Proton-transfer mechanism for dispersed decay kinetics of single molecules isolated in potassium hydrogen phthalate

Eric D. Bott, Erin A. Riley, Bart Kahr, Philip J. Reid

Research output: Contribution to journalArticle

Abstract

The excited-state decay kinetics of single 2′, 7′- dichlorofluorescein (DCF) molecules oriented and overgrown within crystals of potassium acid phthalate (KAP) are reported. Time-correlated single-photon counting measurements (TCSPC) of 56 DCF molecules in KAP reveal that single-exponential decay is exhibited by roughly half of the molecules. The remainder demonstrates complex excited-state decay kinetics that are well fit by a stretched exponential function consistent with dispersed kinetics. Histograms of single-molecule luminescence energies revealed environmental fluctuations and distinct chemical species. The TCSPC results are compared to Monte Carlo simulations employing a first-passage model for excited-state decay. Agreement between experiment and theory, on both bulk and single-molecule levels, suggests that a subset of the DCF molecules in KAP experience fluctuations in the surrounding environment that modify the energy barrier to proton transfer leading to dispersed kinetics.

Original languageEnglish (US)
Pages (from-to)2403-2411
Number of pages9
JournalACS nano
Volume3
Issue number8
DOIs
StatePublished - Aug 25 2009

Keywords

  • Dispersed kinetics
  • Fluorescence intermittency
  • Fluorescence lifetime
  • Proton transfer
  • Single molecule microscopy

ASJC Scopus subject areas

  • Materials Science(all)
  • Engineering(all)
  • Physics and Astronomy(all)

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