CN102709482A - Phosphorescence and fluorescence combined white organic light emitting device - Google Patents
Phosphorescence and fluorescence combined white organic light emitting device Download PDFInfo
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Abstract
The invention belongs to the technical field of organic light emitting, and particularly relates to a phosphorescence and fluorescence combined white organic light emitting device which comprises a transparent substrate, an anode, an organic hole-injection layer, an organic hole-transmission layer, an organic light emitting layer, an electronic transmission layer and a metal cathode, wherein the organic light emitting layer has a structure with a plurality of light emitting layers and is provided with a fluorescence blue light emitting layer and a phosphorescence blue light emitting layer at the same time. The fluorescence blue light emitting layer and the phosphorescence blue light emitting layer are introduced into the same white device at the same time, so that the phosphorescence and fluorescence combined white organic light emitting device with high efficiency, good color purity and high color rendering index is obtained, and has the efficiency index which already exceeds the level of the traditional incandescent lamp.
Description
Technical field
The invention belongs to technical field of organic electroluminescence, be specifically related to a kind of phosphorescence fluorescence mating type white light organic electroluminescent device.
Background technology
In recent years along with the high speed development of Organic Light Emitting Diode (OLEDs), because it has caused attention highly in the potential whole world that is applied in aspect flat panel display and the illumination.White light has light-emitting diode (WOLED) then to play crucial effects in above field.In order to realize white light, no matter be to adopt three primary colors method or color conversion media technology, blue light all is indispensable factor.Therefore, the research to blue-light device just has more important meaning.No matter be fluorescent material or phosphor material, with respect to the material of other colors, the least ideal that also develops the latest that blue light material not only develops.Because the advantage of phosphor material on efficient enjoys researcher's favor in recent years.But fluorescent material has the incomparable advantage of phosphor material, also receives great concern.
The internal quantum efficiency of phosphorescent OLED device can reach 100% in theory, and fluorescent device can only reach 25%.So the efficient of phosphorescent OLED device can be far above fluorescent device, and the colorimetric purity of fluorescence OLED device is better than phosphorescent OLED device.Because phosphorescence device and fluorescent device have pluses and minuses separately, researchers just introduce fluorescent material and phosphor material in the device simultaneously: the people such as Forrest of Princeton university in 2006 (Y.Sun, N.C.Giebink; H.Kanno; B.Ma, M.E Thompson, S.R.Forrest; Nature 440 (2006) 908) made the device of phosphorescence mating type, blue light-emitting is that fluorescent material, ruddiness and green light material are phosphor material in the device.External quantum efficiency that the white light parts of their made is the highest and power efficiency are respectively 18.6% and 37.6lmW
-1People (J.H.Seo, J.H.Park, Y.K.Kim such as the great beneficial Young Kwan Kim of university of Korea S in 2007; J.H.Kim; G.W.Hyung, K.H.Lee, S.S.Yoon; Appl.Phys.Lett.90 (2007) 203507) utilize fluorescence blue light, green light material and phosphorescence red light material to make white light parts, brightness is up to 30500cd/m
2, efficient is up to 38cd/A; The same year, the people such as Leo of Dresden, Germany university (G.Schwartz, M.Pfeiffer; S.Reineke; K.Walzer, K.Leo, Adv.Mater.19 (2007) 3672) utilize fluorescent blue luminescent material and phosphorescence orange light, green light material to produce white light parts; Through introducing outer coupling paper tinsel, the efficient of device reaches 37.5lm/W, 16.1%1000cd/m
2The Wai-Yeung Wong of meeting university and the people (C.-L.Ho such as Dongge Ma of Changchun applied chemistry research institute were invaded in Hong Kong in 2008; W.-Y.Wong, Q.Wang, D.G.Ma; L.X.Wang; Z.Y.Lin, Adv.Funct.Mater.18 (2008) 928) utilize fluorescent blue luminescent material and phosphorescence orange luminescent material to make two luminescent layer white light parts, efficient has reached 26.6cd/A and 13.5lm/W.
Summary of the invention
The phosphorescence fluorescence mating type white light organic electroluminescence luminescent device that the purpose of this invention is to provide a kind of high efficiency, high color purity, high color rendering index (CRI).
The structure of two blue light-emittings of the blue light-emitting of blue light-emitting and the phosphorescence of the present invention through introducing fluorescence is come the exciton recombination zone of trim; Realize low unlatching, high efficiency, the phosphorescence mating type white light organic electroluminescent device that color rendering is good through the design device architecture.
As first kind of execution mode of the present invention; Phosphorescence fluorescence mating type white light organic electroluminescent device is made up of transparent substrates, anode, organic hole implanted layer, organic cavity transmission layer, organic luminous layer, electron transfer layer and metallic cathode successively; It is characterized in that: organic luminous layer is multi-luminescent layer structure and the blue light-emitting that has fluorescence and phosphorescence simultaneously; According to from anode layer order from the near to the remote, be followed successively by fluorescence blue light-emitting, be used to stop insertion layer that energy shifts, phosphorescence the Yellow light emitting layer, be used to stop the insertion layer that energy shifts and the blue light-emitting of phosphorescence.
As another embodiment of the invention; Itself and above-mentioned first kind execution mode difference are mainly reflected on the organic luminous layer structure; This execution mode is that organic luminous layer is the multi-luminescent layer structure and has fluorescence simultaneously and the phosphorescence blue light-emitting equally; According to from anode layer order from the near to the remote, be followed successively by fluorescence blue light-emitting, be used to stop insertion layer that energy shifts, phosphorescence the green luminescence layer, be used to stop insertion layer that energy shifts, phosphorescence red light luminescent layer, be used to stop the insertion layer that energy shifts and the blue light-emitting of phosphorescence.
The blue light emitting layer material of the fluorescence of white light organic electroluminescent device of the present invention is optional with 1-(2,5-dimethoxy-4 '-(1-pyrene) phenyl) pyrene (DOPPP), 2-diphenyl-7-(2, the 2-diphenylethyllene)-9; 9'-spiral shell two fluorenes (DPV), N, N '-two-(1-phenyl)-N; N '-diphenyl-1,1 '-xenyl-4,4 '-diamines (NPB) or 4; 4-two-(2,2 '-diphenylacetylene) biphenyl (DPVBi), its thickness is 5-15nm; The thickness optimum turns to 8nm, and the blue light-emitting of fluorescence also can be used as electronic barrier layer simultaneously.
The blue light-emitting of the phosphorescence of white light organic electroluminescent device of the present invention is single doped structure, and fertile material can select 2 for use, 7-two (diphenyl phosphinylidyne)-9-(4-diphenylamine) phenyl-9'-phenyl fluorenes (POAPF), 4; Two (the 9-carbazyls)-2 of 4'-, 2'-dimethyl (CDBP), 2-(diphenyl phosphine oxide)-9,9'-spiral shell two fluorenes (SPPO1), 9; 9'-(5-(triphen is silica-based)-1; 3-benzene) two (9H-clicks) (SimCP), 1, two (9-carbazyl) benzene (mCP) or 4 of 3-, 4'; 4 " three (9-carbazyl) triphenylamines (TCTA), the present invention is preferably POAPF; The blue light phosphorescent coloring that mixes is two (3; 5-two fluoro-2-(2-pyridine) phenyl-(2-pyridine carboxylic acid root)) close iridium (Firpic), two (2,4-two fluorobenzene pyridines) four (1-pyrazoles) boric acid and close iridium (Fir6), the present invention is preferably Firpic; Doping content is 8-15wt%; Preferred concentration of the present invention is 10wt%, and the blue light emitting layer thickness of phosphorescence is 10-30nm, and it is 12nm that the present invention optimizes thickness.
The doping of the blue light-emitting of phosphorescence adopts the technology of two source vapor depositions to mix (specifically referring to Chinese patent: CN1187470C among the present invention; " the crucible type evaporation source that is used for the organic electroluminescent coating machine "), the doping process is that fertile material and blue light phosphorescent coloring are carried out vapor deposition simultaneously.The vapor deposition speed of blue light phosphorescent coloring Firpic is 0.01 ~ 0.02nm/s among the present invention, and the vapor deposition speed of fertile material POAPF is 0.09 ~ 0.18nm/s.Film thickness and vapor deposition speed are monitored by the SI-TM216B quartz crystal film thickness monitor of Shenyang Sai Ensi in real time in the evaporate process.
The gold-tinted of phosphorescence, green glow, red light luminescent layer are the superthin layer structure in the white light organic electroluminescent device of the present invention, and (4-phenyl thieno [3,2-c] pyridine-N, C2') acetyl acetone iridium (PO-01), three (2-phenylpyridine) closes iridium [Ir (ppy) to be respectively two
3], two-(2-phenylchinoline-N, C2') two pivaloyl group methane close iridium [(PQ)
2Ir], its thickness is 0.05-0.1nm.
The anode material of white light organic electroluminescent device of the present invention can be selected inorganic material for use, is generally the metal with higher work-functions of metal oxide such as ITO, zinc oxide, zinc tin oxide or gold, copper, silver, optimization selection ITO; Hole injection layer adopts the stronger organic semiconducting materials of cavity transmission ability, the optional MoO of material
3Doping N, N '-two-(1-phenyl)-N, N '-diphenyl-1,1 '-xenyl-4,4 '-diamines (NPB) (NPB:MoO
3, doping ratio is 10wt%-50wt%), 4,4 '; 4 "-three (3-aminomethyl phenyl aniline) triphenylamine (m-MTDATA), CuPc (CuPc), 4,4', 4 " three (2 naphthyl phenylamino) triphenylamine (2T-NATA), 4; 4', 4 " three (1 naphthyl phenylamino) triphenylamine (1T-NATA) or 4,4'; 4 " three (benzidino) triphenylamine (NATA), the present invention is preferably NPB:MoO
3Hole transmission layer can be selected NPB, N for use, N '-diphenyl-N, and N '-two (a first class phenyl)-1,1 ,-xenyl-4,4 '-diamines (TPD) or m-MTDATA, the present invention is preferably NPB; Electron transfer layer can adopt metal organic complex, and material is optional 1,3-two [3,5-(pyridin-3-yl) phenyl] benzene (BmPyPB), three (oxine) aluminium (Alq
3), two (2-methyl-8 quinolyl)-4-phenylphenol aluminium (BAlq), 4,7-diphenyl-1,10-o-phenanthroline (Bphen), 1; 3,5-three (2-N-benzene-benzimidazole) benzene (TPBi) or 2,9-dimethyl-4; 7-diphenyl-1,10-joins phenanthroline (BCP), and the present invention is preferably BmPyPB; Cathode material can adopt the alloy of the lower metal of work functions such as lithium that LiF modifies, magnesium, calcium, strontium, aluminium or they and gold, copper, silver etc., and the present invention is preferably LiF/Mg:Ag, and the ratio of Ag is 10-20% (volume ratio) among the Mg:Ag.
Insertion layer in the white light organic electroluminescent device of the present invention between two luminescent layers can be used for stopping that non-radiative energy shifts between the luminescent layer; Material optional 2; 7-two (diphenyl phosphinylidyne)-9-(4-diphenylamine) phenyl-9'-phenyl fluorenes (POAPF) or 4,4 '-N, N-two carbazoles-biphenyl (CBP); The present invention is preferably POAPF, and its thickness is 1-5nm.
The present invention obtains the phosphorescence fluorescence mating type white light organic electroluminescence luminescent device of high efficiency, high color purity, high color rendering index (CRI) through the blue light-emitting of fluorescence and phosphorescence is introduced same white light parts simultaneously.
Set forth content of the present invention in detail below in conjunction with accompanying drawing and practical implementation method, should be appreciated that the present invention is not limited to following preferred implementation, this execution mode is only as illustrative embodiment of the present invention.
Description of drawings
Fig. 1: (a) structural representation of phosphorescence fluorescence mating type white light organic electroluminescence luminescent device;
(b) the device luminous layer structure sketch map of embodiment 1 preparation;
(c) the device luminous layer structure sketch map of embodiment 2 preparations;
Fig. 2: (a) electroluminescent spectrum of embodiment 1 fabricate devices;
(b) electroluminescent spectrum of embodiment 2 fabricate devices;
Current density-voltage, the brightness-voltage curve of Fig. 3: embodiment 1,2 fabricate devices;
Current efficiency-voltage, the power efficiency-voltage curve of Fig. 4: embodiment 1,2 fabricate devices;
Be depicted as the organic electroluminescent white light device structure that the present invention proposes like Fig. 1 (a), wherein 1 is transparent substrates (like glass); 2 is the ito anode layer; 3 is hole injection layer, selects NPB:10wt%MoO for use
34 is hole transmission layer, selects NPB for use; 5 is organic luminous layer; 6 is electron transfer layer, selects BmPyPB for use; 7 is negative electrode, selects LiF/Mg:Ag for use.
Like Fig. 1 (b), each layer is respectively: the blue light-emitting of fluorescence (51), be used to stop insertion layer (52) that energy shifts, phosphorescence Yellow light emitting layer (53), be used to stop the insertion layer (52) that energy shifts and the blue light-emitting (55) of phosphorescence.
Like Fig. 1 (c), each layer is respectively: the blue light-emitting of fluorescence (51), be used to stop insertion layer (52) that energy shifts, phosphorescence green luminescence layer (55), be used to stop insertion layer (52) that energy shifts, phosphorescence red light luminescent layer (56), be used to stop the insertion layer (52) that energy shifts and the blue light-emitting (54) of phosphorescence.
As shown in Figure 3; The curve that filled squares and solid circles were linked to be among this figure is represented current density-voltage curve of embodiment 1 and embodiment 2 respectively, and the individual curve that is linked to be with open circles of open squares is represented brightness-voltage curve of embodiment 1 and embodiment 2 respectively.
As shown in Figure 4; The curve that filled squares and solid circles were linked to be among this figure is represented current efficiency-voltage curve of embodiment 1 and embodiment 2 respectively, and open squares and the hollow round curve that is linked to be are represented power efficiency-voltage curve of embodiment 1 and embodiment 2 respectively.
Embodiment
Because the variation of embodiment of the present invention mainly concentrates on the luminescent layer of white organic light emitting diode, turn round and look at the luminous layer structure of two kinds of embodiment of the present invention is listed in the accompanying drawing 1 simultaneously, wherein the luminous layer structure of embodiment 1,2 is following:
DOPPP(8nm)/POAPF(3nm)/PO-01(0.05nm)/POAPF(1nm)/POAPF:Firpic(12nm)；
DOPPP(8nm)/POAPF(2nm)/Ir(ppy)
3(0.05nm)/POAPF(1nm)/(PQ)
2Ir(0.05nm)/POAPF(1nm)/POAPF:Firpic(12nm)。
Embodiment 1:
(1) to the transparent conduction base sheet ito glass, carry out decon90 (enlightening health 90) cleaning fluid and washed with de-ionized water successively, used the deionized water ultrasonic cleaning again 15 minutes, the oven dry back is carried out uv ozone to it and is handled;
(2) the ito glass substrate of handling well is placed multi-source organic molecule gas-phase deposition system, comprise organic evaporating area (10 source) and evaporation of metal district (2 source) in the same vacuum cavity of system, completely cut off each other between two districts and between each evaporation source; Avoided mutual pollution; Need not destroy system vacuum, substrate can rotate to organic evaporating district or top, evaporation of metal district respectively, makes things convenient for the growth of material; Can rotation with revolution to guarantee the uniformity of metal film and organic membrane; Material therefor is placed on respectively in the different evaporation sources of different evaporating area, the temperature of each evaporation source can be controlled separately, is evacuated to 5 * 10 then
-4Pa;
(3) with mask plate furnishing organic mask plate, the NPB:10wt%MoO of vapor deposition 15nm successively on ito anode
3With the NPB of 25nm, they respectively in device as hole injection layer and hole transmission layer, its vapor deposition speed is 0.1 ~ 0.3nm/s;
(4) keep above-mentioned vacuum chamber internal pressure constant, continue the blue light-emitting of the DOPPP of vapor deposition 8nm as fluorescence, vapor deposition speed is 0.1 ~ 0.2nm/s; The POAPF of vapor deposition 3nm is as inserting layer again, and vapor deposition speed is 0.05 ~ 0.1nm/s, and the PO-01 superthin layer of vapor deposition 0.05nm is as phosphorescence Yellow light emitting layer again, and vapor deposition speed is 0.002nm/s; The POAPF of vapor deposition 1nm is as inserting layer again, and vapor deposition speed is 0.05 ~ 0.1nm/s; The doping content of last vapor deposition 12nm, Firpic is the blue light-emitting of the POAPF layer of 10wt% as phosphorescence;
(5) keep above-mentioned vacuum chamber internal pressure constant, the BmPyPB of vapor deposition 36nm is as electron transfer layer on above-mentioned luminescent layer, and its vapor deposition speed is 0.2 ~ 0.3nm/s;
(6) keep above-mentioned vacuum chamber internal pressure constant, the LiF of vapor deposition 0.5nm is as the cathodic modification layer on above-mentioned electron transfer layer, and its vapor deposition speed is 0.01nm/s;
(7) keep above-mentioned vacuum chamber internal pressure constant, change the organic mask plate into metal mask plate, the Mg:Ag alloy of vapor deposition 150nm is as the negative electrode of metal, and the vapor deposition speed ratio is 15:1, makes device 1.
Embodiment 2:
(1) with embodiment 1;
(2) with embodiment 1;
(3) with embodiment 1;
(4) keep above-mentioned vacuum chamber internal pressure constant, at first the DOPPP of vapor deposition 8nm is as the blue light-emitting of fluorescence, and vapor deposition speed is 0.1 ~ 0.2nm/s; The POAPF of vapor deposition 2nm is as inserting layer again, and vapor deposition speed is 0.05 ~ 0.1nm/s, and the Ir of vapor deposition 0.05nm (ppy) 3 superthin layers are as the green luminescence layer of phosphorescence again, and vapor deposition speed is 0.002nm/s; The POAPF of vapor deposition 1nm is as inserting layer again, and vapor deposition speed is 0.05 ~ 0.1nm/s; (PQ) of vapor deposition 0.05nm again
2The Ir superthin layer is as the phosphorescence red light luminescent layer, and vapor deposition speed is 0.002nm/s; The POAPF of vapor deposition 1nm is as inserting layer again, and vapor deposition speed is 0.05 ~ 0.1nm/s; The doping content of last vapor deposition 12nm, Firpic is the blue light-emitting of the POAPF layer of 10wt% as phosphorescence;
(5) keep above-mentioned vacuum chamber internal pressure constant, the BmPyPhB of vapor deposition 35nm is as electron transfer layer on above-mentioned luminescent layer, and its vapor deposition speed is 0.2 ~ 0.3nm/s;
(6) with embodiment 1;
(7), make device 2 with embodiment 1.
The prepared device performance of the present invention is with the test under the normal temperature condition in air of Minolta LS-110 luminance meter, Ocean Optics Maya 2000-PRO spectrometer and Keithley 2400 current/voltage sources.
The prepared electroluminescent spectrum of device under the 4.5V driving voltage of embodiment 1,2 is as shown in Figure 2, and current density-voltage, the brightness-voltage curve of device are as shown in Figure 3, and current efficiency-voltage, the power efficiency-voltage curve of device are as shown in Figure 4.
Can find out by Fig. 2; The spectrum of the device 1 of embodiment 1 preparation comprises Firpic (470nm), and (~ blue emission 440nm) and the Yellow light emitting of PO-01 (560nm), the spectrum of the device 2 that embodiment 2 prepares comprises Firpic (470nm) and DOPPP (~ blue emission 440nm), Ir (ppy) with DOPPP
3Green emission (510nm) and (PQ)
2The red emission of Ir (610nm).Under the 4.5V driving voltage, the white color coordinate of being launched of device 1 and device 2 is respectively (0.357,0.410) and (0.465,0.383).
Can find out that by Fig. 3 and 4 high-high brightness of device 1, maximum current efficient and maximum power efficiency are respectively 15000cd/m
2, 40.3cd/A, 50.6lm/W; The high-high brightness of device 2, maximum current efficient and maximum power efficiency are respectively 25430cd/m
2, 17.4cd/A, 21.2lm/W.The color rendering index of device 1, device 2 is respectively 66 and 78.The white light parts that has the blue light-emitting of fluorescence and phosphorescence when can find out in this invention by above data has good device performance, and its efficiency index has surpassed the level of conventional incandescent.
The above is merely preferred embodiment of the present invention, can not limit the scope that the present invention implements with it, and the equalization of carrying out according to patent claim of the present invention generally changes and improves, and all should still belong to the scope that patent of the present invention contains.
Claims (6)
1. phosphorescence fluorescence mating type white light organic electroluminescent device; Form by transparent substrates (1), anode (2), organic hole implanted layer (3), organic cavity transmission layer (4), organic luminous layer (5), electron transfer layer (6) and metallic cathode (7) successively; It is characterized in that: organic luminous layer (5) is multi-luminescent layer structure and the blue light-emitting that has fluorescence and phosphorescence simultaneously; According to from anode (2) order from the near to the remote, be followed successively by fluorescence blue light-emitting, be used to stop insertion layer that energy shifts, phosphorescence the Yellow light emitting layer, be used to stop the insertion layer that energy shifts and the blue light-emitting of phosphorescence.
2. phosphorescence fluorescence mating type white light organic electroluminescent device; Form by transparent substrates (1), anode (2), organic hole implanted layer (3), organic cavity transmission layer (4), organic luminous layer (5), electron transfer layer (6) and metallic cathode (7) successively; It is characterized in that: organic luminous layer (5) is for the multi-luminescent layer structure and have fluorescence simultaneously and the phosphorescence blue light-emitting; According to from anode (2) order from the near to the remote, be followed successively by fluorescence blue light-emitting, be used to stop insertion layer that energy shifts, phosphorescence the green luminescence layer, be used to stop insertion layer that energy shifts, phosphorescence red light luminescent layer, be used to stop the insertion layer that energy shifts and the blue light-emitting of phosphorescence.
3. according to claim 1 or claim 2 a kind of phosphorescence fluorescence mating type white light organic electroluminescent device, it is characterized in that: the material of the blue light-emitting of fluorescence is 1-(2,5-dimethoxy-4 '-(1-pyrene) phenyl) pyrene, 2-diphenyl-7-(2; The 2-diphenylethyllene)-9,9'-spiral shell two fluorenes, N, N '-two-(1-phenyl)-N; N '-diphenyl-1,1 '-xenyl-4,4 '-diamines or 4; 4-two-(2,2 '-diphenylacetylene) biphenyl, its thickness is 5-15nm.
4. according to claim 1 or claim 2 a kind of phosphorescence fluorescence mating type white light organic electroluminescent device, it is characterized in that: the blue light-emitting of phosphorescence is single doped structure, fertile material is 2; 7-two (diphenyl phosphinylidyne)-9-(4-diphenylamine) phenyl-9'-phenyl fluorenes, 4, two (the 9-carbazyls)-2 of 4'-, 2'-dimethyl, 2-(diphenyl phosphine oxide)-9; 9'-spiral shell two fluorenes, 9,9'-(5-(triphen is silica-based)-1,3-benzene) two (9H-clicks), 1; Two (9-carbazyl) benzene or 4 of 3-, 4', 4 " three (9-carbazyl) triphenylamine; the blue light phosphorescent coloring of doping is that two (3; 5-two fluoro-2-(2-pyridine) phenyl-(2-pyridine carboxylic acid root)) are closed iridium or two (2,4-two fluorobenzene pyridines) four (1-pyrazoles) boric acid and closed iridium, and doping content is 8-15wt%.
5. according to claim 1 or claim 2 a kind of phosphorescence fluorescence mating type white light organic electroluminescent device; It is characterized in that: the red light luminescent layer of the Yellow light emitting layer of phosphorescence, the green luminescence layer of phosphorescence, phosphorescence is the superthin layer structure; Be respectively two (4-phenyl thieno [3,2-c] pyridine-N, C2') acetyl acetone iridium, three (2-phenylpyridine) closes iridium and two-(2-phenylchinoline-N; C2') two pivaloyl group methane close iridium, and its thickness is 0.05-0.1nm.
6. according to claim 1 or claim 2 a kind of phosphorescence fluorescence mating type white light organic electroluminescent device; It is characterized in that: be used to stop that the insertion layer that non-radiative energy shifts is 2; 7-two (diphenyl phosphinylidyne)-9-(4-diphenylamine) phenyl-9'-phenyl fluorenes or 4; 4 '-N, N-two carbazoles-biphenyl, thickness are 1-5nm.
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