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Author Huang, Chen
Source United States Department of Energy Office of Scientific and Technical Information
Content type Text
Language English
Subject Keyword INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY ♦ BCC LATTICES ♦ COMPUTER CALCULATIONS ♦ COMPUTERIZED SIMULATION ♦ DENSITY FUNCTIONAL METHOD ♦ EFFICIENCY ♦ ELECTRIC POTENTIAL ♦ HETEROGENEOUS CATALYSIS ♦ ITERATIVE METHODS ♦ MAGNETIC MOMENTS ♦ SOLVENTS ♦ SPIN ORIENTATION
Abstract A key element in the density functional embedding theory (DFET) is the embedding potential. We discuss two major issues related to the embedding potential: (1) its non-uniqueness and (2) the numerical difficulty for solving for it, especially for the spin-polarized systems. To resolve the first issue, we extend DFET to finite temperature: all quantities, such as the subsystem densities and the total system’s density, are calculated at a finite temperature. This is a physical extension since materials work at finite temperatures. We show that the embedding potential is strictly unique at T > 0. To resolve the second issue, we introduce an efficient iterative embedding potential solver. We discuss how to relax the magnetic moments in subsystems and how to equilibrate the chemical potentials across subsystems. The solver is robust and efficient for several non-trivial examples, in all of which good quality spin-polarized embedding potentials were obtained. We also demonstrate the solver on an extended periodic system: iron body-centered cubic (110) surface, which is related to the modeling of the heterogeneous catalysis involving iron, such as the Fischer-Tropsch and the Haber processes. This work would make it efficient and accurate to perform embedding simulations of some challenging material problems, such as the heterogeneous catalysis and the defects of complicated spin configurations in electronic materials.
ISSN 00219606
Educational Use Research
Learning Resource Type Article
Publisher Date 2016-03-28
Publisher Place United States
Journal Journal of Chemical Physics
Volume Number 144
Issue Number 12


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