Vibronic and vibrational coherences in two-dimensional electronic spectra of supramolecular J-aggregates

J Phys Chem A. 2013 Jul 25;117(29):6007-14. doi: 10.1021/jp3119605. Epub 2013 Mar 18.

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.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Carbocyanines / chemistry
  • Coloring Agents / chemistry
  • Electrons*
  • Entropy
  • Fourier Analysis
  • Models, Molecular
  • Molecular Conformation
  • Polymers / chemistry
  • Spectrum Analysis*
  • Vibration*
  • Water / chemistry

Substances

  • Carbocyanines
  • Coloring Agents
  • Polymers
  • Water