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1.
Single‐walled carbon nanotubes (SWNTs) are a promising material for future nanotechnology. However, their applications are still limited in success because of the co‐existence of metallic SWNTs and semiconducting SWNTs produced samples. Here, electrochemical etching, which shows both diameter and electrical selectivity, is demonstrated to remove SWNTs. With the aid of a back‐gate electric field, selective removal of metallic SWNTs is realized, resulting in high‐performance SWNT field‐effect transistors with pure semiconducting SWNT channels. Moreover, electrochemical etching is realized on a selective area. These findings would be valuable for research and the application of SWNTs in electrochemistry and in electronic devices.  相似文献   

2.
By using intense terahertz(THz) monocycle pulses, nonlinear light-matter interaction in aligned semiconducting single-walled carbon nanotubes(SWNTs) embedded in a polymer film was investigated. THz electric-field-induced ultrafast Stark effect of one-dimensional excitons in SWNTs was observed at room temperature, suggesting the potential functionality of SWNTs for high speed electro-optic devices operating at telecom wavelength with a THz bandwidth. When the peak electric field amplitude exceeds 200 kV/cm, the generation of excitons by the THz pump becomes prominent. The mechanism is described by the above-gap excitation of electrons and holes in SWNTs due to the impact excitation process induced by the intense THz electric field.  相似文献   

3.
Ultrathin composite films consisting of mixtures of metallic (m‐) and semiconducting (s‐) single‐walled carbon nanotubes (SWNTs) with a conjugated block copolymer are developed from a solution‐based process. The electronic properties of the films are precisely controlled from metallic to semiconducting to insulating. The tunability of the electronic composite sheets is mainly attributed to (1) the efficient dispersion of SWNTs with a conjugated block copolymer in solution, (2) the control of the number of nanotubes by centrifugation, and (3) the individually networked deposition of SWNTs embedded in the conjugated block copolymer on the target substrate by spin‐coating. A highly reliable field‐effect transistor with a networked composite film is realized with a specific range of tube density and a high on/off current ratio of approximately 106 which resulted from the Schottky barriers evolved between the individual m‐ and s‐SWNTs in the network. There is also great freedom when choosing both the gate dielectrics and source‐drain electrodes for transistors containing the composite films. Furthermore, the fabricated electronic composites are highly transparent, flexible, and chemically robust and thus, they can be conveniently micropatterned by photolithography, as well as by unconventional transfer printing techniques.  相似文献   

4.
Polymers which enrich semiconducting single‐walled carbon nanotubes (SWNTs) and are also removable after enrichment are highly desirable for achieving high‐performance field‐effect transistors (FETs). We have designed and synthesized a new class of alternating copolymers containing main‐chain fluorene and hydrofluoric acid (HF) degradable disilane for sorting and preferentially suspending semiconducting nanotube species. The results of optical absorbance, photoluminescence emission, and resonant Raman scattering show that poly[(9,9‐dioctylfluorenyl‐2,7‐diyl)‐alt‐co‐1,1,2,2‐tetramethyl‐disilane] preferentially suspends semiconducting nanotubes with larger chiral angle (25°–28°) and larger diameter (1.03 nm–1.17 nm) (specifically (8,7), (9,7) and (9,8) species) present in HiPCO nanotube samples. Computer simulation shows that P1 preferentially interacts with (8,7) (semiconducting) over (7,7) (metallic) species, confirming that P1 selects larger diameter, larger chiral angle semiconducting tubes. P1 wrapped on the surface of SWNTs is easily washed off through degradation of the disilane bond of the alternating polymer main chain in HF, yielding “clean” purified SWNTs. We have applied the semiconducting species enriched SWNTs to prepare solution‐processed FET devices with random nanotube network active channels. The devices exhibit stable p‐type semiconductor behavior in air with very promising characteristics. The on/off current ratio reaches up to 15 000, with on‐current level of around 10 μA and estimated hole mobility of 5.2 cm2 V?1 s?1.  相似文献   

5.
Polymer wrapped single‐walled carbon nanotubes (SWNTs) have been demonstrated to be a very efficient technique to obtain high purity semiconducting SWNT solutions. However, the extraction yield of this technique is low compared to other techniques. Poly‐alkyl‐thiophenes have been reported to show higher extraction yield compare to polyfluorene derivatives. Here, the affinity for semiconducting SWNTs of two polymers with a backbone containing didodecylthiophene units interspersed with N atoms is reported. It is demonstrated that one of the polymers, namely, poly(2,5‐dimethylidynenitrilo‐3,4‐didodecylthienylene) (PAMDD), has very high semiconducting SWNT extraction yield compared to the poly(3,4‐didodecylthienylene)azine (PAZDD). The dissimilar wrapping efficiency of these two polymers for semiconducting SWNTs is attributed to the interplay between the affinity for the nitrogen atoms of the highly polarizable walls of SWNTs and the mechanical flexibility of the polymer backbones. Photoluminescence (PL) measurements demonstrate the presence of metallic tubes and SWNT bundles in the sample selected with PAZDD and higher purity of SWNT‐PAMDD samples. The high purity of the semiconducting SWNTs selected by PAMDD is further demonstrated by the high performance of the solution‐processed field‐effect transistors (FETs) fabricated using a blade coating technique, which exhibit hole mobilities up to 33.3 cm2 V?1 s?1 with on/off ratios of 106.  相似文献   

6.
Sorting of semiconducting single‐walled carbon nanotubes (SWNTs) by conjugated polymers has attracted considerable attention recently because of its simplicity, high selectivity, and high yield. However, up to now, all the conjugated polymers used for SWNT sorting are electron‐donating (p‐type). Here, a high‐mobility electron‐accepting (n‐type) polymer poly([N,N′‐bis(2‐octyldodecyl)‐naphthalene‐1,4,5,8‐bis(dicarboximide)‐2,6‐diyl]‐alt‐5,5′‐(2,2′‐bithiophene)) (P(NDI2OD‐T2)) is utilized for the sorting of high‐purity semiconducting SWNTs, as characterized by Raman spectroscopy, dielectric force spectroscopy and transistor measurements. In addition, the SWNTs sorted by P(NDI2OD‐T2) have larger diameters than poly(3‐dodecylthiophene) (P3DDT)‐sorted SWNTs. Molecular dynamics simulations in explicit toluene demonstrate distinct linear or helical wrapping geometry between P(NDI2OD‐T2) and different types of SWNTs, likely as a result of the strong interactions between the large aromatic core of the P(NDI2OD‐T2) backbone and the hexagon path of SWNTs. By using high‐mobility n‐type P(NDI2OD‐T2) as the sorting polymer, ambipolar SWNT transistors with better electron transport than that attained by P3DDT‐sorted SWNTs are achieved. As a result, flexible negated AND and negated OR logic circuits from the same set of ambipolar transistors are fabricated, without the need for doping. The use of n‐type polymers for sorting semiconducting SWNTs and achieving ambipolar SWNT transistor characteristics greatly simplifies the fabrication of flexible complementary metal‐oxide‐semiconductor‐like SWNT logic circuits.  相似文献   

7.
Dichlorocarbene is added to the sidewalls of single‐walled carbon nanotubes (SWNTs) with diameters ranging from 1.2 to 2.2 nm. Small diameter SWNTs are found to react much more easily than large diameter SWNTs. Upon functionalization, the conductance could be largely preserved for almost all SWNTs, while an effective bandgap increase for functionalized metallic SWNTs (m‐SWNTs) and a bandgap reduction for functionalized semiconducting SWNTs (s‐SWNTs) are generally observed. The results suggest that [2 + 1] cycloaddition is an excellent choice of processing, resulting in SWNTs over a large diameter range with electronic properties that are almost unaffected. Furthermore, possible separation of SWNTs according to their diameters could be achieved due to the apparent diameter‐dependent reactivity.  相似文献   

8.
The effects of the incorporation of semiconducting single‐walled nanotubes (sc‐SWNTs) with high purity on the bulk heterojunction (BHJ) organic solar cell (OSC) based on regioregular poly(3‐hexylthiophene‐2,5‐diyl):[6,6]‐phenyl‐C61‐butyric acid methyl ester (rr‐P3HT:PCBM) are reported for the first time. The sc‐SWNTs induce the organization of the polymer phase, which is evident from the increase in crystallite size, the red‐shifted absorption characteristics and the enhanced hole mobility. By incorporating sc‐SWNTs, OSC with a power conversion efficiency (PCE) as high as 4% can be achieved, which is ≈8% higher than our best control device. A novel application of sc‐SWNTs in improving the thermal stability of BHJ OSCs is also demonstrated. After heating at 150 °C for 9 h, it is observed that the thermal stability of rr‐P3HT:PCBM devices improves by more than fivefold with inclusion of sc‐SWNTs. The thermal stability enhancement is attributed to a more suppressed phase separation, as shown by the remarkable decrease in the formation of sizeable crystals, which in turn can be the outcome of a more controlled crystallization of the blend materials on the nanotubes.  相似文献   

9.
Low‐voltage, hysteresis‐free, flexible thin‐film‐type electronic systems based on networks of single‐walled carbon nanotubes and bilayer organic–inorganic nanodielectrics are detailed in work by Rogers and co‐workers reported on p. 2355. The cover image shows a schematic array of such thin‐film transistors (TFTs) on a plastic substrate. The structure of the bilayer nanodielectric, which consists of a film of HfO2 formed by atomic layer deposition and an ultrathin layer of epoxy formed by spin‐casting, is also illustrated schematically. High‐capacitance bilayer dielectrics based on atomic‐layer‐deposited HfO2 and spin‐cast epoxy are used with networks of single‐walled carbon nanotubes (SWNTs) to enable low‐voltage, hysteresis‐free, and high‐performance thin‐film transistors (TFTs) on silicon and flexible plastic substrates. These HfO2–epoxy dielectrics exhibit excellent properties including mechanical flexibility, large capacitance (up to ca. 330 nF cm–2), and low leakage current (ca. 10–8 A cm–2); their low‐temperature (ca. 150 °C) deposition makes them compatible with a range of plastic substrates. Analysis and measurements of these dielectrics as gate insulators in SWNT TFTs illustrate several attractive characteristics for this application. Their compatibility with polymers used for charge‐transfer doping of SWNTs is also demonstrated through the fabrication of n‐channel SWNT TFTs, low‐voltage p–n diodes, and complementary logic gates.  相似文献   

10.
An aqueous, protein‐enabled (biomimetic), layer‐by‐layer titania deposition process is developed, for the first time, to convert aligned‐nanochannel templates into high‐aspect‐ratio, aligned nanotube arrays with thin (34 nm) walls composed of co‐continuous networks of pores and titania nanocrystals (15 nm ave. size). Alumina templates with aligned open nanochannels are exposed in an alternating fashion to aqueous protamine‐bearing and titania precursor‐bearing (Ti(IV) bis‐ammonium‐lactato‐dihydroxide, TiBALDH) solutions. The ability of protamine to bind to alumina and titania, and to induce the formation of a Ti–O‐bearing coating upon exposure to the TiBALDH precursor, enables the layer‐by‐layer deposition of a conformal protamine/Ti–O‐bearing coating on the nanochannel surfaces within the porous alumina template. Subsequent protamine pyrolysis yields coatings composed of co‐continuous networks of pores and titania nanoparticles. Selective dissolution of the underlying alumina template through the porous coating then yields freestanding, aligned, porous‐wall titania nanotube arrays. The interconnected pores within the nanotube walls allow enhanced loading of functional molecules (such as a Ru‐based N719 dye), whereas the interconnected titania nanoparticles enable the high‐aspect‐ratio, aligned nanotube arrays to be used as electrodes (as demonstrated for dye‐sensitized solar cells with power conversion efficiencies of 5.2 ± 0.4%).  相似文献   

11.
High‐capacitance bilayer dielectrics based on atomic‐layer‐deposited HfO2 and spin‐cast epoxy are used with networks of single‐walled carbon nanotubes (SWNTs) to enable low‐voltage, hysteresis‐free, and high‐performance thin‐film transistors (TFTs) on silicon and flexible plastic substrates. These HfO2–epoxy dielectrics exhibit excellent properties including mechanical flexibility, large capacitance (up to ca. 330 nF cm–2), and low leakage current (ca. 10–8 A cm–2); their low‐temperature (ca. 150 °C) deposition makes them compatible with a range of plastic substrates. Analysis and measurements of these dielectrics as gate insulators in SWNT TFTs illustrate several attractive characteristics for this application. Their compatibility with polymers used for charge‐transfer doping of SWNTs is also demonstrated through the fabrication of n‐channel SWNT TFTs, low‐voltage p–n diodes, and complementary logic gates.  相似文献   

12.
Here, the use of metal oxide layers both for charge transport and injection into an emissive semiconducting polymer and also for the control of the in‐plane waveguided optical modes in light‐emitting diodes (LEDs) is reported. The high refractive index of zinc oxide is used to confine these modes away from the absorbing electrodes, and include a nano‐imprinted grating in the polymer layer to introduce distributed feedback and enhance optical out‐coupling. These structures show a large increase in the luminescence efficiency over conventional devices, with photoluminescence efficiency increased by up to 45%. Furthermore, optically‐pumped lasing in hybrid oxide polymer LEDs is demonstrated. A tuneable lasing emission is also obtained in a single device structure by employing a graduated thickness of a zinc oxide inter‐layer. This demonstrates the scope for using such architectures to improve the external efficiency of organic semiconductor LEDs, and opens new possibilities for the realization of polymer injection lasers.  相似文献   

13.
Single‐walled carbon nanotube (SWNT) electrodes that are chemically and mechanically robust are fabricated using a simple drop cast method with thermal annealing and acid treatment. An electronic‐type selective decrease in sheet resistance of SWNT electrodes with HNO3 treatment is shown. Semiconducting SWNTs show a significantly higher affinity toward hole doping in comparison to metallic SWNTs; a ≈12‐fold and a ≈fivefold drop in sheet resistance, respectively. The results suggest the insignificance of the electronic type of the SWNTs for the film conductivity after hole doping. The SWNT films have been employed as transparent hole extracting electrodes in bulk heterojunction (BHJ) organic photovoltaics. Performances of the devices enlighten the fact that the electrode film morphology dominates over the electronic type of the doped SWNTs with similar sheet resistance and optical transmission. The power conversion efficiency (PCE) of 4.4% for the best performing device is the best carbon nanotube transparent electrode incorporated large area BHJ solar cell reported to date. This PCE is 90% in terms of PCEs achieved using indium tin oxide (ITO) based reference devices with identical film fabrication parameters indicating the potential of the SWNT electrodes as an ITO replacement toward realization of all carbon solar cells.  相似文献   

14.
We have developed a high performance liquid crystal (LC) alignment layer of ultra‐thin single wall carbon nanotubes (SWNTs) and a conjugated block copolymer nanocomposite that is solution‐processible for conventional twisted nematic (TN) LC cells. The alignment layer is based on the non‐destructive solution dispersion of nanotubes with a poly(styrene‐b‐ paraphenylene) (PS‐b‐PPP) copolymer and subsequent spin coating, followed by conventional rubbing without a post‐annealing process. Topographically grooved nanocomposite films with two dimensionally (2D) networked SWNTs embedded in a block copolymer matrix were created using a rubbing process in which bundles of SWNTs on the composite surface were effectively removed. The LCs were well aligned with a stable pre‐tilt angle of approximately 2° on our extremely transparent nanocomposite, which gave rise to superfast switching of the TN LC molecules that was approximately 3.8 ms, or four times faster than that on a commercial polyimide layer. Furthermore, the TN LCD cells containing our SWNT nanocomposite alignment layers exhibited low power operation at an effective switching voltage amplitude of approximately 1.3 V without capacitance hysteresis.  相似文献   

15.
An aqueous, protein‐enabled (biomimetic), layer‐by‐layer titania deposition process is developed, for the first time, to convert aligned‐nanochannel templates into high‐aspect‐ratio, aligned nanotube arrays with thin (34 nm) walls composed of co‐continuous networks of pores and titania nanocrystals (15 nm ave. size). Alumina templates with aligned open nanochannels are exposed in an alternating fashion to aqueous protamine‐bearing and titania precursor‐bearing (Ti(IV) bis‐ammonium‐lactato‐dihydroxide, TiBALDH) solutions. The ability of protamine to bind to alumina and titania, and to induce the formation of a Ti–O‐bearing coating upon exposure to the TiBALDH precursor, enables the layer‐by‐layer deposition of a conformal protamine/Ti–O‐bearing coating on the nanochannel surfaces within the porous alumina template. Subsequent protamine pyrolysis yields coatings composed of co‐continuous networks of pores and titania nanoparticles. Selective dissolution of the underlying alumina template through the porous coating then yields freestanding, aligned, porous‐wall titania nanotube arrays. The interconnected pores within the nanotube walls allow enhanced loading of functional molecules (such as a Ru‐based N719 dye), whereas the interconnected titania nanoparticles enable the high‐aspect‐ratio, aligned nanotube arrays to be used as electrodes (as demonstrated for dye‐sensitized solar cells with power conversion efficiencies of 5.2 ± 0.4%).  相似文献   

16.
We report a new approach of reactive spinning to fabricate thermosetting cyanate ester micro‐scale diameter fibers with aligned single walled carbon nanotubes (SWNTs). The composite fibers were produced by first dispersing the SWNTs (1 wt %) in cyanate ester (CE) via solvent blending, followed by pre‐polymerization, spinning and then multiple‐stage curing. The pre‐polymerization, spinning and post‐spinning cure temperatures were carefully controlled to achieve good spun crosslinked fibers. Both pristine and amino‐functionalized SWNTs were used for the reinforced fiber spinning. Amino‐functionalized SWNTs (f‐SWNTs) were prepared by reacting acid‐treated SWNTs with toluene 2,4‐diisocyanate and then ethylenediamine (EDA). FTIR, optical microscopy and scanning electron microscopy (SEM) showed that the amino‐functionalized SWNTs were covalently and uniformly dispersed into the cyanate ester matrix and aligned along the fiber axis. The alignment was further confirmed using polarized Raman spectroscopy. The composite fibers with aligned amino‐functionalized SWNTs possess improved tensile properties with respect to neat CE fibers, showing 85, 140, and 420% increase in tensile strength, elongation and stress‐strain curve area (i.e., toughness), respectively. NH2‐functionalization of SWNTs improves their dispersibility, alignment and interfacial strength and hence tensile properties of composite spun fibers. Fiber spinning to align SWNTs using thermosetting resin is novel. Others have reported fiber spinning to align SWNTs in thermoplastics. However, thermosetting CE resins offer the advantages of low and controllable viscosity during spinning and reactivity with amino functional groups to enable f‐SWNT/CE covalent bonding.  相似文献   

17.
The integration of redox proteins with nanomaterials has attracted much interest in the past years, and metallic single‐walled carbon nanotubes (SWNTs) have been introduced as efficient electrical wires to connect biomolecules to metal electrodes in advanced nano‐biodevices. Besides preserving biofunctionality, the protein–nanotube connection should ensure appropriate molecular orientation, flexibility, and efficient, reproducible electrical conduction. In this respect, yeast cytochrome c redox proteins are connected to gold electrodes through lying‐down functionalized metallic SWNTs. Immobilization of cytochromes to nanotubes is obtained via covalent bonding between the exposed protein thiols and maleimide‐terminated functional chains attached to the carbon nanotubes. A single‐molecule study performed by combining scanning probe nanoscopies ascertains that the protein topological properties are preserved upon binding and provides unprecedented current images of single proteins bound to carbon nanotubes that allow a detailed IV characterization. Collectively, the results point out that the use as linkers of suitably functionalized metallic SWNTs results in an electrical communication between redox proteins and gold electrodes more efficient and reproducible than for proteins directly connected with metal surfaces.  相似文献   

18.
Using Raman spectroscopy, we demonstrate that the anisotropic interaction between single‐walled carbon nanotubes (SWNTs) and poly(methyl methacrylate) (PMMA) causes significant changes in the electronic properties of their composites. Two different procedures were used to prepare the composites: melt blending and in‐situ UV polymerization. Resonant Raman studies relate the electronic density of states (DOS) of the SWNTs to the corresponding vibration symmetry changes of both the PMMA and the SWNTs. Our results show that, in the melt‐blended sample, the SWNTs—originally semiconducting—became predominantly metallic. The changes in the electronic properties were also confirmed by dielectric constant measurements. We propose that the anisotropic interaction between PMMA and SWNTs in the melt‐blended composite is the dominant reason for the observed electronic character change.  相似文献   

19.
Field‐effect transistors that employ an electrolyte in place of a gate dielectric layer can accumulate ultrahigh‐density carriers not only on a well‐defined channel (e.g., a two‐dimensional surface) but also on any irregularly shaped channel material. Here, on thin films of 95% pure metallic and semiconducting single‐walled carbon nanotubes (SWNTs), the Fermi level is continuously tuned over a very wide range, while their electronic transport and absorption spectra are simultaneously monitored. It is found that the conductivity of not only the semiconducting but also the metallic SWNT thin films steeply changes when the Fermi level reaches the edges of one‐dimensional subbands and that the conductivity is almost proportional to the number of subbands crossing the Fermi level, thereby exhibiting a one‐dimensional nature of transport even in a tangled network structure and at room temperature.  相似文献   

20.
Poly(m‐aminobenzene sulfonic acid) (PABS), was covalently bonded to single‐walled carbon nanotubes (SWNTs) to form a water‐soluble nanotube–polymer compound (SWNT–PABS). The conductivity of the SWNT–PABS graft copolymer was about 5.6 × 10–3 S cm–1, which is much higher than that of neat PABS (5.4 × 10–7 S cm–1). The mid‐IR spectrum confirmed the formation of an amide bond between the SWNTs and PABS. The 1H NMR spectrum of SWNT–PABS showed the absence of free PABS, while the UV/VIS/NIR spectrum of SWNT–PABS showed the presence of the interband transitions of the semiconducting SWNTs and an absorption at 17 750 cm–1 due to the PABS addend.  相似文献   

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