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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

Starting from the observation that one of the most successful methods for solving the Kohn-Sham equations for periodic systems -- the plane-wave method -- is a spectral method based on eigenfunction expansion, we formulate a spectral method…

Computational Physics · Physics 2016-03-08 Amartya S. Banerjee , Ryan S. Elliott , Richard D. James

In this work we investigate methods to improve the efficiency and scalability of quantum algorithms for quantum chemistry applications. We propose a transformation of the electronic structure Hamiltonian in the second quantization framework…

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

The recent quantum information boom has effected a resurgence of interest in unitary coupled cluster (UCC) theory. Our group's interest in local energy landscapes of unitary ans\"atze prompted us to investigate the classical approach of…

Chemical Physics · Physics 2022-11-01 Harper R. Grimsley , Nicholas J. Mayhall

The coherent potential approximation, CPA, is a useful tool to treat systems with disorder. Cluster theories have been proposed to go beyond the translation invariant single-site CPA approximation and include some short range correlations.…

Condensed Matter · Physics 2009-10-31 C. I. Ventura , R. A. Barrio , .

A new electronic structure model is developed in which the ground state energy of a molecular system is given by a Hartree-Fock-like expression with parametrized one- and two-electron integrals over an extended (minimal + polarization) set…

Chemical Physics · Physics 2014-02-11 Dimitri N. Laikov

Density functional theory (DFT) provides convenient electronic structure methods for the study of molecular systems and materials. Regular Kohn-Sham DFT calculations rely on unitary transformations to determine the ground-state electronic…

Chemical Physics · Physics 2022-10-10 Greta Jacobson , Juan M. Marmolejo-Tejada , Martín A. Mosquera

We present a natural orbital-based implementation of the intermediate Hamiltonian Fock space coupled-cluster method for (1,1) sector of Fock space. The use of natural orbital significantly reduces the computational cost and can…

Chemical Physics · Physics 2021-09-07 Soumi Haldar , Achintya Kumar Dutta

Coupled-cluster theories can be used to compute ab initio electronic correlation energies of real materials with systematically improvable accuracy. However, the widely-used coupled cluster singles and doubles plus perturbative triples…

Materials Science · Physics 2024-03-01 Nikolaos Masios , Andreas Irmler , Tobias Schäfer , Andreas Grüneis

Coupled cluster theory is the method of choice for weakly correlated systems. But in the strongly correlated regime, it faces a symmetry dilemma, where it either completely fails to describe the system, or has to artificially break certain…

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

Quantum--Mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those…

Chemical Physics · Physics 2015-06-12 Michele Pavanello , Troy Van Voorhis , Lucas Visscher , Johannes Neugebauer

We study the application of various forms of the coupled cluster method to systems with paired fermions. The novel element of the analysis is the study of the breaking and eventual restoration of particle number in the CCM variants. We…

Quantum Physics · Physics 2010-11-24 Chris Snape , Niels R. Walet

We consider a new formulation of the stochastic coupled cluster method in terms of the similarity transformed Hamiltonian. We show that improvement in the granularity with which the wavefunction is represented results in a reduction in the…

Chemical Physics · Physics 2016-02-02 Ruth S. T. Franklin , James S. Spencer , Alberto Zoccante , Alex J. W. Thom

The coupled cluster method has been applied to the eigenvalue problem lattice Hamiltonian QCD (without quarks) for SU(2) gauge fields in two space dimensions. Using a recently presented new formulation and the truncation prescription of Guo…

High Energy Physics - Lattice · Physics 2007-05-23 D. Schuette , A. Wichmann , C. Weichmann

Density functional theory (DFT) is the most widely used method for calculating molecular properties; however, its accuracy is often insufficient for quantitative predictions. Coupled-cluster (CC) theory is the most successful method for…

We present a perturbative triples correction to the relativistic quadratic unitary coupled cluster singles and doubles (qUCCSD) method, denoted as qUCCSD[T]. The method builds upon the Hermitian structure of the unitary ansatz and employs a…

Chemical Physics · Physics 2025-10-08 Kamal Majee , Ján Šimunek , Jozef Noga , Achintya Kumar Dutta

We propose a streamlined combination scheme of the transcorrelation (TC) and coupled cluster (CC) theory, which not only increases the convergence rate with respect to the basis set, but also extends the applicability of the lowest order CC…

Strongly Correlated Electrons · Physics 2021-07-28 Ke Liao , Thomas Schraivogel , Hongjun Luo , Daniel Kats , Ali Alavi

We have studied electron correlations in the doped two-dimensional (2D) Hubbard model by using the coupled-cluster method (CCM) to investigate whether or not the method can be applied to correct the independent particle approximations…

Strongly Correlated Electrons · Physics 2009-10-31 Yoshihiro Asai , Hideki Katagiri

While coupled cluster theory accurately models weakly correlated quantum systems, it often fails in the presence of strong correlations where the standard mean-field picture is qualitatively incorrect. In many cases, these failures can be…

Nuclear Theory · Physics 2020-05-14 Y. Qiu , T. M. Henderson , T. Duguet , G. E. Scuseria