title: A Projector-Embedding Approach for Multiscale Coupled-Cluster Calculations Applied to Citrate Synthase.
abstract: Projector-based embedding has recently emerged as a robust multiscale method for the calculation of various electronic molecular properties. We present the coupling of projector embedding with quantum mechanics/molecular mechanics 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.
authors.affiliation: Center for Computational Chemistry, School of Chemistry, University of Bristol , Bristol BS8 1TS, U.K.
authors.forename: Simon J
authors.initials: SJ
authors.lastname: Bennie
authors.affiliation: Center for Computational Chemistry, School of Chemistry, University of Bristol , Bristol BS8 1TS, U.K.|School of Biochemistry, Biomedical Sciences Building, University Walk, University of Bristol , Bristol BS8 1TD, U.K.
authors.forename: Marc W
authors.initials: MW
authors.lastname: van der Kamp
authors.affiliation: Center for Computational Chemistry, School of Chemistry, University of Bristol , Bristol BS8 1TS, U.K.
authors.forename: Robert C R
authors.initials: RC
authors.lastname: Pennifold
authors.affiliation: Center for Computational Chemistry, School of Chemistry, University of Bristol , Bristol BS8 1TS, U.K.
authors.forename: Martina
authors.initials: M
authors.lastname: Stella
authors.affiliation: Center for Computational Chemistry, School of Chemistry, University of Bristol , Bristol BS8 1TS, U.K.
authors.forename: Frederick R
authors.initials: FR
authors.lastname: Manby
authors.affiliation: Center for Computational Chemistry, School of Chemistry, University of Bristol , Bristol BS8 1TS, U.K.
authors.forename: Adrian J
authors.initials: AJ
authors.lastname: Mulholland
mesh_terms: D000105:Acetyl Coenzyme A / Q000737:chemistry / Q000378:metabolism; D055162:Biocatalysis; D002950:Citrate (si)-Synthase / Q000737:chemistry* / Q000378:metabolism; D008958:Models, Molecular; D011522:Protons; D011789:Quantum Theory; D013816:Thermodynamics
chemical_list: D011522:Protons; D000105:Acetyl Coenzyme A; D002950:Citrate (si)-Synthase