Identifying Sources of Entanglement Loss in Photodriven Molecular Electron Spin Teleportation

We report on an electron donor-electron acceptor-stable radical (D-A-R•) molecule in which an electron spin state first prepared on R• is followed by photogeneration of an entangled singlet 1[D•+-A•–] spin pair to produce D•+-A•–-R•. Since the A•– and R• spins within D•+-A•–-R• are uncorrelated, spin teleportation from R• to D•+ occurs with a maximal 25% efficiency only for the singlet pair 1(A•–-R•) by spin-allowed electron transfer from A•– to R•. However, since 1[D•+-A•–] is sufficiently long-lived, coherent spin mixing involving the unreactive 3(A•–-R•) population affects entanglement and teleportation within D•+-A•–-R•. Pulse electron paramagnetic resonance experiments show a direct correlation between electron spin flip-flops and entanglement loss, providing information for designing molecular materials to serve as nanoscale quantum device interconnects.