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Atomic-ResolutionImagingofFastNanoscaleDynamicswithBrightMicrosecondElectronPulsesPavelK.Olshin†,GabrieleBongiovanni†,MarcelDrabbels,andUlrichJ.Lorenz*Affiliation:LaboratoryofMolecularNanodynamics,ÉcolePolytechniqueFédéraledeLausanne,1015Lausanne,Switzerland†Theseauthorscontributedequally.*Towhomcorrespondenceshouldbeaddressed.E-mail:ulrich.lorenz@epfl.ch
1SupplementaryinformationSupplementaryNotesDrift-correctedimagingwithmicrosecondelectronpulsesinthepresenceofbeam-induceddriftInFigure2ofthemaintext,wedemonstratedrift-correctedimagingwithmicrosecondelectronpulsesinthepresenceoflargeamountsofdriftthatweinducebyirradiatingthesamplewithalaserbeam.Here,weshowthatimagingwithmicrosecondelectronpulsesoffersthesameadvantageifthedriftisnotinducedbyanexternalstimulus,butbytheexposureofthesampletotheelectronbeam.Supp.Figure3a,cshowsdrift-correctedimagesofanensembleofgoldnanoparticlesonlaceycarboninanareaofthesamplethatisparticularlysensitivetobeam-induceddrift,withthemicrographin(a)acquiredwithcontinuousbeamandthatin(c)withpulsedillumination(600µspulses).Bothimageswererecordedasmoviesof25frames(1025mstotalexposuretime,sametotaldose)anddrift-correctedwithcisTEM.1Adiffractogramoftheareamarkedwithablackrectangleinthemicrographrecordedwithelectronpulsesrevealsanumberofreflectionsoriginatingfromthegoldnanoparticlesthataremuchweakerorevenabsentinthemicrographacquiredwithacontinuousbeam.Pulsedilluminationthereforebetterpreserveshigh-resolutioninformation,eventhoughthesampleexperiencesmorebeam-induceddrift,asthereconstructeddriftpathsreveal(SupplementaryFig.3b,d).2
2SupplementaryFiguresax104b12x102.0114.61.9101.894.28sr)1.723.871.663.41.5Beamdiameter(nm)5NumberofelectronsBrightness(A/m1.443.01.332.61.2200.10.20.30.40.50.600.10.20.30.40.50.6Laserpower(W)Laserpower(W)Supp.Fig.1.Determinationofthebrightnessofthelaser-boostedelectronpulses.(a)Beamdiameter(bluedots)andnumberofelectronsina10µspulse(reddots)asafunctionofboostlaserpower.(b),Instantaneousbrightnessoftheelectronpulsesasafunctionoflaserpower.3
3aContinuouselectronbeambElectronpulses(480µs)Supp.Fig.2.Drift-correctedimaginginpresenceoflargeamountsofdrift.(a,b)FullframemicrographsfromwhichtheimagesinFig.2a,cofthemaintextweretaken.Scalebar,20nm.4
4Drift-correctedimagingwithmicrosecondelectronpulsesElectronbeam-induceddriftaContinuouselectronbeamcElectronpulses(600µs)bd0.60.80.40.40.20yshift(Å)0yshift(Å)-0.4-0.2-0.8-0.4-1.2-0.400.4-10xshift(Å)xshift(Å)Supp.Fig.3.Drift-correctedimagingwithmicrosecondelectronpulsesinthepresenceofbeam-induceddrift.(a,c)Drift-correctedimagesofanensembleofgoldnanoparticleson5
5laceycarboninasampleareathatexhibitslargebeam-induceddrift.Themicrographin(a)isacquiredwithacontinuouselectronbeam,whilethatin(c)isrecordedwith600µselectronpulses.Diffractogramsoftheareamarkedwitharectanglerevealseveralreflectionsofthegoldnanoparticlesthatarepresentwhenthesampleisimagedwithelectronpulses,butweakerorabsentwhentheimageisrecordedwithacontinuousbeam.Scalebars,50nmand2.5nm-1.(b,d)Driftpathofthespecimenduringacquisitionoftheimagesin(a)and(c),respectively.6
6a(-110)b(110)lead-1-101-10-110110seedcrystalc(200)d(110)randomorientation-200(200)200(-110)Supp.Fig.4.Crystallizationofanindividualleadnanoparticle.(a-c)RepresentativeimagesofdifferentconfigurationsoftheleadnanoparticleofFig.4a-fofthemaintextafterinsitumeltingandrecrystallization(500µslaserpulses,1mW).Diffractogramsoftheleadparticle(circleina)andtheadjacentperovskitenanocrystal(rectangleina)revealthatcrystallizationpreferentiallyoccurswiththelatticeplanesofbothparticlesaligned(highlightedinthediffractograms),suggestingthattheperovskitenanocrystalactsasanucleationseed.Scalebars,10nmand5nm-1.(d)Distributionoftheorientationsofthelatticeplanesoftheleadparticleattheinterfacewiththeperovskitenanocrystal.Inaboutonethirdofcases(27total),thecrystalorientationappearstoberandom.Intheremainingcases,thelatticeplanesoftheleadparticleareparalleltooneofthreesetsoflatticeplanesoftheperovskite.7
7References(1)Grant,T.;Rohou,A.;Grigorieff,N.CisTEM,User-FriendlySoftwareforSingle-ParticleImageProcessing.eLife2018,7,e35383.8
