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This paper presents in detail our fast semistochastic heat-bath configuration interaction (SHCI) method for solving the many-body Schrodinger equation. We identify and eliminate computational bottlenecks in both the variational and…

Chemical Physics · Physics 2019-01-14 Junhao Li , Matt Otten , Adam A Holmes , Sandeep Sharma , Cyrus J. Umrigar

We extend the recently proposed heat-bath configuration interaction (HCI) method [Holmes, Tubman, Umrigar, J. Chem. Theory Comput. 12, 3674 (2016)], by introducing a semistochastic algorithm for performing multireference Epstein-Nesbet…

Chemical Physics · Physics 2017-03-20 Sandeep Sharma , Adam Holmes , Guillaume Jeanmairet , Ali Alavi , C. J. Umrigar

Vibrational heat-bath configuration interaction (VHCI) -- a selected configuration interaction technique for vibrational structure theory -- has recently been developed in two independent works [J. Chem. Phys. 154, 074104 (2021); Mol. Phys.…

Chemical Physics · Physics 2023-07-26 Henry K. Tran , Timothy C. Berkelbach

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

We introduce vibrational heat-bath configuration interaction (VHCI) as an accurate and efficient method for calculating vibrational eigenstates of anharmonic systems. Inspired by its origin in electronic structure theory, VHCI is a selected…

Chemical Physics · Physics 2021-03-17 Jonathan H. Fetherolf , Timothy C. Berkelbach

In this study, we extend the multicomponent heat-bath configuration interaction (HCI) method to excited states. Previous multicomponent HCI studies have been performed using only the variational stage of the HCI algorithm as they have…

Chemical Physics · Physics 2022-01-12 Naresh Alaal , Kurt R. Brorsen

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

Recent advances in selected CI, including the adaptive sampling configuration interaction (ASCI) algorithm and its heat bath extension, have made the ASCI approach competitive with the most accurate techniques available, and hence an…

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

In this work we demonstrate that the heat bath configuration interaction (HCI) and its semistochastic extension can be used to treat relativistic effects and electron correlation on an equal footing in large active spaces to calculate the…

Chemical Physics · Physics 2018-11-08 Bastien Mussard , Sandeep Sharma

We develop an efficient algorithm, coordinate descent FCI (CDFCI), for the electronic structure ground state calculation in the configuration interaction framework. CDFCI solves an unconstrained non-convex optimization problem, which is a…

Chemical Physics · Physics 2019-07-03 Zhe Wang , Yingzhou Li , Jianfeng Lu

Selected configuration interaction (sCI) methods including second-order perturbative corrections provide near full CI (FCI) quality energies with only a small fraction of the determinants of the FCI space. Here, we introduce both a…

Chemical Physics · Physics 2018-08-09 Yann Garniron , Anthony Scemama , Emmanuel Giner , Michel Caffarel , Pierre-François Loos

We use the recently-developed Heat-bath Configuration Interaction (HCI) algorithm as an efficient active-space solver to perform multi-configuration self-consistent field calculations (HCISCF) with large active spaces. We give a detailed…

Chemical Physics · Physics 2018-11-08 James E. T. Smith , Adam A. Holmes , Bastien Mussard , Sandeep Sharma

Even when starting with a very poor initial guess, the iterative configuration interaction (iCI) approach can converge from above to full CI very quickly by constructing and diagonalizing a small Hamiltonian matrix at each…

Chemical Physics · Physics 2020-01-07 Ning Zhang , Wenjian Liu , Mark R. Hoffmann

We present the concept, derivation, and implementation of dynamical configuration interaction, a quantum embedding theory that combines Green's function methodology with the many-body wave function. In a strongly-correlated active space, we…

Chemical Physics · Physics 2019-04-03 Marc Dvorak , Patrick Rinke

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 propose the concept of machine learning configuration interaction (MLCI) whereby an artificial neural network is trained on-the-fly to predict important new configurations in an iterative selected configuration interaction procedure. We…

Chemical Physics · Physics 2018-10-18 J. P. Coe

In this work we present the extension of semistochastic heat-bath configuration interaction (SHCI) to work with any two-component and four-component Hamiltonian. Vertical detachment energy (VDE) of AuH_2^- and zero-field splitting (ZFS) of…

Chemical Physics · Physics 2023-01-18 Xubo Wang , Sandeep Sharma

We introduce a new procedure for iterative selection of determinant spaces capable of describing highly correlated systems. This adaptive configuration interaction (ACI) determines an optimal basis by an iterative procedure in which the…

Chemical Physics · Physics 2016-05-25 Jeffrey B. Schriber , Francesco A. Evangelista

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
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