JournalofElectronSpectroscopyandRelatedPhenomena224(2018)45–50
ContentslistsavailableatScienceDirect
Journal
of
Electron
Spectroscopy
and
Related
Phenomena
j o ur na l ho me p a g e :w w w . e l s e v i e r . c o m / l o c a t e / e l s p e c
Capabilities
of
Angle
Resolved
Time
of
Flight
electron
spectroscopy
with
the
60
◦
wide
angle
acceptance
lens
Danilo
Kühn
a,∗,1,
Florian
Sorgenfrei
a,1,
Erika
Giangrisostomi
b,
Raphael
Jay
a,
Abdurrahman
Musazay
b,
Ruslan
Ovsyannikov
b,
Christian
Stråhlman
b,2,
Svante
Svensson
c,
Nils
Mårtensson
c,
Alexander
Föhlisch
a,baInstitutfürPhysikundAstronomie,UniversitätPotsdam,Karl-Liebknecht-Str.24/25,D-14476Potsdam,Germany
bHelmholtz-ZentrumBerlinfürMaterialienundEnergieGmbH,Albert-Einstein-Straße15,12489Berlin,Germany
cDepartmentofPhysicsandAstronomy,Box516,75120Uppsala,Sweden
a
r
t
i
c
l
e
i
n
f
o
Articlehistory:
Received19December2016
Accepted27June2017
Availableonline11July2017
Keywords: Artof Electronspectroscopy Wideangle Timeofflight Energyresolution Synchrotron
a
b
s
t
r
a
c
t
Thesimultaneousdetectionofenergy,momentumandtemporalinformationinelectronspectroscopyis
thekeyaspecttoenhancethedetectionefficiencyinordertobroadentherangeofscientificapplications.
Employinganovel60◦wideangleacceptancelenssystem,basedonanadditionalacceleratingelectron
opticalelement,leadstoasignificantenhancementintransmissionoverthepreviouslyemployed30◦
electronlenses.Duetotheperformancegain,optimizedcapabilitiesfortimeresolvedelectron
spec-troscopyandotherhightransmissionapplicationswithpulsedionizingradiationhavebeenobtained.
TheenergyresolutionandtransmissionhavebeendeterminedexperimentallyutilizingBESSYIIasa
photonsource.Fourdifferentandcomplementarylensmodeshavebeencharacterized.
©2017TheAuthors.PublishedbyElsevierB.V.ThisisanopenaccessarticleundertheCCBY-NC-ND
license(http://creativecommons.org/licenses/by-nc-nd/4.0/).
1. Introduction
Electronspectroscopyhasbeenapowerfulexperimental tech-niqueforinvestigatingmatterinallphasessinceitsdevelopment inthe1960sbyKaiSiegbahn.Advancingsimultaneousdetection ofbothelectronkineticenergiesandtheirangularormomentum distribution hasbeen the pathway toenhance the experimen-talperformance.Inthisrespect,thecombinationofanadvanced electron opticallens with anhemispherical deflectionanalyzer (HDA)[1]establisheda workhorse that linkshighenergy reso-lution,highangularresolutionand flexibilityinoperationmodi spanningfromhighesttransmissionandenergyresolutionto com-binedhighangularandenergyresolvingoperation.Inordertoavoid thegeometricconstraintsoftheHDAentranceslit,theenergy dis-persivehemispherecanbereplacedbyahightransmissionTime ofFlightenergydispersingunit.Thishasledtothedevelopmentof theAngleResolvedTimeofFlightAnalyzer(ARTOF)[2].Operating
∗ Correspondingauthor.
E-mailaddress:danilo.kuehn@helmholtz-berlin.de(D.Kühn).
1 Previous address: Helmholtz-Zentrum Berlin für Materialien und Energie
GmbH,Albert-Einstein-Straße15,12489Berlin,Germany.
2 Presentaddress:MalmöUniversity,20506Malmö,Sweden.
atanacceptanceangleof30◦theapproachwasestablishedinproof ofprincipleexperiments,utilizingthesinglebunchtimestructure ofsynchrotronradiationandlaboratorysources[3–6].Sincethe electronflighttimewithintheARTOFsetsanupperlimitforthe suitablerepetitionrateforthephotonsourceintherangeoffew MHz,areductionoftheGHzrepetitionratesofmultibunch syn-chrotronradiation,i.e.500MHzatBESSYII,iscrucialforawider applicationof this advancedelectron spectrometer.Thus BESSY IIhasdevelopedPulsePickingbyResonantExcitation(PPRE)[7] andmechanicalpulseselectionbyaMHzChopper[8]aswellas electronicdetectorgating[9].
Combining theseadvances, we have now taken the step to enhancetheacceptanceangleoftheARTOFlenssystemthrough anadditionalacceleratingelectronopticalelementwhichallowsto widentheangularacceptanceto60◦keepingbothenergyand angu-larresolution.UtilizingtheBESSYIIFEMTOSPEXinstallations[10] inthisworkwepresenttheworkingprincipleandtheexperimental parameterspaceofthe60◦ARTOFsystem.
2. Electronanalyzerandsetup
The60◦ wideangleacceptanceARTOFisthecoreofthenew endstationforsurfaceandsolidstatedynamicsattheBESSYIIsoft X-Rayfemtoslicingbeamline.
https://doi.org/10.1016/j.elspec.2017.06.008
0368-2048/©2017TheAuthors.PublishedbyElsevierB.V.ThisisanopenaccessarticleundertheCCBY-NC-NDlicense(http://creativecommons.org/licenses/by-nc-nd/4.
Fig.1.a)Schematicdrawingofthe60◦wideangleacceptanceARTOF.Electronsemittedfromthesampleunderhighangleswithrespecttothesurfacenormal(redand
bluelines),aredeflectedstronglytowardstheopticalaxis(greenline)whenenteringthespectrometerentranceduetotheretardationmesh.Depictedelectronsclosetothe
detectormarkequalflighttimes.b)InsightoftheARTOFentrancec)Photoemissiongeometry.
Fig.2.Left:ContourplotofthesimulatedconversionmatricesfortheAng564-lensmodeforEcen=10eV.TheverticallinesmarkequivalentenergiesineVandthehorizontal
linesmarkequivalentangleindeg.Right:Schematicenergyvs.time-of-flightdependencyforϑ=0(top)anditsderivative∂E
∂t (bottom).
TheARTOFisaTimeofFlightelectronspectrometerwhich con-sistsofa1.3mlongdrifttubewithanadvancedelectrostaticlens systemofmultiplelenselementsandatwo-dimensionaldelayline detectorbyRoentdekGmbHincludingaMCPelectronmultiplier whichenableseventdetectionofarrivaltimeandpositionofevery analyzedelectron.Thewideanglelensis amodularupgradeof theARTOFlenssystemwithanelectronretardationmeshatthe ARTOFentrancewith80%transmissionprovidingadeflectionofall electrontrajectorieswithinthehighacceptanceangleintothedrift tube.Fig.1showsaschematicdrawingoftheARTOFwith trajec-toriesofelectronsemittedunderdifferentangles,afteroptical excitationofthesample.Electronsemittedunderhigherangles withrespecttotheopticalaxisofthespectrometerhavelonger flightpathsand thus longerflighttimes comparedtoelectrons emittedonaxis (ϑ=0).Theelectronarrivaltimetandhitting posi-tionx,yatthedetectordependonthekineticelectronenergyEand thetake-offangleinanon-linearwayandcanbetransformedto energyEandemissionangles,bytwotransformationmatrices incylindricalcoordinatesE (t,r) andϑ (t,r) whichareobtainedby simulations[2](seeFig.2).The-matrixistrivialduetocylindrical symmetry.
TheARTOFisoperatedintheconstantretardationratio(CRR) modewhichmeansthatallvoltagesofthelenssystemareraised proportionallytothecenterenergyEcenoftheanalyzedenergy
win-dow.Conclusivelytheelectrontrajectoriesareindependentfrom Ecenandonlyonesetofconversionmatricesisnecessarytocover
thetransformationforthefullenergyrange.Theenergywindow isaconstantfractionofEcenandtheenergyresolutionisscaling
withE3/2accordingtoEq.(1)forhighenergies.Inthisoperation
modeonecandefinealensmodebyspecifyingalllenselement voltagesforasingleenergye.g.Ecen=10eV.Thesizeoftheenergy
windowinwhichallelectronscanbeanalyzedsimultaneouslyand theangleacceptancecanbederivedfromsimulations.Thestandard nomenclatureofalensmodeis‘Angew’whereisthefullangle acceptanceand‘ew’isthesizeoftheenergywindowinpercentage e.g.‘Ang564’.
AllmeasurementsinthisworkhavebeenperformedattheUE 56/1PGMsoftX-RaybeamlineattheBESSYIIinstandard multi-bunchmode.WhilecommonlyoperatingwithPPRE[7]wehere usedtheunexcitedCamshaftbunchinthemiddleoftheionclearing gaptoavoidanypossibledecreaseinbeamlineenergyresolution which might arise frombunch excitation. We have chosenthe
D.Kühnetal./JournalofElectronSpectroscopyandRelatedPhenomena224(2018)45–50 47
1200l/mmmonochromatorgratingandthe50mexitslitfor opti-malbeamlineenergyresolutionandsmallelectronspotsizeatthe samplerespectively.Thephotonbeamisverticallypolarizedand thephotonenergyrangesbetween260and970eVwithaphoton pulselength<70psFWHM.TheARTOFopticalaxisisparalleltothe samplesurfacenormalandliesinthebeamplane.Thephotonbeam ishittingthesampleunder50◦withrespecttothesurfacenormal. Thebasepressureoftheexperimentalchamberis2·10−10mbarand
allmeasurementswereperformedatroomtemperature.
3. Results
Oneofthemostimportantcharacteristicsofanelectron spec-trometer is its energy resolution Eand the related resolving powerE/E.We haveanalyzed thisproperty inthesoft X-Ray regimefor kineticelectron energies between90eVand 810eV. IntheCRRmodetheenergyresolutionisgivenbythefollowing equation:
E=
˛·E3/2·t2+ˇ·E·d2 (1)Thefirstpartofthisequationcontainsthecontributionfromthe temporalresolutiont,thesecondpartdescribestheeffectofthe spatialdetectorresolutiond.Theparameters␣anddescribethe temporalenergydispersionandspatialenergydispersion, respec-tively,anddependonthespecificlensmode.Theyaregenerallya functionofdetectorhitpositionandflighttime(examplesaregiven below).Furthercontributionsmaycomefromtheelectronsource diameterandarotatedsamplesurfacethatisnotperpendicularto theopticalaxisofthespectrometer.Howeverforhighkinetic ener-giesEkin>50eVandsmallspotsizes≈100mastypicallyexistat
asynchrotronradiationbeamline,thetemporalresolutionisthe dominatingcontributiontotheintrinsicenergyresolution[2]and Eq.(1)simplifiestoEq.(2):
E=˛·E3/2·t (2)
Thetotaltemporalresolutiontisgivenbytheconvolution oftheexcitingphotonpulselengthtph=70ps FWHMandthe
temporalresolutionofthedetectortdet
t=
t2ph+t2det (3)
andcanbedeterminedbymeasuringonlyphotonsatthe detec-tor,whichisachievedbyapplyingalargenegativebias.Herewe determinet=216±2psFWHMfortheglobaltemporalresolution byapplyingaGaussianfittothephotonsignalintegratedoverthe wholedetectorareaandt=166±13psFWHMforthedetector positionadaptedtemporalresolution,asprovidedbythephoton peakfittoolavailablewithintheARTOFLOADERanalysispackage.3
Fortheanalysisoftheenergyresolutionwedistinguishbetween localenergyresolutionElocwheretheelectronspectraare
deter-minedonlyfromasmalldetectorareaaroundtheoriginandthe globalenergyresolutionEglobwherethewholeangleacceptance
is usedto derivethe spectra.Besides thefundamental limit of theenergyresolutiongivenbythetemporalresolution,theglobal energyresolutioncanbefurtheraffectedbyresidualmisalignments andsignalpropagationtimedifferencesofthedetectorwhereas thelocalenergyresolutionisonlylittleaffectedbythose. There-foredeviationsbetweenElocandEglobforagivensettingcan
givehintsof‘howfarthespectrometerisawayfromoptimal per-formance’.
InthisworkweusetheS2pphotoemissionlinesof semicon-ducting2H-MoS2forthecharacterizationoftheenergyresolution.
3ARTOFLOADERv.2.5.−156,seeref.[4]forfurtherinformations.
The sample is preparedby cleaving, which gives reliably clean surfacesleadingtoawelldefinedelectronsourcegeometry.The S2p3/2 andS2p1/2 peakswithEbind=162.7eVandEbind=163.9eV
[11]respectivelyhaveanarrowsymmetriclineshapewitha nat-urallinewidthof0.054eV4andgiveagoodsignaltobackground
ratio.WeobserveanadditionalconstantGaussianlinebroadening
ofEsample=0.19eVFWHMwhichisdominating thelinewidth
atkineticenergiesbelow100eV.Thiswasalsoobservedby Mat-tilaetal.andisattributedtoterraces,stepsandpointdefectsatthe samplesurface[11].InFig.3differentrepresentationsofthespectra fortwodifferentkineticenergiesareshownfortheAng564-lens mode. Theenergy-angle-cuts(topand middlepanels)showthe intensityoftheS2plinesoverthewholeangleacceptance reveal-ingonlyminordistortions.Theenergyspectrawhichareintegrated overasmalldetectorareaandthewholedetectorarearespectively, haveverysimilarlineshapesandshowonlya minoradditional broadeninginthelattercase.Thecountratesofthedifferentlens modesgivequalitativeproofoftheincreasedtransmissionforthe 60◦ instrument.TheintensityratiooftheS2plinesofAng60and Ang50lensmodesisabout1.4,inaccordancewiththeratioofthe solidangles.However,thequantitativedifferencesbetweenAng56, Ang58andAng60aredifficulttodeterminepreciselyduetothe inhomogeneousangulardistributionoftheemittedelectrons.
ForquantifyingtheenergyresolutionwehavemeasuredS2p photoelectron spectrafor five differentkinetic energies in four differentlensmodesandappliedafitconsistingoftwoVoigt pro-filepeakswithafixedspinorbitsplittingof1.19eV,aLorentzian widthof0.054eVconvolvedwithaGaussianbroadeninganda lin-earbackground(seee.g.Fig.4a).Thecenterenergyissettothe kineticenergyoftheS2plinesforeachmeasurement.The spec-trometerenergyresolutioncannowbecalculatedbydeconvolving theGaussianlinewidthfromthesamplebroadeningandthe beam-lineresolutionEph.Inanextstepwehavedeterminedthescaling
parameter␣·tinEq.(2)byapplyingafit(Eq.(4))totheglobal Gaussianlinewidth(seeFig.4b)andthelocalGaussianlinewidth, respectively(seeTable1).
E=
˛·t·Ekin3/2 2 −Eph 2 −Esample 2 (4) Using␣loc·tand␣glob·tonecancalculatethelocalandglobalenergyresolution(seeFig.5a)andtheresolvingpower(seeFig.5b). Theparameters␣andfromEq.(1)canalsobedetermined fromthesimulatedenergyconversionmatricesE (t,r) bynumerical differentiationwithrespecttothetimeofflight(t)orpositionon thedetector(radiusr).
˛matr(t,r) =−
∂E (t,
r)∂t
·E −3/2 cen (5) ˇmatr(t,r) =∂E (t,
r)∂r
·E −1 cenTheparametersdependonrandtitisthereforenotpossibleto giveasingleenergyresolutionforagivenlensmode.Foralllens modesonecanobservearathernarrowdistributionofalpha val-uesaround˛matr(r=0,E=Ecen)(seeTable1).Therelativewidth
ofthedistribution␣matr/␣matrisapproximately±15%.Thevalue
forˇmatrisrather homogeneouslydistributedbetweenˇmatr=0
forr=0andˇmatr=1.5m−1forhigherradii.Thecontributionsof
spatialandtemporalresolutionontheenergyresolutionareabout equalbetweenEcen=10eVand30eVandthetemporalresolution
becomesincreasinglydominantforEcen≥50eV.
Fig.3.Angle/energy2Dmapsfortwodifferentkineticenergies(left:Eph=260eV,right:Eph=790eV)recordedintheAng564-lensmoderepresentedinbipolarcoordinates.
Onthetoppanels,intensityisdisplayedvs.energyandtheverticalanglealphaandintegratedoverthehorizontalanglebeta.Inthemiddlepanels,intensityisdisplayedvs.
energyandbetaandintegratedoveralpha.Atthebottompanel,angleintegratedenergyspectraareplottedfortwodifferentintegrationareas:Theredspectraaretaken
fromanareaaroundthedetectororigin(markedbyredboxesin2Dplots)andthebluespectraaretakenfromfullangleacceptance.Thesmallareaspectrashowrealelectron
yield(counts)whilethefullangleacceptancespectraarenormalizedtosolidangle(scalingfactoramountsto30.8).Notethatonlyafractionoftherecordedenergywindow
isdisplayedforbothkineticenergies.
Table1
ListofexperimentalandsimulatedlensmodeparametersdeterminingtheenergyresolutionaccordingtoEq.(2)andtheangularresolution.
Energywindow[%] ˛
loc·t(local)10−5eV−0.5
˛glob·t(global) 10−5eV−0.5
˛loc ˛glob ˛matr
105eV−0.5s−1
Angularresolution[deg]
ang50 7 5.34±0.04 6.95±0.02 0.77 3.43 0.13±0.02
ang56 4 3.06±0.03 3.67±0.01 0.83 1.76 0.18±0.04
ang58 4 3.41±0.02 4.18±0.01 0.82 1.93 0.20±0.04
ang60 2 4.17±0.03 4.88±0.01 0.85 2.54 0.15±0.02
Theangularresolutioncanbeestimatedfromtheangular
dis-persion of the lens system in the image planeat the detector
bycalculatingthederivativeofthethetaconversionmatrix.For
sourcesizesdsource≤100m,witha spatialdetector resolution
ofddet=100mandneglectingtheminorinfluenceoftemporal
resolution,theangularresolutionisgivenby:
ϑ (r) ≈
∂
ϑ∂
r (r) ·ddet (6)Table1showstheangularresolutionaveragedoverthe accep-tance angle for all lens modes. The uncertainties are given as standarddeviations.
4. Discussion
ThelocalenergyresolutiondeterminedfromtheS2ppeakfits can bedirectly compared withthe expected energy resolution fromtheenergyconversionmatriceswiththetemporalresolution
D.Kühnetal./JournalofElectronSpectroscopyandRelatedPhenomena224(2018)45–50 49
Fig.4.Left:Angleintegrated(±28◦)energyspectrumofS2pphotoelectrons(bluedots)withEph=260eVrecordedintheAng564-lensmode.Afitcontaining2Voigtprofiles
andalinearbackground(redline)isappliedtothedata.Right:GaussianlinewidthcontributioninS2pspectraexperimentallydeterminedforfivedifferentkineticenergies
(dots)fordifferentlensmodes.Thefitstothedataaccountforsamplebroadening(lightbluecurve)andbeamlineresolution(greycurve).
Fig.5.Left:Globalenergyresolution(solidlines)calculatedwith␣globandlocalenergyresolution(dashedlines)calculatedwith␣locRight:Resolvingpowerofthe
spectrometercalculatedwith␣globfromtheenergyresolutionfit.Samecolourcodeasinleft.
obtainedfromthephotonpeakfittool,forexampleforAng56 4-lensmode:
˛matr·tloc=1.76·105eV−0.5·s−1·166ps=
2.92·10−5eV−0.5≈3.06·10−5eV−0.5=˛loc·t
Wefindthatthekineticenergydependenceoftheresolutionfor allfourlensmodesareinverygoodagreementwiththeexpected energyresolutioninthelocalcase,seeFig.4.Thisalreadyshows clearly that thetiming system of the spectrometer is working locallyasexpected.However,itshouldbeemphasizedthatthefits aremadeoverawideenergyrange.Althoughthefitisinverygood agreementwiththeoreticalexpectationsandpointtoaresolving powerasshowninFig.5,theintrinsicsampleenergybroadening istoohightoprovetheresolvingpoweratlowenergies.Further experimentsareneededtodeterminetheenergyresolutioninthe UPSregime.
Onecanfurthercomparethelocalandtheglobalenergy resolu-tion.Wefindthattheglobalenergyresolutionisdecreasedwith respecttothelocalenergy resolution byabout20%for alllens modes.Possiblereasonsareresidualmisalignments,different sig-nalpropagationtimesofdifferentdetectorareasand increasing ␣(fitparameter)athigheremissionangle.Weareconfidentthat carefulalignmentandadetectorpositionadaptedtimecorrection, whichwillbeavailableinfuture,canfurtherimprovetheglobal energyresolution.
Apparentlythedegradationoftheglobalenergyresolutionis sensitivetothesizeoftheenergywindowwhichcouldbeexplained bythefactthattheelectronflight timesneedtobemore com-pressedforlargerenergywindowsandarethereforemorestrongly influencedbysignalpropagationdelaysbetweendifferentdetector positions.
Comparingthefourlens modesonecanclearlyseethe gen-eraltrendthatlargersizeoftheenergywindowandlargerangle acceptancearetothedisadvantageoftheenergyresolution.
There-foretheoptimumchoiceofthelensmodedependsonthespecific experimentaldemands.
5. Conclusion
Inthisworkwehaveoperatedthe60◦wideangleacceptance ARTOFatthefemtoslicingbeamlineatBESSYII.Fourdifferentlens modeshavebeeninvestigatedinthesoftX-Rayregimeforkinetic energiesoftheelectronsrangingfrom90eVto810eV.Alllens modesperformasexpectedinthefullenergyrange,particularlythe resolvingpowerandangleacceptanceareinverygoodagreement withsimulations.Ahighresolvingpowerof1000isdemonstrated evenforhighenergiesandsuggestsaresolvingpowerof3000for 90eVkineticenergy.Electronspectroscopictechniques,drivenby pulsedlightsources,thatrelyonhightransmission,highenergy resolution,wideangleacceptanceorhighangularresolutione.g. ARPES,XPD,pump-probespectroscopymightstronglybenefitfrom thenewwideanglelens.
Acknowledgment
TechnicalsupportbyMikeSperlingisgratefullyacknowledged. PålPalmgrenandPatrikKarlssonfromScientaOmicronGmbHare acknowledgedforfruitfuldiscussionsabouttheARTOF.
D.K.,F.S,R.JandA.F.acknowledgefundingfromthe ERC-ADG-2014 − Advanced Investigator Grant No. 669531 EDAX under the Horizon 2020EU Framework Programme for Research and Innovation.NMandSSacknowledgefundingfromtheEuropean ResearchCouncilundertheEuropeanUnion’sSeventhFramework Programme(FP7/2007-2013)/ERC grant agreementn◦ [321319], and support from the Carl Tryggers foundation for scientific
reseach/CTH),andtheSwedishResearchCouncil(VR) TheauthorsthankHZBfortheallocationofbeamtime.
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