Electronic, redox, and optical property prediction of organic π-conjugated molecules through a hierarchy of machine learning approaches

Abstract

Accelerating the development of π-conjugated molecules for applications such as energy generation and storage, catalysis, sensing, pharmaceuticals, and (semi)conducting technologies requires rapid and accurate evaluation of the electronic, redox, or optical properties. While high-throughput computational screening has proven to be a tremendous aid in this regard, machine learning (ML) and other data-driven methods can further enable orders of magnitude reduction in time while at the same time providing dramatic increases in the chemical space that is explored. However, the lack of benchmark datasets containing the electronic, redox, and optical properties that characterize the diverse, known chemical space of organic π-conjugated molecules limits ML model development. Here, we present a curated dataset containing 25k molecules with density functional theory (DFT) and time-dependent DFT (TDDFT) evaluated properties that include frontier molecular orbitals, ionization energies, relaxation energies, and low-lying optical excitation energies. Using the dataset, we train a hierarchy of ML models, ranging from classical models such as ridge regression to sophisticated graph neural networks, with molecular SMILES representation as input. We observe that graph neural networks augmented with contextual information allow for significantly better predictions across a wide array of properties. Our best-performing models also provide an uncertainty quantification for the predictions. To democratize access to the data and trained models, an interactive web platform has been developed and deployed.