WO2012070586A1 - Dispositif électroluminescent et procédé de production de celui-ci - Google Patents

Dispositif électroluminescent et procédé de production de celui-ci Download PDF

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Publication number
WO2012070586A1
WO2012070586A1 PCT/JP2011/076945 JP2011076945W WO2012070586A1 WO 2012070586 A1 WO2012070586 A1 WO 2012070586A1 JP 2011076945 W JP2011076945 W JP 2011076945W WO 2012070586 A1 WO2012070586 A1 WO 2012070586A1
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light emitting
electrode
electrodes
organic
emitting layer
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PCT/JP2011/076945
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English (en)
Japanese (ja)
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祥司 美馬
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住友化学株式会社
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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K59/00—Integrated devices, or assemblies of multiple devices, comprising at least one organic light-emitting element covered by group H10K50/00
    • H10K59/80—Constructional details
    • H10K59/86—Series electrical configurations of multiple OLEDs

Definitions

  • Embodiments of the present invention relate to a light emitting device and a manufacturing method thereof.
  • An organic electroluminescence element (hereinafter, “electroluminescence” may be referred to as “EL”) is a kind of light-emitting element that emits light when a voltage is applied thereto, and a pair of electrodes and a pair of electrodes. And a light emitting layer disposed on the substrate.
  • EL organic electroluminescence element
  • holes are injected from the anode and electrons are injected from the cathode. Light emission occurs when these holes and electrons are combined in the light emitting layer.
  • Patent Document 1 A light emitting device in which a plurality of such organic EL elements are connected in series has been proposed (see, for example, Patent Document 1).
  • FIG. 7 is a diagram schematically showing a light emitting device 2 in which a plurality (three in FIG. 7) of organic EL elements 1 are connected in series.
  • FIG. 7A is a plan view of the light-emitting device 2
  • FIG. 7B is a cross-sectional view of the light-emitting device 2.
  • the light emitting device 2 shown in FIGS. 7A and 7B includes three organic EL elements 1. These three organic EL elements 1 are arranged on the support substrate 3 along a predetermined arrangement direction X and are connected in series. Each organic EL element 1 includes a pair of electrodes 4 and 5 and a light emitting layer 6 provided between the electrodes.
  • a first electrode 4 one electrode disposed near the support substrate 3 out of the pair of electrodes 4 and 5 is referred to as a first electrode 4, and the other electrode disposed farther from the support substrate 3 than the first electrode 4. Is referred to as a second electrode 5.
  • a predetermined layer different from the light emitting layer may be provided between the first and second electrodes 4 and 5.
  • At least one of the first electrode 4 and the second electrode 5 is formed of a conductive thin film that exhibits optical transparency. This is because light generated in the light emitting layer 6 needs to be emitted to the outside of the organic EL element.
  • conductive thin films are usually indium tin oxide (Indium).
  • Metal oxide thin films such as Tin Oxide (abbreviated as ITO) and Indium Zinc Oxide (abbreviated as IZO) are used.
  • the first electrodes 4 of the organic EL elements 1 are discretely arranged at predetermined intervals in the arrangement direction X, and thus are not electrically connected to each other only by wiring.
  • the second electrodes 5 of each organic EL element 1 are arranged at a predetermined interval in the arrangement direction X, and therefore are not electrically connected to each other only by wiring.
  • the first electrode 4 and the second electrode 5 of the organic EL element 1 adjacent to each other in the arrangement direction X are connected in contact with each other and are electrically connected.
  • the plurality of organic EL elements 1 constitutes a series connection.
  • the first electrode 4 is one of the arrangement directions X (hereinafter, “one of the arrangement directions X” may be referred to as “left”, and “the other of the arrangement directions X” may be referred to as right). Up to a position where the end (hereinafter also referred to as the left end) overlaps the right end (hereinafter also referred to as the right end) of the second electrode 5 of the organic EL element 1 adjacent to the left.
  • the first electrode 4 is formed on the support substrate 3. Specifically, three first electrodes 4 are discretely formed on the support substrate 3 at predetermined intervals in the arrangement direction X (see FIG. 8A).
  • an ink containing a material that becomes the light emitting layer 6 is applied onto the support substrate 3 by a predetermined application method.
  • the coating method it is difficult for the coating method to selectively apply the ink pattern only to the intended portion, so that the ink is also applied to unnecessary portions such as between the first electrodes 4 (see FIG. 8B). Therefore, after applying the ink, a step of removing the ink applied to unnecessary portions is required (see FIG. 8C).
  • the ink can be removed by, for example, a method of wiping ink using a cloth or cotton swab containing a solvent in which the ink is soluble, a laser ablation method, or the like.
  • the second electrode 5 is patterned (see FIG. 8D).
  • a light emitting device 2 including three organic EL elements 1 connected in series can be manufactured.
  • the above-described conventional technique has a problem that the number of steps increases because a step of removing ink applied to unnecessary portions is required. Furthermore, when removing the ink applied to unnecessary portions, there is a possibility that foreign matters may be mixed into the light emitting layer.
  • the ITO thin film or IZO thin film used as an electrode exhibiting optical transparency does not necessarily have sufficient conductivity.
  • an object of the present invention is a structure that does not require a step of removing ink applied to an unnecessary portion when forming a light emitting layer by a coating method, and also in a large area organic EL element, light emission unevenness and heat generation. It is to provide a light emitting device with a small amount of light.
  • the light emitting device includes a plurality of first electrodes arranged on a support substrate, a light emitting layer covering the plurality of first electrodes, and arranged on the light emitting layer and facing each of the plurality of first electrodes.
  • a plurality of second electrodes wherein each organic electroluminescence element is constituted by a pair of the first and second electrodes sandwiching the light emitting layer
  • the first electrode includes a first body portion and And a first extending portion extending from the first body portion so as to protrude from the light emitting layer along a direction perpendicular to the arrangement direction of the first electrodes
  • the second electrode includes a second A main body portion, and a second extending portion extending from the main body portion so as to protrude from the light emitting layer along a direction perpendicular to an arrangement direction of the second electrodes
  • the first and second electrodes At least one of the two has a connection portion extending along the arrangement direction thereof.
  • connections the is connected to the other of the first and second electrodes, at least one of the first and second electrodes, characterized in that it is a mesh electrode (mesh-shaped translucent electrode).
  • mesh electrode mesh-shaped translucent electrode
  • the mesh electrode is preferably made of a mixture of a conductive filler and a resin, or only a conductive material.
  • the sheet resistance of the mesh electrode is preferably 5 ( ⁇ / sq.) Or less.
  • the light transmittance of the mesh electrode is 50% or more.
  • the first electrode includes another extension portion extending from the first main body portion in a direction opposite to the first extension portion so as to protrude from the light emitting layer.
  • the second electrode includes another extension portion extending from the second main body portion in a direction opposite to the second extension portion so as to protrude from the light emitting layer.
  • This manufacturing method is the method for manufacturing the light emitting device described above, wherein the ink containing the material to be the light emitting layer is continuously applied so as to cover the plurality of first electrodes, and the applied ink is solidified. A step of forming the light emitting layer.
  • the method for applying the ink is a cap coating method, a slit coating method, a spray coating method or a printing method.
  • the present invention is a structure that does not require a step of removing ink applied to an unnecessary part when forming a light emitting layer by a coating method, and even in a large-area organic EL element, light emission unevenness and heat generation are eliminated. A small number of light emitting devices can be realized.
  • FIG. 1A is a plan view showing the light emitting device 11 of the first embodiment
  • FIG. 1B is a longitudinal sectional view of the light emitting device 11.
  • FIG. 2 is a diagram for explaining a manufacturing process of the light emitting device 11.
  • FIG. 3 is a diagram for explaining a manufacturing process of the light emitting device 11.
  • FIG. 4 is a diagram schematically showing the light emitting device 31 of the second embodiment.
  • FIG. 5 is a diagram schematically showing the light emitting device 41 of the third embodiment.
  • FIG. 6 is a diagram illustrating a light emitting device 61 according to the fourth embodiment.
  • FIG. 7 schematically shows a light-emitting device 2 in which a plurality of organic EL elements 1 are connected in series.
  • FIG. 7A is a plan view of the light-emitting device 2
  • FIG. FIG. FIG. 8 is a diagram for explaining a manufacturing process of the light emitting device 2.
  • FIG. 9 is a plan view of a mesh electrode.
  • FIG. 10 is a longitudinal sectional view of the organic EL element.
  • FIG. 11 is a longitudinal sectional view of the organic EL element.
  • FIG. 12 is a longitudinal sectional view of the organic EL element.
  • FIG. 13 is a longitudinal sectional view of the organic EL element.
  • FIG. 14 is a longitudinal sectional view of the organic EL element.
  • FIG. 15 is a longitudinal sectional view of the organic EL element.
  • FIG. 16 is a longitudinal sectional view of the organic EL element.
  • FIG. 17 is a longitudinal sectional view of the organic EL element.
  • FIG. 18 is a block diagram of a power supply unit connected to the organic EL element.
  • an XYZ three-dimensional orthogonal coordinate system is set as shown.
  • the thickness direction of the substrate is the Z axis
  • the element arrangement direction is the X axis
  • the direction perpendicular to both is the Y axis.
  • FIG. 1A is a plan view schematically showing the light emitting device 11 of the first embodiment
  • FIG. 1B is a longitudinal sectional view of the light emitting device 11.
  • the light emitting device 11 includes a support substrate 12 and a plurality of organic EL elements 13 provided on the support substrate 12 and connected in series.
  • the predetermined arrangement direction X is set in a direction perpendicular to the thickness direction Z of the support substrate 12. That is, the arrangement direction X is set parallel to the main surface of the support substrate 12.
  • the plurality of organic EL elements 13 are arranged along a predetermined straight line (X), but may be arranged along a predetermined curve.
  • the arrangement direction corresponds to the tangential direction of the predetermined curve.
  • the number of organic EL elements 13 provided on the support substrate 12 is appropriately set according to the design.
  • a light emitting device 11 provided with three organic EL elements 13 will be described below.
  • Each organic EL element 13 includes a pair of electrodes 14 and 15, and a light emitting layer 16 provided between the electrodes 14 and 15 and covering the plurality of electrodes 14.
  • One of the pair of electrodes 14 and 15 functions as an anode of the organic EL element 13, and the other electrode functions as a cathode of the organic EL element 13.
  • an electrode disposed near the support substrate 12 is referred to as a first electrode 14, and the other electrode disposed apart from the support substrate 12 is referred to as a second electrode 15.
  • At least one light emitting layer 16 is provided between the first and second electrodes 14 and 15.
  • the 1st and 2nd electrodes 14 and 15 not only the one light emitting layer 16 but the layer different from a some light emitting layer and a light emitting layer may be provided as needed.
  • the light emitting layer 16 extends along the arrangement direction X across the plurality of organic EL elements 13.
  • the plurality of organic EL elements 13 connected in series, from the light emitting layer 16 of the organic EL element 13 provided at one end in the arrangement direction X (left end in FIG. 1), the other end in the arrangement direction X (in FIG. 1).
  • the light emitting layer extending along the arrangement direction X is continuously and integrally formed up to the light emitting layer 16 of the organic EL element 13 provided at the right end).
  • the predetermined layer extends along the arrangement direction X across the plurality of organic EL elements 13.
  • the organic EL elements 13 may be formed so as to be separated from each other.
  • the predetermined layer different from the light emitting layer 16 is arranged across the plurality of organic EL elements 13 like the light emitting layer 16. It preferably extends along the direction X. This is because, as will be described later, a step of removing a layer formed at an unnecessary portion can be omitted.
  • the first and second electrodes 14 and 15 have extending portions 17 and 18, respectively.
  • the extending portions 17 and 18 are viewed from the thickness direction Z (one direction) of the support substrate 12 (hereinafter sometimes referred to as “in plan view”), and the thickness direction Z and the arrangement direction X of the support substrate 12.
  • the main body portions (referred to as a first main body portion and a second main body portion) extend in the width direction Y perpendicular to the light emitting layer 16 so as to protrude from the light emitting layer 16.
  • the extension part 17 (17 a, 17 b) of the first electrode 14 is formed integrally with the main body part of the first electrode 14.
  • the extending portion 18 (18a, 18b) of the second electrode 15 is formed integrally with the main body portion of the second electrode 15.
  • the first electrode 14 and the second electrode 15 (a pair of electrodes) constituting each organic EL element 13 are not configured to be in contact with each other for each organic EL element 13, and in plan view (Z-axis)
  • the extending portion 17 of the first electrode 14 and the extending portion 18 of the second electrode 15 are arranged so as not to overlap each other.
  • the extending portion 17 of the first electrode 14 extends in the width direction Y from the left end portion (hereinafter also referred to as the left end portion) of the portion facing the second electrode 15 in the first electrode 14. Extend.
  • the extending portion 18 of the second electrode 15 extends in the width direction Y from the right end portion (hereinafter sometimes referred to as the right end portion) of the second electrode 15 facing the first electrode 14. Yes. Therefore, the extending portion 17 of the first electrode 14 and the extending portion 18 of the second electrode 15 do not overlap in a plan view and are not in direct contact.
  • One electrode of the first and second electrodes 14 and 15 has a connection portion.
  • This connecting portion extends from the extending portion to the other electrode of the organic EL element adjacent in the arrangement direction X in the arrangement direction X, and is connected to the other electrode.
  • the connecting portion is not limited to one electrode of the first and second electrodes 14 and 15 (out of the pair of electrodes), but the other electrode of the first and second electrodes 14 and 15 (out of the pair of electrodes). May also be included. That is, the other of the first and second electrodes 14 and 15 (of the pair of electrodes) also extends in the arrangement direction X from the extending portion to one electrode of the organic EL element adjacent in the arrangement direction X. You may have the connection part connected to this one electrode.
  • the first electrode 14 corresponding to one of the first and second electrodes 14 and 15 has a connection portion 19. That is, the first electrode 14 extends to the left from the extending portion 17 of the first electrode 14 to the extending portion 18 of the second electrode 15 (the other electrode) of the organic EL element disposed on the left side.
  • a connection unit 19 is provided. As described above, the connection portion 19 of the first electrode 14 overlaps with the extension portion 18 of the second electrode 15 (the other electrode) of the organic EL element disposed on the left side in a plan view, and directly at the overlapping portion. It is connected to the second electrode 15 (the other electrode).
  • the extending portion 18 extending in the width direction Y from the light emitting layer 16 in a plan view is provided in one or the other of the width directions Y, but is preferably provided in both the width directions Y. That is, the extended portions 17 and 18 protrude from the light emitting layer 16 in the width direction Y and the first extending portions 17a and 18a extending so as to protrude from the light emitting layer in one of the width directions in a plan view. It is preferable to include the second extending portions 17b and 18b extending so as to.
  • the first electrode 14 and the second electrode 15 of the adjacent organic EL element 13 are both in the width direction Y. Will be connected at the end.
  • the first electrode 14 of the organic EL element 13 arranged on the leftmost side and the second electrode 15 of the organic EL element 13 arranged on the rightmost side. are respectively connected to wirings electrically connected to the power supply unit EP (see FIG. 18).
  • the power supply unit EP As a result, power is supplied from the power supply unit EP to the plurality of organic EL elements 13 constituting the series connection, and each organic EL element emits light.
  • Each organic EL element 13 is supplied with power from the connecting portion.
  • the organic EL elements 13 are supplied with power from both ends in the width direction Y by providing the extending portions 17 and 18 extending in the width direction Y from the light emitting layer 16 in plan view.
  • the luminance decreases due to a voltage drop.
  • the luminance decreases due to the voltage drop. Since power is supplied from the end portion, the influence of the voltage drop can be suppressed as compared with the element configuration supplied from one end portion in the width direction Y, and thus luminance unevenness can be suppressed.
  • Organic EL elements include a bottom emission type configuration, a top emission type configuration, and a dual emission type configuration.
  • the bottom emission type organic EL element emits light to the outside through the support substrate
  • the top emission type organic EL element emits light to the outside from the side opposite to the support substrate
  • the double emission type organic EL element is Light is emitted to the outside from both the support substrate side and the opposite side of the support substrate.
  • any of a bottom emission type, a top emission type, and a double emission type organic EL element can be adopted.
  • the first electrode 14 is constituted by an electrode exhibiting optical transparency, and conversely, the second electrode 15 is usually constituted by an electrode that reflects light. Composed.
  • the second electrode 15 is composed of an electrode exhibiting optical transparency, and conversely, the first electrode 14 is usually composed of an electrode that reflects light. Composed.
  • both the first and second electrodes 14 and 15 are composed of electrodes exhibiting light transmittance.
  • the first and second electrodes 14 and 15 are configured by an electrode exhibiting optical transparency.
  • the electrode exhibiting optical transparency is used.
  • 14 (15) consists of a mesh-like translucent electrode (mesh electrode) configured by arranging conductors in a mesh pattern (see FIG. 9). That is, the mesh-like translucent electrode 14 (15) has a plurality of openings OP arranged two-dimensionally.
  • the mesh-like translucent electrode includes a conductor arranged in a mesh shape.
  • This conductor forms a network structure in a two-dimensional plane parallel to the main surface of the support substrate 12.
  • the network structure only needs to have a structure in which conductors are continuously formed in at least the two-dimensional plane and are electrically connected.
  • a regular structure such as a lattice structure or a honeycomb structure is used. It may have or may not have a regular structure.
  • the conductor of the mesh-like translucent electrode is preferably composed of a mixture of a conductive filler and a resin, or only a conductive material.
  • conductive filler metal fine particles made of Au, Ag, Al, carbon or the like, or a conductive wire made of Au, Ag, Al, carbon or the like can be used.
  • the resin mixed with the conductive filler may be a resin such as epoxy, acrylic, nylon, urethane, phenol, or a conductive resin such as 3,4-polyethylenedioxythiophene / polystyrene sulfonic acid. it can.
  • the conductive material constituting the conductor of the mesh-like translucent electrode can be made of Au, Ag, Al, Cu alone or an alloy containing one or more of these metals.
  • the mesh-like translucent electrode has a non-translucent portion made of a conductor that forms a mesh-like structure in a two-dimensional plane parallel to the main surface of the support substrate 12.
  • the light incident on the mesh-like translucent electrode is transmitted through the mesh-like translucent electrode through the remaining region (hereinafter also referred to as a translucent portion) excluding the non-translucent portion.
  • the mesh-like translucent electrode has a non-translucent portion, it has translucency as a whole when viewed macroscopically to the extent that it is visible to the human eye.
  • a transparent conductive layer may be laminated on one main surface or both main surfaces of the mesh-like translucent electrode in contact with the mesh-like translucent electrode. By laminating the transparent conductive layer in this manner, the conductivity of the light transmitting part can be increased, and further, the step between the light transmitting part and the non-light transmitting part can be reduced.
  • a transparent conductive layer a transparent conductive resin such as a metal oxide such as ITO or ZTO, polyaniline or a derivative thereof, or polythiophene or a derivative thereof can be used.
  • the transparent conductive resin has a lower refractive index than metal oxides such as ITO and ZTO, the light emitted from the light emitting layer can be emitted from the light emitting device even when the transparent conductive resin is laminated on the light transmitting portion. It can be taken out efficiently.
  • the transparent conductive layer can be formed by a vacuum deposition method, a sputtering method, an ion plating method, a printing method using ink, an ink jet method, or the like.
  • the sheet resistance of the mesh-like translucent electrode is preferably 10 ( ⁇ / sq.) Or less, and more preferably 5 ( ⁇ / sq.) From the viewpoint of improving the light emission efficiency of the organic EL element, reducing luminance unevenness and heat generation. .) Or less, more preferably 1 ( ⁇ / sq.) Or less.
  • the film thickness of the mesh-like translucent electrode is appropriately selected from the viewpoint of the conductivity of the mesh-like translucent electrode and the ease of production of the organic EL device, and is preferably 50 nm to 1 ⁇ m, more preferably 100 nm to 500 nm. preferable.
  • the aperture ratio of the mesh-like translucent electrode that is, the ratio of the translucent portion per unit area is appropriately selected in consideration of the conductivity and the light extraction efficiency, but is preferably 30 to 95%, and more preferably 50 to 90. % Is more preferable.
  • the line width of the conductors arranged in a mesh shape is appropriately selected in consideration of conductivity and light extraction efficiency, but is preferably 5 ⁇ m to 1 mm, more preferably 10 ⁇ m to 200 ⁇ m.
  • the area of each light-transmitting portion surrounded by the conductors arranged in a mesh shape is preferably 100 ⁇ m 2 to 4 mm 2 on average, and more preferably 400 ⁇ m 2 to 1 mm 2 .
  • the light transmittance of the mesh-like translucent electrode is preferably 30% or more, preferably 50% or more, and more preferably 70% or more.
  • the light transmittance in this specification means visible light transmittance.
  • the mesh-like translucent electrode may be formed by (1) first forming a conductive thin film made of the above-described conductor on one surface and further patterning this conductive thin film into a mesh shape by a predetermined method. (2) The above-described conductor may be directly patterned in a mesh shape.
  • a conductive thin film made of a conductor is formed on one surface by a vacuum deposition method, a sputtering method, an ion plating method, etc., and then the conductive thin film is patterned by a photolithography method.
  • a transparent electrode can be formed.
  • a coating liquid in which the conductive filler and the resin are dispersed in a predetermined dispersion medium is applied and formed by a predetermined application method, and this is patterned by a photolithography method to form a mesh-like translucent electrode. be able to.
  • a mesh-like translucent electrode is formed by forming the conductor in a mesh shape by a vacuum deposition method, a sputtering method, an ion plating method or the like using a mask having a predetermined pattern. Can be formed.
  • a network-like translucent electrode is patterned by applying a coating liquid in which the conductive filler and the resin are dispersed in a predetermined dispersion medium to form a coating liquid by a printing method, an ink-jet method, or the like. can do.
  • a mesh-like translucent electrode prepared in advance on a predetermined base different from the support substrate 12 is transferred onto the support substrate 12 by a laminating method, whereby the mesh-like translucent electrode is formed on the support substrate 12. May be formed.
  • the method for manufacturing a light-emitting device includes a support substrate and a plurality of organic electroluminescent elements provided on the support substrate along a predetermined arrangement direction and connected in series.
  • Each of the organic electroluminescence elements includes a pair of electrodes and a light emitting layer provided between the electrodes, the light emitting layer straddling the plurality of organic electroluminescence elements, the predetermined arrangement
  • Each of the pair of electrodes extends in a direction perpendicular to both the thickness direction of the support substrate and the arrangement direction when viewed from one thickness direction of the support substrate.
  • One of the pair of electrodes is the other of the organic electroluminescence elements adjacent in the arrangement direction.
  • a connecting portion extending from the extending portion to the other electrode in the arrangement direction and connected to the other electrode, wherein at least one of the pair of electrodes has a conductor mesh A method of manufacturing a light-emitting device that is a mesh-like translucent electrode that is arranged in the form of an ink containing a material that becomes the light-emitting layer, the predetermined arrangement direction across the plurality of organic EL elements And a step of forming a light-emitting layer by solidifying the applied coating.
  • FIGS. 2 to 5 (A) is a plan view and (B) is a cross-sectional view.
  • the support substrate 12 is prepared.
  • a support substrate 12 on which a drive circuit (not shown) for driving the organic EL element 13 is formed in advance may be prepared.
  • the first electrode 14 is patterned on the support substrate 12 (see FIGS. 2A and 2B).
  • a mesh-like translucent electrode configured by arranging the above-described conductors in the form of a mesh as the first electrode 14 is formed in a pattern on the support substrate 12. The method for forming this mesh-like translucent electrode is as described above.
  • the first electrode is a non-transparent electrode, for example, a conductor film is formed on the support substrate 12 by sputtering or vapor deposition, and then the conductor film is patterned into a predetermined shape by photolithography. By doing so, the first electrode 14 can be patterned.
  • the first electrode 14 may be pattern-formed only at a predetermined portion by a mask vapor deposition method or the like without performing a photolithography process.
  • the first electrode 14 may be formed by transferring a conductive thin film by a laminating method.
  • a support substrate 12 on which the first electrode 14 is formed in advance may be prepared.
  • the light emitting layer 16 is formed on the support substrate 12 (see FIGS. 3A and 3B).
  • the light emitting layer 16 may be formed by continuously applying an ink containing a material to be the light emitting layer 16 along the arrangement direction X across the plurality of organic EL elements 13 and solidifying the applied coating film. it can.
  • Examples of the ink application method include a cap coating method, a slit coating method, a spray coating method, a printing method, an ink jet method, and a nozzle printing method. Among these methods, a large area can be efficiently applied. Possible cap coating methods, slit coating methods, spray coating methods and printing methods are preferred.
  • the second electrode 15 is formed on the support substrate 12 (see FIGS. 1A and 1B).
  • the second electrode 15 is a light-transmitting electrode
  • a mesh-like translucent electrode configured by arranging the above-described conductors in the form of a mesh is formed on the light-emitting layer 16 as a pattern.
  • the method for forming this mesh-like translucent electrode is as described above.
  • the second electrode 15 is a non-translucent electrode, for example, a conductor film is formed on the support substrate 12 by sputtering or vapor deposition, and then the conductor film is formed into a predetermined shape by photolithography.
  • the second electrode 15 can be patterned by patterning. Note that the second electrode 15 may be patterned only on a predetermined portion by a mask vapor deposition method or the like without performing a photolithography process.
  • a predetermined layer different from the light emitting layer 16 may be provided between the first and second electrodes 14 and 15.
  • a predetermined layer different from the light emitting layer 16 is formed by a coating method
  • a predetermined layer different from 16 is formed.
  • a predetermined layer different from the light emitting layer is formed by a dry method such as vapor deposition
  • the predetermined layer different from the light emitting layer may be selectively formed only on the first electrode 14.
  • Examples of the ink application method include a cap coating method, a slit coating method, a spray coating method, a printing method, an ink jet method, and a nozzle printing method. Among these methods, a large area can be efficiently applied. Possible cap coating methods, slit coating methods, spray coating methods and printing methods are preferred.
  • the light emitting layer 16 not only the light emitting layer 16 but also a predetermined layer different from the light emitting layer 16 may be further provided between the first and second electrodes 14 and 15.
  • the first electrode 14 is an anode
  • the second electrode 15 is a cathode
  • examples of the layer provided between the cathode 15 and the light emitting layer 16 include an electron transport layer and a hole blocking layer.
  • the first electrode 14 will be described as the anode 14 and the second electrode 15 will be described as the cathode 15 as necessary. However, these arrangements can be replaced.
  • the hole blocking layer has a function of blocking hole transport.
  • these layers may also serve as the hole blocking layer.
  • Examples of the layer Y provided between the anode 14 and the light emitting layer 16 include a hole injection layer, a hole transport layer, and an electron block layer.
  • the organic EL element can include a predetermined layer in addition to the light emitting layer between the pair of electrodes as described above.
  • the organic EL layer 10 formed between the electrode (anode) 14 and the electrode (cathode) 15 formed on the support substrate 12 has the following structure.
  • the organic EL element has an organic layer Y between the electrode (anode) 14 and the light emitting layer 16 and an organic layer between the electrode (cathode) 15 and the light emitting layer 16. It can be set as the structure where the layer X interposes.
  • the organic EL element has a structure in which an organic layer Y is interposed between an electrode (anode) 14 and a light emitting layer 16, and an electrode 15 is formed directly on the light emitting layer 16. It can be set as a structure.
  • the organic EL element has a structure in which the organic layer X is interposed between the electrode (cathode) 15 and the light emitting layer 16 and the light emitting layer 16 is in direct contact with the electrode 14. It can be.
  • the organic layer X may be composed of two or more kinds of organic layers X1 and X2 as shown in FIG. 13, and the organic layer Y is composed of two or more kinds of organic layers Y1 and Y2 as shown in FIG. It may be.
  • only the light emitting layer 16 may be formed between the anode 14 and the cathode 15 as shown in FIG.
  • Examples of the layer X provided between the cathode 15 and the light emitting layer 16 include an electron injection layer, an electron transport layer, and a hole blocking layer. As shown in FIG. 13, when both the electron injection layer X1 and the electron transport layer X2 are provided between the cathode 15 and the light emitting layer 16, the layer in contact with the cathode 15 is referred to as the electron injection layer X1, The layer excluding the electron injection layer X1 is referred to as an electron transport layer X2.
  • the layer in contact with the anode 14 is defined as the hole injection layer.
  • the layer excluding the hole injection layer Y1 is referred to as Y1, and is referred to as a hole transport layer Y2.
  • the hole injection layer has a function of improving the hole injection efficiency from the anode.
  • the hole transport layer has a function of improving hole injection from a layer in contact with the surface on the anode side.
  • the electron blocking layer has a function of blocking electron transport. When the hole injection layer and / or the hole transport layer has a function of blocking electron transport, these layers may also serve as an electron blocking layer.
  • the electron injection layer and the hole injection layer may be collectively referred to as a charge injection layer, and the electron transport layer and the hole transport layer may be collectively referred to as a charge transport layer.
  • FIG. 17 Anode 14 / light emitting layer 16 / cathode 15 (see FIG. 17)
  • B Anode 14 / hole injection layer Y / light emitting layer 16 / cathode 15 (see FIG. 11)
  • C Anode 14 / hole injection layer Y / light emitting layer 16 / electron injection layer X / cathode 15 (see FIG. 10)
  • D Anode 14 / hole injection layer Y / light emitting layer 16 / electron transport layer X2 / electron injection layer X1 / cathode 15 (see FIGS.
  • the organic EL element of this embodiment may have two or more light emitting layers.
  • any one of the layer configurations (a) to (i) above if the laminate sandwiched between the anode and the cathode is “structural unit A”, an organic EL device having two light-emitting layers is obtained.
  • the layer configuration shown in the following (j) can be given. Note that the two (structural unit A) layer structures may be the same or different.
  • Anode 14 / structural unit A / charge generation layer Z / structural unit A / cathode 15 see FIG. 15
  • the charge generation layer Z is a layer that generates holes and electrons by applying an electric field.
  • Examples of the charge generation layer Z include vanadium oxide and indium tin oxide (Indium).
  • a thin film made of tin oxide (abbreviated as ITO), molybdenum oxide, or the like can be given.
  • structural unit A / charge generation layer Z is “structural unit B”
  • a layer configuration shown in the following (k) can be given as a configuration of an organic EL element having three or more light emitting layers.
  • Anode 14 / (structural unit B) x / (structural unit A) / cathode 15 see FIG. 16
  • (structural unit B) x represents a stacked body in which the structural unit B is stacked in x stages.
  • a plurality of (structural units B) may have the same or different layer structure.
  • an organic EL element in which a plurality of light emitting layers are directly stacked may be configured without providing the charge generation layer Z.
  • the support substrate 12 is preferably one that does not change chemically in the process of manufacturing the organic EL element.
  • glass, plastic, a polymer film, a silicon plate, and a laminate of these are used.
  • a drive substrate in which a drive circuit for driving the organic EL element is formed in advance may be used as the support substrate.
  • a substrate exhibiting light transmittance is used as the support substrate 12.
  • At least one of the anode and the cathode is composed of a translucent electrode.
  • the said translucent electrode is comprised by the mesh-like translucent electrode mentioned above.
  • an anode and a cathode are translucent electrodes, at least one should just be comprised from the said mesh-like translucent electrode, and the other may be comprised by the electrode which shows a light transmittance.
  • a transparent conductive resin such as metal oxide such as ITO or ZTO, polyaniline or a derivative thereof, polythiophene or a derivative thereof may be used.
  • Such an electrode having optical transparency can be formed by a vacuum deposition method, a sputtering method, an ion plating method, a printing method using ink, an ink jet method, or the like.
  • An electrode exhibiting translucency may be used as one of the anode and the cathode, and the material of the electrode exhibiting such translucency is preferably a material having high electrical conductivity, such as visible light.
  • a highly reflective material is preferred.
  • Gold, silver, platinum, copper, aluminum, manganese, titanium, cobalt, nickel, tungsten, tin, or an alloy containing one or more, or graphite or a graphite intercalation compound is used for the electrode exhibiting light-impermeable properties. It is done.
  • the light-transmitting electrode may be formed of a stacked body in which two or more layers are stacked.
  • the film thickness of the non-translucent electrode is appropriately designed in consideration of required characteristics and process simplicity, and is, for example, 10 nm to 10 ⁇ m, preferably 20 nm to 1 ⁇ m, more preferably 50 nm to 500 nm. It is.
  • Examples of a method for manufacturing an electrode having light-transmitting properties include a vacuum deposition method, a sputtering method, and a lamination method in which a metal thin film is thermocompression bonded.
  • hole injection material constituting the hole injection layer
  • metal oxides such as vanadium oxide, molybdenum oxide, ruthenium oxide and aluminum oxide, phenylamine compounds, starburst amine compounds, phthalocyanines, amorphous carbon, Examples thereof include polyaniline and polythiophene derivatives.
  • Examples of the method for forming the hole injection layer include film formation from a solution containing a hole injection material.
  • a hole injection layer can be formed by coating a film containing a hole injection material by a predetermined coating method and solidifying the solution.
  • Solvents used for film formation from solution include chlorine solvents such as chloroform, methylene chloride and dichloroethane, ether solvents such as tetrahydrofuran, aromatic hydrocarbon solvents such as toluene and xylene, and ketones such as acetone and methyl ethyl ketone. Examples thereof include solvents, ester solvents such as ethyl acetate, butyl acetate, and ethyl cellosolve acetate, and water.
  • chlorine solvents such as chloroform, methylene chloride and dichloroethane
  • ether solvents such as tetrahydrofuran
  • aromatic hydrocarbon solvents such as toluene and xylene
  • ketones such as acetone and methyl ethyl ketone. Examples thereof include solvents, ester solvents such as ethyl acetate, butyl acetate, and ethyl cellosolve acetate, and water.
  • the film thickness of the hole injection layer is appropriately set in consideration of required characteristics and process simplicity, and is, for example, 1 nm to 1 ⁇ m, preferably 2 nm to 500 nm, and more preferably 5 nm to 200 nm.
  • ⁇ Hole transport layer> As the hole transport material constituting the hole transport layer, polyvinylcarbazole or a derivative thereof, polysilane or a derivative thereof, a polysiloxane derivative having an aromatic amine in a side chain or a main chain, a pyrazoline derivative, an arylamine derivative, a stilbene derivative, Triphenyldiamine derivative, polyaniline or derivative thereof, polythiophene or derivative thereof, polyarylamine or derivative thereof, polypyrrole or derivative thereof, poly (p-phenylene vinylene) or derivative thereof, or poly (2,5-thienylene vinylene) or Examples thereof include derivatives thereof.
  • hole transport materials include polyvinyl carbazole or derivatives thereof, polysilane or derivatives thereof, polysiloxane derivatives having aromatic amine compound groups in the side chain or main chain, polyaniline or derivatives thereof, polythiophene or derivatives thereof, poly Polymeric hole transport materials such as arylamine or derivatives thereof, poly (p-phenylene vinylene) or derivatives thereof, or poly (2,5-thienylene vinylene) or derivatives thereof are preferred, and polyvinylcarbazole or derivatives thereof are more preferred. , Polysilane or a derivative thereof, and a polysiloxane derivative having an aromatic amine in the side chain or main chain. In the case of a low-molecular hole transport material, it is preferably used by being dispersed in a polymer binder.
  • Examples of the method for forming the hole transport layer include film formation from a solution containing a hole transport material.
  • a hole transport layer can be formed by coating a film containing a hole transport material by a predetermined coating method and solidifying the solution.
  • a film may be formed using a solution in which a polymer binder is further mixed.
  • Solvents used for film formation from solution include, for example, chlorine solvents such as chloroform, methylene chloride, dichloroethane, ether solvents such as tetrahydrofuran, aromatic hydrocarbon solvents such as toluene and xylene, and ketones such as acetone and methyl ethyl ketone.
  • Examples thereof include ester solvents such as system solvents, ethyl acetate, butyl acetate, and ethyl cellosolve acetate.
  • polystyrene examples include vinyl chloride and polysiloxane.
  • the film thickness of the hole transport layer is appropriately set in consideration of required characteristics and process simplicity, and is, for example, 1 nm to 1 ⁇ m, preferably 2 nm to 500 nm, and more preferably 5 nm to 200 nm. .
  • the light emitting layer is usually formed of an organic substance that mainly emits fluorescence and / or phosphorescence, or an organic substance and a dopant that assists the organic substance. For example, a dopant is added in order to improve luminous efficiency and change the emission wavelength.
  • the organic substance contained in the light emitting layer may be a low molecular compound or a high molecular compound.
  • the light-emitting layer preferably contains a high molecular compound, and the number average molecular weight in terms of polystyrene as the high molecular compound Preferably contain from 10 3 to 10 8 compounds.
  • the light emitting material constituting the light emitting layer include the following dye materials, metal complex materials, polymer materials, and dopant materials.
  • dye-based materials include cyclopentamine derivatives, tetraphenylbutadiene derivative compounds, triphenylamine derivatives, oxadiazole derivatives, pyrazoloquinoline derivatives, distyrylbenzene derivatives, distyrylarylene derivatives, pyrrole derivatives, thiophene ring compounds. Pyridine ring compounds, perinone derivatives, perylene derivatives, oligothiophene derivatives, oxadiazole dimers, pyrazoline dimers, quinacridone derivatives, coumarin derivatives, and the like.
  • Metal complex materials examples include rare earth metals such as Tb, Eu, and Dy, or Al, Zn, Be, Ir, Pt, etc. as a central metal, and oxadiazole, thiadiazole, phenylpyridine, phenylbenzimidazole, quinoline.
  • metal complexes having a structure as a ligand such as metal complexes having light emission from triplet excited states such as iridium complexes and platinum complexes, aluminum quinolinol complexes, benzoquinolinol beryllium complexes, and benzoxazolyl zinc.
  • a complex, a benzothiazole zinc complex, an azomethylzinc complex, a porphyrin zinc complex, a phenanthroline europium complex, and the like can be given.
  • Polymer material As polymer materials, polyparaphenylene vinylene derivatives, polythiophene derivatives, polyparaphenylene derivatives, polysilane derivatives, polyacetylene derivatives, polyfluorene derivatives, polyvinyl carbazole derivatives, the above dye materials and metal complex light emitting materials are polymerized. Things can be mentioned.
  • materials that emit blue light include distyrylarylene derivatives, oxadiazole derivatives, and polymers thereof, polyvinylcarbazole derivatives, polyparaphenylene derivatives, polyfluorene derivatives, and the like.
  • polymer materials such as polyvinyl carbazole derivatives, polyparaphenylene derivatives, and polyfluorene derivatives are preferred.
  • examples of materials that emit green light include quinacridone derivatives, coumarin derivatives, and polymers thereof, polyparaphenylene vinylene derivatives, polyfluorene derivatives, and the like. Of these, polymer materials such as polyparaphenylene vinylene derivatives and polyfluorene derivatives are preferred.
  • Examples of materials that emit red light include coumarin derivatives, thiophene ring compounds, and polymers thereof, polyparaphenylene vinylene derivatives, polythiophene derivatives, and polyfluorene derivatives. Among these, polymer materials such as polyparaphenylene vinylene derivatives, polythiophene derivatives, and polyfluorene derivatives are preferable.
  • Examples of the dopant material include perylene derivatives, coumarin derivatives, rubrene derivatives, quinacridone derivatives, squalium derivatives, porphyrin derivatives, styryl dyes, tetracene derivatives, pyrazolone derivatives, decacyclene, phenoxazone, and the like. Note that the thickness of such a light emitting layer is usually about 2 nm to 200 nm.
  • the light emitting layer is formed, for example, by film formation from a solution.
  • a light emitting layer is formed by applying a solution containing a light emitting material by a predetermined application method and further solidifying the solution.
  • the solvent used for film formation from a solution include the same solvents as those used for forming a hole injection layer from the aforementioned solution.
  • an electron transport material constituting the electron transport layer an oxadiazole derivative, anthraquinodimethane or a derivative thereof, benzoquinone or a derivative thereof, naphthoquinone or a derivative thereof, anthraquinone or a derivative thereof, tetracyanoanthraquinodimethane or a derivative thereof, Fluorenone derivatives, diphenyldicyanoethylene or derivatives thereof, diphenoquinone derivatives, or metal complexes of 8-hydroxyquinoline or derivatives thereof, polyquinoline or derivatives thereof, polyquinoxaline or derivatives thereof, polyfluorene or derivatives thereof, and the like can be given.
  • Examples of the method for forming the electron transport layer include a vapor deposition method and a film formation method from a solution.
  • a polymer binder may be used in combination.
  • the film thickness of the electron transport layer is appropriately set in consideration of required characteristics and process simplicity, and is, for example, 1 nm to 1 ⁇ m, preferably 2 nm to 500 nm, and more preferably 5 nm to 200 nm.
  • the material constituting the electron injection layer includes alkali metal, alkaline earth metal, an alloy containing at least one of alkali metal and alkaline earth metal, oxide of alkali metal or alkaline earth metal, halide, carbonic acid A salt or a mixture of these substances can be used.
  • alkali metals, alkali metal oxides, halides, and carbonates include lithium, sodium, potassium, rubidium, cesium, lithium oxide, lithium fluoride, sodium oxide, sodium fluoride, potassium oxide, potassium fluoride , Rubidium oxide, rubidium fluoride, cesium oxide, cesium fluoride, lithium carbonate, and the like.
  • alkaline earth metals, alkaline earth metal oxides, halides and carbonates include magnesium, calcium, barium, strontium, magnesium oxide, magnesium fluoride, calcium oxide, calcium fluoride, barium oxide, Examples thereof include barium fluoride, strontium oxide, strontium fluoride, and magnesium carbonate.
  • An electron injection layer may be comprised by the laminated body which laminated
  • the electron injection layer is formed by vapor deposition, sputtering, printing, or the like.
  • the thickness of the electron injection layer is preferably about 1 nm to 1 ⁇ m.
  • the first electrode 14 and the second electrode 15 of the adjacent organic EL elements 13 are connected in a region protruding in the width direction Y from the region where the light emitting layer 16 is formed in plan view.
  • the adjacent organic EL elements 13 are connected in series, so that it is not necessary to connect the first electrode 14 and the second electrode 15 of the adjacent organic EL elements 13 in the region between the organic EL elements 13.
  • a light emitting layer or the like may be formed in a region between adjacent organic EL elements 13, whereby a light emitting layer formed in a region between adjacent organic EL elements 13 when forming a light emitting layer by a coating method.
  • the step of removing can be omitted. Therefore, even if it is a coating method such as a cap coat method that is relatively poor at applying a fine pattern, a plurality of organic EL elements 13 connected in series can be easily produced.
  • a light emitting device with little light emission unevenness and heat generation can be realized even if the light emitting area of the organic EL element is increased.
  • FIGS. 4A and 4B are diagrams schematically showing the light emitting device 31 of the second embodiment. Since the light emitting device 31 of the present embodiment is different from the light emitting device 11 of the first embodiment described above only in the shapes of the first electrode 14 and the second electrode 15, only the first electrode 14 and the second electrode 15 will be described. Parts corresponding to those in the first embodiment are denoted by the same reference numerals, and redundant description is omitted.
  • the second electrode 15 in addition to the first electrode 14, the second electrode 15 also has a connection portion 32. That is, the second electrode 15 has a connecting portion 32 that extends from the extending portion to the first electrode 14 of the organic EL element adjacent in the arranging direction X in the arranging direction X and is connected to the first electrode 15.
  • the connecting portion 19 extends to the left from the extending portion 17 of the first electrode 14 of the organic EL element 13 disposed on the right side, and the left side
  • the connecting portion 32 extends rightward from the extending portion 18 of the second electrode 15 of the organic EL element 13 disposed in the connecting portion 19 of the first electrode 14 and the connecting portion 32 of the second electrode 15.
  • the first electrode 14 and the second electrode 15 of the pair of adjacent organic EL elements 13 are connected.
  • FIG. 5 is a diagram schematically showing the light emitting device 41 of the third embodiment. Since the light emitting device 41 of the present embodiment is different from the light emitting device 11 of the first embodiment described above only in the shapes of the first electrode 14 and the second electrode 15, only the first electrode 14 and the second electrode 15 will be described. Parts corresponding to those in the first embodiment are denoted by the same reference numerals, and redundant description is omitted.
  • the first electrode 14 does not have the connection portion 19, and conversely, the second electrode 15 has the connection portion 42. That is, the second electrode 15 has a connecting portion 42 that extends from the extending portion to the first electrode 14 of the organic EL element adjacent in the arranging direction X in the arranging direction X and is connected to the first electrode 15.
  • the said connection parts 19, 32, and 42 are electrically connected by contacting the electrode or connection part which each opposes.
  • the first electrode 14 has the connection portion 19, and conversely, in the light emitting device 41 of the third embodiment shown in FIG. 5, only the second electrode 15 is connected. Part 42.
  • the first and second electrodes Of the electrodes 14 and 15 (a pair of electrodes)
  • it is preferable that only the electrode having the lower sheet resistance has the connection portion. That is, when the sheet resistance of the first electrode 14 is lower than the sheet resistance of the second electrode 15, it is preferable that only the first electrode 14 has the connection portion 19 as in the light emitting device 11 of the first embodiment shown in FIG. 1.
  • the sheet resistance of the second electrode 15 is lower than the sheet resistance of the first electrode 14, only the second electrode 15 may have the connection portion 42 as in the light emitting device 41 of the third embodiment shown in FIG. 5. preferable.
  • each embodiment mentioned above has shown the light-emitting device by which one series connection was comprised by the some organic EL element, even if it is a light-emitting device by which the some series connection was comprised by the some organic EL element, it implements.
  • a form of electrode structure can be employed.
  • the electrode structure of embodiment is employable.
  • FIG. 6 is a view showing a light emitting device 61 according to the fourth embodiment.
  • the light emitting device 61 of the present embodiment is a light emitting device having a configuration in which two rows of organic EL element groups ELA and ELB connected in series are connected in parallel. Each series connection includes three organic EL elements connected in series.
  • the configuration of the individual organic EL element groups ELA and ELB is the same as that of the first embodiment, but this can be replaced with that of the second to third embodiments.
  • Two rows of organic EL element groups ELA and ELB connected in series are electrically connected in parallel with each other at one end and the other end.
  • the voltage of a drive source that drives the elements increases as the number of organic EL elements increases.
  • the supply voltage required for the source can be moderately suppressed.
  • the light-emitting device includes (1) a plurality of organic electroluminescent elements that are provided on the support substrate along a predetermined arrangement direction and connected in series.
  • Each organic electroluminescence element includes a pair of electrodes and a light emitting layer provided between the electrodes, and (3) the light emitting layer includes the plurality of organic electroluminescence elements.
  • the electrode is a mesh-like translucent electrode configured by arranging conductors in a mesh shape.
  • the conductive material of the mesh-like translucent electrode is characterized by comprising only a mixture of a conductive filler and a resin, or a conductive material.
  • the sheet-like translucent electrode has a sheet resistance of 5 ( ⁇ / sq.) Or less.
  • the light transmittance of the mesh-like translucent electrode is 50% or more.
  • the plurality of extending portions extend from the light emitting layer so as to protrude from the light emitting layer to one side in the width direction, and protrude from the light emitting layer to the other in the width direction.
  • another extension part extending to the surface.
  • a method for manufacturing a light-emitting device includes (1) a support substrate and a plurality of organic electroluminescence elements that are provided on the support substrate along a predetermined arrangement direction and connected in series.
  • Each organic electroluminescence element includes a pair of electrodes and a light emitting layer provided between the electrodes, and (3) the light emitting layer is provided on the plurality of organic electroluminescence elements.
  • each of the pair of electrodes is seen in one of the thickness directions of the support substrate, either the thickness direction of the support substrate or the alignment direction.
  • one electrode of the pair of electrodes is adjacent to the array direction in the width direction perpendicular to the light emitting layer.
  • connection part extending from the extension part to the other electrode of the luminescence element in the arrangement direction and connected to the other electrode; (6) at least one electrode of the pair of electrodes Is a method for manufacturing a light-emitting device which is a mesh-like translucent electrode configured by arranging conductors in a mesh pattern, and (7) an ink containing a material to be the light-emitting layer is used as the plurality of organic EL elements. It is characterized by including a step of forming a light emitting layer by applying continuously along the predetermined arrangement direction across the element and solidifying the applied coating film.
  • the ink may be applied by a cap coating method, a slit coating method, or a slit coating method. It is characterized in that it is a coating method, a spray coating method or a printing method.

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  • Electroluminescent Light Sources (AREA)

Abstract

L'invention concerne un dispositif électroluminescent qui comprend: une pluralité de premières électrodes disposées sur un substrat de support; une couche électroluminescente recouvrant la pluralité de premières électrodes; et une pluralité de secondes électrodes disposées sur la couche électroluminescente faisant face à la pluralité de premières électrodes. Chaque électrode des premières et secondes électrodes présente une section corps et une section extension. Au moins une électrode de chaque paire des premières et secondes électrodes présente une section de raccordement qui s'étend dans le sens de la disposition des électrodes et est reliée à l'autre électrode. En outre, au moins l'une des électrodes est une électrode à mailles.
PCT/JP2011/076945 2010-11-24 2011-11-22 Dispositif électroluminescent et procédé de production de celui-ci WO2012070586A1 (fr)

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