Alignment of linear polymeric grains for highly stable N-type thin-film transistors

•Fast deposition of polymer thin films with aligned grains and molecules•The polyacrylonitrile can tune the size pre-aggregates in solution•Microscopic structures polymers affected thermal stability transistors•The electron mobilities transistors were >3.5 cm2V–1s–1 from 200 to 460 K For polymeric thin-film transistors, ordered arrangements backbones, flat face-on crystallites, long linear simultaneously improve carrier transport efficiency. These strategies reduce pinholes, grain boundaries, barriers charge paths. The have smaller extent microscopic structural disorders, fewer localized states, lower energies, thereby improving devices. Temperature-insensitive property is very important for transistors. Based on films, we prepared great stability. based top-gate more than 3.5 at temperatures between K. properties are attractive most electronics, including semiconducting Especially, field-effect (FETs) high mobility been research targets due their broad applications. However, FETs stable operating extremely cold or hot zones faced enormous challenges. In this study, was found significantly sizes solutions crystallinity films. orientation 5–25 μm through bar-coating process as an additive, which stabilized over a wide range temperatures. linear-grain morphology film contributed reducing holes boundaries paths carriers. Typically, P(NDI2OD-T2) displayed transporting behavior K, greater cm2V−1s−1. performance electronic equipment be many extreme environments, such South Pole minimum temperature 191–290 K1Ruhl J.E. Ade P.A.R. Carlstrom Cho H.M. Crawford T. Dobbs M. Greer C.H. Halverson N.W. Holzapfel W.L. Lanting T.M. et al.The south pole telescope.Proc. SPIE. 2004; 5498: 11-29Crossref Scopus (241) Google Scholar Lut desert maximum 253–344 K.2Mildrexler D.J. Zhao M.S. Running S.W. Satellite finds highest land skin earth.Am. Meteorol. 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Facchetti Caironi Macroscopic high-throughput printing nanostructured MHz large-area 8394Crossref (237) work, PAN added poly{[N,N9-bis(2-octyldodecyl)-naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,59-(2,29-bithiophene)} (P(NDI2OD-T2)) solution highly approach (Figure 1). We remarkably increased solution, increasing solid molecules. Furthermore, arrangement backbones stacking direction. backbone defects carriers,11Wang Scholar,27Bucella 28Noriega Rivnay Vandewal Koch F.P.V. Smith general relationship disorder, polymers.Nat. 12: 1038-1044Crossref (1436) 29Diao Shaw Morphology solution-processed films.Energy Environ. 2145-2159Crossref 30Xu X.M. Shan D.Q. Xu J.B. Miao Q. Electron exceeding cm2V−1s−1 band-like n-channel 5276-5283Crossref (149) resulted 1A). Notably, limited grains, so anisotropic film. same time, vapor-deposited parylene-C used layer. Top-gate constructed, above attained 200–460 Figures 1B 1C molecules P(NDI2OD-T2)/PAN calculated Grazing-incidence wide-angle X-ray scattering (GIWAXS) data, respectively. Figure S1 photo actual equipment. tapping mode atomic force microscopy (AFM) images show spin-coated had longer 1F) those 1D). employed 40°C glass substrates air, coating speed 120 mm/s, all bars moved direction indicated blue arrow 1E. After drying, annealed 190°C 30 min under nitrogen atmosphere. observed small closely connected each other 1E), whereas independently 1G). Most 150–350 nm (Figures S2 S3). examination morphologies revealed anisotropic, there few parallel bar movement, perpendicular It noteworthy state linearly limit To verify universality PAN, PCII2T DPPT-TT, improved both sizes. Basically, success rate preparation presence PAN. Root-mean-square (RMS) analysis image height investigate roughness results exhibited RMS surface values 1.10, 0.672, 2.57, 3.92 nm, Additionally, AFM micrographs monolayer 20 PCII2T/PAN DPPT-TT/PAN method, showed contained S4). Since GIWAXS powerful way explain correlation 2D-GIWAXS utilized bar-coated 2A 2 B), 2C), 2D 2E), 2F). light source 2D) 2B 2E) line cuts S5. detailed crystallographic parameters presented Tables S2. diagrams PCII2T, S6–S11, while corresponding listed S3–S6. According 2D-GIWAXS, (010) peaks seen out-of-plane 2), weak in-plane peak appeared (parallel) 2D). result also shows neat adopted π-stacking crystallites arrangements, S12. mainly arrangement, arrangement. intensities (002) signals stronger (001) 2B, 2C, suggesting two adjacent NDI units one molecule tend stack T2 molecule.31Brinkmann Gonthier Bogen Tremel Ludwigs Hufnagel Sommer Segregated versus mixed interchain oriented naphthalene diimidebithiophene copolymers.ACS Nano. 10319-10326Crossref (126) signal intensity quantity obviously better P(NDI2OD-T2), means improved. symmetrical 2A), planes positions, angle 14°–15° substrate, inset 1A. differences directions 2B), phenomenon 2B). Alternatively, divided into 2D–2F). This may fact substrate. Together analysis, undivided poor (Table S3), lamellar lengths 325 Å 270 (perpendicular), 251 141 (perpendicular) Meanwhile, length (181 Å) similar (193 Å), indicating addition formation larger crystallites. indicates prefer π markedly crystallinity, positioned grains. favorable along chances lattice scattering. effects processing methods, related solution.32Zheng Lei Dou Yang C.Y. Meng Ma W. Unraveling supramolecular donor–acceptor charge-transport properties.Adv. 29: 1701072Crossref (78) Scholar,33Li Mangalore D.K. Carpenter Yan H.P. Müllen Blom P.W.M. Pisula al.Integrated circuits monolayer.Nat. 9: 451Crossref (50) UV-vis spectroscopy analyze 3A). test concentration 0.02 mg/mL, 0.004 tetralin solvent. Obvious changes absorption spectra during heating process. From 283 393 absorbance 0–0 718 decreased continuously then disappeared, 0–1 601 gradually appeared. demonstrate strong pre-aggregation low-temperature solution. broken up since chains separate conditions.34Chen J.W. X.C. L.J. Lan L.F. Peng Cao Low band-gap hole towards thick-film solar cells.Adv. 26: 2586-2591Crossref (343) There no obvious change spectrum after transfer P(NDI2OD-T2). ultraviolet photoelectron (UPS) same, confirming P(NDI2OD-T2).12Nikolka comparison, temperature-dependent o-dichlorobenzene S13), S14. further understand effect pre-aggregates, dynamic light-scattering (DLS) technique low solutions, small-angle neutron (SANS) solutions. 3B displays DLS-generated particle where solvents, concentrations 0.01 0.002 respectively, 0.012 mg/mL. diameters particles 67–125 (37–78 nm). tetralin. Correspondingly, containing 127–236 without promoted even dilute SANS 3C 3D. 6 1.2 signal-to-noise ratio, deuterated 1,2-dichlorobenzene-d4 (ODCB-d4) solvent incoherent scattering.35Le Cœur Combet Carrot Busch Teixeira Longeville Conformation poly(ethylene glycol) DiPEGylated hemoglobin specifically probed SANS: PEG vivo efficiency.Langmuir. 8402-8410Crossref power exponent 1.93, 1.82 3D). indicate large rod-like structures.32Zheng Scholar,35Le fitted line,36Chen W.R. Butler P.D. Magid Incorporating intermicellar interactions fitting data cationic wormlike micelles.Langmuir. 2006; 6539-6548Crossref (148) radius 1.6 Kuhn 26 280 lamella density functional theory (DFT), its vale 3.22 nm. experimental rigidity pre-aggregates.37Pedersen Schurtenberger Scattering functions semiflexible excluded volume effects.Macromolecules. 1996; 7602-7612Crossref (474) Long aggregates facilitate Molecular (MD) simulation gain understanding pre-aggregates. MD simulations only reflect accumulation conformation. carried out Gromacs-4.6.7 package Amber field (see Supplemental information details).38Hess Kutzner van der Spoel Lindahl GROMACS algorithms efficient, load-balanced, scalable simulation.J. Theor. Comput. 435-447Crossref (11893) Scholar,39Wang J.M. Wolf R.M. Caldwell Kollman P.A. Case D.A. Development testing amber field.J. 25: 1157-1174Crossref (10866) match mass ratio 5:1 evaporation S15), root-mean-square end-to-end distance (RMSD), gyration, number upon S16), indeed enhance ductility ability illustrate role self-assembly snapshots taken trajectory 3E, 3F, S17. 3E aggregated around acted nucleation center some served bridge cluster 3F). Combined DFT calculations, diameter pre-aggregate (3.2 nm) close (3.22 nm), 3F; is, twining round calculation consistent observation aggregate amount bottom-contact (TGBC) configuration fabricated characterize 4A). gold source-drain electrodes modified cesium carbonate (Cs2CO3), Cs2CO3 substrate 0.27 S18). coating, coating. Parylene-C (200 deposited layer, packaging effect. Aluminum gate electrode. following description, denoted “para” electric electrode drain moved, “perp” other. 36-transistor array counted 4B. Table 1 device tested air (295 K), S19 function time. average 0.23 ± 0.07 cm2V−1s−1; whereas, (μelec,∥) 0.4 cm2V−1s−1, (μelec,⊥) 0.25 0.05 μelec,∥/μelec,⊥= 5–10. Comparatively, 0.45 0.1 4.85 0.3 150–520. morphology. order, μelec,∥, higher μelec,∥ μelec,⊥, anisotropy transport. level layers S20).Table 1OFET saturation regime (Vds = V)Depositionμe (cm2V–1s–1)aData represented mean SD.Von (V)Ion:Ioff (Log10)Vt (V)P(NDI2OD-T2)spin-coat0.23 0.07254–5bar-coat (para)1.6 0.424–55–6bar-coat (perp)0.25 0.05242–3P(NDI2OD-T2)+PANspin-coat0.45 0.1–151–2bar-coat(para)4.85 0.3–0.574–5bar-coat (perp)0.02 0.01–0.540–1The table K).a Data SD. Open new tab K). relationships vacuum evaluated 4C, S21, S22. should emphasized dielectric constant layer temperature, S23. 4D S24), 360 different degrees. As increased, degradation disorder pinholes analyzed generalized Einstein relation (GER) method,40Liu Park W.T. Liang Minari Noh unified semiconductors: importance attenuated delocalization carriers.Mater. Horiz. 608-618Crossref 4D, generally applicable describe various mechanisms, hopping, multiple-trapping releasing, variable etc. Generally, GER completely fits except devices degraded performance. Two characteristics (the states [DOS] width, ΔE, degree parameter, ΔD) figure captions and, general, value ΔE signifies less dispersed distribution Gaussian-like DOS ΔD classic band single crystals). Importantly, transistor smallest (50 meV) largest (0.7), signifying much disorders compared (ΔE 90 meV 0.42). showing former features chain latter Notice that, region (< process, sufficiently eliminated enhanced mobility, but case attributed provided timescale reach minimal disorders. S22), 440 hysteresis voltage 5 V, Although irregular gaps according micrographs. illustrates too static physical cause instability measured 300–460 5.5 0.5 still within S22A), paths, therefore energies keys ensure 160 threshold least 4E). turn-on –0.5 Ioff variation OFET channel current Vgs 0 V) S25. FETs, S23) factor 4F). study controlling multiple making Vapor-deposited provide encapsulation sizes, sum up, successfully method. 3.5–6 5–6