Molecular nanostructures may constitute the fabric of future quantum technologies, if their degrees of freedom can be fully harnessed. Ideally one might use nuclear spins as low-decoherence qubits and optical excitations for fast controllable interactions. Here, we present a method for entangling two nuclear spins through their mutual coupling to a transient optically-excited electron spin, and investigate its feasibility through density functional theory and experiments on a test molecule. From our calculations we identify the specific molecular properties that permit high entangling power gates under simple optical and microwave pulses; synthesis of such molecules is possible with established techniques.
@article{arxiv.0911.5320,
title = {Entangling remote nuclear spins linked by a chromophore},
author = {Marcus Schaffry and Vasileia Filidou and Steven D. Karlen and Erik M. Gauger and Simon C. Benjamin and Harry L. Anderson and Arzhang Ardavan and G. Andrew D. Briggs and Kiminori Maeda and Kevin B. Henbest and Feliciano Giustino and John J. L. Morton and Brendon W. Lovett},
journal= {arXiv preprint arXiv:0911.5320},
year = {2010}
}