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arXiv · 2301.00672

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

LeeAnn M. Sager-Smith·David A. Mazziotti
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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.

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LeeAnn M. Sager-Smith, David A. Mazziotti. 2022-12-29. Reducing the Quantum Many-electron Problem to Two Electrons with Machine Learning. https://doi.org/10.1021/jacs.2c07112

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