Heterogeneity in the fluorescence of graphene and graphene oxide quantum dots

Abstract

Heterogeneity is an inherent property of a wealth of real-world nanomaterials and yet rarely in the reporting of new properties is its effect sufficiently addressed. Graphene quantum dots (GQDs) – fluorescent, nanoscale fragments of graphene - are an extreme example of a heterogeneous nanomaterial. Here, top-down approaches – by far the most predominant – produce batches of particles with a distribution of sizes, shapes, extent of oxidation, chemical impurities and more. This makes characterization of these materials using bulk techniques particularly complex and comparisons of properties across different synthetic methods uninformative. In particular, it hinders the understanding of the structural origin of their fluorescence properties. We present a simple synthetic method, which produces graphene quantum dots with very low oxygen content that can be suspended in organic solvents, suggesting a very pristine material. We use this material to illustrate the limitations of interpreting complex data sets generated by heterogeneous materials and we highlight how misleading this “pristine” interpretation is by comparison with graphene oxide quantum dots synthesized using an established protocol. In addition, we report on the solvatochromic properties of these particles, discuss common characterization techniques and their limitations in attributing properties to heterogeneous materials.

Graphene quantum dots with very low oxygen content were synthesized using a simple method, suggesting a very pristine material. We highlight how misleading this “pristine” term is when applied to a heterogeneous material through comparison with graphene oxide quantum dots.

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Acknowledgment

We would like to acknowledge the work of Anne Wendel, Marek Josianiak and Chris Bassel, who helped us with the XPS measurements as well as the VUW Raman group – specifically Baptiste Auguié and Eric Le Ru for contributing their Raman expertise.

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The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript.

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Correspondence to Thomas Nann.

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Bradley, S.J., Kroon, R., Laufersky, G. et al. Heterogeneity in the fluorescence of graphene and graphene oxide quantum dots. Microchim Acta 184, 871–878 (2017). https://doi.org/10.1007/s00604-017-2075-9

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Keywords

  • Graphene quantum dots
  • Quantum yield
  • Fluorescence lifetime
  • Photoluminescence
  • Characterization
  • TEM
  • NMR
  • Raman spectroscopy