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Overcharging: The crucial role of excluded volume

R. Messina1, E. González-Tovar2,3,4, M. Lozada-Cassou2,4 and C. Holm1

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In this letter we investigate the mechanism for the overcharging of a single spherical colloid in the presence of aqueous salts within the framework of the primitive model by molecular dynamics (MD) simulations as well as integral-equation theory. We find that the occurrence and strength of overcharging strongly depends on the salt-ion size, and the available volume in the fluid. To understand the role of the excluded volume of the microions, we first consider an uncharged system. For a fixed bulk concentration we find that upon increasing the fluid particle size one strongly increases the local concentration nearby the colloidal surface and that the particles become laterally ordered. For a charged system the first surface layer is built up predominantly by strongly correlated counterions. We argue that this is a key mechanism to produce overcharging with a low electrostatic coupling, and as a more practical consequence, to account for charge inversion with monovalent aqueous salt ions.


PACS

87.15.Aa Theory and modeling; computer simulation

61.20.Qg Structure of associated liquids: electrolytes, molten salts, etc.

82.70.Dd Colloids

Subjects

Soft matter, liquids and polymers

Biological physics

Chemical physics and physical chemistry

Dates

Issue 3 (November 2002)

Received 31 May 2002, accepted for publication 22 August 2002, in final form 22 August 2002



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