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We introduce a non-iterative energy correction, added on top of the rank-reduced coupled-cluster method with single, double, and triple substitutions, that accounts for excitations excluded from the parent triple excitation subspace. The…

Chemical Physics · Physics 2022-01-06 Michał Lesiuk

Time-dependent density-functional theory (TDDFT) is widely used to describe electronic excitations in complex finite systems with large numbers of atoms, such as biomolecules and nanocrystals. The first part of this paper will give a simple…

Materials Science · Physics 2008-08-15 C. A. Ullrich , V. Turkowski

In this article, we investigate the numerical and theoretical aspects of the coupled-cluster method tailored by matrix-product states. We investigate chemical properties of the used method, such as energy size extensivity and the…

Density functional theory (DFT)-based simulations of materials have first-principles accuracy, but are very computationally expensive. For simulating various properties of multi-component alloys, the cluster expansion (CE) technique has…

Materials Science · Physics 2026-04-01 Jacob Jeffries , Bochuan Sun , Enrique Martinez

A dynamical formulation of coupled cluster theory is derived using a variational principle. By allowing time-dependent single-particle functions, a high degree of adaptivity is introduced, allowing complex systems to be simulated with high…

Quantum Physics · Physics 2014-11-25 Simen Kvaal

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

Recent developments in high-power ultrafast optical technology and emerging theoretical frameworks in strong-field quantum electrodynamics (SF-QED) are unveiling nuanced differentiations between the semi-classical and full quantum…

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 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

The coupled cluster method is considered a gold standard in quantum chemistry, reliably giving energies that are exact within chemical accuracy (1.6 mHartree). However, even in the CCSD approximation, where the cluster operator is truncated…

Chemical Physics · Physics 2023-03-10 Simon Elias Schrader , Simen Kvaal

In quantum chemistry, one of the most important challenges is the static correlation problem when solving the electronic Schr\"odinger equation for molecules in the Born--Oppenheimer approximation. In this article, we analyze the tailored…

Numerical Analysis · Mathematics 2019-11-21 Fabian M. Faulstich , Andre Laestadius , Örs Legeza , Reinhold Schneider , Simen Kvaal

Accurate and fast treatment of electron-electron interactions remains a central challenge in electronic structure theory because post-Hartree-Fock methods often suffered from the computational cost for 4-index electron repulsion integrals…

Chemical Physics · Physics 2025-12-05 Yueyang Zhang , Xuewei Xiong , Wei Wu , Peifeng Su

We propose a gauge-invariant formulation of the channel orbital-based time-dependent configuration interaction singles (TDCIS) method [Phys. Rev. A 74, 043420 (2006)], one of the powerful ab initio methods to investigate electron dynamics…

Atomic Physics · Physics 2018-02-09 Takeshi Sato , Takuma Teramura , Kenichi L. Ishikawa

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

Recent disagreement between state-of-the-art quantum chemical methods, coupled cluster with single, double and perturbative triples excitations and fixed-node diffusion Monte Carlo, calls for systematic examination of possible sources of…

Chemical Physics · Physics 2025-05-14 S. Lambie , C. Rickert , D. Usvyat , A. Alavi , D. Kats

We introduce a hybrid quantum-classical algorithm, the localized active space unitary selective coupled cluster singles and doubles (LAS-USCCSD) method. Derived from the localized active space unitary coupled cluster (LAS-UCCSD) method,…

Time-dependent Hartree-Fock (TDHF) is one of the fundamental post-Hartree-Fock (HF) methods to describe excited states. In its Tamm-Dancoff form, equivalent to Configuration Interaction Singles, it is still widely used and particularly…

Chemical Physics · Physics 2024-11-18 Uday Panta , David A. Strubbe

This chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly time-dependent formulations. As applied to the…

Chemical Physics · Physics 2023-05-02 John M. Herbert

In this work, we introduce a correction to the unitary coupled cluster method with single and double excitations (UCCSD) that incorporates the effects of missing triple excitations through a treatment that is correct through fifth-order in…

Chemical Physics · Physics 2025-09-08 Zachary W. Windom , Daniel Claudino

We present a method to simulate ultrafast pump-probe time-resolved circular dichroism (TRCD) spectra based on time-dependent density functional theory trajectory surface hopping. The method is applied to simulate the TRCD spectrum along the…

Chemical Physics · Physics 2023-04-11 Enrico Tapavicza , Trevor Reutershan , Travis Thompson