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In this work we investigate methods to improve the efficiency and scalability of quantum algorithms for quantum chemistry applications. We propose a transformation of the electronic structure Hamiltonian in the second quantization framework…

We describe a compilation strategy for Variational Quantum Eigensolver (VQE) algorithms which use the Unitary Coupled Cluster (UCC) ansatz, designed to reduce circuit depth and gate count. This is achieved by partitioning Pauli exponential…

Quantum Physics · Physics 2020-08-28 Alexander Cowtan , Will Simmons , Ross Duncan

The factorized form of the unitary coupled cluster ansatz is a popular state preparation ansatz for electronic structure calculations of molecules on quantum computers. It often is viewed as an approximation (based on the Trotter product…

Chemical Physics · Physics 2022-02-16 Jia Chen , Hai-Ping Cheng , J. K. Freericks

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

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…

Quantum Physics · Physics 2024-06-06 Luca Erhart , Yuichiro Yoshida , Viktor Khinevich , Wataru Mizukami

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

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

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

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…

Chemical Physics · Physics 2025-07-28 Laura Grazioli , Marios-Petros Kitsaras , Stella Stopkowicz

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…

Chemical Physics · Physics 2023-05-29 Mohammad Haidar , Marko J. Rančić , Yvon Maday , Jean-Philip Piquemal

The study and prediction of chemical reactivity is one of the most important application areas of molecular quantum chemistry. Large-scale, fully error-tolerant quantum computers could provide exact or near-exact solutions to the underlying…

Quantum Physics · Physics 2019-09-12 Michael Kühn , Sebastian Zanker , Peter Deglmann , Michael Marthaler , Horst Weiß

Methods which aim at universal applicability must be able to describe both weak and strong electronic correlation with equal facility. Such methods are in short supply. The combination of symmetry projection for strong correlation and…

Chemical Physics · Physics 2020-05-14 Yiheng Qiu , Thomas M. Henderson , Jinmo Zhao , Gustavo E. Scuseria

A major difficulty in quantum simulation is the adequate treatment of a large collection of entangled particles, synonymous with electron correlation in electronic structure theory, with coupled cluster (CC) theory being the leading…

Chemical Physics · Physics 2024-06-06 Zachary W. Windom , Daniel Claudino , Rodney J. Bartlett

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

We present a quantum-classical hybrid algorithm that simulates electronic structures of periodic systems such as ground states and quasiparticle band structures. By extending the unitary coupled cluster (UCC) theory to describe crystals in…

Quantum Physics · Physics 2022-02-16 Nobuyuki Yoshioka , Takeshi Sato , Yuya O. Nakagawa , Yu-ya Ohnishi , Wataru Mizukami

A highly anticipated use of quantum computers is the simulation of complex quantum systems including molecules and other many-body systems. One promising method involves directly applying a linear combination of unitaries (LCU) to…

Quantum Physics · Physics 2022-02-02 Richard Meister , Simon C. Benjamin , Earl T. Campbell

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

Clustering is a fundamental task for analyzing unlabeled data based solely on its underlying distribution. Spectral clustering is a clustering method that represents a dataset as a graph and uses the relationships between data points.…

Quantum Physics · Physics 2025-04-01 Hyeong-Gyu Kim , Siheon Park , June-Koo Kevin Rhee

We present a quantum linear response (qLR) approach within an active-space framework for computing indirect nuclear spin-spin coupling constants, a key ingredient in NMR spectra predictions. The method employs the unitary coupled cluster…

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…