Density-Gradient Control over Nanoparticle Supercrystal Formation

Taegon Oh, Jessie C. Ku, Jae Hyeok Lee, Mark C Hersam, Chad A. Mirkin

Research output: Contribution to journalArticle

3 Citations (Scopus)

Abstract

With the advent of DNA-directed methods to form "single crystal" nanoparticle superlattices, new opportunities for studying the properties of such structures across many length scales now exist. These structure-property relationships rely on the ability of one to deliberately use DNA to control crystal symmetry, lattice parameter, and microscale crystal habit. Although DNA-programmed colloidal crystals consistently form thermodynamically favored crystal habits with a well-defined symmetry and lattice parameter based upon well-established design rules, the sizes of such crystals often vary substantially. For many applications, especially those pertaining to optics, each crystal can represent a single device, and therefore size variability can significantly reduce their scope of use. Consequently, we developed a new method based upon the density difference between two layers of solvents to control nanoparticle superlattice formation and growth. In a top aqueous layer, the assembling particles form a less viscous and less dense state, but once the particles assemble into well-defined rhombic dodecahedral superlattices of a critical size, they sediment into a higher density and higher viscosity sublayer that does not contain particles (aqueous polysaccharide), thereby arresting growth. As a proof-of-concept, this method was used to prepare a uniform batch of Au nanoparticle (20.0 ± 1.6 nm in diameter) superlattices in the form of 0.95 ± 0.20 μm edge length rhombic dodecahedra with body-centered cubic crystal symmetries and a 49 nm lattice parameter (cf. 1.04 ± 0.38 μm without the sublayer). This approach to controlling and arresting superlattice growth yields structures with a 3-fold enhancement in the polydispersity index.

Original languageEnglish
Pages (from-to)6022-6029
Number of pages8
JournalNano Letters
Volume18
Issue number9
DOIs
Publication statusPublished - Sep 12 2018

Fingerprint

Nanoparticles
Superlattices
Crystal symmetry
gradients
nanoparticles
Crystals
Lattice constants
DNA
crystals
superlattices
lattice parameters
deoxyribonucleic acid
habits
symmetry
crystal optics
Polydispersity
Polysaccharides
polysaccharides
assembling
Optics

Keywords

  • assembly
  • colloidal crystals
  • density barrier
  • DNA
  • nanoparticle
  • uniform crystals

ASJC Scopus subject areas

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

Cite this

Density-Gradient Control over Nanoparticle Supercrystal Formation. / Oh, Taegon; Ku, Jessie C.; Lee, Jae Hyeok; Hersam, Mark C; Mirkin, Chad A.

In: Nano Letters, Vol. 18, No. 9, 12.09.2018, p. 6022-6029.

Research output: Contribution to journalArticle

Oh, Taegon ; Ku, Jessie C. ; Lee, Jae Hyeok ; Hersam, Mark C ; Mirkin, Chad A. / Density-Gradient Control over Nanoparticle Supercrystal Formation. In: Nano Letters. 2018 ; Vol. 18, No. 9. pp. 6022-6029.
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