To gain deeper insights into the interfacial interactions, contour plots of charge rearrangement upon adsorption are presented in Fig. , illustrating the difference between the electron density of the adsorption complex and that of the isolated NaOTF ion pair and the bare surface. These plots demonstrate a region of enhanced charge density between the sodium cation and the surface atoms, suggesting some form of covalent interaction, alongside a region of reduced charge density between the triflate anion and the surface atoms. This implies the induction of a horizontal dipole moment in the interfacial region, opposite to that of the ion pair. The observed charge rearrangement is particularly pronounced on sodium surfaces, where regions of charge accumulation and depletion envelop the adsorbed ions (see Fig. , panels b and c).