Izinto ezinezinhlangothi ezimbili, njenge-graphene, zikhanga kukho kokubili izinhlelo zokusebenza ezivamile ze-semiconductor kanye nezinhlelo ezisafufusa kuma-electronics flexible.Kodwa-ke, amandla aqinile we-graphene aphumela ekuqhekekeni kobunzima obuphansi, okwenza kube inselele ukusizakala ngezakhiwo zayo ze-elekthronikhi ezingajwayelekile kuma-elekthronikhi anwebekayo.Ukuze unike amandla ukusebenza okuhle kakhulu okuncike kuhlobo lwamakhondaktha we-graphene abonisa ngale, sidale ama-graphene nanoscroll phakathi kwezendlalelo ze-graphene ezistakiwe, ezibizwa ngokuthi i-multilayer graphene/graphene scrolls (MGGs).Ngaphansi kokucindezeleka, eminye imiqulu ibhuloho izizinda ezihlukene ze-graphene ukuze kugcinwe inethiwekhi ye-percolating evumela ukusebenza okuhle kakhulu ezinkingeni eziphezulu.Ama-MGG e-Trilayer asekelwa kuma-elastomers agcine u-65% wokuqhuba kwawo kwasekuqaleni ku-100% strain, okuhambisana nesiqondiso sokugeleza kwamanje, kanti amafilimu ama-trilayer e-graphene ngaphandle kwe-nanoscroll agcine kuphela u-25% wokuqhuba kwawo kokuqala.I-all-carbon transistor enwebekayo eyenziwe kusetshenziswa ama-MGG njengama-electrode ibonise ukudluliswa kwe->90% futhi igcine u-60% womkhiqizo wayo wamanje ongu-120% wobunzima (okuhambisana nendawo yokuthutha imali).Lawa ma-transistors ekhabhoni anwebeka kakhulu futhi asobala anganika amandla ama-optoelectronics anwebekayo anwebekayo.
I-elekthronikhi ebonakalayo enwebekayo iyinkambu ekhulayo enezinhlelo zokusebenza ezibalulekile kumasistimu ahlanganisiwe we-biointegrated (1, 2) kanye namandla okuhlanganisa nama-optoelectronics anwebekayo (3, 4) ukuze kukhiqizwe amarobhothi athambile nezibonisi.I-Graphene ibonisa izinto ezifiseleka kakhulu zokujiya kwe-athomu, ukukhanya okuphezulu, kanye nokusebenza okuphezulu, kodwa ukuqaliswa kwayo ezinhlelweni ezinwebekayo kuvinjelwe ukuthambekela kwayo kokuqhekeka emigudwini emincane.Ukunqoba imikhawulo yemishini ye-graphene kunganika amandla ukusebenza okusha kumadivayisi abonisa ngale anwebekayo.
Izakhiwo eziyingqayizivele ze-graphene ziyenza ibe ikhandidethi eliqinile esizukulwaneni esilandelayo sama-electrode conductive esobala (5, 6).Uma kuqhathaniswa ne-conductor esobala evame ukusetshenziswa kakhulu, i-indium tin oxide [ITO;100 ohms/square (sq) ekukhanyeni okungu-90% ], i-monolayer graphene ekhuliswe i-chemical vapor deposition (CVD) inenhlanganisela efanayo yokumelana neshidi (125 ohms/sq) nokukhanyela (97.4%) (5).Ngaphezu kwalokho, amafilimu e-graphene anokuguquguquka okungajwayelekile uma kuqhathaniswa ne-ITO (7).Isibonelo, ku-substrate yepulasitiki, ukuqhutshwa kwayo kungagcinwa ngisho nendawo egobileyo yokugoba encane njengo-0.8 mm (8).Ukuze kuqhutshekwe kuthuthukiswe ukusebenza kwawo kukagesi njengomqhubi okhanyelayo oguquguqukayo, imisebenzi yangaphambilini ithuthukise izinto ezixubile ze-graphene ezinama-nanowires esiliva owodwa-ubude (1D) noma i-carbon nanotubes (CNTs) (9–11).Ngaphezu kwalokho, i-graphene isetshenziswe njengama-electrodes kuma-semiconductors e-heterostructural exubile (njenge-2D bulk Si, 1D nanowires/nanotubes, namachashazi angu-0D quantum ) (12), ama-flexible transistors, amaseli elanga, nama-light-emitting diode (LEDs) (13) -23).
Nakuba i-graphene ibonise imiphumela ethembisayo ye-electronics eguquguqukayo, ukusetshenziswa kwayo ku-elekthronikhi enwebekayo kunqunyelwe izakhiwo zayo zemishini (17, 24, 25);I-graphene inokuqina kwendiza okungu-340 N/m kanye nemoduli Yentsha engu-0.5 TPa ( 26).Inethiwekhi ye-carbon-carbon eqinile ayinikezi noma yiziphi izindlela zokulahla amandla obunzima obusetshenzisiwe futhi ngenxa yalokho iqhekeka kalula ngaphansi kobunzima obungu-5%.Isibonelo, i-CVD graphene edluliselwe ku-polydimethylsiloxane (PDMS) enwebekayo substrate ingagcina kuphela ukusebenza kwayo ngaphansi kobunzima obungu-6% (8).Izibalo zetiyori zibonisa ukuthi ukushwabana nokuhlangana phakathi kwezendlalelo ezihlukene kufanele kwehlise kakhulu ukuqina (26).Ngokunqwabelanisa i-graphene izendlalelo eziningi, kubikwa ukuthi le graphene ye-bi- noma i-trilayer inwebeka ibe uhlobo lwama-30%, ikhombisa ukushintshwa kokumelana okuphindwe izikhathi eziyi-13 kune-monolayer graphene (27).Kodwa-ke, lokhu kunwebeka kusengaphansi kakhulu kuma-c onductors we-state-of-the-art anwebekayo (28, 29).
Ama-Transistors abalulekile ezinhlelweni ezinwebekayo ngoba anika amandla ukufundwa kwenzwa okuyinkimbinkimbi nokuhlaziya isignali (30, 31).Ama-transistors ku-PDMS ane-multilayer graphene njengomthombo/drain electrode kanye nezinto zesiteshi zingagcina ukusebenza kukagesi kufikela ku-5% uhlobo (32), okungaphansi Ngokuphawulekayo kwenani elincane elidingekayo (~50%) lezinzwa zokuqapha impilo ezigqokekayo nesikhumba sikagesi ( 33, 34).Muva nje, kuhlolwe indlela ye-graphene kirigami, futhi i-transistor efakwe i-electrolyte ewuketshezi inganwetshwa ifike ku-240% (35).Nokho, le ndlela idinga i-graphene emisiwe, eyenza inqubo yokwenziwa ibe nzima.
Lapha, sifinyelela amadivayisi e-graphene anwebeka kakhulu ngokuhlanganisa imiqulu ye-graphene (~1 ukuya ku-20 μm ubude, ~0.1 ukuya ku-1 μm ububanzi, kanye no-10 ukuya ku-100 nm ukuphakama) phakathi kwezingqimba ze-graphene.Sicabanga ukuthi le miqulu ye-graphene inganikeza izindlela ezisebenzayo zokuvala imifantu kumashidi e-graphene, ngaleyo ndlela igcine ukusebenza okuphezulu ngaphansi kobunzima.Imiqulu ye-graphene ayidingi ukuhlanganiswa okwengeziwe noma inqubo;zakhiwe ngokwemvelo phakathi nenqubo yokudlulisa okumanzi.Ngokusebenzisa i-multilayer G/G (graphene/graphene) scroll (MGGs) ama-electrode anwebekayo e-graphene (umthombo/udoti kanye nesango) kanye nama-CNTs e-semiconducting, sikwazile ukukhombisa ama-transistors e-carbon yonke abonakala esobala kakhulu futhi anwebeka kakhulu, anganwetshwa aze afike ku-120. % uhlobo (oluhambisana nendawo yokushaja ezokuthutha) futhi igcine u-60 % womkhiqizo wayo wamanje wangempela.Lena i-transistor esekwe ku-carbon-based esobala kakhulu elula kakhulu kuze kube manje, futhi inikeza okwamanje okwanele ukushayela i-LED ye-inorganic.
Ukuze unike amandla ama-electrode e-graphene anwebekayo endaweni enkulu, sikhethe i-graphene ekhule i-CVD ku-Cu foil.I-Cu foil imisiwe maphakathi neshubhu le-quartz le-CVD ukuze kuvunyelwe ukukhula kwe-graphene nhlangothi zombili, kwakheka izakhiwo ze-G/Cu/G .Ukuze sidlulisele i-graphene, siqale saphotha ungqimba oluncane lwe-poly(methyl methacrylate) (PMMA) ukuze sivikele uhlangothi olulodwa lwe-graphene, esiluqambe ngokuthi yi-topside graphene (okuphambene nolunye uhlangothi lwe-graphene), futhi kamuva, yonke ifilimu (PMMA/top graphene/Cu/bottom graphene) yacwiliswa ku-(NH4)2S2O8 isisombululo ukuze kukhishwe i-Cu foil.Igraphene eseceleni elingezansi ngaphandle kokunamatheliswa kwe-PMMA nakanjani izoba nemifantu kanye nokukhubazeka okuvumela i-etchant ukuthi ingene (36, 37).Njengoba kubonisiwe ku-Fig. 1A, ngaphansi komthelela wokudonsa phezulu, izizinda ze-graphene ezikhishiwe zagoqwa zaba imiqulu futhi ngemva kwalokho zanamathiselwa kufilimu esele ye-top-G/PMMA.I-top-G/G scrolls ingadluliselwa kunoma iyiphi i-substrate, efana ne-SiO2/Si, ingilazi, noma i-polymer ethambile.Ukuphinda le nqubo yokudlulisa izikhathi eziningana ku-substrate efanayo kunikeza izakhiwo ze-MGG.
(A) Umdwebo wohlelo lwenqubo yokwenziwa kwama-MGG njenge-electrode elula.Ngesikhathi sokudlulisa i-graphene, i-graphene engemuva ku-Cu foil yaphulwa emingceleni nasemigqeni, yagoqwa yaba yizimo ezingafanele, futhi yanamathiselwa ngokuqinile kumafilimu angaphezulu, kwakheka ama-nanoscroll.Ikhathuni yesine ikhombisa isakhiwo se-MGG esistakiwe.(B kanye no-C) Izimpawu ze-TEM zokucaca okuphezulu kwe-MGG ye-monolayer, egxile ku-monolayer graphene (B) kanye nesifunda somqulu (C), ngokulandelanayo.I-inset ethi (B) yisithombe esikhulisa kancane esibonisa ukumila kwemvelo okuphelele kwama-MGG we-monolayer kugridi ye-TEM.Ama-inset of (C) amaphrofayili okuqina athathwe ngamabhokisi angunxande akhonjiswe esithombeni, lapho amabanga phakathi kwezindiza ze-athomu engu-0.34 kanye no-0.41 nm.(D ) I-Carbon K-edge EEL spectrum enesici somfanekiso π* kanye no-σ* iziqongo ezinelebulwe.(E) Isithombe se-AFM sesigaba sokuskrola kwe-G/G ye-monolayer enephrofayela yobude eduze komugqa wamachashazi aphuzi.(F kuya ku-I) Imakhrokhophu yokubona nesithombe se-AFM sika-trilayer G ngaphandle kokuthi (F no-H) kanye nemiqulu (G kanye ne-I) kuma-substrates angu-300-nm-thick SiO2/Si, ngokulandelanayo.Imiqulu emele abanye kanye nemibimbi yayibhalwe ukuze kugqanyiswe umehluko wakho.
Ukuqinisekisa ukuthi imiqulu iyi-graphene egoqiwe ngokwemvelo, senze izifundo ze-electron microscopy (TEM) yokudlulisa amandla aphezulu kanye nokulahlekelwa kwamandla e-electron (EEL) ezakhiweni zokuskrola ze-monolayer top-G/G.Umfanekiso 1B ubonisa ukwakheka kwe-hexagonal ye-graphene ye-monolayer, futhi isethi iyinhlangano ye-morphology iyonke yefilimu embozwe emgodini owodwa wekhabhoni wegridi ye-TEM.I-graphene ye-monolayer inweba ingxenye enkulu yegridi, futhi amanye ama-graphene flakes phambi kwezitaki eziningi zamasongo angama-hexagonal avela (Fig. 1B).Ngokusondeza emqulwini ngamunye (Fig. 1C), sibone inani elikhulu lamaphethelo e-graphene lattice, nesikhala se-lattice kububanzi obungu-0.34 kuya ku-0.41 nm.Lezi zilinganiso ziphakamisa ukuthi ama-flakes asongwa ngokungahleliwe futhi awawona ama-graphite aphelele, anesikhala se-lattice esingu-0.34 nm ku-"ABAB" ekustakhikeni kongqimba.Umfanekiso 1D ubonisa i-carbon K-edge EEL spectrum, lapho ukuphakama okungu-285 eV kuvela ku-π* orbital kanti enye eduze kuka-290 eV kungenxa yokushintshwa kwe-orbital σ*.Kuyabonakala ukuthi i-sp2 bonding ibusa kulesi sakhiwo, iqinisekisa ukuthi imiqulu inemifanekiso eminingi.
I-Optical microscopy kanye ne-atomic force microscopy (AFM) izithombe zinikeza ukuqonda mayelana nokusatshalaliswa kwe-graphene nanoscroll kuma-MGGs (Umfanekiso 1, E kuya ku-G, namakhiwane. S1 kanye ne-S2).Imiqulu isakazwa ngokungahleliwe phezu kwendawo, futhi ukuminyana kwayo endizeni kukhuphuka ngokulingana nenani lezendlalelo ezistakiwe.Imiqulu eminingi iphithene ibe amafindo futhi ibonise ubude obungajwayelekile kububanzi obungu-10 kuye ku-100 nm.Zingu-1 kuya ku-20 μm ubude no-0.1 kuya ku-1 μm ububanzi, kuye ngobukhulu bama-graphene flakes awo okuqala.Njengoba kuboniswe ku-Fig. 1 (H no-I), imiqulu inosayizi abakhulu kakhulu kunemibimbi, okuholela ekuxhumaneni okuqinile phakathi kwezingqimba zegraphene.
Ukuze silinganise izici zikagesi, senze iphethini amafilimu e-graphene anezakhiwo zokuskrola noma ngaphandle kwazo kanye nesendlalelo esinqwabelene sibe yimichilo engu-300-μm-wide kanye ne-2000-μm-ubude sisebenzisa i-photolithography.Ukumelana nama-probe amabili njengomsebenzi wobunzima kuye kwalinganiswa ngaphansi kwezimo ezizungezile.Ukuba khona kwemiqulu kunciphise ukumelana ne-monolayer graphene ngo-80% ngokuncipha kwe-2.2% kuphela ekudluliseni (fig. S4).Lokhu kuqinisekisa ukuthi ama-nanoscroll, anomthamo omkhulu wamanje kuze kufike ku-5 × 107 A/cm2 (38, 39), enza umnikelo omuhle kakhulu kagesi kuma-MGG.Phakathi kwazo zonke i-mono-, bi-, kanye ne-trilayer plain graphene kanye nama-MGG, i-MGG ye-trilayer inokuqhuba okuhle kakhulu nokungafihli cishe okungama-90%.Ukuze siqhathanise neminye imithombo ye-graphene ebikwe ezincwadini, siphinde salinganisa ukuphikiswa kweshidi le-probe emine (fig. S5) futhi sabhala njengomsebenzi wokudlulisa ku-550 nm (fig. S6) ku-Fig. 2A.I-MGG ikhombisa ukusebenza okuqhathanisekayo noma okuphezulu nokuba sobala kune-graphene enqwabelene eyenziwe nge-multila yer plain kanye ne-graphene oxide encishisiwe (RGO) (6, 8, 18).Qaphela ukuthi ukuphikiswa kweshidi le-graphene engenalutho estakiwe eyenziwe yakhiwe ngezigaba eziningi kuphezulu kancane kunokwe-MGG yethu, mhlawumbe ngenxa yezimo zabo zokukhula ezingalungiselelwe kanye nendlela yokudlulisa.
(A) Ukumelana neshidi elineprobe emine uma kuqhathaniswa nokudluliswa kwedatha ku-550 nm ngezinhlobo ezimbalwa zegraphene, lapho izikwele ezimnyama zisho ama-MGG ama-mono-, bi-, kanye nama-trilayer;imibuthano ebomvu nonxantathu abaluhlaza bahambisana ne-multilayer plain graphene etshalwe ku-Cu no-Ni kusukela ezifundweni zika-Li et al.(6) kanye noKim et al.(8), ngokulandelana, futhi kamuva idluliselwe ku-SiO2/Si noma i-quartz;kanye nonxantathu abaluhlaza bangamagugu e-RGO ngamadigri ahlukene okunciphisa kusukela ocwaningweni lukaBonaccorso et al.(18).(B no-C) Ukushintsha kokumelana okujwayelekile kwe-mono-, bi- kanye ne-trilayer MGGs kanye no-G njengomsebenzi we-perpendicular (B) kanye ne-parallel (C) ubunzima ekuqondeni kokugeleza kwamanje.(D) Ukushintsha kokumelana okujwayelekile kwe-bilayer G (bomvu) ne-MGG (emnyama) ngaphansi kobunzima be-cyclic ukulayisha kufika ku-50% uhlobo lwe-perpendicular.(E) Ukushintsha kokumelana okujwayelekile kwe-trilayer G (bomvu) ne-MGG (emnyama) ngaphansi kwe-cyclic strain elayisha kufika ku-90% uhlobo oluhambisanayo.(F) Ukushintsha kwamandla okujwayelekile kwe-mono-, i-bi- kanye ne-trilayer G kanye ne-bi- kanye ne-trilayer MGGs njenge-functio n yobunzima.I-inset iyisakhiwo se-capacitor, lapho i-polymer substrate iyi-SEBS kanye nongqimba lwe-polymer dielectric luyi-SEBS engu-2-μm-thick.
Ukuze sihlole ukusebenza kwe-MGG okuncike ku-strain, sidlulisele i-graphene ku-thermoplastic elastomer styrene-ethylene-butadiene-styrene (SEBS) substrates (~2 cm ububanzi no-~5 cm ubude), futhi conductivity kukalwa njengoba i-substrate yeluliwe. (bheka Izinto Ezisetshenziswayo Nezindlela) kokubili i-perpendicular futhi ihambisana nesiqondiso sokugeleza kwamanje (Umfanekiso 2, B no-C).Ukuziphatha kukagesi okuncike kubunzima kuye kwaba ngcono ngokufakwa kwama-nanoscroll kanye nezinombolo ezikhulayo zezendlalelo ze-graphene.Isibonelo, lapho ubunzima buhambisana nokugeleza kwamanje, ku-monolayer graphene, ukungezwa kwemiqulu kwandisa ubunzima ekuqhekekeni kukagesi kusuka ku-5 kuya ku-70%.Ukubekezelela ubunzima kwe-trilayer graphene nakho kuthuthuke kakhulu uma kuqhathaniswa ne-monolayer graphene.Nge-nanoscroll, ngo-100% we-perpendicular strain, ukumelana kwesakhiwo se-MGG se-trilayer kukhuphuke ngo-50% kuphela, uma kuqhathaniswa no-300% we-trilayer graphene ngaphandle kwemiqulu.Ukuguqulwa kokumelana ngaphansi komthwalo we-cyclic straining kuye kwaphenywa.Ukuze uqhathanise (Fig. 2D), ukumelana nefilimu ye-plain bilayer graphene kukhuphuke cishe izikhathi ezingu-7.5 ngemva kwemijikelezo engu-700 ku-50% we-perpendicular strain futhi kwaqhubeka kwanda ngokucindezeleka kumjikelezo ngamunye.Ngakolunye uhlangothi, ukumelana kwe-bilayer MGG kukhuphuke cishe izikhathi ezingu-2.5 ngemva kwemijikelezo engu-700.Isebenzisa kufika ku-90% uhlobo oluhambisana nendlela efanayo, ukumelana kwe-trilayer graphene kukhuphuke ~ izikhathi ezingu-100 ngemva kwemijikelezo engu-1000, kuyilapho kuyizikhathi ezingu ~ 8 kuphela ku-trilayer MGG (Fig. 2E).Imiphumela yamabhayisikili iboniswa ku fig.S7.Ukwenyuka okushesha kakhulu kokuphikiswa ngakundlela yohlobo olufanayo kungenxa yokuthi umumo wemifantu uncike kuhlangothi lokugeleza kwamanje.Ukuchezuka kokumelana ngesikhathi sokulayisha nokuthulula kudalwa ukutholwa kwe-viscoelastic kwe-SEBS elastomer substrate.Ukumelana okuzinzile kwamapheshana e-MGG ngesikhathi sokuhamba ngebhayisikili kungenxa yokuba khona kwemiqulu emikhulu engakwazi ukuhlanganisa izingxenye eziqhekekile ze-graphene (njengoba i-obse rved by AFM), isiza ukugcina indlela ye-percolating.Lesi senzo sokugcina ukuguquguquka kwendlela yokubhoboza sike sabikwa ngaphambili kumafilimu ensimbi aqhekekile noma ama-semiconductor kuma-elastomer substrates (40, 41).
Ukuze sihlole lawa mafilimu asekelwe ku-graphene njengama-electrode asesangweni kumadivayisi anwebekayo, simboze isendlalelo se-graphene ngesendlalelo se-dielectric se-SEBS (ubukhulu obungu-2 μm) futhi saqapha ushintsho lwe-dielectric capacitance njengomsebenzi wobunzima (bona i-Fig. 2F kanye Nezisetshenziswa Ezingeziwe ze-Supplementary Materials for imininingwane).Siqaphele ukuthi amandla anama-electrode e-monolayer angenalutho kanye nama-electrode e-graphene e-bilayer ehla ngokushesha ngenxa yokulahlekelwa ukuqhutshwa kwe-graphene endizeni.Ngokuphambene, amandla afakwe i-MGGs kanye ne-plain trilayer graphene abonise ukukhuphuka kwe-capacitance ngobunzima, okulindeleke ngenxa yokuncipha kogqinsi lwe-dielectric kanye nobunzima.Ukwanda okulindelekile ku-capacitance kufanelana kahle kakhulu nesakhiwo se-MGG (fig. S8).Lokhu kubonisa ukuthi i-MGG ifaneleka njenge-electrode yesango lama-transistors alula.
Ukuze kuqhutshekwe kuphenywe indima yokuskrola kwe-graphene ye-1D ekubekezeleni kobunzima bokuhamba kukagesi nokulawula kangcono ukuhlukana phakathi kwezendlalelo ze-graphene, sisebenzise ama-CNT afakwe isifutho ukuze amiselele imiqulu ye-graphene (bona Izinto Ezingeziwe).Ukulingisa izakhiwo ze-MGG, sibeke ukuminyana okuthathu kwama-CNTs (okungukuthi, i-CNT1
(A ukuya ku-C) Izithombe ze-AFM zokuminyana okuthathu okuhlukene kwama-CNTs (CNT1
Ukuze siqhubeke siqonde amandla azo njengama-electrodes wezinto zikagesi ezinwebekayo, siphenye ngokuhlelekile i-morphologies ye-MGG ne-G-CNT-G ngaphansi kobunzima.I-Optical microscopy kanye ne-electron microscopy (SEM) yokuskena akuzona izindlela zokufaka izinhlamvu eziphumelelayo ngenxa yokuthi zombili azinakho ukugqama kombala futhi i-SEM ingaphansi kwezithombe zobuciko phakathi nokuskena i-electron lapho i-graphene iku-polymer substrates (amakhiwane. S9 kanye ne-S10).Ukuze ubuke endaweni ye-graphene ngaphansi kokucindezeleka, siqoqe izilinganiso ze-AFM kuma-MGG angama-trilayer kanye ne-graphene engenalutho ngemva kokudlulisela kuma-substrates amancane kakhulu (~0.1 mm) nama-SEBS anwebekayo.Ngenxa yokukhubazeka kwangaphakathi ku-CVD graphene kanye nokulimala kwangaphandle phakathi nenqubo yokudlulisa, imifantu ikhiqizwa ngokungenakugwenywa ku-graphene ehlutshiwe, futhi ngokucindezeleka okwandayo, imifantu yaba minyene (Fig. 4, A kuya ku-D).Kuye ngesakhiwo sokupakisha sama-electrodes asekelwe ku-carbon, imifantu ibonisa i-morphologies ehlukene (umkhiwane S11) (27).Ukuminyana kwendawo yokuqhekeka (echazwa njengendawo yokuqhekeka/indawo ehlaziywe) ye-graphene ye-multilayer incane kunaleyo ye-monolayer graphene ngemva kobunzima, obuhambisana nokwanda kokusebenza kukagesi kuma-MGG.Ngakolunye uhlangothi, imiqulu ivame ukubhekwa ukuze ivale imifantu, inikeze izindlela ezengeziwe zokuqhuba ifilimu ehlungiwe.Isibonelo, njengoba kubhalwe emfanekisweni we-Fig. 4B, umqulu obanzi wawela umfantu ku-MGG ye-trilayer, kodwa awukho umqulu owabonwa ku-graphene ethafeni (Fig. 4, E kuya ku-H).Ngokufanayo, ama-CNT aphinde avala imifantu ku-graphene (fig. S11).Ukuminyana kwendawo yokuqhekeka, ukuminyana kwendawo yokuskrola, kanye nokuqina kwamafilimu kufinyezwa ku-Fig. 4K.
(A ukuya ku-H) Ku-situ ye-AFM izithombe ze-trilayer G/G scrolls (A ukuya ku-D) kanye nezakhiwo ze-trilayer G (E ukuya ku-H) ku-SEBS ezacile kakhulu (~0.1 mm ubukhulu) elastomer ku-0, 20, 60, kanye no-100 % ubunzima.Imifantu emele imifantu nemiqulu ikhombe ngemicibisholo.Zonke izithombe ze-AFM zisendaweni engu-15 μm × 15 μm, zisebenzisa ibha yesikali yombala efanayo naleyo enelebula ngayo.(I) Ijometri yokulingisa yama-electrode e-graphene anephethini ye-monolayer ku-substrate ye-SEBS.(J) Imephu yekhonta yokulingisa yohlobo olukhulu lwe-logarithmic oluyinhloko ku-monolayer graphene kanye ne-SEBS substrate ku-20% uhlobo lwangaphandle.(K) Ukuqhathaniswa kokuminyana kwendawo yokuqhekeka (ikholomu ebomvu), ukuminyana kwendawo yokuskrola (ikholomu ephuzi), kanye nobuhwaqane obungaphezulu (ikholomu eluhlaza okwesibhakabhaka) yezakhiwo ezihlukene zegraphene.
Lapho amafilimu e-MGG enwetshwa, kunenye indlela ebalulekile eyengeziwe yokuthi imiqulu ingakwazi ukuvala izifunda eziqhekekile ze-graphene, igcine inethiwekhi ye-percolating.Imiqulu ye-graphene iyathembisa ngoba ingaba amashumi ama-micrometer ubude futhi ngenxa yalokho ikwazi ukuvala imifantu ngokuvamile efika esikalini se-micrometer.Ngaphezu kwalokho, ngenxa yokuthi imiqulu iqukethe ama-multilayer e-graphene, kulindeleke ukuthi ibe nokumelana okuphansi.Uma kuqhathaniswa, amanethiwekhi e-CNT aminyene kakhulu (adlulisa kancane) ayadingeka ukuze kuhlinzekwe amandla afanayo okubhuloho, njengoba ama-CNT mancane (ngokuvamile ama-micrometer ambalwa ngobude) futhi aqhubeki kahle kunemiqulu.Ngakolunye uhlangothi, njengoba kuboniswe emkhiwaneni.I-S12, kuyilapho i-graphene iqhekeka phakathi nokunwetshwa ukuze ibhekane nobunzima, imiqulu ayiqhekeki, okubonisa ukuthi kungenzeka ukuthi lena yakamuva islayida ku-graphene engaphansi.Isizathu sokuthi zingaqhekeki kungenzeka kungenxa yesakhiwo esigoqiwe, esakhiwe izingqimba eziningi ze-graphene (~1 kuya ku-2 0 μm ubude, ~0.1 kuya ku-1 μm ububanzi, kanye no-10 kuya ku-100 nm ukuphakama), imodulus esebenza kahle ephezulu kunegraphene yesendlalelo esisodwa.Njengoba kubikwe iGreen and Hersam (42), amanethiwekhi e-metallic CNT (ububanzi beshubhu engu-1.0 nm) angafinyelela ukumelana neshidi eliphansi <100 ohms/sq naphezu kokumelana okukhulu kwe-junction phakathi kwama-CNT.Uma sicabangela ukuthi imiqulu yethu ye-graphene inobubanzi obungu-0.1 kuya ku-1 μm nokuthi imiqulu ye-G/G inezindawo zokuthintana ezinkulu kakhulu kune-CNTs, ukumelana nokuxhumana nendawo yokuxhumana phakathi kwemiqulu ye-graphene ne-graphene akumele kube yizici ezikhawulela ukugcina ukuqhutshwa okuphezulu.
I-graphene ine-modulus ephakeme kakhulu kune-substrate ye-SEBS.Nakuba ukushuba okusebenzayo kwe-electrode ye-graphene kuphansi kakhulu kunaleyo ye-substrate, ukuqina kwe-graphene izikhathi ukujiya kwayo kuqhathaniswa nokwengxenye engaphansi (43, 44), okuholela kumphumela omaphakathi wesiqhingi esiqinile.Silingise ukwakheka kwe-graphene engu-1-nm-thick ku-substrate ye-SEBS (bona Izinto Ezingeziwe ukuze uthole imininingwane).Ngokuvumelana nemiphumela yokulingisa, lapho u-20% we-strain usetshenziswa ku-substrate ye-SEBS ngaphandle, ukucindezeleka okujwayelekile ku-graphene ngu-~ 6.6% (Fig. 4J kanye ne-fig. S13D), ehambisana nokubhekwa kokuhlola (bona i-fig. S13) .Siqhathanise ubunzima ezifundeni ezinephethini zegraphene kanye ne-substrate sisebenzisa i-optical microscopy futhi sathola ubunzima esifundeni se-substrate okungenani kabili kunobunzima esifundeni se-graphene.Lokhu kukhombisa ukuthi uhlobo olusetshenziswa kumaphethini e-electrode e-graphene lungavaleka kakhulu, kwakheka iziqhingi eziqinile ze-graphene phezu kwe-SEBS (26, 43, 44).
Ngakho-ke, ikhono lama-electrode e-MGG lokugcina ukusebenza okuphezulu ngaphansi kokucindezeleka okuphezulu kungenzeka linikwe amandla yizindlela ezimbili ezinkulu: (i) Imiqulu ingakwazi ukuhlanganisa izifunda ezinqanyuliwe ukuze kugcinwe umzila we-conductive percolation, futhi (ii) amashidi e-graphene/elastomer amaningi angase aslayide. phezu komunye nomunye, okuholela ekunciphiseni kokucindezeleka kuma-electrode e-graphene.Okwezendlalelo eziningi ze-graphene edluliselwe ku-elastomer, izendlalelo azinamathiselwe ngokuqinile kwenye nenye, ezingase zishelele ekuphenduleni ubunzima (27).Imiqulu iphinde yandisa ukushuba kwezingqimba zegraphene, okungase kusize ekwandiseni ukuhlukana phakathi kwezendlalelo zegraphene futhi ngenxa yalokho inike amandla ukuslayidela kwezendlalelo zegraphene.
Imishini ye-All-carbon ilandelwa ngentshiseko ngenxa yezindleko eziphansi kanye nokusebenza okuphezulu.Esimweni sethu, ama-transistors e-carbon yonke akhiwe kusetshenziswa isango le-graphene eliphansi, umthombo ophezulu we-graphene umthombo / othintana naye wokudonsa amanzi, i-semiconductor ye-CNT ehlungiwe, ne-SEBS njenge-dielectric (Fig. 5A).Njengoba kuboniswe ku-Fig. 5B, idivayisi ye-carbon yonke ene-CNTs njengomthombo/i-drain nesango (idivayisi ephansi) i-opaque kakhulu kunedivayisi ene-graphene electrode (idivayisi ephezulu).Lokhu kungenxa yokuthi amanethiwekhi e-CNT adinga ukujiya okukhudlwana futhi, ngenxa yalokho, ukudluliswa kwe-optical okuphansi ukuze kuzuzwe ukumelana kweshidi okufana nalokho kwe-graphene (fig. S4).Umfanekiso wesi-5 (C no-D) ubonisa amajika amele ukudluliswa nokuphumayo ngaphambi kobunzima be-transistor eyenziwe ngama-electrode e-bilayer MGG.Ububanzi besiteshi nobude be-transistor engacindezelwe bekungu-800 no-100 μm, ngokulandelana.Isilinganiso esilinganisiwe sokuvula/sokuvala sikhulu kuno-103 ngokuvula nokuvala imisinga kumazinga 10−5 kanye no-10−8 A, ngokulandelanayo.Ijika lokuphumayo libonisa izindlela ezifanele zomugqa kanye ne-sa turation ezincike ku-voltage yesango elicacile, okubonisa ukuthintana okuhle phakathi kwama-CNT nama-electrode e-graphene (45).Ukumelana nokuxhumana nama-electrode e-graphene kwaqashelwa ukuthi kuphansi kunalokho ngefilimu ye-Au ehwamukile (bona umkhiwane S14).Ukuhamba kokugcwala kwe-transistor enwebekayo cishe ku-5.6 cm2/Vs, kufana nalokho kwama-transistors e-CNT ahlelwe nge-polymer efanayo kuma-substrates e-Si aqinile ane-300-nm SiO2 njengongqimba lwe-dielectric.Ukuthuthukiswa okuqhubekayo ekuhambeni kungenzeka nge-tube density elungiselelwe kanye nezinye izinhlobo zamashubhu (46).
(A) Uhlelo lwe-graphene-based stretchable transistor.Ama-SWNTs, ama-carbon nanotubes anodonga olulodwa.(B) Isithombe sama-transistors anwebekayo esenziwe ngama-electrode e-graphene (phezulu) nama-electrodes e-CNT (ngezansi).Umehluko obala ubonakala ngokucacile.(C no-D) Ukudlulisa nokuphuma kwamajika we-graphene-based transistor ku-SEBS ngaphambi kobunzima.(E no-F) Dlulisa amajika, ukuvula nokuvala okwamanje, isilinganiso sokuvula/ukuvala, nokuhamba kwe-graphene-based transistor ezinhlobonhlobo ezahlukene.
Lapho idivayisi ebonisa ngale, yonke ikhabhoni yelulelwa ohlangothini oluhambisana nendawo yokuthutha eshaja, ukuwohloka okuncane kwabonwa kufika ku-120%.Ngesikhathi sokwelula, ukuhamba kwehla ngokuqhubekayo kusuka ku-5.6 cm2 / Vs ku-0% ubunzima kuya ku-2.5 cm2 / Vs ku-120% ubunzima (Fig. 5F).Siphinde saqhathanisa ukusebenza kwe-transistor ngobude obuhlukile besiteshi (bona ithebula S1).Ngokuphawulekayo, ngobunzima obungango-105%, wonke lawa ma-transistors asabonisa isilinganiso esiphezulu sokuvula/ukuvala (>103) nokuhamba (>3 cm2/Vs).Ngaphezu kwalokho, sifingqa wonke umsebenzi wakamuva wawo wonke ama-transistors ekhabhoni (bona ithebula S2) (47–52).Ngokuthuthukisa ukwakhiwa kwedivayisi kuma-elastomers nokusebenzisa ama-MGG njengothintana nabo, ama-transistors ethu e-carbon all-carbon abonisa ukusebenza kahle ngokuhamba nokushuba kanye nokunwebeka kakhulu.
Njengokusetshenziswa kwe-transistor esobala ngokugcwele nenwebekayo, siyisebenzisele ukulawula ukushintsha kwe-LED (Fig. 6A).Njengoba kuboniswe ku-Fig. 6B, i-LED eluhlaza ingabonakala ngokucacile ngokusebenzisa idivayisi ye-carbon yonke enwebekayo ebekwe ngaphezulu ngokuqondile.Ngenkathi inweba kufika ku-~100% (Umfanekiso 6, C no-D), ukukhanya kwe-LED akushintshi, okuhambisana nokusebenza kwe-transistor okuchazwe ngenhla (bona i-movie S1).Lona umbiko wokuqala wamayunithi okulawula anwebekayo enziwe kusetshenziswa ama-electrode e-graphene, okubonisa ithuba elisha le-graphene elekwe kagesi.
(A) Umjikelezo we-transistor ukushayela i-LED.GND, phansi.(B) Isithombe se-transistor ye-all-carbon transistor enwebekayo nebonisa ngale ku-0% uhlobo olufakwe ngaphezu kwe-LED eluhlaza.(C) I-transistor ebonisa ngale nenwebekayo ye-carbon all-carbon esetshenziselwa ukushintsha i-LED ikhwezwa ngaphezu kwe-LED ngo-0% (kwesokunxele) kanye no-~100% uhlobo (kwesokudla).Imicibisholo emhlophe ikhomba njengezimpawu eziphuzi kudivayisi ukukhombisa ukuguqulwa kwebanga elelulwayo.(D) Ukubuka okuseceleni kwe-transistor eluliwe, ne-LED iphushelwe ku-elastomer.
Sengiphetha, sithuthukise ukwakheka kwe-graphene ekwazi ukusebenza kahle egcina ukusebenza okuphezulu ngaphansi kwezinkinga ezinkulu njengama-electrode anwebekayo, anikwe amandla ama-graphene nanoscroll phakathi kwezingqimba ze-graphene ezistakiwe.Lezi zakhiwo zama-electrode ze-MGG ze-bi- and trilayer ku-elastomer zingakwazi ukugcina u-21 no-65%, ngokulandelana, we-conductivity yazo engu-0% yobunzima obufinyelela ku-100%, uma kuqhathaniswa nokulahlekelwa okuphelele kokusebenza ku-5% uhlobo lwama-electrode e-monolayer graphene ajwayelekile. .Izindlela ezengeziwe zokuqhuba zemiqulu ye-graphene kanye nokusebenzisana okubuthakathaka phakathi kwezendlalelo ezidlulisiwe kunomthelela ekuzinzeni okuphezulu kwe-conductivity ngaphansi kokucindezeleka.Siphinde sasebenzisa lesi sakhiwo se-graphene ukuze senze ama-transistors anwebekayo ekhabhoni yonke.Kuze kube manje, lena i-graphene-based transistor elula kakhulu enokukhanya okuhle kakhulu ngaphandle kokusebenzisa ukubopha.Nakuba isifundo samanje senziwe ukuze sikwazi i-graphene ye-electronics stretchable, sikholelwa ukuthi le ndlela inganwetshwa kwezinye izinto ze-2D ukuze kunikwe amandla i-electronics ye-2D elula.
Indawo enkulu ye-CVD graphene yakhuliswa kuma-Cu foil amisiwe (99.999%; Alfa Aesar) ngaphansi kwengcindezi eqhubekayo engu-0.5 mtorr no-50–SCCM (i-cubic centimeter evamile ngomzuzu) CH4 kanye no-20–SCCM H2 njengamanduleli ku-1000°C.Zombili izinhlangothi ze-Cu foil zazimbozwe yi-monolayer graphene.Ungqimba oluncane lwe-PMMA (2000 rpm; A4, Microchem) lwaluvalwe ngesipina ohlangothini olulodwa lwe-Cu foil, lwakha isakhiwo se-PMMA/G/Cu foil/G.ngemuva kwalokho, yonke ifilimu yacwiliswa ku-0.1 M ammonium persulfate [(NH4)2S2O8] isixazululo cishe amahora angu-2 ukuze kukhishwe i-Cu foil.Phakathi nale nqubo, i-graphene engemuva engavikelekile iqale yadabula imingcele yokusanhlamvu yase igoqeka yaba imiqulu ngenxa yokungezwani kwendawo.Imiqulu inanyathiselwe efilimini ye-graphene ephezulu esekelwa yi-PMMA, kwakheka imiqulu ye-PMMA/G/G.Amafilimu abe esegezwa emanzini akhishwe kaningi izikhathi eziningana futhi abekwa endaweni engaphansi okuhlosiwe, njenge-SiO2/Si eqinile noma i-plastic substrate.Lapho nje ifilimu enamathiselwe yomile ku-substrate, isampula yacwiliswa ngokulandelana kwe-acetone, 1:1 i-acetone/IPA (isopropyl alcohol), kanye ne-IPA imizuzu engu-30 ngayinye ukuze kukhishwe i-PMMA.Amafilimu ashiswe ku-100 ° C imizuzu engu-15 noma agcinwe ku-vacuum ngobusuku bonke ukuze akhiphe ngokuphelele amanzi avalelwe ngaphambi kokuba esinye isendlalelo somqulu we-G/G sidluliselwe kuwo.Lesi sinyathelo bekuwukugwema ukuhlukaniswa kwefilimu ye-graphene kusuka ku-substrate futhi kuqinisekiswe ukumbozwa okugcwele kwama-MGG ngesikhathi sokukhishwa kwesendlalelo senkampani yenethiwekhi ye-PMMA.
I-morphology yesakhiwo se-MGG yabonwa kusetshenziswa isibonakhulu esibonakalayo (Leica) kanye nesibonakhulu se-electron yokuskena (1 kV; FEI).Isibonakhulu samandla e-athomu (Nanoscope III, Digital Instrument) sasetshenziswa kumodi yokuthepha ukuze kubonwe imininingwane yeskrolo sika-G.Ukuba sobala kwefilimu kuhlolwe i-spectrometer ebonakalayo e-ultraviolet (Agilent Cary 6000i).Ezivivinyweni lapho uhlobo luhambisana ne-perpendicular direction yokugeleza kwamanje, i-photolithography ne-O2 plasma yasetshenziselwa ukuphethini izakhiwo ze-graphene zibe imicu (~300 μm ububanzi kanye ~2000 μm ubude), kanye nama-electrode e-Au (50 nm) afakwa ngokushisa kusetshenziswa. imaski yomthunzi emikhawulweni yomibili yohlangothi olude.Imichilo ye-graphene ibe isixhunywa ne-elastomer ye-SEBS (~2 cm ububanzi no-~5 cm ubude), ene-eksisi ende yemigqa ehambisana nohlangothi olufushane lwe-SEBS elandelwa yi-BOE (i-buffered oxide etch) (HF:H2O 1:6) etching kanye ne-eutectic gallium indium (EGaIn) njengokuxhumana kukagesi.Ngokuhlolwa kohlobo olufanayo, izakhiwo ze-graphene ezingaphethiwe (~5 × 10 mm) zidluliselwe kuma-substrate e-SEBS, anezimbazo ezinde ezihambisana nohlangothi olude lwe-substrate ye-SEBS.Kuzo zombili izimo, i-G yonke (ngaphandle kwemiqulu ye-G)/SEBS yanwetshwa ohlangothini olude lwe-elastomer emshinini ophathwayo, futhi endaweni, silinganise izinguquko zabo zokumelana ngaphansi kokucindezeleka esiteshini sokuhlola esinohlaziyo lwe-semiconductor (Keithley 4200). -SCS).
Ama-transistors e-carbon all-carbon anwebeka kakhulu futhi asobala ku-elastic substrate akhiwe ngezinqubo ezilandelayo ukugwema ukulimala kwe-organic solvent ye-polymer dielectric kanye ne-substrate.Izakhiwo ze-MGG zadluliselwa ku-SEBS njengama-electrode esango.Ukuze uthole ungqimba lwe-dielectric lwefilimu encane yefilimu ye-polymer (ubukhulu obungu-2 μm), isixazululo se-SEBS toluene (80 mg/ml) sasigqunywe nge-spin-coated ku-octadecyltrichlorosilane (OTS)–modified SiO2/Si substrate ngo-1000 rpm iminithi elingu-1.Ifilimu elizacile le-dielectric lingadluliswa kalula lisuka endaweni eyi-hydrophobic OTS liye ku-SEBS substrate embozwe nge-graphene elungiselelwe.I-capacitor ingenziwa ngokufaka i-liquid-metal (EGaIn; Sigma-Aldrich) i-electrode ephezulu ukuze kunqunywe amandla njengomsebenzi wobunzima kusetshenziswa i-LCR (inductance, capacitance, resistance) imitha (Agilent).Enye ingxenye ye-transistor yayinama-CNTs e-polymer-sorted semiconducting, elandela izinqubo ezibikwe ngaphambilini (53).Ama-electrod anephethini womthombo/wokukhipha amanzi akhiwe kuma-substrates e-SiO2/Si aqinile.Kamuva, lezi zingxenye ezimbili, i-dielectric/G/SEBS kanye ne-CNTs/iphethini ye-G/SiO2/Si, yahlanganiswa komunye nomunye, futhi yacwiliswa ku-BOE ukuze isuse i-SiO2/Si substrate eqinile.Ngakho-ke, ama-transistors asobala ngokugcwele futhi anwebekayo akhiwe.Ukuhlolwa kukagesi ngaphansi kokucindezeleka kwenziwa ekusetheni kokunwetshwa kwemanuwali njengendlela eshiwo ngenhla.
Izinto ezingeziwe zalesi sihloko zitholakala kokuthi http://advances.sciencemag.org/cgi/content/full/3/9/e1700159/DC1
umkhiwane.S1.Izithombe ze-Optical microscopy ze-monolayer MGG ku-SiO2/Si substrates ngokukhuliswa okuhlukene.
umkhiwane.S4.Ukuqhathaniswa kokuphikiswa kweshidi le-probe emibili kanye nokudluliselwa @550 nm ye-mono-, i-bi- kanye ne-trilayer plain graphene (izikwele ezimnyama), i-MGG (imibuthano ebomvu), kanye nama-CNT (unxantathu oluhlaza okwesibhakabhaka).
umkhiwane.S7.Ukushintsha kokumelana okujwayelekile kwe-mono- kanye ne-bilayer MGGs (emnyama) kanye no-G (obomvu) ngaphansi ~ ~ 1000 uhlobo lwe-cyclic strain ukulayisha kufika ku-40 kanye no-90% we-parallel strain, ngokulandelanayo.
umkhiwane.I-S10.Isithombe se-SEM se-trilayer MGG ku-SEBS elastomer ngemva kobunzima, sibonisa isiphambano somqulu omude phezu kwemifantu embalwa.
umkhiwane.S12.Isithombe se-AFM se-trilayer MGG ku-SEBS elastomer ezacile kakhulu ngo-20% uhlobo, okubonisa ukuthi umqulu weqe umfantu.
ithebula S1.Ukuhamba kwe-bilayer MGG–i-carbon nanotube transistors enodonga olulodwa ngobude obuhlukene besiteshi ngaphambi nangemuva kobunzima.
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QAPHELA: Sicela ikheli lakho le-imeyili kuphela ukuze umuntu omncomayo ikhasi azi ukuthi ubufuna alibone, nokuthi aliyona i-imeyili eyimfucuza.Asithathi noma yiliphi ikheli le-imeyili.
Lo mbuzo owokuhlola ukuthi uyisivakashi esingumuntu noma cha kanye nokuvikela ukuthunyelwa kogaxekile okuzenzakalelayo.
NguNan Liu, Alex Chortos, Ting Lei, Lihua Jin, Taeho Roy Kim, Won-Gyu Bae, Chenxin Zhu, Sihong Wang, Raphael Pfattner, Xiyuan Chen, Robert Sinclair, Zhenan Bao
NguNan Liu, Alex Chortos, Ting Lei, Lihua Jin, Taeho Roy Kim, Won-Gyu Bae, Chenxin Zhu, Sihong Wang, Raphael Pfattner, Xiyuan Chen, Robert Sinclair, Zhenan Bao
© 2021 Inhlangano YaseMelika Yokuthuthukiswa Kwesayensi.Wonke Amalungelo Agodliwe.I-AAAS inguzakwethu we-HINARI, AGORA, OARE, CHORUS, CLOCKSS, CrossRef kanye ne-COUNTER.Science Advances ISSN 2375-2548.
Isikhathi sokuthumela: Jan-28-2021