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We investigate the basis-set convergence of electronic correlation energies calculated using coupled cluster theory and a recently proposed finite basis-set correction technique. The correction is applied to atomic and molecular systems and…

Chemical Physics · Physics 2019-10-03 Andreas Irmler , Andreas Grüneis

Ab initio methods based on the second-order and higher connected moments, or cumulants, of a reference function have seen limited use in the determination of correlation energies of chemical systems throughout the years. Moment-based…

Chemical Physics · Physics 2023-08-25 Brad Ganoe , Martin Head-Gordon

Simulating molecules using the Variational Quantum Eigensolver method is one of the promising applications for NISQ-era quantum computers. Designing an efficient ansatz to represent the electronic wave function is crucial in such…

Chemical Physics · Physics 2022-05-09 Dmitry A. Fedorov , Yuri Alexeev , Stephen K. Gray , Matthew Otten

Highly accurate methods such as coupled cluster (CC) techniques can be used for periodic systems within the framework of the method of increments. Its extension to low-dimensional conducting system is considered. To demonstrate the…

Materials Science · Physics 2012-01-31 Elena Voloshina

The double ionization potential (DIP) equation-of-motion (EOM) coupled-cluster (CC) method with a full treatment of 4-hole-2-particle (4$h$-2$p$) correlations and triply excited clusters, abbreviated as DIP-EOMCCSDT(4$h$-2$p$), and its…

Chemical Physics · Physics 2025-02-12 Karthik Gururangan , Achintya Kumar Dutta , Piotr Piecuch

The variational quantum eigensolver (VQE) algorithm, designed to calculate the energy of molecular ground states on near-term quantum computers, requires specification of symmetries that describe the system, e.g. spin state and number of…

Quantum Physics · Physics 2020-06-18 Gabriel Greene-Diniz , David Muñoz Ramo

The projection-based quantum embedding method is applied to electronically excited states of valence, Rydberg, and charge-transfer character, valence- and core-ionized states, as well as bound and temporary radical anions. We embed…

Chemical Physics · Physics 2021-06-10 Valentina Parravicini , Thomas-C. Jagau

We introduce a multimodel approach to solve coupled cluster equations, employing a quasi Newton algorithm for the ground state and an Olsen algorithm for the excited states. In these algorithms, both of which can be viewed as Newton…

Chemical Physics · Physics 2020-07-15 Eirik F. Kjønstad , Sarai D. Folkestad , Henrik Koch

We present an implementation of equation of motion coupled-cluster singles and doubles (EOM-CCSD) theory using periodic boundary conditions and a plane wave basis set. Our implementation of EOM-CCSD theory is applied to study $F$-centers in…

Materials Science · Physics 2021-02-09 Alejandro Gallo , Felix Hummel , Andreas Irmler , Andreas Grüneis

We study quantum spin systems in the 1D, 2D square and 3D cubic lattices with nearest-neighbour XY exchange. We use the coupled-cluster method (CCM) to calculate the ground-state energy, the T=0 sublattice magnetisation and the excited…

Condensed Matter · Physics 2009-10-30 D. J. J. Farnell , S. E. Krueger , J. B. Parkinson

The coupled cluster method (CCM) is a method of quantum many-body theory that may provide accurate results for the ground-state properties of lattice quantum spin systems even in the presence of strong frustration and for lattices of…

Strongly Correlated Electrons · Physics 2009-11-11 D. J. J. Farnell , J. Schulenburg , J. Richter , K. A. Gernoth

Quantum embedding methods have recently developed significantly to model large molecular structures. This work proposes a novel wave function theory in density functional theory (WTF-in-DFT) embedding scheme based on pair-coupled cluster…

Chemical Physics · Physics 2024-01-10 Rahul Chakraborty , Katharina Boguslawski , Paweł Tecmer

In this paper, we report on the implementation of CC2 and CC3 in the context of molecules in finite magnetic fields. The methods are applied to the investigation of atoms and molecules through spectroscopic predictions and geometry…

Chemical Physics · Physics 2024-03-08 Marios-Petros Kitsaras , Laura Grazioli , Stella Stopkowicz

This work presents the automatic generation of analytic first derivatives of the energy for general coupled-cluster models using the \text{tenpi} toolchain. We report the first implementation of expectation values for CCSDT and CCSDTQ…

Chemical Physics · Physics 2025-04-28 Gabriele Fabbro , Jan Brandejs , Trond Saue

The search for new \emph{ab initio} models rapidly delivering accurate excited state energies and properties is one of the most active research lines of theoretical chemistry. Along with these methodological developments, the performances…

Chemical Physics · Physics 2020-06-05 Pierre-François Loos , Denis Jacquemin

In truncated coupled-cluster (CC) theories, non-variational and/or generally complex ground-state energies can occur. This is due to the non-Hermitian nature of the similarity transformed Hamiltonian matrix in combination with CC…

Chemical Physics · Physics 2023-09-22 Tanner Culpitt , Erik I. Tellgren , Fabijan Pavosevic

An efficient excited state method, named xCDFCI, in the configuration interaction framework, is proposed. xCDFCI extends the unconstrained nonconvex optimization problem in coordinate descent full configuration interaction~(CDFCI) to a…

Chemical Physics · Physics 2023-08-23 Zhe Wang , Zhiyuan Zhang , Jianfeng Lu , Yingzhou Li

In this article we study the effects of higher body excitations in the relativistic CC calculations for atoms and ions with one valence electron using Fock-space CCSD, CCSD(T) and its unitary variants. The present study demonstrates that…

Atomic Physics · Physics 2009-11-13 Chiranjib Sur , Rajat K Chaudhuri

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 development of variational density functional theory approaches to excited electronic states is impeded by limitations of the commonly used self-consistent field (SCF) procedure. A method based on a direct optimization approach as well…

Chemical Physics · Physics 2022-11-09 Gianluca Levi , Aleksei V. Ivanov , Hannes Jónsson
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