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We present a new linear scaling method for the energy minimization step of semiempirical and first-principles Hartree-Fock and Kohn-Sham calculations. It is based on the self-consistent calculation of the optimum localized orbitals of any…

Materials Science · Physics 2009-11-10 Luis Seijo , Zoila Barandiaran

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,…

We illustrate how the systematic inclusion of multi-spin correlations of the quantum spin-lattice systems can be efficiently implemented within the framework of the coupled-cluster method by examining the ground-state properties of both the…

Statistical Mechanics · Physics 2017-08-24 Chen Zeng , D. J. J. Farnell , R. F. Bishop

In quantum chemistry, one of the most important challenges is the static correlation problem when solving the electronic Schr\"odinger equation for molecules in the Born--Oppenheimer approximation. In this article, we analyze the tailored…

Numerical Analysis · Mathematics 2019-11-21 Fabian M. Faulstich , Andre Laestadius , Örs Legeza , Reinhold Schneider , Simen Kvaal

Accurate modeling of surface catalytic processes often requires methods capable of describing strong correlation, charge transfer, and multiple closely lying electronic states. While density functional theory remains widely used, its…

We describe a modification of the stochastic coupled cluster algorithm that allows the use of multiple reference determinants. By considering the secondary references as excitations of the primary reference and using them to change the…

Chemical Physics · Physics 2020-10-22 Maria-Andreea Filip , Charles J. C. Scott , Alex J. W. Thom

Coupled cluster (CC) theory is often considered the gold standard of quantum-chemistry. For solids, however, the available software is scarce. We present CC-aims, which can interface ab initio codes with localized atomic orbitals and the CC…

Materials Science · Physics 2022-04-14 Evgeny Moerman , Felix Hummel , Andreas Grüneis , Andreas Irmler , Matthias Scheffler

We investigate the use of orbital-optimized references in conjunction with single-reference coupled-cluster theory with single and double substitutions (CCSD) for the study of core excitations and ionizations of 18 small organic molecules,…

We present computational chemistry data for small molecules ($CO$, $HCl$, $F_2$, $NH_4^+$, $CH_4$, $NH_{3}$, $H_3O^+$, $H{_2}O$, $BeH_{2}$, $LiH$, $OH^-$, $HF$, $HeH^+$, $H_2$), obtained by implementing the Unitary Coupled Cluster method…

Quantum Physics · Physics 2019-07-02 V. Armaos , Dimitrios A. Badounas , Paraskevas Deligiannis

In this work, we combine the many-body formulation of the internally contracted multireference coupled cluster (ic-MRCC) method with Evangelista's multireference formulation of the driven similarity renormalization group (DSRG). The DSRG…

Chemical Physics · Physics 2025-03-04 Robin Feldmann , Markus Reiher

We introduce the multistate iterative qubit coupled cluster (MS-iQCC) method, a quantum-inspired algorithm that runs efficiently on classical hardware and is designed to predict both ground and excited electronic states of molecules.…

Chemical Physics · Physics 2026-01-05 Robert A. Lang , Shashank G. Mehendale , Ilya G. Ryabinkin , Artur F. Izmaylov

The practical application of quantum technologies to chemical problems faces significant challenges, particularly in the treatment of realistic basis sets and the accurate inclusion of electron correlation effects. A direct approach to…

In this paper, we have developed a unitary variant of a double exponential coupled cluster theory, which is capable of mimicking the effects of connected excitations of arbitrarily high rank, using only rank-one and rank-two parametrization…

Chemical Physics · Physics 2022-11-23 Dipanjali Halder , V. S. Prasannaa , Rahul Maitra

Modeling multimetallic systems efficiently enables faster prediction of desirable chemical properties and design of new materials. This work describes an initial implementation for performing multireference wave function method localized…

Computational Physics · Physics 2025-05-08 Valay Agarawal , Rishu Khurana , Cong Liu , Matthew R. Hermes , Christopher Knight , Laura Gagliardi

A novel approach to rapidly converging high-level coupled-cluster (CC) energetics in an automated fashion is proposed. The key idea is an adaptive selection of the excitation manifolds defining higher-than-two-body components of the cluster…

Chemical Physics · Physics 2023-08-25 Karthik Gururangan , Piotr Piecuch

Solving problems related to planning and operations of large-scale power systems is challenging on classical computers due to their inherent nature as mixed-integer and nonlinear problems. Quantum computing provides new avenues to approach…

Quantum Physics · Physics 2025-05-02 Willie Aboumrad , Phani R V Marthi , Suman Debnath , Martin Roetteler , Evgeny Epifanovsky

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

In electronic structure theory, restricted single-reference coupled cluster (CC) captures weak correlation but fails catastrophically under strong correlation. Spin-projected unrestricted Hartree-Fock (SUHF), on the other hand, misses weak…

Chemical Physics · Physics 2017-11-22 John A. Gomez , Thomas M. Henderson , Gustavo E. Scuseria

We propose a modified coupled cluster Monte Carlo algorithm that stochastically samples connected terms within the truncated Baker--Campbell--Hausdorff expansion of the similarity transformed Hamiltonian by construction of coupled cluster…

Chemical Physics · Physics 2019-06-19 Charles J. C. Scott , Roberto Di Remigio , T. Daniel Crawford , Alex J. W. Thom

Three fully variational formulations of the complete-active space coupled-cluster (CASCC) method are derived. The formulations include the ability to approximate the model vectors by smooth manifolds, thereby opening up the possibility for…

Chemical Physics · Physics 2023-07-12 Simen Kvaal
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