Surface charge density determination of single conical nanopores based on normalized ion current rectification.

Department of Chemistry, Georgia State University, Atlanta, Georgia 30302, USA.
Langmuir (Impact Factor: 4.38). 12/2011; 28(2):1588-95. DOI: 10.1021/la203106w
Source: PubMed

ABSTRACT Current rectification is well known in ion transport through nanoscale pores and channel devices. The measured current is affected by both the geometry and fixed interfacial charges of the nanodevices. In this article, an interesting trend is observed in steady-state current-potential measurements using single conical nanopores. A threshold low-conductivity state is observed upon the dilution of electrolyte concentration. Correspondingly, the normalized current at positive bias potentials drastically increases and contributes to different degrees of rectification. This novel trend at opposite bias polarities is employed to differentiate the ion flux affected by the fixed charges at the substrate-solution interface (surface effect), with respect to the constant asymmetric geometry (volume effect). The surface charge density (SCD) of individual nanopores, an important physical parameter that is challenging to measure experimentally and is known to vary from one nanopore to another, is directly quantified by solving Poisson and Nernst-Planck equations in the simulation of the experimental results. The flux distribution inside the nanopore and the SCD of individual nanopores are reported. The respective diffusion and migration translocations are found to vary at different positions inside the nanopore. This knowledge is believed to be important for resistive pulse sensing applications because the detection signal is determined by the perturbation of the ion current by the analytes.

  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: Ion current rectification dependent on the concentration gradient of KCl solutions was systematically investigated in polyethyleneimine modified glass nano-pipettes with inner diameter of 105 nm. Peak shape dependence of the rectification factor on outer KCl solution concentration was observed when inner KCl solution with concentration from 1 mM to 500 mM was used. The peak shape dependence was also observed when the concentrations of the inner and outer KCl solutions were identically controlled. The peak shape in the ion current rectification could be explained by the ion conductance changes through the conical nano-pipette, which result from modulation of ion concentration.
    Scientific Reports 01/2014; 4:4005. · 5.08 Impact Factor
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: We demonstrate a stacked graphene- Al2O3 dielectric nanopore architecture to investigate electrochemical activity at graphene edges. It has proven to be difficult to isolate electrochemical activity at the graphene edges from those at the basal planes [1]. We use 24 nm of Al2O3 to isolate the graphene basal planes from an ionic fluid environment. Nanopores ranging from 5 to 20 nm are formed by an electron beam sculpting process to expose graphene edges. Electrochemical measurements at isolated graphene edges show current densities as high as 1.2 x 10^4 A/cm^2, 300x greater than those reported for carbon nanotubes [2]. Additionally, we modulate nanopore conductance by tuning the graphene edge electrochemical current as a function of the applied bias on the embedded graphene electrode. Our results indicate that electrochemical devices based on graphene nanopores have promising applications as sensitive chemical and biological sensors, energy storage devices, and DNA sequencing.[4pt] [1] Ambrosi, et al., Nanoscale 3, 2256 (2011);[0pt] [2] J. Britto, et al., Adv. Mater. 11, 154 (1999)
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: An analytical model for the ionic conductance in a pH-regulated nanochannel gated by a field effect transistor is derived for the first time. In contrast to the existing studies, the developed model takes into account the practical effects of multiple ionic species, surface chemistry reactions, the Stern layer, and electroosmotic flow. The model is validated by the experimental data of ionic conductance available in the literature. Results show that the performance of the field effect control of the ionic conductance in the gated silica nanochannel is remarkable when the solution pH and salt concentration are low. In addition, the Stern layer effect on the ionic conductance is significant when the salt concentration is low.
    Physical Chemistry Chemical Physics 08/2014; · 4.20 Impact Factor


Available from