An ab initio foundation model of wavefunctions that accurately describes chemical bond breaking

arXiv:2506.19960v2 Announce Type: replace-cross Abstract: Reliable description of bond breaking remains a major challenge for quantum chemistry due to the multireference character of the electronic structure in dissociating species. Multireference methods in particular suffer from large computational cost, which under the normal paradigm has to be paid anew for each system at a full price, ignoring commonalities in electronic structure across molecules. Quantum Monte Carlo with deep neural networks uniquely offers to exploit such commonalities by pretraining transferable wavefunction models, but all such attempts were so far limited in scope. Here, we bring this paradigm to fruition with Orbformer, a transferable wavefunction model pretrained on 22,000 equilibrium and dissociating structures that can be fine-tuned on unseen molecules reaching an accuracy-cost ratio rivalling classical multireference methods. On established benchmarks as well as more challenging bond dissociations and Diels-Alder reactions, Orbformer is the only method that consistently converges to chemical accuracy (1 kcal/mol). This work turns the idea of amortizing the cost of solving the Schr\"odinger equation over many molecules into a practical approach in quantum chemistry.

Abstract:Reliable description of bond breaking remains a major challenge for quantum chemistry due to the multireference character of the electronic structure in dissociating species. Multireference methods in particular suffer from large computational cost, which under the normal paradigm has to be paid anew for each system at a full price, ignoring commonalities in electronic structure across molecules. Quantum Monte Carlo with deep neural networks uniquely offers to exploit such commonalities by pretraining transferable wavefunction models, but all such attempts were so far limited in scope. Here, we bring this paradigm to fruition with Orbformer, a transferable wavefunction model pretrained on 22,000 equilibrium and dissociating structures that can be fine-tuned on unseen molecules reaching an accuracy-cost ratio rivalling classical multireference methods. On established benchmarks as well as more challenging bond dissociations and Diels-Alder reactions, Orbformer is the only method that consistently converges to chemical accuracy (1 kcal/mol). This work turns the idea of amortizing the cost of solving the Schrödinger equation over many molecules into a practical approach in quantum chemistry.

Chemical Physics (physics.chem-ph); Artificial Intelligence (cs.AI); Machine Learning (stat.ML)

arXiv:2506.19960 [physics.chem-ph]

(or arXiv:2506.19960v2 [physics.chem-ph] for this version)

https://doi.org/10.48550/arXiv.2506.19960 Focus to learn more arXiv-issued DOI via DataCite

https://doi.org/10.1038/s41467-026-76604-2 Focus to learn more DOI(s) linking to related resources

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An ab initio foundation model of wavefunctions that accurately describes chemical bond breaking

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