Entangled Spin-Polarized Excitons from Singlet Fission in a Rigid Dimer: Article No. 1180

Ryan Dill, Kori Smyser, Brandon Rugg, Niels Damrauer, Joel Eaves

Research output: Contribution to journalArticlepeer-review

12 Scopus Citations

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.
Original languageAmerican English
Number of pages7
JournalNature Communications
Volume14
DOIs
StatePublished - 2023

NREL Publication Number

  • NREL/JA-5900-84834

Keywords

  • electron paramagnetic resonance
  • molecular photophysics
  • quantum information science
  • singlet fission

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