Enhanced coherence by coupling spins through a delocalized π-system: Vanadyl porphyrin dimers

Pozo I, Huang Z, Alexandropoulos DI, Slota MC, Tkach I, Bennati M, Deng J-R, Stawski W, Horton PN, Myers WK, Kong F, Lombardi F
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et al

Vanadium(IV) magnetic centers are prime candidates for molecular quantum units. One long-standing question is how to obtain a scaffold that connects multiple centers and allows two communication modalities: magnetic and electronic. We have synthesized and studied a selection of vanadyl porphyrin dimers as models of the most synthetically accessible linear porphyrin arrays. We show that a strongly π-conjugated backbone places the magnetic system in an intermediate regime dominated by exchange coupling (J) and protects the quantum coherence against electron pair flip-flop processes at low temperatures (<10 K). This result is a fundamental step toward the design of molecular materials for single-molecule devices controlled by microwaves with electrical readout.