Spectral Diffusion of Single Molecules in a Hierarchical Energy Landscape Journalartikel uri icon



  • Spectral diffusion as a result of both the transitions between different molecular conformers and the ′′molecular softness′′ of quasi-free perylene diimides on a SiO2 surface is investigated by means of single-molecule spectroscopy, which reveals the time dependence of both the fluorescence spectra and the three-dimensional orientation. Spectral wavelengths of all single emitters cover a wide energy range of about 0.27 eV, which is due to different types of conformers with large differences in optical transition energy. Time-dependent spectral trajectories of single emitters within this wavelength manifold are evaluated with a model transcribed from the analysis of spatial diffusion. Spectral diffusion processes are closely correlated with fluorescence emission and excitation power. The overall analysis of spectral diffusion reveals, similar to proteins, a hierarchy of energy barriers in a broad energy landscape.


  • Krause, Stefan
  • Kowerko, Danny
  • Börner, Richard
  • Hübner, Christian G.
  • von Borczyskowski, Christian


  • 2011


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  • 303

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