Water alignment, dipolar interactions, and multiple proton occupancy during water-wire proton transport.

Abstract:

:A discrete multistate kinetic model for water-wire proton transport is constructed and analyzed using Monte Carlo simulations. In the model, each water molecule can be in one of three states: oxygen lone-pairs pointing leftward, pointing rightward, or protonated (H(3)O(+)). Specific rules for transitions among these states are defined as protons hop across successive water oxygens. Our model also includes water-channel interactions that preferentially align the water dipoles, nearest-neighbor dipolar coupling interactions, and Coulombic repulsion. Extensive Monte Carlo simulations were performed and the observed qualitative physical behaviors discussed. We find the parameters that allow the model to exhibit superlinear and sublinear current-voltage relationships, and show why alignment fields, whether generated by interactions with the pore interior or by membrane potentials, always decrease the proton current. The simulations also reveal a "lubrication" mechanism that suppresses water dipole interactions when the channel is multiply occupied by protons. This effect can account for an observed sublinear-to-superlinear transition in the current-voltage relationship.

journal_name

Biophys J

journal_title

Biophysical journal

authors

Chou T

doi

10.1016/S0006-3495(04)74335-0

subject

Has Abstract

pub_date

2004-05-01 00:00:00

pages

2827-36

issue

5

eissn

0006-3495

issn

1542-0086

pii

S0006-3495(04)74335-0

journal_volume

86

pub_type

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