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We present phaseless auxiliary-field (AF) quantum Monte Carlo (QMC) calculations of the ground states of some hydrogen-bonded systems. These systems were selected to test and benchmark different aspects of the new phaseless AF QMC method.…

Computational Physics · Physics 2007-05-23 W. A. Al-Saidi , Henry Krakauer , Shiwei Zhang

The energy gap between the lowest-lying singlet and triplet states is an important quantity in chemical photocatalysis, with relevant applications ranging from triplet fusion in optical upconversion to the design of organic light-emitting…

Chemical Physics · Physics 2019-08-29 James Shee , Evan J. Arthur , Shiwei Zhang , David R. Reichman , Richard A. Friesner

We develop a local correlation variant of auxiliary field quantum Monte Carlo (AFQMC) that is based on local natural orbitals (LNO-AFQMC). In LNO-AFQMC, independent AFQMC calculations are performed for each localized occupied orbital using…

Chemical Physics · Physics 2023-08-25 Jo S. Kurian , Hong-Zhou Ye , Ankit Mahajan , Timothy C. Berkelbach , Sandeep Sharma

Selected configuration interaction (SCI) methods, when complemented with a second-order perturbative correction, provide near full configuration interaction (FCI) quality energies with only a small fraction of the Slater determinants of the…

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

Modern quantum Monte Carlo (QMC) methods often capture electron correlation through both explicitly correlating Jastrow factors and small to mid-sized configuration interaction (CI) expansions. Here, we study the additional optimization…

Chemical Physics · Physics 2023-02-08 Scott M. Garner , Eric Neuscamman

We apply the method of Monte Carlo configuration interaction (MCCI) to calculate ground-state potential energy curves for a range of small molecules and compare the results with full configuration interaction. We show that the MCCI…

Chemical Physics · Physics 2012-12-12 J. P. Coe , D. J. Taylor , M. J. Paterson

The so-called phaseless quantum Monte-Carlo method currently offers one of the best performing theoretical framework to investigate interacting Fermi systems. It allows to extract an approximate ground-state wavefunction by averaging…

Strongly Correlated Electrons · Physics 2017-03-31 Olivier Juillet , Alexandre Leprévost , Jérémy Bonnard , Raymond Frésard

We investigate the sign problem for full configuration interaction quantum Monte Carlo (FCIQMC), a stochastic algorithm for finding the ground state solution of the Schr\"odinger equation with substantially reduced computational cost…

Computational Physics · Physics 2014-11-05 James J. Shepherd , Gustavo E. Scuseria , James S. Spencer

We explore the use of the stochastic resolution-of-the-identity (sRI) with the phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC) method. sRI is combined with four existing local energy evaluation strategies in ph-AFQMC, namely (1)…

Chemical Physics · Physics 2020-07-31 Joonho Lee , David R. Reichman

We investigate the use of variational wave-functions that mimic stochastic recurrent neural networks, specifically, unrestricted Boltzmann machines, as guiding functions in projective quantum Monte Carlo (PQMC) simulations of quantum spin…

Statistical Mechanics · Physics 2018-12-27 E. M. Inack , G. E. Santoro , L. Dell'Anna , S. Pilati

Estimating the ground-state energy of a quantum system is one of the most promising applications for quantum algorithms. Here we propose a variational quantum eigensolver (VQE) \emph{Ansatz} for finding ground state configuration…

Quantum Physics · Physics 2026-02-10 Koray Aydoğan , Anna R. Spak , Kade Head-Marsden , Anthony W. Schlimgen

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 develop a formalism and present an algorithm for optimization of the trial wave-function used in fixed-node diffusion quantum Monte Carlo (DMC) methods. We take advantage of a basic property of the walker configuration distribution…

Strongly Correlated Electrons · Physics 2015-05-13 Fernando A. Reboredo , Randolph Q. Hood , Paul R. C. Kent

We present a plane-wave (PW) implementation of the auxiliary-field quantum Monte Carlo (AFQMC) method within the projector augmented-wave (PAW) formalism in the Vienna ab initio Simulation Package (VASP). By employing an exact inversion of…

Computational Physics · Physics 2026-02-17 Moritz Humer , Martin Schlipf , Zoran Sukurma , Sajad Bazrafshan , Georg Kresse

In this work, we test a recently developed method to enhance classical auxiliary-field quantum Monte Carlo (AFQMC) calculations with quantum computers against examples from chemistry and material science, representatives of classes of…

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 propose a new scheme to implement the self-consistent optimization of the trial wave-function in constrained path auxiliary field Quantum Monte Carlo (CP-AFQMC) in the framewok of natural orbitals. In this scheme, a new trial…

Strongly Correlated Electrons · Physics 2023-08-15 Mingpu Qin

Ab initio auxiliary-field quantum Monte Carlo (AFQMC) is a systematically improvable many-body method, but its application to extended solids has been severely limited by unfavorable computational scaling and memory requirements that…

Strongly Correlated Electrons · Physics 2026-02-25 Jinghong Zhang , Meng-Fu Chen , Adam Rettig , Tong Jiang , Paul J. Robinson , Hieu Q. Dinh , Anton Z. Ni , Joonho Lee

We demonstrate a scaling method for non-Markovian Monte Carlo wave-function simulations used to study open quantum systems weakly coupled to their environments. We derive a scaling equation, from which the result for the expectation values…

Quantum Physics · Physics 2009-11-10 J. Piilo , S. Maniscalco , A. Messina , F. Petruccione