Auger recombination and charge-carrier thermalization in Hg-n(-)-cluster photoelectron studies .pdf

Auger recombination and charge-carrier thermalization in Hg-n(-)-cluster photoelectron studies .pdf

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1、PHYSICALREVIEWLETTERSweekendingVOLUME90,NUMBER828FEBRUARY2003AugerRecombinationandCharge-CarrierThermalizationinHg-ClusterPhotoelectronStudiesnR.Busani,R.Giniger,T.Hippler,andO.Cheshnovsky*SchoolofChemistry,theSacklerFacultyofExactSciences,Tel-AvivUn

2、iversity,69978Israel(Received9July2002;published24February2003)Photoelectronspectra(PES)ofHgshowstrongdependenceofspectralfeaturesonphotonenergy,ni.e.,peaktailingandbandgapfilling.Thisdependencesuggeststheexistenceofcomplexphotoinducedprocessesinparal

3、lelwiththedirectphotodetachmentprocess.The‘‘corrupted’’PES,takenwithintermediatephotonenergy,carrythesignatureofinterbandabsorptionfollowedbycharge-carrierthermalizationandAugerelectronejectioninHgn.Theseprocesses,sosignificantinthephotophysicsofbulks

4、emiconductorsandnanoparticles,havenotyetbeenidentifiedinclusters.DOI:10.1103/PhysRevLett.90.083401PACSnumbers:36.40.Wa,33.60.–q,36.40.Cg,36.40.VzInmonovalentmetalclusters,suchasthealkaliorthe(n80–100).Theelectronicstructureofmercuryclus-coinagemetals,

5、thecongestionofstatesdevelopswithtersinthesizerangeofn3to40050isthatofaclustersizeintoacontinuousdensityofstatesofhalf-semiconductorcluster,witha6s‘‘valenceband’’anda6pfilledbands,allowingfortheevolutionofthemetallic‘‘conductionband.’’Itturnedout,ho

6、wever,thatwithstate[1].Inprinciple,bivalentmetalscouldbesemicon-lowerdetachmentenergies(e.g.,4.66eV),thePESvaried,ductors.Inthecondensedphase,itistheoverlapbetweenshowinginsomecasescloggedbandgaps.Toresolvethesandpbands,attainedbythehighcoordinationth

7、eseunexpectedfindings,wehavesystematicallystudiednumber,whichenablestheformationofpartiallyfilledthedependenceofthePESofHgonthedetachmentnbandsand,consequently,bringsaboutthemetallicbe-energy.havior.Inclustersofbivalentmetals,acriticalsizefortheInthisL

8、etter,weshowthatthedetachmentenergys-pbandmergingisexpected.TheonsetofthemetallicdependenceofthePESsuggeststheexistenceofcomplexstateinthebivalentmercuryclustershasbeenthesubjectphotoinducedprocesses,competingwithphotodetach-ofnumerousexperime

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