Macroscopic and tunable nanoparticle superlattices

Zhang, Honghu; Wang, Wenjie; Mallapragada, Surya; Travesset, Alex; Vaknin, David

doi:10.1039/c6nr07136h

Macroscopic and tunable nanoparticle superlattices

Journal Article · Mon Oct 24 00:00:00 EDT 2016 · Nanoscale

DOI:https://doi.org/10.1039/c6nr07136h· OSTI ID:1362278

Zhang, Honghu ^[1]; Wang, Wenjie ^[2]; Mallapragada, Surya ^[3]; Travesset, Alex ^[4]; Vaknin, David ^[4]

Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Materials Science and Engineering
Ames Lab., Ames, IA (United States). Division of Materials Sciences and Engineering
Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Chemical and Biological Engineering
Ames Lab. and Iowa State Univ., Ames, IA (United States). Dept. of Physics and Astronomy

In this paper, we describe a robust method to assemble nanoparticles into highly ordered superlattices by inducing aqueous phase separation of neutral capping polymers. Here we demonstrate the approach with thiolated polyethylene-glycol-functionalized gold nanoparticles (PEG-AuNPs) in the presence of salts (for example, K₂CO₃) in solutions that spontaneously migrate to the liquid–vapor interface to form a Gibbs monolayer. We show that by increasing salt concentration, PEG-AuNP monolayers transform from two-dimensional (2D) gas-like to liquid-like phase and eventually, beyond a threshold concentration, to a highly ordered hexagonal structure, as characterized by surface sensitive synchrotron X-ray reflectivity and grazing incidence X-ray diffraction. Furthermore, the method allows control of the inplane packing in the crystalline phase by varying the K₂CO₃ and PEG-AuNPs concentrations and the length of PEG. Using polymer-brush theory, we argue that the assembly and crystallization is driven by the need to reduce surface tension between PEG and the salt solution. Our approach of taking advantage of the phase separation of PEG in salt solutions is general (i.e., can be used with any nanoparticles) leads to high-quality macroscopic and tunable crystals. In conclusion, we discuss how the method can also be applied to the design of orderly 3D structures.

View Accepted Manuscript (DOE)

Research Organization:: Ames Lab. and Iowa State Univ., Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357; AC02-07CH11358

OSTI ID:: 1362278

Alternate ID(s):: OSTI ID: 1339752

Journal Information:: Nanoscale, Journal Name: Nanoscale Journal Issue: 1 Vol. 9; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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