Embedded-Cluster Calculations in a Numeric Atomic Orbital Density-Functional Theory Framework
Abstract
We integrate the all-electron electronic structure code FHI-aims into the general ChemShell package for solid-state embedding (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 DFT 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).
Keywords
Cite
@article{arxiv.1404.2130,
title = {Embedded-Cluster Calculations in a Numeric Atomic Orbital Density-Functional Theory Framework},
author = {Daniel Berger and Andrew J. Logsdail and Harald Oberhofer and Matthew R. Farrow and C. Richard A. Catlow and Paul Sherwood and Alexey A. Sokol and Volker Blum and Karsten Reuter},
journal= {arXiv preprint arXiv:1404.2130},
year = {2015}
}
Comments
12 pages, 4 figures