Tracking the coherent generation of polaron pairs in conjugated polymers

Antonietta De Sio, Filippo Troiani, Margherita Maiuri, Julien Réhault, Ephraim Sommer, James Lim, Susana F. Huelga, Martin B. Plenio, Carlo Andrea Rozzi, Giulio Cerullo, Elisa Molinari and Christoph Lienau ()
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Antonietta De Sio: Institut für Physik, Carl von Ossietzky Universität
Filippo Troiani: Istituto Nanoscienze—CNR
Margherita Maiuri: IFN-CNR, Politecnico di Milano
Julien Réhault: IFN-CNR, Politecnico di Milano
Ephraim Sommer: Institut für Physik, Carl von Ossietzky Universität
James Lim: Institut für Theoretische Physik and IQST, Universität Ulm
Susana F. Huelga: Institut für Theoretische Physik and IQST, Universität Ulm
Martin B. Plenio: Institut für Theoretische Physik and IQST, Universität Ulm
Carlo Andrea Rozzi: Istituto Nanoscienze—CNR
Giulio Cerullo: IFN-CNR, Politecnico di Milano
Elisa Molinari: Istituto Nanoscienze—CNR
Christoph Lienau: Institut für Physik, Carl von Ossietzky Universität

Nature Communications, 2016, vol. 7, issue 1, 1-8

Abstract: 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.

Date: 2016
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13742

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DOI: 10.1038/ncomms13742

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