Communication: Embedded fragment stochastic density functional theory

2014/06/11 by Daniel Neuhauser, Roi Baer, Eran Rabani · 78 citations
Chemistry · Engineering · Mathematics · Physics and Astronomy · #Advanced Chemical Physics Studies #Atomic orbital #Chemistry #Computational chemistry #Computer science #Convergence (economics) #Density functional theory #Dimer #Mathematics #Molecular Junctions and Nanostructures #Physics #Quantum mechanics #Scaling #Spectroscopy and Quantum Chemical Studies #Spurious relationship #Statistical physics #Stochastic process #Time-dependent density functional theory #cond-mat.mtrl-sci #physics.chem-ph #physics.comp-ph

paper · pdf · doi:10.1063/1.4890651

published in The Journal of Chemical Physics 141(4), 041102 (American Institute of Physics) · 4 pages, 2 figures

arxiv created 2014/06/11 · openalex publication_date 2014/07/23 · arxiv updated 2015/06/19 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/05

Abstract

We develop a method in which the electronic densities of small fragments determined by Kohn-Sham density functional theory (DFT) are embedded using stochastic DFT to form the exact density of the full system. The new method preserves the scaling and the simplicity of the stochastic DFT but cures the slow convergence that occurs when weakly coupled subsystems are treated. It overcomes the spurious charge fluctuations that impair the applications of the original stochastic DFT approach. We demonstrate the new approach on a fullerene dimer and on clusters of water molecules and show that the density of states and the total energy can be accurately described with a relatively small number of stochastic orbitals.

Citations

• Frozen density functional approach for ab initio calculations of solvated molecules
• Is the Ewald summation still necessary? Pairwise alternatives to the accepted standard for long-range electrostatics
• Efficient index handling of multidimensional periodic boundary conditions
• Self-Consistent Equations Including Exchange and Correlation Effects

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