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1、FundamentalsofVibronicSpectroscopyJohnA.ShelnuttDepartmentofChemistryUniversityofGeorgiaAthens,GA30602-2556March6,2013Copyright?2008-2013byJohnA.Shelnutt.Allrightsreserved.FundamentalsofVibronicSpectroscopy2PREFACEThisisacoursedevotedtothedevelopmentofatheoreticalformal
2、ismthatcanbeusedgenerallytodescribetheinteractionbetweenaradiationfield(e.g.,light)andacollectionofchargedparticles(e.g.,molecules).Energymeasurementsonsuchasystem,e.g.,amoleculeinteractingwithlight,constitutethepursuitofmostspectroscopictechniques.Ingeneral,theradiatio
3、nfieldcanbeelectromagneticradiationconsistingof?-rays,X-rays,UV-visible-NIRlight,infraredlight,microwaves,radiowaves,orotherparticlefields.However,wewilllimitourselvestophotonfieldsinthistext.Thecollectionofparticlescanbeassmallasasinglechargedparticle,oraslargeasamolec
4、uleorcondensedmattersuchasacrystaloranamorphoussolid.Thespectroscopicmeasurementprocessisgenerallyanefforttodetectthenumberofphotons(intensity)oflightasafunctionofthephotonenergyE=h?(or,equivalently,thefrequencyorwavelength)ofthephotonsleavingtheinteractionregion.Thissp
5、ectroscopicinformation(i.e.,theenergyspectrum)isgenerallyusedtoobtaininformationaboutthesystemofparticlesbeingprobedbytheradiationfield.(e.g.,molecularinformation)Focusingonmolecularspectroscopy,wewillfirstdevelopageneralformalismthatisadequateforadescriptionofmostspect
6、roscopicmethods.Mostconventionalspectroscopictextspresentanassortmentofdifferentformalismscomprisingadifferentapproachforeachtypeofspectra.Instead,hereinwedevelopageneralformalismthatcanbeappliedinageneralway.Inaddition,thistheoreticalapproachissubjecttofewlimitationson
7、itsapplicabilityandcanbeusedtoactuallycalculatemolecularspectrainmostcases.Wewillapplythisapproachinparticulartovibrationalspectra(infraredandRamanspectra)andtoelectronicspectrawhenvibrationalstructureisevidentintheopticalabsorptionandresonanceRamanexcitationspectra.Oth
8、erspectroscopictechniqueswillalsobediscussedinlessdetail,butthemethodsforapplyingthetheoreticaltreatmenttothes
