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Molecular nanostructures are promising building blocks for future quantumtechnologies, provided methods of harnessing their multiple degrees of freedomcan be identified and implemented. Due to low decoherence rates nuclear spinsare considered ideal candidates for storing quantum information while opticalexcitations can give rise to fast and controllable interactions for informationprocessing. A recent paper (Physical Review Letters \textbf{104} 200501)proposed a method for entangling two nuclear spins through their mutualcoupling to a transient optically excited electron spin. Building on the sameidea, we here present an extended and much more detailed theoretical framework,showing that this method is in fact applicable to a much wider class ofmolecular structures than previously discussed in the original proposal.

Creating nuclear spin entanglement using an optical degree of freedom