Ihe ndị nwere akụkụ abụọ, dị ka graphene, na-adọrọ mmasị maka ngwa semiconductor nkịtị na ngwa ndị ọhụrụ na-agbanwe agbanwe na ngwa eletrọniki na-agbanwe agbanwe. Agbanyeghị, ike nrụgide dị elu nke graphene na-eme ka ọ gbawaa na obere nrụgide, na-eme ka ọ sie ike iji ihe onwunwe eletrọniki pụrụ iche ya na ngwa eletrọniki a na-agbatị agbatị. Iji mee ka arụmọrụ dị mma nke ndị na-eduzi graphene na-agbanwe agbanwe dabere na nrụgide, anyị mepụtara nanoscrolls graphene n'etiti akwa graphene a kpọkọtara, nke a na-akpọ multilayer graphene/graphene scrolls (MGGs). N'okpuru nrụgide, ụfọdụ mpịakọta jikọtara ngalaba graphene nke kewara ekewa iji nọgide na-enwe netwọk na-agbagharị nke na-eme ka njikwa dị mma na nnukwu nsogbu. Trilayer MGGs kwadoro na elastomers nọgidere na 65% nke njikwa mbụ ha na 100% nsogbu, nke dị n'akụkụ ntụziaka nke mmiri ugbu a, ebe ihe nkiri trilayer nke graphene na-enweghị nanoscrolls nọgidere na-enwe naanị 25% nke njikwa mmalite ha. Transistor carbon niile a na-agbatị agbatị nke e ji MGGs mee dị ka elektrọd gosipụtara nnyefe nke >90% ma jigide 60% nke mmepụta ugbu a mbụ ya na nrụgide 120% (dịka ntụziaka nke njem chaja). Transistor carbon niile a na-agbatị agbatị nke ukwuu ma na-apụta ìhè nwere ike ime ka optoelectronics dị mgbagwoju anya nwee ike ịgbatị.
Ngwa eletrọniki na-agbanwe agbanwe nke a na-agbatị agbatị bụ ubi na-eto eto nke nwere ngwa dị mkpa na sistemụ biointegrated dị elu (1, 2) yana ikike ijikọ na optoelectronics a na-agbatị agbatị (3, 4) iji mepụta robotik dị nro na ngosipụta dị elu. Graphene na-egosipụta ihe ndị a na-achọsi ike nke ọkpụrụkpụ atọm, nghọta dị elu, na njikwa dị elu, mana mmejuputa ya na ngwa ndị a na-agbatị agbatị ebelatala site na ọchịchọ ya ịgbawa na obere ụdị. Imeri oke ike nke graphene nwere ike ime ka ọrụ ọhụrụ dị na ngwaọrụ ndị a na-agbatị agbatị.
Njirimara pụrụ iche nke graphene na-eme ka ọ bụrụ ihe kacha mma maka ọgbọ ọzọ nke elektrọd transductive transductive (5, 6). Ma e jiri ya tụnyere onye na-eduzi transparent a na-ejikarị eme ihe, indium tin oxide [ITO; 100 ohms/sq (sq) na 90% transparent], monolayer graphene nke a na-akọ site na ihe nchekwa vapor kemịkalụ (CVD) nwere njikọ yiri nke ahụ nke iguzogide mpempe akwụkwọ (125 ohms/sq) na transparent (97.4%) (5). Na mgbakwunye, ihe nkiri graphene nwere mgbanwe pụrụ iche ma e jiri ya tụnyere ITO (7). Dịka ọmụmaatụ, na ihe mkpuchi plastik, enwere ike idobe conductance ya ọbụlagodi maka radius gbagọrọ agbagọ nke obere dị ka 0.8 mm (8). Iji mee ka arụmọrụ eletriki ya dịkwuo mma dị ka onye na-eduzi mgbanwe na-agbanwe agbanwe, ọrụ ndị gara aga emepụtala ihe ngwakọ graphene nwere otu akụkụ (1D) ọlaọcha nanowires ma ọ bụ nanotubes carbon (CNTs) (9–11). Ọzọkwa, ejirila graphene mee ihe dị ka elektrọd maka semiconductors heterostructural dị iche iche (dịka 2D bulk Si, 1D nanowires/nanotubes, na 0D quantum dots) (12), transistors na-agbanwe agbanwe, mkpụrụ ndụ anyanwụ, na diode na-ewepụta ìhè (LEDs) (13–23).
Ọ bụ ezie na graphene egosila ihe dị mma maka ngwa eletrọniki na-agbanwe agbanwe, ojiji ya na ngwa eletrọniki ndị a na-agbatị agbatịla site na njirimara igwe ya (17, 24, 25); graphene nwere ike isi ike n'ime ikuku nke 340 N/m na modulus Young nke 0.5 TPa (26). Netwọk carbon-carbon siri ike anaghị enye usoro mwepụ ike ọ bụla maka nrụgide etinyere ya, ya mere ọ na-agbawa ngwa ngwa na ihe na-erughị 5% nrụgide. Dịka ọmụmaatụ, CVD graphene ebufere na polydimethylsiloxane (PDMS) elastic substrate nwere ike ịnọgide na-enwe ike ya na ihe na-erughị 6% nrụgide (8). Ngụkọta echiche na-egosi na ịgbagọ na mmekọrịta n'etiti akwa dị iche iche kwesịrị ibelata ike siri ike nke ukwuu (26). Site na itinye graphene n'ọtụtụ akwa, a kọrọ na graphene bi- ma ọ bụ trilayer a nwere ike ịgbatị ruo 30% nrụgide, na-egosi mgbanwe iguzogide ugboro 13 pere mpe karịa nke monolayer graphene (27). Agbanyeghị, ike ịgbatị a ka dị obere karịa ihe ndị na-eme ka ọ gbatịa nke oge a (28, 29).
Transistors dị mkpa n'ọrụ ndị a na-agbatị agbatị n'ihi na ha na-eme ka a gụọ ihe mmetụta sensọ dị elu na nyocha mgbaàmà (30, 31). Transistors na PDMS nwere graphene dị iche iche dị ka elektrọd isi iyi/mgbapụta mmiri na ihe ọwa nwere ike ịnọgide na-arụ ọrụ eletriki ruo 5% nrụgide (32), nke dị oke ala karịa uru kacha nta achọrọ (~50%) maka ihe mmetụta nlekota ahụike na akpụkpọ ahụ elektrọnik (33, 34). N'oge na-adịbeghị anya, a chọpụtala ụzọ graphene kirigami, enwere ike ịgbatị transistor nke electrolyte mmiri mmiri nwere ike ịgbatị ruo 240% (35). Agbanyeghị, usoro a chọrọ graphene a kwụsịtụrụ, nke na-eme ka usoro mmepụta ahụ sie ike.
N'ebe a, anyị na-enweta ngwaọrụ graphene a na-agbatị nke ukwuu site n'ịkpakọba mpịachi graphene (~1 ruo 20 μm n'ogologo, ~0.1 ruo 1 μm n'obosara, na ~10 ruo 100 nm n'elu) n'etiti akwa graphene. Anyị na-eche na mpịachi graphene ndị a nwere ike inye ụzọ ndị na-eduzi ihe iji mechie mgbawa na mpempe akwụkwọ graphene, si otú a na-enwe ike ijikwa ike dị elu n'okpuru nrụgide. Mpịachi graphene anaghị achọ njikọ ma ọ bụ usoro ọzọ; a na-emepụta ha n'ụzọ ebumpụta ụwa n'oge usoro mbufe mmiri. Site na iji ọtụtụ elektrọd graphene G/G (graphene/graphene) (MGGs) graphene a na-agbatị agbatị (isi iyi/drain na ọnụ ụzọ ámá) na semiconductor CNTs, anyị nwere ike igosi transistors niile-carbon niile a na-apụghị ịgbasa nke ọma ma dị oke mma, nke enwere ike ịgbatị ruo 120% nsogbu (yiri ntụziaka nke ụgbọ njem chaja) ma jigide 60% nke mmepụta ugbu a mbụ ha. Nke a bụ transistor dabere na carbon kachasị agbatị ruo ugbu a, ọ na-enyekwa ọkụ zuru oke iji kwọọ LED na-adịghị mma.
Iji mee ka elektrọd graphene ndị a na-agbatị agbatị buru ibu nwee ike ịgbasa, anyị họọrọ graphene toro na CVD na foil Cu. A kwụgidere foil Cu n'etiti tube CVD quartz iji mee ka graphene too n'akụkụ abụọ ahụ, na-emepụta usoro G/Cu/G. Iji bufee graphene, anyị buru ụzọ kpuchie obere oyi akwa poly(methyl methacrylate) (PMMA) iji chebe otu akụkụ nke graphene, nke anyị kpọrọ graphene n'elu (vice versa maka akụkụ nke ọzọ nke graphene), ma emesịa, a mikpuru ihe nkiri ahụ dum (PMMA/top graphene/Cu/bottom graphene) na ngwọta (NH4)2S2O8 iji wepụ foil Cu. Graphene dị n'akụkụ ala na-enweghị mkpuchi PMMA ga-enwe mgbawa na ntụpọ ndị na-ekwe ka ihe e ji kpụọ banye (36, 37). Dịka egosiri na Fig. 1A, n'okpuru mmetụta nke nrụgide elu, ngalaba graphene ewepụtara awụgharịrị na-atụgharị n'ime mpịakọta ma mesịa jikọta ya na ihe nkiri G/PMMA ndị ọzọ dị n'elu. Enwere ike ibufe mpịakọta G/G dị elu n'elu ihe ọ bụla dị na ya, dịka SiO2/Si, iko, ma ọ bụ polima dị nro. Imegharị usoro mbufe a ọtụtụ ugboro n'otu ihe ahụ na-enye usoro MGG.
(A) Ihe osise eserese nke usoro mmepụta maka MGGs dị ka elektrọd a na-agbatị agbatị. N'oge mbufe graphene, graphene azụ dị na foil Cu gbajiri na ókè na ntụpọ, a kpọkọtara ya n'ụdị na-enweghị usoro, ma jikọta ya nke ọma na fim ndị dị n'elu, na-emepụta nanoscrolls. Katuunu nke anọ na-egosi nhazi MGG a kpọkọtara. (B na C) Ngosipụta TEM dị elu nke MGG monolayer, na-elekwasị anya na graphene monolayer (B) na mpaghara mpịakọta (C), n'otu n'otu. Ntinye nke (B) bụ onyonyo dị ala na-egosi ọdịdị zuru oke nke MGG monolayer na grid TEM. Ntinye nke (C) bụ profaịlụ ike e sere n'akụkụ igbe akụkụ anọ egosiri na onyonyo a, ebe anya dị n'etiti oghere atọm bụ 0.34 na 0.41 nm. (D) EEL spectrum Carbon K-edge nwere akara graphitic π* na σ* nke e ji mara ya. (E) Foto AFM nke akụkụ nke mpịakọta G/G monolayer nwere profaịlụ dị elu n'ahịrị ntụpọ odo. (F ruo I) Nlegharị anya na onyonyo AFM nke trilayer G na-enweghị (F na H) yana mpịakọta (G na I) na substrates SiO2/Si 300-nm dị arọ, n'otu n'otu. E tinyere akara mpịakọta na wrinkles ndị a na-anọchite anya iji gosipụta ọdịiche ha.
Iji chọpụta na akwụkwọ mpịakọta ndị ahụ bụ graphene a kpụgharịrị n'okike, anyị mere nnyocha spectroscopy elektrọn transmission high-resolution (TEM) na electron energy loss (EEL) na nhazi monolayer top-G/G scroll. Foto 1B na-egosi nhazi hexagonal nke graphene monolayer, ihe dị n'ime ya bụ ọdịdị zuru oke nke ihe nkiri ahụ kpuchiri n'otu oghere carbon nke TEM grid. Graphene monolayer na-agbasa ọtụtụ grid ahụ, ụfọdụ flakes graphene na-apụtakwa n'ihu ọtụtụ stacks nke mgbaaka hexagonal (Fig. 1B). Site na ibugharị n'ime mpịakọta nke ọ bụla (Fig. 1C), anyị hụrụ nnukwu ọnụ ọgụgụ nke graphene lattice, yana oghere lattice dị n'etiti 0.34 ruo 0.41 nm. Nha ndị a na-egosi na a na-apịachi flakes na-enweghị usoro ma ha abụghị graphite zuru oke, nke nwere oghere lattice nke 0.34 nm na nhazi oyi akwa "ABAB". Foto 1D na-egosi spectrum carbon K-edge EEL, ebe elu dị na 285 eV sitere na orbital π* na nke ọzọ dị ihe dị ka 290 eV bụ n'ihi mgbanwe nke orbital σ*. A pụrụ ịhụ na njikọ sp2 na-achịkwa n'usoro a, na-egosi na akwụkwọ mpịakọta ndị ahụ nwere eserese dị elu.
Foto igwe onyonyo anya na ike atọm (AFM) na-enye nghọta gbasara nkesa nke nanoscrolls graphene na MGGs (Foto 1, E ruo G, na fig. S1 na S2). A na-ekesa akwụkwọ mpịakọta ndị ahụ n'elu elu ahụ n'enweghị usoro, njupụta ha n'ime-plane na-abawanye nha nhata na ọnụọgụ nke akwa ndị a kpọkọtara ọnụ. Ọtụtụ akwụkwọ mpịakọta na-ejikọta ọnụ n'ime eriri ma na-egosipụta elu na-abụghị otu n'etiti 10 ruo 100 nm. Ha dị 1 ruo 20 μm n'ogologo na 0.1 ruo 1 μm n'obosara, dabere na nha nke flakes graphene mbụ ha. Dịka egosiri na Fig. 1 (H na I), akwụkwọ mpịakọta ndị ahụ nwere nnukwu nha karịa wrinkles, na-eduga na njikọ siri ike n'etiti akwa graphene.
Iji tụọ njirimara eletriki, anyị mere ihe nkiri graphene nwere ma ọ bụ na-enweghị nhazi mpịakọta ma tinye akwa n'ime mpempe akwụkwọ 300-μm n'obosara na 2000-μm n'ogologo site na iji fotolithography. A tụrụ mgbochi nyocha abụọ dịka ọrụ nke nrụgide n'okpuru ọnọdụ gburugburu. Ọnụnọ nke mpịakọta belatara iguzogide maka graphene monolayer site na 80% yana naanị mbelata 2.2% na nnyefe (fig. S4). Nke a na-akwado na nanoscrolls, nke nwere njupụta ugbu a dị elu ruo 5 × 107 A/cm2 (38, 39), na-enye aka eletrik dị mma na MGGs. N'ime mono-, bi-, na trilayer plain graphene na MGGs niile, trilayer MGG nwere njikwa kachasị mma yana nghọta nke ihe fọrọ nke nta ka ọ bụrụ 90%. Iji tụnyere isi mmalite ndị ọzọ nke graphene akọpụtara n'akwụkwọ ndị a, anyị tụkwara iguzogide mpempe akwụkwọ anọ (fig. S5) ma depụta ha dị ka ọrụ nke nnyefe na 550 nm (fig. S6) na Fig. 2A. MGG na-egosi conductivity na nghọta dị elu karịa multila yer plain graphene na reduced graphene oxide (RGO) (6, 8, 18). Rịba ama na mgbochi mpempe akwụkwọ nke multilayer plain graphene nke e ji aka rụọ site na akwụkwọ dị elu karịa nke MGG anyị, ikekwe n'ihi ọnọdụ uto ha na-adịghị mma na ụzọ mbufe ha.
(A) Nguzogide mpempe akwụkwọ nyocha anọ megide nnyefe na 550 nm maka ọtụtụ ụdị graphene, ebe square ojii na-egosi mono-, bi-, na trilayer MGG; okirikiri uhie na triangle anụnụ anụnụ kwekọrọ na multilayer plain graphene a kụrụ na Cu na Ni site na ọmụmụ nke Li et al. (6) na Kim et al. (8), n'otu n'otu, wee bufee na SiO2/Si ma ọ bụ quartz; triangle akwụkwọ ndụ akwụkwọ ndụ bụ uru maka RGO na ogo mbelata dị iche iche site na ọmụmụ nke Bonaccorso et al. (18). (B na C) Mgbanwe nguzogide nkịtị nke mono-, bi- na trilayer MGGs na G dịka ọrụ nke perpendicular (B) na parallel (C) nrụgide na ntụziaka nke mmiri ugbu a. (D) Mgbanwe nguzogide nkịtị nke bilayer G (uhie) na MGG (ojii) n'okpuru usoro cyclic na-ebu ruo 50% usoro perpendicular. (E) Mgbanwe nguzogide nkịtị nke trilayer G (uhie) na MGG (ojii) n'okpuru usoro cyclic na-ebu ruo 90% usoro parallel. (F) Mgbanwe ikike nke mono-, bi- na trilayer G na bi- na trilayer MGG dị ka ọrụ n nke nsogbu. Ihe dị n'ime ya bụ nhazi capacitor, ebe ihe polymer substrate bụ SEBS na polymer dielectric oyi akwa bụ SEBS 2-μm-thick.
Iji nyochaa arụmọrụ dabere na nrụgide nke MGG, anyị bufere graphene na ihe ndị dị n'okpuru thermoplastic elastomer styrene-ethylene-butadiene-styrene (SEBS) (~ 2 cm n'obosara na ~ 5 cm n'ogologo), a tụkwara conductivity ka a na-agbatị substrate ahụ (lee Ihe na Usoro) ma n'akụkụ na n'akụkụ ntụziaka nke mmiri ugbu a (Foto 2, B na C). Omume eletriki dabere na nrụgide ka mma site na itinye nanoscrolls na mmụba nke akwa graphene. Dịka ọmụmaatụ, mgbe nrụgide ahụ dị n'akụkụ na mmiri ugbu a, maka graphene monolayer, mgbakwunye nke mpịakọta mụbara nrụgide ahụ na mgbawa eletriki site na 5 ruo 70%. Ndozi nrụgide nke graphene trilayer na-akawanye mma nke ukwuu ma e jiri ya tụnyere graphene monolayer. Site na nanoscrolls, na 100% perpendicular strain, nguzogide nke nhazi MGG trilayer mụbara naanị site na 50%, ma e jiri ya tụnyere 300% maka graphene trilayer na-enweghị mpịakọta. A nyochachara mgbanwe nguzogide n'okpuru ibu nrụgide cyclic. Maka ntụnyere (Foto 2D), nguzogide nke ihe nkiri graphene dị larịị mụbara ihe dị ka ugboro 7.5 mgbe okirikiri ~700 gasịrị na nrụgide perpendicular 50% ma nọgide na-amụba ka nrụgide na okirikiri ọ bụla. N'aka nke ọzọ, nguzogide nke MGG bilayer mụbara naanị ihe dị ka ugboro 2.5 mgbe okirikiri ~700 gasịrị. Site na iji nrụgide ruo 90% n'akụkụ ntụziaka ahụ, nguzogide nke graphene trilayer mụbara ~ ugboro 100 mgbe okirikiri 1000 gasịrị, ebe ọ bụ naanị ~ ugboro 8 na MGG trilayer (Foto 2E). A na-egosi nsonaazụ ịgba ígwè na fig. S7. Mmụba ngwa ngwa na nguzogide n'akụkụ ntụziaka nke mgbawa dị n'akụkụ ntụziaka nke mmiri ugbu a bụ n'ihi na nguzozi nke mgbawa dị n'akụkụ ntụziaka nke mmiri ugbu a. Ngbanwe nke nguzogide n'oge ibu na mbupu nje bụ n'ihi mgbake viscoelastic nke SEBS elastomer substrate. Nguzogide siri ike nke mpempe MGG n'oge ịgba ígwè bụ n'ihi ọnụnọ nke nnukwu mpịakọta nwere ike ijikọ akụkụ ndị gbawara agbawa nke graphene (dịka AFM si hụ), na-enyere aka ịnọgide na-enwe ụzọ na-agbagharị agbagharị. Akọpụtala ihe a nke ịnọgide na-enwe ike site na ụzọ na-agbagharị agbagharị maka ihe nkiri metal ma ọ bụ semiconductor gbawara agbawa na ihe ndị e ji elastomer mee (40, 41).
Iji nyochaa ihe nkiri ndị a dabere na graphene dị ka elektrọd ọnụ ụzọ ámá na ngwaọrụ ndị a na-agbatị agbatị, anyị ji oyi akwa SEBS dielectric (2 μm dị ọkpụrụkpụ) kpuchie oyi akwa graphene ma lelee mgbanwe ike dielectric dị ka ọrụ nke nrụgide (lee Fig. 2F na Ihe Mgbakwunye maka nkọwa zuru ezu). Anyị hụrụ na ike nwere monolayer nkịtị na bilayer graphene electrodes belatara ngwa ngwa n'ihi mfu nke in-plane conductivity nke graphene. N'ụzọ dị iche, capacitances nke MGGs tinyere graphene trilayer dị larịị gosiri mmụba nke capacitance na nrụgide, nke a na-atụ anya ya n'ihi mbelata na ọkpụrụkpụ dielectric na nrụgide. Mmụba a tụrụ anya ya na capacitance dabara nke ọma na nhazi MGG (fig. S8). Nke a na-egosi na MGG dabara adaba dị ka elektrọd ọnụ ụzọ ámá maka transistors a na-agbatị agbatị.
Iji nyochaa ọrụ nke 1D graphene scroll na-arụ na nnabata nrụgide nke ike eletriki na ijikwa nkewa dị n'etiti oyi akwa graphene nke ọma, anyị jiri CNTs a kpuchiri agba iji dochie mpịakọta graphene (lee Ihe Ndị Ọzọ). Iji mee ka usoro MGG dị iche iche, anyị tinyere njupụta atọ nke CNTs (ya bụ, CNT1).
(A ruo C) Foto AFM nke njupụta atọ dị iche iche nke CNTs (CNT1)
Iji ghọtakwuo ikike ha dị ka elektrọd maka elektrọnịkị a na-agbatị agbatị, anyị nyochachara usoro nhazi nke MGG na G-CNT-G n'okpuru nrụgide. Microscopy anya na nyocha elektrọn microscopy (SEM) abụghị ụzọ njirimara dị irè n'ihi na ha abụọ enweghị ọdịiche agba na SEM nwere ike ịnwe ihe oyiyi n'oge nyocha elektrọn mgbe graphene dị na ihe ndị polymer (figs. S9 na S10). Iji hụ na ebe graphene dị n'okpuru nrụgide, anyị chịkọtara nha AFM na MGGs trilayer na graphene nkịtị mgbe anyị tụgharịrị na ihe ndị dị gịrịgịrị (~0.1 mm ọkpụrụkpụ) na ihe ndị na-agbanwe agbanwe SEBS. N'ihi ntụpọ dị n'ime CVD graphene na mmebi mpụga n'oge usoro mbufe, a na-emepụta mgbawa na graphene a gbanyere mkpọrọgwụ, na ka nrụgide na-arị elu, mgbawa ahụ ghọrọ nke buru ibu karị (Fig. 4, A ruo D). Dabere na nhazi nke elektrọd ndị dabere na carbon, mgbawa ndị ahụ na-egosipụta ọdịdị dị iche iche (fig. S11) (27). Njupụta mpaghara mgbawa (a kọwara dị ka mpaghara mgbawa/mpaghara nyochachara) nke graphene multilayer dị obere karịa nke graphene monolayer mgbe nrụgide gasịrị, nke kwekọrọ na mmụba nke ike eletriki maka MGGs. N'aka nke ọzọ, a na-ahụkarị mpịakọta iji mechie mgbawa ndị ahụ, na-enye ụzọ ndị ọzọ na-eduzi na fim ahụ a gbanyere mkpọrọgwụ. Dịka ọmụmaatụ, dịka e dere na foto nke Fig. 4B, mpịakọta sara mbara gafere mgbawa na MGG trilayer, mana ahụghị mpịakọta ọ bụla na graphene nkịtị (Fig. 4, E ruo H). N'otu aka ahụ, CNTs jikọtara mgbawa ndị ahụ na graphene (fig. S11). A chịkọtara njupụta mpaghara mgbawa, njupụta mpaghara mpịakọta, na ịdị njọ nke ihe nkiri ndị ahụ na Fig. 4K.
(A ruo H) Foto AFM dị n'ime ya nke mpịakọta G/G atọ (A ruo D) na nhazi G atọ (E ruo H) na elastomer SEBS dị gịrịgịrị (~0.1 mm ọkpụrụkpụ) na ụdị 0, 20, 60, na 100%. A na-eji akụ tụọ mgbawa na mpịakọta ndị na-anọchite anya ya. Foto AFM niile dị n'ebe dị 15 μm × 15 μm, na-eji otu ogwe nha agba ahụ dị ka akara. (I) Geometry nlereanya nke elektrọd graphene monolayer a haziri ahazi na substrate SEBS. (J) Maapụ nhazi eserese nke ụdị logarithmic kachasị elu na graphene monolayer na substrate SEBS na ụdị 20% mpụga. (K) Ntụnyere nke njupụta mpaghara mgbawa (kọlụm uhie), njupụta mpaghara mpịakọta (kọlụm odo), na oke elu (kọlụm anụnụ anụnụ) maka ụdị graphene dị iche iche.
Mgbe a gbatịpụrụ ihe nkiri MGG, e nwere usoro ọzọ dị mkpa nke mpịachi akwụkwọ mpịakọta ndị ahụ nwere ike ijikọ mpaghara graphene gbawara agbawa, na-eme ka netwọk na-agbagharị agbagharị. Mpịachi akwụkwọ mpịakọta graphene na-ekwe nkwa n'ihi na ha nwere ike ịdị ọtụtụ iri micrometer n'ogologo ma nwee ike ijikọ mgbawa ndị na-adịkarị ruo nha micrometer. Ọzọkwa, n'ihi na mpịachi akwụkwọ mpịakọta ndị ahụ nwere ọtụtụ oyi akwa nke graphene, a na-atụ anya na ha ga-enwe obere iguzogide. Ma e jiri ya tụnyere ya, a chọrọ netwọk CNT dị oke arọ (nke na-adịghị agafe agafe) iji nye ikike njikọ ihe owuwu yiri ya, ebe CNT dị obere (nke na-abụkarị obere micrometer n'ogologo) ma pere mpe karịa mpịachi akwụkwọ mpịakọta. N'aka nke ọzọ, dịka egosiri na fig. S12, ebe mpịachi akwụkwọ mpịakọta ndị ahụ na-agbawa mgbe a na-agbatị iji nabata nrụgide, mpịachi akwụkwọ mpịakọta ndị ahụ anaghị agbawa, nke na-egosi na nke ikpeazụ nwere ike ịmịgharị na graphene dị n'okpuru. Ihe kpatara na ha anaghị agbawa agbawa nwere ike ịbụ n'ihi nhazi a kpọkọtara akpọchi, nke nwere ọtụtụ oyi akwa graphene (~1 ruo 2 0 μm n'ogologo, ~0.1 ruo 1 μm n'obosara, na ~10 ruo 100 nm n'ịdị elu), nke nwere modulus dị irè karịa graphene otu oyi akwa. Dịka Green na Hersam (42) si kọọ, netwọk CNT metallic (dayameta tube nke 1.0 nm) nwere ike iru obere iguzogide mpempe akwụkwọ <100 ohms/sq n'agbanyeghị nnukwu nguzogide njikọ dị n'etiti CNTs. Ebe ọ bụ na mpịachi graphene anyị nwere obosara nke 0.1 ruo 1 μm nakwa na mpịachi G/G nwere nnukwu mpaghara kọntaktị karịa CNTs, nguzogide kọntaktị na mpaghara kọntaktị n'etiti mpịachi graphene na graphene ekwesịghị ịbụ ihe ndị na-egbochi njikwa dị elu.
Graphene nwere modulus dị elu karịa nke SEBS substrate. Ọ bụ ezie na ọkpụrụkpụ dị irè nke electrode graphene dị ala karịa nke substrate, ike nke graphene ugboro ọkpụrụkpụ ya yiri nke substrate (43, 44), na-ebute mmetụta siri ike-àgwàetiti dị mma. Anyị mere ka ọ dị ka mgbanwe nke graphene dị 1-nm na substrate SEBS (lee Ihe Ndị Ọzọ maka nkọwa zuru ezu). Dịka nsonaazụ ihe atụ si dị, mgbe etinyere 20% nje na substrate SEBS n'èzí, nkezi nje na graphene bụ ~6.6% (Fig. 4J na fig. S13D), nke kwekọrọ na ihe nlele nnwale (lee fig. S13). Anyị tụnyere nje na mpaghara graphene na substrate a haziri ahazi site na iji microscopy anya wee chọpụta na nje ahụ dị na mpaghara substrate bụ opekata mpe okpukpu abụọ nke nje ahụ na mpaghara graphene. Nke a na-egosi na nje ahụ etinyere na ụkpụrụ electrode graphene nwere ike ịkpachi nke ukwuu, na-emepụta agwaetiti siri ike graphene n'elu SEBS (26, 43, 44).
Ya mere, o yikarịrị ka usoro abụọ dị mkpa ga-enyere aka mee ka elektrọd MGG nwee ike ịnọgide na-enwe ike ịrụ ọrụ nke ọma n'okpuru nrụgide dị elu: (i) Mpịakọta ndị ahụ nwere ike ijikọ mpaghara ndị a na-anaghị ejikọta iji nọgide na-enwe ụzọ percolation conductive, na (ii) mpempe akwụkwọ graphene/elastomer nwere ọtụtụ oyi akwa nwere ike ịmịgharị n'elu ibe ha, na-ebute mbelata nrụgide na elektrọd graphene. Maka ọtụtụ oyi akwa nke graphene ebufere na elastomer, oyi akwa ahụ anaghị ejikọta nke ọma na ibe ha, nke nwere ike ịmịgharị na nzaghachi maka nrụgide (27). Mpịakọta ndị ahụ mekwara ka ike nke oyi akwa graphene dịkwuo elu, nke nwere ike inye aka mee ka nkewa dị n'etiti oyi akwa graphene dịkwuo elu ma si otú a mee ka oyi akwa graphene na-amịgharị.
A na-achụso ngwaọrụ carbon niile n'ọchịchọ n'ihi ọnụ ahịa dị ala na nnukwu mmepụta. N'ọnọdụ anyị, e ji ọnụ ụzọ graphene dị n'okpuru, njikọ isi iyi/mgbapụta graphene dị n'elu, semiconductor CNT a haziri ahazi, na SEBS dị ka dielectric (Foto 5A). Dịka egosiri na Fig. 5B, ngwaọrụ carbon niile nwere CNT dị ka isi iyi/mgbapụta na ọnụ ụzọ ámá (ngwaọrụ ala) na-adịghị ahụkebe karịa ngwaọrụ nwere electrodes graphene (ngwaọrụ dị n'elu). Nke a bụ n'ihi na netwọk CNT chọrọ ọkpụrụkpụ buru ibu na, n'ihi ya, obere nnyefe anya iji nweta mgbochi mpempe akwụkwọ yiri nke graphene (foto S4). Foto 5 (C na D) na-egosi nguzozi mbufe na mmepụta tupu nrụgide maka transistor ejiri electrodes MGG bilayer mee. Obosara ọwa na ogologo nke transistor na-enweghị nsogbu bụ 800 na 100 μm, n'otu n'otu. Oke mgbanyụ/mgbanyụ a tụrụ karịrị 103 yana ọkụ ọkụ na-agba na ọkwa nke 10−5 na 10−8 A, n'otu n'otu. Usoro mmepụta ahụ na-egosipụta usoro nhazi kwụ ọtọ na saturation zuru oke yana ndabere doro anya nke ọnụ ụzọ ámá-voltaji, na-egosi njikọ zuru oke n'etiti CNT na electrodes graphene (45). A hụrụ na iguzogide kọntaktị na electrodes graphene dị ala karịa nke ihe nkiri Au a gbapụrụ agbapụ (lee fig. S14). Njem saturation nke transistor a na-agbatị dị ihe dị ka 5.6 cm2/Vs, yiri nke transistors CNT nke otu polymer na substrates Si siri ike nwere 300-nm SiO2 dị ka oyi akwa dielectric. Enwere ike imeziwanye mmegharị ahụ site na njupụta tube kachasị mma na ụdị tube ndị ọzọ (46).
(A) Atụmatụ nke transistor agbatị dabere na graphene. SWNTs, nanotubes carbon nwere otu mgbidi. (B) Foto nke transistor agbatị ejiri electrodes graphene (elu) na CNT electrodes mee (ala). Ọdịiche dị na nghọta doro anya. (C na D) Usoro mbufe na mmepụta nke transistor dabere na graphene na SEBS tupu nrụgide. (E na F) Usoro mbufe, oge ọkụ na gbanyụọ, oke ọkụ na gbanyụọ, na mmegharị nke transistor dabere na graphene na ụdị dị iche iche.
Mgbe e tinyere ngwaọrụ transistor, nke nwere carbon niile n'akụkụ ụzọ ahụ dịka ntụziaka njem chajị si dị, a hụrụ obere mmebi ruo 120%. N'oge ịgbatị ahụ, ngagharị ahụ na-ebelata site na 5.6 cm2/V na nrụgide 0% ruo 2.5 cm2/V na nrụgide 120% (Foto 5F). Anyị tụnyerekwara arụmọrụ transistor maka ogologo ọwa dị iche iche (lee tebụl S1). N'ụzọ dị mkpa, na nrụgide buru ibu dịka 105%, transistor ndị a niile ka gosipụtara oke ngbanye/gbanyụọ dị elu (>103) na ngagharị (>3 cm2/Vs). Na mgbakwunye, anyị chịkọtara ọrụ niile emere n'oge na-adịbeghị anya na transistor carbon niile (lee tebụl S2) (47–52). Site na imeziwanye mmepụta ngwaọrụ na elastomers na iji MGGs dị ka kọntaktị, transistor carbon anyị niile na-egosi arụmọrụ dị mma n'ihe gbasara ngagharị na hysteresis yana ịbụ nke a na-agbatị nke ukwuu.
Dịka ojiji nke transistor doro anya ma gbasaa nke ọma, anyị jiri ya chịkwaa mgbanwe LED (Foto 6A). Dịka egosiri na Fig. 6B, enwere ike ịhụ LED akwụkwọ ndụ akwụkwọ ndụ nke ọma site na ngwaọrụ carbon niile a na-agbatị agbatị nke etinyere kpọmkwem n'elu. Ọ bụ ezie na ọ na-agbatị ruo ~100% (Foto 6, C na D), ike ọkụ LED anaghị agbanwe, nke kwekọrọ na arụmọrụ transistor akọwara n'elu (lee ihe nkiri S1). Nke a bụ akụkọ mbụ nke nkeji njikwa a na-agbatị agbatị nke ejiri electrodes graphene mee, na-egosi ohere ọhụrụ maka eletrọniki a na-agbatị graphene.
(A) Okirikiri nke transistor iji kwọọ LED. GND, ala. (B) Foto nke transistor carbon niile a na-agbatị agbatị na nke na-apụta ìhè na 0% nke etinyere n'elu LED akwụkwọ ndụ akwụkwọ ndụ. (C) A na-etinye transistor transistor niile-carbon na nke a na-agbatị agbatị nke ejiri gbanwee LED n'elu LED na 0% (aka ekpe) na ~100% nke nrụgide (n'aka nri). Akụ ọcha na-atụ aka dị ka ihe nrịbama odo odo na ngwaọrụ ahụ iji gosi mgbanwe anya a na-agbatị. (D) Echiche akụkụ nke transistor agbatị, ebe a na-akwanye LED n'ime elastomer.
Na mmechi, anyị emepụtala nhazi graphene doro anya nke na-ejigide ike eletriki dị elu n'okpuru nnukwu nsogbu dịka elektrọd ndị a na-agbatị agbatị, nke graphene nanoscrolls na-eme ka ọ dị n'etiti akwa graphene a kpọkọtara ọnụ. Nhazi elektrọd MGG abụọ na nke atọ a na elastomer nwere ike ịnọgide na-enwe 21 na 65%, n'otu n'otu, nke 0% nke ike eletriki ha na nrụgide dị elu ruo 100%, ma e jiri ya tụnyere mfu zuru oke nke ike eletriki na nrụgide 5% maka elektrọd graphene monolayer nkịtị. Ụzọ ndị ọzọ na-eduzi nke graphene mpịachi yana mmekọrịta adịghị ike n'etiti akwa ndị a na-ebufe na-enye aka na nkwụsi ike ike ikuku ikuku dị elu n'okpuru nrụgide. Anyị tinyekwara usoro graphene a iji mepụta transistors niile a na-agbatị carbon. Ruo ugbu a, nke a bụ transistor dabere na graphene kachasị agbatị nwere nghọta kacha mma na-ejighị buckling. Ọ bụ ezie na emere ọmụmụ ihe a iji mee ka graphene nwee ike ịgbatị elektrọnịkị, anyị kwenyere na enwere ike ịgbatị usoro a gaa na ihe 2D ndị ọzọ iji mee ka elektrọnịkị 2D a na-agbatị agbatị.
A kụrụ graphene CVD nke nwere nnukwu mpaghara na mpempe akwụkwọ Cu a kwụnyere (99.999%; Alfa Aesar) n'okpuru nrụgide na-adịgide adịgide nke 0.5 mtorr na 50–SCCM (sentimita cubic nkịtị kwa nkeji) CH4 na 20–SCCM H2 dị ka ihe ndị na-ebute ụzọ na 1000°C. E ji graphene monolayer kpuchie akụkụ abụọ nke mpempe akwụkwọ Cu ahụ. E ji obere oyi akwa nke PMMA (2000 rpm; A4, Microchem) kpuchie ya n'otu akụkụ nke mpempe akwụkwọ Cu ahụ, wee mepụta usoro PMMA/G/Cu foil/G. Emesịa, e tinyere ihe nkiri ahụ dum na mmiri ammonium persulfate [(NH4)2S2O8] nke 0.1 M ruo ihe dị ka awa abụọ iji wepụ mpempe akwụkwọ Cu ahụ. N'oge usoro a, graphene azụ na-enweghị nchebe buru ụzọ dọwaa ókè ọka wee tụgharịa ya ka ọ bụrụ mpịakọta n'ihi nrụgide elu. E tinyere mpempe akwụkwọ ndị ahụ na fim graphene elu nke PMMA kwadoro, na-emepụta mpịakọta PMMA/G/G. E mesịa, a sachara ihe nkiri ndị ahụ na mmiri e tinyere n'ime ion ọtụtụ ugboro ma tinye ha n'elu ihe e ji achọ ya mma, dịka SiO2/Si siri ike ma ọ bụ ihe e ji plastik mee. Ozugbo ihe nkiri ahụ kpọrọ nkụ n'elu ihe ahụ, a na-etinye ihe nlele ahụ n'ime acetone, 1:1 acetone/IPA (isopropyl alcohol), na IPA n'ime sekọnd iri atọ iji wepụ PMMA. A na-ekpo ọkụ ihe nkiri ndị ahụ na 100°C ruo nkeji iri na ise ma ọ bụ debe ha n'ime oghere ikuku ruo abalị iji wepụ mmiri ahụ kpamkpam tupu e bufee ihe mkpuchi G/G ọzọ na ya. Nzọụkwụ a bụ izere ikewapụ ihe nkiri graphene na ihe ahụ ma hụ na MGG zuru oke n'oge ntọhapụ nke ihe mkpuchi PMMA.
A hụrụ ọdịdị nke nhazi MGG site na iji igwe onyonyo anya (Leica) na igwe onyonyo elektrọn nyocha (1 kV; FEI). E jiri igwe onyonyo ike atọm (Nanoscope III, Digital Instrument) rụọ ọrụ na ọnọdụ ịpị iji hụ nkọwa nke akwụkwọ mpịakọta G. E jiri igwe onyonyo a na-ahụ anya nke ultraviolet (Agilent Cary 6000i) nwalee nghọta ihe nkiri ahụ. Maka ule ndị ahụ mgbe nrụgide ahụ dị n'akụkụ ntụaka nke mmiri ugbu a, ejiri fotolithography na plasma O2 mee ihe iji tụọ nhazi graphene n'ime mpempe akwụkwọ (~ 300 μm n'obosara na ~ 2000 μm n'ogologo), e jikwa ihe mkpuchi onyinyo na nsọtụ abụọ nke akụkụ ogologo ahụ tinye elektrọd Au (50 nm) n'ọkụ. E tinyere mpempe akwụkwọ graphene ahụ na SEBS elastomer (ihe dị ka sentimita 2 n'obosara na sentimita 5 n'ogologo), ya na ogologo axis nke mpempe akwụkwọ ndị ahụ dị ka akụkụ dị mkpụmkpụ nke SEBS, wee soro ya na BOE (ihe e ji oxide etch buffered) (HF:H2O 1:6) na eutectic gallium indium (EGaIn) dị ka kọntaktị eletriki. Maka ule nrụgide ndị yiri ya, e bufere nhazi graphene na-enweghị ụkpụrụ (~5 × 10 mm) na ihe ndị dị na SEBS, ya na ogologo axes dị ka akụkụ ogologo nke ihe ndị dị na SEBS. Maka ikpe abụọ ahụ, a na-agbatị G dum (na-enweghị G scrolls)/SEBS n'akụkụ ogologo nke elastomer na ngwa aka, na ebe a, anyị tụrụ mgbanwe iguzogide ha n'okpuru nrụgide na ọdụ nyocha na ihe nyocha semiconductor (Keithley 4200-SCS).
E jiri usoro ndị a mepụta transistors niile nwere ike ịgbatị ma doo anya na ihe na-agbanwe agbanwe na ihe na-agbanwe agbanwe iji zere mmebi ihe mgbaze organic nke polima dielectric na ihe na-agbanwe agbanwe. E zigara usoro MGG na SEBS dị ka elektrọd ọnụ ụzọ ámá. Iji nweta oyi akwa dielectric polymer dị gịrịgịrị (2 μm ọkpụrụkpụ), e ji ihe ngwọta SEBS toluene (80 mg/ml) kpuchie ya na octadecyltrichlorosilane (OTS) nke agbanwere agbanwe (OTS) na 1000 rpm maka nkeji 1. Enwere ike ibufe ihe nkiri dielectric dị gịrịgịrị site na elu OTS hydrophobic gaa na ihe na-ekpuchi SEBS nke e ji graphene dị njikere kpuchie. Enwere ike ime capacitor site na itinye electrode elu mmiri-metal (EGaIn; Sigma-Aldrich) iji chọpụta capacitance dị ka ọrụ nke nrụgide site na iji mita LCR (inductance, capacitance, resistance) (Agilent). Akụkụ nke ọzọ nke transistor ahụ nwere CNTs semiconducting polymer-assored, na-agbaso usoro ndị akọwara na mbụ (53). E ji ihe siri ike SiO2/Si mepụta elektrọd ndị a na-akpọ isi iyi/drain elektrọd. E mesịa, e tinyere akụkụ abụọ ahụ, dielectric/G/SEBS na CNT/a na-akpọ G/SiO2/Si, n'otu ebe, ma tinye ha na BOE iji wepụ ihe siri ike SiO2/Si. N'ihi ya, e mepụtara transistors ndị ahụ na-enwu enwu ma na-agbatị agbatị. E mere nnwale eletriki n'okpuru nrụgide ahụ na ntọala ịgbatị aka dịka usoro e kwuru n'elu.
E nwere ike ịchọta ihe ndị ọzọ gbasara akụkọ a na http://advances.sciencemag.org/cgi/content/full/3/9/e1700159/DC1.
fig. S1. Foto igwe onyonyo anya nke monolayer MGG na ihe ndị dị na SiO2/Si na mmụba dị iche iche.
fig. S4. Ntụnyere nke mgbochi mpempe akwụkwọ nyocha abụọ na nnyefe @550 nm nke graphene dị larịị mono-, bi- na trilayer (squares ojii), MGG (okirikiri uhie), na CNTs (triangle anụnụ anụnụ).
fig. S7. Mgbanwe nguzogide nkịtị nke mono- na bilayer MGGs (ojii) na G (uhie) n'okpuru ~1000 cyclic strains na-ebu ibu ruo 40 na 90% parallel strains, n'otu n'otu.
fig. S10. Foto SEM nke trilayer MGG na SEBS elastomer mgbe nrụgide gasịrị, na-egosi ogologo mpịakọta gafere ọtụtụ mgbawa.
fig. S12. Foto AFM nke trilayer MGG na SEBS elastomer dị gịrịgịrị na ụdị 20%, na-egosi na mpịachi gafere mgbawa.
Tebụl S1. Njem nke transistors carbon nanotube MGG nke nwere otu mgbidi na 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
© 2021 American Association for the Advancement of Science. Ikike niile echekwabara. AAAS bụ onye mmekọ nke HINARI, AGORA, OARE, CHORUS, CLOCKSS, CrossRef na COUNTER. Ọganihu sayensị ISSN 2375-2548.
Oge ozi: Jenụwarị-28-2021