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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

While there have been many developments in computational probes of both strongly-correlated molecular systems and machine-learning accelerated molecular dynamics, there remains a significant gap in capabilities in simulating accurate…

Chemical Physics · Physics 2025-04-04 Yannic Rath , George H. Booth

Aiming to combine density functional theory (DFT) and wavefunction theory, we study a mapping from the many-body interacting system to an effectively-interacting Kohn-Sham system instead of a non-interacting Kohn-Sham system. Because a…

Chemical Physics · Physics 2020-02-19 Shunsuke A. Sato , Angel Rubio

A strong effort will be dedicated in the coming years to extend the reach of ab initio nuclear-structure calculations to heavy doubly open-shell nuclei. In order to do so, the most efficient strategies to incorporate dominant many-body…

An accurate determination of the electron correlation energy is essential for describing the structure, stability, and function in a wide variety of systems, ranging from gas-phase molecular assemblies to condensed matter and…

Chemical Physics · Physics 2014-03-05 Alberto Ambrosetti , Anthony M. Reilly , Robert A. DiStasio , Alexandre Tkatchenko

The time-dependent restricted-active-space self-consistent-field singles (TD-RASSCF-S) method is presented for investigating TD many-electron dynamics in atoms and molecules. Adopting the SCF notion from the muticonfigurational TD…

Atomic Physics · Physics 2014-05-22 Haruhide Miyagi , Lars Bojer Madsen

By introducing a set of auxiliary equations representing a many-body system, we have derived an extension of the Kohn-Sham scheme for the density functional theory. These equations consist of a Kohn-Sham-type equation determining…

Materials Science · Physics 2009-11-07 Koichi Kusakabe

Multi-configurational approaches yield universal wave function parameterizations that can qualitatively well describe electronic structures along reaction pathways. For quantitative results, multi-reference perturbation theory is required…

Chemical Physics · Physics 2016-09-08 Christopher J. Stein , Vera von Burg , Markus Reiher

Extending many-body numerical techniques which are powerful in the context of simple model calculations to the realm of realistic material simulations can be a challenging task. Realistic systems often involve multiple active orbitals,…

Strongly Correlated Electrons · Physics 2025-07-23 Jonas B. Profe , Jiawei Yan , Karim Zantout , Philipp Werner , Roser Valentí

We present an efficient implementation of ab initio many-body quantum embedding and local correlation methods for infinite periodic systems through translational symmetry adapted interpolative separable density fitting, an approach which…

Strongly Correlated Electrons · Physics 2026-01-26 Junjie Yang , Ning Zhang , Shunyue Yuan , Jincheng Yu , Hong-Zhou Ye , Garnet Chan

We present a new approach to real-space multiple-scattering theory for molecules and clusters, based on the two-potential (distorted-wave) Lippmann-Schwinger equation formalism. Our approach uses a recently developed form [D. L. Foulis,…

Mathematical Physics · Physics 2008-06-04 D. L. Foulis

An accurate treatment of electronic spectra in large systems with a technique such as time dependent density functional theory (TDDFT) is computationally challenging. Due to the Nyquist sampling theorem, direct real time simulations must be…

Materials Science · Physics 2024-01-17 Matthias Kick , Ezra Alexander , Anton Beiersdorfer , Troy Van Voorhis

We present the first open release of the DCA++ project, a high-performance research software framework to solve quantum many-body problems with cutting edge quantum cluster algorithms. DCA++ implements the dynamical cluster approximation…

Recent quantum algorithms pertaining to electronic structure theory primarily focus on threshold-based dynamic construction of ansatz by selectively including important many-body operators. These methods can be made systematically more…

Quantum Physics · Physics 2024-08-26 Chayan Patra , Debaarjun Mukherjee , Sonaldeep Halder , Dibyendu Mondal , Rahul Maitra

We present a cost-effective treatment of the triple excitation amplitudes in the time-dependent optimized coupled-cluster (TD-OCC) framework called TD-OCCDT(4) for studying intense laser-driven multielectron dynamics. It considers triple…

Chemical Physics · Physics 2021-07-07 Himadri Pathak , Takeshi Sato , Kenichi L. Ishikawa

A mixed quantum-classical approach to simulate the coupled dynamics of electrons and nuclei in nanoscale molecular systems is presented. The method relies on a second order expansion of the Lagrangian in time-dependent density functional…

Chemical Physics · Physics 2009-11-10 T. A. Niehaus , D. Heringer , B. Torralva , Th. Frauenheim

Strongly correlated systems containing d/f-electrons present a challenge to conventional density functional theory (DFT), such as the widely used local density approximation (LDA) or generalized gradient approximation (GGA). In this work,…

Strongly Correlated Electrons · Physics 2024-01-19 Bei-Lei Liu , Yue-Chao Wang , Yu Liu , Hai-Feng Liu , Hai-Feng Song

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

The Coupled Cluster (CC) method is used to compute the electronic correlation energy in atoms and molecules and often leads to highly accurate results. However, due to its single-reference nature, standard CC in its projected form fails to…

In this paper, we propose a generic and systematic approach for study of the electronic structure for atoms or molecules. In particular, we address the issue of single particle states, or orbitals, which should be one of the most important…

Chemical Physics · Physics 2007-05-23 Liqiang Wei