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We describe further details of the Stochastic Coupled Cluster method and a diagnostic of such calculations, the shoulder height, akin to the plateau found in Full Configuration Interaction Quantum Monte Carlo. We describe an initiator…

化学物理 · 物理学 2016-03-23 James S. Spencer , Alex J. W. Thom

Coupled-cluster theory with single, double, and perturbative triple excitations (CCSD(T)) -- often considered the "gold standard" of main-group quantum chemistry -- is inapplicable to three-dimensional metals due to an infrared divergence,…

材料科学 · 物理学 2023-03-21 Verena A. Neufeld , Timothy C. Berkelbach

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

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

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 streamlined combination scheme of the transcorrelation (TC) and coupled cluster (CC) theory, which not only increases the convergence rate with respect to the basis set, but also extends the applicability of the lowest order CC…

强关联电子 · 物理学 2021-07-28 Ke Liao , Thomas Schraivogel , Hongjun Luo , Daniel Kats , Ali Alavi

We present a novel combination of quantum Monte Carlo methods and a finite size extrapolation framework with which we calculate the thermodynamic limit of the exact correlation energy of the polarized electron gas at high densities to meV…

强关联电子 · 物理学 2018-10-17 Michele Ruggeri , Pablo López Ríos , Ali Alavi

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 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

The accuracy at which total energies of open-shell atoms and organic radicals may be calculated is assessed for selected coupled cluster perturbative triples expansions, all of which augment the coupled cluster singles and doubles (CCSD)…

化学物理 · 物理学 2016-05-17 Janus Juul Eriksen , Devin A. Matthews , Poul Jørgensen , Jürgen Gauss

Metallic solids are a challenging target for wavefunction-based electronic structure theories and have not been studied in great detail by such methods. Here, we use coupled-cluster theory with single and double excitations (CCSD) to study…

材料科学 · 物理学 2022-04-05 Verena A. Neufeld , Hong-Zhou Ye , Timothy C. Berkelbach

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…

化学物理 · 物理学 2020-02-20 Michał Lesiuk

Basis set convergence of correlation effects on molecular atomization energies beyond the CCSD (coupled cluster with singles and doubles) approximation has been studied near the one-particle basis set limit. Quasiperturbative connected…

化学物理 · 物理学 2008-08-17 Amir Karton , Peter R. Taylor , Jan M. L. Martin

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

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

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,…

We discuss diagrammatic modifications to the coupled cluster doubles (CCD) equations, wherein different groups of terms out of rings, ladders, crossed-rings and mosaics can be removed to form approximations to the coupled cluster method, of…

化学物理 · 物理学 2014-05-06 James J. Shepherd , Thomas. M. Henderson , Gustavo E. Scuseria

Coupled-cluster theories can be used to compute ab initio electronic correlation energies of real materials with systematically improvable accuracy. However, the widely-used coupled cluster singles and doubles plus perturbative triples…

材料科学 · 物理学 2024-03-01 Nikolaos Masios , Andreas Irmler , Tobias Schäfer , Andreas Grüneis

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…

化学物理 · 物理学 2013-07-15 Daniel Kats , Frederick R. Manby

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
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