CN101114700B - Organic electroluminescent device capable of emitting white light and method for fabricating the same - Google Patents
Organic electroluminescent device capable of emitting white light and method for fabricating the same Download PDFInfo
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Abstract
The invention discloses an organic electroluminescent device which can give out light, comprising an organic electroluminescent device or a substrate, an anode layer and a cathode layer, and an electrode on the surface of the substrate, an organic functional layer between the anode layer and the cathode layer that comprises at least a luminescent layer which is an organic material layer giving out white light driven by an additional power, and is characterized in that the organic material layer giving out white light is made up by a plurality of blue organically functional materials with hole-transporting ability, the blue organically functional material can be one or more materials of aromatic diamines compounds, star-shaped triphenyl-amine compounds, carbazole polymer and metal complexes, DPVBi, BCzVB, Perylene and BczVBi.
Description
Technical field
The present invention relates to technical field of organic electroluminescence in the electronic devices and components, be specifically related to a kind of organic electroluminescence device that can send white light.
Background technology
Develop into little demonstration or the large tracts of land information of organic electroluminescent technology show technical support and guarantee are provided, because display of organic electroluminescence has significant advantage: from main light emission, low-voltage DC driven, high-low temperature resistant, complete curings, wide visual angle, color enrich, do not need backlight, the visual angle is big, power is low, response speed can reach LCD 1000 times, and its manufacturing cost is far below the LCD of identical performance, therefore, display of organic electroluminescence becomes the focus of people's research.
But, the previous research work of OLED is owing to the high driving voltage and the low-light level of device do not attract people's attention, up to 1987, people such as the C.W.Tang of Kodak were summing up the device of having invented sandwich structure on forefathers' the basis: they adopt, and fluorescence efficiency is very high, electronic transmission performance and the good organic small molecule material oxine aluminium (Alq of filming performance
3), with the aromatic diamine with hole transport characteristic (diamine) derivative make low driving voltage (＜10V), high-quantum efficiency (1%), high brightness (＞1000cd/m
2) organic EL device, this breakthrough has remotivated the concern of people for organic EL, makes people see the prospect of organic electroluminescence device as flat-panel display device of new generation.From then on, organic electroluminescent has been gone on the road that develops rapidly, and all many-sides such as people are synthetic at material, device architecture design, carrier transport have been carried out deep research, makes the performance of organic electroluminescence device move closer to or reaches the practicability level.Nineteen ninety Friend group has reported high molecule electroluminescent phenomenon under low-voltage, has opened the frontier of the organic flat panel display research of macromolecule; 1997,
Deng discovery phosphorescence electro optical phenomenon, break through the electroluminescent organic material quantum efficiency and be lower than 25% restriction, make the research of organic flat-panel display device enter a new period ... in the 10 short years, the organic electroluminescent technology inorganic display material 30 years of development courses of having passed by, and the industrialization impetus is swift and violent unusually.
Organic elctroluminescent device is as a kind of novel photoconductive organic semiconductor information functional material and solid plate display device, and development in recent years is very fast.White light organic electroluminescent display device is the hot topic of OLED research and development in recent years especially, because white light is contained red, green, blue three kinds of primary colours of whole visible region, easily be converted to full color display device, this is one of best approach that obtains at present the full color demonstration, also will be OLED device practicability, a commercial cutting point.In the life-span of white light organic electroluminescent device, problems such as colorimetric purity and stability are the stumbling-blocks of its practicability of restriction and industrialization always.Complex devices structure and manufacturing process have had a strong impact on its industrialization especially at present, and high manufacturing cost all makes its application reduce with the device performance that is difficult to repetition.
Although the OLED technology has obtained significant progress in recent years, still there are a lot of bottlenecks in present technology in the organic electroluminescent field.No matter be that organic electroluminescence device is realized full-colorization demonstration, still use as single mains lighting supply, the device preparation that can send white light all is vital, and their constructional simplicity, high brightness, high efficiency, long-life all are the key factors that influences device practicability; Especially utilize known material, adopt structure to save the device of material simply, as far as possible as far as possible with good photoelectric properties, method as spin coating or inkjet printing, realize the luminous of white, and obtain efficiently, device aspect cheaply, need people to go continuous exploration especially.
Summary of the invention
Technical problem to be solved by this invention is how to provide a kind of can send organic electroluminescence device of white light and preparation method thereof, this devices use routine, function admirable, functional material is used as the functional material in the organic layer cheaply, passed through to change the component of the 26S Proteasome Structure and Function layer of device, further improved performance, reduced cost of material, industrialization production preferably.
Technical problem proposed by the invention is to solve like this: construct a kind of organic electroluminescence device that can send white light, comprise electrically-conductive backing plate or substrate, anode layer and cathode layer, wherein a kind of electrode is positioned at substrate or electrically-conductive backing plate surface, between described anode layer and the cathode layer organic function layer is set, which comprises at least luminescent layer, this luminescent layer is the organic material layer that sends white light, under the driving of additional power source, send white light, it is characterized in that: the described organic material layer that sends white light is constituted by the blue organic functional material with cavity transmission ability, and this blueness organic functional material is the aromatic diamine compounds, the star triphenyl amine compound, carbazole polymer, metal complex, DPVBi, BCzVB, Perylene, BczVBi etc. one or more.
According to the organic electroluminescence device that can send white light provided by the present invention, it is characterized in that, the described white light that sends is that the blue light that sent by the blue light organic material and the electricity in the organic functional material layer cause that exciplex is luminous to mix, the luminous compound of a kind of energy that the mixture that it is aromatic diamine compounds, star triphenyl amine compound and carbazole polymer that this electricity causes the sharp compound of base is produced after power drives, light and blue light that this compound sent are sent white light.
According to the organic electroluminescence device that can send white light provided by the present invention, it is characterized in that, described aromatic diamine compounds is N, N '-two-(3-aminomethyl phenyl)-N, N '-diphenyl-[1,1 '-xenyl]-4,4 '-diamines or N, N '-two (3-naphthyl)-N, N '-diphenyl-[1,1 '-diphenyl]-4,4 '-diamines, described star triphenyl amine compound is three-[4-(5-phenyl-2-thienyl) benzene] amine or m-TDATA, and described carbazole polymer is a polyvinylcarbazole, and described metal complex is BAlq.
According to the organic electroluminescence device that can send white light provided by the present invention, it is characterized in that, described cathode layer and anode layer are respectively arranged with implanted layer, described organic function layer also comprises electron transfer layer, hole transmission layer and the hole blocking layer with electron transport ability, described electron transfer layer and implanted layer are metal complex material Huo person oxadiazole electron-like transferring material, perhaps imidazoles electron transport material; Described hole transport layer material is aromatic diamine compounds or star triphenyl amine compound, or carbazole polymer etc.
According to the organic electroluminescence device that can send white light provided by the present invention, it is characterized in that, the used material of described hole blocking layer is to have electron transport ability and a class material that can blocking hole, as in poly N-vinyl carbazole, BCP, two (2-methyl-8-quinoline acid group closes) tri-phenyl-silane aluminium alcoholates (III), two (2-methyl-8-quinoline acid group closes) 4-phenol aluminium (III) or two (2-methyl-8-quinoline acid group closes) the 4-phenylphenol aluminium (III) one or more.
According to the organic electroluminescence device that can send white light provided by the present invention, it is characterized in that described metal complex material is to have the compounds that central metal atom constitutes, as oxine aluminium (Alq
3) or oxine gallium (Gaq
3) or two [2-(2-hydroxy phenyl-1)-pyridine] beryllium (Bepp
2) etc.
According to the organic electroluminescence device that can send white light provided by the present invention, it is characterized in that Suo Shu oxadiazole electron-like transferring material is 2-(4-diphenyl)-5-(4-2-methyl-2-phenylpropane base)-1,3,4-oxadiazole (PBD), described imidazoles electron transport material is 1,3,5-three (N-phenyl-2-benzimidazolyl-2 radicals) benzene (TPBI); Described aromatic diamine compounds is N, N '-two-(3-aminomethyl phenyl)-N, N '-diphenyl-[1,1 '-xenyl]-4,4 '-diamines (TPD) or N, N '-two (3-naphthyl)-N, N '-diphenyl-[1,1 '-diphenyl]-4,4 '-diamines (NPB) and derivative thereof, described star triphenyl amine compound is three-[4-(5-phenyl-2-thienyl) benzene] amine (PTDATA series), and described carbazole polymer is polyvinylcarbazole (PVK) or monomer whose etc.
According to the organic electroluminescence device that can send white light provided by the present invention, it is characterized in that described electrically-conductive backing plate is ito substrate or sheet metal or silicon substrate; Described substrate is glass or flexible substrate or sheet metal etc., and wherein flexible substrate is ultra-thin solid-state thin slice, polyesters or poly-phthalimide compounds etc.; Described anode layer is metal-oxide film or metallic film, and this metal-oxide film is ito thin film or zinc-oxide film or zinc tin oxide film, and this metallic film is the higher metallic films of work function such as gold, copper, silver; Described anode layer is PEDOT:PSS or PANI class organic conductive polymer; Described cathode layer comprises resilient coating and metal level, described cushioning layer material is the inorganic molecules compound or has the organic compound of high minimum unoccupied energy level (LUMO) energy level, for example LiF or CsF, described metal layer material is metallic film or alloy firm, and this metallic film is the alloy firm of the lower metallic film of lithium or work functions such as magnesium or calcium or strontium or aluminium or indium or they and copper or gold or silver etc.
The preparation method that this can send the organic electroluminescence device of white light may further comprise the steps:
1. utilize washing agent, ethanolic solution, acetone soln and deionized water that substrate or electrically-conductive backing plate are carried out ultrasonic cleaning, it is dry to clean the back;
2. substrate is sent to the preparation of carrying out electrode in the vacuum evaporation chamber, described electrode comprises anode layer or cathode layer, perhaps electrically-conductive backing plate is carried out array and handles;
The substrate that 3. will prepare electrode moves into vacuum chamber, under oxygen pressure ring border to carrying out the preliminary treatment of low energy oxygen plasma;
4. the substrate after will handling sets gradually organic functional layer according to device architecture, and described organic function layer comprises one or more in luminescent layer, carrier blocking layers, implanted layer and the resilient coating;
5. finish to carry out in the vaporization chamber of back at condition of high vacuum degree the preparation of another electrode in the organic layer spin coating, described electrode comprises cathode layer or anode layer;
6. ready-made device is sent to glove box and encapsulates, glove box is an atmosphere of inert gases;
7. current-voltage-the light characteristic of test component, the luminescent spectrum parameter of test component simultaneously.
Wherein the setting of step organic function layer 4. also can replace with the method that vacuum evaporation or spin coating combine with vacuum evaporation according to the organic material difference that is adopted.
Organic electroluminescence device provided by the present invention, material therefor are organic substance/macromolecule, thereby the range of choice of material is wide, can realize the demonstration of white light; Related material is the organic semiconducting materials of the function admirable of routine, the efficient height of device, synthetic and the device technical maturity of material therefor, cost are low, compare with the device that obtains function admirable by synthetic new material of cost plenty of time, this research has been opened up an approach that shows unique characteristics from the angle of technology, used compound all has stronger fluorescence among the present invention in liquid and solid film, has quite high heat, light, electricity and physical chemistry equistability simultaneously again; Driving voltage is low, and luminosity and luminous efficiency height can be made into flexible display device; Fast, the luminous visual angle of response speed is wide; Device is ultra-thin, volume is little, in light weight; What is more important, the selection that luminous organic material is a functional material with its intrinsic diversity provides broad scope, by to the design of organic molecular structure, assemble and cut out, can satisfy many-sided different needs and be easy to realize that large tracts of land shows, in addition, its preparation method is rationally simple, easy operating.
Description of drawings
Fig. 1 is the structural representation of organic electroluminescence device provided by the present invention and the structural representation of embodiment 1;
Fig. 2 is the structural representation of embodiment 2 provided by the present invention;
Fig. 3 is the structural representation of embodiment 3 provided by the present invention;
Fig. 4 is the test curve figure of the luminescent spectrum of white light parts under the 10V forward voltage described in the embodiment 1 provided by the present invention.
Wherein, 1, substrate (perhaps electrically-conductive backing plate), 2, anode layer, 3, organic layer, 4, cathode layer, 5, additional power source, 31, hole transmission layer is double does white luminous layer, and 32, the double electron transfer layer of doing of hole blocking layer, 33, hole transmission layer is double does white luminous layer, 34, hole blocking layer, 35, electron transfer layer.
Embodiment
The present invention is further illustrated below in conjunction with accompanying drawing.
Technical scheme of the present invention provides a kind of organic electroluminescence device that can send white light, as shown in Figure 1, and 1, substrate, 2, anode layer, 3, organic layer, 4, cathode layer, 5, additional power source.
As shown in Figure 2, the structure of device comprises substrate 1, anode layer 2, and organic layer 3, cathode layer 4, additional power source 5, hole transmission layer is double does white luminous layer 31, the double electron transfer layer 32 of doing of hole blocking layer, device emits white light under the driving of additional power source 5.
As shown in Figure 3, the structure of device comprises substrate 1, anode layer 2, and organic layer 3, cathode layer 4, additional power source 5, hole transmission layer is double does white luminous layer 33, hole blocking layer 34, electron transfer layer 35, device emits white light under the driving of additional power source 5.
Hole transmission layer among the present invention is double, and to do white luminous layer 31,33 material be that aromatic diamine compounds or star triphenyl amine compound or metal complex or other class blue light materials and carbazole polymer mix.Described aromatic diamine compounds can be N, N '-two-(3-aminomethyl phenyl)-N, N '-diphenyl-[1,1 '-xenyl]-4,4 '-diamines or N, N '-two (3-naphthyl)-N, N '-diphenyl-[1,1 '-diphenyl]-4,4 '-diamines, described star triphenyl amine compound can be three-[4-(5-phenyl-2-thienyl) benzene] amine or m-TDATA, and described carbazole polymer can be a polyvinylcarbazole, described metal complex can be BAlq, and other class blue light materials can be DPVBi, BCzVB, Perylene, BczVBi etc.
Hole blocking layer among the present invention is double, and to do electron transfer layer 32,34 materials be the hole barrier materials with electron transport ability, as poly N-vinyl carbazole, BCP, two (2-methyl-8-quinoline acid group closes) tri-phenyl-silane alcohol (silanolate) aluminium (III), two (2-methyl-8-quinoline acid group closes) 4-phenol aluminium (III) or two (2-methyl-8-quinoline acid group closes) 4-phenylphenol aluminium (III).
Adopt the white light OLED device architecture of the present invention's preparation to be exemplified below:
1. glass/ITO/ hole transmission layer is double does white luminous layer/cathode layer
2. the double double electron transfer layer/cathode layer of doing of white luminous layer/hole blocking layer of doing of glass/ITO/ hole transmission layer
3. the double white luminous layer/hole blocking layer/electron transfer layer/cathode layer of doing of glass/ITO/ hole transmission layer
4. glass/ITO/ hole transmission layer/white luminous layer/cathode layer
5. the double electron transfer layer/cathode layer of doing of glass/ITO/ hole transmission layer/white luminous layer/hole blocking layer
6. glass/ITO/ hole transmission layer/white luminous layer/hole blocking layer/electron transfer layer/cathode layer
7. glass/conducting polymer/hole transmission layer is double does white luminous layer/cathode layer
8. the double double electron transfer layer/cathode layer of doing of white luminous layer/hole blocking layer of doing of glass/conducting polymer/hole transmission layer
9. the double white luminous layer/hole blocking layer/electron transfer layer/cathode layer of doing of glass/conducting polymer/hole transmission layer
10. glass/conducting polymer/hole transmission layer/white luminous layer/cathode layer
Below be specific embodiments of the invention:
As shown in Figure 1, the hole transmission layer in the structure of device is double does white luminous layer 3.
The hole transmission layer of device is double, and to do white luminous layer material be PVK:NPB, cathode layer Mg:Ag alloy.The entire device structrual description is:
Glass substrate/ITO/PVK:NPB (80nm)/Mg:Ag (200nm)
The preparation method is as follows:
1. utilize washing agent, ethanolic solution, acetone soln and deionized water that the conductive substrate ito glass is carried out ultrasonic cleaning, clean the back and dry up with drying nitrogen.Wherein the ITO film above the glass substrate is as the anode layer of device, and the square resistance of ITO film is 10 Ω/, and thickness is 180nm.
2. dried substrate being moved into vacuum chamber, is under the oxygen pressure ring border of 20Pa ito glass to be carried out low energy oxygen plasma preliminary treatment 10 minutes at air pressure, and sputtering power is 0～20W.
3. the substrate after will handling carries out the spin coating of white luminous organic film in spin coater.
4. finish the preparation of laggard row metal electrode at the organic layer evaporation.Its air pressure is 3 * 10
-3Pa, evaporation speed is～1nm/s, Mg in the alloy, the Ag ratio is～10: 1, thicknesses of layers is 100nm.Evaporation speed and thickness are by near the film thickness gauge monitoring that is installed in the substrate.
5. ready-made device is encapsulated at glove box, glove box is 99.9% nitrogen atmosphere.
6. current-voltage-the light characteristic of test component, the luminescent spectrum parameter of test component simultaneously.
The luminescent spectrum that device presses down in the 10V forward drive is referring to accompanying drawing 5.
As shown in Figure 2, the organic layer 3 in the structure of device comprises double white luminous layer 31, the double electron transfer layer 32 of doing of hole blocking layer done of hole transmission layer.
The hole transmission layer of device is double, and to do white luminous layer material be PVK:NPB, the double electron transport material BCP that is of hole blocking layer, cathode layer Mg:Ag alloy.The entire device structrual description is:
Glass substrate/ITO/PVK:NPB (80nm)/BCP (20nm)/Mg:Ag (100nm)
The preparation of devices flow process is similar to embodiment 1.
As shown in Figure 3, the organic layer 3 in the structure of device comprises double white luminous layer 33, hole blocking layer 34, the electron transfer layer 35 done of hole transmission layer.
The hole transmission layer of device is double, and to do white luminous layer material be PVK:NPB, hole barrier materials BCP, electron transport material Alq
3, cathode layer Mg:Ag alloy.The entire device structrual description is:
Flexible substrate/ITO/PVK:NPB (80nm)/BCP (20nm)/Alq
3(10nm)/Mg:Ag (100nm)
The preparation of devices flow process is similar to embodiment 1.
Organic layer in the structure of device comprises hole transmission layer, white luminous layer, hole blocking layer, electron transfer layer.
The hole transmission layer of device is NPB, and white luminous layer material is PVK:NPB, hole barrier materials BCP, electron transport material Alq
3, cathode layer Mg:Ag alloy.The entire device structrual description is:
Flexible substrate/ITO/NPB (10nm)/PVK:NPB (80nm)/BCP (20nm)/Alq
3(10nm)/Mg:Ag (100nm)
The preparation of devices flow process is similar to embodiment 1.
Claims (8)
1. organic electroluminescence device that can send white light, comprise electrically-conductive backing plate or substrate, anode layer, cathode layer, described anode layer or cathode layer are positioned at substrate or electrically-conductive backing plate surface, between described anode layer and the cathode layer organic function layer is set, which comprises at least luminescent layer, this luminescent layer is the organic material layer that sends white light, under the driving of additional power source, send white light, it is characterized in that: the described white light that sends is that the blue light that sent by the blue light organic material and the electricity in the organic functional material layer cause that exciplex is luminous to mix, it is aromatic diamines compound N PB that this electricity causes the sharp compound of base, the luminous compound of a kind of energy that the mixture of star triphenyl amine compound and carbazole polymer PVK is produced after power drives, light that this compound sent and blue light are sent white light; This blueness organic material is PVK and NPB.
2. the organic electroluminescence device that can send white light according to claim 1, it is characterized in that, described aromatic diamine compounds is N, N '-two-(3-aminomethyl phenyl)-N, N '-diphenyl-[1,1 '-xenyl]-4,4 '-diamines or N, N '-two (3-naphthyl)-N, N '-diphenyl-[1,1 '-diphenyl]-4,4 '-diamines, described star triphenyl amine compound is three-[4-(5-phenyl-2-thienyl) benzene] amine or m-TDATA, and described carbazole polymer is a polyvinylcarbazole, and described metal complex is BAlq.
3. the organic electroluminescence device that can send white light according to claim 1, it is characterized in that, described cathode layer and anode layer are respectively arranged with implanted layer, described organic function layer also comprises electron transfer layer, hole transmission layer and the hole blocking layer with electron transport ability, described electric transmission layer material and implanted layer material can be metal complex material or person's oxadiazole electron-like transferring material, perhaps imidazoles electron transport material; Described hole transport layer material is aromatic diamine compounds or star triphenyl amine compound, or carbazole polymer.
4. the organic electroluminescence device that can send white light according to claim 3, it is characterized in that described hole blocking layer is one or more in poly N-vinyl carbazole, BCP, two (2-methyl-8-quinoline acid group closes) tri-phenyl-silane aluminium alcoholates (III), two (2-methyl-8-quinoline acid group closes) 4-phenol aluminium (III) or two (2-methyl-8-quinoline acid group closes) the 4-phenylphenol aluminium (III).
5. the organic electroluminescence device that can send white light according to claim 3 is characterized in that, described metal complex material is oxine aluminium or oxine gallium or two [2-(2-hydroxy phenyl-1)-pyridine] beryllium.
6. the organic electroluminescence device that can send white light according to claim 3, it is characterized in that Suo Shu oxadiazole electron-like transferring material is 2-(4-diphenyl)-5-(4-2-methyl-2-phenylpropane base)-1,3, the 4-oxadiazole, described imidazoles electron transport material is 1,3,5-three (N-phenyl-2-benzimidazolyl-2 radicals) benzene; Described aromatic diamine compounds is N, N '-two-(3-aminomethyl phenyl)-N, N '-diphenyl-[1,1 '-xenyl]-4,4 '-diamines or N, N '-two (3-naphthyl)-N, N '-diphenyl-[1,1 '-diphenyl]-4,4 '-diamines (NPB) or its derivative, described star triphenyl amine compound is three-[4-(5-phenyl-2-thienyl) benzene] amine, and described carbazole polymer is polyvinylcarbazole or monomer whose.
7. the organic electroluminescence device that can send white light according to claim 1 is characterized in that, described electrically-conductive backing plate is ito substrate or sheet metal or silicon substrate; Described substrate is glass or flexible substrate or sheet metal, and wherein flexible substrate is ultra-thin solid-state thin slice, polyesters or poly-phthalimide compounds; Described anode layer is metal-oxide film or metallic film, and this metal-oxide film is ito thin film or zinc-oxide film or zinc tin oxide film, and this metallic film is the metallic film of gold or copper or silver; Described anode layer is PEDOT:PSS or PANI class organic conductive polymer.
8. the preparation method that can send the organic electroluminescence device of white light is characterized in that, may further comprise the steps:
1. utilize washing agent, ethanolic solution, acetone soln and deionized water that the conductive substrate ito glass is carried out ultrasonic cleaning, cleaning the back dries up with drying nitrogen, wherein the ITO film above the glass substrate is as the anode layer of device, and the square resistance of ITO film is 10 Ω/, and thickness is 180nm;
2. dried substrate being moved into vacuum chamber, is under the oxygen pressure ring border of 20Pa ito glass to be carried out low energy oxygen plasma preliminary treatment 10 minutes at air pressure, and sputtering power is 0～20W;
3. the substrate after will handling carries out the spin coating of white luminous organic film in spin coater;
4. finish the preparation of laggard row metal electrode at the organic layer evaporation.Its air pressure is 3 * 10
-3Pa, evaporation speed is 1nm/s, Mg in the alloy, the Ag ratio is 10: 1, and thicknesses of layers is 100nm, and evaporation speed and thickness are by near the film thickness gauge monitoring that is installed in the substrate;
5. ready-made device is encapsulated at glove box, glove box is 99.9% nitrogen atmosphere;
6. current-voltage-the light characteristic of test component, the luminescent spectrum parameter of test component simultaneously.
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