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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

We investigate the inclusion of variable spins in electronic structure quantum Monte Carlo, with a focus on diffusion Monte Carlo with Hamiltonians that include spin-orbit interactions. Following our previous introduction of fixed-phase…

Computational Physics · Physics 2016-07-27 Cody A. Melton , M. Chandler Bennett , Lubos Mitas

We present ground and excited state energies obtained from Diffusion Monte Carlo (DMC) calculations, using accurate multiconfiguration wave functions, for $N$ electrons ($N\le13$) confined to a circular quantum dot. We analyze the…

Condensed Matter · Physics 2009-10-31 F. Pederiva , C. J. Umrigar , E. Lipparini

Quantum Monte Carlo methods are accurate and promising many body techniques for electronic structure calculations which, in the last years, are encountering a growing interest thanks to their favorable scaling with the system size and their…

Chemical Physics · Physics 2014-02-17 Andrea Zen , Ye Luo , Sandro Sorella , Leonardo Guidoni

We present a quantum Monte Carlo study of the hydrogen-benzene system where binding is very weak. We demonstrate that the binding is well described at both variational Monte Carlo (VMC) and diffusion Monte Carlo (DMC) levels by a Jastrow…

Materials Science · Physics 2009-11-13 Todd D. Beaudet , Michele Casula , Jeongnim Kim , Sandro Sorella , Richard M. Martin

The self-healing diffusion Monte Carlo algorithm (SHDMC) [Reboredo, Hood and Kent, Phys. Rev. B {\bf 79}, 195117 (2009); Reboredo, {\it ibid.} {\bf 80}, 125110 (2009)] is extended to study the ground and excited states of magnetic and…

Strongly Correlated Electrons · Physics 2011-06-10 Fernando Agustín Reboredo

We extend the recently introduced phaseless auxiliary-field quantum Monte Carlo (QMC) approach to any single-particle basis, and apply it to molecular systems with Gaussian basis sets. QMC methods in general scale favorably with system…

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

A quantum Monte Carlo study of the atomization energies for the G2 set of molecules is presented. Basis size dependence of diffusion Monte Carlo atomization energies is studied with a single determinant Slater-Jastrow trial wavefunction…

Chemical Physics · Physics 2015-06-04 F. R. Petruzielo , Julien Toulouse , C. J. Umrigar

Quantum Monte Carlo approaches such as the diffusion Monte Carlo (DMC) method are among the most accurate many-body methods for extended systems. Their scaling makes them well suited for defect calculations in solids. We review the various…

Materials Science · Physics 2014-04-23 William D. Parker , John W. Wilkins , Richard G. Hennig

One bottleneck of quantum Monte Carlo (QMC) simulation of strongly correlated electron systems lies at the scaling relation of computational complexity with respect to the system sizes. For generic lattice models of interacting fermions,…

Strongly Correlated Electrons · Physics 2019-02-20 Zi Hong Liu , Xiao Yan Xu , Yang Qi , Kai Sun , Zi Yang Meng

While Diffusion Monte Carlo (DMC) is in principle an exact stochastic method for \textit{ab initio} electronic structure calculations, in practice the fermionic sign problem necessitates the use of the fixed-node approximation and trial…

Reliable theoretical predictions of noncovalent interaction energies, which are important e.g. in drug-design and hydrogen-storage applications, belong to longstanding challenges of contemporary quantum chemistry. In this respect, the…

Chemical Physics · Physics 2016-06-06 Matúš Dubecký , René Derian , Petr Jurečka , Lubos Mitas , Pavel Hobza , Michal Otyepka

The small magnitude and long-range character of non-covalent interactions pose a significant challenge for computational quantum chemical and electronic-structure methods alike. State-of-the-art coupled cluster (CC) theory and…

Chemical Physics · Physics 2026-01-22 S. Lambie , P. López-Ríos , D. Kats , Ali Alavi

Fixed node diffusion Monte Carlo (DMC) has been performed on a test set of forward and reverse barrier heights for 19 non-hydrogen-transfer reactions, and the nodal error has been assessed. The DMC results are robust to changes in the nodal…

Chemical Physics · Physics 2017-04-26 Kittithat Krongchon , Brian Busemeyer , Lucas K. Wagner

We present a variational Monte Carlo algorithm for estimating the lowest excited states of a quantum system which is a natural generalization of the estimation of ground states. The method has no free parameters and requires no explicit…

Computational Physics · Physics 2024-09-04 David Pfau , Simon Axelrod , Halvard Sutterud , Ingrid von Glehn , James S. Spencer

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

Quantum computers have a potential for solving quantum chemistry problems with higher accuracy than classical computers. Quantum computing quantum Monte Carlo (QC-QMC) is a QMC with a trial state prepared in quantum circuit, which is…

Quantum Physics · Physics 2024-06-07 Shu Kanno , Hajime Nakamura , Takao Kobayashi , Shigeki Gocho , Miho Hatanaka , Naoki Yamamoto , Qi Gao

Very recently, we introduced a set of correlation consistent effective core potentials (ccECPs) constructed within full many-body approaches. By employing significantly more accurate correlated approaches we were able to reach a new level…

Materials Science · Physics 2020-02-25 Abdulgani Annaberdiyev , Cody A. Melton , M. Chandler Bennett , Guangming Wang , Lubos Mitas

Quantum Monte Carlo (QMC) methods can very accurately compute ground state properties of quantum systems. We applied these methods to a system of boson hard spheres to get exact, infinite system size results for the ground state at several…

Computational Physics · Physics 2016-09-08 Mark Dewing

Accurately predicting the formation energy of a compound, which describes its thermodynamic stability, is a key challenge in materials physics. Here, we employ many-body quantum Monte Carlo (QMC) with single-reference trial functions to…