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The unitary coupled cluster (UCC) algorithm is one of the most promising implementations of the variational quantum eigensolver for quantum computers. However, for large systems, the number of UCC factors leads to deep quantum circuits,…

Quantum Physics · Physics 2026-02-17 Jeremy Canfield , Dominika Zgid , J K Freericks

We report a complete implementation of the coupled-cluster method with single, double, and triple excitations (CCSDT) where tensor decompositions are used to reduce its scaling and overall computational costs. For the decomposition of the…

Chemical Physics · Physics 2020-02-20 Michał Lesiuk

A unitary coupled-cluster (UCC)-based self-consistent electron propagator theory (EPT) is proposed for the description of electron-detached and electron-attached states. Two practical schemes, termed IP/EA-UCC3 and IP/EA-qUCCSD, are…

Chemical Physics · Physics 2026-03-03 Yu Zhang , Junzi Liu

Heavy atom compounds represent a challenge for computational chemistry, due to the need for simultaneous treatment of relativistic and correlation effects. Often such systems exhibit also strong correlation which hampers the application of…

Chemical Physics · Physics 2025-02-10 Jakub Višňák , Jan Brandejs , Mihály Máté , Lucas Visscher , Örs Legeza , Jiří Pittner

In this work, we introduce a correction to the unitary coupled cluster method with single and double excitations (UCCSD) that incorporates the effects of missing triple excitations through a treatment that is correct through fifth-order in…

Chemical Physics · Physics 2025-09-08 Zachary W. Windom , Daniel Claudino

Coupled cluster methods based exclusively on double excitations are comparatively "cheap" and interesting model chemistries, as they are typically able to capture the bulk of the dynamical electron correlation effects. The trade-off in such…

Quantum Physics · Physics 2024-06-14 Zachary W. Windom , Daniel Claudino , Rodney J. Bartlett

We propose a non-iterative, post hoc correction to the unitary coupled cluster theory with single, double, and triple excitations (UCCSDT) ansatz, which considers the leading-order effects of neglected quadruple excitations. We present two…

Chemical Physics · Physics 2025-08-14 Zachary W. Windom , Luke Bertels , Daniel Claudino , Rodney J. Bartlett

We present an efficient algorithm for one- and two-component relativistic exact-decoupling calculations. Spin-orbit coupling is thus taken into account for the evaluation of relativistically transformed (one-electron) Hamiltonian. As the…

Chemical Physics · Physics 2013-05-10 Daoling Peng , Nils Middendorf , Florian Weigend , Markus Reiher

We introduce a unitary coupled-cluster (UCC) ansatz termed $k$-UpCCGSD that is based on a family of sparse generalized doubles (D) operators which provides an affordable and systematically improvable unitary coupled-cluster wavefunction…

Quantum Physics · Physics 2019-01-07 Joonho Lee , William J. Huggins , Martin Head-Gordon , K. Birgitta Whaley

"Addition-by-subtraction" coupled cluster (CC) approaches provide a promising approach to treating the difficult strong correlation problem by simplifying the standard CC equations. In a separate vein, linearized CC methods have drawn…

Strongly Correlated Electrons · Physics 2026-03-02 Sylvia J. Bintrim , Ella R. Ransford , Kevin Carter-Fenk

We introduce a hybrid quantum-classical algorithm, the localized active space unitary selective coupled cluster singles and doubles (LAS-USCCSD) method. Derived from the localized active space unitary coupled cluster (LAS-UCCSD) method,…

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

We tabulate angularly reduced fourth-order many-body corrections to matrix elements for univalent atoms, derived in [A. Derevianko and E.D. Emmons, Phys. Rev. A 65, 052115 (2002)]. In particular we focused on practically important diagrams…

Atomic Physics · Physics 2007-05-23 Andrei Derevianko

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

We present a new method for state preparation using the Unitary Vibrational Coupled-Cluster (UVCC) technique. Our approach utilizes redundancies in the Hilbert space in the direct mapping of vibrational modes into qubits. By eliminating…

Quantum Physics · Physics 2024-12-06 Michal Szczepanik , Emil Zak

A new method that accurately describes strongly correlated states and captures dynamical correlation is presented. It is derived as a modification of coupled-cluster theory with single and double excitations (CCSD) through consideration of…

Chemical Physics · Physics 2013-07-15 Daniel Kats , Frederick R. Manby

The previously proposed ansatz for density cumulant theory that combines orbital-optimization and a parameterization of the 2-electron reduced density matrix cumulant in terms of unitary coupled cluster amplitudes (OUDCT) is carefully…

Chemical Physics · Physics 2020-12-23 Jonathon P. Misiewicz , Justin M. Turney , Henry F. Schaefer , Alexander Yu. Sokolov

It is shown that four-component (4C), quasi-four-component (Q4C), and exact two-component (X2C) relativistic Hartree-Fock (HF) equations can be implemented in an unified manner, by making use of the atomic nature of the small components of…

Chemical Physics · Physics 2023-11-28 Wenjian Liu

Unitary Coupled Cluster (UCC) approaches are an appealing route to utilising quantum hardware to perform quantum chemistry calculations, as quantum computers can in principle perform UCC calculations in a polynomially scaling fashion, as…

Quantum Physics · Physics 2022-06-15 Maria-Andreea Filip , Nathan Fitzpatrick , David Muñoz Ramo , Alex J. W. Thom

Conventional clustering methods based on pairwise affinity usually suffer from the concentration effect while processing huge dimensional features yet low sample sizes data, resulting in inaccuracy to encode the sample proximity and…

Machine Learning · Computer Science 2023-02-06 Hongmin Cai , Fei Qi , Junyu Li , Yu Hu , Yue Zhang , Yiu-ming Cheung , Bin Hu