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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 a new selected configuration interaction plus perturbation theory algorithm that is based on a deterministic analog of our recent efficient heat-bath sampling algorithm. This Heat-bath Configuration Interaction (HCI) algorithm…

Chemical Physics · Physics 2016-08-22 Adam Holmes , Norm Tubman , Cyrus Umrigar

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

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

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

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

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 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

A recent direction in quantum computing for molecular electronic structure sees the use of quantum devices as configuration sampling machines integrated within high-performance computing (HPC) platforms. This appeals to the strengths of…

Quantum Physics · Physics 2026-05-18 Tim Weaving , Angus Mingare , Alexis Ralli , Peter V. Coveney

We study several approaches to orbital optimization in selected configuration interaction plus perturbation theory (SCI+PT) methods, and test them on the ground and excited states of three molecules using the semistochastic heatbath…

Chemical Physics · Physics 2021-07-14 Yuan Yao , C. J. Umrigar

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

The computationally expensive evaluation and storage of high-rank reduced density matrices (RDMs) has been the bottleneck in the calculation of dynamic correlation for multireference wave functions in large active spaces. We present a…

Chemical Physics · Physics 2020-01-08 Ankit Mahajan , Nick S. Blunt , Iliya Sabzevari , Sandeep Sharma

The design and performance of future fusion power plants will depend on accurate atomic data for plasma-facing material and plasma impurity species. A leading candidate for the plasma-facing material is tungsten due to its high melting…

Atomic Physics · Physics 2025-11-20 Zachary T. Jerzyk , David R. Smith , Matthew Otten

Many-body simulations of quantum systems is an active field of research that involves many different methods targeting various computing platforms. Many methods commonly employed, particularly coupled cluster methods, have been adapted to…

Chemical Physics · Physics 2023-06-14 David B. Williams-Young , Norm M. Tubman , Carlos Mejuto-Zaera , Wibe A. de Jong

Quantum-selected configuration interaction (QSCI) is a novel quantum-classical hybrid algorithm for quantum chemistry calculations. This method identifies electron configurations having large weights for the target state using quantum…

Chemical Physics · Physics 2025-03-31 Soichi Shirai , Shih-Yen Tseng , Hokuto Iwakiri , Takahiro Horiba , Hirotoshi Hirai , Sho Koh

Inspired by our earlier semi-stochastic work aimed at converging high-level coupled-cluster (CC) energetics [J. E. Deustua, J. Shen, and P. Piecuch, Phys. Rev. Lett. 119, 223003 (2017); J. Chem. Phys. 154, 124103 (2021)], we propose a novel…

Chemical Physics · Physics 2022-10-06 Karthik Gururangan , J. Emiliano Deustua , Jun Shen , Piotr Piecuch

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

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

We present NECI, a state-of-the-art implementation of the Full Configuration Interaction Quantum Monte Carlo algorithm, a method based on a stochastic application of the Hamiltonian matrix on a sparse sampling of the wave function. The…

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