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In single-reference coupled-cluster (CC) methods, one has to solve a set of non-linear polynomial equations in order to determine the so-called amplitudes which are then used to compute the energy and other properties. Although it is of…

Chemical Physics · Physics 2021-09-10 Antoine Marie , Fábris Kossoski , Pierre-François Loos

The standard and renormalized coupled cluster methods with singles, doubles, and noniterative triples and their generalizations to excited states, based on the equation of motion coupled cluster approach, are applied to the He-4 and O-16…

Nuclear Theory · Physics 2009-11-10 K. Kowalski , D. J. Dean , M. Hjorth-Jensen , T. Papenbrock , P. Piecuch

The factorized form of the unitary coupled cluster ansatz is a popular state preparation ansatz for electronic structure calculations of molecules on quantum computers. It often is viewed as an approximation (based on the Trotter product…

Chemical Physics · Physics 2022-02-16 Jia Chen , Hai-Ping Cheng , J. K. Freericks

The simulation of molecular electronic structure is an important application of quantum devices. Recently, it has been shown that quantum devices can be effectively combined with classical supercomputing centers in the context of the…

Quantum Physics · Physics 2025-02-28 Stefano Barison , Javier Robledo Moreno , Mario Motta

Fault-tolerant quantum computation (FTQC) is essential to implement quantum algorithms in a noise-resilient way, and thus to enjoy advantages of quantum computers even with presence of noise. In FTQC, a quantum circuit is decomposed into…

Quantum Physics · Physics 2025-07-23 Kohdai Kuroiwa , Yuya O. Nakagawa

Unitary coupled cluster (UCC) theory offers a promising Hermitian alternative to conventional coupled cluster (CC) theory, but its practical implementation is hindered by the non-truncating nature of the Baker-Campbell-Hausdorff (BCH)…

Chemical Physics · Physics 2025-05-05 Justin T. Phillips , Lauren N. Koulias , Stephen H. Yuwono , A. Eugene DePrince

In Coupled-Cluster (CC) theory, unphysical complex energies may arise in the presence of strong magnetic fields, near conical intersections, or in systems exhibiting complex Abelian point group symmetries. This issue originates from the…

Chemical Physics · Physics 2025-07-28 Laura Grazioli , Marios-Petros Kitsaras , Stella Stopkowicz

The accurate and efficient description of strongly correlated systems remains an important challenge for computational methods. Doubly occupied configuration interaction (DOCI), in which all electrons are paired and no correlations which…

Chemical Physics · Physics 2016-02-25 Thomas M. Henderson , Ireneusz W. Bulik , Gustavo E. Scuseria

An extensive analysis has been carried out of the performance of standard families of basis sets with the hierarchy of coupled cluster methods CC2, CCSD, CC3 and CCSDT in computing selected Oxygen, Carbon and Nitrogen K-edge (vertical) core…

Chemical Physics · Physics 2019-08-13 Johanna P. Carbone , Lan Cheng , Rolf H. Myhre , Devin Matthews , Henrik Koch , Sonia Coriani

In this work, we revisited the idea of using the coupled-cluster ground state formalism to target excited states. Our main focus was targeting doubly excited states and double core hole states. Typical equation-of-motion (EOM) approaches…

Chemical Physics · Physics 2019-12-04 Joonho Lee , David W. Small , Martin Head-Gordon

We investigate the convergence of coupled-cluster correlation energies and related quantities with respect to the employed basis set size for the uniform electron gas to gain a better understanding of the basis set incompleteness error. To…

Materials Science · Physics 2024-02-27 Nikolaos Masios , Felix Hummel , Andreas Grüneis , Andreas Irmler

The unitary cluster Jastrow (UCJ) ansatz and its variant known as local UCJ (LUCJ) are promising choices for variational quantum algorithms for chemistry due to their combination of physical motivation and hardware efficiency. The…

Quantum Physics · Physics 2025-12-01 Wan-Hsuan Lin , Fangchun Liang , Mario Motta , Haimeng Zhang , Kenneth M. Merz , Kevin J. Sung

We investigate the use of orbital-optimized references in conjunction with single-reference coupled-cluster theory with single and double substitutions (CCSD) for the study of core excitations and ionizations of 18 small organic molecules,…

Applications of quantum simulation algorithms to obtain electronic energies of molecules on noisy intermediate-scale quantum (NISQ) devices require careful consideration of resources describing the complex electron correlation effects. In…

Quantum Physics · Physics 2020-04-17 Mekena Metcalf , Nicholas P. Bauman , Karol Kowalski , Wibe A. de Jong

A relativistic version of the coupled-cluster single-double (CCSD) method is developed for atoms with a single valence electron. In earlier work, a linearized version of the CCSD method (with extensions to include a dominant class of triple…

Atomic Physics · Physics 2009-11-13 Rupsi Pal , M. S. Safronova , W. R. Johnson , Andrei Derevianko , Sergey G. Porsev

The tailored coupled cluster (TCC) approach is a promising ansatz that preserves the simplicity of single-reference coupled cluster theory, while incorporating a multi-reference wave function through amplitudes obtained from a preceding…

Chemical Physics · Physics 2021-01-07 Maximilian Mörchen , Leon Freitag , Markus Reiher

We introduce an approach to improve single-reference coupled cluster theory in settings where the Aufbau determinant is absent from or plays only a small role in the true wave function. Using a de-excitation operator that can be efficiently…

Chemical Physics · Physics 2024-07-03 Harrison Tuckman , Eric Neuscamman

Variational quantum eigensolver (VQE) for electronic structure calculations is believed to be one major potential application of near term quantum computing. Among all proposed VQE algorithms, the unitary coupled cluster singles and doubles…

Quantum Physics · Physics 2020-10-13 Rongxin Xia , Sabre Kais

We describe a compilation strategy for Variational Quantum Eigensolver (VQE) algorithms which use the Unitary Coupled Cluster (UCC) ansatz, designed to reduce circuit depth and gate count. This is achieved by partitioning Pauli exponential…

Quantum Physics · Physics 2020-08-28 Alexander Cowtan , Will Simmons , Ross Duncan

Quantum Phase Estimation (QPE), the quantum algorithm for estimating eigenvalues of a given Hermitian matrix and preparing its eigenvectors, is considered the most promising approach to finding the ground states and their energies of…