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Phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC) has emerged as a promising electronic structure method for correlated electronic systems. However, the quality of its predictions depends critically on the choice of trial…

Chemical Physics · Physics 2026-05-06 Don Danilov , Brad Ganoe , Leon Otis , Zhi Gong , Zixiang Lu , James Shee

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

Neutral molecules with sufficiently large dipole moments can bind electrons in diffuse nonvalence orbitals with most of their charge density far from the nuclei, forming so-called dipole-bound anions. Because long-range correlation effects…

Chemical Physics · Physics 2018-10-30 Hongxia Hao , James Shee , Shiv Upadhyay , Can Ataca , Kenneth D. Jordan , Brenda M. Rubenstein

Fixed-node diffusion Monte Carlo (DMC) is a stochastic algorithm for finding the lowest energy many-fermion wave function with the same nodal surface as a chosen trial function. It has proved itself among the most accurate methods available…

Condensed Matter · Physics 2009-10-31 W. M. C. Foulkes , Randolph Q. Hood , R. J. Needs

We analyze the effect of increasing charge density on the Fixed Node Errors in Diffusion Monte Carlo by comparing FN-DMC calculations of the total ground state energy on a 4 electron system done with a Hartree-Fock based trial wave function…

Chemical Physics · Physics 2013-07-23 Kevin Rasch , Lubos Mitas

Diffusion Monte Carlo (DMC) based on fixed-node approximation has enjoyed significant developments in the past decades and become one of the go-to methods when accurate ground state energy of molecules and materials is needed. The remaining…

Chemical Physics · Physics 2023-08-07 Weiluo Ren , Weizhong Fu , Xiaojie Wu , Ji Chen

In this work density functional theory (DFT) and diffusion Monte Carlo (DMC) methods are used to calculate the binding energy of a H atom chemisorbed on the graphene surface. The Perdew-Burke-Ernzerhof (PBE) value of the binding energy is…

We investigate the binding of single and quadruple hydrogen molecules on a positively charged Ca ion. By comparing with benchmark quantum Monte Carlo (QMC) calculations we demonstrate wide variability in other more approximate electronic…

Materials Science · Physics 2010-08-12 Michal Bajdich , Fernando A. Reboredo , P. R. C. Kent

The impact of residual electron correlation beyond the equation-of-motion coupled-cluster singles and doubles approximation (EOM-CCSD) on positions and widths of electronic resonances is investigated. To establish a method that accomplishes…

Chemical Physics · Physics 2018-02-14 Thomas-C. Jagau

We assess the utility of Hartree-Fock (HF) trial wavefunctions in performing phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC) on the uniform electron gas (UEG) model. The combination of ph-AFQMC with spin-restricted HF…

Chemical Physics · Physics 2019-08-20 Joonho Lee , Fionn D. Malone , Miguel A. Morales

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

We report variational and diffusion quantum Monte Carlo (VMC and DMC) studies of the binding curve of the ground-state chromium dimer. We employed various single determinant (SD) or multi-determinant (MD) wavefunctions multiplied by a…

Chemical Physics · Physics 2012-04-06 Kenta Hongo , Ryo Maezono

The diffusion Monte Carlo technique is used to calculate and analyze the excitation spectrum of a single 3He atom bound to a cluster with N 4He atoms, with the aim of establishing the most adequate filling ordering of single-fermion orbits…

Soft Condensed Matter · Physics 2009-11-10 S. Fantoni , R. Guardiola , J. Navarro

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 many-body diffusion quantum Monte Carlo (DMC) method with twist-averaged boundary conditions is used to calculate the ground-state equation of state and the energetics of point defects in fcc aluminum using supercells up to 1331 atoms.…

Materials Science · Physics 2012-10-22 Randolph Q. Hood , P. R. C. Kent , Fernando A. Reboredo

To make useful connections with experimental measurements, correlated electronic structure theories must accurately predict chemical properties in addition to energies. We present a finite-difference based algorithm to compute first-order…

Chemical Physics · Physics 2025-09-24 Leon Otis , Sri Gudivada , Marvin Friede , James Shee

We present density-functional theory (DFT) and quantum Monte Carlo (QMC) calculations designed to resolve experimental and theoretical controversies over the optical properties of H-terminated C nanoparticles (diamondoids). The QMC results…

Materials Science · Physics 2008-01-03 N. D. Drummond , A. J. Williamson , R. J. Needs , G. Galli

The diffusion Monte Carlo technique is used to calculate and analyze the excitation spectrum of $^3$He atoms bound to a cluster of $^4$He atoms, by using a previously determined optimum filling of single-fermion orbits with well defined…

Atomic and Molecular Clusters · Physics 2009-11-11 S. Fantoni , R. Guardiola , J. Navarro , A. Zuker

We report all-electron and pseudopotential calculations of the ground-stateenergies of the neutral Ne atom and the Ne+ ion using the variational and diffusion quantum Monte Carlo (DMC) methods. We investigate different levels of…

Materials Science · Physics 2008-01-03 N. D. Drummond , P. Lopez Rios , A. Ma , J. R. Trail , G. Spink , M. D. Towler , R. J. Needs

In this work we develop tools that enable the study of non-adiabatic effects with variational and diffusion Monte Carlo methods. We introduce a highly accurate wave function ansatz for electron-ion systems that can involve a combination of…

Chemical Physics · Physics 2014-10-29 Norm M. Tubman , Ilkka Kylänpää , Sharon Hammes-Schiffer , David M. Ceperley
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