Lithium Ion Transport Environment by Molecular Vibrations in Ion‐Conducting Glasses

Controlling Li ion transport in glasses at atomic and molecular levels is key to realizing all-solid-state batteries, a promising technology for electric vehicles. In this context, Li3PS4 glass, solid electrolyte candidate, exhibits dynamic coupling between the Li+ cation mobility PS43− anion libration, which commonly referred as paddlewheel effect. addition, it concerted diffusion effect (i.e., cation–cation interaction), regarded essence of high transport. However, correlation ions within glass structure can only be vaguely determined, due limited experimental information that obtained. Here, study reports present classified by evaluating their valence oscillations via Bader analysis topologically analyze chemical bonds. It found three types are more mobile Li3-type ions) exhibit characteristic relatively long distances 4.0–5.0 Å. Furthermore, reverse Monte Carlo simulations combined with deep learning potentials reproduce X-ray, neutron, electron diffraction pair distribution functions showed an increase number partially crystallized structures improved properties. Our results show order disorder topological valences. Thus, considering vibrations during evaluation valences expected lead development new electrolytes.