jz6b02433_si_001.pdf (3.73 MB)
Correlated Fluctuations and Intraband Dynamics of J‑Aggregates Revealed by Combination of 2DES Schemes
journal contribution
posted on 2016-11-22, 00:00 authored by Luca Bolzonello, Francesca Fassioli, Elisabetta ColliniThe 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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porphyrin aggregatesmodel systems280 fs2 DES SchemesRaman spectroscopyexcitonic coherenceenergy transferspectroscopy schemesone-exciton bandexcitonic systemsantenna complexesinterband relaxation pathwaysexciton fluctuationsmultichromophoric assembliesCorrelated Fluctuationsintraband exciton dynamics2 Dintraband dynamicsIntraband Dynamics
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