JP5989342B2 - Organic EL device and manufacturing method thereof - Google Patents

Description

  The present invention relates to an organic EL device and a method for manufacturing the same, and more particularly to an organic EL device having an improved moisture resistance life and a method for manufacturing the same.

  In recent years, display devices and illumination devices using organic EL (EL) elements as organic light emitting elements have been developed for practical use.

  By the way, since the organic EL element is significantly deteriorated by moisture, it needs to be moisture-proof. Therefore, the organic EL element mounted on the substrate is sealed.

  Conventionally, as a method for sealing an organic EL element, for example, an organic EL element is formed by sequentially laminating a transparent electrode serving as an anode, an organic layer, and a non-transparent back electrode serving as a cathode on a glass substrate. A recess-shaped sealing member made of a glass material covering the organic EL element is hermetically provided on the glass substrate via an ultraviolet curable adhesive (UV curable resin), and is obtained by the glass substrate and the sealing member. A technique for providing a hygroscopic member in an airtight space is known (for example, see Patent Document 1).

JP 2006-272283 A

  However, as in the above prior art, sealing using a UV curable resin cannot completely prevent the penetration of moisture, and the problem remains that the organic EL element deteriorates.

  Conventionally, in order to accommodate the organic EL element, a gap is ensured by using an engraved glass in which an inner side is dug as a glass substrate. However, the engraved glass is relatively expensive and has a problem that it is difficult to reduce the cost.

  On the other hand, when vacuum sealing is performed using a relatively inexpensive flat glass instead of the dug glass, the flat glass may be distorted by atmospheric pressure or external force. In this case, there is a problem in that the gap cannot be maintained, the organic EL element and the glass substrate come into contact with each other, a short circuit occurs, and the organic EL element is destroyed.

  An object of the present invention is to provide an organic EL device capable of improving reliability at low cost and a method for manufacturing the same.

According to one aspect of the present invention for achieving the above object, a substrate and a first electrode layer disposed on the substrate, over the first electrode layer on the end portion of the first electrode layer and arranged organic EL layer from the organic EL layer, and a second electrode layer disposed over the end of the organic EL layer of the first is arranged over the ends of the electrode layer side, The sealing glass plate disposed on the second electrode layer is sealed with a predetermined gap between the substrate and the sealing glass plate, and is composed of a moisture-proof inorganic material. An organic EL device including a peripheral sealing material is provided.

According to another aspect of the present invention, a step of preparing a substrate, a step of forming a first electrode layer on the substrate, and an organic layer extending from the first electrode layer to the end of the first electrode layer. A step of forming an EL layer, and a step of forming a second electrode layer across the end portion of the organic EL layer on the side disposed across the end portion of the first electrode layer from above the organic EL layer, and A step of forming a sealing glass plate on the second electrode layer with a predetermined gap, and a step of forming a peripheral sealing material made of glass frit between the substrate and the sealing glass plate And a method for producing an organic EL device, comprising melting and sealing the peripheral sealing material.

According to another aspect of the present invention, a step of preparing a sealing glass plate, a step of applying and baking a glass frit on an edge side on the sealing glass plate, and an outer side of the glass frit A step of applying an ultraviolet curable resin for temporary sealing, a step of dropping a filler in the central portion surrounded by the glass frit, and a substrate on which an organic EL element is formed , which is disposed on the substrate. The first electrode layer, the organic EL layer disposed over the end of the first electrode layer from the first electrode layer, and the end of the first electrode layer from the organic EL layer A step of preparing the substrate including a second electrode layer disposed across the end of the organic EL layer on the side disposed, a substrate on which the organic EL element is formed, and the sealing glass plate, Facing each other and adhering under vacuum, and the ultraviolet curable resin is purple Irradiating the glass frit with a laser beam, irradiating the glass frit with a laser beam to fuse the sealing glass plate and the substrate, and temporarily sealing the glass frit. A method of manufacturing an organic EL device having a step of cutting off a stop is provided.

  ADVANTAGE OF THE INVENTION According to this invention, the organic electroluminescent apparatus which can improve reliability at low cost, and its manufacturing method can be provided.

1 is a schematic sectional view of an organic EL device according to a first embodiment. The enlarged view of the P section of the organic EL device shown in FIG. The typical cross-section figure of the organic EL device concerning a 2nd embodiment. FIG. 4A is an enlarged view of a Q portion of the organic EL device shown in FIG. 3, and FIG. 4B is a schematic cross-sectional structure diagram showing a spacer according to a comparative example. The typical cross-section figure of the organic EL device concerning a 3rd embodiment. The typical cross-section figure of the organic EL device concerning a 4th embodiment. FIG. 7 is an enlarged view of an R portion of the organic EL device shown in FIG. 6. It is typical sectional structure drawing of the organic EL device concerning a 5th embodiment, (a) Structure figure in case peripheral sealing material and dam material are arranged in contact, (b) Peripheral sealing material The structure figure when a dam material is arrange | positioned through a clearance gap. FIG. 10 is a schematic sectional view showing an organic EL device according to a sixth embodiment. In the organic EL device according to the second, fourth, and sixth embodiments, it is a schematic plane pattern configuration diagram of a spacer, and (a) a square pattern example, (b) a circular pattern example, and (c) a triangle. Example of circular pattern based on tone, (d) Example of square pattern based on hexagon, (e) Example of hexagon pattern. FIG. 3 is a photographing view showing the appearance of an organic EL device provided with a fine spacer. The photography figure which shows the example of formation of the spacer of a hexagonal pattern. The graph which shows the relationship between dark spot diameter (micrometer) and time (h) about the evaluation result of a moisture-resistant lifetime. It is a photography figure which shows the mode of advancing of the dark spot of the organic EL device concerning a comparative example, Comprising: In an 85 degreeC / 85% RH evaluation experiment of moisture-proof life, after (a) 0h and (b) 200h progress, (c) A photograph taken after 400 hours. It is a photography figure which shows the mode of progress of the dark spot of the organic EL device concerning this embodiment, Comprising: (a) 0h, (b) After 200h progress in 85 degreeC / 85% RH evaluation experiment of moisture resistance life, c) Photograph taken after 400 hours. The graph which shows the relationship between the current density (A / cm < ² >) of leak current, and the cumulative occurrence probability about the example of self-repair. FIG. 10 is a schematic bird's-eye view showing a state in which a plurality of cells Cij of an organic EL device according to a third embodiment are formed in a matrix. Sectional drawing which is a process of the manufacturing process of the organic electroluminescent apparatus concerning 3rd Embodiment, and shows the state which apply | coated and baked the glass frit on the edge part side on the glass plate for sealing. It is one process of the manufacturing process of the organic electroluminescent apparatus which concerns on 3rd Embodiment, Comprising: (a) Sectional drawing which shows the board | substrate in which the organic EL element was formed, (b) It pinched | interposed the predetermined clearance gap outside the glass frit Sectional drawing which shows the state which apply | coated the ultraviolet curing resin for temporary sealing, and dripped the filler in the center part enclosed by the glass frit. Sectional drawing which is one process of the manufacturing process of the organic electroluminescent apparatus which concerns on 3rd Embodiment, Comprising: The board | substrate in which the organic EL element was formed, and the glass plate for sealing are made to oppose and contact | adhere in vacuum. In one step of the manufacturing process of the organic EL device according to the third embodiment, the substrate on which the organic EL element is formed and the sealing glass plate are brought into close contact with each other under vacuum, and are brought into close contact with each other Sectional drawing which shows the state temporarily open | released by irradiating an ultraviolet-ray cured resin in the state which open | released to atmospheric pressure in the state, and the pressing pressure of atmospheric pressure was applied. Sectional drawing which is a process of the manufacturing process of the organic electroluminescent apparatus which concerns on 3rd Embodiment, and irradiates a laser beam to a glass frit and shows the state which fused | fused the glass plate for sealing and the board | substrate. FIG. 14 shows a step of manufacturing an organic EL device according to the third embodiment, in which the organic EL device is completed by cutting off the temporary sealing portion located outside the glass frit from the state shown in FIG. Sectional drawing. Sectional drawing which is a process of the manufacturing process of the organic electroluminescent apparatus concerning 4th Embodiment, Comprising: The board | substrate which formed the organic EL element provided with a spacer. It is one process of the manufacturing process of the organic EL device which concerns on 4th Embodiment, Comprising: (a) Sectional drawing which shows the board | substrate which formed the organic EL element provided with a spacer, (b) A predetermined clearance gap outside a glass frit Sectional drawing which shows the state which apply | coated the ultraviolet curing resin for temporary sealing on both sides, and dripped the filler in the center part enclosed by the glass frit. Sectional drawing which is a process of the manufacturing process of the organic electroluminescent apparatus which concerns on 4th Embodiment, Comprising: The board | substrate in which the organic EL element provided with a spacer was formed, and the glass plate for sealing were made to oppose. In one step of the manufacturing process of the organic EL device according to the fourth embodiment, the substrate on which the organic EL element including the spacer is formed and the sealing glass plate are brought into close contact with each other under a vacuum, Sectional drawing which shows the state which irradiated the ultraviolet-ray to the ultraviolet curable resin, and was temporarily sealed. Sectional drawing which is a process of the manufacturing process of the organic electroluminescent apparatus which concerns on 4th Embodiment, and irradiates a laser beam to a glass frit and shows the state which fused | fused the glass plate for sealing and the board | substrate. FIG. 28 shows a step of manufacturing the organic EL device according to the fourth embodiment, in which the organic EL device is completed by cutting off the temporary sealing portion located outside the glass frit from the state shown in FIG. Sectional drawing.

  Next, embodiments will be described with reference to the drawings. In the following description of the drawings, the same or similar parts are denoted by the same or similar reference numerals. However, it should be noted that the drawings are schematic, and the relationship between the thickness and the planar dimensions, the ratio of the thickness of each layer, and the like are different from the actual ones. Therefore, specific thicknesses and dimensions should be determined in consideration of the following description. Moreover, it is a matter of course that portions having different dimensional relationships and ratios are included between the drawings.

  Further, the embodiments described below exemplify apparatuses and methods for embodying the technical idea of the present invention, and the embodiments of the present invention include the material, shape, structure, The layout is not specified as follows. Various modifications can be made to the embodiment of the present invention within the scope of the claims.

  In the organic EL devices according to the following embodiments, “transparent” is defined as having a transmittance of about 50% or more. Further, “transparent” is also used to mean colorless and transparent with respect to visible light in the organic EL device according to the embodiment. Visible light corresponds to a wavelength of about 360 nm to 830 nm and an energy of about 3.45 eV to 1.49 eV, and is transparent if the transmittance is 50% or more in this region.

[First embodiment]
(Organic EL device)
A schematic cross-sectional structure of the organic EL device 1 according to the first embodiment is expressed as shown in FIG.

  As shown in FIG. 1, the organic EL device 1 according to the first embodiment includes a substrate 10, a first electrode layer 12 disposed on the substrate 10, and an organic disposed on the first electrode layer 12. EL layer 40, second electrode layer 20 disposed on organic EL layer 40, sealing glass plate 50 disposed on second electrode layer 20, substrate 10 and sealing glass plate 50 And a peripheral sealing material 100 that is sealed with a predetermined gap therebetween and made of a moisture-proof inorganic material. Here, the predetermined gap refers to the distance between the substrate 10 and the sealing glass plate 50.

  The gap distance is about 1 μm to 500 μm, preferably 10 μm to 100 μm.

  The peripheral sealing material 100 is disposed between the sealing glass plate 50 and the first electrode layer 12 and between the sealing glass plate 50 and the second electrode layer 20.

  The peripheral sealing material 100 is made of glass frit. The glass frit is powdered glass, but a melt can be formed by irradiating laser light.

  More specifically, as shown in FIG. 1, the first electrode layer 12 is formed from the left end portion on the substrate 10 to a position past the central portion. The organic EL layer 40 is formed so as to cover the right end from the vicinity of the left end on the first electrode layer 12. The second electrode layer 20 is formed from the vicinity of the left end on the organic EL layer 40 to the right end on the substrate 10.

  In the vicinity of the left end on the first electrode layer 12 and the vicinity of the right end on the second electrode layer 20, a peripheral sealing material 100 made of a moisture-proof inorganic material is disposed.

  As shown in FIG. 2, in the organic EL layer 40, for example, a hole transport layer 14, a light emitting layer 16, and an electron transport layer 18 are sequentially stacked from the substrate 10 side. Alternatively, the electron transport layer 18, the light emitting layer 16, and the hole transport layer 14 may be stacked in the reverse order.

  The hole transport layer 14 is a layer for smoothly transporting holes injected from the first electrode layer 12 to the light emitting layer. For example, 4,4′-bis [N- (1-naphthyl-1- ) N-phenyl-amino] -biphenyl and the like.

  The light emitting layer 16 is a layer for emitting light by recombination of injected holes and electrons. For example, aluminum (8-hydroxy) quinolinate doped with rubrene or a complex containing a transition metal atom as a dopant. Can be formed.

  The electron transport layer is a layer for smoothly transporting electrons injected from the second electrode layer 20 to the light emitting layer, and can be formed of, for example, aluminum (8-hydroxy) quinolinate.

  In addition, you may comprise the organic EL layer 40 using layers other than the said positive hole transport layer and an electron carrying layer, for example, a positive hole injection layer, an electron injection layer, etc.

  As shown in FIG. 1, the organic EL device 1 according to the first embodiment has a bottom emission configuration in which light (hν) emitted from the light emitting layer 16 is emitted from the substrate 10 side.

  According to the organic EL device 1 according to the first embodiment, since the peripheral sealing material 100 made of a moisture-proof inorganic material is provided, the space between the substrate 10 and the sealing glass plate 50 is provided. Intrusion of moisture and oxygen into 80 can be almost completely blocked, and the reliability of the organic EL element, particularly the moisture resistance life can be improved.

  Further, the glass frit constituting the peripheral sealing material 100 is relatively inexpensive, and according to the first embodiment, it is possible to provide an organic EL device capable of improving reliability at low cost.

[Second Embodiment]
(Organic EL device)
A schematic cross-sectional structure of the organic EL device 1 according to the second embodiment is expressed as shown in FIG.

  In the organic EL device 1 according to the second embodiment, as shown in FIG. 3, in the first embodiment shown in FIG. 1, there is a predetermined gap between the substrate 10 and the sealing glass plate 50. The spacer (column) 60 which keeps this gap is provided. The other configuration is the same as that of the first embodiment, and a duplicate description is omitted.

  The gap distance is about 1 μm to 500 μm, preferably 10 μm to 100 μm.

  As shown in FIG. 3, the spacer 60 is provided between the substrate 10 and the first electrode layer 12.

  The thickness of the spacer 60 is preferably within ± 30% of the predetermined gap distance. The spacer 60 can be made of a resist such as a photoresist or a bead material.

  If the spacer part of FIG. 3 is expanded, it will be comprised as shown in FIG.

 That is, as shown in FIG. 4A in which the Q portion of FIG. 3 is enlarged, the spacer 60 is disposed on the first electrode layer 12, and the organic EL layer 40 is formed so as to cover the spacer 60. The second electrode layer 20 is arranged on the organic EL layer 40.

  As shown in FIG. 4A, the spacer 60 has a forward tapered shape in which the cross-sectional area decreases from the substrate 10 toward the sealing glass plate 50. More specifically, the angle θ between the side wall portion of the spacer 60 and the horizontal plane of the first electrode layer 12 is set to 30 to 90 degrees. Thereby, the organic EL layer 40 and the second electrode layer 20 can be formed so as to cover the entire spacer 60.

  FIG. 4B shows a spacer 60a as a comparative example. As shown in FIG. 4B, the spacer 60a as a comparative example has a reverse taper. In such an inversely tapered spacer 60a, it is difficult to form the organic EL layer 40 and the second electrode layer 20 so as to cover the spacer 60a. Moreover, as shown in FIG.4 (b), the organic EL layer 40 and the 2nd electrode layer 20 are not formed continuously in the vicinity of the spacer 60a, but will be interrupted.

  Further, as shown in the enlarged portions A1 and A2 of FIG. 4B, the first electrode layer 12 and the second electrode layer 20 are likely to be short-circuit broken. However, if the short circuit is mild, current concentration occurs due to reverse bias application, and the short circuit part can be separated to avoid the short circuit state.

  As shown in FIG. 3, the organic EL device 1 according to the second embodiment has a bottom emission configuration in which light (hν) emitted from the light emitting layer 16 is emitted from the substrate 10 side.

  According to the organic EL device 1 according to the second embodiment, the space between the substrate 10 and the sealing glass plate 50 is provided because the peripheral sealing material 100 made of a moisture-proof inorganic material is provided. Intrusion of moisture and oxygen into 80 can be almost completely blocked, and the reliability of the organic EL element, particularly the moisture resistance life can be improved.

  Furthermore, since the spacer 60 that keeps a predetermined gap is provided, it is possible to avoid a situation in which the sealing glass plate 50 is distorted by atmospheric pressure or external force. Thereby, the situation where the organic EL layer 40 and the glass plate 50 for sealing contact and an organic EL element is destroyed can be prevented beforehand.

  Moreover, a relatively inexpensive flat glass can be used as the sealing glass plate 50, and according to the second embodiment, an organic EL device that can improve reliability at low cost is provided. it can.

[Third embodiment]
(Organic EL device)
A schematic cross-sectional structure of the organic EL device 1 according to the third embodiment is expressed as shown in FIG.

  In the organic EL device 1 according to the third embodiment, as shown in FIG. 5, it is formed between the substrate 10 and the sealing glass plate 50 in the first embodiment shown in FIG. 1. The space 80 is filled with a predetermined filler 30. The other configuration is the same as that of the first embodiment, and a duplicate description is omitted.

  The filler 30 can be composed of a solid or liquid resin, glass, fluorine-based inert oil or gel material, or an inert gas such as nitrogen gas or He gas. As the solid resin, a photo-curing resin such as an ultraviolet curable resin or a thermosetting resin such as an epoxy resin can be used.

 As the liquid resin, liquid plastic, liquid epoxy resin, or the like can be used. As the oil, fluorine oil or silicon oil can be used. This is because fluorine-based oil and silicon-based oil do not react with the organic EL layer 40 and are excellent in heat resistance, nonflammability, and chemical resistance. As the gel material, a silicon-based or fluorine-based gel material can be used. Nitrogen gas or the like can be used as the inert gas. This is because these fillers do not react with the organic EL layer 40 and are excellent in heat resistance, incombustibility, and chemical resistance.

  Further, a predetermined hygroscopic material may be added to the filler 30 as a filler.

  Examples of the hygroscopic material include silica gel, zeolite, alumina, magnesium oxide, calcium oxide, barium oxide, sodium sulfate, magnesium sulfate, and calcium sulfate.

  In the case of using a hygroscopic material, residual moisture or the like inside the organic EL element can be adsorbed to reduce damage to the organic EL element, and the life can be improved.

  As shown in FIG. 5, the organic EL device 1 according to the third embodiment has a bottom emission configuration in which light (hν) emitted from the light emitting layer 16 is emitted from the substrate 10 side.

  According to the organic EL device 1 according to the third embodiment, since the peripheral sealing material 100 made of a moisture-proof inorganic material is provided, the space between the substrate 10 and the sealing glass plate 50 is provided. Intrusion of moisture and oxygen into 80 can be almost completely blocked, and the reliability of the organic EL element, particularly the moisture resistance life can be improved.

  Furthermore, since the filler 30 is filled between the substrate 10 and the sealing glass plate 50, it is possible to avoid a situation where the sealing glass plate 50 is distorted by atmospheric pressure or external force. Thereby, the situation where the organic EL layer 40 and the glass plate 50 for sealing contact and an organic EL element is destroyed can be prevented beforehand.

  Further, a relatively inexpensive flat glass can be used as the sealing glass plate 50, and according to the third embodiment, an organic EL device capable of improving reliability at low cost is provided. it can.

  Further, when the filler 30 is a liquid resin, a fluorine-based inert oil, a gel material, or an inert gas such as nitrogen gas, self-repair of a short portion in the organic EL element can be achieved, and the yield is increased. Can be improved.

  Further, the introduction of the liquid filler 30 makes it easier to release heat generated from the organic EL element to the outside than gas sealing. Thereby, the temperature rise of an organic EL element can be suppressed and the lifetime of an organic EL apparatus can be improved.

[Fourth embodiment]
(Organic EL device)
A schematic cross-sectional structure of the organic EL device 1 according to the fourth embodiment is expressed as shown in FIG.

  In the organic EL device 1 according to the fourth embodiment, as shown in FIG. 6, in the third embodiment shown in FIG. 5, there is a predetermined gap between the substrate 10 and the sealing glass plate 50. The spacer 60 that keeps the gap is provided. The other configuration is the same as that of the third embodiment, and a duplicate description is omitted.

  The gap distance is about 1 μm to 500 μm, preferably 10 μm to 100 μm. As shown in FIG. 6, the spacer 60 is provided between the substrate 10 and the first electrode layer 12.

  The thickness of the spacer 60 is preferably within ± 30% of the predetermined gap distance.

  The spacer 60 can be made of a resist such as a photoresist or a bead material.

  If the spacer part of FIG. 6 is expanded, it will be comprised as shown in FIG.

 That is, as shown in FIG. 7 in which the R portion of FIG. 6 is enlarged, the spacer 60 is disposed on the first electrode layer 12, and the organic EL layer 40 is formed on the first electrode layer 12 so as to cover the spacer 60. The second electrode layer 20 is arranged on the organic EL layer 40.

  As shown in FIG. 7, the spacer 60 has a forward tapered shape in which the cross-sectional area decreases from the substrate 10 toward the sealing glass plate 50. More specifically, the angle θ between the side wall portion of the spacer 60 and the horizontal plane of the first electrode layer 12 is set to 30 to 90 degrees. Thereby, the organic EL layer 40 and the second electrode layer 20 can be formed so as to cover the entire spacer 60.

  As shown in FIG. 6, the organic EL device 1 according to the fourth embodiment has a bottom emission configuration in which light (hν) emitted from the light emitting layer 16 is emitted from the substrate 10 side.

  According to the organic EL device 1 according to the fourth embodiment, since the peripheral sealing material 100 made of a moisture-proof inorganic material is provided, the space between the substrate 10 and the sealing glass plate 50 is provided. Intrusion of moisture and oxygen into 80 can be almost completely blocked, and the reliability of the organic EL element, particularly the moisture resistance life can be improved.

  Furthermore, since the spacer 60 that keeps a predetermined gap is provided, it is possible to avoid a situation in which the sealing glass plate 50 is distorted by atmospheric pressure or external force. Thereby, the situation where the organic EL layer 40 and the glass plate 50 for sealing contact and an organic EL element is destroyed can be prevented beforehand.

  Further, a relatively inexpensive flat glass can be used as the sealing glass plate 50, and according to the fourth embodiment, an organic EL device capable of improving reliability at a low cost is provided. it can.

  In addition, when the filler 30 is a liquid resin, a fluorine-based inert oil, a gel material, or an inert gas such as nitrogen gas or He gas, self-repair of a short portion in the organic EL element can be achieved. And the yield can be improved.

  Moreover, the introduction of the filler 30 makes it easy to release heat generated from the organic EL element to the outside. Thereby, the temperature rise of an organic EL element can be suppressed and the lifetime of the organic EL apparatus 1 can be improved.

[Fifth embodiment]
(Organic EL device)
A schematic cross-sectional structure of an organic EL device 1 according to the fifth embodiment is expressed as shown in FIG.

  In the organic EL device 1 according to the fifth embodiment, as shown in FIGS. 8A and 8B, the filler 30 is a liquid resin in the third embodiment shown in FIG. In the case of an inert oil such as glass or fluorine, or a gel material, a dam material 70 for preventing the filler 30 from leaking is provided inside the peripheral sealing material 100. The other configuration is the same as that of the third embodiment, and a duplicate description is omitted.

  FIG. 8A shows a configuration in which the filler 30 and the dam material 70 are provided in contact with each other. FIG. 8B shows a configuration in which the filler 30 and the dam material 70 are provided with the space 80 interposed therebetween.

  As the dam material 70, an adhesive material such as an epoxy resin or a silicon resin can be used.

  Further, a predetermined moisture absorbing material may be added to the dam material 70 as a filler.

  Examples of the hygroscopic material include silica gel, zeolite, alumina, magnesium oxide, calcium oxide, barium oxide, sodium sulfate, magnesium sulfate, and calcium sulfate.

  As shown in FIG. 8, the organic EL device 1 according to the fifth embodiment has a bottom emission configuration in which light (hν) emitted from the light emitting layer 16 is emitted from the substrate 10 side.

  According to the organic EL device 1 according to the fifth embodiment, the space between the substrate 10 and the sealing glass plate 50 is provided because the peripheral sealing material 100 made of a moisture-proof inorganic material is provided. Intrusion of moisture and oxygen into 80 or the filler 30 can be almost completely blocked, and the reliability of the organic EL element, in particular, the moisture resistance life can be improved.

  In addition, since the dam material 70 that prevents the filler 30 from leaking is disposed, it is possible to prevent the filler 30 from leaking outside the peripheral sealing material 100. Further, by providing the dam material 70, the manufacturing process in the case of using a liquid for the filler 30 can be simplified.

  Moreover, when a dam material is provided with a moisture absorption function, the residual moisture etc. inside an organic EL element can be adsorbed, damage to the organic EL element can be reduced, and the life can be improved.

[Sixth embodiment]
(Organic EL device)
A schematic cross-sectional structure of an organic EL device 1 according to the sixth embodiment is expressed as shown in FIG.

  In the organic EL device 1 according to the sixth embodiment, as shown in FIG. 9, between the substrate 10 and the sealing glass plate 50 in the fifth embodiment shown in FIG. In addition, a configuration is provided in which a spacer 60 for maintaining a predetermined gap is provided. The other configuration is the same as that of the fifth embodiment, and a duplicate description is omitted.

  The gap distance is about 1 μm to 500 μm, preferably 10 μm to 100 μm. As shown in FIG. 9, the spacer 60 is provided between the substrate 10 and the first electrode layer 12.

  The thickness of the spacer 60 is preferably within ± 30% of the predetermined gap distance. The spacer 60 can be made of a resist such as a photoresist or a bead material.

9 may be configured as shown in FIG. 4A or FIG.
As shown in FIG. 9, the organic EL device 1 according to the sixth embodiment has a bottom emission configuration in which light (hν) emitted from the light emitting layer 16 is emitted from the substrate 10 side.

  According to the organic EL device 1 according to the sixth embodiment, since the peripheral sealing material 100 made of a moisture-proof inorganic material is provided, the space between the substrate 10 and the sealing glass plate 50 is provided. Intrusion of moisture and oxygen into 80 can be almost completely blocked, and the reliability of the organic EL element, particularly the moisture resistance life can be improved.

  In addition, since the dam material 70 that prevents the filler 30 from leaking is disposed, it is possible to prevent the filler 30 from leaking outside the peripheral sealing material 100. Further, by providing the dam material 70, the manufacturing process in the case of using a liquid for the filler 30 can be simplified.

  Moreover, when a dam material is provided with a moisture absorption function, the residual moisture etc. inside an organic EL element can be adsorbed, damage to the organic EL element can be reduced, and the life can be improved.

  Furthermore, since the spacer 60 that keeps a predetermined gap is provided, it is possible to avoid a situation in which the sealing glass plate 50 is distorted by atmospheric pressure or external force. Thereby, the situation where the organic EL layer 40 and the glass plate 50 for sealing contact and an organic EL element is destroyed can be prevented beforehand.

  Further, a relatively inexpensive flat glass can be used as the sealing glass plate 50. According to the sixth embodiment, an organic EL device that can improve reliability at low cost is provided. it can.

  In addition, when the filler 30 is a liquid resin, a fluorine-based inert oil, a gel material, or an inert gas such as nitrogen gas or He gas, self-repair of a short portion in the organic EL element can be achieved. And the yield can be improved.

  Further, the introduction of the liquid filler 30 makes it easier to release heat generated from the organic EL element to the outside than gas sealing. Thereby, the temperature rise of an organic EL element can be suppressed and the lifetime of the organic EL apparatus 1 can be improved.

(Spacer formation pattern)
The formation pattern of the spacer 60 in the organic EL device according to the second, fourth, and sixth embodiments will be described with reference to FIGS.

  The spacer 60 can be arranged by being patterned with a predetermined pattern structure. The pattern structure can be any of a rectangular pattern, a circular pattern, and a hexagonal pattern.

  FIG. 10 is a schematic plane pattern configuration diagram of the spacer 60 in the organic EL devices according to the second, fourth, and sixth embodiments.

  10, (a) is a square pattern example, (b) is a circular pattern example, (c) is a circular pattern example based on a triangle, (d) is a square pattern example based on a hexagon, (e) Is an example of a hexagonal pattern. “A” represents the distance between the spacers, and “b” represents the width of the spacer.

  FIG. 11 is a photograph showing an external appearance of a production example of the organic EL device 1 according to the sixth embodiment provided with fine spacers. The spacer can be made invisible to the naked eye by photolithography, for example, with a width of 10 μm or less.

  FIG. 12 is a photograph showing an example of forming a hexagonal pattern spacer 60. In this example, each spacer 60 is formed in a hexagonal pattern having a width of 7.7 μm. Thereby, while being able to make the spacer 60 invisible with the naked eye, the intensity | strength with respect to the external force etc. of the organic EL apparatus 1 can be improved.

(Evaluation results of moisture resistance life)
Next, with reference to FIGS. 13 to 15, the evaluation results of the moisture resistance life of the organic EL device 1 according to the first to sixth embodiments will be described.

  FIG. 13 is a graph showing the relationship between the dark spot diameter (μm) and time (h) for the evaluation results of the moisture resistance life.

  In FIG. 13, a graph curve A is an organic EL device using a liquid filler in a resin sealing structure as a comparative example, a graph curve B is an organic EL device 1 using a liquid filler in a sealing structure using a glass frit, a graph A curve C shows an evaluation result of the organic EL device 1 using nitrogen gas filling in a sealing structure with a glass frit.

  The evaluation experiment is an accelerated test at a temperature of 85 ° C. and a humidity of 85% RH.

  As shown in FIG. 13, in the organic EL device as a comparative example related to the graph curve A, it is estimated that the diameter of the dark spot suddenly increases in about 200 to 300 h, and the infiltration of moisture is progressing.

  On the other hand, in the organic EL device 1 according to the present embodiment related to the graph curves B and C, it is understood that the progress of dark spots is not seen even after about 700 hours, and the moisture resistance life is improved.

  FIG. 14 is a shooting diagram illustrating the progress of dark spots in the organic EL device according to the comparative example. The organic EL device according to the comparative example has a configuration in which the space between the substrate and the sealing glass plate is sealed with a resin. In the experiment for evaluating the moisture resistance life, at 0h shown in FIG. 14A, there is no dark spot in a predetermined region having a width of 1 mm. After 200 hours shown in FIG. 14B, several dark spots are generated. It can be seen that the dark spots have grown greatly after 400 hours have elapsed as shown in FIG.

  FIG. 15 is a shooting diagram illustrating the progress of dark spots in the organic EL device 1 according to the present embodiment. In the experiment for evaluating the moisture resistance life, at 0h shown in FIG. 15A, there is no dark spot in a predetermined region having a width of 1 mm. Several 200 dark spots are generated after 200 hours shown in FIG. However, it can be seen that the dark spots have not grown even after 400 hours have elapsed as shown in FIG.

  As described above, in the organic EL device 1 according to the present embodiment, the moisture resistance life is improved by sealing the space between the substrate 10 and the sealing glass plate 50 with a moisture-proof inorganic material such as glass frit. Yes.

(Example of self-repair)
When the filler 30 is a liquid resin, a fluorine-based inert oil, a gel material, or an inert gas such as nitrogen gas or He gas, a self-short circuit in the organic EL element is applied by applying a reverse bias. It can be repaired.

FIG. 16 is a graph showing the relationship between the current density (A / cm ² ) of leakage current and the cumulative occurrence probability for an example of self-repair.

  As shown in FIG. 16, it can be seen that the leakage current decreases after self-repair as compared to the initial state. As a result, short-circuit breakdown of the organic EL element can be prevented in advance, and the yield can be improved.

(Method for manufacturing organic EL device according to the third embodiment)
With reference to FIGS. 17-23, the manufacturing method of the organic electroluminescent apparatus 1 which concerns on 3rd Embodiment shown in FIG. 5 is demonstrated.

  FIG. 17 is a schematic bird's-eye view showing a state in which a plurality of organic EL devices 1 according to the third embodiment are formed in a matrix. Note that SL is a scribe line that separates the organic EL devices 1. A line I-I indicates a cross section of the organic EL device 1.

  The steps of the manufacturing method are as follows.

(A) First, as shown in FIG. 18, a glass frit is applied as a peripheral sealing material 100 to the edge side on the sealing glass plate 50 and fired.

(B) Next, as shown in FIG. 19B, an ultraviolet curable resin 101 for temporary sealing is applied to the outside of the peripheral sealing material 100 with a predetermined gap therebetween, and the peripheral sealing material 100 surrounds the peripheral sealing material 100. The filler 30 is dropped on the center part.

(C) Further, as shown in FIG. 19A, the substrate 10 on which the organic EL element composed of the first electrode layer 12, the organic EL layer 40, and the second electrode layer 20 is formed is sealed with the element side facing downward. It is made to oppose the glass plate 50 for a stop.

(D) Next, as shown in FIG. 20, the substrate 10 on which the organic EL element is formed and the sealing glass plate 50 are brought into close contact with each other under vacuum. At this time, the portion surrounded by the substrate 10, the sealing glass plate 50, and the ultraviolet curable resin 101 is kept in a vacuum state. At this time, the distance between the substrate 10 and the sealing glass plate 50 is W1.

(E) Next, as shown in FIG. 21, the substrate 10 and the sealing glass are returned to the atmospheric pressure with the substrate 10 on which the organic EL element is formed and the sealing glass plate 50 facing each other. The plate 50 is pressed by the atmospheric pressure Pa. Thereby, the distance between the substrate 10 and the sealing glass plate 50 is in a state of W2 that is smaller than W1, and the filler 30 spreads over the entire space. Specifically, a plurality of cells Cij of the organic EL device 1 shown in FIG. 17 formed in a matrix are accommodated in a vacuum chamber and are pressed in a vacuum state. Thereafter, the substrate 10 and the sealing glass plate 50 are pressed by the atmospheric pressure Pa by returning to the atmospheric pressure state. Thereby, the distance between the substrate 10 and the sealing glass plate 50 is in a state of W2 that is smaller than W1, and the filler 30 spreads over the entire space.

(F) Next, the ultraviolet curable resin 101 is irradiated with ultraviolet rays so that the ultraviolet curable resin 101 is cured and temporarily sealed.

(G) Next, as shown in FIG. 22, the peripheral sealing material 100 is irradiated with the laser beam PL, and the sealing glass plate 50 and the substrate 10 are fused and sealed. Here, FIG. 22 corresponds to a cross-sectional view of the cell Cij along the line II in FIG. However, in FIG. 22, by inverting the substrate 10 and the sealing glass plate 50 up and down, the cell Cij corresponding to the cross-sectional view taken along the line II of FIG. 17 can be obtained.

(H) Next, in FIG. 22, scribing is performed along the scribe lines SL <b> 1 and SL <b> 2, the temporary sealing portion is cut off, and the filler remaining on the cutting portion is cleaned and removed.

  Through the above steps, the organic EL device shown in FIG. 23 can be mass-produced.

(Method for Manufacturing Organic EL Device According to Fourth Embodiment)
A method for manufacturing the organic EL device 1 according to the fourth embodiment shown in FIG. 6 will be described with reference to FIGS.

  A plurality of organic EL devices 1 according to the fourth embodiment are formed in a matrix like FIG.

  The steps of the manufacturing method are as follows.

(A) First, as shown in FIG. 24, a spacer 60 is formed on the substrate 10 having the first electrode layer 12 by photolithography. Thereafter, the organic EL layer 40 and the second electrode layer 20 are stacked.

(B) Next, as shown in FIG. 25B, the peripheral sealing material 100 is applied to the edge side on the sealing glass plate 50 and fired.

(C) Next, as shown in FIG. 25 (b), an ultraviolet curable resin 101 for temporary sealing is applied outside the peripheral sealing material 100 with a predetermined gap therebetween, and the peripheral sealing material 100 surrounds the peripheral sealing material 100. The filler 30 is dropped on the center part.

(D) Next, as shown in FIG. 25A, the substrate 10 on which the spacer 60 and the organic EL element are formed is opposed to the sealing glass plate 50 with the element side facing downward.

(E) Next, as shown in FIG. 26, the substrate 10 on which the organic EL element is formed and the sealing glass plate 50 are brought into close contact with each other under vacuum. At this time, the portion surrounded by the substrate 10, the sealing glass plate 50, and the ultraviolet curable resin 101 is kept in a vacuum state. At this time, the distance between the substrate 10 and the sealing glass plate 50 is W1.

(F) Next, as shown in FIG. 27, by returning the substrate 10 on which the organic EL element is formed and the glass plate 50 for sealing to the atmospheric pressure state, the substrate 10 and the glass for sealing are returned. The plate 50 is pressed by the atmospheric pressure Pa. Thereby, the distance between the substrate 10 and the sealing glass plate 50 is in a state of W2 that is smaller than W1, and the filler 30 spreads over the entire space. Specifically, a plurality of cells Cij of the organic EL device 1 shown in FIG. 17 formed in a matrix are accommodated in a vacuum chamber and are pressed in a vacuum state. Thereafter, the substrate 10 and the sealing glass plate 50 are pressed by the atmospheric pressure Pa by returning to the atmospheric pressure state. Thereby, the distance between the substrate 10 and the sealing glass plate 50 is in a state of W2 that is smaller than W1, and the filler 30 spreads over the entire space. Further, the tip of the spacer 60 comes into contact with the sealing glass plate 50.

(F) Next, the ultraviolet curable resin 101 is irradiated with ultraviolet rays so that the ultraviolet curable resin 101 is cured and temporarily sealed.

(G) Next, as shown in FIG. 28, the peripheral sealing material 100 is irradiated with laser light PL, and the sealing glass plate 50 and the substrate 10 are fused and sealed. Here, FIG. 28 corresponds to a cross-sectional view of the cell Cij along the line II in FIG. However, in FIG. 28, the cell Cij corresponding to the cross-sectional view taken along the line II in FIG. 17 can be obtained by turning the substrate 10 and the sealing glass plate 50 upside down.

(H) Next, in FIG. 28, scribing is performed along the scribe lines SL1 and SL2, and the temporarily sealed portion is cut off, and the filler remaining on the cut portion is cleaned and removed.

  Through the above steps, the organic EL device shown in FIG. 29 can be mass-produced.

[Other embodiments]
As described above, the present invention has been described according to the first to sixth embodiments. However, it should be understood that the descriptions and drawings constituting a part of this disclosure are exemplary and limit the present invention. should not do. From this disclosure, various alternative embodiments, examples and operational techniques will be apparent to those skilled in the art.

  As described above, the present invention includes various embodiments not described herein.

  The organic EL device of the present invention can be applied to the field of high-brightness organic EL lighting, the field of high-brightness organic EL display, and the like.

DESCRIPTION OF SYMBOLS 1 ... Organic EL apparatus 10 ... Board | substrate 12 ... 1st electrode layer 14 ... Hole transport layer 16 ... Light emitting layer 18 ... Electron transport layer 20 ... 2nd electrode layer 30 ... Filler 40 ... Organic EL layer 50 ... Glass for sealing Plate 60 ... Spacer 70 ... Dam material 100 ... Peripheral sealing material 101 ... UV curable resin

Claims (24)

A substrate,
A first electrode layer disposed on the substrate;
An organic EL layer disposed over the end of the first electrode layer from the first electrode layer;
From the organic EL layer, a second electrode layer disposed across the end of the organic EL layer on the side disposed across the end of the first electrode layer;
A sealing glass plate disposed on the second electrode layer;
An organic EL device comprising: a peripheral sealing material configured to seal between the substrate and the sealing glass plate with a predetermined gap therebetween and configured with a moisture-proof inorganic material.   The peripheral sealing material is disposed between the sealing glass plate and the first electrode layer and between the sealing glass plate and the second electrode layer. The organic EL device described in 1.   The organic EL device according to claim 1, wherein the peripheral sealing material is a glass frit.   The organic EL device according to claim 1, further comprising a spacer that keeps the predetermined gap between the substrate and the sealing glass plate. The organic EL device according to claim 4, wherein the spacer is disposed between the sealing glass plate and the first electrode layer.   6. The organic EL device according to claim 4, wherein the thickness of the spacer is within ± 30% of the distance of the predetermined gap.   The organic EL device according to any one of claims 4 to 6, wherein the spacer has a forward tapered shape in which a cross-sectional area decreases from the substrate in the sealing glass plate direction.   The organic EL device according to claim 7, wherein a taper angle between a side wall portion of the spacer and a horizontal plane of the first electrode layer is 30 to 90 degrees. The spacer is disposed on the first electrode layer;
The organic EL layer is disposed on the first electrode layer so as to cover the spacer,
The organic EL device according to claim 4, wherein the second electrode layer is disposed on the organic EL layer.   The organic EL device according to claim 4, wherein the spacer is made of a resist or a bead material.   The organic EL device according to any one of claims 4 to 10, wherein the spacer is arranged by being patterned with a predetermined pattern structure.   The organic EL device according to claim 11, wherein the pattern structure has any one of a rectangular pattern, a circular pattern, and a hexagonal pattern.   The organic EL device according to any one of claims 1 to 12, wherein a space formed between the substrate and the sealing glass plate is filled with a predetermined filler.   The organic EL device according to claim 13, wherein the filler is made of a solid or liquid resin, glass, oil or gel material, or an inert gas.   The organic EL device according to claim 14, wherein the solid resin is made of a photo-curing resin or a thermosetting resin.   The dam material for preventing leakage of the filler is disposed inside the peripheral sealing material when the filler is a liquid resin, glass, oil, or gel material. 15. The organic EL device according to 15.   The organic EL device according to claim 16, wherein the dam material has a moisture absorption function.   17. The organic EL device according to claim 16, wherein one or both of the dam material and the filler has a moisture absorption function. Preparing a substrate;
Forming a first electrode layer on the substrate;
Forming an organic EL layer from above the first electrode layer across the edge of the first electrode layer;
Forming a second electrode layer across the end of the organic EL layer on the side disposed across the end of the first electrode layer from the organic EL layer;
Forming a sealing glass plate with a predetermined gap on the second electrode layer;
Forming a peripheral sealing material made of glass frit between the substrate and the sealing glass plate;
And a step of melting and sealing the peripheral sealing material.   20. The method of manufacturing an organic EL device according to claim 19, further comprising a step of forming a spacer that maintains a predetermined gap between the substrate and the sealing glass plate.   21. The method of manufacturing an organic EL device according to claim 19, further comprising a step of filling a space formed between the substrate and the sealing glass plate with a predetermined filler. A step of preparing a sealing glass plate;
Applying and baking a glass frit on the edge side on the sealing glass plate;
Applying an ultraviolet curable resin for temporary sealing to the outside of the glass frit;
Dropping a filler into a central portion surrounded by the glass frit;
A substrate on which an organic EL element is formed, the first electrode layer disposed on the substrate, and the organic EL layer disposed across the first electrode layer from the first electrode layer; And a step of preparing the substrate including the second electrode layer disposed across the end portion of the organic EL layer on the side disposed across the end portion of the first electrode layer from above the organic EL layer. When,
A step in which the substrate on which the organic EL element is formed and the glass plate for sealing are opposed to each other and adhered under vacuum;
Irradiating the ultraviolet curable resin with ultraviolet rays and temporarily sealing the ultraviolet curable resin;
Irradiating the glass frit with a laser beam to fuse the sealing glass plate and the substrate;
And a step of cutting off a temporary sealing portion located outside the glass frit. The step of preparing the substrate on which the organic EL element is formed includes
Forming a spacer in a predetermined pattern on the substrate;
The method of manufacturing an organic EL device according to claim 22, further comprising: forming an organic EL element on the substrate. Forming a spacer in a predetermined pattern on the substrate;
23. The method of manufacturing an organic EL device according to claim 22, further comprising a step of patterning and forming a photoresist applied on the substrate.