JP5056834B2 - Method for manufacturing electroluminescent device - Google Patents

Description

  The present invention relates to an electroluminescent element having an electroluminescent layer formed by using a photolithography method (hereinafter, electroluminescent may be abbreviated as EL) and a method for manufacturing the same.

  In an EL element, holes and electrons injected from opposing electrodes are combined in a light emitting layer, and the energy of the fluorescent material in the light emitting layer is excited to emit light of a color corresponding to the fluorescent material. It attracts attention as a light-emitting planar display element. Among them, organic thin-film EL displays using organic substances as light-emitting materials have high light-emission efficiency such as high-luminance light emission even when the applied voltage is less than 10 V, and can emit light with a simple element structure. It is expected to be applied to advertisements that emit light and other simple display displays at a low price.

  In manufacturing a display using such an EL element, patterning of an electrode layer or an organic EL layer is usually performed. As a patterning method of this EL element, there are a method of vapor-depositing a luminescent material through a shadow mask, a method of separately coating by ink jet, a method of destroying a specific luminescent dye by ultraviolet irradiation, a screen printing method and the like. However, these methods cannot provide an EL element that realizes all of light emission efficiency, high light extraction efficiency, simple manufacturing process, and high-definition pattern formation.

  As means for solving such problems, a method for manufacturing an EL element formed by patterning a light emitting layer by a photolithography method has been proposed. According to this method, when compared with a conventional patterning method by vapor deposition, it is possible to manufacture relatively easily and inexpensively because a vacuum facility or the like having a highly accurate alignment mechanism is unnecessary. On the other hand, compared with the patterning method using the inkjet method, it is preferable in that it does not perform pre-processing on a structure or a substrate that assists patterning, and is further manufactured by a photolithography method in view of the discharge accuracy of the inkjet head. The method has an advantage that it is a preferable method for forming a high-definition pattern.

  As a method for forming a plurality of light emitting portions by such a photolithography method, for example, a method shown in FIG. 4 has been proposed (Patent Document 1).

  First, as shown in FIG. 4A, a light emitting layer 4 is applied on a substrate 1 provided with electrodes, and as shown in FIG. 4B, a photoresist layer 6 is laminated thereon. Next, as shown in FIG. 4 (c), only the portion for forming the first light emitting portion is masked with the photomask 7, and the other portions are exposed with the ultraviolet rays 8. This is developed with a photoresist developer and washed to remove the photoresist layer 6 in the exposed portion as shown in FIG. 4 (d). Further, the portion where the photoresist layer is removed and the light emitting layer is exposed is removed by etching, and FIG. 4E is obtained.

  By repeating the above steps three times, patterning of three types of light emitting portions can be performed. Finally, when the stripping process is performed with a photoresist stripping solution, the three types of light emitting portions 6, 9, and 10 are exposed as shown in FIG. 4 (n). Thereafter, an EL element that emits light in the lower part of the figure is manufactured through a process of forming a second electrode layer on each light emitting part.

JP 2002-170673 A

  In patterning by the photolithography method as described above, dry etching is often used as an etching method. This is because dry etching can efficiently remove organic substances and can be performed without residue. However, dry etching has a slightly different etching rate depending on the type of organic material, but as a result, most organic materials are etched without selectivity.

  In order to prevent a short circuit between an anode or wiring and a cathode, an organic EL element is generally provided with an insulating layer. Since this insulating layer is made of an organic material such as thermosetting resin or ultraviolet curable resin, the insulating layer is also eroded during dry etching, losing insulation and shorting between the anode, wiring, and cathode. There was a problem of causing.

  The present invention has been made in view of the above-mentioned problems, and its purpose is to have a long lifetime in which the loss of the insulating layer due to etching is prevented and the short-circuit defect of the element is prevented while having the advantages of the photolithography method. The main object of the present invention is to provide a device capable of obtaining stable light emission and a method for producing the same.

The present invention relates to a method of manufacturing an electroluminescent device having at least a first electrode, a plurality of types of electroluminescent layers, and a second electrode on a substrate.
Methyltrichlorosilane, methyltribromosilane, methyltrimethoxysilane, methyltriethoxysilane, methyltriisopropoxysilane, methyltrit-butoxysilane; ethyltrichlorosilane, ethyltribromosilane, ethyltrimethoxysilane, ethyltriethoxysilane, Ethyltriisopropoxysilane, ethyltri-t-butoxysilane; n-propyltrichlorosilane, n-propyltribromosilane, n-propyltrimethoxysilane, n-propyltriethoxysilane, n-propyltriisopropoxysilane, n -Propyltri-t-butoxysilane; n-hexyltrichlorosilane, n-hexyltribromosilane, n-hexyltrimethoxysilane, n-hexyltriethoxysilane, n-hexyltriiso Lopoxysilane, n-hexyltri-t-butoxysilane; n-decyltrichlorosilane, n-decyltribromosilane, n-decyltrimethoxysilane, n-decyltriethoxysilane, n-decyltriisopropoxysilane, n-decyltrit- N-octadecyltrichlorosilane, n-octadecyltribromosilane, n-ortadecyltrimethoxysilane, n-octadecyltriethoxysilane, n-octadecyltriisopropoxysilane, n-octadecyltri-t-butoxysilane; phenyltrichloro Silane, phenyltribromosilane, phenyltrimethoxysilane, phenyltriethoxysilane, phenyltriisopropoxysilane, phenyltri-t-butoxysilane; tetrachlorosilane, tetrabro Silane, tetramethoxysilane, tetrabutoxysilane, trichlorohydrosilane, tribromohydrosilane, trimethoxyhydrosilane, triethoxyhydrosilane, triisopropoxyhydrosilane, tri-t-butoxyhumanrosilane; trifluoropropyltrichlorosilane, trifluoropropyltribromosilane, Trifluoropropyltrimethoxysilane, trifluoropropyltriethoxysilane, trifluoropropyltriisopropoxysilane, trifluoropropyltri-t-butoxysilane; γ-glycidoxypropyltrimethoxysilane, γ-glycidoxypropyltriethoxysilane Γ-glycidoxypropyltriisopropoxysilane, γ-glycidoxypropyltri-t-butoxysilane; γ-aminopropyltri Toxisilane, γ-aminopropyltriethoxysilane, γ-aminopropyltriisopropoxysilane, γ-aminopropyltrit-butoxysilane; γ-mercaptopropyltrimethoxysilane, γ-mercaptopropyltriethoxysilane, γ-mercaptopropyltri Isopropoxysilane, γ-mercaptopropyltri-t-butoxysilane; β- (3,4-epoxycyclohexyl) ethyltrimethoxysilane, β- (3,4-epoxycyclohexyl) ethyltriethoxysilane, CF ₃ (CF ₂ ) ₃ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₅ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₇ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₉ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , (CF ₃ ) ₂ CF (CF ₂ ) ₄ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , (CF ₃ ) ₂ CF (CF ₂ ) ₆ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , (CF ₃ ) ₂ CF (CF ₂ ) ₈ CH ₂ CH ₂ Si ( OCH ₃ ) ₃ , CF ₃ (C ₆ H ₄ ) C ₂ H ₄ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₃ (C ₆ H ₄ ) C ₂ H ₄ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₅ (C ₆ H ₄ ) C ₂ H ₄ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₇ (C ₆ H ₄ ) C ₂ H ₄ Si (OCH ₃ ) ₃ , CF ₃ (CF _{2) 3 CH 2 CH 2 Si} (OCH 2 CH 3) 3, CF 3 (CF 2) 5 CH 2 CH 2 Si (OCH 2 CH 3) 3, CF 3 (CF 2) 7 CH 2 CH 2 Si (OCH ₂ CH ₃ ) ₃ , CF ₃ (CF ₂ ) ₉ CH ₂ CH ₂ Si (OCH ₂ CH ₃ ) ₃ , and CF ₃ (CF ₂ ) ₇ SO ₂ N (C ₂ H ₅ ) C ₂ H ₄ CH ₂ Si (OC One or more of the _{3) 3} silicon compound selected from dissolved in a solvent, coated and heated, by hydrolysis polycondensation reaction of one or more of the silicon compounds a step of the organopolysiloxane to form a including insulating layers 90 weight or more in the insulating layer is a hydrolytic condensate or cohydrolysis condensate,
An electroluminescent layer is formed by a coating method on a substrate on which at least the first electrode is formed, and patterned by using a photolithography method including a dry etching process using a predetermined gas, thereby patterning the electroluminescent layer. Forming a nescent layer ;
A method for manufacturing an electroluminescent device is provided , which includes the step of forming the patterned electroluminescent layer a plurality of times .

The method for producing an electroluminescent device according to the present invention forms an insulating layer containing an organopolysiloxane that is one or two or more hydrolysis condensates or co-hydrolysis condensates of the above silicon compounds. By having a process , even when using dry etching when patterning by a photolithography method, even the insulating layer is prevented from being eroded, without causing a short circuit between the electrodes or between the electrode and the wiring, It can have the advantage of photolithography. That is, according to the present invention, it is possible to obtain an element in which a high-definition pattern is formed relatively easily and inexpensively and which can provide a long-life and stable light emission in which a short circuit defect of the element is prevented. it can.

In the patterning step using the photolithography method, a photoresist is applied on the electroluminescent layer to be patterned, exposed, and developed to pattern the photoresist, and then a dry etching process using a predetermined gas It is preferable to remove the portion of the electroluminescent layer from which the photoresist has been removed by the above because a high-definition pattern can be obtained.

In addition, the dry etching process in the manufacturing method according to the present invention is preferably a reactive ion etching process from the viewpoint of an effective etching method.
Furthermore, the dry etching process in the manufacturing method according to the present invention preferably uses oxygen alone or a gas containing oxygen. This is because oxygen is a safe, non-toxic material that can be stably obtained, and the electroluminescent layer can be effectively etched by an oxidation reaction without affecting the substrate such as glass or ITO.

  In the manufacturing method according to the present invention, the insulating layer is preferably provided between the first electrode and the second electrode from the viewpoint of preventing a short circuit.

  In the manufacturing method according to the present invention, the insulating layer is preferably provided between the wiring on the substrate and the first electrode and / or between the wiring on the substrate and the second electrode from the viewpoint of preventing a short circuit.

  According to the electroluminescent device and the method for manufacturing the same according to the present invention, even when dry etching is used for patterning by a photolithography method, even the insulating layer is prevented from being eroded. The advantages of the photolithography method can be obtained without causing a short circuit between the wirings. That is, according to the present invention, it is possible to obtain an element in which a high-definition pattern is formed relatively easily and inexpensively and which can provide a long-life and stable light emission in which a short circuit defect of the element is prevented. it can.

It is sectional drawing which shows an example of the EL element which concerns on this invention. It is sectional drawing which shows an example of the patterning using the photolithographic method. (A) is an example of an EL element using a photolithography method, and (b) and (c) are cross-sectional views showing an example of a conventional EL element. It is sectional drawing which shows an example of the patterning using the photolithographic method. It is sectional drawing which shows an example of the conventional EL element.

1. Electroluminescent Element The electroluminescent element according to the present invention has at least a first electrode, an electroluminescent layer, and a second electrode on a substrate, and at least one of the electroluminescent layers is a predetermined layer. An electroluminescent element obtained by patterning by a photolithography method including a dry etching process using any of the above gases, wherein the selectivity to the organic compound is 2.5 or more in the dry etching process using the predetermined gas. It has an insulating layer containing an inorganic material.

The electroluminescent device according to the present invention has at least a first electrode, an electroluminescent layer, and a second electrode on a substrate, and at least one of the electroluminescent layers is patterned by a photolithography method. Y _n SiX _(4-n) (wherein Y represents an alkyl group, a fluoroalkyl group, a vinyl group, an amino group, a phenyl group or an epoxy group, and X represents an alkoxyl group) An insulating layer containing an organopolysiloxane that is one or more of the hydrolytic condensates or co-hydrolytic condensates of a silicon compound represented by: It is characterized by having.

  Conventionally, as shown in FIG. 5, the insulating layer 20 is made of an organic material such as a thermosetting resin or an ultraviolet curable resin. Therefore, when the EL layer 4 is patterned by a photolithography method, the insulating layer 20 reaches the insulating layer during dry etching. As a result, the wiring 21 was exposed and a gap was formed between the first electrode 2 and the insulating layer 20 (FIG. 5B). When the second electrode is laminated in a state where the insulating layer 20 is eroded in this way, the second electrode comes into contact with the side surface of the first electrode to form a conduction path to cause a short circuit 22 or to the exposed wiring 21. There was a problem that the electrodes contacted to form a conduction path, causing a short circuit 22 (FIG. 5C).

  As shown in FIG. 1, the EL element according to the present invention is an inorganic material having a selectivity with an organic compound of 2.5 or more in a dry etching process using a predetermined gas, or a silicon compound as described above. Dry etching when patterning is performed by a photolithography method by having an insulating layer containing organopolysiloxane which is one or two or more kinds of hydrolysis condensates or cohydrolysis condensates (FIG. 1 (a)) Even if it is used, even the insulating layer is prevented from being eroded (FIG. 1B). Therefore, in the EL element according to the present invention, the second electrode does not contact the first electrode 2 or the wiring (not shown) even when the second electrode is stacked (FIG. 1C). The advantage of the photolithography method can be obtained without causing a short circuit between the two electrodes or between the electrode and the wiring. That is, according to the present invention, it is possible to obtain an element in which a high-definition pattern is formed relatively easily and inexpensively and which can provide a long-life and stable light emission in which a short circuit defect of the element is prevented. it can.

  FIG.1 (c) is a schematic sectional drawing which shows an example of the EL element based on this invention. 1C, the EL element is formed so as to cover the substrate 1, the first electrode 2 formed on the substrate 1, the edge portion on the first electrode 2, and the non-light emitting portion of the element. It has an insulating layer 3, an EL layer 4 formed on the first electrode and having at least a light emitting layer, and a second electrode 5 formed on the EL layer 4. One layer is patterned by photolithography.

  Hereinafter, components of the EL element of the present invention will be described. The patterning by the photolithography method will be described in detail in the EL element manufacturing method according to the present invention described later.

(substrate)
The substrate serves as a support for the EL element. For example, the substrate may be a flexible material or a hard material. The substrate of the EL element used in the present invention is not particularly limited as long as it is a substrate such as glass or plastic sheet used in conventional EL elements. The thickness of these substrates is usually about 0.1 to 2.0 mm.

(First and second electrodes)
In the present invention, the first electrode is formed on the substrate, and the second electrode is formed on the EL layer. These electrodes consist of an anode and a cathode. Depending on the extraction direction of the light emitted from the EL layer 4, which electrode is required to have transparency or not, when extracting light from the substrate 1 side, the first electrode is formed of a transparent or translucent material. In addition, when light is extracted from the second electrode side, the second electrode needs to be formed of a transparent or translucent material.

  The electrode is preferably made of a conductive material and has a resistance as small as possible. Generally, a metal material is used, but an organic compound or an inorganic compound may be used. Further, a plurality of materials may be mixed and formed.

  The anode is preferably formed from a conductive material having a large work function so that holes can be easily injected. Examples of preferable anode materials include indium oxide and gold.

  The cathode is preferably formed from a conductive material having a low work function so that electrons can be easily injected. Preferable cathode materials include, for example, magnesium alloys (Mg—Ag, etc.), aluminum alloys (Al—Li, Al—Ca, Al—Mg, etc.), metallic calcium, and metals having a small work function. The thickness of these electrode layers is usually about 20 to 1000 mm, respectively.

(Insulating layer)
When an insulating layer is required in the EL element, the insulating layer is usually provided between the first electrode and the second electrode from the viewpoint of preventing a short circuit. In addition, when the wiring is provided on the substrate, the insulating layer is also provided between the wiring on the substrate and the first electrode and / or between the wiring on the substrate and the second electrode in order to prevent a short circuit. It should be noted that “between” the first electrode and the second electrode and “between” the wiring on the substrate and the electrode include not only spatially intervening but also intervening between conduction paths. It is.

  In order to prevent a short circuit at a portion unnecessary for light emission, the insulating layer covers, for example, the edge portion of the first electrode formed in a pattern on the substrate and the non-light emitting portion of the element so that the light emitting portion becomes an opening. By providing in advance, it is formed between the first electrode and the second electrode, and between the wiring on the substrate and the first electrode and / or between the wiring on the substrate and the second electrode. By doing in this way, the defect by the short circuit of an element, etc. reduces, and the element which emits light stably with a long lifetime is obtained.

  When the EL layer is patterned by dry etching in the photolithography method, the insulating layer is preferably resistant to dry etching. When the main component of the EL layer to be patterned is an organic material, reactive ion etching that is preferably used in dry etching is, for example, plasma using a reactive gas such as oxygen alone or a gas containing oxygen. The organic material is generated by being chemically reacted with these reaction gases and removed as a gas. Therefore, an insulating layer that does not react with a predetermined gas used for dry etching is required as a preferable one.

In the present invention, the insulating layer is an insulating layer (first aspect of the insulating layer) containing an inorganic material having a selectivity with an organic compound of 2.5 or more in a dry etching process using a predetermined gas, Or Y _n SiX _(4-n) (wherein Y represents an alkyl group, a fluoroalkyl group, a vinyl group, an amino group, a phenyl group or an epoxy group, and X represents an alkoxyl group or a halogen. An insulating layer (second embodiment of the insulating layer) containing an organopolysiloxane which is one or two or more hydrolysis condensates or cohydrolysis condensates of silicon compounds represented by is there. For this reason, even if dry etching is used for patterning by a photolithography method, the insulating layer is prevented from being eroded.

  In general, in the substrate cleaning process, plasma treatment using argon or oxygen is used as the dry cleaning process. In the case of cleaning, damage to the substrate is not as great as in dry etching for patterning, but the film surface may be roughened. When the inorganic insulating layer as in the present invention is used, there is an effect of preventing the film surface from being roughened in a general dry cleaning process.

i) First Aspect of Insulating Layer The inorganic material used in the first aspect of the insulating layer has an insulating property among the inorganic materials, and is selected from an organic compound in a dry etching process using a predetermined gas. The ratio is 2.5 or more.

  Here, the selection ratio in the dry etching process refers to the ratio of the etching rate of the material to be etched to the etching rate of the material not to be etched (etching rate of the material to be etched / etching rate of the material not to be etched). In this case, the ratio between the etching rate of the organic compound and the etching rate of the inorganic material used for the insulating layer (the etching rate of the organic compound / the etching rate of the inorganic material used for the insulating layer). The organic compound here is a main component of a material for forming at least one layer of an electroluminescent layer formed by patterning by a photolithography method including a dry etching process, and a standard material includes a luminescent material, for example, Polyvinylcarbazole, polyparaphenylene vinylene, polythiophene, and polyfluorene can be used.

  In the dry etching process, an inorganic material having a selectivity ratio with respect to an organic compound of 2.5 or more has selectivity with the EL layer under the etching conditions for etching an EL layer mostly formed of the organic compound. High and not eroded.

In the inorganic material in the present invention, the selection ratio with respect to the organic compound in the dry etching process using a predetermined gas is 2.5 or more, more preferably 3 or more, particularly 4 or more, especially 5 or more. Preferably there is.
The inorganic material in the present invention refers to a material mainly composed of an inorganic compound, and includes an organic-inorganic composite.

Further, from the viewpoint of insulation, it is necessary to select an inorganic material having a specific resistance (Ωcm) of 10 ¹⁰ or more, and it is preferable to select a material having a specific resistance of 10 ¹² or more. Here, the specific resistance (Ωcm) can be obtained by (electric resistivity × cross-sectional area / length).

  The dry etching process preferably uses simple oxygen or a gas containing oxygen. This is because oxygen is a material that can be safely and stably obtained without toxicity, and has high reactivity and is useful as an etching gas. Therefore, oxygen is a gas that can be suitably used in a dry etching process that can be used in the photolithography method of the present invention. .

  As an example of an inorganic material having an insulating property and having a selectivity to an organic compound of 2.5 or more in a dry etching process, for example, an oxide of silicon (for example, SiOx (x is 1 to 2) )), Silicon nitride (for example, SiNx (x is 1/2 or more and 4/3 or less)), SiON, SiAlON, SiOF, aluminum oxide, tantalum oxide, titanium oxide, tin oxide, vanadium oxide, barium strontium titanate , Barium zirconate titanate, lead zirconate titanate, lanthanum titanate, strontium titanate, barium titanate, barium fluoride, magnesium bismuth titanate, strontium bismuth titanate, strontium bismuth tantalate, bismuth tantalate niobate , Trioxide yttrium Etc., and the like.

  Among these, the inorganic material is preferably made of silicon oxide and / or nitride. This is because silicon oxide and / or nitride is an insulating material that can be stably obtained without toxicity. Moreover, it is because a film can be easily formed by sputtering, vapor deposition or the like. Among oxides and / or nitrides of silicon, SiOx (x is 1 or more and 2 or less) and SiNx (x is ½ or more and 4/3 or less) can be preferably used. 2) SiNx (x is 4/3) can be used particularly preferably in the present invention.

  The first aspect of the insulating layer may contain other components other than the inorganic material having a selectivity ratio with respect to the organic compound of 2.5 or more in the dry etching process as long as the effects of the present invention are not impaired. Even in that case, an inorganic material having a selectivity to an organic compound of 2.5 or more in the dry etching process is 50% by weight or more in the insulating layer, more preferably 70% by weight or more, particularly 90% from the viewpoint of dry etching resistance. It is preferable that it is contained by weight% or more. The insulating layer is particularly preferably made of an inorganic material having a selectivity with respect to an organic compound of 2.5 or more in the dry etching process from the viewpoint of dry etching resistance and insulating properties.

ii) Second embodiment of insulating layer YnSiX (4-n) (where Y is an alkyl group, a fluoroalkyl group, a vinyl group, an amino group, a phenyl group, or an epoxy group) used in the second embodiment of the insulating layer X represents an alkoxyl group or halogen, n is an integer from 0 to 3.) One or two or more hydrolyzed condensates or cohydrolyzed condensates of a silicon compound represented by Polysiloxane is hydrolyzed and polycondensed by halogen and / or alkoxyl groups by sol-gel reaction or the like, and molecules are polymerized to form a strong and uniform layer having dry etching resistance. It is preferable because it can be coated by the method.

  Specific examples of the silicon compound represented by YnSiX (4-n) include methyltrichlorosilane, methyltribromosilane, methyltrimethoxysilane, methyltriethoxysilane, methyltriisopropoxysilane, and methyltrit-butoxysilane; Ethyltrichlorosilane, ethyltribromosilane, ethyltrimethoxysilane, ethyltriethoxysilane, ethyltriisopropoxysilane, ethyltrit-butoxysilane; n-propyltrichlorosilane, n-bromotribromosilane, n-bromotritri Methoxysilane, n-propyltriethoxysilane, n-propyltriisopropoxysilane, n-propyltrit-butoxysilane; n-hexyltrichlorosilane, n-hexyltribromosilane, n-hexyltrimethoxysila N-hexyltriethoxysilane, n-hexyltriisopropoxysilane, n-hexyltri-t-butoxysilane; n-decyltrichlorosilane, n-decyltribromosilane, n-decyltrimethoxysilane, n-decyltriethoxy Silane, n-decyltriisopropoxysilane, n-decyltrit-butoxysilane; n-octadecyltrichlorosilane, n-octadecyltribromosilane, n-ortadecyltrimethoxysilane, n-octadecyltriethoxysilane, n-octadecyltri Isopropoxysilane, n-octadecyltri-t-butoxysilane; phenyltrichlorosilane, phenyltribromosilane, phenyltrimethoxysilane, phenyltriethoxysilane, phenyltriisopropoxysilane, phenyl Tri-t-butoxysilane; tetrachlorosilane, tetrabromosilane, tetramethoxysilane, tetraethoxysilane, tetrabutoxysilane, dimethoxydiethoxysilane; dimethyldichlorosilane, dimethyldibromosilane, dimethyldimethoxysilane, dimethyldiethoxysilane; Diphenyldichlorosilane, diphenyldibromosilane, diphenyldimethoxysilane, diphenyldiethoxysilane; phenylmethyldichlorosilane, phenylmethyldibromosilane, phenylmethyldimethoxysilane, phenylmethyldiethoxysilane; trichlorohydrosilane, tribromohydrosilane, triphenyl Methoxyhydrosilane, triethoxyhydrosilane, triisopropoxyhydrosilane, tri-t-butoxyhumanrosilane; vinyl tric Silane, vinyltribromosilane, vinyltrimethoxysilane, vinyltriethoxysilane, vinyltriisopropoxysilane, vinyltri-t-butoxysilane; trifluoropropyltrichlorosilane, trifluoropropyltribromosilane, trifluoropropyltrimethoxysilane, tri Fluoropropyltriethoxysilane, trifluoropropyltriisopropoxysilane, trifluoropropyltri-t-butoxysilane; γ-glycidoxypropylmethyldimethoxysilane, γ-glycidoxypropylmethyldiethoxysilane, γ-glycidoxypropyl Trimethoxysilane, γ-glycidoxypropyltriethoxysilane, γ-glycidoxypropyltriisopropoxysilane, γ-glycidoxypropyltri-t-butoxy Run: γ-methacryloxypropylmethyldimethoxysilane, γ-methacryloxypropylmethyldiethoxysilane, γ-methacryloxypropyltrimethoxysilane, γ-methacryloxypropyltriethoxysilane, γ-methacryloxypropyl Triisopropoxysilane, γ-methacryloxypropyltri-t-butoxysilane; γ-aminopropylmethyldimethoxysilane, γ-aminopropylmethyldiethoxysilane, γ-aminopropyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ-aminopropyltriisopropoxysilane, γ-aminopropyltri-t-butoxysilane; γ-mercaptopropylmethyldimethoxysilane, γ-mercaptopropylmethyldiethoxysilane, γ-mercaptopropyltri Toxisilane, γ-mercaptopropyltriethoxysilane, γ-mercaptopropyltriisopropoxysilane, γ-mercaptopropyltri-t-butoxysilane; β- (3,4-epoxycyclohexyl) ethyltrimethoxysilane, β- (3,4 -Epoxycyclohexyl) ethyltriethoxysilane; a fluoroalkylsilane generally known as a fluorine-based silane coupling agent, an example of which is shown below; and their hydrolysis condensates or cohydrolysis condensates; and Mention may be made of mixtures.

CF ₃ (CF ₂ ) ₃ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₅ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₇ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₉ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , (CF ₃ ) ₂ CF (CF ₂ ) ₄ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , (CF ₃ ) ₂ CF _{(CF 2) 6 CH 2 CH} 2 Si (OCH 3) 3, (CF 3) 2 CF (CF 2) 8 CH 2 CH 2 Si (OCH 3) 3, CF 3 (C 6 H 4) C 2 H 4 Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₃ (C ₆ H ₄ ) C ₂ H ₄ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₅ (C ₆ H ₄ ) C ₂ H ₄ Si ( OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₇ (C ₆ H ₄ ) C ₂ H ₄ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₃ CH ₂ CH ₂ SiCH ₃ (OCH ₃ ) ₂ , CF ₃ ( _{F 2) 5 CH 2 CH 2} SiCH 3 (OCH 3) 2, CF 3 (CF 2) 7 CH 2 CH 2 SiCH 3 (OCH 3) 2, CF 3 (CF 2) 9 CH 2 CH 2 SiCH 3 (OCH _{3) 2, (CF 3)} 2 CF (CF 2) 4 CH 2 CH 2 SiCH 3 (OCH 3) 2, (CF 3) 2 CF (CF 2) 6 CH 2 CH 2 SiCH 3 (OCH 3) 2, (CF ₃ ) ₂ CF (CF ₂ ) ₈ CH ₂ CH ₂ SiCH ₃ (OCH ₃ ) ₂ , CF ₃ (C ₆ H ₄ ) C ₂ H ₄ SiCH ₃ (OCH ₃ ) ₂ , CF ₃ (CF ₂ ) ₃ (C ₆ H ₄ ) C ₂ H ₄ SiCH ₃ (OCH ₃ ) ₂ , CF ₃ (CF ₂ ) ₅ (C ₆ H ₄ ) C ₂ H ₄ SiCH ₃ (OCH ₃ ) ₂ , CF ₃ (CF ₂ ) _{7 (C 6 H 4) C 2} H 4 SiCH 3 (OCH 3) 2, CF 3 (CF 2) 3 CH 2 CH 2 Si (OCH 2 CH 3) 3, CF 3 ( _{F 2) 5 CH 2 CH 2} Si (OCH 2 CH 3) 3, CF 3 (CF 2) 7 CH 2 CH 2 Si (OCH 2 CH 3) 3, CF 3 (CF 2) 9 CH 2 CH 2 Si ( OCH ₂ CH ₃ ) ₃ , CF ₃ (CF ₂ ) ₇ SO ₂ N (C ₂ H ₅ ) C ₂ H ₄ CH ₂ Si (OCH ₃ ) ₃

  Among the above-mentioned organopolysiloxanes, it is preferable to contain a large number of functional groups that can be crosslinking points, such as alkoxyl groups or halogens, in order to form a strong film by crosslinking in order to improve dry etching resistance. Accordingly, YnSiX (4-n) (wherein Y represents an alkyl group, a fluoroalkyl group, a vinyl group, an amino group, a phenyl group or an epoxy group, X represents an alkoxyl group or a halogen. N represents 0 to 3) In the silicon compound represented by the following formula, n is preferably as small as possible, and it is particularly preferable that n = 0.

  In addition, the second aspect of the insulating layer may contain other components other than the organopolysiloxane within a range not impairing the effects of the present invention, but in that case, the organopolysiloxane is dry-etched. From the viewpoint of resistance, the insulating layer is preferably contained in an amount of 50% by weight or more, more preferably 70% by weight or more, and particularly preferably 90% by weight or more. The insulating layer is particularly preferably made of the above organopolysiloxane from the viewpoints of dry etching resistance and insulating properties.

Also in the second aspect, it is necessary to select a specific resistance (Ωcm) of the insulating layer of 10 ¹⁰ or more in the present invention, and it is preferable to select a specific resistance of 10 ¹² or more.

  In the present invention, the thickness of the insulating layer is preferably 0.1 μm to 5 μm, more preferably 0.5 μm to 1.5 μm from the viewpoint of insulation. This is because if the thickness is too thick, the second electrode may be disconnected or a patterning failure of the insulating layer may occur, and if it is too thin, a short circuit may occur.

(EL layer)
The EL layer 4 is formed by patterning at least one layer by photolithography. The EL layer needs to include at least a light emitting layer, and in addition, a buffer layer, a hole transport layer, a hole injection layer, an electron transport layer, an electron injection layer, and the like may be combined.

  Further, the EL layer to be patterned may be any layer constituting the EL layer described above, but in the present invention, it is preferably a light emitting layer or a buffer layer, and among them, the light emitting layer is used as an EL layer. Patterning is preferable from the viewpoint of producing an area color or full color display element. Furthermore, it is more preferable that the light emitting layer and the buffer layer are patterned as an EL layer from the viewpoint of the carrier injection balance of the EL element.

  In the case of a full-color EL element, the EL layer may be an EL layer that is patterned by a photolithography method three times, with the light emitting layer being three types of light emitting layers.

[Light emitting layer]
The light-emitting layer formed on the first electrode is preferably an organic light-emitting layer in the present invention. Usually, organic substances (low molecular compounds and high molecular compounds) that mainly emit fluorescence or phosphorescence and assist this. Formed from a dopant. The material for forming the light emitting layer is insoluble in the following photoresist solvent, the following photoresist developer, and the following photoresist stripping solution used in the photolithography method when the light emitting layer is formed by patterning by a photolithography method. It is preferable that the material is

Examples of the material for forming the light emitting layer that can be used in the present invention include the following.
<Dye-based material>
Examples of dye-based materials include cyclopentamine derivatives, tetraphenylbutadiene derivative compounds, triphenylamine derivatives, oxadiazole derivatives, pyrazoloquinoline derivatives, distyrylbenzene derivatives, distyrylarylene derivatives, pyrrole derivatives, thiophene ring compounds. Pyridine ring compounds, perinone derivatives, perylene derivatives, oligothiophene derivatives, trifumanylamine derivatives, oxadiazole dimers, pyrazoline dimers, and the like.

<Metal complex materials>
Examples of metal complex materials include aluminum quinolinol complex, benzoquinolinol beryllium complex, benzoxazolyl zinc complex, benzothiazole zinc complex, azomethylzinc complex, porphyrin zinc complex, europium complex, etc. Examples thereof include metal complexes having a rare earth metal such as Be or Tb, Eu, or Dy, and having an oxadiazole, thiadiazole, phenylpyridine, phenylbenzimidazole, quinoline structure, or the like as a ligand.

<Polymer material>
Polymeric materials include polyparaphenylene vinylene derivatives, polythiophene derivatives, polyparaphenylene derivatives, polysilane derivatives, polyacetylene derivatives, polyfluorene derivatives, polyvinylcarbazole derivatives, and polymerized chromophores and metal complex light emitting materials. Etc.

  Among the light emitting materials, examples of the material that emits blue light include distyrylarylene derivatives, oxadiazole derivatives, and polymers thereof, polyvinylcarbazole derivatives, polyparaphenylene derivatives, and polyfluorene derivatives. Of these, polymer materials such as polyvinyl carbazole derivatives, polyparaphenylene derivatives, and polyfluorene derivatives are preferred.

  Examples of materials that emit green light include quinacridone derivatives, coumarin derivatives, and polymers thereof, polyparaphenylene vinylene derivatives, polyfluorene derivatives, and the like. Of these, polymer materials such as polyparaphenylene vinylene derivatives and polyfluorene derivatives are preferred.

  Examples of materials that emit red light include coumarin derivatives, thiophene ring compounds, and polymers thereof, polyparaphenylene vinylene derivatives, polythiophene derivatives, and polyfluorene derivatives. Among these, polymer materials such as polyparaphenylene vinylene derivatives, polythiophene derivatives, and polyfluorene derivatives are preferable.

<Dopant material>
A dopant can be added to the light emitting layer for the purpose of improving the light emission efficiency and changing the light emission wavelength. Examples of such dopants include perylene derivatives, coumarin derivatives, rubrene derivatives, quinacridone derivatives, squalium derivatives, porphyrin derivatives, styryl dyes, tetracene derivatives, pyrazolone derivatives, decacyclene, phenoxazone, and the like.
In addition, the thickness of such a light emitting layer is about 20-2000 mm normally.

[Buffer layer]
The buffer layer in the present invention is provided between the anode and the light emitting layer or between the cathode and the light emitting layer so that charges can be easily injected into the light emitting layer. It is a layer containing. For example, it can be formed from a conductive polymer having a function of increasing the efficiency of hole injection into the light emitting layer and flattening irregularities such as electrodes.

  When the buffer layer has high conductivity, it is desirable that the buffer layer be patterned in order to maintain the diode characteristics of the device and prevent crosstalk. When the resistance of the buffer layer is high, the patterning may not be necessary. In the case of an element that can omit the buffer layer, the buffer layer may not be provided.

  In the present invention, when both the buffer layer and the light emitting layer are formed by patterning by photolithography, the material forming the buffer layer is insoluble in the following photoresist solvent and the solvent used for forming the light emitting layer. Preferably, the material for forming the buffer layer is more preferably a material that is insoluble in the following photoresist stripping solution.

  On the other hand, when the light emitting layer is formed by vacuum deposition or the like and the layer patterned by the photolithography method as the EL layer is only the buffer layer, the material for forming the buffer layer is the following photoresist solvent and the following photoresist stripping solution. It is preferable to select a material that is insoluble in water.

Specific examples of the material for forming the buffer layer include polyalkylthiophene derivatives, polyaniline derivatives, polymers of hole transporting substances such as triphenylamine, sol-gel films of inorganic compounds, and polymer films of organic substances such as trifluoromethane. An organic compound film containing a Lewis acid can be used, but it is not particularly limited as long as the above-described solubility conditions are satisfied, and the above conditions may be satisfied by reaction, polymerization, or baking after film formation. . Moreover, when forming a light emitting layer by vacuum film forming etc., the buffer material, hole injection material, and hole transport material which are generally used can be used.
In addition, the thickness of such a buffer layer is about 100-2000 mm normally.

[Charge transport / injection layer]
In the EL device of the present invention, a hole transport layer, a hole injection layer, an electron transport layer, and an electron injection layer may be formed. These are not particularly limited as long as they are generally used in conventional EL elements such as those described in JP-A-11-4011.

2. Method for manufacturing electroluminescent device The method for manufacturing an electroluminescent device according to the present invention includes an insulating layer formed using a material including an inorganic material having a selectivity to an organic compound of 2.5 or more in a dry etching process. And a step of patterning at least one electroluminescent layer constituting the electroluminescent element using a photolithography method.

In addition, the manufacturing method of the electroluminescent device according to the present invention is Y _n SiX _(4-n) (where Y represents an alkyl group, a fluoroalkyl group, a vinyl group, an amino group, a phenyl group, or an epoxy group). , X represents an alkoxyl group or halogen, and n is an integer of 0 to 3.) An organopolysiloxane which is one or more hydrolyzed condensates or cohydrolyzed condensates of a silicon compound represented by A step of forming an insulating layer using a material containing, and a step of patterning at least one electroluminescent layer constituting the electroluminescent element by using a photolithography method.

  The method for producing an electroluminescent device according to the present invention includes an inorganic material having a selectivity to an organic compound of 2.5 or more in a dry etching process, or one or more of the above silicon compounds. Since it has a step of forming an insulating layer containing an organopolysiloxane that is a hydrolysis condensate or a co-hydrolysis condensate, even if dry etching is used in the patterning step using a photolithography method, even the insulating layer is eroded. Therefore, it is possible to have an advantage of the photolithography method without causing a short circuit between the electrodes or between the electrode and the wiring.

(Process for forming an insulating layer)
i) First Aspect of Insulating Layer A method for forming an insulating layer containing an inorganic material having a selectivity to an organic compound of 2.5 or more in the dry etching process described above is not particularly limited. It is possible to suitably use a known dry film forming method for depositing a coating material on the coating surface in a gas phase state, such as a sputtering method or a vapor deposition method.

ii) Second Embodiment of Insulating Layer The method for forming the insulating layer containing organopolysiloxane described above is not particularly limited, but is often soluble in a solvent, so spin coating, spray coating, dip coating, Known wet film forming methods such as roll coating and bead coating can be suitably used. In this case, Y _n SiX _(4-n) (wherein Y represents an alkyl group, a fluoroalkyl group, a vinyl group, an amino group, a phenyl group or an epoxy group, X represents an alkoxyl group or a halogen. N represents 0. 1 or 2 or more of the silicon compounds represented by the formula (2) is dissolved in a solvent as appropriate, and coating or the like is performed using the above-described wet film forming method. A film is formed by heating using a heating means such as hydrolytic polycondensation reaction and drying.

Solvents that can be used are those that dissolve Y _n SiX _(4-n) , such as alcohols such as ethanol and isopropanol, acetone, acetonitrile, ethylene glycol monomethyl ether, ethylene glycol dimethyl ether, dimethylformamide, and dimethyl. It can be selected from sulfoxide, dioxane, ethylene glycol, hexamethylphosphoric triamide, pyridine, tetrahydrofuran, N-methylpyrrolidinone and the like and mixed solvents thereof.

(Step of patterning at least one EL layer using a photolithography method)
The photolithographic method is a method of forming an arbitrary pattern according to the light irradiation pattern by utilizing the fact that the solubility of the light irradiation portion of the film is changed by light irradiation.

  Patterning using a photolithography method does not require a vacuum device or the like as compared with a conventional vapor deposition method performed through a shadow mask, and thus it is possible to pattern an organic EL layer easily and inexpensively. . On the other hand, compared with patterning by the ink jet method, high-definition patterning can be performed without performing pretreatment of the substrate or providing a liquid-repellent convex portion between the patterns. That is, when a step of patterning at least one EL layer using a photolithography method is performed, a high-quality EL element having a high-definition pattern can be obtained at low cost.

[Photoresist]
The photoresist that can be used in the present invention may be positive type or negative type, and is not particularly limited, but it is soluble in a solvent that does not dissolve the undercoat and can be applied. And what is insoluble in the solvent used for EL layer formation, such as a light emitting layer, is preferable.
Specific examples of the photoresist that can be used include novolak resin-based, rubber + bisazide-based, and the like.

[Photoresist solvent]
In the present invention, as the photoresist solvent used when coating the photoresist, the EL layer such as the light-emitting layer and the photoresist material are prevented from being mixed or dissolved during the photoresist film formation. In order to maintain the light emission characteristics, it is desirable to use a material that does not dissolve the EL layer forming material such as the light emitting layer material. In consideration of this point, the photoresist solvent that can be used in the present invention has a solubility in an EL layer forming material such as a light emitting layer material of 0.001 (g / g solvent) or less at 25 ° C. and 1 atm. It is preferable to select a certain one, and it is more preferable to select one that is 0.0001 (g / g solvent) or less. In general, in order to prevent mixing and dissolution with the base, it is preferable to use this solubility condition in any of the following cases.

  For example, as a photoresist solvent that can be used when the buffer layer forming material is dissolved in an aqueous solvent and the light emitting layer is dissolved in an aromatic non-polar organic solvent, ketones such as acetone and methyl ethyl ketone are used. Cellosolve acetates such as propylene glycol monoethyl ether acetate, propylene glycol monomethyl ether acetate, ethylene glycol monomethyl ether acetate, ethylene glycol monoethyl ether acetate, propylene glycol monoethyl ether, propylene glycol monomethyl ether, ethylene glycol monomethyl ether Cellosolves such as ethylene glycol monoethyl ether, methanol, ethanol, 1-butanol, 2-butanol , Alcohols such as cyclohexanol, ester solvents such as ethyl acetate and butyl acetate, cyclohexane, decalin and the like can be used. It may be a solvent.

[Photoresist developer]
The photoresist developer that can be used in the present invention is not particularly limited as long as it does not dissolve the EL layer forming material. Specifically, a commonly used organic alkaline developer can be used, but in addition, an inorganic alkali or an aqueous solution capable of developing a resist can be used. It is desirable to wash with water after developing the resist.

  As the developer that can be used in the present invention, a developer whose solubility in an EL layer forming material such as a light emitting layer material is the above-mentioned solubility condition can be used.

[Photoresist stripper]
Furthermore, as the photoresist stripping solution that can be used in the present invention, it is necessary not to dissolve the EL layer but to dissolve the photoresist layer, and the photoresist solvent as described above is used as it is. It comes out. Further, when a positive resist is used, it can be peeled off using the solution mentioned as the resist developer after UV exposure.

  Further, a strong alkaline aqueous solution, a solvent such as dimethylformamide, dimethylacetamide, dimethyl sulfoxide, N-methyl-2-pyrrolidone, a mixture thereof, or a commercially available resist stripping solution may be used. After the resist is peeled off, it may be rinsed with 2-propanol or the like and further rinsed with water.

[Patterning method]
Specifically, in the patterning by the photolithography method used in the present invention, when a positive type photoresist is used, an EL layer is first formed on the entire surface, and then the photoresist material is dissolved in the photoresist solvent thereon. First, a photoresist layer is formed by applying and drying a photoresist solution over the entire surface. Next, this photoresist layer is subjected to pattern exposure, and the exposed portion of the photoresist is developed with a resist developer as described above. This development leaves only the unexposed photoresist. Then, the EL layer is patterned by removing the portion of the EL layer not covered with the photoresist.

  In addition, the method for forming the entire surface of the EL layer such as the light emitting layer and the buffer layer as described above is the same as the formation of the normal EL layer and is not particularly limited. Examples include spin coating methods, casting methods, dipping methods, bar coating methods, blade coating methods, roll coating methods, gravure coating methods, flexographic printing methods, spray coating methods, etc. It is done.

  When forming the buffer layer, it is desirable that the light-emitting layer coating solvent prevents the buffer layer and the light-emitting layer material from being mixed or dissolved during film formation of the light-emitting layer, and does not dissolve the buffer layer. From such a point of view, a solvent for coating the light emitting layer can be used in which the solubility in the buffer layer material is the above-mentioned solubility condition.

  Further, when two or more light emitting layers are formed in parallel, the light emitting layer coating solvent prevents the photoresist layer and the light emitting layer material from being mixed or dissolved during the formation of the light emitting layer for the second and subsequent colors, Furthermore, it is desirable not to dissolve the photoresist to protect the already patterned light emitting layer.

  From such a viewpoint, the light emitting layer coating solvent may be one having a solubility in a photoresist that satisfies the above-mentioned solubility conditions. For example, when the buffer layer is dissolved in a polar solvent such as water or DMF, DMSO or alcohol and the photoresist is a general novolak positive resist, isomers of benzene, toluene and xylene and their mixtures, mesitylene, tetralin , P-cymene, cumene, ethylbenzene, diethylbenzene, butylbenzene, chlorobenzene, dichlorobenzene isomers and mixtures thereof, anisole, phenetol, butylphenyl ether, tetrahydrofuran, 2-butanone, Ether solvents such as 1,4-dioxane, diethyl ether, diisopropyl ether, diphenyl ether, dibenzyl ether, diglyme, dichloromethane, 1,1-dichloroethane, 1,2-dichloroethane Chloro-based solvents such as chlorobenzene, trichloroethylene, tetrachloroethylene, chloroform, carbon tetrachloride, 1-chloronaphthalene, cyclohexanone, etc., but any other solvent that satisfies the conditions can be used. It may be.

  In addition, the buffer layer coating solvent in the case where the buffer layer is formed using a solvent as in the coating method is not particularly limited as long as the buffer material is dispersed or dissolved. For example, when it is necessary to form a buffer layer a plurality of times, it is necessary to use a buffer layer solvent that does not dissolve the photoresist material, and more preferably a buffer layer solvent that does not dissolve the light emitting layer. As the buffer layer solvent that can be used in the present invention, those having a solubility of the resist material that satisfies the above-mentioned solubility conditions can be used. More preferably, a buffer layer solvent having a solubility of the luminescent material that satisfies the above-mentioned solubility conditions can be used. Examples include solvents such as water, methanol, ethanol and other alcohols, dimethylformamide, dimethylacetamide, dimethyl sulfoxide, N-methyl-2-pyrrolidone, and other solvents that satisfy the conditions can be used. It is. Two or more solvents may be mixed and used.

  In the photolithography method, a wet method using a solvent that dissolves the EL layer and a dry etching process (dry method) can be used as a method for removing the EL layer in a portion not covered with the photoresist. It is preferable to use a dry etching process characterized by anisotropy.

  Accordingly, in the patterning using the photolithography method, the photoresist is patterned by applying a photoresist on the EL layer to be patterned, exposing and developing, and then removing the photoresist by a dry etching process. The patterning is preferably performed by removing the electroluminescent layer. If the electroluminescent layer where the photoresist has been removed by the dry etching process is removed, the edge of the etching can be made sharper. This is because it is possible to narrow the width of the film, and as a result, it is possible to perform patterning with higher definition.

  In the present invention, the reactive ion etching process is preferable among the dry etching processes. By using the reactive ion etching method, the organic material undergoes a chemical reaction and becomes a compound with a low molecular weight, so that it can be vaporized and evaporated to be removed from the substrate, resulting in high etching accuracy and a short time. This is because it is possible to process with

  In the dry etching process, it is preferable to use oxygen alone or a gas containing oxygen. By using oxygen alone or a gas containing oxygen, the organic light emitting layer can be decomposed and removed by oxidation reaction, unnecessary organic substances can be removed from the substrate, and etching accuracy is high and processing can be performed in a short time. This is because it becomes possible. Further, under this condition, the normally used oxide transparent conductive film such as ITO is not etched, and therefore, it is effective in that the electrode surface can be purified without impairing the electrode characteristics.

  Furthermore, it is preferable to use atmospheric pressure plasma for the dry etching process. By using atmospheric pressure plasma, dry etching, which normally requires a vacuum apparatus, can be performed under atmospheric pressure, and the processing time and cost can be reduced. In this case, the etching can utilize the fact that the organic material is oxidatively decomposed by oxygen in the atmosphere converted into plasma, but the gas composition of the reaction atmosphere may be arbitrarily adjusted by gas replacement and circulation.

  On the other hand, a method of removing a part of the EL layer by a wet method includes a method of removing the EL layer using a solvent capable of dissolving or peeling the EL layer, and further removing the EL layer in an ultrasonic bath using the solvent. And the like.

  As the solvent used at this time, it is necessary to dissolve or peel off the light emitting layer without peeling off the photoresist. In addition to the coating solvent for the light emitting layer, a solvent satisfying the above conditions can be selected.

  Furthermore, in the case of using an ultrasonic bath, patterning of an EL layer using a photoresist can be performed with high precision without any problems such as thinning of each pattern and outflow of material for forming an EL layer, and in a short time. This is preferable in that high-precision patterning is possible. Note that this ultrasonic bath may also be used when developing the photoresist.

  In the present invention, the ultrasonic conditions used in this ultrasonic bath are preferably performed at 25 ° C. at an oscillation frequency of 20 to 100 kilohertz for 0.1 to 60 seconds. Patterning with high accuracy is possible in a short time.

[Protective layer]
In particular, when the light emitting layer includes three types of light emitting layers and a full-color EL element is formed by patterning three times by a photolithography method, the first and second EL layers previously formed and It is preferable to include a step of forming a protective layer so that the end portion is not exposed. In the case where the first and second EL layers and the protective layer that covers the end portions thereof are not exposed, the second or third EL layer is formed in the second EL layer forming step and the third EL layer forming step. In addition, problems such as elution of the first and second EL layers and color mixing and pixel thinning can be prevented. Thereby, an EL element having a plurality of types of high-definition light emitting portions can be manufactured.

  The protective layer forming step in the present invention comprises a step of applying a protective layer forming coating solution so as to cover the EL layer formed by the above step, and a protective layer patterning step to be described later. To cover.

  The material used as such a protective layer-forming coating solution is not particularly limited as long as it is a material that can be patterned by a protective layer patterning step described later, but is easy to pattern, In addition, it is preferable to use the above-described photoresist or the like from the viewpoint that it can be stripped with a resist stripping solution used when finally removing each photoresist layer and each protective layer.

  In addition, the application | coating method of a protective layer, etc. in this process can be performed by the method similar to the EL layer etc. which were mentioned above. Further, this step may be performed after the photoresist layer remaining on the EL layer is peeled off with a photoresist stripping solution or the like. This is because a better protective layer can be formed.

  Next, the protective layer patterning step in the present invention is a step of developing after exposing the above-described protective layer so that the EL layer and its end portions are not exposed. About exposure and development in patterning of such a protective layer, patterning is performed so as to cover the EL layer with a larger width than the EL layer. That is, the edge of the EL layer is covered, and the protective layer is exposed and developed with a size that does not reach the position where the adjacent EL layer is formed. Thereby, the EL layer and its end are protected by the protective layer. Therefore, in the subsequent EL layer formation, the first or second EL layer does not come into contact with the second or third EL layer and can be prevented from eluting, and problems such as color mixing and pixel thinning can be prevented. be able to.

  The exposure and development methods in the protective layer patterning step can be performed by the same method as the above-described step of patterning the photoresist layer for EL layer.

  The following is an example of a step of patterning a light emitting layer by a photolithography method three times when a full color EL element is manufactured, and includes a step of forming a protective layer. In the following, “light emitting layer” means a layer formed by applying and drying a light emitting layer forming coating solution, and “light emitting part” means a light emitting layer formed at a predetermined position. It shall be.

  First, as shown in FIG. 2 (a), a light emitting layer 4 is applied on a substrate 1 provided with electrodes, and as shown in FIG. 2 (b), a photoresist layer 6 is laminated thereon. Next, as shown in FIG. 2 (c), only the portion for forming the first light emitting portion is masked with the photomask 7, and the other portions are exposed with the ultraviolet rays 8.

This is developed with a photoresist developer and washed to remove the photoresist layer in the exposed portion as shown in FIG. As shown in FIG. 2 (e), the portion where the photoresist layer is removed and the light emitting layer is exposed is removed by etching, and then the photoresist of the first light emitting portion is removed as shown in FIG. 2 (f). The first light emitting unit 4 is obtained by peeling the layer.
Next, a protective layer forming coating solution is applied so as to cover the first light emitting part 4 to form the protective layer 11, and further, the protective layer 11 is exposed and developed, whereby the first light emitting part 4 and its A protective layer 11 covering the end is formed (FIG. 2G).

  Next, in the same manner as described above, the second light emitting layer forming coating solution is applied to form the second light emitting layer 9. Further, a positive photoresist is applied on the entire surface thereof to form a second light emitting layer photoresist layer 6 '(FIG. 2 (h)).

  Next, as shown in FIG. 2 (i), the mask 8 is masked only at the position where the second light emitting portion is formed, and the ultraviolet ray 8 is exposed at a position other than the position where the second light emitting portion is formed, as described above. Then, the second light emitting layer photoresist layer 6 'is developed with a photoresist developer and washed. As a result, the second light emitting layer photoresist layer 6 'remains only in the portion where the second light emitting portion is formed (FIG. 2 (j)).

  Further, the second light emitting layer photoresist layer 6 ′ is removed, and the exposed second light emitting layer 9 is removed, so that the substrate 1 is covered with the second light emitting layer photoresist layer 6 ′. The 2nd light emission part 9 and the 1st light emission part 4 coat | covered with the 1st protective layer 11 remain (FIG.2 (k)).

  Here, the second light emitting layer photoresist layer 6 'on the second light emitting unit 9 is peeled off to expose the second light emitting unit 9 (FIG. 2L). Usually, at this time, the first protective layer 11 formed on the first light emitting portion 2 is also peeled off at the same time as the second light emitting layer photoresist layer 6 ′.

  Subsequently, as shown in FIG. 2 (m), a coating liquid for forming a protective layer is applied so as to cover the first light-emitting portion 4 and the second light-emitting portion 9 exposed in the above process, and further a second protective layer. 11 ′ is exposed and developed to form a second protective layer 11 ′ so that the first and second light emitting portions and the respective end portions thereof are not exposed. Thus, a second protective layer 11 ′ is formed to cover the first light emitting unit 4 and its end, the second light emitting unit 9 and its end. In addition, the 2nd protective layer formed on the 1st light emission part 2 and the 2nd protective layer formed on the 2nd light emission part may be connected, or may mutually be independent.

  Next, patterning of the light emitting portion of the third color is performed. The first light emitting unit 4 covered with the second protective layer 11 ′ formed so as to cover the first light emitting unit 4 and the end thereof, and the second light emitting unit 9 and the second light emitting unit 9 formed so as to cover the end thereof. As shown in FIG. 2 (n), a third light emitting layer forming coating solution is applied onto the substrate 1 on which the second light emitting portion 9 covered with the second protective layer 11 ′ is formed, and the third light emitting Layer 10 is formed. Further, a positive photoresist is applied thereon to form a third light emitting layer photoresist layer 6 ″. At this time, the first light emitting portion 4 and the second light emitting portion 9 are formed by the second protective layer 11 ′. The first light emitting part 4 and its end part, and the second light emitting part 9 and its end part are protected, so that they do not come into contact with the third light emitting layer 10. Thereby, the first light emitting part 4 And it becomes possible to prevent the 2nd light emission part 9 from eluting in the 3rd light emission layer 10 from an edge part.

  Next, as shown in FIG. 2 (o), only the position where the third light-emitting portion is formed is masked with a photomask 7, and an area other than the masked area is exposed with ultraviolet rays 8, and then developed with a photoresist developer. By washing, the third light emitting layer photoresist layer 6 ″ located outside the region where the third light emitting portion is formed is removed (FIG. 2 (p)).

  Next, the third light emitting layer 10 having the third light emitting layer photoresist layer 6 ″ on the surface remains by removing the exposed third light emitting layer 10 after the third light emitting layer photoresist layer 6 ″ is removed ( FIG. 2 (q)). In the third light emitting layer photoresist layer patterning step, when only the position where the third light emitting part is formed is subjected to pattern exposure through the photomask, one layer of second protection is provided on the first light emitting part 4 and the second light emitting part 9. The layer 11 ′ can be stacked.

  Finally, as shown in FIG. 2 (r), the photoresist layer and the protective layer located in the uppermost layer are peeled off (peeling step), and a second electrode layer is formed on each exposed light emitting layer. An EL element that emits light downward can be manufactured.

  The EL element manufactured by using the photolithography process as described above has the following characteristics different from those of EL elements manufactured by other manufacturing methods.

  First, unlike other manufacturing methods, the photolithographic method is characterized by the shape 12 of the end portion of the EL layer in order to remove unnecessary portions of the film once applied to the entire surface by etching (see FIG. 3A). In general manufacturing methods such as vapor deposition and coating, as shown in FIG. 3 (b), there is a thickness gradient at the end and the width of the non-uniform film thickness region is wide, whereas in the photolithography method, Since the patterning is performed by etching, as shown in FIG. 3A, the film thickness at the end is equal to the center, that is, the width of the non-uniform film thickness at the end is 15 μm or less, preferably 10 μm or less, particularly preferably. Is characterized by being 7 μm or less. The “film thickness non-uniform region” refers to a region where the film thickness is 90% or less of the average film thickness of the flat portion.

  In addition, for example, the inkjet method requires a structure called a partition wall (FIG. 3C), and the EL layer is structured to fit inside the insulating layer or the partition wall, whereas the photolithography method assists the partition wall and patterning. It is characterized in that it does not have any of the constituents to be formed and the surface treatment for assisting the patterning, and the EL layer end portion is formed on the insulating layer.

  EXAMPLES Next, although an Example demonstrates this invention further more concretely, this invention is not limited to description of a following example.

( Reference Example 1)
(Formation of insulating layer)
A patterned ITO substrate having a size of 6 inches and a thickness of 1.1 mm was washed to obtain a substrate and a first electrode layer. On the obtained substrate, silicon dioxide (SiO ₂ ) having a selectivity to an organic compound of 2.5 in a dry etching process was formed on the entire surface to a thickness of 2000 Å by sputtering. Further, a positive photoresist (manufactured by Tokyo Ohka Co., Ltd .; OFPR-800) was formed on the silicon dioxide film to a thickness of 1 μm. Then, it set to the alignment exposure machine with the exposure mask, and only the light emission part was exposed to ultraviolet rays. After developing for 20 seconds with a resist developer (manufactured by Tokyo Ohka Kogyo Co., Ltd .; NMD-3), it was washed with water to remove the photoresist in the exposed area. Thereafter, silicon dioxide in a portion where the photoresist was removed was removed by reactive ion etching using tetrafluoromethane as a reaction gas. The photoresist was removed with acetone to obtain an insulating layer of silicon dioxide.

(Deposition of the first buffer layer)
On the obtained substrate, 0.5 mL of a buffer layer coating solution (Bayer; BaytronP) was taken and dropped at the center of the substrate, and spin coating was performed on the opening of the insulating layer. The layer was formed by holding at 2500 rpm for 20 seconds. As a result, the film thickness was 800 angstroms.

(Deposition of the first light emitting layer)
As a first light emitting layer, 1 mL of a coating solution (70 parts by weight of polyvinyl carbazole, 30 parts by weight of oxadiazole, 1 part by weight of dicyanomethylenepyran derivative, 4900 parts by weight of monochlorobenzene) as a red light emitting organic material is taken on the buffer layer. Then, the solution was dropped on the center of the substrate, and spin coating was performed on the opening of the insulating layer. The layer was formed by holding at 2000 rpm for 10 seconds. As a result, the film thickness was 800 angstroms.

  2 mL of a positive type photoresist solution (manufactured by Tokyo Ohka Co., Ltd .; OFPR-800) was taken and dropped onto the center of the substrate to perform spin coating. The layer was formed by holding at 500 rpm for 10 seconds and then holding at 2000 rpm for 20 seconds. As a result, the film thickness was about 1 μm. Pre-baking was performed at 80 ° C. for 30 minutes. After that, it was set in an alignment exposure machine together with an exposure mask, and the portion where the light emitting layer other than the first light emitting portion was to be removed was exposed to ultraviolet rays. After developing with a resist developer (manufactured by Tokyo Ohka Co., Ltd .; NMD-3) for 20 seconds, it was washed with water to remove the photoresist layer in the exposed area. After post-baking at 120 ° C. for 30 minutes, the buffer layer and the light emitting layer in the portion where the photoresist layer was removed were removed by reactive ion etching using oxygen plasma. After removing the photoresist with acetone, 2 mL of a positive photoresist solution (manufactured by Tokyo Ohka Co., Ltd .; OFPR-800) was again taken and dropped onto the center of the substrate to perform spin coating. The layer was formed by holding at 500 rpm for 10 seconds and then holding at 2000 rpm for 20 seconds. As a result, the film thickness was about 1 μm. Pre-baking was performed at 80 ° C. for 30 minutes. Then, it set to the alignment exposure machine with the exposure mask, and exposed to ultraviolet rays so as to leave a photoresist layer having a width 10 μm larger than the width of the first light emitting portion. After developing with a resist developer (manufactured by Tokyo Ohka Co., Ltd .; NMD-3) for 20 seconds, it was washed with water to remove the photoresist layer in the exposed area. Post baking was performed at 120 ° C. for 30 minutes to obtain a substrate in which the first light emitting portion was protected with a photoresist layer having a width 10 μm larger than the width of the first light emitting portion.

(Deposition of second buffer layer)
0.5 mL of a buffer layer coating solution (Bayer; BaytronP) was taken on the obtained substrate and dropped onto the center of the substrate, and spin coating was performed on the opening of the insulating layer. The layer was formed by holding at 2500 rpm for 20 seconds. As a result, the film thickness was 800 angstroms.

(Deposition of second light emitting layer)
As a second light emitting layer, 1 mL of a coating liquid (70 parts by weight of polyvinylcarbazole, 30 parts by weight of oxadiazole, 1 part by weight of coumarin 6 and 4900 parts by weight of monochlorobenzene) as a green light emitting organic material is taken on the buffer layer, The solution was dropped on the center of the substrate, and spin coating was performed on the opening of the insulating layer. The layer was formed by holding at 2000 rpm for 10 seconds. As a result, the film thickness was 800 angstroms.

  2 mL of a positive type photoresist solution (Tokyo Ohka Co., Ltd .; OFPR-800) was taken and dropped onto the center of the substrate to perform spin coating. Hold at 500 rpm for 10 seconds, and then hold at 2000 rpm for 20 seconds. Layer formation. As a result, the film thickness was about 1 μm. Pre-baking was performed at 80 ° C. for 30 minutes. Then, it set to the alignment exposure machine with the exposure mask, and exposed the ultraviolet-ray to the part which wants to remove light emitting layers other than a 1st light emission part and a 2nd light emission part. After developing with a resist developer (manufactured by Tokyo Ohka Kogyo Co., Ltd .; NMD-3) for 20 seconds, it was washed with water to remove the photoresist in the exposed area. After post-baking at 120 ° C. for 30 minutes, the buffer layer and the light emitting layer in the portion where the photoresist layer was removed were removed by reactive ion etching using oxygen plasma. After removing the photoresist with acetone, 2 mL of a positive photoresist solution (OFPR-800 manufactured by Tokyo Ohka Kogyo Co., Ltd.) was again taken and dropped onto the center of the substrate to perform spin coating. The layer was formed by holding at 500 rpm for 10 seconds and then holding at 2000 rpm for 20 seconds. As a result, the film thickness was about 1 μm. Pre-baking was performed at 80 ° C. for 30 minutes. Then, it set to the alignment exposure machine with the exposure mask, and ultraviolet-ray-exposed so that a photoresist layer might remain in the width | variety 10 micrometers larger than the width | variety of a 1st light emission part and a 2nd light emission part. After developing with a resist developer (manufactured by Tokyo Ohka Kogyo Co., Ltd .; NMD-3) for 20 seconds, it was washed with water to remove the photoresist in the exposed area. The substrate was post-baked at 120 ° C. for 30 minutes to obtain a substrate protected with a photoresist having a width 10 μm larger than the width of the first light emitting portion and the second light emitting portion.

(Deposition of the third buffer layer)
0.5 mL of a buffer layer coating solution (Bayer; BaytronP) was taken on the obtained substrate and dropped onto the center of the substrate, and spin coating was performed on the opening of the insulating layer. The layer was formed by holding at 2500 rpm for 20 seconds. As a result, the film thickness was 800 angstroms.

(Deposition of the third light emitting layer)
As a third light emitting layer, 1 mL of a coating solution (70 parts by weight of polyvinyl carbazole, 30 parts by weight of oxadiazole, 1 part by weight of perylene, 4900 parts by weight of monochlorobenzene), which is a blue light emitting organic material, is taken on the buffer layer. It was dripped at the center and spin coating was performed on the opening of the insulating layer. The layer was formed by holding at 2000 rpm for 10 seconds. As a result, the film thickness was 800 angstroms.

  2 mL of a positive type photoresist solution (manufactured by Tokyo Ohka Co., Ltd .; OFPR-800) was taken and dropped onto the center of the substrate to perform spin coating. The layer was formed by holding at 500 rpm for 10 seconds and then holding at 2000 rpm for 20 seconds. As a result, the film thickness was about 1 μm. Pre-baking was performed at 80 ° C. for 30 minutes. Then, it set to the alignment exposure machine with the exposure mask, and exposed the ultraviolet-ray to the part which wants to remove light emitting layers other than a 1st light emission part, a 2nd light emission part, and a 3rd light emission part. After developing with a resist developer (manufactured by Tokyo Ohka Kogyo Co., Ltd .; NMD-3) for 20 seconds, it was washed with water to remove the photoresist in the exposed area. After post-baking at 120 ° C. for 30 minutes, the buffer layer and the light emitting layer where the photoresist layer has been removed are removed by reactive ion etching using oxygen plasma, and the first light emitting unit, the second light emitting unit, and A substrate in which the third light emitting portion was protected with a photoresist was obtained. Thereafter, all of the photoresist was removed with acetone to expose the patterned light emitting layer.

  After drying at 100 ° C. for 1 hour, Ca was deposited as a second electrode layer to a thickness of 500 angstroms, and Ag was deposited as a protective layer to a thickness of 2500 angstroms on the resulting substrate. Was made.

(Example 1 )
An organic EL device was produced in the same manner as in Reference Example 1 except that the insulating layer was formed as follows.

(Formation of insulating layer)
A patterned ITO substrate having a size of 6 inches and a thickness of 1.1 mm was washed to obtain a substrate and a first electrode layer. Take 0.5 ml of organoalkoxysilane (5% by weight isopropyl alcohol solution of TSL8113 manufactured by Toshiba Silicone Co., Ltd.) on the obtained substrate, drop it onto the center of the substrate, spin-coat, and 2000 angstrom over the entire surface. A film was formed. After the film formation, it was heated at 200 ° C. for 30 minutes to form a cured organopolysiloxane film. Further, a positive type photoresist (manufactured by Tokyo Ohka Co., Ltd .; OFPR-800) was formed on the obtained substrate with a thickness of 1 μm. Then, it set to the alignment exposure machine with the exposure mask, and only the light emission part was exposed to ultraviolet rays. After developing for 20 seconds with a resist developer (manufactured by Tokyo Ohka Kogyo Co., Ltd .; NMD-3), it was washed with water to remove the photoresist in the exposed area. Thereafter, the portion of the organopolysiloxane from which the photoresist was removed was removed by reactive ion etching using tetrafluoromethane as a reaction gas. The photoresist was removed with acetone to obtain an insulating layer of organopolysiloxane.

<Result>
In Reference Example 1 and Example 1 , an element on which a high-definition pattern was formed relatively easily and inexpensively could be obtained.

(Evaluation of light emission characteristics of EL elements)
In Reference Example 1 and Example 1 , the ITO electrode side was connected to the positive electrode, the Ag electrode side was connected to the negative electrode, and a direct current was applied by a source meter. Light emission was recognized from each of the first, second, and third light emitting portions when 10 V was applied.

(Insulation)
In Reference Example 1 and Example 1 , light emission could be confirmed only by the opening by visual evaluation. Moreover, when the voltage-current density characteristic was measured, the diode characteristic was shown and it confirmed that the short circuit did not occur. Even when dry etching is used for patterning by a photolithography method, the insulating layer is prevented from being eroded, and a short circuit between electrodes or between an electrode and a wiring is not caused.

1 substrate 2 first electrode 3 insulating layer 4 EL layer (light emitting layer, first light emitting part)
5 Second electrode 6, 6 ', 6 "Photoresist layer 7 Photomask 8 Ultraviolet light 9 Second light emitting layer (second light emitting portion)
10 3rd light emitting layer (3rd light emission part)
11, 11 ′ Protective layer 12 End shape 13 Partition wall 20 Insulating layer made of organic material 21 Wiring 22 Short circuit

Claims (9)

In a method for manufacturing an electroluminescent element having at least a first electrode, a plurality of types of electroluminescent layers, and a second electrode on a substrate,
Methyltrichlorosilane, methyltribromosilane, methyltrimethoxysilane, methyltriethoxysilane, methyltriisopropoxysilane, methyltrit-butoxysilane; ethyltrichlorosilane, ethyltribromosilane, ethyltrimethoxysilane, ethyltriethoxysilane, Ethyltriisopropoxysilane, ethyltri-t-butoxysilane; n-propyltrichlorosilane, n-propyltribromosilane, n-propyltrimethoxysilane, n-propyltriethoxysilane, n-propyltriisopropoxysilane, n -Propyltri-t-butoxysilane; n-hexyltrichlorosilane, n-hexyltribromosilane, n-hexyltrimethoxysilane, n-hexyltriethoxysilane, n-hexyltriiso Lopoxysilane, n-hexyltri-t-butoxysilane; n-decyltrichlorosilane, n-decyltribromosilane, n-decyltrimethoxysilane, n-decyltriethoxysilane, n-decyltriisopropoxysilane, n-decyltrit- Butoxysilane; n-octadecyltrichlorosilane, n-octadecyltribromosilane, n-ortadecyltrimethoxysilane, n-octadecyltriethoxysilane, n-octadecyltriisopropoxysilane, n-octadecyltri-t-butoxysilane; phenyltrichloro Silane, phenyltribromosilane, phenyltrimethoxysilane, phenyltriethoxysilane, phenyltriisopropoxysilane, phenyltri-t-butoxysilane; tetrachlorosilane, tetrabro Silane, tetramethoxysilane, tetrabutoxysilane, trichlorohydrosilane, tribromohydrosilane, trimethoxyhydrosilane, triethoxyhydrosilane, triisopropoxyhydrosilane, tri-t-butoxyhumanrosilane; trifluoropropyltrichlorosilane, trifluoropropyltribromosilane, Trifluoropropyltrimethoxysilane, trifluoropropyltriethoxysilane, trifluoropropyltriisopropoxysilane, trifluoropropyltri-t-butoxysilane; γ-glycidoxypropyltrimethoxysilane, γ-glycidoxypropyltriethoxysilane Γ-glycidoxypropyltriisopropoxysilane, γ-glycidoxypropyltri-t-butoxysilane; γ-aminopropyltri Toxisilane, γ-aminopropyltriethoxysilane, γ-aminopropyltriisopropoxysilane, γ-aminopropyltrit-butoxysilane; γ-mercaptopropyltrimethoxysilane, γ-mercaptopropyltriethoxysilane, γ-mercaptopropyltri Isopropoxysilane, γ-mercaptopropyltri-t-butoxysilane; β- (3,4-epoxycyclohexyl) ethyltrimethoxysilane, β- (3,4-epoxycyclohexyl) ethyltriethoxysilane, CF ₃ (CF ₂ ) ₃ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₅ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₇ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₉ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , (CF ₃ ) ₂ CF (CF ₂ ) ₄ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , (CF ₃ ) ₂ CF (CF ₂ ) ₆ CH ₂ CH ₂ Si (OCH ₃ ) ₃ , (CF ₃ ) ₂ CF (CF ₂ ) ₈ CH ₂ CH ₂ Si ( OCH ₃ ) ₃ , CF ₃ (C ₆ H ₄ ) C ₂ H ₄ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₃ (C ₆ H ₄ ) C ₂ H ₄ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₅ (C ₆ H ₄ ) C ₂ H ₄ Si (OCH ₃ ) ₃ , CF ₃ (CF ₂ ) ₇ (C ₆ H ₄ ) C ₂ H ₄ Si (OCH ₃ ) ₃ , CF ₃ (CF _{2) 3 CH 2 CH 2 Si} (OCH 2 CH 3) 3, CF 3 (CF 2) 5 CH 2 CH 2 Si (OCH 2 CH 3) 3, CF 3 (CF 2) 7 CH 2 CH 2 Si (OCH ₂ CH ₃ ) ₃ , CF ₃ (CF ₂ ) ₉ CH ₂ CH ₂ Si (OCH ₂ CH ₃ ) ₃ , and CF ₃ (CF ₂ ) ₇ SO ₂ N (C ₂ H ₅ ) C ₂ H ₄ CH ₂ Si (OC One or more of the _{3) 3} silicon compound selected from dissolved in a solvent, coated and heated, by hydrolysis polycondensation reaction of one or more of the silicon compounds Forming an insulating layer containing 90 wt% or more of an organopolysiloxane that is a hydrolysis condensate or a cohydrolysis condensate in the insulating layer;
An electroluminescent layer is formed by a coating method on a substrate on which at least the first electrode is formed, and patterned by using a photolithography method including a dry etching process using a predetermined gas, thereby patterning the electroluminescent layer. Forming a nescent layer;
A method for producing an electroluminescent device, comprising the step of forming the patterned electroluminescent layer a plurality of times.   The plurality of types of electroluminescent layers are three types of electroluminescent layers, and a full color electroluminescent device is manufactured by patterning the electroluminescent layer using a photolithography method three times. The manufacturing method of the electroluminescent element of Claim 1. A step of forming a protective layer on the patterned electroluminescent layer by a coating method so that an end thereof is not exposed;
Forming a type of electroluminescent layer different from the patterned electroluminescent layer by a coating method so as to cover a protective layer formed on the patterned electroluminescent layer. The manufacturing method of the electroluminescent element of Claim 1 or 2.   In the patterning step using the photolithography method, a photoresist is applied on the electroluminescent layer to be patterned, exposed, and developed to pattern the photoresist, and then a dry etching process using a predetermined gas 4. The method of manufacturing an electroluminescent element according to claim 1, wherein the electroluminescent layer in a portion where the photoresist is removed by the step is removed.   5. The method for manufacturing an electroluminescent element according to claim 1, wherein the dry etching process is a reactive ion etching process.   6. The method for manufacturing an electroluminescent element according to claim 1, wherein the predetermined gas is a simple oxygen or a gas containing oxygen.   The method for manufacturing an electroluminescent element according to claim 1, wherein the insulating layer is provided between the first electrode and the second electrode.   8. The electroluminescent layer according to claim 1, wherein the insulating layer is provided between the wiring on the substrate and the first electrode and / or between the wiring on the substrate and the second electrode. A method for manufacturing a nescent element. The step of forming the protective layer by a coating method includes a step of applying a coating liquid for forming a protective layer so as to cover the patterned electroluminescent layer, the patterned electroluminescent layer, and an end thereof. 4. The method of manufacturing an electroluminescent element according to claim 3 , further comprising a step of developing after exposing the protective layer so that the portion is not exposed.

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