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We provide a pedagogical introduction to the two main variants of real-space quantum Monte Carlo methods for electronic-structure calculations: variational Monte Carlo (VMC) and diffusion Monte Carlo (DMC). Assuming no prior knowledge on…

Chemical Physics · Physics 2015-08-13 Julien Toulouse , Roland Assaraf , C. J. Umrigar

We propose a Monte Carlo sampler from the reverse diffusion process. Unlike the practice of diffusion models, where the intermediary updates -- the score functions -- are learned with a neural network, we transform the score matching…

Machine Learning · Statistics 2024-03-14 Xunpeng Huang , Hanze Dong , Yifan Hao , Yi-An Ma , Tong Zhang

The Kinetic Monte Carlo (KMC) method has become an important tool for examination of phenomena like surface diffusion and thin film growth because of its ability to carry out simulations for time scales that are relevant to experiments. But…

Materials Science · Physics 2007-05-23 Talat S. Rahman , Abdelkader Kara , Altaf Karim , Oleg Trushin

The disiloxane molecule is a prime example of silicate compounds containing the Si-O-Si bridge. The molecule is of significant interest within the field of quantum chemistry, owing to the difficulty in theoretically predicting its…

The Diffusion Monte Carlo method is devoted to the computation of electronic ground-state energies of molecules. In this paper, we focus on implementations of this method which consist in exploring the configuration space with a {\bf fixed}…

Numerical Analysis · Mathematics 2007-05-23 Tony Lelievre , Mohamed El Makrini , Benjamin Jourdain

Quantum-mechanical methods are widely used for understanding molecular interactions throughout biology, chemistry, and materials science. Quantum diffusion Monte Carlo (DMC) and coupled cluster with single, double, and perturbative triple…

While it is empirically accepted that the fixed-node diffusion Monte-Carlo (FN-DMC) depends only weakly on the size of the one-particle basis sets used to expand its guiding functions, limits of this observation are not settled yet. Our…

Chemical Physics · Physics 2017-02-07 Matúš Dubecký

We report results of both the Diffusion Quantum Monte Carlo (DMC) and Reptation Quantum Monte Carlo (RMC) methods on the potential energy curve of the helium dimer. We show that it is possible to obtain a highly accurate description of the…

Chemical Physics · Physics 2010-05-07 Xuebin Wu , Chenlei Du , Jianbo Deng

We modify the reweighting factor of the projector used in diffusion Monte Carlo to reduce the time-step error of the total energy. Further, we present a reweighting scheme that has the desirable feature that it is exactly size-consistent,…

Chemical Physics · Physics 2024-03-18 Tyler A. Anderson , Manolo C. Per , C. J. Umrigar

We develop a novel multilevel asymptotic-preserving Monte Carlo method, called Multilevel Kinetic-Diffusion Monte Carlo (ML-KDMC), for simulating the kinetic Boltzmann transport equation with a Bhatnagar-Gross-Krook (BGK) collision…

Numerical Analysis · Mathematics 2020-10-23 Bert Mortier , Pieterjan Robbe , Martine Baelmans , Giovanni Samaey

We report diffusion Monte Carlo (DMC) calculations on MgO in the rock-salt and CsCl structures. The calculations are based on Hartree-Fock pseudopotentials, with the single-particle orbitals entering the correlated wave function being…

Strongly Correlated Electrons · Physics 2016-08-16 D. Alfè , M. Alfredsson , J. Brodholt , M. J. Gillan M. D. Towler , R. J. Needs

Employing a classical density-functional description of liquid environments, we introduce a rigorous method for the diffusion quantum Monte Carlo calculation of free energies and thermodynamic averages of solvated systems that requires…

The yardstick of new first-principles approaches to key points on reaction paths at metal surfaces is chemical accuracy compared to reliable experiment. By this we mean that such values as the activation barrier are required to within 1…

Materials Science · Physics 2017-05-24 Philip E Hoggan

We report results of both Diffusion Quantum Monte Carlo(DMC) method and Reptation Quantum Monte Carlo(RMC) method on the potential energy curve of the helium dimer. We show that it is possible to obtain a highly accurate description of the…

Chemical Physics · Physics 2015-05-18 Xuebin Wu , Xianru Hu , Chenlei Du , Yunchuan Dai , Shibin Chu , Leibo Hu , Jianbo Deng , Yuanping Feng

Pseudopotential locality errors have hampered the applications of the diffusion Monte Carlo (DMC) method in materials containing transition metals, in particular oxides. We have developed locality error free effective core potentials,…

The Diffusion Monte Carlo (DMC) method is applied to compute the ground state energies of the water monomer and dimer and their D 2 O isotopomers using MB-pol; the most recent and most accurate ab inito- based potential energy surface…

Chemical Physics · Physics 2015-10-28 Joel Mallory , Vladimir Mandelshtam

Efficient Monte Carlo (MC) sampling of many-body systems with long-range electrostatics is often limited by the cost of per-move energy-difference evaluation under periodic boundary conditions. We present DMK-MC, an accelerated MC method…

Computational Physics · Physics 2026-01-15 Xuanzhao Gao , Shidong Jiang , Jiuyang Liang , Qi Zhou

The dissociation energies of four transition metal dimers are determined using diffusion Monte Carlo. The Jastrow, CI, and molecular orbital parameters of the wave function are both partially and fully optimized with respect to the…

Chemical Physics · Physics 2019-09-06 Jil Ludovicy , Kaveh Haghighi Mood , Arne Lüchow

In this paper we study from a numerical analysis perspective the Fractional Step Kinetic Monte Carlo (FS-KMC) algorithms proposed in [1] for the parallel simulation of spatially distributed particle systems on a lattice. FS-KMC are…

Numerical Analysis · Mathematics 2012-08-07 Giorgos Arampatzis , Markos A. Katsoulakis , Petr Plechac

The stochastic density functional theory (sDFT) has exhibited advantages over the standard Kohn-Sham DFT method and has become an attractive approach for large-scale electronic structure calculations. The sDFT method avoids the expensive…

Computational Physics · Physics 2025-12-08 Xue Quan , Huajie Chen
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