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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 present a new approach to calculate excited states with the full configuration interaction quantum Monte Carlo (FCIQMC) method. The approach uses a Gram-Schmidt procedure, instantaneously applied to the stochastically evolving…

Computational Physics · Physics 2015-10-28 N. S. Blunt , Simon D. Smart , George H. Booth , Ali Alavi

We propose the use of preconditioning in FCIQMC which, in combination with perturbative estimators, greatly increases the efficiency of the algorithm. The use of preconditioning allows a time step close to unity to be used (without…

Chemical Physics · Physics 2019-05-17 Nick S. Blunt , Alex J. W. Thom , Charles J. C. Scott

We have implemented recently developed multiple-projector pseudopotentials into the planewave based auxiliary-field quantum Monte Carlo (pw-AFQMC) method. Multiple-projector pseudopotentials can yield smaller planewave cut-offs while…

Materials Science · Physics 2017-04-06 Fengjie Ma , Shiwei Zhang , Henry Krakauer

Accurate determination of electronic properties of correlated oxides remains a significant challenge for computational theory. Traditional Hubbard-corrected density functional theory (DFT+U) frequently encounters limitations in precisely…

Materials Science · Physics 2024-03-19 Hyeondeok Shin , Kevin Gasperich , Tomas Rojas , Anh T. Ngo , Jaron T. Krogel , Anouar Benali

We propose a novel algorithm for calculating the ground-state energy of quantum many-body systems by combining auxiliary-field quantum Monte Carlo (AFQMC) with tensor-train sketching. In AFQMC, a good trial wavefunction to guide the random…

Numerical Analysis · Mathematics 2026-02-17 Ziang Yu , Shiwei Zhang , Yuehaw Khoo

The auxiliary-field quantum Monte Carlo (AFQMC) method is a general numerical method for correlated many-electron systems, which is being increasingly applied in lattice models, atoms, molecules, and solids. Here we introduce the theory and…

Computational Physics · Physics 2021-02-24 Hao Shi , Shiwei Zhang

The potential energy curve of the F$_2$ molecule is calculated with Fixed-Node Diffusion Monte Carlo (FN-DMC) using Configuration Interaction (CI)-type trial wavefunctions. To keep the number of determinants reasonable (the first and second…

Chemical Physics · Physics 2016-07-25 Emmanuel Giner , Anthony Scemama , Michel Caffarel

Auxiliary Field Quantum Monte Carlo (AFQMC) has emerged as a powerful framework for treating strongly correlated electronic systems, offering a favorable balance between computational cost and accuracy. In this paper, we present a novel…

Chemical Physics · Physics 2026-04-03 Maxine Luo , Victor Chen , Yu Wang , Christian B. Mendl

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 high-accuracy correlated calculations of small Si$_x$H$_y$ molecular systems both in the ground and excited states. We employ quantum Monte Carlo (QMC) together with a variety of many-body wave function approaches based on basis…

Chemical Physics · Physics 2020-10-21 Guangming Wang , Abdulgani Annaberdiyev , Lubos Mitas

We consider gradient descent and quasi-Newton algorithms to optimize the full configuration interaction (FCI) ground state wavefunction starting from an arbitrary reference state $|0 \rangle$. We show that the energies obtained along the…

Chemical Physics · Physics 2021-02-03 Carlos A. Jiménez-Hoyos

Quantum Monte Carlo (QMC) is a stochastic method which has been particularly successful for ground-state electronic structure calculations but mostly unexplored for the computation of excited-state energies. Here, we show that, within a…

Chemical Physics · Physics 2018-08-09 Anthony Scemama , Anouar Benali , Denis Jacquemin , Michel Caffarel , Pierre-François Loos

We investigate the accuracy of trial wave function for quantum Monte Carlo based on pfaffian functional form with singlet and triplet pairing. Using a set of first row atoms and molecules we find that these wave functions provide very…

Other Condensed Matter · Physics 2009-02-20 M. Bajdich , L. Mitas , G. Drobný , L. K. Wagner , K. E. Schmidt

The concept of machine learning configuration interaction (MLCI) [J. Chem. Theory Comput. 2018, 14, 5739], where an artificial neural network (ANN) learns on the fly to select important configurations, is further developed so that accurate…

Chemical Physics · Physics 2019-10-31 J. P. Coe

Quantum-selected configuration interaction (QSCI) utilizes an input quantum state on a quantum device to select important bases (electron configurations in quantum chemistry) that define a subspace in which to diagonalize a target…

Quantum Physics · Physics 2025-10-22 Mathias Mikkelsen , Yuya O. Nakagawa

Development of exponentially scaling methods has seen great progress in tackling larger systems than previously thought possible. One such technique, full configuration interaction quantum Monte Carlo, is a useful algorithm that allows…

Strongly Correlated Electrons · Physics 2016-08-23 Norm M. Tubman , Joonho Lee , Tyler Y. Takeshita , Martin Head-Gordon , K. Birgitta Whaley

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

The auxiliary-field quantum Monte Carlo (AFMC) method is a powerful and widely used technique for ground-state and finite-temperature simulations of quantum many-body systems. We introduce several algorithmic improvements for…

Computational Physics · Physics 2021-03-18 C. N. Gilbreth , S. Jensen , Y. Alhassid

The pressure-induced structural phase transition from diamond to beta-tin in silicon is an excellent test for theoretical total energy methods. The transition pressure provides a sensitive measure of small relative energy changes between…

Materials Science · Physics 2009-12-24 Wirawan Purwanto , Henry Krakauer , Shiwei Zhang
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