Spin relaxation of electron and hole polarons in ambipolar conjugated polymers

Remington L. Carey, Samuele Giannini, Sam Schott, Vincent Lemaur, Mingfei Xiao, Suryoday Prodhan, Linjun Wang, Michelangelo Bovoloni, Claudio Quarti, David Beljonne and Henning Sirringhaus ()
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Remington L. Carey: University of Cambridge
Samuele Giannini: University of Mons
Sam Schott: University of Cambridge
Vincent Lemaur: University of Mons
Mingfei Xiao: University of Cambridge
Suryoday Prodhan: University of Liverpool
Linjun Wang: Zhejiang University
Michelangelo Bovoloni: University of Mons
Claudio Quarti: University of Mons
David Beljonne: University of Mons
Henning Sirringhaus: University of Cambridge

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-023-43505-7

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