Localising Multiple Spin-Charge States in Bridgehead-to-peri Annulated Triptycenes

The development of quantum and spintronic technologies based on organic materials requires new molecular design principles yet to be established. Nitrogen-vacancy (NV) defects in the three-dimensional (3D) structure of diamond have emerged as pivotal elements in emerging quantum technologies. Inspired by the structure of NVs here we use the archetypical 3D polycyclic aromatic compound triptycene as a molecular scaffold from which to construct structural analogues of a proximal pair of NVs. We have annulated new rings between the bridgehead and peri-positions of the triptycene and then appended electroactive moieties in a manner that allows the molecules to support multiple spin and charge states. We show that those spin/charge states can be switched on or off electrochemically under very narrow applied potentials, and that each state remains localised in its own well-defined region of intramolecular 3D space, representing an initial step in the realisation of modular molecular quantum materials.