Hybrid Materials Interfaces Group, Faculty of Production Engineering and Bremen Center for Computational Materials Science, University of Bremen, D-28359 Bremen, Germany.
J Am Chem Soc. 2012 Feb 1;134(4):2407-13. doi: 10.1021/ja210744g. Epub 2012 Jan 20.
We present evidence that specific material recognition by small peptides is governed by local solvent density variations at solid/liquid interfaces, sensed by the side-chain residues with atomic-scale precision. In particular, we unveil the origin of the selectivity of the binding motif RKLPDA for Ti over Si using a combination of metadynamics and steered molecular dynamics simulations, obtaining adsorption free energies and adhesion forces in quantitative agreement with corresponding experiments. For an accurate description, we employ realistic models of the natively oxidized surfaces which go beyond the commonly used perfect crystal surfaces. These results have profound implications for nanotechnology and materials science applications, offering a previously missing structure-function relationship for the rational design of materials-selective peptide sequences.
我们提出证据表明，小肽对特定物质的识别是由固/液界面处局部溶剂密度变化控制的，这种变化可以被侧链残基以原子级精度感知。特别是，我们使用元动力学和导向分子动力学模拟的组合，揭示了结合基序 RKLPDA 对 Ti 比对 Si 具有选择性的起源，获得的吸附自由能和粘附力与相应的实验结果定量一致。为了进行准确的描述，我们采用了真实的、经过自然氧化的表面模型，这些模型超越了常用的完美晶体表面。这些结果对纳米技术和材料科学应用具有深远的影响，为材料选择性肽序列的合理设计提供了以前缺失的结构-功能关系。
