Quantum computing for accurate large-scale electronic-structure calculations: DFT-embedded, post-processed quantum-selected configuration interaction

Abstract:We present a multilevel embedding framework for quantum chemistry calculations on a quantum computer. In our framework, a quantum algorithm treats the strongly correlated active space, while a high-level wave-function method such as coupled cluster theory or multireference perturbation theory recovers the remaining correlation in the surrounding region. A sampling-based quantum algorithm, quantum-selected configuration interaction, bridges the quantum and classical treatments. The entire calculation is embedded in a low-cost density functional theory description of the surrounding environment using Manby's projection technique. We apply the framework to organic, metal-organic, and metallic systems, computing bond dissociation energies, adsorption energies, and reaction barriers using only the subset of qubits of a 144-qubit superconducting quantum computer at the University of Osaka and achieving $\sim$1 kcal/mol agreement with classical references for a Menshutkin $\mathrm{S_N2}$ reaction inside a carbon nanotube. Our results may open the way to quantitatively reliable quantum-classical hybrid calculations for large-scale chemical systems.

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

arXiv:2606.06015 [physics.chem-ph]

(or arXiv:2606.06015v1 [physics.chem-ph] for this version)

https://doi.org/10.48550/arXiv.2606.06015 Focus to learn more arXiv-issued DOI via DataCite (pending registration)

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