Microscopic Properties of Na and Li—A First Principle Study of Metal Battery Anode Materials

Using density functional theory, we studied the bulk and surface properties of Li and Na electrodes on an atomistic level. To get a better understanding of the initial stages of surface growth phenomena (and thus dendrite formation), various self‐diffusion mechanisms were studied. For this purpose, dedicated diffusion pathways on the surfaces of Na and Li were investigated within the terrace‐step‐kink (TSK) model utilizing nudged elastic band calculations. We were able to prove that the mere investigation of terrace self‐diffusion on the respective low‐index surfaces does not provide a possible descriptor for dendritic growth. Finally, we provide an initial view of the surface growth behavior of both alkali metals as well as provide a basis for experimental investigations and theoretical long‐scale kinetic Monte Carlo simulations.