Zeng Chenjie, Chen Yuxiang, Kirschbaum Kristin, Appavoo Kannatassen, Sfeir Matthew Y, Jin Rongchao
Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA 15213, USA.
College of Natural Sciences and Mathematics, University of Toledo, Toledo, OH 43606, USA.
Sci Adv. 2015 Mar 20;1(2):e1500045. doi: 10.1126/sciadv.1500045. eCollection 2015 Mar.
Structural ordering is widely present in molecules and materials. However, the organization of molecules on the curved surface of nanoparticles is still the least understood owing to the major limitations of the current surface characterization tools. By the merits of x-ray crystallography, we reveal the structural ordering at all scales in a super robust 133-gold atom nanoparticle protected by 52 thiolate ligands, which is manifested in self-assembled hierarchical patterns starting from the metal core to the interfacial -S-Au-S- ladder-like helical "stripes" and further to the "swirls" of carbon tails. These complex surface patterns have not been observed in the smaller nanoparticles. We further demonstrate that the Au133(SR)52 nanoparticle exhibits nonmetallic features in optical and electron dynamics measurements. Our work uncovers the elegant self-organization strategies in assembling a highly robust nanoparticle and provides a conceptual advance in scientific understanding of pattern structures.
结构有序性广泛存在于分子和材料中。然而，由于当前表面表征工具的主要局限性，纳米颗粒曲面上分子的组织情况仍了解最少。借助X射线晶体学的优势，我们揭示了由52个硫醇盐配体保护的超稳定133金原子纳米颗粒在所有尺度上的结构有序性，这表现为从金属核到界面-S-Au-S-阶梯状螺旋“条纹”，再到碳尾“漩涡”的自组装层次模式。这些复杂的表面模式在较小的纳米颗粒中尚未观察到。我们进一步证明，Au133(SR)52纳米颗粒在光学和电子动力学测量中表现出非金属特征。我们的工作揭示了组装高度稳定纳米颗粒时优雅的自组织策略，并在对图案结构的科学理解上取得了概念性进展。
