Although distinct growth behaviors on different faces of hexagonal ice have long been suggested, their understanding on a molecular scale has been hampered due to experimental difficulties near interfaces. We present a molecular dynamics simulation study to unravel the molecular origin of anisotropy in the growth kinetics of hexagonal ice by visualizing the formation of transient water structures in the growing ice interface. During ice growth, the formation of transient structures and their rearrangement to the final ice configuration are observed irrespective of growth direction. However, we find that their structure and duration differ significantly depending on growth direction. In the direction perpendicular to the basal face of hexagonal ice along which growth occurs most slowly, a two-dimensional transient structure, which is formed by competing hexagonal and cubic arrangements within the same layer, persists for a significant period of time, contrasted with short-lived transient structures in other directions. This observation of such transient water structures and their rearrangement during ice growth provides a clear explanation of different growth rates on each face of hexagonal ice on a molecular scale.
Here we report a novel approach to prepare all-nanoparticle vesicles using ligand-stabilized gold particles as a building block. Hydroxyalkyl-terminated gold nanoparticles were spontaneously organized into well-defined hollow vesicle-like assemblies in water without any template. The unusual anisotropic self-assembly was attributed to the ligand rearrangement on nanoparticles, which leads to increased hydroxyl group density at the nanoparticle/water interface. One-dimensional strings were formed instead of vesicles with increasing surface ligand density, which supports the hypothesis. The size and the wall thickness of vesicles were controlled by adjusting the concentration of nanoparticles or by adding extra surfactants. The work presented here highlights the dynamic nature of surface ligands on gold particles and demonstrates that the combination of ligand rearrangement and the hydrophobic effect can be used as a versatile tool for anisotropic self-assembly of nanoparticles.
Inorganic nanoparticles modified with simple alkylthiol ligands can organize into unique vesicle-like hollow assemblies with controllable membrane thickness, composition, and properties.
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