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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

We recently proposed a novel approach to converging electronic energies equivalent to high-level coupled-cluster (CC) computations by combining the deterministic CC($P$;$Q$) formalism with the stochastic configuration interaction (CI) and…

Chemical Physics · Physics 2021-03-23 J. Emiliano Deustua , Jun Shen , Piotr Piecuch

We present an efficient algorithm for one- and two-component relativistic exact-decoupling calculations. Spin-orbit coupling is thus taken into account for the evaluation of relativistically transformed (one-electron) Hamiltonian. As the…

Chemical Physics · Physics 2013-05-10 Daoling Peng , Nils Middendorf , Florian Weigend , Markus Reiher

Numerous numerical studies have shown that geminal-based methods are a promising direction to model strongly correlated systems with low computational costs. Several strategies have been introduced to capture the missing dynamical…

Chemical Physics · Physics 2023-03-22 Artur Nowak , Katharina Boguslawski

An externally corrected coupled cluster (CC) method, where an adaptive configuration interaction (ACI) wave function provides the external cluster amplitudes, named ACI-CC, is presented. By exploiting the connection between configuration…

Chemical Physics · Physics 2023-09-27 Gustavo J. R. Aroeira , Madeline M. Davis , Justin M. Turney , Henry F. Schaefer

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.…

Materials Science · Physics 2021-06-16 James M. Callahan , Malte F. Lange , Timothy C. Berkelbach

Tailored coupled cluster theory represents a computationally inexpensive way to describe static and dynamical electron correlation effects. In this work, we scrutinize the performance of various tailored coupled cluster methods externally…

Chemical Physics · Physics 2021-03-24 Aleksandra Leszczyk , Mihály Máté , Örs Legeza , Katharina Boguslawski

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…

Chemical Physics · Physics 2015-06-19 Jason N. Byrd , Victor F. Lotrich , Rodney J. Bartlett

We present an efficient implementation of the random phase approximation (RPA) for molecular systems within the domain-based local pair natural orbital (DLPNO) framework. With optimized parameters, DLPNO-RPA achieves approximately 99.9%…

Chemical Physics · Physics 2025-08-18 Yu Hsuan Liang , Xing Zhang , Garnet Kin-Lic Chan , Timothy C. Berkelbach , Hong-Zhou Ye

The distinguishable cluster approximation applied to coupled cluster doubles equations greatly improves absolute and relative energies. We apply the same approximation to the triples equations and demonstrate that it can also improve…

Chemical Physics · Physics 2019-05-01 Daniel Kats , Andreas Köhn

We present the algorithmic details of the dynamical cluster approximation (DCA) algorithm. The DCA is a fully-causal approach which systematically restores non-local correlations to the dynamical mean field approximation (DMFA). The DCA is…

Strongly Correlated Electrons · Physics 2007-05-23 S. Moukouri , C. Huscroft , M. Jarrell

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

The main task of an energy calibration is to find a relation between pulse-height values and the corresponding energies. Doing this for each pulse-height channel individually requires an elaborated input spectrum with an excellent counting…

Instrumentation and Detectors · Physics 2016-02-17 Daniel Maier , Olivier Limousin

Recent years have seen the development of two types of non-local extensions to the single-site dynamical mean field theory. On one hand, cluster approximations, such as the dynamical cluster approximation, recover short-range…

Strongly Correlated Electrons · Physics 2018-03-21 Sergei Iskakov , Hanna Terletska , Emanuel Gull

Ab initio methods based on the second-order and higher connected moments, or cumulants, of a reference function have seen limited use in the determination of correlation energies of chemical systems throughout the years. Moment-based…

Chemical Physics · Physics 2023-08-25 Brad Ganoe , Martin Head-Gordon

Correlation clustering is perhaps the most natural formulation of clustering. Given $n$ objects and a pairwise similarity measure, the goal is to cluster the objects so that, to the best possible extent, similar objects are put in the same…

Data Structures and Algorithms · Computer Science 2013-12-19 Francesco Bonchi , David García-Soriano , Konstantin Kutzkov

We have investigated the efficacy of two recently proposed variations of the pair-natural-orbital approach to reducing the scaling of coupled cluster property calculations. In particular, we have extended our implementations of the PNO++…

Chemical Physics · Physics 2023-07-26 Ruhee D'Cunha , T. Daniel Crawford

We recently introduced the dynamical cluster approximation(DCA), a new technique that includes short-ranged dynamical correlations in addition to the local dynamics of the dynamical mean field approximation while preserving causality. The…

Strongly Correlated Electrons · Physics 2009-10-31 M. H. Hettler , M. Mukherjee , M. Jarrell , H. R. Krishnamurthy

Local electronic-structure methods in quantum chemistry operate on the ability to compress electron correlations more efficiently in a basis of spatially localized molecular orbitals than in a parent set of canonical orbitals. However, many…

Chemical Physics · Physics 2024-08-01 Jonas Greiner , Jürgen Gauss , Janus J. Eriksen

We evaluate the dependence of the cluster correlation length r_c on the mean intercluster separation D_c, for three models with critical matter density, vanishing vacuum energy (Lambda = 0) and COBE normalized: a tilted CDM (tCDM) model…

Astrophysics · Physics 2009-10-31 A. Gardini , S. A. Bonometto , G. Murante , G. Yepes