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).
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14 July 2014
Research Article|
July 10 2014
Embedded-cluster calculations in a numeric atomic orbital density-functional theory framework
Daniel Berger;
Daniel Berger
a)
1Chair for Theoretical Chemistry and Catalysis Research Center,
Technische Universität München, Lichtenbergstr. 4
, D-85747 Garching, Germany
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Andrew J. Logsdail;
Andrew J. Logsdail
b)
2Department of Chemistry, Kathleen Lonsdale Materials Chemistry,
University College London
, 20 Gordon St., London WC1H 0AJ, United Kingdom
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Harald Oberhofer;
Harald Oberhofer
1Chair for Theoretical Chemistry and Catalysis Research Center,
Technische Universität München, Lichtenbergstr. 4
, D-85747 Garching, Germany
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Matthew R. Farrow;
Matthew R. Farrow
2Department of Chemistry, Kathleen Lonsdale Materials Chemistry,
University College London
, 20 Gordon St., London WC1H 0AJ, United Kingdom
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C. Richard A. Catlow;
C. Richard A. Catlow
2Department of Chemistry, Kathleen Lonsdale Materials Chemistry,
University College London
, 20 Gordon St., London WC1H 0AJ, United Kingdom
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Paul Sherwood;
Paul Sherwood
3Scientific Computing Department,
STFC Daresbury Laboratory
, Daresbury, Warrington, United Kingdom
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Alexey A. Sokol;
Alexey A. Sokol
2Department of Chemistry, Kathleen Lonsdale Materials Chemistry,
University College London
, 20 Gordon St., London WC1H 0AJ, United Kingdom
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Volker Blum;
Volker Blum
4Department of Mechanical Engineering and Materials Science,
Duke University
, Durham, North Carolina 27708, USA
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Karsten Reuter
Karsten Reuter
1Chair for Theoretical Chemistry and Catalysis Research Center,
Technische Universität München, Lichtenbergstr. 4
, D-85747 Garching, Germany
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a)
Electronic mail: [email protected]
b)
Electronic mail: [email protected]
J. Chem. Phys. 141, 024105 (2014)
Article history
Received:
April 08 2014
Accepted:
June 18 2014
Citation
Daniel Berger, Andrew J. Logsdail, Harald Oberhofer, Matthew R. Farrow, C. Richard A. Catlow, Paul Sherwood, Alexey A. Sokol, Volker Blum, Karsten Reuter; Embedded-cluster calculations in a numeric atomic orbital density-functional theory framework. J. Chem. Phys. 14 July 2014; 141 (2): 024105. https://doi.org/10.1063/1.4885816
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