Position: The Inevitable Transition to Machine Learning in Quantum Chemistry
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Abstract (arXiv)
Finding exact solutions to the quantum many-body problem is computationally intractable (QMA-hard). Traditional approximations for electrons in an atom or molecule -- density functional theory and wavefunction methods -- have been indispensable, but their development shows signs of saturation: DFT functionals have proliferated without converging toward the exact functional, and strong correlation remains largely unsolved after decades of effort. This position paper argues that machine learning represents the most promising path forward -- not as a proof of logical necessity, but as a decision-theoretic argument: ML succeeds whether the underlying problems are truly hard or merely lack simple analytical solutions. We reframe recent traditional method development as ``hand-crafted machine learning'' that has exhausted the hypothesis space accessible to human intuition. Significant challenges remain, but these have clear research paths forward, unlike the fundamental barriers facing traditional approaches. ML-based approaches merit strategic priority in quantum chemistry's next phase.
Key facts. No citing papers in the map yet (data through 7 Oct 2026). Builds on 16 of its 107 references that are in the map. First posted on arXiv 30 Jun 2026.
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References · 16
- 2017A Unified Approach to Interpreting Model Predictionscited by 6,488
- 2017Neural Message Passing for Quantum Chemistrycited by 3,460
- 2021E(3)-Equivariant Graph Neural Networks for Data-Efficient and Accurate Interatomic Potentialscited by 701
- 2018Barren plateaus in quantum neural network training landscapescited by 624
- 2022MACE: Higher Order Equivariant Message Passing Neural Networks for Fast and Accurate Force Fieldscited by 467
- 2021Equivariant message passing for the prediction of tensorial properties and molecular spectracited by 438
- 2022Learning Local Equivariant Representations for Large-Scale Atomistic Dynamicscited by 254
- 2019Ab-Initio Solution of the Many-Electron Schr"odinger Equation with Deep Neural Networkscited by 195
- 2023Reducing SO(3) Convolutions to SO(2) for Efficient Equivariant GNNscited by 113
- 2019Machine learning for molecular simulationcited by 109
- 2022Electronic excited states in deep variational Monte Carlocited by 21
- 2022HelixFold: An Efficient Implementation of AlphaFold2 using PaddlePaddlecited by 12
4 more
- 2023Overcoming the Barrier of Orbital-Free Density Functional Theory for Molecular Systems Using Deep Learningcited by 11
- 2025An ab initio foundation model of wavefunctions that accurately describes chemical bond breakingcited by 11
- 2024Transferable Neural Wavefunctions for Solidscited by 7
- 2026Excited Pfaffians: Generalized Neural Wave Functions Across Structure and Statecited by 1
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