【外文原著】Ultrafast Infrared Vibrational Spectroscopy.pdf
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【外文原著】Ultrafast Infrared Vibrational Spectroscopy.pdf
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ULTRAFASTINFRAREDVIBRATIONALSPECTROSCOPYEditedbyMICHAELD.FAYERFAYERULTRAFASTINFRAREDVIBRATIONALSPECTROSCOPYCRCPressisanimprintoftheTaylor&FrancisGroup,aninformabusinessBocaRatonLondonNewYorkULTRAFASTINFRAREDVIBRATIONALSPECTROSCOPYEditedbyMICHAELD.FAYERCRCPressTaylor&FrancisGroup6000BrokenSoundParkwayNW,Suite300BocaRaton,FL33487-27422013byTaylor&FrancisGroup,LLCCRCPressisanimprintofTaylor&FrancisGroup,anInformabusinessNoclaimtooriginalU.S.GovernmentworksVersionDate:
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/vContentsPreface.viiEditor.ixContributors.xiChapter1VibrationalEchoChemicalExchangeSpectroscopy.1MichaelD.FayerChapter2UltrafastVibrationalDynamicsofHydrogen-BondedDimersandBasePairs.35ThomasElsaesserChapter3WaterReorientationandUltrafastInfraredSpectroscopy.73DamienLaageandJamesT.HynesChapter4FemtosecondVibrationalSpectroscopyofAqueousSystems.99H.J.BakkerandM.BonnChapter5SolvationDynamicsofVibrationalStatesinHydrogen-BondingSolvents:
VibrationalFrequencyFluctuationsStudiedbytheThree-PulseInfraredPhotonEchoMethod.149KaoruOhta,JumpeiTayama,ShinjiSaito,andKeisukeTominagaChapter6PolarizationAnisotropyEffectsforDegenerateVibrationalLevels.169DanielG.KurodaandRobinM.HochstrasserChapter7Polarization-ControlledChiropticaland2DOpticalSpectroscopy.203Kyung-WonKwak,Kwang-HeePark,andMinhaengChoChapter8UltrafastInfraredProbesofElectronicProcessesinMaterials.239JohnB.AsburyChapter9VibrationalEnergyandMolecularThermometersinLiquids:
UltrafastIR-RamanSpectroscopy.269BrandtC.PeinandDanaD.DlottChapter10UltrafastProcessesatLiquidInterfacesInvestigatedwithTime-ResolvedSumFrequencyGeneration.305YiRao,BenjaminDoughty,NicholasJ.Turro,andKennethB.EisenthalviContentsChapter11EnergyTransportinMoleculesStudiedbyRelaxation-Assisted2DIRSpectroscopy.333IgorV.RubtsovChapter12AnIntroductiontoProtein2DIRSpectroscopy.361CarlosR.Baiz,MikeReppert,andAndreiTokmakoffChapter13Quasi-ParticleApproachto2DIRSpectraofVibrationalExcitonsinBiomolecules:
MolecularDynamicsversusStochasticSimulationProtocols.405CyrilFalvo,Frantiekanda,andShaulMukamelChapter14UltrafastInfraredSpectroscopyofAmylinSolutionandFibrils.437L.Wang,L.E.Buchanan,E.B.Dunkelberger,J.J.dePablo,M.T.Zanni,andJ.L.SkinnerviiPrefaceThedynamicaltimescalesassociatedwithmolecularmotionsareveryshort.MoleculescanrangeinsizefromwatertoproteinsandDNA.WhileproteinsandDNAarenotsmallmolecules,theyarecomposedofaminoacidsandnucleotides.Thesebuildingblocksareinessencesmallmolecules,andthepropertiesanddynamicsoflargebiologicalmoleculescandependonthemotionsanddynamicalinteractionsofthesmall-molecule-sizedsubunitsthat,liketheirsmallmoleculebreth-ren,areinherentlyveryfast.Ultrafastspectroscopyhasprovidedtoolsthatmakeitpossibletostudyveryfastmotionsofmolecularsystemsonthetimescalesonwhichtheyactuallyoccur.Initially,ultrafastlaserspectroscopywaslimitedtothevisibleandultravioletspectralregimesbecauseoftheavailablelasertechnology.Formanydecades,UV/Visultrafastexperimentshaveprovidedawealthofinformationbyexcitingandprobingmolecularelectronic-excitedstates.Overapproximatelythelastdecade,sourcesofultrafastinfrared(IR)pulseshavebecomeread-ilyavailable.TheIRregionofthespectrumcorrespondstoenergiesassociatedwithmolecularvibrations.Thevibrationalmodesarethemechanicaldegreesoffreedomofmolecules.Time-independentlinearIRabsorptionspectracanprovideavastamountofstructuralinformationaboutmolecules.Themid-IRisoftenreferredtoasthefingerprintregionbecausevibrationalabsorp-tionspectrainthisregionaresensitivetomolecularstructure,conformation,andenvironment.Inorganicchemistry,vibrationalspectraareoftenusedtoverifythepresenceofparticularsubstituentsandtodeterminetheconformations.Vibrationalspectraaresensitivetosmalldifferencesinstruc-ture.Forexample,asystemoflongalkylchainsboundtoagoldsurfacethatisalltranshasaslightlydifferentspectrumthanthesamesystemwithgauchedefects.Theadventoflaser-basedsourcesofultrafastIRpulseshasextendedthestudyofveryfastmoleculardynamicstotheobservationofprocessesmanifestedthroughtheireffectsonthevibra-tionsofmolecules.Inaddition,nonlinearIRspectroscopictechniquesmakeitpossibletoexamineintra-andintermolecularinteractionsandhowsuchinteractionsevolveonveryfasttimescales,butalsoinsomeinstancesonveryslowtimescales.ToseetheefficacyofusingIRexperimentstostudymoleculardynamicsandinteractions,itisusefultocompareandcontrastNMR,IR,andUV/Visexperiments.NMRspectraformoleculesinliquidshaveverysharplinesthatareexquisitelysensi-tivetostructure.Thesharpfeaturesofone-dimensional(1D)NMRspectraareaugmentedbytwo-dimensional(2D)andmultidimensionalmethodsandcomplexpulsesequencesthatmakeitpossibletopullapartdetailsofverycomplicatedspectraoflargemolecules,includingproteins.However,NMRinherentlyoperatesonslowtimescales.Directmeasurementsofdynamicsaregenerallylim-itedtomillisecondsandmuchlonger.Usinglineshapeanalysis,NMRcanprovideinformationonfasttimescales,butthesearehighlymodeldependent.IncontrasttotheexceedinglysharpfeaturesofNMRspectraofmoleculesinliquids,1DUV/Visabsorptionspectraofchromophoresinliquidsgenerallyareverybroadandalmostfeatureless.Verylimitedstructuralinformationisavailablefroma1Dspectrum.UltrafastUV/Visspectroscopydoespermitdirectmeasurementsofultrafastprocessesthatoccuronexcited-statepotentialsurfaces,suchasphotoinducedelectrontransferorthetranstocisisomerizationofstilbene.However,withtheexceptionofafewveryspecializedchromophoresystems,particularlyphotosyntheticchro-mophorecomplexes,UV/Vis2Dmethodsprovidelimitedimprovementinthemeasurementofthedetailsofstructuraldynamicsandinter-andintramolecularinteractions.NMRandUV/Visspectroscopiesareinsomesense-limitingextremes.NMRhasverysharpspectralfeaturesthatwithmultidimensionalmethodsandpulsesequencesgiveagreatdealofstruc-turalinformationbutcandirectlyinvestigatedynamicsonlyonslowtimescales.UV/VisspectraareviiiPrefaceverybroadandmainlyfeaturelessbutcanprovidedynamicalinformationofultrafasttimescalesusuallywithlimitedstructuraldetail.Vibrationalspectroscopybridgesthegap.Vibrational1Dabsorptionspectra,inmostcases,haverelativelysharplinesthatcanbeidentifiedwithspecificmolecularfunctionalgroups.Asmentionedabove,vibrationalspectraarequitesensitivetostructureandconformationalthoughnotnearlyassensitiveasNMR.Vibrationalexperimentscanbeperformedonultrafasttimescales.Thetypicalwavelengthofatimedomainvibrationalexperimentisabout10timeslongerthanaUV/Visexperiment,whichmeansthatvibrationalexperimentscannothavethetimeresolutionofUV/Visexperiments.However,time-dependentIRexperimentsareroutinelyconductedwithsubhundredfemtosecondtimeresolution,whichprovidessufficienttimeresolutiontostudymostmolecularprocesses.Theinverseofthevibrationallinewidthultimatelysetsthetimeresolutionnecessaryforadynamicalexperiment.Typicalvibrationallineshavelinewidthsoflessthanafewtensofwavenumbers(thehydroxylstretchofwaterisanimportantexception),whichsetsthefastestdynamicaltimescaleataboutapicosecond.Thetimeresolutionofmid-IRexperimentsismanyordersofmagnitudefasterthancanbeachievedwithNMR.Inaddition,therelativelysharpspectralfeaturesassociatedwithvibrationalspectramakethemamenabletotime-dependent2DexperimentsthatcanextractagreatdealofinformationthatisnotaccessiblebyeitherNMRorUV/Vismethods.Evenforphysicalproblemsthatinherentlyinvolveelectronic-excitedstates,combinedtime-dependentUV/VisIRexperimentscanprovideinformationnotreadilyascertain-ableinstraightUV/Visexperiments.Forexample,aUV/Visexcitationpulsecanb
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