期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 139, 期 32, 页码 11254-11260出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b06485
关键词
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资金
- NIH, National Institute of General Medical Sciences
- HHMI
- U.S. DOE [DE-AC02-05CH11231]
- DOE Office of Science [DE-AC02-06CH11357]
- NSF [1360635, 1334109, EFRI-1332411, CCF-1526650]
- ARO [W911NF-12-1-0420, MURI W911NF-11-1-0024]
- NIH [R01GM104960]
- Presidential Strategic Initiative Fund from Arizona State University
- Center for Molecular Design and Biomimetics at the Arizona State University Biodesign Institute
- ONR [MURI N000140911118]
- Gordon and Betty Moore Foundation [GBMF3849]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1360635] Funding Source: National Science Foundation
The foundational goal of structural DNA nanotechnology-the field that uses oligonucleotides as a molecular building block for the programmable self-assembly of nanostructured systems-was to use DNA to construct three-dimensional (3D) lattices for solving macromolecular structures. The programmable nature of DNA makes it an ideal system for rationally constructing self-assembled crystals and immobilizing guest molecules in a repeating 3D array through their specific stereospatial interactions with the scaffold. In this work, we have extended a previously described motif (4 x 5) by expanding the structure to a system that links four double-helical layers; we use a central weaving oligonucleotide containing a sequence of four six-base repeats (4 X 6), forming a matrix of layers that are organized and dictated by a series of Holliday junctions. In addition, we have assembled mirror image crystals (L-DNA) with the identical sequence that are completely resistant to nucleases. Bromine and selenium derivatives were obtained for the L- and D-DNA forms, respectively, allowing phase determination for both forms and solution of the resulting structures to 3.0 and 3.05 angstrom resolution. Both right- and left-handed forms crystallized in the trigonal space groups with mirror image 3-fold helical screw axes P3(2) and P3(1) for each motif, respectively. The structures reveal a highly organized array of discrete and well-defined cavities that are suitable for hosting guest molecules and allow us to dictate a priori the assembly of guest-DNA conjugates with a specified crystalline hand.
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