Rapid Prediction of Bimetallic Mixing Behavior at the Nanoscale

The nanoparticle (NP) design space allows for variations in size, shape, composition, and chemical ordering. In the search for low-energy structures, this results in an extremely large search space which cannot be screened by brute force methods. In this work, we develop a genetic algorithm to predict stable bimetallic NPs of any size, shape, and metal composition. Our method predicts nanostructures in agreement with experimental trends and it captures the detailed chemical ordering of an experimental 23,196-atom FePt NP with nearly atom-by-atom accuracy. Our developed screening process is extremely fast, allowing us to generate and analyze a database of 5454 low-energy bimetallic NPs. By identifying thermodynamically stable NPs, we rationalize bimetallic mixing at the nanoscale and reveal metal-, size-, and temperature-dependent mixing behavior. Importantly, our method is applicable to any bimetallic NP size, bridging the materials gap in nanoscale simulations, and guides experimentation in the lab by elucidating stability, mixing, and detailed chemical ordering behavior of bimetallic NPs.