Spectral diffusion of single molecules in a hierarchical energy landscape

Stefan Krause*, Danny Kowerko, Richard Börner, Christian G. Hübner, Christian Von Borczyskowski

*Corresponding author for this work
18 Citations (Scopus)


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.

Original languageEnglish
Issue number2
Pages (from-to)303-312
Number of pages10
Publication statusPublished - 07.02.2011


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