CN102769104A - Flexible two-sided light-emitting organic electroluminescence device and preparation method thereof - Google Patents
Flexible two-sided light-emitting organic electroluminescence device and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a flexible two-sided light-emitting organic electroluminescence device, which comprises a light-transmitting flexible substrate layer, an anode layer, a first organic electroluminescence structure, a reflecting connecting layer, a second organic electroluminescence structure and a cathode layer which are arranged in an overlying mode in sequence, wherein the first organic electroluminescence structure and the second organic electroluminescence structure respectively have a light emitting layer; and the reflecting connecting layer comprises a first reflecting conducting layer, an insulation layer and a second reflecting conducting layer which are arranged in an overlying mode in sequence. The flexible two-sided light-emitting organic electroluminescence device is excellent in flexure property and flexibility; two light-emitting surfaces can emit light independently; the emitted light is high in luminance; and moreover the light emitted from the two light-emitting surfaces does not influence each other. A preparation method of the flexible two-sided light-emitting organic electroluminescence device has simple processes, the production efficiency is improved, the production cost is reduced, and thus the flexible two-sided light-emitting organic electroluminescence device is applicable for industrial production.
Description
Technical field
The invention belongs to the electric light source technology field, relate to a kind of flexible double-sided light emitting organic electroluminescence device and preparation method thereof specifically.
Background technology
The electric light source industry is the focus that countries in the world are competitively studied always, in World Economics in occupation of important status.Present widely used light source is a glow discharge spot lamp, and the principle of this light source is that the inside with lamp charges into mercurous mist after vacuumizing, and utilizes the ultraviolet excitation light-emitting phosphor that gas discharge is luminous or gas discharge produces.Yet the pulse color break-up of glow discharge spot lamp causes people's visual fatigue easily, and the mercury pollution environment, and along with the progress of society with science and technology, the green light source of researching and developing energy-conservation environmental protection again substitutes conventional light source, becomes the important topic that various countries are competitively studied.
Organnic electroluminescent device (OLED) is a kind of in the electric light source.OLED is based on a kind of current mode light emitting semiconductor device of organic material.Its typical structure is that the luminous organic material of on ito glass, making one deck tens nanometer thickness is made luminescent layer, and there is the metal electrode of one deck low work function the luminescent layer top.When being added with voltage on the electrode, luminescent layer just produces light radiation.Advantages such as active illuminating, luminous efficiency higher, low in energy consumption, light, thin, the no visual angle restriction that the OLED display device has are thought to be most likely at the display device of new generation that occupies the dominance on following display device market by the insider.Because global increasing display producer drops into research and development one after another, has promoted the industrialization process of OLED greatly, makes that the growth rate of OLED industry is surprising, has arrived the eve of scale of mass production at present.As a brand-new Display Technique, the ten years development in the past of OLED technology is swift and violent, has obtained huge achievement.1987, the C.W.Tang of U.S. Eastman Kodak company and VanSlyke reported the breakthrough in the organic electroluminescent research.Utilize the ultrathin film technology to prepare high brightness, high efficiency double-deck micromolecule Organnic electroluminescent device.In this double-deck device, brightness reaches 1000cd/m under the 10V
2, its luminous efficiency is that 1.51lm/W, life-span were greater than 100 hours.Nineteen ninety; People such as the Burronghes of univ cambridge uk propose to process polymer electroluminescence (EL) device with macromolecule conjugated polymer polyphenylene ethylene (PPV) first; Subsequently; Professor Heeger of California university leader's experimental group was further proved conclusively the polymer electroluminescence characteristic in 1991, and improved.From then on brand-new field one polymer electroluminescent device (PLED) has been opened up in organic light-emitting device research.Since then, Organnic electroluminescent device has obtained development rapidly in the short more than ten years.
At present, Organnic electroluminescent device has obtained some following 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; (3) OLED can make on multiple substrate such as glass, pottery, metal, plastic or other material, and this is 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; (6) OLED can make light penetrating device, and when device application was on window-glass, light was light source beyond daytime like this, and night then can be as lighting source.
Though OLED has above-mentioned described advantage at present, also has following weak point:
1. in the existing OLED device, adopt the substrate of glass material, cause the OLED device can not be crooked as the OLED device, poor toughness, frangible, limited the range of application of OLED;
2. existing OLED device major part can only go out the side-draw of light from anode or negative electrode, makes end emission or top emission OLED device, and such OLED device can not double-side, has also limited the OLED device in needs double-side Application for Field;
3. the OLED device that existing OLED device is also sought at double-side, but when having a plurality of luminescent layer, the only a kind of mixed light that sends, the light of multiple color can not separately be launched, and can not get the emission of the light of solid color.Showing application facet, because whole light-emitting device all is transparent, so the background of any one side of light-emitting device all can impact the demonstration of another side.
Summary of the invention
Technical problem to be solved by this invention is to overcome the defective of prior art; Provide a kind of flexural property with flexible good; Two exiting surfaces can be launched light separately, and luminosity is high, and the flexible double-sided light emitting organic electroluminescence device that is independent of each other of the light that sends of two exiting surfaces.
And, the preparation method of above-mentioned flexible double-sided light emitting organic electroluminescence device.
In order to realize the foregoing invention purpose, technical scheme of the present invention is following:
A kind of flexible double-sided light emitting organic electroluminescence device comprises printing opacity flexible substrate layer, anode layer, first organic electroluminescence structure, reflective articulamentum, second organic electroluminescence structure and cathode layer that stack successively is provided with; Said first organic electroluminescence structure and second organic electroluminescence structure contain luminescent layer; Reflective articulamentum comprises first reflective conductive layer, insulating barrier, second reflective conductive layer that stack successively is provided with.
And a kind of flexible double-sided light emitting organic electroluminescence device preparation method comprises the steps:
The printing opacity flexible substrate layer is provided;
On said printing opacity flexible substrate layer, plate anode layer;
On said anode layer, plate first organic electroluminescence structure, reflective articulamentum, second organic electroluminescence structure successively, wherein, said first organic electroluminescence structure and second organic electroluminescence structure contain luminescent layer; Reflective articulamentum comprises first reflective conductive layer, insulating barrier, second reflective conductive layer that stack successively is provided with;
Said second organic electroluminescence structure with reflective articulamentum facing surfaces plating cathode layer, obtain said flexible double-sided light emitting organic electroluminescence device.
The flexible double-sided light emitting organic electroluminescence device of the present invention is through first organic electroluminescence structure, reflective articulamentum and second organic electroluminescence structure of stack setting successively; The light that this reflective articulamentum can be effectively sends first organic electroluminescence structure and second organic electroluminescence structure reflexes to printing opacity flexible substrate layer and cathode layer respectively and penetrates; Realize that two exiting surfaces launch light separately, having strengthened simultaneously should flexibility double-sided light emitting organic electroluminescence device luminous efficiency and intensity.Because reflective articulamentum contains first reflective conductive layer, insulating barrier, second reflective conductive layer that stack successively is provided with; This two conductive layer can play the reflecting surface effect; The light that first organic electroluminescence structure and second organic electroluminescence structure are sent reflexes to printing opacity flexible substrate layer and cathode layer respectively and penetrates; The light of having avoided first organic electroluminescence structure and second organic electroluminescence structure to send interacts, and the background that efficiently solves the OLED one side of existing double-side impacts the demonstration of another side.This first reflective conductive layer is simultaneously also as the effect of cathode layer; Second reflective conductive layer is also as the effect of anode layer; Insulating barrier can be effectively separated first reflective conductive layer and the insulation of first reflective conductive layer, makes win organic electroluminescence structure and second organic electroluminescence structure luminous respectively.
The substrate layer of the flexible double-sided light emitting organic electroluminescence device of the present invention is the printing opacity flexible substrate layer, makes this flexibility double-sided light emitting organic electroluminescence device have good flexural property and flexible ability.
The mode that the flexible double-sided light emitting organic electroluminescence device of the present invention preparation method adopts coating is coating on the printing opacity flexible substrate layer successively, makes to form good Ohmic contact, compact conformation between this each layer of Organnic electroluminescent device; Improved its luminescent properties; And stable luminescent property, preparation method's operation is simple, has improved production efficiency; Reduce production cost, be suitable for suitability for industrialized production.
Description of drawings
Fig. 1 is a kind of preferred structure sketch map of the flexible double-sided light emitting organic electroluminescence device of the embodiment of the invention;
Fig. 2 is the another kind of preferred structure sketch map of the flexible double-sided light emitting organic electroluminescence device of the embodiment of the invention;
Fig. 3 is another preferred structure sketch map of the flexible double-sided light emitting organic electroluminescence device of the embodiment of the invention;
Fig. 4 is the flexible double-sided light emitting organic electroluminescence device of embodiment of the invention preparation method's a schematic flow sheet.
Embodiment
Clearer for technical problem, technical scheme and beneficial effect that the present invention will be solved, below in conjunction with embodiment, the present invention is further elaborated.Should be appreciated that specific embodiment described herein only in order to explanation the present invention, and be not used in qualification the present invention.
The embodiment of the invention provides a kind of flexural property with flexible good, and two exiting surfaces can be launched light separately, and luminosity is high, and the flexible double-sided light emitting organic electroluminescence device that is independent of each other of the light that sends of two exiting surfaces.To shown in Figure 3, this flexibility double-sided light emitting organic electroluminescence device comprises printing opacity flexible substrate layer 1 that stack successively is provided with, anode layer 2, first organic electroluminescence structure 3, reflective articulamentum 4, second organic electroluminescence structure 5 and cathode layer 6 like Fig. 1.Wherein, first organic electroluminescence structure 3 and second organic electroluminescence structure 5 contain luminescent layer 33 respectively and luminescent layer 53 are arranged; First reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ' that reflective articulamentum 4 comprises successively that stack is provided with.Like this; First organic electroluminescence structure 3, reflective articulamentum 4 and second organic electroluminescence structure 5 that this flexibility double-sided light emitting organic electroluminescence device is provided with through stack successively; The light that this reflective articulamentum 4 can be effectively sends first organic electroluminescence structure 3 and second organic electroluminescence structure 5 reflexes to printing opacity flexible substrate layer 1 respectively with cathode layer 6 and penetrate; Realize that two exiting surfaces launch light separately, having strengthened simultaneously should flexibility double-sided light emitting organic electroluminescence device luminous efficiency and intensity.Because first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ' that reflective articulamentum 4 contains successively that stack is provided with; This first reflective conductive layer 41 and second reflective conductive layer 41 ' can play the reflecting surface effect; The light that first organic electroluminescence structure 3 and second organic electroluminescence structure 5 are sent reflexes to printing opacity flexible substrate layer 1 respectively with cathode layer 6 and penetrate; The light of having avoided first organic electroluminescence structure 3 and second organic electroluminescence structure 5 to send interacts, and the background that efficiently solves the OLED one side of existing double-side impacts the demonstration of another side.This first reflective conductive layer 41 is simultaneously also as the effect of cathode layer; Second reflective conductive layer 41 ' is also as the effect of anode layer; Insulating barrier 42 can be effectively separated the insulation of two reflective conductive layers, makes the organic electroluminescence structure 3 of winning distinguish luminous with second organic electroluminescence structure 5.In addition, the substrate layer of this flexibility double-sided light emitting organic electroluminescence device is a printing opacity flexible substrate layer 1, makes this flexibility double-sided light emitting organic electroluminescence device have good flexural property and flexible ability.
Particularly, the material of above-mentioned printing opacity flexible substrate layer 1 is preferably flexible polymer thin-film material such as PETG (PET), polyether sulfone (PES), PEN (PEN), clear polyimides (PI), cyclic olefine copolymer (COC), Merlon (PC) or polyethylene (PE).Such preferred polymer thin-film material flexural property is good with flexible ability, gives the flexible double-sided light emitting organic electroluminescence device of present embodiment good flexural property and flexible ability.The thickness of this printing opacity flexible substrate layer 1 is preferably 0.1mm～0.5mm, and the printing opacity flexible substrate layer 1 of this preferred thickness can effectively improve the penetrability of light, and further enhancing should flexibility double-sided light emitting organic electroluminescence device light extraction efficiency.
Above-mentioned anode layer 2 thickness are preferably 18nm-25nm, more excellent 20nm, and its material is preferably used silver (Ag), also can adopt the Al material certainly.The anode 2 of this preferred thickness and material can effectively reduce the resistance of electrode when energising; Reduce the heat release of electrode and the heat dispersion of intensifier electrode; Reduce production costs accordingly, simultaneously, anode 2 can effectively guarantee penetrating of light; Be also referred to as well-illuminated electrode, thus strengthen the flexible double-sided light emitting organic electroluminescence device of present embodiment printing opacity flexible substrate layer 1 go out luminous intensity.
Further, between the Ag layer 2 and first organic electroluminescence structure 3 also stack be provided with the hole and inject reinforced layer 9.The thickness that reinforced layer 9 is injected in this hole is preferably 3-10nm, 6nm more preferably, and its material is preferably WO
3, MoO
3, V
2O
5In at least a, more preferably WO
3Further hole injectability of reinforced layer 9 is injected in this hole, has improved flexible double-sided light emitting organic electroluminescence device luminosity.In addition, further strengthen the ohmic contact that reinforced layer 9 and 2 formation of anode layer are injected in the cave, strengthen the electric conductivity of anode layer 2.
Further; Above-mentioned first organic electroluminescence structure 3 also comprises one deck at least and/or the electron transfer layer 34 in hole injection layer 31, the hole transmission layer 32, the one deck at least in the electron injecting layer 35; Wherein, At least one range upon range of adding in hole injection layer 31, the hole transmission layer 32, be arranged between anode layer 2 and the luminescent layer 33, and at least one range upon range of the adding in electron transfer layer 34, the electron injecting layer 35 is arranged between luminescent layer 33 and the reflective articulamentum 4.Second organic electroluminescence structure 5 also comprises one deck at least and/or the electron transfer layer 54 in hole injection layer 51, the hole transmission layer 52, the one deck at least in the electron injecting layer 55; Wherein, At least one range upon range of adding in hole injection layer 51, the hole transmission layer 52, be arranged between first organic electroluminescence structure 3 and the luminescent layer 53, and at least one range upon range of the adding in electron transfer layer 54, the electron injecting layer 55 is arranged between luminescent layer 53 and the cathode layer 6.
Above-mentioned hole injection layer 31 and 51 thickness are preferably 10nm～15nm; Its material be preferably CuPc (CuPc), 4,4 ', 4 " at least a in three (N-3-aminomethyl phenyl-N-phenyl-amino)-triphenylamines (m-MTDATA), the transition metal oxide; wherein, transition metal oxide such as V
2O
5, MoO
3, WO
3, RuO
x(x=2,3,4 or 5). Hole transmission layer 32 and 52 thickness are preferably 40nm～60nm; Its material is preferred but be not limited only to phenyl beautiful jade (NPB), can certainly be N, N '-two (3-aminomethyl phenyl)-N; N '-diphenyl-4; 4 '-benzidine (TPD), 1,3, at least a in 5-triphenylbenzene (TDAPB), tetrafluoro tetra cyanogen subculture dimethyl benzene quinone (F4-TCNQ) doping MeO-TPD, CuPc CuPc or the P type doping inorganic semiconductor. Electron transfer layer 34 and 54 thickness are preferably 20nm～80nm, its material preferred but be not limited only to that n mixes 4,7-diphenyl-1; At least a among 10-phenanthroline (n-Bphen), the BPhen can certainly be oxine aluminium (Alq3), 2-(4-xenyl)-5-(the 4-tert-butyl group) phenyl-1,3; 4-oxadiazole (PBD), 2; 5-two (1-naphthyl)-1,3,4-diazole (BND), 1; 2, at least a in 4-triazole derivative (like TAZ etc.), N-aryl benzimidazole (TPBI), quinoxaline derivant (TPQ) or the n type doping inorganic semiconductor. Electron injecting layer 35 and 55 thickness are preferably 0.5nm～20nm; Its material is preferably lithium fluoride (LiF), caesium lithium (CsF), caesium (Cs), lithium (Li) and/or calcium low-work-function materials such as (Ca); Can certainly substitute with this area other materials commonly used; As, alkali earth metal fluoride (NaF, CaF
2, MgF
2) or chloride (NaCl, KCl, RbCl).
In above-mentioned first organic electroluminescence structure 3 and second organic electroluminescence structure 5, hole and electronics meet each other and are compound, and luminescent material directly or through NE BY ENERGY TRANSFER is excited, and the luminescent material that excites is through the luminous ground state of returning.In first organic electroluminescence structure 3 and second organic electroluminescence structure 5, preferably add carrier injection layer respectively and improved the injection efficiency of charge carrier; Not only guaranteed the good adhesion between organic function layer and anode layer 2, reflective articulamentum 4 and the cathode layer 6, but also feasible easier being injected in the organic functional thin film of charge carrier from anode layer 2 and cathode layer 6.When being preferably transition metal oxide like hole injection layer 31 and 51; This material and organic cavity transmission layer 32 and 52 energy level comparison match make the hole of second reflective conductive layer 41 ' of anode layer 2 and reflective articulamentum 4 inject and have obtained tangible reinforcement, in addition; Can form ohmic contact between hole injection layer 31 and anode layer 2 and hole injection layer 51 and second reflective conductive layer 41 '; Strengthen electric conductivity, further improved the hole injectability of this flexibility double-sided light emitting organic electroluminescence device, improved its luminosity and intensity; Effectively regulate the injection and the transmission rate in electronics and hole; Equilibrium carrier, the control recombination region has obtained desirable luminosity and luminous efficiency.
Particularly, first reflective conductive layer 41 that above-mentioned reflective articulamentum 4 comprises and the material of second reflective conductive layer 41 ' are preferably at least a among Ag, the Al, and its thick end is preferably 60nm～200nm.First reflective conductive layer 41 of this preferred thickness and material and second reflective conductive layer 41 ' can effectively reflect its surperficial light of directive; The light of avoiding first organic electroluminescence structure 3 and second organic electroluminescence structure 5 to send interacts; Simultaneously; Can also effectively reduce resistance when energising, reduce the heat release and the heat dispersion that strengthens it of first reflective conductive layer 41 and second reflective conductive layer 41 ', reduce production costs accordingly.The material of insulating barrier 42 is SiO, and its thickness is preferably 200nm～1000nm.The insulating barrier 42 of this thickness and material can effectively play the penetration of insulating effect and block light, guarantees that further the light that first organic electroluminescence structure 3 and second organic electroluminescence structure 5 send is independent of each other.
The material of above-mentioned cathode layer 6 is preferably argent (Ag), samarium (Sm), ytterbium (Yb) or its alloy.The preferred of cathode layer 6 is 18nm～25nm.The light transmission rate of the cathode layer 6 of this preferred material and thickness can be up between 55～75%; The cathode layer 6 of this preferred thickness and material can also effectively reduce the resistance of electrode when energising simultaneously; Reduce the heat release of electrode and the heat dispersion of intensifier electrode, reduce production costs accordingly.Certainly, also can adopt other metal substitutes commonly used of this area.When choosing the material of this cathode layer 6 and above-mentioned anode layer 2, should make the work function value that is lower than the material of above-mentioned anode layer 2 as the work function value of the material of this cathode layer 6.
Further, between above-mentioned anode layer 2 and the printing opacity flexible substrate layer 1 also stack be provided with antireflective coating 7 or/and cathode layer 6 with second organic electroluminescence structure, 5 facing surfaces on also stack be provided with antireflective coating 7 '.This antireflective coating 7 is or/and 7 ' thickness is preferably 40nm～100nm, and its material is preferably zinc sulphide (ZnS), zinc selenide (ZnSe), oxine aluminium (Alq
3), bromocresol purple (BCP), phenyl beautiful jade (NPB), 4,4 ', 4 " at least a in three (N-3-aminomethyl phenyl-N-phenyl-amino)-triphenylamines (m-MTDATA).This antireflective coating 7 can effectively strengthen the light emission rate of anode layer 2 or/and antireflective coating 7 ' can effectively strengthen the light emission rate of cathode layer 6.When cathode layer 6 with second organic electroluminescence structure, 5 facing surfaces on stack when antireflective coating 7 ' is set; Can also effectively completely cut off cathode layer 6 and avoid its outer surface generation oxidation with contacting of air and make the electric conductivity of cathode layer 6 and the defective that light transmission reduces, thereby prolong the above-mentioned flexible double-sided light emitting organic electroluminescence of the present invention device lifetime.
Further, when stack was provided with antireflective coating 7 between above-mentioned anode layer 2 and printing opacity flexible substrate layer 1, also stack was provided with resilient coating 8 between this antireflective coating 7 and printing opacity flexible substrate layer 1; Perhaps further, when stack was not provided with antireflective coating 7 between above-mentioned anode layer 2 and printing opacity flexible substrate layer 1, also stack was provided with resilient coating 8 between anode layer 2 and printing opacity flexible substrate layer 1.The material of this resilient coating 8 is preferably light-cured resin, and its thickness is preferably 0.5 μ m～10 μ m.This resilient coating 8 can effectively improve between antireflective coating 7 and the printing opacity flexible substrate layer 1 or the adhesion of anode layer 2 and printing opacity flexible substrate layer 1.
In sum, the flexible double-sided light emitting organic electroluminescence device of the embodiment of the invention can be the preferred embodiment of following several kinds of structures at least, is not limited only to following structure certainly:
First kind of structure: as shown in Figure 1, the flexible double-sided light emitting organic electroluminescence device of the embodiment of the invention comprises printing opacity flexible substrate layer 1 that stack successively is provided with, anode layer 2, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ', hole transmission layer 52, luminescent layer 53, electron transfer layer 54 and cathode layer 6.Wherein, this hole transmission layer 32, luminescent layer 33, electron transfer layer 34 constitute first organic electroluminescence structure 3; Hole transmission layer 52, luminescent layer 53, electron transfer layer 54 constitute second organic electroluminescence structure 5; First reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ' constitute reflective articulamentum 4.
Second kind of structure: as shown in Figure 2, the flexible double-sided light emitting organic electroluminescence device of the embodiment of the invention comprises printing opacity flexible substrate layer 1 that stack successively is provided with, anode layer 2, hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35, first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ', hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 and cathode layer 6, antireflective coating 7 '.Wherein, hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35 constitute first organic electroluminescence structure 3; Hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 constitute second organic electroluminescence structure 5; First reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ' constitute reflective articulamentum 4.
The third structure: as shown in Figure 3, the flexible double-sided light emitting organic electroluminescence device of the embodiment of the invention comprises that printing opacity flexible substrate layer 1, resilient coating 8, antireflective coating 7, anode layer 2, hole that stack successively is provided with inject reinforced layer 9, hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35, first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ', hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 and cathode layer 6, antireflective coating 7.Wherein, hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35 constitute first organic electroluminescence structure 3; Hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 constitute second organic electroluminescence structure 5; First reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ' constitute reflective articulamentum 4.
The embodiment of the invention also provides the preparation method of above-mentioned flexible double-sided light emitting organic electroluminescence device, and this method process chart is as shown in Figure 4, and simultaneously referring to Fig. 1 or Fig. 2 or Fig. 3, this method comprises the steps:
S1., printing opacity flexible substrate layer 1 is provided;
S2. on printing opacity flexible substrate layer 1, plate anode layer 2;
S3. on anode layer 2, plate first organic electroluminescence structure 3, reflective articulamentum 4, second organic electroluminescence structure 5 successively, wherein, first organic electroluminescence structure 3 and second organic electroluminescence structure 5 contain luminescent layer 33 respectively; First reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ' that reflective articulamentum 4 comprises successively that stack is provided with;
S4. said second organic electroluminescence structure 5 with reflective articulamentum 4 facing surfaces plating cathode layer 6, obtain flexible double-sided light emitting organic electroluminescence device.
Particularly, in above-mentioned flexible double-sided light emitting organic electroluminescence device preparation method's the S1 step, the preposition place that preferably includes printing opacity flexible substrate layer 1 preferably manages.This pre-process can comprise chemical reagent cleaning, ultrasonic waves for cleaning, water cleaning etc., and is after cleaning finishes, for use with the IR bake oven dry.This pre-process adsorptivity and its surperficial organic pollution of removal.
In above-mentioned flexible double-sided light emitting organic electroluminescence device preparation method's the S2 step, the mode of plating anode layer 2 is preferably vapor deposition, sputter or spraying plating, more preferably the mode of magnetron sputtering.The material of anode layer 2 and the thickness of plating are set forth hereinbefore, repeat no more at this.
In above-mentioned flexible double-sided light emitting organic electroluminescence device preparation method's the S3 step, the mode of plating first organic electroluminescence structure 3, reflective articulamentum 4 and second organic electroluminescence structure 5 is preferably vapor deposition, sputter, spraying plating or chemical deposition mode.The material of this first organic electroluminescence structure 3, reflective articulamentum 4 and second organic electroluminescence structure 5 and thickness are set forth hereinbefore, in order to practice thrift length, repeat no more at this.
In above-mentioned flexible double-sided light emitting organic electroluminescence device preparation method's the S4 step, the mode of plating cathode layer 6 is preferably vapor deposition, sputter or spraying plating, more preferably the vapor deposition mode.The material of cathode layer 6 and the thickness of plating are set forth hereinbefore, repeat no more at this.
Further; Between above-mentioned flexible double-sided light emitting organic electroluminescence device preparation method's S1 and S2 step; Any one deck on a surface of printing opacity flexible substrate layer 1 in plating resilient coating 8, the antireflective coating 7 is again in the step of plating anode layer 2 with printing opacity flexible substrate layer 1 facing surfaces of resilient coating 8 or antireflective coating 7; Perhaps on a surface of printing opacity flexible substrate layer 1, plate resilient coating 8, antireflective coating 7 successively, again in the step of plating anode layer 2 with resilient coating 8 facing surfaces of antireflective coating 7.The thickness of resilient coating 8, antireflective coating 7 and material are set forth hereinbefore, repeat no more at this.
Further; Between above-mentioned flexible double-sided light emitting organic electroluminescence device preparation method's S2 and S3 step; Reinforced layer 9 is injected in plating hole on the surface of first organic electroluminescence structure 3 at anode layer 2; After plating finished, that then injects reinforced layer 9 again in the hole carried out above-mentioned S3 step with anode layer 2 facing surfaces.The thickness of this cave implanted layer 9 and material are set forth hereinbefore, repeat no more at this.
Further; In above-mentioned flexible double-sided light emitting organic electroluminescence device preparation method's S3 step, when first organic electroluminescence structure 3 comprises that also one deck at least and/or electron transfer layer 34 in hole injection layer 31, the hole transmission layer 32, one deck at least and/or second organic electroluminescence structure 5 in the electron injecting layer 35 also comprise one deck at least and/or electron transfer layer 54 in hole injection layer 51, the hole transmission layer 52, one deck at least in the electron injecting layer 55.Preferred adopt vapor deposition anode layer 2 or hole injection layer 9 with printing opacity flexible substrate layer 1 facing surfaces on plate hole injection layer 31 and/or hole transmission layer 32, luminescent layer 33, electron transfer layer 34 and/or electron injecting layer 35 successively, and/or reflective articulamentum 4 with first organic electroluminescence structure, 3 facing surfaces on plate hole injection layer 51 and/or hole transmission layer 52, luminescent layer 53, electron transfer layer 54 and/or electron injecting layer 55 successively.Material of organic electroluminescence structure 3 each layers and thickness are set forth hereinbefore, in order to practice thrift length, repeat no more at this.
Further, after above-mentioned flexible double-sided light emitting organic electroluminescence device preparation method's S4 step, above-mentioned cathode layer 6 with second organic electroluminescence structure, 5 facing surfaces be that the outer surface of cathode layer 6 also is coated with another antireflective coating 7 '.The material of antireflective coating 7 ' and the thickness of plating repeat no more at this to set forth hereinbefore.
The mode that above-mentioned flexible double-sided light emitting organic electroluminescence device preparation method adopts coating is coating on printing opacity flexible substrate layer 1 successively; Make and to form good Ohmic contact between each layer of flexibility double-sided light emitting organic electroluminescence device; Improved its luminescent properties, preparation method's operation is simple, has improved production efficiency; Reduce production cost, be suitable for suitability for industrialized production.
Combine instantiation at present, the present invention is further elaborated.
Embodiment 1
The flexible double-sided light emitting organic electroluminescence apparatus structure of present embodiment is as shown in Figure 1, and this flexibility double-sided light emitting organic electroluminescence device comprises successively printing opacity flexible substrate layer 1 that stack is provided with, anode layer 2, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ', hole transmission layer 52, luminescent layer 53, electron transfer layer 54 and cathode layer 6.Wherein, printing opacity flexible substrate layer 1 is the PC of 0.1mm, and anode layer 2 is the thick Ag layer of 20nm; Hole transmission layer 32 and 52 is the thick NPB layer of 60nm, and luminescent layer 33 is the thick white light emitting material layer of 20nm, and luminescent layer 53 is the thick blue light emitting material layer of 30nm; Electron transfer layer 34 and 54 is the thick n-Bphen layer of 20nm; First reflective conductive layer 41 and second reflective conductive layer 41 ' are the thick Ag layer of 60nm, and insulating barrier 42 is the thick SiO layer of 1000nm, and cathode layer 6 is the thick Ag of 18nm; Hole transmission layer 32, luminescent layer 33, electron transfer layer 34 constitute first organic electroluminescence structure 3; Hole transmission layer 52, luminescent layer 53, electron transfer layer 54 constitute second organic electroluminescence structure 5; First reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ' constitute reflective articulamentum 4.
Its preparation method is following:
(1) PC is provided substrate, this PC substrate is cut into required shape and area, again this transparent substrates is cleaned by the flow process that liquid detergent cleaning → ethanol cleaning → acetone → pure water cleans; Each cleaning step all cleans with supersonic wave cleaning machine, and preferred employing of each washing cleaned 5 minutes, stopped 5 minutes; Repeat 3 times method respectively; After cleaning finishes,, obtain printing opacity flexible substrate layer 1 with the IR bake oven dry;
(2) vapor deposition Ag layer on a surface of printing opacity flexible substrate layer 1 forms anode layer 2;
(3) anode layer 2 with printing opacity flexible substrate layer 1 facing surfaces vapor deposition hole transmission layer 32 successively, luminescent layer 33, electron transfer layer 34, first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ', hole transmission layer 52, luminescent layer 53, electron transfer layer 54;
(4) electron transfer layer 54 with luminescent layer 53 facing surfaces vapor deposition cathode layers 6;
(5) evaporation encapsulates device after accomplishing, and obtains the flexible double-sided light emitting organic electroluminescence device of present embodiment.
Embodiment 2
The flexible double-sided light emitting organic electroluminescence apparatus structure of present embodiment is as shown in Figure 2, and this flexibility double-sided light emitting organic electroluminescence device comprises successively printing opacity flexible substrate layer 1 that stack is provided with, anode layer 2, hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35, first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ', hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 and cathode layer 6, antireflective coating 7.Wherein, printing opacity flexible substrate layer 1 is the COC of 0.5mm, and anode layer 2 is the thick Ag layer of 40nm, and hole injection layer 31 is the thick WO of 13nm
3, hole transmission layer 32 is the thick NPB layer of 60nm, luminescent layer 33 is the thick white light emitting material layer of 20nm, electron transfer layer 34 is the thick n-Bphen layer of 20nm; Hole transmission layer 52 is the thick TPD layer of 50nm; Luminescent layer 53 is the thick green light luminescent material layer of 5nm, and electron transfer layer 54 is the thick Bphen layer of 80nm, and electron injecting layer 38 is the thick Li of 20nm; First reflective conductive layer 41 and second reflective conductive layer 41 ' are the thick Ag layer of 200nm; Insulating barrier 42 is the thick SiO layer of 200nm, and cathode layer 6 is the thick Yb layer of 25nm, and antireflective coating 7 is the thick ZnSe layer of 100nm; Hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35 constitute first organic electroluminescence structure 3; Hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 constitute second organic electroluminescence structure 5; First reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ' constitute reflective articulamentum 4.
Its preparation method is following:
(1) COC is provided substrate, this COC substrate is cut into required shape and area, again this transparent substrates is cleaned by the flow process that liquid detergent cleaning → ethanol cleaning → acetone → pure water cleans; Each cleaning step all cleans with supersonic wave cleaning machine, and preferred employing of each washing cleaned 5 minutes, stopped 5 minutes; Repeat 3 times method respectively; After cleaning finishes,, obtain printing opacity flexible substrate layer 1 with the IR bake oven dry;
(2) vapor deposition Ag layer on a surface of printing opacity flexible substrate layer 1 forms anode layer 2;
(3) adopt the vapor deposition mode to plate hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35, first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ', hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 successively at anode layer 2 with printing opacity flexible substrate layer 1 opposed outer surface;
(4) electron injecting layer 55 with electron transfer layer 54 facing surfaces vapor deposition Yb layers, form cathode layer 6;
(5) cathode layer 6 with electron injecting layer 55 facing surfaces vapor deposition ZnSe layers, form antireflective coating 7;
(6) evaporation encapsulates device after accomplishing, and obtains the flexible double-sided light emitting organic electroluminescence device of present embodiment;
The flexible double-sided light emitting organic electroluminescence apparatus structure of present embodiment is as shown in Figure 3, and this flexibility double-sided light emitting organic electroluminescence device comprises that successively printing opacity flexible substrate layer 1, resilient coating 8, antireflective coating 7, anode layer 2, hole that stack is provided with inject reinforced layer 9, hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35, first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ', hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 and cathode layer 6, another antireflective coating 7 '.Wherein, printing opacity flexible substrate layer 1 is the thick PET of 0.15mm, and resilient coating 8 is the thick photo-curing epoxy resin layer of 0.5 μ m, and antireflective coating 7 and 7 ' is the thick ZnS layer of 45nm, and anode layer 2 is the thick Ag layer of 20nm, and hole injection layer 9 is the thick WO of 6nm
3, hole injection layer 31 is the thick V of 20nm
2O
5, hole transmission layer 32 is the thick m-MTDATA layer of 40nm, hole transmission layer 32 is that the thick α of 20nm-NPD layer, luminescent layer 33 are the thick α-NPD:Ir (MDQ) of 20nm
2(acac) layer, electron transfer layer 34 are the thick Alq of 40nm
3Layer, electron injecting layer 35 are the thick LiF layer of 1nm; First reflective conductive layer 41 is the thick Ag layer of 100nm; Insulating barrier 42 is the thick SiO layer of 200nm, and second reflective conductive layer 41 ' is the thick Ag layer of 60nm, and hole injection layer 51 is the thick m-MTDATA layer of 40nm; Hole transmission layer 52 is the thick α of 20nm-NPD layer, and luminescent layer 53 is the thick TCTA:Ir of 20nm (ppy)
3Layer, electron transfer layer 54 is the thick Alq of 40nm
3Layer, electron injecting layer 55 are that thick LiF layer of 1nm and cathode layer 6 are the thick Ag layer of 18nm; Hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35 constitute first organic electroluminescence structure 3; Hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 constitute second organic electroluminescence structure 5; First reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ' constitute reflective articulamentum 4.
Its preparation method is following:
(1) pet substrate is provided, this pet substrate is cut into required shape and area, again this transparent substrates is cleaned by the flow process that liquid detergent cleaning → ethanol cleaning → acetone → pure water cleans; Each cleaning step all cleans with supersonic wave cleaning machine, and preferred employing of each washing cleaned 5 minutes, stopped 5 minutes; Repeat 3 times method respectively; After cleaning finishes,, obtain printing opacity flexible substrate layer 1 with the IR bake oven dry;
(2) on a surface of printing opacity flexible substrate layer 1, apply the photo-curing epoxy resin layer, form resilient coating 8;
(3) resilient coating 8 with printing opacity flexible substrate layer 1 facing surfaces vapor deposition ZnS layer, form antireflective coating 7;
(4) antireflective coating 7 with resilient coating 8 facing surfaces vapor deposition Ag layers, form anode layer 2;
(5) inject reinforced layer 9 at anode layer 2 with antireflective coating 7 facing surfaces vapor deposition holes;
That (6) injects reinforced layer 9 in the hole adopts the vapor deposition mode to plate hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35, first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ', hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 successively with anode layer 2 opposed outer surface;
(7) electron injecting layer 55 with electron transfer layer 54 facing surfaces vapor deposition cathode layers 6;
(8) at cathode layer 6 and sub-another ZnS layer of implanted layer 55 facing surfaces vapor depositions, form another antireflective coating 7 ';
(9) evaporation encapsulates device after accomplishing, and obtains the flexible double-sided light emitting organic electroluminescence device of present embodiment.
The flexible double-sided light emitting organic electroluminescence apparatus structure of present embodiment is as shown in Figure 3, and this flexibility double-sided light emitting organic electroluminescence device comprises that successively printing opacity flexible substrate layer 1, resilient coating 8, antireflective coating 7, anode layer 2, hole that stack is provided with inject reinforced layer 9, hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35, first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ', hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 and cathode layer 6, another antireflective coating 7 '.Wherein, printing opacity flexible substrate layer 1 is the thick PET of 0.18mm, and resilient coating 8 is the thick photo-curing epoxy resin layers of 10 μ m, and antireflective coating 7 is the thick ZnS layer of 45nm, and anode layer 2 is the thick Ag layer of 20nm, and hole injection layer 9 is the thick WO of 6nm
3Hole injection layer 31 is the thick m-MTDATA layer of 30nm; Hole transmission layer 32 is that the thick NPD layer of 30nm, luminescent layer 33 are the thick LiF layer of 1nm for the thick DPVBi layer of 30nm, electron transfer layer 34 for the thick Bphen layer of 40nm, electron injecting layer 35, and first reflective conductive layer 41 is the thick Ag layer of 120nm, and insulating barrier 42 is the thick SiO layer of 500nm; Second reflective conductive layer 41 ' is the thick Ag layer of 80nm; Hole injection layer 51 is the thick m-MTDATA layer of 40nm, and hole transmission layer 52 is the thick NPB layer of 20nm, and luminescent layer 53 is the thick DCJTB:Alq of 20nm
3Layer, electron transfer layer 54 is the thick Alq of 40nm
3Layer, electron injecting layer 55 be that the thick LiF layer of 1nm and cathode layer 6 is the thick Sm layer of 20nm, antireflective coating 7 ' be the organic anti-reflection film of the thick BCP of 80nm layer by layer; Hole injection layer 31, hole transmission layer 32, luminescent layer 33, electron transfer layer 34, electron injecting layer 35 constitute first organic electroluminescence structure 3; Hole injection layer 51, hole transmission layer 52, luminescent layer 53, electron transfer layer 54, electron injecting layer 55 constitute second organic electroluminescence structure 5; First reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ' constitute reflective articulamentum 4.
The preparation method of the flexible double-sided light emitting organic electroluminescence device of present embodiment is referring to the preparation method of flexible double-sided light emitting organic electroluminescence device among the embodiment 3.
With the flexible double-sided light emitting organic electroluminescence device of the foregoing description 3 and embodiment 4 preparations under the driving voltage of 10V; Following bright dipping (printing opacity flexible substrate layer 1 exiting surface) and last bright dipping (cathode terminal exiting surface) go out light color and brightness compares test, test result is seen shown in the below table 1:
Table 1
Can know by above-mentioned table 1; First organic electroluminescence structure 3, reflective articulamentum 4 and second organic electroluminescence structure 5 that the flexible double-sided light emitting organic electroluminescence device of this inventive embodiments is provided with through stack successively; The light that this reflective articulamentum 4 can be effectively sends first organic electroluminescence structure 3 and second organic electroluminescence structure 5 reflexes to printing opacity flexible substrate layer 1 respectively with cathode layer 6 and penetrate; Realize that two exiting surfaces launch light separately, having strengthened simultaneously should flexibility double-sided light emitting organic electroluminescence device luminous efficiency and intensity.Because first reflective conductive layer 41, insulating barrier 42, second reflective conductive layer 41 ' that reflective articulamentum 4 contains successively that stack is provided with; This two reflective conductive layer can play the reflecting surface effect; The light that first organic electroluminescence structure 3 and second organic electroluminescence structure 5 are sent reflexes to printing opacity flexible substrate layer 1 respectively with cathode layer 6 and penetrate; The light of having avoided first organic electroluminescence structure 3 and second organic electroluminescence structure 5 to send interacts; The glow color of last bright dipping and following bright dipping all is independent emission separately, does not have interactive situation.In addition; Through setting up resilient coating 8, antireflective coating 7 between printing opacity flexible substrate layer 1 and the anode layer 2 and between the anode layer 2 and first organic electroluminescence structure 3, setting up the hole and inject reinforced layer 9; And set up antireflective coating 7 ' at cathode layer 6 outer surfaces; Further strengthened the luminous intensity of the flexible double-sided light emitting organic electroluminescence device of the embodiment of the invention, like the last emitting brightness of the flexible double-sided light emitting organic electroluminescence device of preparation among the embodiment 3 up to 8454cd/m
2, last emitting brightness is up to 8650cd/m
2
The above is merely preferred embodiment of the present invention, not in order to restriction the present invention, all any modifications of within spirit of the present invention and principle, being done, is equal to and replaces and improvement etc., all should be included within protection scope of the present invention.
Claims (10)
1. a flexible double-sided light emitting organic electroluminescence device comprises printing opacity flexible substrate layer, anode layer, first organic electroluminescence structure, reflective articulamentum, second organic electroluminescence structure and cathode layer that stack successively is provided with; Said first organic electroluminescence structure and second organic electroluminescence structure contain luminescent layer respectively; Said reflective articulamentum comprises first reflective conductive layer, insulating barrier, second reflective conductive layer that stack successively is provided with.
2. flexible double-sided light emitting organic electroluminescence device according to claim 1 is characterized in that: first reflective conductive layer of said reflective articulamentum and the material of second reflective conductive layer are at least a among Ag, the Al;
The material of said insulating barrier is SiO.
3. flexible double-sided light emitting organic electroluminescence device according to claim 1 and 2 is characterized in that: first reflective conductive layer of said reflective articulamentum and the thickness of second reflective conductive layer are 60nm～200nm; The thickness of said insulating barrier is 200nm～1000nm.
4. flexible double-sided light emitting organic electroluminescence device according to claim 1 is characterized in that: the material of said printing opacity flexible substrate layer is PETG, polyether sulfone, PEN, clear polyimides, cyclic olefine copolymer or Merlon or polyethylene;
The thickness of said printing opacity flexible substrate layer is 0.1mm～0.5mm.
5. flexible double-sided light emitting organic electroluminescence device according to claim 1; It is characterized in that: also comprise resilient coating and/or antireflective coating that stack successively is provided with between said printing opacity flexible substrate layer and the anode layer; The stacked system of said resilient coating is for being close to the printing opacity flexible substrate layer, and the stacked system of said antireflective coating is for being close to anode layer;
The thickness of said resilient coating is 0.5 μ m～10 μ m; The material of said resilient coating is photo-curing epoxy resin and/or light-cured acrylic resin;
The thickness of said antireflective coating is 40nm～100nm; The material of said antireflective coating be zinc sulphide, zinc selenide, oxine aluminium, bromocresol purple, phenyl beautiful jade, 4,4 ', 4 " at least a in three (N-3-aminomethyl phenyl-N-phenyl-amino)-triphenylamines.
6. according to claim 1 or 5 described flexible double-sided light emitting organic electroluminescence devices, it is characterized in that: also superposeing between the said anode layer and first organic electroluminescence structure is provided with hole injection reinforced layer;
The thickness of said hole injection layer is 3 μ m～10 μ m; The material that reinforced layer is injected in said hole is WO
3, V
2O
5, MoO
3In at least a.
7. flexible double-sided light emitting organic electroluminescence device according to claim 1 is characterized in that: also superposeing with the second organic electroluminescence structure facing surfaces of said cathode layer is provided with antireflective coating.
8. a flexible double-sided light emitting organic electroluminescence device preparation method comprises the steps:
The printing opacity flexible substrate layer is provided;
On said printing opacity flexible substrate layer, plate anode layer;
On said anode layer, plate first organic electroluminescence structure, reflective articulamentum, second organic electroluminescence structure successively, wherein, said first organic electroluminescence structure and second organic electroluminescence structure contain luminescent layer respectively; Said reflective articulamentum comprises first reflective conductive layer, insulating barrier, second reflective conductive layer that stack successively is provided with;
Said second organic electroluminescence structure with reflective articulamentum facing surfaces plating cathode layer, obtain said flexible double-sided light emitting organic electroluminescence device.
9. flexible double-sided light emitting organic electroluminescence device preparation method according to claim 8; It is characterized in that: said printing opacity flexible substrate layer step is provided after; Surface in said printing opacity flexible substrate layer is further plated resilient coating and/or antireflective coating successively, plates anode layer 2 again.
10. according to Claim 8 or 9 described flexible double-sided light emitting organic electroluminescence device preparation methods; It is characterized in that: after said plating anode layer step, before the said plating first organic electroluminescence structure step, further plating the hole with printing opacity flexible substrate layer facing surfaces and inject reinforced layer at said anode layer; Or/and after said plating cathode layer step, further plate antireflective coating with the second organic electroluminescence structure facing surfaces at said cathode layer.
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