Structure of Polyelectrolyte Solutions at a Charged Surface

Patra, Chandra N.; Chang, Rakwoo; Yethiraj, Arun

doi:10.1021/jp0373200

Cited by 40 publications

(40 citation statements)

References 47 publications

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“…This single-chain problem is then solved using a partial enumeration scheme or resorting to a Gaussian chain model. In this review we use the notation of SCF theories [24,40] although a completely equivalent description can be obtained using the density functional theory formalism [41][42][43][44].…”

Section: General Formalismmentioning

confidence: 99%

“…• YP. Patra and Yethiraj [43] (YP-to avoid confusion with Percus-Yevick) separated the free energy functional into a repulsive and an attractive contribution with a simple weighting function for the hard sphere contribution and a van der Waals approximation for the attractive contribution. Unfortunately the latter gives a rather poor representation of the equation of state.…”

Section: Related Theoretical Approachesmentioning

confidence: 99%

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Pulsed Laser Annealing of Thin Silicon Films

Sameshima¹,

Watakabe²,

Andoh³

et al. 2006

jjap

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Using Monte Carlo simulations and self-consistent field (SCF) theory we study the surface and interface properties of a coarse grained off-lattice model. In the simulations we employ the grand canonical ensemble together with a reweighting scheme in order to measure surface and interface free energies and discuss various methods for accurately locating the wetting transition. In the SCF theory, we use a partial enumeration scheme to incorporate singlechain properties on all length scales and use a weighted density functional for the excess free energy. The results of various forms of the density functional are compared quantitatively to the simulation results. For the theory to be accurate, it is important to decompose the free energy functional into a repulsive and an attractive part, with different approximations for the two parts.Measuring the effective interface potential for our coarse grained model we explore routes for controlling the equilibrium wetting properties. (i) Coating of the substrate by an oxide layer gives rise to a subtle interplay between shortrange and long-range forces,which may stabilize a film of mesoscopic thickness or result in the formation of nano-droplets. (ii) Coating the substrate with a polymer brush, we observe second-order wetting transitions at intermediate grafting densities, while the wetting transition is of first order at low and high grafting densities. In the latter limit, polymers of the same chemical structure as the brush do not wet the surface (autophobicity). (iii) Surface pattern (stripes) might give rise to unusual adsorption properties, which are related to morphological transitions. We relate our findings to experiments and discuss perspectives and limitations of the computational methods.

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Section: General Formalismmentioning

confidence: 99%

Section: Related Theoretical Approachesmentioning

confidence: 99%

Pulsed Laser Annealing of Thin Silicon Films

Sameshima¹,

Watakabe²,

Andoh³

et al. 2006

jjap

View full text Add to dashboard Cite

show abstract

“…Polyelectrolyte adsorption has been the subject of numerous experimental [12][13][14][15][16][17][18][19][20][21][22][23][24][25], theoretical [26][27][28][29][30][31][32][33][34], and simulation [35][36][37][38][39][40][41][42] studies. Due to the importance of electrostatic interactions, the focus is often on effects of solution pH and ionic strength, variables directly influencing charge-charge interactions.…”

Section: Introductionmentioning

confidence: 99%

Polyelectrolyte adsorption kinetics under an applied electric potential: Strongly versus weakly charged polymers

Olsen

Tassel

2009

Journal of Colloid and Interface Science

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“…34,35 Patra and his colleagues successfully applied WDA for EDLs of RPM and SRPM electrolytes at different geometrical interfaces. 24,25,39,58,59 However, the single weighted density used in WDA is not sufficient enough to account for the steric interactions in primitive and solvent primitive electrolytes containing ionic size asymmetry. Thus, we base our study on modified fundamental-measure theory, 36,47 a generalized form of WDA.…”

Section: Hard Sphere Direct Correlation Function Approximation: Fundamentioning

confidence: 99%

“…[24][25][26][27][28][29][30][31] These theories go beyond size-modified PB and NLPB with Stern layer since most of them include ion correlations and are quite accurate in predicting the ion distributions at the interfaces, except at high salt concentration conditions or for highly charged ions. The last decade saw a rise in the studies of EDLs based on different flavors of classical density functional theory (DFT).…”

Section: Introductionmentioning

confidence: 99%

Ionic asymmetry and solvent excluded volume effects on spherical electric double layers: A density functional approach

Medasani

Ovanesyan

Thomas

et al. 2014

The Journal of Chemical Physics

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In this article, we present a classical density functional theory for electrical double layers of spherical macroions that extends the capabilities of conventional approaches by accounting for electrostatic ion correlations, size asymmetry, and excluded volume effects. The approach is based on a recent approximation introduced by Hansen-Goos and Roth for the hard sphere excess free energy of inhomogeneous fluids [J. Chem. Phys. 124, 154506 (2006); J. Phys.: Condens. Matter 18, 8413 (2006)]. It accounts for the proper and efficient description of the effects of ionic asymmetry and solvent excluded volume, especially at high ion concentrations and size asymmetry ratios including those observed in experimental studies. Additionally, we utilize a leading functional Taylor expansion approximation of the ion density profiles. In addition, we use the mean spherical approximation for multi-component charged hard sphere fluids to account for the electrostatic ion correlation effects. These approximations are implemented in our theoretical formulation into a suitable decomposition of the excess free energy which plays a key role in capturing the complex interplay between charge correlations and excluded volume effects. We perform Monte Carlo simulations in various scenarios to validate the proposed approach, obtaining a good compromise between accuracy and computational cost. We use the proposed computational approach to study the effects of ion size, ion size asymmetry, and solvent excluded volume on the ion profiles, integrated charge, mean electrostatic potential, and ionic coordination number around spherical macroions in various electrolyte mixtures. Our results show that both solvent hard sphere diameter and density play a dominant role in the distribution of ions around spherical macroions, mainly for experimental water molarity and size values where the counterion distribution is characterized by a tight binding to the macroion, similar to that predicted by the Stern model. © 2014 AIP Publishing LLC. [http://dx

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Structure of Polyelectrolyte Solutions at a Charged Surface

Cited by 40 publications

References 47 publications

Pulsed Laser Annealing of Thin Silicon Films

Pulsed Laser Annealing of Thin Silicon Films

Polyelectrolyte adsorption kinetics under an applied electric potential: Strongly versus weakly charged polymers

Ionic asymmetry and solvent excluded volume effects on spherical electric double layers: A density functional approach

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