KR20170097944A - Light extracting layer for OLED, OLED using the same and method for preparing the OLED - Google Patents
Light extracting layer for OLED, OLED using the same and method for preparing the OLED Download PDFInfo
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Abstract
Description
The present disclosure relates to an organic light emitting device light extracting layer having improved light extraction efficiency, an organic light emitting device using the same, and a method of manufacturing the same.
An organic light emitting diode (OLED) has characteristics of a planar light source unlike an existing light emitting device such as an incandescent lamp, a fluorescent lamp, or a point light source LED (light emitting diode). In addition, it has various advantages such as wide viewing angle, low voltage driving method and plasticity. Therefore, technology development and research are being conducted to utilize an organic light emitting device as well as a display device.
However, in the organic light emitting device, light loss occurs between the thin film layer and the substrate due to a difference in the refractive index of the device, and only light in a specific angle region is emitted to the outside. The amount of light emitted to the outside is about 20%, and the light extraction efficiency is extremely limited. Without increasing the light extraction efficiency, the efficiency and utilization of the organic light emitting device will be lowered.
Therefore, studies have been made on a light extraction layer for increasing the light extraction efficiency. As such a light extraction layer technique, there is a method of manufacturing a light extraction layer by a method such as a photolithography process or a femto laser.
However, according to the study of the present inventors, the conventional method of manufacturing a light extracting layer has the following problems.
That is, the conventional light extraction layer manufacturing method has a burden and a disadvantage to use expensive equipment. In addition, as a material for forming the inner light extracting layer of the conventional organic light emitting device, an inorganic material such as inorganic oxide or nitride is used, which is also a factor for increasing the manufacturing cost of the organic light emitting device. In addition, in order to use the above-described inorganic materials, a certain type of texturing structure must be formed, so crystallinity is also an important factor in using inorganic materials. However, since crystallinity and crystalline orientation are determined by high-temperature and pressure conditions such as an atmospheric-pressure chemical vapor phase measurement process, and compositional composition ratios, very careful control is required, .
In addition, in the case of the conventional method of manufacturing a light extracting layer, the surface roughness is increased due to texturing and inorganic scattering particles formed on the surface of the light extracting layer. Accordingly, There is also a problem that electrons are collected and the device efficiency and electrical characteristics are deteriorated.
In an exemplary embodiment of the present invention, in one aspect, there is provided an organic light emitting device comprising: an organic light emitting device light extracting layer capable of increasing the efficiency of a light extracting layer in the organic light emitting device and thereby improving the overall efficiency and electrical characteristics of the organic light emitting device; A manufacturing method thereof, and an organic light emitting device using the same.
Further, in the exemplary embodiments of the present invention, in another aspect, the manufacturing process of the inner light extracting layer is simple and the inorganic material is not used compared to the conventional method, so that the process becomes simple and has a considerable advantage in terms of cost And a method for manufacturing the organic light emitting device, and an organic light emitting device using the same.
In an exemplary embodiment of the present invention, a light extraction layer of an organic light emitting device includes organic nano-scattering particles having pores and a binder polymer, and an organic light emitting device including the same. to provide.
According to another exemplary embodiment of the present invention, there is provided a method of manufacturing an organic light emitting device, comprising: preparing a light extracting layer composition by dissolving organic nano-scattering particles having pores and a binder polymer in a solvent; And coating the light extracting layer composition on a substrate and drying the solvent to form a light extracting layer.
According to exemplary embodiments of the present invention, the light extraction efficiency of the organic light emitting device can be increased, thereby improving the overall efficiency and electrical characteristics of the organic light emitting device. In addition, the manufacturing method of the organic light emitting diode according to the exemplary embodiments of the present invention has a considerable advantage in terms of cost since the manufacturing process of the inner light extracting layer is simpler than the conventional method.
BRIEF DESCRIPTION OF THE DRAWINGS FIG. 1 is a schematic view showing that hollow carbon particles (FIG. 1A) or cyclodextrin particles (FIG. 1B) are present between binder polymers in an embodiment of the present invention.
Figure 2 shows schematically a method of making hollow carbon particles and photographs thereof in an exemplary embodiment of the present invention.
3 is a schematic view showing an organic light emitting device and a light extracting layer according to an embodiment of the present invention.
4 is a schematic view showing the structure of an organic light emitting device according to embodiments and comparative examples of the present invention. FIG. 4A shows Comparative Example 1, FIG. 4B shows Comparative Example 2, and FIG. 4C shows an embodiment.
FIG. 5 is a graph showing luminescence (FIG. 5A) and current efficiency (FIG. 5B) according to voltages of an organic light emitting diode according to embodiments and comparative examples of the present invention.
Hereinafter, exemplary embodiments of the present invention will be described in detail.
In exemplary embodiments of the present invention, an organic light emitting device light extracting layer including organic nano-scattering particles having pores and a binder polymer is provided as a light extracting layer of an organic light emitting device.
The organic nano-scattering particle is a scattering particle composed of an organic material and has pores, and the particle size is nano-sized, that is, less than 1000 nm. These organic materials are advantageous not only in cost but also in crystallinity at low temperatures as compared with inorganic materials. When the organic nano-scattering particles having such pores, preferably cyclodextrin or hollow carbon particles described later, are mixed with a polymer binder to form a light extracting layer, the uneven surface formed by the polymer binder is separated into organic nanospores Depending on the zoom, the surface roughness can be reduced. Accordingly, the concentration of holes and electrons in a specific region can be reduced, and the interfacial resistance between each layer contacting the light extracting layer can be reduced. Thus, the efficiency of the light extracting layer can be increased. In addition, fine pore control is possible and it is advantageous to control the light extraction efficiency. The micro pores can improve the light extraction efficiency by refracting and scattering the light emitted from the light emitting layer in various directions, thereby forming the incident angle smaller than the critical angle. In addition, since the organic material has low-temperature crystallinity, the process is simple and the process cost can be reduced unlike the case of the inorganic material.
In an exemplary embodiment, the organic nano-scattering particles having pores are preferably hollow carbon particles or cyclodextrin particles.
BRIEF DESCRIPTION OF THE DRAWINGS FIG. 1 is a schematic view showing that hollow carbon particles (FIG. 1A) or cyclodextrin particles (FIG. 1B) are present between binder polymers in an embodiment of the present invention.
1A and 1B, hollow carbon particles 21 (FIG. 1A) or cyclodextrin particles 22 (FIG. 1B) are positioned between the
In one exemplary embodiment, cyclodextrin (CD) can be divided into alpha, beta, and gamma-forms. Cyclodextrins are synthesized using enzymes and result in α, β, γ-cyclodextrins with cavities with pores as a result of synthesis. Subsequently, β-cyclodextrin is firstly separated from the α, β, γ-cyclodextrins using water, and the α, γ-cyclodextrins are separated by a finer method such as a chromatography technique.
In one illustrative embodiment, cyclodextrins in alpha, beta, gamma -cyclodextrin Cyclodextrin is the most cheap and easiest to separate after synthesis.
Cyclodextrin has an outer diameter of about 1.37 nm, a pore size of about 0.57 nm, an outer diameter of about 1.53 nm and a pore size of about 0.78 nm, a? -Cyclodextrin having a? The cyclodextrin has an outer diameter of about 1.69 nm and a pore size of about 0.95 nm.
Increasing the concentration of cyclodextrin in aqueous solution can result in aggregation and thus control / enhance the refractive index value. Cyclodextrin has a basic refractive index of about 1.59 and can obtain a refractive index corresponding to 90 to 100% of ITO (refractive index: 1.8) through the above-described refractive index control method, thereby obtaining a light extracting effect.
In an exemplary embodiment, the hollow carbon particles may have a size of, for example, from several nanometers to several hundreds of nanometers.
In the synthesis of hollow carbon particles, for example, SiO 2 nanoparticles are mainly used, and the size of the hollow carbon particles can be adjusted according to the size of SiO 2 .
Figure 2 shows schematically a method of making hollow carbon particles and photographs thereof in an exemplary embodiment of the present invention.
As shown in FIG. 2, the carbon material surrounds the SiO 2 nanoparticles, and then SiO 2 is removed to produce hollow carbon having pores. Thus, single pattern and multilayered pattern hollow carbon particles can be formed depending on the pore size and pattern of the matrix such as SiO 2 .
In one exemplary embodiment, the organic nano-scattering particles having pores and the organic nano-scattering particles having pores may be 10 to 30 wt%, and preferably 15 to 25 wt%, based on 100 wt% of the total of the polymer nano- . The number of pores (the number of pores can be confirmed, for example, by measuring the UV-spectrum by controlling the ratio of the organic nano-scattering particles having pores. That is, for example, the UV- And the number of pores can be predicted by measuring the UV-intensity of the remaining solvent after using a solvent containing nano-scattering particles), and the light extraction efficiency can be controlled. Thus, the efficiency and electrical characteristics of the organic light emitting device can be controlled. That is, as the content of the organic material increases, the number of micropores in the inner light extracting layer increases, so that the incident angle of light emitted from the light emitting layer can be made smaller than the critical angle.
If the content of the organic material is less than 10% by weight, the number of micropores may not be sufficient, and therefore it may be difficult to affect the efficiency improvement. When the content of the organic material is more than 30% by weight, the surface roughness of the thin film of the light extracting layer may become rough, thereby reducing the overall efficiency of the organic light emitting device.
In an exemplary embodiment, the surface roughness of the light extracting layer thin film is preferably as flat as possible. For example, it is preferable to have a surface roughness (RMS surface roughness) within a range of about 0.01% of the entire thickness of the light extracting layer.
In a non-limiting example, the surface roughness of the thin film of the light extracting layer may be RMS (Root Mean Square), e.g., 10 nm or less, or 2 to 10 nm.
In an exemplary embodiment, the binder polymer may use, for example, UV or thermosetting resin. For example, at least one selected from a silicone resin, a silicon oxide resin, a phenol resin, a silsesquioxane resin, a siloxane binder, and the like can be used.
In an exemplary embodiment, the light extracting layer may further comprise a crosslinking agent. As the crosslinking agent, one or more crosslinking agents selected from melamine-based, urea-based, and alkyurea-based resins can be used. The content of the crosslinking agent may be added within a range that does not impair the effect depending on the content of the organic material, for example, 0.5 to 5 parts by weight based on 100 parts by weight of the organic nano-scattering particles and the polymeric binder.
Exemplary embodiments of the present invention also provide an organic light emitting device comprising the above-described light extracting layer.
3 is a schematic view showing an organic light emitting device and a light extracting layer according to an embodiment of the present invention.
FIG. 3 first shows the overall structure for forming the OLED illumination, in which the light extraction layer is enlarged and expressed in more detail. Further, the structure for forming the light extracting layer is also described.
As shown in FIG. 3, the organic light emitting device includes a substrate, a light extraction layer disposed on the substrate, a planar layer disposed on the light extraction layer, a first electrode disposed on the planar layer, At least one light emitting layer disposed on the first electrode, and a second electrode disposed on the light emitting layer.
The flat layer may be additionally formed to prevent the surface of the light extracting layer from deteriorating due to surface irregularities and scattering. As described above, when unevenness is formed on the surface, electrical characteristics are reduced due to deterioration phenomenon in which holes and electrons are concentrated in a specific region in a specific region.
In an exemplary embodiment, the flat layer comprises a metal oxide and a polymeric binder, and the polymeric binder may be the same or different component than the polymeric binder of the light extracting layer. When the polymer binder of the light extracting layer and the polymer binder of the flat layer are the same, the bonding strength between the light extracting layer and the flat layer is improved and the resistance between layers is reduced.
In an exemplary embodiment, the metal oxide may have an average particle size of from 5 to 20 nm and may include one inorganic material selected from the group consisting of titanium oxide, aluminum oxide, silicon oxide, zinc oxide, tungsten oxide, Can be mixed and used.
In an exemplary embodiment, the substrate may be a transparent substrate.
In one exemplary embodiment, the electrode is capable of applying metal oxides with high transparency and conductivity and high work function values. For example, the metal oxide may be a transparent conductive oxide such as indium tin oxide (ITO_Indium Tin Oxide), indium zinc oxide (IZO_Indium Zinc Oxide), tin oxide (SnO 2 ), and zinc oxide (ZnO 2 ). In addition, graphene or graphene added with defects can be used.
In an exemplary embodiment, known materials may be used for the light emitting layer, the hole injection layer (HIL), the hole transport layer (HTL), the active layer (EML), the electron transport layer / hole blocking layer (ETL) Can be used. As the electrode, a conductive metal material having excellent reflectivity can be used. As the metal material, metals such as gold (Au), platinum (Pt), aluminum (Al), silver (Ag), and palladium (Pd) and alloys thereof can be used.
In an exemplary embodiment of the present invention, there is also provided a method of manufacturing an organic light emitting device, comprising: preparing a light extracting layer composition by dissolving organic nano-scattering particles having pores and a binder polymer in a solvent; Forming a light extracting layer by coating on a substrate and drying the solvent.
In an exemplary embodiment, the light extracting layer composition preferably further comprises a co-solvent having a higher boiling point than the solvent. By using such a co-solvent, the dispersibility of the polymeric binder and / or organic material having pores can be improved and coagulation can be prevented. That is, in forming the light extracting layer, in order to avoid coagulation of organic nano-scattering particles having pores such as cyclodextrin or hollow carbon due to aggregation of the binder polymer as the solvent is dried, a co-solvent ) May be introduced to adjust the drying time of the solvent to suppress aggregation of the polymer and aggregation of the organic material having pores.
In an exemplary embodiment, the organic solvent may be, for example, tetrahydrofuran (THF), dichloromethane (DCM), chloroform, chlorobenzene (BZ), or the like.
In an exemplary embodiment, the co-solvent may be an organic solvent having a boiling point higher than that of the above-mentioned organic solvent. For example, 1,2-dichlorobenzene (DBZ) or N, N-dimethylformamide can be used.
In an exemplary embodiment, the co-solvent may be used at 5 vol% to 20 vol% relative to the total solvent (organic solvent + co-solvent). If the specific gravity of the co-solvent is lower than the above-mentioned range, the advantage of using the co-solvent will be less. If the specific gravity of the co-solvent is higher than the above range, the breaking point of the co-solvent is higher than the organic solvent Which may damage the process time and the production substrate. Further, the ratio of the residual solvent (co-solvent) increases, and the layer structure of the light extracting layer may collapse.
In an exemplary embodiment, the pore size of the light extraction layer can be adjusted to control the light extraction efficiency. For this purpose, the pore size of the light extracting layer can be controlled by adjusting the composition ratio of the organic material having pores and the binder polymer.
In an exemplary embodiment, the light extracting layer composition may be formed by a spin coating method or a slot-die coating method when forming the light extracting layer.
More specifically, in a non-limiting example, the spin coating rate is, for example, 3000 rpm to 5000 rpm and the spin coating time is, for example, 30 seconds to 60 seconds, the solvent drying temperature is 100 to 150 ° C, To 20 minutes.
In an exemplary embodiment, the solvent drying time may be adjusted to inhibit agglomeration of the binder polymer or agglomeration of the organic material having pores.
In an exemplary embodiment, the light extracting layer may be formed to a thickness of 200 nm to 2 占 퐉.
In an exemplary embodiment, a planar layer may be additionally introduced on the light extraction layer to perform planarization of the surface of the light extraction layer. The flat layer can be formed by performing spin coating, slot die coating, or the like under the same conditions as those for forming the light extracting layer using a metal oxide having a particle size of 5 to 20 nm and a polymeric binder as described above.
According to the exemplary embodiments of the present invention, the light extraction efficiency of the organic light emitting device can be increased. For example, when the conventional light extraction efficiency is 20%, an efficiency increase of about 3 to 5% can be achieved. Accordingly, the overall efficiency and electrical characteristics of the organic light emitting device can be improved. In addition, the manufacturing method of the organic light emitting diode according to the exemplary embodiments of the present invention has a considerable advantage in terms of cost since the manufacturing process of the inner light extracting layer is simpler than the conventional method. The organic light emitting device including the light extracting layer thus manufactured can be widely applied not only to an illumination field but also to a display device.
Hereinafter, embodiments of the present invention will be described in more detail with reference to embodiments of the present invention. The following examples are provided to aid understanding of the present invention, and thus the scope of the present invention is not limited thereto.
4 is a schematic view showing a structure and a manufacturing process of an organic light emitting diode according to embodiments and comparative examples of the present invention. FIG. 4A shows Comparative Example 1, FIG. 4B shows Comparative Example 2, and FIG. 4C shows an embodiment.
The device manufacturing process will be described with reference to FIG. First, a glass substrate coated with indium tin oxide (ITO) having a thickness of 150 nm and a sheet resistance of 20 Ω / sq was used as a transparent anode.
4, the hole transport layer (HTL) [TAPC] / blue emissive layer (EML) [mCP: Firpic (ETL) [3 TPYMB] was prepared by vacuum evaporation of the organic material in the order of [15 wt%] / orange light emitting layer (Orange EML) [mCP: Ir (2-phg 3 ) (10 wt%)] / electron transport layer (ETL)
After deposition of the organic material, LiF as an electron injection layer (EIL) and Al as a cathode were sequentially deposited using a metal mask having a 4 mm line width to form a basic OLED device (Comparative Example 1, 4a).
As Comparative Example 2, a conventional OLED was manufactured by applying a light extraction film to the basic OLED device (Comparative Example 2, FIG. 4B).
The light extraction film was formed by mixing and spin coating (conditions such as cyclodextrin described below) with an inorganic oxide (aqueous solution of 5 to 10 nm TiO 2 , available from ENB KOREA) and a polymeric binder (silicone resin). The thickness was about 100 nm.
As an example, a cyclodextrin layer was formed in the basic OLED device, not a light extraction film (FIG. 4C). Specifically, a cyclodextrin (obtained from Aldrich) is mixed with an organic solvent (THF) and a co-solvent (1,2-DBZ) together with a silicone resin as a binder polymer to prepare a coating composition, , And the solvent was dried to prepare an OLED device to which the cyclodextrin light extracting layer of this example was applied (Example, Fig. 4C). The thickness was about 400 nm.
As described above,? -Cyclodextrin in the cyclodextrin has an outer diameter of about 1.37 nm, a pore size of about 0.57 nm, an outer diameter of about 1.53 nm and a pore size of about 0.78 nm, The? -cyclodextrin has an outer diameter of about 1.69 nm and a pore size of about 0.95 nm.
The cyclodextrin was used in an amount of 20% by weight based on 100% by weight of the total binder polymer and cyclodextrin. In addition, the co-solvent was used at 10 vol% based on the total volume of organic solvent and cosolvent. Cyclodextrin was used in an amount of about 0.2 g per 100 g of the entire solvent (organic solvent and cosolvent).
FIG. 5 is a graph showing luminescence (FIG. 5A) and current efficiency (FIG. 5B) according to voltages of an organic light emitting diode according to embodiments and comparative examples of the present invention.
As can be seen from FIG. 5, the luminance increased by about 5,000 cd / m 2 or more compared with the case where the cyclodextrin, which is organic nano-scattering particles having pores, was not used, and the current efficiency was about 1.3 times to 1.5 times or more.
Claims (17)
An organic nano-scattering particle having pores, and a binder polymer.
Wherein the organic nano-scattering particles having pores are hollow carbon material particles or cyclodextrin particles.
Wherein the organic nano-scattering particles having pores are present in an amount of 10 to 30% by weight based on 100% by weight of the organic nano-scattering particles and the binder polymer.
Wherein the cyclodextrin particle is at least one selected from the group consisting of? -Cyclodextrin,? -Cyclodextrin and? -Cyclodextrin.
Wherein the binder polymer is at least one selected from the group consisting of a silicone resin, a silicon oxide resin, a phenol resin, a silsesquioxane resin, and a siloxane resin.
Wherein the light extracting layer further comprises a crosslinking agent.
An organic light emitting device comprising the light extracting layer according to any one of claims 1 to 6.
And a flat layer disposed on the light extracting layer and including a metal oxide and a binder polymer.
The organic light-
Board;
The light extraction layer disposed on the substrate;
The planarizing layer disposed on the light extracting layer;
A first electrode disposed on the planar layer;
At least one light-emitting layer disposed on the first electrode; And
And a second electrode disposed on the light emitting layer.
Wherein the binder polymer of the planarizing layer is the same as the binder polymer of the light extracting layer.
Preparing a light extracting layer composition by dissolving organic nano-scattering particles having pores and a binder polymer in a solvent; And
Coating the light extracting layer composition on a substrate, and drying the solvent to form a light extracting layer.
Wherein the light extracting layer composition further comprises a co-solvent having a boiling point higher than that of the solvent, and the organic solvent comprises 5 vol% to 20 vol% of the solvent.
The solvent is at least one selected from the group consisting of tetrahydrofuran (THF), dichloromethane (DCM), chloroform, chlorobenzene (BZ)
The co-solvent may be at least one selected from the group consisting of 1,2-dichlorobenzene (DBZ) and N, N-dimethylformamide. Gt; < / RTI >
And adjusting the pore size of the light extraction layer to adjust the light extraction efficiency.
Wherein the pore size of the light extracting layer is controlled by adjusting the composition ratio of the organic nano-scattering particles having pores and the binder polymer.
Wherein the solvent drying time is controlled to suppress agglomeration of organic nano-scattering particles having aggregation or pores of the binder polymer.
And a flat layer including a metal oxide and a binder polymer is further formed on the light extracting layer.
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| KR20060016261A (en) * | 2004-08-17 | 2006-02-22 | 삼성코닝 주식회사 | Composition for preparing materials having nano-porosity |
| KR20100001581A (en) * | 2008-06-27 | 2010-01-06 | 동우 화인켐 주식회사 | Light diffusion plate, backlight device having the same and liquid crystal display device |
| KR20140032471A (en) * | 2010-09-06 | 2014-03-14 | 주식회사 엘지화학 | Substrate for organic electronic device and organic electronic device comprising thereof |
| WO2014185562A1 (en) * | 2013-05-13 | 2014-11-20 | 주식회사 나노신소재 | Light scattering film for organic light emitting element and manufacturing method therefor |
| KR20160016683A (en) * | 2014-08-02 | 2016-02-15 | 주식회사 엘지화학 | Dye complex, light conversion film, and electronic device comprising the same |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR20060016261A (en) * | 2004-08-17 | 2006-02-22 | 삼성코닝 주식회사 | Composition for preparing materials having nano-porosity |
| KR20100001581A (en) * | 2008-06-27 | 2010-01-06 | 동우 화인켐 주식회사 | Light diffusion plate, backlight device having the same and liquid crystal display device |
| KR20140032471A (en) * | 2010-09-06 | 2014-03-14 | 주식회사 엘지화학 | Substrate for organic electronic device and organic electronic device comprising thereof |
| WO2014185562A1 (en) * | 2013-05-13 | 2014-11-20 | 주식회사 나노신소재 | Light scattering film for organic light emitting element and manufacturing method therefor |
| KR20160016683A (en) * | 2014-08-02 | 2016-02-15 | 주식회사 엘지화학 | Dye complex, light conversion film, and electronic device comprising the same |
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