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We propose a non-iterative, post hoc correction to the unitary coupled cluster theory with single, double, and triple excitations (UCCSDT) ansatz, which considers the leading-order effects of neglected quadruple excitations. We present two…

Chemical Physics · Physics 2025-08-14 Zachary W. Windom , Luke Bertels , Daniel Claudino , Rodney J. Bartlett

An implementation of the coupled-cluster single- and double excitations (CCSD) method on two-dimensional quantum dots is presented. Advantages and limitations are studied through comparison with other high accuracy approaches for two to…

Mesoscale and Nanoscale Physics · Physics 2013-05-30 Erik Waltersson , Eva Lindroth

Molecular ground-state simulation is one of the most promising fields for demonstrating practical quantum advantage on near-term quantum computers. However, the Variational Quantum Eigensolver (VQE), a leading algorithm for this task, still…

Quantum Physics · Physics 2025-07-08 Runhong He , Qiaozhen Chai , Xin Hong , Ji Guan , Guolong Cui , Shengbin Wang , Shenggang Ying

The unitary coupled cluster (UCC) algorithm is one of the most promising implementations of the variational quantum eigensolver for quantum computers. However, for large systems, the number of UCC factors leads to deep quantum circuits,…

Quantum Physics · Physics 2026-02-17 Jeremy Canfield , Dominika Zgid , J K Freericks

One of the commonly used chemical-inspired approaches in variational quantum computing is the unitary coupled-cluster (UCC) ansatze. Despite being a systematic way of approaching the exact limit, the number of parameters in the standard UCC…

Quantum Physics · Physics 2023-06-06 Shashank G Mehendale , Bo Peng , Niranjan Govind , Yuri Alexeev

Non-unitary theories are commonly seen in the classical simulations of quantum systems. Among these theories, the method of moments of coupled-cluster equations (MMCCs) and the ensuing classes of the renormalized coupled-cluster (CC)…

Quantum Physics · Physics 2022-12-13 Bo Peng , Karol Kowalski

We present a review of the Unitary Coupled Cluster (UCC) ansatz and related ans\"atze which are used to variationally solve the electronic structure problem on quantum computers. A brief history of coupled cluster (CC) methods is provided,…

Quantum computation represents a revolutionary approach for solving problems in quantum chemistry. However, due to the limited quantum resources in the current noisy intermediate-scale quantum (NISQ) devices, quantum algorithms for large…

Quantum Physics · Physics 2023-04-17 Yi Fan , Changsu Cao , Xusheng Xu , Zhenyu Li , Dingshun Lv , Man-Hong Yung

Due to their non-iterative nature, fixed Unitary Coupled-Cluster (UCC) ans\"atze are attractive for performing quantum chemistry Variational Quantum Eigensolver (VQE) computations as they avoid pre-circuit measurements on a quantum…

Immense interest in quantum computing has prompted development of electronic structure methods that are suitable for quantum hardware. However, the slow pace at which quantum hardware progresses, forces researchers to implement their ideas…

Quantum Physics · Physics 2025-02-26 Ilya G. Ryabinkin , Seyyed Mehdi Hosseini Jenab , Scott N. Genin

A formal analysis is conducted on the exactness of various forms of unitary coupled cluster (UCC) theory based on particle-hole excitation and de-excitation operators. Both the conventional single exponential UCC parameterization and a…

Chemical Physics · Physics 2020-01-29 Francesco A. Evangelista , Garnet Kin-Lic Chan , Gustavo E. Scuseria

The coupled cluster method is considered a gold standard in quantum chemistry, reliably giving energies that are exact within chemical accuracy (1.6 mHartree). However, even in the CCSD approximation, where the cluster operator is truncated…

Chemical Physics · Physics 2023-03-10 Simon Elias Schrader , Simen Kvaal

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 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

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

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

Quantum chemistry calculations of large, strongly correlated systems are typically limited by the computation cost that scales exponentially with the size of the system. Quantum algorithms, designed specifically for quantum computers, can…

We consider the rank-reduced coupled-cluster theory with single and double excitations (RR-CCSD) introduced recently [Parrish \emph{et al.}, J. Chem. Phys. {\bf 150}, 164118 (2019)]. The main feature of this method is the decomposed form of…

Chemical Physics · Physics 2022-02-21 Michał Lesiuk

We present the quantum-selected configuration interaction-tailored coupled-cluster (QSCI-TCC) method, a hybrid quantum-classical scheme that tailors coupled-cluster (CC) theory with a quantum-selected configuration interaction (QSCI) wave…

Chemical Physics · Physics 2025-06-23 Luca Erhart , Yuichiro Yoshida , Wataru Mizukami

The pair coupled cluster doubles (pCCD) method (where the excitation manifold is restricted to electron pairs) has a series of interesting features. Among others, it provides ground-state energies very close to what is obtained with…