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

TitleCalculating solution redox free energies with ab initio quantum mechanical/molecular mechanical minimum free energy path method
Authors
Issue Date2009
PublisherAmerican Institute of Physics. The Journal's web site is located at http://jcp.aip.org/jcp/staff.jsp
Citation
Journal Of Chemical Physics, 2009, v. 130 n. 16 How to Cite?
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 "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.
Persistent Identifierhttp://hdl.handle.net/10722/168371
ISSN
2013 Impact Factor: 3.122
ISI Accession Number ID
References

 

Author Affiliations
  1. Duke University
DC FieldValueLanguage
dc.contributor.authorZeng, Xen_US
dc.contributor.authorHu, Hen_US
dc.contributor.authorHu, Xen_US
dc.contributor.authorYang, Wen_US
dc.date.accessioned2012-10-08T03:18:04Z-
dc.date.available2012-10-08T03:18:04Z-
dc.date.issued2009en_US
dc.identifier.citationJournal Of Chemical Physics, 2009, v. 130 n. 16en_US
dc.identifier.issn0021-9606en_US
dc.identifier.urihttp://hdl.handle.net/10722/168371-
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.en_US
dc.languageengen_US
dc.publisherAmerican Institute of Physics. The Journal's web site is located at http://jcp.aip.org/jcp/staff.jspen_US
dc.relation.ispartofJournal of Chemical Physicsen_US
dc.subject.meshComputer Simulationen_US
dc.subject.meshFlavins - Chemistryen_US
dc.subject.meshMetals - Chemistryen_US
dc.subject.meshModels, Molecularen_US
dc.subject.meshOxidation-Reductionen_US
dc.subject.meshQuantum Theoryen_US
dc.subject.meshRiboflavin - Chemistryen_US
dc.subject.meshSolutions - Chemistryen_US
dc.subject.meshThermodynamicsen_US
dc.titleCalculating solution redox free energies with ab initio quantum mechanical/molecular mechanical minimum free energy path methoden_US
dc.typeArticleen_US
dc.identifier.emailHu, H:haohu@hku.hken_US
dc.identifier.authorityHu, H=rp00707en_US
dc.description.naturelink_to_subscribed_fulltexten_US
dc.identifier.doi10.1063/1.3120605en_US
dc.identifier.pmid19405565en_US
dc.identifier.scopuseid_2-s2.0-65149099599en_US
dc.relation.referenceshttp://www.scopus.com/mlt/select.url?eid=2-s2.0-65149099599&selection=ref&src=s&origin=recordpageen_US
dc.identifier.volume130en_US
dc.identifier.issue16en_US
dc.identifier.isiWOS:000266885200012-
dc.publisher.placeUnited Statesen_US
dc.identifier.scopusauthoridZeng, X=7403247770en_US
dc.identifier.scopusauthoridHu, H=7404097564en_US
dc.identifier.scopusauthoridHu, X=12782008400en_US
dc.identifier.scopusauthoridYang, W=7407757509en_US

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