Power-law blinking in the fluorescence of single organic molecules.
The blinking behavior of perylene diïmide molecules is investigated at the single-molecule level. We observe long-time scale blinking of individual multi-chromophoric complexes embedded in a poly(methylmethacrylate) matrix, as well as for the monomeric dye absorbed on a glass substrate at ambient conditions. In both these different systems, the blinking of single molecules is found to obey analogous power-law statistics for both the on and off periods. The observed range for single-molecular power-law blinking extends over the full experimental time window, covering four orders of magnitude in time and six orders of magnitude in probability density. From molecule to molecule, we observe a large spread in off-time power-law exponents. The distributions of off-exponents in both systems are markedly different whereas both on-exponent distributions appear similar. Our results are consistent with models that ascribe the power-law behavior to charge separation and (environment-dependent) recombination by electron tunneling to a dynamic distribution of charge acceptors. As a consequence of power-law statistics, single molecule properties like the total number of emitted photons display non-ergodicity.
Hoogenboom
Jacob P
JP
Applied Optics Group, Faculty of Science and Technology and MESA+ Institute for Nanotechnology, University of Twente, P.O. Box 217, 7500AE Enschede, The Netherlands. jacob.hoogenboom@icfo.es
Hernando
Jordi
J
van Dijk
Erik M H P
EM
van Hulst
Niek F
NF
García-Parajó
Maria F
MF
D005456:Fluorescent Dyes / Q000032:analysis* / Q000737:chemistry; D007094:Imides / Q000032:analysis* / Q000737:chemistry; D008958:Models, Molecular; D015233:Models, Statistical; D015394:Molecular Structure; D010569:Perylene / Q000031:analogs & derivatives* / Q000032:analysis / Q000737:chemistry; D017785:Photons; D012235:Rhodamines / Q000737:chemistry; D013050:Spectrometry, Fluorescence / Q000379:methods* / Q000706:statistics & numerical data; D016008:Statistical Distributions; D013997:Time Factors
D005456:Fluorescent Dyes; D007094:Imides; D012235:Rhodamines; C510697:perylene bisimide; C026188:rhodamine 6G; D010569:Perylene