English

Coupled cluster method tailored by quantum selected configuration interaction

Chemical Physics 2025-06-23 v1 Quantum Physics

Abstract

We present the quantum-selected configuration interaction-tailored coupled-cluster (QSCI-TCC) method, a hybrid quantum-classical scheme that tailors coupled-cluster (CC) theory with a quantum-selected configuration interaction (QSCI) wave function. QSCI provides a scalable, shot-efficient approach to reconstructing the many-electron state prepared on quantum hardware on a classical computer. The resulting active-space CI coefficients, which are free from additive shot noise, are mapped to fixed cluster amplitudes within the tailored coupled-cluster framework, after which a conventional CC calculation optimizes the remaining amplitudes. This workflow embeds static (strong) correlation from the quantum device and subsequently recovers dynamical (weak) correlation, yielding a balanced description of both. The method is classically simulated and applied to the simultaneous O-H bond dissociation in H2_2O and the triple-bond dissociation in N2_2. QSCI-TCC and its perturbative-triples variant, QSCI-TCC(T), provide accurate results even where CCSD or CCSD(T) begin to break down. Shot-count tests for the N2_2 (6e, 6o) active space demonstrate that, with the (c) correction, chemically sufficient precision (1\leq 1 kcal/mol) is achieved with only 1.0×1051.0 \times 10^5 shots in the strongly correlated regime (r=2.2r=2.2 \r{A}) -- an order of magnitude fewer than required by an earlier matchgate-shadows implementation [J. Chem. Theory Comput., 20, 5068 (2024)]. By pairing resource-efficient quantum sampling with the CC theory, QSCI-TCC provides a promising pathway to quantum-chemical calculations of classically intractable systems.

Keywords

Cite

@article{arxiv.2506.16911,
  title  = {Coupled cluster method tailored by quantum selected configuration interaction},
  author = {Luca Erhart and Yuichiro Yoshida and Wataru Mizukami},
  journal= {arXiv preprint arXiv:2506.16911},
  year   = {2025}
}

Comments

9 pages, 4 figures

R2 v1 2026-07-01T03:26:27.666Z