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A rigorous generation of spin-adapted (spin-free) substitution operators for high spin ($S=S_z$) references of arbitrary substitution order and spin quantum number $S$ is presented. The generated operators lead to linearly independent but…

Chemical Physics · Physics 2023-03-06 Nils Herrmann , Michael Hanrath

In spin-adapted open-shell coupled cluster (CC) theory, the choice of spin-free spatial substitution operators is generally not unique. Due to an increasing linear dependence of the cluster operator (with increasing substitution level), the…

Chemical Physics · Physics 2022-04-27 Nils Herrmann , Michael Hanrath

We have presented the theory, implementation, and benchmark results for the one-electronic variant of spin-free exact two-component (SFX2C1e) linear response coupled cluster (LRCCSD) theory for static and dynamic polarizabilities of atoms…

Chemical Physics · Physics 2024-05-31 Sudipta Chakraborty , Tamoghna Mukhopadhyay , Achintya Kumar Dutta

The extension of the highly-optimized local natural orbital (LNO) CCSD(T) method is presented for high-spin open-shell molecules. The techniques enabling the outstanding efficiency of the closed-shell LNO-CCSD(T) variant are adopted,…

Chemical Physics · Physics 2023-11-17 P. Bernát Szabó , József Csóka , Mihály Kállay , Péter R. Nagy

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 consider the rank-reduced coupled-cluster theory with single and double excitations (RR-CCSD) introduced recently [Parrish \emph{et al.}, J. Chem. Phys. {\bf 150}, 164118 (2019)]. The main feature of this method is the decomposed form of…

Chemical Physics · Physics 2022-02-21 Michał Lesiuk

We present a general-order spin-free formulation of the single-reference closed-shell coupled-cluster method. We show that the working equations of a fully biorthogonal contravariant projection formulation of the residual equations, as…

Chemical Physics · Physics 2018-05-03 Cong Wang , Gerald Knizia

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)…

Chemical Physics · Physics 2016-05-17 Janus Juul Eriksen , Devin A. Matthews , Poul Jørgensen , Jürgen Gauss

In this paper, an efficient implementation of the renormalized internally-contracted multreference coupled cluster with singles and doubles (RIC-MRCCSD) into the ORCA quantum chemistry program suite is reported. To this end, Evangelista's…

Chemical Physics · Physics 2026-04-24 Kalman Szenes , Riya Kayal , Kantharuban Sivalingam , Robin Feldmann , Frank Neese , Markus Reiher

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

We present a near-linear scaling formulation of the explicitly-correlated coupled-cluster singles and doubles with perturbative triples method (CCSD(T)$_{\overline{\text{F12}}}$) for high-spin states of open-shell species. The approach is…

Chemical Physics · Physics 2024-07-30 Ashutosh Kumar , Frank Neese , Edward F. Valeev

Selected configuration interaction (SCI) methods, when complemented with a second-order perturbative correction, provide near full configuration interaction (FCI) quality energies with only a small fraction of the Slater determinants of the…

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

We present a spin-free, size-extensive, and size-consistent coupled cluster method based on a generalised normal ordered exponential ansatz. This approach is a natural generalisation of single-reference coupled cluster theory for arbitrary…

Chemical Physics · Physics 2025-07-21 Nicholas Lee , David P. Tew

We present and benchmark a quantum computing approach to calculate the two-dimensional coherent spectrum (2DCS) of high-spin models. Our approach is based on simulating their real-time dynamics in the presence of several magnetic field…

Quantum Physics · Physics 2024-07-02 Martin Mootz , Peter P. Orth , Chuankun Huang , Liang Luo , Jigang Wang , Yong-Xin Yao

We propose a size-consistent generalization of the recently developed spin-extended configuration interaction with singles and doubles (ECISD), where a CI wave function is explicitly spin-projected. The size-consistent effect is effectively…

Chemical Physics · Physics 2017-01-25 Takashi Tsuchimochi , Seiichiro Ten-no

A novel implementation of the coupled-cluster singles and doubles (CCSD) approach is presented that is specifically tailored for the treatment of large, symmetric systems. It fully exploits Abelian point-group symmetry and the use of the…

Chemical Physics · Physics 2023-12-07 Tommaso Nottoli , Jürgen Gauss , Filippo Lipparini

Spin Hamiltonians, like the Heisenberg model, are used to describe magnetic properties of exchange-coupled molecules and solids. For finite clusters, physical quantities such as heat capacities, magnetic susceptibilities or…

Strongly Correlated Electrons · Physics 2025-06-24 Shadan Ghassemi Tabrizi , Thomas D. Kühne

The dual exponential coupled cluster (CC) theory proposed by Tribedi et al.[J. Chem. Theory Comput. 2020, 16, 10, 6317-6328] performs significantly better than the coupled cluster theory with singles and doubles excitations (CCSD) due to…

Computational Physics · Physics 2023-07-26 Anish Chakraborty , Rahul Maitra

We present a basis set correction scheme for the coupled-cluster singles and doubles (CCSD) method. The scheme is based on employing frozen natural orbitals (FNOs) and diagrammatically decomposed contributions to the electronic correlation…

Materials Science · Physics 2021-06-18 Andreas Irmler , Alejandro Gallo , Andreas Grüneis
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