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Vibrational coherence probes the mechanism of ultrafast electron transfer in polymer-fullerene blends.

Authors
  • Song, Yin
  • Clafton, Scott N
  • Pensack, Ryan D
  • Kee, Tak W
  • Scholes, Gregory D
Type
Published Article
Journal
Nature Communications
Publisher
Springer Nature
Publication Date
Jan 01, 2014
Volume
5
Pages
4933–4933
Identifiers
DOI: 10.1038/ncomms5933
PMID: 25215959
Source
Medline
License
Unknown

Abstract

The conversion of photoexcitations into charge carriers in organic solar cells is facilitated by the dissociation of excitons at the donor/acceptor interface. The ultrafast timescale of charge separation demands sophisticated theoretical models and raises questions about the role of coherence in the charge-transfer mechanism. Here, we apply two-dimensional electronic spectroscopy to study the electron transfer process in poly(3-hexylthiophene)/PCBM (P3HT/PCBM) blends. We report dynamics maps showing the pathways of charge transfer that clearly expose the significance of hot electron transfer. During this ultrafast electron transfer, vibrational coherence is directly transferred from the P3HT exciton to the P3HT hole polaron in the crystalline domain. This result reveals that the exciton converts to a hole with a similar spatial extent on a timescale far exceeding other photophysical dynamics including vibrational relaxation.

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