Cluster-MLP: An Active Learning Genetic Algorithm Framework for Accelerated Discovery of Global Minimum Configurations of Pure and Alloyed Nanoclusters

• Published in: Journal of chemical information and modeling Vol. 63; no. 20; pp. 6192 - 6197
• Main Authors: Raju, Rajesh K., Sivakumar, Saurabh, Wang, Xiaoxiao, Ulissi, Zachary W.
• Format: Journal Article
• Language: English
• Published: Washington American Chemical Society 23.10.2023
• Subjects: Accuracy; Active learning; Application Note; Clusters; Configurations; Evolutionary algorithms; Genetic algorithms; Machine learning; Minima; Nanoalloys; Nanoclusters; Potential energy; Prototyping; Search methods; Structural analysis
• ISSN: 1549-9596; 1549-960X; 1549-960X
• DOI: 10.1021/acs.jcim.3c01431

Structural characterization of nanoclusters is one of the major challenges in nanocluster modeling owing to the multitude of possible configurations of arrangement of cluster atoms. The genetic algorithm (GA), a class of evolutionary algorithms based on the principles of natural evolution, is a commonly employed search method for locating the global minimum configuration of nanoclusters. Although a GA search at the DFT level is required for the accurate description of a potential energy surface to arrive at the correct global minimum configuration of nanoclusters, computationally expensive DFT evaluation of the significantly larger number of cluster geometries limits its practicability. Recently, machine learning potentials (MLP) that are learned from DFT calculations gained significant attention as computationally cheap alternative options that provide DFT level accuracy. As the accuracy of the MLP predictions is dependent on the quality and quantity of the training DFT data, active learning (AL) strategies have gained significant momentum to bypass the need of large and representative training data. In this application note, we present Cluster-MLP, an on-the-fly active learning genetic algorithm framework that employs the Flare++ machine learning potential (MLP) for accelerating the GA search for global minima of pure and alloyed nanoclusters. We have used a modified version the Birmingham parallel genetic algorithm (BPGA) for the nanocluster GA search which is then incorporated into distributed evolutionary algorithms in Python (DEAP), an evolutionary computational framework for fast prototyping or technical experiments. We have shown that the incorporation of the AL framework in the BPGA significantly reduced the computationally expensive DFT calculations. Moreover, we have shown that both the AL-GA and DFT-GA predict the same global minima for all the clusters we tested.