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Guided by perturbative analysis, we improve the accuracy of Aufbau suppressed coupled cluster theory in simple single excitations, multi-configurational single excitations, and charge transfer excitations while keeping the cost of its…

Chemical Physics · Physics 2025-03-26 Harrison Tuckman , Ziheng Ma , Eric Neuscamman

We generalize the Aufbau suppressed coupled cluster formalism into the realm of doubly excited states by deriving, implementing, and testing a wave function initialization strategy that allows the zeroth order wave function to match the…

Chemical Physics · Physics 2026-05-11 Qasim Javed , Harrison Tuckman , Eric Neuscamman

We introduce an approach to improve single-reference coupled cluster theory in settings where the Aufbau determinant is absent from or plays only a small role in the true wave function. Using a de-excitation operator that can be efficiently…

Chemical Physics · Physics 2024-07-03 Harrison Tuckman , Eric Neuscamman

Modeling charge transfer well can require treating post-excitation orbital relaxations and handling medium to large molecules in realistic environments. By combining a state-specific correlation treatment with such orbital relaxations,…

Chemical Physics · Physics 2025-07-28 Harrison Tuckman , Eric Neuscamman

We present an excited-state-specific coupled-cluster approach in which both the molecular orbitals and cluster amplitudes are optimized for an individual excited state. The theory is formulated via a pseudoprojection of the traditional…

Chemical Physics · Physics 2023-11-27 Harrison Tuckman , Eric Neuscamman

We derived and implemented the calculation of the one-body reduced density matrix for Aufbau suppressed coupled cluster theory, from which excited state natural orbitals and one-body properties, like atomic populations and dipole moments,…

Chemical Physics · Physics 2026-03-20 Conor Bready , Harrison Tuckman , Eric Neuscamman

Introducing an active space approximation is inevitable for the quantum computations of chemical systems. However, this approximation ignores the electron correlations related to non-active orbitals. Here, we propose a computational method…

Quantum Physics · Physics 2024-06-06 Luca Erhart , Yuichiro Yoshida , Viktor Khinevich , Wataru Mizukami

In this work we present a coupled-cluster theory for the propagation of multireference electronic systems initiating at general quantum mechanical states. Our formalism is based on the infinitesimal analysis of modified cluster operators,…

Chemical Physics · Physics 2025-05-09 Martín A. Mosquera

The Coupled-Cluster theory is one of the most successful high precision methods used to solve the stationary Schr\"odinger equation. In this article, we address the mathematical foundation of this theory with focus on the advances made in…

Chemical Physics · Physics 2019-09-04 Andre Laestadius , Fabian M. Faulstich

A full coupled-cluster expansion suitable for sparse algebraic operations is developed by expanding the commutators of the Baker-Campbell-Hausdorff series explicitly for cluster operators in binary representations. A full coupled-cluster…

Chemical Physics · Physics 2018-09-13 Enhua Xu , Motoyuki Uejima , Seiichiro L. Ten-no

Excited-state electronic structure in strongly correlated systems remains challenging due to the exponential scaling of the many-body Hilbert space and the difficulty of constructing systematically controlled active spaces. Building on the…

Chemical Physics · Physics 2026-05-05 Annabelle Canestraight , Russell Miller , Libor Veis , Vojtech Vlcek

We present a newly developed scheme for atomic relaxations of magnetic supported clusters. Our approach is based on the full potential Korringa-Kohn-Rostoker Green's function method and the second moment tight-binding approximation for…

Materials Science · Physics 2007-05-23 V. S. Stepanyuk , A. L. Klavsyuk , L. Niebergall , A. M. Saletsky , W. Hergert , P. Bruno

A wide class of coupled-cluster methods is introduced, based on Arponen's extended coupled-cluster theory. This class of methods is formulated in terms of a coordinate transformation of the cluster operators. The mathematical framework for…

Chemical Physics · Physics 2020-12-02 Simen Kvaal , Andre Laestadius , Tilmann Bodenstein

This work presents a first time accurate calculation of the magnetic dipole hyperfine structure constants for the ground state and some low-lying excited states of Pb$^+$. By comparing different levels of approximation with experimental…

Atomic Physics · Physics 2009-11-10 Bijaya K. Sahoo , Rajat K. Chaudhuri , B. P. Das , Holger Merlitz , Debashis Mukherjee

We present excitation energies for molecular doublets from a spin-adapted formulation of coupled cluster singles and doubles theory. The entanglement coupled cluster approach represents an unconventional take on the notorious problem of…

Chemical Physics · Physics 2025-04-08 Sarai Dery Folkestad , Kristine Lauvstad Kruken , Henrik Koch

Coupled cluster methods based exclusively on double excitations are comparatively "cheap" and interesting model chemistries, as they are typically able to capture the bulk of the dynamical electron correlation effects. The trade-off in such…

Quantum Physics · Physics 2024-06-14 Zachary W. Windom , Daniel Claudino , Rodney J. Bartlett

The dielectric behavior of a linear cluster of two or more living cells connected by tight junctions is analyzed using a spectral method. The polarizability of this system is obtained as an expansion over the eigenmodes of the linear…

Biological Physics · Physics 2010-02-12 Titus Sandu , Daniel Vrinceanu , Eugen Gheorghiu

We consider the sampling of the coupled cluster expansion within stochastic coupled cluster theory. Observing the limitations of previous approaches due to the inherently non-linear behaviour of a coupled cluster wavefunction representation…

Chemical Physics · Physics 2018-08-14 Charles J. C. Scott , Alex J. W. Thom

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

Methods which aim at universal applicability must be able to describe both weak and strong electronic correlation with equal facility. Such methods are in short supply. The combination of symmetry projection for strong correlation and…

Chemical Physics · Physics 2020-05-14 Yiheng Qiu , Thomas M. Henderson , Jinmo Zhao , Gustavo E. Scuseria
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