To capture the restructuring of surface atoms in the presence of adsorbed ions, we calculate the displacements of relaxing atoms in each surface model from their respective positions in the bare surface. This includes the topmost layer for all surface models, as well as the layer directly below it for graphite and the two layers below it for the sodium surfaces. The maximum displacements obtained for each layer are presented in Fig. , denoted by 𝛿 4 for the topmost layer, and 𝛿 2 and 𝛿 + for the subsequent layers. These results suggest a restructuring of the topmost layer atoms in the sodium metal surfaces, especially for the bcc (100) lattice, likely due to their strong chemical interactions with the adsorbate atoms. The positions of graphite atoms, however, remain almost unchanged after adsorption, indicating their weaker interactions with the ion pair, which are likely purely electrostatic, as discussed next. obtained from Eq. 1, alongside key structural properties, including the vertical distance between the cation and the average position of atoms in the topmost surface layer, 𝑟 !"#$ ! or 𝑟 !"#!" ! , the vertical distance between the closest anion oxygen to the surface and the average position of atoms in the topmost surface layer, 𝑟 %#$ ! or 𝑟 %#!" ! , the angle between the S-C bond in the triflate anion and the surface plane, 𝛼 %&' , and the maximum atomic displacements in surface layers relative to the bare surface (𝛿 ) for the topmost layer, 𝛿 * for the second layer, and 𝛿 + for the third layer).