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Formulation of a new and simple nonuniform size-modified Poisson-Boltzmann description.

ABSTRACT: The nonlinear Poisson-Boltzmann equation (PBE) governing biomolecular electrostatics neglects ion size and ion correlation effects, and recent research activity has focused on accounting for these effects to achieve better physical modeling realism. Here, attention is focused on the comparatively simpler challenge of addressing ion size effects within a continuum-based solvent modeling framework. Prior works by Borukhov et al. (Phys. Rev. Lett. 1997, 79, 435; Electrochim. Acta 2000, 46, 221) have examined the case of uniform ion size in considerable detail. Generalizations to accommodate different species ion sizes have been performed by Li (Nonlinearity 2009, 22, 811; SIAM J. Math. Anal. 2009, 40, 2536) and Zhou et al. (Phys. Rev. E 2011, 84, 021901) using a variational principle, Chu et al. (Biophys. J. 2007, 93, 3202) using a lattice gas model, and Tresset (Phys. Rev. E 2008, 78, 061506) using a generalized Poisson-Fermi distribution. The current work provides an alternative derivation using simple statistical mechanics principles that place the ion size effects and energy distributions on a consistent statistical footing. The resulting expressions differ from the prior nonuniform ion-size developments. However, all treatments reduce to the same form in the cases of uniform ion-size and zero ion size (the PBE). Because of their importance to molecular modeling and salt-dependent behavior, expressions for the salt sensitivities and ionic forces are also derived using the nonuniform ion size description. Emphasis in this article is on formulation and numerically robust evaluation; results are presented for a simple sphere and a previously considered DNA structure for comparison and validation. More extensive application to biomolecular systems is deferred to a subsequent article.

SUBMITTER: Boschitsch AH

PROVIDER: S-EPMC3306476 | biostudies-literature | 2012 Apr

REPOSITORIES: biostudies-literature

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Formulation of a new and simple nonuniform size-modified Poisson-Boltzmann description.

Boschitsch Alexander H AH Danilov Pavel V PV

Journal of computational chemistry 20120227 11

The nonlinear Poisson-Boltzmann equation (PBE) governing biomolecular electrostatics neglects ion size and ion correlation effects, and recent research activity has focused on accounting for these effects to achieve better physical modeling realism. Here, attention is focused on the comparatively simpler challenge of addressing ion size effects within a continuum-based solvent modeling framework. Prior works by Borukhov et al. (Phys. Rev. Lett. 1997, 79, 435; Electrochim. Acta 2000, 46, 221) hav ...[more]

PMID: 22370918

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Project description:The Poisson-Nernst-Planck (PNP) model is based on a mean-field approximation of ion interactions and continuum descriptions of concentration and electrostatic potential. It provides qualitative explanation and increasingly quantitative predictions of experimental measurements for the ion transport problems in many areas such as semiconductor devices, nanofluidic systems, and biological systems, despite many limitations. While the PNP model gives a good prediction of the ion transport phenomenon for chemical, physical, and biological systems, the number of equations to be solved and the number of diffusion coefficient profiles to be determined for the calculation directly depend on the number of ion species in the system, since each ion species corresponds to one Nernst-Planck equation and one position-dependent diffusion coefficient profile. In a complex system with multiple ion species, the PNP can be computationally expensive and parameter demanding, as experimental measurements of diffusion coefficient profiles are generally quite limited for most confined regions such as ion channels, nanostructures and nanopores. We propose an alternative model to reduce number of Nernst-Planck equations to be solved in complex chemical and biological systems with multiple ion species by substituting Nernst-Planck equations with Boltzmann distributions of ion concentrations. As such, we solve the coupled Poisson-Boltzmann and Nernst-Planck (PBNP) equations, instead of the PNP equations. The proposed PBNP equations are derived from a total energy functional by using the variational principle. We design a number of computational techniques, including the Dirichlet to Neumann mapping, the matched interface and boundary, and relaxation based iterative procedure, to ensure efficient solution of the proposed PBNP equations. Two protein molecules, cytochrome c551 and Gramicidin A, are employed to validate the proposed model under a wide range of bulk ion concentrations and external voltages. Extensive numerical experiments show that there is an excellent consistency between the results predicted from the present PBNP model and those obtained from the PNP model in terms of the electrostatic potentials, ion concentration profiles, and current-voltage (I-V) curves. The present PBNP model is further validated by a comparison with experimental measurements of I-V curves under various ion bulk concentrations. Numerical experiments indicate that the proposed PBNP model is more efficient than the original PNP model in terms of simulation time.

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Formulation of a new and simple nonuniform size-modified Poisson-Boltzmann description.

Publications

Formulation of a new and simple nonuniform size-modified Poisson-Boltzmann description.

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