TWI295901B - Electroluminescent device - Google Patents

Description

Α7 Β7 Ministry of Economic Affairs, Department of Consumers, Cooperatives, Printing and Intellectual Property Bureau 1295901 V. Description of the Invention (The present invention relates to a novel organic light-emitting 1 electro-electric device having a novel hole-transferring layer between a hole-generating electrode and an organic light-emitting device These devices are highly efficient, easy to manufacture, and inexpensive. In recent years, there has been great interest in luminescent organic materials such as light-weight polymers. Luminescent polymers have non-limiting redundant electronic systems along the polymer backbone. Non-limiting 7Γ The electronic system imparts semiconductivity to the polymer, allowing the polymer to support positive and negative charge carriers and is highly mobile along the polymer chain. Conjugated polymer films can be used to make optical devices such as light-emitting devices. Advantages over devices using conventional semiconducting materials, including wide field display, low DC operating voltage, and ease of fabrication. Devices of this type are described, for example, in WO-A-90/13148, UW 5,512,654 and WO- A-95/06400. The global market for display devices based on organic and polymer luminescent materials has recently been estimated by Stanford Resources to 22.2 years. 200 million yuan, the growth rate has quickly contributed to the high interest and attention of the industry in this field (d r. Mentley, "Flat Information Display Devices: Market and Technology Trends", 9th Edition, 1998). It can meet commercial needs and consume electricity. Low effective and stable lEd devices have been manufactured by Xusun and academic research groups (for example, reference rh.

Friend et al., Nature 1999, 397, 12). Currently working on a full color full plastic screen. The main challenges to achieve this project are: (1) access to conjugated polymers of luminescent three primary colors of light red, green and blue; and (2) conjugated polymers must be easily processed to produce full color display. Organic electroluminescent devices such as polymer LEDs (PLEDs) can achieve luminescent color by changing the chemical structure of the organic luminescent compound (please read the back of the note first and then fill out this page)

4 1295901 A7 B7 V. Invention description () ~ 2 Control. However, the regulation of the chemical properties of the luminescent layer is true: the size of the laboratory is often easy and inexpensive, but becomes an expensive and complicated process at the industrial scale. The second requirement for easy handling and stacking of full-color matrix devices creates the following problems, how to micro-pattern small and colorful pixels, and how to achieve full-color lighting. Inkjet printing and hybrid inkjet printing technologies have recently gained a lot of attention for patterned PLED devices (eg, RF Service, Science 1998, 73, 2561; J. Bharathan, Y. Yang, Applied Physics Letters 1998, 72, 2660; tR Hebner, CC Wu, D. Marcy, ML Lu, J. Sturm, Applied Physics Letters 1998, 72, 519). In terms of the most basic structure, an organic electroluminescent device usually comprises an organic light-emitting material disposed between a hole injecting electrode and an electron injecting electrode. The hole injection electrode (anode) is typically a transparent tin-doped indium oxide (ITO) coated glass substrate. The material commonly used for electron injection electrodes (cathodes) is a low work function metal such as #5 or Ming. Ministry of Economic Affairs: The Intellectual Property Bureau of the Yimeng Bureau employee consumption cooperatives (please read the notes on the back and fill out this page) Materials commonly used in organic light-emitting layers include conjugated polymers such as polyphenylene-ethylene (PPV) and Its derivatives (for example, refer to WO-A-90/13148), polydiene derivatives (for example, reference AW Grice, DdC Bradley, Μ·Τ·Bernius, Μ·Inbasekaran, WW Wu, and Ε·Ρ·Woo, applications Physical Letters 1998, 73, 629, WO-A-pp/55927 and Bernius et al., Advanced Materials, Vol. 12, No. 23, 1737, 2000), poly-naphthene derivatives and polyphenene derivatives; and small organic molecules such as Aluminum quinolol complex (Alq3 complex: for example, see US-A-4,539,507) and acridone, redene and styrene dyes (for example, refer to JP-A-264692/1988). The organic light-emitting layer may comprise a mixture or a separate layer of two or more different light-emitting organic materials. This paper scale applies to China National Standard (CNS) A4 specification (210X297 mm) '' : Ministry of Economic Affairs, Department of Consumers, Cooperatives, Printed Intellectual Property Bureau, 1295901 at Β7 V. Inventions () - 3 Typical device architecture, for example, reveals WO-A-90/13148; US-A_5,512,654; WO-A-95/06400; RF Service, Science 1998, 279, 1135; Wudl et al., Applied Physics Letters 1998, 73, 2561; Bharathan, Y. Yang , Applied Physics Letters 1998, 72, 2660; 1\11· Hebner, CC Wu, D. Marcy, ML Lu, J. Sturm, Applied Physics Letters 1998, 72, 519); and WO 99/48160; The way is incorporated here. From the hole injection layer, such as the ITO injection hole to the organic light-emitting layer, the energy difference between the work function of the hole injection layer and the highest occupied molecular structure of the luminescent material (HOMO), and the interface chemistry between the hole injection layer and the luminescent layer Control of the role of care. The high work function organic material is deposited on the hole injection layer, such as poly(styrene sulfonate)-doped poly(3,4-extended ethyldioxythiophene) (PEDOT/PSS), N,N,-diphenyl -N,N,-(2-naphthyl)-(1,1,-phenyl)-4,4'-diamine (NBP) and hydrazine, Ν'-贰 (3-methylphenylbiphenyl- 4,4'-Diamine (TPD) provides a "hole transport" layer that facilitates the injection of holes into the luminescent layer. 'The hole is injected into the electrode to stabilize the transport hole and block the electrons. These layers can be added and introduced. The number of holes in the luminescent layer. However, the boundary between the surface of the ruthenium is poor, and the interface chemistry between the conventional hole transport materials is difficult to control. As for the high work function organic materials such as PEDOT/PSS, a high-resistance inorganic layer has been proposed. The hole transport layer is, for example, referred to as ΕΡ-Α-1009045, ΕΡ-Α-1022789, ΕΡ-Α-1030539, and ΕΡ-Α-1041654. ΕΡ-Α-1022789 discloses an inorganic hole that blocks electrons and has a hole conduction path. Transport layer. This layer has a high electrical resistance and is said to be better than the 103 to 108 ohm-cm zone. The disclosed materials have the general purpose of this paper scale applicable to Chinese national standards ( CNS ) Α4 Specifications (210, 乂297 mm) ' ' :― -6 - (Please read the notes on the back and fill out this page)

41295901 A7 B7 Economic Department's mouth ^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^ The difficulty is not clearly defined and may vary with the actual size of 1 and y. EP-A-1083776 and EP-A-1111967 disclose an EL device having an inorganic hole transport layer comprising a metal chalcogenide and a periodic table 5 A combination of inorganic compounds of Groups 8 to 8. It is important that the two component systems are used to provide the desired effect of adjusting the number of difficulties, but it has not been suspected that the metal chalcogenide must be a layered metal chalcogenide. US-A- 6023128 discloses an EL device having a hole transport layer 'the hole transport layer comprising a matrix in which a transition metal chalcogenide cluster' is stabilized by an organic ligand shell. The regulation of electronic properties can be quantum through clustering. The size effect is achieved. It has not been revealed that a single continuous layer of layered metal chalcogen is used as the hole transport layer. However, there is still a need for a hole transport material that is superior to such prior art materials, particularly materials that are chemically inert to the interface with the organic light-emitting layer. , And the material has a simple and low-cost manufacturing device, and the device has excellent power supply efficiency, low driving voltage, high light-emitting degree, etc. Therefore, the object of the present invention is to provide an electroluminescent device which combines novel inorganic electroporation The electroluminescent device has excellent properties in terms of ease of manufacture and performance. Thus, in a first aspect of the invention, an electroluminescent device comprising a hole injecting electrode, an electron injecting electrode, and at least one An organic light-emitting layer is disposed between the hole injection electrode and the electron injection electrode, wherein a layered metal chalcogenide layer is sold between the injection electrode and the light-emitting layer, and the chalcogen component of the chalcogenide is selected from the group consisting of Sulfur, selenium and tellurium. Layered metal chalcogenides are well known compounds (eg, n.-n !.. ' I - I- . , Γ n (please read the notes on the back) )

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1295901 A7 A7 ---- V. INSTRUCTIONS (5) Physico-chemical and chemistry with layered structural materials, published by D Reidei/Dorway, Boston, USA), including metal oxides selected from sulfur, Any of various compounds in which the atom of the genus genus is a layered structure. For example, it includes a layered metal dichalcogenide and a layered large metal-chalcogenide. The layered metal disulfide compound has the chemical formula MX2' wherein M represents a metal and ruthenium represents sulphur, habitat or ruthenium. The layered metal dichalcogenide structure preferably comprises a metal atom sandwiched between two chalcogen atoms. Among the layered metal dichalcogenides, the metal component is preferably selected from transition metals such as titanium, erbium, ruthenium, osmium, iridium, iridium, and non-transition metals such as tin. More preferably, it is group H, tin and crane and is preferably bismuth, molybdenum and button. More preferred sulfur is sulfur and selenium. The metals forming a chalcogenide include gallium, indium and antimony. through

In detail, the layered metal chalcogenide has several properties that make it particularly suitable for use as a hole transport layer. The layered metal dichalcogenide is chemically inert and contains no pendant bonds, thus overcoming the chemical interactions encountered between the prior art hole transport layer and the interface between the organic light-emitting layer and the anode. The layered metal chalcogenide has a high work function and is easy to transport holes from the metalloid layer to the organic light-emitting layer. In addition, it is possible to obtain a film using a chemical method which is simple and inexpensive. The metal chalcogenide structure comprises a metal atomic sheet sandwiched between the chalcogenogen sheets. For example, in a layered metal dichalcogenide, the metal sheet is covalently bonded to two adjacent chalcogenide sheets. The two adjacent Μχ2 layers are maintained by the combination of Van der Valli. Such structural results result in mechanical, chemical and electrical properties with extreme anisotropy. The exposed side of the material does not have a side dangling bond and is therefore chemically inert. So that it is particularly suitable for use as an electroluminescent device

1295901 A7 B7 V. INTRODUCTION OF THE INVENTION (The hole transport layer is due to the fact that this structure eliminates the interface between the hole injection layer (such as IT0) and the luminescent layer (such as PPV) due to the reduced efficiency and effective service life of the prior art device. The problem of chemical reaction occurs. The layered metal chalcogenide has a high work function in the range of 4-6.5 electron volts (ev), especially 5-6.5 eV, such as bismuth selenide, molybdenum disulfide, tin sulphide, The work functions of disulfide knob, vanadium diselide, indium selenide and gallium selenide are 5.9, 4.8, 5.2, 5.2, 5.6, 4.55 and 5.8 eV, respectively. [Measurement by photon emission technology] revealed in T· Shimada, FS Ohuchi And BA Parkinson, Japanese Journal of Applied Physics 33, 2696 (1994). The work function of these materials makes them particularly suitable for use as a hole transport layer, because the value of these work functions is close to the free potential of the organic light-emitting layer. It facilitates the transport of holes to the luminescent layer. The high work function, reasonable conductivity, and the inertness of the exposed surface of the layered metal chalcogenide greatly contribute to the injection of the holes into the electrode of the electroluminescent device of the present invention. example ITO) is injected into the luminescent layer, thus making the electroluminescent device particularly effective. Printed by the T-Commerce Consumer Cooperative of the Ministry of Economic Affairs, the Property Bureau (please read the notes on the back and fill in this page) The electronic properties of the layered metal chalcogenide can be There are wide variations, from insulators to semiconductors and semi-metals to true metals. The resistivity of layered metal chalcogenides is very low for sulfur disulfide and disulfide knobs, for example about 4 乂 10 _ ohm-cm (Ω-cm The high value of bismuth disulfide is, for example, 1 〇 ohm_cm. As described above, the disclosure of the prior inorganic hole transport layer, for example, as disclosed in EP-A-1022789, teaches that the preferred resistivity is lxl 〇 3-lxl 〇 8 ohm - Cm. The low resistivity of several layered metal chalcogenides results in a decrease in the driving voltage requirement of the device of the invention. The layered metal dichalcogenide structure comprises a piece of hexahedral plug metal 9 1295901 V. Description of the invention The material clip is placed between two hexahedral sulfur atoms. The metal atom is a hexahedron (for example, titanium disulfide and disulfide) or a trihedral prism (for example, disulfide and disulfide). ) β MX The second layer borrows the van der Waals force to maintain the bond in, and there are several kinds of stacked multi-dragons (refer to the weak bond between the layers of Figure 1b, where the layer-μ layer of metal atom single layer is covalently bonded by the ς 包In the composition, weak bonding results in extremely anisotropic mechanical and electrical properties. For example, the conductivity of the vertical plane is at least 1〇2 lower than the disulfide turning plane [Refer to JA View _ and AD·Y〇ffe, Advanced Physics 18 193 (1969)] The layered metal-chalcogenide structure consists of two hexahedral packed metal atom sheets sandwiched between two hexahedral sulfur atomic sheets in a χ_Μ_Μ sequence. In the di-compound, the cation preference is that the bond of the tetrahedral valence layer is a covalent bond. Metal/metal bonding is responsible for producing the electrical conductivity of such materials. Each layer maintains a bond with Van der Valli and there are several piles of polymorphism. Layer (4) weak bonding results in extremely anisotropic machinery and electrical properties. The metal atom's valence and oxidation state determine the electronic properties of the material. For example, group V metal atoms (铌 and titanium) are trigonal prismatic valences, corresponding to disulfide materials are metals; group VI atoms (molybdenum and cranes) are also trihedral prisms, but with complete dz bands, so For the semiconductor. Molybdenum disulfide has a hexahedral dihedral prismatic coordinate, which is metal or semiconducting, respectively. The metallic metal chalcogenide absorption spectrum shows that the material absorbs the external light and visible light regions. However, a trihedral prismatic material film such as bismuth selenide free carrier absorbs less than 1 eV and is separated from the direct absorption edge by more than 2 eV.

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X semi-stacked and red paper size applicable to the Central Standard (CNS) A4 specification (21GX297 mm)

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, 1T 铧. Ministry of Economic Affairs, the central government ^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^^ Therefore, the luminescence absorption of the layered metal chalcogenide can be minimized by treating the extremely thin film of the layered metal chalcogenide. Thus, although the layer thickness is not particularly limited, the layered metal chalcogenide hole transport layer preferably has a thickness of 3 to 20 nm, more preferably 3 to 10 nm, and most preferably 3 to 7 nm. Thicker films, while still effective, may absorb more than 20% of the emitted light, thus reducing the emission of light. The preferred layered metal chalcogenide is the only hole transport material. In addition, it is understood that the layered metal chalcogenide hole transport layer forms a single continuous sheet at the hole injection electrode, with reference to the cluster suspended in the matrix disclosed in US-A-6,023,128. If the emitter is annealed at a temperature of at least 10 ° C (eg, 250 ° C) before the emissive layer is deposited on the layered metal chalcogenide hole transport layer, then in some cases a particularly good property is obtained because The ordering of several layered metal chalcogenide material films can be improved, thereby improving the electrical conductivity. The luminescent layer can comprise one or more organic luminescent materials. If there is more than one organic luminescent material, it may be provided as a separate layer or as a single layer. Any two organic luminescent materials can be used for the luminescent layer. Suitable examples include: conjugates such as poly-phenylene-ethylene (PPV) and its derivatives (for example, see WO-A-90/13148), polydecene derivatives (for example, reference AW· Grice, DDC Bradley, Μ·Τ· Bernius, M. Inbasekaran, WW Wu, and Ε·Ρ·Woo, Applied Physics Letters 1998, 73, 629, WO-A-OO/55927 and Bernius et al., Advanced Materials, 2000, Vol. 12, No. 23 1737 pages), poly-naphthene derivatives, polyfluorene-deuterium derivatives and polyphenanthrenyl derivatives; and small organic molecules such as σ quinolol complex (Alq3 complex: This paper scale applies to Chinese national standards (CNS) A4 size (21〇X297 mm) (Please read the note on the back and fill out this page)

, 1T ·· 11 1295901 A7 B7 V. Description of the invention () A 9 for example, see US-A-4,539,507), transition metal ruthenium complexes, lanthanides with organic ligands and actinides such as TMHD ( Reference is made to WO-A-00/26323) as well as acridone, redene and styrenic dyes (for example, see 抒-八-264692/1988); the contents of each of which are incorporated herein by reference. Specific examples of preferred luminescent polymer materials include polymers comprising conjugate units of the following formulae (VIII), (IX), (X), (XI), (XII), (XIII), (XIV) and (XV). These polymers may be homopolymers or contain two or more different conjugate units, such as alternating AB copolymers and terpolymers; and statistical copolymers and terpolymers. (Please read the notes on the back and fill out this page.) Printed by the Ministry of Economic Affairs, T-Commerce Consumer Cooperatives

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This paper scale applies to the Chinese National Standard (CNS) A4 specification (210X297 mm) 12 !2959〇1 A7

R8 to R15 and r17 to R33 are the same or different and are selected from the group consisting of alkyl groups as defined below, alkyl groups as defined below, alkoxy groups as defined below, as defined below An alkoxyalkyl group, an aryl group as defined below, an aryloxy group as defined below, an aryl group as defined below, and a formula _c〇r group, wherein R16 is selected from the group consisting of: hydroxy, as follows An alkyl group; a haloalkyl group as defined below, an alkoxy group as defined below, an alkoxyalkyl group as defined below, an aryl group as defined below, an aryloxy group as defined below, an aralkyl group as defined below, an amine group, an alkyl group The alkyl group of the amine group is defined as the latter alkylamino group wherein each alkyl moiety is the same or different and is defined as a post-aralkyloxy group, the aralkyl moiety of which is defined as follows, and the haloalkoxy group comprises as defined The alkoxy group is substituted with at least one deuterium atom, or if r or s is an integer of 2, the R32 or R33 diradical, together with the ring carbon atom to which it is attached, form a heterocyclic group containing 5 to 7 ring atoms, A plurality of ring atoms are heteroatoms composed of nitrogen, oxygen and sulfur atoms, and are defined as follows: The paper scale applies to the Chinese National Standard (CNS) A4 specification (210χ297 mm) 13 1295901 A7 B7 V. Description of invention (11 Z1, Z2 and Z3 are the same or different and are selected *self, s, s〇, 、, NR3, Nf'XR; ''), C(r4)(r5), Si(R4;)(R5,) and the resulting group 'where R, R3, and r3' are the same or different and each is selected A group consisting of the following groups: a hydrogen atom, a dentate group as defined below, an alkoxy group as defined below, an alkoxy group as defined below, a oxyalkyl group as defined below, an aryl group as defined below a aryl group, as defined below, and a decyl group, as defined below, substituted with at least one group of the formula _n+(r7)3, wherein each R7 group is the same or different and is selected from a gas atom, as defined below a group consisting of an alkyl group and an aryl group as defined below, r4, r5, fluorene, and r5, which are the same or different and each selected from a hydrogen atom, a halogen group as defined below, as defined below Alkoxy, a southern atom nitro, an aryl group, an alkoxyalkyl group as defined below, an aryl group as defined below, an aryloxy group as defined below, and a *T definition a group consisting of a technical group, or r4&r5 together with a carbon atom to which it is attached, represents a group, and r6 is selected from a hydrogen atom, an alkyl group as defined below, a haloalkyl group as defined below, an alkoxylated alkane as defined below a group of aryl groups, an aryloxy group as defined below, and an arylalkyl group as defined below; the oxime bureaux consumer cooperatives X, X, X and X4 are each identical or different and are selected from the group consisting of An aromatic aryl group having one or more rings containing from 6 to 14 carbon atoms which may optionally be substituted with a substituent of at least one group selected from the group consisting of nitro, A cyano group, an amino group, an alkyl group as defined below, a dentate alkyl group as defined below, an alkoxyalkyl group as defined below, an aryloxy group as defined below, and an alkoxy group as defined below; containing 1 to 6 carbon atoms Straight or branched chain alkyl; This paper scale applies to Chinese National Standard (CNS) A4 specification (2丨〇'乂297 public shame) 12 1295901 V. Description of invention (linear or branched with 2 to 6 carbon atoms) a chain extending alkenyl; and a straight or branched chain extending from 1 to 6 carbon atoms Group; or X and X3 and / or X4 and X2 together represent the formula of the linking group.丫 丫. (V) wherein X5 represents an aryl group which is an aromatic hydrocarbon group having one or more rings having 6 to 14 carbon atoms, which may optionally be substituted with a substituent of at least one group selected from the group consisting of: Nitro, cyano, amine, alkyl as defined below, alkyl as defined below, alkoxyalkyl as defined below, aryloxy as defined below, and alkoxy as defined below; el, e2, fl And f2 are each the same or different and are 〇 or an integer from 1 to 3; g, ql, q2, q3 and q4 are each the same or different and are 〇, 丨 or 2; Μ, h2, 'jl, j2 J3, 11, 12, 13, 14 are each the same or different and are 0 or an integer from 1 to 4; 1. kl, k2, 〇1 and 〇2 are each the same or different and are 〇 or 1 to 5 And pl, p2, p3 and p4 each being 0 or 1; the aforementioned alkyl group is a linear or branched alkyl group having 1 to 20 carbon atoms; the aforementioned haloalkyl group is an alkyl group as defined above Replace with at least one halogen atom; This paper scale applies to Chinese National Standard (CNS) A4 specification (210X297 mm I丨丨-----丨#~ (please read the notes on the back and fill in the form) ] Order 15--

5. Description of the Invention (13 1295901) The alkoxy group is a straight or branched alkoxy group having 1 to 20 carbon atoms; the alkoxyalkyl group is an alkyl group as defined above which has at least one alkane as defined above An oxy group; and the aryl group of the foregoing aryl group and the aforementioned aralkyl group (the alkyl moiety has 1 to 2 carbon atoms) and the aryloxy group are aromatic having 6 to 14 carbon atoms in one or more rings. a hydrocarbyl group which may optionally be substituted with a substituent of at least one group selected from the group consisting of nitro, cyano, amine ', alkyl as defined above, haloalkyl as defined above, as defined above Alkoxyalkyl, and alkoxy as defined above. Particularly preferred luminescent polymers include homopolymers, copolymers and terpolymers comprising formula (VIII), (IX), (X), (XIV), And (xv) groups, for example, including PPV, poly(2-methoxy-5-(2'-ethyl)hexyloxyphenylene-ethylene) ("MEH-PPV"), PPV derivatives such as Dialoxane and dialkyl derivatives, poly derivatives and related copolymers; and the best polymers include PPV, MEH-PPV, poly(2,7-(9,9-) Di-n-hexyl fluorene)), poly(2,7-(9,9-di-n-octyl)), poly'(2,7-(9,9-di-n-octyl)-( ι,4-phenylphenyl 't-butylphenyl)imido)-1,4-phenylene)) ("TFB"), and poly(2,7-(9,9-di-positive) Octyl)-3,6-benzothiadiazole) ("F8BT"). The best luminescent organic molecules include Alq3 complexes. The thickness of the light-emitting layer is not particularly limited. The precise thickness of the layer will vary depending on a number of factors such as the luminescent layer material and other component materials of the device. However, typically the thickness of the luminescent layer (combined thickness if there is more than one layer) is 1 to 250 nm, preferably 50 to 120 nm and better 70 to 1 Å nanometer and the most paper size is applicable to the Chinese country. Standard (CNS) M specification (21〇χ297 mm) (Please read the notes on the back and fill out this page again) d

1T Ministry of Economic Affairs tp workers consumption combined with the company's printed intellectual property bureau 16 Ministry of Economic Affairs printed by the Bureau of Staff and Consumers Cooperatives Intellectual Property Office 1295901 at B7 V. Invention Description () A 14 good 75 to 85 nm. * The organic light-emitting layer can be deposited on the layered metal chalcogenide hole transport layer using any method suitable for depositing such an organic layer. Since the layered metal chalcogenide is insoluble in the organic solvent, it is particularly spin-coated from the organic light-emitting material solution. It is suitable for use in this project (for example, refer to WO-A-90/13148). The electroluminescent device of the present invention typically has a substrate (e.g., glass), a hole injecting electrode (e.g., ITO), a layered metal chalcogenide hole transport layer, an organic light emitting layer (e.g., polyfluorene), and an electron injecting electrode (e.g., Stack configuration of Ca/Al). In addition, the device has a reverse stacking configuration of a substrate, an electron injecting electrode, an organic light emitting layer, a layered metal chalcogenide hole transport layer, and a hole injecting electrode. Any suitable technique known in the art can be used to deposit a layered metal chalcogenide hole transport layer at the anode. However, since the ultrathin film can be deposited on the anode at a low cost, it is preferable to use a chemical route. The chemical method for properly depositing layered metal dichalcogenides at the anode is based on methods developed by Frindt et al. [Ref. P. Joensen, RF Frindt and SR Morrisoii, Materials Research Bulletin 21, 457 (1986) and U.S. Patent 4,996,108] . This method involves the following steps: (a) insertion of a lithium atom into the MX2 compound; (b) addition of water to the intercalation material, resulting in the reduction of water by the lithium atom. As a result of the MX2 layer, the resulting hydrogen collapses in each layer stack (off-layer), resulting in a single layer of MX2 suspended in water; (c) adding a water-immiscible solvent to the MX2 monolayer aqueous suspension, followed by agitation of the resulting mixture, Manufacture of MX2 film, which is formed on the solvent/water boundary of this paper. It is applicable to China National Standard (CNS) Α4 specification (210><297 mm) (please read the note on the back and fill out this page)

1T altar 17 A7 B7 1295901 V. Inventive Note () 15 face; and (d) Soaking the lower end of the wet ITO coated glass substrate at the solvent/water interface, resulting in the MX2 film unfolding into a thin oriented film on the surface of I το. MX: The film is oriented with the c-axis perpendicular to the ITO coated substrate. The layered metal chalcogenide hole transport layer provides a hole conduction path created by the excellent hole injection electrode. The layered metal chalcogenide of a plurality of semiconducting materials also blocks electrons escaping from the luminescent organic layer to some extent, thus assisting in balancing the electron flow and the hole flow of the luminescent layer, as well as enhancing its capture. However, the resistance of the electron Sb can be wrong. The material can be greatly enhanced. The material can restrict the migration of electrons from the light-emitting layer and the layer of the material is deposited on the inorganic layered metal chalcogenide hole transport layer and the organic light-emitting layer. Between layers.

In a preferred embodiment of the apparatus of the present invention, a layer of material is provided between the organic light-emitting layer and the layered metal chalcogenide hole transport layer, the layer material constraining the migration of electrons emitted by the organic light-emitting layer to Layered metal chalcogenide hole transport layer. Such materials are, for example, materials known in the prior art to constrain electron migration from organic light-emitting layers, such as oxides of metals and metalloids, carbon compounds, nitrides, tellurides, and borides, which are disclosed in EP-A. -10227 § 9 and EP-A-1041654, for example, the general formula (Sii xGex) 〇 y where OSxS 1 and 1.7 SyS 2.2. However, it is particularly preferred that the thin layer of material for constraining electron transport is an oxide of the same metal of the metal chalcogenide layer. Metal oxides are highly effective electron blockers. Further, the deposition of the metal oxide layer is extremely simple, and after the layered metal chalcogenide layer is deposited on the hole injection layer, it is formed via the exposed surface of the oxide layered metal chalcogenide layer. Metal oxides can be stoichiometric

-18 1295901 A7 B7 V. INSTRUCTIONS (• JIANGXI PRINT 16 Non-stoichiometric quantities; the actual composition of the oxide layer will vary depending on the oxidizing conditions used to make this layer. In addition, the polymer solution wets the metal oxide layer much better than The layered metal chalcogenide layer results in fewer pinholes and lower leakage current (ie, higher efficiency). It is preferred to combine metal oxides (MOs) on the layered metal chalcogenide (LMC) layer. The electroluminescent device has the following typical structure: glass/ITO/LMC/MO/organic light-emitting layer/Ca/Al. Such device has low manufacturing cost, low operating voltage and high efficiency. Method for depositing electron blocking metal oxide film Including a variety of physical and chemical film formation methods such as sputtering and evaporation. Oxygen plasma generator oxide layered metal chalcogenide layer is particularly good. Typical oxidation is based on RF oxygen plasma generator at 0.3-0.5 mbar Oxygen pressure and 250 watts. The thickness of the oxide film is controlled by the length of the treatment time. The preferred thickness of the metal oxide film is determined by the nature of the device, and there is no special limit on the effect of the device. However, a particularly effective electron-hole balance can be achieved in a device comprising a 1-10 nm metal oxide film; a metal oxide film having a thickness of 2 to 6 nm is preferred; and a thickness of 2-3 nm is used. The metal oxide film is optimal. The film having a thickness smaller than that of 丨 nanometer has a reduced effect on the electron resistance, and in the film having a thickness of more than 4 nm, in some cases, the injection of the hole into the organic light-emitting layer is ineffective. Determined according to the relevant LMC/MO material and generator settings. %, in an apparatus comprising an electron blocking film such as an oxide of a layered metal chalcogenide layer, the organic light-emitting layer is deposited on the electron blocking thin: layer. Because of the layered metal chalcogenide layer and the metal oxide layer, the organic light-emitting layer can be coated by solution 2 (cNs) by a simple and low-cost procedure (A): A4im\ 2i〇xl^jy

(Please read the note on the back and fill out this page) 19 1295901 A7 B7 V. INSTRUCTIONS (17 deposited on the inorganic layer. * In some devices, the 'electron transport' layer is also placed between the electron injection layer and the light-emitting layer ( Suitable compounds, for example, include alkali metals, earth-suppressing metals and lanthanide oxides having a work function of up to 4 eV, as disclosed, for example, in EP-A-1009045. This compound assists electron injection into the luminescent layer and stably transports electrons from the electron-injecting layer. And blocking the holes. These layers can effectively increase the number of electrons entering the luminescent layer. Particularly preferred are cerium oxide, magnesium oxide, calcium oxide, lithium oxide, oxide I, potassium oxide, sodium oxide and oxidized planing. The thickness is determined according to the material it contains, and the typical thickness is from 1 to 2 nm and preferably from 0.3 to 0.8 nm. The substrate on which the organic electroluminescent device of the present invention can be formed can be any of the typical ones used in this type. The substrate of the device includes, for example, a crystal substrate of glass, quartz, and Si, GaAs 'ZnSe, ZnS, GaP, and InP. Among them, a glass substrate is particularly preferable. A material for use in electroluminescent devices for this purpose. Suitable materials include, for example, tin-doped indium oxide (ITO), zinc-doped lanthanum oxide (120), indium oxide, tin oxide, and zinc oxide. ?το is particularly good. The thickness of the hole injection electrode will vary with the hole injection material and other components of the electroluminescent device. The typical thickness of the electrode is 50 to 500 nm and especially 50 to 300 nm. The electron injection electrode can be Typically used in electroluminescent devices for any of the materials used in this project. Suitable materials include, for example, low work function metals such as clocks, linings, sodium, magnesium, strontium, garnish, #5, 钡, 钡, aluminum, silver, Indium, tin, zinc and recorded and binary or ternary alloys containing these metals. Among them, the Chinese National Standard (C.NS) Α4 specification (210Χ297 mm) is applied to the paper scale (please read the precautions on the back) Fill in this page), π 20 181295901 A7 B7 by |1 Production Bureau 1 Consumer Cooperatives Printing 5, invention description (Ming and series continuous layer and containing 丨 to Cong weight 33 alloy is better. Electron injection electrode thickness will be with electricity The injection material and other components of the electroluminescent device vary. A typical electrode thickness is from 01 to 5 nanometers and preferably at least one nanometer. A typical organic electroluminescent device of the invention comprises an inorganic layered metal chalcogenide. a hole transport layer, an inorganic metal oxide electron blocking layer, and an organic light-emitting layer sandwiched between the cathode and the anode. These devices are inexpensive to manufacture because the processing required for depositing the layers is simple, and most of the layered metal chalcogenide It is cheap and easy to obtain. In particular, the above-mentioned all-chemical cheap device processing technology can be long: easy to prepare and low-cost devices. The electroluminescent device of the present invention is highly effective, and the power efficiency of some devices is greater than 10 lm/W, which is obviously bright. Some devices have a brightness of 6 volts above 60,000 candelas per square meter. The mixed organic/inorganic device has the advantages of materials and inorganic materials, and the superior characteristics of the device of the present invention confirm the synergistic effect of organic/inorganic. BRIEF DESCRIPTION OF THE DRAWINGS The invention will be further understood by considering the following examples in which: FIG. 1 shows the atomic structure of 2H-MoS2; FIG. 2 shows the electroluminescent device according to the invention having a layered shape Schematic representation of a metal dichalcogenide hole transport layer; Figure 3-5 shows an IVL plot of a glass/it〇/]V[s2/F8BT.: TFB/Ca/Al device according to the present invention; The figure shows a schematic representation of an electroluminescent device according to the present invention having a layered metal dichalcogenide hole transport layer and a metal (please read the back of the back sheet and fill out this page)

, 1T -21 1295901 at B7 V. Inventive Note (), 19 Oxide Electronic Barrier Layer; 'Figure 7 shows the glass/IT0/NbSe2/Nb205/F8BT: FB/Ca/Al device IVL mapping according to the present invention Figure 8 shows the power supply and luminous efficiency spectrum of the glass/IT0/NbSe2/Nb205/F8BT: .TFB/Ca/Al device according to the present invention; Figure 9 shows the glass/ITO/MoS2/Mo03/F8BT according to the present invention; : IVL plot of TFB/Ca/Al device; Figure 10 shows power supply and luminous efficiency of glass/ITO/MoS2/Mo03/F8BT: TFB/Ca/Al device according to the present invention; Figure 11 shows Invention of the glass / IT0 / TaS2 / Ta203 / F8BT: IVL drawing of the TFB / Ca / Al device; Figure 12 shows the glass / ITO / TaS2 / Mo03 / F8BT: TFB / Ca / Al device power supply according to the present invention Luminous efficiency mapping. The Ministry of Economic Affairs, the Central Government, and the Consumers' Cooperatives, Printed the Intellectual Property Office (please read the notes on the back and fill out this page). First, explain the structure of the substrate/hole injection layer/layered metal chalcogenide hole transport layer. The manufacturing method then illustrates the fabrication of two types of alternating type electroluminescent devices based on such a structure, one with a metal oxide layer between the layered metal chalcogenide and the organic light-emitting layer and the other type. In the examples, the layered chalcogenides used are all layered metal dichalcogenides. Lithium insertion, peeling, and film formation: Insertion of n-butyllithium (Bu-Li) in a hexane solution for inserting lithium atoms into the layered metal dichalcogenide compound. In a typical reaction, 0.5 g of commercially available layered metal dichalcogenide (MX2) powder was immersed in a dry Schlank vessel at 1.6 M n-butyl clock under argon for 3 Torr. The treatment procedure was based on DW Murphy. This paper scale applies Chinese national standard (cns) A4 specification (210X297 mm) "~" Γ -22 - Ministry of Economic Affairs T Central Mongolian Consumer Cooperatives Printed Intellectual Property Bureau 1295901 at B7 V. Inventions () 20 FJ Di Salvo, GW Hull Jr. and JV Waszczak, Revelation of Inorganic Chemistry 15, 17 (1976). The insertion reaction was as follows: yBu-Li+MX2------> LiyMX2+(y/2)C8H18 The product LiyMX2 was washed with anhydrous hexane, dehydrated under vacuum, and then transferred to a glove box. In the intercalation compound, the lithium atom is located in the van der Waals gap between the MX2 layers [Ref. R. H. Friend and A. D. Yoffe, Advanced Physics 36, 1 (1987)]. Peeling methods of use are based on P. Joensen, R. F. Friendt and S. R. Morrison, Materials Research Bulletin, 21, 457 (1986) and U.S. Patent 4,996,108. The vial was loaded with 15-20 mg of the LiyMX 2 manufactured by the aforementioned insertion step in a glove box and then taken out. Immediately add 5-10 ml of deionized water and subject the solution to ultrasonic vibration (typically 1 hour). The glass reaction proceeds as follows

LiyMX2+H20------> yLiOH+(y/2)H2+MX2 stacks hydrogen depletion layers that escape between the Mx2 layers, producing a mx2 monolayer (SL) with a single layer suspended in water. The SL suspension was centrifuged and the precipitate was washed/stirred and re-centrifuged until the pH of the supernatant dropped to 7, indicating that no lithium hydroxide remained in the deposit. Film formation: The method used is based on P. Joensen, R. F. Frindt and S. R. Morrison, Materials Research Bulletin 21, 457 (1986) and U.S. Patent 4,996,108. Add 3 ml of deionized water to the SL precipitate, suspension. Ultrasonic treatment for a few minutes. Then add 2-3 ml of xylene or toluene to the Chinese National Standard (CNS) A4 specification (210X: 297 mm) according to the paper scale (please read the notes on the back and fill out this page)

23 1295901 at ________B7 V. INSTRUCTIONS () -: 21 Ultrasonic treatment of S L suspension. > The granules are not mixed. The inorganic material is in the aqueous phase (lower phase). Once the vial is shaken, the MX® film grows between the water and the organic solvent and climbs onto the vial wall. It should be noted that in some cases, depending on the nature of the material used and the type of film desired, ultrasonic treatment can be performed after the solvent is added and before shaking. A wet, clean and oxygen plasma treated ITO coated glass substrate (e.g., as described in WO-A-90/13148; Figs. 2 and 6 1 '2) was subsequently impregnated at the interface. The MX2 film (Fig. 2 and Fig. 3) is spread on the substrate at the interface. Film thickness is controlled by SL suspension concentration, typically 4-7 nm thick [determined by AFM (atomic force spectroscopy) and xpS (X-ray photoelectron spectroscopy) measurements]. Device Structure An organic light-emitting material film can be applied to the surface of the inorganic layer prepared as described above using any of the techniques suitable for use in this project. It is particularly preferred to spin-coat a polymer in an organic solvent solution (for example, as disclosed in W〇_A-90/13 148). In the following Baye, poly(2,7-(9,9-di-n-octylfluorene)-(ι,4-phenylene-(4.t-butylphenyl)imide)-1,4-stretch Phenyl)) ("TFB") and poly(2,7-(9,9-di-n-octyl)-3)6-benzothiadiazole) ("F8BT") The material [F8BT.TFB (3:1)] was spin-coated on the inorganic layer of the coated substrate as described above at a concentration of 15 g/ml (rotary coating was applied at 2500 rpm for 6 sec, using progressive acceleration). To achieve the final speed) to obtain a film thickness of 75-80 nm (4 of Figures 2 and 6). In order to complete the device, an electron injecting layer is then deposited on the upper surface of the organic light-emitting film deposited on the electrical & transfer layer as previously described. Any material suitable for use as an electron injecting material can be used. Examples of such materials and their deposition hands 1295901 Industrial Consumer Cooperatives Printing Intellectual Property Office A7 B7 V. Invention Description (), paragraph 22 is listed as before. In this case, first, a layer of calcium (5th of Figs. 2 and 6) is deposited on the surface of the polymer film by evaporation of less than 8 χ1 (Γ6 mbar evaporation, followed by evaporation of the aluminum layer at a pressure of less than 5 x 10_6 mbar. (6 of Figures 2 and 6). In the example, two sets of devices were fabricated. In the first set of devices, molybdenum disulfide, antimony diselenide, or antimony disulfide is shown in Figure 2 (not drawn to scale) for deposition. Before the polymer layer (in other words, the metal dichalcogenide layer and the polymer layer do not contain an oxide layer) are deposited on the ITO layer as a hole transfer layer. In addition, a device for manufacturing each metal dichalcogenide is also used, wherein the metal II The chalcogenide layer (which was subjected to a pressure of 1 〇 5 mbar and a temperature of 230-240 ° C for 10 hours) was deposited before the polymer layer. This was used to investigate the effect of metal disulfide film annealing on device performance. Each batch of devices was also prepared as a control device having the following structure: glass/ITO/PEDOT:PSS/F8BT: TFB/Ca/Al俾 to compare device performance with prior art devices. IVL plots are shown in Figures 3 to 5 for a total of 6 devices. (3 materials, annealed and unannealed), data can be listed in Table 1 below Table 1 μχ2 material · , current density at 6 volts (milliamps per square centimeter) at 6 volts brightness (candles per square meter) TaS2 unannealed 68 1.4 TaS2 annealing 250 7.0 MoS2 unannealed 2660 110 MoS2 annealing 2140 300 NbS2 unannealed 590 120 NbS2 annealed, 2440 490 PEDOT-PSS 1500 60000 The structure shown in Figure 2 with MX2 as a hole transport layer L is applicable to China National Standard (CNS) A4 specification (210 X 297厘) ' ' ' 25 - (Please read the notes on the back and fill out this page)

1295901 A7 ______ B7 V. INSTRUCTIONS () 23 The low current and brightness values obtained for the disulfide button (TaS2) may be due to the discontinuity of the film observed for the XPS and AFM measurements. Compared with the unannealed film, the annealed molybdenum disulfide (MoS2) layer device has a lower current density because the metal phase changes to a semiconductor phase when the material is annealed [Ref. JA· Wilson and AD Yoffe, Advanced Physics 18, 193 (1969)]. Annealing can be seen in each case to result in improved brightness of the device. In the second set of devices, the metal dichalcogenide layer was treated with oxygen, at 25 watts for 1, 5, 10 or 20 minutes. This results in the formation of a thin metal oxide film on the surface of the metal dichalcogenide layer (Fig. 6-7). The longer the oxygen plasma treatment time, the thicker the metal oxide layer produced. As explained above, it is desirable to improve the electron trapping property, increase the retention of electrons in the luminescent polymer layer, and thereby increase the brightness. Taking molybdenum disulfide as an example, the oxide layer composition is M〇〇3; and the disulfide button and the bismuth selenide are used as an example, and the oxide compositions are determined by XPS measurement to be Ta2〇5 and Nb2〇5. As for the first set of devices, for each mx2/MO combination, an additional device is created in which the metal dichalcogenide layer is annealed. The structure of the device is shown in Figure 6 (not drawn to scale).

The inventor of the Consumers Co., Ltd. invented the metal disulfide layer annealing before the electropolymerization treatment, and the length of the electricity processing time affected the performance of the device. The selected I_V_L and power range are plotted in Figures 7-12 (Figures 7 and 8 show sharp-based device results, Figures 9 and 10 show molybdenum-based device results, and Figures 11 and 12 show Button-based device results). The data obtained from this graph is shown in Table 2 below. 26 1295901 A7

B V. INSTRUCTIONS () 24 Table 2 The Ministry of Economic Affairs is not covered by the consumer cooperatives. The printed intellectual property bureau sheet is at 250〇C. The oxygen plasma is 6 volts at 6 volts. The power efficiency is luminous efficiency, the annealing efficiency is mx2 minutes, and the current density is Ampere / square centimeter candle / square meter lumen / watt candle / ampere NbSe2 no 5 1400 23000 (31500 at 5.7 volts) 7.9 at 2.8 volts 7.8 at 3.4 volts NbSe2 no 10 3300 24000 (30000 at 5.1 volts) 9 at 2.6 volts 7.6 at 2.6 volts NbSe2 No 20 1200 27500 7.5 at 2.7 volts 7 at 3.2 volts NbSe2 is 5 500 24000 7.2 at 3.0 volts. 7.5 at 3.7 volts NbSe2 is 10 2550 48000 at 5.5 volts saturation 6.8 at 2.8 volts 6.3 at 3.1 volts NbSe2 is 20 1100 20000 5.7 at 2.5 volts at 8 volts 2.5 volts MoS2 no 1 750 31000 9.4 at 2.4 volts 8.4 at 2.7 volts MoS2 no 5 2300 58000 at 6.0 volts saturation 5.9 at 2.8 volts 5.4 at 2_8 volts MoS2. No 10 3000 56000 at 5.5 volts saturation 7 At 2.7 volts 6 to 2.7 volts MoS2 no 20 1000 40000 7 at 2.4 volts 6 to 2.8 volts MoS2 is 1 1600 40000 at 5.6 volts saturation 9.5 at 2.5 volts 7.5 at 2.5 volts M oS2, is 5 2000 50000 at 5.7 volts saturation 7.5 at 2.6 volts 6.5 at 2.6 volts MoS2 * / is 10 700 20000 10 at 2.6 volts 8 at 2.6 volts MoS2 is · 20 1900 53000 9.5 at 2.4 volts 7.7 at 2.9 volts TaS2 No 10 1400 23000 (31500 is saturated at 5.7 volts) 10 at 2.6 volts 1.5 at 2.8 volts TaS2 is 10 3300 24000 (30000 at 5.1 volts saturation) 3.2 at 2.5 volts 4.5 at 3.3 volts Control device PEDOT 1400 61000 10.5 at 2.4 volts 9.4 at 2.91⁄2 The temple has MX2 as the electricity, the hole transport layer and the corresponding LED oxide as the electron blocking layer of the device structure of the LED performance, although the thickness of the injection layer and the barrier layer as well as the composition of the composition of the compound and the standard country 9 · 2 27 (Please read the notes on the back and fill out this page)

1T 25 1295901 V. INSTRUCTIONS (not idealized, but as can be seen from the foregoing, the device has extremely high luminous efficiency and power efficiency. It is important to note that life and stability measurements have not been made. However, due to metal chalcogenides and corresponding metals Oxides are stable at high temperatures (greater than 75 〇t:), and it is expected that these devices will be reasonably stable and have a long service life. In summary, the foregoing results show that the layered metal chalcogenide has several important properties 'to make the layered metal chalcogenide The hole transport layer used for organic electroluminescence is highly prospective: ^ I·Work function π·Chemical (solution) treatment is easy to ΠΙ. Continuous formation of ultra-thin film IV· can be simply converted into corresponding insulating oxide V·High temperature stability VI. Chemical inertness This paper scale applies to China National Standard (CNS) A4 specification (210X297 mm) Ministry of Economic Affairs Central Government Mongolian Consumer Cooperatives Printed Intellectual Property Bureau 1295901 A7 B7 V. Invention Description () 26 Components Label comparison 1... Glass substrate 2. Hole injection electrode 3.. Layered metal chalcogenide layer 4. Organic light-emitting layer 5-6... Electron injection electrode 7.. Oxide film This paper size is applicable to China National Standard (CNS) A4 specification (210X297 mm) (please read the note on the back and fill out this page)

29

Claims (1)

1295901 AS BS C8 D8 Important person: The beer has a copy of the application of the patent. The Ministry of Economic Affairs, the Ministry of Economic Affairs, the Intellectual Property Bureau, the employee, the cooperative cooperative, the printing or the drawing, the reduction of the ilfg, the 091 1 10436 patent application, the patent scope revision, the amendment date: April 1996 An electroluminescent device includes a hole injecting electrode, an electron injecting electrode, and at least one organic light emitting layer disposed between the hole injecting electrode and the electron injecting electrode, wherein the layered metal remnant layer is And disposed between the hole injection electrode and the luminescent layer, the chalcogenide composition of the chalcogenide is selected from the group consisting of sulfur, lithus and hoof. 2. The electroluminescent device of claim 1, wherein the layered metal chalcogenide is the only hole transport material. 3. The electroluminescent device of claim 1 or 2, wherein the layered metal chalcogenide has a work function of 4 to 6.5 eV. 4. The electroluminescent device of claim 3, wherein the layered metal chalcogenide has a work function of 5 to 6 · 5 eV. 5. The electroluminescent device of claim 2 or 2, wherein the layered metal chalcogenide has an electrical resistivity of 1 X 6 , such as the electroluminescent device of claim 3, wherein the layered The metal chalcogenide is a layered metal dichalcogenide. 7. The electroluminescent device of claim 6, wherein the metal component of the layered metal dichalcogenide is selected from the group consisting of titanium, zirconium, hafnium, vanadium, niobium, sharp, molybdenum, tungsten and tin. group. 8. The electroluminescent device of claim 6, wherein the metal component of the layered metal dichalcogenide is selected from the group consisting of ruthenium, molybdenum, niobium, tin and tungsten. 9. The electroluminescent device of claim 1, wherein the layered gold ----------••—fb (•Please read the notice on the back of the wSHt page first) Book the i ΙΓ line' This paper scale applies to the Chinese National Standard (CNS) A4 specification (210—X 297 PCT> 30 098 008 ABCD Economic Zou Intellectual Property Bureau employee consumption cooperative printed! 2959〇1,, the patent application scope belongs to the group consisting of sulfur and selenium. The sub-system is selected from the group consisting of sulfur and selenium. The electroluminescent device of claim i, wherein the layered metal chalcogenide is selected from the group consisting of a disulfide group, a disulfide bond, and a second listener silver. The electroluminescent device, wherein the layered metal chalcogenide layer has a thickness of 3 to 20 nm. U. The electroluminescent device of claim 1, wherein the layered metal chalcogenide layer has a thickness of 3 U. The electroluminescent device of claim 1, wherein the layered metal chalcogenide layer has a thickness of 3 to 7 nm. Μ a light-emitting device in which the layered metal chalcogenide layer is deposited in a hole and injected into the electricity An electroluminescent device according to the invention of claim 2, wherein the organic light-emitting layer comprises one or more layers of one or more organic light-emitting materials or organic light-emitting material composition layers. Wherein the organic light-emitting material is selected from the group consisting of polyphenylene-ethylene (PPV) and its derivatives, polyfluorene and its derivatives, polynaphthalene and its derivatives, polyfluorene and its derivatives, polyphenanthrene and its Derivatives, aluminum decanols (Alqd complexes, transition metal complexes, lanthanides with organic ligands and lion elements, and acridine, redene and styrene oxime dyes) 16. The electroluminescent device of claim 1, wherein the organic light-emitting layer comprises one or more layers of one or more organic light-emitting materials or organic light-emitting material composition layers, wherein the organic light-emitting material is selected from the group consisting of aluminum germanium. The paper size of Nocol is applicable to the Chinese national standard (CNS>A4 specification (210 X 297 mm) Eg 0088 ABCD 1295901 夂, the scope of the patent application (Alq3) complex and the luminescent conjugate polymer material. The polymer may be a homopolymer or may contain two or more different light-synthesis units. The polymer comprises a conjugate unit selected from the group consisting of the following formulae (VIII), (IX), (X), (XI), (XII), (XIII), (XIV) and (xv): ----- -----TIJ! Packing - G, please read the note on the back of this page) - Embroidery. Printed by the Ministry of Economic Affairs, Intellectual Property Bureau, Staff Consumer Cooperative (XII ) 32 This paper scale applies to China National Standard (CNS) A4 specification (210 X 297 mm) 1295901 CQCC8 8 ABCD VI. Patent application scope _ I (X2)(X4) (XIII) (XIV) --- ί -装 * C Please read the back note on this page) Where: 订-------r.绨I Ministry of Economic Affairs Intellectual Property Bureau Employees Consumption Cooperative Prints R to R and R to R3 3 is a group which is the same or different and is selected from the group consisting of a group as defined below, a halogen group as defined in T, an alkoxy group as defined below, an alkoxyalkyl group as defined below, as defined below An aryl group, an aryloxy group as defined below, an aralkyl group as defined below, and a group of the formula -COR16 group wherein the group 6 is selected from the group consisting of a hydroxyl group, an alkyl group as defined below, a halogen group as defined below An alkoxy group, as defined below, an alkoxyalkyl group, as defined below, an aryl group, as defined below, an aryloxy group, as defined below, an aralkyl group, an amine group, an alkylamino group, and an alkyl group thereof, as defined below, Thereafter, the dialkylamino group wherein each alkyl moiety is the same or different and is defined as follows, the aralkyloxy group has an aralkyl moiety as defined below, and the haloalkoxy group comprises an alkoxy group as defined below Substituting at least one halogen atom, or if r or s is an integer of 2, the R32*R33 diradical may be attached separately The ring carbon atoms on it form a heterocyclic ring containing 5 to 7 ring atoms. The paper scale applies to the Chinese National Standard (CNS) A4 specification (210 X 2^Love 1295901 0988 8 ABCD Patent Application Scope of Economic Affairs Intellectual Property Bureau Consumer Cooperative The printing group, or more than one of the ring atoms is a hetero atom selected from nitrogen, oxygen and sulfur atoms; z Z and Z are each the same or different and are selected from 〇, s, S02 ^ NR3 > N+ (R3)(R3^^C(R4)(r5)^ si(R4)(R^)^ P(0)(0R) consisting of groups, where r3, r3, & r3, are the same or phase Each is selected from the group consisting of a hydrogen atom, an alkyl group as defined below, an alkyl group as defined below, an alkoxy group as defined below, a calcined wire as defined below, an aryl group as defined below, An aryloxy group, as defined below, an aralkyl group as defined below and an alkyl group, as defined below, substituted with a group of the formula -n+(r7)3 wherein each &7 group is the same or acupoints and is selected from a hydrogen atom, an alkyl group as defined below, and an aryl group as defined below, and the groups 'R, r5, r4 and R5 are the same or different and each A hydrogen atom, an alkyl group as defined below, an alkyl group as defined below, an alkoxy group as defined below, an atom, a nitro group, a cyano group, an alkoxyalkyl group as defined below, an aryl group as defined below, as defined below a group consisting of an aryloxy group and an aralkyl group as defined below, or a group of 5 and a carbon atom to which 5 is attached, and a ring group selected from the group consisting of a hydrogen atom, a group as defined below, a decyl group, an alkoxyalkyl group as defined below, an aryl group as defined below, an aryloxy group as defined below, and a group consisting of aralkyl groups as defined below; X, x, x3 and X4 are each identical or different And is selected from the group consisting of: an aromatic hydrocarbon group having one or more rings having 6 to 4 carbon atoms, which may optionally be substituted with a substituent of at least one group selected from the group consisting of the following groups: · Nitro, cyano, amine, as defined below, I. Less than page, 297 mm) 1295901 A8 B8 C8 D8 VI. Patent range Alkyl, as defined below, alkyl, alkoxylated as defined below a aryloxy group as defined below, and an alkane as defined below a linear or branched alkyl group having 1 to 6 carbon atoms; a linear or branched alkyl group having 2 to 6 carbon atoms; and a linear or branched chain having 1 to 6 carbon atoms; An alkynyl group; or X1 and X3 and/or X2 and X4 together represent a bond group of the following formula (7): 0 Please read the back note (V) This page is printed by the Ministry of Economic Affairs, Intellectual Property Office, and the Consumer Cooperatives. X5 represents an extended aromatic group, which is an aromatic hydrocarbon group containing 6 to 14 stone anion atoms in one or more rings. Substituent substituted with at least one group selected from the group consisting of nitro, cyano, amine, alkyl as defined below, haloalkyl as defined below, alkoxyalkyl as defined below, aryl as defined below An oxy group, and an alkoxy group as defined below; el, e2, fl and f2 are each the same or different and are 〇 or an integer from 1 to 3; g, ql, q2, q3 and q4 are each the same or different and Is (), 1 or 2; hi 'h2, jl, j2, j3, u, 12, 13, 14, _ are each the same or different and are 〇 or an integer from 1 to 4; 1, kl, k2, 〇 1 and 〇2 are each the same or different and are 〇 or an integer from 1 to 5; Order----- MB I-' 35 1295901 AS BS C8 D8 Economy Zou Intellectual Property Bureau employee consumption cooperative printed 'patent patent range pi, p2, p3 and P4 are each 0 or 1; the aforementioned alkyl group contains 1 to a linear or branched alkyl group of 20 carbon atoms; the aforementioned halogen group is a group as defined above which is substituted with at least one atom; the alkoxy group is a linear or branched chain having 1 to 20 carbon atoms An alkoxy group; the alkyl group as defined above is substituted with at least one alkoxy group as defined above; and the aforementioned aryl group and the aforementioned aryl group (the alkyl group contains 1 to 2 carbon atoms) and The aryl moiety of the aryloxy group is an aromatic hydrocarbon group having from 6 to 14 carbon atoms in one or more rings, which may optionally be substituted with a substituent of at least one group selected from the group consisting of: nitro , cyano, amine, alkyl as defined above, haloalkyl as defined above, alkyloxyalkyl as defined above, and alkoxy as defined above. 17. The electroluminescent device of claim 1, wherein the organic light-emitting layer is selected from the group consisting of PPV, poly(2-methoxy-5-(2,-ethyl)hexyloxyphenylene-vinyl ("MEH_PPV"), a PPV dialkoxy and dialkyl derivative, a polyfluorene derivative and related copolymer, and an Alq3 complex composition group. 18. The electroluminescent device of claim 1, wherein a layer of material is disposed between the organic light-emitting layer and the layered metal chalcogenide hole transport layer. The material of the layer constrains electron migration from the organic light-emitting layer to the layered layer. Metal chalcogenide hole transport layer. This paper scale applies to Chinese national standards (CNS>A4 specifications (210 297 297 mm) 36 ΓPlease read the notes on the back page first) Binding-------ί线. QQ 5 9 2 ΠΛ88 8 AB- CD Ministry of Economic Affairs Intellectual Property Bureau employee consumption cooperative printing, application for patent scope 19 · For example, the electroluminescent device of claim 18, wherein the constrained electrons migrate from the organic light-emitting layer to the layered metal chalcogenide hole transport layer The material is the same metal oxide as the metal of the metal chalcogenide layer. 2. The electroluminescent device of claim 18, wherein the metal oxide layer which is the same as the metal of the layered metal chalcogenide layer is deposited on the hole injection electrode via the layered metal chalcogenide Afterwards, it is formed via the exposed face of the oxide layered metal chalcogenide layer. The electroluminescent device of claim 19 or 20, wherein the metal oxide layer which is the same as the metal of the layered metal chalcogenide layer has a thickness of from 1 to 10 nm. The electroluminescent device of claim 19, wherein the metal oxide layer having the same metal as the layered metal chalcogenide layer has a thickness of 2 to 6 nm. 23. The electroluminescent device of claim 19, wherein the metal oxide layer of the same metal as the layered metal chalcogenide layer has a thickness of from 2 to 3 nm. 24. The electroluminescent device of claim 2, wherein an electron transport layer is disposed between the electron injecting electrode and the organic light emitting layer. 25. The electroluminescent device of claim 24, wherein the electron transporting layer is selected from the group consisting of cerium oxide, magnesium oxide, calcium oxide, lithium oxide, cerium oxide, potassium oxide, sodium oxide, and oxidized planer. . 26·If you apply for a patent scope! The electroluminescent device of the present invention, wherein the hole injection electrode is formed on a substrate selected from the group consisting of glass, quartz, and Si, GaAs, ZnSe' ZnS, GaP, and InP crystalline substrates. _(*Please read the note on the back page first) Binding-----na-fc-I line ' 37 C9CC88 ABCD 1295901 VI. Patent application scope 27. Electroluminescence in item 1 of the application patent scope The device, wherein the hole injecting electrode is made of a material selected from the group consisting of tin-doped indium oxide (IT0), zinc-doped steel oxide (yttrium), indium oxide, tin oxide, and zinc oxide. 28. The electroluminescent device of claim 1, wherein the electron injecting electrode is selected from the group consisting of potassium, lithium, sodium, magnesium, strontium, barium, calcium, strontium, samarium, samarium, silver, indium, tin. , zinc and erroneous, and materials containing a group consisting of binary or ternary alloys of such metals. 29. A method of producing an electroluminescent device having a layered metal dichalcogenide layer as in claim 6 of the patent application, the method comprising depositing the layered metal dichalcogenide in accordance with the following steps The step of injecting a hole into the electrode: (a) inserting a clock atom into the metal dichalcogenide; (b) adding water to the resulting intercalation material resulting in a stripping reaction, thereby producing a monolayer of metal dichalcogenide suspended in water; Adding a water-immiscible solvent to the product of step (b), followed by agitating the mixture obtained by the Ministry of Commerce, Intellectual Property Office, the Consumer Cooperative, and obtaining a layered metal dichalcogenide film at the solvent/water interface; and (d) wetting The hole injection layer on the substrate is supported, and then immersed in the solvent/water interface generated in the above step (c), allowing the layered metal dichalcogenide film to spread over the surface of the hole injection layer. This paper scale applies to the Chinese National Standard (^NS) A4 specification 38