Orbital Mixer: Using Atomic Orbital Features for Basis Dependent Prediction of Molecular Wavefunctions

Abstract

Leveraging ab initio data at scale has enabled the development of machine learning models capable of extremely accurate and fast molecular property prediction. A central paradigm of many previous works focuses on generating predictions for only a fixed set of properties. Recent lines of research instead aim to explicitly learn the electronic structure via molecular wavefunctions from which other quantum chemical properties can directly be derived. While previous methods generate predictions as a function of only the atomic configuration, in this work we present an alternate approach that directly purposes basis dependent information to predict molecular electronic structure. The backbone of our model, Orbital Mixer, uses MLP Mixer layers within a simple, intuitive, and scalable architecture and achieves competitive Hamiltonian and molecular orbital energy and coefficient prediction accuracies compared to the state-of-the-art.

Orbital Mixer: Using Atomic Orbital Features for Basis-Dependent Prediction of Molecular Wavefunctions

“…A full accounting of all neural network, optimizer, and scheduler hyperparameters is provided in the Supporting Information along with a complete PyTorch 61 implementation using PyTorch Lightning 62 publicly available at doi: 10.18126/ cu4h-d2mm. 63…”