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

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 re...

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Autores principales: Dill, Ryan D., Smyser, Kori E., Rugg, Brandon K., Damrauer, Niels H., Eaves, Joel D.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9977721/
https://www.ncbi.nlm.nih.gov/pubmed/36859382
http://dx.doi.org/10.1038/s41467-023-36529-6
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author Dill, Ryan D.
Smyser, Kori E.
Rugg, Brandon K.
Damrauer, Niels H.
Eaves, Joel D.
author_facet Dill, Ryan D.
Smyser, Kori E.
Rugg, Brandon K.
Damrauer, Niels H.
Eaves, Joel D.
author_sort Dill, Ryan D.
collection PubMed
description 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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spelling pubmed-99777212023-03-03 Entangled spin-polarized excitons from singlet fission in a rigid dimer Dill, Ryan D. Smyser, Kori E. Rugg, Brandon K. Damrauer, Niels H. Eaves, Joel D. Nat Commun Article 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. Nature Publishing Group UK 2023-03-02 /pmc/articles/PMC9977721/ /pubmed/36859382 http://dx.doi.org/10.1038/s41467-023-36529-6 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Dill, Ryan D.
Smyser, Kori E.
Rugg, Brandon K.
Damrauer, Niels H.
Eaves, Joel D.
Entangled spin-polarized excitons from singlet fission in a rigid dimer
title Entangled spin-polarized excitons from singlet fission in a rigid dimer
title_full Entangled spin-polarized excitons from singlet fission in a rigid dimer
title_fullStr Entangled spin-polarized excitons from singlet fission in a rigid dimer
title_full_unstemmed Entangled spin-polarized excitons from singlet fission in a rigid dimer
title_short Entangled spin-polarized excitons from singlet fission in a rigid dimer
title_sort entangled spin-polarized excitons from singlet fission in a rigid dimer
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9977721/
https://www.ncbi.nlm.nih.gov/pubmed/36859382
http://dx.doi.org/10.1038/s41467-023-36529-6
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