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Neutral uranium (U I) is a very difficult atom for theoretical calculations due to a large number of valence electrons, six, strong valence-valence and valence-core correlations, high density of states, and relativistic effects.…

Atomic Physics · Physics 2020-10-14 Igor M. Savukov

Incremental full configuration interaction (iFCI) is polynomial-cost approach to the FCI limit of electronic structure. This article introduces the many-body basis set amelioration (MBBSA) method, which is designed to allow iFCI to be…

Chemical Physics · Physics 2025-03-12 Jeffrey P Hatch , Alan E Rask , Duy-Khoi Dang , Paul M Zimmerman

[Background] Single-reference density functional theory is very successful in reproducing bulk nuclear properties like binding energies, radii, or quadrupole moments throughout the entire periodic table. Its extension to the multi-reference…

Nuclear Theory · Physics 2017-01-30 W. Satula , P. Baczyk , J. Dobaczewski , M. Konieczka

An accurate description of electron correlation is one of the most challenging problems in quantum chemistry. The exact electron correlation can be obtained by means of full configuration interaction (FCI). A simple strategy for…

Chemical Physics · Physics 2021-05-14 Jae Woo Park

The recently developed semistochastic heat-bath configuration interaction (SHCI) method is a systematically improvable selected configuration interaction plus perturbation theory method capable of giving essentially exact energies for…

Chemical Physics · Physics 2020-10-01 Yuan Yao , Emmanuel Giner , Junhao Li , Julien Toulouse , C. J. Umrigar

Methods for correcting residual energy errors of configuration interaction (CI) calculations of molecules and other electronic systems are discussed based on the assumption that the energy defect can be mapped onto atomic regions. The…

Chemical Physics · Physics 2022-10-05 Jerry L. Whitten

Numerous numerical studies have shown that geminal-based methods are a promising direction to model strongly correlated systems with low computational costs. Several strategies have been introduced to capture the missing dynamical…

Chemical Physics · Physics 2023-03-22 Artur Nowak , Katharina Boguslawski

Traditional multiconfiguration Hartree-Fock (MCHF) and configuration interaction (CI) methods are based on a single orthonormal orbital basis (OB). For atoms with complicated shell structures, a large OB is needed to saturate all the…

Atomic Physics · Physics 2015-06-12 S. Verdebout , P. Rynkun , P. Jönsson , G. Gaigalas , C. Froese Fischer , M. Godefroid

Accurate computation of non-covalent, intermolecular interaction energies is important to understand various chemical phenomena, and quantum computers are anticipated to accelerate it. Although the state-of-the-art quantum computers are…

Quantum Physics · Physics 2025-12-29 Yuhei Tachi , Akihiko Arakawa , Taisei Osawa , Masayoshi Terabe , Kenji Sugisaki

We extend our recently-developed heat-bath configuration interaction (HCI) algorithm, and our semistochastic algorithm for performing multireference perturbation theory, to the calculation of excited-state wavefunctions and energies. We…

Strongly Correlated Electrons · Physics 2017-11-22 Adam A. Holmes , C. J. Umrigar , Sandeep Sharma

The accurate determination of the preferred ${\rm Si}_{12}{\rm C}_{12}$ isomer is important to guide experimental efforts directed towards synthesizing SiC nano-wires and related polymer structures which are anticipated to be highly…

We report no-core solutions for properties of light nuclei with three different approaches in order to assess the accuracy and convergence rates of each method. Full configuration interaction (FCI), Monte Carlo shell model (MCSM) and no…

Nuclear Theory · Physics 2012-11-09 T. Abe , P. Maris , T. Otsuka , N. Shimizu , Y. Utsuno , J. P. Vary

To follow up on the unexpectedly-good performance of several coupled-cluster models with approximate inclusion of 3-body clusters [J. Chem. Phys. 151, 064102 (2019)] we performed a more complete assessment of the 3CC method [J. Chem. Phys.…

Chemical Physics · Physics 2025-10-13 Nakul Teke , Ajay Melekamburath , Bimal Gaudel , Edward F. Valeev

We present a basis set correction scheme for the coupled-cluster singles and doubles (CCSD) method. The scheme is based on employing frozen natural orbitals (FNOs) and diagrammatically decomposed contributions to the electronic correlation…

Materials Science · Physics 2021-06-18 Andreas Irmler , Alejandro Gallo , Andreas Grüneis

This work explores the ability of classical electronic structure methods to efficiently represent (compress) the information content of full configuration interaction (FCI) wave functions. We introduce a benchmark set of four hydrogen model…

Chemical Physics · Physics 2020-08-20 Nicholas H. Stair , Francesco A. Evangelista

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 employ \textit{ab initio} methods of quantum chemistry to investigate spin-1/2 fermions interacting via a two-body contact potential in a one-dimensional harmonic trap. The convergence of the total energy with the size of the…

The combinatorial scaling of configuration interaction (CI) has long restricted its applicability to only the simplest molecular systems. Here, we report the first numerically exact CI calculation exceeding one quadrillion ($10^{15}$)…

Chemical Physics · Physics 2025-12-16 Agam Shayit , Can Liao , Shiv Upadhyay , Hang Hu , Tianyuan Zhang , Eugene DePrince , Chao Yang , Xiaosong Li

We apply the method of Monte Carlo configuration interaction (MCCI) to calculate ground-state potential energy curves for a range of small molecules and compare the results with full configuration interaction. We show that the MCCI…

Chemical Physics · Physics 2012-12-12 J. P. Coe , D. J. Taylor , M. J. Paterson

In common with many high-accuracy electronic structure methods, the initiator adaptation of full configuration interaction quantum Monte Carlo (i-FCIQMC) has difficulty treating realistic systems with large numbers of electrons. This…