2008
Quantum 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 attack
2006
Molecular Recognition in the Selective Oxygenation of Saturated C-H Bonds by a Dimanganese Catalyst
Das S, Incarvito CD, Crabtree RH, Brudvig GW. Molecular Recognition in the Selective Oxygenation of Saturated C-H Bonds by a Dimanganese Catalyst. Science 2006, 312: 1941-1943. PMID: 16809537, DOI: 10.1126/science.1127899.Peer-Reviewed Original ResearchConceptsHydrogen bondingMolecular recognitionH bondsCarboxylic acid groupsMolecular recognition elementsSynthetic catalystsSaturated CKemp's triacidSelective oxygenationCOOH groupRegioselective functionalizationH activationHigh selectivityAcid groupsRecognition groupReactive centerRecognition elementCatalystTriacidOrient substratesSelectivityBondingBondsControl experimentsSubstrate
2005
New Linear High-Valent Tetranuclear Manganese-Oxo Cluster Relevant to the Oxygen-Evolving Complex of Photosystem II with Oxo, Hydroxo, and Aqua Coordinated to a Single Mn(IV)
Chen, Collomb M, Duboc C, Blondin G, Rivière E, Faller J, Crabtree R, Brudvig G. New Linear High-Valent Tetranuclear Manganese-Oxo Cluster Relevant to the Oxygen-Evolving Complex of Photosystem II with Oxo, Hydroxo, and Aqua Coordinated to a Single Mn(IV). Inorganic Chemistry 2005, 44: 9567-9573. PMID: 16323946, DOI: 10.1021/ic051462m.Peer-Reviewed Original ResearchConceptsGround stateSpin statesFirst excited spin stateExcited spin statesSpin-triplet stateLarge energy gapOxygen-Evolving ComplexMn–Mn distanceDiamagnetic ground stateEnergy gapVariable-temperature magnetic susceptibility dataX-ray powder diffractionTriplet stateMagnetic susceptibility dataTetranuclear manganeseMnIV ionsConstruction and Characterization of Genetically Modified Synechocystis sp. PCC 6803 Photosystem II Core Complexes Containing Carotenoids with Shorter π-Conjugation than β-Carotene*
Bautista J, Tracewell C, Schlodder E, Cunningham F, Brudvig G, Diner B. Construction and Characterization of Genetically Modified Synechocystis sp. PCC 6803 Photosystem II Core Complexes Containing Carotenoids with Shorter π-Conjugation than β-Carotene*. Journal Of Biological Chemistry 2005, 280: 38839-38850. PMID: 16159754, DOI: 10.1074/jbc.m504953200.Peer-Reviewed Original ResearchMeSH KeywordsBeta CaroteneCarotenoidsCationsChlorophyllChromatographyChromatography, High Pressure LiquidElectronsGene DeletionLightManganeseModels, ChemicalModels, MolecularMutationOxidation-ReductionOxidoreductasesOxygenPhotosynthetic Reaction Center Complex ProteinsPhotosystem II Protein ComplexPigmentationRhodobacter capsulatusSpectrophotometrySpectrophotometry, InfraredSynechocystisTemperatureTime FactorsTyrosineConceptsPhytoene desaturase geneII core complexesDesaturase genePS II core complexesSynechocystis spCore complexPS II assemblyCarotene desaturase genePhotosystem II core complexPCC 6803Rhodobacter capsulatusWild typeMutant strainRedox functionPhotosystem IISecondary electron transfer pathwayGenesElectron transfer pathwayLight-induced formationCarotenoidsSpChlorophyllConjugated pi-electron systemPathwayComplexesHigh‐Spin Chloro Mononuclear MnIII Complexes: A Multifrequency High‐Field EPR Study
Mantel C, Chen H, Crabtree R, Brudvig G, Pécaut J, Collomb M, Duboc C. High‐Spin Chloro Mononuclear MnIII Complexes: A Multifrequency High‐Field EPR Study. ChemPhysChem 2005, 6: 541-546. PMID: 15799481, DOI: 10.1002/cphc.200400484.Peer-Reviewed Original ResearchConceptsElectronic propertiesLigand field strengthHigh-Field EPR StudyPorphyrinic systemsTridentate ligandMnIII complexesDistorted octahedronLigands decreasesSolid stateJahn-Teller distortionPrevious complexesStructural characterizationCrystallographic dataEPR studiesMultifrequency EPRManganese ionsComplexesOctahedraTetragonal distortionE termDifferent temperaturesAnionsEPRLigandsProperties
2001
Carotenoid Photooxidation in Photosystem II
Tracewell C, Vrettos J, Bautista J, Frank H, Brudvig G. Carotenoid Photooxidation in Photosystem II. Archives Of Biochemistry And Biophysics 2001, 385: 61-69. PMID: 11361027, DOI: 10.1006/abbi.2000.2150.Peer-Reviewed Original ResearchConceptsPhotosystem IIElectron transfer reactionsPhotosynthetic reaction centersWater oxidationLight-harvesting pigmentsCarotenoid cationOxidizing intermediatesElectron transferRedox roleBacterial photosynthesisReaction centersPhysical methodsCationsPhotooxidationCarotenoid compositionRedoxOxidationIntermediatesAlternate pathwayCarotenoidsMinireviewReactionPhotoprotectionPossible rolePigmentsMechanism of photosynthetic water oxidation: combining biophysical studies of photosystem II with inorganic model chemistry
Vrettos J, Limburg J, Brudvig G. Mechanism of photosynthetic water oxidation: combining biophysical studies of photosystem II with inorganic model chemistry. Biochimica Et Biophysica Acta 2001, 1503: 229-245. PMID: 11115636, DOI: 10.1016/s0005-2728(00)00214-0.Peer-Reviewed Original ResearchMeSH KeywordsCrystallographyElectron TransportHemerythrinHydrogen-Ion ConcentrationKineticsManganeseModels, ChemicalModels, MolecularOrganometallic CompoundsOxidation-ReductionOxygenPhotosynthesisPhotosynthetic Reaction Center Complex ProteinsPhotosystem II Protein ComplexProtonsThylakoidsTyrosineWaterConceptsPhotosynthetic water oxidationWater oxidationOxygen-evolving complexProton-coupled electron transferTetranuclear manganese clusterMu-oxo bridgePhotosystem IIReduction of manganeseOOH speciesWater moleculesElectron transferModel chemistryManganese clusterNucleophilic attackDiferric siteFerric hydroperoxideOxidationD1 polypeptideBiophysical studiesOxyhemerythrinBiophysical resultsStructural modelDioxygenChemistryProtonation
1999
Competitive Binding of Acetate and Chloride in Photosystem II †
Kühne H, Szalai V, Brudvig G. Competitive Binding of Acetate and Chloride in Photosystem II †. Biochemistry 1999, 38: 6604-6613. PMID: 10350479, DOI: 10.1021/bi990341t.Peer-Reviewed Original ResearchA Functional Model for O-O Bond Formation by the O2-Evolving Complex in Photosystem II
Limburg J, Vrettos J, Liable-Sands L, Rheingold A, Crabtree R, Brudvig G. A Functional Model for O-O Bond Formation by the O2-Evolving Complex in Photosystem II. Science 1999, 283: 1524-1527. PMID: 10066173, DOI: 10.1126/science.283.5407.1524.Peer-Reviewed Original ResearchConceptsMolecular oxygenPhotosystem IIO bond formationPhotosynthetic water oxidationWater oxidationManganese dimerBond formationOxygen atomsActive siteIsotope labelingManganese ionsOxygenPhotosynthesisWaterSodium hypochloriteOxidationIonsFormationAtomsDimersComplexesO2Functional modelConversionHypochlorite
1998
Catalase-Free Photosystem II: The O2-Evolving Complex Does Not Dismutate Hydrogen Peroxide †
Sheptovitsky Y, Brudvig G. Catalase-Free Photosystem II: The O2-Evolving Complex Does Not Dismutate Hydrogen Peroxide †. Biochemistry 1998, 37: 5052-5059. PMID: 9548736, DOI: 10.1021/bi972872s.Peer-Reviewed Original Research
1996
Formation and Decay of the S3 EPR Signal Species in Acetate-Inhibited Photosystem II †
Szalai V, Brudvig G. Formation and Decay of the S3 EPR Signal Species in Acetate-Inhibited Photosystem II †. Biochemistry 1996, 35: 1946-1953. PMID: 8639678, DOI: 10.1021/bi952378t.Peer-Reviewed Original Research
1995
Spectroscopic evidence for the symmetric location of tyrosines D and Z in photosystem II.
Koulougliotis D, Tang X, Diner B, Brudvig G. Spectroscopic evidence for the symmetric location of tyrosines D and Z in photosystem II. Biochemistry 1995, 34: 2850-6. PMID: 7893698, DOI: 10.1021/bi00009a015.Peer-Reviewed Original Research
1994
Location of chlorophyllZ in photosystem II.
Koulougliotis D, Innes J, Brudvig G. Location of chlorophyllZ in photosystem II. Biochemistry 1994, 33: 11814-22. PMID: 7918399, DOI: 10.1021/bi00205a018.Peer-Reviewed Original ResearchBacteriochlorophyllsChlorophyllCold TemperatureCyanidesDarknessDysprosiumEdetic AcidElectron Spin Resonance SpectroscopyIronLightLight-Harvesting Protein ComplexesManganeseMicrowavesModels, ChemicalOxidation-ReductionPhotosynthetic Reaction Center Complex ProteinsPhotosystem II Protein ComplexSpinacia oleracea
1986
Mechanism for photosynthetic O2 evolution.
Brudvig G, Crabtree R. Mechanism for photosynthetic O2 evolution. Proceedings Of The National Academy Of Sciences Of The United States Of America 1986, 83: 4586-4588. PMID: 3460059, PMCID: PMC323785, DOI: 10.1073/pnas.83.13.4586.Peer-Reviewed Original ResearchConceptsO2-evolving complexManganese complexesPhotosynthetic O2 evolutionS2 stateCubane-like complexCubane-like structureIntermediate oxidation statesEPR spectral dataO2 evolutionSpectral dataDisplacement of O2Coordination chemistryOxidation stateO bondS4 stateRecent EPRUV spectral dataManganese sitesStructural conversionComplexesMolecular mechanismsMn4O4ChemistryStructureEPR
1979
Structure of cytochrome a3-Cua3 couple in cytochrome c oxidase as revealed by nitric oxide binding studies.
Stevens T, Brudvig G, Bocian D, Chan S. Structure of cytochrome a3-Cua3 couple in cytochrome c oxidase as revealed by nitric oxide binding studies. Proceedings Of The National Academy Of Sciences Of The United States Of America 1979, 76: 3320-3324. PMID: 226967, PMCID: PMC383817, DOI: 10.1073/pnas.76.7.3320.Peer-Reviewed Original Research