Long spin lifetimes of charge carriers in rubrene crystals due to fast transient-localization motion

Abstract Field-induced electron spin resonance provides valuable insights into the interplay between spin and charge dynamics in organic semiconductors. We apply this technique to ion-gel-gated capacitors and conventional field-effect transistors to study the temperature-dependent carrier dynamics o...

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Main Authors: Remington L. Carey, Xinglong Ren, Ian E. Jacobs, Jan Elsner, Sam Schott, Elliot Goldberg, Zichen Wang, Jochen Blumberger, Henning Sirringhaus
Format: Article
Language:English
Published: Nature Portfolio 2025-08-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-62830-7
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author Remington L. Carey
Xinglong Ren
Ian E. Jacobs
Jan Elsner
Sam Schott
Elliot Goldberg
Zichen Wang
Jochen Blumberger
Henning Sirringhaus
author_facet Remington L. Carey
Xinglong Ren
Ian E. Jacobs
Jan Elsner
Sam Schott
Elliot Goldberg
Zichen Wang
Jochen Blumberger
Henning Sirringhaus
author_sort Remington L. Carey
collection DOAJ
description Abstract Field-induced electron spin resonance provides valuable insights into the interplay between spin and charge dynamics in organic semiconductors. We apply this technique to ion-gel-gated capacitors and conventional field-effect transistors to study the temperature-dependent carrier dynamics of high-mobility rubrene single-crystals. Unlike previous measurements on other molecular and polymer semiconductors, we observe remarkably long spin relaxation times—on the order of microseconds—persisting from room temperature down to 15 K. Such long relaxation times are caused by the rapid transient-localization motion of charge carriers, which induces efficient motional narrowing. Additionally, by leveraging the high injection efficiency of ion-gel-gated devices, we observe spin lifetimes shortening at high carrier concentrations. This is attributed to emerging spin-spin dipolar interactions and can be modelled using an approach adapted from fluid-phase nuclear magnetic resonance. Our work demonstrates that field-induced electron spin resonance provides a powerful probe of the transient-localization physics of high-mobility molecular crystals.
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spelling doaj-art-b9133d2dae8641f2b4b400f60d278be72025-08-20T04:02:55ZengNature PortfolioNature Communications2041-17232025-08-0116111110.1038/s41467-025-62830-7Long spin lifetimes of charge carriers in rubrene crystals due to fast transient-localization motionRemington L. Carey0Xinglong Ren1Ian E. Jacobs2Jan Elsner3Sam Schott4Elliot Goldberg5Zichen Wang6Jochen Blumberger7Henning Sirringhaus8Cavendish Laboratory, University of CambridgeCavendish Laboratory, University of CambridgeCavendish Laboratory, University of CambridgeDepartment of Physics and Astronomy and Thomas Young Centre, University College LondonCavendish Laboratory, University of CambridgeCavendish Laboratory, University of CambridgeCavendish Laboratory, University of CambridgeDepartment of Physics and Astronomy and Thomas Young Centre, University College LondonCavendish Laboratory, University of CambridgeAbstract Field-induced electron spin resonance provides valuable insights into the interplay between spin and charge dynamics in organic semiconductors. We apply this technique to ion-gel-gated capacitors and conventional field-effect transistors to study the temperature-dependent carrier dynamics of high-mobility rubrene single-crystals. Unlike previous measurements on other molecular and polymer semiconductors, we observe remarkably long spin relaxation times—on the order of microseconds—persisting from room temperature down to 15 K. Such long relaxation times are caused by the rapid transient-localization motion of charge carriers, which induces efficient motional narrowing. Additionally, by leveraging the high injection efficiency of ion-gel-gated devices, we observe spin lifetimes shortening at high carrier concentrations. This is attributed to emerging spin-spin dipolar interactions and can be modelled using an approach adapted from fluid-phase nuclear magnetic resonance. Our work demonstrates that field-induced electron spin resonance provides a powerful probe of the transient-localization physics of high-mobility molecular crystals.https://doi.org/10.1038/s41467-025-62830-7
spellingShingle Remington L. Carey
Xinglong Ren
Ian E. Jacobs
Jan Elsner
Sam Schott
Elliot Goldberg
Zichen Wang
Jochen Blumberger
Henning Sirringhaus
Long spin lifetimes of charge carriers in rubrene crystals due to fast transient-localization motion
Nature Communications
title Long spin lifetimes of charge carriers in rubrene crystals due to fast transient-localization motion
title_full Long spin lifetimes of charge carriers in rubrene crystals due to fast transient-localization motion
title_fullStr Long spin lifetimes of charge carriers in rubrene crystals due to fast transient-localization motion
title_full_unstemmed Long spin lifetimes of charge carriers in rubrene crystals due to fast transient-localization motion
title_short Long spin lifetimes of charge carriers in rubrene crystals due to fast transient-localization motion
title_sort long spin lifetimes of charge carriers in rubrene crystals due to fast transient localization motion
url https://doi.org/10.1038/s41467-025-62830-7
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