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The Coupled Cluster (CC) method is used to compute the electronic correlation energy in atoms and molecules and often leads to highly accurate results. However, due to its single-reference nature, standard CC in its projected form fails to…

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…

化学物理 · 物理学 2021-01-07 Maria-Andreea Filip , Alex J. W. Thom

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…

化学物理 · 物理学 2023-09-22 Tanner Culpitt , Erik I. Tellgren , Fabijan Pavosevic

We introduce a hybrid quantum-classical algorithm, the localized active space unitary selective coupled cluster singles and doubles (LAS-USCCSD) method. Derived from the localized active space unitary coupled cluster (LAS-UCCSD) method,…

Unitary Coupled Cluster (UCC) approaches are an appealing route to utilising quantum hardware to perform quantum chemistry calculations, as quantum computers can in principle perform UCC calculations in a polynomially scaling fashion, as…

量子物理 · 物理学 2022-06-15 Maria-Andreea Filip , Nathan Fitzpatrick , David Muñoz Ramo , Alex J. W. Thom

We introduce a unitary coupled-cluster (UCC) ansatz termed $k$-UpCCGSD that is based on a family of sparse generalized doubles (D) operators which provides an affordable and systematically improvable unitary coupled-cluster wavefunction…

量子物理 · 物理学 2019-01-07 Joonho Lee , William J. Huggins , Martin Head-Gordon , K. Birgitta Whaley

The unitary coupled cluster (UCC) approximation is one of the more promising wave-function ans\"atze for electronic structure calculations on quantum computers via the variational quantum eigensolver algorithm. However, for large systems…

量子物理 · 物理学 2021-09-30 Jia Chen , Hai-Ping Cheng , James K. Freericks

A unitary coupled-cluster (UCC) form for the wavefunction in the variational quantum eigensolver has been suggested as a systematic way to go beyond the mean-field approximation and include electron correlation in solving quantum chemistry…

量子物理 · 物理学 2018-09-12 Ilya G. Ryabinkin , Tzu-Ching Yen , Scott N. Genin , Artur F. Izmaylov

In this work, we investigate the possibility of improving multireference-driven coupled cluster (CC) approaches with an algorithm that iteratively combines complete active space (CAS) calculations with tailored CC and externally corrected…

化学物理 · 物理学 2025-03-06 Robin Feldmann , Max Mörchen , Jakub Lang , Michał Lesiuk , Markus Reiher

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…

化学物理 · 物理学 2022-05-09 Dmitry A. Fedorov , Yuri Alexeev , Stephen K. Gray , Matthew Otten

In Coupled-Cluster (CC) theory, unphysical complex energies may arise in the presence of strong magnetic fields, near conical intersections, or in systems exhibiting complex Abelian point group symmetries. This issue originates from the…

化学物理 · 物理学 2025-07-28 Laura Grazioli , Marios-Petros Kitsaras , Stella Stopkowicz

Introducing an active space approximation is inevitable for the quantum computations of chemical systems. However, this approximation ignores the electron correlations related to non-active orbitals. Here, we propose a computational method…

量子物理 · 物理学 2024-06-06 Luca Erhart , Yuichiro Yoshida , Viktor Khinevich , Wataru Mizukami

The Trotterized Unitary Coupled Cluster Single and Double (UCCSD) ansatz has recently attracted interest due to its use in Variation Quantum Eigensolver (VQE) molecular simulations on quantum computers. However, when the size of molecules…

化学物理 · 物理学 2023-05-29 Mohammad Haidar , Marko J. Rančić , Yvon Maday , Jean-Philip Piquemal

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…

化学物理 · 物理学 2022-11-01 Harper R. Grimsley , Nicholas J. Mayhall

The tailored coupled cluster (TCC) approach is a promising ansatz that preserves the simplicity of single-reference coupled cluster theory, while incorporating a multi-reference wave function through amplitudes obtained from a preceding…

化学物理 · 物理学 2021-01-07 Maximilian Mörchen , Leon Freitag , Markus Reiher

We present a four-component relativistic unitary coupled cluster method for molecules. We have used commutator-based non-perturbative approximation using the ''Bernoulli expansion'' to derive an approximation to the relativistic unitary…

化学物理 · 物理学 2024-03-06 Kamal Majee , Tamoghna Mukhopadhyay , Malaya K. Nayak , Achintya Kumar Dutta

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,…

量子物理 · 物理学 2026-02-17 Jeremy Canfield , Dominika Zgid , J K Freericks

The factorized form of the unitary coupled-cluster approximation is one of the most promising methodologies to prepare trial states for strongly correlated systems within the variational quantum eigensolver framework. The factorized form of…

量子物理 · 物理学 2022-01-05 Luogen Xu , Joseph T. Lee , J. K. Freericks

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,…

量子物理 · 物理学 2017-03-01 Yangchao Shen , Xiang Zhang , Shuaining Zhang , Jing-Ning Zhang , Man-Hong Yung , Kihwan Kim

Hybrid quantum-classical approaches offer potential solutions to quantum chemistry problems, yet they often manifest as constrained optimization problems. Here, we explore the interconnection between constrained optimization and generalized…

量子物理 · 物理学 2025-03-27 Muqing Zheng , Bo Peng , Ang Li , Xiu Yang , Karol Kowalski
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