One of the two key requirements of n-dimensional ferroic systems is the spontaneous formation of homogeneously ordered areas, called domains, separated one from another by distinct (n − 1)-dimensional entities, called domain walls, see Sect. 2.1.4 on page 16. These walls constitute natural interfaces within the system between two or more energetically degenerate realisations of a particular order. For the artificial nanomagnetic arrays investigated throughout this work, the spontaneous formation of long-range order connected to an order parameter is a hallmark for their classification as primary ferroic order [1]. Suitable symmetry groups allowing for toroidal order have already been identified a few decades ago and are listed in Sect. 2.1.6 on page 19. The nanomagnetic arrays that have been investigated here, see Fig. 4.1 on page 83, fall in one of these groups, setting the basis for their further scrutiny not only on the macroscopic but also on the microscopic scale. Since ferrotoroidicity has been explored as a macroscopic phenomenon so far, microscopic origins of the ordering remain largely unexplored. In conventional materials, spins in a toroidally ordered crystal do not couple directly but via a fragile and wellbalanced competition of different inter-and intra-exchange paths [2,3]. These are typically variants of superexchange-or super-superexchange interaction via nonmagnetic ligands, e.g., oxoanions (such as phosphates, silicates, germanates) [4]. For the present work, a substitution of microscopic exchange interactions with magnetic dipole-dipole interaction provides a direct geometric access to inherent coupling mechanisms, see for instance Fig. 2.13. Note that toroidal moments and toroidal crystals with a significant contribution from the magnetic-dipole interaction [5] have also been found and studied in systems with a ring-like arrangement of high-magneticmoment rare-earth ions in molecular metal-organic frameworks [4], see Section 2.1.6. At this point, it is worth to recapitulate that ferroic order constitutes a macroscopic phenomenon without any constraints on the microscopic level. This allows for the engineering of a particular ferroic state using 'unconventional' constituents and arbitrary underlying interactions.