Quantum Computing Enabled ab initio Molecular Dynamics Simulations

Abstract:We demonstrate a quantum-classical workflow for ab initio molecular dynamics (AIMD) in which quantum measurements from a chemistry-inspired LUCJ ansatz are post-processed using Sample-based Quantum Diagonalization (SQD) to recover determinant subspaces and deliver energies and analytical nuclear gradients for dynamics. As an exact benchmark, we use full configuration interaction (FCI) in the STO-3G basis, enabling a direct assessment of the accuracy of SQD. In gas-phase benchmarks, SQD reproduces FCI energies and gradients to within 1 kcal mol$^{-1}$ of the FCI reference and yields stable AIMD trajectories. In explicit-solvent QM/MM simulations, SQD retains this agreement, matching FCI energy fluctuations and RMS gradient profiles and reproducing solute-solvent structure as quantified by radial distribution functions. Overall, these benchmarks establish LUCJ+SQD as a practical route for integrating current quantum hardware into QM/MM molecular dynamics and provide an early demonstration of condensed-phase QM/MM dynamics driven by a quantum electronic-structure engine.

45 pages, 7 figures. Supporting Information included as an ancillary file

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

arXiv:2607.28548 [physics.chem-ph]

(or arXiv:2607.28548v1 [physics.chem-ph] for this version)

https://doi.org/10.48550/arXiv.2607.28548 Focus to learn more arXiv-issued DOI via DataCite (pending registration)

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