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Dill, Ryan D. ; Smyser, Kori E. ; Rugg, Brandon K. ; Damrauer, Niels H. ; Eaves, Joel D. ( , Nature Communications)
Abstract 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.
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Nelson, Jordan N. ; Zhang, Jinyuan ; Zhou, Jiawang ; Rugg, Brandon K. ; Krzyaniak, Matthew D. ; Wasielewski, Michael R. ( , The Journal of Chemical Physics)