JP2017033849A - Organic electroluminescent element, manufacturing method of organic electroluminescent element, and illumination device - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide an organic electroluminescent element capable of displaying images in different shapes from the same region in spite of a further simplified structure.SOLUTION: The organic electroluminescent element comprises: a transparent electrode; a reflection electrode; a plurality of light-emitting function layers each including a light-emitting layer that is configured using an organic material and disposed while being overlapped between the transparent electrode and the reflection electrode; and an intermediate electrode which is held between the light-emitting function layer and the light-emitting function layer and has light permeability. Each of the plurality of light-emitting function layers includes a light-emitting region and a light-non-emitting region that are patterned. In a first light-emitting function layer positioned closer to the transparent electrode among the plurality of light-emitting function layers, a wavelength for the light permeability to reach an upper limit value is set to a short wavelength side rather than a second light-emitting function layer positioned closer to the reflection electrode.SELECTED DRAWING: Figure 1

Description

  The present invention relates to an organic electroluminescent element, a method for manufacturing an organic electroluminescent element, and an illumination device, and more particularly to an organic electroluminescent element having a patterned light emitting region and a method for manufacturing the same.

  An organic electroluminescent element (so-called organic EL element) using electroluminescence (hereinafter referred to as EL) of an organic material has a structure in which an organic functional layer is sandwiched between two electrodes, and is generated in the organic functional layer. The emitted light passes through the electrode and is extracted outside. In recent years, as a method for manufacturing such an organic electroluminescent element, each of the light emitting patterns provided with a specific light emitting pattern after irradiating light to a light emitting unit composed of a pair of electrodes and an organic functional layer. A method of manufacturing an organic electroluminescent element that displays images of different shapes in the same region by stacking light emitting units has been proposed (see Patent Document 1 below).

Japanese Patent Laying-Open No. 2015-46364

  However, in the manufacturing method described above, since the light emitting unit having two electrodes is stacked, the thickness is large, the number of electrodes is large, and the element configuration is complicated.

  Accordingly, the present invention provides an organic electroluminescent device capable of displaying images of different shapes from the same region while having a simpler structure, and further provides a method for manufacturing the organic electroluminescent device, and the organic electroluminescent device. An object of the present invention is to provide an illumination device using an electroluminescent element.

  In order to achieve such an object, the present invention has a transparent electrode, a reflective electrode, and a light emitting layer composed of an organic material, and is disposed between the transparent electrode and the reflective electrode. A plurality of light emitting functional layers, and a light-transmitting intermediate electrode sandwiched between the light emitting functional layers and the light emitting functional layers, and each of the plurality of light emitting functional layers includes a patterned light emitting region and a non-light emitting region. The first light emitting functional layer located on the transparent electrode side of the plurality of light emitting functional layers has an upper light transmittance than the second light emitting functional layer located on the reflective electrode side. This is an organic electroluminescence device having a short wavelength side.

  The present invention also provides a method for producing an organic electroluminescent element having the above structure, and an illumination device using the organic electroluminescent element.

  According to the present invention as described above, it is possible to simplify the structure of the organic electroluminescent element capable of displaying images of different shapes from the same region, thereby enabling cost reduction. Become.

It is a section lineblock diagram showing an outline of an organic electroluminescent element of an embodiment. It is a principal part top view for demonstrating the structure of the organic electroluminescent element of embodiment. It is a light transmission spectrum of the light emission functional layer in the organic electroluminescent element of embodiment. It is sectional process drawing which shows the manufacturing method of the organic electroluminescent element of embodiment.

  Hereinafter, embodiments of the present invention will be described in detail in the order of an organic electroluminescent element, a method for manufacturing an organic electroluminescent element, and an illumination device in this order.

≪Organic electroluminescent element≫
FIG. 1 is a cross-sectional configuration diagram illustrating an outline of an organic electroluminescent element 1 according to an embodiment. Moreover, FIG. 2 is a principal part top view for demonstrating the structure of the organic electroluminescent element of embodiment.

  The organic electroluminescent element 1 shown in these drawings is provided on one main surface of the transparent substrate 10, and in order from the transparent substrate 10 side, the transparent electrode 11, the first light emitting functional layer 13, the intermediate electrode 15, and the second electrode. The light emitting functional layer 17 and the reflective electrode 19 are laminated. Each of the first light emitting functional layer 13 and the second light emitting functional layer 17 has light emitting regions 13a and 17a and non-light emitting regions 13b and 17b. In addition, a power source 23 is provided between the transparent electrode 11 and the intermediate electrode 15, and a power source 27 is provided between the intermediate electrode 15 and the reflective electrode 19. The power source 27 is independently controlled. Yes.

  The organic electroluminescent element 1 as described above has the other main surface of the transparent substrate 10 as the light extraction surface 10a, the first emitted light h1 obtained in the light emitting region 13a of the first light emitting functional layer 13, and the second light emitting function. The second emission light h2 obtained in the light emission region 17a of the layer 17 is configured as a bottom emission type that is extracted from the transparent substrate 10 side.

  In particular, the organic electroluminescent element 1 is characterized in that the first light emitting functional layer 13 and the second light emitting functional layer 17 are formed using materials having individual optical characteristics.

  Hereinafter, the detail of each component which comprises this organic electroluminescent element 1 is demonstrated in an order from the transparent substrate 10 side.

<Transparent substrate 10>
The transparent substrate 10 has optical transparency with respect to the first emitted light h1 generated in the first light emitting functional layer 13 and the second emitted light h2 generated in the second light emitting functional layer 17 in visible light. Further, the transparent substrate 10 has light transmittance with respect to the first processing light L1 and the second processing light L2 used for pattern processing of the first light emitting functional layer 13 and the second light emitting functional layer 17. The first processing light L1 and the second processing light L2 will be described in detail in the subsequent manufacturing method.

  Examples of the transparent substrate material constituting the transparent substrate 10 as described above include, but are not limited to, glass, quartz, and resin substrates. A particularly preferable transparent substrate 10 is a resin substrate capable of giving flexibility to an organic electroluminescent element formed using the same. The resin substrate may have a configuration in which a gas barrier layer is provided as necessary.

  In the present invention, conventionally known resin materials are used as the resin material constituting the resin substrate. For example, acrylic resins such as acrylic acid ester, methacrylic acid ester and polymethyl methacrylate (PMMA), polyethylene terephthalate (PET), poly Butylene terephthalate, polyethylene naphthalate (PEN), polycarbonate (PC), polyarylate, polyvinyl chloride (PVC), polyethylene (PE), polypropylene (PP), polystyrene (PS), nylon (Ny), aromatic polyamide, poly Examples include resin films such as ether ether ketone, polysulfone, polyether sulfonate, polyimide, polyetherimide, polyolefin, and epoxy resin, and cycloolefin-based and cellulose ester-based ones. It can be used. In addition, a heat-resistant transparent film (product name Sila-DEC, manufactured by Chisso Corporation) having silsesquioxane having an organic-inorganic hybrid structure as a basic skeleton, and a resin film formed by laminating two or more layers of the resin material, etc. Can be mentioned.

<Transparent electrode 11>
The transparent electrode 11 is provided as an anode or a cathode with respect to the first light emitting functional layer 13, and is used as an anode when the intermediate electrode 15 is a cathode, and is used as a cathode when the intermediate electrode 15 is an anode.

  In addition, the transparent electrode 11 has a light transmission property with respect to the first emitted light h <b> 1 generated in the first light emitting functional layer 13 and the second emitted light h <b> 2 generated in the second light emitting functional layer 17 in the visible light. Further, the transparent electrode 11 has light transmittance with respect to the first processed light L1 and the second processed light L2 used for processing the first light emitting functional layer 13 and the second light emitting functional layer 17.

  Such a transparent electrode 11 is comprised using the electroconductive material excellent in the light transmittance mentioned above from the electroconductive material suitable for each. Examples of the conductive material suitably used for the configuration of the transparent electrode 11 include transparent conductive materials such as oxide semiconductors such as ITO, ZnO, TiO2, and SnO2.

  In addition, the transparent electrode 11 may be configured as a metal thin film containing metal as a main component. The metal thin film referred to here is a thin film having a thickness in the range of 8 to 30 nm. If the metal contained in the transparent electrode 11 comprised as a metal thin film is a metal with high electroconductivity, it will not restrict | limit especially, For example, silver, copper, gold | metal | money, platinum group, titanium, chromium etc. are illustrated. The transparent electrode 11 may contain only one kind of these metals or two or more kinds. From the viewpoint of high conductivity, the transparent electrode 11 is preferably composed of silver as a main component and is composed of silver or an alloy containing silver as a main component.

  Examples of the alloy mainly composed of silver (Ag) constituting the transparent electrode 11 include silver magnesium (AgMg), silver copper (AgCu), silver palladium (AgPd), silver palladium copper (AgPdCu), and silver indium (AgIn). ) And the like.

  Moreover, when the transparent electrode 11 is comprised as a metal thin film, it is preferable that this transparent electrode 11 is provided through the base layer which abbreviate | omitted illustration here. The foundation layer is a layer provided on the transparent substrate 10 side of the transparent electrode 11. The material constituting the underlayer is not particularly limited as long as it can suppress aggregation of silver when forming the transparent electrode 11 made of silver or an alloy containing silver as a main component. As a nitrogen-containing compound containing a nitrogen atom, or a sulfur-containing compound.

  When the transparent electrode 11 is formed as a metal thin film, the transparent electrode 11 is a semi-reflective layer, and a resonator structure for the first emitted light h1 or the second emitted light h2 is formed between the transparent electrode 11 and the reflective electrode 19. May be.

  The transparent electrode 11 made of the material as described above has a sheet resistance of 30Ω / sq. Or less, preferably 10 Ω / sq. The following is more preferable. The transparent electrode 11 preferably has a light transmittance at a wavelength of 550 nm of 30% or more, and more preferably 50% or more.

  The transparent electrode 11 is in a state of being electrically connected to the intermediate electrode 15 via the power source 23.

<First light emitting functional layer 13>
The 1st light emission functional layer 13 is provided in the transparent electrode 11 side among the some light emission functional layers which have the light emitting layer comprised using the organic material. This 1st light emission functional layer 13 is a laminated body containing the light emitting layer comprised with the organic material at least, Comprising: The whole laminated structure is not limited, An example is shown to following (i)-(vi) It may be any one of the general laminated structures shown, and may further have layers as required.

(I) (anode) / hole injection transport layer / light emitting layer / electron injection transport layer / (cathode)
(Ii) (anode) / hole injection transport layer / light emitting layer / hole blocking layer / electron injection transport layer / (cathode)
(Iii) (anode) / hole injection transport layer / electron blocking layer / light emitting layer / hole blocking layer / electron injection transport layer / (cathode)
(Iv) (anode) / hole injection layer / hole transport layer / light emitting layer / electron transport layer / electron injection layer / (cathode)
(V) (anode) / hole injection layer / hole transport layer / light emitting layer / hole blocking layer / electron transport layer / electron injection layer / (cathode)
(Vi) (anode) / hole injection layer / hole transport layer / electron blocking layer / light emitting layer / hole blocking layer / electron transport layer / electron injection layer / (cathode)
Details of the constituent materials of these layers will be described in detail later.

  The first light emitting functional layer 13 is characterized in that a light emitting region 13a and a non-light emitting region 13b are patterned. The light emitting region 13a and the non-light emitting region 13b in the first light emitting functional layer 13 are partially irradiated with the first processing light L1 having a specific wavelength when at least one of the layers constituting the first light emitting functional layer 13 is irradiated. This is a region that has been patterned by being altered.

  The first light emitting functional layer 13 has optical characteristics different from those of the second light emitting functional layer 17. FIG. 3 is a light transmission spectrum of the light emitting functional layer, and is a graph of light transmittance (T) with respect to wavelength [λ]. As shown in FIG. 3, the first light emitting functional layer 13 and the second light emitting functional layer 17 configured using an organic material are in a wavelength region including visible light and light used for pattern processing of a general organic material. The transmittance increases as the long wave increases. Such a transmittance spectrum is characterized by a layer in which the wavelength at which the light transmittance [T] reaches the upper limit among the multiple layers constituting the light emitting functional layer is located on the longest wavelength side.

  In particular, in this embodiment, the wavelength at which the light transmittance [T] of the first light emitting functional layer 13 reaches the upper limit [Tmax] is defined as the first wavelength [λ1], and the light transmittance of the second light emitting functional layer 17 [ Assuming that the second wavelength [λ2] at which T] reaches the upper limit [Tmax], the first wavelength [λ1] <the second wavelength [λ2] is characteristic.

  The light transmission spectra of the first light-emitting functional layer 13 and the second light-emitting functional layer 17 are obtained by forming each layer structure on a transparent substrate and using a spectroscope (for example, U-3310: Hitachi High-Tech, Ocean Optics: HR2000 + / 4000).

  In addition, the first light emitting functional layer is obtained by measuring the transmittance of the laminated structures (A) to (C) below and comparing the values (B)-(C) with the values (A). 13 and the transmittance of the second light emitting functional layer 17 can be determined.

(A) the transmittance of the second light emitting functional layer 17 / intermediate electrode 15,
(B) The transmittance of the second light emitting functional layer 17 / intermediate electrode 15 / first light emitting functional layer 13 / transparent electrode 11 (C) The transmittance of the transparent electrode 11 is measured,

  In addition, the first wavelength [λ1] in the first light emitting functional layer 13 has a wavelength λ of the first processing light L1 suitable for patterning of the first light emitting functional layer 13 in a region shorter than the first wavelength [λ1]. A value including (L1). Further, the first wavelength [λ1] is a value including the wavelength λ (L2) of the second processing light L2 suitable for patterning of the second light emitting functional layer 17 in the region on the long wavelength side longer than the first wavelength [λ1]. .

  As a result, the first light emitting functional layer 13 uses the second processing light L2 when patterning the second light emitting functional layer 17 as the light on the long wavelength side longer than the first wavelength [λ1]. The processed light L2 is transmitted without being absorbed.

  Further, the first light emitting functional layer 13 has at least one layer that satisfactorily absorbs and alters the first processed light L1 on the short wavelength side of the first wavelength [λ1] or less. 13b is a pattern formed.

  In the first light emitting functional layer 13, for example, a hole transport layer is applied as the layer having the altered portion, and the hole transport layer is a layer that characterizes the light transmission spectrum of the first light emitting functional layer 13. It has become. Such a first light-emitting functional layer 13 does not have an absorption wavelength in a longer wavelength region than the first wavelength [λ1], that is, emits light having a shorter wavelength, for example, blue to The light-emitting layer is configured to emit green light (emission peak of 500 nm or less).

<Intermediate electrode 15>
The intermediate electrode 15 is provided as an anode or a cathode for the first light emitting functional layer 13, and is used as a cathode when the transparent electrode 11 is an anode, and is used as an anode when the transparent electrode 11 is a cathode. The intermediate electrode 15 is also used as an anode or a cathode for the second light emitting functional layer 17, and is used as a cathode when the reflective electrode 19 is an anode, and as an anode when the reflective electrode 19 is a cathode. It is done.

  Further, the intermediate electrode 15 has a light transmission property with respect to the second emitted light h2 generated in the second light emitting functional layer 17 in the visible light, and also with respect to the second processed light L2 used for processing the second light emitting functional layer 17. It has optical transparency. In consideration of the improvement of light extraction efficiency due to reflection by the reflection electrode 19 described later, the intermediate electrode 15 has light transmittance with respect to the first emission light h <b> 1 generated in the first emission function layer 13.

  Such an intermediate electrode 15 is configured using the above-described conductive material having an excellent light transmission property among the materials suitable for the transparent electrode 11 exemplified above, and has the same sheet resistance and light as the transparent electrode 11. It is preferable to have transmittance. When the intermediate electrode 15 is configured as a metal thin film, the intermediate electrode 15 is a semi-reflective layer, and a resonator structure for the first emitted light h1 or the second emitted light h2 is formed between the intermediate electrode 15 and the reflective electrode 19. It may be configured.

  The intermediate electrode 15 is in a state of being electrically connected to the transparent electrode 11 via the power source 23 and electrically connected to the reflective electrode 19 via the power source 27.

<Second light emitting functional layer 17>
The 2nd light emission functional layer 17 is laminated | stacked on the reflective electrode 19 side rather than the 1st light emission functional layer 13 among the several light emission functional layers which have the light emitting layer comprised using the organic material. The second light emitting functional layer 17 is a laminate including at least a light emitting layer made of an organic material like the first light emitting functional layer 13, and the overall laminated structure is not limited. It may be any one of general laminated structures as shown in examples i) to (vi), and may further have layers as necessary. Further, the second light emitting functional layer 17 may have a laminated structure different from that of the first light emitting functional layer 13, and the order of the above (i) to (vi) may be reversed.

  The second light emitting functional layer 17 is characterized in that the light emitting region 17a and the non-light emitting region 17b are patterned. The pattern of the light emitting region 17a may have a planar shape different from that of the light emitting region 13a of the first light emitting functional layer 13, or may be arranged so as to overlap.

  The light emitting region 17a and the non-light emitting region 17b in the second light emitting functional layer 17 are partially irradiated with the second processing light L2 having a specific wavelength when any one of the second light emitting functional layers 17 is irradiated. This is a region that has been patterned by being altered.

  As described above, the second light emitting functional layer 17 has optical characteristics different from those of the first light emitting functional layer 13, and as shown in FIG. 3, the first wavelength [λ1] <second. Wavelength [λ2]. The second wavelength [λ2] in the second light emitting functional layer 17 has a wavelength λ of the second processing light L2 suitable for patterning of the second light emitting functional layer 17 in a region shorter than the second wavelength [λ2]. It is a value including (L2).

  Further, the second light emitting functional layer 17 has at least one layer that satisfactorily absorbs and alters the second processed light L2 on the short wavelength side of the second wavelength [λ2] or less. 17b is a pattern formed.

  In the second light emitting functional layer 17, for example, a light emitting layer is applied as the layer having the altered portion, and this light emitting layer is a layer characterizing the light transmission spectrum of the second light emitting functional layer 17. In this case, the light emitting layer of the second light emitting functional layer 17 has an absorption wavelength between the first wavelength [λ1] and the second wavelength [λ2]. For this reason, when the light emitting layer of the first light emitting functional layer 13 is a light emitting layer emitting blue to green light, the light emitting layer of the second light emitting functional layer 17 is capable of obtaining emitted light having a longer wavelength than this, For example, the light emitting layer is configured to emit green to red light (emission peak: 540 nm to 640 nm).

  In addition, as described above, the light emitting layer that is altered by irradiation with the second processed light L2 having a wavelength equal to or shorter than the second wavelength [λ2] preferably has a higher dopant content than the light emitting layer, for example, 15 vol. It is assumed that the dopant is contained at a content of at least%. Thereby, it becomes the structure which changes easily by light irradiation.

<Reflective electrode 19>
The reflective electrode 19 is provided as an anode or a cathode for the second light emitting functional layer 17, and is used as an anode when the intermediate electrode 15 is a cathode, and as a cathode when the intermediate electrode 15 is an anode.

  In addition, the reflective electrode 19 has good reflection characteristics particularly for the first emitted light h1 generated in the first light emitting functional layer 13 and the second emitted light h2 generated in the second light emitting functional layer 17 in the visible light. It is preferable to have. Such a reflective electrode 19 is composed of a conductive material suitable as a cathode or an anode by using a metal material having excellent reflection characteristics, and is composed of, for example, gold, platinum, silver, copper, aluminum, or the like. .

  The reflective electrode 19 is in a state of being electrically connected to the intermediate electrode 15 via the power source 27.

<Power source 23 and power source 27>
One of the power sources 23 and 27 is connected to the transparent electrode 11 and the intermediate electrode 15. The power source 23 has a positive electrode connected to the anode side of the transparent electrode 11 and the intermediate electrode 15 with respect to the first light emitting functional layer 13 and a negative electrode connected to the cathode side. The other power source 27 is connected to the intermediate electrode 15 and the reflective electrode 19. The power source 27 has a positive electrode connected to the anode side of the intermediate light emitting layer 15 and the reflective electrode 19 with respect to the second light emitting functional layer 17 and a negative electrode connected to the cathode side.

  In the illustrated example, the positive electrode is connected to the first light emitting functional layer 13 with the transparent electrode 11 as an anode, and the negative electrode of the power source 23 is connected with the intermediate electrode 15 as a cathode. The positive electrode of the power source 27 is connected to the second light emitting functional layer 17 with the intermediate electrode 15 as an anode, and the negative electrode of the power source 27 is connected with the reflective electrode 19 as a cathode. When the laminated structure of the first light emitting functional layer 13 is reversed, the connection state of the power source 23 may be reversed. When the laminated structure of the second light emitting functional layer 17 is reversed, the connection state of the power source 27 is changed. Just reverse.

  The power sources 23 and 27 include a control unit (not shown), and the control unit controls the voltage and current applied to the transparent electrode 11, the intermediate electrode 15, and the reflective electrode 19. ing.

  This control unit can be configured by a computer, for example. Thereby, the light emission ratio and light emission quantity of the 1st light emission functional layer 13 and the 2nd light emission functional layer 17 can be controlled, and light control property and toning property can be improved. It is also possible to individually control the light emission of the first light emitting functional layer 13 and the second light emitting functional layer 17.

  In addition, the control unit performs control to make the total of currents supplied to the first light emitting functional layer 13 and the second light emitting functional layer 17 constant, or performs control to make the current of the light emitting functional layer having high visibility constant. Can be. Thereby, light control and color adjustment can be performed effectively.

  The organic electroluminescent element 1 may have at least two power supplies 23 and 27, but may have a larger number of power supplies. However, in order not to complicate the apparatus, it is preferable that the number of power sources is smaller than the number of electrodes.

<Other components>
In addition to the above, the organic electroluminescent element 1 may be provided with a protective member between the transparent substrate 10 and the transparent electrode 11 to the reflective electrode 19 and the sealing material. This protective member is for mechanically protecting the organic electroluminescent element 1, and in particular, when the sealing material is a sealing film, mechanical protection for the organic electroluminescent element 1 is not sufficient. Therefore, it is preferable to provide such a protective member.

  A glass plate, a polymer plate, a thinner polymer film, a metal plate, a thinner metal film, a polymer material film or a metal material film is applied to the protective member as described above. Among these, it is particularly preferable to use a polymer film because it is light and thin.

  Further, the organic electroluminescent element 1 requires a light extraction layer for efficiently extracting the first emitted light h1 and the second emitted light h2 generated in the first light emitting functional layer 13 and the second light emitting functional layer 17. Accordingly, it may be provided at a necessary portion.

  Further, in the organic electroluminescent element 1, an auxiliary electrode having good conductivity may be connected to the transparent electrode 11 and the intermediate electrode 15 at a position that does not overlap the light emitting regions 13a and 17a. The material for forming such an auxiliary electrode is preferably a metal having low resistance such as gold, platinum, silver, copper, or aluminum.

<Driving of organic electroluminescent element 1>
In the organic electroluminescent element 1 configured as described above, the first emitted light h <b> 1 is generated in the light emitting region 13 a of the first light emitting functional layer 13 by applying a voltage between the transparent electrode 11 and the intermediate electrode 15 in a predetermined state. Occur. The first emitted light h1 passes through the transparent electrode 11 and the transparent substrate 10, and light emission in the shape of the light emitting region 13a is observed on the light extraction surface 10a of the transparent substrate 10. In addition, by applying a voltage between the intermediate electrode 15 and the reflective electrode 19 in a predetermined state, the second light emission light h <b> 2 is generated in the light emitting region 17 a of the second light emitting functional layer 17. The second emitted light h2 passes through the transparent electrode 11 and the transparent substrate 10, and light emission in the shape of the light emitting region 17a is observed on the light extraction surface 10a of the transparent substrate 10.

  If a voltage is applied to the transparent electrode 11, the intermediate electrode 15, and the reflective electrode 19 in a predetermined state, the light emitting region 13 a of the first light emitting functional layer 13 and the light emitting region 17 a of the second light emitting functional layer 17 are overlapped. The combined light emission is observed.

  The driving of the organic electroluminescent element 1 may be performed by applying an alternating voltage, and the applied alternating current waveform may be arbitrary.

<Other modified configurations>
The organic electroluminescent element 1 described above has a configuration in which two light emitting functional layers, the first light emitting functional layer 13 and the second light emitting functional layer 17, are laminated. However, the organic electroluminescent element of the present invention may have a structure in which a plurality of light emitting functional layers are further laminated. Even in this case, the relationship between the optical characteristics of the light emitting functional layer on the transparent electrode 11 side and the light emitting functional layer on the reflective electrode 19 side is more than the first light emitting functional layer 13 and the second light emitting functional layer described above. 17 is sufficient.

  Moreover, the organic electroluminescent element 1 demonstrated above is a layer which characterizes the light transmission characteristic of the 1st light emission functional layer 13, Comprising: The hole transport layer was illustrated as a layer which changes the part. In addition, the light emitting layer is exemplified as a layer that characterizes the light transmission characteristics of the second light emitting functional layer 17 and partially changes its quality. However, such a layer is not limited to being a hole transport layer or a light emitting layer, and may be another layer or a plurality of layers. In this case, it can also be configured to obtain emitted light in the same wavelength region from the light emitting region of each light emitting functional layer.

<Material of each layer constituting first light emitting functional layer 13 and second light emitting functional layer 17>
Details of the constituent materials of the respective layers constituting the first light emitting functional layer 13 and the second light emitting functional layer 17 are as follows. However, for the first light emitting functional layer 13 and the second light emitting functional layer 17, it is assumed that a material suitable for the configuration of the organic electroluminescent element 1 is selected from the materials shown below.

[Light emitting layer]
The light emitting layer used in the present invention preferably contains a phosphorescent light emitting compound as a light emitting material. Note that a fluorescent material may be used as the light emitting material, or a phosphorescent light emitting compound and a fluorescent material may be used in combination.

  The light-emitting layer is a layer that emits light by recombination of electrons injected from the cathode side and holes injected from the anode side, and the light-emitting portion is adjacent to the light-emitting layer even in the layer of the light-emitting layer. It may be an interface with the layer to be used.

  Such a light emitting layer is not particularly limited in its configuration as long as the contained light emitting material satisfies the light emission requirements. There may be a plurality of layers having the same emission spectrum and emission maximum wavelength. In this case, it is preferable to have a non-light emitting intermediate layer (not shown) between the light emitting layers.

  The total thickness of the light emitting layers is preferably in the range of 1 to 100 nm, and more preferably in the range of 1 to 40 nm because a lower driving voltage can be obtained.

  Note that the total film thickness of the light emitting layer is a film thickness including the intermediate layer when a non-light emitting intermediate layer exists between the light emitting layers. However, in the case of a so-called tandem element in which a plurality of light emitting layer units are stacked via an intermediate connector portion, the light emitting layer here refers to a light emitting layer portion in each light emitting unit.

  In the case of a light emitting layer having a configuration in which a plurality of layers are laminated, the thickness of each light emitting layer is preferably adjusted within a range of 1 to 50 nm, and more preferably adjusted within a range of 1 to 20 nm. . When the plurality of stacked light emitting layers correspond to blue, green, and red light emitting colors, there is no particular limitation on the relationship between the film thicknesses of the blue, green, and red light emitting layers.

  The light emitting layer as described above is formed by forming a known light emitting material or host compound by a known thin film forming method such as a vacuum deposition method, a spin coating method, a casting method, an LB method, or an ink jet method. Can do.

  The light emitting layer may be a mixture of a plurality of light emitting materials.

  As a structure of the light-emitting layer, it is preferable that a light-emitting material contains a host compound (also referred to as a light-emitting host) and a light-emitting material (also referred to as a light-emitting dopant).

  Examples of the light-emitting dopant applicable to the present invention include International Publication No. WO 2005/076380, International Publication No. 2010/032663, International Publication No. 2008/140115, International Publication No. 2007/052431, International Publication No. 2011. No. 134013, International Publication No. 2011/157339, International Publication No. 2010/086089, International Publication No. 2009/113646, International Publication No. 2012/020327, International Publication No. 2011/051404, International Publication No. 2011/004639. No., WO 2011/073149, JP 2012-069737, JP 2009-114086, JP 2003-81988, JP 2002-302671, JP 2002-363552, etc. Compounds described in It can be mentioned.

  Examples of the host compound include JP-A Nos. 2001-257076, 2002-308855, 2001-313179, 2002-319491, 2001-357777, and 2002-334786. Gazette, 2002-8860, 2002-334787, 2002-15871, 2002-334788, 2002-43056, 2002-334789, 2002-75645 2002-338579, 2002-105445, 2002-343568, 2002-141173, 2002-352957, 2002-203683, 2002-363227 2002-231453, 2003-3165, 2002-234888, 2003-27048, 2002-255934, 2002-260861, 2002-280183, 2002-299060, 2002-302516, 2002-305083, 2002-305084, 2002-308837, US 2003/0175553, US 2006 No. 0280965, U.S. Patent Publication No. 2005/0112407, U.S. Patent Publication No. 2009/0017330, U.S. Patent Publication No. 2009/0030202, U.S. Patent Publication No. 2005/238919, International Publication No. 2001/039234, International Publication No. 2009/021126, International Publication No. 2008/056746, International Publication No. 2004/093207, International Publication No. 2005/089025, International Publication No. 2007/063796, International Publication No. 2007/063754, International Publication No. 2004/107822, International Publication No. 2005/030900, International Publication No. 2006/114966, International Publication No. 2009/086028, International Publication No. 2009/003898, International Publication No. 2012 No. 023947, JP 2008-074939 A, JP 2007-254297 A, EP 2034538, and the like.

[Hole injection layer / electron injection layer]
An injection layer is a layer provided between an electrode and a light-emitting layer in order to lower drive voltage or improve light emission luminance. “An organic EL element and its forefront of industrialization (November 30, 1998, NTS) The details are described in Chapter 2 “Electrode Material” (pages 123 to 166) of the second volume of “Shin-ken”, and there are a hole injection layer and an electron injection layer.

  An injection | pouring layer is a structure layer which can be provided as needed. If it is a hole injection layer, it may exist between the anode and the light emitting layer or the hole transport layer, and if it is an electron injection layer, it may exist between the cathode and the light emitting layer or the electron transport layer.

  The details of the hole injection layer 15e are described in JP-A-9-45479, JP-A-9-260062, JP-A-8-288069, and the like. Specific examples thereof include phthalocyanine represented by copper phthalocyanine. Examples thereof include a layer, an oxide layer typified by vanadium oxide, an amorphous carbon layer, and a polymer layer using a conductive polymer such as polyaniline (emeraldine) or polythiophene. Moreover, it is also preferable to use the material described in Japanese translations of PCT publication No. 2003-519432 gazette.

  The details of the electron injection layer are also described in JP-A-6-325871, JP-A-9-17574, JP-A-10-74586, and the like, and specifically, metals represented by strontium, aluminum and the like. Examples thereof include an alkali metal halide layer typified by potassium fluoride, an alkaline earth metal compound layer typified by magnesium fluoride, and an oxide layer typified by molybdenum oxide. In the present invention, the electron injection layer is preferably a very thin film, and the film thickness is preferably in the range of 1 nm to 10 μm although it depends on the material.

[Hole transport layer]
The hole transport layer is made of a hole transport material having a function of transporting holes, and in a broad sense, a hole injection layer and an electron blocking layer are also included in the hole transport layer. The hole transport layer can be provided as a single layer or a plurality of layers.

  The hole transport material has any of the characteristics of hole injection or transport and electron barrier properties, and may be either organic or inorganic. For example, triazole derivatives, oxadiazole derivatives, imidazole derivatives, polyarylalkane derivatives, pyrazoline derivatives and pyrazolone derivatives, phenylenediamine derivatives, arylamine derivatives, amino-substituted chalcone derivatives, oxazole derivatives, styrylanthracene derivatives, fluorenone derivatives, hydrazone derivatives, Examples thereof include stilbene derivatives, silazane derivatives, aniline copolymers, and conductive polymer oligomers, particularly thiophene oligomers.

  As the hole transport material, those described above can be used, and it is further preferable to use a porphyrin compound, an aromatic tertiary amine compound and a styrylamine compound, particularly an aromatic tertiary amine compound.

  Representative examples of aromatic tertiary amine compounds and styrylamine compounds include, for example, N, N, N ′, N′-tetraphenyl-4,4′-diaminophenyl; N, N′-diphenyl-N, N '-Bis (3-methylphenyl)-[1,1'-biphenyl] -4,4'-diamine (abbreviation: TPD); 2,2-bis (4-di-p-tolylaminophenyl) propane; 1 , 1-bis (4-di-p-tolylaminophenyl) cyclohexane; N, N, N ′, N′-tetra-p-tolyl-4,4′-diaminobiphenyl; 1,1-bis (4-di -P-tolylaminophenyl) -4-phenylcyclohexane; bis (4-dimethylamino-2-methylphenyl) phenylmethane; bis (4-di-p-tolylaminophenyl) phenylmethane; N, N'-dipheni -N, N'-di (4-methoxyphenyl) -4,4'-diaminobiphenyl; N, N, N ', N'-tetraphenyl-4,4'-diaminodiphenyl ether; 4,4'-bis ( N, N, N-tri (p-tolyl) amine; 4- (di-p-tolylamino) -4 ′-[4- (di-p-tolylamino) styryl] stilbene; N, N-diphenylamino- (2-diphenylvinyl) benzene; 3-methoxy-4′-N, N-diphenylaminostilbenzene; N-phenylcarbazole, and further in US Pat. No. 5,061,569 Those having two fused aromatic rings described in the molecule, for example, 4,4′-bis [N- (1-naphthyl) -N-phenylamino] biphenyl (abbreviation: NPD) 4,4 ′, 4 ″ -tris [N- (3-methylphenyl) -N-phenylamino, wherein three triphenylamine units described in JP-A-4-308688 are linked in a starburst type ] Triphenylamine (abbreviation: MTDATA) and the like.

  Furthermore, a polymer material in which these materials are introduced into a polymer chain or these materials are used as a polymer main chain can also be used. In addition, inorganic compounds such as p-type-Si and p-type-SiC can also be used as the hole injection material and the hole transport material.

  JP-A-11-251067, J. Org. Huang et. al. , Applied Physics Letters, 80 (2002), p. A so-called p-type hole transport material as described in 139 can also be used. In the present invention, it is preferable to use these materials because a light-emitting element with higher efficiency can be obtained.

  The hole transport layer is formed by thinning the hole transport material by a known method such as a vacuum deposition method, a spin coating method, a casting method, a printing method including an ink jet method, or an LB method. Can do. Although there is no restriction | limiting in particular about the film thickness of a positive hole transport layer, Usually, 5 nm-about 5 micrometers, Preferably it is 5-200 nm. The hole transport layer may have a single layer structure composed of one or more of the above materials.

  In addition, impurities can be doped into the material of the hole transport layer to increase transportability. Examples thereof include JP-A-4-297076, JP-A-2000-196140, 2001-102175, J.A. Appl. Phys. 95, 5773 (2004), and the like.

[Electron transport layer]
The electron transport layer is made of a material having a function of transporting electrons, and in a broad sense, an electron injection layer and a hole blocking layer (not shown) are also included in the electron transport layer. The electron transport layer can be provided as a single layer structure or a stacked structure of a plurality of layers.

  In the electron transport layer having a single layer structure and the electron transport layer having a multilayer structure, an electron transport material (also serving as a hole blocking material) constituting a layer portion adjacent to the light emitting layer emits electrons injected from the cathode. What is necessary is just to have the function to transmit to a layer. As such a material, any one of conventionally known compounds can be selected and used. Examples include nitro-substituted fluorene derivatives, diphenylquinone derivatives, thiopyran dioxide derivatives, carbodiimides, fluorenylidenemethane derivatives, anthraquinodimethane, anthrone derivatives, and oxadiazole derivatives. Furthermore, in the above oxadiazole derivative, a thiadiazole derivative in which the oxygen atom of the oxadiazole ring is substituted with a sulfur atom, and a quinoxaline derivative having a quinoxaline ring known as an electron-withdrawing group can also be used as a material for the electron transport layer. it can. Furthermore, a polymer material in which these materials are introduced into a polymer chain or these materials are used as a polymer main chain can also be used.

  In addition, metal complexes of 8-quinolinol derivatives such as tris (8-quinolinol) aluminum (abbreviation: Alq3), tris (5,7-dichloro-8-quinolinol) aluminum, tris (5,7-dibromo-8-quinolinol) ) Aluminum, tris (2-methyl-8-quinolinol) aluminum, tris (5-methyl-8-quinolinol) aluminum, bis (8-quinolinol) zinc (abbreviation: Znq), and the central metals of these metal complexes Metal complexes replaced with In, Mg, Cu, Ca, Sn, Ga, or Pb can also be used as the material for the electron transport layer.

  In addition, metal-free or metal phthalocyanine, or those having terminal ends substituted with alkyl groups or sulfonic acid groups can be preferably used as the material for the electron transport layer. Further, distyrylpyrazine derivatives exemplified as the material of the light emitting layer can also be used as the material of the electron transport layer, and n-type-Si, n-type-SiC, etc. as well as the hole injection layer and the hole transport layer. These inorganic semiconductors can also be used as a material for the electron transport layer.

  The electron transport layer can be formed by thinning the above material by a known method such as a vacuum deposition method, a spin coating method, a casting method, a printing method including an inkjet method, or an LB method. Although there is no restriction | limiting in particular about the film thickness of an electron carrying layer, Usually, 5 nm-about 5 micrometers, Preferably it is 5-200 nm. The electron transport layer may have a single layer structure composed of one or more of the above materials.

  In addition, the electron transport layer can be doped with impurities to increase transportability. Examples thereof include JP-A-4-297076, JP-A-10-270172, JP-A-2000-196140, 2001-102175, J.A. Appl. Phys. 95, 5773 (2004), and the like. Furthermore, it is preferable that potassium, a potassium compound, etc. are contained in an electron carrying layer. As the potassium compound, for example, potassium fluoride can be used. Thus, when the n property of the electron transport layer is increased, an element with lower power consumption can be manufactured.

  Further, as the material for the electron transport layer (electron transport compound), the same material as that for the above-described underlayer may be used. The same applies to the electron transport layer that also serves as the electron injection layer, and the same material as that for the above-described underlayer may be used.

[Electron blocking layer / hole blocking layer]
The electron blocking layer / hole blocking layer is disclosed in, for example, JP-A Nos. 11-204258 and 11-204359, and “Organic EL device and its forefront of industrialization (November 30, 1998, NTS Corporation). Issue) ”on page 237, etc., there is a hole blocking layer.

  The hole blocking layer has a function of an electron transport layer in a broad sense. The hole blocking layer is made of a hole blocking material that has a function of transporting electrons but has a very small ability to transport holes, and recombines electrons and holes by blocking holes while transporting electrons. Probability can be improved. Moreover, the structure of the said electron carrying layer can be used as a hole-blocking layer as needed. The hole blocking layer is preferably provided adjacent to the light emitting layer.

  On the other hand, the electron blocking layer has a function of a hole transport layer in a broad sense. The electron blocking layer is made of a material that has a function of transporting holes but has a very small ability to transport electrons, and improves the probability of recombination of electrons and holes by blocking electrons while transporting holes. be able to. Moreover, the structure of the said positive hole transport layer can be used as an electron blocking layer as needed. In the present invention, the thickness of the hole blocking layer is preferably in the range of 3 to 100 nm, more preferably in the range of 5 to 30 nm.

<Effect of the organic electroluminescent element 1>
The organic electroluminescent element 1 having the above-described configuration has a configuration in which the intermediate electrode 15 is shared by the first light emitting functional layer 13 and the second light emitting functional layer 17 in which the light emitting regions 13a and 17a are individually patterned. . For this reason, the number of electrodes can be reduced as compared with a conventional configuration in which a plurality of light emitting units each having a light emitting functional layer sandwiched between two electrodes are stacked. As a result, the structure of the organic electroluminescent element 1 capable of displaying images of different shapes from the same region is simplified, and thus the organic electroluminescent element 1 can be reduced in thickness and cost. .

≪Method for manufacturing organic electroluminescent element≫
FIG. 4 is a cross-sectional process diagram illustrating the method for manufacturing the organic electroluminescent element of the embodiment. The manufacturing method shown in this figure is the manufacturing method of the organic electroluminescent element 1 described with reference to FIGS. Hereinafter, a method for manufacturing the organic electroluminescent element will be described with reference to FIG. In addition, the same code | symbol is attached | subjected about the component same as the component of the organic electroluminescent element 1 demonstrated using FIGS. 1-3, and the detailed description which overlaps is abbreviate | omitted.

<Lamination process>
First, as shown in FIG. 4A, on a transparent substrate 10, a transparent electrode 11, a first light emitting functional layer 13 ′ whose entire area is a light emitting area 13a, an intermediate electrode 15, and a second light emitting function whose entire area is a light emitting area 17a. The layer 17 ′ and the reflective electrode 19 are formed in this order. Further, before the transparent electrode 11 and the intermediate electrode 15 are formed, a base layer is formed as necessary.

  In film formation of these members, film formation methods suitable for the members may be applied. Examples of film formation methods include vacuum deposition, sputtering, reactive sputtering, molecular beam epitaxy, cluster ion beam, ion plating, plasma polymerization, atmospheric pressure plasma polymerization, plasma CVD, and laser. Examples thereof include a CVD method, a thermal CVD method, and a coating method.

  When forming each member, each member can be patterned into a predetermined shape by performing film formation using a mask as necessary. Each member may be patterned into a predetermined shape after each layer is formed. In addition, before and after the film formation of the transparent electrode 11 and the intermediate electrode 15, an auxiliary electrode pattern may be formed as necessary.

  Moreover, it is preferable to implement the above lamination process in the procedure which forms into a film from the transparent electrode 11 to the reflective electrode 19 consistently by one vacuum drawing.

<Sealing process>
Next, although not shown here, sealing from the reflective electrode 19 side is performed. Here, in a state where the terminal portions of the transparent electrode 11, the intermediate electrode 15, and the reflective electrode 19 are exposed, a sealing material is provided so as to cover the laminated body of the transparent electrodes 11 to 19 with the transparent substrate 10. Provided, and a protective member through a sealing material is attached if necessary.

<The patterning process of the 1st light emission functional layer 13>
After that, as shown in FIG. 4B, at least one layer constituting the first light emitting functional layer 13 ′ is partially altered by irradiation with the first processing light L1 from the transparent substrate 10 side, and this altered region is formed. A patterning process for forming the non-light emitting region 13b is performed.

  As shown in FIG. 3, the first processed light L1 used here has a shorter wavelength than the first wavelength [λ1] at which the light transmittance [T] of the first light emitting functional layer 13 ′ reaches the upper limit [Tmax]. The light having the wavelength λ (L1) on the side. The first processing light L1 is absorbed in any of the layers constituting the first light emitting functional layer 13 'and changes the quality of this layer.

  Such first processed light L1 is preferably of a lower wavelength so that the light emission layer in the first light emitting functional layer 13 'can be efficiently absorbed. For example, in the first light emitting functional layer 13 ′, when changing the light emitting layer of blue to green light emission (emission peak 500 nm or less), ultraviolet to blue light having a wavelength of about 300 nm to 500 nm is used as the first processed light L1. . The first processing light L1 may further contain light on the short wavelength side.

  Further, here, a light emitting region 13a is set in the first light emitting functional layer 13 ', and the first processing light L1 is selectively irradiated to a region obtained by inverting the light emitting region 13a. At this time, as shown in the drawing, the first processing light L1 is collectively irradiated through the light shielding mask 31 covering the light emitting region 13a, or the spot-shaped first processing light L1 is drawn and irradiated so as to fill the irradiation region. .

  As the irradiation condition of the first processing light L1, it is assumed that the irradiation portion of the first processing light L1 in the light emitting layer is sufficiently irradiated so as to sufficiently change into the non-light emitting region 13b. As a specific example, the irradiation is performed so that the luminance of the non-light emitting region 13b and the luminance of the light emitting region 13a are at least 1:10 or more, preferably 1:50 or more. Further, the irradiation of the first processing light L1 is performed in a range where the transparent substrate 10 is not discolored by the irradiation of the first processing light L1.

  As described above, the first light emitting functional layer 13 constituted by the non-light emitting region 13b in which at least one layer constituting the first light emitting functional layer 13 'is partially altered and the other light emitting regions 13a is formed.

<Patterning step of second light emitting functional layer 17>
Next, as shown in FIG. 4C, at least one layer constituting the second light emitting functional layer 17 ′ is partially altered by irradiation with the second processing light L2 from the transparent substrate 10 side, and this altered region is converted into the altered region. A patterning process for forming the non-light emitting region 17b is performed.

  As shown in FIG. 3, the second processed light L2 used here has a second wavelength of not less than the first wavelength [λ1] at which the light transmittance [T] of the first light emitting functional layer 13 reaches the upper limit [Tmax]. Light having a wavelength λ (L2) shorter than the second wavelength [λ2] at which the light transmittance [T] of the light emitting functional layer 17 ′ reaches the upper limit [Tmax]. The second processed light L2 is absorbed in any of the layers that constitute the second light emitting functional layer 17 'to alter this layer.

  Such a second processed light L2 is preferably of a lower wavelength so that the light emission layer in the second light emitting functional layer 17 'can be efficiently absorbed. For example, when the light emitting layer of green to red light emission (light emission peak 540 nm to 640 nm) is altered in the second light emitting functional layer 17 ′, green light to red light having a wavelength of about 500 nm to 650 nm is used as the second processed light L2. Used.

  Further, here, a light emitting region 17a is set in the second light emitting functional layer 17 ', and the second processing light L2 is selectively irradiated to a region obtained by inverting the light emitting region 17a. At this time, as shown in the drawing, the second processing light L2 is collectively irradiated through the light shielding mask 35 covering the light emitting region 17a, or the spot-shaped second processing light L2 is drawn and irradiated so as to fill the irradiation region. . In the case of performing irradiation using the light shielding mask 35, the light shielding mask 35 includes a band pass filter 35a for cutting light having a shorter wavelength than the second processing light L2, and a light shielding pattern 35b laminated thereon. It is configured.

  The irradiation conditions of the second processing light L2 are the same as the patterning process of the first light emitting functional layer 13.

  In this way, the second light emitting functional layer 17 constituted by the non-light emitting region 17b in which at least one layer constituting the second light emitting functional layer 17 'is partially altered and the other light emitting regions 17a is formed.

  Note that the patterning step of the second light emitting functional layer 17 may be performed before the patterning step of the first light emitting functional layer 13.

<Light source used for patterning process>
As the light sources of the first processing light L1 and the second processing light L2 used in the patterning process described above, a high pressure mercury lamp, a low pressure mercury lamp, a hydrogen (deuterium) lamp, a rare gas (xenon, argon, helium, neon) Discharge lamp, argon laser, nitrogen laser, excimer laser (XeCl, XeF, KrF, KrCl, etc.), hydrogen laser, halogen laser, various visible (LD), infrared laser harmonics (THG (Third HarmonicGeneration) of YAG laser ) Light etc.).

Examples of the gas laser light source include a CO ₂ laser (10.6 μm, 9.4 μm) and an excimer laser (XeCl 308 nm, KrF 248 nm, ArF 193 nm). Furthermore, YAG laser (1064nm, SHG532nm, THG355nm, FHG266nm), YVO4 laser (1064nm, SHG532nm, THG355nm, FHG266nm), YLF laser (1064nm, SHG532nm, THG355nm, FHG266nm), fiber laser (1070nm, SHG532nm) as solid laser light sources Illustrated.

  In each patterning step, a light source that generates laser light having an appropriate wavelength is selected and used as the first processing light L1 and the second processing light L2 from these light sources.

<Effect of manufacturing method of organic electroluminescence device>
In the manufacturing method described above, the first light-emitting functional layer 13 and the second light-emitting functional layer 17 having different optical characteristics are laminated in a predetermined order via the intermediate electrode 15 having optical transparency. By irradiating the first processing light L1 and the second processing light L2 from one direction, the first light emitting functional layer 13 and the second light emitting functional layer 17 are individually patterned to form the light emitting regions 13a and 17a. This is a procedure that has been made possible.

  Therefore, in the manufacture of an organic electroluminescence device that can display images of different shapes from the same region, all the layers from the transparent electrode 11 to the reflective electrode 19 are formed on the transparent substrate 10 in a continuous process. Therefore, the manufacturing process can be simplified. Moreover, since the irradiation of the 1st process light L1 and the 2nd process light L2 is only from the transparent substrate 10 side, the simplification of a manufacturing process is achieved. This makes it possible to reduce the manufacturing cost.

≪Lighting device≫
The organic electroluminescent element 1 of the embodiment obtained as described above can be used as a planar illumination device.

  Further, the lighting device can increase the area of the light emitting surface by using a plurality of organic electroluminescent elements 1. In this case, the light emitting surface is enlarged by arranging (that is, tiling) the plurality of organic electroluminescent elements 1 on the support substrate. The support substrate may also serve as a sealing material. In a state where the laminate of the transparent electrode 11 to the reflective electrode 19 is sandwiched between the support substrate and the transparent substrate 10 of the organic electroluminescent element 1, The organic electroluminescent element 1 is tiled. An adhesive may be filled between the support substrate and the transparent substrate 10 to seal the transparent electrode 11 to the reflective electrode 19 of the organic electroluminescent element 1. Note that the terminals of the transparent electrode 11, the intermediate electrode 15, and the reflective electrode 19 are exposed around the support substrate.

  In the illuminating device having such a configuration, a large-area light emitting region obtained by connecting the light emitting regions 13a and 17a formed in the plurality of organic electroluminescent elements 1 can be displayed in a pattern. In such a configuration, a non-light emitting region is generated at the joint of each organic electroluminescent element 1. For this reason, a light extraction member for increasing the amount of light extracted from the non-light-emitting region is provided in the non-light-emitting region of the light extraction surface, particularly at a portion that becomes a joint between the light-emitting regions 13a and 17a between the organic electroluminescent elements 1. It may be provided. As the light extraction member, a light collecting sheet or a light diffusion sheet can be used.

  Hereinafter, the present invention will be described in detail by way of an example with reference to FIG. 4, but the present invention is not limited thereto. In addition, although the display of "%" is used in an Example, unless otherwise indicated, "mass%" is represented.

<< Production of organic electroluminescence element >>
An organic electroluminescent element having an element area of 5 cm × 5 cm was produced as follows.

(1) Formation of Transparent Electrode 11 First, a glass substrate having a thickness of 0.7 mm was prepared as the transparent substrate 10. The transparent substrate 10 was subjected to ultrasonic cleaning with isopropyl alcohol, dried with dry nitrogen gas, and UV ozone cleaning was performed for 5 minutes. Then, Ag (silver) was mask-deposited with a thickness of 20 nm on the transparent substrate 10 to form a transparent electrode 11 serving as an anode.

(2) Formation of 1st light emission functional layer 13 'Next, the transparent substrate 10 in which the transparent electrode 11 was formed was fixed to the substrate holder of a commercially available vacuum evaporation system. Then, the materials for the respective layers constituting the first light emitting functional layer 13 ′ were filled in the respective crucibles for vapor deposition in the vacuum vapor deposition apparatus with the optimum amounts for device fabrication. As each evaporation crucible, an evaporation crucible made of a resistance heating material made of molybdenum or tungsten was used.

(2.1) Formation of hole injection layer After depressurizing to a vacuum degree of 1 × 10 −4 Pa, an evaporation crucible containing the following compound (HAT-CN: hexaazatriphenylenehexacarbonitrile) was energized and heated, Vapor deposition was performed on the transparent electrode at a deposition rate of 0.1 nm / second to form a hole injection layer having a layer thickness of 5 nm.

(2.2) Formation of Hole Transport Layer Next, the following compound 1-A (glass transition point (Tg) = 140 ° C.) was deposited to a layer thickness of 65 nm to form a hole transport layer.

(2.3) Formation of Electron Blocking Layer Next, the following compound 1-B was deposited to a layer thickness of 20 nm to form an electron blocking layer.

  Compound 1-B is a material having a lower LUMO (Lowest Unoccupied Molecular Orbital) and higher minimum excited triplet energy (T1) than those of Compound 2-A and Compound 2-B constituting the light emitting layer described later. is there. That is, in the LUMO energy level, LUMO (1-B)> LUMO (host compound) and LUMO (1-B)> LUMO (light emitting dopant) are satisfied. Moreover, in T1, it becomes the relationship of T1 (1-B)> T1 (host compound) and T1 (1-B)> T1 (light emitting dopant). By using the compound 1-B satisfying such a relationship in a layer in contact with the light emitting layer, an electron and triplet energy blocking layer was formed in the hole transport layer.

(2.4) Formation of Light-Emitting Layer Next, the following compound 2-A (Tg = 189 ° C.) is deposited as a host compound so that 98 vol% and the following compound 2-B as a blue fluorescent light-emitting dopant is 2 vol%. A fluorescent light emitting layer having a blue layer thickness of 15 nm was formed.

(2.5) Formation of Electron Transport Layer Next, the following compound 3 was deposited on the light emitting layer so that 86 vol% and LiF were 14 vol%, thereby forming a layer having a thickness of 20 nm. Furthermore, it vapor-deposited so that the compound 3 might be 98 vol% and Li might be 2 vol%, and the layer with a layer thickness of 10 nm was formed. As a result, an electron transport layer that also serves as an electron injection layer composed of two layers of the compound 3 and LiF and the compound 3 and Li is formed, and the first light emitting functional layer having a stacked structure from the hole injection layer to the electron transport layer 13 'was formed.

(3) Formation of Intermediate Electrode 15 Next, Ag was formed into a film with a thickness of 2 nm on the first light emitting functional layer 13 ′ to form the intermediate electrode 15.

(4) Formation of Second Light-Emitting Functional Layer 17 ′ Except for the light-emitting layer, the second light-emitting functional layer 17 is set in the same manner using the same material as that of the first light-emitting functional layer 13 ′, and the film thickness is set for each. Formed.

(4.1) Formation of hole injection layer HAT-CN was deposited to a layer thickness of 10 nm to form a hole injection layer.

(4.2) Formation of Hole Transport Layer Next, Compound 1-A was vapor deposited to a layer thickness of 80 nm to form a hole transport layer.

(4.3) Formation of electron blocking layer Next, the compound 1-B was vapor-deposited so as to have a layer thickness of 10 nm to form an electron blocking layer.

(4.4) Formation of Light-Emitting Layer Next, the following compound 4-A (Tg = 143 ° C.) is 85 vol% as a host compound, and the following compound 4-B (Ir (bzq) 3) is 15 vol as a yellow phosphorescent dopant. The phosphorescent light-emitting layer having a layer thickness of 10 nm and exhibiting yellow was formed.

(4.5) Formation of Electron Transporting Layer An electron transporting layer similar to the first light emitting functional layer was formed, and a second light emitting functional layer 17 ′ having a stacked structure from the hole injection layer to the electron transporting layer was formed.

(5) Formation of reflective electrode Next, 150 nm of aluminum was vapor-deposited to form a reflective electrode 19 serving as a cathode.

(6) Sealing and connection of power supply Next, the laminated body from the transparent electrode 11 to the reflective electrode 19 is covered with a glass case from the reflective electrode 19 side, and an epoxy-based photocurable adhesive (Toagosei Co., Ltd.) is provided on the periphery of the glass case. The sealing agent by LUX TRACK LC0629B) manufactured by the company was provided. The glass case and the transparent substrate 10 were brought into close contact with each other through this sealing agent. Then, the laminated body from the transparent electrode 11 to the reflective electrode 19 was sealed by irradiating UV light from the glass case side and curing the sealing agent. However, the terminals of the transparent electrode 11, the intermediate electrode 15, and the reflective electrode 19 were brought out from the glass case, and a power source was connected to these electrodes.

  In addition, the sealing operation in the glass case is performed in a glove box under a nitrogen atmosphere without contacting the laminated body from the transparent electrode 11 to the reflective electrode 19 to the atmosphere (in a high purity nitrogen gas atmosphere having a purity of 99.999% or more). )

(7) Patterning-1
Next, a negative mask having a pattern in which the red component was decomposed was used as a light shielding mask 31 and was brought into close contact with the transparent substrate 10 under reduced pressure. Next, using a UV tester (Iwasaki Electric Co., Ltd., SUV-W151: 100 mW / cm 2), ultraviolet light having a wavelength of 385 nm was used as the first processing light L 1 and irradiated from the light shielding mask 31 side for 3 hours. As a result, the non-light-emitting region 13b obtained by modifying the light-emitting layer of the first light-emitting functional layer 13 ′ was patterned to form the first light-emitting functional layer 13 having the light-emitting region 13a and the non-light-emitting region 13b.

(8) Patterning-2
Next, a light-shielding mask 35 comprising a band-pass filter 35a that absorbs an ultraviolet component and a light-shielding pattern 35b of a negative mask having a pattern obtained by decomposing a red component was brought into close contact with the transparent substrate 10 under reduced pressure. Next, using an argon ion laser (Showa Optronics Co., Ltd .: 100 mW / cm 2), light having a wavelength of 514.5 nm was used as the second processing light L 2 and irradiated from the light shielding mask 35 side for 5 hours. As a result, the non-light emitting region 17b obtained by altering the light emitting layer of the second light emitting functional layer 17 ′ was patterned, and the second light emitting functional layer 17 having the light emitting region 17a and the non-light emitting region 17b was formed.

  The organic electroluminescent element was produced by the above.

≪Evaluation≫
About the produced organic electroluminescent element, the 1st light emission functional layer 13 and the 2nd light emission functional layer 17 were light-emitted separately on the conditions from which a current density will be 5 mA / cm <2> at room temperature (25 degreeC). The luminance of the light emitting regions 13a and 17a and the luminance of the non-light emitting regions 13b and 17b during light emission were measured using a spectral radiance meter CS-2000 (manufactured by Konica Minolta Sensing Co., Ltd.).

  As a result of the measurement, the luminance of the non-light emitting regions 13b and 17b with respect to the luminance of the light emitting regions 13a and 17a is 1:50 or more in both the first light emitting functional layer 13 and the second light emitting functional layer 17, and the pattern of the light emitting regions 13a and 17a Was successfully confirmed.

DESCRIPTION OF SYMBOLS 1 ... Organic electroluminescent element 11 ... Transparent electrode 13, 13 '... 1st light emission functional layer 13a ... Light emission area | region 13b ... Non light emission area | region [(lambda) 1] ... 1st wavelength (wavelength in which light transmittance reaches an upper limit)
h1 ... first emission light L1 ... first processed light 15 ... point intermediate electrode 17, 17 '... second light emission functional layer 17a ... light emission region 17b ... non-light emission region [λ2] ... second wavelength (light transmittance is upper limit value) To reach the wavelength)
h2 ... second emitted light L2 ... second processed light 19 ... reflective electrode

Claims (6)

A transparent electrode;
A reflective electrode;
A plurality of light emitting functional layers having a light emitting layer constituted by using an organic material, and disposed so as to overlap between the transparent electrode and the reflective electrode;
An intermediate electrode having light transmission sandwiched between the light emitting functional layer and the light emitting functional layer,
Each of the plurality of light emitting functional layers has a patterned light emitting region and a non-light emitting region,
Among the plurality of light emitting functional layers, the first light emitting functional layer located on the transparent electrode side has a shorter wavelength at which the light transmittance reaches the upper limit value than the second light emitting functional layer located on the reflective electrode side. The side is an organic electroluminescent device. The organic electroluminescent element according to claim 1, wherein the non-light emitting region is patterned on the light emitting layer in each light emitting region. The organic electroluminescent element according to claim 2, wherein an emission wavelength of the first light emitting functional layer is shorter than an emission wavelength of the second light emitting functional layer. The organic electroluminescent element according to claim 1, wherein the light emitting region of the first light emitting functional layer and the light emitting region of the second light emitting functional layer are patterned in different planar shapes.   The illuminating device which has an organic electroluminescent element in any one of Claims 1-4. On the transparent substrate, a transparent electrode, a first light emitting functional layer, a light-transmitting intermediate electrode, and a second light emitting functional layer in which the wavelength at which the light transmittance reaches the upper limit is longer than that of the first light emitting functional layer And a step of forming a reflective electrode in this order;
By irradiating from the transparent substrate side first processing light having a wavelength shorter than the wavelength at which the light transmittance of the first light emitting functional layer reaches the upper limit, the first light emitting functional layer is partially altered. Patterning the non-light emitting region on the first light emitting functional layer;
The second processed light having a wavelength longer than the wavelength at which the light transmittance of the first light emitting functional layer reaches the upper limit value and shorter than the wavelength at which the light transmittance of the second light emitting functional layer reaches the upper limit value, And a step of patterning a non-light emitting region in which the second light emitting functional layer is partially altered by irradiating from the substrate side on the second light emitting functional layer.

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