Abstract
AbstractThe 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.
Authors
12
- Antonietta De Sio (first)
- Filippo Troiani (additional)
- Margherita Maiuri (additional)
- Julien Réhault (additional)
- Ephraim Sommer (additional)
- James Lim (additional)
- Susana F. Huelga (additional)
- Martin B. Plenio (additional)
- Carlo Andrea Rozzi (additional)
- Giulio Cerullo (additional)
- Elisa Molinari (additional)
- Christoph Lienau (additional)
References
58
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Dates
Type | When |
---|---|
Created | 8 years, 8 months ago (Dec. 8, 2016, 5:09 a.m.) |
Deposited | 2 years, 7 months ago (Jan. 4, 2023, 4:31 a.m.) |
Indexed | 1 week, 2 days ago (Aug. 21, 2025, 1:58 p.m.) |
Issued | 8 years, 8 months ago (Dec. 8, 2016) |
Published | 8 years, 8 months ago (Dec. 8, 2016) |
Published Online | 8 years, 8 months ago (Dec. 8, 2016) |
@article{De_Sio_2016, title={Tracking the coherent generation of polaron pairs in conjugated polymers}, volume={7}, ISSN={2041-1723}, url={http://dx.doi.org/10.1038/ncomms13742}, DOI={10.1038/ncomms13742}, number={1}, journal={Nature Communications}, publisher={Springer Science and Business Media LLC}, author={De Sio, Antonietta and Troiani, Filippo and Maiuri, Margherita and Réhault, Julien and Sommer, Ephraim and Lim, James and Huelga, Susana F. and Plenio, Martin B. and Rozzi, Carlo Andrea and Cerullo, Giulio and Molinari, Elisa and Lienau, Christoph}, year={2016}, month=dec }