Jia Yuhan, Xu Cong-Qiao, Cui Chaonan, Geng Lijun, Zhang Hanyu, Zhang Yang-Yang, Lin Shiquan, Yao Jiannian, Luo Zhixun, Li Jun
Beijing National Laboratory for Molecular Sciences (BNLMS), State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
University of Chinese Academy of Sciences, Beijing 100049, China.
Sci Adv. 2023 Aug 18;9(33):eadi0214. doi: 10.1126/sciadv.adi0214. Epub 2023 Aug 16.
Probing atomic clusters with magic numbers is of supreme importance but challenging in cluster science. Pronounced stability of a metal cluster often arises from coincident geometric and electronic shell closures. However, transition metal clusters do not simply abide by this constraint. Here, we report the finding of a magic-number cluster Rh with prominent inertness in the sufficient gas-collision reactions. Photoelectron spectroscopy experiments and global-minimum structure search have determined the geometry of Rh to be a regular ‑[Rh@Rh@Rh] with unusual high-spin electronic configuration. The distinct stability of such a strongly magnetic cluster Rh consisting of a nonmagnetic element is fully unveiled on the basis of its unique bonding nature and superatomic states. The 1-nanometer-sized -Rh cluster corresponds to a fragment of the face-centered cubic lattice of bulk rhodium but with altered magnetism and electronic property. This cluster features exceptional electron-spin state isomers confirmed in photoelectron spectra and suggests potential applications in atomically precise manufacturing involving spintronics and quantum computing.
利用幻数探测原子团簇在团簇科学中至关重要但具有挑战性。金属团簇显著的稳定性通常源于几何和电子壳层闭合的巧合。然而，过渡金属团簇并不简单地遵循这一限制。在此，我们报告在充分的气体碰撞反应中发现了具有显著惰性的幻数团簇Rh。光电子能谱实验和全局最小结构搜索确定了Rh的几何结构为规则的-[Rh@Rh@Rh]，具有不寻常的高自旋电子构型。基于其独特的键合性质和超原子态，这种由非磁性元素组成的强磁性团簇Rh的独特稳定性得以充分揭示。1纳米大小的-Rh团簇对应于块状铑面心立方晶格的一个片段，但具有改变的磁性和电子性质。该团簇具有在光电子能谱中得到证实的特殊电子自旋态异构体，并暗示了在涉及自旋电子学和量子计算的原子精确制造中的潜在应用。
