CN100521285C - Organic electroluminescent apparatus and its manufacturing method, positive hole refiller - Google Patents
Organic electroluminescent apparatus and its manufacturing method, positive hole refiller Download PDFInfo
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Abstract
The OEL device comprises an anode on a substrate, and at least one hole injection device that includes at least a first and second material layer stacked on anode, an organic luminescent layer on the injection device, and an electron source layer on the luminescent layer. Wherein, the former first material layer comprises at least a mixture of the first conductive material and an organic material, and the second material layer comprises at least a second conductive material.
Description
Technical field
The present invention relates to a kind of Organnic electroluminescent device and manufacture method thereof, refer to a kind of Organnic electroluminescent device and manufacture method thereof that can reduce driving voltage that have especially.
Background technology
Flat-panel monitor have conventional cathode ray tube (Cathode Ray Tube, CRT) the incomparable advantage of display: power saving, radiationless, volume is little, so flat-panel monitor has replaced cathode-ray tube display gradually.Lifting along with flat panel display, the product price of flat-panel monitor constantly reduces, make flat-panel monitor more universal and towards the development of big display size, and among various flat-panel monitors now, the product that display of organic electroluminescence attracts most attention especially at present.
Please refer to Fig. 1.Fig. 1 is the schematic diagram of existing Organnic electroluminescent device.As shown in Figure 1, existing Organnic electroluminescent device comprises that the anode of being located on the substrate 10 12, is located at the negative electrode 14 of anode 12 tops, and an organic luminous layer 16 of being located between anode 12 and the negative electrode 14.In addition, existing Organnic electroluminescent device also comprises a hole injection layer 18 and a hole transmission layer 20, be located between anode 12 and the organic luminous layer 16, and an electron injecting layer 22 and an electron transfer layer 24, be located between organic luminous layer 16 and the negative electrode 14.The principle of luminosity of Organnic electroluminescent device is summarized as follows.When existing between anode 12 and the negative electrode 14 under the situation of a bias voltage, the hole can enter in the organic luminous layer 16 with characteristics of luminescence through hole injection layer 18 and hole transmission layer 20, and similarly electronics also can enter in the organic luminous layer 16 via electron injecting layer 22 and electron transfer layer 24.Compound tense in organic luminous layer 16 can form exciton (exciton) when electronics and hole, again energy is discharged and get back to ground state (ground State), and in the energy that these are released, because the difference of selected luminescent material, the part energy is discharged with the form of the light of different colours, and form the luminescence phenomenon of Organnic electroluminescent device.
For Organnic electroluminescent device, one of hole injection layer 18 effects are to reduce driving voltage, and then lower the potential barrier between anode 12 and the hole transmission layer 20, and promote luminous efficiency.Generally speaking, existing hole injection layer 18 uses the single organic material layer, NPB for example, or single metal oxide layer, yet on using, exist restriction, particularly under the work function at anode 12 and hole transmission layer 20 interfaces differed bigger situation, existing hole injection layer 18 was limited for the effect that reduces driving voltage, thus cause life-span of Organnic electroluminescent device to shorten or luminous efficiency not good.
Summary of the invention
One of purpose of the present invention is to provide a kind of hole injection device and its manufacture method of Organnic electroluminescent device, to reduce the driving voltage of Organnic electroluminescent device.
For reaching above-mentioned purpose, the invention provides a kind of Organnic electroluminescent device.Above-mentioned Organnic electroluminescent device comprises at least one anode on the substrate, at least one hole injection device be located at, it comprises at least one first material layer of being stacked on this anode and at least one second material layer, at least one organic luminous layer of being located on this hole injection device, and at least one electron source layer of being located on this organic luminous layer.Above-mentioned this first material layer comprises a mixture of at least one first electric conducting material (first conductive material) and at least one organic material, and this second material layer comprises at least one second electric conducting material (secondconductive material).
For reaching above-mentioned purpose, the present invention provides a kind of method of making Organnic electroluminescent device in addition.At first form at least one anode on a substrate.Then form at least one hole injection device on this anode, wherein this hole injection device comprises at least one first material layer and at least one second material layer, and this first material layer comprises a mixture of at least one first electric conducting material and at least one organic material, and this second material layer comprises at least one second electric conducting material.Form at least one organic luminous layer subsequently on this hole injection device, and form at least one electron source layer on this organic luminous layer.
For reaching above-mentioned purpose, the present invention provides a kind of hole injection device in addition.Above-mentioned hole injection device comprises at least one first material layer and at least one second material layer.Above-mentioned this first material layer comprises a mixture of at least one first electric conducting material and at least one organic material, and this second material layer comprises at least one second electric conducting material.
Below be about detailed description of the present invention and accompanying drawing.Yet accompanying drawing is only for reference and aid illustration usefulness, is not to be used for the present invention is limited.
Description of drawings
Fig. 1 is the schematic diagram of existing Organnic electroluminescent device.
Fig. 2 to Fig. 4 is the manufacture method schematic diagram of the Organnic electroluminescent device of one embodiment of the present invention.
Fig. 5 is the voltage of Organnic electroluminescent device of the present invention and the graph of a relation of current density.
Fig. 6 to Fig. 8 is the CONCENTRATION DISTRIBUTION schematic diagram of first material layer of other embodiment of the present invention.
The main element symbol description
10 substrates, 12 anodes
14 negative electrodes, 16 organic luminous layers
18 hole injection layers, 20 hole transmission layers
22 electron injecting layers, 24 electron transfer layers
30 substrates, 32 element regions
34 viewing areas, 40 thin-film transistors
41 grids, 42 dielectric layers
43 semiconductor layers, 44 doped amorphous silicon layers
45 source/drains, 46 protective layers
50 anodes, 52 first material layers
54 second material layers, 56 hole injection devices
58 hole transmission layers, 60 organic luminous layers
62 electron source layers, 64 negative electrodes
66 electron injecting layers, 68 electron transfer layers
Embodiment
Please refer to Fig. 2 to Fig. 4.Fig. 2 to Fig. 4 is the manufacture method schematic diagram of the Organnic electroluminescent device of one embodiment of the present invention.As shown in Figure 2, at first provide a substrate 30, wherein substrate 30 is divided into an element region 32 and a viewing area 34.Because present embodiment selects for use an active organic LED display floater (AMOLED) to be example explanation the present invention, therefore be formed with thin film transistor (TFT) array (TFT array) on the substrate 30, yet if Organnic electroluminescent device is applied to a passive type organic LED display panel, then can not establish thin film transistor (TFT) array, and utilize scan line control Organnic electroluminescent device.In addition, for showing characteristics of the present invention, only demonstrate a thin-film transistor that is electrically connected with Organnic electroluminescent device 40 in the icon.Thin-film transistor comprises that a grid 41, is covered in dielectric layer 42, on the grid 41 and is positioned at semiconductor layer 43 on the dielectric layer 42, is positioned at the doped amorphous silicon layer 44 on the semiconductor layer 43 of grid 41 2 sides, and is stacked in the source/drain 45 on the doped amorphous silicon layer 44.Present embodiment is an example with a bottom gate (bottom gate) thin-film transistor 40, on actual fabrication, also can use the thin-film transistor of top grid (topgate) thin-film transistor 40 or its type, and semiconductor layer 43 can be polysilicon layer, amorphous silicon layer or monocrystalline silicon layer etc.In addition, the material of substrate 30 also can be light-transmitting materials such as glass or quartz, light tight material such as pottery or semiconductor material, or bendable material such as plastics.
Then on the dielectric layer 42 of viewing area 34, form an anode 50, and be electrically connected with the source/drain 45 of thin-film transistor 40, wherein present embodiment selects for use work function to be about the material of the aluminium neodymium alloy (AlNd) of 3.8 electron-volts (eV) as anode 50, the material that can select for use other to be suitable for but the material of anode 50 is not limited thereto.On source/drain 45, cover a protective layer 46 subsequently.
As shown in Figure 3, then on anode 50, form at least one first material layer 52.First material layer comprises the mixture of at least one first electric conducting material and at least one organic material.Present embodiment selects for use silver (work function is about 4.7ev) as first electric conducting material, organic material is then selected N for use, N '-two-((1-naphthyl)-N, N '-diphenyl-1,1 '-xenyl)-4,4 '-diamines (NPB), simultaneously in said mixture the shared ratio of silver approximately between 1% to 10%, and serve as preferred with 5%, the shared ratio of organic material and serves as preferred with 95% then approximately between 90% to 99%.It should be noted that in addition first electric conducting material and organic material are a homogeneous mixture in the present embodiment, but be not limited to this, first electric conducting material is not limited to silver simultaneously, also can select for example nickel of other metal for use, gold, platinum etc., or other work function is greater than 4 electron-volts metal or alloy, and organic material also is not limited to use NPB, and can be the organic material that other is suitable for, polyethylene dioxythiophene/kayexalate (polyethylenedioxythiophene/polystyrene sulphonate for example, PEDOT:PSS), pi-conjugated molecule-4,4 ', 4 ＂-three idol (3-aminomethyl phenyl aniline) triphenylamine (4,4 ', 4 ＂-tris (3-methylphenylphenylamino) triphenylamine, m-MTDATA) or polyaniline (polyaniline) etc.Then, on first material layer 52, form one second material layer 54 again.Second material layer 54 comprises at least one second electric conducting material, and second electric conducting material selects for use work function to be about the tungsten oxide of 5.2ev in the present embodiment, but second electric conducting material also can be selected other metal oxide for use, for example praseodymium oxide, vanadium oxide or molybdenum oxide etc., or other metal that is fit to, also or the mixture of metal and metal oxide.Above-mentioned first material layer 52 and second material layer 54 promptly constitute the hole injection device 56 of present embodiment.
As shown in Figure 4, on second material layer 54, form a hole transmission layer 58, an organic luminous layer 60 subsequently in regular turn, and an electron source layer 62, promptly constitute Organnic electroluminescent device of the present invention.Wherein electron source layer 62 comprises a negative electrode 64 and an electron transfer layer 68, can comprise an electron injecting layer 66 again between electron transfer layer 68 and the negative electrode 64 certainly.In addition, above-mentioned hole transmission layer 58, organic luminous layer 60, electron transfer layer 68, electron injecting layer 66 can be existing any suitable material with negative electrode 64 employed materials, and there is no particular restriction to this in the present invention.For instance, hole transmission layer 58 can use NPB, and electron transfer layer 62 can use Alq, and organic luminous layer 60 then can use any luminous organic material or high-molecular luminous material.
The Organnic electroluminescent device of the invention described above embodiment uses metal and organic material first material layer of forming 52 and second material layer 54 that metal oxide is formed to form hole injection device 56, use the effect that reaches effective attenuating driving voltage, yet organic light emitting apparatus of the present invention is not limited to the foregoing description, and can select for use the material of other kind to form hole injection device 56.Please continue with reference to figure 4, in another preferred embodiment of the present invention, first electric conducting material of first material layer 52 is selected tungsten oxide (work function is about 5.2ev) for use, and organic material is then selected NPB for use, and second electric conducting material of second material layer 54 is then also selected tungsten oxide for use.In the mixture of above-mentioned tungsten oxide and NPB, the shared ratio of tungsten oxide is approximately between 1% to 99%, and serving as preferred between 10% to 30%, and the shared ratio of NPB is approximately between 1% to 99%, and serving as preferred between 70% to 90%, in the present embodiment simultaneously, tungsten oxide and NPB are a homogeneous mixture, but are not limited to this.Other first electric conducting material also can be selected other metal oxide for use, for example praseodymium oxide, vanadium oxide or molybdenum oxide etc., or the mixture of metal and metal oxide, and organic material also is not limited to NPB.In addition, second electric conducting material also is not limited to tungsten oxide, and can be praseodymium oxide, vanadium oxide, molybdenum oxide or other metal oxide that is fit to, or other metal that is fit to, also or the mixture of metal and metal oxide.
Above-mentioned is two preferred embodiments of the hole injection device of Organnic electroluminescent device of the present invention.Please refer to Fig. 5, Fig. 5 is the voltage of Organnic electroluminescent device of the present invention and the graph of a relation of current density.The voltage of five kinds of different holes of A to E injection device compositions and the relation of current density have been compared among Fig. 5, wherein in this experimental data with the aluminium neodymium alloy as anode, NPB as hole transmission layer, Alq as organic luminous layer, cesium carbonate and Alq as electron transfer layer, lithium fluoride as electron injecting layer, and silver as negative electrode.In addition, data A is that the homogeneous mixture by silver and NPB that first embodiment is disclosed constitutes first material layer, and the hole injection device that constitutes second material layer by tungsten oxide, data B then is that the homogeneous mixture by tungsten oxide and NPB that second embodiment is disclosed constitutes first material layer, and the hole injection device that is made of second material layer tungsten oxide.In addition, data C to E then is a control group, wherein data C for use separately tungsten oxide as the practice of hole injection device, data D for utilizing NPB separately as first material layer, and with the practice of tungsten oxide as second material layer formation hole injection device, data E then constitutes the practice of hole injection device for the mixture that utilizes tungsten oxide and NPB separately.As shown in Figure 5, the hole injection device of the present invention two embodiment (data A, B) all can effectively reduce the driving voltage of Organnic electroluminescent device, by contrast, the then obvious driving voltage of the driving voltage of other hole injection device (data C, D, E) greater than hole of the present invention injection device.
What be worth explanation separately is that first material layer of above-mentioned two embodiment of the present invention is an example with the homogeneous mixture of first electric conducting material and organic material all, feature of the present invention and effect are described, yet the composition of first material layer is not limited to homogeneous mixture, and also can be heterogeneous mixture, for example have the mixture that gradient concentration distributes.Please refer to Fig. 6 to Fig. 8, Fig. 6 to Fig. 8 is the CONCENTRATION DISTRIBUTION schematic diagram of first material layer of other embodiment of the present invention, wherein in Fig. 6 to Fig. 8, transverse axis is represented the thickness percentage of first material layer, and the longitudinal axis is then represented the percentage of first electric conducting material and organic material.As shown in Figure 6, the concentration of first electric conducting material of first material layer and presents and increases progressively distribution between 1% to 10%, and the concentration of organic material and presents the distribution of successively decreasing then between 90% to 99%.As shown in Figure 7, the concentration of first electric conducting material of first material layer and presents the distribution of successively decreasing between 1% to 10%, and the concentration of organic material and presents and increases progressively distribution then between 90% to 99%.Shown in 8, the concentration of first electric conducting material of first material layer is between 1% to 10%, the concentration of interface portion that is positioned at two sides simultaneously is lower and present Gradient distribution, the concentration of organic material is then between 90% to 99%, and the concentration of the interface portion of two sides is higher and present Gradient distribution simultaneously.Above-mentioned Fig. 6 extremely CONCENTRATION DISTRIBUTION shown in Figure 8 is that metal is an example with first electric conducting material, the embodiment of the inhomogeneous CONCENTRATION DISTRIBUTION of the present invention's first material layer is described, if first electric conducting material is selected the mixture of metal oxide or metal/metal oxide for use, then the scope of CONCENTRATION DISTRIBUTION should be looked hole injection effect and be done appropriateness adjustment.
Hole of the present invention injection device utilizes the part of the mixture of metal or metal oxide and organic material as the hole injection device, can effectively promote hole concentration and hole transport speed, and then effectively reduces the driving voltage of Organnic electroluminescent device.What deserves to be explained is selection and its mixed proportion of above-mentioned first electric conducting material and organic material in addition, and the selection of second electric conducting material can differently according to the material of anode and hole transmission layer or organic luminous layer suitably adjust, to be applicable to the interface of various work functions.
In sum, the hole injection device of Organnic electroluminescent device of the present invention can effectively reduce driving voltage, promote hole concentration and hole transport speed, for various different work functions interface good electrical properties is arranged all simultaneously.
The above only is the preferred embodiments of the present invention, and all equalizations of doing according to claim of the present invention change and modify, and all should belong to covering scope of the present invention.
Claims (37)
1. Organnic electroluminescent device comprises:
One anode is located on the substrate;
One hole injection device, comprise at least one first material layer and at least one second material layer that are stacked on this anode, this first material layer comprises a mixture of at least one first electric conducting material and at least one organic material, and this second material layer comprises at least one second electric conducting material, and wherein this second electric conducting material comprises the mixture of metal, metal oxide or above-mentioned material;
One organic luminous layer is located on this hole injection device; And
One electron source layer is located on this organic luminous layer.
2. Organnic electroluminescent device as claimed in claim 1, wherein included this first electric conducting material of this first material layer and this mixture of this organic material are a homogeneous mixture.
3. Organnic electroluminescent device as claimed in claim 1, wherein this mixture of included this first electric conducting material of this first material layer and this organic material is one to have the mixture that gradient concentration distributes.
4. Organnic electroluminescent device as claimed in claim 1, wherein this first electric conducting material comprises the mixture of metal, metal oxide or above-mentioned material.
5. Organnic electroluminescent device as claimed in claim 4, wherein this first electric conducting material is a metal, and this metal account for this mixture 1% to 10% between, and this organic material account for this mixture 90% to 99% between.
6. Organnic electroluminescent device as claimed in claim 5, wherein this metal of this first electric conducting material accounts for 5% of this mixture, and this organic material accounts for 95% of this mixture.
7. Organnic electroluminescent device as claimed in claim 4, wherein this first electric conducting material is a metal, and the work function of this metal is greater than 4 electron-volts.
8. Organnic electroluminescent device as claimed in claim 4, wherein this first electric conducting material is a metal oxide, and this metal oxide account for this mixture 1% to 99% between, and this organic material account for this mixture 1% to 99% between.
9. Organnic electroluminescent device as claimed in claim 8, wherein this metal oxide of this first electric conducting material accounts for 10% to 30% of this mixture, and this organic material account for this mixture 70% to 90% between.
10. Organnic electroluminescent device as claimed in claim 1, wherein this organic material of this first material layer comprises N, N '-two-((1-naphthyl)-N, N '-diphenyl-1,1 '-xenyl)-4,4 '-diamines, polyethylene dioxythiophene/kayexalate, pi-conjugated molecule-4,4 ', 4 ＂-three idol (3-aminomethyl phenyl aniline) triphenylamine or polyaniline.
11. Organnic electroluminescent device as claimed in claim 1, wherein this second electric conducting material is a metal oxide, and this metal oxide comprises tungsten oxide, praseodymium oxide, vanadium oxide or molybdenum oxide.
12. Organnic electroluminescent device as claimed in claim 1 also comprises a hole transmission layer, is located between this organic luminous layer and this hole injection device.
13. Organnic electroluminescent device as claimed in claim 1, this electron source layer wherein, comprise a negative electrode and an electron transfer layer, this electron transfer layer is located between this organic luminous layer and this negative electrode, wherein can comprise an electron injecting layer in addition between this electron transfer layer and this negative electrode.
14. a method of making Organnic electroluminescent device comprises:
On a substrate, form an anode;
Form a hole injection device on this anode, this hole injection device comprises at least one first material layer and at least one second material layer, this first material layer comprises a mixture of at least one first electric conducting material and at least one organic material, and this second material layer comprises at least one second electric conducting material;
On this hole injection device, form an organic luminous layer; And
Form an electron source layer on this organic luminous layer, wherein this second electric conducting material comprises the mixture of metal, metal oxide or above-mentioned material.
15. method as claimed in claim 14 also is included in and forms a hole transmission layer between this organic luminous layer and this hole injection device.
16. method as claimed in claim 14, wherein this electron source layer comprises a negative electrode and an electron transfer layer, and this electron transfer layer is formed between this organic luminous layer and this negative electrode, can comprise an electron injecting layer in addition between this electron transfer layer and the negative electrode.
17. method as claimed in claim 14, wherein this first electric conducting material comprises the mixture of metal, metal oxide or above-mentioned material.
18. method as claimed in claim 17, wherein this first electric conducting material is a metal, and this metal account for this mixture 1% to 10% between, and this organic material account for this mixture 90% to 99% between.
19. method as claimed in claim 18, wherein this metal of this first electric conducting material accounts for 5% of this mixture, and this organic material accounts for 95% of this mixture.
20. method as claimed in claim 17, wherein this first conductive material layer is a metal, and the work function of this metal is greater than 4 electron-volts.
21. method as claimed in claim 17, wherein this first electric conducting material is a metal oxide, and this metal oxide account for this mixture 1% to 99% between, and this organic material account for this mixture 1% to 99% between.
22. method as claimed in claim 21, wherein this metal oxide of this first electric conducting material of this first material layer accounts for 10% to 30% of this mixture, and this organic material account for this mixture 70% to 90% between.
23. method as claimed in claim 14, wherein this organic material of this first material layer comprises N, N '-two-((1-naphthyl)-N, N '-diphenyl-1,1 '-xenyl)-4,4 '-diamines, polyethylene dioxythiophene/kayexalate, pi-conjugated molecule-4,4 ', 4 ＂-three idol (3-aminomethyl phenyl aniline) triphenylamine or polyaniline.
24. method as claimed in claim 14, wherein this second electric conducting material is a metal oxide, and this metal oxide comprises tungsten oxide, praseodymium oxide, vanadium oxide or molybdenum oxide.
25. method as claimed in claim 14, wherein included this first electric conducting material of this first material layer and this mixture of this organic material are a homogeneous mixture.
26. method as claimed in claim 14, wherein this mixture of included this first electric conducting material of this first material layer and this organic material is one to have the mixture that gradient concentration distributes.
27. a hole injection device comprises:
At least one first material layer and at least one second material layer, this first material layer comprises a mixture of at least one first electric conducting material and at least one organic material, and this second material layer comprises at least one second electric conducting material, and wherein this second electric conducting material comprises the mixture of metal, metal oxide or above-mentioned material.
28. hole as claimed in claim 27 injection device, wherein included this first electric conducting material of this first material layer and this mixture of this organic material are a homogeneous mixture.
29. hole as claimed in claim 27 injection device, wherein this mixture of included this first electric conducting material of this first material layer and this organic material is one to have the mixture that gradient concentration distributes.
30. hole as claimed in claim 27 injection device, wherein this first electric conducting material comprises the mixture of metal, metal oxide or above-mentioned material.
31. hole as claimed in claim 30 injection device, wherein this first electric conducting material is a metal, and this metal account for this mixture 1% to 10% between, and this organic material account for this mixture 90% to 99% between.
32. hole as claimed in claim 31 injection device, wherein this metal of this first electric conducting material of this first material layer accounts for 5% of this mixture, and this organic material accounts for 95% of this mixture.
33. hole as claimed in claim 30 injection device, wherein this first material layer is a metal, and the work function of this metal is greater than 4 electron-volts.
34. hole as claimed in claim 30 injection device, wherein this first electric conducting material of this first material layer is a metal oxide, and this metal oxide account for this mixture 1% to 99% between, and this organic material account for this mixture 1% to 99% between.
35. hole as claimed in claim 34 injection device, wherein this metal oxide of this first electric conducting material of this first material layer accounts for 10% to 30% of this mixture, and this organic material account for this mixture 70% to 90% between.
36. hole as claimed in claim 27 injection device, wherein this organic material of this first material layer comprises N, N '-two-((1-naphthyl)-N, N '-diphenyl-1,1 '-xenyl)-4,4 '-diamines, polyethylene dioxythiophene/kayexalate, pi-conjugated molecule-4,4 ', 4 ＂-three idol (3-aminomethyl phenyl aniline) triphenylamine or polyaniline.
37. hole as claimed in claim 27 injection device, wherein this second electric conducting material is a metal oxide, and this metal oxide comprises tungsten oxide, praseodymium oxide, vanadium oxide or molybdenum oxide.
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| CN104009177A (en) * | 2013-02-26 | 2014-08-27 | 海洋王照明科技股份有限公司 | Organic electroluminescent device and preparation method |
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