chain compounds · cobalt · hysteresis · magnetic properties · radicals Magnetism, and in particular the force that magnetic materials exert at a distance, have fascinated mankind from the beginning of civilization. A material exposed to a magnetic field can retain its magnetized state after the field is removed. The magnetization in this case is cancelled only by applying a field in the opposite direction. The larger the field required to cancel the magnetization, also known as coercive field H c , the harder the magnet. Very hard magnets are important for mechanical devices, and nowadays they are based on intermetallic compounds, mainly SmCo and NdFeB alloys. However, a comparison of hardness based on the coercive field is made difficult by the strong dependence of H c on the preparation process, because the irreversible motion of the domain walls is heavily affected by defects, grain boundaries, and so forth.To date, molecular magnetism has failed to provide materials that at high temperature can compete with metallic hard magnets. Nevertheless, it has played a crucial role in lowdimensional magnetism. In fact, the appropriate choice of building blocks and linkers out of a huge library allows for an efficient confinement of the magnetic interaction. In particular, molecular magnetism has shown that magnetic hysteresis can be observed in the absence of long-range magnetic order in materials in which the magnetic interaction is either restricted to zero dimensions (that is, it has a finite length in three dimensions) or is confined in one dimension. [1] Polynuclear clusters [2] and chains [3] are now being widely investigated for their ability to retain a magnetic memory of purely molecular origin as well as for interesting quantum effects.[4] These two classes of materials have been given the evocative names single molecule magnets, SMM, [5] and single chain magnets, SCM, [6] respectively. For SCM, the possibility to observe the freezing of the magnetization was predicted in the 1960s by Glauber, [7] who developed the kinetic model for a chain of ferromagnetically coupled spins showing Ising-type anisotropy, that is, the spin is confined in one direction and can assume only the up/down configurations. In this case, the hysteresis results from the progressive slowing of the relaxation mechanism as its characteristic time, t, diverges exponentially at low temperature [Eq. (1)]The barrier DE is given by the energy required to nucleate two domain walls, that is, inverting the direction of one spin as shown in Figure 1. This energy is proportional to the intrachain exchange interaction J intra . For the Ising Hamiltonian written as h = JS 2 Ss i s i+1 (where s can only assume the values AE 1, and S is the spin value), the energy difference becomes DE = 4S 2 J intra .The first system to be well rationalized with the Glauber model was a cobalt(II) chain [8] in which the metal ions are linked by nitronyl-nitroxide radicals (Figure 2, top). These radicals have the unpaired electron essentially delocalized on the two NO g...