CN103746079B - A kind of inversion top radiation organic EL part of single layer structure - Google Patents

A kind of inversion top radiation organic EL part of single layer structure Download PDF

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CN103746079B
CN103746079B CN201410035606.9A CN201410035606A CN103746079B CN 103746079 B CN103746079 B CN 103746079B CN 201410035606 A CN201410035606 A CN 201410035606A CN 103746079 B CN103746079 B CN 103746079B
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organic
iridium
dyestuff
layer structure
single layer
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CN103746079A (en
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陈平
段羽
薛凯文
赵毅
刘式墉
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Jilin University
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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
    • H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
    • H10K50/11—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers
    • H10K50/12—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers comprising dopants
    • H10K50/121—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers comprising dopants for assisting energy transfer, e.g. sensitization
    • 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
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
    • H10K71/10—Deposition of organic active material
    • H10K71/16—Deposition of organic active material using physical vapour deposition [PVD], e.g. vacuum deposition or sputtering
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
    • H10K85/10—Organic polymers or oligomers
    • H10K85/111—Organic polymers or oligomers comprising aromatic, heteroaromatic, or aryl chains, e.g. polyaniline, polyphenylene or polyphenylene vinylene
    • 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
    • H10K2102/301—Details of OLEDs
    • H10K2102/321—Inverted OLED, i.e. having cathode between substrate and anode

Abstract

The inversion top radiation organic EL part of a kind of single layer structure, belongs to organic optoelectronic device technical field.The inversion top radiation organic EL part of structure of the present invention is made up of substrate, negative electrode, monolayer organic function layer, transparent anode successively.Monolayer organic function layer is made up of with the form co-doped of adulterant two kinds of organic dyestuff in single fertile material, wherein fertile material uses the organic material that electron mobility is higher, and two kinds of organic dyestuff Each performs its own functions, a kind of organic dyestuff effect is trapped hole, and another kind of organic dyestuff is for luminescence.The device of structure of the present invention, expands exciton recombination region, is advantageously implemented the balance in the electronics in monolayer organic function layer, hole, has high efficiency, an advantage such as poor efficiency is roll-offed, electroluminescent spectrum-stable.

Description

A kind of inversion top radiation organic EL part of single layer structure
Technical field
The invention belongs to organic optoelectronic device technical field, the inversion top emitting being specifically related to a kind of single layer structure is organic Electroluminescent device.
Background technology
Organic electroluminescence device (OLED) has lot of advantages, such as solid luminescent, energy consumption are little, active illuminating, Visual angle is wide, fast response time, be easily achieved Flexible Displays, low cost etc., shows at colour, the field such as solid-state illumination Having huge using value, a lot of research institutions have all put into substantial amounts of manpower and materials in the world, have promoted OLED The fast development of technology.
OLED can be divided into bottom emitting OLED and top emitting OLED by the taking-up mode of light.Bottom emitting OLED deposits In the contradiction that the drive circuit of display light-emitting area with pixel is vied each other, but according to top emitting OLED, due to light Taking-up end be top, it is possible to obtain higher aperture opening ratio, be advantageously implemented high display brightness, high-resolution have Machine luminescence display.Additionally, for the active organic light emitting display using n-channel TFT, OLED need to take hearth electrode Inverted structure for negative electrode.If therefore wanting utilize the low cost of OLED, high aperture and be easily achieved large-area displays Advantage, to being inverted top emitting OLED, to conduct a research be the most necessary.
The application prospect potential based on being inverted top emitting OLED, a lot of scientific research institutions have carried out this respect in succession in the world Work.1997, the S.R.Forrest seminar of Princeton university [Appl.Phys.Lett.70, (1997) 2954.] report the inversion top emitting OLED using magnesium, silver alloy to be negative electrode, but the performance of this device is relatively Difference, external quantum efficiency is less than 1%.2003, W.Kowalsky of Germany et al. [Appl.Phys.Lett.82, (2003) 284.] using Au (100nm)/Mg (100nm) is end negative electrode, is prepared for based on Alq3Luminous inversion top Launching green glow OLED, the efficiency of device reaches 3.9cd/A.2002, the K.Leo of Dresden, Germany university ground Study carefully group [Appl.Phys.Lett.81, (2002) 922.] and be prepared for inversion top emitting OLED based on p-i-n structure, green Optical device brightness under 4V is up to 100cd/m2.2011, they report again [Appl.Phys.Lett.98, (2011) 083304.] the inversion top emitting OLED of high efficiency yellow phosphor material is used, by whole device is annealed Processing, the carrier in luminous zone reaches balance, and the brightness that the external quantum efficiency of device reaches under 15%, 2.9V reaches To 1000cd/m2。
But owing to preparation order is different with traditional structure OLED of just putting, cause electronics in being inverted OLED Inject, transmission more difficult relative to hole, electronics, the unbalanced phenomenon in hole are more serious, and this is also why to be inverted The reason that the performance of OLED is poor relative to just putting OLED.At present, that reports in the world sends out about being inverted to push up The research penetrating OLED has focused largely on injection and the transmission how improving electronics, such as designs new negative electrode and negative electrode is repaiied The aspects such as decorations layer, employing p-i-n structure.Organic function layer in view of single layer structure OLED typically can only transmit certain Therefore a kind of carrier, if introduce the monolayer organic material conduct that electron mobility is higher in being inverted top emitting OLED Fertile material, not only can simplify the preparation process of device, and by device structure design, introduces one capture sky Organic blended dose of cave, it is possible to solve to be inverted electronics and the unbalanced problem in hole in top emitting OLED, but this The inversion top emission OLED device of structure have not been reported in the world.
Summary of the invention
The present invention is directed to impact and be inverted the key factor of top emitting OLED performance, it is provided that the inversion of a kind of single layer structure Top emission OLED device.
It is different from traditional multilamellar organic function layer being made up of hole transmission layer, luminescent layer, electron transfer layer, this The inversion top emitting OLED organic function layer between negative electrode, anode of bright described structure is single layer structure.This device Part is made up of substrate, negative electrode, monolayer organic function layer, transparent anode successively:
Substrate；Backing material can be the rigid substrate such as glass, silicon, or polyethylene terephthalate, poly- The flexible substrate such as methymethacrylate.
Negative electrode；The composite cathode that negative electrode is constituted by molybdenum/low work function metal.The thickness of molybdenum layer is 10～200nm, The metal of low work function can be the metals such as Al, Ca, Ba, Sm, or is other cathode material, and thickness is 1～100 nm.Also Al can be inserted in the middle of organic function layer with composite cathode2O3、CsF、CaF2、MgF2、NaF、LiF、 Cs2CO3Improve the injection of electronics on cathodic modification layer, the thickness of cathodic modification layer is 0.5～5nm, can be by heat Prepared by the techniques such as evaporation, sputtering.
Anode；Anode can be transparent metal oxide, such as tin indium oxide (ITO), aluminum zinc oxide (AZO) etc., or Metal for high work functions such as Ag, Au, Cu, it is possible to use any anode material, described anode thickness is 15～100 nm.Also can improve the injection in hole at anode and organic functions Intercalation reaction anode modification layer, anode modification layer is permissible Employing 2,3,5,6-tetra-fluoro-7,7 ', 8,8 '-four cyano quinoline diformazan (tetrafluorotetracyanoquinodimethane, F4-TCNQ), FeCl3, or use MoO3、WO3、V2O5Deng oxide, it is possible to use any anode modification Layer and be not limited to this, the thickness of anode modification layer is generally 1～10nm.
The thickness of the monolayer organic function layer between negative electrode and anode is 50～150nm, by organic dyestuff 1, has engine dyeing Material 2 is constituted in single fertile material with the form co-doped of adulterant, and wherein fertile material uses electron mobility Higher organic material, such as 1,3,5-tri-(1-phenyl-1H-benzimidazolyl-2 radicals-yl) benzene (1,3,5-Tris (1-phenyl-1H- Benzimidazol-2-yl)-benzene, TPBi), 2,9-dimethyl-4,7-biphenyl-1,10-phenanthroline (2,9-Dimethyl-4,7-diphenyl-1,10-phenanhroline, BCP), 4,7-diphenyl-1,10-phenanthroline (4,7-diphenyl-1,10-Phenanthroline, Bphen), three (8-hydroxyquinoline) aluminum (Aluminum Tris (8-Hydroxyquinolinate), Alq3) etc., and it is not limited to this.Organic dyestuff 1,2 can use organic glimmering Light luminescent material or Phosphorescent luminescent material, such as two (4,6-difluorophenyl pyridinato-C2, N) pyridinecarboxylic closes iridium (Bis [2-(4,6-difluorophenyl) pyridinato-C2, N] (picolinato) iridium (III), FIrPic), three (2-phenyl Pyridine-C2, N) close iridium (III) (Tris (2-phenylpyridinato-C2, N) iridium (III), Ir (ppy)3), acetopyruvic acid Two (1-phenyl isoquinolin quinoline-C2, N) closes iridium (III) (Bis (1-phenyl-isoquinoline-C2, N) (acetylacetonato) iridium (III), Ir (piq)2(acac)), acetopyruvic acid two (2-phenylbenzothiazol-C2, N) Conjunction iridium (III) (Bis (2-phenyl-benzothiazole-C2, N) (acetylacetonate) iridium (III), Ir(bt)2(acac)), two (4-tolylthiophene also [3,2-c] pyridine-N, C2 ') second phthalein acetone closes iridium (iridium (III) Bis (4-phenylthieno [3,2-c] pyridinato-N, C20) acetylacetonate, PO-01), three (1-phenyl-different Quinoline-C2, N) close iridium (III) (Tris (1-phenylisoquinolinato-C2, N) iridium (III), Ir (piq)3), three [2-is (right Tolyl) pyridine-C2, N) conjunction iridium (III) (Tris [2-(p-tolyl) pyridine-C2, N)] iridium (III), Ir (mppy)3) etc., Any high performance organic dyestuff can be used and be not limited to this.The doping content scope of organic dyestuff is 0.1wt%～40 Wt%, is beneficial to the transmission of carrier and the energy transfer of exciton.
The device of structure of the present invention, the Main Function of organic dyestuff 1 is in order to realize in monolayer organic function layer Electronics, the balance in hole, organic dyestuff 2 mainly utilizes the exciton shifted from fertile material, organic dyestuff 1 multiple Close luminescence.Organic dyestuff of the present invention need to meet following condition: first, the HOMO energy of organic dyestuff 1 Level can need to be injected from anode with direct capture between the HOMO energy level of the work function of anode and fertile material Hole.Secondly, the photoluminescence spectra of organic dyestuff 1 has with the absorption spectrum of organic dyestuff 2 and preferably overlaps.This The specific works principle of the device inventing described structure is as follows: electronics is transmitted by fertile material, and organic dyestuff 1 is permissible Direct capture hole, then with the form transmission jumped on organic dyestuff 1, exciton is mainly at fertile material and organic Being formed on dyestuff 1, the exciton after formation transfers to recombination luminescence on organic dyestuff 2 by energy.
The invention has the beneficial effects as follows: use a kind of new composite cathode, be used in combination the monolayer that electron mobility is bigger The injection of the fertile material of organic function layer, beneficially electronics and transmission.The HOMO energy level of organic dyestuff 1 and sun The work function of pole matches, can be with trapped hole, it is easy to accomplish be inverted the electronics in top emitting OLED, hole number Balance, be conducive to obtaining high efficiency luminescence.Additionally, due to expand the recombination region of exciton, the device of the present invention Part has low efficiency roll-off, it is ensured that the most still keep higher efficiency.
Accompanying drawing explanation
Fig. 1: the structural representation being inverted top radiation organic EL part based on single layer structure of the present invention.
Wherein 1 is substrate, and 2 is negative electrode, 3 is monolayer organic function layer, 4 for transparent anode.
Fig. 2: embodiment 1 prepares the current efficiency-current density plot of device.
Fig. 3: embodiment 2 prepares the luminance-current density curve of device.
Fig. 4: embodiment 2 prepares the current efficiency-brightness curve of device.
Detailed description of the invention
In example, the implication about abbreviation title is as follows:
Mo/Al: molybdenum/aluminum；As negative electrode.
Mo/Mg:Ag: molybdenum/magnesium；Silver, the volume ratio of the doping of Mg:Ag is 10:1, as negative electrode.
Cs2CO3: cesium carbonate；As cathodic modification layer；
TPBi:1,3,5-tri-(1-phenyl-1H-benzimidazolyl-2 radicals-yl) benzene；Fertile material as monolayer organic function layer Or electron transport material, electron transport ability is strong；
FIrPic: two (4,6-difluorophenyl pyridinato-C2, N) pyridinecarboxylic closes iridium；As organic dyestuff 1；
Ir(ppy)3: three (2-phenylpyridine-C2, N) closes iridium；As organic dyestuff 1；
PO-01: two (4-tolylthiophene also [3,2-c] pyridine-N, C2 ') second phthalein acetone closes iridium；As organic dyestuff 2；
TAPC:4,4'-cyclohexyl two [N, N-bis-(4-aminomethyl phenyl) aniline]；As hole transmission layer；
MoO3: molybdenum oxide；As anode modification layer；
Ag: silver；As transparent anode.
Embodiment 1:
The structure being inverted top radiation organic EL part of preparation is:
Device A: silicon substrate/Mo (50nm)/Al (5nm)/Cs2CO3(1nm)/TPBi:10wt%FIrPic:6 wt%PO-01(100nm)/MoO3(10nm)/Ag(20nm)
Device B: silicon substrate/Mo (50nm)/Al (5nm)/Cs2CO3(1nm)/TPBi:6wt%PO-01(100 nm)/MoO3(10nm)/Ag(20nm)
Wherein device A is the structure using present invention design, and device B is only comparative device doped with organic dye 1.
The preparation of device can be carried out by multi-source organic-metal molecules gas-phase deposition system, and detailed process is as follows:
[1] backing material in experiment selects surface to cover the silicon substrate of silicon dioxide insulating layer, first by silicon substrate with third Ketone, ethanol cotton balls are cleaned repeatedly；
[2] silicon substrate of scrub is put in clean beaker successively with acetone, ethanol, deionized water ultrasonic 10 Minute, then put and dry in an oven；
[3] silicon substrate handled well is placed in multi-source organic-metal molecules gas-phase deposition system and (sees China specially Profit: ZL03110977.2, " for the increasing cooking-pot type evaporation source of organic electroluminescent coater "), the vacuum of vapo(u)rization system Cavity comprises organic evaporating area (8 evaporation sources) and evaporation of metal district (3 evaporation sources), between twoth district and each evaporation Mutually completely cut off between source, it is to avoid mutual pollution.Each two evaporation source shares a set of temperature control system, can enter simultaneously 2 kinds of metal materials of row or the evaporation of 4 kinds of organic materials, for ensureing evaporation uniformity, substrate distance evaporation source 25cm, Simultaneously can be with rotation or the uniformity to ensure thin evaporated film that revolves round the sun, the vacuum of system can reach 10-5Pa, thin During film growth, the vacuum of system maintains 3 × 10-4About Pa.The thickness of Material growth and growth rate by American I L-400 type film-thickness monitoring is controlled.The electroluminescent spectrum of device, brightness and current-voltage characteristic The test system synchronization being made up of spectrogrph PR655, galvanometer Keithley-2400 and computer is measured.All of survey Examination is all to complete in atmosphere at room temperature.
Current efficiency-the electric current density being inverted top emitting device of the present invention is as shown in Figure 2.It can be seen that The device A of present invention design compares with comparative device B has higher efficiency.The maximum of device A and B differs only in In device A, introduce the FIrPic of 10wt%.The maximum current efficiency of device A up to 32.4cd/A, device B's Maximum current efficiency is only 20.3cd/A.At 1000cd/m2Brightness under, the current efficiency of device A is 31.8 Cd/A, and device B is only 20.2cd/A.
Embodiment 2:
The structure of the inversion top radiation organic EL part C of preparation is: silicon substrate/Mo (50nm)/Mg:Ag (5 nm)/Cs2CO3(1nm)/TPBi:10wt%Ir(ppy)3:6wt%PO-01(100nm)/MoO3(10nm)/Ag (20nm).Wherein the volume ratio of Mg:Ag doping is 10:1, detailed process prepared by device such as embodiment 1.
The luminance-current density being inverted top emitting device of the present invention is as shown in Figure 3.It can be seen that this The high-high brightness of the device C of bright design is up to 57384cd/m2.The maximum current efficiency of device C is up to 30.1cd/A. As shown in Figure 4, device C is at 1000cd/m for the current efficiency-brightness curve of device C2Brightness under current efficiency be 26.3cd/A。
Although describing the present invention in conjunction with example, but the invention is not limited in examples detailed above and accompanying drawing, for For the research worker of the art, it is also possible to modify the present invention, these improvement fall within right of the present invention In the protection domain required.

Claims (6)

1. the inversion top radiation organic EL part of a single layer structure, it is characterised in that: it is made up of substrate, negative electrode, monolayer organic function layer, transparent anode successively；
Wherein:
The composite cathode that-negative electrode is constituted by molybdenum/low work function metal；
-monolayer organic function layer is made up of with the form co-doped of adulterant organic dyestuff 1 and organic dyestuff 2 in single fertile material, and the doping content of organic dyestuff 1 is 10wt%, and the doping content of organic dyestuff 2 is 6wt%；
-single fertile material uses the organic material that electron mobility is higher；
The HOMO energy level of-organic dyestuff 1 is between the work function and the HOMO energy level of fertile material of anode material, organic dyestuff 1 is different with the material of organic dyestuff 2 and is respectively selected from two (4, 6-difluorophenyl pyridinato-C2, N) pyridinecarboxylic closes iridium, three (2-phenylpyridine-C2, N) iridium is closed, acetopyruvic acid two (1-phenyl isoquinolin quinoline-C2, N) iridium (III) is closed, acetopyruvic acid two (2-phenylbenzothiazol-C2, N) iridium (III) is closed, two (4-tolylthiophene also [3, 2-c] pyridine-N, C2 ') second phthalein acetone closes iridium or three (1-phenyl-isoquinolin-C2, N) iridium is closed.
The inversion top radiation organic EL part of a kind of single layer structure the most as claimed in claim 1, it is characterised in that: the thickness of monolayer organic function layer is 50～150nm.
The inversion top radiation organic EL part of a kind of single layer structure the most as claimed in claim 1, it is characterized in that: fertile material is 1,3,5-tri-(1-phenyl-1H-benzimidazolyl-2 radicals-yl) benzene, 2,9-dimethyl-4,7-biphenyl-1,10-phenanthroline, 4,7-diphenyl-1,10-phenanthroline or three (8-hydroxyquinoline) aluminum.
The inversion top radiation organic EL part of a kind of single layer structure the most as claimed in claim 1, it is characterised in that: substrate is glass, silicon, polyethylene terephthalate or polymethyl methacrylate.
The inversion top radiation organic EL part of a kind of single layer structure the most as claimed in claim 1, it is characterised in that: in composite cathode, low workfunction metal is Al, Ca, Ba or Sm；The thickness of molybdenum layer is 10～200nm, and the thickness of low work function metal is 1～100nm.
The inversion top radiation organic EL part of a kind of single layer structure the most as claimed in claim 1, it is characterised in that: anode is ITO, AZO, Ag, Au or Cu, and thickness is 15～100nm.
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