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 Jaeho Lee Tae-Hee Han Min-Ho Park Dae Yool Jung Jeongmin Seo Hong-Kyu Seo Hyunsu Cho Eunhye Kim Jin Chung Sung-Yool Choi Taek-Soo Kim Tae-Woo Lee Seunghyup Yoo Isishwankathelo I-OLED ezisekelwe kwigraphene zeqonga lokukhanya okusuka kwizinto eziphilayo (i-OLEDs) zivelile kutshanje njengeyona nto ibalulekileyo kwiziboniso ezilandelayo kunye nezibane, ikakhulu ngenxa yesithembiso sabo sokukhanya okuguquguqukayo. Nangona kunjalo, ukusebenza kwazo kube, ngcono, kufana nezo ziqhelekileyo, ezisekelwe kwi-indium tin oxide. Apha siphakamisa ulwakhiwo olugqwesileyo lwe-electrode olusekelwe kwidabi elinamandla leziciko ze-TiO2 ezine-index ephezulu kunye neziciko zokujova i-hole ezine-index ephantsi ezijikeleze ii-electrode zegraphene, nto leyo ekhokelela kwimeko egqwesileyo apho ukuphuculwa kokuthuthuka kwe-cavity kubekwe kwisilinganiso esiphezulu kodwa ilahleko kwii-plasmon polariton povr efakwe kwisikhumba yancitshiswa. Indlela enikiweyo ikhokelela kwi-OLEDs ezibonisa ukusebenza okuphezulu kwe-quantum yangaphandle ye-40.8 kunye ne-62.1% (64.7 kunye ne-103% kunye nelensi yebhola enesiqingatha) kusukelo kwi-single-kunye nezixhobo ze-multi-junction, ngokulandelanayo. I-OLEDs ezenziwe ngeplastiki kunye nezi-electrode zinokugoba ngokuphindaphindiweyo kwi-radius ye-2.3 mm, ngenxalenye ngenxa yeziciko ze-TiO2 ezinyamezela uxinzelelo lwe-flexural ukuya kutsho kwi-4% nge-crack-deflection toughening. Isingeniso Iingenelo zefom-factor ezinje ngokuguquguquka kunye nokutshona ziye zabangela ukuba iziboniso zokukhanya ezisekelwe kwizinto eziphilayo (i-OLEDs) zifumane ingqalelo enkulu kusetyenziso kwizixhobo ezivelayo ezinje ngeziboniso ezinokunxitywa, ezinokugungxulwa okanye ezinokugungxulwa ezifuna ukuhamba, ukuguquguquka kunye/okanye ukwandiswa , . Ukuzalisekiswa ngokupheleleyo kwesicelo esinjalo, nangona kunjalo, akunzima kwaye kufuna umzamo omkhulu kwiinkalo ezahlukeneyo ezifana nophuhliso lweetekhnoloji ze-transistor ezine-thin-film ezinobushushu obuphantsi kunye/okanye ukugquma okuguquguqukayo . Elinye inqaku elibalulekileyo ekufuneka ligqalwe kwiziboniso ezigugu kakhulu kukufumana ii-electrode ezicacileyo (i-TEs) ezinokutshintsha ii-electrode ze-indium tin oxide (ITO), ezihlala zineengxaki ngokuguquguquka okulinganiselweyo kunye neengxaki zexabiso ezinokubakho ngenxa yemfuno ephezulu kunye/okanye ukubonelelwa okungazinzanga . Ngolu hlobo, iintlobo ezininzi zee-electrode ezicacileyo neziyimfudumalo ezifana ne-metal nanowires, izinto eziqulunqwe yi-carbon (umzekelo, i-carbon nanotubes okanye igraphene) kunye ne-metal grids ezidibene nezinye iintlobo zee-TEs ziphakanyiswe kwi-OLEDs , , , , , . Phakathi kwezi, igraphene—isikhumba esingaqhelekanga se-carbon atoms ezine-sp2 hybridization—iye yabonwa njengento ethembisayo ngenxa yokudibanisa kwayo okukhethekileyo kobukhulu bayo obungaqhelekanga kunye neempawu zayo zombane ezibalaseleyo kulindeleke ukuba zivumelle ii-electrode ezicacileyo ezigqibeleleyo ezine-haze engabonakaliyo okanye ingekho, ubungqongileyo bomgangatho ongajijanga obuthintela ukulungiswa komsindo okubangelwa kukungalunganga kunye nokubola, ukudluliselwa okuphezulu, ukumelana nomgca ongaphantsi kunye nokuguquguquka okuphezulu konke ngaxeshanye , . Ukulungiswa okulula kwe-graphene ekumgangatho ophezulu kwii-substrates zeplastiki ezinkulu kuye kwaboniswa kutshanje kwi-electrode ezicacileyo ngeendlela ezihambelana nemveliso ngamashishini, kubonisa ukusebenza kwazo okusebenzayo , . Zombini i-single-layer graphene (i-SLG) kunye ne-multi-layer graphene (i-MLG) ziboniswe ukuba zinenqanaba elaneleyo lokusebenza kwi-TEs kwi-OLEDs , . Ngokukodwa, i-OLEDs eziphumeleleyo ezisekelwe kwigraphene ziye zafunyanwa ngoncedo lweziciko zokujova i-hole (i-HILs) ezisetyenziselwa ukoyisa ukumelana kwazo kwombane okungaphantsi, okwaziwayo ukuba malunga ne-4.5 eV. Ezi ziciko zokujova zibandakanya ii-polymers ezihambisa uombane kunye neempawu zombane eziguquguqukayo ezibizwa ngokuba yi-self-organized gradient HIL (GraHIL) , kunye neziciko ezincinci ze-buffer ze-MoO3 ezidibene nee-polymers ezihambisa uombane ze-poly(3,4-ethylenedioxythiophene): polystyrene sulfonate (PEDOT:PSS) . Nangona kunjalo, ukusebenza kwe-power kunye nokusebenza okuphezulu kwe-quantum (i-EQE) kwezi-OLEDs zigqwesileyo ezisekelwe kwigraphene zazisenje nezo ze-OLEDs ezisekelwe kwi-ITO, ngaphandle kokuba kusetyenziswe ilensi yebhola enkulu enesiqingatha ukuze kuphuculwe i-outcoupling . Ukuqinisekisa ukusebenza okuphezulu kangangoko kunokwenzeka kubaluleke kakhulu kwiziboniso ezigugu ezisetyenziselwa izicelo eziphathwayo kakhulu okanye ezinokunxitywa, njengoko zihlala zixhomekeke kubalelwa ibhetri enamandla omelelekileyo ngenxa yemida kubungqongileyo, ubunzima okanye iifom. Oku kufuna uphuhliso lolwakhiwo lwesi gizmo elinokwandisa ukusebenza kwe-OLEDs ezisekelwe kwigraphene. Ingxaki ephambili kukuyila ulwakhiwo okanye indlela yokukhupha izakhono zazo zembonakalo kwaye ugcine izibonelelo zegraphene kwii-form factors kangangoko kunokwenzeka. 1 2 3 4 4 5 6 7 8 9 10 11 11 12 13 14 13 14 14 Ngolu hlobo, apha siphanda ulwakhiwo olulula lwe-electrode olusekelwe kwiziciko ze-TiO2 ezinemindex ephezulu kunye nee-HILs ezine-index ephantsi ezijikeleze ii-electrode zegraphene. Ngoyilo lwembonakalo elithatha inzuzo epheleleyo yedabi elinamandla phakathi kweziciko eziphezulu nezingaphantsi ezilawula zombini i-resonance ye-cavity kunye nelahleko kwii-plasmon polariton (SPP), ii-OLEDs ezisekelwe kwigraphene eziphakanyisiweyo zibonisa i-EQE ephezulu engagqithisi apho kusetyenziswa igraphene njenge-electrode ecacileyo. Ngaphezu koko, ukumelana okuphezulu okungaqhelekanga kwe-TiO2 kuxinzelelo lwe-flexural kuboniswa okuvumela i-OLEDs zeplastiki ezingezizo kuphela ezisebenzayo kodwa kunye neziguquguqukayo. Iziphumo Uyilo lombonakalo we-OLEDs ezisekelwe kwigraphene eziphumeleleyo Ukusebenza kwe-OLEDs kulinganiselwe kwi-outcoupling efficiency ethile esoloko malunga ne-20% ngcono kwizixhobo ezinabashicileli abanjengayo. Phakathi kweendlela ezahlukeneyo zokuphucula i-outcoupling eziphakanyiswe ukuza kuthi ga ngoku , indlela esekelwe kwi-microcavity resonance inezibonelelo kuyo yokuba igcina ubume be-planar ngaphandle kokusebenzisa nakuphi na ukwakhiwa kwe-micro/nano okanye ulwakhiwo lwelensi ukuze ii-OLEDs ezenziwe ngayo zingabi naxesha lokuqala uombane kunye neziphumo ezimbalwa zembonakalo ezingafunekiyo kusetyenziso lwesiboniso (umzekelo, ukufiphaza, i-diffraction nokunye) kodwa zinokubonisa imibala engundoqo ebomvu (R), eluhlaza (G), eluhlaza okwesibhakabhaka (B) egqibeleleyo kunye nokusebenza okuphuculweyo , . Ngomphumo omncinci kodwa osasebenza kakhulu we-microcavity, ii-OLEDs ezisekelwe kwi-ITO zinokulungiswa ngokusebenza okuphezulu, ngaphandle kokubangela nayiphi na i-haze yembonakalo okanye ukufiphaza, ngokulungisa nje ubukhulu beziciko ze-ITO; kule nkqubo, i-first-order, i-3 /4 cavity design, apho i-  imele ubude bobude, ifunyanwa ngomngxuma ovulekileyo we-cavity mode obekwe kwi-ITO/substrate interface , . Kwiimeko ze-OLEDs ezingenayo i-ITO, ezisekelwe kwigraphene, ii-electrode zegraphene azikwazi ukwenziwa zibe zinkulu ngokwaneleyo ukulawula ubude be-cavity, nto leyo eyenza kube nzima ukuphucula ukusebenza ngomphumo we-resonance . 15 16 17 λ λ 18 19 20 Njengenye indlela, umntu angabeka isiciko esine-index yobude ephakamileyo ( H) ngaphantsi kweziciko zegraphene njengoko kubonisiwe kwi-  ngendlela efanayo neziciko ze-metal ezicwetyiweyo nge-dielectric , , , . Ngenxa yokuba ukukhanya kunokudlula kwigraphene kunye nobunzima obuncinci bokutshintsha kwesigaba ngenxa yobukhulu bayo obungaqhelekanga besiciko segraphene, i-3 /4 cavity design inokufumaneka ngokulula, umzekelo, kunye nobude bobude bomzimba be-organic kunye neziciko zokujova kunye nesiciko esine-index yobude ephakamileyo esibekwe malunga ne-2 /4 kunye ne- /4, ngokulandelanayo ( ). Ngokukodwa, isiciko esine-index ephezulu esine-‘ /4-thick’ sisebenza njengelensi yokubonisa engenayo i-metal, i-dielectric ekuvumela ukuba ibonise kakhulu kwindawo yendibano ye-electrode esezantsi ( bot) yokukhanya okungena kwiiziciko ze-organic, njengoko kunokuqinisekiswa kwii-graphs eziboniswe ezantsi kwe- . Oku kubonelela nge-OLEDs ezisekelwe kwigraphene ngezithuba zokwandisa ukusebenza kwazo ngomphumo we-resonance, ongayenziyo ngenye indlela. Kubonisiwe ukuba i- bot kunye nokuphuculwa kwe-resonance okuhambelanayo kuyanda kunye ne- H ( ). I-index yobude ephakamileyo ikwakhona iluncedo malunga nokuguquguquka njengoko ubude bomzimba obujoliswe kuko ( H H) bunokufunyanwa kunye nobunzima bomzimba obuncinci obungekho- H, kwaye ngenxa yokuba ukugoba okubangela ukuqhekeka kwesiciko esinye ngokubanzi kudla ngokubunjwa kwi-strain yokuqala ephantsi kunye nobunzima bomzimba obukhulu . Isiciko esine-index ephezulu esiphumeleleyo kwesi sigqibo kufuneka sibe ne- H enkulu kangangoko. Ngaphezu koko, kufuneka ibe nombala, kwaye, ngaphezu kwako konke, ayifanele yonakaliswe yinkqubo ethile yokudlulisa i-graphene. Phakathi kwezinto ezininzi ezinokubakho, isiciko se-TiO2 esiboshiweyo sikhona esibonakala kumda wobude obubonakalayo kwaye sine-index yobude ephakamileyo ( =2.5). Ngokungafaniyo nezinye iziciko eziphakamileyo esizizamileyo, isiciko se-TiO2 sibonakala sinokumelana nemichiza okunzima ukuba sibekho kwiinkqubo zokudlulisa i-graphene ezisebenzisa ulwelo, ezifana ne-acetone okanye i-isopropyl alcohol (IPA), sivumela ukubunjwa kwe-electrode yegraphene ekumgangatho ophezulu phezu kwayo ( ). n Fig. 1a 17 20 21 22 λ λ λ Fig. 1b λ R Fig. 1c,d R n Supplementary Fig. 1 n d d 23 n n Supplementary Fig. 2   ( ) Umyalezo ongqongqo wesakhiwo ses Gizmo se-OLEDs eziphakanyisiweyo. ( ) Ukusasazwa kwamandla ombane (imigca eyahlukileyo) ye-OLEDs phantsi kophando kwi-design yabo yokuqala ye-cavity. Ukusasazwa kwamandla ombane we-OLEDs ezisekelwe kwigraphene ngaphandle kwe-TiO2 kuboniswa kunye nokuboniswa kwimeko apho ubukhulu beziciko ze-organic ziyafana neze-OLEDs kunye ne-TiO2 kodwa ngaphandle kwe-HIL enomthamo ongaphantsi. ( , ) Ukuqikelelwa okuphezulu kwe-quantum efficiency yangaphandle ( EQE) ye-OLEDs ezisekelwe kwigraphene kunye ne-TiO2 phantsi njengomsebenzi wobukhulu be-TiO2 kunye no-organic ( TiO2 kunye no- org, ngokulandelanayo). Imigca eyahlukileyo imele imigca ye-contour ye- EQE ye-10, 20, 30 okanye 40% njengoko kuchaziwe kwigrafti. ( ) Ngaphandle kwe-HIL enomthamo ongaphantsi; ( ) kunye ne-GraHIL njenge-HIL enomthamo ongaphantsi. Ezantsi kwimeko nganye, ukubonakaliswa ( bot) kwindibano ye-electrode esezantsi (TiO2/graphene/(HIL)) iyonke iboniswa njengomsebenzi we- TiO2 wokukhanya okungena kwiiziciko ze-organic. a b c d η d d η c d R d Kubalulekile ukuba i-micro-cavity structure yomyalelo ophezulu (umzekelo, umyalelo wesibini, i-5 /4 cavity) esekelwe kwisiqwenga esikhulu se-organic kunokwenzeka. Kulo msebenzi, nangona kunjalo, i-first-order cavity design yagqitywa kuqala kuba iye yavelisa i-Purcell effect eyomeleleyo kwaye yaba nemixholo ye-waveguide encinci kuneyo yommiselo ophezulu, ekugqibeleni ikhokelela kwi-outcoupling efficiency kunye ne-EQE enkulu , . Iingxaki zisasele zikhona kwi-first-order cavity design kuba indawo egqibeleleyo yendawo yokukhutshwa ibe mda kwindawo yokuqala ye-antinode ukusuka kwi-organic/metal interface, yenza kube nzima ukunciphisa imixholo ye-SPP ngomgama omde we-emitter-to-metal , . Indlela enye esetyenziswa ngokuqhelekileyo ekunciphiseni i-SPP kukudibanisa ii-structures zangaphakathi ezijijwayo okanye i-corrugations , kodwa ukunyamezela kwi-shorts zombane kunokungahambelani ngezindlela ezinjalo. Indlela esiyisebenzisayo apha kukudibanisa isiciko esine-index yobude obuphantsi, esibonisiwe ukuba sinciphisa ngokufanelekileyo imixholo ye-SPP , . Ngokuthamsanqelayo, i-GraHIL okanye i-self-organized gradient hole-injection layer equkethe i-PEDOT:PSS kunye ne-tetra-fluoroethylene-perfluoro-3, 6-dioxa-4-methyl-7-octenesulphonic acid copolymer (PFI), eyayiphakanyiswe ngaphambili ngababhali kwaye yabonisa ukuba isebenza kakhulu ekuphuculeni ukujotshwa kwem Hole kwi-OLEDs ezisekelwe kwigraphene , ine-index yobude malunga ne-1.42 kwi-  ye-550 nm ( ), nto leyo engaphantsi kakhulu kunezo zee-organic layers eziqhelekileyo ( =1.8). Ngodlame olunamandla phakathi kweziciko ze-index ephezulu (H) ze-TiO2 kunye ne-index ephantsi (L) ze-GraHIL ezijikeleze ii-graphene layers, ukuphuculwa komphumo we-cavity resonance kunye nokunciphiswa kwe-SPP modes kungadibaniswa ngaxeshanye ukuze i-EQE inokuphuculwa kakhulu nangaphandle kweziciko zokukhupha. λ 24 25 25 26 27 28 29 13 λ Supplementary Fig. 3 n  bubonisa iziphumo zokulinganisa imbonakalo ngokusekelwe kumgaqo omkhulu we-classical electromagnetic theory oqukunjelwe nguFurno .  kulo lonke ubude obubonakalayo bobude, kwaye kwi-  ye-550 nm. Ifomula iqwalasela i-Purcell factor, i-dipole orientation effect, kunye neziyobisi kwi-SPP kunye nemixholo ye-waveguide. Ukubandakanya ngokupheleleyo kwezi zinto zonke kubaluleke kakhulu kuhlalutyo oluchanekileyo kunye noyilo olunokulinganiselwa njengoko i-under- okanye i-overestimation ingenzeka xa kusetyenziswa indlela elula engabandakanyiyo enye okanye ngaphezulu kwezi ziphumo (bona  ;   kunye   kwimizekelo). Iziphumo zibonisa ukuba ukusetyenziswa kwe-GraHIL kubuyisela ubuninzi bamandla phakathi kweemode ezahlukeneyo ukuya kwi-wave vectors ezingaphantsi kakhulu ukuze amandla angene kwi-SPP modes ancitshiswe kwaye iziphumo ezikhuphukayo ziphuculwe ngakumbi ( ). Kungabonwa kwakhona kwi-  ukuba ukusetyenziswa kwesiciko se-TiO2 ngaphantsi kwegraphene kucinezela ngokufanelekileyo ubungakanani bamandla angena kwi-waveguided kunye ne-substrate modes ngokuphuculwa kwe-resonance. Oku kukhokelela ekwandeni okukhulu kwe-outcoupling efficiency, nangona ilahleko kwii-evanescent modes nayo iboniswe ukuba iyanda ngenxa yotshintsho lwee-transverse-electric waveguided modes ukuya kwi-in-plane wave vectors ephezulu ( ). Ukudibanisa ukusetyenziswa kwe-index ephezulu (H) i-TiO2 kunye ne-index ephantsi (L) i-GraHIL layers, kuvelisa imeko egqibeleleyo apho ukuphuculwa kwe-resonance kukhulu, kodwa ilahleko kwii-SPP/evanescent modes iyancitshiswa. Ukongeza, ukudibanisa ukusetyenziswa kudala imeko efana ne HL-stacks, esetyenziswa ngokuqhelekileyo kulwelo lwe-thin-film coating , kwaye uphucula ngakumbi i- bot ( ), ivumela ukuphuculwa okongeziweyo kumphumo we-Fabry–Perot resonance effect. Oko kwenza ubuchwepheshe obuphakanyisiweyo bube yikhethekileyo kwaye buphumeleleyo xa kuthelekiswa nobuchwepheshe obuqhelekileyo kukudibana okunamandla kwezi ziciko eziphezulu nezingaphantsi ezivumela ulawulo lombonakalo lwe-resonance effect kunye nelahleko ye-SPP ukuya kwisibonelelo sokukhutshwa okuphezulu; kunye nokuphuculwa kwe-resonance eyongezelelweyo nge HL stacking. Kunye neenqwelo zabo zokudibanisa nezicelo zombane ezifunekayo (umzekelo, i-hole injection esebenzayo), zonke ezi zibonelelo zembonakalo zivumela umntu ukuba aphumeze ngokupheleleyo ngisho ne-potential efihliweyo ye-OLEDs ze-planar ezinokubonelela ngokwenyani. I-Contour plots ezifunyenweyo zeqhudelelo ye-EQE ephezulu enokwenzeka ( EQE(max)) njengomsebenzi wobukhulu be-organic ( org) kunye nobukhulu be-TiO2 ( TiO2) eziboniswe kwi-  zibonisa ukuba i- EQE(max) ingaba phezulu njenge-44% kwizixhobo ezine-GraHIL kunye ne-TiO2 layers ngelixa ingabakho kwi-38% ngaphandle kwe-GraHIL okanye kwi-31% ngaphandle kwe-TiO2. Iimeko ezingcono ziyahambelana nemeko apho i- H (kunye ne-H ibe yi-TiO2) isondela kwi- /(4 H) (55 nm ye- =550 nm). Kungabonwa kwakhona ukuba i- EQE(max) ye-44% iphezulu kunezo zilindelekileyo kwi-optimized, i-OLEDs ze-metal ezisekelwe kwi-cavity kunye nomshicileli ofanayo. Oku kunokubangelwa yinyani yokuba ulwakhiwo oluphakanyisiweyo alubandakanyeki kulahleko ngenxa yokufunxa kwamandla okanye/okanye ukukhutshwa komxholo we-SPP kwi-electrodes ezicacileyo (bona   kunye   ukuboniswa kwezo ze-OLEDs ze-cavity ezisekelwe kwi-metal ezisekelwe kwi-metal). Umfanekiso 2a,b  et al 19 λ Supplementary Fig. 4 Supplementary Table 1 Supplementary Note 1 Supplementary Fig. 5a Supplementary Table 2 Supplementary Fig. 5b 30 R Fig. 1d η d d Fig. 1c,d η d λ n λ η Supplementary Fig. 6 Supplementary Table 3  

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