Dispersive kinetics from single molecules oriented in single crystals of potassium acid phthalate

Kristin L. Wustholz, Eric D. Bott, Christine M. Isborn, Xiaosong Li, Bart Kahr, Philip J. Reid

Research output: Contribution to journalArticle

Abstract

The intermittent emission or "blinking" of single violamine R (1) and 2',7'-dichlorofluorescein (2) molecules incorporated into single crystals of potassium acid phthalate (KAP) is studied using confocal fluorescence microscopy. Blinking dynamics are quantified in terms of switching rates and on- and off-length probability distributions. Mixed crystals of KAP/1 and KAP/2 consist of photophysical subpopulations with ∼40% and ∼20% exhibiting persistent emission, respectively, and the remainder demonstrating a broad range of blinking behavior that is well described by a power-law distribution. The dependence of the power-law exponent on chromophore, experimental bin time, intensity threshold, and excitation power is examined. The blinking dynamics are also modeled using Monte Carlo simulations on the basis of a three-level electronic system with the rate constants for population and depopulation of the "dark" state being distributed. No correlation between molecular orientation and blinking dynamics is observed, suggesting that intermolecular electron transfer is not the origin of power-law behavior. Alternative origins for this behavior (e.g., conformational flexibility and spectral diffusion) are explored using a combination of experimental and computational techniques. Of these possibilities, the distributed kinetics exhibited by KAP/1 and KAP/2 are attributed to spectral diffusion.

Original languageEnglish (US)
Pages (from-to)9146-9156
Number of pages11
JournalJournal of Physical Chemistry C
Volume111
Issue number26
DOIs
StatePublished - Jul 5 2007

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blinking
phthalates
Potassium
potassium
Single crystals
acids
Molecules
Kinetics
Acids
single crystals
kinetics
molecules
Molecular orientation
Confocal microscopy
Fluorescence microscopy
Bins
Chromophores
Probability distributions
Rate constants
electronic levels

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Electronic, Optical and Magnetic Materials
  • Surfaces, Coatings and Films
  • Energy(all)

Cite this

Dispersive kinetics from single molecules oriented in single crystals of potassium acid phthalate. / Wustholz, Kristin L.; Bott, Eric D.; Isborn, Christine M.; Li, Xiaosong; Kahr, Bart; Reid, Philip J.

In: Journal of Physical Chemistry C, Vol. 111, No. 26, 05.07.2007, p. 9146-9156.

Research output: Contribution to journalArticle

Wustholz, Kristin L. ; Bott, Eric D. ; Isborn, Christine M. ; Li, Xiaosong ; Kahr, Bart ; Reid, Philip J. / Dispersive kinetics from single molecules oriented in single crystals of potassium acid phthalate. In: Journal of Physical Chemistry C. 2007 ; Vol. 111, No. 26. pp. 9146-9156.
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