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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

In order to explore the effects of high levels of electron correlation on the real-time coupled cluster formalism and algorithmic behavior, we introduce a time-dependent implementation of the CC3 singles, doubles and approximate triples…

Chemical Physics · Physics 2025-01-23 Zhe Wang , Håkon Emil Kristiansen , Thomas Bondo Pedersen , T. Daniel Crawford

The time-dependent equation-of-motion coupled cluster (TD-EOM-CC) and time-dependent coupled cluster (TDCC) methods are compared by simulating Rabi oscillations for different numbers of non-interacting atoms in a classical electromagnetic…

Chemical Physics · Physics 2023-10-02 Andreas S. Skeidsvoll , Henrik Koch

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 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

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

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…

Simulations of laser-induced electron dynamics in a molecular system are performed using time-dependent (TD) equation-of-motion (EOM) coupled-cluster (CC) theory. The target system has been chosen to highlight potential shortcomings of…

Chemical Physics · Physics 2023-08-09 Stephen H. Yuwono , Brandon C. Cooper , Tianyuan Zhang , Xiaosong Li , A. Eugene DePrince

We have verified a mechanism for Raman excitation of atoms through continuum levels previously obtained by quantum optimal control using the multi-configurational time-dependent Hartree-Fock (MCTDHF) method. For the optimal control, which…

Atomic Physics · Physics 2017-07-19 Loren Greenman , K. Birgitta Whaley , Daniel J. Haxton , C. William McCurdy

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

A novel approach to rapidly converging high-level coupled-cluster (CC) energetics in an automated fashion is proposed. The key idea is an adaptive selection of the excitation manifolds defining higher-than-two-body components of the cluster…

Chemical Physics · Physics 2023-08-25 Karthik Gururangan , Piotr Piecuch

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

In the present work we report an implementation of the rank-reduced equation-of-motion coupled cluster method with approximate triple excitations (RR-EOM-CC3). The proposed variant relies on tensor decomposition techniques in order to…

Chemical Physics · Physics 2025-08-26 Piotr Michalak , Michał Lesiuk

Time-dependent quantum chemical methods coupled to Gaussian basis sets are gaining popularity in modeling the electron dynamics of atoms and molecules interacting with intense laser fields. Two approaches most widely used for this purpose,…

Chemical Physics · Physics 2023-01-18 Aleksander P. Woźniak , Maciej Lewenstein , Robert Moszyński

In parallel with the evolution of femtosecond and attosecond laser as well as free-electron laser technology, a variety of theoretical methods have been developed to describe the behavior of atoms, molecules, clusters, and solids under the…

Atomic Physics · Physics 2015-11-12 Kenichi L. Ishikawa , Takeshi Sato

In this contribution, we extend our framework for analyzing and visualizing correlated many-electron dynamics to non-variational, highly scalable electronic structure method. Specifically, an explicitly time-dependent electronic wave packet…

Chemical Physics · Physics 2017-04-27 Gunter Hermann , Vincent Pohl , Jean Christophe Tremblay

In this work, we investigate the possibility of improving multireference-driven coupled cluster (CC) approaches with an algorithm that iteratively combines complete active space (CAS) calculations with tailored CC and externally corrected…

Chemical Physics · Physics 2025-03-06 Robin Feldmann , Max Mörchen , Jakub Lang , Michał Lesiuk , Markus Reiher

We investigate the use of orbital-optimized references in conjunction with single-reference coupled-cluster theory with single and double substitutions (CCSD) for the study of core excitations and ionizations of 18 small organic molecules,…

The multi-reference Coupled Cluster method first proposed by Meller et al (J. Chem. Phys. 1996) has been implemented and tested. Guess values of the amplitudes of the single and double excitations (the ${\hat T}$ operator) on the top of the…

Chemical Physics · Physics 2016-04-11 Emmanuel Giner , Grégoire David , Anthony Scemama , Jean Paul Malrieu

When the number of strongly correlated electrons becomes larger, the single-reference coupled-cluster (CC) CCSD, CCSDT, etc. hierarchy displays an erratic behavior, while traditional multi-reference approaches may no longer be applicable…

Chemical Physics · Physics 2025-12-12 Ilias Magoulas , Jun Shen , Piotr Piecuch