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 language | English |
|---|---|
| Pages (from-to) | 6022-6029 |
| Number of pages | 8 |
| Journal | Nano Letters |
| Volume | 18 |
| Issue number | 9 |
| DOIs | |
| Publication status | Published - Sep 12 2018 |
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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 journal › Article
}
TY - JOUR
T1 - Density-Gradient Control over Nanoparticle Supercrystal Formation
AU - Oh, Taegon
AU - Ku, Jessie C.
AU - Lee, Jae Hyeok
AU - Hersam, Mark C
AU - Mirkin, Chad A.
PY - 2018/9/12
Y1 - 2018/9/12
N2 - 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.
AB - 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.
KW - assembly
KW - colloidal crystals
KW - density barrier
KW - DNA
KW - nanoparticle
KW - uniform crystals
UR - http://www.scopus.com/inward/record.url?scp=85053242939&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85053242939&partnerID=8YFLogxK
U2 - 10.1021/acs.nanolett.8b02910
DO - 10.1021/acs.nanolett.8b02910
M3 - Article
C2 - 30101587
AN - SCOPUS:85053242939
VL - 18
SP - 6022
EP - 6029
JO - Nano Letters
JF - Nano Letters
SN - 1530-6984
IS - 9
ER -