties.

We obtained a new material called monolayer 1T-Ag 6 S 2 by replacing metal atoms in 1T phase transition-metal dichalcogenide sulfides (TMDs) with octahedral Ag 6 clusters. Subsequently, the thermoelectric transport properties of monolayer 1T-Ag 6 S 2 were systematically investigated using first-principles calculations and the generalized gradient approximation (GGA-PBE) exchange correlation functional. The findings demonstrate that monolayer 1T-Ag 6 S 2 displays characteristics of a wide-bandgap semiconductor, with a bandgap of 2.48 eV. Notably, the incorporation of Ag 6 clusters disrupts the structural symmetry, effectively enhancing the electronic structure and phonon properties of the material. Due to the flat valence band near the Fermi level, the extended relaxation time of the hole results in a greater effective mass compared to the electron, leading to a significant increase in the Seebeck coefficient. Under optimal doping conditions, the power factor of monolayer 1T-Ag 6 S 2 can achieve 14.9 mW/mK 2 at 500 K. The intricate crystal structure induces phonon path bending, reduces the overall frequency of phonon vibrations (<10 THz), and causes hybridization of low-frequency optical and acoustic branches, resulting in remarkably low lattice thermal conductivity (0.20 and 0.17 W/mK along the x and y axes at 500 K, respectively). The monolayer 1T-Ag 6 S 2 demonstrates a remarkably high figure of merit ZT of 3.14 (3.15) on the x ( y ) axis at 500 K, significantly higher than those of conventional TMD materials. Such excellent thermoelectric properties suggest that monolayer 1T-Ag 6 S 2 is a promising thermoelectric (TE) material. Our work reveals the deep mechanism of cluster substitution to optimize the thermoelectric properties of materials and provides a useful reference for subsequent research.