The ability to modulate nanoparticle (NP) assemblies with atomic precision is still lacking, which hinders us from creating hierarchical NP organizations with desired properties. In this work, a hierarchical fibrous assembly of Au NPs is realized and further modulated with atomic-precision via site-specific tailoring of a surface “hook” which is composed of four phenyl ligands and an associated counterion. Especially, this fibrous assembly can be exquisitely modulated via tailoring of the associated counterion, which significantly changes the electrical transport properties of the NP-assembled solids by two orders of magnitude. This notable change is primarily due to the altered configuration of the interacting π-π pairs of the surface “hooks”, instead of the commonly invoked factor of interparticle distance. Overall, our success in atomic-level tailoring of the surface “hook” directly evidences how the ligands and associated counterions can function to realize two-dimensional and one-dimensional assembly of NPs and further modulate the one-dimensional assembly of NPs in a delicate manner. The success in atomic-level modulation of the hierarchical NP assembly offers new insight into the structural factors for controlling the electron transport in NP solids. This work expands our skills (<i>e.g.</i> tailoring the counterions) in rationally programming the NP-assembled materials with controllable structures and properties.

Modulating the hierarchical fibrous assembly of Au nanoparticles with atomic precision

256th National Meeting (2018)

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