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A Technique to Functionalize and Self-assemble Macroscopic Nanoparticle-ligand Monolayer Films onto Template-free Substrates

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Dynamic Diglyme-Mediated Self-Assembly of Gold Nanoclusters.

W Scott Compel¹, O Andrea Wong¹, Xi Chen²

¹Department of Chemistry, Colorado State University , Fort Collins, Colorado 80523, United States.

|November 5, 2015

Summary

Gold nanoclusters can assemble using diglyme, a nonthiolate ligand, forming dynamic structures. These assemblies exhibit unique optical and electronic properties due to electron delocalization between nanoparticle cores.

Keywords:

diglyme dynamic assembly gold nanoclusters transient absorption spectroscopy

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Area of Science:

Nanomaterials Science
Supramolecular Chemistry
Physical Chemistry

Background:

Gold nanoclusters are typically stabilized by thiolate ligands.
Nonthiolate ligands are not commonly associated with the assembly of gold nanoclusters.

Purpose of the Study:

To investigate the surprising assembly of gold nanoclusters facilitated by diglyme.
To characterize the structure and properties of diglyme-mediated gold nanocluster assemblies.

Main Methods:

High-angle annular dark field scanning transmission electron microscopy (HAADF-STEM)
Size exclusion chromatography (SEC)
Mass spectrometry (MS)
Infrared (IR) spectroscopy
Calorimetry
Transient absorption spectroscopy (TAS)
Theoretical modeling

Main Results:

Diglyme mediates the formation of discrete, dynamic gold nanocluster assemblies.
A dissociation constant (Kd) of 20.4 μM for dimer to monomer conversion was determined.
Theoretical models and TAS indicate a low-spin monomer and a high-spin dimer.
Assembly is driven by weak diglyme oxygen-gold interactions, enabling electron delocalization.

Conclusions:

Nonthiolate ligands like diglyme can induce the assembly of gold nanoclusters.
The assembly process leads to emergent optical and electronic properties.
This work expands the understanding of ligand-directed self-assembly in nanomaterials.