Fluorescence intermittency originates from reclustering in two-dimensional organic semiconductors

Anthony Ruth, Michitoshi Hayashi, Peter Zapol, Jixin Si, Matthew P. McDonald, Yurii V. Morozov, Masaru Kuno and Boldizsár Jankó ()
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Anthony Ruth: University of Notre Dame
Michitoshi Hayashi: National Taiwan University, Center for Condensed Matter Sciences, National Taiwan University,
Peter Zapol: Argonne National Laboratory
Jixin Si: University of Notre Dame
Matthew P. McDonald: Max Planck Institute for the Science of Light
Yurii V. Morozov: University of Notre Dame
Masaru Kuno: University of Notre Dame
Boldizsár Jankó: University of Notre Dame

Nature Communications, 2017, vol. 8, issue 1, 1-7

Abstract: Abstract 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 sp2 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.

Date: 2017
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DOI: 10.1038/ncomms14521

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