"Ion Correlations at Electrified Soft Matter Interfaces"
presents an investigation that combines experiments, theory, and
computer simulations to demonstrate that the interdependency
between ion correlations and other ion interactions in solution can
explain the distribution of ions near an electrified liquid/liquid
interface. The properties of this interface are exploited to vary
the coupling strength of ion-ion correlations from weak to strong
while monitoring their influence on ion distributions at the
nanometer scale with X-ray reflectivity and on the macroscopic
scale with interfacial tension measurements.
This thesis demonstrates that a parameter-free density
functional theory that includes ion-ion correlations and
ion-solvent interactions is in agreement with the data over the
entire range of experimentally tunable correlation coupling
strengths. The reported findings represent a significant advance
towards understanding the nature and role of ion correlations in
charged soft-matter.
Ion distributions underlie many scientific phenomena and
technological applications, including electrostatic interactions
between charged biomolecules and the efficiency of energy storage
devices. These distributions are determined by interactions
dictated by the chemical properties of the ions and their
environment, as well as the long-range nature of the electrostatic
force. The presence of strong correlations between ions is
responsible for counterintuitive effects such as like-charge
attraction.
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