CN102842678A - Organic electroluminescent device and method for producing same - Google Patents
Organic electroluminescent device and method for producing same Download PDFInfo
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- CN102842678A CN102842678A CN2011101679340A CN201110167934A CN102842678A CN 102842678 A CN102842678 A CN 102842678A CN 2011101679340 A CN2011101679340 A CN 2011101679340A CN 201110167934 A CN201110167934 A CN 201110167934A CN 102842678 A CN102842678 A CN 102842678A
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Abstract
The invention relates to an organic electroluminescent device. The organic electroluminescent device comprises an anode electric conduction substrate, a light-emitting layer and a cathode which are sequentially stacked, and further comprises a mixing layer which is arranged between the anode electric conduction substrate and the light-emitting layer and is used for reducing the hole transmission rate, the mixing layer comprises multiple layers of sub mixing layers which are formed by mixing a hole-transport material and an electron transport material according to a progressive ratio, and the molar ratio of the hole-transport material and the electron transport material in the sub mixing layers is gradually reduced along the direction approaching the light-emitting layer. The organic electroluminescent device adopts the hole-transport material and the electron transport material to form the mixing layer in a mixing manner according to the progressive ratio, hole transmission capacity can be effectively alleviated, the hole transmission rate can be reduced, balance between the hole transmission rate and carrier transmission rate can be achieved, hole electrons are composited in the electroluminescent layer as much as possible, and accordingly, the light-emitting efficiency of the whole organic electroluminescent device is improved. In addition, the invention further relates to a method for producing the organic electroluminescent device.
Description
[technical field]
The present invention relates to the electronic device correlative technology field, relate in particular to a kind of organic electroluminescence device and preparation method thereof.
[background technology]
Organic electroluminescence device (OLED) has some unique advantages: (1) OLED belongs to the diffused area source, need not obtain large-area white light source through extra light-conducting system as light-emitting diode (LED); (2) owing to the diversity of luminous organic material, the OLED illumination is the light of design color as required, no matter be micromolecule OLED at present, or polymer organic LED (PLED) has all obtained to comprise the light of white-light spectrum at interior all colours; (3) OLED can make on multiple substrate such as glass, pottery, metal, plastic or other material, thereby free more when making the design lighting source; (4) adopt to make the mode that OLED shows and make the OLED illumination panel, can be in illumination display message; (5) OLED also can be used as controlled look in illuminator, allows the user to regulate the light atmosphere according to individual demand.
Yet because OLED holes transmission rate is higher than electric transmission speed, this unbalanced transmission rate tends to cause the exciton recombination zone territory not at luminescent layer, thereby influences the luminous efficiency of OLED.
[summary of the invention]
Based on this, be necessary to provide the comparatively organic electroluminescence device and preparation method thereof of balance of a kind of hole and electric transmission speed.
A kind of organic electroluminescence device; Comprise the anode conducting substrate, luminescent layer and the negative electrode that stack gradually; In addition; This organic electroluminescence device also comprises the mixed layer that is used to reduce hole transport speed that is located between said anode conducting substrate and the said luminescent layer; Said mixed layer comprises the sub-mixed layer of multilayer that is formed by gradual mixed by hole mobile material and electron transport material, and the mol ratio of said multilayer sub-mixed layer holes transferring material and electron transport material reduces with the direction near said luminescent layer gradually.
In preferred embodiment, said hole mobile material is phenylmorpholine, N, N '-diphenyl-N, and N '-two (3-aminomethyl phenyl)-(1,1 '-xenyl)-4,4 '-diamines or 4,4 ', 4 " three (carbazole-9-yl) triphenylamines; Said electron transport material is that oxine aluminium, 4-biphenyl phenolic group-two (2-methyl-oxine) close aluminium, N-aryl benzimidazole or 4,7-diphenyl-1,10-phenanthroline.
In preferred embodiment, the scope of the mol ratio of said multilayer sub-mixed layer holes transferring material and electron transport material is 6: 1～1: 6.
In preferred embodiment, said mixed layer comprises 3～6 straton mixed layers.
In preferred embodiment, the thickness of said anode conducting substrate is that the thickness of the thickness 3～5nm of 100～150nm, said mixed layer, said luminescent layer is that the thickness of 5～20nm, said negative electrode is 80～200nm.
In preferred embodiment, said mixed layer comprises 5 straton mixed layers, and the mol ratio of said 5 straton mixed layer holes transferring materials and electron transport material was followed successively by 6: 1,5: 2,4: 3,3: 4,2: 5; The thickness of every layer of said sub-mixed layer is 1nm.
In preferred embodiment, also comprise the hole injection layer and the hole transmission layer that are formed on successively between said anode conducting substrate and the said mixed layer, and be formed on electron transfer layer and electron injecting layer between said luminescent layer and the said negative electrode successively.
This organic electroluminescence device forms mixed layer through adopting hole mobile material and electron transport material by gradual mixed; Can effectively alleviate the transmittability in hole; Reduce hole transport speed; Reach the transmission rate balance with charge carrier, make as much as possible compound of both hole and electron, thereby improve the luminous efficiency of whole organic electroluminescence device at luminescent layer.
A kind of manufacture method of above-mentioned organic electroluminescence device comprises the steps:
The anode pattern of preparation organic electroluminescence device forms the anode conducting substrate on electrically-conductive backing plate;
On said anode conducting substrate, deposit the sub-mixed layer that forms by gradual mixed by hole mobile material and electron transport material successively; Wherein, The mol ratio of said sub-mixed layer holes transferring material of multilayer and electron transport material reduces successively, and the said sub-mixed layer of multilayer constitutes mixed layer;
Depositing light emitting layer and negative electrode successively on said mixed layer form said organic electroluminescence device.
In preferred embodiment, said mixed layer comprises 5 straton mixed layers, and the mol ratio of said 5 straton mixed layer holes transferring materials and electron transport material was followed successively by 6: 1,5: 2,4: 3,3: 4,2: 5; The thickness of every layer of said sub-mixed layer is 1nm.
In preferred embodiment; Above-mentioned manufacture method also is included between said anode conducting substrate and the said mixed layer and deposits hole injection layer, hole transmission layer successively, and between said luminescent layer and said negative electrode the step of electron transport layer and electron injecting layer successively.
The manufacture method of above-mentioned organic electroluminescence device, the material of employing is cheap, and preparation technology is simple, is prone to large-area preparation, and the organic electroluminescence device luminous efficiency that makes significantly improves.
[description of drawings]
Fig. 1 is the structural representation of the organic electroluminescence device of an execution mode;
Fig. 2 be mixed layer holes transferring material, electron transport material the mole value with the gradual variation diagram of the distance of luminescent layer;
Fig. 3 is the structural representation of organic electroluminescence device among the embodiment 1;
The current efficiency and the current density comparison diagram of the organic electroluminescence device that Fig. 4 makes for embodiment 1 and Comparative Examples.
[embodiment]
Mainly combine accompanying drawing and specific embodiment that organic electroluminescence device and preparation method thereof is done further detailed explanation below.
As shown in Figure 1, the organic electroluminescence device 100 of this execution mode comprises: the anode conducting substrate 110 that stacks gradually, mixed layer 120, luminescent layer 130 and negative electrode 140.
Anode conducting substrate 110 has conducting glass substrate (like ito glass substrate) or organic PET (PETG) film substrate of anode pattern for surface etch.The thickness of anode conducting substrate 110 is 100～150nm.
Mixed layer 120 comprises the sub-mixed layer of multilayer that is formed by gradual mixed by hole mobile material and electron transport material.As shown in Figure 2, the hole mobile material in every straton mixed layer and the ratio of electron transport material remain unchanged, and the mol ratio of multilayer sub-mixed layer holes transferring material and electron transport material reduces with the direction near luminescent layer gradually.Preferably, the mol ratio of multilayer sub-mixed layer holes transferring material and electron transport material can be in the gradual variation of 6: 1,5: 2,4: 3,3: 4,2: 5,1: 6 ratio with the direction near luminescent layer, and at this moment, mixed layer comprises 6 straton mixed layers.Other preferred embodiment in, mixed layer can also comprise 3～5 straton mixed layers, the molar ratio range of corresponding hole mobile material of every straton mixed layer and electron transport material got final product between 6: 1～1: 6.
Used hole mobile material is phenylmorpholine (NPB), N in the mixed layer 120, N '-diphenyl-N, and N '-two (3-aminomethyl phenyl)-(1,1 '-xenyl)-4,4 '-diamines (TPD) or 4,4 ', 4 " three (carbazole-9-yl) triphenylamines (TCTA).Electron transport material is oxine aluminium (Alq
3), 4-biphenyl phenolic group-two (2-methyl-oxine) closes aluminium (BAlq), N-aryl benzimidazole (TPBi) or 4,7-diphenyl-1,10-phenanthroline (BPhen).
The thickness of every straton mixed layer is 1nm in the mixed layer of this execution mode.
The making of organic electroluminescence device 100, can carry out according to following steps:
Step 1: the anode pattern of preparation organic electroluminescence device on electrically-conductive backing plate forms anode conducting substrate 110.
Preferably; Before carrying out the anode pattern preparation, also comprise the step of electrically-conductive backing plate being carried out pre-treatment: liquid detergent cleaning → ethanol cleaning → acetone → pure water cleans, and all cleans with supersonic wave cleaning machine; Each washing is adopted and was cleaned 5 minutes; Stop 5 minutes, repeat 3 times method respectively, and then for use with oven for drying; Electrically-conductive backing plate to after cleaning carries out surface activation process again, to increase the oxygen content of conductive surface layer, improves the work function of conductive layer surface.
Step 2: on anode conducting substrate 110, deposit the sub-mixed layer that forms by gradual mixed by hole mobile material and electron transport material successively; Wherein, The mol ratio of said sub-mixed layer holes transferring material of multilayer and electron transport material reduces successively, and the said sub-mixed layer of multilayer constitutes mixed layer 120.
Preferably, adopt the method for vacuum evaporation, vacuum degree is 5 * 10
-5Pa～3 * 10
-5Pa, evaporation rate
Evaporation thickness 3～5nm.
Step 3: depositing light emitting layer 130 and negative electrode 140 successively on mixed layer 120 form said organic electroluminescence device 100.
Preferably, the deposition process of luminescent layer 130 and negative electrode 140 all adopts the method for vacuum evaporation.Wherein, in the evaporate process of luminescent layer 130, vacuum degree 8 * 10
-5Pa～3 * 10
-5Pa, evaporation rate
Monolayer evaporation thickness 5～20nm; In the evaporate process of negative electrode 140, vacuum degree 7 * 10
-5Pa～5 * 10
-5Pa, evaporation rate
Evaporation thickness is 80～200nm.
The manufacture method of this organic electroluminescence device, the material of employing is cheap, and preparation technology is simple, is prone to large-area preparation, and the organic electroluminescence device luminous efficiency that makes significantly improves.
Other preferred embodiment in; Organic electroluminescence device can also adopt following enhancement function structure, comprises the anode conducting substrate, hole injection layer, hole transmission layer, mixed layer, luminescent layer, electron transfer layer, electron injecting layer and the negative electrode that stack gradually.
Hole injection layer can be MoO
3, WO
3, V
2O
5Make Deng hole-injecting material.Manufacturing process adopts the method for vacuum evaporation, vacuum degree 7 * 10
-5Pa～5 * 10
-5Pa, evaporation rate
Evaporation thickness is 10～15nm.
Hole transmission layer can adopt phenylmorpholine (NPB), N, N '-diphenyl-N, N '-two (3-aminomethyl phenyl)-(1; 1 '-xenyl)-4,4 '-diamines (TPD), 4,4 '; 4 " three (carbazole-9-yl) triphenylamine (TCTA) or N, N '-diphenyl-N, N '-(1-naphthyl)-1; 1 '-biphenyl-4,4 '-diamines (α-NPD) wait hole mobile material to make.Manufacturing process adopts the method for vacuum evaporation, vacuum degree 5 * 10
-5Pa～3 * 10
-5Pa, evaporation rate
Evaporation thickness 40～60nm.
Electron transfer layer can adopt oxine aluminium (Alq
3), 4-biphenyl phenolic group-two (2-methyl-oxine) closes aluminium (BAlq), N-aryl benzimidazole (TPBi) or 4,7-diphenyl-1,10-phenanthroline electron transport materials such as (BPhen) is made.Manufacturing process adopts the method for vacuum evaporation, vacuum degree 5 * 10
-5Pa～3 * 10
-5Pa, evaporation rate
Evaporation thickness 20～80nm.
Electron injecting layer can be that thickness is CsF or the liF layer of 1～2nm.Manufacturing process adopts the method for vacuum evaporation, vacuum degree 7 * 10
-5Pa～5 * 10
-5Pa, evaporation rate
Evaporation thickness is 1～2nm.Below be specific embodiment and comparative example part:
Embodiment 1:
Please join Fig. 3
A) ito glass substrate 210 pre-treatments: liquid detergent cleaning → ethanol cleaning → acetone → pure water cleans; All clean with supersonic wave cleaning machine, each washing is adopted and was cleaned 5 minutes, stops 5 minutes; Repeat 3 times method respectively, and then for use with the IR bake oven dry; Ito glass substrate 210 to after cleaning carries out surface activation process, to increase the oxygen content of ITO superficial layer, improves the work function on ITO surface.
Ito glass substrate 210 thickness 100nm.
B) preparation of hole injection layer 220: vapor deposition one layer thickness is the MoO of 10nm on ito glass substrate 210
3As hole injection layer 220.Vacuum degree 5 * 10
-5Pa, evaporation rate
C) preparation of hole transmission layer 230: with NPB as hole mobile material.Vacuum degree 3 * 10
-5Pa, evaporation rate
Evaporation thickness 50nm.
D) preparation of mixed layer 240: mixed layer is by NPB and Alq
3By the graded composition of proportions, mol ratio becomes 6: 1 respectively, 5: 2,4: 3,3: 4,2: 5.Vacuum degree 3 * 10
-5Pa, evaporation rate
Evaporation thickness 5nm, wherein, the thickness of the sub-mixed layer of every kind of molar ratio is 1nm.
E) preparation of luminescent layer 250: material of main part adopts TPBi, and green object adopts Ir (ppy)
3, doping content 1wt%.Vacuum degree 3 * 10
-5Pa, evaporation rate
Evaporation thickness 10nm.
F) preparation of electron transfer layer 260: vapor deposition one deck Alq on luminescent layer 250
3As electron transfer layer 260.Vacuum degree 3 * 10
-5Pa, evaporation rate
Evaporation thickness 40nm.
G) preparation of electron injecting layer 270: vapor deposition one layer thickness is that the LiF of 1nm is as electron injecting layer 270.Vacuum degree 5 * 10
-5Pa, evaporation rate
H) place metallic cathode 280 on the electron injecting layer 270, it is that the aluminium electrode of 100nm is as negative electrode 280 that vapor deposition is made thickness.Vacuum degree 5 * 10
-5Pa, evaporation rate
Embodiment 2: embodiment 2 and embodiment 1 is identical substantially, and its difference is: among the embodiment 2 a) thickness of ito glass substrate be 150nm; D) mixed layer adopts TPD to mix formation in 6: 1 in molar ratio, 5: 2,4: 3,3: 4,2: 5,1: 6 with BAlq, every layer thickness 1nm; E) light emitting layer thickness 5nm in; H) cathode thickness 200nm in.
Embodiment 3: embodiment 3 and embodiment 1 is identical substantially, and its difference is: among the embodiment 3 a) thickness of ito glass substrate be 120nm; D) mixed layer adopts TCTA to mix formation in 5: 2 in molar ratio, 1: 1,2: 5 with TPBi, every layer thickness 1nm; E) light emitting layer thickness 20nm in; H) cathode thickness 80nm in.
Embodiment 4: embodiment 4 and embodiment 1 is identical substantially, and its difference is: among the embodiment 4 a) thickness of ito glass substrate be 110nm; D) mixed layer adopts NPB to mix formation in 5: 2 in molar ratio, 4: 3,3: 4,2: 5 with BPhen, every layer thickness 1nm; E) light emitting layer thickness 15nm in; H) cathode thickness 120nm in.
Comparative example: do not have mixed layer 240, other is with embodiment 1.
The current efficiency and the correlation curve figure of current density of the organic electroluminescence device that Fig. 4 makes for embodiment 1 and Comparative Examples, wherein, curve 1 is represented the organic electroluminescence device in embodiment 1 and the Comparative Examples respectively with curve 2.Table 1 is some coordinate figure data of intercepting from Fig. 4, as follows:
Table 1
Can find out in conjunction with Fig. 4 and table 1; The luminous efficiency that includes the organic electroluminescence device of the mixed layer 240 that is used for reducing hole transport speed among the embodiment 1 is significantly higher than the organic electroluminescence device of Comparative Examples, and the luminous efficiency of embodiment 1 is about 1.5 times of Comparative Examples.
The above embodiment has only expressed several kinds of execution modes of the present invention, and it describes comparatively concrete and detailed, but can not therefore be interpreted as the restriction to claim of the present invention.Should be pointed out that for the person of ordinary skill of the art under the prerequisite that does not break away from the present invention's design, can also make some distortion and improvement, these all belong to protection scope of the present invention.Therefore, the protection range of patent of the present invention should be as the criterion with accompanying claims.
Claims (10)
1. organic electroluminescence device; Comprise the anode conducting substrate, luminescent layer and the negative electrode that stack gradually; It is characterized in that; Also comprise the mixed layer that is used to reduce hole transport speed that is located between said anode conducting substrate and the said luminescent layer; Said mixed layer comprises the sub-mixed layer of multilayer that is formed by gradual mixed by hole mobile material and electron transport material, and the mol ratio of said multilayer sub-mixed layer holes transferring material and electron transport material reduces with the direction near said luminescent layer gradually.
2. organic electroluminescence device as claimed in claim 1 is characterized in that, said hole mobile material is phenylmorpholine, N; N '-diphenyl-N, N '-two (3-aminomethyl phenyl)-(1,1 '-xenyl)-4; 4 '-diamines or 4,4 ', 4 " three (carbazole-9-yl) triphenylamine; Said electron transport material is that oxine aluminium, 4-biphenyl phenolic group-two (2-methyl-oxine) close aluminium, N-aryl benzimidazole or 4,7-diphenyl-1,10-phenanthroline.
3. according to claim 1 or claim 2 organic electroluminescence device is characterized in that the molar ratio range of said multilayer sub-mixed layer holes transferring material and electron transport material is 6: 1～1: 6.
4. according to claim 1 or claim 2 organic electroluminescence device is characterized in that said mixed layer comprises 3～6 straton mixed layers.
5. organic electroluminescence device as claimed in claim 1; It is characterized in that; Said anode conducting substrate thickness is: 100～150nm, said mixed layer thickness is: 3～5nm, said light emitting layer thickness is: the thickness of 5～20nm and said negative electrode is: 80～200nm.
6. like claim 1 or 5 described organic electroluminescence devices; It is characterized in that; Said mixed layer comprises 5 straton mixed layers, and the mol ratio of said 5 straton mixed layer holes transferring materials and electron transport material was followed successively by 6: 1,5: 2,4: 3,3: 4,2: 5; The thickness of every layer of said sub-mixed layer is 1nm.
7. organic electroluminescence device as claimed in claim 1; It is characterized in that; Also comprise the hole injection layer and the hole transmission layer that are formed on successively between said anode conducting substrate and the said mixed layer, and be formed on electron transfer layer and electron injecting layer between said luminescent layer and the said negative electrode successively.
8. the manufacture method of an organic electroluminescence device is characterized in that, comprises the steps:
The anode pattern of preparation organic electroluminescence device forms the anode conducting substrate on electrically-conductive backing plate;
On said anode conducting substrate, deposit the sub-mixed layer that forms by gradual mixed by hole mobile material and electron transport material successively; Wherein, The mol ratio of said sub-mixed layer holes transferring material of multilayer and electron transport material reduces successively, and the said sub-mixed layer of multilayer constitutes mixed layer;
Depositing light emitting layer and negative electrode successively on said mixed layer form said organic electroluminescence device.
9. the manufacture method of organic electroluminescence device as claimed in claim 8; It is characterized in that; Said mixed layer comprises 5 straton mixed layers, and the mol ratio of said 5 straton mixed layer holes transferring materials and electron transport material was followed successively by 6: 1,5: 2,4: 3,3: 4,2: 5; The thickness of every layer of said sub-mixed layer is 1nm.
10. like the manufacture method of claim 8 or 9 described organic electroluminescence devices; It is characterized in that; Also be included between said anode conducting substrate and the said mixed layer and deposit hole injection layer, hole transmission layer successively, and between said luminescent layer and said negative electrode the step of electron transport layer and electron injecting layer successively.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107749442A (en) * | 2017-10-16 | 2018-03-02 | 京东方科技集团股份有限公司 | OLED and preparation method thereof, display device |
| CN109628886A (en) * | 2019-01-10 | 2019-04-16 | 云谷（固安）科技有限公司 | A kind of evaporation coating device, evaporation coating method, mixed layer and display panel |
| CN110707227A (en) * | 2019-10-17 | 2020-01-17 | 昆山国显光电有限公司 | Light-emitting device and display panel |
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| CN1362746A (en) * | 2000-12-28 | 2002-08-07 | 株式会社半导体能源研究所 | Light-emitting device |
| CN1897777A (en) * | 2006-05-16 | 2007-01-17 | 清华大学 | Organic electroluminescent device |
| WO2007074879A1 (en) * | 2005-12-28 | 2007-07-05 | Rohm Co., Ltd. | Organic el element |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN1362746A (en) * | 2000-12-28 | 2002-08-07 | 株式会社半导体能源研究所 | Light-emitting device |
| WO2007074879A1 (en) * | 2005-12-28 | 2007-07-05 | Rohm Co., Ltd. | Organic el element |
| CN1897777A (en) * | 2006-05-16 | 2007-01-17 | 清华大学 | Organic electroluminescent device |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107749442A (en) * | 2017-10-16 | 2018-03-02 | 京东方科技集团股份有限公司 | OLED and preparation method thereof, display device |
| CN109628886A (en) * | 2019-01-10 | 2019-04-16 | 云谷（固安）科技有限公司 | A kind of evaporation coating device, evaporation coating method, mixed layer and display panel |
| CN109628886B (en) * | 2019-01-10 | 2021-01-19 | 云谷（固安）科技有限公司 | Evaporation device, evaporation method, mixing layer and display panel |
| CN110707227A (en) * | 2019-10-17 | 2020-01-17 | 昆山国显光电有限公司 | Light-emitting device and display panel |
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Application publication date: 20121226 |