Coupled cluster method tailored by quantum selected configuration interaction

TL;DR

The paper introduces QSCI-TCC, a hybrid quantum-classical method that effectively captures static and dynamic electron correlation, enabling accurate quantum-chemical calculations with fewer quantum resources.

Contribution

It presents a novel quantum-selected configuration interaction-tailored coupled-cluster approach that improves accuracy and efficiency over traditional methods in strongly correlated systems.

Findings

QSCI-TCC accurately models bond dissociation in H₂O and N₂.

The method achieves chemical accuracy with significantly fewer quantum shots.

It outperforms traditional CCSD and CCSD(T) in strongly correlated regimes.

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 H$_2$O and the triple-bond dissociation in N$_2$. 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 N$_2$ (6e, 6o) active space demonstrate that, with the (c) correction, chemically sufficient precision ($\leq 1$ kcal/mol) is achieved with only $1.0 \times 10^5$ shots in the strongly correlated regime ($r=2.2$ \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.