Metallofullerenes: One of the ideal basic units for constructing atomic-scale manufacturing devices

Atomic-scale manufacturing centers on precisely manipulating the position and state of individual atoms or molecules, enabling functional construction and regulation of materials at the smallest scale. It serves as a crucial foundational technology supporting future advancements in novel semiconductors, energy catalysis, quantum information, and related fields. Fullerenes, as typical carbon atom clusters, possess both outstanding structural stability and tunable electronic properties. By embedding or attaching different metals, metallic fullerenes can precisely regulate electronic structures and spin coupling at the atomic scale. They enable the controlled introduction of properties such as magnetism, electric polarization, catalytic activity, and quantum anomalous Hall effects, achieving the coupling and integration of multiple physicochemical properties. This makes them ideal building blocks for bottom-up construction of atom-scale manufacturing devices. This paper reviews our group’s recent fundamental and applied research on metallic fullerenes: Using density functional theory and multiple bonding analysis methods, we systematically revealed the relationship between carbon cage size and metal elements on the covalent bonding between embedded metals and the metal-carbon cage coupling. Through non-adiabatic molecular dynamics simulations, we elucidated the ultrafast excited-state relaxation and charge transfer mechanisms in metallic fullerenes. For functional device applications, we have focused on performance regulation and physical mechanisms of metal fullerenes in single-atom catalysis, single-molecule transistors, two-dimensional multifunctional materials, perovskite solar cells, and nuclear physics. These studies not only enrich the theoretical framework and scientific understanding of metal fullerenes but also advance the application development of such atomic clusters in molecular electronics, topological electronics, and energy conversion devices. They provide new theoretical perspectives and methodological insights for the advancement of atomically tunable materials.