Site‐Specific Wetting of Iron Nanocubes by Gold Atoms in Gas‐Phase Synthesis

Abstract A key challenge in nanotechnology is the rational design of multicomponent materials that beat the properties of their elemental counterparts. At the same time, when considering the material composition of such hybrid nanostructures and the fabrication process to obtain them, one should favor the use of nontoxic, abundant elements in view of the limited availability of critical metals and sustainability. Cluster beam deposition offers a solvent‐ and, therefore, effluent‐free physical synthesis method to achieve nanomaterials with tailored characteristics. However, the simultaneous control of size, shape, and elemental distribution within a single nanoparticle in a small‐size regime (sub‐10 nm) is still a major challenge, equally limiting physical and chemical approaches. Here, a single‐step nanoparticle fabrication method based on magnetron‐sputtering inert‐gas condensation is reported, which relies on selective wetting of specific surface sites on precondensed iron nanocubes by gold atoms. Using a newly developed Fe–Au interatomic potential, the growth mechanism is decomposed into a multistage model implemented in a molecular dynamics simulation framework. The importance of growth kinetics is emphasized through differences between structures obtained either experimentally or computationally, and thermodynamically favorable configurations determined via global optimization techniques. These results provide a roadmap for engineering complex nanoalloys toward targeted applications.