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 Li on 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. © 2024 Elsevier B.V.