Reducing the Quantum Many-Electron Problem to Two Electrons with Machine Learning.

Abstract

An outstanding challenge in chemical computation is the many-electron problem where computational methodologies scale prohibitively with system size. The energy of any molecule can be expressed as a weighted sum of the energies of two-electron wave functions that are computable from only a two-electron calculation. Despite the physical elegance of this extended "aufbau" principle, the determination of the distribution of weights─geminal occupations─for general molecular systems has remained elusive. Here we introduce a new paradigm for electronic structure where approximate geminal-occupation distributions are "learned" via a convolutional neural network. We show that the neural network learns the N-representability conditions, constraints on the distribution for it to represent an N-electron system. By training on hydrocarbon isomers with only 2-7 carbon atoms, we are able to predict the energies for isomers of octane as well as hydrocarbons with 8-15 carbons. The present work demonstrates that machine learning can be used to reduce the many-electron problem to an effective two-electron problem, opening new opportunities for accurately predicting electronic structure.