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Fluorescence intermittency originates from reclustering in two-dimensional organic semiconductors

MPG-Autoren
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McDonald,  Matthew P.
Sandoghdar Division, Max Planck Institute for the Science of Light, Max Planck Society;

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Zitation

Ruth, A., Hayashi, M., Zapol, P., Si, J., McDonald, M. P., Morozov, Y. V., et al. (2017). Fluorescence intermittency originates from reclustering in two-dimensional organic semiconductors. NATURE COMMUNICATIONS, 8: 14521. doi:10.1038/ncomms14521.


Zitierlink: https://hdl.handle.net/21.11116/0000-0000-8039-F
Zusammenfassung
Fluorescence intermittency or blinking is observed in nearly all nanoscale fluorophores. It is characterized by universal power-law distributions in on- and off-times as well as 1/f behaviour in corresponding emission power spectral densities. Blinking, previously seen in confined zero- and one-dimensional systems has recently been documented in two-dimensional reduced graphene oxide. Here we show that unexpected blinking during graphene oxide-to-reduced graphene oxide photoreduction is attributed, in large part, to the redistribution of carbon sp(2) domains. This reclustering generates fluctuations in the number/size of emissive graphenic nanoclusters wherein multiscale modelling captures essential experimental aspects of reduced graphene oxide's absorption/emission trajectories, while simultaneously connecting them to the underlying photochemistry responsible for graphene oxide's reduction. These simulations thus establish causality between currently unexplained, long timescale emission intermittency in a quantum mechanical fluorophore and identifiable chemical reactions that ultimately lead to switching between on and off states.