2024
Photoinduced Surface Oxidation of GaN Nanowires Facilitates Hydrogen Evolution
Menzel J, Dong W, Gruszecki E, Yang K, Mi Z, Batista V. Photoinduced Surface Oxidation of GaN Nanowires Facilitates Hydrogen Evolution. ACS Catalysis 2024, 14: 13314-13323. DOI: 10.1021/acscatal.4c00308.Peer-Reviewed Original ResearchHydrogen evolutionDensity functional theoryEffect of surface oxidationGaN NWsSurface oxidationPhotocatalytic hydrogen evolutionWater oxidation capabilityPhotoelectrochemical hydrogen evolutionLinear sweep voltammetrySolar energy storageCatalytic performanceGallium nitride nanowiresPhotocatalytic surfacesWater oxidationLight irradiationSweep voltammetryGallium oxynitrideFunctional theoryChronoamperometric measurementsElectronic structureValence band edge statesOxide surfaceAdsorbed hydroxideOxidation capabilityNitride nanowiresModeling Electrochemical Vacancy Regeneration in Single-Walled Carbon Nanotubes
Jelušić J, Menzel J, Bertrand Q, Crabtree R, Wang H, Brudvig G, Batista V. Modeling Electrochemical Vacancy Regeneration in Single-Walled Carbon Nanotubes. The Journal Of Physical Chemistry Letters 2024, 15: 7788-7792. PMID: 39048317, DOI: 10.1021/acs.jpclett.4c01293.Peer-Reviewed Original ResearchProton-coupled electron transferDensity functional theorySingle-walled carbon nanotubesC-H bondsQuantum mechanics/molecular mechanicsDiverse catalytic reactionsCarbene characterCarbon nanotubesC-HAdjacent carbonWater dissociationElectron transferCatalytic reactionsCatalytic intermediatesFunctional theoryHydrogen atomsKetone groupForce-fieldCarbon atomsHydroxyl groupsElectrochemical regenerationZigzag single-walled carbon nanotubesElectrochemical potentialKetonesVacancy defectsA Resilient Platform for the Discrete Functionalization of Gold Surfaces Based on N‑Heterocyclic Carbene Self-Assembled Monolayers
Palasz J, Long Z, Meng J, Videla P, Kelly H, Lian T, Batista V, Kubiak C. A Resilient Platform for the Discrete Functionalization of Gold Surfaces Based on N‑Heterocyclic Carbene Self-Assembled Monolayers. Journal Of The American Chemical Society 2024, 146: 10489-10497. PMID: 38584354, DOI: 10.1021/jacs.3c14113.Peer-Reviewed Original ResearchN-heterocyclic carbeneSelf-assembled monolayersCalculations of vibrational spectraAu(I) complexesLigand exchange reactionFunctionalization of gold surfacesX-ray photoelectron spectroscopyDensity functional theoryExperimental spectroscopic signaturesSurface-enhanced Raman spectroscopyVibrational spectraBinding geometryFunctional theoryBinding modePhotoelectron spectroscopyExchange reactionGold surfaceOn-surfaceSpectroscopic signaturesRaman spectroscopyX-rayAmbient conditionsCarbeneSpectroscopyAcid-base
2022
Binding of the substrate analog methanol in the oxygen-evolving complex of photosystem II in the D1-N87A genetic variant of cyanobacteria
Kalendra V, Reiss KM, Banerjee G, Ghosh I, Baldansuren A, Batista VS, Brudvig GW, Lakshmi KV. Binding of the substrate analog methanol in the oxygen-evolving complex of photosystem II in the D1-N87A genetic variant of cyanobacteria. Faraday Discussions 2022, 234: 195-213. PMID: 35147155, DOI: 10.1039/d1fd00094b.Peer-Reviewed Original ResearchConceptsOxygen-evolving complexDensity functional theorySolar water-splitting protein complexTwo-dimensional hyperfine sublevel correlation spectroscopyPhotosystem IIQuantum mechanics/molecular mechanicsHyperfine sublevel correlation spectroscopyWater oxidation reactionWater oxidationCatalytic clustersOxidation reactionSubstrate waterMolecular mechanicsCorrelation spectroscopyFunctional theorySubstrate analoguesLight energyMethanolComplexesReactionIntermediatesDetailed mechanismCatalystSpectroscopyWater
2018
Water-Nucleophilic Attack Mechanism for the CuII(pyalk)2 Water-Oxidation Catalyst
Rudshteyn B, Fisher K, Lant H, Yang K, Mercado B, Brudvig G, Crabtree R, Batista V. Water-Nucleophilic Attack Mechanism for the CuII(pyalk)2 Water-Oxidation Catalyst. ACS Catalysis 2018, 8: 7952-7960. DOI: 10.1021/acscatal.8b02466.Peer-Reviewed Original ResearchKinetic isotope effectsWater nucleophilic attack mechanismWater oxidation catalystsWater nucleophilic attackD Kinetic Isotope EffectO bond formationUV-visible spectraDensity functional theoryElectrochemical stepWater oxidationElectrochemical analysisTurnover frequencyDerivative complexesBond formationRadical speciesRational designCis formFunctional theoryIsotope effectRate-limiting stepCatalystComplexesAttack mechanismMechanistic findingsDeprotonationDopant-Dependent SFG Response of Rhenium CO2 Reduction Catalysts Chemisorbed on SrTiO3 (100) Single Crystals
Ge A, Videla P, Rudshteyn B, Liu Q, Batista V, Lian T. Dopant-Dependent SFG Response of Rhenium CO2 Reduction Catalysts Chemisorbed on SrTiO3 (100) Single Crystals. The Journal Of Physical Chemistry C 2018, 122: 13944-13952. DOI: 10.1021/acs.jpcc.8b01123.Peer-Reviewed Original ResearchDensity functional theorySFG responseVibrational sum frequency generation spectroscopySum frequency generation spectroscopyCO2 reduction catalystsFrequency generation spectroscopySrTiO3 single crystalsSTO surfaceReduction catalystDFT calculationsSFG resultsGeneration spectroscopySingle crystalsMolecular probesElectronic structureFunctional theoryCl atomsMetallic natureConduction bandSubstrateSurfaceCrystalsCatalystSpectroscopyFac
2017
Inferring Protonation States of Hydroxamate Adsorbates on TiO2 Surfaces
Rudshteyn B, Negre C, Oliboni R, Monti A, Chen J, Crabtree R, Rego L, Batista V. Inferring Protonation States of Hydroxamate Adsorbates on TiO2 Surfaces. The Journal Of Physical Chemistry C 2017, 121: 11985-11990. DOI: 10.1021/acs.jpcc.7b01272.Peer-Reviewed Original ResearchDensity functional theoryRed-shifted spectraSimulation of UVAbsorption measurementsBinding calculationsMolecular adsorbatesBinding HamiltonianFunctional theoryProtonation stateChanges of pKMain adsorption modeExperimental measurementsSemiconductor electrode surfaceSpectraAdsorbatesUVTiO2 surfaceSpectroscopic methodsTiO2 anataseMeasurements
2016
Ab initio tensorial electronic friction for molecules on metal surfaces: Nonadiabatic vibrational relaxation
Maurer R, Askerka M, Batista V, Tully J. Ab initio tensorial electronic friction for molecules on metal surfaces: Nonadiabatic vibrational relaxation. Physical Review B 2016, 94: 115432. DOI: 10.1103/physrevb.94.115432.Peer-Reviewed Original ResearchMetal surfaceElectronic frictionElectron-hole pair excitationsVibrational relaxationDensity functional theoryMolecular adsorbatesNonadiabatic coupling matrix elementsCoupling matrix elementsVibrational relaxation rateFunctional theoryAtomic orbital basis setsBasis setKohn-Sham density functional theoryEnergy transferAdsorbatesDiatomic moleculesPair excitationsMoleculesRelaxation rateTensorial propertiesSurfaceExperimental findingsChemistryFriction tensorCOOrientation of Cyano-Substituted Bipyridine Re(I) fac-Tricarbonyl Electrocatalysts Bound to Conducting Au Surfaces
Clark M, Rudshteyn B, Ge A, Chabolla S, Machan C, Psciuk B, Song J, Canzi G, Lian T, Batista V, Kubiak C. Orientation of Cyano-Substituted Bipyridine Re(I) fac-Tricarbonyl Electrocatalysts Bound to Conducting Au Surfaces. The Journal Of Physical Chemistry C 2016, 120: 1657-1665. DOI: 10.1021/acs.jpcc.5b10912.Peer-Reviewed Original ResearchSum frequency generation spectroscopyGold surfaceAu surfaceCO2 reduction catalystsFrequency generation spectroscopyReduction of CO2Density functional theoryMolecular catalystsReduction catalystBipyridine ligandsElectrochemical experimentsGeneration spectroscopyCatalytic turnoverSFG spectraElectrocatalystsFunctional theoryCatalystWeak bindingTheoretical methodsSurfaceBipyridineCatalysisSpectroscopyLigandsTriply
2014
Single Molecule Rectification Induced by the Asymmetry of a Single Frontier Orbital
Ding W, Negre C, Vogt L, Batista V. Single Molecule Rectification Induced by the Asymmetry of a Single Frontier Orbital. Journal Of Chemical Theory And Computation 2014, 10: 3393-3400. PMID: 26588307, DOI: 10.1021/ct5004687.Peer-Reviewed Original ResearchDye-sensitized solar cellsFrontier orbitalsDensity functional theoryInterfacial electron transferLow bias potentialNonequilibrium Green's function formalismMolecular assembliesElectron transferElectronic rectificationOrbital leadsFunctional theoryCharge transportFermi levelBias potentialSolar cellsOrbitalsSimple design principlesElectron densityTransport propertiesSuppress recombinationFunction formalismDesign principlesAsymmetric characterGreen's function formalismDominant contribution
2013
Photoinduced Proton Coupled Electron Transfer in 2‑(2′-Hydroxyphenyl)-Benzothiazole
Luber S, Adamczyk K, Nibbering E, Batista V. Photoinduced Proton Coupled Electron Transfer in 2‑(2′-Hydroxyphenyl)-Benzothiazole. The Journal Of Physical Chemistry A 2013, 117: 5269-5279. PMID: 23718689, DOI: 10.1021/jp403342w.Peer-Reviewed Original ResearchExcited-state intramolecular proton transferElectron transferState intramolecular proton transferTime-dependent density functional theoryQuantum chemical modelingIR-probe spectroscopyIntramolecular proton transferConjugated double bondsDensity functional theoryEnol-keto tautomerizationPhotoinduced ProtonBenzothiazole ringNonpolar solventsProton transferChemical modelingMid-infrared spectroscopyMolecular chromophoresMarker modesPrototypical moleculeDouble bondElectronic changesIsomerization dynamicsElectronic chargeFunctional theoryBenzothiazole
2012
Reduction of Systematic Uncertainty in DFT Redox Potentials of Transition-Metal Complexes
Konezny S, Doherty M, Luca O, Crabtree R, Soloveichik G, Batista V. Reduction of Systematic Uncertainty in DFT Redox Potentials of Transition-Metal Complexes. The Journal Of Physical Chemistry C 2012, 116: 6349-6356. DOI: 10.1021/jp300485t.Peer-Reviewed Original ResearchTransition metal complexesRedox potentialActive transition metal complexesThird-row transition metal complexesCyclic voltammetry measurementsDensity functional theoryNew electrocatalystsRedox propertiesRedox coupleVoltammetry measurementsWorking electrodesElectrochemical measurementsNonaqueous solventsCatalytic mechanismFunctional theorySolventComplexesInternal referenceQuantitative theoretical predictionTypical experimental errorsExperimental conditionsElectrocatalystsElectrolyteElectrodeExperimental error
2011
The O–H Stretching Mode of a Prototypical Photoacid as a Local Dielectric Probe
Prémont-Schwarz M, Xiao D, Batista V, Nibbering E. The O–H Stretching Mode of a Prototypical Photoacid as a Local Dielectric Probe. The Journal Of Physical Chemistry A 2011, 115: 10511-10516. PMID: 21851092, DOI: 10.1021/jp207642k.Peer-Reviewed Original ResearchDensity functional theoryFemtosecond mid-infrared spectroscopySolvatochromic effectH stretching modeB3LYP/TZVPVibrational frequency shiftsMid-infrared spectroscopyNuclear rearrangementsFrequency shiftPerturbative approachFunctional theoryDielectric responseStretching modeDielectric probeTZVP levelTheoretical modelPhotoacidSpectroscopyTZVPStateChromophoreTheoryProbeAgreementMode
2006
Density Functional Theory and DFT+U Study of Transition Metal Porphines Adsorbed on Au(111) Surfaces and Effects of Applied Electric Fields
Leung K, Rempe S, Schultz P, Sproviero E, Batista V, Chandross M, Medforth C. Density Functional Theory and DFT+U Study of Transition Metal Porphines Adsorbed on Au(111) Surfaces and Effects of Applied Electric Fields. Journal Of The American Chemical Society 2006, 128: 3659-3668. PMID: 16536538, DOI: 10.1021/ja056630o.Peer-Reviewed Original ResearchDensity functional theoryPorphine moleculeTransition metal ion complexesFunctional theoryMetal ion complexesLow-spin ground stateIon spin statesSpin-state orderingIon complexesGold substrateSubstituted porphyrinsDFT calculationsErnzerhof (PBE) exchange correlationCovalent bondingUseful general methodApplied Electric FieldPorphine macrocycleD electronsState orderingPerdew-BurkeAdsorptionMagnetic propertiesExchange correlationSpin statesMn d electrons