Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 7, Issue 24, Pages 4996-5001Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.6b02433
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Funding
- ERC Starting Grant QUENTRHEL [278560]
- FP7 EU STREP project PAPETS [323901]
- Marie Curie Individual Fellowships FP7-PEOPLE-IEF project QUANTUM VIBES [629254]
- European Research Council (ERC) [278560] Funding Source: European Research Council (ERC)
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The intraband exciton dynamics of molecular aggregates is a crucial initial step to determine the possibly coherent nature of energy transfer and its implications for the ensuing interband relaxation pathways in strongly coupled excitonic systems. In this work, we fully characterize the intraband dynamics in linear J-aggregates of porphyrins, good model systems for multichromophoric assemblies in biological antenna complexes. Using different 2D electronic spectroscopy schemes together with Raman spectroscopy and theoretical modeling, we provide a full characterization of the inner structure of the main one-exciton band of the porphyrin aggregates. We find that the redistribution of population within the band occurs with a characteristic time of 280 fs and dominates the modulation of an electronic coherence. While we do not find that the coupling to vibrations significantly affects the dynamics of excitonic coherence, our results suggest that exciton fluctuations are nevertheless highly correlated.
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