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Cited by 278Photochemistry and Electron Transfer StudiesAdvanced Fluorescence Microscopy TechniquesLuminescence and Fluorescent Materials

Photoblinking of Rhodamine 6G in Poly(vinyl alcohol): Radical Dark State Formed through the Triplet

Zondervan, Rob, Kulzer, Florian, Orlinskii, Sergei B., Orrit, Michel·2003·The Journal of Physical Chemistry A
DOI 10.1021/jp034723r
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Abstract

We investigate the fluorescence intensity of rhodamine 6G in poly(vinyl alcohol) as a function of excitation intensity, illumination time, the presence of oxygen, and temperature. The variations in emissivity (or fluorescence brightness) are attributed to a dark state, which shows populating kinetics resembling those of the triplet state, but a much longer lifetime. We simulate the observed kinetics by a four-level model, in which a long-lived dark state is formed through the triplet as an intermediate state. The weak temperature dependence of the lifetime of the dark state points to electron tunneling as the main recovery process. This intermolecular mechanism also explains the observed broad distribution of lifetimes. An electron-spin-resonance experiment confirms the assignment of the dark state to a radical. For the first time, photoinduced charge transfer is identified as a source of blinking in single-molecule measurements.

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Crossref · 10.1021/jp034723r

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  • The complexity and flexibility of the environment at room temperature allows the existence of metastable dark states, leading to extended dark periods, during which emission stops.

    “Furthermore, the complexity and flexibility of the environment at room temperature allows the existence of metastable dark states, leading to extended dark periods, during which emission stops (Zondervan et al 2003(Zondervan et al , 2004)).”

    From Single-photon sources (2005) · cites this paper as Zondervan et al 2003

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Authors
Zondervan, R., Kulzer, F., Orlinskii, S. B., & Orrit, M.
Affiliations
  • Leiden University (NL)
  • Molecular Nano-Optics and Spins (MoNOS), Leiden Institute of Physics (LION), Huygens Laboratory, Leiden University, P.O. Box 9504, 2300 RA Leiden, The Netherlands
Corresponding author
Orrit, Michel
ORCID
Venue
The Journal of Physical Chemistry A
Publisher
American Chemical Society (ACS)
Published
2003-08-06
Volume
107
Issue
35
Pages
6770-6776
ISSN
  • 1089-5639 (ISSN-L)
  • 1520-5215
DOI
10.1021/jp034723r
OpenAlex
W2029370337
Cited by
278
References
44
Citations by year
2026: 3 · 2025: 4 · 2024: 5 · 2023: 7 · 2022: 8 · 2021: 7 · 2020: 6 · 2019: 8 · 2018: 8 · 2017: 10 · 2016: 11 · 2015: 15 · 2014: 15 · 2013: 13 · 2012: 20
FWCI
11.01
Type
journal article
Language
en
Open access
closed
Locations
The Journal of Physical Chemistry A (publishedVersion)
Topics
  • Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
  • Life Sciences › Biochemistry, Genetics and Molecular Biology › Biophysics › Advanced Fluorescence Microscopy Techniques
  • Physical Sciences › Materials Science › Materials Chemistry › Luminescence and Fluorescent Materials
Keywords
photoblinking, rhodamine 6G, polyvinyl alcohol, dark states, triplet state, electron tunneling, photoinduced charge transfer, fluorescence lifetime, four-level model, single-molecule fluorescence, electron spin resonance

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