From sparse quantum-computing data to atomistic simulation with universal machine-learning interatomic potentials

arXiv:2609.21536v1 Announce Type: cross Abstract: We propose a framework for incorporating quantum-computing-based electronic-structure calculations into universal machine-learning interatomic potentials (uMLIPs). Rather than constructing an interatomic potential from scratch, we refine a pretrained DFT-based uMLIP using a small set of accurate reference energies obtained from quantum computing. We demonstrate the approach for three chemically distinct applications: the Menshutkin reaction, water adsorption in the metal-organic framework HKUST-1, and CO hopping on a high-entropy-alloy nanoparticle. For the Menshutkin reaction, fine-tuning on gas-phase configurations improves the transition-state energy inside a carbon nanotube but not the product energy. For water adsorption in HKUST-1, fine-tuning with only 14 reference configurations brings adsorption thermodynamics obtained from millions of configurations sampled by Widom insertion into closer agreement with reference values. For CO hopping on an IrPdPtRhRu nanoparticle, the preference for on-top over bridge adsorption is recovered in the finite-temperature free-energy profile obtained from enhanced-sampling molecular dynamics, even though the reference data contain only energies. These results demonstrate that the proposed framework provides a practical route for incorporating quantum-computing calculations into realistic atomistic simulations and that quantum-computing reference data can improve pretrained uMLIPs.

Abstract:We propose a framework for incorporating quantum-computing-based electronic-structure calculations into universal machine-learning interatomic potentials (uMLIPs). Rather than constructing an interatomic potential from scratch, we refine a pretrained DFT-based uMLIP using a small set of accurate reference energies obtained from quantum computing. We demonstrate the approach for three chemically distinct applications: the Menshutkin reaction, water adsorption in the metal-organic framework HKUST-1, and CO hopping on a high-entropy-alloy nanoparticle. For the Menshutkin reaction, fine-tuning on gas-phase configurations improves the transition-state energy inside a carbon nanotube but not the product energy. For water adsorption in HKUST-1, fine-tuning with only 14 reference configurations brings adsorption thermodynamics obtained from millions of configurations sampled by Widom insertion into closer agreement with reference values. For CO hopping on an IrPdPtRhRu nanoparticle, the preference for on-top over bridge adsorption is recovered in the finite-temperature free-energy profile obtained from enhanced-sampling molecular dynamics, even though the reference data contain only energies. These results demonstrate that the proposed framework provides a practical route for incorporating quantum-computing calculations into realistic atomistic simulations and that quantum-computing reference data can improve pretrained uMLIPs.

Chemical Physics (physics.chem-ph); Quantum Physics (quant-ph)

arXiv:2609.21536 [physics.chem-ph]

(or arXiv:2609.21536v1 [physics.chem-ph] for this version)

https://doi.org/10.48550/arXiv.2609.21536 Focus to learn more arXiv-issued DOI via DataCite (pending registration)

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From sparse quantum-computing data to atomistic simulation with universal machine-learning interatomic potentials

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