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A major difficulty in quantum simulation is the adequate treatment of a large collection of entangled particles, synonymous with electron correlation in electronic structure theory, with coupled cluster (CC) theory being the leading…

化学物理 · 物理学 2024-06-06 Zachary W. Windom , Daniel Claudino , Rodney J. Bartlett

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…

化学物理 · 物理学 2025-07-28 Laura Grazioli , Marios-Petros Kitsaras , Stella Stopkowicz

We present a perturbative triples correction to the relativistic quadratic unitary coupled cluster singles and doubles (qUCCSD) method, denoted as qUCCSD[T]. The method builds upon the Hermitian structure of the unitary ansatz and employs a…

化学物理 · 物理学 2025-10-08 Kamal Majee , Ján Šimunek , Jozef Noga , Achintya Kumar Dutta

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…

化学物理 · 物理学 2025-09-08 Zachary W. Windom , Daniel Claudino

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…

化学物理 · 物理学 2026-03-03 Yu Zhang , Junzi Liu

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…

量子物理 · 物理学 2024-06-14 Zachary W. Windom , Daniel Claudino , Rodney J. Bartlett

Unitary Coupled Cluster (UCC) theory is a promising variational method for electronic structure calculations, especially for strongly correlated systems and quantum computers. However, its practical application is limited by the steep…

化学物理 · 物理学 2026-02-05 Prateek Vaish , Brenda Rubenstein

The recent quantum information boom has effected a resurgence of interest in unitary coupled cluster (UCC) theory. Our group's interest in local energy landscapes of unitary ans\"atze prompted us to investigate the classical approach of…

化学物理 · 物理学 2022-11-01 Harper R. Grimsley , Nicholas J. Mayhall

The Trotterized Unitary Coupled Cluster Single and Double (UCCSD) ansatz has recently attracted interest due to its use in Variation Quantum Eigensolver (VQE) molecular simulations on quantum computers. However, when the size of molecules…

化学物理 · 物理学 2023-05-29 Mohammad Haidar , Marko J. Rančić , Yvon Maday , Jean-Philip Piquemal

Unitary coupled cluster (UCC), originally developed as a variational alternative to the popular traditional coupled cluster method, has seen a resurgence as a functional form for use on quantum computers. However, the number of excitors…

化学物理 · 物理学 2021-01-07 Maria-Andreea Filip , Alex J. W. Thom

In truncated coupled-cluster (CC) theories, non-variational and/or generally complex ground-state energies can occur. This is due to the non-Hermitian nature of the similarity transformed Hamiltonian matrix in combination with CC…

化学物理 · 物理学 2023-09-22 Tanner Culpitt , Erik I. Tellgren , Fabijan Pavosevic

We propose a relativistic unitary coupled cluster (UCC) expectation value approach for computing first-order properties of heavy-element systems. Both perturbative (UCC3) and non-perturbative (qUCC) commutator-based formulations are applied…

化学物理 · 物理学 2026-02-03 Kamal Majee , Somesh Chamoli , Malaya K. Nayak , Achintya Kumar Dutta

We present a four-component relativistic unitary coupled cluster method for molecules. We have used commutator-based non-perturbative approximation using the ''Bernoulli expansion'' to derive an approximation to the relativistic unitary…

化学物理 · 物理学 2024-03-06 Kamal Majee , Tamoghna Mukhopadhyay , Malaya K. Nayak , Achintya Kumar Dutta

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…

化学物理 · 物理学 2025-08-14 Zachary W. Windom , Luke Bertels , Daniel Claudino , Rodney J. Bartlett

An efficiency of the Tucker decomposition of amplitude tensors within the single-reference relativistic coupled cluster method with single and double excitations (RCCSD) was studied in a series of benchmark calculations for (AuCl)$_n$…

The Coupled Cluster (CC) method is used to compute the electronic correlation energy in atoms and molecules and often leads to highly accurate results. However, due to its single-reference nature, standard CC in its projected form fails to…

The development of a quadratic unitary coupled-cluster singles and doubles (qUCCSD) based self-consistent polarization propagator method is reported. We present a simple strategy for truncating the commutator expansion of the UCC…

化学物理 · 物理学 2024-06-19 Junzi Liu , Lan Cheng

This work introduces various approaches to include connected three-body terms in unitary many-body theories, focusing a representative example on the driven similarity renormalization group (DSRG). Starting from the least approximate method…

化学物理 · 物理学 2020-07-15 Chenyang Li , Francesco A. Evangelista

The unitary coupled cluster (UCC) approximation is one of the more promising wave-function ans\"atze for electronic structure calculations on quantum computers via the variational quantum eigensolver algorithm. However, for large systems…

量子物理 · 物理学 2021-09-30 Jia Chen , Hai-Ping Cheng , James K. Freericks

We introduce a range-separation approximation to coupled cluster doubles (CCD) theory that successfully overcomes limitations of regular CCD when applied to the uniform electron gas. We combine the short-range ladder channel with the…

化学物理 · 物理学 2014-05-07 James J. Shepherd , Thomas M. Henderson , Gustavo E. Scuseria
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