2022
Ultrafast Charge Relocation Dynamics in Enol–Keto Tautomerization Monitored with a Local Soft-X-ray Probe
Soley M, Videla P, Nibbering E, Batista V. Ultrafast Charge Relocation Dynamics in Enol–Keto Tautomerization Monitored with a Local Soft-X-ray Probe. The Journal Of Physical Chemistry Letters 2022, 13: 8254-8263. PMID: 36018775, PMCID: PMC9465716, DOI: 10.1021/acs.jpclett.2c02037.Peer-Reviewed Original ResearchConceptsSoft X-ray probeSoft X-ray spectroscopyFull quantum treatmentPump-probe spectroscopyUltrafast time scaleQuantum treatmentHydrogen fuel cellsNuclear dynamicsElectronic excitationEnol-keto tautomerizationPCET mechanismOxygen reductionInterplay of protonsFrontier orbitalsWater splittingCharge relocationElectron transferElectronic structure rearrangementLocal excitationTautomerization reactionImportant reactionsFuel cellsElementary stepsChemical reactionsH atoms
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 densityPhotodissociationLineshape
2017
Charge Transport and Rectification in Donor–Acceptor Dyads
Hedström S, Matula A, Batista V. Charge Transport and Rectification in Donor–Acceptor Dyads. The Journal Of Physical Chemistry C 2017, 121: 19053-19062. DOI: 10.1021/acs.jpcc.7b05749.Peer-Reviewed Original ResearchFrontier orbitalsConjugated donor–acceptor systemA systemDensity functional theory levelDonor-acceptor dyadsDonor-acceptor systemsAppropriate transport propertiesGold electrodeA dyadsMolecular conformationTransport propertiesMolecular junctionsTheory levelRational designPhotovoltaic devicesCharge transportStructure-function relationshipsChemical compositionLarge rectification ratioOrbitalsFundamental physical insightsMolecular levelRectification propertiesRectification ratioFermi levelThermodynamic and Structural Factors That Influence the Redox Potentials of Tungsten–Alkylidyne Complexes
Rudshteyn B, Vibbert H, May R, Wasserman E, Warnke I, Hopkins M, Batista V. Thermodynamic and Structural Factors That Influence the Redox Potentials of Tungsten–Alkylidyne Complexes. ACS Catalysis 2017, 7: 6134-6143. DOI: 10.1021/acscatal.7b01636.Peer-Reviewed Original ResearchTungsten alkylidyne complexesRedox propertiesOxidation potentialGas-phase ionization energiesKey frontier orbitalsDensity functional theory levelX bond lengthsFree energy calculationsSolvation free energy differencesAlkylidyne ligandFrontier orbitalsHOMO energyFree energy differenceBond lengthsObserved linear correlationRedox potentialTheory levelEnergy calculationsIonization energyEnergy differenceComplexesStructural factorsElectrochemistryGood descriptorLinear correlation
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