Quantum technologies require understanding and deep control of systems at the molecular and atomic scale, both experimentally and theoretically. All well-designed quantum technologies proposed here are relevant to the implementation of quantum sensing and practical quantum computing as current and near-term innovative technologies. In this proposal, we focus on a prototypical class of quantum systems, molecular spins, for which the possibility to control quantum coherence and entanglement at the molecular level has been demonstrated. We plan to experimentally use advanced microwave magnetic resonance techniques with three main objectives in mind: (1) the exploration of a new class of fluorescent magnetic molecules with a view to initialization and readout of molecular spins states with photons in the visible range; and (2) the development and testing of highly sophisticated microwave pulse sequences designed to optimize the coherent manipulation of molecular spins with high fidelity. This second activity will allow us to test general concepts of the theory of quantum control and to develop advanced magnetic resonance techniques of general interest for the manipulation of quantum spin systems and any open-shell chemical/biological entities. The theoretical aspect of this proposal includes (3) the implementation of practical quantum algorithms for disruptive quantum chemical calculations beyond the current state-of-the-art of any quantum calculations on classical computers. Due to the multidisciplinary nature of these activities, collaboration between three leading teams in Osaka (JP), Modena (IT) and Tallahassee (FL, US) will allow for sharing of complementary skills and facilities, while coordination of these activities at an international level is of strategic importance to this field.