Ortony Julia H, Newcomb Christina J, Matson John B, Palmer Liam C, Doan Peter E, Hoffman Brian M, Stupp Samuel I
Institute for BioNanotechnology in Medicine, Northwestern University, 303 East Superior Street, Suite 11-131, Chicago, Illinois 60611, USA.
1] Institute for BioNanotechnology in Medicine, Northwestern University, 303 East Superior Street, Suite 11-131, Chicago, Illinois 60611, USA [2] Department of Materials Science and Engineering, Northwestern University, 2220 Campus Drive, Evanston, Illinois 60208, USA.
Nat Mater. 2014 Aug;13(8):812-6. doi: 10.1038/nmat3979. Epub 2014 May 25.
A large variety of functional self-assembled supramolecular nanostructures have been reported over recent decades. The experimental approach to these systems initially focused on the design of molecules with specific interactions that lead to discrete geometric structures, and more recently on the kinetics and mechanistic pathways of self-assembly. However, there remains a major gap in our understanding of the internal conformational dynamics of these systems and of the links between their dynamics and function. Molecular dynamics simulations have yielded information on the molecular fluctuations of supramolecular assemblies, yet experimentally it has been difficult to obtain analogous data with subnanometre spatial resolution. Using site-directed spin labelling and electron paramagnetic resonance spectroscopy, we measured the conformational dynamics of a self-assembled nanofibre in water through its 6.7 nm cross-section. Our measurements provide unique insight for the design of supramolecular functional materials.
近几十年来,人们已经报道了各种各样功能性自组装超分子纳米结构。对这些体系的实验方法最初集中于设计具有特定相互作用从而导致离散几何结构的分子,最近则集中于自组装的动力学和机理途径。然而,我们对这些体系的内部构象动力学以及它们的动力学与功能之间的联系仍然知之甚少。分子动力学模拟已经得出了有关超分子聚集体分子涨落的信息,但在实验上,很难获得具有亚纳米空间分辨率的类似数据。我们使用定点自旋标记和电子顺磁共振光谱,通过其6.7纳米的横截面测量了水中自组装纳米纤维的构象动力学。我们的测量为超分子功能材料的设计提供了独特的见解。