The structure with the lowest potential energy, from now on referred to as lowest-energy structure, was selected for further investigations (e.g. charge transport calculations, calculating the average preferred surface-to-surface distance). The surface-to-surface distance is calculated from the edge of the upper gold surface to the edge of the bottom gold surface, as indicated in Figure , so they can be compared directly with experimental GISAXS and SAXS data. Therefore, we calculated the distance from the centre of the Au atoms of the outer, fixed layers and subtracted twice the width of the surfaces, and twice the van-der-Waals radius of Au atoms. To get a statistical analysis of the surface-to-surface distance, MD simulations were repeated 10 times from the same starting structure but with different seed velocities. This also allowed for a sampling of different conformations of the ligands in the lowest-energy structure and for a range of different preferred surface-to-surface distances, depending on the arrangement of the ligand molecules. The average preferred surface-tosurface distances were calculated from the minima of the 10 MD run. To investigate the dependence of the most favorable surface-to-surface distances on the averaging procedure, we also extracted the surface-to-surface distances from the minimum of a parabola fit we applied on the average potential energy vs. surface-to-surface distance curves, which resulted in similar distances (see Supporting Information, Section S2.3.5).