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We present ab initio absorption spectra of six three-dimensional semiconductors and insulators calculated using Gaussian-based periodic equation-of-motion coupled-cluster theory with single and double excitations (EOM-CCSD). The spectra are…

化学物理 · 物理学 2021-07-13 Xiao Wang , Timothy C. Berkelbach

We report the core binding energies of K-edge and L-edge transitions in simple semiconducting and insulating solids using periodic equation-of-motion coupled-cluster theory with single and double excitations (EOM-CCSD). In our all-electron…

化学物理 · 物理学 2025-08-04 Ethan A. Vo , Timothy C. Berkelbach

While the periodic equation-of-motion coupled-cluster (EOM-CC) method promises systematic improvement of electronic band gap calculations in solids, its practical application at the singles and doubles level (EOM-CCSD) is hindered by severe…

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…

化学物理 · 物理学 2019-07-10 Alan M. Lewis , Timothy C. Berkelbach

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…

化学物理 · 物理学 2023-09-18 Loïc Halbert , Andre Severo Pereira Gomes

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…

化学物理 · 物理学 2025-03-26 Devin A. Matthews

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…

材料科学 · 物理学 2017-01-19 James McClain , Qiming Sun , Garnet Kin-Lic Chan , Timothy C. Berkelbach

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…

材料科学 · 物理学 2021-02-09 Alejandro Gallo , Felix Hummel , Andreas Irmler , Andreas Grüneis

We report in this paper an implementation of 4-component relativistic Hamiltonian based Equation-of-Motion Coupled-Cluster with singles and doubles (EOM-CCSD) theory for the calculation of ionization potential (IP), electron affinity (EA)…

化学物理 · 物理学 2018-11-09 Avijit Shee , Trond Saue , Lucas Visscher , Andre Severo Pereira Gomes

Understanding the process of molecular photoexcitation is crucial in various fields, including drug development, materials science, photovoltaics, and more. The electronic vertical excitation energy is a critical property, for example in…

化学物理 · 物理学 2025-03-26 Tingting Zhao , Devin A. Matthews

A new perturbative approach to canonical equation-of-motion coupled-cluster theory is presented using coupled-cluster perturbation theory. A second-order M{\o}ller-Plesset partitioning of the Hamiltonian is used to obtain the well known…

化学物理 · 物理学 2015-07-09 Jason N. Byrd , Varun Rishi , Ajith Perera , Rodney J. Bartlett

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…

材料科学 · 物理学 2023-01-25 Bryan T. G. Lau , Brian Busemeyer , Timothy C. Berkelbach

Similarity transformed equation-of-motion coupled cluster theory (STEOM-CC) is an alternative approach to equation-of-motion coupled cluster theory for excited states (EOMEE-CC) which uses a second similarity transformation of the…

化学物理 · 物理学 2025-03-26 Megan Simons , Devin A. Matthews

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…

材料科学 · 物理学 2022-04-05 Verena A. Neufeld , Hong-Zhou Ye , Timothy C. Berkelbach

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,…

材料科学 · 物理学 2023-03-21 Verena A. Neufeld , Timothy C. Berkelbach

We report the first investigation of the performance of EOM-CC4 -- an approximate equation-of-motion coupled-cluster model which includes iterative quadruple excitations -- for vertical excitation energies in molecular systems. By…

化学物理 · 物理学 2021-06-14 Pierre-François Loos , Devin A. Matthews , Filippo Lipparini , Denis Jacquemin

The accurate description of doubly-excited states using conventional electronic structure methods is remarkably challenging, primarily because such excited states require the inclusion of doubly or higher excited configurations or the…

化学物理 · 物理学 2019-05-01 Katharina Boguslawski

The projection-based quantum embedding method is applied to electronically excited states of valence, Rydberg, and charge-transfer character, valence- and core-ionized states, as well as bound and temporary radical anions. We embed…

化学物理 · 物理学 2021-06-10 Valentina Parravicini , Thomas-C. Jagau

We introduce a new equation-of-motion coupled-cluster method based on a pair coupled-cluster doubles (pCCD) reference, termed frozen-pair EOM-CCSD (EOM-fpCCSD). This approach combines the computational efficiency of the pCCD ansatz with a…

化学物理 · 物理学 2026-05-06 Katharina Boguslawski , Paweł Tecmer

The phenomenon of orbital relaxation upon excitation of core electrons is a major problem in the linear-response treatment of core-hole spectroscopies. Rather than addressing relaxation through direct dynamical correlation of the excited…

化学物理 · 物理学 2025-03-26 Megan Simons , Devin A. Matthews
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