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Issue 5, 2011
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Two mechanisms for fluorescence intermittency of single violamine R molecules

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Abstract

The environment and temperature-dependent photoluminescence (PL) intermittency or “blinking” demonstrated by single violamine R (VR) molecules is investigated in two environments: poly(vinyl alcohol) (PVOH) and single crystals of potassium acid phthalate (KAP). In addition, temperatures ranging from 23 °C to 85 °C are studied, spanning the glass-transition temperature of PVOH (Tg = 72 °C). The PL intermittency exhibited by VR is analyzed using probability histograms of emissive and non-emissive periods. In both PVOH and KAP, these histograms are best fit by a power law, consistent with the kinetics for dark state production and decay being dispersed as observed in previous studies. However, these systems have different temperature dependences, signifying two different blinking mechanisms for VR. In PVOH, the on- and off-event probability histograms do not vary with temperature, consistent with electron transfer via tunneling between VR and the polymer. In KAP the same histograms are temperature dependent, and show that blinking slows down at higher temperatures. This result is inconsistent with an electron-transfer process being responsible for blinking. Instead, a non-adiabatic proton-transfer between VR and KAP is presented as a model consistent with this temperature dependence. In summary, the results presented here demonstrate that for a given luminophore, the photochemical processes responsible for PL intermittency can change with environment.

Graphical abstract: Two mechanisms for fluorescence intermittency of single violamine R molecules

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Publication details

The article was received on 04 Sep 2010, accepted on 04 Jan 2011 and first published on 07 Jan 2011


Article type: Paper
DOI: 10.1039/C0CP01716G
Citation: Phys. Chem. Chem. Phys., 2011,13, 1879-1887

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    Two mechanisms for fluorescence intermittency of single violamine R molecules

    E. A. Riley, C. Bingham, E. D. Bott, B. Kahr and P. J. Reid, Phys. Chem. Chem. Phys., 2011, 13, 1879
    DOI: 10.1039/C0CP01716G

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