Entangled spin-polarized excitons from singlet fission in a rigid dimer.
Ryan D DillKori E SmyserBrandon K RuggNiels H DamrauerJoel D EavesPublished in: Nature communications (2023)
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.
Keyphrases
- density functional theory
- molecular dynamics
- energy transfer
- room temperature
- single molecule
- magnetic resonance
- transition metal
- healthcare
- quantum dots
- magnetic resonance imaging
- air pollution
- ionic liquid
- mass spectrometry
- deep learning
- contrast enhanced
- convolutional neural network
- machine learning
- social media
- molecular dynamics simulations