skip to main content

SciTech ConnectSciTech Connect

Title: Embedded-cluster calculations in a numeric atomic orbital density-functional theory framework

We integrate the all-electron electronic structure code FHI-aims into the general ChemShell package for solid-state embedding quantum and molecular mechanical (QM/MM) calculations. A major undertaking in this integration is the implementation of pseudopotential functionality into FHI-aims to describe cations at the QM/MM boundary through effective core potentials and therewith prevent spurious overpolarization of the electronic density. Based on numeric atomic orbital basis sets, FHI-aims offers particularly efficient access to exact exchange and second order perturbation theory, rendering the established QM/MM setup an ideal tool for hybrid and double-hybrid level density functional theory calculations of solid systems. We illustrate this capability by calculating the reduction potential of Fe in the Fe-substituted ZSM-5 zeolitic framework and the reaction energy profile for (photo-)catalytic water oxidation at TiO{sub 2}(110)
Authors:
; ;  [1] ; ; ; ;  [2] ;  [3] ;  [4]
  1. Chair for Theoretical Chemistry and Catalysis Research Center, Technische Universit√§t M√ľnchen, Lichtenbergstr. 4, D-85747 Garching (Germany)
  2. Department of Chemistry, Kathleen Lonsdale Materials Chemistry, University College London, 20 Gordon St., London WC1H 0AJ (United Kingdom)
  3. Scientific Computing Department, STFC Daresbury Laboratory, Daresbury, Warrington (United Kingdom)
  4. Department of Mechanical Engineering and Materials Science, Duke University, Durham, North Carolina 27708 (United States)
Publication Date:
OSTI Identifier:
22308250
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 141; Journal Issue: 2; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CATIONS; DENSITY; DENSITY FUNCTIONAL METHOD; ELECTRONIC STRUCTURE; ELECTRONS; ENERGY-LEVEL DENSITY; HYBRIDIZATION; OXIDATION; PERTURBATION THEORY; SOLIDS; TITANIUM OXIDES; WATER; ZEOLITES