Structural and Dynamic Heterogeneity of Capillary Wave Fronts at Aqueous Interfaces
TC Zhou and A McCue and Y Ghadar and I Bako and AE Clark, JOURNAL OF PHYSICAL CHEMISTRY B, 121, 9052-9062 (2017).
Using a unique combination of slab-layering analyses and identification of truly interfacial molecules, this work examines water/vapor and water/n-hexane interfaces, specifically the structural and dynamic perturbations of the interfacial water molecules at different locations within the surface capillary waves. From both the structural and dynamic properties analyzed, it is found that these interfacial water molecules dominate the perturbations within the interfacial region, which can extend deep into the water phase relative to the Gibbs dividing surface. Of more importance is the demonstration of structural and dynamic heterogeneity of the interfacial water molecules at the capillary wave front, as indicated by the dipole orientation and the structural and dynamic behavior of hydrogen bonds and their networks.
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