Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 114, Issue 29, Pages 7537-7542Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1621186114
Keywords
orientation-dependent interparticle forces; dynamic force spectroscopy; atomic force microscopy; solvent structure; DLVO theory
Categories
Funding
- US Department of Energy (DOE), Office of Basic Energy Sciences (BES), Division of Materials Science and Engineering (DMSE) [67037]
- DOE BES DMSE
- National Science Foundation [DMR-1312697]
- Materials Synthesis and Simulations across Scales Initiative, a Laboratory Directed Research and Development Program at Pacific Northwest National Laboratory (PNNL)
- Office of Biological and Environmental Research
- DOE [DE-AC05-76RL01830]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1312697] Funding Source: National Science Foundation
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Oriented attachment of nanocrystalline subunits is recognized as a common crystallization pathway that is closely related to formation of nanoparticle superlattices, mesocrystals, and other kinetically stabilized structures. Approaching particles have been observed to rotate to achieve coalignment while separated by nanometer-scale solvent layers. Little is known about the forces that drive coalignment, particularly in this solvent-separated regime. To obtain a mechanistic understanding of this process, we used atomic-force-microscopy-based dynamic force spectroscopy with tips fabricated from oriented mica to measure the adhesion forces between mica (001) surfaces in electrolyte solutions as a function of orientation, temperature, electrolyte type, and electrolyte concentration. The results reveal an similar to 60 degrees periodicity as well as a complex dependence on electrolyte concentration and temperature. A continuum model that considers the competition between electrostatic repulsion and van der Waals attraction, augmented by microscopic details that include surface separation, water structure, ion hydration, and charge regulation at the interface, qualitatively reproduces the observed trends and implies that dispersion forces are responsible for establishing coalignment in the solvent-separated state.
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