A Projector-Embedding Approach for Multiscale Coupled-Cluster Calculations Applied to Citrate Synthase

Simon Bennie, Marc Van der Kamp, Robert Pennifold, Martina Stella, Fred Manby, Adrian Mulholland

Research output: Contribution to journalArticle (Academic Journal)

34 Citations (Scopus)
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Abstract

Projector-based embedding has recently emerged as a robust and accurate method for the calculation of various electronic molecular properties. We present the coupling of projector embedding with quantum mechanical / molecular mechanical (QM/MM) modeling and apply it for the first time to an enzyme-catalyzed reaction. Using projector-based embedding, we combine coupled-cluster theory, density-functional theory (DFT) and molecular mechanics to compute energies for the proton abstraction from acetyl-coenzyme A by citrate synthase. By embedding correlated ab initio methods in DFT we eliminate functional sensitivity and obtain high-accuracy profiles in a procedure that is straightforward to apply.
Original languageEnglish
Pages (from-to)2689-2697
Number of pages9
JournalJournal of Chemical Theory and Computation
Volume12
Issue number6
Early online date19 May 2016
DOIs
Publication statusPublished - 14 Jun 2016

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Keywords

  • Enzyme reaction
  • multiscale modeling
  • QM/MM
  • CCSD(T)
  • DFT

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