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Density functional theory (DFT) is widely used in surface science, but gives poor accuracy for oxide surface processes, while high-level quantum chemistry methods are hard to apply without losing basis-set quality. We argue that quantum…

Materials Science · Physics 2007-05-23 D. Alfe` , M. J. Gillan

We have applied the many-body ab-initio diffusion quantum Monte Carlo (DMC) method to study Zn and ZnO crystals under pressure, and the energetics of the oxygen vacancy, zinc interstitial and hydrogen impurities in ZnO. We show that DMC is…

Materials Science · Physics 2015-05-01 Juan A. Santana , Jaron T. Krogel , Jeongnim Kim , Paul R. C. Kent , Fernando A. Reboredo

Density functional theory (DFT) is widely used to study defects in monolayer graphene with a view to applications ranging from water filtration to electronics to investigation of radiation damage in graphite moderators. To assess the…

Materials Science · Physics 2022-06-16 D. M. Thomas , Y. Asiri , N. D. Drummond

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

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…

The equations of state, formation energy and migration energy barrier of the oxygen vacancy in SrFeO${_3}$ and LaFeO${_3}$ were calculated with the diffusion quantum Monte Carlo (DMC) method. Calculations were also performed with various…

Materials Science · Physics 2017-07-19 Juan A. Santana , Jaron T. Krogel , Paul R. C. Kent , Fernando A. Reboredo

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

The precise understanding of adsorption energetics and molecular geometry at catalytic sites is fundamental for advancing catalysis, particularly under the constraints of resource efficiency and environmental sustainability. This study…

Materials Science · Physics 2025-12-16 Jeonghwan Ahn , Iuegyun Hong , Gwangyoung Lee , Hyeondeok Shin , Anouar Benali , Yongkyung Kwon

We have applied the diffusion quantum Monte Carlo (DMC) method to calculate the cohesive energy and the structural parameters of the binary oxides CaO, SrO, BaO, Sc2O3, Y2O3 and La2O3. The aim of our calculations is to systematically…

Materials Science · Physics 2016-08-24 Juan A. Santana , Jaron T. Krogel , Paul R. C. Kent , Fernando A. Reboredo

Cubic hafnia (HfO$_2$) is of great interest for a number of applications in electronics because of its high dielectric constant. However, common defects in such applications degrade the properties of hafina. We have investigated the…

Materials Science · Physics 2019-07-31 Raghuveer Chimata , Hyeondeok Shin , Anouar Benali , Olle Heinonen

We present a detailed study of the energetics of water clusters (H$_2$O)$_n$ with $n \le 6$, comparing diffusion Monte Carlo (DMC) and approximate density functional theory (DFT) with well converged coupled-cluster benchmarks. We use the…

Materials Science · Physics 2015-06-04 M. J. Gillan , F. R. Manby , M. D. Towler , D. Alfè

The fixed node diffusion Monte Carlo (DMC) method has attracted interest in recent years as a way to calculate properties of solid materials with high accuracy. However, the framework for the calculation of properties such as total…

Materials Science · Physics 2016-01-20 Jaehyung Yu , Lucas K. Wagner , Elif Ertekin

Diffusion Monte Carlo (DMC) is being recognized as a higher-accuracy, albeit more computationally expensive, alternative to Density Functional Theory (DFT) for energy predictions of catalytic systems. A major computational bottleneck in the…

Materials Science · Physics 2022-10-12 Gopal R. Iyer , Brenda M. Rubenstein

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

We present an approach to calculation of point defect optical and thermal ionization energies based on the highly accurate quantum Monte Carlo methods. The use of an inherently many-body theory that directly treats electron correlation…

Materials Science · Physics 2015-06-11 Elif Ertekin , Lucas K. Wagner , Jeffrey C. Grossman

The oxygen vacancy formation energy ($\Delta E_{vf}$) governs defect dynamics and is a useful metric to perform materials selection for a variety of applications. However, density functional theory (DFT) calculations of $\Delta E_{vf}$ come…

The electronic structure and total energy were calculated for ordered and disordered MgO-CaO solid solutions within the multiple scattering theory in real space and the local density approximation. Based on the dependence of the total…

Materials Science · Physics 2009-11-07 S. V. Stolbov , R. E. Cohen

We combine density functional theory (DFT) with molecular dynamics simulations based on an accurate atomistic force field to calculate the pressure derivative of the melting temperature of magnesium oxide at ambient pressure - a quantity…

Materials Science · Physics 2009-11-30 Paul Tangney , Sandro Scandolo

We perform quantum Monte Carlo (QMC) calculations to determine minimum energy pathways of simple chemical reactions, and compare the computed geometries and reaction barriers with those obtained with density functional theory (DFT) and…

Chemical Physics · Physics 2015-06-12 Sebastiano Saccani , Claudia Filippi , Saverio Moroni

Recent technical advances in dealing with finite-size errors make quantum Monte Carlo methods quite appealing for treating extended systems in electronic structure calculations, especially when commonly-used density functional theory (DFT)…

Materials Science · Physics 2016-10-06 Kyle G. Reeves , Yi Yao , Yosuke Kanai
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