Stacked Ensemble Machine Learning for Range-Separation Parameters

Abstract

Density functional theory-based high-throughput materials and drug discovery has achieved tremendous success in recent decades, but its power on organic semiconducting molecules suffered catastrophically from the self-interaction error until the nonempirical but expensive optimally tuned range-separated hybrid (OT-RSH) functionals were developed. An OT-RSH transitions from a short-range (semi)local functional to a long-range Hartree-Fock exchange at a distance characterized by a molecule-specific range-separation parameter (ω). Herein, we propose a stacked ensemble machine learning model that provides an accelerated alternative of OT-RSH based on system-dependent structural and electronic configurations. We trained ML-ωPBE, the first functional in our series, using a database of 1970 molecules with sufficient structural and functional diversity, and assessed its accuracy and efficiency using another 1956 molecules. Compared with nonempirical OT-ωPBE, ML-ωPBE reaches a mean absolute error of 0.00504a0-1 for optimal ω's, reduces the computational cost by 2.66 orders of magnitude, and achieves comparable predictive power in optical properties.