Vibronic and vibrational coherences in two-dimensional electronic spectra of supramolecular J-aggregates
Franz Milota1, Valentyn I Prokhorenko, Tomas Mancal
1Photonics Institute, Vienna University of Technology, Gusshausstrasse 27, 1040 Vienna, Austria.
Abstract:
In J-aggregates of cyanine dyes, closely packed molecules form mesoscopic tubes with nanometer-diameter and micrometer-length. Their efficient energy transfer pathways make them suitable candidates for artificial light harvesting systems. This great potential calls for an in-depth spectroscopic analysis of the underlying energy deactivation network and coherence dynamics. We use two-dimensional electronic spectroscopy with sub-10 fs laser pulses in combination with two-dimensional decay-associated spectra analysis to describe the population flow within the aggregate. Based on the analysis of Fourier-transform amplitude maps, we distinguish between vibrational or vibronic coherence dynamics as the origin of pronounced oscillations in our two-dimensional electronic spectra.
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