Nonlinear relaxation and solvation dynamics in a Coulomb lattice gas

Knödler, D.; Dieterich, W.; Lonsky, Ch.; Nitzan, Abraham

doi:10.1063/1.469424

Cited by 7 publications

(3 citation statements)

References 11 publications

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“…Strong nonlinearity has also been observed in simulations of solvation dynamics in Coulomb lattice gases. 17 As mentioned above, the dependence of the solvation dynamics on the structure of the solute was a subject of several experimental, 13,18 numerical, 13 and analytical 19,20 studies. Less is known about the corresponding effect of solvent structure.…”

Section: S͑t ͒ϭmentioning

confidence: 99%

Solvation dynamics in dielectric solvents with restricted molecular rotations: Polyethers

Olender

Nitzan

1995

The Journal of Chemical Physics

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A molecular dynamics study of macromolecules in good solvents: Comparison with dielectric spectroscopy experiments Molecular dynamics simulations are used to study solvation and solvation dynamics of a classic charge in a series of ethers of increasing molecular weights, CH 3 ͑CH 2 OCH 2 ͒ n H with nϭ1, 2, and 4. Equilibrium structures of the solvated species, ion mobility, linear response solvation functions, and nonequilibrium solvation are studied and compared with the corresponding results for a simple ͑Stockmayer͒ fluid. For a typical positive ion, Na ϩ , solvation in these systems is found to belong to the nonlinear response regime; the nonlinear behavior is associated with the specific binding of the cation to the negative oxygen sites. Solvation dynamics in the timescale studied ͑tϽ0.5 ns͒ is found to be essentially bimodal, with a short component similar in duration and magnitude to that found in simpler solvents. However, except for the simplest system studied ͑ethyl methyl ether͒ the short time component is not Gaussian ͑i.e., its Gaussian part is limited to insignificantly short times͒ and cannot be interpreted as inertial free streaming of solvent molecules in the potential field of the solute. Instead we suggest that it originates from damped solvent vibrations about solvent inherent structures. The character of the solvent motions that drive the solvation process changes as the molecular size increases: From overall molecular rotations in the monoether, to intramolecular segmental motions in the larger solvents. It is suggested that solvation dynamics ͑studied, e.g., by laser induced fluorescence͒ can be used as a probe for the dynamics of such segmental motions in polymer electrolytes.

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Section: S͑t ͒ϭmentioning

confidence: 99%

Solvation dynamics in dielectric solvents with restricted molecular rotations: Polyethers

Olender

Nitzan

1995

The Journal of Chemical Physics

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“…The treatment of the ion-ion interaction is thus promoted from the continuum mean field level used in the PB and PNP levels of description, and the model can describe ionion correlations that are disregarded by mean field theories. Similar DLMC models were previously used in studies of ion equilibrium dynamics in glassy and polymer electrolytes; [29][30][31] however, these studies were limited to infinite macroscopically homogeneous systems without dielectric boundaries.…”

Section: Introductionmentioning

confidence: 99%

A Dynamic Lattice Monte Carlo Model of Ion Transport in Inhomogeneous Dielectric Environments: Method and Implementation

Gräf¹,

Nitzan²,

Kurnikova³

et al. 2000

J. Phys. Chem. B

140

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A dynamic lattice Monte Carlo (DLMC) simulation approach to the description of ion transport in dielectric environments is presented. Conventional approaches using periodic boundary conditions are inefficient for nonequilibrium situations in inhomogeneous systems. Instead, the simulated system is embedded in a bigger system that determines the average electrostatic potential and the ionic concentrations at its boundaries. Two issues are of special importance: implementing the given boundary conditions in the treatment of dynamical processes at and near the boundaries, and efficient evaluation of ion-ion interaction in the heterogeneous dielectric medium during the Monte Carlo simulation. The performance of the method is checked by comparing numerical results to exact solutions for simple geometries, and to mean field (Poisson-Nernst-Planck, PNP) theory in a system where the latter should provide a reasonable description. Other examples in which the PNP theory fails in various degrees are shown and discussed. In particular, PNP results deviate considerably from the DLMC dynamics for ion transport through rigid narrow membrane channels with large disparity between the dielectric constants of the protein and the water environments.

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“…If the charge correlation function ρ(x) minimizes free energy, and is at equilibrium, as in ionic solutions, the far field potential is strongly screened. However, the relaxation into such a state takes time, typically psec to nsec in an ionic solution under biological conditions (see measurements reported in [10], and theory summarized in [19]). As long as local charge neutrality exists during the relaxation period, the potential changes from attenuated (as described above) to exponentially screened, as equilibrium is reached.…”

Section: B the Condition Of Local Electroneutralitymentioning

confidence: 99%

Attenuation of the Electric Potential and Field in Disordered Systems

2005

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We study the electric potential and field produced by disordered distributions of charge to see why clumps of charge do not produce large potentials or fields. The question is answered by evaluating the probability distribution of the electric potential and field in a totally disordered system that is overall electroneutral. An infinite system of point charges is called totally disordered if the locations of the points and the values of the charges are random. It is called electroneutral if the mean charge is zero. In one dimension, we show that the electric field is always small, of the order of the field of a single charge, and the spatial variations in potential are what can be produced by a single charge. In two and three dimensions, the electric field in similarly disordered electroneutral systems is usually small, with small variations. Interestingly, in two and three dimensional systems, the electric potential is usually very large, even though the electric field is not: large amounts of energy are needed to put together a typical disordered configuration of charges in two and three dimensions, but not in one dimension. If the system is locally electroneutral--as well as globally electroneutral--the potential is usually small in all dimensions. The properties considered here arise from the superposition of electric fields of quasi-static distributions of charge, as in nonmetallic solids or ionic solutions. These properties are found in distributions of charge far from equilibrium

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Nonlinear relaxation and solvation dynamics in a Coulomb lattice gas

Cited by 7 publications

References 11 publications

Solvation dynamics in dielectric solvents with restricted molecular rotations: Polyethers

Solvation dynamics in dielectric solvents with restricted molecular rotations: Polyethers

A Dynamic Lattice Monte Carlo Model of Ion Transport in Inhomogeneous Dielectric Environments: Method and Implementation

Attenuation of the Electric Potential and Field in Disordered Systems

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