Entangled spin-polarized excitons from singlet fission in a rigid dimer

Nat Commun. 2023 Mar 2;14(1):1180. doi: 10.1038/s41467-023-36529-6.


Singlet fission, a process that splits a singlet exciton into a biexciton, has promise in quantum information. We report time-resolved electron paramagnetic resonance measurements on a conformationally well-defined acene dimer molecule, TIPS-BP1′, designed to exhibit strongly state-selective relaxation to specific magnetic spin sublevels. The resulting optically pumped spin polarization is a nearly pure initial state from the ensemble. The long-lived spin coherences modulate the signal intrinsically, allowing a measurement scheme that substantially removes noise and uncertainty in the magnetic resonance spectra. A nonadiabatic transition theory with a minimal number of spectroscopic parameters allows the quantitative assignment and interpretation of the spectra. In this work, we show that the rigid dimer TIPS-BP1′ supports persistent spin coherences at temperatures far higher than those used in conventional superconducting quantum hardware.

PMID:36859382 | PMC:PMC9977721 | DOI:10.1038/s41467-023-36529-6


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