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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
2013 Impact Factor: 3.122
 
DOIhttp://dx.doi.org/10.1063/1.3120605
 
ReferencesReferences in Scopus
 
DC FieldValue
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
2013 Impact Factor: 3.122
 
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
 
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<contributor.author>Hu, X</contributor.author>
<contributor.author>Yang, W</contributor.author>
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<description.abstract>A 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 &quot;on-the-fly&quot; 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. &#169; 2009 American Institute of Physics.</description.abstract>
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Author Affiliations
  1. Duke University