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Ligand-Ligand-Interaction-Dominated Self-Assembly of Gold Nanoparticles at the Oil/Water Interface: An Atomic-Scale Simulation. | LitMetric

AI Article Synopsis

Article Abstract

The self-assembly of nanoparticles (NPs) into ordered superlattices is a powerful strategy to fabricate functional nanomaterials. Subtle variations in the interactions between NPs will influence the self-assembled superlattices. Using all-atom molecular dynamics simulations, we explore the self-assembly of 16 gold NPs, 4 nm in diameter, capped with ligands at the oil-water interface, and quantify the interactions between NPs at the atomic scale. We demonstrate that the interaction between capping ligands rather than that between NPs is dominant during the assembly process. For dodecanethiol (DDT)-capped Au NPs, the assembled superlattice is highly ordered in a close-packed configuration at a slow evaporation rate, while it is disordered at a fast evaporation rate. When replacing the capping ligands with stronger polarization than DDT molecules, the NPs form a robust ordered configuration at different evaporation rates due to the stronger electrostatic attraction between capping ligands from different NPs. Moreover, Au-Ag binary clusters exhibit similar assembly behavior with Au NPs. Our work uncovers the nonequilibrium nature of NP assembly at the atomic scale and would be helpful in rationally controlling NPs superlattice by changing passivating ligands, solvent evaporation rate, or both.

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Source
http://dx.doi.org/10.1021/acs.jpcb.2c07937DOI Listing

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