Abstract
It is critical to assemble nanoparticles (NPs) into superlattices with controlled symmetries and spacings on substrates for metamaterials applications, where such structural parameters dictate their properties. Here, we use DNA to assemble anisotropic NPs of three shapes—cubes, octahedra, and rhombic dodecahedra—on substrates and investigate their thermally induced reorganization into two-dimensional (2D) crystalline films. We report two new low-density 2D structures, including a honeycomb lattice based on octahedral NPs. The low-density lattices favored here are not usually seen when particles are crystallized via other bottom-up assembly techniques. Furthermore, we show that, consistent with the complementary contact model, a primary driving force for crystallization is the formation of directional, face-to-face DNA bonds between neighboring NPs and between NPs and the substrate. Our results can be used to deliberately prepare crystalline NP films with novel morphologies.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 19035-19040 |
| Number of pages | 6 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 60 |
| Issue number | 35 |
| DOIs | |
| State | Published - Aug 23 2021 |
Funding
This material is based upon work supported by the Air Force Office of Scientific Research under awards FA9550‐17‐1‐0348 (superlattice assembly) and FA9550‐16‐1‐0150 (SAXS experiments); the Sherman Fairchild Foundation, Inc (nanoparticle synthesis); the Center for Bio‐Inspired Energy Science, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under award DE‐SC0000989 (computational studies); and the Air Force Research Laboratory under agreement FA8650‐15‐2‐5518 (SEM characterization). The U.S. Government is authorized to reproduce and distribute reprints for Governmental purposes notwithstanding any copyright notation thereon. The views and conclusions contained herein are those of the authors and should not be interpreted as necessarily representing the official policies or endorsements, either expressed or implied, of Air Force Research Laboratory or the U.S. Government. This research used resources of the APS, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE‐AC02‐06CH11357. The authors would like to thank Dr. Xiaobing Zuo for his assistance with the GISAXS experiments. This work made use of the EPIC facility of Northwestern University's NU Center, which receives support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐1542205); the MRSEC program (NSFDMR‐1121262) at the Materials Research Center; the International Institute for Nanotechnology (IIN) and the State of Illinois, through the IIN. ANCE This material is based upon work supported by the Air Force Office of Scientific Research under awards FA9550-17-1-0348 (superlattice assembly) and FA9550-16-1-0150 (SAXS experiments); the Sherman Fairchild Foundation, Inc (nanoparticle synthesis); the Center for Bio-Inspired Energy Science, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under award DE-SC0000989 (computational studies); and the Air Force Research Laboratory under agreement FA8650-15-2-5518 (SEM characterization). The U.S. Government is authorized to reproduce and distribute reprints for Governmental purposes notwithstanding any copyright notation thereon. The views and conclusions contained herein are those of the authors and should not be interpreted as necessarily representing the official policies or endorsements, either expressed or implied, of Air Force Research Laboratory or the U.S. Government. This research used resources of the APS, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The authors would like to thank Dr. Xiaobing Zuo for his assistance with the GISAXS experiments. This work made use of the EPIC facility of Northwestern University's NUANCE Center, which receives support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the MRSEC program (NSFDMR-1121262) at the Materials Research Center; the International Institute for Nanotechnology (IIN) and the State of Illinois, through the IIN.
Keywords
- DNA
- colloidal crystals
- nanoparticle superlattice
- nanoparticles
- small-angle X-ray scattering
ASJC Scopus subject areas
- General Chemistry
- Catalysis