Interaction forces between charged interfaces in the presence of oppositely charged dendrimers are studied by experiment and simulation. The experiments involve direct force measurements with an atomic force microscope (AFM) between two negatively charged colloidal particles in the presence of adsorbed, positively charged globular dendrimers. The simulations are carried out by treating the macroions explicitly, while the small salt ions are treated implicitly through the Debye-Huckel approximation. The system undergoes overcharging, and at the isoelectric point long-ranged attractive electrostatic forces are present. The range of the attraction is on the order of half the Debye length at high salt concentration, but it becomes smaller at low salt concentration. Away from the isoelectric point, repulsive electrostatic forces are observed due to diffuse layer overlap. A semiquantitative agreement between experiment and simulation is obtained, despite the fact that the simple theoretical model does not involve any adjustable parameters. This study provides for the first time detailed comparison between experimental and simulation data of interaction forces between colloidal particles in the presence of multivalent macroions and monovalent salt ions.
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http://dx.doi.org/10.1021/la902617x | DOI Listing |
J Chem Phys
November 2024
Department of Chemical and Biomolecular Engineering, University of California, Berkeley, California 94720, USA.
The electrostatic correlations between ions profoundly influence the structure and forces within electrical double layers. Here, we apply the modified Gaussian renormalized fluctuation theory to investigate the counter-intuitive phenomenon of repulsion between two oppositely charged surfaces and discuss its relationship with overcharging. By accurately accounting for the effect of spatially varying ion-ion correlations, we capture these repulsive forces for divalent, trivalent, as well as tetravalent ions, in quantitative agreement with reported simulation results.
View Article and Find Full Text PDFACS Nano
July 2024
Pacific Northwest National Laboratory, Richland, Washington 99354, United States.
Oriented attachment (OA) occurs when nanoparticles in solution align their crystallographic axes prior to colliding and subsequently fuse into single crystals. Traditional colloidal theories such as DLVO provide a framework for evaluating OA but fail to capture key particle interactions due to the atomistic details of both the crystal structure and the interfacial solution structure. Using zinc oxide as a model system, we investigated the effect of the solvent on short-ranged and long-ranged particle interactions and the resulting OA mechanism.
View Article and Find Full Text PDFPhys Rev E
April 2024
Department of Physics, University of South Florida, Tampa, Florida 33620, USA.
We observe homogeneous crystallization in simulated high-dimensional (d>3) liquids that follow physically realistic dynamics and have system sizes that are large enough to eliminate the possibility that crystallization was induced by the periodic boundary conditions. Supercooled four-dimensional (4D) Lennard-Jones (LJ) liquids maintained at zero pressure and constant temperatures 0.59
J Phys Chem B
April 2024
Sonny Astani Department of Civil and Environmental Engineering, University of Southern California, Los Angeles, California 90089, United States.
The organization of water molecules and ions between charged mineral surfaces determines the stability of colloidal suspensions and the strength of phase-separated particulate gels. In this article, we assemble a density functional that measures the free energy due to the interaction of water molecules and ions in electric double layers. The model accounts for the finite size of the particles using fundamental measure theory, hydrogen-bonding between water molecules using Wertheim's statistical association theory, long-range dispersion interactions using Barker and Henderson's high-temperature expansion, electrostatic correlations using a functionalized mean-spherical approximation, and Coulomb forces through the Poisson equation.
View Article and Find Full Text PDFSmall
August 2024
Institute of Physics and Astronomy, University of Potsdam, 14476, Potsdam, Germany.
On-demand switch on/off blood clogging is of paramount importance for the survival of mammals, for example as a quick response to seal damage wounds to minimize their bleeding rate. This mechanism is a complex chain process from initiated red blood cell aggregation at the target location (open wound) that quickly seals on a macroscopic scale the damaged flash. Inspired by nature an on-demand switchable particle clogging mechanism is developed with high spatial resolution down to micrometer size using light as an external non-invasive stimulation.
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