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CN104183711A - Organic light emission diode, display screen and terminal - Google Patents

Organic light emission diode, display screen and terminal Download PDF

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Publication number
CN104183711A
CN104183711A CN201310192344.2A CN201310192344A CN104183711A CN 104183711 A CN104183711 A CN 104183711A CN 201310192344 A CN201310192344 A CN 201310192344A CN 104183711 A CN104183711 A CN 104183711A
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CN
China
Prior art keywords
layer
interfering
electroluminescent device
thickness
semi
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CN201310192344.2A
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Inventor
周明杰
冯小明
黄辉
王平
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Oceans King Lighting Science and Technology Co Ltd
Shenzhen Oceans King Lighting Science and Technology Co Ltd
Shenzhen Oceans King Lighting Engineering Co Ltd
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Oceans King Lighting Science and Technology Co Ltd
Shenzhen Oceans King Lighting Engineering Co Ltd
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Application filed by Oceans King Lighting Science and Technology Co Ltd, Shenzhen Oceans King Lighting Engineering Co Ltd filed Critical Oceans King Lighting Science and Technology Co Ltd
Priority to CN201310192344.2A priority Critical patent/CN104183711A/en
Publication of CN104183711A publication Critical patent/CN104183711A/en
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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K50/00—Organic light-emitting devices
    • H10K50/80—Constructional details
    • H10K50/86—Arrangements for improving contrast, e.g. preventing reflection of ambient light
    • H10K50/865—Arrangements for improving contrast, e.g. preventing reflection of ambient light comprising light absorbing layers, e.g. light-blocking layers
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K50/00—Organic light-emitting devices
    • H10K50/80—Constructional details
    • H10K50/805—Electrodes
    • H10K50/82—Cathodes
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K2102/00—Constructional details relating to the organic devices covered by this subclass

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  • Physics & Mathematics (AREA)
  • Optics & Photonics (AREA)
  • Electroluminescent Light Sources (AREA)

Abstract

The invention discloses an organic light emission diode, a display screen and a terminal. The organic light emission diode includes a transmitting substrate, an anode layer, an organic function layer and a cathode layer, which are sequentially laminated and combined. The cathode layer includes a metal reflection layer, at least two interference layers and at least two transflective metal layers. The interferences layers and the transflective metal layers are alternatively laminated and combined between the metal reflection layer and the organic function layer. The interference layers and the metal reflection layers are laminated and combined. The transflective metal layer and the organic function layer are laminated and combined, wherein the material of the interference layers includes an organic electron transmission material and an alkali metal compound doped therein, and the mass of the alkali metal compound is 5-50% of the total mass of the interference layers. The cathode of the organic light emission diode effectively reduces a light reflectivity of the cathode of the organic light emission diode and improves the contrast ratio thereof. The display screen which includes the organic light emission diode, and the terminal have high contrast ratios and clear display pictures.

Description

Organnic electroluminescent device, display screen and terminal thereof
Technical field
The invention belongs to electric light source technology field, relate to specifically a kind of Organnic electroluminescent device, display screen and terminal thereof.
Background technology
Organic electroluminescence device (Organic Light Emission Diode, hereinafter to be referred as OLED) is a kind of current mode light emitting semiconductor device based on organic material.Its typical structure is that the luminous organic material of making one deck tens nanometer thickness on ito glass is made luminescent layer, and there is the metal electrode of one deck low work function luminescent layer top.
The principle of luminosity of OLED is based under the effect of extra electric field, and electronics is injected into organic lowest unocccupied molecular orbital (LUMO) from negative electrode, and hole is injected into organic highest occupied molecular orbital (HOMO) from anode.Electronics and hole meet at luminescent layer, compound, form exciton, exciton moves under electric field action, and energy is passed to luminescent material, and excitation electron is from ground state transition to excitation state, excited energy, by Radiation-induced deactivation, produces photon, discharges luminous energy.
The advantages such as OLED has that luminous efficiency is high, material range of choice is wide, driving voltage is low, entirely solidifies active illuminating, light, thin, have high definition, wide viewing angle, fast response time, low cost and the advantage such as bright in luster simultaneously, a kind of Display Technique and light source that has potentiality, meet the development trend that information age mobile communication and information show, and the requirement of green lighting technique, therefore, thought to be most likely at by insider the device of new generation that occupies dominance on following illumination and display device market.As a brand-new illumination and Display Technique, the ten years development in the past of OLED technology is swift and violent, has obtained huge achievement.Throw light on because the whole world is increasing and show that producer drops into research and development one after another, having promoted greatly the industrialization process of OLED, making the growth rate of OLED industry surprising, having arrived the eve of scale of mass production at present.
But the negative electrode of existing OLED device is generally the metallic cathode material that uses high reflectance, particularly, the metallic cathode of the high reflectance that the metallic cathode material of this high reflectance is prepared into has the reflectivity that exceedes 90% in visible ray section, therefore this high reflectance negative electrode like this brings obstruction but to the application of OLED on display device.This be because, as display device, high-contrast is the long-term pursuits of people, requirement to Display Contrast is higher, if when the application by the OLED device of existing high reflectance negative electrode on display device, under solar light irradiation, due to the high reflectance effect of its high reflectance negative electrode, make the contrast of display device low, the content of demonstration cannot be seen clearly.Therefore,, when OLED device is applied in display, the negative electrode reflectivity that how to reduce OLED device is technical barrier to be solved.
In order to reduce the reflectivity of OLED, people have also done some explorations and have obtained certain achievement, as adopted organic material Alq 3, TPBi material is as dielectric layer, although although easily masking of this material has certain light transmission rate, but its electric conductivity is not strong, therefore, can only prepare thinner dielectric layer, common thickness below 5nm, thereby just can avoid causing due to blocked up thickness the increase of driving voltage.But for the large area preparation of OLED, this thickness as thin as a wafer needs accurate control in preparation process, and its homogeneity is difficult to obtain and ensures, for the rete of homogeneous, conventionally needs point-device watch-dog and high-precision evaporated device.Thereby the invisible production cost that increases OLED, and yields is low.In addition, adopt organic material Alq 3, TPBi material can only, for a certain specific wavelength as the light of 550nm wavelength reduces reflection, almost not act on the light of other wavelength as dielectric layer, therefore, its reflectivity is still undesirable.
Summary of the invention
The object of the invention is to overcome the above-mentioned deficiency of prior art, provide a kind of negative electrode to there is the Organnic electroluminescent device of antiradar reflectivity.
The display screen that provides a kind of contrast high is provided.
Another object of the present invention is to provide a kind of terminal that contains above-mentioned display screen.
In order to realize foregoing invention object, technical scheme of the present invention is as follows:
A kind of Organnic electroluminescent device, comprise the transparent substrates, anode layer, organic function layer and the cathode layer that stack gradually combination, described organic function layer is included in luminescent layer luminous under the driving of additional power source, described cathode layer comprises metallic reflector, at least two interfering layers and at least two semi-transparent metal levels, described interfering layer and semi-transparent metal level are alternately laminated to be incorporated between described metallic reflector and organic function layer, the stacked combination of described interfering layer and metallic reflector, semi-transparent metal level and organic function layer; Wherein, described interfering layer material comprises Organic Electron Transport Material and is doped in alkali metal compound wherein, and described alkali metal compound quality is 5～50% of interfering layer gross mass.
And a kind of display screen, comprises display module and for controlling the control module of display module, wherein said display module contains Organnic electroluminescent device described above.
And, a kind of terminal that is provided with display screen, the display screen of described terminal is the above-mentioned display that contains Organnic electroluminescent device.
Above-mentioned Organnic electroluminescent device is by being arranged to negative electrode to stack gradually the metallic reflector of combination, the structure of (interfering layer/semi-transparent metal level) n, realize the interference effect to multi-wavelength light, effectively reduce the negative electrode of this Organnic electroluminescent device to reflection of light rate, improved its contrast.By the material selection alkali metal compound doping Organic Electron Transport Material of interfering layer, effectively strengthen the conductance of this interfering layer, realize the increase of avoiding the drive current of this Organnic electroluminescent device on the basis that increases interfering layer thickness, therefore, realized the large area preparation of this Organnic electroluminescent device, and make the Organnic electroluminescent device even film layer of preparation, yields is high, low for equipment requirements, and cost is low, drive current is little, long service life.
Above-mentioned display screen is owing to containing above-mentioned Organnic electroluminescent device, and therefore it has high-contrast, and its display frame is clear.Due to the display screen that is provided with the terminal of display screen and contains this high-contrast, therefore the display screen picture of this terminal is clear.
Brief description of the drawings
Fig. 1 is embodiment of the present invention Organnic electroluminescent device structural representation;
Fig. 2 is another preferred structure schematic diagram of embodiment of the present invention Organnic electroluminescent device;
Fig. 3 is embodiment of the present invention Organnic electroluminescent device preparation method's schematic flow sheet.
Embodiment
In order to make the technical problem to be solved in the present invention, technical scheme and beneficial effect clearer, below in conjunction with embodiment and accompanying drawing, the present invention is further elaborated.Should be appreciated that specific embodiment described herein, only in order to explain the present invention, is not intended to limit the present invention.
Organic electroluminescent pixel contrast=(environmental light brightness of device luminosity (opening)+device reflection)/(environmental light brightness of device luminosity (pass)+device reflection), according to these computational methods, in the OLED of transparent anode device, one of method that improves contrast is exactly to reduce the light reflection of device to environment, namely reduces the reflectivity of reflecting electrode.
Based on above-mentioned theory, the embodiment of the present invention adopts the approach that reduces negative electrode reflectivity to improve organic electroluminescent pixel contrast.Therefore, the Organnic electroluminescent device that the embodiment of the present invention provides a kind of negative electrode to have antiradar reflectivity, its structure is as shown in Figure 1 to Figure 2.This Organnic electroluminescent device comprises the transparent substrates 1, anode layer 2, organic function layer 3 and the cathode layer 4 that stack gradually combination.
Particularly, above-mentioned cathode layer 4 comprises metallic reflector 43, at least two interfering layers 42 and at least two semi-transparent metal levels 41, wherein, this interfering layer 42 and semi-transparent metal level 41 are alternately laminated to be incorporated between metallic reflector 43 and organic function layer 3, and interfering layer 42 and the stacked combination of metallic reflector 43, semi-transparent metal level 41 and organic function layer 3.Thus, the structure of this cathode layer 4 can be expressed as: metallic reflector 43/ (the saturating metal level 41 of interfering layer 42/) n, wherein, the natural number of n >=2.Therefore, this cathode layer 4 at least has following concrete structure:
The first, when n=2, the structure of this cathode layer 4 as shown in Figure 1, its structure is metallic reflector 43, interfering layer 42a, semi-transparent metal level 41a, interfering layer 42b and the semi-transparent metal level 41b that stacks gradually combination, the structure that is cathode layer 4 is: the semi-transparent metal level 41b of the semi-transparent metal level 41a/ of metallic reflector 43/ interfering layer 42a/ interfering layer 42b/, and this semi-transparent metal level 41b and the stacked combination of organic function layer 3.
The second, when n=3, the structure of this cathode layer 4 as shown in Figure 2, its structure is metallic reflector 43, interfering layer 42a, semi-transparent metal level 41a, interfering layer 42b, semi-transparent metal level 41b, interfering layer 42c and the semi-transparent metal level 41c that stacks gradually combination, the structure that is cathode layer 4 is: the semi-transparent metal level 41c of metallic reflector 43/ interfering layer 42a/ semi-transparent metal level 41a/ interfering layer 42b/ semi-transparent metal level 41b/ interfering layer 42c/, and this semi-transparent metal level 41c and the stacked combination of organic function layer 3.
、、、
The like, deserve n>=4 o'clock, the structure of cathode layer 4 is: metallic reflector 43/ interfering layer 42m 1/ semi-transparent metal level 41m 1/ interfering layer 42m 2/ semi-transparent metal level 41m 2/ interfering layer 42m 3/ semi-transparent metal level 41m 3/ interfering layer 42m 4/ semi-transparent metal level 41m 4/,, ,/interfering layer 42m nsemi-transparent metal level 41m n(figure does not show), and this semi-transparent metal level 41m nwith the stacked combination of organic function layer 3.
Therefore, in the time that this Organnic electroluminescent device is connected to additional power source, the negative pole of additional power source is connected on metallic reflector 43, and its positive pole is connected on anode layer 2.Cathode layer 4 operation principles of this structure are: in the time being incident to each semi-transparent metal level 41 from the light of anode tap incident, this semi-transparent metal level 41 has played semi-transflective reflective to incident light, the interference effect that the visible ray that each semi-transparent metal level 41 refraction is carried out different wave length by each interfering layer 42 reflects, the visible ray that makes different wave length after reflecting at metallic reflector 43 interfaces with the catoptrical single spin-echo of each semi-transparent metal level 41, reach the effect that interference disappears mutually, effectively reduce the total reflection of multi-wavelength visible ray light, realized low reflectivity.
Inventor finds under study for action, suitable control interfering layer 42 and the alternately laminated number of times of semi-transparent metal level 41, can effectively realize the interference effect to multi-wavelength visible ray, make multi-wavelength visible ray that reverberation occur in cathode layer 4 and interfere the effect disappearing mutually, effectively reduced the total reflection of multi-wavelength visible ray, realize low reflectivity, the effective gross thickness of control cathode layer 4 again, strengthen electronic injection ability, thereby improve the luminous intensity of Organnic electroluminescent device, and reduce production costs.Accordingly, in a preferred embodiment, the natural number that this interfering layer 42 and the alternately laminated frequency n of semi-transparent metal level 41 are 2～5.
In cathode layer 4, one of object that this semi-transparent metal level 41 arranges is the light being come by anode layer 2 end-fires, at its interface, part permeation parts to be occurred to reflect, its another effect is to use as electrode, plays electronic injection effect, improves the electronic injection ability of cathode layer 4.For reflection and the transmitance of better light regulating, as preferred embodiment, the thickness of this semi-transparent metal level 41 is 5nm～10nm, and its thickness can also be adjusted flexibly according to the difference of material.As another preferred embodiment, above-mentioned semi-transparent metal level 41 metal materials are any or both the above alloys in Au, Ag, Al, Ca.This preferred metal material can strengthen the electronic injection ability of cathode layer 4 and the semi-transparent semi-reflecting effect to multi-wavelength luminous ray.Should be appreciated that, as long as can realize these semi-transparent metal level 41 part permeation parts reflections and there are other thickness of electronic injection performance and other can do cathodic metal material and also belong to the framework of the present definition.
This interfering layer 42 plays reflection interference effect to the multi-wavelength visible ray that sees through semi-transparent metal level 41, and as a part for cathode layer 4, it must possess photopermeability and conductivity, therefore, each interfering layer 42 material in the various embodiments described above comprise Organic Electron Transport Material and are doped in alkali metal compound wherein, and alkali metal compound quality is 5～50% of interfering layer gross mass.In these interfering layer 42 materials, the doping of alkali metal compound to Organic Electron Transport Material, effectively improve on the basis of this Organic Electron Transport Material light transmission performance, there is excellent electric conductivity, thereby can realize increasing on the basis of each interfering layer 42 thickness, avoid causing the increase of Organnic electroluminescent device driving voltage.In order to make each interfering layer 42 have more excellent light transmission performance and electric conductivity, in a preferred embodiment, this alkali metal compound is alkali-metal carbonate and or alkali-metal nitride.Wherein, this alkali-metal carbonate is preferably Li 2cO 3, Cs 2cO 3, Rb 2cO 3in at least one, alkali-metal nitride is preferably LiN 3with or CsN 3.In another preferred embodiment, this Organic Electron Transport Material is oxine aluminium (Alq 3), 4,7-diphenyl-1,10-phenanthroline (BPhen), 1,3,5-tri-(1-phenyl-1H-benzimidazolyl-2 radicals-yl) benzene (TPBi), 2-(4-xenyl)-5-(the 4-tert-butyl group) phenyl-1,3,4-oxadiazole (PBD), 3-(biphenyl-4-yl)-5-(4-tert-butyl-phenyl)-4-phenyl-4H-1, at least one in 2,4-triazole (TAZ).Certainly, this Organic Electron Transport Material can also be other conventional electron transport materials of this area.
In order further to improve the refraction interference effect of cathode layer 4 to multi-wavelength visible ray, make multi-wavelength visible ray that reverberation occur in cathode layer 4 and interfere the better effects if disappearing mutually, further reduce the total reflection of multi-wavelength visible ray.In a preferred embodiment, the thickness of the adjacent interfering layer 42 between two in this cathode layer 4 in gradient, in further preferred embodiment, this between two the thickness of adjacent interfering layer 42 differ the gradient into the integral multiple of 5nm.
Contain Organic Electron Transport Material described above and be doped in alkali metal compound wherein just because of these interfering layer 42 materials.Accordingly, in a preferred embodiment, the thickness of this each interfering layer 42 is 20～80nm.Because each interfering layer 42 contains Organic Electron Transport Material described above and is doped in alkali metal compound wherein, make the thickness of this interfering layer 42 can be designed to obviously be greater than the thickness of existing 1nm, as increase to 20～80nm, thereby very accurately watch-dog and the high-precision evaporated device of interfering layer 42 as common needs are effectively avoided preparing, thereby its preparation cost and difficulty are reduced, make this each interfering layer 42 even thickness simultaneously, ensured interfering layer 42 quality.Meanwhile, this thickness range also has excellent light transmission performance and electronic transmission performance, and can not increase the driving voltage of Organnic electroluminescent device.
Arranging of this metallic reflector 43 can be reflected the light that sees through interfering layer 42 on its surface, and interfere transmission light rear and that each semi-transparent metal level 41 interface occurs to reflect to be cancelled each other by the refraction of interfering layer 42 this reverberation, further to reduce the reflectivity of cathode layer 4.Therefore,, as preferred embodiment, the thickness of this metallic reflector 43 is 70～200nm.As another preferred embodiment, above-mentioned metallic reflector 43 metal materials are any in Ag, Al, Mg-Ag alloy, Mg-Al.Should be appreciated that, can do cathodic metal material and also belong to the framework of the present definition as long as can realize other thickness of reflection action of this metallic reflector 43 and other, as disregard cost, the thickness of this metallic reflector 43 can also be more than 200nm.
As another preferred embodiment of above-mentioned Organnic electroluminescent device, the thickness of above-mentioned semi-transparent metal level 41 is 5nm～10nm, and its thickness can also be adjusted flexibly according to the difference of material; The thickness of each interfering layer 42 is 20nm～80nm, and the thickness of adjacent interfering layer 42 is the gradient differing as the integral multiple of 5nm between two; The thickness of metallic reflector 43 is 70nm～200nm.The combination of each layer thickness in the preferred embodiment, the better effects if that the interference of light that the refraction interference effect by each interfering layer 42 to light and each semi-transparent metal level 41 reflect with metallic reflector 43 disappears mutually, makes the reflectivity that cathode layer 4 is lower.
As a preferred embodiment again of above-mentioned Organnic electroluminescent device, above-mentioned each semi-transparent metal level 41 material are any or both the above alloys in Au, Ag, Al, Ca, each interfering layer 42 as described above comprise Organic Electron Transport Material and be doped in alkali metal compound wherein, and alkali metal compound quality is 5～50% of interfering layer gross mass; Metallic reflector 43 materials are any in Ag, Al, Mg-Ag alloy, Mg-Al.The combination of each layer of selected material in the preferred embodiment, gives reflectivity and electronic injection performance that cathode layer 4 is lower.
As the another preferred embodiment of above-mentioned Organnic electroluminescent device, the thickness of above-mentioned semi-transparent metal level 41 is 5nm～10nm, its thickness can also be according to the difference of material and adjust flexibly, and material is any or both above alloys in Au, Ag, Al, Ca; The thickness of each interfering layer 42 is 20nm～80nm, and between two the thickness of adjacent interfering layer 42 be differ for the gradient of the integral multiple of 5nm with and include organic electronic transferring material and be doped in alkali metal compound wherein, wherein alkali metal compound quality is 5～50% of interfering layer gross mass; The thickness of metallic reflector 43 is 70nm～200nm, and its material is any in Ag, Al, Mg-Ag alloy, Mg-Al.The combination of each layer thickness and material in the preferred embodiment, makes cathode layer 4 have lower reflectivity and excellent electronic injection performance.
Organic function layer 3 in above-mentioned Organnic electroluminescent device embodiment comprises the hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, the electron injecting layer 35 that stack gradually combination, and the stacked combination in the relative surface of face that combines with substrate layer 1 of hole injection layer 31 and anode layer 2, electron injecting layer 35 and the stacked combination of cathode layer 4, as shown in Figure 1, 2.
In specific embodiment, above-mentioned hole injection layer 31 materials can be ZnPc (Phthalocyanine Zinc), CuPc(CuPc), at least one in VOPc (ranadylic phthalocyanine), TiOPc (TiOPc).Certainly, these hole injection layer 31 materials can also be the conventional other materials in this area, as WO 3, VO x, WO xor MoO 3deng oxide, or the dopant mixture of inorganic hole injection layer material and organic hole implanted layer material.The thickness of hole injection layer 31 also can arrange according to the thickness of this area routine.The setting of this hole injection layer 31, can effectively strengthen the ohmic contact between itself and anode layer 2, has strengthened electric conductivity, improves the hole injectability of anode layer 2 ends.Just because of this, this hole injection layer 31 also can not arrange according to the actual needs, that is to say, hole transmission layer 32 can be directly and the direct stacked combination of anode layer 2.
Above-mentioned hole transmission layer 32 materials can be NPB (N, N'-diphenyl-N, N'-bis-(1-naphthyl)-1,1'-biphenyl-4,4'-diamines), TPD (N, N'-diphenyl-N, N'-bis-(3-aminomethyl phenyl)-1,1'-biphenyl-4,4'-diamines), MeO-TPD (N, N, N', N '-tetramethoxy phenyl)-benzidine), MeO-Sprio-TPD(2, the two (N of 7-, N-bis-(4-methoxyphenyl) amino)-9,9-spiral shell two fluorenes) at least one.Certainly, these hole transmission layer 32 materials can also be the conventional other materials in this area, as 4,4', and 4''-tri-(N-3-aminomethyl phenyl-N-phenyl amino) triphenylamine (m-MTDATA) etc.The thickness of hole transmission layer 32 also can arrange according to the thickness of this area routine.
Above-mentioned luminescent layer 33 materials can be guest materials and material of main part dopant mixture.Wherein, guest materials is luminescent material, it comprises 4-(dintrile methyl)-2-butyl-6-(1, 1, 7, 7-tetramethyl Lip river of a specified duration pyridine-9-vinyl)-4H-pyrans (DCJTB), two (4, 6-difluorophenyl pyridine-N, C2) pyridine formyl closes iridium (FIrpic), two (4, 6-difluorophenyl pyridine)-tetra-(1-pyrazolyl) boric acid closes iridium (FIr6), two (2-methyl-diphenyl [f, h] quinoxaline) (acetylacetone,2,4-pentanedione) close iridium (Ir (MDQ) 2 (acac)), three (1-phenyl-isoquinolin) close iridium (Ir (piq) 3), three (2-phenylpyridines) close at least one in iridium (Ir (ppy) 3), material of main part comprises 4,4'-bis-(9-carbazole) biphenyl (CBP), oxine aluminium (Alq 3), 1,3,5-tri-(1-phenyl-1H-benzimidazolyl-2 radicals-yl) benzene (TPBi), N, N'-diphenyl-N, N'-bis-(1-naphthyl)-1,1'-biphenyl-4, at least one in 4'-diamines (NPB).Main, guest materials can carry out according to the needs of actual production and application compound flexibly, and the mass ratio of guest materials and material of main part can be 1～10:100.
In addition, these luminescent layer 33 materials can also be selected fluorescent material 4,4'-bis-(2,2-diphenylethyllene)-1,1'-biphenyl (DPVBi), 4, two [4-(di-p-tolyl amino) styryl] biphenyl (DPAVBi), 5,6 of 4'-, at least one in the materials such as 11,12-tetraphenyl naphthonaphthalene (Rubrene), dimethylquinacridone (DMQA).The thickness of this luminescent layer 33 also can arrange according to the thickness of this area routine.
Above-mentioned electron transfer layer 34 materials can be 2-(4-xenyl)-5-(the 4-tert-butyl group) phenyl-1,3,4-oxadiazole (PBD), (oxine)-aluminium (Alq 3), 4,7-diphenyl-o-phenanthroline (Bphen), 1,3,5-tri-(1-phenyl-1H-benzimidazolyl-2 radicals-yl) benzene (TPBi), 2,9-dimethyl-4,7-biphenyl-1,10-phenanthrolene (BCP), 1,2, in 4-triazole derivative (TAZ) at least one.Certainly, electron transfer layer 34 materials can also be other electron transport materials well known in the art, and its thickness also can adopt the conventional thickness in this area.
Above-mentioned electron injecting layer 35 materials can LiF, CsF, NaF, MgF 2deng at least one etc. alkali-metal halide, certainly, these electron injecting layer 35 materials can also be selected the alkali-metal halide such as at least one in lithium iodide, KI, sodium iodide, cesium iodide, rubidium iodide.The thickness of electron injecting layer 35 also can arrange according to the thickness of this area routine.The arranging of this electron injecting layer 35 can effectively strengthen the ohmic contact between itself and cathode layer 4, strengthen electric conductivity, further improve the electronic injection ability of cathode layer 4 ends, with further equilibrium carrier, control recombination region, in luminescent layer, increase exciton amount, obtained desirable luminosity and luminous efficiency.Just because of this, this electron injecting layer 35 also can not arrange according to the actual needs, that is to say, electron transfer layer 34 can be directly and the direct stacked combination of cathode layer 4.
In further preferred embodiment, on the basis of organic function layer 3 as shown in Figure 1, 2, above-mentioned organic function layer 3 can also arrange electronic barrier layer and hole blocking layer (without diagram).Wherein, this electronic barrier layer is stacked to be combined between hole transmission layer 32 and luminescent layer 33, and hole blocking layer is stacked to be combined between luminescent layer 33 and electron transfer layer 34.Arranging of this electronic barrier layer can stop the electronics that does not form exciton in luminescent layer 33 as much as possible and be trapped in luminescent layer 33, arranging of hole blocking layer can stop the hole that does not form exciton in luminescent layer 33 as much as possible and be trapped in luminescent layer 33, to improve electronics and the hole meeting rate in luminescent layer 33, to improve both exciton amounts compound and that form, and exciton energy is passed to luminescent material, thereby the electronics of excitation light-emitting material is from ground state transition to excitation state, excited energy passes through Radiation-induced deactivation, produce photon, discharge luminous energy, to reach the object of the luminous intensity that strengthens luminescent layer 33.Certainly, this electronic barrier layer and hole blocking layer can according to the situation of actual production and application need to select a setting, the material that it is selected and thickness can arrange according to the conventional material in this area and conventional thickness.
Above-mentioned anode layer 2 materials are transparent conductive oxide.This transparent conductive oxide is preferably at least one in tin oxide film (ITO), indium-zinc oxide (IZO), aluminium zinc oxide (AZO), gallium zinc oxide (GZO).This preferred transparent conductive oxide has excellent light transmission rate, can effectively improve the light emission rate of this Organnic electroluminescent device, in addition, and this preferred transparent conductive oxide electric conductivity excellence.These anode layer 2 thickness are preferably 70～200nm.Certainly, the material of this anode layer 2 and thickness can also be other materials and the thickness of this area routine.
The material of above-mentioned transparent substrates 1 is transparent glass, transparent polymer film material etc., as simple glass, polymer thin-film material substrate etc.Certainly, the material of transparent substrates 1 also can adopt this area other materials to substitute.The thickness of transparent substrates 1 also can adopt the conventional thickness in this area or select flexibly according to the requirement of application.
From the above, above-mentioned Organnic electroluminescent device is by being arranged to negative electrode stack gradually metallic reflector 43, (the semi-transparent metal level 41 of interfering layer 42/) n(n >=2 of combination) structure, effectively realize the interference effect to multi-wavelength light, effectively reduce the negative electrode of this Organnic electroluminescent device to reflection of light rate, improved its contrast.By the material selection alkali metal compound doping Organic Electron Transport Material of interfering layer 42, effectively strengthen the conductance of this interfering layer 42, realize the increase of avoiding the drive current of this Organnic electroluminescent device on the basis that increases interfering layer 42 thickness, therefore, realized the large area preparation of this Organnic electroluminescent device, and make the Organnic electroluminescent device even film layer of preparation, yields is high, low for equipment requirements, and cost is low, drive current is little, long service life.In addition, by selecting material and the thickness of metallic reflector 43, interfering layer 42, semi-transparent metal level 41, particularly the thickness of adjacent interfering layer is arranged to gradient, can multi-wavelength's light be produced and be interfered like this, can further reduce the negative electrode of above-mentioned Organnic electroluminescent device to reflection of light rate, improve its contrast.
Correspondingly, so above-described embodiment Organnic electroluminescent device preparation method can be according to showing as Fig. 3.Technological process preparation, simultaneously referring to Fig. 1～2, its preparation method comprises the steps:
S01., transparent substrates 1 is provided;
S02. prepare anode layer 2: in vacuum systems, transparent conductive oxide magnetron sputtering is prepared to anode layer 2 on substrate 1 one surfaces of step S01;
S03. prepare organic function layer 3: prepare anode layer 2 at step S02 with light-transmissive substrates layer 1 relative surface evaporation hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, the electron injecting layer 35 successively of face that combine, form organic function layer 3;
S04. prepare cathode layer 4: in vacuum coating system, at the organic function layer 3 outer surfaces successively semi-transparent metal layer material of evaporation, interfering layer material, and repeat the step at least twice of the semi-transparent metal layer material of evaporation, interfering layer material successively, form (semi-transparent metal level 41/ interfering layer 42) n, wherein n >=2;
Again by metallic reflection layer material evaporation at outermost interfering layer 42 surface filmings, form metallic reflector 43, thereby form (semi-transparent metal level 41/ interfering layer 42) n/ metallic reflector 43(n >=2) cathode layer 4 of structure.
Particularly, in above-mentioned S01 step, structure, material and the specification of transparent substrates 1 as described above, for length, do not repeat them here.In addition, in this S01 step, also comprise the treatment step in early stage to transparent substrates 1, as cleaned the step of decontamination, the step of specifically cleaning decontamination is as the step 1 of embodiment 1 below.
In above-mentioned steps S02, transparent conductive oxide and anode layer 2 thickness all as described above, do not repeat them here.Preferably, to become the sputtering technology condition of anode layer 2 be that base vacuum degree is 1 × 10 to sputter transparent conductive oxide -5～1 × 10 -3pa, the evaporation rate of magnetron sputtering is 0.2～2nm/s.Certainly the process conditions of, preparing anode layer 2 also can be carried out according to existing processing parameter setting.
Preferably, before carrying out following step S03, also comprise the anode layer 2 in step S02 is carried out to plasma treatment: this substrate that is coated with anode layer 2 is placed in to plasma processing chamber, carries out plasma treatment.This plasma treatment condition adopts the process conditions of this area routine.After plasma treatment, anode layer 2 can effectively improve anode work function, reduces the injection barrier in hole.
Certainly, also can directly select and be coated with anode as being coated with the transparent substrates of ITO, this transparent substrates that is coated with anode be carried out to the preliminary treatment in early stage, as carried out following step S03 after the PROCESS FOR TREATMENT such as cleaning, plasma treatment.
In above-mentioned steps S03, the material that evaporation hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35 are selected and even thickness are as described above.The operating pressure that each layer of involved process conditions of evaporation are preferably vacuum moulding machine film forming is 1 × 10 -5～1 × 10 -3pa, the evaporation rate of organic material is 0.01～1nm/s.
When organic function layer 3 as described above, when it comprises hole injection layer 31, hole transmission layer 32, electronic barrier layer, luminescent layer 33, hole blocking layer, electron transfer layer 34, the electron injecting layer 35 that stacks gradually combination, or when it comprises hole transmission layer 32, electronic barrier layer, luminescent layer 33, hole blocking layer, the electron transfer layer 34 that stacks gradually combination, or when it comprises hole transmission layer 32, luminescent layer 33, the electron transfer layer 34 that stacks gradually combination, the method for preparing organic function layer 3 is in this each layer of structure of anode layer 2 outer surfaces successively evaporation.
In above-mentioned steps S04, the material that evaporation metal reflector 43, interfering layer 42, semi-transparent metal level 41 are selected and even thickness are as described above.The evaporation rate of the metal in evaporation metal reflector 43, interfering layer 42, semi-transparent metal level 41 time is preferably 0.2～2nm/s, and the operating pressure of vacuum moulding machine film forming is 1 × 10 -5～1 × 10 -3pa.When evaporation interfering layer 42, the evaporation rate of Organic Electron Transport Material is 0.01～1nm/s, and the operating pressure of vacuum moulding machine film forming is 1 × 10 -5～1 × 10 -3pa.
In this step S04, while repeating the step of the semi-transparent metal layer material of evaporation, interfering layer material successively, preferably repeating 2～5 times, is (semi-transparent metal level 41/ interfering layer 42) n, wherein natural number of n=2～5.
Certainly, it is also understood that about the preparation method of embodiment of the present invention Organnic electroluminescent device and also should comprise the method for packing that this Organnic electroluminescent device is follow-up.
Correspondingly, the embodiment of the present invention also provides a kind of display screen, and it comprises display module and for controlling the control module of display module, certainly also comprises other necessary modules of application and display screen.Wherein, this display module comprises Organnic electroluminescent device described above, and particularly, in display module, Organnic electroluminescent device mentioned above is arranged according to matrix.Because this display screen contains above-mentioned Organnic electroluminescent device, therefore it has high-contrast, and its display frame is clear.
Correspondingly, the embodiment of the present invention further provides a kind of terminal that is provided with display screen, and the display screen of this terminal is the above-mentioned display that contains Organnic electroluminescent device.Certainly, should be appreciated that, according to the type difference of this terminal, this terminal, except containing display screen mentioned above, also contains other necessary modules or/and device.Therefore, this terminal can be non-portable terminal and portable terminal.Non-portable terminal can be that large-scale household electrical appliances (as television set, desktop computer display, be provided with air-conditioning, the washing machine etc. of display screen), factory are provided with lathe of display screen etc.; Portable terminal can be mobile phone, panel computer, notebook, personal digital assistant, game machine and e-book etc.Like this, because the display screen of this terminal is the above-mentioned display screen that contains Organnic electroluminescent device, therefore the display screen contrast of electronic device is high, and picture is clear.
Certainly, Organnic electroluminescent device mentioned above can also be applied in characteristic lighting field, as applied in the lighting field that reflectivity is low requiring.
Illustrate above-mentioned Organnic electroluminescent device aspect by multiple embodiment below.
Embodiment 1
That a kind of negative electrode has an antiradar reflectivity and anode is as the Organnic electroluminescent device of exiting surface, its structure is: glass substrate/ITO (70nm)/hole injection layer (CuPc, 20nm)/hole transmission layer (NPB, 40nm)/luminescent layer (Alq 3: C545T (10%), 10nm)/electron transfer layer (TPBi, 40nm)/electron injecting layer (LiF, 1nm)/Cr (10nm)/Alq 3: Li 2cO 3(60nm)/Cr (10nm)/Alq 3: Li 2cO 3(80nm)/Ag (100nm).Wherein, Cr (10nm)/Alq 3: Li 2cO 3(60nm)/Cr (10nm)/Alq 3: Li 2cO 3(80nm)/Ag (100nm) forms anode, and Cr layer is semi-transparent metal level, Alq 3: Li 2cO 3layer is interfering layer, and Ag (100nm) is metallic reflector.
Its preparation method is as follows:
(1) be 10 in vacuum degree -4in the vacuum coating system of Pa, prepare, glass substrate is cleaned with cleaning agent, then use distilled water, acetone is ultrasonic cleaning successively, then in coating system;
(2) first on substrate, prepare anode, its material is as transparent conductive oxide film ITO;
(3) at the CuPc of anode surface thermal evaporation 20nm thickness as hole injection layer, the NPB that thermal evaporation 40nm is thick on hole injection layer is as hole transmission layer, the Alq of the C545T doping that thermal evaporation 10nm is thick on hole transmission layer 3as luminescent layer, on luminescent layer, the TPBi film of thermal evaporation 40nm forms electron transfer layer, evaporates the LiF of 1nm as electron injecting layer on electron transfer layer, forms organic function layer;
(4) prepare Cr (10nm)/Alq at organic function layer outer surface successively evaporation 3: Li 2cO 3(60nm)/Cr (10nm)/Alq 3: Li 2cO 3(80nm)/Ag (100nm) forms negative electrode; Wherein, Cr metal level is as semi-transflective reflective layer; Alq 3middle Li doped 2cO 3as dielectric layer, its doping ratio is 20%, forms interfering layer, and last Ag layer is as reflector;
(5), after preparation, adopt glass cover-plate to encapsulate.
Embodiment 2
That a kind of negative electrode has an antiradar reflectivity and anode is as the Organnic electroluminescent device of exiting surface, its structure is: glass substrate/ITO (100nm)/hole injection layer (CuPc, 20nm)/hole transmission layer (NPB, 40nm)/luminescent layer (Alq 3: C545T (10%), 10nm)/electron transfer layer (TPBi, 40nm)/electron injecting layer (LiF, 1nm)/Al (7nm)/TPBi:Cs 2cO 3(20nm)/Al (7nm)/TPBi:Cs 2cO 3(30nm)/Al (7nm)/TPBi:Cs 2cO 3(40nm)/Mg-Al (70nm).Wherein, Al (7nm)/TPBi:Cs 2cO 3(20nm)/Al (7nm)/TPBi:Cs 2cO 3(30nm)/Al (7nm)/TPBi:Cs 2cO 3(40nm)/Mg-Al (70nm) forms anode, and Al layer is semi-transparent metal level, TPBi:Cs 2cO 3layer is interfering layer, and Mg-Al (70nm) is metallic reflector.
Its preparation method is as follows:
(1) be 10 in vacuum degree -4in the vacuum coating system of Pa, prepare, glass substrate is cleaned with cleaning agent, then use distilled water, acetone is ultrasonic cleaning successively, then in coating system;
(2) first on substrate, prepare anode, with reference to the step (2) of embodiment 1;
(3) prepare organic function layer at anode surface, with reference to the step (3) of embodiment 1;
(4) prepare Al (7nm)/TPBi:Cs at organic function layer outer surface successively evaporation 2cO 3(20nm)/Al (7nm)/TPBi:Cs 2cO 3(30nm)/Al (7nm)/TPBi:Cs 2cO 3(40nm)/Mg-Al (70nm) forms negative electrode; Wherein, Al metal level is as semi-transflective reflective layer, and Cs adulterates in TPBi 2cO 3as dielectric layer, its doping ratio is 5%, and last Mg-Al alloy is as reflector;
(5), after preparation, adopt glass cover-plate to encapsulate.
Embodiment 3
That a kind of negative electrode has an antiradar reflectivity and anode is as the Organnic electroluminescent device of exiting surface, its structure is: glass substrate/ITO (200nm)/hole injection layer (CuPc, 20nm)/hole transmission layer (NPB, 40nm)/luminescent layer (Alq 3: C545T (10%), 10nm)/electron transfer layer (TPBi, 40nm)/electron injecting layer (LiF, 1nm)/Au (5nm)/Bphen:Rb 2cO 3(25nm)/Au (5nm)/Bphen:Rb 2cO 3(30nm)/Au (5nm)/Bphen:Rb 2cO 3(35nm)/Au (5nm)/Bphen:Rb 2cO 3(40nm)/Mg-Ag (200nm).Wherein, Au (5nm)/Bphen:Rb 2cO 3(25nm)/Au (5nm)/Bphen:Rb 2cO 3(30nm)/Au (5nm)/Bphen:Rb 2cO 3(35nm)/Au (5nm)/Bphen:Rb 2cO 3(40nm)/Mg-Ag (200nm) forms anode, and Au layer is semi-transparent metal level, Bphen:Rb 2cO 3layer is interfering layer, and Mg-Ag (200nm) is metallic reflector.
Its preparation method is as follows:
(1) be 10 in vacuum degree -4in the vacuum coating system of Pa, prepare, glass substrate is cleaned with cleaning agent, then use distilled water, acetone is ultrasonic cleaning successively, then in coating system;
(2) first on substrate, prepare anode, with reference to the step (2) of embodiment 1;
(3) prepare organic function layer at anode surface, with reference to the step (3) of embodiment 1;
(4) prepare Au (5nm)/Bphen:Rb at organic function layer outer surface successively evaporation 2cO 3(25nm)/Au (5nm)/Bphen:Rb 2cO 3(30nm)/Au (5nm)/Bphen:Rb 2cO 3(35nm)/Au (5nm)/Bphen:Rb 2cO 3(40nm)/Mg-Ag (200nm) forms negative electrode; Wherein, Au metal level is as semi-transflective reflective layer, and Rb adulterates in Bphen 2cO 3as dielectric layer, its doping ratio is 50%, and last Mg-Ag alloy is as reflector;
(5), after preparation, adopt glass cover-plate to encapsulate.
Embodiment 4
That a kind of negative electrode has an antiradar reflectivity and anode is as the Organnic electroluminescent device of exiting surface, its structure is: glass substrate/ITO (100nm)/hole injection layer (CuPc, 20nm)/hole transmission layer (NPB, 40nm)/luminescent layer (Alq 3: C545T (10%), 10nm)/electron transfer layer (TPBi, 40nm)/electron injecting layer (LiF, 1nm)/Au (5nm)/PBD:CsN 3(20nm)/Au (5nm)/TAZ:LiN 3(30nm)/Au (5nm)/PBD:CsN 3(40nm)/Au (5nm)/TAZ:LiN 3(50nm)/Al (7nm)/PBD:CsN 3(60nm)/Mg-Ag (200nm).Wherein, Au (5nm)/PBD:CsN 3(20nm)/Au (5nm)/TAZ:LiN 3(30nm)/Au (5nm)/PBD:CsN 3(40nm)/Au (5nm)/TAZ:LiN 3(50nm)/Al (7nm)/PBD:CsN 3(60nm)/Mg-Ag (200nm), and Au layer, Al layer be semi-transparent metal level, TAZ:LiN 3layer, PBD:CsN 3layer is interfering layer, and Mg-Ag (200nm) is metallic reflector.
Its preparation method is as follows:
(1) be 10 in vacuum degree -4in the vacuum coating system of Pa, prepare, glass substrate is cleaned with cleaning agent, then use distilled water, acetone is ultrasonic cleaning successively, then in coating system;
(2) first on substrate, prepare anode, with reference to the step (2) of embodiment 1;
(3) prepare organic function layer at anode surface, with reference to the step (3) of embodiment 1;
(4) prepare Au (5nm)/PBD:CsN at organic function layer outer surface successively evaporation 3(20nm)/Au (5nm)/TAZ:LiN 3(30nm)/Au (5nm)/PBD:CsN 3(40nm)/Au (5nm)/TAZ:LiN 3(50nm)/Al (7nm)/PBD:CsN 3(60nm)/Mg-Ag (200nm) forms negative electrode; Wherein, having two kinds of semi-transparent reflection layers, is respectively Au metal level and Al metal level; Also having the interfering layer of two types, is respectively CsN 3the PBD of doping, doping mass ratio is 10%, also having one is LiN 3the TAZ of doping, doping mass ratio is 20%, last Mg-Ag alloy is as reflector;
(5), after preparation, adopt glass cover-plate to encapsulate.
Comparison example 1
The OLED structure of comparative example 1 is identical with embodiment 1, and its electrode does not adopt black electrode, directly adopts the metal A g of condition of equivalent thickness as negative electrode, and its cathode construction is with Ag (100nm).
Comparison example 2
The structure of comparative example 2 is identical with embodiment 1, and it has adopted a black electrode, but only adopting a dielectric layer structure, its cathode construction is Cr (10nm)/Alq 3: Li 2cO 3(80nm)/Ag (100nm).
Organnic electroluminescent device carries out correlated performance test
When Organnic electroluminescent device is not lighted in Organnic electroluminescent device prepared by above-described embodiment 1 to embodiment 4 and comparison example 1,2, carry out reflectance test, test result is as following table 1.
Table 1
From above-mentioned table 1, the Organnic electroluminescent device of preparing in above-described embodiment 1-4 is owing to adopting negative electrode to be arranged to stack gradually metallic reflector 43, (the semi-transparent metal level 41 of interfering layer 42/) n(n >=2 of combination) structure form black anode, by the synergy of each layer, effectively reduce the total reflection of light, realized low reflectivity.The particularly interfering layer of alternately laminated combination and semi-transparent metal level, and the thickness of two adjacent interfering layers is arranged to gradient, can multi-wavelength's light be produced and be interfered like this, can further reduce the negative electrode of above-mentioned Organnic electroluminescent device to reflection of light rate, improve its contrast.The reflectivity of Organnic electroluminescent device prepared by embodiment 1-4 is compared with Organnic electroluminescent device in comparison example 1,2, and do not adopt the comparison example 1 of the OLED of black electrode, its device has very high reflectivity, has reached 87.6%, and obviously the contrast of this device is lower.The black electrode that has adopted the embodiment of the present invention to provide, because adopted multiple dielectric layers, can disappear by force mutually to the light of multiple wavelength, and therefore its reflectivity is quite low, minimumly reaches 10.4%.And the comparison example 2 of the black electrode that adopts a dielectric layer that arrives, its reflectivity also has 25.4%, and the black electrode that the embodiment of the present invention provides is described, and its effect that reduces reflectivity is more obvious.
The foregoing is only preferred embodiment of the present invention, not in order to limit the present invention, all any amendments of doing within the spirit and principles in the present invention, be equal to and replace and improvement etc., within all should being included in protection scope of the present invention.

Claims (10)

1. an Organnic electroluminescent device, comprise the transparent substrates, anode layer, organic function layer and the cathode layer that stack gradually combination, described organic function layer is included in luminescent layer luminous under the driving of additional power source, it is characterized in that: described cathode layer comprises metallic reflector, at least two interfering layers and at least two semi-transparent metal levels, described interfering layer and semi-transparent metal level are alternately laminated to be incorporated between described metallic reflector and organic function layer, the stacked combination of described interfering layer and metallic reflector, the stacked combination of semi-transparent metal level and organic function layer; Wherein, described interfering layer material comprises Organic Electron Transport Material and is doped in alkali metal compound wherein, and described alkali metal compound quality is 5～50% of interfering layer gross mass.
2. Organnic electroluminescent device as claimed in claim 1, is characterized in that: described alkali metal compound be alkali-metal carbonate and or alkali-metal nitride.
3. Organnic electroluminescent device as claimed in claim 1, is characterized in that: the number of plies of described interfering layer is 2～5 layers.
4. the Organnic electroluminescent device as described in claim 1～3 any one, is characterized in that: the thickness of described each interfering layer is 20～80nm.
5. the Organnic electroluminescent device as described in claim 1～3 any one, is characterized in that: the thickness of described adjacent interfering layer between two in gradient.
6. the Organnic electroluminescent device as described in claim 1～3 any one, is characterized in that: described each semi-transparent metal layer thickness is 5nm～10nm.
7. the Organnic electroluminescent device as described in claim 1～3 any one, is characterized in that: described metallic reflection layer thickness is 70nm～200nm.
8. the Organnic electroluminescent device as described in claim 1～3 any one, is characterized in that: the thickness of described each interfering layer is 20nm～80nm, and between two adjacent described interfering layer thickness in gradient;
The thickness of described each semi-transparent metal level is 5nm～10nm, and the thickness of described metallic reflector is 70nm～200nm.
9. a display screen, comprises display module and for controlling the control module of display module, it is characterized in that: described display module contains just like the Organnic electroluminescent device described in claim 1～8 any one.
10. be provided with a terminal for display screen, the display screen of described terminal is display screen as claimed in claim 9.
CN201310192344.2A 2013-05-22 2013-05-22 Organic light emission diode, display screen and terminal Pending CN104183711A (en)

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Application publication date: 20141203