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A systematic method for determining correlated wavefunctions of extended systems in the ground and excited states is presented. It allows to fully exploit the power of quantum-chemical programs designed for correlation calculations of…

Other Condensed Matter · Physics 2007-05-23 V. Bezugly

The calculation of excited state energies of electronic structure Hamiltonians has many important applications, such as the calculation of optical spectra and reaction rates. While low-depth quantum algorithms, such as the variational…

Quantum Physics · Physics 2019-07-03 Oscar Higgott , Daochen Wang , Stephen Brierley

Arguably the most widely used approaches for obtaining highly accurate molecular ground-state energies are coupled cluster methods. Despite introducing two layers of approximation, a linear and a nonlinear one, coupled cluster methods…

Numerical Analysis · Mathematics 2026-05-22 Jonas Beck , Benjamin Stamm

Unitary coupled cluster (UCC), originally developed as a variational alternative to the popular traditional coupled cluster method, has seen a resurgence as a functional form for use on quantum computers. However, the number of excitors…

Chemical Physics · Physics 2021-01-07 Maria-Andreea Filip , Alex J. W. Thom

Inspired by our earlier semi-stochastic work aimed at converging high-level coupled-cluster (CC) energetics [J. E. Deustua, J. Shen, and P. Piecuch, Phys. Rev. Lett. 119, 223003 (2017); J. Chem. Phys. 154, 124103 (2021)], we propose a novel…

Chemical Physics · Physics 2022-10-06 Karthik Gururangan , J. Emiliano Deustua , Jun Shen , Piotr Piecuch

The reformulated coupled-cluster method (CCM), in which average many-body potentials are introduced, provides a useful framework to organize numerous terms appearing in CCM equations, which enables us to clarify the structure of the CCM…

Nuclear Theory · Physics 2015-06-05 M. Kohno , R. Okamoto

The central problem in electronic structure theory is the computation of the eigenvalues of the electronic Hamiltonian -- an unbounded, self-adjoint operator acting on a Hilbert space of antisymmetric functions. Coupled cluster (CC)…

Numerical Analysis · Mathematics 2023-01-30 Muhammad Hassan , Yvon Maday , Yipeng Wang

Recent work from our research group has demonstrated that symmetry-projected Hartree--Fock (HF) methods provide a compact representation of molecular ground state wavefunctions based on a superposition of non-orthogonal Slater determinants.…

Chemical Physics · Physics 2015-06-17 Carlos A. Jiménez-Hoyos , R. Rodríguez-Guzmán , Gustavo E. Scuseria

We extend the CIPSI-driven CC($P$;$Q$) methodology [K. Gururangan et al., J. Chem. Phys. 155 (2021) 174114], in which the leading higher-than-doubly excited determinants are identified using the selected configuration interaction (CI)…

Chemical Physics · Physics 2026-02-24 Swati S. Priyadarsini , Karthik Gururangan , Piotr Piecuch

Tailored coupled cluster theory represents a computationally inexpensive way to describe static and dynamical electron correlation effects. In this work, we scrutinize the performance of various tailored coupled cluster methods externally…

Chemical Physics · Physics 2021-03-24 Aleksandra Leszczyk , Mihály Máté , Örs Legeza , Katharina Boguslawski

When electron correlations are important it is often necessary to use numerical methods to solve the Hamiltonian for a finite system (cluster) "exactly". Unfortunately, such methods are restricted to small systems. We propose to combine the…

Strongly Correlated Electrons · Physics 2009-10-31 Maciej M. Maska

The coupled cluster method (CCM) has previously been applied to study the ground- and excited-state properties of many different types of frustrated and unfrustrated quantum spin systems. A common feature in the application of the CCM is to…

Strongly Correlated Electrons · Physics 2014-02-20 Damian J. J. Farnell , Andrew I. Croudace

Based on a parametric point-wise decomposition, a kind of isospectral deformation, of the exact one-particle probability density of an externally confined, analytically solvable interacting two-particle model system we introduce the…

Quantum Physics · Physics 2014-06-12 C. L. Benavides-Riveros , I. Nagy

A central difficulty of state-specific Multi-Reference Coupled Cluster (MR-CC) formalisms concerns the definition of the amplitudes of the single and double excitation operators appearing in the exponential wave operator. If the reference…

Chemical Physics · Physics 2017-04-20 Yann Garniron , Emmanuel Giner , Jean-Paul Malrieu , Anthony Scemama

We implement the Multi-Reference Unitary Coupled Cluster Singles and Doubles (MR-UCCSD) model with a quantum circuit that conserves the particle number to study the ground state energies of LiH, BeH$_2$, and H$_6$. This approach simplifies…

Quantum Physics · Physics 2025-04-15 Di Wu , C. L. Bai , H. Sagawa , H. Q. Zhang

Using the ground-state energy of 16-O obtained with the realistic V_UCOM interaction as a test case, we present a comprehensive comparison of different configuration interaction (CI) and coupled-cluster (CC) methods, analyzing the intrinsic…

Nuclear Theory · Physics 2009-06-30 R. Roth , J. R. Gour , P. Piecuch

We report the first investigation of the performance of EOM-CC4 -- an approximate equation-of-motion coupled-cluster model which includes iterative quadruple excitations -- for vertical excitation energies in molecular systems. By…

Chemical Physics · Physics 2021-06-14 Pierre-François Loos , Devin A. Matthews , Filippo Lipparini , Denis Jacquemin

Despite their high accuracy, standard coupled cluster models cannot be used for nonadiabatic molecular dynamics simulations because they yield unphysical complex excitation energies at conical intersections between same-symmetry excited…

Chemical Physics · Physics 2025-04-16 Leo Stoll , Sara Angelico , Eirik F. Kjønstad , Henrik Koch

The phenomenon of orbital relaxation upon excitation of core electrons is a major problem in the linear-response treatment of core-hole spectroscopies. Rather than addressing relaxation through direct dynamical correlation of the excited…

Chemical Physics · Physics 2025-03-26 Megan Simons , Devin A. Matthews

While limited coupled cluster theory is \textit{formally} nonvariational, it is not broadly appreciated whether this is a major issue \textit{in practice}. We carried out a detailed comparison with \textit{de facto} full CI energies for a…

Chemical Physics · Physics 2024-10-03 Jan M. L. Martin , Emmanouil Semidalas
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