Journal
NATURE COMMUNICATIONS
Volume 6, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms8755
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Funding
- Austrian Science Fund (FWF): START project [Y 631-N27]
- COST Action [CM1202-PERSPECT-H2O]
- EU STREP PAPETS
- ERC Synergy Grant BioQ
- Deutsche Forschungsgemeinschaft (DFG) [SFB/TRR21]
- Alexander von Humboldt Professorship
- Spanish Ministerio de Economia y Competitividad [FIS2012-30625]
- Swedish Research Council
- Knut and Alice Wallenberg Foundation
- EU QUCHIP
- Austrian Science Fund (FWF) [Y631] Funding Source: Austrian Science Fund (FWF)
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Natural and artificial light-harvesting processes have recently gained new interest. Signatures of long-lasting coherence in spectroscopic signals of biological systems have been repeatedly observed, albeit their origin is a matter of ongoing debate, as it is unclear how the loss of coherence due to interaction with the noisy environments in such systems is averted. Here we report experimental and theoretical verification of coherent exciton-vibrational (vibronic) coupling as the origin of long-lasting coherence in an artificial light harvester, a molecular J-aggregate. In this macroscopically aligned tubular system, polarization-controlled 2D spectroscopy delivers an uncongested and specific optical response as an ideal foundation for an in-depth theoretical description. We derive analytical expressions that show under which general conditions vibronic coupling leads to prolonged excited-state coherence.
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