PhaseDefectsonSi(100)Surface …...DefectandDI'uusionForumVo/S.160-161 59...
Transcript of PhaseDefectsonSi(100)Surface …...DefectandDI'uusionForumVo/S.160-161 59...
DejectandD炉 ∫̀io77For7JmVols./60-16](1998)pp_57164㊨J998SciLecPubZicaLions,SwiIzer/077d
PhaseDefectsonSi(100)Surface,StudiedbyScannlngTunne=ngMicroscopy
H.Shigekawa,K.Miyake.M.lshida,S.OzawaandK.Hata
lnstituteofMaterialsScience,CenterforTsukubaAdvancedResearchATliance(TARA).UniversrtyofTsukuba,Tsukuba305,Japan
CREST,JapanScienceandTechnologyCorporation(JST)
Keywords:Phasons.phasetransition.surfacedefects,lsingmodel.dimerinteraction
Abstract:DynamicsofanewmovabletypePphasedefect,thatis,phasonsformedonSi(1(刀)dimer
rows,andrelatedstructuralchilngeSWereStudiedfromroomtemperatureto6Konanatomicscale,in
relationtotheinteractJOnbetweenSi(100)surfacediners.At~200K,dinernip-flopmotionbegan
tofreezefromthedefectsondinerrows,andtheantiferomagneticcorrelationappearedalongdjmer
rowsfirsLWithfurtherdecl'eaSeintemperature,C(4x2)Structurebegantocoverthesurface・While
typePdefectsnligratedonthesurface,thec(4x2)arTangementperSistedasthetemperaturedecreased
to30K・TheobservedchangewasconsistentwiththeordeトdlSOrderphasetransitionwhichhasbeen
observedontheSi(100)surface・At6K,incontrast,themigratlOnOfthephasonsresultedinanapparent
phasetransitionbetweenc(4x2)andp(2x2)amngementS,Whichindicatesthattheinteractionbetween
dimerTOWSissignificantlyweilkeratthistemperature,andsuggestssomecharacteristlCChangebetween
ト 30Kand6K.Long,angeinteractionwasfoundtoplayanimportant,oleonSi(100)surface.
Withtheprogressofthenanoscalescienceandtechnology,atomicdefectsinmaterlalsurfaces/
Interfacesbegintoplayanincl▲eaSinglyimportantrole,andthereforeitisnecessarytocharacterizethe
structureofthedefectsatanatomicscale・FortheSi(100)surface,itisweLlestablishedthatpairsof
top-layeratomsformdimeJ.ゝ・AsIdentifiedbyHamersetal・,therearethreetypicaltypesofdefects-
typeAcorrespondingtoasing一edimervacancy;typeBtoadoubledimervacancy;andtypeCtotwo
half-dimersresultingfromtwoadjacentSivacanciesalongthe<110>directionll〕.Recently,anew
type ofmovabledefectknownastypepdefect,wasfoundtoexistontheSi(loo)surface,andthe
dynamicsOfthephasedefectthephason,wasdirectlyobservedbyscanningtunneLingmicroscopy
(STM)at80Kand6K[2-5],ThetypePdefecthasastructuresimilartothetypeCdefectwhichacts
toinduceaphaseshift:atypePdefectconsistsoftwoadjacentdimerswhicharebuckledwiththe
sameorientation・However,incontrasttothetype Cdefect,type Pdefectcanmlgratealongdiner
rowsduetodin ernip-mopmotionatthephaseboundaries.Inthispaper,therecentSTMstudieson
thesedefectswillbesummarized,andthecharacteristicsofthetypePdefect.inrelationoftheinteraction
betweenSi(100)surfacedjnlerSWilldiscussed.
FordefectsoftypesAandB,structuralmodelswhichhaverebondedconfigurationsinthe
secondlayerwereproposedoriginallyl6]・TheelectronicstructureofthetypeAdefectandthecross
sectionofthetypeBdefectdeterminedbySTM atroomtemperaturewereconsideredtoprovidethe
58 SurfaceDWus10nandSurfaceStructure
evidencefortheapplicabilJt7e."ftherebondedmodell7,8]・However,recently,theeffectsofthese
defectsonthebucklingofadjacentdinerswerestudiedbySTM at80K,whichraisedquestions
relatedtothestructuresofthesedefectsl9].FromtheSTMobservationsofSi(loo)surfacesatroom
temperature,typeAandtypeBdefectsdidnotcausedetectablestaticbuck]ingora叫acentdimers・At
80K,ouトof-phasebucklingofadjacentdimerswasobservedinthecaseofthedoublevacancydefect
(typeB)・However,thesinglevacancydefect(typeA)wasfoundtobefurthersubdividedintothree
types,Al,A2,andA3:AIsuppressesbucklingofadjacentdinersevenatlowtemperatures,A2
inducesin-phasebuckling,andA3inducesout-of-phasebuckling・lfthesethreeeffectsaredueto
differencesinthestructuresofthetypeAdefects,theremustbethreedifferentinternals(rtlCtureSfor
thetypeAdefect・Detailswerestudiedbyobservlngthebias-dependentSTMImages,andtypeAand
typeBdefectswerefoundtohaveacharacteristicrelationshipbetweenthelrelectronicstructuresand
theireffectsonbucklingofadjacentdlmerSinducedat80K.Therelationshipbetweenthephaseof
dinerbucklingandtheeleclronicstructureofthedefectcou一dbecomprehensivelyexplainedinterms
ofthedinerstructureofthedefectl10].
RegardingthetypeCdefect,sincefromtheresultsofthespectroscoplCStudyonlythisdefect
showedastrongmetalliccharacteritisconslderedtoformasurfacestatewhichcausesFermilevel
pinningl11・AstructuralmodelwithdimerfomlationinthesecondlayerwasproposedbyUdaetaL
l11】,Sincethecalculatedelectronicstructureofthetype Cdefectwasingoodagreementwiththe
STMresults,thestructureofthetype Cdefectwasconsideredtohavebeencompletelydetermined・
However,recently,Semiconductivepropertywasobservedtobeinducedat80K〔12]・Inaddition,
slngletype CdefectwasfoundtoInducealongrangeinteractiononthesurface;whenthetypeC
defectwasremovedbytheatomicmanlPUlationtechnique,thestmctureofthelargeareasurrounding
thedefectwasobservedtobestronglyaffected[13].Theseresultsarerelatedtothefactthattype C
defectinducesaphaseshlfLandstrongInteractionbetweenthetypeCdefectandthesurrounding
buckJeddinerswasobserveddirectlyl13].
Fromtheexperimentalresultsdescribedabove,defectsoftypesA,BandCmustplayamuch
moreimportantroleinthemnOSCaletechnologythanexpected.Therefore,moredetailedanalysisis
requiredtoclarifytheircharacterlStlCS.Inanycase,itisclearthatphaseshiftinducedinthebuckled
dinerarrangementbythedefectsisquiteimportantonthesurface・Ontheotherhand,asdescribed
above,typePdefectisamovablephasedefect,andmigrationofthedefectsisstronglyrelatedtothe
characteristicsoftheSi(100)surfacestructure.However,littleisknownaboutthetypePdefect.h
thispaper,wepresen(OurrecentresultsontheSTM observationofthedynamicsoftheSi(100)
surfacecausedbythetype Pdefectfromroomtemperatureto6K,byfocusLngOntheinteraction
betweendinersonthesurface.
As iswellknown,thedetailsofthedimerarrangementhavebeencontroversialduringthelast
twodecades・Namely,dimer.<giveriselo(hesymmetric(2xl)structure;however,the(2xl)phaseis
nottheSi(100)groundstate,anddlfferentreconskuctionswithinsimilardinerstructureswereproposed
l14]・Anenergeticallyfavoredalternationofdimerbucklingalongthedinerrowsleads【othec(4x2)
reconstruction,inwhichaltema【lngbucklingaELglesarealsopresentbetweentwoneighboringdiners
DefectandDI'uusionForum Vo/S.160-161 59
belonglngtOdifferentrowsAnotherpossible
phaseisthep(2x2)phase,inwhichthebuckling
angleisthesamebetweenlWOneighboring
dinersbelonglngtOdifferentrows.Figurel
showsaschematicof(a)symmetric2xl,(b)
C(4x2),(C)p(2x2),and(d)coexistingc(4x2)and
p(2x2)strt)cturesw∫thasingletypePdefect・
Here,onlytheupperSlatomsOfthebuckJed
dinersareillustratedusingcircles・Lines
betweenthecirclesaredrawninordertocompare
thephaseshift.InFig.I,theantiferomagnetic
arrangementsofthebuckleddimers,whichforms
azigzagStnlCturealongthedlmerrows,Shows
theout-of-phase(Fig11(b))andln-Phase(Fig・
1(C))re一ationshipsbetweendimeHowsfor
c(4x2)andp(2x2)StfuClureS.reSpeCtively-
Whatmakestheill-gumentmore
complicatedisthatthedifferencebetweenthe
(a)く=∋く≡)
冒く∋(=)∈∋く∋
(C)
′…
ヽ
主
犯川騨
馴
mn
,DOO○○①①00
◎◎⑳⑬⑳e@◎
Fig.ISchematicof(a)symmetric2xJ,(b)C(4x2),
(C)p(2x2),and(d)coexTStingc(4x2)aTldp(2x2)
S帆CtureSWithasLngletypePdefecL
energiesofthep(2x2)andc(4x2)reconstructionsobtainedbytheoreticalcalculaLionsisonlyonthe
orderofImeVperdlmerH4].FromLEEDmeasurements,areversiblephasetransitionoccursbetween
theorderedc(4x2)anddisorderedphasesat-2CM)K【15]andthemoststablephasewasconcludedlo
bec(4x2)・Basedtotherecentlow-temperatureSTM studiesaL- 100Konthesurface,thec(4x2)
structurewasalsoconf)rmedtobethemoststablearrangementofthebuckleddinersl16-18].These
resultswerethoughttohavel̀eSu】tedthecontroversy,however,morerecently,l九ep(2x2)Structure
wasfoundtoreemergeatalowertemperatureof-6K,andfluctuationsbetweenthec(4x2)and
p(2x2)structureswasdlreCl】yobservedbySTM [2].
Theobservedphenomenonat-6Kisunderstoodtobecausedbythedynamicsofthemovab一e
phasedefectsformedonthedinerrows,thatis,type Pdefects・SincetypePdefectscauseaphase
shift,whenatype-Pdefectchangesitsposition,apparentphasetransitionbetweenthec(4x2)and
p(2x2)structuresoccurs(Fig・1(d)).Existenceofasimilardefectwasconfirmedevenatroom
temperature,andthestabilityofthec(4x2)structureandtheoriglnOfthesymmetricdinerswere
comprehensivelyexplainedbythedynamicsofthephasedefectl5]・Ontheotherhand,typePdefects
tendtoformpairsat80KsoilStOreducetheareaofthep(2x2)arrangementl31,whichdiffersfromthe
characteristicpropertyofthetypePdefectat6K;ぬosemovemoreindependentlyofeachotherat6K
l2]・Therefore.inordertounderstandtheobservedchangeontheSi(leo)surface;(1)>150K:disorder
(C(4x2)+p(2x2))→ (b)~ 150K:C(4x2)- (C)~ 6K:C(4x2)+p(2x2).itisnecessarytostudythe
temperature-dependenceofthesurfacedynamicsinmoredetail.
Experimentswereperrormeduslngalow-temperatureSTM,whichallowsobservationwith
atomicresolutionat-6Klnultrahighvacuum(5xlOl9pa).Aphosphorus-doped(0.010cm)Si(100)
SurfaceDiffusionandSurfaceStructure
samplesurfacewasheatedupt0-1200℃ afterprebakingforoneday,andcooledveryslowlyto
reducethedensityofthesurfacedefects・Basepressurewas~110xl0-8pa,andpressureduringtheheat
treatmentwaskeptbelow-5xl0-8pa.
Figure2showsSTMimagestakenat(a)roomtemperature,(b)-200K,(C)~80K,(d)30K,
and(e)~6K・AsisshowninFig・2(a),dinersappearsymmetricatroomtemperatureasiswell
knownJtiswidelyacceptedthatdinersarebuckledevenatroomtemperature,andswitchbackand
forthbetweenthetwopossibleorientationsinatimemuchshorterthanthelimescaleoftheSTM
measurement,whichresultsintheobservedsymm etricconfigurationintheSTMimagesIHowever,
whenthedinersnip-nopwlthoutcorrelation,thef一ip-mopmotionimplleSaCOmpletelydisordered
surface・Ontheotherhand,whenthephasedefectsmigraterapidlycomparedtothetimescaleofSTM
measurement,symmetricdimerscanbefb-edwithoutcompletelydestroylngthe2xanticorrelation
arrangement,whichagreeswellwiththefactthattheelectronicstructureobtainedbyphotoemission
spectroscopyatroomtempemtureisconsistentwiththetheoreticalresultcalculatedundertheassumpt10n
oforderedasymmetrlCdlmerSl19]Consideringtheseresults,thesymmetricdinerslntheSi(100)
SurfaceareconsideredtobecausedbythecharacteristicpropertiesofthetypePphasedefectofthe
dimerrowsl5】.Somedimersneardefectsa一ebuckled,whichisunderstoodtobecausedbytheeffect
ofthedefects;bucklingphaseisfixedbythedefects.
At、200K,asshowninFig.2(b),buckleddlmerSfrozennearthedefectsarelongercompared
tothosefrozenatroomtemperature.Evenat~200K,buckleddimersal.eJocaJizednearthedefects
onthedinerrows.TnFig.2(b),symmetricdinerregionsarecausedbythemlgratlOnOrthetype P
defectsasdescribedabove.Fromtheresultsat200Kanda【roomtemperature,interactionbetween
dimersisconcludedtobestrongeralongthedinerrowscomparedtothatbetweendユmerrowsatthis
temperaturerange・
Fig.2STMImagesOrS】()00)川rfacetakenal(a)rooTTltemperature,(b)200K,(C)80K,(d)30Kand(e)6K
DefectandDjffus/'onForumVo/S.160-161 61
AccordingtothepreviousSTM measurementat144K〔16】,anorderedc(4x2)structurewas
observedtocoverthesurface・【nthiscase,sym etricdinerdoma山swereobservedononesideofthe
typeCdefects・SinceatypeCdefectproducesaphaseshift,andintroducesaLnantiphasedomainon
oneofitssides,theobservedresultindicatesthatadomainwiththecompletep(2x2)aLTTangementWith
thetwoadjacentdinerrowsisveryunstableat144KJntheSTMimageobtainedat120K,thep(2x2)
arrangementwasobservedntdomalnboundaries[17】,whichindicatesthatthep(2x2)arrangement
whichexistsattheboundariesisstableinthistemperaturerange・
At~ 80K,asshownlnFig.2(C),thec(4x2)structurecoversthesurface・Thestructureofthe
completep(2x2)arrangementisunstableatthistemperature.AsimilarCharacteristicpropertytOthat
obtainedat80Kwasobservedonthesurfaceat30K.Thestructureofthec(4x2)Observedat30Kis
showninFig,2(d).ThlSindicatesthatthec(4x2)structureisthemoststableevenat30K・ASWas
previouslyshown,type Pdefectsexistonthesurface,andwhenthesurfaceisperturbed,rnLgrationof
thetypePdefectsisinitiatedcausingareductionintheareaofthep(2x2)arrangement〔4]・
A【6K,domalnSWiththecompletep(2x2)stn1Cturereemergedonthesu血ce・Figure2(e)Shows
anexampleoftheSTMimageobtainedat~6K,inwhichc(4x2)andp(2x2)structurescoexisHogether,
andf)uctuationbetweenthetwostructureswasobserved.Thephasetransitionbetweenc(4x2)and
p(2x2)structuresisexplainedbythecharacteristicprope托yofthetypePdefectwhichisformedon
dinerrows.NameJy,typePdefecthasastructwesimilartothatofthetypeCdefect,thatis,ilconsists
0ftwoadjacentdimerswhichLLrebuckledwiththesameorientation.lnaddition,sincetheyproducea
phaseshift.migrationofthetypePdefectcausedbythedinerf)ip-flopmotionaHhephaseboundaries
ondinerrowsinducestheapparentphasetransitionbetweenthec(4x2)andp(2x2)arrangements
肝ig・2(d)).WhenthephasedefectaHheboundarymigratesrapidlycomparedtothetimescaleofthe
STMmeasurement,itresultsinthesymmetricimagingofdimersintheSTMmeasurementst5]・
Nextletusconsiderthecharacteristicpropertyofthe
typePdefectusingthekingmodel.Figure3Shows
schematicdiagramsofthearrangementofasymmetric
dimersrepresentedbylsjngsplnS.Ingeneral,thetiltangle
ofthebuckleddinersISassumedtolakeonlytwovalues,♂oand-♂o・Therefore,thermalmotionofthediners
inducesf)ip-flopmotionbetweenthetwoangles.The
absolutevaluesofthecouplingconslantsdeterminedby
lnoueetal.areV=5I.9meV.H=6.6meV,andD=3.6meV
-+ 一一1-■- →
G… H: + I-I--・・:
vr-,-一一p≡_ 二=■ I=
Fig.3SchematicofthelsingSplnmodel
andcouplingconstantsdefinedinterms
ofV,G,H,andD.
[201.Whenatype Pdefectexists,astructurewithparallelspinisintroduced.Inthiscasethecoupling
constantVismodlfiedandbecomesequaltoG,ofabout40meVl21].Herethedefinitionandvalue
ofeachinteractionistakenfromTnoueetaI.
InteractionbetweendlmerSObtainedbylnoueeta】.ishighlyanisotropic・StrongCOrrelalion
alongdimerrowsevenatroomtemperatureWasactuallyconfinedbytheLE仁DmeasuremenlS【151.
Thecharacteristicpropertycol・reSPOndstoourSTMobservationat200K.Asimilarcharacteristicwas
alsoobservedat-6K;C(4x2)Structuraldomainsareformedasone-dimensionalratherthantwo-
62 SurfaceDiqusionandSurfaceStructure
dimensionalstructures・Theseresultsindicatethat (a)一博
interactionbetweendinersisstrongeralongdiner
rowstharHhatbetweenadjacentdinerrows.
Figure4(a)showsascL●iesofSTM Images
takenat200K(Vs=-2・OV.lt=1.OnA),wherea
symmetricdinerreglOnexistsonadinerrow
sandwichedbetweentwobuckleddinerreglOnS.By
companng山ephaseofthebuckユeddinersonei山er
sideofthesymmetricdineral'ea,WeSeethatthere
isonetypePdefectinthesymmetricdinerreglOn,
ThesymmetricdinerregionChangesitsposition
accordingtothemigrationofthetypePdefect,but
isl∝atedonlyaroundtheside.iOfthedinerdomain,
andneverappearsinthecentralpan.Theobserved
resultssuggestthepotentiaJshdpeShowninFig・4(b)
蔚 逐 建碑 J;,i.二二:≡..一一■jp
至萄 -. ' 亮 一-I_一 正
歴 空 軍軍 慧
一丁 . .__・▼
憲 塁-'IleIごO'二oIa'-vOr■ 一竃L_l■■■-
(b) \、ーノ //′{ \ J
forthetype Pdefect,asafunctionofitsposition
alongthedinerrow.Foranalysispurposes,the (C)
schematicsoranlsingsplnmodelfbr山etwocases
inwhichatype Pdefectexin aroundthesideand (d)centralareaOfthedomainaL.eShowninFigs.4(C)
and4(d),respectively・0111ywhenthenearest-
neighborinteractionalongthedinerrow is
considered,doestheInteractionenergyofthe10
asymmetricdinersinthedomainshowninFigs.
4(C)and4(d)becomethesome:(C)H.o=-10Vand
(d)2H~=-10V・Here,VjstheattractlVeinteraction
er)ergybetweentwodiners.andH meansthesum
▲-
▲T
Hu
11Hu
▲T
▲T
l
・⊥▼
【V〓>&
Fig・4(a)STM imagesofSi(100)surface
continuous一yobtainedat200K,(b)Apotentia一
modelforthetypePdefec【in(a).Schematicsof
theIsingsplnmodelfortwocasesinwhichatype
Pdefec(existsaround(C)theside,and(d)central
areaorthedomain.
oftheintemctionenergiesofnasymmetricdimers・However,theobservedphenomenon(H .o<2H,)is
differentfromthecalculatedresult,andsuggeststheexistenceofalongerrangeinteraction,which
mayalsoagreewiththetendencyofthe2xorderingofthedimerarrangement,
From144Kl16]to30K.acompletec(4x2)structurewasobservedonthesurface,indicatingthe
stronginteractionbetweendimerrows.Infact,whenthesurfaceisperturbed,thec(4x2)structure
recoversbythedynamicsofthetypePdefectsltypePdefectsreamngetheirlocationstoincreasethe
areaofthec(4x2)structure.Figure5Showsanexampleofthestructuralchangeinducedbythe
destructionofatypeCdefectat80K(Vs=一0.6V,It=1.OnA).SlnCetypeCdefectpr∝luceaphaseshift,
ap(2x2)arrangementexistsontheleftofthetypeCdefectindicatedbyanaJTOWinFig・5(a).Inorder
tostudytheinteractionbetweendlmerrows,thetype CdefectwasremovedbyapplylngaVOJtage
usingtheSTM tip.As issh()wncLearly,thep(2x2)domaininFig.5(a)changedintothec(4x2)
arrangementjnFigl5(b).Theobservedchangeisexplainedbythecreationaridmovementofthetype
DefectandDJ'ffusI'onFonJm Vo/S.160-161 63
逮
Fig-5STMimagestakenn【80K(a)beforeand(b)a鮎rdestructionofthe(ypeCdeFectjndicatedby
ana汀OWin(a).
Pdefec【onthedinerrowbythedestructionofthetypeCdefect・Theobservedresultsdirectlyindicate
thestronginteractionbetweendinerrowsandstabilityofthec(4x2)arrangementcomparedtothatof
thep(2x2)arrangementutthlHemperature.
Downto30J(,thep(2x2)domainformedononesideofthe【ype Cdefectwasunstablebutit
stabilizedwhenthetempel-aturewasdecreasedto6K.Letusdiscusstheobservedstructuralchange
from30Kto6K・ThestructL=eOfthep(2x2)arrangementreemergesat6K.Apossibleexp一anationis
torelatetheobservedslfuCrurulchangetothecoherentlengthofthecorrelationofdinerarrangement
alongdinerrows.Whenthecorrelationbecomesstrongeratlowertemperatures,coITeliltionbetween
dinerrowsmaybecomeweaker.However,asiswellknown,theorder-disordertransitiontemperature
isaround200K・Anotherexr)1ilnationistoconsiderthechangeintheinteractionbetweendimers・
SinceintefaCtlOnenergiesoradimerinc(4x2)andp(2x2)arrangementsare-2V十2H-4Dand-2V-
2H+4D,respectively,ChangeintheWDratiomaycausetheobservedsurfacestructuralchange・
Inconclusion,phaseorthebuckleddinerswasfoundtobestrateglCallyrelatedtotheatomic
defectsontheSi(loo)surface.Sincebuckleddinersarefrozenatlowtemperatures,thephaseeffect
becomesmoredomjnarItat一owtemperatures,Fromtheanalysisofthetemperaturedependentdynamics
ofthetypePdefect,interactionbetweendinerswasshowndirectly.
ThisworkwassuppolledbytheShigekawaProjectofTjN ,UniversltyOfTsukuba・Thesupport
ofaGrant-in-AidforScientLrLCResearchfromtheMinistryofEducation,Science,SportsandCulture
ofJapanisalsoacknowledged.
SurfaceDMusionandSurfaceStructu/守
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Forcorrespondence,
Electronicmai一:[email protected]
http:〟www.ims・tsukuba.ac.jp/lab/shgekawa
Fax:十8ト298-55-7440