Exciton Diffusion in Highly-Ordered One Dimensional Conjugated Polymers: Effects of Back-Bone Torsion, Electronic Symmetry, Phonons and Annihilation.
J Phys Chem Lett
American Chemical Society (ACS)
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Pandya, R., Alvertis, A., Gu, Q., Sung, J., Legrand, L., Kréher, D., Barisien, T., et al. (2021). Exciton Diffusion in Highly-Ordered One Dimensional Conjugated Polymers: Effects of Back-Bone Torsion, Electronic Symmetry, Phonons and Annihilation.. J Phys Chem Lett, 12 (14), 3669-3678. https://doi.org/10.1021/acs.jpclett.1c00193
Many optoelectronic devices based on organic materials require rapid and long-range singlet exciton transport. Key factors controlling exciton transport include material structure, exciton-phonon coupling and electronic state symmetry. Here, we employ femtosecond transient absorption microscopy to study the influence of these parameters on exciton transport in one-dimensional conjugated polymers. We find that excitons with 21Ag- symmetry and a planar backbone exhibit a significantly higher diffusion coefficient (34 ± 10 cm2 s-1) compared to excitons with 11Bu+ symmetry (7 ± 6 cm2 s-1) with a twisted backbone. We also find that exciton transport in the 21Ag- state occurs without exciton-exciton annihilation. Both 21Ag- and 11Bu+ states are found to exhibit subdiffusive behavior. Ab initio GW-BSE calculations reveal that this is due to the comparable strengths of the exciton-phonon interaction and exciton coupling. Our results demonstrate the link between electronic state symmetry, backbone torsion and phonons in exciton transport in π-conjugated polymers.
Is supplemented by: https://doi.org/10.17863/CAM.66251
Winton Program for Physics of Sustainability
Engineering and Physical Sciences Research Council (EP/L015552/1)
European Research Council (758826)
External DOI: https://doi.org/10.1021/acs.jpclett.1c00193
This record's URL: https://www.repository.cam.ac.uk/handle/1810/319573
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