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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…

Unitary Coupled Cluster (UCC) theory is a promising variational method for electronic structure calculations, especially for strongly correlated systems and quantum computers. However, its practical application is limited by the steep…

Chemical Physics · Physics 2026-02-05 Prateek Vaish , Brenda Rubenstein

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…

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…

Chemical Physics · Physics 2025-03-06 Robin Feldmann , Max Mörchen , Jakub Lang , Michał Lesiuk , Markus Reiher

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 implement the Multi-Reference Unitary Coupled Cluster Singles and Doubles (MR-UCCSD) model with a quantum circuit that conserves the particle number to study the ground state energies of LiH, BeH$_2$, and H$_6$. This approach simplifies…

Quantum Physics · Physics 2025-04-15 Di Wu , C. L. Bai , H. Sagawa , H. Q. Zhang

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

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…

Chemical Physics · Physics 2021-01-07 Maria-Andreea Filip , Alex J. W. Thom

Accurately describing strongly correlated systems with affordable quantum resources remains a central challenge for quantum chemistry applications on near and intermediate-term quantum computers. The localized active space self-consistent…

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…

Quantum Physics · Physics 2019-01-07 Joonho Lee , William J. Huggins , Martin Head-Gordon , K. Birgitta Whaley

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…

Quantum Physics · Physics 2022-06-15 Maria-Andreea Filip , Nathan Fitzpatrick , David Muñoz Ramo , Alex J. W. Thom

The localized active space self consistent field (LASSCF) method factorizes a complete active space (CAS) wave function into an antisymmetrized product of localized active space wave function fragments. Correlation between fragments is then…

Chemical Physics · Physics 2024-03-26 Valay Agarawal , Daniel King , Matthew R. Hermes , Laura Gagliardi

The factorized form of unitary coupled cluster theory (UCC) is a promising wave-function ansatz for the variational quantum eigensolver algorithm. Here, we present a quantum inspired algorithm for UCC based on an exact operator identity for…

Strongly Correlated Electrons · Physics 2020-09-24 Jia Chen , Hai-Ping Cheng , James Freericks

Fragmentation methods applied to multireference wave functions constitute a road towards the application of highly accurate ab initio wave function calculations to large molecules and solids. However, it is important for reproducibility and…

Chemical Physics · Physics 2020-07-23 Matthew R. Hermes , Laura Gagliardi

Localized orbital coupled cluster theory has recently emerged as an nonempirical alternative to DFT for large systems. Intuitively, one might expect such methods to perform less well for highly delocalized systems. In the present work, we…

Chemical Physics · Physics 2020-10-16 Nitai Sylvetsky , Ambar Banerjee , Mercedes Alonso , Jan M. L. Martin

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

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 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…

Chemical Physics · Physics 2022-11-01 Harper R. Grimsley , Nicholas J. Mayhall

A relativistic version of the coupled-cluster single-double (CCSD) method is developed for atoms with a single valence electron. In earlier work, a linearized version of the CCSD method (with extensions to include a dominant class of triple…

Atomic Physics · Physics 2009-11-13 Rupsi Pal , M. S. Safronova , W. R. Johnson , Andrei Derevianko , Sergey G. Porsev

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
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