JP5999789B2 - Method for manufacturing organic electroluminescent lighting device - Google Patents

Description

The present invention (also referred to as an organic EL lighting device.) The organic electroluminescent lighting device using an organic material in the light emitting element relates to a method for manufacturing, and more particularly, efficient method for manufacturing an organic EL lighting equipment can be produced.

  An organic EL lighting device has a structure in which a light-transmitting electrode layer, an organic layer containing an organic light-emitting material, and an electrode layer regardless of light-transmitting properties are sequentially stacked on a light-transmitting substrate. A planar light source that transmits generated light through a translucent electrode layer and translucent substrate and emits it from the light emitting surface to the outside. It is a thin film that emits light at a low voltage and has excellent high-speed response. Therefore, the utility value is high.

  As shown in the top view of FIG. 5 and the side view of FIG. 6, this type of organic EL lighting device has a translucent electrode layer 2 and an organic layer 3 on a translucent substrate 1, regardless of translucency. The light emitting material having a configuration in which the electrode layer 4 is sequentially stacked and the holes and electrons injected from the electrodes sandwiching the organic layer into the organic layer are combined to be in an excited state is a low energy level or Light emitted when returning to the ground state is emitted from the light emitting surface L.

  In such an organic EL lighting device, the translucent electrode layer is made of indium tin oxide (ITO) or the like, and compared with the other electrode layer formed of a metal thin film or the like regardless of translucency. The resistance increases and the resistance increases as the distance from the power supply terminal of the translucent electrode layer increases, and a voltage drop occurs due to the wiring resistance, so that the electric field also decreases, resulting in darkness and inevitably uneven brightness. For this reason, the auxiliary electrode 5 is provided on the translucent electrode layer, and the fall of resistance value is suppressed. Since this auxiliary electrode is made of metal or the like and has a light-shielding property, it is formed by patterning on a part of the surface of the translucent electrode layer, and further for suppressing conduction between the electrode layers through the auxiliary electrode and the organic layer. It is necessary to provide an insulating coating 6 that covers the auxiliary electrode.

  Such an auxiliary electrode and an insulating film are manufactured as follows using photolithography. A light transmissive electrode layer is formed by stacking a light transmissive electrode material on a light transmissive substrate. An auxiliary electrode material having a desired pattern is formed thereon by a photolithography process or the like. Specifically, an auxiliary electrode material film is formed on one surface on the translucent electrode layer, a negative or positive resist is applied thereto, and exposure, development, and development are performed through a mask formed in a desired pattern. After the auxiliary electrode material film is formed in a desired pattern by etching, the resist remaining on the auxiliary electrode is peeled off to create an auxiliary electrode layer. On the obtained auxiliary electrode layer, an insulating film made of a polyimide material is formed by the same photolithography process. Then, an organic layer and an electrode layer are formed, and an organic EL lighting device is manufactured. Since the organic EL lighting device repeatedly performs the photolithography process in order to form the auxiliary electrode and the insulating film, the number of manufacturing processes is large and the increase in cost cannot be avoided.

  As a manufacturing method that improves the efficiency of an organic EL device having an auxiliary electrode, for example, an auxiliary electrode is provided on a transparent electrode layer on a substrate, the auxiliary electrode is covered with an insulating layer, and then the transparent electrode layer excluding the light emitting region An insulating layer is formed on the second terminal portion, an organic layer is formed over the entire surface of the substrate, a second electrode layer is formed on the light emitting region and the second terminal portion on the formed organic layer, and a second electrode layer is formed An organic EL device manufacturing method (Patent Document 1) that removes an organic layer in a region that is not exposed, exposes the first electrode layer of the first terminal portion, and forms a sealing film in a portion excluding the terminal portion. It has been reported. The manufacturing method of the organic EL device described in Patent Document 1 is a method of increasing the manufacturing efficiency by reducing the number of times of alignment between the substrate and the mask in order to form the connection between the electrode and the terminal on the substrate. The formation efficiency of the insulating film cannot be achieved.

  In addition, after forming the metal pattern using the photosensitive resin pattern on the substrate as a mask, the substrate is heated to flow the photosensitive resin pattern, and the side surface region of the metal pattern is covered with the photosensitive resin, A method for protecting a metal pattern that suppresses oxidation of the metal pattern (Patent Document 2) has been reported.

JP2007-733338 JP-A-57-53966

An object of the present invention can be efficiently produced, it is to provide a method of manufacturing an organic EL lighting equipment which can be reduced in cost.

  As a result of studying a method capable of reducing the number of manufacturing steps of the organic EL lighting device, the present inventor has obtained an insulating film provided by covering the auxiliary electrode by etching in the final stage of the photolithography process for forming the auxiliary electrode. If the resist remaining on the auxiliary electrode formed in the pattern is used to cover and form the side surface of the auxiliary electrode, the knowledge that the photolithography process for forming the insulating film can be omitted is obtained. Based on this, the present invention has been completed.

That is, the present invention includes a pair of electrode layers including a light-transmitting electrode layer provided on a light-transmitting substrate, and an organic layer sandwiched between the pair of electrode layers and containing an organic electroluminescent material. A light-shielding auxiliary electrode provided on and in contact with a part of the light-transmitting electrode layer, and an organic electroluminescence lighting device manufacturing method comprising an insulating film covering the auxiliary electrode, An auxiliary electrode material film was formed on the translucent electrode layer, a resist was applied on the auxiliary electrode material film, and a residual resist not having a reverse tapered portion and an auxiliary electrode having a tapered portion were formed by a photolithography process. after, Seki the residual resist in the production method of the organic electroluminescent lighting device characterized by forming the insulating film by covering the auxiliary electrodes to flow by heating above the glass transition temperature That.

The present invention also includes a pair of electrode layers including a light-transmitting electrode layer provided on a light-transmitting substrate, and an organic layer sandwiched between the pair of electrode layers and containing an organic electroluminescent material. A light-shielding auxiliary electrode provided on and in contact with a part of the light-transmitting electrode layer, and an organic electroluminescence lighting device manufacturing method comprising an insulating film covering the auxiliary electrode , An auxiliary electrode material film is formed on the translucent electrode layer, a resist is coated on the auxiliary electrode material film to form a resist film, and exposure and development are performed to form a residual resist having no reverse taper portion. Etching the auxiliary electrode material film to form an auxiliary electrode having a tapered portion, and then heating and flowing the residual resist to a temperature higher than the glass transition temperature to cover the auxiliary electrode to form the insulating film. Characterize Machine method of manufacturing an electroluminescent lighting device.

The manufacturing method of the organic electroluminescence lighting device of the present invention can reduce the number of manufacturing steps and reduce the manufacturing cost.

It is explanatory drawing which shows a part of process of the manufacturing method of the organic electroluminescent illuminating device of this invention. It is explanatory drawing which shows a part of process of the manufacturing method of the organic electroluminescent illuminating device of this invention. It is a block diagram which shows an example of the organic electroluminescent illuminating device obtained by the manufacturing method of the organic electroluminescent illuminating device of this invention. It is process drawing which shows an example of the manufacturing method of the organic electroluminescent illuminating device of this invention. It is a top view which shows an example of an organic electroluminescent illuminating device. It is a side view which shows an example of an organic electroluminescent illuminating device.

A method of manufacturing an organic electroluminescence lighting device according to the present invention includes a pair of electrode layers including a light-transmitting electrode layer provided on a light-transmitting substrate, and an organic EL substance sandwiched between the pair of electrode layers. A light-shielding auxiliary electrode provided in contact with a part of the light-transmitting electrode layer, and an insulating film covering the auxiliary electrode. An auxiliary electrode material film is formed on the translucent electrode layer, a resist is applied on the auxiliary electrode material film, and an auxiliary having a residual resist and a taper portion not having a reverse taper portion by a photolithography process. After the electrode is formed, the residual resist is heated to flow above the glass transition temperature to flow, and the auxiliary electrode is covered to form the insulating film.

  The manufacturing method of the organic EL lighting device of the present invention includes a step of forming a translucent electrode layer which is one electrode layer of a pair of electrode layers mainly on a translucent substrate, and an auxiliary electrode on the translucent electrode layer. And a step of forming an insulating film, a step of forming an organic layer containing an organic EL material, and a step of forming the other electrode layer of the pair of electrode layers.

  The light-transmitting substrate used for manufacturing the organic EL lighting device receives light from a light-emitting material contained in an organic layer provided via a light-transmitting electrode layer described later, and emits light from a light-emitting surface facing the incident surface. It is preferable that the transmittance of light emitted from the light emitting material is high. As the translucent substrate, for example, quartz glass, soda glass, borosilicate glass, lead glass, aluminosilicate glass, borate glass, phosphate glass, a resin film, or the like can be used. As the translucent substrate, for example, a substrate having a thickness of 0.1 to 2 mm can be used.

  A translucent electrode layer is laminated on the translucent substrate. The translucent electrode layer constitutes a pair of electrode layers sandwiching the organic layer, and is preferably formed of a material having a high light transmittance from the organic layer. The translucent electrode layer may be an anode or a cathode, but can be formed as an anode of indium tin oxide (ITO), indium zinc oxide (IZO), or the like. The translucent electrode layer is laminated on a predetermined region of the translucent substrate by a sputtering method, vapor deposition method, CVD method, etc. through a shadow mask, or is uniformly formed by a sputtering method, vapor deposition method, CVD method, etc. The translucent electrode film thus formed can be formed by a photolithography method. In order to form a connection portion with a wiring member at one end of the translucent electrode layer, it is preferable to extend one end. The translucent electrode layer can be formed to a thickness of 100 to 300 nm, for example.

  An auxiliary electrode is formed on the translucent electrode layer. The auxiliary electrode is preferably formed of a conductive material that can reduce the resistance of the translucent electrode layer. As the auxiliary electrode material, metals such as chromium, aluminum, molybdenum, niobium, and neodymium, and these An alloy, aluminum-neodymium (ANL), molybdenum-niobium, molybdenum-aluminum, or the like can be used. These may have a laminated structure, for example, a two-layer structure such as Mo / Al · Nd, Mo · Nb / Al · Nd, or a three-layer structure such as Mo / Al / Mo. Since these auxiliary electrode materials do not have translucency, it is preferable to provide them in a part of the surface of the translucent electrode layer. For example, a comb shape, a ladder shape, a lattice shape, or the like is selected. Can do. Moreover, it is preferable to provide also in the edge part of a translucent electrode layer from the further reduction in resistance and uniform resistance of a translucent electrode layer being attained. After the auxiliary electrode material film is formed on the translucent electrode layer uniformly, for example, to a thickness of 10 to 500 nm, etc., using the auxiliary electrode material by sputtering, vacuum deposition, CVD, or the like. The auxiliary electrode material film is formed by a photolithography method while suppressing a decrease in the light emission area of the illumination device such as a desired pattern, for example, a width of 10 to 100 μm. Specifically, a resist is applied on the auxiliary electrode material film, and pre-baking, exposure, development for solidifying the applied resist, removal of the rinse liquid used for development as necessary, and the resist and auxiliary electrode material film After baking for improving the adhesiveness, etching is performed to form an auxiliary electrode material film in a desired pattern, that is, an auxiliary electrode having a desired shape.

  The resist may be either a negative type in which the solubility in the developing solution is reduced by exposure or a positive type in which the solubility in the developing solution is increased by exposure, but the resist used here forms an insulating film of the auxiliary electrode It is a material that can suppress conduction between the auxiliary electrode and the electrode layer, and has high adhesion to the translucent electrode layer and the organic layer, and preferably has high light transmittance from the organic layer. Polyimide photosensitive resin, acrylic photosensitive resin, novolak photosensitive resin, and the like can be used. These can be prepared by dispersing a binder resin, a photosensitive monomer such as polyimide, acrylic or novolac, a photopolymerization initiator, and a coupling agent in a solvent. Examples of the solvent used for the resist include propylene glycol monomethyl ether acetate (PGMEA) and diethylene glycol methyl ethyl ether (MEC). A dispersant, a concentration adjusting agent, and the like can be used as necessary. As an example of the composition of these resists, the binder resin is 10 to 20% by mass, the photosensitive monomer is 10 to 20% by mass, the photopolymerization initiator is 1 to 5% by mass, the coupling agent is 0.1 to 2% by mass, and the solvent. 60-80 mass% can be mentioned. The resist can be applied by using a coater or the like, and the coating thickness can be 0.1 to 5 μm, preferably 0.5 to 2 μm, for example.

  Further, although related to the developer used for the development described later, in order to facilitate the flow to the side surface of the auxiliary electrode and to facilitate the coating thereof, it is formed as shown by the dotted line in FIG. It is preferable that the residual resist 5f remaining on the auxiliary electrode has a reverse taper shape. Here, in FIG. 1A, 1 is a translucent substrate, 2 is a translucent electrode layer, 5a is an auxiliary electrode material film formed on the translucent electrode layer, and 5b is applied to the auxiliary electrode material film. A resist film is shown. In order to form a reverse-tapered residual resist from the resist film, it is preferable to use an acrylic photosensitive resin or the like for the resist.

  The pre-baking after the resist coating is intended to solidify the resist by volatilizing and removing the solvent, and can be performed at around 100 ° C. for 30 to 180 seconds, for example.

  The exposure is performed using a mask capable of exposing the auxiliary electrode portion when the resist to be used is negative, and using a mask capable of exposing the portion excluding the auxiliary electrode in the case of a positive resist. The mask used for the exposure is preferably selected according to the shape of the resist remaining on the auxiliary electrode pattern after the etching in accordance with a development or etching process described later. In order to form the inversely tapered residual resist 5f, for example, when the auxiliary electrode is formed to have a width of 10 to 100 μm, the negative resist is formed so that the upper surface width of the developed residual resist 5f is 20 to 200 μm. It is preferable to use the mask 5c (FIG. 1A). The light ray used for the exposure may be any active ray that can polymerize the monomer contained in the resist, and ultraviolet rays are preferably used. In order to form a reverse-tapered residual resist, although it is related to the developer used, the traveling distance in the resist film, that is, the arrival point becomes shorter as exposure using the negative mask becomes the peripheral portion. Exposure is preferably performed. For example, mixed lines such as g-line (wavelength 436 nm), h-line (wavelength 405 nm), i-line (wavelength 365 nm) can be used.

  Any method may be used for development after exposure, and a shower method, a dip method, a paddle method, or the like can be selected as appropriate. As the developer, an organic alkali developer such as tetramethylammonium hydroxide (TMAH) or an inorganic alkali developer such as alkali hydroxide or alkali carbonate such as potassium hydroxide is used for the positive resist. A developer such as TMAH or xylene-based organic solvent can be used for the negative resist. To form the inversely tapered residual resist 5f (FIG. 1B), it is preferable to use TMAH as the developer. After the developing solution, unnecessary portions are completely removed with a rinsing solution such as pure water, and if necessary, the substrate is heated at a temperature lower than the glass transition temperature of the resist, for example, 90 to 150 ° C. for 30 seconds to 5 minutes. As the liquid is dried, the adhesion between the resist and the auxiliary electrode and between the auxiliary electrode and the translucent electrode can be improved.

Etching of the auxiliary electrode material film can be performed by either dry etching or wet etching. As dry etching, any method such as plasma etching, chemical etching, reactive ion etching, etc. may be used. Fluorine compounds such as F ₂ , CF ₄ , C ₂ F ₆ , CHF ₃ , SF ₆ , carbon tetrachloride, Isotropic dry etching using an etching gas containing oxygen and oxygen, and other examples of indium tin oxide include those using methanol and argon. As wet etching, any method such as shower type, dip type, batch type, etc. may be used.For aluminum, etc., for phosphoric acid and nitric acid and, if necessary, acetic acid, molybdenum, tungsten, tantalum, etc. For hydrofluoric acid, nitric acid and, if necessary, acetic acid, chromium, etc., ceric ammonium nitrate and perchloric acid, and for indium tin oxide, use an etching solution containing hydrochloric acid and nitric acid. it can. Etching of the auxiliary electrode material film is preferably performed so as to have a tapered portion that expands toward the translucent electrode layer on the side surface of the auxiliary electrode in order to facilitate the covering of the insulating film. When the inversely tapered residual resist 5f is formed, the auxiliary electrode material film tends to be isotropically etched as shown in FIG. 1C, and a tapered portion 5t is formed on the side surface of the auxiliary electrode 5. There is a high possibility. As shown in FIG. 2A, when the residual resist 5h having no reverse tapered portion is formed, as shown in FIG. 2B, the auxiliary electrode material film has the tapered portion 5t together with the ashing of the residual resist. It is preferable to perform etching. In order to form the tapered portion 5t on the side surface of the auxiliary electrode, it is preferable to perform dry etching using a mixed gas containing oxygen gas.

  The residual resist remaining on the auxiliary electrode formed in a desired pattern is heated to the glass transition temperature or higher to flow from the upper surface to the side surface of the auxiliary electrode to cover the entire auxiliary electrode, thereby forming an insulating film. When the auxiliary electrode has a tapered portion that expands toward the translucent electrode layer on the side surface, the residual resist flows and is easily guided to the tapered portion, so that the insulating film 5e covering the auxiliary electrode can be easily formed. (FIG. 1 (d), FIG. 2 (d)). It is preferable to adjust the heating within a range in which the resist flows sufficiently on the side surface of the auxiliary electrode to sufficiently cover the flow amount onto the translucent electrode layer. The heat treatment may be a batch treatment or a single wafer treatment, and can be performed using a firing furnace or a heat circulation furnace. The conditions are, for example, 180 to 250 ° C. in a nitrogen atmosphere, preferably 200 to 230. Examples thereof include 10 to 90 minutes at 0 ° C. For example, the insulating coating can have a thickness of 0.1 to 3 μm, more preferably a thickness of 1 to 2 μm.

  Thereafter, an organic layer is formed on the translucent electrode layer and the insulating coating. The formation method of the organic layer is not limited as long as a light emitting material is used, but there are a plurality of hole transport layers, electron transport layers, and a plurality of hole injection layers, electron injection layers, and the like sandwiching the light emitting layer. It is good also as what is comprised by these layers.

  The hole injection layer lowers the hole injection barrier from the translucent electrode layer of the anode to the organic layer, and relaxes the difference in energy level between the anode and the hole transport layer, so that holes injected from the anode For example, an arylamine derivative such as copper phthalocyanine or a star-bust type aromatic amine, or these hole-injecting organic materials. It can be formed using a hole injection material capable of lowering a driving voltage by chemically doping an inorganic material such as molybdenum oxide or an organic material such as F4-TCNQ to lower the injection barrier.

  The hole transport layer is, for example, bis (di (p-tolyl) aminophenyl) -1,1-cyclohexane, TPD, N, N′-diphenyl-NN—bis (1-naphthyl) -1,1 ′. -Biphenyl) -4,4'-diamine (α-NPD) and other hole transport materials such as starburst aromatic amines and triphenyldiamines.

  The light-emitting layer is a layer containing a light-emitting material that can recombine electrons and holes injected from an electrode. When electrons and holes are recombined in the light-emitting material, excitons are formed to enter an excited state. Become. Here, an excited state having the same electron spin multiplicity as the ground state is a singlet excited state, and an excited state having a different electron spin multiplicity is a triplet excited state. Luminescence is obtained when returning from the excited state to the low level or ground state, and fluorescence is emitted when returning from the singlet excited state to the low level or ground state. Alternatively, phosphorescence is emitted when returning to the ground state. Examples of the luminescent material include tris (8-quinolinol) aluminum complex (Alq3), bisdiphenylvinylbiphenyl (BDPVBi), 1,3-bis (pt-butylphenyl-1,3,4-oxadiazolyl). ) Phenyl (OXD-7), N, N′-bis (2,5-di-t-butylphenyl) perylenetetracarboxylic acid diimide (BPPC), 1,4 bis (Np-tolyl-N-4-) Examples thereof include low-molecular compounds such as (4-methylstyryl) phenylamino) naphthalene and high-molecular compounds such as polyphenylene vinylene polymers.

  In addition, the light emitting material may be composed of a binary system of a host and a dopant. In a binary light emitting material, the excited state energy generated by the host molecule is transferred to the dopant molecule, and the dopant molecule is Emits light. As the host compound, the above light-emitting material, electron transporting material, or hole transporting material can be used. For example, quinolinol metal complexes such as Alq3 and quinacridone derivatives such as 4-dicyanomethylene-2-methyl-6- (p-dimethylaminostyryl) -4H-pyran (DCM) and 2,3-quinacridone, and 3- (2 '-Benzothiazole) -7-diethylaminocoumarin and the like doped with a coumarin derivative, electron transporting material bis (2-methyl-8-hydroxyquinoline) -4-phenylphenol-aluminum complex, condensed with perylene, etc. Doped with ring aromatic, or 4,4'-bis (m-tolylphenylamino) biphenyl (TPD), a hole transporting material doped with rubrene, etc., doped with carbazole compound with platinum complex or iridium complex Can be used.

  These luminescent materials can be selected according to the target luminescent color of the organic EL lighting device, specifically, Alq3 for green light emission, quinacdrine or coumarin as a dopant, DPVBi for blue light emission, Perylene and distyrylarylene derivatives as dopants, such as OXD-7 for green to bluish green emission, DCM, DCJTB, etc. for red to orange emission, and rubrene as dopant for yellow emission. Can be used. In order to obtain white light emission, a combination of Alq3 as a host and DCM (orange) as a guest can be used as a light emitting material. As the light emitting layer for white light emission, a three-layer laminated structure containing light emitting materials emitting red, green, and blue, or a two-layer laminated structure containing light emitting materials emitting complementary colors such as blue and yellow, respectively. Further, by forming the light emitting materials of these colors by multi-component co-evaporation or the like, a single layer structure in which they are mixed can be obtained. Furthermore, the light-emitting material constituting each layer in the three-layer or two-layer stacked structure can be a light-emitting layer in which red, blue, green, and the like are sequentially arranged in the horizontal direction.

  The electron transport layer may be, for example, an oxadiazole derivative such as 2- (4-biphenylyl) -5- (4-t-butylphenyl) -1,3,4-oxadiazole (Bu-PBD), OXD-7, etc. In addition, an organic material such as a triazole derivative or a quinolinol-based metal complex, or an electron transporting material obtained by chemically doping an electron donating material such as an alkali metal such as lithium to these electron transporting organic materials can be used.

  The electron injection layer alleviates the difficulty in injecting electrons due to the large energy difference between the work function of a metal material such as aluminum used for the cathode and the electron affinity (LUMO level) of the electron transport layer. Therefore, it may be formed of a substance having a small work function selected from an alkali metal such as lithium or cesium, a fluoride or oxide of an alkaline earth metal such as calcium, or magnesium silver or a lithium aluminum alloy. preferable. The thickness of the electron injection layer can be set to 1 to 10 nm, for example.

  These electron injection layer, electron transport layer, light-emitting layer, hole transport layer, and hole injection layer are desired through a shadow mask by a resistance heating vacuum deposition method, MBE method, laser ablation method, or the like using the above materials. You may form into a film in this shape. In addition, when a polymer material is used for forming these layers, it can be formed into a desired shape by using an ink-jet method in a liquid state, and spin coating or slit coating is performed as a photosensitive coating solution, and photolithography is performed. It can also be formed into a desired shape by the method. As for the thickness of the organic layer, each layer can be formed to have a thickness of 5 to 500 nm and a total of 100 to 1000 nm.

  The other electrode layer of the pair of electrode layers is formed on the organic layer. The other electrode layer provided on the organic layer constitutes a pair of electrode layers together with the translucent electrode layer, and is not required to be translucent. When the translucent electrode layer is formed of the above translucent electrode material, for example, it can be formed as a light-shielding cathode of a metal thin film such as aluminum or silver, so that the organic layer emits light toward the translucent electrode layer. It is preferable because it can reflect and suppress a decrease in the amount of light emitted from the light emitting surface. The electrode layer can be formed by a vacuum deposition method, a sputtering method, or the like. Moreover, in order to form a connection part with a wiring member in the end of an electrode layer, it is preferable to provide one end extended. The thickness of the electrode layer is preferably thick considering the voltage drop due to the wiring resistance, and can be set to, for example, 50 to 300 nm.

  One end of the wiring member is connected to a connection portion formed by extending one end of the translucent electrode layer and the electrode layer. A wiring member having a width over the entire width of one end of the electrode can be used in order to suppress an increase in resistance of the connection portion. A film such as copper polyimide can be applied as the wiring member. Copper polyimide is preferable because it has electrical conductivity, low resistance, and flexibility, so that it can be connected without precise positioning. Further, the other end of the wiring member is connected to a connection terminal of a substrate provided with a lighting circuit, a control circuit for the lighting circuit, and the like, so that external power can be supplied to the translucent electrode layer and the electrode layer.

The organic EL lighting device obtained by the method for manufacturing an organic EL lighting device of the present invention is characterized in that an insulating film is formed of a resist remaining on an auxiliary electrode formed by a photolithography process. After etching the auxiliary electrode formation by photolithography, the resist remaining on the auxiliary electrode formed in a desired pattern is heated above its glass transition temperature to form an insulating film, thereby reducing the number of manufacturing steps and efficiently It is possible to manufacture, and it is possible to emit light with a certain luminance while suppressing conduction between the auxiliary electrode and the electrode. As the organic EL lighting device, an example of a white light emitting organic EL lighting device is shown in FIG. The white light-emitting organic EL lighting device shown in FIG. 3 covers the translucent electrode layer 2 on the translucent substrate 1, the auxiliary electrode 5 formed on a part of the translucent electrode layer 2, and the auxiliary electrode 5. The insulating layer 5e, the organic layer 3, and the electrode layer 4 are provided. The organic layer 3 is sequentially formed on the translucent electrode layer 2 and the insulating layer 5e with a hole injection layer 31a, a hole transport layer 32a, and a red light emitting layer. It consists of a laminated body in which an RGB light emitting layer 3b having 3Rb, a green light emitting layer 3Gb, and a blue light emitting layer 3Bb, an electron transport layer 3c, and an electron injection layer 3d are laminated.

  An example of the manufacturing method of the organic EL lighting device of the present invention will be specifically described.

As shown in FIG. 4, an ITO light-transmitting electrode film is laminated on a glass substrate 1 which is a light-transmitting substrate by a vacuum sputtering method, a vacuum evaporation method, or the like, and the light-transmitting electrode film is formed by a photolithography method. It exposes and forms in a desired shape by dry etching or wet etching, and the translucent electrode layer 2 is formed. Thereafter, an auxiliary electrode material such as ANL or Cr is used, and an auxiliary electrode material film 5a is formed on the entire surface of the translucent electrode layer 2 by a vacuum deposition method, a sputtering method, a CVD method, or the like (a). A negative resist is applied on the auxiliary electrode material film in a thickness of 0.1 to 5 μm and heated at about 90 ° C. for 90 seconds to form a resist film 5b (b). Thereafter, the resist film 5b is exposed through the mask 5c formed in the auxiliary electrode pattern (c). As the mask 5c, a mask having a pattern wider than the width of the auxiliary electrode pattern by a taper is used so as to form a residual resist having a reverse taper shape. Exposure using a crosstalk of g-line, h-line, i-line, performs the irradiation dose as 50~200mJ / cm ^2. Development using TMAH, rinsing with pure water, forming a resist film 5b on the resist pattern 5d, heating at 90 to 150 ° C. for less than the glass transition temperature of the resist for 1 minute, drying the rinsing liquid and resist and auxiliary electrode (D). The portion of the auxiliary electrode material film 5a not covered with the resist pattern 5d is removed by dry etching (e). In a nitrogen atmosphere, heating is performed for 30 minutes at a temperature of 230 ° C., which is equal to or higher than the glass transition temperature of the resist, and the resist pattern on the auxiliary electrode 5 is caused to flow to the side surface of the auxiliary electrode to form an insulating film 5e covering the auxiliary electrode .

  Then, a hole transport material such as α-NPD, a light emitting material selected such that Alq3, DPVBi, DCM or the like can obtain white light, an electron transport material such as OXD-7, a vacuum evaporation method by resistance heating, or the like Then, a thin film is sequentially formed to form a hole injection / transport layer 3a, a light emitting layer 3b, and an electron transport layer 3c. Next, an electron injection material such as lithium fluoride is stacked on the electron transport layer 3c by a vacuum deposition method to form an electron injection layer 3d. Further, an electrode layer 4 is formed by laminating thin films by vacuum deposition using an electrode material such as aluminum (g).

  Also, as a hole transport material, an ink for ink jet is prepared using poly (3,4-ethylenedioxythiophene) (PEDOT) and polystyrene sulfonic acid (PSS) system, polyaniline and PSS system, A hole transport layer is formed, and a polyparaphenylene vinylene (PPV) derivative, a polyfluorene (PF) derivative, other polythiophene (PAT), polyparaphenylene (PPP) is used as a light emitting material, and ink jet A light emitting layer can also be formed by an ink jet method.

  After that, a wiring member made of a polyimide film laminated with a copper foil is connected to the connection end of the translucent electrode layer and the electrode layer by thermocompression bonding, and the other end is connected to a lighting circuit, a lighting circuit control circuit, and the like. An organic EL lighting device is obtained by connecting to the connection terminal of the provided substrate.

  As another example of the manufacturing method of the organic EL lighting device of the present invention, a resist film to be formed on the auxiliary electrode material film 5a is formed using a positive resist, and a mask capable of exposing portions other than the auxiliary electrode is used. Exposure may be performed.

DESCRIPTION OF SYMBOLS 1 Translucent substrate 2 Translucent electrode layer 3 Organic layer 31a Hole injection layer 32a Hole transport layer 3b Light emission layer 3Rb Red light emission layer 3Gb Green light emission layer 3Bb Blue light emission layer 3c Electron transport layer 3d Electron injection layer 4 Electrode layer 5 Auxiliary Electrode 5a Auxiliary Electrode Material Film 5b Resist Film 5c Mask 5d Resist Pattern 5e Insulating Film 5f Reverse Tapered Residual Resist 5h Residual Resist

Claims (4)

A pair of electrode layers including a light-transmitting electrode layer provided on the light-transmitting substrate; and an organic layer sandwiched between the pair of electrode layers and containing an organic electroluminescent material, A method for producing an organic electroluminescent lighting device, comprising: a light-shielding auxiliary electrode provided in contact with a part of the conductive electrode layer; and an insulating film covering the auxiliary electrode,
An auxiliary electrode material film is formed on the translucent electrode layer, a resist is applied on the auxiliary electrode material film, and a residual resist having no reverse taper portion and an auxiliary electrode having a taper portion are formed by a photolithography process. Thereafter, the residual resist is heated to flow above the glass transition temperature to flow, and the auxiliary electrode is covered to form the insulating film, and the method for manufacturing the organic electroluminescent lighting device is characterized in that: 2. The method of manufacturing an organic electroluminescence lighting device according to claim 1, wherein a mixed gas containing oxygen gas is used in the etching in the photolithography process . 3. The method of manufacturing an organic electroluminescence lighting device according to claim 1, wherein the resist is an acrylic photosensitive resin . Has a pair of electrode layers including a light-transmitting electrode layer provided on a transparent substrate, is sandwiched electrode layer of said pair, and an organic layer containing the organic electroluminescence Sumine' sense material, the translucent A method for producing an organic electroluminescent lighting device, comprising: a light-shielding auxiliary electrode provided in contact with a part of the conductive electrode layer; and an insulating film covering the auxiliary electrode ,
An auxiliary electrode material film is formed on the translucent electrode layer, a resist is coated on the auxiliary electrode material film to form a resist film, and exposure and development are performed to form a residual resist having no reverse taper portion. The auxiliary electrode material film is etched to form an auxiliary electrode having a tapered portion, and then the residual resist is heated to flow above the glass transition temperature to flow to cover the auxiliary electrode to form the insulating film. A method for manufacturing an organic electroluminescence lighting device.

Images