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Observation and Analysis of Blinking Surface-enhanced Raman Scattering
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Single molecule power-law behavior on a crystalline surface.

Laura K Schirra1, Brandon S Tackett, Michael L Blumenfeld

  • 1Department of Chemistry, The University of Arizona, 1306 E. University Blvd., Tucson, Arizona 85721, USA.

The Journal of Chemical Physics
|October 2, 2009
PubMed
Summary

Single perylene bisimide molecules on aluminum oxide exhibit fluorescence intermittency due to interfacial charge transfer. This behavior, observed on a crystalline surface, is explained by polaron formation, offering insights into single-molecule surface interactions.

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Area of Science:

  • Surface science
  • Single-molecule spectroscopy
  • Organic electronics

Background:

  • Fluorescence intermittency is a known phenomenon in single molecules.
  • Interfacial charge transfer is crucial for organic electronic devices.
  • Understanding molecular behavior on crystalline surfaces is key for device optimization.

Purpose of the Study:

  • To investigate fluorescence intermittency of single perylene bisimide molecules on Al(2)O(3) (0001).
  • To elucidate the underlying mechanism of interfacial charge transfer.
  • To develop a kinetic model for observed intermittency patterns.

Main Methods:

  • Deposition of single perylene bisimide molecules onto Al(2)O(3) (0001) surface.
  • Investigation under controlled ultrahigh vacuum conditions.
  • Analysis of fluorescence intermittency and power-law distributions.

Main Results:

  • Observed fluorescence intermittency (blinking) in single perylene bisimide molecules.
  • Identified power-law distributions for bright and dark periods.
  • Attributed the behavior to activated formation of small polaron states in Al(2)O(3).

Conclusions:

  • The study provides a kinetic scheme explaining single-molecule fluorescence intermittency on crystalline surfaces.
  • Findings offer a fundamental understanding of interfacial charge transfer at the single-molecule level.
  • This work is a step towards controlling molecular behavior on well-defined surfaces for applications.