2014
Structural Studies of Oxomanganese Complexes for Water Oxidation Catalysis
Rivalta I, Brudvig G, Batista V. Structural Studies of Oxomanganese Complexes for Water Oxidation Catalysis. 2014, 1-14. DOI: 10.1002/9781118698648.ch1.Peer-Reviewed Original ResearchOxygen-evolving complexBiomimetic oxomanganese complexesOxomanganese complexesDensity functional theoryQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsHigh-resolution spectroscopyPhotosystem IIStructure of PSIIX-ray absorption fine structure spectraX-ray radiationExtended X-ray absorption fine structure (EXAFS) spectraProteinaceous side chainsWater oxidation catalysisArtificial photosynthetic devicesFine structure spectraO bond formationWater splitting mechanismX-ray crystallographyOxomanganese clusterResolution spectroscopyX-ray diffraction dataSemiconductor surfacesOxidation catalysisPhotosynthetic devicesX-ray model
2012
Oxomanganese complexes for natural and artificial photosynthesis
Rivalta I, Brudvig GW, Batista VS. Oxomanganese complexes for natural and artificial photosynthesis. Current Opinion In Chemical Biology 2012, 16: 11-18. PMID: 22481113, PMCID: PMC3335890, DOI: 10.1016/j.cbpa.2012.03.003.Peer-Reviewed Original ResearchConceptsOxygen-evolving complexOxomanganese complexesArtificial photosynthesisQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsArtificial photosynthetic devicesVisible-light photoexcitationInterfacial electron transferRecent X-ray dataX-ray crystallographyPhotosystem IIPhotosynthetic devicesMn catalystStructure/function relationsX-ray dataCarboxylate moietyElectron transferProton abstractionMn centersChromophoric linkersElectrostatic interactionsOEC structureCovalent attachmentS1 stateOxygen evolutionInexpensive materials
2009
The MoD-QM/MM methodology for structural refinement of photosystem II and other biological macromolecules
Sproviero EM, Newcomer MB, Gascón JA, Batista ER, Brudvig GW, Batista VS. The MoD-QM/MM methodology for structural refinement of photosystem II and other biological macromolecules. Photosynthesis Research 2009, 102: 455-470. PMID: 19633920, PMCID: PMC2954272, DOI: 10.1007/s11120-009-9467-6.Peer-Reviewed Original ResearchConceptsElectrostatic interactionsMM methodQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsForce fieldQM/MM hybrid methodsQM/MM methodologyQM/MM methodsMolecular mechanics force fieldQuantum chemistry techniquesMM force fieldsStructural refinementPhotosystem IIChemistry techniquesStructure/function relationsCharge transferQM layerMolecular fragmentsChemical modificationBiological macromoleculesSteric hindranceComputational protocolSpectroscopic dataMolecular domainsStructural propertiesHigh-resolution spectroscopic data
2008
Computational insights into the O2-evolving complex of photosystem II
Sproviero EM, McEvoy JP, Gascón JA, Brudvig GW, Batista VS. Computational insights into the O2-evolving complex of photosystem II. Photosynthesis Research 2008, 97: 91-114. PMID: 18483777, PMCID: PMC2728911, DOI: 10.1007/s11120-008-9307-0.Peer-Reviewed Original ResearchConceptsOxygen-evolving complexX-ray diffractionQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsPhotosystem IIMass spectrometryX-ray absorption fine structure spectroscopyExtended X-ray absorption fine structure (EXAFS) spectroscopyQM/MM modelingElectron paramagnetic resonance spectroscopyAbsorption fine structure spectroscopyCatalytic metal clustersWater splitting reactionIntermediate oxidation statesParamagnetic resonance spectroscopyFine structure spectroscopyO2-evolving complexDensity functional theoryInorganic coreMM modelingOxidation stateMetal clustersStructure spectroscopyOEC structureCrystallographic resultsComputational insightsQuantum Mechanics/Molecular Mechanics Study of the Catalytic Cycle of Water Splitting in Photosystem II
Sproviero EM, Gascón JA, McEvoy JP, Brudvig GW, Batista VS. Quantum Mechanics/Molecular Mechanics Study of the Catalytic Cycle of Water Splitting in Photosystem II. Journal Of The American Chemical Society 2008, 130: 3428-3442. PMID: 18290643, DOI: 10.1021/ja076130q.Peer-Reviewed Original ResearchConceptsSubstrate water moleculesWater moleculesMu-oxo bridgeOxygen-evolving complexWater splittingQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsQuantum Mechanics/Molecular Mechanics StudySolar fuel production systemsPhotosystem IIX-ray diffraction structureMolecular mechanics studySecond coordination shellCyanobacterium Thermosynechococcus elongatusOxomanganese clusterDioxygen evolutionTerminal ligandsXRD structureCatalytic clustersCP43-R357Ligand exchangeCatalytic reactionCatalytic cycleReaction intermediatesS0 stateNucleophilic attackComputational studies of the O2-evolving complex of photosystem II and biomimetic oxomanganese complexes
Sproviero EM, Gascón JA, McEvoy JP, Brudvig GW, Batista VS. Computational studies of the O2-evolving complex of photosystem II and biomimetic oxomanganese complexes. Coordination Chemistry Reviews 2008, 252: 395-415. PMID: 19190716, PMCID: PMC2350217, DOI: 10.1016/j.ccr.2007.09.006.Peer-Reviewed Original ResearchBiomimetic oxomanganese complexesOxygen-evolving complexOxomanganese complexesWater oxidationPhotosystem IIQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsCatalytic centerQM/MM modelCatalytic metal clustersPhotosynthetic water oxidationX-ray crystallographyX-ray absorption fine structure measurementsAbsorption fine structure measurementsQuantum mechanical studyO2-evolving complexX-ray diffraction dataAmino acid residuesExtended X-ray absorption fine structure (EXAFS) measurementsDetailed molecular levelComputational chemistsWater splittingCatalytic cycleComparative quantum mechanical studyMetal clustersFine structure measurementsLigation Of The C-Terminus Of The D1 Polypeptide Of Photosystem Ii To The Oxygen Evolving Complex: A Dft-Qm/Mm Study
Gascón J, Sproviero E, McEvoy J, Brudvig G, Batista V. Ligation Of The C-Terminus Of The D1 Polypeptide Of Photosystem Ii To The Oxygen Evolving Complex: A Dft-Qm/Mm Study. 2008, 363-368. DOI: 10.1007/978-1-4020-6709-9_82.Peer-Reviewed Original ResearchOxygen-evolving complexC-terminal carboxylateD1-Ala344OEC of PSIIQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsX-ray diffraction modelPhotosystem IID1 polypeptideFTIR difference spectraX-ray diffraction experimentsMM studyFTIR dataCalcium ligationElectronic propertiesVibrational frequenciesS2 stateSymmetric stretchPSII particlesXRD modelFTIRCarboxylateDiffraction experimentsDifference spectraComplexes
2007
Quantum mechanics/molecular mechanics structural models of the oxygen-evolving complex of photosystem II
Sproviero EM, Gascón JA, McEvoy JP, Brudvig GW, Batista VS. Quantum mechanics/molecular mechanics structural models of the oxygen-evolving complex of photosystem II. Current Opinion In Structural Biology 2007, 17: 173-180. PMID: 17395452, DOI: 10.1016/j.sbi.2007.03.015.Peer-Reviewed Original ResearchConceptsOxygen-evolving complexPhotosystem IIWater oxidationOEC of PSIIQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsPhotocatalytic water oxidationGreen plant chloroplastsX-ray crystallographyX-ray absorption fine structure measurementsProcess of photosynthesisAmino acid residuesAbsorption fine structure measurementsExtended X-ray absorption fine structure (EXAFS) measurementsIntrinsic electronic propertiesComputational structural modelsFine structure measurementsOEC modelsAvailable mechanistic dataProtein environmentThylakoid membranesCatalytic mechanismX-ray diffraction modelElectronic propertiesInternal membranesCatalytic center
2006
Computational Studies of the Primary Phototransduction Event in Visual Rhodopsin
Gascón J, Sproviero E, Batista V. Computational Studies of the Primary Phototransduction Event in Visual Rhodopsin. Accounts Of Chemical Research 2006, 39: 184-193. PMID: 16548507, DOI: 10.1021/ar050027t.Peer-Reviewed Original ResearchConceptsG protein-coupled receptorsRecent computational studiesPrimary photochemical eventQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsComputational studyPhotochemical eventsEnergy storage mechanismPrototypical G protein-coupled receptorX-ray structureVisual rhodopsinHigh-resolution X-ray structuresBovine visual rhodopsinWater moleculesSpectroscopic changesRetinyl chromophoreStorage mechanismActive siteMolecular rearrangementTrans isomerizationPhototransduction eventsMolecular originIndividual residuesStructural refinementPhototransduction mechanismChromophore
2005
QM/MM Study of the NMR Spectroscopy of the Retinyl Chromophore in Visual Rhodopsin
Gascón J, Sproviero E, Batista V. QM/MM Study of the NMR Spectroscopy of the Retinyl Chromophore in Visual Rhodopsin. Journal Of Chemical Theory And Computation 2005, 1: 674-685. PMID: 26641690, DOI: 10.1021/ct0500850.Peer-Reviewed Original ResearchGauge independent atomic orbital (GIAO) methodQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsSolid-state NMR experimentsQM/MM studyDensity functional theory B3LYP/6Nuclear magnetic resonance spectraNMR chemical shiftsFirst-principles interpretationLevel of theoryMagnetic resonance spectraAtomic orbitals methodNMR spectroscopyChemical shiftsMM studyNMR experimentsRetinyl chromophoreAb initioOrbital methodResonance spectraAtomistic modelVisual rhodopsinChromophoreField calculationsPrototypical G protein-coupled receptorB3LYP/6
2004
QM/MM Study of Energy Storage and Molecular Rearrangements Due to the Primary Event in Vision
Gascon J, Batista V. QM/MM Study of Energy Storage and Molecular Rearrangements Due to the Primary Event in Vision. Biophysical Journal 2004, 87: 2931-2941. PMID: 15339806, PMCID: PMC1304767, DOI: 10.1529/biophysj.104.048264.Peer-Reviewed Original ResearchConceptsMolecular rearrangementQuantum mechanics/molecular mechanics (QM/MM) hybrid methodsEnergy storageQM/MM studyPolyene chainEnergy storage mechanismElectronic excitation energiesHigh-resolution structural dataBovine visual rhodopsinMolecular structureMM studyNet positive chargePrimary photochemical eventSchiff baseC13 positionSchiff base linkageStorage mechanismSteric interactionsTrans productsSteric constraintsPreferential senseFirst-principles understandingPositive chargePhotochemical eventsStructural data