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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…

Quantum Physics · Physics 2025-03-27 Muqing Zheng , Bo Peng , Ang Li , Xiu Yang , Karol Kowalski

Applications of quantum simulation algorithms to obtain electronic energies of molecules on noisy intermediate-scale quantum (NISQ) devices require careful consideration of resources describing the complex electron correlation effects. In…

Quantum Physics · Physics 2020-04-17 Mekena Metcalf , Nicholas P. Bauman , Karol Kowalski , Wibe A. de Jong

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

We demonstrate the use of the Variational Quantum Eigensolver (VQE) to simulate solid state crystalline materials. We adapt the Unitary Coupled Cluster ansatz to periodic boundary conditions in real space and momentum space representations…

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

We present a general approach within the relativistic coupled-cluster theory framework to calculate exactly the first order wave functions due to any rank perturbation operators. Using this method, we calculate the static dipole and…

Atomic Physics · Physics 2009-11-13 B. K. Sahoo

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

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…

Quantum Physics · Physics 2018-09-12 Ilya G. Ryabinkin , Tzu-Ching Yen , Scott N. Genin , Artur F. Izmaylov

Downfolding coupled cluster (CC) techniques have recently been introduced into quantum chemistry as a tool for the dimensionality reduction of the many-body quantum problem. As opposed to earlier formulations in physics and chemistry based…

Quantum Physics · Physics 2022-03-23 Nicholas P. Bauman , Karol Kowalski

We have developed a relativistic coupled-cluster theory to incorporate nuclear spin-dependent interaction Hamiltonians perturbatively. In this theory, the coupled-cluster operators in the electronic sector are defined as tensor operators of…

Atomic Physics · Physics 2011-05-19 B. K. Mani , D. Angom

Quantum simulation of chemical systems is one of the most promising near-term applications of quantum computers. The variational quantum eigensolver, a leading algorithm for molecular simulations on quantum hardware, has a serious…

Quantum Physics · Physics 2019-07-16 Harper R. Grimsley , Sophia E. Economou , Edwin Barnes , Nicholas J. Mayhall

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

There have been assertions in the literature that the variational and unitary forms of coupled cluster theory lead to the same energy functional. Numerical evidence from previous authors was inconsistent with this claim, yet the small…

Strongly Correlated Electrons · Physics 2020-05-14 Gaurav Harsha , Toru Shiozaki , Gustavo E. Scuseria

Variational quantum eigensolver (VQE) for electronic structure calculations is believed to be one major potential application of near term quantum computing. Among all proposed VQE algorithms, the unitary coupled cluster singles and doubles…

Quantum Physics · Physics 2020-10-13 Rongxin Xia , Sabre Kais

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

We present a study of the two dimensional circular quantum dot model Hamiltonian using a range of quantum chemical ab initio methods. Ground and excited state energies are computed on different levels of perturbation theories including the…

Chemical Physics · Physics 2022-03-23 Faruk Salihbegović , Alejandro Gallo , Andreas Grüneis

In this work, we combine the recently developed double unitary coupled cluster (DUCC) theory with the adaptive, problem-tailored variational quantum eigensolver (ADAPT-VQE) to explore accuracy of unitary downfolded Hamiltonians for quantum…

In single-reference coupled-cluster (CC) methods, one has to solve a set of non-linear polynomial equations in order to determine the so-called amplitudes which are then used to compute the energy and other properties. Although it is of…

Chemical Physics · Physics 2021-09-10 Antoine Marie , Fábris Kossoski , Pierre-François Loos

We propose an orbital optimized method for unitary coupled cluster theory (OO-UCC) within the variational quantum eigensolver (VQE) framework for quantum computers. OO-UCC variationally determines the coupled cluster amplitudes and also…

Strongly Correlated Electrons · Physics 2020-09-23 Wataru Mizukami , Kosuke Mitarai , Yuya O. Nakagawa , Takahiro Yamamoto , Tennin Yan , Yu-ya Ohnishi

A dynamical formulation of coupled cluster theory is derived using a variational principle. By allowing time-dependent single-particle functions, a high degree of adaptivity is introduced, allowing complex systems to be simulated with high…

Quantum Physics · Physics 2014-11-25 Simen Kvaal