Combining Deep Learning Neural Networks with Genetic Algorithms to Map Nanocluster Configuration Spaces with Quantum Accuracy at Low Computational Cost

The configuration spaces for bimetallic AuPd nanoclusters of various sizes are explored efficiently and analyzed accurately by combining genetic algorithms with neural networks trained on density functional theory. The methodology demonstrated herein provides an optimizable solution to the problem of searching vast configuration spaces with quantum accuracy in a way that is computationally practical. We implement a machine learning algorithm which learns the density functional theory potential with increasing performance while simultaneously generating and relaxing structures within the system’s global configuration space unbiasedly. As a result, the algorithm naturally converges onto the system’s energy minima while mapping the configuration space as a function of energy. The algorithm’s simple design applies not only to nanocluster configurations, as demonstrated, but to bulk, substrate, and adsorption sites as well, and it is designed to scale. To demonstrate its computational efficiency, we work with AuPd nanoclusters of sizes 15, 20, and 25 atoms. Results focus primarily on evaluating the algorithm’s performance; however, several physical insights into possible configurations for these nanoclusters naturally emerge as well, such as geometric Au surface segregation and stoichiometric Au minimization as a function of stability.