Discussing the influence of other factors that influence the structure of the interfaces Other contributing factors, as summarized in Figure , that influence the structure of the particle-particle interfaces and that may be responsible for deviations of our model from the experiment will be discussed in the following. First, we assume highly ordered assemblies of GNPs with no voids or non-parallel facet orientations, as these structures would be non-periodic. In experiments, however, GNP assemblies are usually disordered to a certain degree, and the structural disorder was shown to have a significant impact especially on the electron transport properties of the assemblies. 33 Second, we did not consider different ligand coverages. It is likely that the ligand coverage that we obtained from SAM simulations reflects the average ligand coverage on the GNPs in assemblies. In each of the interfaces, the ligand coverage may, however, deviate slightly from the optimal coverage, resulting in some interfaces where the coverage is slightly higher or slightly lower than the optimal coverage. ) of the linear regressions can be found in Table of the Supporting Information.