Lithiated Single-Layer Holey Mo8s12: Electronic, Magnetic and Vibrational Characteristics

Abstract

Motivated by the recent experimental realization of holey transition metal chalcogenides[ACS Applied Materials & Interfaces 2022, 14(23), 27056-27062], in this study, the holey structure of Mo8S12 is investigated by means of density functional theory-based calculations. The geometry optimization and phonon band dispersion calculations show the structural and dynamical stability of free-standing holey single-layer Mo8S12. In addition, electronic band dispersions reveal the direct band gap semiconducting nature of the structure. In order to investigate the lithiation capacity of single-layer Mo8S12, effect of Li doping on the properties of Mo8S12 is analyzed by considering both one- and double-sided lithiation. Our calculations indicate that single Li atom is chemically adsorbed on top of Mo8S12 through the Mo-Mo bridge site and experiences relatively high diffusion barrier at room temperature, which shows the chemical stability of adsorbed Lion the surface. As one surface of single-layer Mo8S12 is fully saturated with Li atoms, a dynamically stable semiconducting structure is formed. Moreover, the double-side lithiated structure is found to be dynamically stable derivative of Mo8S12. The corresponding electronic band structures reveals the semiconducting behavior of the double-side lithiated single-layer. The predicted voltage of lithiated Mo8S12 reveal its potential for battery applications as a cathode material. Apparently, either one or two side lithiation allows one to significantly tune the electronic and magnetic properties of Mo8S12. Overall, tunable electronic band gap of single-layer holey Mo8S12 via lithiation could make it suitable candidate for optoelectronic devices.