Electrostatic interactions across a charged lipid bilayer

TL;DR

This paper uses nonlinear Poisson-Boltzmann theory to analyze electrostatic interactions across charged lipid bilayers, revealing regimes of macroion interaction and their impact on DNA array ordering in lipoplexes.

Contribution

It introduces an analytical and numerical approach to quantify electrostatic coupling across lipid bilayers, including a new lattice Boltzmann method for solving the Poisson-Boltzmann equation.

Findings

Significant electrostatic contribution to DNA array ordering despite low dielectric membranes.

Identification of three regimes of macroion interaction based on charge density.

Development of a new lattice Boltzmann method for electrostatic potential calculations.

Abstract

We present theoretical work in which the degree of electrostatic coupling across a charged lipid bilayer in aqueous solution is analyzed on the basis of nonlinear Poisson-Boltzmann theory. In particular, we consider the electrostatic interaction of a single, large macroion with the two apposed leaflets of an oppositely charged lipid bilayer where the macroion is allowed to optimize its distance to the membrane. Three regimes are identified: a weak and a high macroion charge regime, separated by a regime of close macroion-membrane contact for intermediate charge densities. The corresponding free energies are used to estimate the degree of electrostatic coupling in a lamellar cationic lipid-DNA complex. That is, we calculate to what extent the one-dimensional DNA arrays in a sandwich-like lipoplex interact across the cationic membranes. We find that, in spite of the low dielectric constant inside a lipid membranes, there can be a significant electrostatic contribution to the experimentally observed cross-bilayer orientational ordering of the DNA arrays. Our approximate analytical model is complemented and supported by numerical calculations of the electrostatic potentials and free energies of the lamellar lipoplex geometry. To this end, we solve the nonlinear Poisson-Boltzmann equation within a unit cell of the lamellar lipoplex using a new lattice Boltzmann method.