Langner Alexander, Tait Steven L, Lin Nian, Rajadurai Chandrasekar, Ruben Mario, Kern Klaus
Max Planck Institute for Solid State Research, Heisenbergstrasse 1, D-70569 Stuttgart, Germany.
Proc Natl Acad Sci U S A. 2007 Nov 13;104(46):17927-30. doi: 10.1073/pnas.0704882104. Epub 2007 Nov 1.
Self-recognition, self-selection, and dynamic self-organization are of fundamental importance for the assembly of all supramolecular systems, but molecular-level information is not generally accessible. We present direct examples of these critical steps by using scanning tunneling microscopy to study mixtures of complementary organic ligands on a copper substrate. The ligands coordinate cooperatively with iron atoms to form well ordered arrays of rectangular multicomponent compartments whose size and shape can be deliberately tuned by selecting ligands of desired length from complementary ligand families. We demonstrate explicitly that highly ordered supramolecular arrays can be produced from redundant ligand mixtures by molecular self-recognition and -selection, enabled by efficient error correction and cooperativity, and show an example of failed self-selection due to error tolerance in the ligand mixture, leading to a disordered structure.
自我识别、自我选择和动态自组装对于所有超分子系统的组装至关重要,但分子水平的信息通常难以获取。我们通过使用扫描隧道显微镜研究铜基底上互补有机配体的混合物,给出了这些关键步骤的直接示例。这些配体与铁原子协同配位,形成排列有序的矩形多组分隔室阵列,通过从互补配体家族中选择所需长度的配体,可以有意调节其大小和形状。我们明确证明,通过分子自我识别和选择,在高效纠错和协同作用的支持下,高度有序的超分子阵列可以从冗余配体混合物中产生,并展示了由于配体混合物中的容错性导致自我选择失败而产生无序结构的示例。