WO2004006337A1 - 半導体装置及びその製造方法 - Google Patents
半導体装置及びその製造方法 Download PDFInfo
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- WO2004006337A1 WO2004006337A1 PCT/JP2003/008403 JP0308403W WO2004006337A1 WO 2004006337 A1 WO2004006337 A1 WO 2004006337A1 JP 0308403 W JP0308403 W JP 0308403W WO 2004006337 A1 WO2004006337 A1 WO 2004006337A1
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- fine particles
- semiconductor device
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- organic
- semiconductor
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Classifications
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
- H10K85/60—Organic compounds having low molecular weight
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having potential barriers
- H10K10/40—Organic transistors
- H10K10/46—Field-effect transistors, e.g. organic thin-film transistors [OTFT]
- H10K10/462—Insulated gate field-effect transistors [IGFETs]
- H10K10/464—Lateral top-gate IGFETs comprising only a single gate
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having potential barriers
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- H10K10/462—Insulated gate field-effect transistors [IGFETs]
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- H10K10/46—Field-effect transistors, e.g. organic thin-film transistors [OTFT]
- H10K10/462—Insulated gate field-effect transistors [IGFETs]
- H10K10/484—Insulated gate field-effect transistors [IGFETs] characterised by the channel regions
- H10K10/488—Insulated gate field-effect transistors [IGFETs] characterised by the channel regions the channel region comprising a layer of composite material having interpenetrating or embedded materials, e.g. a mixture of donor and acceptor moieties, that form a bulk heterojunction
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- Y10S977/938—Field effect transistors, FETS, with nanowire- or nanotube-channel region
Definitions
- the present invention relates to a semiconductor device in which a conductive path is formed by fine particles made of a conductor or a semiconductor and organic semiconductor molecules, and a method of manufacturing the same.
- TFTs Thin film transistors
- LCDs Thin film transistors
- TFTs are Si-based inorganic semiconductor transistors using amorphous silicon (a-Si) or polycrystalline silicon (Poly-Si) as a semiconductor layer (channel layer).
- a-Si amorphous silicon
- Poly-Si polycrystalline silicon
- CVD plasma chemical vapor deposition
- organic semiconductor transistors using organic semiconductor materials have been actively developed because they can be manufactured by low-cost processes and can be formed on flexible substrates such as plastics that do not have heat resistance.
- the organic semiconductor materials that are being used are capable of producing TFTs at lower temperatures and at lower temperatures, such as spin coating and immersion.
- mobility a characteristic index of TFTs, is typically 1 be in 0- 3 ⁇ 1 cm 2 / V s is obtained (D. Dimi trakopoulos et al., Adv. Mater. (2002), 14, 99).
- ⁇ _ S i approximately 1 0 0 cm 2 / V s lower than in
- Display for TFT is the mobility of the number is a mobility cm / V s and P o 1 y- S i of The required mobility of 1 to 3 cmWs has not been reached, so improving mobility is a major challenge for organic semiconductor materials.
- the mobility of organic semiconductor materials is determined by intramolecular and intermolecular charge transfer.
- Intramolecular charge transfer is made possible by the delocalization of electrons to form a conjugated system.
- the transfer of charge between molecules is performed by bonding between molecules, conduction by overlapping of molecular orbitals by Van Der and Waalska, or hopping conduction through trap levels between molecules.
- SAMF ET Monolayer Field-Effect Transistor
- the gate length is determined by the thickness of the monomolecular film, so the gate length is very short at several nanometers, so that the withstand voltage between the source and the drain is reduced and the driving voltage may be increased.
- the substrate temperature must be cooled to 117 ° C to 130 ° C to form the electrode on the monolayer so that the monolayer is not broken, which increases the process cost. This method is impractical, as it may be soggy.
- a channel material using an organic-inorganic hybrid material has been proposed by International Business Machines (IBM) (see, for example, Japanese Patent Application Laid-Open No. 2000-26099). ).
- IBM International Business Machines
- the inorganic component and the organic component form a layered structure and utilize the high carrier mobility characteristics of the inorganic crystalline solid, while utilizing the function of the organic component to promote the self-organization of the inorganic material.
- a mobility of 1 to 100 cm 2 / Vs is expected, the mobility actually achieved is 0.25 cm 2 / Vs. This is generally higher than that of an organic semiconductor formed by spin coating, but is comparable to that of an organic semiconductor formed by vapor deposition or the like, and a mobility higher than a—Si is not obtained. .
- the present invention has been made in view of the above circumstances, and has as its object a semiconductor device in which a conductive path formed using organic semiconductor molecules as a material has a novel structure and exhibits high mobility. And a method for producing the same. Disclosure of the invention
- the present invention is configured such that a conductive path is formed by fine particles made of a conductor or a semiconductor and organic semiconductor molecules bonded to the fine particles, and the conductivity of the conductive path is controlled by an electric field.
- the present invention relates to a semiconductor device and a method for manufacturing the same.
- the conductive path in the fine particle and the conductive path along the molecular skeleton in the organic semiconductor molecule are connected.
- a network-type conductive path can be formed.
- the structure is such that the charge transfer in the conductive path occurs predominantly in the axial direction of the molecule along the main chain of the organic semiconductor molecule. Since the conductive path does not include the electron transfer between molecules, the mobility is not limited by the electron transfer between molecules, which is the cause of the low mobility of the conventional organic semiconductor. Therefore, the axial charge transfer in the organic semiconductor molecule can be maximally utilized. For example, a molecule having a conjugated system formed along the main chain When used as the organic semiconductor molecule, high mobility due to delocalized pit electrons can be used.
- the channel region forming the conductive path can be formed one layer at a time under normal pressure by a low-temperature process of 200 ° C. or less, a channel layer having a desired thickness can be easily formed.
- a semiconductor device can be manufactured at low cost on a flexible substrate such as a substrate.
- FIGS. 1A to 1C are views showing an example of the structure of a MIS type field effect transistor according to the first embodiment of the present invention.
- FIG. 1A is a schematic sectional view (FIG. 1A), and FIG. Fig. 1 (Fig. 1B) and image diagram of charge transfer (Fig. 1C).
- FIGS 2A to 2C are schematic cross-sectional views showing the structure of another MOS type field effect transistor.
- FIG. 3A to FIG. 3E are schematic cross-sectional views showing steps of manufacturing an MS type field effect transistor based on Embodiment 2 of the present invention.
- FIGS. 4A to 4D are schematic cross-sectional views showing steps of fabricating the same MOS-type field-effect transistor.
- FIG. 5 is a partially enlarged schematic cross-sectional view showing a structure of a MOS type field-effect transistor based on Embodiment 4 of the present invention.
- FIG. 6 is a transmission electron micrograph of the gold nanoparticles when dodecanethiol was used as a protective film for the gold nanoparticles.
- Fig. 7 is a transmission electron micrograph of the gold nanoparticles (Harima Chemical Co., Ltd.) when an organic molecule having an amino group at the terminal is used as the protective film for the gold nanoparticles.
- Fig. 8 shows the particle size distribution of gold nanoparticles measured and analyzed by small-angle X-ray scattering.
- Figure 9 is the same, in the organic semiconductor molecule and the gold scanning electron micrograph of S i 0 2 / S i substrate the conjugate is formed between the nanoparticles (Harima Chemicals, Inc.) of having an amino group at the end is there.
- FIG. 10 is a transmission electron micrograph when dodecanethiol and gold nanoparticles serving as the organic semiconductor molecules are clearly adhered on a MoS 2 substrate.
- FIG. 12A to FIG. 12B are conceptual diagrams when nanorods are used as the fine particles.
- FIG. 13 is a conceptual diagram when a nanorod is used as the fine particles.
- FIGS. 14A to 14B are partially enlarged schematic cross-sectional views showing a MOS type field-effect transistor according to the fifth embodiment of the present invention in comparison.
- FIG. 15 is a transmission electron micrograph of gold particles based on Embodiment 6 of the present invention applied on a SiO 2 / Si substrate and rinsed with toluene, and FIG. same, the gold fine particles onto coated on S i 0 2 ZS i substrate, further subjected to a surface treatment with AE AP TMS, is a transmission electron micrograph of the rinsed with toluene.
- FIGS. 17A to 17C are partially enlarged schematic cross-sectional views showing an example of a manufacturing process of a MOS-type field-effect transistor based on the embodiment of the present invention.
- FIG. 18 is a partially enlarged schematic cross-sectional view showing one example of a manufacturing process of the MOS field-effect transistor.
- Figure 19 shows the source-drain voltage of the field-effect transistor.
- Isd source-drain current
- FIG. 20 is a partially enlarged schematic cross-sectional view showing another example of the manufacturing process of the MOS field-effect transistor. BEST MODE FOR CARRYING OUT THE INVENTION
- the functional group at the terminal of the organic semiconductor molecule is chemically bonded to the fine particle, and the organic semiconductor molecule and the fine particle are alternately bonded to each other by the functional group at both ends of the organic semiconductor molecule. It is preferable that a network-type conductive path is formed in which the conductive path in the fine particles and the conductive path in the organic semiconductor molecule are connected two-dimensionally or three-dimensionally.
- an organic semiconductor transistor that can achieve an unprecedentedly high mobility comparable to a monolayer transistor can be provided.
- a channel region having the conductive path is formed, a source electrode and a drain electrode are provided on both sides of the channel region, a gate electrode is provided between these two electrodes, and an insulating gate (for example, MOS: Metal Oxide
- a semiconductor field-effect transistor may be formed.
- This structure can also operate as an optical sensor or the like by using a dye that absorbs light near the visible region as an organic semiconductor molecule having a conjugated system.
- the field effect transistor is preferably formed on a full substrate made of an organic material, and the gate insulating film on the gate electrode is preferably made of an organic material.
- the source and drain electrodes are preferably made of the same material as the fine particles.
- the conductive path is preferably formed by a single layer or a plurality of layers of a combination of the fine particles and the organic semiconductor molecules.
- a single layer of the conjugate is formed by performing the step of contacting the organic semiconductor molecules once after forming the layer of the fine particles, or this step is repeated twice or more.
- a plurality of layers are formed.
- the first layer of the fine particles is preferably formed on a base layer having good adhesion to the fine particles.
- the underlayer is preferably made of a silanol derivative, that is, a silane coupling agent.
- the underlayer can be used also as a gate insulating film on the gate electrode.
- the gate insulating film such as an oxide film by a costly and time-consuming process. Therefore, the configuration of the entire transistor becomes simpler, and the number of steps in the manufacturing process is reduced. Further, the thickness of the entire transistor can be reduced, and the gate insulating film composed of the underlayer can be manufactured by a manufacturing process using a solution, so that the cost of the device and the time required for the manufacturing are reduced. It becomes possible to reduce.
- the silane coupling agent has one end, such as an amino group or a thiol group, which reacts with the fine particles.
- One end such as an amino group or a thiol group, which reacts with the fine particles.
- Has functional groups It is important that the other end has an alkoxyl group which reacts with a hydroxyl group on the substrate.
- silane coupling agent examples include N-2 (aminoethyl) aminopropylmethyldimethoxysilane and N-2 (aminoethyl) aminopropyltrimethoxysilane (AEAPTMS; 1))), N-2 (aminoethyl) r-aminopropyltriethoxysilane, 3-aminopropyltrimethoxysilane (AP TMS, structural formula (2) below), 3-aminobutyrylmethylpytoxysilane (APM DES, the following structural formula (3)), 3-aminopropyltriethoxysilane.
- MPMDMS 3—Mercaptopropy
- silane coupling agent only needs to be capable of chemically bonding to both the substrate provided with the gate electrode and the fine particles, and it is considered that a dithiol-based substance having thiol groups at both ends may be used.
- decanedithiol HS one C 10 H 20 - SH
- the like decanedithiol
- the basic structure of the silane coupling agent has a quasi-one-dimensional-like structure in which most of the silane coupling agent can define the main chain, but is not limited thereto, and a two-dimensional or three-dimensional-like molecule is used.
- the fine particles The element parts to be connected may be connected to each of the children. However, at that time, the characteristics of the transistor formed by the network structure composed of the fine particles should not be deteriorated or destroyed.
- the silane coupling agent when the underlayer is used also as the gate insulating film, the silane coupling agent must have poor electric conductivity. Therefore, there is no problem if the main chain of the silane coupling agent is an alkyl chain, but it is difficult to use a conjugated chain considered to have good conductivity for the purpose of the present invention.
- a nucleic acid (DNA) or the like can be used.
- the fine particles are preferably fine particles made of gold, silver, platinum, copper, or aluminum as the conductor, or cadmium sulfide, selenide dome, or silicon as the semiconductor. Also, the particle size is preferably 10 nm or less.
- the shape of the fine particles may be a sphere, but the present invention is not limited to this.
- a triangle, a cube, a cuboid, a cone, or the like may be used.
- the fine particles are nanorods (or nanofibers) having an anisotropic shape in a one-dimensional direction and having a minor axis of 10 nm or less (Ser-Sing Chang, Chao-Wen Shih, Cheng-Dah Chen, Wei-Cheng Lai , and CR Chris Wang,. "The Shape Transition of Gold Nanorods Langmoir (1999), 15, 701-709.) or a nanotube.
- the distance between the source and drain electrodes described above. is preferably shorter than the major axis of the nanopad.
- the organic semiconductor molecule is an organic semiconductor molecule having a conjugated bond, and a thiol group (—SH), an amino group (_NH 2 ), an isocyano group (—NC), and a thioacetoxyl group (one SC It is preferably a molecule having (CH 3 ) or a carboxyl group (_C ⁇ OH).
- dendrimers represented by the following structural formula (17) can also be used as the organic semiconductor molecules.
- Embodiment 1 MOS type field effect transistor
- FIGS. 1A to 1C are diagrams illustrating a MOS field-effect transistor according to the first embodiment.
- FIG. 1A is a schematic cross-sectional view (FIG. 1A), FIG. It is an image diagram of charge transfer (Fig. 1C).
- Fig. 1A shows one of the device structures of a MOS field-effect transistor commonly used as a TFT.
- the gate electrode 2, gate insulating film 3, and source electrode 4 are formed on a substrate 1 by a known technique.
- the drain electrode 5 is formed first, and a channel composed of a combination of the fine particles 8 and the organic semiconductor molecules 9 is formed thereon.
- the metal layer 6 Here, illustration and description of a molecular solder layer (the underlayer) described later are omitted.
- a plastic substrate such as polyimide-polypropylene or polyethylene terephthalate (PET), glass, quartz, or a silicon substrate is used.
- PET polyethylene terephthalate
- a flexible semiconductor device such as a display having a curved shape can be manufactured.
- the transistors formed on the substrate 1 may be used as a monolithic integrated circuit in which a large number of transistors are integrated with the substrate 1 as in the case of application as a display device, or each transistor may be cut and individualized. It may be used as a discrete component.
- Examples of the material for the gate electrode 2 include conductive polymers, conductive materials such as gold (Au), platinum (Pt), aluminum (A1), nickel (Ni), titanium (Ti), and polysilicon. A substance or a combination thereof can be used.
- the gate insulating ⁇ 3 As a material of the gate insulating ⁇ 3, for example, polymethyl methacrylate (PMMA), spin-on-glass (S OG), oxide Kei element (S i 0 2). Nitride Kei element (S i 3 N 4), a metal oxide high dielectric An insulating film or the like or a combination thereof can be used.
- PMMA polymethyl methacrylate
- S OG spin-on-glass
- oxide Kei element S i 0 2
- Nitride Kei element S i 3 N 4
- a metal oxide high dielectric An insulating film or the like or a combination thereof can be used.
- Examples of the material of the source electrode 4 and the drain electrode 5 include gold (Au), palladium (Pd), platinum (Pt), chromium (Cr), nickel (Ni), and conductive polymer. A conductive substance or a combination thereof can be used.
- the processing temperature in the manufacturing process can be suppressed to 200 ° C. or less, so that all of the above materials can be composed of organic compounds.
- the channel layer 6 is formed of a combined body in which fine particles 8 and organic semiconductor molecules 9 are combined in a network, and the carrier movement is controlled by the gate voltage of the gate electrode 2.
- the fine particles 8 are fine particles having a particle diameter of 1 O nm or less.
- the material include conductors such as gold (Au), silver (Ag), and platinum (Pt), and cadmium sulfide (CdS ), Cadmium selenide (CdSe), and silicon (Si).
- the organic semiconductor molecule 9 is an organic semiconductor molecule having a conjugated bond in the molecular skeleton, and a functional group capable of chemically bonding to the microparticle 8 at an end of the molecule, for example, a thiol group (—SH), an amino group (_NH 2 ), An isocyano group (—NC), a thioacetoxyl group (—SCOCH 3 ), a cycoxyl group (—COOH), or the like.
- a thiol group, an amino group, an isocyano group, and a thioacetoxyl group are functional groups that bind to conductive fine particles such as Au, and a force-sipoxyl group is a functional group that binds to semiconductor fine particles.
- organic semiconductor molecule 9 for example, 4,4′-biphenyldithiol of the following structural formula (12), 4,4′-diisocyanobiphenyl of the following structural formula (13), 4,4'-Diisocyano-p-terphenyl in the structural formula (14), 2,5-bis (5'-thioacetoxyl 2'-thiophenyl) thiophene in the following structural formula (15), 1 4) 4, 4'-diisocyanophenyl or Bovin Serum
- a dendrimer represented by the following structural formula (17) can be used as the organic semiconductor molecule 9.
- the fine particles 8 are two-dimensionally or three-dimensionally linked by the organic semiconductor molecules 9, and the conductive paths in the fine particles 8 and the conductive paths along the molecular skeleton in the organic semiconductor molecules 9 are connected.
- a network-type conductive path is formed.
- the above-mentioned conductive path does not include the electron transfer between molecules, which caused the low mobility of the conventional organic semiconductor, and furthermore, High mobility is expected because intramolecular electron transfer is performed through a conjugated system formed along the molecular skeleton.
- Electron conduction in the channel layer 6 is performed through a network-type conductive path 10 as shown in FIG. 1C, and the conductivity of the channel layer 6 is controlled by a voltage applied to the gate electrode 2. You.
- a molecular solder layer (not shown) is provided as the base layer, which serves as an adhesive for fixing the fine particles 8 by one layer.
- a silane-based compound that uses a molecule having a functional group that can chemically bond to both the substrate provided with the gate electrode and the fine particles is used.
- ATMS (3-aminopropyl) trimethoxysilane
- the organic semiconductor molecules 9 are brought into contact with the fine particles 8 to form a conjugate of the fine particles 8 and the organic semiconductor molecules 9, thereby forming a conjugate. Is formed for one layer. Since the channel layer 6 is thus formed one layer at a time, the channel layer 6 having a desired thickness can be formed by repeating this step several times.
- the channel layer 6 may be a single layer, but is usually two or more layers, preferably about 10 layers.
- the thickness of one layer is not much different from the particle size (several nm) of the fine particles 8. Assuming that the fine particles 8 are made of gold and have a particle size of about 1 O nm and that 10 layers are laminated, the thickness of the channel layer 6 is approximately 100 nm. Therefore, it is preferable that the thickness of the source electrode 4 and the drain electrode 5 is 100 nm or more. Since the channel layer 6 is independently formed one layer at a time, the material constituting the fine particles 8, the particle diameter of the fine particles 8, or the organic semiconductor molecules 9 is changed for each of the binder layers or for each of the plurality of binder layers. Alternatively, the characteristics of the channel layer may be controlled.
- the channel layer 6 may be formed first, and the source electrode 4 and the drain electrode 5 may be formed thereon by vapor deposition or the like.
- the structure is, for example, the top gate type shown in FIG. 2 Bottom gate type shown in Fig. B.
- the dual gate type shown in FIG. 2C can be used, in which case the conductivity of the channel layer 6 can be more effectively controlled.
- Embodiment 2 Fabrication of MOS transistor
- a gate electrode 2, a gate insulating film 3, a source electrode 4, and a drain electrode 5 are formed on a substrate 1 by using a known method.
- a plastic substrate such as polyimide-polycarbonate, glass, quartz, or a silicon substrate is used.
- gold (Au) is vapor-deposited while masking other portions to form a gate electrode 2.
- a material of the gate electrode 2 besides gold (Au), for example, conductive polymer, platinum (Pt), aluminum (A 1), nickel Conductive materials such as metal (N i) and titanium (T i) or a combination thereof can be used, and are formed by a lift-off method, a shadow mask method, a screen printing method, an ink jet printing method, or the like.
- the gate insulating film 3 is formed by a spin coating method, a sputtering method, an immersion method, a casting method, or the like.
- a material of the gate insulating film 3 for example, polymethyl methacrylate (PMMA), Supin'ongara scan (S OG), oxide Kei element (S i 0 2), nitride Kei element (S i 3 N 4), metallic oxide A high dielectric insulating film or the like, or a combination thereof can be used.
- a source electrode 4 and a drain electrode 5 are formed on the gate insulating film 3 by evaporating gold (Au) while masking other portions.
- Au gold
- a channel layer 6 composed of fine particles 8 and organic semiconductor molecules 9 connected to each other in a three-dimensional network structure is formed.
- the surface of the region where the channel layer 6 is to be formed is immersed in a solution of (3-aminopropyl) trimethoxysilane (APTMS) in toluene or hexane having a volume concentration of several percent, and then washed with toluene or hexane. Clean and replace the solution, then evaporate the solvent, and only one layer of gold microparticles 8 A molecular solder layer 7 as the underlayer to be fixed is formed.
- APTMS (3-aminopropyl) trimethoxysilane
- the substrate 1 on which the molecular solder layer 7 is formed is immersed in a dispersion liquid (concentration: several mM) in which the gold fine particles 8 are dispersed in a solvent such as toluene-chloroform for several minutes to several hours, and then the solvent is evaporated. .
- a dispersion liquid concentration: several mM
- the gold fine particles 8 are fixed on the surface of the molecular solder layer 7, and the gold fine particle layer 8 a including the gold fine particles 8 is formed on the molecular solder layer 7.
- the molecular solder layer 7 has a functional group such as an amino group capable of chemically bonding to the gold microparticles 8, and only one layer of the gold microparticle layer 8a bonded to this functional group is formed on the molecular solder layer 7. Fixed. Excess gold particles 8 not fixed to the molecular solder layer 7 are washed away.
- the substrate 1 is immersed in a solution of 4,4'-biphenyldithiol, which is an organic semiconductor molecule 9, dissolved in toluene at a molar concentration of several mM or less, washed with toluene to replace the solution, and then the solvent is removed. Is evaporated.
- 4,4′-biphenyldithiol binds to the surface of the fine gold particles 8 through the reaction of the thiol group at the end of the molecule.
- a large number of 4,4 ′ biphenyldithiol molecules bind to the surface of one gold particle 8 so as to surround the gold particle 8.
- the substrate 1 is immersed in a dispersion liquid in which the gold fine particles 8 are dispersed in a solvent such as toluene or chloroform for several minutes to several hours in the same manner as in Step 5, and then the solvent is evaporated.
- the gold fine particles 8 are bonded and fixed to the surface of the first combined body layer 6a, and the second gold fine particle layer 8b is formed.
- the second layer of gold particles 8 is connected to the first layer of gold particles 8 by 4,4'-biphenyldithiol, and the first layer of gold particles 8 connected to the same second layer of gold particles 8
- the fine particles 8 are connected indirectly via the second-layer gold fine particles 8, and the connection becomes three-dimensional.
- the substrate 1 is immersed in a solution of 4, 4'-biphenyldithiol in toluene having a molar concentration of several mM or less, as in step 6, and then washed with toluene to remove the solution. Substitute and then evaporate the solvent, as in step 6, a number of 4,4'-biphenyldithiols are bound to enclose the gold microparticles 8, and by the 4,4, -biphenyldithiol molecules The second combined layer 6b to which the gold fine particles 8 are connected is formed.
- Steps 7 and 8 it is possible to form a channel layer in which three-dimensional network-type conductive paths are formed one by one.
- a channel layer 6 having a desired thickness can be formed (M. D. Musick et al., Chem. Mater.
- each composite layer is formed of the same material, but each composite layer or a plurality of composite layers is formed.
- the characteristics of the channel layer may be controlled by changing the material constituting the fine particles 8, the particle diameter of the fine particles 8, or the organic semiconductor molecules 9.
- the channel layer 6 is also formed above the electrode 4 and the drain electrode 5, the channel layer 6 may be formed only in the concave portion sandwiched between both electrodes.
- only the channel layer may be separately formed in advance, and this may be adhered to the substrate 1 and the gate insulating film 3 to produce a field effect transistor having the structure shown in FIG. 2A or 2B. .
- nanoparticles such as gold are used as the fine particles.How to regularly adhere the fine particles on a substrate and bridge with the organic semiconductor molecules having a certain length is important.
- Nanometer-sized particles are clusters of hundreds to thousands of metal atoms, and are actually polyhedral, but generally approximate to spherical. Nanoparticles have different diameter distribution widths depending on the raw materials. Narrow distribution width means, in other words, that the diameters of the particles are well-aligned. If this is used to construct a two-dimensional network, it will be neatly close-packed. Conversely, if the particle diameters are not uniform, it is difficult to form a regular two-dimensional network.
- the following shows how the variation in the diameter of gold nanoparticles affects the binding of particles on a substrate.
- FIG. 5 is a schematic view of an organic semiconductor transistor as a semiconductor device according to the present invention.
- a space where a gate insulating film 3 between a source electrode 4 and a drain electrode 5 having a macro size is evident.
- nanoparticles for example, gold fine particles 8
- organic semiconductor molecules 9 are bonded to the nanoparticles.
- the surface of the nanoparticles is coated with a protective film made of chain insulating organic molecules, the nanoparticles do not aggregate.
- the insulating organic molecule is bonded to a metal cluster (the nanoparticle) corresponding to a core portion, and the magnitude of the bonding force greatly affects the final diameter distribution when the nanoparticle is synthesized. are doing.
- One end of the insulating organic molecule has a functional group that chemically reacts (bonds) with the nanoparticles.
- the functional group can be exemplified thiol group (one SH), mention may be made of dodecanethiol (C 12 H 25 SH) in one molecule with a thiol group at the end. If the thiols group is bonded to the nanoparticle such as gold, is a hydrogen atom C 12 H 25 S out - is said to be A u.
- FIG. 6 is a transmission electron micrograph of gold nanoparticles actually synthesized using dodecanethiol as the protective film. As can be seen from Fig. 6, the size of the gold nanoparticles is very uniform. (Note that the preparation of gold nanoparticles using the insulating organic molecule having a thiol group as the protective film is described in the literature Mathias Brnst, et al., J. Chem. Soc., Chem. Commun., 801 (1994) See).)
- FIG. 7 is a transmission electron micrograph of gold nanoparticles actually synthesized using the insulating organic molecule having the amino group as a terminal functional group as the protective film. As is clear from FIG. 7, the size of the gold nanoparticles is larger than that of the thiol group in FIG. (For the preparation of gold nanoparticles using the insulating organic molecule having an amino group as the protective film, refer to literature Daniel V. Leff, et al., Langmuir 12, 4723 (1996).)
- the bond of the “thiol group” is stronger than that of the “amino group”.
- the insulating organic molecule having an amino group as the protective film to synthesize gold nanoparticles, a general tendency is considered. Due to the weakness of the “amino group-gold” bond, the insulating organic molecules may aggregate with other nanoparticles (gold atoms) before completely encapsulating the nanoparticles (gold atoms). As a result, it is considered that particles having a large particle diameter are easily formed.
- an amino group there are quite a few that appear to be bonded to each other even after the nanoparticles are wrapped in the protective film. Fig.
- FIG. 8 shows the results of measurement and analysis of the size distribution of gold nanoparticles synthesized using the above-mentioned insulative organic molecules having a thiol group or an amino group by small-angle X-ray scattering (transmission type). .
- the diameter of the gold nanoparticles protected by the thiol group is smaller than that of the amino group, and that the degree of distribution of the diameter is also smaller. This result seems to be a good reflection of what was seen in Figures 6 and 7.
- FIG. 9 is a scanning electron micrograph of a case where a single layer of gold nanoparticles having the protective film made of the insulating organic molecule having an amino group on the surface is attached to a substrate.
- the gold nanoparticle deposition process has not been optimized, but focusing on the clogged particles, it is more likely that particles of irregular size will be densely arranged rather than regularly arranged. Have been.
- FIG. 10 shows a case where a single layer of gold nanoparticles having a very uniform particle size and having the protective film made of the insulating organic molecule having a thiol group on the surface is attached to the substrate.
- This is a transmission electron micrograph (this transmission electron micrograph is based on a study by Professor Andres of Purdue University, USA).
- nanorods such as gold having a more one-dimensional shape are used as the fine particles instead of the nanoparticles having a pseudo zero-dimensional shape.
- the size major axis / minor axis
- the minor diameters vary, when one nanorod is focused on, even if minor diameters vary between the nanorods, it is easy to align them in parallel when arranging them.
- a transistor can be formed by bridging the nanorods with the organic semiconductor molecules in the same manner as described above.
- Using one organic semiconductor molecule means that a certain length is required between nanorods (or nanoparticles), and it is easy to understand that the regular arrangement of rods (particles) is very important. I understand.
- the synthesis of the nano-adhesive itself has been carried out so far, starting from a small one with a short diameter of just under 10 nm, to a long diameter of several tens of nm, and a long one to 500 nm. It has been synthesized to a submicron size that exceeds. In addition, the aspect ratio is close to 20 and it is possible to synthesize a very one-dimensional rod (see Ser-Sing Chang, et al., Langmuir 15, 701 (1999), Hiroshi Yao, et al. Chemistry Letters, 458 (2002).).
- an ammonium bromide-based molecule typified by cetyl trimethyl ammonium bromide is used as a protective film thereof.
- a protective film here is a general “surfactant”.
- cetyl / trimethylammonium bromide is a “cationic surfactant”
- anionic bromine will face nanorods such as gold. That is, there is no precedent that the nanorod of gold or the like is bonded to the substrate with the nanohead of t- gold or the like formed in a surfactant micelle.
- Fig. 11 is a transmission electron micrograph (Ser-Sing Chang, et al., Langmuir 15, 701 (1999)) ⁇ The ratio of gold nanorods in Fig. 11 Is 6: 1 with a minor axis of 10.6 nm and a major axis of 62.6 nm.
- the nanorods can be used as the fine particles instead of the nanoparticles in the preparation of the organic semiconductor transistor.
- the path for optimizing the process of bonding the nanorods to the substrate is also expected to be less rugged than for the nanoparticles ⁇ in this case, the source and drain electrodes in a transistor structure It is preferable that the distance between them is shorter than the major axis of the nanorod.
- a substrate in which parallel electrodes (source and drain electrodes) are formed in advance so that the distance between the electrodes is shorter than the major axis of the nanorod is immersed in the nanorod solution, and the nanorod is bonded to the substrate.
- the nanorod can enter the gate insulating film between the parallel electrodes only when the nanorod is positioned parallel to the electrode.
- FIG. 12A shows that the distance between the source electrode 4 and the drain electrode 5 in the transistor structure is shorter than the major diameter of the nanorod 14,
- FIG. 4 is a conceptual diagram when 4 forms a large angle with respect to electrodes 4 and 5.
- an external stimulus for example, the substrate of the nanorod solution is shaken while the substrate is immersed in the nanorod solution
- the nanorod 14 changes its angle
- FIG. 12B it is considered that the nanorod 14 fits between the electrodes 4.5.
- the nanorods 14 that do not fit between the electrodes 4 and 5 even when the external stimulus is applied can be removed by removing the substrate from the nanorod solution and rinsing with a solvent or the like.
- Nanorods 14 may be formed.
- FIG. 13 is a conceptual diagram when a plurality of nanorods 14 are arranged in parallel between the electrodes 4 and 5 using the one-dimensionality of the nanorods 14.
- the organic semiconductor molecules are bonded to the nanorods 14 to form a channel layer in the same manner as described above, thereby forming a transistor.
- the channel layer may be a single layer, but is usually preferably at least two layers and about ten layers.
- the thickness of one layer is not much different from the minor axis (10 nm or less) of the nanorod. Assuming that the fine particles are nanorods made of gold and have a particle size of about 10 nm and that 10 layers are laminated, the thickness of the channel layer is approximately 100 nm. Therefore, it is preferable that the thickness of the source electrode and the drain electrode is 100 nm or more.
- the channel layer is made of a material including the organic semiconductor molecules and the fine particles.
- the organic semiconductor molecule has a group capable of chemically bonding to the fine particles at the end. Then, a structure is formed in which the organic semiconductor molecules and the fine particles are alternately bonded to form a network.
- a material formed as a network with the organic semiconductor molecules and the fine particles is used as a channel material,
- a gate insulating film used a conventional silicon transistors where the groups are silicon oxide (S i 0 2).
- a thermal oxidation method for treating a silicon substrate at a high temperature is usually used.
- organic transistors which use semiconductor organic materials for the channel layer, which has recently attracted attention
- the production process using solutions that make use of the characteristics of organic materials is promising from an industrial point of view.
- Conventional silicon transistors require vacuum, high temperature, lithography, etc. in their processes, and are extremely time consuming, energy and cost intensive.
- the development of smaller structures requires more investment than before, and the rate of increase is exponential. Is said to be.
- the technology for fabricating transistors using a solution-based manufacturing process is attracting attention.
- Specific method Examples of the method include immersing the substrate in a solution, applying the solution to the substrate with a spot, and thinning it with a spin coater, etc., and forming a thin film using a printing technique such as an inkjet printer. No.
- a printing technique such as an inkjet printer.
- the substrate, the electrodes, the insulating layer, and the semiconductor channel layer could be formed of organic materials.
- organic transistor the majority are mostly obtained by replacing only the channel layer Trang Soo evening with organic (that is, the gate insulating film S I_ ⁇ 2, the substrate is silicon
- conventional film forming methods do not make use of the characteristics of organic substances, for example, a conventional vacuum deposition method is used.
- the underlayer having good adhesion to the fine particles having good adhesion to the fine particles
- a layer of the fine particles is formed on (the above-described molecular solder layer), and a silanol derivative, specifically, a silane coupling agent is used as the underlayer.
- the underlayer can be used not only for fixing the fine particles constituting the channel layer of the transistor but also as a gate insulating film.
- a gate insulating film 3 is formed on a substrate 1 such as silicon as shown in FIG.
- a molecular solder layer (the underlayer) 7 for promoting adhesion is formed on the gate insulating film 3.
- a molecular solder layer made of a silane coupling agent A layer 7 is formed, and a channel layer 6 is formed on the molecular solder layer 7.
- the molecular solder layer 7 is chemically bonded to the substrate 1 and the channel layer 6 on both sides thereof. That is, the silane coupling agent forming the molecular solder layer 7 has, on the channel layer 6 side, a functional group such as an amino group or a thiol group that reacts with the fine particles (for example, gold). On one side, there are appropriate functional groups corresponding to the materials constituting the substrate 1 and the gate electrode (not shown).
- the gate insulating film such as an oxide film by a costly and time-consuming process. Therefore, the configuration of the entire transistor becomes simpler, and the number of steps in the manufacturing process is reduced. In addition, the thickness of the entire transistor can be reduced, and the gate insulating film composed of the molecular solder layer 7 can be manufactured by a manufacturing process using a solution. Time can be reduced.
- silane coupling agent examples include N-2 (aminoethyl) aminopropylmethyldimethoxysilane, N-2 (aminoethyl) aminopropyltrimethoxysilane (AEAPTMS, and the following structural formula ( 1)), N-2 (aminoethyl) aminopropyltriethoxysilane, 3-aminopropyltrimethoxysilane (APTMS, structural formula (2) below), 3-aminobutyrylmethylpytoxysilane (APM DE S, Structural formula (3) below), 3-Aminobutylpyrutriethoxysilane-N-phenyl-3-aminopropyltrimethoxysilane, 3-mercaptopropyltrimethoxysilane (MPTMS, Structural formula (4) ), 3-Mercaptopropylmethyldimethoxysilane (MPMDMS, structural formula (5) below), Mercaptomethyldimethylethoxysilane (MMDMES), Mer
- the molecular solder layer only needs to be capable of chemically bonding to both the substrate provided with the gate electrode and the fine particles, and it is considered that a dithiol-based material having thiol groups at both ends may be used.
- a dithiol-based material having thiol groups at both ends may be used.
- deca Njichioru HS - C I 0 H 20 - SH
- the basic structure of the silane coupling agent has a quasi-one-dimensional-like structure in which most of the silane coupling agent can define the main chain, but is not limited thereto, and a two-dimensional or three-dimensional-like molecule is used. In this case, it is only necessary that the gate electrode (or the substrate) and the element portion to be bonded to each of the fine particles be properly bonded. However, at this time, the characteristics of the transistor formed by the network structure composed of the fine particles should not be deteriorated or destroyed. When the underlayer is also used as the gate insulating film, the silane coupling agent Must have poor electrical conductivity.
- the main chain of the silane coupling agent is an alkyl chain, but it is difficult to use a conjugated chain considered to have good conductivity for the purpose of the present invention.
- a nucleic acid (DNA) or the like can be used.
- substrate a molecular solder layer composed of a silane coupling agent (underlayer) —one channel layer
- underlayer a silane coupling agent
- a single layer of tetradecyl-1-enyltrichlorosilane, a silane coupling agent is formed on a substrate, and the vinyl group at the top is oxidized.
- another organic monolayer film (vurt conjugate system) that reacts with —C ⁇ H is formed.
- the silane coupling agent is a non-conjugated (parasitic) system
- a single-layer film of a sigma-based silane coupling agent-a 7 ⁇ -based single-layer film can be formed here. However, they did not fabricate the transistor as in this embodiment, but only investigated the anisotropic conduction of the thin film configured as described above.
- the present invention is directed to a channel layer of a transistor, in which a portion where carriers actually flow and which is a source of transistor operation is a conjugated molecule bridging the fine particles (the organic semiconductor molecule). It is.
- the present embodiment has a configuration of “substrate one-molecule solder layer (base layer) one channel layer”, but the silane coupling agent constituting the molecular solder layer binds to (gold) particles in the channel layer. However, it does not necessarily bind to the semiconductor conjugated molecule (the organic semiconductor molecule) bridging the fine particles.
- the first 5 figures gold particles coated on S i 0 2 / S i (substrate native oxide film S i 0 2 is formed on the S i surface of the substrate) the substrate, then the substrate surface with preparative Ruen It is a transmission electron microscope photograph at the time of washing.
- a white dot gold particles, background is S i 0 2 ZS i substrates.
- the fine particles are only physically weakly adsorbed to the substrate, it can be seen that most of the fine particles are removed after washing with toluene.
- FIG. 16 shows that AE APTMS (N- 2) as the silane coupling agent was placed on a Si 0 2 / Si substrate (a substrate having a native oxide film Si 0 2 formed on the surface of the Si substrate).
- FIG. 4 is a transmission electron micrograph of a thin film of (aminoethyl) aminopropyltrimethoxysilane) formed, gold fine particles are further applied on the thin film, and the substrate surface is washed with toluene.
- the white dots are gold particles
- the background is the S i ⁇ 2 / S i substrate.
- AEAPTMS first reacts with an alkoxyl group on the substrate (however, the surface is cleaned beforehand and the hydroxyl groups fill the surface).
- AEAPTMS having a chain shape has an amino group at an end other than the substrate side, and binds to the fine particles such as gold. Thereby, the substrate and the fine particles can be chemically bonded via AEAPTMS, and the bond is not broken only by washing with toluene.
- the layer made of the silane coupling agent is used as it is as the gate insulating layer, so that a conventional gate insulating film such as silicon oxide is not required. Therefore, the transistor can be made thinner as a whole. It also satisfies the desire to replace more components with organic materials in organic transistors, If all the components of an organic transistor are made of organic materials, the cost and time required for the production will be very small. For example, according to a report from the Philips research institute in the Netherlands, they have succeeded in fabricating all of the transistors, not only the channel layer but also the electrodes and the gate insulating film, with organic materials (polymers). See M. Matters, et a., Optical Materials, vol.
- Examples of reported materials include polyimide and polyethylene terephthalate (PET) for the substrate, polyaniline for the electrodes, and photoresist and polyvinylphenol (PVP) for the gate insulating film.
- PET polyethylene terephthalate
- PVP polyvinylphenol
- the terminal functional groups of the silane coupling agent that chemically bond to the fine particles serving as the base are regularly arranged.
- a solvent eg, hexane
- the insulating film When a thin film layer made of a silane coupling agent is also used as a gate insulating film, the insulating film must be adjacent to the gate electrode, so it is convenient if the gate electrode is also a substrate at the same time.
- the most typical practical example is a doped silicon substrate (note that the surface of the silicon substrate usually has a very thin native oxide film, without the need for additional time and money in a separate process). ing) . It is in a low resistance state because of its doping and can be used as a (gate) electrode.
- This substrate is immersed in a high-temperature (for example, 60 to 110 ° C) heated piranha solution (a mixture of sulfuric acid and an aqueous solution of hydrogen peroxide (30%) mixed at a volume ratio of 3: 1). (Typically immersed for 20 minutes or more), thereby removing the organic impurities adhering to the surface and simultaneously hydroxylating the substrate surface.
- a high-temperature for example, 60 to 110 ° C
- heated piranha solution a mixture of sulfuric acid and an aqueous solution of hydrogen peroxide (30%) mixed at a volume ratio of 3: 1.
- the treatment with an oxygen plasma asher device can also effectively obtain the same effect.
- an ordinary alkoxyl-terminated silane-based printing agent is suitable for this substrate.
- the fine particles preferably have a particle diameter of 10 nm or less as described above. It is known that fine particles having a size on the order of nanometers can be synthesized relatively easily chemically. Nanoparticles are not thermally stable because they aggregate by themselves. For this reason, each nanoparticle must be protected with a chain organic molecule having a thiol group or an amino group at one end. However, the chain organic molecule is different from the silane coupling agent, and the other end is terminated with, for example, a methyl group. When the other end facing the fine particles of gold or the like is also a thiol group, the nanoparticles are considered to be easily aggregated.
- the semiconductor device is configured such that the conductive path is formed by the fine particles made of a conductor or a semiconductor and the organic semiconductor molecules chemically bonded to the fine particles, and the conductivity of the conductive path is controlled by an electric field.
- the conductive path is formed by the fine particles made of a conductor or a semiconductor and the organic semiconductor molecules chemically bonded to the fine particles, and the conductivity of the conductive path is controlled by an electric field.
- the surface of the substrate is modified so that the silane coupling agent can be easily bonded.
- it is effective to hydroxylate the surface of the substrate by immersing the substrate in a Piranha solution composed of sulfuric acid and hydrogen peroxide solution, or by irradiating the substrate surface with oxygen plasma or ozone.
- a Piranha solution composed of sulfuric acid and hydrogen peroxide solution
- oxygen plasma or ozone oxygen plasma or ozone.
- the substrate surface is modified by irradiation with oxygen plasma or ozone. Good to qualify.
- a silane coupling agent is attached to the surface of the substrate whose surface has been hydroxylated as described above to form a thin film made of a silane coupling agent.
- a silane coupling agent is a substance consisting of gayne (S i) and an organic substance, and generally has two types of functional groups having different reactivities. It has such a hydrolyzability and easily reacts with inorganic substances, and the other functional group easily reacts with organic substances such as thiol group (-1 SH) and amino group (-1 NH 2 ).
- the reactive group (1-SiOR) chemically bonded to the fine particles in the silane coupling agent is silanolized (1-SiOH) by hydrolysis with water, and is partially dehydrated and condensed to form an oligomer. I have. At this time, the water may be from the atmosphere or may be intentionally dissolved in the water. This silanol group and the hydroxyl group on the surface of the substrate are easily adsorbed by hydrogen bonding, so that the silane coupling agent can be attached to the substrate.
- the silane coupling agent can be attached to the substrate surface by immersing the substrate in a solution obtained by diluting the silane coupling agent with an appropriate solvent.
- a method using steam as a completely different method from immersion. For example, a diluted solution of a silane coupling agent or a stock solution of a silane coupling agent is placed in a closed container, a substrate is placed in the container, and the diluted solution of the silane coupling agent or a stock solution of the silane coupling agent is vaporized.
- a silane coupling agent can be attached to the substrate surface.
- dehydration condensation for strengthening the bond between the substrate surface and the surface of the thin film made of the silane coupling agent and dehydration condensation for strengthening the bond between molecules in the thin film are performed.
- the dehydration condensation can accelerate the dehydration condensation reaction by heating the substrate to a high temperature (see Shin-Etsu Chemical Co., Ltd., "Silane Coupling Agent, 1 (2002) J)."
- This dehydration-condensation reaction may be carried out after the step of removing the silane coupling agent adhering to the substrate surface, which will be described later, in any order.
- the dehydration condensation can be performed, for example, by warming the substrate from the back side to 10 ° C. or more with a hot plate or the like.
- a process of making the thickness of the thin film made of the silane coupling agent on the substrate uniform by an external force is performed. It is considered that the more uniform the thickness of the thin film, the more uniform the thickness of the channel layer produced through the subsequent steps, and hence the smaller the scattering of electrons passing through the channel layer. As a result, the current value that can flow as a semiconductor device can be further increased, which leads to an improvement in characteristics.
- the silane coupling agent that has excessively adhered to the substrate surface is removed.
- the above-mentioned silane coupling agent that is excessively attached is not a covalent bond or a hydrogen bond on the surface of the substrate but a silane coupling agent that has a van der Waals bond or is on the surface of the substrate.
- Point. for example, by immersing the substrate in hexane and performing ultrasonic cleaning, molecules weakly bonded to the substrate, that is, a silane coupling agent that has not been dehydrated and condensed can be removed. Ultrasonic cleaning allows weakly bound molecules to dissolve into the hexane and be removed.
- the fine particles made of a conductor or a semiconductor are chemically bonded to a thin film made of a silane coupling agent. Further, the fine particles not chemically bonded to the thin film made of the silane coupling agent may be removed.
- the fine particles are generally used in a dispersed (colloidal) state in a suitable solvent. After the solvent is dried, the fine particles that are not chemically bonded to the silane coupling agent are rinsed with a separately prepared solvent. , Get rid of.
- the fine particles that have already been bonded to the thin film made of the silane coupling agent are bonded to the organic semiconductor molecules having conductivity, and the fine particles are crosslinked by the organic semiconductor molecules.
- the organic semiconductor molecules that are not chemically bonded to the fine particles are removed. In the case where the organic semiconductor molecules are dissolved in a liquid and bound to the liquid, excess organic semiconductor molecules can be removed by drying the solvent used.
- the conductive path is formed by the fine particles made of a conductor or a semiconductor and the organic semiconductor molecule chemically bonded to the fine particles, and the conductivity of the conductive path is controlled by an electric field.
- a field-effect transistor which is a semiconductor device manufactured in this way, can be manufactured.
- FIGS. 3A to 3C a silicon dioxide as a gate insulating film is formed by thermal oxidation on a silicon substrate on which a gate electrode is formed and doped, and then the gate is formed. Titanium was placed on the insulating film, and electrodes corresponding to the source electrode and the drain electrode were formed therefrom using gold.
- a base Such a structure in which the electrode and the gate insulating film are formed on the substrate.
- FIGS. 17A to 17C and FIG. 18, show the electrodes and the electrodes on the substrate as shown in FIGS. 3A to 3C.
- FIG. 4 is a partially enlarged cross-sectional view for describing a surface state between a source and a drain electrode after performing a step of forming a gate oxide film.
- the surface of the substrate 15 on which the electrodes and the gate oxide film are formed on the substrate as described above is chemically bonded with a silane coupling agent in a later step. Hydroxylated for ease. Specifically, a pyranha solution, which is a mixed solution of sulfuric acid and a concentration of 30% hydrogen peroxide in a volume ratio of 3 to 1, is prepared, and this pyranha solution is heated to several tens of degrees (for example, about 60 ° C). Then, the substrate 15 was immersed in this solution for several tens minutes (for example, about 10 minutes). After removing the substrate 15 from the solution, the piranha solution remaining on the surface of the substrate 15 was washed away with running water of high purity for several tens minutes (for example, about 20 minutes).
- a pyranha solution which is a mixed solution of sulfuric acid and a concentration of 30% hydrogen peroxide in a volume ratio of 3 to 1
- this pyranha solution is heated to several tens of degrees (for example, about
- the surface of the substrate 15 may be hydroxylated by irradiating the surface of the substrate 15 with oxygen plasma. Irradiation with oxygen plasma is performed, for example, at an output of 200 W and a pressure of 133 MPa for 3 minutes.
- the substrate 15 was immersed once or several times (for example, twice) in ethanol (purity of 99.5% or more; for high-performance liquid chromatography; the same applies hereinafter).
- the substrate 15 is immersed in a mixture of equal amounts of ethanol and hexane (purity 96.0% or more; for high performance liquid chromatography; the same applies hereinafter) once or several times (for example, twice). went.
- the work of immersing the substrate 15 in hexane was performed once or several times (for example, twice). These steps are intended to make the formation of the layer comprising the silane coupling agent in the next step on the surface of the substrate 15 easier.
- the substrate 15 is referred to as AEAP TMS) in a 0.01 to 10% by volume (eg, 0.5% by volume) dilute solution of hexane dissolved in hexane. 10 minutes), so that the silane coupling agent could be bonded to the surface of the substrate 15 as shown in FIG. 17B (in FIG. 17B, the alkyl chain is This is represented by a simplified line of refraction.
- the substrate 15 may be placed in a saturated vapor composed of an AEAP TMS dilute hexane solution or a stock solution and left for tens of minutes to several hours (for example, 30 minutes).
- the substrate 15 is taken out of the above-mentioned AEAP TM S dilute hexane solution (or saturated vapor composed of the AEAP TM S dilute hexane solution or stock solution), and the substrate 15 is placed in hexane or high-purity water. After immersion and ultrasonic cleaning for several minutes to several tens minutes, the substrate 15 was heated at a temperature of 100 to 120 ° C. The ultrasonic treatment was performed, for example, at an output of 110 W to 120 W and an oscillation frequency of 38 kHz for 10 minutes.
- the AEAP TMS that is excessively attached to the surface of the substrate 15, that is, is not chemically bonded to a hydroxyl group on the surface of the substrate 15 can be removed by the above-described cleaning by ultrasonic treatment.
- the dehydration condensation reaction in the AEAP TMS thin film and between the AEAP TMS and hydroxyl groups on the substrate surface is promoted.
- the chemical bond can be strengthened. More specifically, a dehydration-condensation reaction changes from a hydrogen bond to a covalent bond, and the bonding strength increases.
- the operation of immersing the substrate 15 in a hexane solution was performed once or several times (for example, twice).
- the substrate 15 is immersed once or several times (for example, twice) in a mixed solution of hexane and toluene (purity of 997% or more; for high-performance liquid chromatography; the same applies hereinafter).
- a mixed solution of hexane and toluene purity of 997% or more; for high-performance liquid chromatography; the same applies hereinafter.
- the operation of immersing the substrate 15 in the toluene solution was performed once or several times (for example, twice). These steps are for facilitating the subsequent bonding of the fine gold particles to the silane coupling agent.
- a solution of 100 to 100 ppm (for example, l OOO ppm) in which gold fine particles having a diameter of several nanometers are dissolved in toluene is prepared, and the substrate 15 is placed in the toluene solution of gold fine particles. Immersed for several hours (for example, about 1 hour). As a result, as shown in FIG. 17C, a chemical bond occurs between the fine gold particles 8 and the AEAP TMS thin film.
- the substrate 15 was removed from the gold fine particle-toluene solution, and the operation of gently washing away the gold fine particles 8 not chemically bonded to the AEAP TMS thin film with toluene was performed once or several times (for example, twice).
- the substrate 15 was placed in a 1 mM solution of 4,4′-biphenyldithiol (HSC 6 H 4 C 6 H 4 SH) as the organic semiconductor molecule dissolved in toluene for several hours to one day ( For example, about 1 day).
- HSC 6 H 4 C 6 H 4 SH 4,4′-biphenyldithiol
- the gold fine particles 8 and 4,4, -biphenyldithiol are chemically bonded.
- the substrate 15 is removed from the toluene solution of 4,4'-biphenyldithiol, and the 4,4'-biphenyldithiol not chemically bonded to the gold microparticles 8 is lightly washed with toluene once or once. I went several times (for example, twice). Thereafter, the substrate 15 was dried.
- the gold fine particles 8 and the organic semiconductor molecules 4 As described above, the gold fine particles 8 and the organic semiconductor molecules 4,
- the current flowing between the source electrode and the drain electrode was measured with respect to the voltage applied between the source electrode and the drain electrode while changing the voltage applied to the gate electrode. As shown in the figure, the semiconductor operation was confirmed.
- the numerical value at the right end means the voltage value applied to the gate electrode in each measurement.
- Example A MOS field-effect transistor was fabricated in the same manner as in 1 (Fig. 20). When the current-voltage characteristics of the transistor were measured in the same manner as described above, the semiconductor operation was confirmed.
- fine particles made of silver or platinum, or sulfide, selenide, or silicon as the semiconductor may be used. it can.
- the particle size is preferably 10 nm or less.
- shape of the fine particles has been described by taking a spherical shape, a rectangular shape, and a nanorod as an example. However, the present invention is not limited to this shape.
- the fine particles are connected by the organic semiconductor molecules to form a conductive path
- a network type in which the conductive paths in the fine particles and the conductive paths along the molecular skeleton in the organic semiconductor molecules are connected.
- a conductive path can be formed.
- the structure is such that charge transfer in the conductive path occurs predominantly in the axial direction of the molecule along the main chain of the organic semiconductor molecule. Since the conduction path does not include the electron transfer between molecules, the mobility is not limited by the electron transfer between molecules, which has caused the low mobility of the conventional organic semiconductor.
- the axial charge transfer in the organic semiconductor molecule can be maximally utilized.
- a molecule having a conjugated system formed along the main chain is used as the organic semiconductor molecule, high mobility due to delocalized 7T electrons can be used.
- the channel region for forming the conductive path can be formed one layer at a time under normal pressure by a low-temperature process of 200 or less, so that a channel layer having a desired thickness can be easily formed, and a plastic substrate can be formed.
- a semiconductor device can be manufactured at low cost on such a flexible substrate.
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Abstract
Description
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Priority Applications (5)
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KR1020047006215A KR100987399B1 (ko) | 2002-07-02 | 2003-07-02 | 반도체 장치 및 그 제조 방법 |
EP03762870A EP1519418B1 (en) | 2002-07-02 | 2003-07-02 | Semiconductor device and method for manufacturing same |
US10/493,556 US7615775B2 (en) | 2002-07-02 | 2003-07-02 | Semiconductor apparatus and process for fabricating same |
US11/241,177 US7579223B2 (en) | 2002-07-02 | 2005-09-30 | Semiconductor apparatus and process for fabricating the same |
US12/614,070 US9356247B2 (en) | 2002-07-02 | 2009-11-06 | Semiconductor device and method for manufacturing the same |
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- 2003-06-27 JP JP2003184860A patent/JP4635410B2/ja not_active Expired - Fee Related
- 2003-07-02 EP EP10175410A patent/EP2251918A1/en not_active Withdrawn
- 2003-07-02 CN CNB038017385A patent/CN100440534C/zh not_active Expired - Fee Related
- 2003-07-02 KR KR1020047006215A patent/KR100987399B1/ko not_active IP Right Cessation
- 2003-07-02 TW TW092118084A patent/TWI232587B/zh not_active IP Right Cessation
- 2003-07-02 US US10/493,556 patent/US7615775B2/en not_active Expired - Fee Related
- 2003-07-02 WO PCT/JP2003/008403 patent/WO2004006337A1/ja active Application Filing
- 2003-07-02 EP EP03762870A patent/EP1519418B1/en not_active Expired - Fee Related
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2005
- 2005-09-30 US US11/241,177 patent/US7579223B2/en not_active Expired - Fee Related
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2009
- 2009-11-06 US US12/614,070 patent/US9356247B2/en not_active Expired - Lifetime
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JPS6489368A (en) * | 1987-09-29 | 1989-04-03 | Noboru Koyama | Field-effect transistor |
JPH06273811A (ja) * | 1993-03-22 | 1994-09-30 | Mitsubishi Electric Corp | 光・電子機能材料およびその薄膜の製法 |
Non-Patent Citations (1)
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See also references of EP1519418A4 * |
Cited By (10)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US7564051B2 (en) | 2003-07-17 | 2009-07-21 | Panasonic Corporation | Thin-film transistor including organic semiconductor and inorganic particles, and manufacturing method therefor |
WO2006076036A2 (en) * | 2004-05-25 | 2006-07-20 | The Trustees Of The University Of Pennsylvania | Nanostructure assemblies, methods and devices thereof |
WO2006076036A3 (en) * | 2004-05-25 | 2007-01-18 | Univ Pennsylvania | Nanostructure assemblies, methods and devices thereof |
US8828792B2 (en) | 2004-05-25 | 2014-09-09 | The Trustees Of The University Of Pennsylvania | Nanostructure assemblies, methods and devices thereof |
EP1797584A2 (en) * | 2004-06-08 | 2007-06-20 | Nanosys, Inc. | Methods and devices for forming nanostructure monolayers and devices including such monolayers |
EP1797584A4 (en) * | 2004-06-08 | 2014-08-13 | Sandisk Corp | METHODS AND DEVICES FOR FORMING NANOSTRUCTURE MONOLAYERS AND DEVICES COMPRISING SUCH SINGLES |
WO2006025353A1 (ja) * | 2004-08-31 | 2006-03-09 | Matsushita Electric Industrial Co., Ltd. | 電界効果トランジスタおよびその製造方法、ならびにそれを用いた電子機器 |
US7772125B2 (en) * | 2005-02-10 | 2010-08-10 | Panasonic Corporation | Structure in which cylindrical microstructure is maintained in anisotropic groove, method for fabricating the same, and semiconductor device, TFT driving circuit, panel, display and sensor using the structure in which cylindrical microstructure is maintained in anisotropic groove |
CN112563330A (zh) * | 2020-12-06 | 2021-03-26 | 南开大学 | 一种基于二维材料纳米孔的垂直单分子场效应晶体管集成器件及制备方法 |
CN112563330B (zh) * | 2020-12-06 | 2022-10-28 | 南开大学 | 一种垂直单分子场效应晶体管集成器件及制备方法 |
Also Published As
Publication number | Publication date |
---|---|
JP4635410B2 (ja) | 2011-02-23 |
US20100051931A1 (en) | 2010-03-04 |
US7579223B2 (en) | 2009-08-25 |
US9356247B2 (en) | 2016-05-31 |
EP1519418A1 (en) | 2005-03-30 |
US7615775B2 (en) | 2009-11-10 |
TW200406925A (en) | 2004-05-01 |
EP2251918A1 (en) | 2010-11-17 |
CN1602551A (zh) | 2005-03-30 |
US20060024860A1 (en) | 2006-02-02 |
CN100440534C (zh) | 2008-12-03 |
KR100987399B1 (ko) | 2010-10-13 |
TWI232587B (en) | 2005-05-11 |
US20050056828A1 (en) | 2005-03-17 |
KR20050012716A (ko) | 2005-02-02 |
JP2004088090A (ja) | 2004-03-18 |
EP1519418B1 (en) | 2012-05-02 |
EP1519418A4 (en) | 2008-06-25 |
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