Representation of the QM Subsystem for Long-Range Electrostatic Interaction in Non-Periodic Ab Initio QM/MM Calculations

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dc.contributor.authorPan, Xaoliang
dc.contributor.authorRosta, Edina
dc.contributor.authorShao, Yihan
dc.date.accessioned2018-12-06T21:35:21Z
dc.date.available2018-12-06T21:35:21Z
dc.date.issued2018-09-29
dc.descriptionThis paper is published as part of a thematic issue of Molecules on “Combined Quantum Mechanical and Molecular Mechanical Methods and Simulations”. http://www.mdpi.com/journal/molecules/special_issues/QMen_US
dc.description.abstractIn QM/MM calculations, it is essential to handle electrostatic interactions between the QM and MM subsystems accurately and efficiently. To achieve maximal efficiency, it is convenient to adopt a hybrid scheme, where the QM electron density is used explicitly in the evaluation of short-range QM/MM electrostatic interactions, while a multipolar representation for the QM electron density is employed to account for the long-range QM/MM electrostatic interactions. In order to avoid energy discontinuity at the cutoffs, which separate the short- and long-range QM/MM electrostatic interactions, a switching function should be utilized to ensure a smooth potential energy surface. In this study, we benchmarked the accuracy of such hybrid embedding schemes for QM/MM electrostatic interactions using different multipolar representations, switching functions and cutoff distances. For test systems (neutral and anionic oxyluciferin in MM (aqueous and enzyme) environments), the best accuracy was acquired with a combination of QM electrostatic potential (ESP) charges and dipoles and two switching functions (long-range electrostatic corrections (LREC) and Switch) in the treatment of long-range QM/MM electrostatics. It allowed us to apply a 10Å distance cutoff and still obtain QM/MM electrostatics/polarization energies within 0.1 kcal/mol and time-dependent density functional theory (TDDFT)/MM vertical excitation energies within 10−3 eV from theoretical reference values.en_US
dc.description.peerreviewYesen_US
dc.description.sponsorshipThis research was funded by the U.S. Department of Energy Office of Science (DE-SC0011297), EPSRC (EP/R013012/1, EP/L027151/1 and EP/N020669), and ERC (Project 757850 BioNet).en_US
dc.identifier.citationPan, X.; Rosta, E.; Shao, Y. Representation of the QM Subsystem for Long-Range Electrostatic Interaction in Non-Periodic Ab Initio QM/MM Calculations. Molecules 2018, 23, 2500.en_US
dc.identifier.doi10.3390/molecules23102500en_US
dc.identifier.urihttps://hdl.handle.net/11244/316285
dc.languageen_USen_US
dc.rightsAttribution-NonCommercial 4.0 International*
dc.rights.urihttp://creativecommons.org/licenses/by-nc/4.0/*
dc.subjectelectrostaticsen_US
dc.subjectmultipolar expansionen_US
dc.subjectmultiscale modelingen_US
dc.subjectQM/MMen_US
dc.titleRepresentation of the QM Subsystem for Long-Range Electrostatic Interaction in Non-Periodic Ab Initio QM/MM Calculationsen_US
dc.typeArticleen_US
ou.groupCollege of Arts and Sciences::Department of Chemistry and Biochemistryen_US

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