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Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

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

Quantum embedding schemes have the potential to significantly reduce the computational cost of first principles calculations, whilst maintaining accuracy, particularly for calculations of electronic excitations in complex systems. In this…

Materials Science · Physics 2022-03-10 Joseph C. A. Prentice

We present an embedding approach to treat local electron correlation effects in periodic environments. In a single, consistent framework, our plane-wave based scheme embeds a local high-level correlation calculation (here Coupled Cluster…

Chemical Physics · Physics 2021-01-07 Tobias Schäfer , Florian Libisch , Georg Kresse , Andreas Grüneis

The tailored coupled cluster (TCC) approach is a promising ansatz that preserves the simplicity of single-reference coupled cluster theory, while incorporating a multi-reference wave function through amplitudes obtained from a preceding…

Chemical Physics · Physics 2021-01-07 Maximilian Mörchen , Leon Freitag , Markus Reiher

Simulating liquid water to an accuracy that matches its wealth of available experimental data requires both precise electronic structure methods and reliable sampling of nuclear (quantum) motion. This is challenging because applying the…

Localized molecular orbitals are often used for the analysis of chemical bonds, but they can also serve to efficiently and comprehensibly compute linear response properties. While conventional canonical molecular orbitals provide an…

Chemical Physics · Physics 2023-02-08 Souloke Sen , Bruno Senjean , Lucas Visscher

In this work, we revisited the idea of using the coupled-cluster ground state formalism to target excited states. Our main focus was targeting doubly excited states and double core hole states. Typical equation-of-motion (EOM) approaches…

Chemical Physics · Physics 2019-12-04 Joonho Lee , David W. Small , Martin Head-Gordon

Electrodynamical coupled cluster (CC) methodologies have been formulated employing standard QED Hamiltonian that is written in Coulomb gauge while using the DF and the MCDF pictures of the matter field for closed-shell and open-shell cases…

Quantum Physics · Physics 2024-01-15 Sambhu N. Datta

We present the first application to real molecular systems of the recently proposed linear-response theory for the density-based basis-set correction method [J. Chem. Phys. 158, 234107 (2023)]. We apply this approach to accelerate the…

Chemical Physics · Physics 2024-02-27 Diata Traore , Julien Toulouse , Emmanuel Giner

A unitary coupled-cluster (UCC) form for the wavefunction in the variational quantum eigensolver has been suggested as a systematic way to go beyond the mean-field approximation and include electron correlation in solving quantum chemistry…

Quantum Physics · Physics 2018-09-12 Ilya G. Ryabinkin , Tzu-Ching Yen , Scott N. Genin , Artur F. Izmaylov

In single-reference coupled-cluster (CC) methods, one has to solve a set of non-linear polynomial equations in order to determine the so-called amplitudes which are then used to compute the energy and other properties. Although it is of…

Chemical Physics · Physics 2021-09-10 Antoine Marie , Fábris Kossoski , Pierre-François Loos

The dipole moment is a crucial molecular property linked to a molecular system's bond polarity and overall electronic structure. To that end, the electronic dipole moment, which results from the electron density of a system, is often used…

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

Polaritonic chemistry relies on the strong light-matter interaction phenomena for altering the chemical reaction rates inside optical cavities. To explain and to understand these processes, the development of reliable theoretical models is…

Chemical Physics · Physics 2022-09-14 Fabijan Pavošević , Angel Rubio

An implementation of the coupled-cluster single- and double excitations (CCSD) method on two-dimensional quantum dots is presented. Advantages and limitations are studied through comparison with other high accuracy approaches for two to…

Mesoscale and Nanoscale Physics · Physics 2013-05-30 Erik Waltersson , Eva Lindroth

A new method that accurately describes strongly correlated states and captures dynamical correlation is presented. It is derived as a modification of coupled-cluster theory with single and double excitations (CCSD) through consideration of…

Chemical Physics · Physics 2013-07-15 Daniel Kats , Frederick R. Manby

An electrodynamical coupled cluster (CC) methodology starting from a covariant formalism and an equal time approximation, and finally based on the Dirac-Fock picture of the electron and positron fields and Coulomb gauge, is given here. The…

Atomic Physics · Physics 2019-04-30 Sambhu N. Datta

We introduce a novel class of coupled cluster (CC) methods that leverage the seniority concept to enhance efficiency and accuracy in electronic structure calculations. While existing approaches, such as the pair coupled cluster doubles…

Unitary Coupled Cluster (UCC) theory is a promising variational method for electronic structure calculations, especially for strongly correlated systems and quantum computers. However, its practical application is limited by the steep…

Chemical Physics · Physics 2026-02-05 Prateek Vaish , Brenda Rubenstein