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Cited by 197

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Tracking the coherent generation of polaron pairs in conjugated polymers

Open access
De Sio, Antonietta, Troiani, Filippo, Maiuri, Margherita, Réhault, Julien, Sommer, Ephraim, Lim, James, Huelga, Susana F., Plenio, Martin B., Rozzi, Carlo Andrea, Cerullo, Giulio, Molinari, Elisa, Lienau, Christoph·2016·Nature Communications

Abstract

The optical excitation of organic semiconductors not only generates charge-neutral electron-hole pairs (excitons), but also charge-separated polaron pairs with high yield. The microscopic mechanisms underlying this charge separation have been debated for many years. Here we use ultrafast two-dimensional electronic spectroscopy to study the dynamics of polaron pair formation in a prototypical polymer thin film on a sub-20-fs time scale. We observe multi-period peak oscillations persisting for up to about 1 ps as distinct signatures of vibronic quantum coherence at room temperature. The measured two-dimensional spectra show pronounced peak splittings revealing that the elementary optical excitations of this polymer are hybridized exciton-polaron-pairs, strongly coupled to a dominant underdamped vibrational mode. Coherent vibronic coupling induces ultrafast polaron pair formation, accelerates the charge separation dynamics and makes it insensitive to disorder. These findings open up new perspectives for tailoring light-to-current conversion in organic materials.

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Metadata

Authors
De Sio, A., Troiani, F., Maiuri, M., Réhault, J., Sommer, E., Lim, J., Huelga, S. F., Plenio, M. B., Rozzi, C. A., Cerullo, G., Molinari, E., & Lienau, C.
Venue
Nature Communications
Published
2016-12-08
Volume
7
Issue
1
Pages
13742-13742
ISSN
2041-1723 (ISSN-L)
OpenAlex
W2543110117
Cited by
197
References
7
FWCI
8.23
Type
journal article
Language
en
Open access
gold

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CoChat. (2026). Citation check: Tracking the coherent generation of polaron pairs in conjugated polymers. https://app.cochat.ai/papers/10.1038/ncomms13742
The paper
De Sio, A., Troiani, F., Maiuri, M., Réhault, J., Sommer, E., Lim, J., Huelga, S. F., Plenio, M. B., Rozzi, C. A., Cerullo, G., Molinari, E., & Lienau, C. (2016). Tracking the coherent generation of polaron pairs in conjugated polymers. Nature Communications. https://doi.org/10.1038/ncomms13742

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