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1、Quantumtheoryofdiffusion-acceleratedremotetransferA.B.DoktorovandA.I.BurshtelnInstituteofChemicalKineticsandCombustion,SiberianBranch,USSRAcademyofSciences(SubmittedSeptemberII,1974)Zh.Eksp.Teor.Fiz,68,1349-1362(April1975)Atheoryofremotequenchingofexcitedmoleculesinencounterswithaquenchin
2、gimpurityisconstructedwhichallowsaconsistentdescriptionofthecourseoftheelementaryenergy-transferevent.Thequenchingrateconstantforan(exchange)interactionthatdecreasesexponentiallywithdistanceiscomputed.Itisestablishedthatqualitativedeviationsfromthecontactmodelalwaysoccurnotonlyinthecaseof
3、tooslowdiffusion,butalsointhecaseofrapiddiffusion,whenstochasticenergytransferisreplacedbydynamictransfer,asmanifestedintheunusualhyperbolicdecreaseofthequenchingratewiththegrowthofdiffusion.PACSnumbers:32.20.11.INTRODUCTIONwhereNisthedenSityoftheexciteddonorsinthesample,Cistheconcentrati
4、onofthequenchingimpurity,Themigrationofexcitedatomsandmoleculesfacili•andn(r,t)istheexcitationdensityinthevicinityofatatestheirencounterwithquenchingimpuritycenters.quencher,normalizedtounityeverywhereattheinitialTheresultoftheencounterdependsnotonlyonhowmomentandatalltimesatpointsfarfrom
5、thequencher:closethepartnersgetandwhatinteractionmechanismobtains,butalsoonhowquicklythequenchingzoneisn(r,O)=n(oo,t)=L(1.3)crossed.Itisclearthattheeffectivenesswoftheen•Suchanapproachtotheproblemallowsaunifiedde•countershouldbeafunctionofthediffusioncoefficientscriptionofbothstaticdecay(
6、D=0),whenanexcita•D,whichdeterminesthedurationoftheencounter.How•tiondecaysatthelocationwhereitarises,anddiffu•ever,thecontacttheoryofluminescencequenching[l,2lsion-acceleratedquenching.eitherentirelyignoresthiscircumstance(the"black"spheremodel),ortakesitintoaccountinthemostForanyDquench
7、ingbeginswithstaticdecayandprimitivemanner,conSideringthequenchingratedur•endswithdiffusion-assisteddecay.When,however,aingthetimeofcontactaconstant(the"gray"spherestableconcentrationprofilens=t!!..~n(r,t)getsmodel).Themorerefinedtheory[3-5l,whichtakestheestabliShed