use the naturally occurring dipolar interactions to realize interacting spin systems. This opens the way toward the realization of a broad class of tunable spin models in both two- and one-dimensional geometries. We illustrate the potential offered by these systems in the context of dimerized Majumdar-Ghosh-type phases, archetypical examples of quantum magnetism, showing how such phases are robust against disorder and decoherence, and could be observed within state-of-the-art experiments.