IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v16y2025i1d10.1038_s41467-025-56480-y.html
   My bibliography  Save this article

Machine learning photodynamics decode multiple singlet fission channels in pentacene crystal

Author

Listed:
  • Zhendong Li

    (Shenzhen Polytechnic University)

  • Federico J. Hernández

    (University College London)

  • Christian Salguero

    (Northeastern University)

  • Steven A. Lopez

    (Northeastern University)

  • Rachel Crespo-Otero

    (University College London)

  • Jingbai Li

    (Shenzhen Polytechnic University)

Abstract

Crystalline pentacene is a model solid-state light-harvesting material because its quantum efficiencies exceed 100% via ultrafast singlet fission. The singlet fission mechanism in pentacene crystals is disputed due to insufficient electronic information in time-resolved experiments and intractable quantum mechanical calculations for simulating realistic crystal dynamics. Here we combine a multiscale multiconfigurational approach and machine learning photodynamics to understand competing singlet fission mechanisms in crystalline pentacene. Our simulations reveal coexisting charge-transfer-mediated and coherent mechanisms via the competing channels in the herringbone and parallel dimers. The predicted singlet fission time constants (61 and 33 fs) are in excellent agreement with experiments (78 and 35 fs). The trajectories highlight the essential role of intermolecular stretching between monomers in generating the multi-exciton state and explain the anisotropic phenomenon. The machine-learning-photodynamics resolved the elusive interplay between electronic structure and vibrational relations, enabling fully atomistic excited-state dynamics with multiconfigurational quantum mechanical quality for crystalline pentacene.

Suggested Citation

  • Zhendong Li & Federico J. Hernández & Christian Salguero & Steven A. Lopez & Rachel Crespo-Otero & Jingbai Li, 2025. "Machine learning photodynamics decode multiple singlet fission channels in pentacene crystal," Nature Communications, Nature, vol. 16(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-56480-y
    DOI: 10.1038/s41467-025-56480-y
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-025-56480-y
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-025-56480-y?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Bruno Ehrler & Brian J. Walker & Marcus L. Böhm & Mark W.B. Wilson & Yana Vaynzof & Richard H. Friend & Neil C. Greenham, 2012. "In situ measurement of exciton energy in hybrid singlet-fission solar cells," Nature Communications, Nature, vol. 3(1), pages 1-6, January.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.

      More about this item

      Statistics

      Access and download statistics

      Corrections

      All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-56480-y. See general information about how to correct material in RePEc.

      If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

      If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

      If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

      For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

      Please note that corrections may take a couple of weeks to filter through the various RePEc services.

      IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.