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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…

Materials Science · Physics 2022-04-05 Verena A. Neufeld , Hong-Zhou Ye , 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

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

In this work, we introduce a differentiable implementation of the local natural orbital coupled cluster (LNOCC) method within the automatic differentiation framework of the PySCFAD package. The implementation is comprehensively tuned for…

Chemical Physics · Physics 2024-07-08 Xing Zhang , Chenghan Li , Hong-Zhou Ye , Timothy C. Berkelbach , Garnet Kin-Lic Chan

We present an implementation of equation of motion coupled-cluster singles and doubles (EOM-CCSD) theory using periodic boundary conditions and a plane wave basis set. Our implementation of EOM-CCSD theory is applied to study $F$-centers in…

Materials Science · Physics 2021-02-09 Alejandro Gallo , Felix Hummel , Andreas Irmler , Andreas Grüneis

Low-scaling electron correlation theory based on the pair natural orbital approximation, PNO-CCSD(T), has become a powerful computational tool. Motivated by the recent discovery of large errors for organometallic molecules, we assess the…

Chemical Physics · Physics 2023-10-10 Reka A. Horvath , Kesha Sorathia , Isabelle Saint , David P. Tew

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,…

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

Localized orbital coupled cluster theory has recently emerged as an nonempirical alternative to DFT for large systems. Intuitively, one might expect such methods to perform less well for highly delocalized systems. In the present work, we…

Chemical Physics · Physics 2020-10-16 Nitai Sylvetsky , Ambar Banerjee , Mercedes Alonso , Jan M. L. Martin

The $\Delta \text{NO}$ method for static correlation is combined with second-order M{\o}ller-Plesset perturbation theory (MP2) and coupled-cluster singles and doubles (CCSD) to account for dynamic correlation. The MP2 and CCSD expressions…

Chemical Physics · Physics 2020-06-05 Joshua W. Hollett , Pierre-François Loos

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 present a simple and general method for construction of localized orbitals to describe electronic structure of extended periodic metals and insulators as well as confined systems. Spatial decay of these orbitals is found to exhibit…

Materials Science · Physics 2007-05-23 Joydeep Bhattacharjee , Umesh V Waghmare

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

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

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 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

An efficient O($N$) divide-conquer (DC) method based on localized natural orbitals (LNOs) is presented for large-scale density functional theories (DFT) calculations of gapped and metallic systems. The LNOs are non-iteratively calculated by…

Computational Physics · Physics 2019-01-02 Taisuke Ozaki , Masahiro Fukuda , Gengping Jiang

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

Quantum embedding methods have recently developed significantly to model large molecular structures. This work proposes a novel wave function theory in density functional theory (WTF-in-DFT) embedding scheme based on pair-coupled cluster…

Chemical Physics · Physics 2024-01-10 Rahul Chakraborty , Katharina Boguslawski , Paweł Tecmer

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
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