Three-Dimensional Convolutional Neural Networks Utilizing Molecular Topological Features for Accurate Atomization Energy Predictions

Deep learning methods provide a novel way to establish a correlation between two quantities. In this context, computer vision techniques such as three-dimensional (3D)-convolutional neural networks become a natural choice to associate a molecular property with its structure due to the inherent 3D nature of a molecule. However, traditional 3D input data structures are intrinsically sparse in nature, which tend to induce instabilities during the learning process, which in turn may lead to underfitted results. To address this deficiency, in this project, we propose to use quantum-chemically derived molecular topological features, namely, localized orbital locator and electron localization function, as molecular descriptors, which provide a relatively denser input representation in a 3D space. Such topological features provide a detailed picture of the atomic and electronic configuration and interatomic interactions in the molecule and hence are ideal for predicting properties that are highly dependent on the physical or electronic structure of the molecule. Herein, we demonstrate the efficacy of our proposed model by applying it to the task of predicting atomization energies for the QM9-G4MP2 data set, which contains ∼134k molecules. Furthermore, we incorporated the Δ-machine learning approach into our model, which enabled us to reach beyond benchmark accuracy levels (∼1.0 kJ mol-1). As a result, we consistently obtain impressive mean absolute errors of the order 0.1 kcal mol-1 (∼0.42 kJ mol-1) versus the G4(MP2) theory using relatively modest models, which could potentially be improved further in a systematic manner using additional compute resources.