Slow vibrational relaxation drives ultrafast formation of photoexcited polaron pair states in glycolated conjugated polymers

Katia Pagano, Jin Gwan Kim, Joel Luke, Ellasia Tan, Katherine Stewart, Igor V. Sazanovich, Gabriel Karras, Hristo Ivov Gonev, Adam V. Marsh, Na Yeong Kim, Sooncheol Kwon, Young Yong Kim, M. Isabel Alonso, Bernhard Dörling, Mariano Campoy-Quiles, Anthony W. Parker, Tracey M. Clarke, Yun-Hi Kim () and Ji-Seon Kim ()
Additional contact information
Katia Pagano: Imperial College London
Jin Gwan Kim: Department of Chemistry and Research Institute of Molecular Alchemy (RIMA) Gyeongsang National University Jinju
Joel Luke: Imperial College London
Ellasia Tan: Imperial College London
Katherine Stewart: Imperial College London
Igor V. Sazanovich: STFC Rutherford Appleton Laboratory
Gabriel Karras: STFC Rutherford Appleton Laboratory
Hristo Ivov Gonev: Christopher Ingold Building
Adam V. Marsh: King Abdullah University of Science and Technology (KAUST)
Na Yeong Kim: Department of Chemistry and Research Institute of Molecular Alchemy (RIMA) Gyeongsang National University Jinju
Sooncheol Kwon: Dongguk University-Seoul
Young Yong Kim: Pohang University of Science and Technology
M. Isabel Alonso: ICMAB-CSIC
Bernhard Dörling: ICMAB-CSIC
Mariano Campoy-Quiles: ICMAB-CSIC
Anthony W. Parker: STFC Rutherford Appleton Laboratory
Tracey M. Clarke: Christopher Ingold Building
Yun-Hi Kim: Department of Chemistry and Research Institute of Molecular Alchemy (RIMA) Gyeongsang National University Jinju
Ji-Seon Kim: Imperial College London

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Glycol sidechains are often used to enhance the performance of organic photoconversion and electrochemical devices. Herein, we study their effects on electronic states and electronic properties. We find that polymer glycolation not only induces more disordered packing, but also results in a higher reorganisation energy due to more localised π-electron density. Transient absorption spectroscopy and femtosecond stimulated Raman spectroscopy are utilised to monitor the structural relaxation dynamics coupled to the excited state formation upon photoexcitation. Singlet excitons are initially formed, followed by polaron pair formation. The associated structural relaxation slows down in glycolated polymers (5 ps vs. 1.25 ps for alkylated), consistent with larger reorganisation energy. This slower vibrational relaxation is found to drive ultrafast formation of the polaron pair state (5 ps vs. 10 ps for alkylated). These results provide key experimental evidence demonstrating the impact of molecular structure on electronic state formation driven by strong vibrational coupling.

Date: 2024
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DOI: 10.1038/s41467-024-50530-7

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