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Vallée RA, Van der Auweraer M, Paul W, et al. Fluorescence lifetime of a single molecule as an observable of meta-basin dynamics in fluids near the glass transition. Phys Rev Lett. 2006;97(21):217801doi: 10.1103/PhysRevLett.97.217801.
Vallée, R. A., Van der Auweraer, M., Paul, W., & Binder, K. (2006). Fluorescence lifetime of a single molecule as an observable of meta-basin dynamics in fluids near the glass transition. Physical review letters, 97(21), 217801. https://doi.org/10.1103/PhysRevLett.97.217801
Vallée, R A L, et al. "Fluorescence lifetime of a single molecule as an observable of meta-basin dynamics in fluids near the glass transition." Physical review letters vol. 97,21 (2006): 217801. doi: https://doi.org/10.1103/PhysRevLett.97.217801
Vallée RA, Van der Auweraer M, Paul W, Binder K. Fluorescence lifetime of a single molecule as an observable of meta-basin dynamics in fluids near the glass transition. Phys Rev Lett. 2006 Nov 24;97(21):217801. doi: 10.1103/PhysRevLett.97.217801. Epub 2006 Nov 22. PMID: 17155773.
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Phys Rev Lett. 2006 Nov 24;97(21):217801. doi: 10.1103/PhysRevLett.97.217801. Epub 2006 Nov 22.

Fluorescence lifetime of a single molecule as an observable of meta-basin dynamics in fluids near the glass transition.

Physical review letters

R A L Vallée, M Van der Auweraer, W Paul, K Binder

Affiliations

  1. Department of Chemistry and Institute of Nanoscale Physics and Chemistry (INPAC), Katholieke Universiteit Leuven, Heverlee, Belgium. [email protected]

PMID: 17155773 DOI: 10.1103/PhysRevLett.97.217801

Abstract

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.

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