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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

The recent many-body expanded full configuration interaction (MBE-FCI) method is reviewed by critically assessing its advantages and drawbacks in the context of contemporary near-exact electronic structure theory. Besides providing a…

Chemical Physics · Physics 2021-03-02 Janus J. Eriksen , Jürgen Gauss

We present a wide-reaching revamp of the generalized many-body expanded full configuration interaction (MBE-FCI) method. First, we outline how to automatize the selection of reference active spaces whereby the inherent bias introduced…

Chemical Physics · Physics 2024-06-18 Jonas Greiner , Jürgen Gauss , Janus J. Eriksen

In this second part of our series on the recently proposed many-body expanded full configuration interaction (MBE-FCI) method, we introduce the concept of multideterminantal expansion references. Through theoretical arguments and numerical…

Chemical Physics · Physics 2019-09-23 Janus J. Eriksen , Jürgen Gauss

The recently proposed many-body expanded full configuration interaction (MBE-FCI) method is extended to excited states and static first-order properties different from total, ground state correlation energies. Results are presented for…

Chemical Physics · Physics 2020-10-20 Janus J. Eriksen , Jürgen Gauss

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

The many-body expansion (MBE) is an efficient tool which has a long history of use for calculating interaction energies, binding energies, lattice energies, and so on. In the past, applications of MBE to correlation energy have been…

Strongly Correlated Electrons · Physics 2021-08-11 Vibin Abraham , Nicholas Mayhall

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

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

We present a novel implementation of the complete active space self-consistent field (CASSCF) method that makes use of the many-body expanded full configuration interaction (MBE-FCI) method to incrementally approximate electronic structures…

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

The Many-Body Expansion (MBE) is a useful tool to simulate condensed phase chemical systems, often avoiding the steep computational cost of usual electronic structure methods. However, it often requires higher than 2-body terms to achieve…

Chemical Physics · Physics 2019-11-21 Srimukh Prasad Veccham , Joonho Lee , Martin Head-Gordon

Fragmentation methods such as the many-body expansion (MBE) are a common strategy to model large systems by partitioning energies into a hierarchy of decreasingly significant contributions. The number of fragments required for chemical…

Chemical Physics · Physics 2017-09-13 Kun Yao , John E. Herr , John Parkhill

We propose a lattice density-functional theory for {\it ab initio} quantum chemistry or physics as a route to an efficient approach that approximates the full configuration interaction energy and orbital occupations for molecules with…

Strongly Correlated Electrons · Physics 2019-04-19 J. P. Coe

Many-body interactions (MBIs) such as exciton-exciton interactions significantly affect the optical response of semiconductor nanostructures. These interactions can be rigorously modeled through microscopic calculations. However, these…

Mesoscale and Nanoscale Physics · Physics 2025-09-03 Pradeep Kumar , Bhaskar De , Rishabh Tripathi , Rohan Singh

Incremental full configuration interaction (iFCI) closely approximates the FCI limit with polynomial cost through a many-body expansion of the correlation energy, providing highly accurate total energies within a given basis set. To extend…

Chemical Physics · Physics 2025-02-26 Jeffrey Hatch , Paul M. Zimmerman

Following our recent work on the benzene molecule [\href{https://doi.org/10.1063/5.0027617}{J.~Chem.~Phys.~\textbf{153}, 176101 (2020)}], itself motivated by the blind challenge of Eriksen \textit{et al.}…

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 extend the scope of full configuration interaction quantum Monte Carlo (FCIQMC) to be applied to coupled fermion-boson hamiltonians, alleviating the a priori truncation in boson occupation which is necessary for many other wave function…

Strongly Correlated Electrons · Physics 2022-11-09 Robert J. Anderson , Charles C. J. Scott , George H. Booth

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…

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