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While providing a highly accurate framework for simulating laser-induced many-electron dynamics in atom and molecules, including linear and nonlinear steady-state and transient absorption spectra, time-dependent coupled-cluster theory does…

Electronic structure methods built around double-electron excitations have a rich history in quantum chemistry. However, it seems to be the case that such methods are only suitable in particular situations and are not naturally equipped to…

Chemical Physics · Physics 2024-07-12 Zachary W. Windom , Ajith Perera , Rodney J. Bartlett

We present a new implementation of DMRG-based tailored coupled clusters method (TCCSD), which employs the domain-based local pair natural orbital approach (DLPNO-TCCSD). Compared to the previous LPNO version of the method, the new…

Chemical Physics · Physics 2020-05-08 Jakub Lang , Andrej Antalík , Libor Veis , Jan Brandejs , Jiří Brabec , Örs Legeza , Jiří Pittner

In this work, we derive working equations for the Linear Response pair Coupled Cluster Doubles (LR-pCCD) ansatz and its extension to singles (S), LR-pCCD+S. These methods allow us to compute electronic excitation energies and transition…

Chemical Physics · Physics 2025-03-18 Somayeh Ahmadkhani , Katharina Boguslawsk , Paweł Tecmer

The accuracy at which total energies of open-shell atoms and organic radicals may be calculated is assessed for selected coupled cluster perturbative triples expansions, all of which augment the coupled cluster singles and doubles (CCSD)…

Chemical Physics · Physics 2016-05-17 Janus Juul Eriksen , Devin A. Matthews , Poul Jørgensen , Jürgen Gauss

The pair coupled cluster doubles (pCCD) method (where the excitation manifold is restricted to electron pairs) has a series of interesting features. Among others, it provides ground-state energies very close to what is obtained with…

The curse of dimensionality (COD) limits the current state-of-the-art {\it ab initio} propagation methods for non-relativistic quantum mechanics to relatively few particles. For stationary structure calculations, the coupled-cluster (CC)…

Quantum Physics · Physics 2015-06-03 Simen Kvaal

In this work we present a derivation of the real-time time-dependent orbital-optimized M{\o}ller-Plesser TDOMP2 and its biorthogonal companion, time-dependent non-orthogonal OMP2 (TDNOMP2), theory starting from the time-dependent…

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…

Accurately resolving many-body satellite features in molecular core-level spectra requires theoretical approaches that capture electron correlation both efficiently and systematically. The recently developed time-dependent double…

Quantum Physics · Physics 2026-05-12 Vibin Abraham , Priyabrata Senapati , Himadri Pathak , Bo Peng

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

We present the numerical implementation of the time-dependent complete-active-space self-consistent-field (TD-CASSCF) method [Phys. Rev. A, 88, 023402 (2013)] for atoms driven by a strong linearly polarized laser pulse. The present…

We report a complete implementation of the coupled-cluster method with single, double, and triple excitations (CCSDT) where tensor decompositions are used to reduce its scaling and overall computational costs. For the decomposition of the…

Chemical Physics · Physics 2020-02-20 Michał Lesiuk

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

We develop a time-dependent multi-configurational numerical technique for calculating ionization by short laser pulses of many-electron molecules. The method is based on the expansion of the wave function of a molecule into the eigenstates…

Atomic Physics · Physics 2024-05-22 Vladislav V. Serov

We present a new formulation of the time-dependent self-interaction correction (TDSIC). It is derived variationally obeying explicitly the constraints on orthonormality of the occupied single-particle orbitals. The thus emerging rather…

Quantum Physics · Physics 2009-03-02 J. Messud , P. M. Dinh , P. -G. Reinhard , E. Suraud

We present a numerical implementation of the time-dependent surface flux (tSURFF) method [New J. Phys. 14, 013021 (2012)], an efficient computational scheme to extract photoelectron energy spectra, to the time-dependent multiconfiguration…

Atomic Physics · Physics 2019-08-07 Yuki Orimo , Takeshi Sato , Kenichi L. Ishikawa

Wave functions based on electron-pair states provide inexpensive and reliable models to describe quantum many-body problems containing strongly-correlated electrons, given that broken-pair states have been appropriately accounted for by,…

Chemical Physics · Physics 2021-03-17 Artur Nowak , Ors Legeza , Katharina Boguslawski

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

We present the working equations for a reduced-scaling method of evaluating the perturbative triples (T) energy in coupled-cluster theory, through the tensor hypercontraction (THC) of the triples amplitudes ($t_{ijk}^{abc}$). Through our…

Chemical Physics · Physics 2024-06-12 Andy Jiang , Justin M. Turney , Henry F. Schaefer