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Related papers: Accurate full configuration interaction correlatio…

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We report on the findings of a blind challenge devoted to determining the frozen-core, full configuration interaction (FCI) ground state energy of the benzene molecule in a standard correlation-consistent basis set of double-$\zeta$…

Following the recent work of Eriksen et al. [arXiv:2008.02678], we report the performance of the \textit{Configuration Interaction using a Perturbative Selection made Iteratively} (CIPSI) method on the non-relativistic frozen-core…

Chemical Physics · Physics 2020-11-04 Pierre-François Loos , Yann Damour , Anthony Scemama

We present a perspective on what the future holds for full configuration interaction (FCI) theory, with an emphasis on conceptual rather than technical details. Upon revisiting the early history of FCI, a number of its key contemporary…

Chemical Physics · Physics 2020-12-29 Janus J. Eriksen

Recently, a new distributed implementation of the full configuration interaction (FCI) method has been reported [Gao et al. J. Chem Theory Comput. 2024, 20, 1185]. Thanks to a hybrid parallelization scheme, the authors were able to compute…

We employ correlation-consistent effective core potentials (ccECPs) to perform exact or nearly exact correlation and total energy calculations for the fifth-row elements (Rb-Xe). Total energies are calculated using various correlated…

Materials Science · Physics 2025-12-22 Aqsa Shaikh , Omar Madany , Benjamin Kincaid , Lubos Mitas

Local electronic-structure methods in quantum chemistry operate on the ability to compress electron correlations more efficiently in a basis of spatially localized molecular orbitals than in a parent set of canonical orbitals. However, many…

Chemical Physics · Physics 2024-08-01 Jonas Greiner , Jürgen Gauss , Janus J. Eriksen

Facilitated by a rigorous partitioning of a molecular system's orbital basis into two fundamental subspaces - a reference and an expansion space, both with orbitals of unspecified occupancy - we generalize our recently introduced many-body…

Chemical Physics · Physics 2019-12-12 Janus J. Eriksen , Jürgen Gauss

Very recently, we introduced a set of correlation consistent effective core potentials (ccECPs) constructed within full many-body approaches. By employing significantly more accurate correlated approaches we were able to reach a new level…

Materials Science · Physics 2020-02-25 Abdulgani Annaberdiyev , Cody A. Melton , M. Chandler Bennett , Guangming Wang , Lubos Mitas

We have performed a FCI-quality benchmark calculation for the tetramethyleneethane molecule in cc-pVTZ basis set employing a subset of CASPT2(6,6) natural orbitals for the FCIQMC calculation. The results are in an excellent agreement with…

Chemical Physics · Physics 2018-05-30 Libor Veis , Andrej Antalík , Örs Legeza , Ali Alavi , Jiří Pittner

Over the course of the past few decades, the field of computational chemistry has managed to manifest itself as a key complement to more traditional lab-oriented chemistry. This is particularly true in the wake of the recent renaissance of…

Chemical Physics · Physics 2018-10-16 Janus J. Eriksen , Jürgen Gauss

Full configuration interaction (FCI) solvers are limited to small basis sets due to their expensive computational costs. An optimal orbital selection for FCI (OptOrbFCI) is proposed to boost the power of existing FCI solvers to pursue the…

Chemical Physics · Physics 2020-09-01 Yingzhou Li , Jianfeng Lu

We present a stable and systematically improvable quantum Monte Carlo (QMC) approach to calculating excited-state energies, which we implement using our fast randomized iteration method for the full configuration interaction problem…

Computational Physics · Physics 2023-10-03 Samuel M. Greene , Robert J. Webber , James E. T. Smith , Jonathan Weare , Timothy C. Berkelbach

We report ground- and excited-state dipole moments and oscillator strengths (computed in different ``gauges'' or representations) of full configuration interaction (FCI) quality using the selected configuration interaction method known as…

The semistochastic heat-bath configuration interaction (SHCI) method is a selected configuration interaction plus perturbation theory method that has provided near-full configuration interaction (FCI) levels of accuracy for many systems…

Chemical Physics · Physics 2021-11-30 Yuan Yao , Emmanuel Giner , Tyler A. Anderson , Julien Toulouse , C. J. Umrigar

Striving to define very accurate vertical transition energies, we perform both high-level coupled cluster (CC) calculations (up to CCSDTQP) and selected configuration interaction (sCI) calculations (up to several millions of determinants)…

Approximate full configuration interaction (FCI) calculations have recently become tractable for systems of unforeseen size thanks to stochastic and adaptive approximations to the exponentially scaling FCI problem. The result of an FCI…

Strongly Correlated Electrons · Physics 2017-10-25 Susi Lehtola , Norm M. Tubman , K. Birgitta Whaley , Martin Head-Gordon

We propose an efficient deterministic method to calculate the full configuration interaction (FCI) ground state energy. This method leverages the sparseness of the Lanczos basis vectors that span the Krylov subspace associated with the…

Chemical Physics · Physics 2024-01-08 Lijun Wang

In the present letter, it is demonstrated how full configuration interaction (FCI) results in extended basis sets may be obtained to within sub-kJ/mol accuracy by decomposing the energy in terms of many-body expansions in the virtual…

Chemical Physics · Physics 2017-09-15 Janus J. Eriksen , Filippo Lipparini , Jürgen Gauss

By performing a stochastic dynamic in a space of Slater determinants, the Full Configuration Interaction Quantum Monte Carlo (FCIQMC) method has been able to obtain energies which are essentially free from systematic error to the basis set…

Computational Physics · Physics 2014-10-10 George H. Booth , Deidre Cleland , Ali Alavi , David P. Tew

The benzene...ethene and parallel-displaced (PD) benzene...benzene dimers are the most fundamental systems involving p-p stacking interactions. Several high-level ab initio investigations calculated the binding energies of these dimers at…

Chemical Physics · Physics 2021-03-29 Amir Karton , Jan M. L. Martin
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