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

Hoyeon Choi; Stefan Skalsky; David G. Bossanyi; Jenny Clark; Patrick Parkinson

doi:10.1038/s41598-025-08427-y

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

Hoyeon Choi, Stefan Skalsky, David G. Bossanyi, Jenny Clark, Patrick Parkinson

Research output: Contribution to journal › Article › peer-review

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.

Original language	English
Article number	23737
Journal	Scientific Reports
Volume	15
Issue number	1
Early online date	3 Jul 2025
DOIs	https://doi.org/10.1038/s41598-025-08427-y
Publication status	E-pub ahead of print - 3 Jul 2025

Data Availability Statement

Data is provided within the manuscript and supplementary information. Raw datasets on transmission and absorption are available on Institutional Figshare (10.48420/28512701).

Funding

PP acknowledges funding under the UKRI Future Leaders Fellowship program [MR/T021519/1], and from the EPSRC (UK) [EP/V036343/1]. DGB acknowledges the EPSRC Centre for Doctoral Training in New and Sustainable Photovoltaics [EP/L01551X/1]. JC acknowledges the EPSRC (UK) [EP/T012455/1]. We acknowledge Sarah Wall (The University of Manchester) for AFM characterization.

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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.",

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

Abstract

Data Availability Statement

Funding

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