Microstructure determines crystallinity-driven singlet fission efficiency in diF-TES-ADT

Abstract Singlet fission (SF) describes the conversion of a single photon-generated excited state into two triplet excitons through an initial singlet state. Despite its significance for solar energy applications, the relationship between microstructure, temperature, and SF efficiency remains poorly...

Full description

Saved in:
Bibliographic Details
Main Authors: Hoyeon Choi, Stefan Skalsky, David G. Bossanyi, Jenny Clark, Patrick Parkinson
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Scientific Reports
Online Access:https://doi.org/10.1038/s41598-025-08427-y
Tags: Add Tag
No Tags, Be the first to tag this record!
_version_ 1849335250539249664
author Hoyeon Choi
Stefan Skalsky
David G. Bossanyi
Jenny Clark
Patrick Parkinson
author_facet Hoyeon Choi
Stefan Skalsky
David G. Bossanyi
Jenny Clark
Patrick Parkinson
author_sort Hoyeon Choi
collection DOAJ
description Abstract Singlet fission (SF) describes the conversion of a single photon-generated excited state into two triplet excitons through an initial singlet state. Despite its significance for solar energy applications, the relationship between microstructure, temperature, and SF efficiency remains poorly understood. Using cryogenic fluorescence microscopy, we correlate primary singlet fission (PSF) efficiency with local film morphology in a prototypical high-efficiency anthradithiophene (diF-TES-ADT) thin film. Our hyperspectral microscopy measurements of absorption and emission with sub-micron resolution reveal spatially inhomogeneous PSF efficiency that correlates directly with local crystallinity. Temperature- and time-resolved spectroscopy demonstrate that enhanced PSF efficiency in highly crystalline regions results from favorable endothermic alignment of a charge-transfer (CT) state. These findings emphasize how spatial inhomogeneity critically impacts SF film performance and caution against relying solely on spatially averaged metrics when evaluating SF materials.
format Article
id doaj-art-e2f47358c6bb49b3ab078d25ab5fa675
institution Kabale University
issn 2045-2322
language English
publishDate 2025-07-01
publisher Nature Portfolio
record_format Article
series Scientific Reports
spelling doaj-art-e2f47358c6bb49b3ab078d25ab5fa6752025-08-20T03:45:20ZengNature PortfolioScientific Reports2045-23222025-07-011511910.1038/s41598-025-08427-yMicrostructure determines crystallinity-driven singlet fission efficiency in diF-TES-ADTHoyeon Choi0Stefan Skalsky1David G. Bossanyi2Jenny Clark3Patrick Parkinson4Department of Physics and Astronomy and the Photon Science Institute, University of ManchesterDepartment of Physics and Astronomy and the Photon Science Institute, University of ManchesterSchool of Mathematical and Physical Sciences, The University of SheffieldSchool of Mathematical and Physical Sciences, The University of SheffieldDepartment of Physics and Astronomy and the Photon Science Institute, University of ManchesterAbstract Singlet fission (SF) describes the conversion of a single photon-generated excited state into two triplet excitons through an initial singlet state. Despite its significance for solar energy applications, the relationship between microstructure, temperature, and SF efficiency remains poorly understood. Using cryogenic fluorescence microscopy, we correlate primary singlet fission (PSF) efficiency with local film morphology in a prototypical high-efficiency anthradithiophene (diF-TES-ADT) thin film. Our hyperspectral microscopy measurements of absorption and emission with sub-micron resolution reveal spatially inhomogeneous PSF efficiency that correlates directly with local crystallinity. Temperature- and time-resolved spectroscopy demonstrate that enhanced PSF efficiency in highly crystalline regions results from favorable endothermic alignment of a charge-transfer (CT) state. These findings emphasize how spatial inhomogeneity critically impacts SF film performance and caution against relying solely on spatially averaged metrics when evaluating SF materials.https://doi.org/10.1038/s41598-025-08427-y
spellingShingle Hoyeon Choi
Stefan Skalsky
David G. Bossanyi
Jenny Clark
Patrick Parkinson
Microstructure determines crystallinity-driven singlet fission efficiency in diF-TES-ADT
Scientific Reports
title Microstructure determines crystallinity-driven singlet fission efficiency in diF-TES-ADT
title_full Microstructure determines crystallinity-driven singlet fission efficiency in diF-TES-ADT
title_fullStr Microstructure determines crystallinity-driven singlet fission efficiency in diF-TES-ADT
title_full_unstemmed Microstructure determines crystallinity-driven singlet fission efficiency in diF-TES-ADT
title_short Microstructure determines crystallinity-driven singlet fission efficiency in diF-TES-ADT
title_sort microstructure determines crystallinity driven singlet fission efficiency in dif tes adt
url https://doi.org/10.1038/s41598-025-08427-y
work_keys_str_mv AT hoyeonchoi microstructuredeterminescrystallinitydrivensingletfissionefficiencyindiftesadt
AT stefanskalsky microstructuredeterminescrystallinitydrivensingletfissionefficiencyindiftesadt
AT davidgbossanyi microstructuredeterminescrystallinitydrivensingletfissionefficiencyindiftesadt
AT jennyclark microstructuredeterminescrystallinitydrivensingletfissionefficiencyindiftesadt
AT patrickparkinson microstructuredeterminescrystallinitydrivensingletfissionefficiencyindiftesadt