A Self-Attention Ansatz for Ab-initio Quantum ChemistryDownload PDF

Published: 01 Feb 2023, Last Modified: 12 Mar 2024ICLR 2023 posterReaders: Everyone
Keywords: Machine learning for science, attention, Transformers, Monte Carlo, MCMC, self-generative learning, quantum physics, chemistry, machine learning for physics, machine learning for molecules, machine learning for chemistry
TL;DR: We use a novel self-attention neural network to make quantum chemistry calculations from first principles much more accurate.
Abstract: We present a novel neural network architecture using self-attention, the Wavefunction Transformer (PsiFormer), which can be used as an approximation (or "Ansatz") for solving the many-electron Schrödinger equation, the fundamental equation for quantum chemistry and material science. This equation can be solved *from first principles*, requiring no external training data. In recent years, deep neural networks like the FermiNet and PauliNet have been used to significantly improve the accuracy of these first-principle calculations, but they lack an attention-like mechanism for gating interactions between electrons. Here we show that the PsiFormer can be used as a drop-in replacement for these other neural networks, often dramatically improving the accuracy of the calculations. On larger molecules especially, the ground state energy can be improved by dozens of kcal/mol, a qualitative leap over previous methods. This demonstrates that self-attention networks can learn complex quantum mechanical correlations between electrons, and are a promising route to reaching unprecedented accuracy in chemical calculations on larger systems.
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