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We present several coupled-cluster calculations of ground and excited states of 4He and 16O employing methods from quantum chemistry. A comparison of coupled cluster results with the results of exact diagonalization of the hamiltonian in…

In this tutorial-style review we discuss basic concepts of coupled cluster theory and recent developments that increase its computational efficiency for calculations of molecules, solids and materials in general. We will touch upon the…

Materials Science · Physics 2020-04-15 Igor Ying Zhang , Andreas Grüneis

Quantum computational chemistry has emerged as an important application of quantum computing. Hybrid quantum-classical computing methods, such as variational quantum eigensolvers (VQE), have been designed as promising solutions to quantum…

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

In classical computational chemistry, the coupled-cluster ansatz is one of the most commonly used $ab~initio$ methods, which is critically limited by its non-unitary nature. The unitary modification as an ideal solution to the problem is,…

Quantum Physics · Physics 2017-03-01 Yangchao Shen , Xiang Zhang , Shuaining Zhang , Jing-Ning Zhang , Man-Hong Yung , Kihwan Kim

Coupled cluster theory produced arguably the most widely used high-accuracy computational quantum chemistry methods. Despite the approach's overall great computational success, its mathematical understanding is so far limited to results…

Algebraic Geometry · Mathematics 2024-03-29 Fabian M. Faulstich , Mathias Oster

Molecular fragment or embedding methods are powerful techniques for overcoming scalability limitations in electronic structure theory by dividing large molecular systems into individual units that are small enough to be treated using…

Chemical Physics · Physics 2017-08-14 Jason N. Byrd , Robert W. Molt, , Rodney J. Bartlett , Beverly A. Sanders

Computationally efficient and accurate quantum mechanical approximations to solve the many-electron Schr\"odinger equation are at the heart of computational materials science. In that respect the coupled cluster hierarchy of methods plays a…

Materials Science · Physics 2022-01-11 Tina N. Mihm , Tobias Schäfer , Sai Kumar Ramadugu , Andreas Grüneis , James J. Shepherd

We propose a relativistic unitary coupled cluster (UCC) expectation value approach for computing first-order properties of heavy-element systems. Both perturbative (UCC3) and non-perturbative (qUCC) commutator-based formulations are applied…

Chemical Physics · Physics 2026-02-03 Kamal Majee , Somesh Chamoli , Malaya K. Nayak , Achintya Kumar Dutta

In order to explore the effects of high levels of electron correlation on the real-time coupled cluster formalism and algorithmic behavior, we introduce a time-dependent implementation of the CC3 singles, doubles and approximate triples…

Chemical Physics · Physics 2025-01-23 Zhe Wang , Håkon Emil Kristiansen , Thomas Bondo Pedersen , T. Daniel Crawford

Coupled cluster calculations are traditionally performed over Hartree-Fock reference orbitals (HF-CC methodology). However, it has been repeatedly argued in the literature that the use of a Kohn-Sham reference (KS-CC methodology) might…

Chemical Physics · Physics 2025-03-10 Zsolt Benedek , Paula Tímár , Tibor Szilvási , Gergely Barcza

The development of multireference coupled cluster (MRCC) techniques has remained an open area of study in electronic structure theory for decades due to the inherent complexity of expressing a multi-configurational wavefunction in the…

Chemical Physics · Physics 2023-05-24 Maria-Andreea Filip , Alex J. W. Thom

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

This chapter discusses contemporary quantum chemical methods and provides general insights into modern electronic structure theory with a focus on heavy-element-containing compounds. We first give a short overview of relativistic…

Chemical Physics · Physics 2020-02-18 Aleksandra Leszczyk , Paweł Tecmer , Katharina Boguslawski

A unitary coupled-cluster (UCC)-based self-consistent electron propagator theory (EPT) is proposed for the description of electron-detached and electron-attached states. Two practical schemes, termed IP/EA-UCC3 and IP/EA-qUCCSD, are…

Chemical Physics · Physics 2026-03-03 Yu Zhang , Junzi Liu

The practical application of quantum technologies to chemical problems faces significant challenges, particularly in the treatment of realistic basis sets and the accurate inclusion of electron correlation effects. A direct approach to…

Coupled cluster theory is one of the most popular post-Hartree-Fock methods for ab initio molecular quantum chemistry. The finite-size error of the correlation energy in periodic coupled cluster calculations for three-dimensional insulating…

Numerical Analysis · Mathematics 2024-04-02 Xin Xing , Lin Lin

We introduce perturbation and coupled-cluster theories based on a cluster mean-field reference for describing the ground state of strongly-correlated spin systems. In cluster mean-field, the ground state wavefunction is written as a simple…

The pair-coupled-cluster doubles (pCCD) method has emerged as a viable approach for quantum-chemical studies of strongly correlated systems. Despite its lower formal scaling (O(N$^4$)) compared to other versions of coupled cluster (CC)…

Chemical Physics · Physics 2026-04-17 Rahul Chakraborty , Paweł Tecmer

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