Department of Chemistry, Biochemistry and Pharmaceutical Sciences, University of Bern, Freiestrasse 3, CH-3012 Bern, Switzerland.
Institute of Anatomy, University of Bern, Baltzerstrasse 2, CH-3012 Bern, Switzerland.
Bioconjug Chem. 2023 Jan 18;34(1):70-77. doi: 10.1021/acs.bioconjchem.2c00077. Epub 2022 Mar 31.
The precise arrangement of structural subunits is a key factor for the proper shape and function of natural and artificial supramolecular assemblies. In DNA nanotechnology, the geometrically well-defined double-stranded DNA scaffold serves as an element of spatial control for the precise arrangement of functional groups. Here, we describe the supramolecular assembly of chemically modified DNA hybrids into diverse types of architectures. An amphiphilic DNA duplex serves as the sole structural building element of the nanosized supramolecular structures. The morphology of the assemblies is governed by a single subunit of the building block. The chemical nature of this subunit, i.e., polyethylene glycols of different chain length or a carbohydrate moiety, exerts a dramatic influence on the architecture of the assemblies. Cryo-electron microscopy revealed the arrangement of the individual DNA duplexes within the different constructs. Thus, the morphology changes from vesicles to ribbons with increasing length of a linear polyethylene glycol. Astoundingly, attachment of a -acetylgalactosamine carbohydrate to the DNA duplex moiety produces an unprecedented type of star-shaped architecture. The novel DNA architectures presented herein imply an extension of the current concept of DNA materials and shed new light on the fast-growing field of DNA nanotechnology.
结构亚基的精确排列是自然和人工超分子组装具有适当形状和功能的关键因素。在 DNA 纳米技术中,几何形状明确的双链 DNA 支架可作为精确排列功能基团的空间控制元件。在这里,我们描述了化学修饰的 DNA 杂交体组装成多种类型的结构。两亲性 DNA 双链体是纳米级超分子结构的唯一结构构建元件。组装体的形态由构建块的单个亚基控制。该亚基的化学性质,即不同链长的聚乙二醇或糖基部分,对组装体的结构有显著影响。低温电子显微镜揭示了不同结构中单个 DNA 双链体的排列。因此,随着线性聚乙二醇长度的增加,形态从囊泡变为带状。令人惊讶的是,将 N-乙酰半乳糖胺糖基附着到 DNA 双螺旋部分会产生一种前所未有的星型结构。本文提出的新型 DNA 结构扩展了当前 DNA 材料的概念,并为 DNA 纳米技术这一日益发展的领域提供了新的思路。