Abstract
Theworkpresentedinthisthesisisfocussingontheutilizationofgraphenederivativesas
electrodematerialindifferentapplications.Itcanbedividedintotwomainapplications.The
firstisregardingprintingoflarge-areathinfilmsofreduced grapheneoxide,andtheelectron
conductanceofthese.Thesecondisfocussingonmolecularelectronicdevices,andhowgraphene
derivativescanbeimplementedasantopelectrode.
Large-areathinfilmsofreducedgrapheneoxidewereinvestigated,asapotentialmaterial
forfabricationoftransparentandflexibleelectrodesatan industrialscale.Differentvariations
oftheHummers’oxidationreactionwasutilizedtoproducegrapheneoxidefromgraphite.A
grapheneoxidesuspensionwasup-concentratedintoahighly viscousaqueousgrapheneoxide
ink.Theinkwasscreenprintedintomacroscopicelectrodestructures.Theinsulatinggraphene
oxideelectrodeswerereducedwithhydroiodicacidvapourintosemi-transparent,flexibleand
conductivereducedgrapheneoxideelectrodes.
Itwasshownthatmicroscopicstructuresinthethinfilms,introducedbytheprintingpro-
cess,influencedtheoptoelectronicpropertiesofthereducedgrapheneoxideelectrodes.The-
refore,wesetouttoinvestigatethechargetransportinreducedgrapheneoxidethinfilms,
inordertoimprovethenext-generationgrapheneoxideinks forscreenprintingmacroscopic
electrodes.Itwasfound,thatbettercontroloverthephysicalpropertiesofthegrapheneoxide
inkwasofdemandforprintingofhighlytransparentandconductiveelectrodes.
Anotherfindingfromthechargetransportstudies,wasthatan improvedqualityofredu-
cedgrapheneoxideshowednearlytemperatureindependentchargetransport.Thisfinding
openedupforlowtemperatureconductancemeasurementsand InelasticElectronTunnelling
spectroscopyoflargeareamolecularmonolayers.
Theusabilityofgrapheneoxideinmolecularsolidstatedeviceswasfurtherinvestigated.It
wasshownthatasinglesheetofgrapheneoxidecouldfunction asamonoatomicprotectionlayer
inmolecularjunctions,preservingtheintegrityofthemolecularmonolayer.TheLangmuir-
Blodgetttechniquewasutilizedfortheassemblyandtransferofloosely-packedmonolayered
filmsofgrapheneoxidesheet.
Itwasinvestigatedwhethermonolayeredchemicalvapourdepositiongrowngraphenecould
beutilizedasalowelectric-fieldscreeningelectrode,intopgatedmolecularelectronicdevicesof
large-areaself-assembledmonolayersofmolecules.Sofar thefabricationofatopgateddevices
withoutmoleculeshasbeendemonstrated.Thegatingeffectin themonolayeredgraphene
electrodewasmeasuredforaseriesofdifferentdielectriclayers,inordertofindthemostsuitable
dielectricmaterialforthefabricationofverticalmolecularfield-effecttunnellingtransistors.
electrodematerialindifferentapplications.Itcanbedividedintotwomainapplications.The
firstisregardingprintingoflarge-areathinfilmsofreduced grapheneoxide,andtheelectron
conductanceofthese.Thesecondisfocussingonmolecularelectronicdevices,andhowgraphene
derivativescanbeimplementedasantopelectrode.
Large-areathinfilmsofreducedgrapheneoxidewereinvestigated,asapotentialmaterial
forfabricationoftransparentandflexibleelectrodesatan industrialscale.Differentvariations
oftheHummers’oxidationreactionwasutilizedtoproducegrapheneoxidefromgraphite.A
grapheneoxidesuspensionwasup-concentratedintoahighly viscousaqueousgrapheneoxide
ink.Theinkwasscreenprintedintomacroscopicelectrodestructures.Theinsulatinggraphene
oxideelectrodeswerereducedwithhydroiodicacidvapourintosemi-transparent,flexibleand
conductivereducedgrapheneoxideelectrodes.
Itwasshownthatmicroscopicstructuresinthethinfilms,introducedbytheprintingpro-
cess,influencedtheoptoelectronicpropertiesofthereducedgrapheneoxideelectrodes.The-
refore,wesetouttoinvestigatethechargetransportinreducedgrapheneoxidethinfilms,
inordertoimprovethenext-generationgrapheneoxideinks forscreenprintingmacroscopic
electrodes.Itwasfound,thatbettercontroloverthephysicalpropertiesofthegrapheneoxide
inkwasofdemandforprintingofhighlytransparentandconductiveelectrodes.
Anotherfindingfromthechargetransportstudies,wasthatan improvedqualityofredu-
cedgrapheneoxideshowednearlytemperatureindependentchargetransport.Thisfinding
openedupforlowtemperatureconductancemeasurementsand InelasticElectronTunnelling
spectroscopyoflargeareamolecularmonolayers.
Theusabilityofgrapheneoxideinmolecularsolidstatedeviceswasfurtherinvestigated.It
wasshownthatasinglesheetofgrapheneoxidecouldfunction asamonoatomicprotectionlayer
inmolecularjunctions,preservingtheintegrityofthemolecularmonolayer.TheLangmuir-
Blodgetttechniquewasutilizedfortheassemblyandtransferofloosely-packedmonolayered
filmsofgrapheneoxidesheet.
Itwasinvestigatedwhethermonolayeredchemicalvapourdepositiongrowngraphenecould
beutilizedasalowelectric-fieldscreeningelectrode,intopgatedmolecularelectronicdevicesof
large-areaself-assembledmonolayersofmolecules.Sofar thefabricationofatopgateddevices
withoutmoleculeshasbeendemonstrated.Thegatingeffectin themonolayeredgraphene
electrodewasmeasuredforaseriesofdifferentdielectriclayers,inordertofindthemostsuitable
dielectricmaterialforthefabricationofverticalmolecularfield-effecttunnellingtransistors.
Originalsprog | Engelsk |
---|
Forlag | Department of Chemistry, Faculty of Science, University of Copenhagen |
---|---|
Status | Udgivet - 2017 |