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

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-mo...

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Veröffentlicht in:	Nature communications Jg. 16; H. 1; S. 7605 - 11
Hauptverfasser:	Carey, Remington L., Ren, Xinglong, Jacobs, Ian E., Elsner, Jan, Schott, Sam, Goldberg, Elliot, Wang, Zichen, Blumberger, Jochen, Sirringhaus, Henning
Format:	Journal Article
Sprache:	Englisch
Veröffentlicht:	London Nature Publishing Group UK 15.08.2025 Nature Publishing Group Nature Portfolio
Schlagworte:	639/301/119/998 639/766/119/995 Crystals Current carriers Electron paramagnetic resonance Electron spin Electron spin resonance Electrons Field effect transistors Graphene Humanities and Social Sciences Localization Magnetic fields multidisciplinary NMR Nuclear magnetic resonance Organic semiconductors Polymers Room temperature Science Science (multidisciplinary) Semiconductor devices Semiconductors Single crystals Spin resonance Temperature Temperature dependence
ISSN:	2041-1723, 2041-1723
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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. Spin relaxation in organic semiconductors is normally strongly correlated with temperature, varying over many orders of magnitude from 4 K to 300 K. Here, the authors report stable, microsecond-long spin lifetimes in rubrene single crystals due to the rapid transient localization of charge carriers.
AbstractList	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. 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. 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.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. 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. Spin relaxation in organic semiconductors is normally strongly correlated with temperature, varying over many orders of magnitude from 4 K to 300 K. Here, the authors report stable, microsecond-long spin lifetimes in rubrene single crystals due to the rapid transient localization of charge carriers. 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. Spin relaxation in organic semiconductors is normally strongly correlated with temperature, varying over many orders of magnitude from 4 K to 300 K. Here, the authors report stable, microsecond-long spin lifetimes in rubrene single crystals due to the rapid transient localization of charge carriers.
ArticleNumber	7605
Author	Carey, Remington L. Jacobs, Ian E. Wang, Zichen Schott, Sam Blumberger, Jochen Goldberg, Elliot Ren, Xinglong Elsner, Jan Sirringhaus, Henning
Author_xml	– sequence: 1 givenname: Remington L. surname: Carey fullname: Carey, Remington L. organization: Cavendish Laboratory, University of Cambridge – sequence: 2 givenname: Xinglong orcidid: 0000-0001-9824-5767 surname: Ren fullname: Ren, Xinglong email: xr216@cam.ac.uk organization: Cavendish Laboratory, University of Cambridge – sequence: 3 givenname: Ian E. orcidid: 0000-0002-1535-4608 surname: Jacobs fullname: Jacobs, Ian E. organization: Cavendish Laboratory, University of Cambridge – sequence: 4 givenname: Jan orcidid: 0000-0002-3685-3940 surname: Elsner fullname: Elsner, Jan organization: Department of Physics and Astronomy and Thomas Young Centre, University College London – sequence: 5 givenname: Sam surname: Schott fullname: Schott, Sam organization: Cavendish Laboratory, University of Cambridge – sequence: 6 givenname: Elliot orcidid: 0009-0007-3640-8699 surname: Goldberg fullname: Goldberg, Elliot organization: Cavendish Laboratory, University of Cambridge – sequence: 7 givenname: Zichen orcidid: 0009-0002-7852-558X surname: Wang fullname: Wang, Zichen organization: Cavendish Laboratory, University of Cambridge – sequence: 8 givenname: Jochen orcidid: 0000-0002-1546-6765 surname: Blumberger fullname: Blumberger, Jochen organization: Department of Physics and Astronomy and Thomas Young Centre, University College London – sequence: 9 givenname: Henning orcidid: 0000-0001-9827-6061 surname: Sirringhaus fullname: Sirringhaus, Henning email: hs220@cam.ac.uk organization: Cavendish Laboratory, University of Cambridge
BackLink	https://www.ncbi.nlm.nih.gov/pubmed/40817376$$D View this record in MEDLINE/PubMed
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Snippet	Field-induced electron spin resonance provides valuable insights into the interplay between spin and charge dynamics in organic semiconductors. We apply this... Abstract Field-induced electron spin resonance provides valuable insights into the interplay between spin and charge dynamics in organic semiconductors. We...
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SubjectTerms	639/301/119/998 639/766/119/995 Crystals Current carriers Electron paramagnetic resonance Electron spin Electron spin resonance Electrons Field effect transistors Graphene Humanities and Social Sciences Localization Magnetic fields multidisciplinary NMR Nuclear magnetic resonance Organic semiconductors Polymers Room temperature Science Science (multidisciplinary) Semiconductor devices Semiconductors Single crystals Spin resonance Temperature Temperature dependence
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Title	Long spin lifetimes of charge carriers in rubrene crystals due to fast transient-localization motion
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