Journal
CHEMPHYSCHEM
Volume 12, Issue 2, Pages 303-312Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201000678
Keywords
conformation analysis; fluorescence spectroscopy; molecular dynamics; photophysics; single-molecule studies
Funding
- German Science Foundation within the research unit [FOR 877]
- VW foundation in the priority area Physics, Chemistry and Biology with Single Molecules
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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.
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