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Issue 4, 2017
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Dynamic behaviour of the silica-water-bio electrical double layer in the presence of a divalent electrolyte

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Abstract

Electronic devices are becoming increasingly used in chemical- and bio-sensing applications and therefore understanding the silica-electrolyte interface at the atomic scale is becoming increasingly important. For example, field-effect biosensors (BioFETs) operate by measuring perturbations in the electric field produced by the electrical double layer due to biomolecules binding on the surface. In this paper, explicit-solvent atomistic calculations of this electric field are presented and the structure and dynamics of the interface are investigated in different ionic strengths using molecular dynamics simulations. Novel results from simulation of the addition of DNA molecules and divalent ions are also presented, the latter of particular importance in both physiological solutions and biosensing experiments. The simulations demonstrated evidence of charge inversion, which is known to occur experimentally for divalent electrolyte systems. A strong interaction between ions and DNA phosphate groups was demonstrated in mixed electrolyte solutions, which are relevant to experimental observations of device sensitivity in the literature. The bound DNA resulted in local changes to the electric field at the surface; however, the spatial- and temporal-mean electric field showed no significant change. This result is explained by strong screening resulting from a combination of strongly polarised water and a compact layer of counterions around the DNA and silica surface. This work suggests that the saturation of the Stern layer is an important factor in determining BioFET response to increased salt concentration and provides novel insight into the interplay between ions and the EDL.

Graphical abstract: Dynamic behaviour of the silica-water-bio electrical double layer in the presence of a divalent electrolyte

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Publication details

The article was received on 13 Jun 2016, accepted on 18 Oct 2016 and first published on 19 Oct 2016


Article type: Paper
DOI: 10.1039/C6CP04101A
Citation: Phys. Chem. Chem. Phys., 2017,19, 2687-2701
  • Open access: Creative Commons BY license
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    Dynamic behaviour of the silica-water-bio electrical double layer in the presence of a divalent electrolyte

    B. M. Lowe, Y. Maekawa, Y. Shibuta, T. Sakata, C.-K. Skylaris and N. G. Green, Phys. Chem. Chem. Phys., 2017, 19, 2687
    DOI: 10.1039/C6CP04101A

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