Embedded-cluster calculations in a numeric atomic orbital density-functional theory framework.
Journal Article (Journal Article)
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 TiO2(110).
- Berger, D; Logsdail, AJ; Oberhofer, H; Farrow, MR; Catlow, CRA; Sherwood, P; Sokol, AA; Blum, V; Reuter, K
- July 2014
Volume / Issue
- 141 / 2
Start / End Page
- 024105 -
Electronic International Standard Serial Number (EISSN)
International Standard Serial Number (ISSN)
Digital Object Identifier (DOI)