TW550964B - Organic electro luminescence device - Google Patents

Abstract

A kind of organic electro luminescence (EL) device is provided in the present invention, in which the light transparent efficiency, electric characteristic and lifetime of the device are improved. In the organic EL device, the injection and transmission of both positive and negative charges can be conducted. In addition, the positive holes generated by the positive and negative charges can recombine with electrons to emit light. The invention is provided with a light emission layer that contains the followings: light emitting material, which is generated under the recombination in the organic EL device; or the fluorescent material, which can perform the secondary light elision after the light emitting material is subjected to light. The invention is featured with containing the first kind of middle layer, which is located between outside of the light emitting layer and the light transparent interface that transmits the light toward the outside of the organic EL device. In addition, for the position distribution of light intensity transmitting from the light-emitting layer, it is amplified after transmitting the first kind of middle layer.

Description

f 550964 A7 B7 V. Description of the Invention (1) Technical Field The present invention relates to a new type of organic electric field light-emitting element, and particularly relates to the recombination of positive holes and electrons generated by the positive and negative charges after the positive and negative charges are injected. Organic light-emitting elements that emit light. 2. Description of the Related Art Recently, with the popularity of various mobile phones, mobile terminal devices, mobile computers, and car navigation systems, the demand for light-weight, high-resolution, high-brightness, and low-cost small flat-panel displays is increasing. In addition, flat displays such as desktop monitors or wall-mounted televisions that do not occupy space in homes and businesses have also replaced conventional CRT (Cathode Ray Tube) tube displays. In particular, with the popularization of high-speed Internet and the development of digital playback technology, wired and wireless two-way transmission that transmits hundreds or even hundreds of millions of digital signals per second has become practical, and ordinary users are gradually moving towards the real-time of a large amount of information. In the era of processing, the above-mentioned flat panel display not only requires lighter weight, better resolution and brightness, and lower price than the past, but also must have high-speed display capability capable of processing digital signals. Research and development of such flat displays include: Liquid Crystal Display (LCD), Plasma Display (PD), and Field Emission Display (FED). In addition to the above flat-panel displays, new flat-panel displays called Organic Electro Luminescense Device (OELD) or Organic Light Emitted Diode (OLED) have attracted the most attention in recent years. -4-This paper size is in accordance with Chinese National Standard (CNS) A4 specification (210 X 297 mm) 550964 A7 _ B7 V. Description of the invention (2) The so-called organic electric field light-emitting element 'encloses the current through the cathode and anode The organic compound is sandwiched, so that the fluorescent or phosphorescent organic molecules contained therein emit light. According to "Key Issues to be Solved and Practical Strategies for Organic LED Components" (edited by the Organic Electronic Materials Research Society, extended article, 1999) on page u, "Prologue: Current Status of Materials and Components" In the study of “Organic 黾% light-emitting elements” described in the topic, organic semiconductor single crystals such as molds (Anthracene) and perylene were mainly discussed in the early stage. By 1987, Tang et al. (C · W · Tang and S · A · VanSlykw ^, published by Appl. Phys · Let · M, 913, 1987) proposed a two-layer organic electric field light-emitting element under the lamination of a light-emitting organic compound film and a positive-hole transporting organic compound film. The starting point of this research is to improve the light-emitting characteristics (light-emitting efficiency 1.51 m / W, driving voltage 10v, brightness 100cd / m2). Since then, element technology such as pigment doping technology, polymer 0LED (organic electroluminescent display), low work function electrode, and hood evaporation method have been developed. In 1997, a so-called simple array method of charge injection method was developed. To complete the practical application of some organic electric field light-emitting elements, and continue to explore the development of organic electric field light-emitting elements with a new type of charge injection method called an active matrix. _ 木 The driving principle of this organic electric field light-emitting element is as follows. After the fluorescent or phosphorescent organic light-emitting material is filmed between a pair of electrodes, electrons and positive holes are injected from the positive and negative electrodes. The injected electrons in the organic light-emitting material are the lowest non-occupied molecular orbitals that enter the light-emitting molecules. -5-550964 A7 B7 V. Description of the invention

(Lowest Unoccupied Molecular Orbital, LUMO) is one of the electronic organic molecules (referred to as electrons). / The main entrance pore becomes one of the highest occupied molecular orbitals (Highest Occupied Molecular Orbital 'HOMO) of the luminescent molecule. Orthoporous organic molecules (referred to as positive pores), and in organic materials, they face the opposite electrode. On the way, you will encounter electrons and electric motors, that is, singlet or triplet excitatory reactions that form luminescent molecules, which will deactivate the light while radiating it, thereby emitting light. In general organic light-emitting materials, like various laser pigments, materials with high quantum efficiency relative to light-excited states are very common. For example, these materials emit light by charge injection. Because many organic compounds are insulators, their electrons and The positive hole has a low charge-transporting property. Therefore, an initial organic electric field light-emitting element requires a high voltage of several hundreds of V levels. The aforementioned Tang ’s double-layer organic electric field light-emitting element is effective in utilizing the high charge-transporting performance of the photoreceptor's organic photoreceptor and using the thin film knife to transfer charge (positive holes) and emit light. Improve luminous characteristics. ^ At present, a three-layer organic electric field light-emitting device has been developed, which is provided with an additional organic thin film, which bears one charge electron transportability. + In addition, organic electric field light-emitting devices with functional separation and multi-layer films have been successively proposed, which are enhanced by adding thin films that perform various functions, such as adding a charge injection layer to enhance the positive holes and electron injection organic materials. Injection characteristics, or adding a positive hole stop layer to increase the recombination probability of the two, etc. The only constant is that, as part of its light emitting source, during the deactivation of the organic light emitting molecules contained in the organic light emitting layer, the light is still emitted. -6-550964 A7 B7 V. Description of the invention (According to "Important Issues to be Solved for Organic LED Components (Organic Electricity, Materials Research Society, Text Extended Edition, 1999), Page 2 of War 2: n: / Section 2: Current Status and Issues of Luminescent Materials "It is very common for organic light-emitting materials that emit light or phosphorescence to be developed for various uses such as inks, dyes, glitters, etc. These organic light-emitting materials are used in organic electric field light-emitting devices. It is used. For example, it can be divided into low molecular weight and high molecular weight by molecular weight. Low molecular weight is formed in dry processes such as vacuum evaporation, and high molecular weight is formed by casting. Originally (before Tang's) using organic electric field light-emitting devices, but failed to produce high-efficiency devices, it is generally believed that one of the reasons is the inability to form high-quality organic thin films, especially the necessary conditions required for low-molecular types. : (1) thin film (about 100 nm) can be manufactured by vacuum evaporation method; (2) uniform film structure can be maintained after film formation (no need to filter out crystals); (3) solid Nanao light's quantum absorptivity in the state of sadness; (4) Moderate carrier transport; (5) Heat resistance; (6) Easy purification; (7) Chemical and electrical stability. In addition, if classified from the light-emitting process, it is also It can be divided into: luminescent materials, which emit light through the combination of direct electrons and positive holes, and fluorescent materials, which emit light when excited by the light generated by the luminescent material. If viewed from the difference in chemical structure , Common people have metal misalignment type. The paper size is applicable to China National Standard (CNS) A4 specification (210 X 297 mm)

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550964 A7 B7 V. Description of the invention (5) Materials (such as 8-Quinolinol in ligands, Benzoxazole, Azomethine and Flavone) Etc.), and Al, Be, Zn, Ga, Eu, Pt, etc. in the center metal, as well as light-emitting pigments (such as Oxadiazoles, Pyroxilin, Biphenylacetamidine, etc.) (Distyryl-allylene), Cyclopentadiene, Tetraphenyl-butadiene, Bis-styryrl-anthracene, Dichasylbenzene, Phenoanthrene, Low thiophene (〇iig0-thiophene), Pyrazoloquinoline (Thyadiazole-pyridine), layered Qin # 5 ore, p-sexiphenyl, and spiro compounds, etc.) Wait. Regarding the light-emitting materials and element-forming processes of these organic electric-field light-emitting elements, various materials and methods have been discussed in the past, but from these organic electric-field light-emitting elements, how much light can be obtained at the maximum or the degree of efficiency? Volume, there are still many doubts with clarification. According to "Important Issues and Practical Strategies for Organic LED Components to Be Solved" (edited by the Organic Electronic Materials Research Society, extended article, 1999) on pages 105 ~ ^ 18, "The First Section: Interpretation and Boundary of Luminous Efficiency "According to the description, the energy source for the external light emission of an organic electric field light-emitting element is equivalent to the number of photons emitted by the electrons flowing in the element or a positive hole, such as the external quantum efficiency of electric light emission 7? 4 (eXt) indicates that the following relations can be obtained: [Formula 1] T] ψ (ext) = 7? ext XV φ (int) = ?? ext (7 χ η τχ η ^ ····· (1) -8 · This paper size applies to China National Standard (CNS) Α4 specification (210 X 297 public concern) _ 550964 A7 B7 V. Description of the invention (6

Here, '7/4 (int) is the internal quantum efficiency, which means that a person and a dry clothes are not equivalent to the number of photons emitted by an electron flowing inside a piece or a positive hole. A, Taizhi 1 ★ K, 々 ext is the light transmission efficiency, which means that the light that occurs inside the component is reduced by the interface of the component and | called w Jiu Cai or absorption, 'the light transmission efficiency to the outside of the component.

In addition, τ is the charge balance, which is equivalent to the ratio of the number of electrons injected into the element to the center of the positive hole; 7? R is the singlet state exciton production efficiency, which means that from the injected charge, multiple state excitons that contribute to light emission are generated. proportion;. For the light emission quantum efficiency, it represents the proportion of singlet excitons that are deactivated after light emission. X corresponds to the external quantum efficiency of the amount of light emitted from these elements ^ "M", which can be roughly divided into: determined by the properties of the luminescent material itself ^ and ^ determined by the injection ratio of electrons and positive holes in the element In terms of f and 々eja, which are determined by the structure of the element, 0 r and 7? F are the efficiency of the physical properties of the light-emitting material itself, which is determined solely based on the light-emitting material used ^ r is based on the electrode and the electrode connected to the electrode The amount determined by the electrical potential difference, the interface potential difference of the organic layer, and the mobility of the electrons and the positive holes in the organic layer is an efficiency determined unilaterally based on the physical properties of the electrode material and the organic material inside the element. These Among the factors, the charge balance is ^^ 丨. The singlet exciton production efficiency r is generally determined to be ~ $ 025 from the spin relationship of the charge. The luminescence quantum efficiency 77 f is outside the superradioactive process, ^ 丨 < 1, Therefore, the factor part determined by the organic material and the electrode material inside the element [the part of the formula (7 X 77 rx 77 f)] is generally considered to be below 0. On the other hand, according to Nc Greenham R. H. Friend, DDC. Bradley, Adv. Mater. 491, 1994 paper pointed out that the light transmission efficiency __ _-9-This paper size applies the Chinese National Standard (CNS) A4 specification (210 X 297 mm) 550964 A7 B7 V. Description of the invention (7 is determined according to the law of reflection and refraction of classical optics. Assuming the refractive index of the light-emitting layer is η, then: [Formula 2] V ext = l / (2n2) ......折射率 The refractive index of the light-emitting layer of the final multi-organic electric field light-emitting element, or the refractive index of the glass substrate holding the light-emitting layer is about 1.6. The following assumes that ^ ^ = 0.2 The quantum efficiency is ^ (ext) $ 0.2 X 0.25 = 0.05, and its external quantum efficiency is generally considered to be a maximum of 5%. In order to make the organic electric field light-emitting element practical, this external quantum efficiency must be improved. There is an upper limit to the external quantum efficiency of organic electric field light-emitting elements. Therefore, the industry continues to develop organic electric field light-emitting elements with different functions. One of the methods is to try to improve the light-emitting quantum efficiency of the light-emitting material itself. 7 r. In the previous charge injection and recombination process, a singlet exciton of 0.25 and a triplet exciton of 0.75 will be generated. In view of this, the spin-orbit angle of organic light-emitting materials containing heavy metals is generated. The interaction of excitons under the interaction of motion causes the triplet exciton spin to flip into a singlet exciton, or under the conflict between triplet excitons enclosed in a nanoscale region, The conversion to singlet excitons and the like causes the generated triplet excitons to be converted to singlet excitons, thereby amplifying the proportion of excitons that contribute to light emission. Use materials such as fac tris containing this new exciton generator (2--10-This paper size applies to China National Standard (CNS) A4 specification (210X297 mm)

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Line 550964 A7 B7 V. Description of the invention (8

Phenylpyridine) iridium [Ir (ppy) 3], an organic electric field light-emitting device capable of emitting light with high efficiency, in M, A. BaldQUamansky, P1 Burrows, M · E · Thompson, S. R · Frorrest Paper Appl Phys Lett · II, 4-6, introduced in mid-1999. Another method is to try to improve the light transmission efficiency "... in order to improve the external quantum efficiency generated by the outside of the element, that is, a uniform thin film structure without previously filtering out crystals, which is a necessary condition for the manufacture of organic electric field light emitting elements, However, at this time, the organic light-emitting material constituting the light-emitting layer is in a spatially random alignment state, so it will be emitted in all directions isotropically inside the light-emitting element. In view of this, the light-emitting surface of the element is controlled in parallel directions, and A method of amplifying light emission in a vertical direction, for example, an organic electric field light emitting device described in Japanese Patent Application Laid-Open No. 40413 has a light emitting layer containing molecules that are aligned in a uniaxial direction by a lapping method. As described in Japanese Patent Application Laid-Open No. 11-102783, after the light-emitting layer is formed by a dry process in a vacuum, the photo-anisotropic reaction is used to orient the organic molecules constituting the light-emitting layer in parallel on the light-emitting surface. An organic electric field light-emitting element can also obtain anisotropic light-emitting characteristics inside the light-emitting layer. However, in the above-mentioned publication, it does not have It is explained that alignment improves the light transmission efficiency. Only Japanese Patent Application Laid-Open No. 11-102783 states that the light emission efficiency outside the element is increased from 0.51 m / W to 0.81 m / W, which is about ι. · Approximately 6 times. ° Relative 'In earlier papers "M. Hamaguchi and K. Yoshino, Jpn · J · Appl. PhyS · Vol. 34, p. L712, 1995", the organic Luminous anisotropy and light transmission efficiency of electric field light-emitting elements __-11-t paper size suitable financial _ house materials (CNS) A4 ^ g (21G χ 297 public love) -----------

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Line 550964 A7 — B7 V. Issue date > ^^ 0 month (September 1) '--~-’has been measured in more detail. As shown in Figure 1, a significant difference in light transmission between the two directions parallel and perpendicular to the alignment direction was found, but no significant light transmission was observed between the sample after alignment and the four materials without alignment. difference. Another method proposes that, in the light randomly generated inside the light-emitting layer, the design of the element structure is used to transform the components propagating in the film surface to the vertical direction of the film surface. For example, as disclosed in Japanese Patent Application Laid-Open No. 10-172766, the lateral end surface of the light-emitting layer is formed by dry etching, and the end surface of the film is used as a semi-transparent mirror < function, and then a certain proportion of the light is used to reflect the interior of the film. The loss is reduced, so that the total amount of effective light emitted from the front side of the film is increased, so as to increase the output luminous amount equivalent to the input energy of the light emitting element. In this method, the organic film needs to be dry-etched. However, since the organic film has weak mechanical strength, it is very difficult to form a high-quality optical surface to prevent the film from being damaged or used as a reflector. It is extremely difficult. . Similarly, according to the organic electric field light-emitting element of Japanese Patent Application Laid-Open No. 10-229243, which has a resonator structure perpendicular to the film surface, the proposed method is to 'make a fine periodic structure in the parallel direction of the film by using adjacent field light, so that The film surface has a fine periodic structure in a direction parallel to the reflection function, and this structure is used to change the emitted light. However, this method also has the problem of processability of the film, especially when the resonator structure is formed in the film surface, 'more precise processing precision is needed, plus the thickness of the organic light emitting layer itself is only about 100 nm. This end surface is processed by optical technology. It is really difficult. In addition, according to the proposal of Japanese Unexamined Patent Publication No. 10_398 η, which is based on bending -12-This paper size applies the Chinese National Standard (CNS) A4 specification (210 X 297 mm) 550964 5. Description of the invention (10 transparent substrate A thin-film electric field light-emitting element is formed on the inner side surface of the recessed portion to improve the efficiency of f. However, it is necessary to form a pixel electrode, a light-emitting layer, and a positive-hole transport layer on a flexible substrate to display complex images. It is extremely difficult to use a thin film. In addition, from the perspective of a display element, since the entire display area is greatly bent, it will cause a lot of restrictions on the field of view of the user. The luminous efficiency of the organic electric field light-emitting element has not yet emerged due to the above-mentioned multiple factors. The present invention must not only make the organic electric field light-emitting element practical, but also improve the external quantum efficiency. However, the above-mentioned past organic The electric field light emitting element has its upper limit of external quantum efficiency, and the solution includes improving the singlet state of the light emitting quantum efficiency of the light emitting material itself. The hair generation efficiency 々r, and the external quantum efficiency outside the element are improved by improving the light transmission efficiency 7; ext. Among them, the present invention particularly provides the latter method, which is to improve the light transmission efficiency 0 ext 'to greatly increase its efficiency. That is, the method proposed by the present invention improves the light transmission efficiency by adopting an element structure that is easier to form, and also for organic field light-emitting elements of the same composition disclosed in the past, under the same driving conditions, Allows more light to be transmitted to the outside of the device. The purpose is to reduce the power required to achieve pixel size optimization and high precision through this efficiency method, thereby increasing the life of the device. Especially ten inches When the above large-screen display elements and small-area but high-precision image display elements are used as driving elements, 13 paper sizes are applicable to the Chinese National Standard (CNS) A4 (210 X 297 mm) 550964. A7

Due to the inherent problems of mechanical materials, it cannot be used as a high-precision image display device. The previous proposal provided only a maximum of eight inches of image display devices. The present invention proposes a necessary basic structure for the next-generation organic electric field light-emitting element. Disclosure of the Invention In order to achieve the above-mentioned purpose of improving the light transmission efficiency of the organic electric field light-emitting element, the following describes the gist of the present invention: [1] An organic electric field light-emitting element, which can inject and transmit positive and negative charges, and can borrow The positive hole (Positive Hole) generated by the positive and negative charges and electrons recombine to emit light, and has a light-emitting layer containing a fluorescent substance, which can receive light from the light-emitting substance or the light-emitting substance to generate secondary The light-emitting substance is generated by recombination contained in the organic electric field light-emitting element; it is characterized by having a first intermediate layer, which is located outside the light-emitting light-emitting layer, and to the outside of the organic electric field light-emitting element. Between light-transmitting interfaces, and the azimuth distribution of light intensity transmitted from the aforementioned light-emitting layer is enlarged after passing through the first intermediate layer. [2] The organic electric field light-emitting device according to the above 1, the first intermediate layer can perform light scattering or optical path diffusion. [3] As for the organic electric field light-emitting element of 1 or 2 above, the first intermediate layer is separated one by one according to pixels having a specific shape, or the pixels are separated one by one by using a partition wall that includes properties different from the properties of the intermediate layer. substance. [4] As mentioned above, the first intermediate layer of the organic electric field light-emitting element is separated one by one according to the pixels adjacent to the light-transmitting interface, and its shape or the partition wall-14 This paper size applies to China National Standard (CNS) A4 specifications (210 X 297 mm) 550964 A7 B7 V. Description of the invention (12) "The shape of a ~ is a polygon, and at least two of the polygons are parallel. [5] The organic electric field light-emitting element according to the aforementioned 4, wherein the length of at least one of the parallel-opposite shaped surfaces that are polygonal is 0.25 to 2 times as long as the emission wavelength. [6] The organic electric field light-emitting element according to the above 3, the first intermediate layer is separated one by one according to the pixels adjacent to the light-transmitting interface, and the shape or the shape of the partition wall is circular. [7] The organic electric field light-emitting element according to the aforementioned 6, wherein the diameter of the circular first intermediate layer or the partition wall 'is 0.25 to 2 times as long as the light emission wavelength. [8] As mentioned above, the first intermediate layer of the organic electric field light-emitting element is separated one by one according to the pixels adjacent to the light-transmitting interface. The cross-sectional shape or the shape of the partition wall has a plane that is not parallel to the light-transmitting interface. Structure or surface structure. [9] As described in the foregoing organic electric field light-emitting element, the first intermediate layer is separated one by one according to the pixels adjacent to the light-transmitting interface, and the first intermediate layer or the partition wall is not connected to the light-transmitting interface or the light-emitting layer. Interface that allows light to be reflected or refracted. [10] The organic electric field light-emitting element as described above, the reflection at the interface is not regular reflection. [11] As described above, the cross-sectional shape of the first intermediate layer of the organic electric field light-emitting element is a shape in which the opening portion expands from the light emitting surface end to the light transmitting surface end, and the side surface of the first intermediate layer can reflect light And, in the first type of light-transmitting surface end of the intermediate layer, the side of the intermediate layer has a tapered inclination angle of 7 ° to a total reflection angle of -15-This paper size applies to China National Standard (CNS) A4 (210 X 297 mm) 550) 550964

V. Description of the invention (13) The angle is lower than 0 c. [12] As in the organic electric field light-emitting element described above, the shape of the other surface of the first intermediate layer is a shape in which the opening portion expands from the end of the light-emitting surface to the end of the light-transmitting surface. I The side surface of the first intermediate layer can make light Reflection; in the light-transmitting surface end of the first intermediate layer, the side of the intermediate layer has a tapered inclination angle of 7 / total reflection angle of 0 C and an angle of 0. Tied to 45. -0C / 2, and on the same section, the thickness d of the width a of the opening at the end of the light emitting surface of the first intermediate layer is lower than a / 2 tan 7 / ^ [13] The organic electric field as described above The device has a light-guiding layer having a cross-sectional area between the first intermediate layer and the electrode layer, and the area is smaller than the area of the light-emitting layer; the electrode layer has a light-transmitting property related to the light-emitting layer. [14] The organic electric field light-emitting element as described above, which has a light-guiding layer, the light-guiding layer has a cross-sectional area between the first intermediate layer and the electrode layer; the electrode layer has light permeability related to the light-emitting layer, The cross-sectional area is smaller than the area of the light-emitting layer and is not connected to the light-transmissive electrode layer. [15] The organic electric field light-emitting element as described above includes a light-emitting substance that absorbs light emitted by the first intermediate layer in the light-emitting layer and emits light of other colors. [16] The organic electric field light-emitting element as described above, wherein the first intermediate layer is formed inside the substrate ', and the substrate has a light-emitting layer on it. [17] The organic electric field light-emitting element as described above, wherein the first intermediate layer is formed on the outside of a light-transmitting substrate on which a light-emitting layer is carried. [18] The light-emitting layer of the organic electric field light-emitting element described above is formed on a substrate, and an amorphous silicon thin film transistor or a polycrystalline silicon thin film is formed in the substrate 550964 A7 _____ —_B7 V. Description of the Invention (14) Transistor , Or formed with a base film transistor. [19] The organic electric field light-emitting element as described above, the light-emitting layer is formed on the substrate, and an amorphous silicon thin film transistor or a polycrystalline silicon thin film transistor is formed in the tritium substrate, or an organic thin film transistor is formed. Integrated molding. The organic electric field light-emitting element mentioned here can inject positive holes from the anode electrode and electrons from the k cathode electrode into the light-emitting layer containing organic light-emitting molecules, and emit light by recombination of the positive holes in the light-emitting layer with the electrons. The light emitting layer may be a single layer or a plurality of layers. In addition, in addition to the organic light-emitting molecules that emit light through the positive holes and electrons recombination, the light-emitting layer may also contain a fluorescent substance (or a scale substance) that absorbs light generated by the organic light-emitting molecules, and Can emit other kinds of light. In addition, the light-emitting layer may also include a positive-hole transporting substance or an electron-transporting substance, which can improve the mobility of the positive-hole or electron in the light-emitting layer. In addition, the light-emitting layer may also contain a positive-hole-trapping substance or an electron-trapping substance, which is used to complement the positive-hole or electron in a specific spatial position, or to reduce the transmissivity of the positive-hole or electron. Furthermore, these organic light-emitting molecules, fluorescent substances (or phosphorescent substances), positive-hole transporting substances, electron-transporting substances, positive-hole trapping substances, and electron-trapping substances 'whether contained in the same layer or dispersed in each layer' Both. A layer formed by dispersing in several layers and containing these constituent substances is referred to as a light-emitting layer in the present invention. In addition, a positive hole injection layer or an electron injection can also be provided between the light-emitting layer of the present invention and the anode or cathode injecting positive holes or electrons into the light-emitting layer. The paper size is applicable to China National Standard (CNS) A4 Specifications (210 X 297 mm) 550964 A7 B7 5. Description of the invention (15), in order to improve the injection efficiency of positive holes or electrons. In addition, a substrate may also be provided to carry the light-emitting layer, anode, cathode, positive hole injection layer, and electron injection layer; or an intermediate layer may be appropriately added separately. The type of this intermediate layer can be exemplified by: a mirror or a part of a lens for changing the reflection characteristic of light, a filter for filtering specific light, an optical switch for adjusting the light exit time, and a phase characteristic for adjusting the light The wavelength plate, the diffusion plate for diffusing the light emission direction, and the protective film are used to prevent the element from being deteriorated due to light, heat, oxygen, moisture, etc. from the material constituting the element. These intermediate layers can be appropriately designed to prevent the characteristics of the light-emitting layer, the anode, the cathode, the positive hole injection layer, the electron injection layer, the intermediate layer and the substrate, or the components outside the substrate from deteriorating significantly. Among them, the outermost surface layer which transmits light from the organic electric field light-emitting element to the outside is particularly fixedly referred to as the outermost surface layer. In addition, the electric field light-emitting materials that can be used in the present invention include: various metal complex-type light-emitting materials (such as 8-Quinolinol in the ligand, Benzoxazole, methylimine) Compounds (Azomethine, Flavones, etc.), and Al, Be, Zn, Ga, Eu, Ru, Pt, etc. in the center metal, and fluorescent pigments such as 17 oxodiazoles (Oxadiazoles) , Pyroxilin, Distyryl-allylene, Cyclopentadiene, Tetraphenyl-butadiene, Bis-styryrl-anthracene, Dichaline, Phenoanthrene, Oligo-thiophene, Pyrazoloquinoline, Thiadiazole-pyridine, layered “# 5 ore, p- Bi-hexaphenyl (p- Sex ip henyl) -18-This paper size applies to Chinese National Standard (CNS) A4 (210 x 297 mm) 550964 A7 ______ B7 5. Description of the invention (16) 'and spiro compounds etc.) Wait. Alternatively, various polymer materials such as polyphenyl vinyl (Phenylene-vinylene), polyvinyl carbazole (Poly (Wnyi · carbaz_)), and polygolyl (Poly-flUOrene) are used. Etc.) as light-emitting materials, or non-luminous polymer materials (such as polyethylene, polystyrene, polyoxyethylene), polyvinyl alcohol (Poly (vinyl alc〇h〇1) )), Polymethylmethacrylate (Poly (methacrylic acid), polymethylmethacrylate, polymethylpropionate, polyisoprene, polyimide, and polyimide, and Polycarbonate, etc.) As a matrix, various luminescent materials or fluorescent materials may be mixed or copolymerized. In addition, various organic positive pores or electron transport materials (TdPhenylamine, etc.) can also be mixed therein. Various kinds of positive holes or electron injection layers (such as Li, Ca, Mg, Cs, CuPc, etc.) can be further mixed, and appropriate materials can be selected according to the component structure. As for the manufacturing method of the organic electric field light emitting device of the present invention, various thin film forming technologies can be used, such as a spin coating method, a coating method, a die casting method, a sputtering method, a true two-evaporation method, a molecular wire vapor-bonding method, a liquid Phase epitaxial growth method, atomic layer epitaxial growth method, rolling method, screen printing method, inkjet printing method Takinoki & method, grinding method, mouth plating method, water surface diffusion method, and Langmuir- Blodgett) thin film deposition method. In addition, in order to promote the alignment during or after such film formation, a crystalline substrate having an alignment limiting force on the substrate itself, an alignment film-coated substrate, and a substrate with a surface subjected to physical or chemical treatment can be used. In addition, the molecular structure of compounds suitable for such an alignment process is to match 550964 A7

During the processing, Gu + and Zhiri are better from soil a to m 1…. After the alignment process is performed, a new chemical bond is formed between the molecules at a temperature of τ field from the glass transition temperature of the cold heading to the Wudeng temperature, which is effective under the reaction. The method of fixing its alignment form is also used. In addition, the material of the substrate can be used, such as ..., the substrate includes polycarbonate, polydiethyl: ethylene, polymethyl methacrylate, and other organic substances such as acrylic acid, τ卞 bait (substrate, or copolymerization of both substrates). These substrates can be formed by various methods, such as cutting and grinding from the base material of the substrate, injection molding, mouth sand method, and cutting method. In addition, In order to control the light-emitting state, a substrate having a thin-film transistor formed thereon may be used, and an airport light-emitting layer may be formed on such a substrate with a thin-film transistor formed, or a substrate having a thin-film transistor and an organic substrate may be separately formed. After the substrate of the electric field light-emitting layer, 'the two are integrated into one by joining them. In addition, the organic electric field light-emitting element of the present invention can use various precision processing techniques' to facilitate the formation of desired elements in the process of element formation Structures can be exemplified by: precision stone cutting, laser processing, etching, photolithography, reactive ion, and focused ion beam etching (Focusin g Ion Beam Etching), etc. In addition, the processed organic electric field light-emitting elements can be arranged in a plurality of arrays in advance, 'multilayered', and connected by optical waveguide circuits, or packaged in this state. , Can also store components filled with inactive gas or inactive liquid-20-This paper size is suitable for towels ® ® Home Standard (CNS) A4 specification (210 X 297 public ^: 丨 _ ----------- 550964 A7 B7 5. In the container of the invention body, a cooling or heating mechanism can be further co-existed to adjust its operating environment. The materials that can be used for these containers include: copper, silver, stainless steel, aluminum, brass, iron and Various metals such as chromium and their alloys, or polymer materials such as polyethylene and polystyrene which are dispersed in these materials, as well as ceramic materials. In addition, the material for the thermal insulation layer can be used: foamed styrene. , Porous ceramics, glass fiber board, paper, etc. In particular, it can be painted to prevent condensation. In addition, the inactive liquid filled in the container can be a liquid with a low melting point, mercury, or a mixture thereof. The inert gas filled in the container can be helium, argon, nitrogen, etc. In addition, in order to reduce the humidity inside the container, a desiccant can be added. The organic electric field light-emitting element of the present invention can also be processed after the product is formed. In order to enhance the appearance, improve the characteristics or increase the life. Such post-treatments include, for example, thermal annealing, radiation irradiation, electron beam irradiation, light irradiation, radio wave irradiation, magnetic field irradiation, and ultrasonic irradiation. Furthermore, The organic electric field light emitting element can also be compounded by various methods according to various uses and purposes, such as adhesion, fusion, electroplating, vapor deposition, lamination, dyeing, dissolution molding, mixing, pressure molding, and painting. In addition, the organic electric field light-emitting element of the present invention can also be placed next to the driving electronic circuit and can be constructed with high density, and can be integrated with external signal receiving interfaces and antennas. Brief Description of the Drawings Figs. 1a and 1b show the basic element structure of an organic electric field light emitting element, which transmits light from the substrate end of the present invention. -21-This paper size is in accordance with Chinese National Standard (CNS) A4 (210 X 297 mm) 550964 A7 B7 V. Description of the invention (19 Figure 2 is the basic element structure of the organic electric field light-emitting element, which is derived from the Extremely transparent. Figures 3a, 3b, 3c, and 3d are the geometry of the first intermediate layer of the present invention. Figures 4a, 4b, and 4c are diagrams of the mirror structure inside the first intermediate layer of the present invention. Figure 5 ( 1) '5 (2), 5 (3), 5 (4), 5 (5), 5 (6), 5 (7), 5 (8) are one example of the manufacturing steps of organic electric field light-emitting devices. The organic electric field light emitting element has the first intermediate layer of the present invention. Figs. 6 (4 ') and 6 (5') are examples of manufacturing steps of the organic electric field light emitting element. The organic electric field light emitting element has the first intermediate layer of the present invention. An intermediate layer. Fig. 7 is a structural diagram of an element manufacturing device in an embodiment of an organic electric field light-emitting element of the present invention. Figs. 8a and 8b are structural diagrams of a test element for confirming the first aspect of the present invention. The effect of an intermediate layer is shown in Fig. 9. Fig. 9 is a principle for measuring characteristics of a test element, which is used to confirm the first aspect of the present invention. The effect of the intermediate layer. Figures 10a and 10b illustrate the pixel configuration of the first intermediate layer of the present invention. Figure 11 illustrates the optimal pixel size of the first intermediate layer of the present invention. Figures 12a, m and 12c are examples of the present invention. First Intermediate Layer for Display Pixels First First Interlayer Example Crystal Built-in Pixel Display Figures 13a and 13b are for display pixels of the present invention.-Figures 14a and 14b illustrate the thin film electrical components of the present invention. The case of using the first intermediate layer. -22-550964 A7 V. Description of the invention (20 The best form for implementing the present invention [Embodiment 1] Figure 1 is a basic structural diagram of an organic electric field light-emitting element of the present invention. Organic electricity The 7G light emitting device can perform the injection and transmission of positive and negative charges, and can emit light by recombination with the positive holes and electrons generated by the positive and negative charges. The organic electric field light emitting device includes: a light emitting substance, which It is generated by the recombination of the organic electric field light-emitting element; or it contains a fluorescent substance, which can emit light twice after receiving light from the light-emitting substance; It is characterized by containing a first intermediate layer, which is It is located between the light-emitting light-emitting layer and the light-transmitting interface that transmits light to the outside of the organic electric-field light-emitting element, and the azimuth distribution of the light intensity transmitted from the light-emitting layer is enlarged after passing through the first intermediate layer In general, an organic electric field light-emitting element is an organic electric field light-emitting material sandwiched between a pair of electrodes. After the electrons are injected from the cathode and the positive holes are injected from the anode, the two are in the light-emitting material. For example, in FIG. 1 (a), light is emitted from the light-emitting layer 2, which is sandwiched between the cathode 1 and the transparent anode 3. In FIG. 1 (b), it is emitted from the light-emitting layer. 2. The light emitting 'the light emitting layer 2' is sandwiched between the cathode 1 'and the transparent anode 3. In these light emitting layers 2 and 2 ', various conventional organic electric field light emitting materials can be used. Although not shown here, it can be multi-layered as necessary, and functional layers such as a positive hole transport layer and an electron transport layer, a positive hole injection layer, and an electron injection layer are added. Since the electric field emitting part of the two is a thin film with a thickness of at most several hundred nm, it is formed on the substrates 4 and 4 made of glass or transparent plastic. Luminous layer-23-This paper size applies Chinese National Standard (CNS) A4 specification (210 X 297 mm) 550964 A7 __B7 V. Description of the invention (21) 2, 2 'The light generated inside 2' will pass through the transparent anode 3, 3 *, And further passes through the substrates 4, 4 *, and penetrates to the outside of the element. This light finally passes out to the component interface outside the component, which is fixedly referred to here as the light-transmitting interface 6, 6 *. The basic structure in the features of the present invention is formed on the outside of the light-emitting layers 2, 2, and the portion between the light-transmitting interfaces 6, 6, and forms a region of the so-called first intermediate layer 5, 5 '. It is characterized in that the light intensity and azimuth distribution will be enlarged after passing through the first intermediate layer 5 during the process of light being induced to the outside through the field. Fig. 1 (a) shows the case where the first intermediate layer is formed inside the substrate 4. Fig. 1 (b) shows the first intermediate layer 5, which is formed after the substrate 4 and the external storage medium 7 are bonded inside. structure. FIG. 2 shows the structure of the light emitted from the opposite end of the substrate. The stacking order of the anode 8, the light emitting layer 9, and the transparent anode 10 on the substrate 11 is reversed, and the light generated inside the light emitting layer 9 is induced to the upper part of the element. In this case, after the upper portion of the transparent anode 10 and the first intermediate layer 12 formed inside the storage medium 14 are joined, the internal light will pass through this intermediate layer 12 and reach the light-transmitting interface 13 to emit light to the outside of the element. The structure of the first intermediate layer of the present invention is, for example, the first intermediate layer facing inward in the substrate in FIG. 丨 (a), or the internal type facing inward in the storage medium in FIG. 1 (b) or FIG. 2. At the interface, light can be reflected or diffused, and the inside of the first intermediate layer is formed as a uniform optical medium. The light generated inside the light-emitting layer is generally isotropic, so before the light reaches the interface, it will be lost due to the reflection on the interface of each film or a large amount of outside the element. The larger the difference in refractive index between the films, the reflection is -24-This paper size applies the Chinese National Standard (CNS) A4 specification (210X297 mm) 550964 V. Description of the invention (22 1 The greater the loss of buckle, especially the substrate The largest deduction occurs in the interface with air. Such reflection generally increases as the normal angle of the interface's normal increases, and the 'light' emitted by the azimuth that exceeds the total reflection angle will be completely impossible. For example, if the refractive index of the substrate is 15 and the refractive index of air is 丨, the total reflection angle (9c = Sin-i (1 / 1.50, 41.8.), If the emitted light is greater than this angle Therefore, it can only be propagated in the direction of the substrate and become a total loss. For this reason, imitating the first intermediate layer, by forming the first intermediate layer with a specific structure in the film surface of the _ layer, the direction can be changed The light path that propagates in this direction and induces light to propagate out of the plane. In order to further exert the light scattering or light path diffusion effect of this first intermediate layer, it is necessary to reduce the light emitting layer / transparent anode and the first type as much as possible. Interlayer The reflection on the surface, that is, it is best to reduce the difference in refractive index as much as possible, or = the refractive index on the first intermediate layer is greater. However, in the latter case, the difference between the refractive index of the final light-transmitting interface and the air is more Large, sometimes necessary other methods to prevent refraction. Tochigi takes an intermediate layer S formed one by one according to each pixel, which is the light-emitting unit of its Thai field light-emitting element. That is, it is characterized by: the first layer Separate pixels one by one with a specific shape; or use i to separate pixels one by one, and the partition wall contains objects with properties different from that of the intermediate layer: Figure 3 shows an example of the geometry of this first intermediate layer. In (d), the left row is a cross-sectional structure, and the right row is a three-dimensional structure, but each has a light-emitting layer above and a light-transmitting interface below. White Figure 3 (a) is a trapezoid with four sides, which emits light from the upper side. Light entering through the layer -25-This paper size applies Chinese National Standard (CNS) A4 specification (21〇X 297 public love) 550964 A7 B7 V. Description of the invention (23) --- ^ The line will reflect on the four sides and Change its marching woman a.] Reverse the universal , Reaching the light-producing interface on the lower side, so that light can be reflected and diffused in four directions. Although the cross-sectional view in Fig. 3 (b) is trapezoidal, it is actually a circular t-shape. | The shape of the reflecting surface is circular, so the light reflects and diffuses in the same direction in the plane. Figure 3 (c) is a cube structure, the light will only be reflected on its side, and the light at the ends of the light-emitting layer and the light-transmitting interface will enter and exit. The angles are the same, so other interface structures must be designed on the light-transmitting interface to reduce its reflection loss. If the side has light scattering, it can increase the amount of light transmission. Figure 3 (d) is hemispherical, and the first This kind of intermediate layer has a parabolic reflective structure 'so that the light propagating in the plane can be changed, and it can be largely reflected in the direction of light transmission outside the element. In addition to the above, with a special optical design, the first intermediate layer is separated one by one according to the pixels adjacent to the light-transmitting interface, and the shape or shape of the partition wall has a planar structure that is not parallel to the light-transmitting interface. Or the curved surface structure can be designed so that the light in the in-plane direction changes out of the plane. Especially in the structure of FIG. 3 (b), the first intermediate layer is separated according to the pixels adjacent to the light-transmitting interface one by one, and the shape or the shape of the partition wall is a polygon and has a polygonal shape. , At least two faces are parallel. In this parallel plane, a polygonal and parallel-opposite shape plane is set to have at least one group with a length of 0.25 to 2 times the light emission wavelength. In this way, the shape plane can be made under the effect of a microresonator. The light reflected between them is optically amplified. This effect can be achieved in particular by dispersing the pigments together. The pigment-26-SS reading accuracy (CNS) A4 specification (2iQχ 29? Public love) 550964 A7 __B7 V. Description of the invention (24 ) Is sufficient for laser oscillation on light-induced media. Although the first intermediate medium is also omitted from the illustration, its shape is cylindrical, and even if the diameter of the circle is 0.25 to 2 times as long as the light emission wavelength, it can still have the effect of a micro-resonator inside. FIG. 4 shows the specific structure of the first intermediate layer, which is separated one by one according to the pixels adjacent to such a light-transmitting interface, and is at the light-transmitting interface of the first intermediate layer or the partition wall, and The interface not connected to the light emitting layer has a function of reflecting or refracting light. FIG. 4 (a) is an example in which a reflecting mirror is formed on the side of the first intermediate medium. A reflecting mirror 16 is formed on the side of the trapezoidal first intermediate layer 18 formed in the storage medium 15, and the central portion is filled. There is a light-inducing medium ι7 for adjusting the refractive index. FIG. 4 (b) is a first intermediate medium 18 formed in the storage medium 15, and instead of the reflecting mirror 16 in FIG. 4 (a), a diffuser 19 is formed, and a central portion thereof is filled with a light-inducing medium 17. To adjust the refractive index. When the refractive index difference between the first intermediate layer and its storage medium is large, such a reflection or scattering function can still be retained. For example, the structure of the first intermediate medium 18 in the figure can also perform the same function. The first intermediate medium 18 is formed in the storage medium 15, and has the same shape as that of FIG. 4 (the central portion is also filled with a light-inducing medium i7 "to adjust the refractive index. But here In some cases, some of the light reaching the side may be lost to the storage medium 15 ". The light-inducing medium in the central part guides the light from the light-emitting layer to the outside, but it can disperse various functional pigments in it, thereby improving | Electromechanical field emission-27-This paper size applies to Chinese National Standard (CNS) A4 specification (210X297 mm) '--550964 A7 -------- -B7 _ V. Function description of the invention (25) In particular, the right side contains light that can absorb the light emitting layer, and produces other colors of light. 2 Substances can perform color conversion of light. Let each pixel share the main colors that red, green, and i primary colors can have. The light layer's light color is changed to emit several colors of light, which can realize simple and efficient color display. This first intermediate layer prevents interference with the multiple internal reflections to prevent the color of light from emitting outside the device. From this point of view, it is better that the thickness is substantially thicker than the wavelength of light. In addition, in order to direct the light generated by the light-emitting layer to the first intermediate layer, as described above, the refractive indices of the two The difference is preferably zero. The light emitting layer end of the surface of the contact part should be covered with the first intermediate layer end, because if the refractive index of the light emitting layer end is large, the light emitting part will be generated outside the first intermediate layer. It is difficult to fully induce the light emitted by the light-emitting layer. In addition, the pixel size should be the same as the area of the light-transmitting interface end of the first intermediate layer, and the area of the light-emitting layer end should be smaller. Usually the total reflection in the interface is due to total reflection. When the loss caused is taken into consideration, at most only 20% of the light generated in the light-emitting layer will be transmitted to the outside, but if the first intermediate layer is used, all the light propagating in the plane will be induced. To the outside of the element, 100% light transmission efficiency will be achieved. Therefore, the area of the light-emitting layer equivalent to one pixel may be 1/5. In addition, as shown in FIG. 1 (b), when the transparent anode 3 and the first In the case where the intermediate layer 5 is separated by the transparent substrate 4, the light generated by the light emitting layer 2 will diffuse before reaching the first intermediate layer 5, so the distance between the two should be short. The paper size applies the Chinese National Standard (CNS) A4 specification (210 X 297 mm) 550964 A7 __B7 5. Description of the invention (26) Specifically, it must be greater than the wavelength of light and less than 1 mm. By making the first intermediate The layer satisfies the above-mentioned conditions of shape, size, and refractive index, and is placed between the light-emitting layer and the light-transmitting interface, which can direct a large amount of light to the outside of the element. [Embodiment 2] The following uses FIG. 5 to show an example of manufacturing steps of the first intermediate layer of the 'conical shape' in the first intermediate layer structure shown in Example 1. (1) To form an organic electric field light-emitting element The glass substrate 20 is made of borosilicate glass (size 40X 40X 0.8 mm, double-sided grinding). (2) Use a sandblasting method (a processing method of spraying fine sand-like particles with a high-speed nozzle) on a glass substrate to open a cone-shaped processing hole with a spray range of 〇〇〇 × 60mm and an upper processing hole of 295.5 # m The lower hole is 836 5 and the taper angle is 70 °. (3) A molecular beam deposition apparatus' was used to deposit a 100 nm chain on this substrate from one end of the lower processed hole to form a reflecting mirror 22. (4) The processed hole is filled with a refractive index adjusting resin 23 as a light-inducing medium. The refractive index adjustment resin should be selected whose refractive index is close to that of the organic electric field light-emitting layer. In this embodiment, one of the following is selected: polymethylpropionate, polyphenylenesulfonium, polyethylene glycol, and polyfluorene Amines and the like. (5) After hardening sufficiently, grind with an abrasive to remove excess resin that oozes up and down, and flatten the surface. (6) Next, at the substrate temperature and room temperature, a thin film was formed by sputtering IZO (indiUm Zinc Oxide, InZnO) on the top surface with a sputtering device as a transparent anode 25. The film thickness of IZO is 100 nm, and the sheet resistance is -29.-This paper size is applicable to the Chinese National Standard (CNS) A4 specification (210 X 297 male cage) 550964 A7 B7 5. Description of the invention (27) is 60 Ω / □. The substrate manufactured so far is rinsed with pure water for one hour, and then subjected to two 15-minute ultrasonic cleanings in pure water, and then immersed in acetone (a special reagent manufactured by Wako Pure Chemicals) for 15-minute ultrasonic cleaning. Clean and dry with dry nitrogen. After being placed in the air for 5 minutes under ultraviolet light irradiation, it was mounted on a molybdenum substrate holder (manufactured by Japan VacsMetal), and the entire substrate holder was quickly installed in the replacement chamber of the molecular wire evaporation device. (7) In this molecular wire vapor deposition device, an organic electric field light emitting layer 26 is formed, and further through a patterned light shield, a cathode 27 is formed. In order to confirm the effect of the present invention, the light-emitting layer here has a double-layer structure, which includes a positive hole transport layer and an organic electric field light-emitting material layer. The positive hole transport layer uses a-NPD (4,4-bis [N- (l-naphthyl) -N-phenylamino] biphenyl); the organic light-emitting substance uses Alq3 (aluminium tris (8-hydroquinoline)). At 60 nm, a positive hole transport layer and an organic light-emitting substance were sequentially vapor-deposited on the IZO, and then 0.5 nm of LiF was vapor-deposited thereon to form an electron injection layer. The layers such as the positive hole transport layer and the electron injection layer are equivalent to the organic electric field light emitting layer 26. Thereafter, A1 was further evaporated to form a cathode. Fig. 7 is a diagram showing a device configuration of a molecular wire vapor deposition device used in the production of a sample in this embodiment. The positive-hole transport layer, the light-emitting layer, and the cathode are formed by vapor-bonding in a molecular wire evaporation device (referred to as OMBE type, IMBE-620 manufactured by Dennel Annelva). The molecular wire evaporation device includes: a replacement chamber for replacing and installing a substrate holder; a pre-processing chamber for carrying the substrate in the replacement chamber and heating it to a maximum of 1300 ° C; a first growth chamber, which Form a positive hole transport layer -30-This paper size applies Chinese National Standard (CNS) A4 specification (210 X 297 mm) 550964 A7 _ B7 V. Description of the invention (28), organic light emitting material layer and inorganic barrier layer; Two growth chambers, which form metal electrodes; and an analysis chamber, which analyzes the surface state of the formed thin film by ESCA (Chemical Analysis Electron Spectrometer) and AES (European Electronic Spectrometer). Its structure is: the basic pressure of each room is about 10-10 GT0rr outside the exchange room, the exchange room is 1 (about T9 Torr, each room is separated by a gate valve (Gate Valve), and if necessary, can be The entire substrate holder is moved under ultra-high vacuum. In addition, 'the substrate is installed in the replacement chamber, and the samples after film formation can be removed through a hand-held work box (G1ove Β〇χ separated by a gate valve). (Manufacturing) 'and in a dry nitrogen environment under the pressure of air but removing oxygen and moisture. During vapor deposition,' if necessary, the substrate is moved to the first and second growth chambers. For vapor bonding, 'liquid first Nitrogen cools the growth chambers, and at the same time, the raw material substances previously installed in each growth chamber are sublimated or evaporated in order to be evaporated on the substrate to form a thin film and the raw material substances. The organic substances are placed in a quartz steel stack (Nippon Electric Anelva Corporation). In the production), the inorganic substance is placed in a crucible made of boron nitride (manufactured by Shin-Etsu Chemical Co., Ltd.), and after being installed in each growth chamber, it is "vacuumed" and heated by a heater to make the raw material gas The outlet of the crucible is equipped with a mechanical shutter (Shutter). The shutter is switched on and off for a fixed time to evaporate the vaporized raw material onto the substrate. Using a crystal vibrator film thickness meter placed near the substrate, Measure the thickness of the raw material film after evaporation to form a film with a predetermined film thickness. In addition, the temperature of the substrate can be maintained in the range of -90X: ~ 150 ° C. -31- (CNS) A4 size (210 X 297 male f 550964 A7

__BV 5. Description of the invention (29)-In terms of evaporation rate, the temperature of the crucible is set according to the organic and inorganic barrier layer 0 ″ and the cathode material at about 30 nm / s. …, The plating sequence is: firstly forming a positive-hole transport layer with a predetermined film thickness in the first growth chamber, and then forming a light-emitting layer with a predetermined film thickness in the same chamber, which includes an organic light-emitting material layer and an inorganic barrier layer, and then The sample is temporarily transferred to the replacement puppet, and the sample is transferred to a substrate holder at the child's place. The substrate holder is equipped with a stainless steel metal hood; the sample is then transferred to the second growth chamber and turned into a cathode. The mixing ratio of the alloy cathode is determined by the presence of each element in the analysis room (electronic edge detector). The substrate temperature during the formation of the cathode was set at _90. (: ~ 3 (A predetermined temperature in the range of rc. After the cathode is formed, the sample is transferred to the replacement chamber, and then taken out of the glove box, a glass plate cover is made inside the glove box, and the resin is cured with ultraviolet rays) The end of the package is sealed. In the final sample, the light-emitting layer area is encapsulated, and the anode and cathode are led out to the outside so that a voltage can be applied to the two electrodes from the outside using gloves. In addition, FIG. The element manufacturing steps are transparent anodes that are difficult to form at low temperatures. (1) substrate preparation; (2) tapered hole processing; and (3) mirror evaporation steps are exactly the same as in Figure 5, Therefore, the description is omitted here. In FIG. 5, the transparent resin sealed in FIG. 5 (4) is a substrate, and then a transparent anode made of ιζο and the like is formed. In contrast, IT0 (indium tin oxide, Indium) is used. Tin Oxide (InSnO) transparent anode to form a low sheet resistance -32-This paper size is applicable to China National Standard (CNS) A * specifications (21G X 297 public directors)-550964

The electrode ’must make the substrate temperature rigid. C is vapor-deposited above. Therefore, the substrate method uses a resin filled with a refractive index adjusting resin in advance. In this case, it is necessary to separately deposit IT0 on a glass substrate 31 with a thickness of 50 by sputtering to form a transparent anode 30, and then use a molecular wire evaporation device to sequentially vaporize the positive hole transport layer, organic The light-emitting material and the electron injection layer form a light-emitting layer 29, and the Ai cathode 28 is vapor-deposited thereon, followed by glass encapsulation to form a substrate organic electric field light-emitting element portion 32. As shown in FIG. 6 (4 '), the basic organic electric field light-emitting element portion 32 is bonded to the bonding surface 33 of the substrate. At this time, the dilute solution of the resin for adjusting the refractive index is first penetrated into the bonding surface 33, and the effect is better. . Next, as shown in FIG. 6 (5,), the refractive index adjusting resin 33 is filled in the aforementioned processing hole ', and the exuding resin is removed by grinding, and the element is completed. The above-mentioned work is to calibrate and join the positions of the two outside the hand box. What are the steps? In the case of manufacturing an image display element, it is necessary to pattern the transparent anode and cathode to form display pixels, but the illustration is omitted here. In order to drive as an image display element, several processing holes are formed in a substrate during manufacturing to form a first intermediate medium. However, due to the current processing precision, it is difficult to perform drilling operations smaller than this processing hole size. Due to technical limitations, the anode and cathode of the light-emitting layer are simple array structures with a width of 300. This electrode is then spaced at 100 intervals to form 40 rows in vertical and horizontal directions, and the intersection is a pixel. On this anode and cathode, the external wires are joined by soldering silver. Any anode and cathode are arbitrarily selected, and a voltage of 8 V is applied, so that all -33-550964 A7 _ ____ B7 can be confirmed. 5. Description of the invention (31 ~- -Light emission situation at the pixel position. [Example 3] Next, a test organic electric field light-emitting element having a single-pixel is formed, and its light diffusion characteristics are evaluated in the following description method. FIG. 8 shows the test organic electric field light-emitting element. Figure 8 (a) is a component with a first type of intermediate layer, the same as Figure 不 is a component without a first type of intermediate layer. The principle of the part that generates an organic electric field is the same, and its manufacturing method is implemented by The method of FIG. 6 of Example 2 is performed. That is, in FIG. 8 (a), a cathode 35, an electron injection layer 36, an organic light emitting material ^, a positive hole transport layer 38, and a transparent anode 39 are formed on the substrate 40 from top to bottom. That is the substrate organic electric field light-emitting element portion 41. Next, according to the method of FIG. 6, after drilling a processing hole in the first intermediate layer, the element portion 41 is bonded to a storage medium 43, and a reflective medium is deposited on the storage medium. Here, in order to prevent light leakage, a light-shielding cover 42 is formed on the top surface other than the hole. The specific method is to coat a thin layer of resin on the top surface, and then spray carbon powder on it. Then, the storage medium 43 manufactured in this manner is bonded to the basic organic electric field generating element portion 41, and the refractive index adjusting resin material is sealed after the bonding to form an element. Here, the glass of the storage medium portion 43 and the basic element portion q are formed. The broken glass substrate 40 is made of the same glass material, and the same refractive index adjustment resin is used as the glass. + In addition, the comparative organic electric field light-emitting element is also the same as the principle of the organic light-emitting part knife, and its manufacturing The method was carried out using the -34-National Standard (CNS) A4 specification (210 X 297 public love) 550964 A7 _ _ B7 of the second embodiment V. Description of the invention (32) The method shown in Figure 6 was performed, that is, shown in Figure 8 ( b) In the substrate 40, a cathode 35 ·, an electron injection layer 36 ', an organic light-emitting material 37, a positive hole rotation layer 38, and a transparent anode 39' are formed on the substrate 40 from top to bottom. Element 41, should be associated with this element The storage medium 4 3 'bonded by 4Γ without the first intermediate layer is a glass plate directly before drilling, in which a light shield 421 is formed on a part of the area, which is the same as that of FIG. 8 ( a) The size of the openings on the top surface of the first intermediate layer, so that light can pass through β from the storage medium 43f completed in the above-mentioned method, and the above-mentioned element portion 41, after joining, becomes a comparison element. This is a block diagram for element evaluation, which evaluates the difference in light diffusion characteristics. A voltage is supplied to the organic light-emitting element 45 after manufacturing, and a voltage supply / current measurement device 48 (manufactured by Hewlett-Packard Company, pA Meter / DC) is used to measure the amount of current. Voltage Source 4140B) Apply voltage to make the current flow from the anode to the cathode inside the element, so that the element emits light. ^ The photometer camera 46 and its photometric controller 47 (Spectra, manufactured by Photoresearch, Spectra) Pritchard

Photometer (Model 1980 A-PL), which measures the amount of light emitted. The relative azimuth angle β with respect to the normal direction of the light transmitting interface of the photometer camera was measured using a rotary table 5 (manufactured by Chuo Seiki Co., Ltd.) driven by a pulse motor. The photometer control sensor 47, the electric dust supply / current measurement device 4 §, and the rotary table 50 are controlled by a control computer 49 which controls and measures the same. Measurements are always performed at room temperature, and no temperature control is performed. Using the components in Fig. 9 (a) and Fig. 9 (b), compare the observed development from the outside of the component. -35-This paper size applies the Chinese National Standard (CNS) A4 specification (210 X 297 mm).

Binding

Line 550964 A7 ____ B7 V. Description of the invention (33) In the light characteristics, it is found that if the component of FIG. 9 (b) takes the frontal brightness (θ = 0.) as the maximum value, then at about cos2 Θ, the luminous intensity decays. The so-called Lambertian light-emitting characteristic has a light amount of 12,000 cd / m2 and 0 = 20 at a voltage of 10 v. 1000 cd / m2. In contrast, at 00 ° ~ ± 30. Observed in the fan garden with approximately equal brightness, the light amount of the element in Fig. 9 (a) is 630,000 cd / m at a voltage of 10 v. This data shows that in the element in Fig. 9 (b), the light is stored in the direction of The medium 43, propagates in the in-plane direction, and transmits almost all light that could not be transmitted out of the plane to the outside. In addition, from the taper inclination of the machined hole, it can be presumed that this element is within ± 20. Light can be observed in the bottom, but it was found in the experiment that the angle at which the light can be observed is slightly wider. It is presumed that the processing surface was roughened by sand blasting and unexpectedly caused a random reflection effect. [Embodiment 4] The structure size and design example of the present invention will be described below for an organic electric field light-emitting element used for image display applications. When used as an image display element, the light emitting portion 77 of each organic electric field light emitting element is divided into regions of the stomach pixels, and the light emission amount and light emission time of each pixel are controlled by the control circuit of the image display element. The pixels in the image display element are arranged in two dimensions, and the number of pixels is standardized according to the resolution of the image display element.

For example: VGA = 640X 480, SVGA = 800 X 600, XGA = 1024 X 768, SXGA = 1280 X 1024, UXGA = 1600 X 1200, HDTV = 1920X 1080, and qxga = 2048 X 1536. -36-This paper is suitable for a country's fresh (CNS) A4 specification (21GX 297 public directors) 550964

For this reason, the size of each pixel in the image display element, 夂, and σ ^ γ, is determined according to the screen size and resolution. For example, the full screen size is 123 X 31 mm, and the resolution is XGA (number of pixels 1024X) In the case of / 〇 * · >-8768), the size of each pixel must be within the area of 120X 40 / zm or less. Figure 10 shows the layout of the pixels and the relationship between (a) and (b); (a) Bi Yijun Yi using a general organic electric field light-emitting element-the image display is not good, (b) is the use of the present invention Image display element with a structure of an organic electric field light emitting element. For simplicity, Fig. 2 shows the pixels on the substrate of the organic electric field emitting light, and -law_ is shown as a pixel. As for the pixels formed on the substrate of the substrate thickness d, 2, and 3, if it is assumed that the pixel size is M and the pixel pitch representing the pixel pitch is L2, then the size of a pixel includes the light emitting pixel portion and the pixel pitch. Its length is L1 + L2. Although not specifically described here, the vertical direction of the paper surface is also a pixel region ', and its length is also equal to the sum of the pixel size and the pixel pitch. If the light emission of each pixel is emitted from the substrate to the outside, the light emitted from the interface between the pixel and the substrate will diffuse light during the process of reaching the light-transmitting interface at the bottom of the substrate and partially reflect at the interface between the substrate and air. 'And the light arriving at an angle greater than the critical angle will be fully reflected and transmitted to the lateral direction of the substrate #, so if it is too close to the adjacent pixels, the light will be mixed, and the color will be generated in the full-color image display. Color mixing effect. • In this case, the pixel itself adopts an optical resonator structure ’or a conical surface is provided in the lateral direction of each pixel to improve the alignment of light entering the substrate & the substrate can propagate laterally. However, when light is transmitted to the outside of the device, it also produces -37-

550964 A7 B7

V. Description of the invention (35) The residual light alignment property not only narrows the viewing angle of the image display element, but also causes the interference effect of the resonator to mix light interference colors, resulting in non-uniform display colors. This problem is solved by including the present invention. An organic electric field light-emitting element like an image display element is taken as an example. The first intermediate layer is set, for example, an angle of 7 ° formed by the cone surface and the normal line of the substrate surface is set at the midpoint between the pixels on the transparent interface. The position can prevent the light emission of each pixel from being mixed in the substrate, or the alignment of the light can be avoided, and the light can be radiated to the outside of the substrate. FIG. 11 illustrates a method for determining the size of the first intermediate layer of the organic electric field light-emitting device of the present invention for such an image display device. The light that enters the substrate from the pixel is emitted by the pixel at various azimuth angles because the pixel itself is a two-dimensional light emitter. It restricts the horizontal interface reflection of the substrate of the first intermediate layer and finally reaches the light-transmitting interface at various angles. Therefore, part of the light on the transparent interface will be reflected. When the reflection angle is wider than the total reflection angle, the light will return to the pixel again and cannot be transmitted out. Therefore, the best cone of the first intermediate layer must be calculated. Shape inclination, and its thickness and refractive index. If the angle formed by the tapered surface of the first intermediate layer and the normal to the substrate surface is 7 / ', the tapered inclination angle is 7Γ / 2-77. Assume that from the light emitting point p at the bottom of the substrate, the position where the light emitted in the azimuth 4 reaches the tapered surface is W, and the position at which the W reflects and reaches the top surface of the substrate is V, and the point corresponding to the height of the point w on the Z axis is G. The point where the normal of the cone surface at the point W intersects with the z-axis is ρ, and the point where the cone surface intersects with the χ-axis is E. It should be noted that the incident angle of the radiated light relative to the cone is ZPWF, the direction of the reflected light is only the azimuth vector of the incident light at the point W, and the negative square of the inverse vector -38-This paper scale applies the Chinese national standard (CNS ) A4 size (210 X 297 mm)

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Line 550964 V. Description of the invention (36 A7 B7 '^ — Direction rotation ZPWV = 2 ZPWF. At this time, pay attention to 0>, Bei 1J: [Formula 3] △ GWP ^ a φ, B GWE-η ZJ ^ WE = B GWE — ZX ^ WP = φ — tj Z ^ PWF Z ^ WE --- (0 _ ”) (The radiation vector at point X is: The normal vector of the cone surface is ···

Z rsin0 ^, cos ^ i fx \ SS cos (-sin (-y) (sinrj, / 一 cos 17 ,, / -sin (-―) [2J cos (-| \ (cosr ^ {sin? 7 y radiated light The angle at which the inverse vector of the azimuth vector and the conical surface of the conical surface and the spring vector form, can be obtained from its inner product: [Formula 4] (-cos 7 /) (-sin 0) + sin 7? (-Cos 0) = sin (0-7 /) whose angle is (; t / 2) —4 + 7; With a positive rotation of only twice the angle as the orientation of the reflected light, the orientation vector of the reflected light is: [Formula 5] cos (--φ + η) (X, 丨 Z 丨 (cos [jt-2 (φ-η)] sin [; r — 2 (φ-η)] γ-sin 沴, bu sin [ 7r-2 (0-77)] cos〇r — 2 (0-η)] cos (^-sin (^ r-0 + 2? 7) \ /-sin (^)-2η) \ 「cos (; r + 2η) wide (cos (Bu 2rj) y -39-This paper size is applicable to the Chinese National Standard (CNS) A4 specification (210 x 297 mm) 550964 A7 B7 V. Description of the invention (37 The azimuth angle is: [Formula 6]-$ in (^-2η) cos (彡 一 277) _ arctan = arctan [tan (2; 7 = ...... (3) It can be seen that the angle of the reflected light incident on the top surface The above formula. Specifically, 'can be calculated based on the shape of the first intermediate layer. The optical path of the light from the surface can be obtained. Its range is that before the direct light reaches the conical surface EV, so that it does not exceed the critical angle 0e = sin (i / n), that is, 7 < 0C, and the conical surface The maximum wide-angle (0 = 90) of the reflected light on the surface must not exceed the critical angle, so: [Formula 7]-Jiu < 2 Bu Fen, ^ -γ < τ7 If n = 1.6 then 25.66. ≪ 77 & lt 38.68., But when η = 2.2, 0c = 27.〇4. And (7Γ / 4)-(0C / 2) = 31.48. 'Cannot determine the optimal taper angle. Therefore, by using The central part of the taper is filled with a resin with a refractive index of about 1.6, which can guide the light to the outside. If the angle of the light is too close to the critical angle, the light transmission rate is not high. For practical results, set the angle at (25.66+ 38.68) / 2 = 32.17. About, < make both the direct reflected light and the reflected light within a range slightly smaller than the critical angle. Then find the thickness of the substrate that can produce a favorable amount of light transmission. Suppose the lower side of the pixel is -40-This paper size applies Chinese National Standard (CNS) A4 specification (210 X 297 mm) 550964 A7 ----B7 V. Description of the invention (38) The surface is straight, the second is a, and the thickness of the substrate Is d, the radius of the upper transparent surface is a / 2 + d tan 77. If the light on the lower side is 100% transparent, the amount of light emitted by a simple pixel (assuming transmission efficiency τ) the same as that on the upper side, is equal to the amount of light on the lower side: [Formula 8] Yes "忐 (1 ++ ... (5: assuming τ = 0.2, fuo _, ..., then d = 3〇" m.) In this way, the thickness d will be thinner and can produce a favorable amount of light transmission. On the contrary, the above If the size of the side is 120 #m, then a = 107 and d = 105. It can be seen from this that once the 'pixel size a' is determined, the angle 工 can be determined by the aforementioned working formula 々 and an effective substrate The thickness 4 can be determined by the aforementioned formula (5). If the substrate thickness is larger than this data, it will not be able to make the pixel's light emission fully transparent to the outside, which is not necessarily beneficial. Figure 12 shows the structure of the element using the first intermediate layer. For example, the first intermediate layer has this optimal thickness. Figure 12 (a) shows the case where the first intermediate layer is directly bonded to the lower part of the pixel. The thickness of the first intermediate layer is much thinner than the overall thickness of the substrate. In this configuration, the effect is not good because the light is diffused before finally reaching the light-transmitting interface ⑻ Shows that the overall thickness of the substrate is the same as the thickness of the first intermediate layer. In this case, 'Although the advantages of the aforementioned light transmission can be obtained, the thickness of the substrate is thin. Therefore, in order to maintain the mechanical strength of the substrate, it can be shown in Figure I " Magic show -41-This paper size applies the Chinese National Standard (CNS) A4 specification (210 X 297 mm) 550964 A7 ________B7 5. Description of the invention (39) " Between the pixel and the first intermediate layer, The substrate is separated by a certain distance dw. In this case, before the light from the pixel reaches the first intermediate layer, in order to avoid mixing with the light from adjacent pixels, the value of # above must not be too large. Figure 13 shows a component structure, which is Under the condition that the first intermediate layer is isolated from the pixel, a waveguide layer connecting the two is formed in the substrate. At this time, it can be divided into two cases: one is shown in Figure n (a). The wave layer joins the direct pixel portion with the first intermediate layer; the second is shown in Figure 13 (b), where the wave guide layer joins the first intermediate layer at a distance dw. Especially in the latter case, when the light passes from Before the pixels reach the first intermediate layer, To avoid mixing with the light from adjacent pixels, the value of the above dw must not be too large. As mentioned above, in the organic electric field light-emitting element, the cross-sectional shape of the first intermediate layer is a shape in which the opening portion expands from the light emitting surface end to the light transmitting surface end And the side surface of the first intermediate layer can reflect light, and in the light-transmitting surface of the first intermediate layer, the angle of the tapered inclination of the side surface of the intermediate layer to the total reflection angle is less than 0 c. Especially when When the element structure is designed to be 77 at 45.-0e / 2 or more and 0. or less, and the thickness d of the first intermediate layer in the same section with respect to the width a of the light-emitting surface end opening a is less than a / 2 tan 7? Almost all the light generated in the pixel portion can be maintained within the pixel size limit of the display element and can be transmitted to the outside of the element. [Embodiment 5] This embodiment uses FIG. 14 to describe an element structure of an image display element for an amorphous silicon thin film transistor or a polycrystalline silicon thin film transistor, or an organic thin film transistor, and the like on a substrate. And driving circuit. -42-This paper size is in accordance with Chinese National Standard (CNS) A4 specification (21〇X 297 public love) 550964 A7 -----__________ B7 V. Description of the invention (4〇) When the organic electric field light emitting element is displayed as an image It is necessary to control the light emitting state of each pixel by using the device. When the screen size increases, an effective method is to form a thin film transistor that can drive each pixel independently in each pixel inside the cow. Figure M⑷ shows the structure of a single pixel section with this thin film transistor built in. A thin film transistor layer is formed on the top surface opposite to the light-transmitting surface of the substrate, and is driven by two transistors (Tsw: Switching Transistor, Swifching Transistor; ydr: Non-polar Transistor, Ding Caoru) One pixel is formed on the thin film transistor layer to form a transparent anode, a light emitting layer and a cathode of an organic electric field light emitting element. Part of the transparent anode and part of the cathode are connected to the transistor through wiring. The first intermediate layer is formed under the light-emitting layer, and the structure can adopt various structures shown in the fourth embodiment. 14 is a circuit diagram of a transistor for driving each pixel, and gate wirings for driving a switching transistor are formed between each pixel < and G4), and a drain for driving a drain transistor Wiring (di ~ d4). In order to make a special pixel display, select from these two kinds of wiring, and drive the transistor at a specific pixel position to make the light emitting part emit light. The emitted light is introduced into the first intermediate layer formed under the built-in transistor layer, where the optical path is diffused and reaches the light-transmitting interface. In an image reading display device including such a thin-film transistor built-in organic electric field light-emitting layer, in order to coexist the transistor part and the wiring part outside the light-emitting pixel part, a non-light-emitting area must be included, but by The first type—the tapered part of the middle layer—configures these drive circuits to make the components more precise. The organic electric field light emitting device of the present invention does not need to change the basic structure of the light emitting part of the organic electric field light emitting device disclosed in many previous researches, but can improve the light transmission efficiency in a simpler way and allow more light to penetrate to the outside of the device. In particular, when a large-screen display element of more than ten inches and an image display element with a small area but a high degree of precision are used as the driving element, due to the inherent problems when using organic materials, it cannot be used as a high precision. The use of image display elements, the previous proposal only provides up to eight inches of image display elements. Among such high-precision devices and large-screen devices, organic electric field light-emitting devices can also be used. With the improvement of the electrical characteristics of these devices, it is expected that the device drive will achieve lower voltage, higher brightness, and longer life. Possibility of industrial utilization Using the present invention, an organic electric field light-emitting element that is thin and light, high precision and high efficiency can be manufactured, and the organic electric field light-emitting element using the present invention can provide various new types of photovoltaic elements, and use System and services of these components, such as: thin film flat panel display, small mobile projection display, mobile phone display element, stereo display, electronic paper, mobile computer display TF device, real-time electronic bulletin board, light emitting diode, Laser, two-dimensional light pattern generating element, optical computer, optical cross connector (CrOss Connector), and optical router. -44 · This paper size applies to China National Standard (CNS) A4 (21 × 297 mm)

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Claims (1)

A8 B8 C8 D8 Patent Application No. 091101580 Chinese Application for Patent Scope Replacement (July 1992) 々, Application for Patent Scope 1. An organic electric field light-emitting element, which can be used for the injection and transmission of positive and negative charges. A person who emits light by recombination with positive holes and electrons generated by the positive and negative charges; it has a light-emitting layer, and the light-emitting layer contains a light-emitting substance, which is formed by recombination in the organic electric field light-emitting element. Generated; or contains a fluorescent substance, which can emit light twice after receiving light from the luminescent substance; characterized by having a first intermediate layer, which is located outside the light-emitting layer and emits light to the organic electric field Between the light-transmitting interfaces that are externally transparent, and the azimuth distribution of the light intensity transmitted from the aforementioned light-emitting layer is enlarged after passing through the first intermediate layer. 2. For the organic electric field light-emitting device according to the scope of the patent application, the first intermediate layer can perform light scattering or optical path diffusion. 3 · For the organic electric field light-emitting element according to the scope of the patent application, wherein the first intermediate layer is separated one by one according to pixels having a specific shape, or the pixels are separated one by one by a partition wall, the partition wall contains properties different from the intermediate layer. Of matter. 4. For an organic electric field light-emitting device according to item 3 of the patent application, wherein the first intermediate layer is separated one by one according to the pixels adjacent to the light-transmitting interface, and the shape or the shape of the partition wall is a polygonal shape and has multiple shapes. Of the angular shaped surfaces, at least two surfaces are parallel. 5. For the organic electric field light-emitting device according to item 4 of the scope of patent application, at least one of the parallel-opposite shaped surfaces having a polygonal shape is 0.25 to 2 times as long as the light-emitting wavelength. 6. The organic electric field light-emitting element according to item 3 of the patent application scope, in which the first O: \ 76 \ 76355-920710DOC \ 5 ^ Zhang scale suitable for financial _ home standard (CN ^ 74 specifications (21G x