Chemistry (all); Biochemistry, Genetics and Molecular Biology (all); Physics and Astronomy (all); General Physics and Astronomy; General Biochemistry, Genetics and Molecular Biology; General Chemistry; Multidisciplinary
Abstract :
[en] The charge-transport properties of conjugated polymers have been studied extensively for opto-electronic device applications. Some polymer semiconductors not only support the ambipolar transport of electrons and holes, but do so with comparable carrier mobilities. This opens the possibility of gaining deeper insight into the charge-transport physics of these complex materials via comparison between electron and hole dynamics while keeping other factors, such as polymer microstructure, equal. Here, we use field-induced electron spin resonance spectroscopy to compare the spin relaxation behavior of electron and hole polarons in three ambipolar conjugated polymers. Our experiments show unique relaxation regimes as a function of temperature for electrons and holes, whereby at lower temperatures electrons relax slower than holes, but at higher temperatures, in the so-called spin-shuttling regime, the trend is reversed. On the basis of theoretical simulations, we attribute this to differences in the delocalization of electron and hole wavefunctions and show that spin relaxation in the spin shuttling regimes provides a sensitive probe of the intimate coupling between charge and structural dynamics.
Disciplines :
Chemistry
Author, co-author :
Carey, Remington L; Cavendish Laboratory, University of Cambridge, Cambridge, CB3 0HE, UK
Giannini, Samuele ; Université de Mons - UMONS > Faculté des Sciences > Service de Chimie des matériaux nouveaux ; Institute of Chemistry of OrganoMetallic Compounds, National Research Council (ICCOM-CNR), I-56124, Pisa, Italy
Schott, Sam; Cavendish Laboratory, University of Cambridge, Cambridge, CB3 0HE, UK
LEMAUR, Vincent ; Université de Mons - UMONS > Faculté des Science > Service de Chimie des matériaux nouveaux
Xiao, Mingfei; Cavendish Laboratory, University of Cambridge, Cambridge, CB3 0HE, UK
Prodhan, Suryoday ; Université de Mons - UMONS > Faculté des Sciences > Service de Chimie des matériaux nouveaux ; Department of Chemistry, University of Liverpool, Liverpool, L69 3BX, UK
Wang, Linjun ; Université de Mons - UMONS > Faculté des Sciences > Chimie des matériaux nouveaux ; Key Laboratory of Excited-State Materials of Zhejiang Province, Department of Chemistry, Zhejiang University, Hangzhou, 310058, China
Bovoloni, Michelangelo ; Université de Mons - UMONS > Faculté des Sciences > Service de Chimie des matériaux nouveaux
Quarti, Claudio ; Université de Mons - UMONS > Faculté des Science > Service de Chimie des matériaux nouveaux
Beljonne, David ; Université de Mons - UMONS > Faculté des Science > Service de Chimie des matériaux nouveaux
Sirringhaus, Henning ; Cavendish Laboratory, University of Cambridge, Cambridge, CB3 0HE, UK. hs220@cam.ac.uk
Language :
English
Title :
Spin relaxation of electron and hole polarons in ambipolar conjugated polymers.
Research Institute for Materials Science and Engineering
Funding text :
We acknowledge funding from the European Research Council through a Synergy grant (610115). H.S. also acknowledges support by a Royal Society Research Professorship (RP⧹R1⧹201082) and an ERC Advanced grant (101020872). The work in Mons received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No. 964677, the Consortium des Équipements de Calcul Intensif (CÉCI), funded by the Fonds National de la Recherche Scientifique (F.R.S.-FNRS) under Grant No. 2.5020.11 as well as the Tier-1 supercomputer of the Fédération Wallonie-Bruxelles, infrastructure funded by the Walloon Region under Grant Agreement n1117545, and F.R.S.-FNRS. S.G. is Chargé de recherches FNRS, C.Q. is FNRS research associate and D.B. is FNRS Research Director. L.W. acknowledges support from the National Natural Science Foundation of China (Grant No. 22273082). S.P. acknowledges financial support from the European Research Council (Grant No. 101020369).We acknowledge funding from the European Research Council through a Synergy grant (610115). H.S. also acknowledges support by a Royal Society Research Professorship (RP⧹R1⧹201082) and an ERC Advanced grant (101020872). The work in Mons received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No. 964677, the Consortium des Équipements de Calcul Intensif (CÉCI), funded by the Fonds National de la Recherche Scientifique (F.R.S.-FNRS) under Grant No. 2.5020.11 as well as the Tier-1 supercomputer of the Fédération Wallonie-Bruxelles, infrastructure funded by the Walloon Region under Grant Agreement n1117545, and F.R.S.-FNRS. S.G. is Chargé de recherches FNRS, C.Q. is FNRS research associate and D.B. is FNRS Research Director. L.W. acknowledges support from the National Natural Science Foundation of China (Grant No. 22273082). S.P. acknowledges financial support from the European Research Council (Grant No. 101020369).
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