Electrode za graphene zibonerana cyane kandi zishobora kurambura

Ibikoresho bifite imiterere ibiri, nka graphene, birakurura haba mu bikorwa bisanzwe bya semiconductor ndetse no mu bikorwa bishya bya elegitoroniki byoroshye. Ariko, imbaraga nyinshi za graphene zituma icikagurika ku munota muto, bigatuma bigorana kubyaza umusaruro imiterere yayo idasanzwe ya elegitoroniki mu bikoresho bya elegitoroniki byoroshye kurambura. Kugira ngo dukore neza cyane mu mikorere ya graphene igaragara, twakoze graphene nanoscrolls hagati y’ibice bya graphene byashyizwemo, byitwa multilayer graphene/graphene scrolls (MGGs). Mu gihe cyo gukaraba, hari Scrolls zahuje imiterere ya graphene kugira ngo zigumane umuyoboro uhuza amashanyarazi watumaga habaho imikorere myiza ya fercolating mu miterere myinshi. Trilayer MGGs zishyigikiwe na elastomers zagumanye 65% by’imikorere yazo ya mbere ku munota 100%, ari nabyo bigororotse mu cyerekezo cy’umuvuduko w’amashanyarazi, mu gihe filime za graphene za trilayer zidafite nanoscrolls zagumanye 25% gusa by’imikorere yazo ya mbere. Transistor ishobora kurambura karubone yose yakozwe hakoreshejwe MGGs ubwo electrodes yagaragazaga ubushobozi bwo kohereza ibintu bwa >90% kandi igumana 60% by'umusaruro wayo w'umwimerere ku kigero cya 120% (bijyanye n'icyerekezo cyo gutwara umuriro). Izi transistor zishobora kurambura karubone yose kandi zibonerana zishobora gutuma optoelectronics zigezweho zirambura.
Ikoranabuhanga ribonerana rishobora gukururwa ni urwego rukura rufite akamaro kanini muri sisitemu zigezweho zihuza ibintu (1, 2) ndetse n'ubushobozi bwo guhuza na optoelectronics zibasha gukururwa (3, 4) kugira ngo hakorwe robotike zoroshye zigezweho n'ibimenyetso. Graphene igaragaza imiterere myiza cyane y'ubugari bwa atome, ubwisanzure buhanitse, n'ubushobozi bwo gutwara ibintu bwinshi, ariko ishyirwa mu bikorwa ryayo mu bikorwa bishobora gukururwa ryarahagaritswe n'uburyo ikunda gucikamo uduce duto. Kurenga imbogamizi za graphene mu buryo bwa tekiniki bishobora gutuma habaho imikorere mishya mu bikoresho bishobora gukururwa bifatika.
Imiterere yihariye ya graphene ituma iba umukandida ukomeye mu gisekuru gitaha cya electrode zitwara urumuri (5, 6). Ugereranyije na kondakteri itwara urumuri ikoreshwa cyane, indium tin oxide [ITO; 100 ohms/kare (sq) kuri 90% by'ubugaragare], graphene imwe ihingwa hakoreshejwe chemical vapor deposition (CVD) ifite uburyo busa bwo kwirinda sheet (125 ohms/sq) no kugaragara neza (97.4%) (5). Byongeye kandi, filime za graphene zifite ubworoherane budasanzwe ugereranije na ITO (7). Urugero, ku gice cya pulasitiki, uburyo bwayo bwo kuyobora bushobora kugumana ndetse no ku gice cyo hagati cy'umurambararo gito nka 0.8 mm (8). Kugira ngo yongere imikorere yayo y'amashanyarazi nk'kondakteri itwara urumuri, imirimo yabanje yakoze ibikoresho bya graphene hybrid bifite insinga za silver nano zigize uburebure bumwe (1D) cyangwa nanotubes za karuboni (CNTs) (9–11). Byongeye kandi, graphene yakoreshejwe nk'ama-electrode kuri semiconductors zivanze zifite imiterere itandukanye (nk'insinga za 2D bulk Si, 1D nanotubes, na 0D quantum dots) (12), transistors zihindagurika, selile z'izuba, na diodes zitanga urumuri (LEDs) (13–23).
Nubwo graphene yagaragaje umusaruro mwiza ku bikoresho by'ikoranabuhanga byoroshye, ikoreshwa ryayo mu bikoresho by'ikoranabuhanga byoroshye ryagabanijwe n'imiterere yayo ya mekanike (17, 24, 25); graphene ifite ubukana bwa 340 N / m na modulus ya Young ya 0.5 TPa (26). Urusobe rukomeye rwa karubone-karubone ntirutanga uburyo bwo gukwirakwiza ingufu ku bukana bukoreshwa bityo ihita icikagurika ku bukana buri munsi ya 5%. Urugero, CVD graphene yimuwe kuri polydimethylsiloxane (PDMS) elastic substrate ishobora kugumana gusa ubukana bwayo ku bukana buri munsi ya 6% (8). Imibare y'inyigisho igaragaza ko gucika no gukorana hagati y'ibice bitandukanye bigomba kugabanya cyane ubukana (26). Mu gushyira graphene mu bice byinshi, bivugwa ko iyi graphene y'ibice bibiri cyangwa bitatu ishobora kuramburwa ku bukana bwa 30%, igaragaza impinduka ku bukana inshuro 13 kurusha iya monolayer graphene (27). Ariko, uku gukomereka kuracyari hasi cyane ugereranije n’ibikoresho bigezweho byo gukomereka (28, 29).
Transistors ni ingenzi mu mikoreshereze yoroshye kurambura kuko ituma sensor irushaho gusoma no gusesengura ibimenyetso (30, 31). Transistors kuri PDMS zifite graphene nyinshi nk'amashanyarazi yo gusohora/gusohora amashanyarazi hamwe n'ibikoresho byo mu miyoboro zishobora kugumana imikorere y'amashanyarazi kugeza kuri 5% (32), iri munsi cyane y'agaciro gasabwa (~50%) ku byuma bigenzura ubuzima n'uruhu rw'ikoranabuhanga (33, 34). Vuba aha, uburyo bwa graphene kirigami bwarasuzumwe, kandi transistors zikingiwe na electrolyte y'amazi zishobora kurambura kugeza kuri 240% (35). Ariko, ubu buryo busaba graphene ihagaze, ibyo bikaba bigora inzira yo gukora.
Aha, tugera ku bikoresho bya graphene byoroshye kurambura cyane binyuze mu guhuza imiyoboro ya graphene (uburebure bwa ~ 1 kugeza kuri 20 μm, ubugari bwa ~ 0.1 kugeza kuri 1 μm, na ~ 10 kugeza kuri 100 nm) hagati y’ibice bya graphene. Dutekereza ko iyi miyoboro ya graphene ishobora gutanga inzira zo kuyobora zihuza imyobo mu mpapuro za graphene, bityo igakomeza gutwara neza mu gihe cyo gukomeretsa. Imiyoboro ya graphene ntisaba gukora cyangwa gukora ibindi bikorwa; ikorwa mu buryo busanzwe mu gihe cyo kohereza amazi. Dukoresheje imiyoboro ya G/G (graphene/graphene) (MGGs) electrodes zoroshye kurambura (isoko/gusohora amazi n'irembo) na CNTs zikora neza, twashoboye kwerekana transistors za carbon zose zibonerana cyane kandi zishobora kurambura cyane, zishobora kurambura kugeza ku ngano ya 120% (zijyanye n'icyerekezo cyo gutwara umuriro) kandi zikagumana 60% by'umusaruro wazo w'umwimerere. Iyi ni transistors iboneye cyane ishingiye kuri karuboni kugeza ubu, kandi itanga umuriro uhagije wo gutwara LED idakora.
Kugira ngo dushobore gukoresha electrode za graphene zigaragara neza zo mu gace kanini, twahisemo graphene yatewe na CVD kuri Cu foil. Cu foil yamanitswe hagati mu muyoboro wa quartz wa CVD kugira ngo graphene ikure ku mpande zombi, ikora imiterere ya G/Cu/G. Kugira ngo twimure graphene, twabanje gusiga urwego rworoshye rwa poly (methyl methacrylate) (PMMA) kugira ngo turinde uruhande rumwe rwa graphene, twise graphene yo hejuru (ibinyuranye n'ibyo ku rundi ruhande rwa graphene), hanyuma, filime yose (PMMA/top graphene/Cu/bottom graphene) yinjizwa mu muti wa (NH4)2S2O8 kugira ngo ikureho Cu foil. Graphene yo hasi idafite PMMA coating nta gushidikanya ko izaba ifite imiyoboro n'ubusembwa butuma ikintu kinyuramo (36, 37). Nkuko bigaragara ku Ishusho ya 1A, bitewe n'imbaraga z'ubuso, imiterere ya graphene yarekuwe yazingitswe mu miyoboro hanyuma ishyirwa kuri filime ya G/PMMA isigaye. Imirongo yo hejuru ya G/G ishobora kwimurirwa kuri substrate iyo ari yo yose, nka SiO2/Si, ikirahure, cyangwa polymer yoroshye. Gusubiramo iyi nzira yo kwimura inshuro nyinshi kuri substrate imwe biha imiterere ya MGG.
(A) Ishusho y'icyitegererezo cy'uburyo bwo gukora MGGs nk'igikoresho cyoroshye kurambura. Mu gihe cyo kwimura graphene, graphene y'inyuma kuri Cu foil yaciwe ku mbibi no ku bisembwa, izunguruka mu buryo butunguranye, maze ifatanywa neza ku mashusho yo hejuru, ikora nanoscrolls. Igishushanyo cya kane kigaragaza imiterere ya MGG ishyizwe hamwe. (B na C) Ibimenyetso bya TEM bya MGG y'urukiramende rumwe, byibanda kuri graphene y'urukiramende rumwe (B) n'agace k'umusemburo (C), uko bikurikirana. Ishusho y'imbere ya (B) ni ishusho y'ubwinshi buke igaragaza imiterere rusange ya MGG z'urukiramende rumwe kuri TEM grid. Ishusho y'imbere ya (C) ni imiterere y'ubukana yafashwe ku dusanduku tw'urukiramende tugaragara ku ishusho, aho intera iri hagati y'indege za atome ari 0.34 na 0.41 nm. (D) Karuboni K-edge EEL spectrum ifite imiterere ya π* na σ* peaks zanditseho. (E) Ishusho ya AFM y'imisemburo ya G/G y'urukiramende rumwe ifite uburebure ku murongo w'umuhondo ufite utudomo. (F kugeza kuri I) Mikroskopi y'amashusho n'ishusho ya AFM ya G y'urukiramende rutatu nta (F na H) hamwe n'imizingo (G na I) ku duce twa SiO2/Si tw'ubugari bwa 300-nm, uko bikurikirana. Imizingo n'iminkanyari byerekana itandukaniro ryabyo byashyizwe mu majwi kugira ngo bigaragaze itandukaniro ryabyo.
Kugira ngo twemeze ko imizingo ari graphene izungurutse mu buryo bugaragara, twakoze inyigo za spectroscopy ya electron microscopy (TEM) na electron energy loss (EEL) ku miterere ya monolayer top-G/G scroll. Ishusho ya 1B igaragaza imiterere ya hexagonal ya monolayer graphene, kandi igice cy’imbere ni imiterere rusange ya filime itwikiriwe ku mwobo umwe wa karuboni wa TEM grid. Graphene ya monolayer izenguruka igice kinini cya grid, kandi uduce twa graphene tumwe na tumwe turimo uduce twinshi tw’impeta za hexagonal tugaragara (Ishusho ya 1B). Mu gukurura mu muzingo umwe (Ishusho ya 1C), twabonye ingano nini y’uduce twa graphene, aho intera iri hagati ya 0.34 na 0.41 nm. Ibi bipimo bigaragaza ko uduce duzungurutse mu buryo butunguranye kandi ntabwo ari graphite itunganye, ifite intera ya 0.34 nm muri "ABAB" layer stacking. Ishusho ya 1D igaragaza spectrum ya karuboni K-edge EEL, aho uburebure bwa 285 eV buturuka kuri orbital ya π* naho ubundi hafi ya 290 eV buterwa n'impinduka ya orbital ya σ*. Bigaragara ko guhuza sp2 ari byo byiganje muri iyi miterere, byemeza ko imizingo ifite grafiti nyinshi.
Amashusho ya mikorosikopi y'urumuri n'amashusho ya mikorosikopi y'imbaraga za atome (AFM) atanga ibisobanuro ku ikwirakwizwa rya nanoscrolls za graphene muri MGGs (Ishusho ya 1, E kugeza kuri G, n'amashusho ya S1 na S2). Imirongo ikwirakwizwa ku buryo butunguranye hejuru y'ubuso, kandi ubucucike bwayo buriyongera ugereranyije n'umubare w'imirongo ishyizwe hamwe. Imirongo myinshi ifatanye mu migozi kandi igaragaza uburebure butari bumwe buri hagati ya nm 10 na 100. Ifite uburebure bwa μm 1 kugeza kuri 20 n'ubugari bwa μm 0.1 kugeza kuri 1, bitewe n'ingano y'imirongo yayo ya mbere ya graphene. Nkuko bigaragara ku Ishusho ya 1 (H na I), imizingo ifite ingano nini cyane kuruta iminkanyari, bigatuma habaho ihuriro rikomeye hagati y'imirongo ya graphene.
Kugira ngo dupime imiterere y'amashanyarazi, twashushanyije filime za graphene zifite cyangwa zitarimo imiterere y'imirongo n'ibice byashyizwe mu duce twa 300-μm ubugari n'uburebure bwa 2000-μm hakoreshejwe photolithography. Ubudahangarwa bubiri bw'ibipimo nk'uburyo bwo guhindagurika bwapimwe mu bihe by'ikirere. Kuba hariho imirongo byagabanije ubushobozi bwo guhangana na graphene imwe ku kigero cya 80%, hagabanutseho 2.2% gusa mu buryo bwo kohereza (ishusho ya S4). Ibi byemeza ko nanoscrolls, zifite ubucucike bwinshi bw'amashanyarazi kugeza kuri 5 × 107 A/cm2 (38, 39), zigira uruhare rwiza cyane mu by'amashanyarazi kuri MGGs. Muri mono-, bi-, na trilayer plain graphene na MGGs zose, trilayer MGG ifite ubushobozi bwo gutwara neza cyane hamwe n'ubuhanga bugera hafi kuri 90%. Kugira ngo tugereranye n'andi masoko ya graphene yavuzwe mu nyandiko, twapimye kandi ubwiyongere bw'impapuro enye (ishusho ya S5) maze tubishyira ku rutonde nk'uburyo bwo kohereza kuri 550 nm (ishusho ya S6) mu Ishusho ya 2A. MGG igaragaza ubushobozi bwo gutwara no kubonerana bingana cyangwa biri hejuru kurusha graphene yakozwe mu buryo bw'ubukorano na oxide ya graphene yagabanijwe (RGO) (6, 8, 18). Menya ko ubwiyongere bw'impapuro za graphene yakozwe mu buryo bw'ubukorano bugizwe n'impapuro nyinshi ziruta ubw'iya MGG yacu, birashoboka ko ari ukubera ko zitari nziza mu mikurire yazo n'uburyo bwo kuyimura.
(A) Ubudahangarwa bw'urupapuro rupima ibintu bine ugereranije n'uburyo bwo kohereza kuri 550 nm ku bwoko butandukanye bwa graphene, aho kare z'umukara zigaragaza mono-, bi-, na trilayer MGGs; uruziga rutukura na trilayer z'ubururu bihuye na multilayer plain graphene yakuwe kuri Cu na Ni bivuye mu bushakashatsi bwa Li et al. (6) na Kim et al. (8), hanyuma bigashyirwa kuri SiO2 / Si cyangwa quartz; kandi trilayer y'icyatsi kibisi ni agaciro ka RGO ku rugero rutandukanye rwo kugabanya uhereye ku bushakashatsi bwa Bonaccorso et al. (18). (B na C) Impinduka mu buryo busanzwe bwa mono-, bi- na trilayer MGGs na G nk'uko bigendekera ku buryo bugororotse (B) na parallel (C) ku cyerekezo cy'umuvuduko w'amazi. (D) Impinduka mu buryo busanzwe bwa bilayer G (umutuku) na MGG (umukara) munsi y'umuvuduko w'amazi ugera kuri 50% by'umuvuduko w'amazi ugera kuri perpendicular. (E) Impinduka mu buryo busanzwe bwa trilayer G (umutuku) na MGG (umukara) munsi y'umuvuduko w'amazi ugera kuri 90%. (F) Impinduka mu buryo busanzwe ya mono-, bi- na trilayer G na bi- na trilayer MGGs nk'imikorere y'umuvuduko. Imbere ni imiterere ya capacitor, aho substrate ya polymer ari SEBS naho urwego rwa polymer dielectric rukaba SEBS ifite ubugari bwa 2-μm.
Kugira ngo dusuzume imikorere ya MGG ishingiye ku bushyuhe, twimuriye graphene kuri thermoplastic elastomer styrene-ethylene-butadiene-styrene (SEBS) substrates (~2 cm ubugari na ~ 5 cm uburebure), maze imikorere y’amashanyarazi ipimwa uko substrate yagutse (reba Ibikoresho n’Uburyo) haba ku ruhande rumwe kandi ijyanye n’icyerekezo cy’umuvuduko w’amashanyarazi (Ishusho ya 2, B na C). Imyitwarire y’amashanyarazi ishingiye ku bushyuhe yarushijeho kuba myiza hamwe no gushyiramo nanoscrolls no kwiyongera kw’imibare y’ibice bya graphene. Urugero, iyo ubushyuhe buhagaze ku ruhande rumwe n’umuvuduko w’amashanyarazi, kuri monolayer graphene, kongeramo imizingo byongera ubushyuhe igihe amashanyarazi yacitse kuva kuri 5 kugeza kuri 70%. Ubushobozi bwo kwihanganira ubushyuhe bwa trilayer graphene nabwo burarushaho kwiyongera ugereranije na monolayer graphene. Hamwe na nanoscrolls, kuri 100% perpendicular strain, ubushyuhe bwa trilayer MGG bwiyongereyeho 50% gusa, ugereranije na 300% kuri trilayer graphene idafite imizingo. Impinduka mu bushyuhe munsi y’umutwaro w’ubushyuhe bwa cyclic bwakoreweho ubushakashatsi. Kugereranya (Ishusho ya 2D), ubushobozi bwo guhangana n'ingufu za graphene y'urubara rw'ibice bibiri (bilayer graphene) bwiyongereye inshuro zigera kuri 7.5 nyuma y'ingendo za ~700 ku kigero cya 50% cy'ubugari bw'impande kandi bukomeza kwiyongera uko ibintu bihinduka muri buri ngendo. Ku rundi ruhande, ubushobozi bwo guhangana n'ingufu za MGG y'urubara rwiyongereye inshuro zigera kuri 2.5 gusa nyuma y'ingendo za ~700. Gukoresha imbaraga zigera kuri 90% mu cyerekezo kimwe, ubushobozi bwo guhangana n'ingufu za graphene y'urubara rw'ibice bibiri (trilayer graphene) bwiyongereye inshuro ~100 nyuma y'ingendo 1000, mu gihe ari ~8 gusa muri MGG y'urubara rw'ibice bibiri (Ishusho ya 2E). Ibisubizo ku ngendo bigaragara ku ishusho ya S7. Ukwiyongera kwihuta k'ubugari bw'ingufu mu cyerekezo kimwe ni uko icyerekezo cy'imivuniko giteye ku cyerekezo cy'umuvuduko w'amazi. Guhindagurika k'ubugari mu gihe cyo gupakira no gupakurura imbaraga biterwa no kugaruka kwa viscoelastic kwa substrate ya elastomer ya SEBS. Ubudahangarwa buhamye bw'imirongo ya MGG mu gihe cyo gusiganwa kw'amagare buterwa no kuba hari imizingo minini ishobora kuroba ibice bya graphene byacitse (nk'uko byagaragajwe na AFM), bigafasha mu kubungabunga inzira izunguruka. Iki kintu cyo kubungabunga imikorere y'inzira izunguruka cyavuzwe mbere ku byuma byacitse cyangwa semiconductor films kuri substrates za elastomer (40, 41).
Kugira ngo dusuzume izi filime zishingiye kuri graphene nk'ama-electrode y'irembo mu bikoresho bishobora kurambura, twapfundikiye urwego rwa graphene dukoresheje urwego rwa dielectric rwa SEBS (ubugari bwa 2 μm) kandi dukurikirana impinduka mu bushobozi bwa dielectric nk'uko bigaragazwa n'uburyo ibintu bihinduka (reba Ishusho ya 2F n'Ibikoresho by'Inyongera ku bisobanuro birambuye). Twabonye ko ubushobozi bufite electrode ya graphene ya monolayer isanzwe na bilayer yagabanutse vuba bitewe n'ibura ry'ubushobozi bwa graphene mu ndege. Mu buryo bunyuranye, ubushobozi bugenzurwa na MGGs kimwe na graphene ya trilayer isanzwe byagaragaje ukwiyongera kwa capacitance hamwe n'uburyo ibintu bihinduka, ibi bikaba byitezwe kubera kugabanuka k'ubunini bwa dielectric hamwe n'uburyo ibintu bihinduka. Ubwiyongere bw'ubushobozi bwari bwitezwe bwahuye neza n'imiterere ya MGG (Ishusho ya S8). Ibi bigaragaza ko MGG ikwiriye nk'i-electrode y'irembo kuri transistors zishobora kurambura.
Kugira ngo dukore ubushakashatsi ku ruhare rwa 1D graphene scroll ku kwihanganira strain ya electron conductivity no kugenzura neza itandukanyirizo riri hagati y’ibice bya graphene, twakoresheje CNTs za spray-coated kugira ngo dusimbuze graphene scrolls (reba Ibikoresho by'inyongera). Kugira ngo twigane imiterere ya MGG, twashyizemo ubucucike butatu bwa CNTs (ni ukuvuga CNT1).
(Kuva kuri A kugeza kuri C) Amashusho ya AFM y'ubucucike butatu butandukanye bwa CNTs (CNT1)
Kugira ngo dusobanukirwe neza ubushobozi bwazo nk'amashanyarazi yo gukoresha ikoranabuhanga rishobora kurambura, twasesenguye ku buryo bwimbitse imiterere ya MGG na G-CNT-G biri mu gukurura. Mikroskopi y'amatara na mikroskopi y'amashanyarazi yo gukurura (SEM) ntabwo ari uburyo bwiza bwo kugaragaza ibimenyetso kuko byombi bitagira itandukaniro ry'amabara kandi SEM ikorerwa amashusho mu gihe cyo gukurura amashanyarazi iyo graphene iri ku duce twa polymer (ishusho ya S9 na S10). Kugira ngo turebe ubuso bwa graphene buri mu gukurura, twakusanyije ibipimo bya AFM kuri MGGs eshatu na graphene isanzwe nyuma yo kwimurirwa ku duce duto cyane (~0.1 mm ubugari) na elastic SEBS. Kubera inenge ziri muri CVD graphene no kwangirika kw'inyuma mu gihe cyo kwimura, gukurura gukunze kugaragara kuri graphene iri mu gukurura, kandi uko gukurura kwiyongera, gukurura gukomeye (Ishusho ya 4, A kugeza kuri D). Bitewe n'imiterere y'uduce twa electrodes zishingiye kuri karuboni, uduce tugaragaza imiterere itandukanye (ishusho ya S11) (27). Ubucucike bw'agace k'imfuruka (busobanurwa nk'agace k'imfuruka/agace gasesenguwe) bwa graphene y'ibice byinshi ni buke ugereranyije n'ubwa graphene y'ibice bimwe nyuma yo gukururwa, ibi bikaba bihuye n'ubwiyongere bw'ubushobozi bw'amashanyarazi kuri MGGs. Ku rundi ruhande, imizingo ikunze kugaragara kugira ngo ihuze imiyoboro, itanga inzira z'inyongera zo kuyobora muri filime ihujwe. Urugero, nk'uko byanditse ku ishusho ya 4B, umuzingo mugari wambukiranyije umuyoboro uri muri MGG y'ibice bitatu, ariko nta muzingo wagaragaye muri graphene isanzwe (Ishusho ya 4, E kugeza kuri H). Mu buryo nk'ubwo, CNTs nazo zahujije imiyoboro muri graphene (Ishusho ya S11). Ubucucike bw'agace k'imfuruka, ubucucike bw'agace k'imfuruka, n'ubukana bwa filime bikubiye muri Ishusho ya 4K.
(Kugeza kuri A) Amashusho ya AFM y’imirongo itatu ya G/G (kuva kuri A kugeza kuri D) n’imiterere ya G itatu (kuva kuri E kugeza kuri H) kuri elastomer nto cyane ya SEBS (~0.1 mm) ku bunini bwa 0, 20, 60, na 100%. Imyanya n’imirongo byihariye bigaragazwa n’imyambi. Amashusho yose ya AFM ari mu buso bwa 15 μm × 15 μm, hakoreshejwe umurongo umwe w’amabara nk’uko byanditse. (I) Imiterere y’imirongo ya electrode za graphene za monolayer zifite ibishushanyo kuri substrate ya SEBS. (J) Ikarita y’imiterere y’imirongo ya logarithmic ikomeye muri graphene ya monolayer na substrate ya SEBS ku bunini bwa 20%. (K) Kugereranya ubucucike bw’ahantu hacitse (inkingi itukura), ubucucike bw’aha hantu hasohoka (inkingi y’umuhondo), n’ubushyuhe bw’ubuso (inkingi y’ubururu) ku miterere itandukanye ya graphene.
Iyo filime za MGG zarambuwe, hari ubundi buryo bw'ingenzi bwo ko imizingo ishobora guhuza uturere twa graphene twacitsemo ibice, bigatuma habaho umuyoboro uzenguruka. Imizingo ya graphene iratanga icyizere kuko ishobora kuba ifite uburebure bwa mikorometero icumi bityo ikabasha guhuza imiyoboro isanzwe igera kuri mikorometero. Byongeye kandi, kubera ko imizingo igizwe n'ibice byinshi bya graphene, byitezwe ko ifite ubushobozi buke bwo guhangana n'ibice. Ugereranije, imiyoboro ya CNT ifite ubucucike buciriritse (yohereza ibintu bike) irakenewe kugira ngo itange ubushobozi bwo guhuza imiyoboro, kuko CNT ari nto (ubusanzwe mikorometero nke) kandi ikaba idatwara ibintu byinshi ugereranyije n'imizingo. Ku rundi ruhande, nk'uko bigaragara ku ishusho ya S12, mu gihe graphene icikamo ibice mu gihe cyo kurambura kugira ngo ijyane n'imitsi, imizingo nticikamo ibice, bigaragaza ko iyi ya nyuma ishobora kuba irimo kunyerera kuri graphene iri munsi. Impamvu zidacika ishobora kuba iterwa n'imiterere izinze, igizwe n'ibice byinshi bya graphene (uburebure bwa ~ 1 kugeza 2 0 μm, ubugari bwa ~ 0.1 kugeza 1 μm, na ~ 10 kugeza 100 nm), ifite modulus nziza kurusha graphene y'urwego rumwe. Nk'uko byatangajwe na Green na Hersam (42), imiyoboro ya CNT y'icyuma (umurambararo wa tube wa 1.0 nm) ishobora kugera ku burambe buke bwo kugabanya impapuro ziri munsi ya 100 ohms/sq nubwo hari ubudahangarwa bunini hagati ya CNTs. Ukurikije ko imiyoboro yacu ya graphene ifite ubugari bwa 0.1 kugeza 1 μm kandi ko imiyoboro ya G/G ifite ahantu hanini cyane ho guhuza kurusha CNTs, ubudahangarwa bwo guhuza n'agace ko guhuza hagati ya graphene na graphene scrolls ntibigomba kuba ibintu bibangamira kugumana imikorere myiza.
Graphene ifite modulus iri hejuru cyane kurusha substrate ya SEBS. Nubwo ubunini bufatika bwa electrode ya graphene buri hasi cyane ugereranyije n'ubw'substrate, ubukana bwa graphene butera ubunini bwayo bugereranywa n'ubw'substrate (43, 44), bigatuma habaho ingaruka iringaniye ku kirwa. Twiganye uburyo graphene ifite ubunini bwa 1-nm kuri substrate ya SEBS (reba Ibikoresho by'inyongera ku bisobanuro birambuye). Dukurikije ibyavuye mu bushakashatsi, iyo 20% by'ubunini bishyizwe kuri substrate ya SEBS hanze, ubunini busanzwe muri graphene ni ~6.6% (Ishusho ya 4J n'ishusho ya S13D), ibi bikaba bihuye n'ibyagaragaye mu bushakashatsi (reba ishusho ya S13). Twagereranije ubunini mu duce twa graphene n'uduce twa substrate hakoreshejwe mikorosikopi y'amajwi kandi twasanze ubunini mu gace ka substrate buri nibura inshuro ebyiri z'ubunini mu gace ka graphene. Ibi bigaragaza ko ubunini bukoreshwa ku miterere ya electrode ya graphene bushobora kuba buto cyane, bugakora ibirwa bikomeye bya graphene hejuru ya SEBS (26, 43, 44).
Kubwibyo, ubushobozi bwa electrode za MGG bwo kugumana amashanyarazi menshi mu gihe cy’imbaraga nyinshi bushobora gushobozwa n’uburyo bubiri bw’ingenzi: (i) Imirongo ishobora guhuza uturere dutandukanye kugira ngo ikomeze inzira yo gukwirakwiza amashanyarazi, na (ii) impapuro za graphene z’urwego rwinshi zishobora kunyererana, bigatuma imbaraga ku electrode za graphene zigabanuka. Ku byiciro byinshi bya graphene yimuwe kuri elastomer, ibice ntibifatanye cyane, bishobora kunyerera bitewe n’imbaraga (27). Imirongo kandi yongereye ubukana bw’ibice bya graphene, bishobora gufasha kongera itandukanyirizo hagati y’ibice bya graphene bityo bigatuma ibice bya graphene bigenda binyerera.
Ibikoresho bya karubone byose bikurikiranwa cyane kubera ko bihendutse kandi bitanga umusaruro mwinshi. Muri uru rubanza rwacu, transistors za karubone zose zakozwe hakoreshejwe gate ya graphene yo hasi, top graphene source/drain contact, CNT semiconductor yatoranyijwe, na SEBS nk'amashanyarazi (Ishusho ya 5A). Nkuko bigaragara ku Ishusho ya 5B, igikoresho cya karubone cyose gifite CNTs nk'isoko/drain na gate (igikoresho cyo hasi) ntabwo kigaragara neza kurusha igikoresho gifite electrodes za graphene (igikoresho cyo hejuru). Ibi biterwa nuko imiyoboro ya CNT isaba ubugari bunini, bityo bigatuma habaho transmittance nke z'urumuri kugira ngo habeho resistance nke nk'iza graphene (Ishusho ya S4). Ishusho ya 5 (C na D) igaragaza imiyoboro ihagarariye transmission n'ibisohoka mbere yo gukurura transistors zakozwe na electrodes za MGG za bilayer. Ubugari bw'umuyoboro n'uburebure bwa transistors zitarakururwa byari 800 na 100 μm, uko bikurikirana. Igipimo cya on/off cyapimwe kirenze 103 hamwe n'imiyoboro yo kuva no kuva ku rwego rwa 10−5 na 10−8 A, uko bikurikirana. Umuyoboro w'umusaruro ugaragaza uburyo bwiza bwo guhuza umurongo n'umuyoboro hamwe n'uburyo bwo guhuza neza amarembo n'amashanyarazi, bigaragaza uburyo bwiza bwo guhuza CNTs na electrodes za graphene (45). Ubudahangarwa bwo guhuza na electrodes za graphene bwagaragaye ko buri hasi ugereranyije n'ubwo muri filime ya Au yakuwemo umwuka (reba ishusho ya S14). Ubushobozi bwo kugenda bwa transistor ishobora kurambura ni hafi 5.6 cm2/Vs, bisa n'ubwa transistor za CNT za polymer ku duce duto twa Si dufite 300-nm SiO2 nk'urwego rwa dielectric. Uburyo bwo kugenda burushaho kunozwa birashoboka hamwe n'ubucucike bw'imiyoboro n'ubundi bwoko bw'imiyoboro (46).
(A) Igishushanyo cya transistor irambura ishingiye kuri graphene. SWNTs, nanotubes za karuboni zifite inkuta imwe. (B) Ifoto ya transistor irambura ikozwe muri electrodes za graphene (hejuru) na electrodes za CNT (hejuru). Itandukaniro mu mucyo riragaragara neza. (C na D) Imirongo yo kohereza no gusohora transistor ishingiye kuri graphene kuri SEBS mbere yo gukurura. (E na F) Imirongo yo kohereza, umuriro wo kuri no kuzima, igipimo cyo kuri/kuzimya, n'uburyo transistor ishingiye kuri graphene igenda ku moko atandukanye.
Iyo igikoresho cya karuboni yose cyarambuwe mu cyerekezo gihuye n'icyerekezo cyo gutwara umuriro, cyagaragaye ko cyangiritse cyane kugeza ku kigero cya 120%. Mu gihe cyo kurambura, kugenda kwaragabanutse kuva kuri 5.6 cm2/Vs kuri 0% kugera kuri 2.5 cm2/Vs kuri 120% (Ishusho ya 5F). Twanagereranije imikorere ya transistor ku burebure butandukanye bw'imiyoboro (reba imbonerahamwe ya S1). By'umwihariko, kuri stress nini nka 105%, izi transistor zose zagaragaje igipimo cyo hejuru cyo kuva/kuvaho (>103) no kugenda (>3 cm2/Vs). Byongeye kandi, twasobanuye muri make imirimo yose iherutse gukorwa kuri transistor zose (reba imbonerahamwe ya S2) (47–52). Mu kunoza ikorwa ry'ibikoresho kuri elastomer no gukoresha MGGs nk'aho zihurira, transistor zacu zose za karuboni zigaragaza imikorere myiza mu bijyanye no kugenda no kwangirika ndetse no kuba zishobora kuramburwa cyane.
Mu rwego rwo gukoresha transistor ibonerana kandi irambura, twayikoresheje mu kugenzura uburyo LED ihinduranya (Ishusho ya 6A). Nkuko bigaragara ku Ishusho ya 6B, LED y'icyatsi kibisi igaragara neza binyuze mu gikoresho gishobora kurambura karubone cyose gishyizwe hejuru. Mu gihe cyo kurambura kugeza kuri ~ 100% (Ishusho ya 6, C na D), ubukana bw'urumuri rwa LED ntibuhinduka, ibi bikaba bihuye n'imikorere ya transistor yavuzwe haruguru (reba filime S1). Iyi ni raporo ya mbere y'ibikoresho byo kugenzura bishobora kurambura byakozwe hakoreshejwe electrode za graphene, bigaragaza uburyo bushya bwo gukoresha ikoranabuhanga rya graphene rishobora kurambura.
(A) Uruziga rwa transistor kugira ngo ikore LED. GND, hasi. (B) Ifoto ya transistor ishobora kurambura kandi ibonerana kuri 0% y'umuvuduko ishyizwe hejuru ya LED y'icyatsi kibisi. (C) Transistor ikoresha transistor ibonerana kandi ibonerana ikoreshwa mu guhindura LED iri gushyirwa hejuru ya LED kuri 0% (ibumoso) na ~100% y'umuvuduko (iburyo). Utwambi tw'umweru twerekana nk'ibimenyetso by'umuhondo ku gikoresho kugira ngo tugaragaze impinduka z'intera iri kurambura. (D) Ishusho ku ruhande rwa transistor irambuye, LED ishyizwe muri elastomer.
Mu gusoza, twakoze imiterere ya graphene ibonerana ikomeza gutwara neza munsi y’imitsi minini nk’iy’amashanyarazi ashobora kurambura, ikoresheje graphene nanoscrolls iri hagati y’imitsi ya graphene. Iyi miterere ya electrode ya MGG y’ibice bibiri na bitatu kuri elastomer ishobora kugumana 21 na 65% by’ubushobozi bwayo bwo gutwara ibintu ku rugero rwa 0% ku rugero rwa 100%, ugereranije no gutakaza burundu ubushobozi bwo gutwara ibintu ku rugero rwa 5% kuri electrode za graphene zisanzwe. Inzira z’inyongera zo gutwara ibintu za graphene scrolls hamwe n’imikoranire mike hagati y’imitsi yahinduriwe bigira uruhare mu gutuma habaho kudahungabana kw’imikorere mu gihe cy’imbaraga. Twakomeje gukoresha iyi miterere ya graphene mu gukora transistors zishobora kurambura karuboni zose. Kugeza ubu, iyi ni transistors ishingiye kuri graphene ishobora kurambura cyane ifite ubushobozi bwo gutanga umusaruro mwiza idakoresheje gufunga. Nubwo ubu bushakashatsi bwakozwe kugira ngo graphene ikoreshwe mu bikoresho bya elegitoroniki bishobora kurambura, twizera ko ubu buryo bushobora kwaguka no ku bindi bikoresho bya 2D kugira ngo habeho ikoranabuhanga rya 2D rishobora kurambura.
Graphene ya CVD yo mu buso bunini yahingwaga ku dupapuro twa Cu duhagaze (99.999%; Alfa Aesar) munsi y'umuvuduko uhoraho wa 0.5 mtorr hamwe na 50–SCCM (sentimetero kibe isanzwe ku munota) CH4 na 20–SCCM H2 nk'ibibanziriza kuri 1000°C. Impande zombi za Cu foil zari zitwikiriwe na monolayer graphene. Urwego rworoshye rwa PMMA (2000 rpm; A4, Microchem) rwashyizwe ku ruhande rumwe rwa Cu foil, rukora imiterere ya PMMA/G/Cu foil/G. Nyuma yaho, firime yose yashyizwe mu gisubizo cya 0.1 M ammonium persulfate [(NH4)2S2O8] mu gihe cy'amasaha 2 kugira ngo ikureho Cu foil. Muri iki gikorwa, graphene idakingiwe inyuma yabanje gushwanyagurika ku mbibi z'ingano hanyuma izunguruka ihinduka imizingo kubera imbaraga z'ubuso. Imizingo yashyizwe kuri firime ya graphene yo hejuru ishyigikiwe na PMMA, ikora imizingo ya PMMA/G/G. Nyuma y’aho, firime zogejwe mu mazi yakuwemo iayoni inshuro nyinshi hanyuma zishyirwa ku kintu cyagenewe, nka SiO2/Si cyangwa pulasitiki. Filime ikimara kuma kuri icyo kintu, icyitegererezo cyashyizwe muri acetone, acetone/IPA ya 1:1 (isopropyl alcohol), na IPA mu gihe cy’amasegonda 30 buri kimwe kugira ngo PMMA ikureho. Filime zashyushywaga kuri dogere selisiyusi 100 mu gihe cy’iminota 15 cyangwa zigashyirwa mu cyuma ijoro ryose kugira ngo amazi yose yari yafashwe akurweho mbere y’uko ikindi gice cya G/G scroll cyimurirwaho. Iyi ntambwe yari iyo kwirinda ko firime ya graphene iva muri icyo kintu no kwemeza ko MGGs zitwikiriwe neza mu gihe cyo kurekura urwego rwa PMMA.
Imiterere y'imiterere ya MGG yagaragaye hakoreshejwe mikorosikopi y'urumuri (Leica) na mikorosikopi y'urumuri rwo gupima (1 kV; FEI). Mikorosikopi y'imbaraga za atome (Nanoscope III, Digital Instrument) yakoreshejwe mu buryo bwo gukanda kugira ngo harebwe utuntu duto twa G scrolls. Ubuhanga bwa filime bwageragejwe hakoreshejwe spectrometer igaragara na ultraviolet (Agilent Cary 6000i). Mu bizamini igihe strain yari ku cyerekezo cy'umuvuduko w'amazi, photolithography na plasma ya O2 byakoreshejwe mu gushushanya imiterere ya graphene mo uduce (~300 μm ubugari na ~2000 μm uburebure), naho electrode za Au (50 nm) zashyizwe mu bushyuhe hakoreshejwe udupfukamunwa tw'igicucu ku mpera zombi z'uruhande rurerure. Hanyuma uduce twa graphene twashyizwe hamwe na elastomer ya SEBS (~2 cm ubugari na ~5 cm uburebure), aho umurongo muremure w'uduce uhuye n'uruhande rugufi rwa SEBS hagakurikiraho BOE (buffered oxide etch) (HF:H2O 1:6) etching na eutectic gallium indium (EGaIn) nk'aho ari amashanyarazi. Ku bipimo by'ubushyuhe bungana, imiterere ya graphene idashushanyije (~5 × 10 mm) yimuriwe kuri substrates za SEBS, aho imigozi miremire ihuye n'uruhande rurerure rwa substrate ya SEBS. Kuri ibyo byombi, G yose (idafite G scrolls)/SEBS yarambuwe ku ruhande rurerure rwa elastomer mu gikoresho gikoreshwa n'intoki, kandi aho hantu, twapimye impinduka z'ubudahangarwa bwazo mugihe cyo gukomeretsa kuri probe station dukoresheje semiconductor analyzer (Keithley 4200-SCS).
Transistors zoroshye cyane zoroshye kandi zibonerana zakozwe hakoreshejwe uburyo bukurikira kugira ngo hirindwe kwangirika kwa polymer dielectric na substrate. Imiterere ya MGG yimuriwe kuri SEBS nk'ama-electrode y'irembo. Kugira ngo haboneke urwego rumwe rw'ama-polymer dielectric (ubugari bwa 2 μm), umuti wa SEBS toluene (80 mg/ml) washyizwe ku gikoresho cya octadecyltrichlorosilane (OTS) - cyahinduwe cya SiO2/Si ku muvuduko wa 1000 rpm mu gihe cy'umunota 1. Filimi yoroheje ya dielectric ishobora kwimurwa byoroshye iva ku buso bwa OTS budafite amazi ijya kuri substrate ya SEBS itwikiriwe na graphene yateguwe. Capacitor yashoboraga gukorwa hashyirwamo electrode y'icyuma gikozwe mu mazi (EGaIn; Sigma-Aldrich) kugira ngo hamenyekane ubushobozi nk'uburyo bwo gukurura hakoreshejwe metero ya LCR (inductance, capacitance, resistance) (Agilent). Igice kindi cya transistors cyari kigizwe na CNTs za semiconducting za polymer, hakurikijwe inzira zavuzwe mbere (53). Amashanyarazi y’inkomoko/amashanyarazi yakozwe ku byuma bikomeye bya SiO2/Si. Nyuma yaho, ibice bibiri, dielectric/G/SEBS na CNTs/byitwa G/SiO2/Si, byashyizwe hamwe, binigwa muri BOE kugira ngo bikureho byitwa SiO2/Si. Bityo, transistors zibonerana kandi zishobora kurambura zakozwe. Igeragezwa ry’amashanyarazi ryakozwe ku buryo bwo kurambura bwakozwe n’intoki nk’uko byavuzwe haruguru.
Ibikoresho by'inyongera kuri iyi nkuru biraboneka kuri http://advances.sciencemag.org/cgi/content/full/3/9/e1700159/DC1
ishusho ya S1. Amashusho ya mikorosikopi y'urumuri rw'izuba rwa monolayer MGG kuri substrates za SiO2/Si ku buryo butandukanye bwo kongera ubwinshi.
ifoto ya S4. Kugereranya uburyo bwo guhangana n'impapuro ebyiri za probe na transmittances @550 nm bya mono-, bi- na trilayer plain graphene (kabure k'umukara), MGG (uruziga rutukura), na CNTs (impandeshatu y'ubururu).
ishusho ya S7. Impinduka zisanzwe zo guhangana na MGGs za mono- na bilayer (umukara) na G (umutuku) munsi ya ~1000 cyclic strain zishyirwa kuri 40 na 90% parallel strain, uko bikurikirana.
ishusho ya S10. Ishusho ya SEM ya trilayer MGG kuri elastomer ya SEBS nyuma yo gukururwa, igaragaza uruziga rurerure rwambukiranyije imiyoboro myinshi.
ishusho ya S12. Ishusho ya AFM ya MGG y'urukiramende rwa trilayer kuri elastomer yoroheje cyane ya SEBS ku kigero cya 20%, igaragaza ko umuzingo wanyuze hejuru y'umuyoboro.
Imbonerahamwe S1. Uburyo transistors za MGG-nanotube za karuboni zifite urukuta rumwe zigenda ku burebure butandukanye mbere na nyuma yo gukurura.
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Na Nan 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
Na Nan 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
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