“…In order to understand the connection between structure and properties of these materials, the combination of TEM and theoretical calculations is very powerful. − However, it is important to realize that TEM images only correspond to a two-dimensional (2D) projection of a three-dimensional (3D) object. In order to gain the necessary structural information concerning the 3D nanoassemblies, 3D TEM, so-called electron tomography, has to be performed. − Recently, this technique has proven its power in the investigation of 3D nanoassemblies, especially when quantitative data, such as particle diameters or positions, are required. , 2D self-assembled systems have been theoretically studied in depth during the past decade, − and the transition between 2D and 3D assemblies has been recently investigated . However, these studies are mainly based on phenomenological models, ,,− but do not yield insight concerning the underlying physical processes involved during the formation of the 3D assemblies.…”