Abstract. We present a novel method for the fabrication of well-ordered, two-dimensional nanocluster arrays. The method is based on the confined nucleation of adatoms within the superstructure cells of periodic surface dislocation networks, which form in many heteroepitaxial systems. We show how quantitative understanding of adatom diffusion and heterogeneous nucleation on such surfaces can be obtained through kinetic Monte-Carlo simulations and discuss the potential of this approach.PACS. 61.46.+w Clusters, nanoparticles, and nanocrystalline materials -81.15.Hi Molecular, atomic, ion, and chemical beam epitaxy -68.65.+g Low-dimensional structures (superlattices, quantum well structures, multilayers): structure, and nonelectronic properties During the last years, much effort has been devoted to the fabrication of nanostructures on semiconductor and metal surfaces. Research first focused on the variety of structures that could be produced, either by serial techniques such as atom manipulation with the tip of a scanning tunneling microscope (STM) [1], or by parallel processes such as self-organized growth [2][3][4][5]. Recently, the interest turned towards the problem of increasing homogeneity and spatial regularity of the nanostructure populations. The controlled deposition of size-selected clusters from the gas phase [6], e.g., produces nanostructures of nearly uniform dimensions. But, like the approach of self-organized growth, this method suffers from the statistics inherent in deposition and leads to largely uncorrelated spatial distributions. Improved lateral order was obtained by exploiting the spatial correlation of island nucleation in a sequence of island and spacer layers in semiconductor superlattices [7]. In a different approach, the preferred nucleation of Ni at the elbows of the Au(111) herringbone reconstruction resulted in ordered lines of islands [8], which later could be explained with a site-specific exchange process for this specific system [9].In the present contribution we present a method to fabricate ordered arrays of equally spaced nanostructures that is of potential applicability in a large variety of systems. On substrates with a periodic arrangement of dislocations, regular superlattices of almost monodispersed islands can be created by self-organized growth. Due to mutual long range repulsions the dislocations arrange into highly ordered periodic patterns that can be transferred into nanostructure superlattices through heterogeneous nucleation. The mechanism imposing the inhomogeneous substrate structure on the nucleation and growth process a Corresponding author. e-mail: harald.brune@epfl.ch is the strong repulsion of dislocations towards diffusing adatoms. Here, we illustrate this method for Ag nucleation on the second monolayer (ML) of Ag on a Pt(111) substrate (see Fig. 1b). The method, however, is of general importance as the required periodic substrates are provided by numerous epitaxial systems that show strain relief through dislocation formation. So far, besides the above men...