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Erik Donovan Hedegård

Postdoctoral fellow

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Exploration of H2 binding to the [NiFe]-hydrogenase active site with multiconfigurational density functional theory

Author

  • Geng Dong
  • Ulf Ryde
  • Hans Jørgen Aa Jensen
  • Erik D. Hedegård

Summary, in English

The combination of density functional theory (DFT) with a multiconfigurational wave function is an efficient way to include dynamical correlation in calculations with multiconfiguration self-consistent field wave functions. These methods can potentially be employed to elucidate reaction mechanisms in bio-inorganic chemistry, where many other methods become either too computationally expensive or too inaccurate. In this paper, a complete active space (CAS) short-range DFT (CAS-srDFT) hybrid was employed to investigate a bio-inorganic system, namely H2 binding to the active site of [NiFe] hydrogenase. This system was previously investigated with coupled-cluster (CC) and multiconfigurational methods in the form of cumulant-approximated second-order perturbation theory, based on the density matrix renormalization group (DMRG). We find that it is more favorable for H2 to bind to Ni than to Fe, in agreement with previous CC and DMRG calculations. The accuracy of CAS-srDFT is comparable to both CC and DMRG, despite much smaller active spaces were employed than in the corresponding DMRG calculations. This enhanced efficiency at the smaller active spaces shows that CAS-srDFT can become a useful method for bio-inorganic chemistry.

Department/s

  • Computational Chemistry
  • eSSENCE: The e-Science Collaboration

Publishing year

2018

Language

English

Pages

794-801

Publication/Series

Physical Chemistry Chemical Physics

Volume

20

Issue

2

Document type

Journal article

Publisher

Royal Society of Chemistry

Topic

  • Physical Chemistry (including Surface- and Colloid Chemistry)

Status

Published

ISBN/ISSN/Other

  • ISSN: 1463-9076