Prehistory probability distribution of ion transition through graphene nanopore

Guardiani, Carlo; Barabash, Miroslav; Gibby, William; Luchinsky, D. G.; Khovanov, I. A.; McClintock, Peter V. E.

doi:10.29007/46wd

Cited by 7 publications

(7 citation statements)

References 17 publications

(25 reference statements)

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“…Note that the force estimates shown in Figure a are close to our earlier estimates, 0.35 nN per particle, of the maximal total electrostatic force experienced by an ion near a graphene nanopore . It is also worth noting that the field-induced asymmetry of the hydration shells may be strongly correlated with the local polarization of water molecules under the incident field, as discussed earlier . The two mechanisms leading to field-induced barrier changes oppose the original bias field and consequently limit transport, providing yet another example of solvent screening at the nanoscale.…”

Section: Asymmetry Of Hydration Shells and Field-induced Barriersupporting

confidence: 84%

“… 47 It is also worth noting that the field-induced asymmetry of the hydration shells may be strongly correlated with the local polarization of water molecules under the incident field, as discussed earlier. 41 The two mechanisms leading to field-induced barrier changes oppose the original bias field and consequently limit transport, providing yet another example of solvent screening at the nanoscale. Interestingly, field-induced asymmetry of hydration shells along the z direction may be combined with in-plane manipulation of the shells induced by directed membrane strains, 59 potentially yielding a path toward hybrid mechano-electric gating.…”

Section: Asymmetry Of Hydration Shells and Field-induced Barriermentioning

confidence: 99%

“…Initial insight into the ionic permeation process can be obtained from an examination of escape trajectories. The statistically significant structure of these trajectories can be obtained from the prehistory probability distribution (PPD). − The underlying concept is that the probability of observing an ion escaping near the boundary x f of the attractors of two metastable states is small, due to the relatively high transition barrier separating them. In this system the boundary separates the pre-escape and postescape bulk solutions.…”

Section: Trajectories and Prehistory Probability Distributionmentioning

confidence: 99%

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Field-Dependent Dehydration and Optimal Ionic Escape Paths for C₂N Membranes

et al. 2021

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Most analytic theories describing electrostatically driven ion transport through water-filled nanopores assume that the corresponding permeation barriers are bias-independent. While this assumption may hold for sufficiently wide pores under infinitely small bias, transport through subnanometer pores under finite bias is difficult to interpret analytically. Given recent advances in subnanometer pore fabrication and the rapid progress in detailed computer simulations, it is important to identify and understand the specific field-induced phenomena arising during ion transport. Here we consider an atomistic model of electrostatically driven ion permeation through subnanoporous C 2 N membranes. We analyze probability distributions of ionic escape trajectories and show that the optimal escape path switches between two different configurations depending on the bias magnitude. We identify two distinct mechanisms contributing to field-induced changes in transport-opposing barriers: a weak one arising from field-induced ion dehydration and a strong one due to the field-induced asymmetry of the hydration shells. The simulated current–voltage characteristics are compared with the solution of the 1D Nernst–Planck model. Finally, we show that the deviation of simulated currents from analytic estimates for large fields is consistent with the field-induced barriers and the observed changes in the optimal ion escape path.

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Section: Asymmetry Of Hydration Shells and Field-induced Barriersupporting

confidence: 84%

Section: Asymmetry Of Hydration Shells and Field-induced Barriermentioning

confidence: 99%

Section: Trajectories and Prehistory Probability Distributionmentioning

confidence: 99%

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Field-Dependent Dehydration and Optimal Ionic Escape Paths for C₂N Membranes

et al. 2021

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“…For example, by iteratively choosing the most appropriate combination of pore geometric parameters, and subsequently manipulating the pore shape externally (e.g. by stretching), the nanopore's permeability and selectivity can be optimised and regulated, providing for permeation along specified pathways [73][74][75]. The same strategy should serve to slow down the translocation and guide the orientation of DNA, which constitutes one of the current challenges to fast genome sequencing [11].…”

Section: Discussionmentioning

confidence: 99%

Origin and control of ionic hydration patterns in nanopores

Barabash

Gibby

Guardiani

et al. 2020

Preprint

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In order to permeate a nanopore, an ion must overcome a dehydration energy barrier caused by the redistribution of surrounding water molecules. The redistribution is inhomogeneous, anisotropic and strongly position-dependent, resulting in complex patterns that are routinely observed in molecular dynamics simulations. We now address the questions of the physical origin of these patterns and of how they can be predicted and controlled. We introduce an analytic model able to predict the patterns in terms of experimentally accessible radial distributions functions, yielding results that agree well with molecular dynamics simulations. We show that the patterns are attributable to a complex interplay of ionic hydration shells with water layers adjacent to the membrane and with the hydration cloud of the nanopore rim atoms, and we discuss ways of controlling them. Our findings pave the way to designing required transport properties into nanoionic devices by optimising the structure of the hydration patterns.

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“…Their work was further improved by numerous theoretical studies and simulations taking into account the asymmetry of the size of the ions, direct interactions between ions, orientational ordering of water dipoles, discrete charge distribution of the surface, quantum mechanical approach, etc. [ 1 , 72 , 73 , 74 , 76 , 84 , 85 , 86 , 88 , 90 , 93 , 94 , 95 , 96 , 97 , 98 , 99 , 100 , 101 , 102 , 103 , 104 , 105 , 106 , 107 , 108 , 109 , 110 , 111 , 112 , 113 , 114 , 115 ]. The physical properties of the EDL are crucial in understanding the interaction between charged surfaces in electrolyte solutions [ 34 , 38 , 43 , 116 , 117 , 118 , 119 , 120 , 121 , 122 , 123 , 124 ].…”

Section: On the Role Of Electrostatic Interactionsmentioning

confidence: 99%

Mechanical and Electrical Interaction of Biological Membranes with Nanoparticles and Nanostructured Surfaces

et al. 2021

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In this review paper, we theoretically explain the origin of electrostatic interactions between lipid bilayers and charged solid surfaces using a statistical mechanics approach, where the orientational degree of freedom of lipid head groups and the orientational ordering of the water dipoles are considered. Within the modified Langevin Poisson–Boltzmann model of an electric double layer, we derived an analytical expression for the osmotic pressure between the planar zwitterionic lipid bilayer and charged solid planar surface. We also show that the electrostatic interaction between the zwitterionic lipid head groups of the proximal leaflet and the negatively charged solid surface is accompanied with a more perpendicular average orientation of the lipid head-groups. We further highlight the important role of the surfaces’ nanostructured topography in their interactions with biological material. As an example of nanostructured surfaces, we describe the synthesis of TiO2 nanotubular and octahedral surfaces by using the electrochemical anodization method and hydrothermal method, respectively. The physical and chemical properties of these nanostructured surfaces are described in order to elucidate the influence of the surface topography and other physical properties on the behavior of human cells adhered to TiO2 nanostructured surfaces. In the last part of the paper, we theoretically explain the interplay of elastic and adhesive contributions to the adsorption of lipid vesicles on the solid surfaces. We show the numerically predicted shapes of adhered lipid vesicles corresponding to the minimum of the membrane free energy to describe the influence of the vesicle size, bending modulus, and adhesion strength on the adhesion of lipid vesicles on solid charged surfaces.

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Prehistory probability distribution of ion transition through graphene nanopore

Cited by 7 publications

References 17 publications

Field-Dependent Dehydration and Optimal Ionic Escape Paths for C₂N Membranes

Field-Dependent Dehydration and Optimal Ionic Escape Paths for C₂N Membranes

Origin and control of ionic hydration patterns in nanopores

Mechanical and Electrical Interaction of Biological Membranes with Nanoparticles and Nanostructured Surfaces

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Prehistory probability distribution of ion transition through graphene nanopore

Cited by 7 publications

References 17 publications

Field-Dependent Dehydration and Optimal Ionic Escape Paths for C2N Membranes

Field-Dependent Dehydration and Optimal Ionic Escape Paths for C2N Membranes

Origin and control of ionic hydration patterns in nanopores

Mechanical and Electrical Interaction of Biological Membranes with Nanoparticles and Nanostructured Surfaces

Contact Info

Product

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Field-Dependent Dehydration and Optimal Ionic Escape Paths for C₂N Membranes

Field-Dependent Dehydration and Optimal Ionic Escape Paths for C₂N Membranes