Abstract
DNA-programmable assembly has been used to deliberately synthesize hundreds of different colloidal crystals spanning dozens of symmetries, but the complexity of the achieved structures has so far been limited to small unit cells. We assembled DNA-modified triangular bipyramids (∼250-nanometer long edge, 177-nanometer short edge) into clathrate architectures. Electron microscopy images revealed that at least three different structures form as large single-domain architectures or as multidomain materials. Ordered assemblies, isostructural to clathrates, were identified with the help of molecular simulations and geometric analysis. These structures are the most sophisticated architectures made via programmable assembly, and their formation can be understood based on the shape of the nanoparticle building blocks and mode of DNA functionalization.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 931-935 |
| Number of pages | 5 |
| Journal | Science |
| Volume | 355 |
| Issue number | 6328 |
| DOIs | |
| State | Published - Mar 3 2017 |
Funding
This work was supported as part of 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. C.A.M. additionally acknowledges support from the Air Force Office of Scientific Research awards FA9550-11-1-0275 and FA9550-12-1-0280. H.L. is grateful to a scholarship from the China Scholarship Council (CSC) under Grant CSC no. 201306310060. M.E. acknowledges funding by Deutsche Forschungsgemeinschaft through the Cluster of Excellence Engineering of Advanced Materials and support from the Interdisciplinary Center for Functional Particle Systems (FPS) and Central Institute for Scientific Computing (ZISC). M.S. acknowledges support from the University of Michigan Rackham Predoctoral Fellowship Program. S.C.G. was partially supported by a Simons Investigator award from the Simons Foundation. Computational resources and services were supported by Advanced Research Computing at the University of Michigan, Ann Arbor. This work made use of the Electron Probe Instrumentation Center (EPIC) facility [Northwestern University's Atomic and Nanoscale Characterization Experimental Center (NUANCE)], which has received support from the Materials Research Science and Engineering Center program (NSF DMR-1121262) at the Materials Research Center, the International Institute for Nanotechnology (IIN), and the State of Illinois, through the IIN. All results are reported in the main paper and supplementary materials. H.L. synthesized, functionalized, and assembled the particles; H.L. and L.S. synthesized and purified the DNA; H.L. collected ultraviolet-visible data; H.L. and L.S. collected EM data; S.L., M.S., M.E., and S.C.G. developed the simulation model; S.L. and M.S. implemented the model in the DEM module of HOOMD-Blue; S.L. performed the simulations; S.L., M.E., and S.C.G. analyzed and discussed the simulation data; S.L. and M.E. performed the structural identification analysis on the simulation data and on the TEM images supplied by H.L.; H.L., S.L., M.E., S.C.G., and C.A.M. wrote the paper; M.E., S.C.G., and C.A.M. supervised the research; C.A.M. is the developer of the concept of programmable colloidal crystallization and the concept of controlled valency through anisotropic particle functionalization with nucleic acids that led to the formation of the observed clathrate structures. The authors declare no competing financial interests.
ASJC Scopus subject areas
- General