Article: Calculating solution redox free energies with ab initio quantum mechanical/molecular mechanical minimum free energy path method

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TitleCalculating solution redox free energies with ab initio quantum mechanical/molecular mechanical minimum free energy path method
AuthorsZeng, X1
Hu, H1
Hu, X1
Yang, W1
Issue Date2009
PublisherAmerican Institute of Physics. The Journal's web site is located at http://jcp.aip.org/jcp/staff.jsp
CitationJournal Of Chemical Physics, 2009, v. 130 n. 16 [How to Cite?]
DOI: http://dx.doi.org/10.1063/1.3120605
AbstractA quantum mechanical/molecular mechanical minimum free energy path (QM/MM-MFEP) method was developed to calculate the redox free energies of large systems in solution with greatly enhanced efficiency for conformation sampling. The QM/MM-MFEP method describes the thermodynamics of a system on the potential of mean force surface of the solute degrees of freedom. The molecular dynamics (MD) sampling is only carried out with the QM subsystem fixed. It thus avoids "on-the-fly" QM calculations and thus overcomes the high computational cost in the direct QM/MM MD sampling. In the applications to two metal complexes in aqueous solution, the new QM/MM-MFEP method yielded redox free energies in good agreement with those calculated from the direct QM/MM MD method. Two larger biologically important redox molecules, lumichrome and riboflavin, were further investigated to demonstrate the efficiency of the method. The enhanced efficiency and uncompromised accuracy are especially significant for biochemical systems. The QM/MM-MFEP method thus provides an efficient approach to free energy simulation of complex electron transfer reactions. © 2009 American Institute of Physics.
ISSN0021-9606
2011 Impact Factor: 3.333
2011 SCImago Journal Rankings: 0.155
DOIhttp://dx.doi.org/10.1063/1.3120605
ReferencesReferences in Scopus
DC Field
Value
dc.contributor.authorZeng, X
dc.contributor.authorHu, H
dc.contributor.authorHu, X
dc.contributor.authorYang, W
dc.date.accessioned2012-10-08T03:18:04Z
dc.date.available2012-10-08T03:18:04Z
dc.date.issued2009
dc.description.abstractA quantum mechanical/molecular mechanical minimum free energy path (QM/MM-MFEP) method was developed to calculate the redox free energies of large systems in solution with greatly enhanced efficiency for conformation sampling. The QM/MM-MFEP method describes the thermodynamics of a system on the potential of mean force surface of the solute degrees of freedom. The molecular dynamics (MD) sampling is only carried out with the QM subsystem fixed. It thus avoids "on-the-fly" QM calculations and thus overcomes the high computational cost in the direct QM/MM MD sampling. In the applications to two metal complexes in aqueous solution, the new QM/MM-MFEP method yielded redox free energies in good agreement with those calculated from the direct QM/MM MD method. Two larger biologically important redox molecules, lumichrome and riboflavin, were further investigated to demonstrate the efficiency of the method. The enhanced efficiency and uncompromised accuracy are especially significant for biochemical systems. The QM/MM-MFEP method thus provides an efficient approach to free energy simulation of complex electron transfer reactions. © 2009 American Institute of Physics.
dc.description.natureLink_to_subscribed_fulltext
dc.identifier.citationJournal Of Chemical Physics, 2009, v. 130 n. 16 [How to Cite?]
DOI: http://dx.doi.org/10.1063/1.3120605
dc.identifier.doihttp://dx.doi.org/10.1063/1.3120605
dc.identifier.issn0021-9606
2011 Impact Factor: 3.333
2011 SCImago Journal Rankings: 0.155
dc.identifier.issue16
dc.identifier.pmid19405565
dc.identifier.scopuseid_2-s2.0-65149099599
dc.identifier.urihttp://hdl.handle.net/10722/168371
dc.identifier.volume130
dc.languageeng
dc.publisherAmerican Institute of Physics. The Journal's web site is located at http://jcp.aip.org/jcp/staff.jsp
dc.publisher.placeUnited States
dc.relation.ispartofJournal of Chemical Physics
dc.relation.referencesReferences in Scopus
dc.subject.meshComputer Simulation
dc.subject.meshFlavins - Chemistry
dc.subject.meshMetals - Chemistry
dc.subject.meshModels, Molecular
dc.subject.meshOxidation-Reduction
dc.subject.meshQuantum Theory
dc.subject.meshRiboflavin - Chemistry
dc.subject.meshSolutions - Chemistry
dc.subject.meshThermodynamics
dc.titleCalculating solution redox free energies with ab initio quantum mechanical/molecular mechanical minimum free energy path method
dc.typeArticle
Author Affiliations
  1. Duke University