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Lookup NU author(s): Emeritus Professor Anthony Harriman
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© 2021 American Chemical Society. All rights reserved.Light-induced blinking, an inherent feature of many forms of super-resolution microscopy, has been linked to transient reduction of the fluorescent cyanine dye used as an imaging agent. There is, however, only scant literature information related to one-electron reduced cyanine dyes, especially in an aqueous environment. Here, we examine a small series of cyanine dyes, possessing disparate π-conjugation lengths, under selective reducing or oxidizing conditions. The experiment allows recording of both differential absorption spectra and decay kinetics of the resultant one-electron reduced or oxidized transient species in water. Relative to the ground state, absorption transitions for the various radicals are weak and somewhat broadened but do allow correlation with the π-conjugation length. In all cases, absorption maxima lie to the blue of the main ground-state transition. Under anaerobic conditions, the transient species decay on the microsecond to millisecond time scale, with the mean lifetime depending on molecular structure, radiation dose, and dye concentration. The experimental absorption spectra recorded for the one-electron reduced radicals and the presumed dimer cation radical compare well to spectra obtained from time-dependent density functional theory calculations. The results allow conclusions to be drawn regarding the plausibility of the reduced species being responsible for light-induced blinking in direct stochastic optical reconstruction microscopy.
Author(s): Lisovskaya A, Carmichael I, Harriman A
Publication type: Article
Publication status: Published
Journal: Journal of Physical Chemistry A
Print publication date: 08/07/2021
Online publication date: 24/06/2021
Acceptance date: 08/06/2021
ISSN (print): 1089-5639
ISSN (electronic): 1520-5215
Publisher: American Chemical Society
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