pump-probespectraandnucleardynamicsforadissipativemolecularsysteminastronglaserfieldpredissociationdynamics》

pump-probespectraandnucleardynamicsforadissipativemolecularsysteminastronglaserfieldpredissociationdynamics》

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1、31July1998ChemicalPhysicsLetters292199828±34.Pump-probespectraandnucleardynamicsforadissipativemolecularsysteminastronglaserfield:predissociationdynamicsYutakaMaruyama,YoshitakaTanimuraTheGraduateUniÍersityforAdÍancedStudiesandInstituteforMolecularScience,Myodaiji,Okazaki444-8585,JapanReceiv

2、ed28April1998;infinalform14May1998AbstractThepredissociationdynamicsofamolecularsystemunderastronglaserfieldinthecondensedphaseisinvestigatedbydirectnumericalintegrationofthemulti-statequantumFokker-Planckequation.Numericalcalculationsofprobeabsorptionspectradrivenbyastrongpumppulsearepresent

3、ed,anddiscussed.TheresultsshowdynamicalStarksplitting,but,incontrasttotheBlochequationswhichcontainaninfinite-temperaturedephasing,wefindthatatfinitetemperaturestheirpeakshavedifferentheightsevenwhenthepumppulseisonresonance.Furthermoreweobservetheeffectofthediabaticcouplingbetweenexcitedandd

4、issociativestatesasthepeaksonthespectra.q1998PublishedbyElsevierScienceB.V.Allrightsreserved.1.Introductionmulti-stateFokker-PlanckequationforaGaussian-Markoviannoisebath9,10.TheresultsshowedthewxProgressinultrafastexperimentaltechniquespro-effectoffinitetemperatureaswellasanharmonicitypelnot

5、onlythelinearbutalsothenonlinearspec-ofapotential,whichwouldnotbeobtainedfromthetroscopy,whichprovideadirectmeansforstudyingopticalBlochequation11,12orthestochasticLiou-wxnucleardynamicsinthecondensedphase.Furthervilleequation13approach.Inthispaper,weinves-wxthelasertechniquesbecometoallowhig

6、hintensitytigatetheprobeabsorptionspectraforaMorsepo-andshortpulse.Oneofthecentralquestionsistentialssystemwithadissociativestateinastrongwhethertheinteractionbetweenthehigh-intensitylaserfield.Ouraimistoobservetheeffectofelectromagneticfieldandthemoleculegivesrisetodiabaticcouplingbetweenthe

7、excitedanddissocia-newphenomenawhichdonotoccurunder``normal''tivestatesunderthestronglaserfield.conditions,i.e.lowintensitiesandlargepulsedura-tions1±4.wxOntheotherhand,thepredissociation,causedby2.Pump-probespectroscopycurvecrossingbetweenbo

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