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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 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

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

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…

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

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

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

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 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

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 three modifications to our recently introduced fast randomized iteration method for full configuration interaction (FCI-FRI) and investigate their effects on the method's performance for Ne, H$_2$O, and N$_2$. The initiator…

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

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…

In this study, we utilize the many-body expansion (MBE) framework to decompose electronic structures into fragments by incrementing the virtual orbitals. Our work aims to accurately solve the ground and excited state energies of each…

Chemical Physics · Physics 2023-10-09 Enhua Xu , Yuma Shimomoto , Seiichiro L. Ten-no , Takashi Tsuchimochi

Graph-based machine learning models for materials properties show great potential to accelerate virtual high-throughput screening of large chemical spaces. However, in their simplest forms, graph-based models do not include any 3D…

Chemical Physics · Physics 2024-10-15 Ralf Meyer , Daniel Benjamin Kasman Chu , Heather J. Kulik

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

One of the key challenges of quantum-chemical multi-configuration methods is the necessity to manually select orbitals for the active space. This selection requires both expertise and experience and can therefore impose severe limitations…

Chemical Physics · Physics 2016-04-25 Christopher J. Stein , Markus Reiher

Full Configuration Interaction Quantum Monte Carlo (FCIQMC) has been effectively applied to very large configuration interaction (CI) problems, and was recently adapted for use as an active space solver and combined with orbital…

Chemical Physics · Physics 2020-02-19 Robert J. Anderson , Toru Shiozaki , George H. Booth

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

In this paper, we propose a general analysis framework for inexact power iteration, which can be used to efficiently solve high dimensional eigenvalue problems arising from quantum many-body problems. Under the proposed framework, we…

Numerical Analysis · Mathematics 2018-06-29 Jianfeng Lu , Zhe Wang

Accurate many-body treatments of condensed-phase systems are challenging because correlated solvers such as full configuration interaction (FCI) and the density matrix renormalization group (DMRG) scale exponentially with system size.…

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