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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

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

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

An implementation of the coupled-cluster single- and double excitations (CCSD) method on two-dimensional quantum dots is presented. Advantages and limitations are studied through comparison with other high accuracy approaches for two to…

介观与纳米尺度物理 · 物理学 2013-05-30 Erik Waltersson , Eva Lindroth

The (T) and [T] perturbative corrections are derived for multicomponent coupled-cluster theory with single and double excitations (CCSD). Benchmarking shows that multicomponent CCSD methods that include the perturbative corrections are more…

化学物理 · 物理学 2022-07-01 Dylan Fowler , Kurt R. Brorsen

Coupled-cluster theory with single and double excitations (CCSD) is a promising ab initio method for the electronic structure of three-dimensional metals, for which second-order perturbation theory (MP2) diverges in the thermodynamic limit.…

材料科学 · 物理学 2021-06-16 James M. Callahan , Malte F. Lange , Timothy C. Berkelbach

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) 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)…

化学物理 · 物理学 2025-05-05 Justin T. Phillips , Lauren N. Koulias , Stephen H. Yuwono , A. Eugene DePrince

Fourth-order many-body corrections to matrix elements for atoms with one valence electron are derived. The obtained diagrams are classified using coupled-cluster-inspired separation into contributions from n-particle excitations from the…

原子物理 · 物理学 2009-11-07 Andrei Derevianko , Erik D. Emmons

A new state specific correlation correction to configuration interaction singles (CIS) excitation energies is preseted using coupled cluster perturbation theory (CCPT). General expressions for CIS-CCPT are derived and expanded explicitly to…

化学物理 · 物理学 2015-06-19 Jason N. Byrd , Victor F. Lotrich , Rodney J. Bartlett

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

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

We have studied electron correlations in the doped two-dimensional (2D) Hubbard model by using the coupled-cluster method (CCM) to investigate whether or not the method can be applied to correct the independent particle approximations…

强关联电子 · 物理学 2009-10-31 Yoshihiro Asai , Hideki Katagiri

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

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

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,…

Electronic structure methods built around double-electron excitations have a rich history in quantum chemistry. However, it seems to be the case that such methods are only suitable in particular situations and are not naturally equipped to…

化学物理 · 物理学 2024-07-12 Zachary W. Windom , Ajith Perera , Rodney J. Bartlett

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…

化学物理 · 物理学 2016-02-25 Thomas M. Henderson , Ireneusz W. Bulik , Gustavo E. Scuseria

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…

量子物理 · 物理学 2019-01-07 Joonho Lee , William J. Huggins , Martin Head-Gordon , K. Birgitta Whaley

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…

材料科学 · 物理学 2024-02-27 Nikolaos Masios , Felix Hummel , Andreas Grüneis , Andreas Irmler
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