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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,…

Materials Science · Physics 2023-03-21 Verena A. Neufeld , Timothy C. Berkelbach

A relativistic version of the coupled-cluster single-double (CCSD) method is developed for atoms with a single valence electron. In earlier work, a linearized version of the CCSD method (with extensions to include a dominant class of triple…

Atomic Physics · Physics 2009-11-13 Rupsi Pal , M. S. Safronova , W. R. Johnson , Andrei Derevianko , Sergey G. Porsev

We present the results of Gaussian-based ground-state and excited-state equation-of-motion coupled-cluster theory with single and double excitations for three-dimensional solids. We focus on diamond and silicon, which are paradigmatic…

Materials Science · Physics 2017-01-19 James McClain , Qiming Sun , Garnet Kin-Lic Chan , Timothy C. Berkelbach

We describe the implementation details of periodic local coupled-cluster theory with single and double excitations (CCSD) and perturbative triple excitations [CCSD(T)] using local natural orbitals (LNOs) and $k$-point symmetry. We discuss…

Chemical Physics · Physics 2024-11-13 Hong-Zhou Ye , Timothy C. Berkelbach

Modern electronic structure theories can predict and simulate a wealth of phenomena in surface science and solid-state physics. In order to allow for a direct comparison with experiment, such ab initio predictions have to be made in the…

Materials Science · Physics 2020-04-15 Thomas Gruber , Ke Liao , Theodoros Tsatsoulis , Felix Hummel , Andreas Grüneis

Many-electron correlation methods offer a systematic approach to predicting material properties with high precision. However, practically attaining accurate ground-state properties for bulk metals presents significant challenges. In this…

Materials Science · Physics 2025-01-07 Tobias Schäfer

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…

Materials Science · Physics 2024-03-01 Nikolaos Masios , Andreas Irmler , Tobias Schäfer , Andreas Grüneis

Computationally efficient and accurate quantum mechanical approximations to solve the many-electron Schr\"odinger equation are at the heart of computational materials science. In that respect the coupled cluster hierarchy of methods plays a…

Materials Science · Physics 2022-01-11 Tina N. Mihm , Tobias Schäfer , Sai Kumar Ramadugu , Andreas Grüneis , James J. Shepherd

The study of isolated defects in solids is a natural target for classical or quantum embedding methods that treat the defect at a high level of theory and the rest of the solid at a lower level of theory. Here, in the context of…

Materials Science · Physics 2023-01-25 Bryan T. G. Lau , Brian Busemeyer , Timothy C. Berkelbach

We present an ab initio study of electronically excited states of three-dimensional solids using Gaussian-based periodic equation-of-motion coupled-cluster theory with single and double excitations (EOM-CCSD). The explicit use of…

Materials Science · Physics 2020-01-31 Xiao Wang , Timothy C. Berkelbach

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

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…

Chemical Physics · Physics 2024-06-06 Zachary W. Windom , Daniel Claudino , Rodney J. Bartlett

The electronic properties of two-dimensional transition metal dichalcogenides (2D TMDs) have attracted much attention during the last decade. We show how a diagrammatic ab initio coupled cluster singles and doubles (CCSD) treatment paired…

Materials Science · Physics 2020-07-01 Artem Pulkin , Garnet Kin-Lic Chan

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

In this article, the molecular permanent electric dipole moments and components of static dipole polarizabilities for the electronic ground state of singly charged aluminum monohalides are reported. The coupled-cluster method by considering…

Atomic Physics · Physics 2024-06-18 Ankush Thakur , Renu Bala , H. S. Nataraj , V. S. Prasannaa

The equation of motion coupled cluster singles and doubles model (EOM-CCSD) is an accurate, black-box correlated electronic structure approach to investigate electronically excited states and electron attachment or detachment processes. It…

Chemical Physics · Physics 2023-09-18 Loïc Halbert , Andre Severo Pereira Gomes

The accurate calculation of excited state properties of interacting electrons in the condensed phase is an immense challenge in computational physics. Here, we use state-of-the-art equation-of-motion coupled-cluster theory with single and…

Chemical Physics · Physics 2019-07-10 Alan M. Lewis , Timothy C. Berkelbach

Machine learning (ML) plays an important role in quantum chemistry, providing fast-to-evaluate predictive models for various properties of molecules. However, most existing ML models for molecular electronic properties use density…

Chemical Physics · Physics 2024-06-26 Hao Tang , Brian Xiao , Wenhao He , Pero Subasic , Avetik R. Harutyunyan , Yao Wang , Fang Liu , Haowei Xu , Ju Li

In the molecular quantum chemistry community, coupled-cluster (CC) methods are well-recognized for their systematic convergence and reliability. The extension of the theory to extended systems has been comparably recent, so that…

Chemical Physics · Physics 2024-10-31 Andreas Grüneis , Evgeny Moerman , Matthias Scheffler , Tonghao Shen , Igor Ying Zhang

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
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