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Related Experiment Videos

Nonclassical photon statistics in single-molecule fluorescence at room temperature

Fleury1, Segura, Zumofen

  • 1Physical Chemistry Laboratory, Swiss Federal Institute of Technology, ETH-Z, CH-8092 Zurich, Switzerland.

Physical Review Letters
|October 4, 2000
PubMed
Summary

Single terrylene molecules exhibit unique fluorescence patterns, showing photon antibunching and bunching. This reveals insights into molecular dynamics and accelerated reverse intersystem crossing in crystalline hosts.

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Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics·2000

Area of Science:

  • Single-molecule spectroscopy
  • Photophysics of organic molecules
  • Condensed matter optics

Background:

  • Understanding molecular photophysics is crucial for developing advanced optical materials and quantum technologies.
  • Single-molecule fluorescence provides a powerful tool to probe complex systems beyond ensemble averages.
  • Terrylene molecules are known for their stable fluorescence, making them suitable for optical studies.

Purpose of the Study:

  • To investigate the fluorescence dynamics of single terrylene molecules in a crystalline environment at room temperature.
  • To analyze photon statistics and correlations to understand underlying photophysical processes.
  • To elucidate the role of intersystem crossing in the observed fluorescence behavior.

Main Methods:

  • Scanning confocal optical microscopy was employed to isolate and measure single terrylene molecules.

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  • Photon arrival times were analyzed using interphoton time distributions and second-order correlation functions (g(2)(τ)).
  • The variance of the photon number probability distribution was calculated to characterize photon statistics.

    • Main Results:

    • Observed photon antibunching at short times, indicative of single-photon emission.
    • Observed photon bunching at longer times, suggesting multi-photon processes or blinking.
    • Sub-Poissonian and super-Poissonian statistics were identified, correlating with antibunching and bunching, respectively.
    • Rate-equation analysis indicated an accelerated reverse intersystem crossing (RISC) pathway.

    Conclusions:

    • Single terrylene molecules display complex fluorescence dynamics influenced by intersystem crossing.
    • The observed photon statistics provide direct evidence for distinct photophysical pathways.
    • Accelerated RISC significantly impacts the fluorescence emission and photon statistics of terrylene molecules in crystalline hosts.