2024
Spectroscopic Quantification of the Inverted Singlet–Triplet Gap in Pentaazaphenalene
Wilson K, Styers W, Wood S, Woods R, McMahon R, Liu Z, Yang Y, Garand E. Spectroscopic Quantification of the Inverted Singlet–Triplet Gap in Pentaazaphenalene. Journal Of The American Chemical Society 2024, 146: 15688-15692. PMID: 38815061, DOI: 10.1021/jacs.4c05043.Peer-Reviewed Original ResearchSinglet-triplet gapComputational electronic structure methodsInverted singlet-triplet gapAnion photoelectron spectroscopyExcited singlet stateDouble excitation characterElectronic structure methodsHund's multiplicity ruleVisible absorption spectroscopySpectroscopic quantificationArgon matrixLowest singletTriplet stateOrganic chromophoresSinglet stateExcitation characterAbsorption spectroscopyElectronic statesPhotoelectron spectroscopyStructure methodsSpectroscopyAccurate quantificationChromophoreSingletQuantification
2023
Active Sites of Cobalt Phthalocyanine in Electrocatalytic CO2 Reduction to Methanol
Rooney C, Lyons M, Wu Y, Hu G, Wang M, Choi C, Gao Y, Chang C, Brudvig G, Feng Z, Wang H. Active Sites of Cobalt Phthalocyanine in Electrocatalytic CO2 Reduction to Methanol. Angewandte Chemie International Edition 2023, 63: e202310623. PMID: 37820079, DOI: 10.1002/anie.202310623.Peer-Reviewed Original ResearchActive siteCobalt phthalocyanineSitu X-ray absorption spectroscopyX-ray absorption spectroscopy characterizationX-ray absorption spectroscopyElectrocatalytic CO2 reductionStructure-reactivity correlationsAbsorption spectroscopy characterizationElectrocatalytic measurementsMetal coordinationElectrocatalytic performanceCoordination environmentMolecular dispersionRelated porphyrinsCNT surfaceElectron transferAbsorption spectroscopyConductive carbonElectronic interactionsKey intermediateCO2 reductionPc macrocycleReaction mechanismSpectroscopy characterizationMethanol pathwayActive Sites of Cobalt Phthalocyanine in Electrocatalytic CO2 Reduction to Methanol
Rooney C, Lyons M, Wu Y, Hu G, Wang M, Choi C, Gao Y, Chang C, Brudvig G, Feng Z, Wang H. Active Sites of Cobalt Phthalocyanine in Electrocatalytic CO2 Reduction to Methanol. Angewandte Chemie 2023, 136 DOI: 10.1002/ange.202310623.Peer-Reviewed Original ResearchCO 2 reductionActive siteCobalt phthalocyanineSitu X-ray absorption spectroscopyX-ray absorption spectroscopy characterizationX-ray absorption spectroscopyElectrocatalytic CO2 reductionStructure-reactivity correlationsAbsorption spectroscopy characterizationCO 2 electroreductionCO 2Electrocatalytic measurementsCoordination environmentElectrocatalytic performanceMolecular dispersionRelated porphyrinsCNT surfaceElectron transferAbsorption spectroscopyConductive carbonElectronic interactionsKey intermediateCO2 reductionPc macrocycleReaction mechanismDominant Role of Hole Transport Pathway in Achieving Record High Photoconductivity in Two‐Dimensional Metal–Organic Frameworks
Wang D, Ostresh S, Streater D, He P, Nyakuchena J, Ma Q, Zhang X, Neu J, Brudvig G, Huang J. Dominant Role of Hole Transport Pathway in Achieving Record High Photoconductivity in Two‐Dimensional Metal–Organic Frameworks. Angewandte Chemie 2023, 135 DOI: 10.1002/ange.202309505.Peer-Reviewed Original ResearchTransient absorption spectroscopyX-ray transient absorption spectroscopyPhotoelectric devicesAbsorption spectroscopyOptical transient absorption spectroscopyTime-resolved terahertz spectroscopyHigh photoconductivityHole transport mechanismTwo-dimensional metalsElectron dynamicsDensity functional theory calculationsTerahertz spectroscopyElectronic statesFunctional theory calculationsMetal-organic frameworksPhotoconductivityTheory calculationsCharge transportMobile chargesSpectroscopyHole transport pathwaysCharge transport pathwaysDominant Role of Hole Transport Pathway in Achieving Record High Photoconductivity in Two‐Dimensional Metal–Organic Frameworks
Wang D, Ostresh S, Streater D, He P, Nyakuchena J, Ma Q, Zhang X, Neu J, Brudvig G, Huang J. Dominant Role of Hole Transport Pathway in Achieving Record High Photoconductivity in Two‐Dimensional Metal–Organic Frameworks. Angewandte Chemie International Edition 2023, 62: e202309505. PMID: 37872121, DOI: 10.1002/anie.202309505.Peer-Reviewed Original ResearchTransient absorption spectroscopyX-ray transient absorption spectroscopyPhotoelectric devicesAbsorption spectroscopyOptical transient absorption spectroscopyTime-resolved terahertz spectroscopyHigh photoconductivityHole transport mechanismTwo-dimensional metalsElectron dynamicsDensity functional theory calculationsTerahertz spectroscopyElectronic statesFunctional theory calculationsMetal-organic frameworksPhotoconductivityTheory calculationsCharge transportMobile chargesSpectroscopyHole transport pathwaysCharge transport pathways
2022
PM-IRRAS and DFT investigation of the surface orientation of new Ir piano-stool complexes attached to Au(111)
Miller C, Brunner F, Kelly H, Cheung P, Torquato N, Gembicky M, Okuno S, Chan T, Batista V, Kubiak C. PM-IRRAS and DFT investigation of the surface orientation of new Ir piano-stool complexes attached to Au(111). Dalton Transactions 2022, 51: 17688-17699. PMID: 36345597, DOI: 10.1039/d2dt02730e.Peer-Reviewed Original ResearchPiano-stool complexesPhenylpyridine ligandsPM-IRRASPolarization modulation infrared reflection absorption spectroscopyInfrared reflection absorption spectroscopySelf-assembled monolayersNew catalytic systemReflection absorption spectroscopyMinimum energy orientationMolecular catalystsOrganometallic catalystsCatalytic systemDFT calculationsSurface immobilizationDFT investigationAbsorption spectroscopyCatalystSurface mechanismBipyridineLigandsHeterogenous surfaceComplexesEnergy orientationSuch hybrid systemsSurface orientationMicrobial biofilms as living photoconductors due to ultrafast electron transfer in cytochrome OmcS nanowires
Neu J, Shipps CC, Guberman-Pfeffer MJ, Shen C, Srikanth V, Spies JA, Kirchhofer ND, Yalcin SE, Brudvig GW, Batista VS, Malvankar NS. Microbial biofilms as living photoconductors due to ultrafast electron transfer in cytochrome OmcS nanowires. Nature Communications 2022, 13: 5150. PMID: 36071037, PMCID: PMC9452534, DOI: 10.1038/s41467-022-32659-5.Peer-Reviewed Original ResearchConceptsUltrafast electron transferElectron transferPhotoconductive atomic force microscopyFemtosecond transient absorption spectroscopyQuantum dynamics simulationsMicrobial electron transferAtomic force microscopyTransient absorption spectroscopyValue-added chemicalsIndividual nanowiresWhole-cell catalysisPhotoconductive materialForce microscopyCarrier densityCatalytic performanceNanowiresAbsorption spectroscopyPhotoactive proteinsEfficient productionPhotoconductorsSynthetic photosensitizersDynamics simulationsGeobacter sulfurreducensBiodegradable materialsElectronic interfaceDe novo protein design of photochemical reaction centers
Ennist N, Zhao Z, Stayrook S, Discher B, Dutton P, Moser C. De novo protein design of photochemical reaction centers. Nature Communications 2022, 13: 4937. PMID: 35999239, PMCID: PMC9399245, DOI: 10.1038/s41467-022-32710-5.Peer-Reviewed Original ResearchConceptsCharge separationSolar-to-fuel energy conversionReaction centerLight-driven charge separationX-ray crystal structurePhotosynthetic reaction center proteinCharge separation lifetimeSolar fuel productionTransient absorption spectroscopyPhotosynthetic reaction centersPhotochemical charge separationModify natural proteinsPhotochemical reaction centerReaction center proteinCluster oxidationRedox centersCrystal structureAbsorption spectroscopyElectron transfer activityNatural protein structuresDe novo protein designPhotosynthetic protein complexesEnergy conversionX-rayProtein frameworkRevealing the Structure of Single Cobalt Sites in Carbon Nitride for Photocatalytic CO2 Reduction
Huang P, Huang J, Li J, Pham T, Zhang L, He J, Brudvig G, Deskins N, Frenkel A, Li G. Revealing the Structure of Single Cobalt Sites in Carbon Nitride for Photocatalytic CO2 Reduction. The Journal Of Physical Chemistry C 2022, 126: 8596-8604. DOI: 10.1021/acs.jpcc.2c01216.Peer-Reviewed Original ResearchPhotocatalytic CO2 reductionSingle CO2CO2 reductionCarbon nitrideX-ray absorption spectroscopyCo-N bond lengthsImproved catalytic propertiesSingle Cobalt SitesMode of coordinationMore edge sitesGraphitic carbon nitrideObserved enhancement effectMetal centerCatalytic propertiesC3N4 materialsAbsorption spectroscopyBond lengthsSpectroscopic toolsPhotocatalytic propertiesExcellent activityCobalt sitesEdge sitesC3N4 flakesBinding energiesLight absorption
2021
Tuning the Conduction Band for Interfacial Electron Transfer: Dye-Sensitized Sn x Ti1–x O2 Photoanodes for Water Splitting
Spies J, Swierk J, Kelly H, Capobianco M, Regan K, Batista V, Brudvig G, Schmuttenmaer C. Tuning the Conduction Band for Interfacial Electron Transfer: Dye-Sensitized Sn x Ti1–x O2 Photoanodes for Water Splitting. ACS Applied Energy Materials 2021, 4: 4695-4703. DOI: 10.1021/acsaem.1c00305.Peer-Reviewed Original ResearchDFT calculationsAbsorption spectroscopyInterfacial electron transfer dynamicsUltrafast transient absorption spectroscopyInterfacial electron transferElectron transfer dynamicsUltrafast electron injectionConduction bandPeriodic DFT calculationsTransient absorption spectroscopyLinear absorption spectroscopyDye sensitizersWater splittingElectron transferTransfer dynamicsComposition of SnElectron acceptorAbsorption spectraElectron injectionD characterElectronic statesSpectroscopyPhotoanodeSnDyePhotoinduced Charge Transport in Conductive Metal Organic Frameworks
Ostresh S, Nyakuchena J, Pattenale B, Neu J, Streater D, Fiankor C, Hu W, Kinigstein E, Zhang J, Zhang X, Schmuttenmaer C, Huang J, Brudvig G. Photoinduced Charge Transport in Conductive Metal Organic Frameworks. 2021, 00: 1-2. DOI: 10.1109/irmmw-thz50926.2021.9567551.Peer-Reviewed Original ResearchConductive metal-organic frameworksMetal-organic frameworksPhotocatalytic applicationsCharge transport mechanismOrganic frameworksPorous crystalline materialsCharge transportTerahertzCrystalline materialsTransport mechanismRational designPromising classConductivityApplicationsAbsorption spectroscopyTransient absorption spectroscopyMaterials
2020
Vibronic Dynamics of Photodissociating ICN from Simulations of Ultrafast X‐Ray Absorption Spectroscopy
Morzan U, Videla P, Soley M, Nibbering E, Batista V. Vibronic Dynamics of Photodissociating ICN from Simulations of Ultrafast X‐Ray Absorption Spectroscopy. Angewandte Chemie 2020, 132: 20219-20223. DOI: 10.1002/ange.202007192.Peer-Reviewed Original ResearchUltrafast X-ray absorption spectroscopySoft X-ray spectral regionSpectral regionDetailed dynamical informationX-ray absorption spectroscopyPhotodissociation of ICNProbe spectroscopyCoherent vibrationsProbe spectraUltrafast resolutionVibronic dynamicsExcited statesAtomic specificitySpectral lineshapesAbsorption spectroscopyDynamical informationCN fragmentsTime-domain signaturesPhotochemical processesFrontier orbitalsDirect insightSpectroscopyProbability densityPhotodissociationLineshapeHighly Diastereoselective Functionalization of Piperidines by Photoredox-Catalyzed α‑Amino C–H Arylation and Epimerization
Walker MM, Koronkiewicz B, Chen S, Houk KN, Mayer JM, Ellman JA. Highly Diastereoselective Functionalization of Piperidines by Photoredox-Catalyzed α‑Amino C–H Arylation and Epimerization. Journal Of The American Chemical Society 2020, 142: 8194-8202. PMID: 32286827, PMCID: PMC7318553, DOI: 10.1021/jacs.9b13165.Peer-Reviewed Original ResearchConceptsDensity functional theoryH arylation reactionTransient absorption spectroscopyArylation reactionFluorescent spectroscopic methodDiastereomer ratiosΑ-amino CElectron transfer processAbsorption spectroscopyMultiple substitution patternsFunctional theoryDiastereoselective functionalizationRelative energiesSlow epimerizationReaction conditionsSpectroscopic methodsH arylationPure productsGood yieldsSubstitution patternTransfer processObserved distributionHigh diastereoselectivityPiperidine derivativesRadical formation
2019
Vibronic Effects in the Ultrafast Interfacial Electron Transfer of Perylene-Sensitized TiO2 Surfaces
Oliboni R, Yan H, Fan H, Abraham B, Avenoso J, Galoppini E, Batista V, Gundlach L, Rego L. Vibronic Effects in the Ultrafast Interfacial Electron Transfer of Perylene-Sensitized TiO2 Surfaces. The Journal Of Physical Chemistry C 2019, 123: 12599-12607. DOI: 10.1021/acs.jpcc.9b02106.Peer-Reviewed Original ResearchVibronic effectsAbsorption spectraNonadiabatic quantum dynamics simulationsOptical gap decreasesUltrafast transient absorption spectroscopyUltrafast interfacial electron transferQuantum dynamics simulationsEnergy modesTransient absorption spectroscopyTransient absorption spectraQuantum dynamicsBroadband spectroscopyElectron transferVelocity autocorrelation functionClassical trajectoriesExcited statesEnergy shiftGap decreasesWide-band limitS1 stateElectronic populationAbsorption spectroscopyInterfacial electron transferCondon approximationNonequilibrium modes
2018
Direct Interfacial Electron Transfer from High-Potential Porphyrins into Semiconductor Surfaces: A Comparison of Linkers and Anchoring Groups
Jiang J, Spies J, Swierk J, Matula A, Regan K, Romano N, Brennan B, Crabtree R, Batista V, Schmuttenmaer C, Brudvig G. Direct Interfacial Electron Transfer from High-Potential Porphyrins into Semiconductor Surfaces: A Comparison of Linkers and Anchoring Groups. The Journal Of Physical Chemistry C 2018, 122: 13529-13539. DOI: 10.1021/acs.jpcc.7b12405.Peer-Reviewed Original ResearchMetal oxide surfacesDirect interfacial electron transferTime-resolved terahertzInterfacial electron transferOxide surfaceSemiconductor surfacesPhotoelectrochemical stabilitySnO2 substratePhotoelectrochemical cellsInjection yieldTransient spectroscopySurfaceAqueous photoelectrochemical cellDye photosensitizerIET dynamicsTerahertzElectron transferSeries of linkersDirect contactSpectroscopyAbsorption spectroscopyTransferTransient absorption spectroscopyOverall length
2017
Photodriven Oxidation of Surface-Bound Iridium-Based Molecular Water-Oxidation Catalysts on Perylene-3,4-dicarboximide-Sensitized TiO2 Electrodes Protected by an Al2O3 Layer
Kamire R, Materna K, Hoffeditz W, Phelan B, Thomsen J, Farha O, Hupp J, Brudvig G, Wasielewski M. Photodriven Oxidation of Surface-Bound Iridium-Based Molecular Water-Oxidation Catalysts on Perylene-3,4-dicarboximide-Sensitized TiO2 Electrodes Protected by an Al2O3 Layer. The Journal Of Physical Chemistry C 2017, 121: 3752-3764. DOI: 10.1021/acs.jpcc.6b11672.Peer-Reviewed Original ResearchMolecular water oxidation catalystsDye-sensitized photoelectrochemical cellsWater oxidation catalystsCharge transfer dynamicsSolar fuel productionCharge recombinationAtomic layer depositionHigher photocurrentTransfer dynamicsDye-sensitized TiO2 photoanodesFemtosecond transient absorption spectroscopyCharge transfer rateTransient absorption spectroscopyALD layersFuel productionDicarboximide chromophorePhotodriven oxidationMononuclear catalystsDinuclear catalystsCatalyst oxidationDye moleculesInitial charge injectionMolecular structurePhotoelectrochemical experimentsAbsorption spectroscopy
2016
High-Potential Porphyrins Supported on SnO2 and TiO2 Surfaces for Photoelectrochemical Applications
Jiang J, Swierk J, Materna K, Hedström S, Lee S, Crabtree R, Schmuttenmaer C, Batista V, Brudvig G. High-Potential Porphyrins Supported on SnO2 and TiO2 Surfaces for Photoelectrochemical Applications. The Journal Of Physical Chemistry C 2016, 120: 28971-28982. DOI: 10.1021/acs.jpcc.6b10350.Peer-Reviewed Original ResearchMetal oxide surfacesTiO2 surfaceTerahertz measurementsPhotoelectrochemical applicationsWater-splitting dye-sensitized photoelectrochemical cellsPhotoelectrochemical cellsOxide surfaceSnO2WS-DSPECsInterfacial electron transferDye-sensitized photoelectrochemical cellsSurfaceHigh potentialCharge recombination kineticsComputational modelingAbsorption spectroscopy
2015
Behavior of the Ru-bda Water Oxidation Catalyst Covalently Anchored on Glassy Carbon Electrodes
Matheu R, Francàs L, Chernev P, Ertem M, Batista V, Haumann M, Sala X, Llobet A. Behavior of the Ru-bda Water Oxidation Catalyst Covalently Anchored on Glassy Carbon Electrodes. ACS Catalysis 2015, 5: 3422-3429. DOI: 10.1021/acscatal.5b00132.Peer-Reviewed Original ResearchWater oxidation catalystsX-ray absorption spectroscopyElectrode surfaceHybrid materialsGlassy carbonOxidation catalystHeterogeneous water oxidation catalystsGC electrode surfaceGlassy carbon electrodeRu-aqua complexesLow catalytic performanceOxidation of waterNew hybrid materialsGC electrodeElectrochemical reductionCarbon electrodeCovalent graftingActive catalystGood electrocatalystCatalytic performanceVoltammetric experimentsElectrochemical techniquesMetal oxidesAbsorption spectroscopyMolecular complexes
2011
Thermal stability of [Mn(III)(O)2Mn(IV)(H2O)2(Terpy)2](NO3)3 (Terpy=2,2′:6′,2″-terpyridine) in aqueous solution
Zhang F, Cady C, Brudvig G, Hou H. Thermal stability of [Mn(III)(O)2Mn(IV)(H2O)2(Terpy)2](NO3)3 (Terpy=2,2′:6′,2″-terpyridine) in aqueous solution. Inorganica Chimica Acta 2011, 366: 128-133. DOI: 10.1016/j.ica.2010.10.021.Peer-Reviewed Original ResearchOxo dimerMn4Ca clusterAqueous solutionThermal stabilitySolar fuel productionOxygen evolution activityFirst fast stepMn valence changeAtomic absorption spectroscopyCatalytic materialsElemental analysisPS IIManganese dioxideAbsorption spectroscopyConversion of waterNovel MnDimer compoundsMn valenceSlow stepFast stepSolid MnThermal decompositionValence changeUnique materialFuel production
2001
Ultrafast lasers and x-ray absorption spectroscopy in chemical research: observing molecular structures of solvated molecules
Rose-Petruck C, Jiang Y, Li W, Cao G, Lee T, Ketwaroo G, Rose-Petruck C. Ultrafast lasers and x-ray absorption spectroscopy in chemical research: observing molecular structures of solvated molecules. 2001, tud3. DOI: 10.1364/hfsw.2001.tud3.Peer-Reviewed Original Research
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