Ihe akụkụ abụọ, dị ka graphene, na-adọrọ mmasị maka ma ngwa semiconductor na ngwa ngwa na ngwa eletrọnịkị na-agbanwe agbanwe. Agbanyeghị, ike dị elu nke graphene na-ebute mgbaji na obere nsogbu, na-eme ka ọ bụrụ ihe ịma aka iji nweta akụrụngwa eletrọnịkị ya pụrụ iche na ngwa elektrọn nwere ike ịgbatị. Iji mee ka arụmọrụ dị mma dabere na eriri nke ndị na-eduzi graphene, anyị mepụtara graphene nanoscrolls n'etiti akwa graphene, nke akpọrọ multilayer graphene/graphene mpịakọta (MGGs). N'okpuru nsogbu, ụfọdụ akwụkwọ mpịakọta kpuchiri ngalaba graphene ndị kewara ekewa iji nọgide na-enwe netwọk na-ekpo ọkụ nke nyere aka ịrụ ọrụ dị mma n'ụdị dị elu. Trilayer MGGs na-akwado na elastomers jigidere 65% nke omume izizi ha na 100% strain, bụ nke dabara na ntụzịaka nke erute ugbu a, ebe ihe nkiri trilayer nke graphene na-enweghị nanoscrolls na-ejigide naanị 25% nke omume mmalite ha. Carbon transistor nke nwere ike ịgbatị agbatị site na iji MGG dị ka eletrọd gosipụtara nnyefe nke>90% wee jigide 60% nke ihe nrụpụta mbụ ya dị ugbu a na eriri 120% (yiri na ntụzịaka nke mbufe ụgwọ). Ndị transistor carbon carbon niile nwere ike ịgbatị nke ukwuu nwere ike mee ka optoelectronics gbatịa ọkaibe.
Eletrọnịkị transperent nwere ike ịgbatị bụ ubi na-eto eto nke nwere ngwa dị mkpa na sistemụ biointegrated dị elu (1, 2) yana ikike ijikọ na optoelectronics gbatịa (3, 4) iji mepụta roboti dị nro na ngosipụta ọkaibe. Graphene na-egosiputa ihe ndị a na-achọsi ike nke ọkpụrụkpụ atomiki, nghọta dị elu na ịdị elu, mana mmejuputa ya na ngwa ndị nwere ike ịgbatị egbochiri ya site n'ọchịchọ ọ na-agbawa na obere nsogbu. Imeri njedebe ọrụ nke graphene nwere ike ime ka arụ ọrụ ọhụrụ dị na ngwaọrụ ndị nwere ike ịgbatị.
Njirimara pụrụ iche nke graphene na-eme ka ọ bụrụ onye na-akwado ike maka ọgbọ na-esote nke electrodes transperent transperent (5, 6). E jiri ya tụnyere onye nduzi transperent a na-ejikarị eme ihe, indium tin oxide [ITO; 100 ohms/square (sq) na 90% nghọta ], monolayer graphene toro site na ikuku vapor deposition (CVD) nwere ngwakọta yiri nke mgbochi mpempe akwụkwọ (125 ohms / sq) na nghọta (97.4%) (5). Na mgbakwunye, ihe nkiri graphene nwere mgbanwe pụrụ iche ma e jiri ya tụnyere ITO (7). Dịka ọmụmaatụ, na mkpụrụ rọba, enwere ike idowe omume ya ọbụlagodi maka radius na-ehulata nke obere ka 0.8 mm (8). Iji kwalite arụmọrụ eletrik ya dị ka onye nduzi na-agbanwe agbanwe, ọrụ ndị gara aga emepụtala ngwakọ graphene nwere otu -dimensional (1D) silver nanowires ma ọ bụ carbon nanotubes (CNTs) (9-11). Ọzọkwa, ejiri graphene mee ihe dị ka electrodes maka ngwakọta akụkụ heterostructural semiconductors (dị ka 2D nnukwu Si, 1D nanowires / nanotubes, na 0D quantum dots) (12), transistors na-agbanwe agbanwe, mkpụrụ ndụ anyanwụ, na diodes na-emitting ọkụ (LEDs) (13). —23).
Ọ bụ ezie na graphene egosila nsonaazụ na-ekwe nkwa maka ngwa eletrọnịkị na-agbanwe agbanwe, ngwa ya na ngwa elektrọn nwere ike ịgbatị ejedebere site na akụrụngwa ya (17, 24, 25); graphene nwere ihe isi ike n'ime ụgbọ elu nke 340 N/m yana modul nke Young nke 0.5 TPa (26). Netwọk carbon-carbon siri ike anaghị enye usoro mkpofu ume maka eriri etinyere ya mere ọ na-agbaji ngwa ngwa na ihe na-erughị 5% ahụhụ. Dịka ọmụmaatụ, CVD graphene bufere na polydimethylsiloxane (PDMS) na-agbanwe agbanwe nwere ike ịnọgide na-arụ ọrụ ya na ihe na-erughị 6% nje (8). Ngụkọta usoro ihe ọmụmụ na-egosi na nchikota na mkparịta ụka n'etiti ọkwa dị iche iche kwesịrị ibelata isi ike (26). Site n'ịkọba graphene n'ime ọtụtụ ọkwa, a na-akọ na graphene bi- ma ọ bụ trilayer nwere ike ịgbatị ruo 30%, na-egosipụta mgbanwe nguzogide ugboro iri na atọ karịa nke monolayer graphene (27). Agbanyeghị, ndọtị a ka dị ala karịa ka ndị c onductor nwere ike ịgbatị ọgbara ọhụrụ (28, 29).
Transistor dị mkpa na ngwa nwere ike ịgbatị n'ihi na ha na-eme ka ọgụgụ ihe mmetụta ọkaibe na nyocha mgbaàmà (30, 31). Transistors na PDMS nwere multilayer graphene dị ka isi iyi / igbapu electrodes na ọwa ihe nwere ike ịnọgide na-arụ ọrụ eletriki ruo 5% nsogbu (32), nke dị ịrịba ama n'okpuru uru kacha nta achọrọ (~ 50%) maka ndị na-ahụ maka nlekọta ahụike na anụ eletrọnịkị. 33, 34). N'oge na-adịbeghị anya, a nyochara ụzọ graphene kirigami, na transistor gated site na mmiri mmiri electrolyte nwere ike ịgbatị ruo 240% (35). Otú ọ dị, usoro a chọrọ graphene kwụsịtụrụ, nke na-eme ka usoro mmepụta ahụ sie ike.
N'ebe a, anyị na-enweta ngwaọrụ graphene nwere ike ịgbatị nke ukwuu site na ịgbanye akwụkwọ mpịakọta graphene (~ 1 ruo 20 μm ogologo, ~ 0.1 ruo 1 μm n'obosara, na ~ 10 ruo 100 nm dị elu) n'etiti ọkwa graphene. Anyị na-eche na akwụkwọ mpịakọta graphene ndị a nwere ike inye ụzọ ndị na-eduzi iji kpuchido mgbape na mpempe akwụkwọ graphene, si otú a na-enwe mmetụta dị elu n'okpuru nsogbu. Akwụkwọ mpịakọta graphene anaghị achọ njikọ ma ọ bụ usoro ọzọ; a na-etolite ha n'oge usoro mbufe mmiri. Site na iji multilayer G/G (graphene / graphene) mpịakọta (MGGs) graphene agbatị electrodes (isi iyi / drain na ọnụ ụzọ ámá) na semiconducting CNTs, anyị na-enwe ike igosipụta nke ukwuu transperent na nke ukwuu na-agbatị ihe niile-carbon transistors, nke nwere ike gbatịa na 120. % nsogbu (yiri na ntụzịaka nke mbufe ụgwọ) ma na-ejigide 60% nke mmepụta mbụ ha dị ugbu a. Nke a bụ transistor dabere na carbon kachasị agbatị ruo ugbu a, ọ na-enye ugbu a zuru oke iji kwọọ LED inorganic.
Iji mee ka igwe elektrọd graphene nwere ike ịgbatị nke ukwuu, anyị họọrọ graphene toro CVD na Cu foil. A kwụsịtụrụ Cu foil n'etiti etiti CVD quartz tube iji kwe ka uto nke graphene n'akụkụ abụọ, na-akpụ ihe owuwu G/Cu/G. Iji nyefee graphene, anyị na-ebu ụzọ kpuchie obere oyi akwa nke poly (methyl methacrylate) (PMMA) iji chebe otu akụkụ nke graphene, nke anyị kpọrọ topside graphene (ọzọ maka akụkụ nke ọzọ nke graphene), ma emesịa, A na-etinye ihe nkiri dum (PMMA/top graphene/Cu/n'okpuru graphene) na (NH4) 2S2O8 ngwọta iji kpochapụ Cu foil. Graphene dị n'akụkụ ala na-enweghị mkpuchi PMMA ga-enwekwa mgbawa na ntụpọ nke na-ekwe ka ihe na-eme ka ọ banye (36, 37). Dị ka e gosiri na fig. 1A, n'okpuru mmetụta nke erughị ala nke elu, ngalaba graphene ewepụtara na-atụgharị n'ime akwụkwọ mpịakọta ma mesịa tinye ya na ihe nkiri G/PMMA fọdụrụnụ. Enwere ike ibufe akwụkwọ mpịakọta G/G n'elu na mkpụrụ ọ bụla, dị ka SiO2/Si, iko, ma ọ bụ polymer dị nro. Ịmegharị usoro mbufe a ọtụtụ ugboro n'otu mkpụrụ na-enye nhazi MGG.
(A) Ntụle atụmatụ nke usoro nrụpụta maka MGG dị ka electrode nwere ike ịgbatị. N'oge mbufe graphene, a na-agbaji graphene azụ na Cu foil na oke na ntụpọ, tụgharịa n'ụdị aka ike, wee tinye ya na fim ndị dị elu, na-akpụ nanoscrolls. Katuun nke anọ na-egosi nhazi MGG ekpokọtara. (B na C) njirimara TEM dị elu nke monolayer MGG, na-elekwasị anya na monolayer graphene (B) na mpaghara mpịakọta (C), n'otu n'otu. Ntinye nke (B) bụ onyonyo na-ebuwanye elu dị ala na-egosi mkpokọta ọdịdị nke monolayer MGGs na grid TEM. Ntinye nke (C) bụ profaịlụ siri ike ewepụtara n'akụkụ igbe akụkụ anọ egosipụtara na onyonyo a, ebe anya n'etiti ụgbọ elu atọm bụ 0.34 na 0.41 nm. (D) Carbon K-eti EEL ụdịdị dị iche iche nwere njirimara eserese π* na σ* kacha elu akpọrọ. (E) Foto akụkụ AFM nke akwụkwọ mpịakọta monolayer G/G nwere profaịlụ dị elu n'akụkụ ahịrị nwere ntụpọ edo edo. (F ruo I) microscopy anya na onyonyo AFM nke trilayer G na-enweghị (F na H) yana akwụkwọ mpịakọta (G na I) na 300-nm-oke SiO2/Si substrates, n'otu n'otu. Akpọnyere akwụkwọ mpịakọta ndị nnọchite anya na wrinkles iji gosipụta ọdịiche ha.
Iji chọpụta na akwụkwọ mpịakọta ndị ahụ bụ graphene n'okike, anyị duziri ihe nyocha eletrọnịkị eletrọnịkị nke ukwuu (TEM) na ọnwụ ike elektrọn (EEL) n'ihe gbasara akwụkwọ mpịakọta monolayer top-G/G. Onyonyo 1B na-egosi nhazi hexagonal nke monolayer graphene, na ntinye bụ mkpokọta morphology nke ihe nkiri ahụ kpuchiri n'otu oghere carbon nke grid TEM. The monolayer graphene na-agbasa ọtụtụ n'ime grid, na ụfọdụ graphene flakes na ọnụnọ nke multiple stacks nke hexagonal yiri mgbaaka na-apụta (Fig. 1B). Site n'ịbanye n'ime akwụkwọ mpịakọta nke ọ bụla (Fig 1C), anyị hụrụ ọnụ ọgụgụ dị ukwuu nke graphene lattice fringes, na oghere lattice dị na 0.34 ruo 0.41 nm. Ntụle ndị a na-egosi na a na-atụgharị flakes ndị ahụ na-enweghị usoro na ha ezughị oke graphite, nke nwere oghere lattice nke 0.34 nm na akwa akwa "ABAB". Ihe osise 1D na-egosi ụdị carbon K-edge EEL, ebe ọnụ ọgụgụ kasị elu na 285 eV sitere na π * orbital na nke ọzọ gburugburu 290 eV bụ n'ihi mgbanwe nke σ * orbital. Enwere ike ịhụ na njikọ sp2 na-achịkwa n'usoro a, na-achọpụta na akwụkwọ mpịakọta ndị ahụ nwere nnukwu eserese.
Ihe onyonyo anya na ihe onyonyo atomiki (AFM) na-enye nghọta na nkesa graphene nanoscrolls na MGG (Fig 1, E ruo G, na fig S1 na S2). A na-ekesa akwụkwọ mpịakọta ndị ahụ na-akpaghị aka n'elu elu, njupụta nke ụgbọ elu ha na-abawanye nha anya na ọnụ ọgụgụ nke akwakọbara. Ọtụtụ akwụkwọ mpịakọta ka a na-atụgharị n'ime mara mma ma gosipụta ịdị elu na-adịghị ahụkebe n'ogo nke 10 ruo 100 nm. Ha dị 1 ruo 20 μm ogologo yana 0.1 ruo 1 μm n'obosara, dabere na nha nke flakes graphene mbụ ha. Dị ka e gosiri na Fig. 1 (H na I), akwụkwọ mpịakọta ndị ahụ nwere nnukwu nnukwu nha karịa wrinkles, na-eduga n'ọhụụ dị njọ karịa n'etiti ọkwa graphene.
Iji tụọ akụrụngwa eletrik, anyị na-eji fotolithography were ma ọ bụ na-enweghị usoro mpịakọta mee ihe nkiri graphene na oyi akwa na-etinye n'ime ibe 300-μm n'obosara na 2000-μm ogologo. A tụrụ nkwụsi ike nyocha abụọ dịka ọrụ nke nsogbu n'okpuru ọnọdụ gburugburu. Ọnụnọ nke akwụkwọ mpịakọta belatara resistivity maka monolayer graphene site na 80% na naanị 2.2% mbelata na nnyefe (fig. S4). Nke a na-akwado na nanoscrolls, nke nwere njupụta dị elu ugbu a ruo 5 × 107 A / cm2 (38, 39), na-enye onyinye eletrik dị mma na MGG. N'ime mono-, bi-, na trilayer plain graphene na MGGs, trilayer MGG nwere omume kacha mma yana nghọta nke ihe fọrọ nke nta ka ọ bụrụ 90%. Iji tụnyere isi mmalite ndị ọzọ nke graphene a kọrọ na akwụkwọ ndị ahụ, anyị tụlekwara ihe mgbochi mpempe akwụkwọ anọ (fig. S5) ma depụta ha dị ka ọrụ nke nnyefe na 550 nm (fig. S6) na Fig. 2A. MGG na-egosi nhụsianya na nghọta atụnyere ma ọ bụ dị elu karịa graphene multila yer plain graphene na mbelata graphene oxide (6, 8, 18). Rịba ama na mpempe akwụkwọ resistances nke artificially stacked multilayer plain graphene si akwụkwọ dị ubé elu karịa nke anyị MGG, eleghị anya n'ihi na ha unoptimized uto ọnọdụ na nyefe usoro .
(A) Mgbochi mpempe akwụkwọ nyocha anọ na mbufe na 550 nm maka ọtụtụ ụdị graphene, ebe oghere ojii na-egosi mono-, bi-, na trilayer MGGs; okirikiri uhie na triangles na-acha anụnụ anụnụ kwekọrọ na graphene multilayer toro na Cu na Ni site na ọmụmụ nke Li et al. (6) na Kim et al. (8), n'otu n'otu, ma emesịa bufee ya na SiO2/Si ma ọ bụ quartz; na triangles akwụkwọ ndụ akwụkwọ ndụ bụ ụkpụrụ maka RGO na ọkwa dị iche iche ibelata site na ọmụmụ nke Bonaccorso et al. ( nke iri na asatọ). (B na C) Ngbanwe nguzogide ngbanwe nke mono-, bi- na trilayer MGGs na G dị ka ọrụ nke perpendicular (B) na myirịta (C) na ntụzịaka nke eruba ugbu a. (D) Mgbanwe nguzogide nke bilayer G (acha uhie uhie) na MGG (ojii) n'okpuru ụdị cyclic na-ebufe ihe ruru 50% perpendicular strain. (E) Mgbanwe nguzogide nke trilayer G (acha uhie uhie) na MGG (ojii) n'okpuru ụdị cyclic na-ebufe ruo 90% ụdị yiri ya. (F) Mgbanwe ikike nke mono-, bi- na trilayer G na bi- na trilayer MGG dị ka ọrụ n nke nje. Ihe ntinye bụ ihe nrụpụta capacitor, ebe mkpụrụ okwu polymer bụ SEBS na oyi akwa polymer dielectric bụ 2-μm-oke SEBS.
Iji nyochaa arụmọrụ na-adabere na MGG, anyị na-ebufe graphene na thermoplastic elastomer styrene-etylene-butadiene-styrene (SEBS) substrates (~ 2 cm n'obosara na ~ 5 cm ogologo), na a na-atụle conductivity ka a na-agbatị mkpụrụ ahụ. (lee Akụrụngwa na Ụzọ) ma perpendicular na yiri ntụziaka nke ugbu a eruba (Fig. 2, B na C). Omume eletrik na-adabere na eriri ahụ kwalitere site na ntinye nke nanoscrolls na ọnụ ọgụgụ graphene na-abawanye. Dịka ọmụmaatụ, mgbe nsogbu na-adaba n'ụzọ dị ugbu a, maka monolayer graphene, mgbakwunye nke akwụkwọ mpịakọta na-abawanye nsogbu na mgbaji eletrik site na 5 ruo 70%. A na-abawanye nnabata nke graphene trilayer nke ukwuu ma e jiri ya tụnyere graphene monolayer. Site na nanoscrolls, na 100% perpendicular strain, nguzogide nke trilayer MGG Ọdịdị na-abawanye site na 50%, ma e jiri ya tụnyere 300% maka trilayer graphene na-enweghị akwụkwọ mpịakọta. A nyochara mgbanwe nguzogide n'okpuru ibu ibu cyclic. Maka ntụnyere (Fig. 2D), nkwụsị nke ihe nkiri graphene dị larịị mụbara ihe dị ka ugboro 7.5 mgbe usoro ~ 700 gasịrị na 50% perpendicular strain ma nọgide na-abawanye na nsogbu na nke ọ bụla okirikiri. N'aka nke ọzọ, nguzogide nke MGG bilayer na-abawanye ihe dị ka ugboro 2.5 mgbe ~ 700 cycles gasịrị. N'itinye ihe ruru 90% nsogbu n'akụkụ ntụziaka yiri ya, nkwụsị nke trilayer graphene mụbara ~ 100 ugboro mgbe 1000 cycles, ebe ọ bụ nanị ~ 8 ugboro na trilayer MGG (Fig 2E). E gosipụtara nsonaazụ ịgba ígwè na fig. S7. Mmụba na-adị ngwa ngwa na nguzogide n'akụkụ ntụzịaka nhịahụ yiri ya bụ n'ihi na nghazi nke mgbape na-adaba na ntụzịaka nke eruba ugbu a. Ntughari nke nguzogide n'oge ibu na ibu ibu bu n'ihi mgbake viscoelastic nke mkpụrụ osisi elastomer SEBS. Nkwụsi ike siri ike nke ibe MGG n'oge ịgba ígwè bụ n'ihi ọnụnọ nke nnukwu akwụkwọ mpịakọta ndị nwere ike imechi akụkụ ndị gbawara agbawa nke graphene (dị ka AFM na-ahụ anya), na-enyere aka ịnọgide na-enwe okporo ụzọ na-asọ oyi. A kọwapụtala ihe omume a nke idowe conductivity site n'ụzọ na-agbawa agbawa na mbụ maka igwe gbawara agbawa ma ọ bụ ihe nkiri semiconductor na elastomer substrates (40, 41).
Iji nyochaa ihe nkiri ndị a dabeere na graphene dị ka electrodes ọnụ ụzọ na ngwaọrụ ndị nwere ike ịgbatị, anyị kpuchiri graphene oyi akwa na SEBS dielectric oyi akwa (2 μm oké) ma nyochaa mgbanwe ike dielectric dị ka ọrụ nke nsogbu (lee fig. 2F na ihe mgbakwunye maka nkọwa). Anyị chọpụtara na ike nwere monolayer larịị na bilayer graphene electrodes belatara ngwa ngwa n'ihi mfu nke graphene n'ime ụgbọ elu. N'ụzọ dị iche, ikike ikike nke MGG gbakọtara yana trilayer graphene dị larịị gosipụtara mmụba nke ikike ya na eriri, nke a na-atụ anya ya n'ihi mbelata ọkpụrụkpụ dielectric na eriri. Mmụba a na-atụ anya ya na capacitance dabara nke ọma na nhazi MGG (fig. S8). Nke a na-egosi na MGG kwesịrị ekwesị dị ka ọnụ ụzọ ámá electrode maka agbatị transistor.
Iji nwetakwuo nyocha ọrụ nke akwụkwọ mpịakọta graphene 1D na ntachi obi nke eletriki ma jikwaa nkewa nke ọma nke dị n'etiti ọkwa graphene, anyị na-eji CNT nwere mkpuchi mmiri dochie akwụkwọ mpịakọta graphene (lee Ngwa mgbakwunye). Iji ṅomie ihe owuwu MGG, anyị debere njupụta atọ nke CNT (ya bụ, CNT1).
(A ruo C) onyonyo AFM nke njupụta atọ dị iche iche nke CNT (CNT1
Iji ghọtakwuo ikike ha dị ka electrodes maka ngwa eletrọnịkị nwere ike ịgbatị, anyị nyochara usoro nke MGG na G-CNT-G n'okpuru nsogbu. Optical microscopy na scanning eletrọn microscopy (SEM) na-adịghị irè e ji mara ụzọ n'ihi na ma enweghị agba iche na SEM bụ isiokwu image artifacts n'oge eletrọn scanning mgbe graphene bụ na polymer substrates (fig. S9 na S10). Iji hụ na ebe dị n'elu graphene dị n'okpuru nsogbu, anyị na-anakọta nha AFM na trilayer MGGs na graphene dị larịị mgbe ebufechara n'elu dị ezigbo mkpa (~ 0.1 mm thick) na ihe na-agbanwe SEBS. N'ihi nrụrụ dị n'ime na CVD graphene na mmebi extrinsic n'oge usoro mbufe, a na-emepụta ihe mgbawa na graphene dị mgbagwoju anya, ma na-abawanye ụba, mgbawa ahụ ghọrọ denser (Fig 4, A na D). Dabere na stacking Ọdịdị nke carbon dabeere na electrodes, cracks na-egosipụta dị iche iche morphologies (fig. S11) (27). Njupụta mpaghara mgbawa (akọwapụtara dị ka ebe mgbape / ebe a na-enyocha) nke graphene multilayer dị obere karịa nke monolayer graphene mgbe nsogbu gasịrị, nke kwekọrọ na mmụba nke eletriki eletrik maka MGG. N'aka nke ọzọ, a na-ahụkarị akwụkwọ mpịakọta ka ọ na-ejikọta ihe ndị ahụ gbawara agbawa, na-enye ụzọ ndị ọzọ na-eduzi na fim ahụ nwere nsogbu. Dịka ọmụmaatụ, dị ka akpọrọ na foto nke 4B, akwụkwọ mpịakọta buru ibu gafere n'elu mgbape na trilayer MGG, ma ọ dịghị akwụkwọ mpịakọta a hụrụ na graphene dị larịị (Fig 4, E ruo H). N'otu aka ahụ , CNTs nwekwara bridged na cracks na graphene (fig. S11). A na-achịkọta njupụta ebe mgbape, njupụta mpaghara mpịakọta, na adịghị ike nke ihe nkiri ahụ na Fig. 4K.
(A ruo H) N'ebe ahụ, onyonyo AFM nke akwụkwọ mpịakọta G/G trilayer (A ruo D) na ihe owuwu trilayer G (E ruo H) na elastomer SEBS (~ 0.1 mm gbara ọkpụrụkpụ) na 0, 20, 60, na 100 % nje. E ji akụ tụọ mgbawa na akwụkwọ mpịakọta ndị nnọchite anya. Ihe oyiyi AFM niile dị na mpaghara 15 μm × 15 μm, na-eji otu ihe nrịbama agba dị ka akpọpụtara. (I) Geometry simulation nke electrodes monolayer graphene e depụtara na mkpụrụ SEBS. (J) Map contour nke simulation nke oke logarithmic kacha dị na monolayer graphene na mkpụrụ SEBS na eriri mpụta 20%. (K) Ntụle nke njupụta ebe mgbape (kọlụm uhie), njupụta mpaghara mpịakọta (kọlụm odo), na njupụta elu (kọlụm na-acha anụnụ anụnụ) maka nhazi graphene dị iche iche.
Mgbe ihe nkiri MGG gbatịpụrụ, enwere usoro mgbakwunye dị mkpa nke akwụkwọ mpịakọta ndị ahụ nwere ike ijikọ mpaghara graphene gbawara agbawa, na-ejigide netwọkụ na-eme mkpọtụ. Akwụkwọ mpịakọta graphene na-ekwe nkwa n'ihi na ha nwere ike ịdị ọtụtụ iri micrometer n'ogologo wee nwee ike ijikwa mgbawa ndị na-adịkarị ihe ruru micrometer. Ọzọkwa, n'ihi na akwụkwọ mpịakọta ndị ahụ nwere ọtụtụ graphene, a na-atụ anya na ha ga-enwe obere nguzogide. N'iji ya tụnyere, a chọrọ netwọk CNT dị oke oke (mgbanwe dị ala) iji nye ikike ijikọ ọnụ, ebe CNT dị obere (nke na-abụkarị micrometer ole na ole n'ogologo) ma na-eduzi ya karịa akwụkwọ mpịakọta. N'aka nke ọzọ, dị ka e gosiri na fig. S12, ebe graphene na-agbaji n'oge ọ na-agbatị iji nabata nsogbu, akwụkwọ mpịakọta ndị ahụ adịghị agbawa, na-egosi na nke ikpeazụ nwere ike na-adaba na graphene dị n'okpuru. Ihe kpatara na ha anaghị agbawa nwere ike ịbụ n'ihi usoro a kpọkọtara, nke nwere ọtụtụ graphene (~ 1 ruo 2 0 μm ogologo, ~ 0.1 ruo 1 μm n'obosara, na ~ 10 ruo 100 nm elu), nke nwere. modul dị elu dị elu karịa graphene otu oyi akwa. Dị ka a kọrọ Green na Hersam (42), dara CNT netwọk (tube dayameta nke 1.0 nm) nwere ike nweta ala mpempe akwụkwọ resistances <100 ohms/sq n'agbanyeghị nnukwu junction eguzogide n'etiti CNTs. N'iburu n'uche na akwụkwọ mpịakọta graphene anyị nwere obosara nke 0.1 ruo 1 μm yana na akwụkwọ mpịakọta G/G nwere mpaghara kọntaktị buru ibu karịa CNT, nkwụsị kọntaktị na mpaghara kọntaktị n'etiti akwụkwọ mpịakọta graphene na graphene ekwesịghị ịbụ ihe na-amachi ihe iji nọgide na-arụ ọrụ dị elu.
Graphene nwere modul dị elu karịa mkpụrụ nke SEBS. Ọ bụ ezie na ịdị irè ọkpụrụkpụ nke graphene electrode dị nnọọ ala karịa nke mkpụrụ, isi ike nke graphene ugboro ya ọkpụrụkpụ bụ tụnyere nke mkpụrụ (43, 44), na-akpata a agafeghị oke isiike-agwaetiti mmetụta. Anyị mere nrụrụ nke graphene dị 1 nm na mkpụrụ SEBS (lee Ngwa mgbakwunye maka nkọwa). Dị ka simulation simulation, mgbe 20% nsogbu na-etinyere na SEBS substrate n'èzí, nkezi nsogbu na graphene bụ ~ 6.6% (Fig. 4J na fig. S13D), nke kwekọrọ na nnwale nlele (lee fig. S13) . Anyị na-atụnyere nhụsianya dị na mpaghara graphene e kpụrụ akpụ na mkpụrụ osisi site na iji microscopy anya wee hụ na nsogbu dị na mpaghara mkpụrụ osisi dị ma ọ dịkarịa ala ugboro abụọ na mpaghara graphene. Nke a na-egosi na enwere ike ịjichi ụdị ahụ a na-etinye na usoro electrode graphene, na-eme agwaetiti graphene siri ike n'elu SEBS (26, 43, 44).
Ya mere, ike nke MGG electrodes iji nọgide na-arụ ọrụ dị elu n'okpuru nnukwu nsogbu nwere ike ime ya site na usoro abụọ bụ isi: (i) Akwụkwọ mpịakọta ndị ahụ nwere ike ijikọ mpaghara ndị a kwụsịrị iji nọgide na-enwe okporo ụzọ percolation, na (ii) multilayer graphene sheets / elastomer nwere ike ịfefe. n'elu ibe ha, na-akpata mbelata nsogbu na graphene electrodes. Maka ọtụtụ ọkwa nke graphene bufee na elastomer, a naghị ejikọta akwa ahụ na ibe ya nke ọma, nke nwere ike ịfesa na nzaghachi na nsogbu (27). Akwụkwọ mpịakọta ndị ahụ mekwara ka ọ dị njọ nke n'ígwé graphene, nke nwere ike inye aka mee ka nkewa dị n'etiti graphene dị elu ma mee ka ọkpụkpụ graphene dị elu.
A na-eji ịnụ ọkụ n'obi na-achụ ngwaọrụ carbon niile n'ihi ọnụ ahịa dị ala yana nnukwu mmepụta ya. N'ọnọdụ anyị, a na-emepụta transistor-carbon niile site na iji ọnụ ụzọ graphene nke ala, kọntaktị graphene dị elu / mmiri mmiri, ihe nchịkọta CNT nke edoziri, na SEBS dị ka dielectric (Fig 5A). Dị ka e gosiri na fig. 5B, ihe niile-carbon ngwaọrụ na CNTs dị ka isi iyi/drain na ọnụ ụzọ (ala ngwaọrụ) bụ ihe opaque karịa ngwaọrụ na graphene electrodes (top ngwaọrụ). Nke a bụ n'ihi na netwọk CNT chọrọ ibu ọkpụrụkpụ na, ya mere, nnyefe ngwa anya dị ala iji nweta ihe mgbochi mpempe akwụkwọ yiri nke graphene (fig. S4). Ọnụọgụ 5 (C na D) na-egosi nnyefe nnọchite anya na mpụta mmepụta tupu nsogbu maka transistor nke ejiri bilayer MGG electrodes mee. Obosara ọwa na ogologo nke transistor enweghị eriri bụ 800 na 100 μm, n'otu n'otu. Oke ngbanyụ/mgbanyụ tụrụ atụ karịa 103 yana mgbanyụ ọkụ ma ọ bụ mgbanyụ na ọkwa 10−5 na 10–8 A, n'otu n'otu. Usoro mmepụta ahụ na-egosipụta usoro usoro ahịrị dị mma yana n'ụzọ doro anya dabere n'ọnụ ụzọ voltaji, na-egosi ezigbo kọntaktị n'etiti CNTs na graphene electrodes (45). Achọpụtara nguzogide kọntaktị na electrodes graphene ka ọ dị ala karịa nke ihe nkiri Au kpochapuru (lee fig S14). Ntugharị saturation nke transistor nwere ike ịgbatị bụ ihe dịka 5.6 cm2/Vs, yiri nke otu polymer-iche CNT transistor na siri ike Si substrates na 300-nm SiO2 dị ka dielectric oyi akwa. Ọganihu ọzọ na ngagharị ga-ekwe omume site na njupụta tube kachasị mma na ụdị tubes ndị ọzọ (46).
(A) Atụmatụ transistor dabere na graphene. SWNTs, carbon nanotubes nwere otu mgbidi. (B) Foto nke transistor nwere ike ịgbatị nke electrodes graphene (n'elu) na electrodes CNT (n'okpuru). Ọdịiche dị na nghọta pụtara nke ọma. (C na D) Ntufe na mmepụta nke transistor dabeere na graphene na SEBS tupu nsogbu. (E na F) Nyefee akụkụ, ngbanyụ na gbanyụọ ugbu a, nha ọkụ/ gbanyụọ, yana ngagharị nke transistor dabere na graphene n'ụdị dị iche iche.
Mgbe ngwaọrụ ikuku carbon niile gbatịpụrụ n'ụzọ dị ka usoro mbufe chaja, ahụrụ obere mmebi ihe ruru 120%. N'oge ịgbatị, mmegharị ahụ nọgidere na-ebelata site na 5.6 cm2/Vs na 0% stran' na 2.5 cm2 / Vs na 120% nsogbu (Fig. 5F). Anyị tụlekwara arụmọrụ transistor maka ogologo ọwa dị iche iche (lee tebụl S1). N'ụzọ doro anya, n'ụdị buru ibu dị ka 105%, transistor ndị a niile ka gosipụtara oke ngbanyụ ma ọ bụ gbanyụọ (> 103) na ngagharị (> 3 cm2 / Vs). Na mgbakwunye, anyị chịkọtara ọrụ niile na-adịbeghị anya na transistor carbon niile (lee tebụl S2) (47-52). Site na ịkwalite nrụpụta ngwaọrụ na elastomers yana iji MGG dị ka kọntaktị, transistor carbon anyị niile na-egosi arụmọrụ dị mma n'ihe gbasara ngagharị na hysteresis yana ịdị ogologo ogologo.
Dị ka ngwa nke transistor transperent zuru oke na nke nwere ike ịgbatị, anyị na-eji ya chịkwaa ngbanwe nke LED (Fig 6A). Dị ka e gosiri na fig. 6B, green LED nwere ike ịhụ n'ụzọ doro anya site na stretchable niile-carbon ngwaọrụ etinye ozugbo n'elu. Ka ọ na-agbatị ruo ~ 100% (Fig 6, C na D), ọkụ ọkụ ọkụ LED adịghị agbanwe agbanwe, nke kwekọrọ na arụmọrụ transistor nke akọwara n'elu (lee ihe nkiri S1). Nke a bụ akụkọ mbụ nke nkeji njikwa na-agbatị agbatị mere site na iji electrodes graphene, na-egosipụta ohere ọhụrụ maka ngwa elektrọnik agbatị graphene.
(A) Circuit nke transistor iji kwọọ LED. GND, ala. (B) Foto nke transistor carbon nke nwere ike ịgbatị na nke na-enweghị atụ na eriri 0% etinyere n'elu ọkụ ọkụ ndụ ndụ. (C) transistor transperent na ndọtị na-agbatị carbon niile ejiri iji gbanwee LED na-etinye ya n'elu LED na 0% (n'aka ekpe) na ~ 100% nje (n'aka nri). Àkụ́ ọcha na-atụ aka dị ka ihe nrịbama edo edo dị na ngwaọrụ ahụ iji gosi mgbanwe anya na-agbatị. (D) Nleba anya n'akụkụ transistor agbatị agbatị, ebe ọkụ na-agbanye n'ime elastomer.
N'ikpeazụ, anyị ewepụtala ihe owuwu graphene na-eduzi transperent nke na-edobe ụkpụrụ dị elu n'okpuru nnukwu nsogbu dị ka electrodes nwere ike ịgbatị, nke graphene nanoscrolls na-enyere ya aka n'etiti ọkwa graphene. Ndị a bi- na trilayer MGG electrode Ọdịdị na elastomer nwere ike idowe 21 na 65%, n'otu n'otu, nke ha 0% nje conductivities na a nsogbu dị elu dị ka 100%, ma e jiri ya tụnyere zuru ezu ọnwụ nke conductivity na 5% nje maka ahụkarị monolayer graphene electrodes. . Ụzọ ndị ọzọ na-eduzi akwụkwọ mpịakọta graphene yana mmekọrịta adịghị ike n'etiti ọkwa ndị a bufere ya na-enye aka na nkwụsi ike conductivity dị elu n'okpuru nsogbu. Anyị gara n'ihu tinye usoro graphene a iji mepụta transistor nwere ike ịgbatị carbon niile. Ka ọ dị ugbu a, nke a bụ transistor dabere na graphene nke nwere nghọta kachasị mma na-ejighi ihe mgbochi. Ọ bụ ezie na e mere ọmụmụ ihe ugbu a iji mee ka graphene maka ngwá electronic nwere ike ịgbatị, anyị kwenyere na a ga-agbatị usoro a na ihe 2D ndị ọzọ iji mee ka ngwá electronic 2D nwee ike ịgbatị.
A na-etolite nnukwu mpaghara CVD graphene na nkwụsịtụ Cu (99.999%; Alfa Aesar) n'okpuru nrụgide mgbe nile nke 0.5 mtorr na 50-SCCM (ọkọlọtọ cubic centimita kwa nkeji) CH4 na 20-SCCM H2 dị ka ndị na-ebu ụzọ na 1000 ° C. E ji monolayer graphene kpuchie akụkụ abụọ nke foil Cu. Ekpuchiri oyi akwa dị mkpa nke PMMA (2000 rpm; A4, Microchem) n'otu akụkụ nke foil Cu, na-akpụ usoro PMMA/G/Cu foil/G. N'ikpeazụ, etinyere ihe nkiri ahụ dum na 0.1 M ammonium persulfate [(NH4) 2S2O8] ngwọta maka ihe dị ka awa 2 iji wepụsịa foil Cu. N'oge usoro a, graphene azụ azụ na-enweghị nchebe na-ebu ụzọ dọwaa n'akụkụ oke ọka wee tụgharịa n'ime akwụkwọ mpịakọta n'ihi esemokwu elu. E tinyere akwụkwọ mpịakọta ndị ahụ na ihe nkiri graphene elu nke PMMA na-akwado, na-akpụ akwụkwọ mpịakọta PMMA/G/G. A na-asachapụ ihe nkiri ndị ahụ na mmiri deionized ọtụtụ oge ma dọba ya na mkpụrụ ezubere iche, dị ka SiO2/Si siri ike ma ọ bụ mkpụrụ rọba. Ozugbo ihe nkiri ahụ agbakwunyere akpọnwụwo na mkpụrụ, ihe nlele w dị ka nke a na-agbanye na acetone, 1: 1 acetone / IPA ( mmanya isopropyl), na IPA maka 30 s nke ọ bụla iji wepụ PMMA. A na-ekpo ọkụ na ihe nkiri ahụ na 100 ° C maka 15 min ma ọ bụ debe ya n'ime oghere n'abali iji wepụ mmiri ahụ ejidere kpamkpam tupu e nyefee akwụkwọ mpịakọta G/G ọzọ na ya. Nzọụkwụ a bụ iji zere iwepụ ihe nkiri graphene site na mkpụrụ osisi ahụ ma hụ na mkpuchi MGG zuru ezu n'oge mwepụta nke oyi akwa ụgbọelu PMMA.
A na-ahụ morphology nke ihe owuwu MGG site na iji microscope anya (Leica) na microscope eletrọn na-enyocha (1 kV; FEI). A na-arụ ọrụ microscope nke ike atomic (Nanoscope III, Digital Instrument) na ọnọdụ ịpị iji hụ nkọwa nke akwụkwọ mpịakọta G. A nwalere nghọta ihe nkiri site na ultraviolet na-ahụ anya spectrometer (Agilent Cary 6000i). Maka ule ndị ahụ mgbe eriri ahụ dị n'akụkụ ụzọ ntụgharị nke ugbu a, a na-eji fotolithography na plasma O2 mee ka usoro graphene dị n'ime ibe (~ 300 μm n'obosara na ~ 2000 μm ogologo), na Au (50 nm) electrodes na-echekwara site na iji ọkụ. ihe mkpuchi onyinyo na nsọtụ abụọ nke ogologo akụkụ. A na-etinye eriri graphene na kọntaktị na SEBS elastomer (~ 2 cm n'obosara na ~ 5 cm ogologo), na ogologo axis nke ibe ya na akụkụ dị mkpirikpi nke SEBS na-esote BOE (buffered oxide etch) (HF: H2O). 1: 6) etching na eutectic gallium indium (EGaIn) dị ka kọntaktị eletrik. Maka ule nhụsianya yiri ya, a na-ebufe graphene structur es (~ 5 × 10 mm) na-enweghị usoro na mpaghara SEBS, nke nwere ogologo axes yiri ogologo akụkụ nke SEBS. Maka ikpe abụọ ahụ, G (na-enweghị akwụkwọ mpịakọta G) / SEBS gbatịpụrụ n'akụkụ ogologo nke elastomer na ngwa akwụkwọ ntuziaka, na n'ọnọdụ ahụ, anyị tụlere mgbanwe nguzogide ha n'okpuru nsogbu na ọdụ nyocha nke nwere onye nyocha semiconductor (Keithley 4200). -SCS).
Ndị transistor carbon niile nwere ike ịgbatị nke ukwuu na nke na-agbanwe agbanwe bụ usoro ndị a ka emere iji zere mmebi ihe mgbaze nke polymer dielectric na mkpụrụ. Ebufere ihe owuwu MGG na SEBS ka ọnụ ụzọ ámá electrodes. Iji nweta otu oyi akwa polymer dielectric dị mkpa (oke 2 μm), ihe ngwọta SEBS toluene (80 mg / ml) bụ nke ekpuchiri na octadecyltrichlorosilane (OTS) - gbanwere SiO2/Si na 1000 rpm maka 1 min. Enwere ike ibufe ihe nkiri dielectric dị gịrịgịrị n'ụzọ dị mfe site na elu hydrophobic OTS n'elu mkpụrụ SEBS nke ejiri graphene akwadoro kpuchie ya. Enwere ike ịme capacitor site n'itinye igwe eletrik dị elu (EGaIn; Sigma-Aldrich) iji chọpụta ike dị ka ọrụ nke eriri site na iji LCR (inductance, capacitance, resistance) mita (Agilent). Akụkụ nke ọzọ nke transistor nwere CNT nke semiconducting nke polymer, na-agbaso usoro akọwara na mbụ (53). Emebere igwe elektrọd isi iyi/mmiri mmiri ahụ n'ụdị SiO2/Si siri ike. Mgbe nke ahụ gasịrị, akụkụ abụọ ahụ, dielectric / G / SEBS na CNTs / G / SiO2 / Si, na-ejikọta ibe ha, ma tinye ya na BOE iji wepụ ihe SiO2 / Si siri ike. Ya mere, a na-emepụta transistor ndị a na-ahụ anya nke ọma ma nwee ike ịgbatị. Emere ule eletrik n'okpuru nsogbu na nhazi nkwụtị aka dịka usoro ekwuru n'elu.
Ihe mgbakwunye maka akụkọ a dị na http://advances.sciencemag.org/cgi/content/full/3/9/e1700159/DC1
fig. S1. Onyonyo nyocha anya nke monolayer MGG na mkpụrụ SiO2/Si n'ogo dị iche iche.
fig. S4. Ntụle nke mgbochi mpempe akwụkwọ nyocha abụọ na nnyefe @550 nm nke mono-, bi- na trilayer plain graphene ( square ojii), MGG ( okirikiri uhie), na CNT (triangle anụnụ anụnụ).
fig. S7. Mgbanwe nguzogide nke mono- na bilayer MGGs (ojii) na G (red) n'okpuru ~ 1000 cyclic strain loading to 40 and 90% parallel strain, n'otu n'otu.
fig. S10. Onyinyo SEM nke trilayer MGG na SEBS elastomer mgbe nsogbu gasịrị, na-egosi ogologo akwụkwọ mpịakọta gafee ọtụtụ mgbape.
fig. S12. Ihe onyonyo AFM nke trilayer MGG na elastomer SEBS dị gịrịgịrị na eriri 20%, na-egosi na akwụkwọ mpịakọta gafere n'elu mgbape.
okpokoro S1. Mobilities nke bilayer MGG-carbon nanotube transistors nwere otu mgbidi n'ogologo ọwa dị iche iche tupu na mgbe nsogbu gasịrị.
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Site 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
Site 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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Oge nzipu: Jan-28-2021