Diffusion quantum Monte Carlo study of the equation of state and point defects in aluminum

TL;DR

This study employs diffusion quantum Monte Carlo to accurately compute the equation of state and defect energetics in aluminum, demonstrating DMC's potential as a predictive benchmark tool for metallic defects.

Contribution

The paper applies advanced DMC methods to calculate defect energetics in aluminum, providing highly accurate benchmarks and comparing results with DFT and experimental data.

Findings

DMC predicts lattice constant within 0.2% of experiment.

Defect formation energies agree with experimental data, except for some discrepancies.

DMC and DFT results are in close agreement for vacancy defects.

Abstract

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. The DMC equilibrium lattice constant differs from experiment by 0.008 A, or 0.2%, while the cohesive energy using DMC with backflow wave functions with improved nodal surfaces differs by 27 meV. DMC-calculated defect formation and migration energies agree with available experimental data, except for the nearest-neighbor divacancy, which is found to be energetically unstable, in agreement with previous density functional theory (DFT) calculations. DMC and DFT calculations of vacancy defects are in reasonably close agreement. Self-interstitial formation energies have larger differences between DMC and DFT, of up to 0.33eV, at the tetrahedral site. We also computed formation energies of helium interstitial defects where energies differed by up to 0.34eV, also at the tetrahedral site. The close agreement with available experiments demonstrates that DMC can be used as a predictive method to obtain benchmark energetics of defects in metals.