Vibronic and Vibrational Coherences in Two-Dimensional Electronic Spectra of Supramolecular J-Aggregates

摘要: 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 an in-depth spectroscopic analysis the underlying deactivation network coherence dynamics. We use two-dimensional electronic spectroscopy sub-10 fs laser pulses in combination decay-associated spectra to describe population flow within aggregate. Based on Fourier-transform amplitude maps, we distinguish between vibrational or vibronic dynamics as origin pronounced oscillations our spectra.