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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…

Chemical Physics · Physics 2019-05-01 Katharina Boguslawski

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 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…

Chemical Physics · Physics 2025-03-26 Megan Simons , Devin A. Matthews

We scrutinize the performance of different variants of equation of motion coupled cluster (EOM-CC) methods to predict electronic excitation energies and excited state potential energy surfaces in closed-shell actinide species. We focus our…

Chemical Physics · Physics 2020-02-26 Artur Nowak , Paweł Tecmer , Katharina Boguslawski

The quantum equation-of-motion (qEOM) method with singles and doubles has been suggested to study electronically excited states while it fails to predict the excitation energies dominated by double excitations. In this work, we present an…

Quantum Physics · Physics 2024-06-18 Yuhan Zheng , Jie Liu , Zhenyu Li , Jinlong Yang

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…

Chemical Physics · Physics 2025-03-26 Devin A. Matthews

Wavefunctions restricted to electron pair states are promising models for strongly-correlated systems. Specifically, the pair Coupled Cluster Doubles (pCCD) ansatz allows us to accurately describe bond dissociation processes and…

Strongly Correlated Electrons · Physics 2019-05-01 Katharina Boguslawski

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…

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

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

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…

Chemical Physics · Physics 2025-03-26 Megan Simons , Devin A. Matthews

We reexamine $\Delta$CCSD, a state-specific coupled-cluster (CC) with single and double excitations (CCSD) approach that targets excited states through the utilization of non-Aufbau determinants. This methodology is particularly efficient…

Chemical Physics · Physics 2024-06-13 Yann Damour , Anthony Scemama , Denis Jacquemin , Fábris Kossoski , Pierre-François Loos

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

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…

Chemical Physics · Physics 2026-05-06 Katharina Boguslawski , Paweł Tecmer

A reduced-complexity variant of equation-of-motion coupled-cluster singles and doubles (EOM-CCSD) method is formulated in terms of state-averaged excited state pair natural orbitals (PNO) designed to describe manifolds of excited states.…

Chemical Physics · Physics 2020-06-09 Chong Peng , Marjory C. Clement , Edward F. Valeev

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…

Chemical Physics · Physics 2015-07-09 Jason N. Byrd , Varun Rishi , Ajith Perera , Rodney J. Bartlett

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…

Chemical Physics · Physics 2021-06-14 Pierre-François Loos , Devin A. Matthews , Filippo Lipparini , Denis Jacquemin

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…

Chemical Physics · Physics 2021-06-10 Valentina Parravicini , Thomas-C. Jagau

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)…

Chemical Physics · Physics 2018-11-09 Avijit Shee , Trond Saue , Lucas Visscher , Andre Severo Pereira Gomes

Excited states exhibiting double excitation character are notoriously difficult to model using conventional single-reference methods, such as adiabatic time-dependent density-functional theory (TD-DFT) or equation-of-motion coupled cluster…

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