Li, Zhendong;
Hernández, Federico J;
Salguero, Christian;
Lopez, Steven A;
Crespo-Otero, Rachel;
Li, Jingbai;
(2025)
Machine learning photodynamics decode multiple singlet fission channels in pentacene crystal.
Nature Communications
, 16
, Article 1194. 10.1038/s41467-025-56480-y.
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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.
| Type: | Article |
|---|---|
| Title: | Machine learning photodynamics decode multiple singlet fission channels in pentacene crystal |
| Location: | England |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1038/s41467-025-56480-y |
| Publisher version: | https://doi.org/10.1038/s41467-025-56480-y |
| Language: | English |
| Additional information: | 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 licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence 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 licence, visit http://creativecommons.org/licenses/by/4.0/. |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10204490 |
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