Presentation
1 August 2021 Efficient energy transport in an organic semiconductor mediated by transient exciton delocalisation
Alexander J. Sneyd, Tomoya Fukui, David Paleček, Suryoday Prodhan, Isabella Wagner, Yifan Zhang, Jooyoung Sung, Sean M. Collins, Thomas J. A. Slater, Zahra Andaji-Garmaroudi, Liam R. MacFarlane, J. Diego Garcia-Hernandez, Linjun Wang, George R. Whittell, Justin M. Hodgkiss, Kai Chen, David Beljonne, Ian Manners, Richard H. Friend, Akshay Rao
Author Affiliations +
Abstract
Efficient energy transport is highly desirable for organic semiconductor (OSC) devices such as photovoltaics, photodetectors, and photocatalytic systems. However, photo-generated excitons in OSC films mostly occupy highly localized states over their lifetime. Energy transport is hence thought to be mainly mediated by the site-to-site hopping of localized excitons, limiting exciton diffusion coefficients to below ~10-2 cm2/s with corresponding diffusion lengths below ~50 nm. Here, using ultrafast optical microscopy combined with non-adiabatic molecular dynamics simulations, we present evidence for a new highly-efficient energy transport regime: transient exciton delocalization, where energy exchange with vibrational modes allows excitons to temporarily re-access spatially extended states under equilibrium conditions. In films of highlyordered poly(3-hexylthiophene) nanofibers, prepared using living crystallization-driven self-assembly, we show that this enables exciton diffusion constants up to 1.1 ± 0.1 cm2/s and diffusion lengths of 300 ± 50 nm. Our results reveal the dynamic interplay between localized and delocalized exciton configurations at equilibrium conditions, calling for a re-evaluation of the basic picture of exciton dynamics. This establishes new design rules to engineer efficient energy transport in OSC films, which will enable new devices architectures not based on restrictive bulk heterojunctions.
Conference Presentation
© (2021) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only.
Alexander J. Sneyd, Tomoya Fukui, David Paleček, Suryoday Prodhan, Isabella Wagner, Yifan Zhang, Jooyoung Sung, Sean M. Collins, Thomas J. A. Slater, Zahra Andaji-Garmaroudi, Liam R. MacFarlane, J. Diego Garcia-Hernandez, Linjun Wang, George R. Whittell, Justin M. Hodgkiss, Kai Chen, David Beljonne, Ian Manners, Richard H. Friend, and Akshay Rao "Efficient energy transport in an organic semiconductor mediated by transient exciton delocalisation", Proc. SPIE 11799, Physical Chemistry of Semiconductor Materials and Interfaces XX, 117990A (1 August 2021); https://doi.org/10.1117/12.2594688
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KEYWORDS
Excitons

Nanofibers

Diffusion

Picosecond phenomena

Crystals

Absorption

Diffraction

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