Electron–Ion Coupling and Li-Ion Dynamics Interplay in the Correlated Kagome Network Li_xScMo₃O₈

The Kagome material, Li_xScMo₃O₈, displays a breathing distortion leading to magnetic Mo₃ trimer clusters whose properties can be reversibly controlled through electrochemical Li insertion. While previous studies have shown that Li diffusion can control the magnetic ground state of the material, the interplay between localized electronic states, crystal structure, and Li-ion transport remains unexplored. In this study, we use first-principles calculations, including density functional theory and nudged elastic band, to investigate the coupling between Li migration and the electronic structure of the breathing distortion of the Kagome network. By tracking charge, spin and magnetic moment along in-plane diffusion pathways, we reveal how structural distortions and electron localization on the Mo₃ clusters modify the Li migration landscape, and determine its resulting correlated electron properties.