6533b85efe1ef96bd12c097f
RESEARCH PRODUCT
Fluorescence Lifetime of a Single Molecule as an Observable of Meta-Basin Dynamics in Fluids Near the Glass Transition
Kurt BinderWolfgang PaulRenaud A. L. ValléeM. Van Der Auweraersubject
Molecular dynamicsNuclear magnetic resonanceMaterials scienceResonance fluorescenceChemical physicsRelaxation (NMR)General Physics and AstronomyMoleculeFluorescence cross-correlation spectroscopyObservableLaser-induced fluorescenceFluorescence spectroscopydescription
Using single molecule spectroscopy, we show that the fluorescence lifetime trajectories of single probe molecules embedded in a glass-forming polymer melt exhibit strong fluctuations of a hopping character. Using molecular dynamics simulations targeted to explain these experimental observations, we show that the lifetime fluctuations correlate strongly with the average square displacement function of the matrix particles. The latter observable is a direct probe of the meta-basin transitions in the potential energy landscape of glass-forming liquids. We thus show here that single molecule experiments can provide detailed microscopic information on system properties that hitherto have been accessible via computer simulations only.
| year | journal | country | edition | language |
|---|---|---|---|---|
| 2006-11-22 | Physical Review Letters |