Chembot: A Machine Learning Approach to Selective Configuration Interaction

We introduce a machine learning-based approach to selective configuration interaction, dubbed Chembot, that utilizes many novel choices for its model design and training. These choices include the use of a support vector machine to select important configurations, the use of the charge density matrix and configuration energy as features, and heuristics to improve the quality of training data. We test Chembot’s ability to obtain near full configuration interaction quality energies and find that it definitively outperforms its purely Stochastic cousin Monte Carlo configuration interaction by requiring fewer iterations to converge, fewer determinants in the variational space, and fewer important configurations to achieve the same energy. In addition, Chembot at times requires fewer determinants in its variational space than the heat-bath configuration interaction method to achieve the same energy. We demystify Chembot’s innards and then showcase our claims on the set of small but challenging systems: the hydrogen ring (H4), stretched methylene (H2C), and stretched water (H2O).