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We introduce a non-iterative energy correction, added on top of the rank-reduced coupled-cluster method with single, double, and triple substitutions, that accounts for excitations excluded from the parent triple excitation subspace. The…

Chemical Physics · Physics 2022-01-06 Michał Lesiuk

We extend the CCSDTQ implementation in CFOUR to UHF and ROHF references and demonstrate its efficiency. We apply it to basis set convergence of post-CCSDT(Q) corrections for the W4-08 thermochemical dataset. Convergence of…

Chemical Physics · Physics 2026-05-20 Aditya Barman , Gregory H. Jones , Jan M. L. Martin

Two new schemes for computing molecular total atomization energies (TAEs) and/or heats of formation ($\Delta H^\circ_f$) of first-and second-row compounds to very high accuracy are presented. The more affordable scheme, W1 (Weizmann-1)…

Chemical Physics · Physics 2009-10-31 Jan M. L. Martin , Glenisson de Oliveira

Coupled cluster theory has had a momentous impact on the ab initio prediction of molecular properties, and remains a staple ingratiate in high-accuracy thermochemical model chemistries. However, these methods require inclusion of at least…

Chemical Physics · Physics 2025-03-26 James H. Thorpe , Zachary W. Windom , Rodney J. Bartlett , Devin A. Matthews

In an attempt to improve on our earlier W3 theory [J. Chem. Phys. {\bf 120}, 4129 (2004)] we consider such refinements as more accurate estimates for the contribution of connected quadruple excitations ($\hat{T}_4$), inclusion of connected…

Chemical Physics · Physics 2007-05-23 Amir Karton , Elena Rabinovich , Jan M. L. Martin , Branko Ruscic

We demonstrate the accuracy of ground-state energies of the transcorrelated Hamiltonian, employing sophisticated Jastrow factors obtained from variational Monte Carlo, together with the coupled cluster and distinguishable cluster methods at…

In this work, we investigate the possibility of improving multireference-driven coupled cluster (CC) approaches with an algorithm that iteratively combines complete active space (CAS) calculations with tailored CC and externally corrected…

Chemical Physics · Physics 2025-03-06 Robin Feldmann , Max Mörchen , Jakub Lang , Michał Lesiuk , Markus Reiher

A number of iterative and perturbative approximations to the full equation-of-motion coupled cluster method with single, double, and triple excitations (EOM-CCSDT) are evaluated in the context of calculating the K-edge core-excitation and…

Chemical Physics · Physics 2025-03-26 Devin A. Matthews

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

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

For noncovalent interactions, it is generally assumed that CCSD(T) is nearly the exact solution within the 1-particle basis set. For the S66 noncovalent interactions benchmark, we present for the majority of species CCSDT and CCSDT(Q)…

Chemical Physics · Physics 2025-01-22 Emmanouil Semidalas , A. Daniel Boese , Jan M. L. Martin

We incorporate a solver for the fragment problem with accuracy beyond coupled cluster singles and doubles (CCSD) into the previously proposed static embedding framework, MPCC. To this end, we employ a CCSDT solver for the fragment…

Chemical Physics · Physics 2026-02-16 Avijit Shee , Fabian M. Faulstich , K. Birgitta Whaley , Lin Lin , Martin Head-Gordon

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…

Mesoscale and Nanoscale Physics · Physics 2013-05-30 Erik Waltersson , Eva Lindroth

In order to explore the effects of high levels of electron correlation on the real-time coupled cluster formalism and algorithmic behavior, we introduce a time-dependent implementation of the CC3 singles, doubles and approximate triples…

Chemical Physics · Physics 2025-01-23 Zhe Wang , Håkon Emil Kristiansen , Thomas Bondo Pedersen , T. Daniel Crawford

When the number of strongly correlated electrons becomes larger, the single-reference coupled-cluster (CC) CCSD, CCSDT, etc. hierarchy displays an erratic behavior, while traditional multi-reference approaches may no longer be applicable…

Chemical Physics · Physics 2025-12-12 Ilias Magoulas , Jun Shen , Piotr Piecuch

Electrodynamical coupled cluster (CC) methodologies have been formulated employing standard QED Hamiltonian that is written in Coulomb gauge while using the DF and the MCDF pictures of the matter field for closed-shell and open-shell cases…

Quantum Physics · Physics 2024-01-15 Sambhu N. Datta

We investigate the accuracies of different coupled cluster levels in a finite model solid, the 14 electron spin-non-polarised uniform electron gas. For densities between $\mathrm{r}_\mathrm{s}$ = 0.5 $\mathrm{a}_\mathrm{0}$ and…

Chemical Physics · Physics 2018-03-28 Verena A. Neufeld , Alex J. W. Thom

We investigate the basis-set convergence of electronic correlation energies calculated using coupled cluster theory and a recently proposed finite basis-set correction technique. The correction is applied to atomic and molecular systems and…

Chemical Physics · Physics 2019-10-03 Andreas Irmler , Andreas Grüneis

We present a massive-parallel implementation of the resolution-of-identity (RI) coupled-cluster approach that includes single, double and perturbatively triple excitations, namely RI-CCSD(T), in the FHI-aims package for molecular systems. A…

Computational Physics · Physics 2018-10-19 Tonghao Shen , Igor Ying Zhang , Matthias Scheffler

The search for new \emph{ab initio} models rapidly delivering accurate excited state energies and properties is one of the most active research lines of theoretical chemistry. Along with these methodological developments, the performances…

Chemical Physics · Physics 2020-06-05 Pierre-François Loos , Denis Jacquemin