US20170077407A1 - Carbon nanotube array, material, electronic device, process for producing carbon nanotube array, and process for producing field effect transistor - Google Patents

Carbon nanotube array, material, electronic device, process for producing carbon nanotube array, and process for producing field effect transistor Download PDF

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US20170077407A1
US20170077407A1 US15/122,658 US201515122658A US2017077407A1 US 20170077407 A1 US20170077407 A1 US 20170077407A1 US 201515122658 A US201515122658 A US 201515122658A US 2017077407 A1 US2017077407 A1 US 2017077407A1
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carbon nanotube
nanotube array
cnts
producing
carbon nanotubes
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Shigeo Maruyama
Shohei Chiashi
Keigo OHTSUKA
Taiki INOUE
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University of Tokyo NUC
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Showa Denko KK
University of Tokyo NUC
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Assigned to THE UNIVERSITY OF TOKYO, SHOWA DENKO K.K. reassignment THE UNIVERSITY OF TOKYO ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: CHIASHI, SHOHEI, INOUE, TAIKI, MARUYAMA, SHIGEO, OHTSUKA, KEIGO
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Assigned to THE UNIVERSITY OF TOKYO reassignment THE UNIVERSITY OF TOKYO ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: SHOWA DENKO K.K.
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    • Y10S977/938—Field effect transistors, FETS, with nanowire- or nanotube-channel region

Definitions

  • the present invention relates to a carbon nanotube array, a material, an electronic device, a process for producing a carbon nanotube array, and a process for producing a field effect transistor.
  • the present invention particularly relates to a carbon nanotube array in which semiconducting carbon nanotubes are horizontally aligned densely, specifically at a density of 1 line/ ⁇ m or more, and a process for producing the same.
  • the present invention relates to a material formed with the carbon nanotube array, for example, an electronic material, an optical material, or an electrochemical material.
  • the present invention relates to an electronic device formed with the carbon nanotube array, specifically, a field effect transistor (FET), a solar cell, a chemical sensor, a photosensor, an optical element, or a terahertz sensor.
  • FET field effect transistor
  • solar cell a solar cell
  • chemical sensor a photosensor
  • optical element an optical element
  • terahertz sensor a terahertz sensor
  • a carbon nanotube particularly, a semiconducting carbon nanotube (hereinafter, referred to as an “s-CNT” in some cases) is expected to be applicable to next-generation devices due to superiority in electronic properties, optical properties, mechanical properties, thermal properties, and the like.
  • m-CNTs metallic carbon nanotubes
  • NPL 1 discloses a method of “electrical breakdown”. This method is a method of applying voltage to each carbon nanotube of a carbon nanotube array having s-CNTs and m-CNTs in a long axis direction so as to allow a current to flow into only the m-CNTs.
  • the m-CNT in which a current flows can be locally burned out by self Joule heating.
  • the length of the m-CNT that can be removed is 100 nm at most. Therefore, this method has a problem that the method is not applicable to a carbon nanotube array in which the length of each carbon nanotube is long.
  • the method is applied to the carbon nanotube array in which the length of each carbon nanotube is long, there arises a problem that even when the m-CNT is cut, the m-CNT remains after cutting.
  • NPL 2 discloses a method of using nanoscale thermocapillary flow.
  • a thin film made of only ⁇ , ⁇ , ⁇ ′-tris(4-hydroxyphenyl)-1-ethyl-4-isopropylbenzene is provided on a carbon nanotube array having s-CNTs and m-CNTs.
  • voltage is applied to each carbon nanotube of the carbon nanotube array in the long axis direction so as to allow a current to flow into only the m-CNT. Due to self Joule heating of the m-CNT, the thin film in the vicinity thereof is torn and/or broken by the thermocapillary flow. As a result, the m-CNT is exposed.
  • the s-CNT is present under the thin film. Then, the exposed m-CNT is removed by reactive ion etching (RIE, O 2 /CF 4 ). Finally, the thin film is removed and thus a carbon nanotube array including only the s-CNTs is obtained.
  • RIE reactive ion etching
  • thermocapillary flow since thermocapillary flow is used, the density of the s-CNTs in the carbon nanotube array is low (1 line/3 ⁇ m). Therefore, there is another problem that properties required for an electronic material formed with the carbon nanotube array cannot be obtained.
  • thermocapillary flow is limited to ⁇ , ⁇ , ⁇ ′-tris(4-hydroxyphenyl-1-ethyl-4-isopropylbenzene or the like.
  • An object of the present invention is to provide a method for solving the above problems.
  • an object of the present invention is to provide a process for obtaining a carbon nanotube array including no m-CNTs obtained by removing m-CNTs from a carbon nanotube array having s-CNTs and m-CNTs through simple steps using a mechanism that is different from thermocapillary flow.
  • Another object of the present invention is to provide a carbon nanotube array including no m-CNTs in which the density of s-CNTs is high.
  • a carbon nanotube array according to an aspect of the present invention is a carbon nanotube array including no metallic carbon nanotubes in which semiconducting carbon nanotubes are horizontally aligned at a density of 1 line/ ⁇ m or more.
  • a density of the semiconducting carbon nanotubes may be 1,000 lines/ ⁇ m or more.
  • a length of each semiconducting carbon nanotube of the carbon nanotube array may be 10 ⁇ m or more.
  • the length of each semiconducting carbon nanotube may be preferably 100 ⁇ m or more and more preferably 1,000 ⁇ m or more.
  • an ON/OFF ratio of the FET may be 10,000 or more.
  • the ON/OFF ratio of the FET may be preferably 100,000 or more and more preferably 1,000,000 or more.
  • a material according to an aspect of the present invention is formed with the carbon nanotube array according to any one of the above ⁇ 1> to ⁇ 4>.
  • This material may be, for example, an electronic material, an optical material, an electrochemical material, or the like.
  • An electronic device is formed with the carbon nanotube array according to any one of the above ⁇ 1> to ⁇ 4>.
  • the electronic device may be, for example, a field effect transistor (FET), a solar cell, a chemical sensor, a photosensor, an optical element, or a terahertz sensor.
  • FET field effect transistor
  • a process for producing a carbon nanotube array includes: (A) a step of preparing a carbon nanotube array in which metallic carbon nanotubes and semiconducting carbon nanotubes are horizontally aligned; (B) a step of forming an organic layer on the carbon nanotube array; (C) a step of applying voltage to the horizontally aligned carbon nanotube array in a long axis direction of the carbon nanotubes constituting the carbon nanotube array in the air; and (D) a step of removing the organic layer.
  • the organic substance in the (B) step may have a thermal diffusion coefficient of 2'10 ⁇ 7 m 2 /s or less.
  • the thermal diffusion coefficient thereof may be preferably 1 ⁇ 10 ⁇ 7 m 2 /s or less and more preferably 0.2 ⁇ 10 ⁇ 7 m 2 /s or less.
  • the organic layer in the (B) step may be a layer made of only ⁇ , ⁇ , ⁇ ′-tris(4-hydroxyphenyl)-1-ethyl-4-isopopylbenzene or a layer made of only poly(methyl methacrylate).
  • the semiconducting carbon nanotubes may be horizontally aligned at a density of 1 line/ ⁇ m or more.
  • the semiconducting carbon nanotubes may be horizontally aligned preferably at a density of 3 lines/ ⁇ m or more, more preferably at a density of 10 lines/ ⁇ m or more, and most preferably at a density of 30 lines/ ⁇ m or more.
  • a length of the semiconducting carbon nanotube may be 10 ⁇ m or more.
  • the length of the semiconducting carbon nanotube may be preferably 100 ⁇ m or more and more preferably 1,000 ⁇ m or more.
  • a process for producing a field effect transistor (FET) according to an aspect of the present invention may he a process using a carbon nanotube array that is produced using the process for producing a carbon nanotube array according to any one of the above ⁇ 7> to ⁇ 11>.
  • An ON/OFF ratio of the field effect transistor may be 10,000 or more, preferably 100,000 or more, and more preferably 1,000,000 or more.
  • thermocapillary flow it is possible to obtain a carbon nanotube array including no m-CNTs by removing m-CNTs from a carbon nanotube array having s-CNTs and m-CNTs through simple steps using a mechanism that is different from thermocapillary flow.
  • FIG. 1 is a graph showing the ON/OFF ratio of a FET using a carbon nanotube array before a series of steps of applying voltage and removing a film are performed (“Before”) and after the steps are performed (“After”).
  • FIG. 2 is a schematic view when voltage is applied to a carbon nanotube array including m-CNTs and s-CNTs.
  • FIG. 3 shows SEM images of the carbon nanotube array before a series of steps of applying voltage and removing a film are performed (“Before”) and after the steps are performed (“After”).
  • FIG. 4 shows SEM images of the carbon nanotube array before a series of steps of applying voltage and removing a film are performed (“Before”) and after the steps are performed (“After”) and a graph showing measurement results of spots shown in the SEM images using Raman spectroscopy.
  • the present invention provides a carbon nanotube array including no metallic carbon nanotubes and a process for producing the same.
  • the present invention provides a material and an electronic device formed with a carbon nanotube array including no metallic carbon nanotubes.
  • the expression “including no metallic carbon nanotubes” means that the carbon nanotube array does not have properties of metallic carbon nanotubes.
  • a including no metallic carbon nanotubes means that the electrical conductivity of “A” does not exhibit metallic properties, more specifically, semiconductor properties.
  • a carbon nanotube array including no metallic carbon nanotubes is produced from a carbon nanotube array in which metallic carbon nanotubes and semiconducting carbon nanotubes are horizontally aligned.
  • the process has the following steps.
  • the process for producing a carbon nanotube array includes: (A) a step of preparing a carbon nanotube array in which metallic carbon nanotubes and semiconducting carbon nanotubes are horizontally aligned; (B) a step of forming an organic layer on the carbon nanotube array; (C) a step of applying voltage to the horizontally aligned carbon nanotube array in a long axis direction of the carbon nanotubes constituting the carbon nanotube array in the air; and (D) a step of removing the organic layer. After the (C) step is completed, the carbon nanotube array is free from metallic carbon nanotubes.
  • Step (A) is a step of preparing a carbon nanotube array in which metallic carbon nanotubes and semiconducting carbon nanotubes are horizontally aligned.
  • the carbon nanotube array in which metallic carbon nanotubes and semiconducting carbon nanotubes are horizontally aligned can be produced by a conventionally known process.
  • the process is not limited to the following processes, for example, a method using a single crystal substrate having an R-cut surface described in WO2011/108545, which partially matches with the process of the present inventors of the present invention, a method using a SiO 2 single crystal substrate having a ST-cut surface, a method using a sapphire substrate having an R-cut surface, and a method using single crystal substrate having a step may be used.
  • the carbon nanotube array to be prepared in Step (A) has metallic carbon nanotubes and semiconducting carbon nanotubes.
  • the carbon nanotube array may include carbon nanotubes having other properties, for example, a carbon nanotube which is a metallic carbon nanotube but has defects and is thereby formed into a semiconductor-like carbon nanotube. However, it is preferable to suppress the amount of the carbon nanotube having other properties contained as much as possible in the case of using an electronic material or the like.
  • the length of each semiconducting carbon nanotube in the carbon nanotube array does not change. Accordingly, the length of each semiconducting carbon nanotube in the carbon nanotube array in Step (A) may be 10 ⁇ m or more, preferably 100 ⁇ m or more, and more preferably 1,000 ⁇ m or more.
  • Step (A) when the length of each semiconducting carbon nanotube is set to the above length, the carbon nanotube array having the above length can be easily produced. In addition, a material having the carbon nanotube array can be easily produced in large quantity. Further, using the carbon nanotube array, an integrated circuit in which a large number of FETs are also arranged in the axial direction of the array can be produced.
  • Step (C) the metallic carbon nanotubes in the carbon nanotube array are removed, but the density of the semiconducting carbon nanotubes does not change. Accordingly, the density of the semiconducting carbon nanotubes in the carbon nanotube array in Step (A) is 1 line/ ⁇ m or more, preferably 3 lines/ ⁇ m or more, more preferably 10 lines/ ⁇ m or more, and more preferably 30 lines/ ⁇ m or more.
  • a substrate may be provided or may not be provided under the carbon nanotube array.
  • a substrate is provided under the carbon nanotube array.
  • the substrate may be a substrate (first substrate) used for obtaining a carbon nanotube array in which metallic carbon nanotubes and semiconducting carbon nanotubes are horizontally aligned or may be another substrate (second substrate) that is different from the first substrate. That is, in the case of using the second substrate, the array may be moved onto from the first substrate used for obtaining the carbon nanotube array to the second substrate.
  • first substrate used for obtaining a carbon nanotube array in which metallic carbon nanotubes and semiconducting carbon nanotubes are horizontally aligned
  • second substrate another substrate that is different from the first substrate. That is, in the case of using the second substrate, the array may be moved onto from the first substrate used for obtaining the carbon nanotube array to the second substrate.
  • Step (B) is a step of forming an organic layer on the carbon nanotube array prepared in Step (A) above.
  • Step (C) the organic layer exhibits an effect of maintaining a combustion reaction of the metallic carbon nanotube. Since the organic layer more easily burns than the carbon nanotube, the organic layer can support the combustion. It is considered that the combustion reaction of each metallic carbon nanotube is conducted in the following steps while the combustion reaction is supported by combustion of the organic layer.
  • the carbon nanotube transports combustion heat at the end portion in the axial direction.
  • the organic layer is heated by the transported combustion heat. Combustion starts in the organic layer of the heated portion by applying the combustion heat.
  • the organic layer in which combustion has started applies the heat to the carbon nanotube again and combustion starts at a portion of the carbon nanotube to which heat is applied. By repeating the above steps, the combustion reaction of each metallic carbon nanotube is maintained.
  • the organic layer is a layer which exhibits the above effect and as long as an organic substance is used to form the layer, the organic substance is not particularly limited. Only one or wo or more organic substances may be used.
  • the layer may be formed on the carbon nanotube array in any form. It is preferable that the organic layer is formed so as to cover the entire carbon nanotube array.
  • the thickness thereof is not particularly limited.
  • the thickness may be 3 to 1,000 nm, preferably 10 to 100 nm and more preferably 20 to 60 nm.
  • the thermal diffusion coefficient of the organic substance may be 2 ⁇ 10 ⁇ 7 m 2 /s or less, preferably 1 ⁇ 10 ⁇ 7 m 2 /s or less, and more preferably 0.2 ⁇ 10 ⁇ 7 m 2 /s or less.
  • the organic substance has good heat retention to exhibit the above effect.
  • the organic layer may be a layer particularly made of only ⁇ , ⁇ , ⁇ ′-tris(4-hydroxyphenyl)-1-ethyl-4-isopropylbenzene or a layer made of only poly(methyl methacrylate).
  • the organic layer varies depending on an organic substance to be used, the molecular weight thereof, and the like.
  • the layer can be obtained by applying a solution of an organic substance to be used so as to cover the entire carbon nanotube array by a conventionally known method.
  • the conventional known method is not limited to the following methods, for example, spin coating, heat resistance deposition, and the like may be used.
  • Step (C) is a step of applying voltage to the horizontally aligned carbon nanotube array provided with the organic layer obtained in Step (B) above in the long axis direction of the carbon nanotubes constituting the carbon nanotube array in the air.
  • Step (C) is completed, the carbon nanotube array is free from the metallic carbon nanotubes.
  • Step (C) voltage is applied to the carbon nanotube array in which metallic carbon nanotubes and semiconducting carbon nanotube are horizontally aligned.
  • the voltage application direction is a direction along the long axis direction of the carbon nanotubes constituting the carbon nanotube array and it does not matter whether the direction is normal or revered. Since the voltage pplied, an electrode may be appropriately provided.
  • the voltage is set such that a current flows only into the metallic carbon nanotubes in the carbon nanotube array.
  • the metallic carbon nanotubes are heated by self Joule heating, heat generation does not occur in the semiconducting carbon nanotubes.
  • Step (C) of the present invention due to the presence of the organic layer, the effect of maintaining the combustion reaction of the metallic carbon nanotube is exhibited. Due to this effect, it is considered that the metallic carbon nanotubes burn over the entire length and the carbon nanotube array is free from the metallic carbon nanotubes.
  • Step (C) The voltage application in Step (C) is performed in the air in contrast with “in vacuum or in an inert gas such as nitrogen” in NPL 2 using “thermocapillary flow”.
  • Step (C) it is preferable to perform Step (C) in the air having a high steam pressure as much as possible within a range not causing dew condensation.
  • Step (C) can be completed by monitoring the current at the time of the voltage application.
  • Step (C) the current is allowed to flow only into the metallic carbon nanotubes. When the whole metallic carbon nanotubes are burned out, the current becomes zero and thus the voltage application can be completed at the time when the current becomes zero or after few minutes has passed from the zero current, that is, Step (C) can be completed.
  • Step (D) is a step of removing the organic layer.
  • Step (D) is dependent on an organic substance to be used for the organic layer.
  • an organic substance may be dissolved and removed by using a solvent for dissolving the organic substance.
  • a solvent for dissolving the organic substance for example, in the case of using a layer made of only ⁇ , ⁇ , ⁇ ′-tris(4-hydroxyphenyl)-1-ethyl-4-isopropylbenzene for the organic layer, as a good solvent for the layer, for example, acetone or the like is preferably used.
  • a layer made of only poly(methyl methacrylate) for the organic layer as a good solvent for the layer, for example, acetone or the like is preferably used.
  • the process for producing the carbon nanotube array according to the present invention having Steps (A) to (D) may include steps other than Steps (A) to (D) above.
  • steps other than Steps (A) to (D) above examples include an observation step with an electron microscope (SEM), and an observation step using Raman spectroscopy.
  • the carbon nanotube array of the present invention is a carbon nanotube array including no metallic carbon nanotubes.
  • the semiconducting carbon nanotubes constituting the carbon nanotube array are horizontally aligned at a density of 1 line/ ⁇ m or more.
  • the density is preferably 3 lines/ ⁇ m or more, more preferably 10 lines/ ⁇ m or more, and still more preferably 30 lines/ ⁇ m or more.
  • the semiconducting carbon nanotubes are horizontally aligned preferably at a density of 1,000 lines/ ⁇ m or less, more preferably at a density of 500 lines/ ⁇ m or less, and most preferably at a density of 250 lines/ ⁇ m or less.
  • the density of the semiconducting carbon nanotubes is within the above range, in the case of forming a field effect transistor (FET) with the carbon nanotube array including no metallic carbon nanotubes, electrolytic concentration on the semiconducting carbon nanotubes is easily achieved.
  • FET field effect transistor
  • the broken metallic carbon nanotubes remain. However, in the carbon nanotube array of the present invention, the broken metallic carbon nanotubes do not remain. That is, it is possible to provide a carbon nanotube array including no metallic carbon nanotubes. Herein, it is possible to confirm that the metallic carbon nanotubes “do not remain” from the fact that the metallic carbon nanotubes are not detected in analysis through a “SEM image and the Raman spectroscopy”, which will be described later. In NPL 2, since “thermocapillary flow” is used, the density of the semiconducting carbon nanotubes is only about 1 line/3 ⁇ m. In contrast, it is possible to increase the density of the semiconducting carbon nanotubes in the carbon nanotube array of the present invention.
  • each semiconducting carbon nanotube of the carbon nanotube array may be 10 ⁇ m or more, preferably 100 ⁇ m or more, and more preferably 1,000 ⁇ m or more.
  • each semiconducting carbon nanotube of the carbon nanotube array including no metallic carbon nanotubes is 100 nm at most. Therefore, it is not possible to obtain a carbon nanotube having the same length as the carbon nanotube array of the present invention.
  • each semiconducting carbon nanotube of the carbon nanotube array When the length of each semiconducting carbon nanotube of the carbon nanotube array is set as described above, a material having the carbon nanotube array can be easily produced in a large quantity. Further, when the carbon nanotube array is used, an integrated circuit in which a large number of FETs are also arranged in the axial direction of the array can be produced.
  • the carbon nanotube array of the present invention is free from metallic carbon nanotubes. Therefore, in the case of forming a field effect transistor (FET) with the carbon nanotube array, the ON/OFF ratio of the FET may be 10,000 or more, preferably 100,000 or more, and more preferably 1,000,000 or more.
  • FET field effect transistor
  • the material of the present invention has the above-described carbon nanotube array.
  • examples thereof include an electronic material, an optical material, or an electrochemical material.
  • the electronic device of the present invention has the above-described carbon nanotube array.
  • the electronic device is not limited to the following examples, examples thereof include a field effect transistor (FET), a solar cell, a chemical sensor, a photosensor, an optical element, or a terahertz sensor.
  • FET field effect transistor
  • solar cell a solar cell
  • chemical sensor a photosensor
  • optical element an optical element
  • terahertz sensor a terahertz sensor
  • a resist pattern was formed on the substrate by photolithography.
  • a catalyst was deposited on the entity of a substrate provided with a resist by vacuum deposition and then the resist was removed so that a catalyst (Fe metal) pattern was formed on the substrate.
  • the substrate having the catalyst (Fe metal) pattern was used to obtain a horizontally aligned carbon nanotube array having s-CNTs and m-CNTs by an alcohol CVD method.
  • the substrate having the catalyst (Fe metal) pattern was placed in a chamber and the inside of the chamber was evacuated. Then, an Ar gas was allowed to flow at a flow rate of 300 sccm for 5 minutes. Next, an Ar/H 2 mixed gas was allowed to flow at a flow rate of 300 sccm, and the pressure in the chamber was set to 40 kPa. Further, the temperature in the chamber was increased to 800° C. for 30 minutes and the temperature was maintained for 10 minutes. The inside of the chamber was evacuated again while maintaining the temperature.
  • the obtained horizontally aligned carbon nanotube array has s-CNTs and m-CNTs both horizontally aligned.
  • the average length thereof was 30 ⁇ m.
  • the density of the horizontally aligned s-CNTs was 1 to 4 lines/ ⁇ m.
  • the horizontally aligned carbon nanotube array formed on the above-described crystal substrate having an r-cut surface was transferred to a p-type Si substrate via poly(methyl methacrylate) (PMMA).
  • an anisole solution (10 wt %) of PMMA was applied on the horizontally aligned carbon nanotube array formed on the above-described crystal substrate having an r-cut surface by spin coating and a PMMA film was formed on the horizontally aligned carbon nanotube array.
  • the crystal substrate having the horizontally aligned carbon nanotube array and provided with the PMMA film was immersed in a 1 M aqueous potassium hydroxide solution. Then, the immersion state was maintained for a while, and then the PMMA film was peeled off in the aqueous solution. As a result, the horizontally aligned carbon nanotube array was transferred onto the PMMA film.
  • the obtained PMMA film was attached to a p-type Si substrate such that the side of the obtained PMMA film having the horizontally aligned carbon nanotube array was brought into contact with the p-type Si substrate. Thereafter, the PMMA film was removed with acetone. Further, the horizontally aligned carbon nanotube array was transferred to the p-type Si substrate by annealing at 350° C. for 3 hours in vacuum.
  • the carbon nanotube array on the p-type Si substrate was observed with an SEM
  • the carbon nanotube array exhibited the same properties before being transferred.
  • the average length of each carbon nanotube had the same value before being transferred
  • the density of the horizontally aligned s-CNTs had the same value before being transferred.
  • Electrodes were arranged on the horizontally aligned carbon nanotube array provided on the obtained p-type Si substrate.
  • the electrode is used for the following reasons. First, the electrode is used as an electrode (source electrode or drain electrode) of a field effect transistor (FET). In the case of removing the m-CNTs, the electrode is also used as an electrode used for voltage application when the m-CNTs are removed.
  • FET field effect transistor
  • the electrodes were provided on the side of the p-type Si substrate having the horizontally aligned carbon nanotube array so as to be orthogonal to each carbon nanotube of the horizontally aligned carbon nanotube array in the long axis direction.
  • the electrodes arranged as described above respectively function as a source electrode and a drain electrode in the FET.
  • Ti/Pd (5/50 nm) was used for an electrode metal and a resist patterned into an electrode having a desired shape by photolithography.
  • the substrate having the resist was placed in a film forming chamber and plasma was generated under the conditions of 0.2 Pa, an Ar gas flow rate of 10 sccm, and an output of 100 W.
  • electrodes were provided on the substrate.
  • an electrode which functions as a gate electrode in the FET was also provided on the side of the p-type Si substrate not having the horizontally aligned carbon nanotube array.
  • the ON/OFF ratio is 1 order. From the result, it is found that the carbon nanotube array includes m-CNTs and thus a short circuit occurs due to the m-CNTs.
  • a layer made of ⁇ , ⁇ , ⁇ -tris(4-hydroxyphenyl)-1-ethyl-4-isopopylbenzene (represented by the following Formula (I)) was formed on the carbon nanotube array having m-CNTs and s-CNTs provided with the electrodes by vacuum deposition, which was obtained in the above ⁇ c.>.
  • the substrate obtained in the above ⁇ c.> was arranged on a stage.
  • a sample of ⁇ , ⁇ , ⁇ -tris(4-hydroxyphenyl)-1-ethyl-4-isopropylbenzene was placed on a tungsten boat connecting between the electrodes.
  • the stage and the boat were covered with the chamber and the inside of the chamber was evaluated to 2.0 ⁇ 10 ⁇ 3 Pa using a rotary pump and an oil diffusion pump.
  • voltage was applied between the electrodes, a current of about 20 A was allowed to flow into the boat, and the sample was evaporated to be deposited on the substrate. It was confirmed that the film thickness was 60 nm (0.06 ⁇ m) with a crystal vibrator arranged in the chamber.
  • one of the electrodes provided on the carbon nanotube array having m-CNTs and s-CNTs was set to a source electrode and the other one was set to a drain electrode.
  • the source electrode was grounded and a drain voltage was applied such that a current flows from the drain electrode to the source electrode.
  • a gate voltage while setting a direction in which the current flows from the gate electrode to the source electrode as a positive direction, +10 V was applied.
  • a distance between the drain electrode and the source electrode was 16.4 ⁇ m.
  • the drain voltage was applied at a voltage increase rate of 0.67 V/min, the current accompanying the voltage application was measured and after about 1 minute had passed from the time when the current value becomes zero, the voltage application was terminated.
  • the voltage at the time of termination was about 40 V.
  • the layer made of ⁇ , ⁇ , ⁇ -tris(4-hydroxyphenyl)-1-ethyl-4-isopropylbenzene on the substrate obtained in the above ⁇ e.> was removed with acetone.
  • the substrate obtained in the above ⁇ e.> was immersed in acetone for several minutes and then rinsed with isopropanol and distilled water. Thereafter, the layer made of ⁇ , ⁇ , ⁇ -tris(4-hydroxyphenyl)-1-ethyl-4-isopropylbenzene was removed by drying the substrate.
  • the substrate having the carbon nanotube array obtained in the above ⁇ f.> is provided with a gate electrode, a source electrode, and a drain electrode.
  • the ON/OFF ratio of the FET having the carbon nanotube array was measured. The result is indicated by “After” in FIG. 1 .
  • the ON/OFF ratio is 10 4 order. From the result, the carbon nanotube array is free from m-CNTs and made up of only s-CNTs.
  • the carbon nanotube array obtained in the above ⁇ f.> was compared with the carbon nanotube array obtained before voltage application in the above ⁇ e.>.
  • SEM images and Raman spectroscopy were used. The results are shown in FIGS. 3 and 4 , respectively.
  • FIG. 3 shows SEM images in which the carbon nanotube array obtained in the above ⁇ f.> (indicated by “After”) is compared with the carbon nanotube array obtained before voltage application in the above ⁇ e.> (indicated by “Before”). From the SEM images, it is found that the m-CNT present within a distance of 1 ⁇ m between s-CNTs is removed. From the result, it is found that the density of the s-CNTs of the carbon nanotube array obtained in the above ⁇ f.> is 1 line/ ⁇ m.
  • FIG. 4 shows SEM images, that is, SEM images of the carbon nanotube array obtained in the above ⁇ f.> (indicated by “After”) on the right side and the carbon nanotube array obtained before voltage application in the above ⁇ e.>(indicated by “Before”) are shown on the right side and results of measuring Raman scattering of spots shown in the SEM images by Raman spectroscopy (“After” and “Before” are the same as described above) on the left side.
  • the carbon nanotube array obtained in the above ⁇ f.> is free from m-CNTs.
  • the layer made of ⁇ , ⁇ , ⁇ -tris(4-hydroxyphenyl)-1-ethyl-4-isopropylbenzene is simply removed. Therefore, it is found that at the tune when voltage application is terminated in the above ⁇ e.>, the carbon nanotube array is free from m-CNTs.
  • the carbon nanotube array obtained in the above ⁇ f.> is useful as a FET from the result of the ON/OFF ratio of the FET.
  • ⁇ a.> to ⁇ g.> in Example 1 were performed except that instead of ⁇ d.
  • Formation of Layer made of PMMA> was used and instead of ⁇ f.
  • Removal of Layer Made of ⁇ , ⁇ , ⁇ -Tris(4-Hydroxyphenyl)-1-Ethyl-4-Isopropylbenzene>, ⁇ f′. Removal of Layer Made of PMMA> was used.
  • a 1 wt % anisole solution of PMMA was prepared.
  • the solution was applied to the carbon nanotube array having m-CNTs and s-CNTs by spin coating and then the solution was removed at 120° C.
  • a layer made of PMMA was formed on the carbon nanotube array having m-CNTs and s-CNTs.
  • the thickness of the layer was measured using a stylus type surface profiler (Dektak XT, manufactured by ULVAC, Inc.), it was confirmed that the thickness is 20 to 50 nm.
  • the layer made of PMMA on the substrate obtained in the above ⁇ e.> was removed with acetone.
  • the substrate obtained in the above ⁇ e.> was immersed in acetone for several minutes and rinsed with isopropanol and distilled water. Thereafter, the layer made of PMMA was removed by drying the substrate.
  • Example 2 From the results of the ON/OFF ratio measurement of the FET (10,000), SEM image observation, and AFM measurement (none of these are shown in the drawing), it was found that the carbon nanotube array obtained in Example 2 is free from m-CMTs similar to Example 1. In addition, it was found that the carbon nanotube array obtained in Example 2 was useful as a FET from the results of the ON/OFF ratio of the FET.

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