CN109830612A - Organic electroluminescence device - Google Patents
Organic electroluminescence device Download PDFInfo
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- CN109830612A CN109830612A CN201910094910.3A CN201910094910A CN109830612A CN 109830612 A CN109830612 A CN 109830612A CN 201910094910 A CN201910094910 A CN 201910094910A CN 109830612 A CN109830612 A CN 109830612A
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Abstract
The present embodiments relate to organic electroluminescence device fields, disclose a kind of organic electroluminescence device, including substrate and the anode being successively set on substrate, electron injecting layer, electron transfer layer, luminescent layer, hole transmission layer, hole injection layer and cathode, the luminescent layer includes at least one by phosphor bodies and to be set to each pair of described for phosphor bodies and described at least one wall by between phosphor bodies and doped with fluorescent emitter for phosphor bodies and at least one described being arranged in pairs for phosphor bodies.The advantages of organic electroluminescence device provided by embodiment of the present invention has while being easy to industrialization manufacture, improving luminous efficiency.
Description
Technical field
The present embodiments relate to organic electroluminescence device field, in particular to a kind of organic electroluminescence device.
Background technique
Currently, in the prior art, organic electroluminescence device (OLED) is considered as flat panel display of new generation, have light
It is thin, inexpensive, can Flexible Displays the advantages that, gradually Stepping into daily life.The luminescent material that traditional OLED is used mainly has
Fluorescent material and two kinds of phosphor material.Under the conditions of electrically excited, Organic Light Emitting Diode can generate 25% singlet exciton
With 75% triplet excitons.Traditional fluorescent material can only utilize 25% singlet exciton due to spin forbidden,
Almost all of triplet excitons can only be lost by way of heat, and luminous efficiency is lower.Phosphor material is due to introducing weight
Atom, there are spin-orbit cou-pling effects, therefore can make full use of 75% triplet excitons, to realize 100% interior quantum
Efficiency, luminous efficiency are higher.Since phosphor material has used rare heavy metal, such as iridium, lead, so that material expensive, product
Higher cost, and heavy metal is very big to the pollution of environment.Therefore, to realize efficient electroluminescent fluorescent, it is necessary to solve
The recycling problem of a large amount of triplet excitons.
The method commonly used in the prior art for recycling triplet excitons mainly has following a few classes: the first kind is to utilize three lines
State-triplet state buries in oblivion (Triplet-TripletAnnihilation, TTA) process and generates singlet exciton, but this process is still
So having the 37.5% raw exciton of electricity cannot be utilized；Second class is to construct reversed intersystem crossing using the charge transfer state that weak beam is tied up
(RISC) the thermotropic delayed fluorescence (Thermally-ActivatedDelayedFluorescence, TADF) in channel, Ke Yishi
Now complete singlet exciton utilizes；Third class is hydridization local-electric charge transfer (HybridLocally-
ExcitedandCharge-Transfer, HLCT) excitation state and " hot CT exciton " material, it theoretically also may be implemented completely
Triplet excitons utilize；4th class is that some spin statistics rules of avoiding being recently proposed directly utilize the raw two-wire state of electricity
(Doublet) luminous special system can also theoretically realize that the raw triplet excitons of complete electricity utilize.
It wherein, is current most effective solution using thermotropic delayed fluorescence.It is identical due to spinning according to Hund rule
Two electronics between repulsive force be less than the repulsive forces of opposite two electronics, therefore triplet state T1Always than singlet S1 energy
Grade is low, there is energy gap Δ E between the twoST.But triplet excitons can by the reversed intersystem crossing of endothermic process of molecule, to
Singlet exciton conversion, T1And S1Energy it is closer, i.e. Δ ESTIt is smaller, more process is altered between this inverse system more is easy to happen.
Due to triplet state T1To there are forbidden transition, the triplet state not radiated in thermotropic delayed fluorescence material molecule can lead between ground state
It crosses reversed intersystem crossing and translates into singlet exciton, to significantly improve fluorescence radiation efficiency by delayed fluorescence.In addition,
Low in cost, the advantages of quantum efficiency is theoretically limited to 100% of heat lag fluorescent material.Therefore, how to apply on a large scale
Heat lag fluorescent material becomes one and main studies a question.
However, it was found by the inventors of the present invention that up to the present, most of heat lag fluorescent material both is from small molecule
Material, in order to guarantee the luminous efficiency of heat lag fluorescence, need to adulterate to be formed be spatially separating to phosphor bodies (D) and by phosphor bodies
(A) part, since doping concentration is difficult to obtain optimal repeatability, this brings extreme difficulty to industrialization manufacture.
Summary of the invention
Embodiment of the present invention is designed to provide a kind of organic electroluminescence device, can be easy to industrialization manufacture
While, effectively promote the luminous efficiency of organic electroluminescence device.
In order to solve the above technical problems, embodiments of the present invention provide a kind of organic electroluminescence device, including base
Plate and the anode being successively set on substrate, hole injection layer, hole transmission layer, luminescent layer, electron transfer layer, electron injection
Layer and cathode, the luminescent layer include at least one for phosphor bodies and described at least one receptor being arranged in pairs for phosphor bodies
It main body and is set to each pair of described for phosphor bodies and at least one described by between phosphor bodies and doped with fluorescent emitter
Wall.
Embodiment of the present invention in terms of existing technologies, for phosphor bodies and by being inserted into wall among phosphor bodies,
So that electrons and holes space delocalization, while by the thickness of control wall, regulate and control the HOMO highest occupied molecular orbital energy for phosphor bodies
Grade and by phosphor bodies the minimum orbital energy level that accounted in the overlapping degree of energy level rail flanges, realize lesser Δ EST, so that three
Line state exciton is converted more easily by reversed intersystem crossing to singlet exciton, and then is sent out using the fluorescence adulterated in wall
Beam, the efficiency that organic electroluminescence device is promoted by delayed fluorescence；Further, since in donor in embodiment of the present invention
Main body and by added between phosphor bodies the way of wall without control for phosphor bodies with by the doping ratio of phosphor bodies, Neng Gouchong
It is multiple to realize, it is easy to industrially manufacture.
In addition, described for phosphor bodies and described by being capable of forming exciplex, the exciplex between phosphor bodies
Triplet lower than described for phosphor bodies and the triplet by phosphor bodies.
In addition, the energy gap between the triplet of the exciplex and the triplet for phosphor bodies is big
In or be equal to 0.4eV, energy gap between the triplet of the exciplex and the triplet by phosphor bodies
More than or equal to 0.4eV.
In addition, the absolute value of the HOMO highest occupied molecular orbital energy level for phosphor bodies is less than or equal to 5.5eV, the receptor master
The absolute value of the lowest unoccupied molecular orbital energy level of body is greater than or equal to 2.5eV.
In addition, the wall and the triplet state energy gap for phosphor bodies are greater than or equal to 0.1eV, the wall and
The triplet state energy gap by phosphor bodies is greater than or equal to 0.1eV.
In addition, the wall and the HOMO highest occupied molecular orbital energy gap for phosphor bodies are greater than or equal to 0.4eV, between described
Interlayer and the lowest unoccupied molecular orbital energy gap by phosphor bodies are greater than or equal to 0.4eV.
In addition, described for phosphor bodies and the thickness range by phosphor bodies is 20nm~40nm.
In addition, the thickness range of the wall is 5nm~12nm.
In addition, the singlet energy level of the fluorescent emitter is lower than the singlet energy level of the wall, the fluorescence hair
Singlet energy gap between beam and the wall is less than or equal to 0.3eV.
In addition, doping concentration of the fluorescent emitter in the wall is 2%~10%.
Detailed description of the invention
Fig. 1 is the structural schematic diagram of organic electroluminescence device provided by first embodiment of the invention；
Fig. 2 is the structural schematic diagram of luminescent layer in organic electroluminescence device provided by first embodiment of the invention；
Fig. 3 is the formation mechenism of exciplex in organic electroluminescence device provided by first embodiment of the invention
Schematic diagram；
Fig. 4 is the program flow diagram of the preparation method of organic electroluminescence device 100 provided by embodiment of the present invention.
Specific embodiment
In order to make the object, technical scheme and advantages of the embodiment of the invention clearer, below in conjunction with attached drawing to the present invention
Each embodiment be explained in detail.However, it will be understood by those skilled in the art that in each embodiment party of the present invention
In formula, many technical details are proposed in order to make reader more fully understand the present invention.But even if without these technical details
And various changes and modifications based on the following respective embodiments, claimed technical solution of the invention also may be implemented.
The first embodiment of the present invention is related to a kind of organic electroluminescence devices 100, as shown in Figure 1, including substrate 10
And set gradually anode 20, hole injection layer 30, hole transmission layer 40, luminescent layer 50, electron transfer layer on the substrate 10
60, electron injecting layer 70 and cathode 80.Wherein, as shown in Fig. 2, luminescent layer 50 includes at least one for phosphor bodies (m-MTDATA)
51, be arranged in pairs for phosphor bodies 51 at least one by phosphor bodies (T2T) 52 and be set to it is each pair of for phosphor bodies 51 and by
Wall (mCBP) 53 between phosphor bodies 52.Doped with fluorescent emitter (DBP) in wall 53.
The luminescent layer 50 of organic electroluminescence device 100 provided by first embodiment of the invention, passes through donor master
Body-receptor agent model constructs molecule.Due to having significant intramolecular/intermolecular for phosphor bodies-receptor agent model molecule
Electric charge transfer (CT) characteristic, not needing heavy metal ion can be such that HOMO highest occupied molecular orbital and the minimum orbital energy level that accounted for separates, it may be assumed that
By the HOMO highest occupied molecular orbital of entire molecule and the minimum track difference localization that accounted for for phosphor bodies 51 and by phosphor bodies 52, thus
Reduce the Δ E of entire Model MoleculeST(difference of singlet energy level and triplet).For phosphor bodies 51 HOMO highest occupied molecular orbital and
By phosphor bodies 52 it is minimum accounted for track energy level rail flanges be overlapped fewer, Δ ESTIt is smaller, be more conducive to triplet excitons to
Singlet exciton converts, and then the efficiency of organic electroluminescence device is promoted by delayed fluorescence.
Specifically, compared with prior art, for phosphor bodies 51 and by between being inserted among phosphor bodies 52 in present embodiment
Interlayer 53 makes electrons and holes space delocalization, while by the thickness of control wall 53, i.e., controllable donor main body 51 is most
Height accounted for track and by phosphor bodies 52 the minimum track that accounted in energy level rail flanges overlapping degree, thus to entire Model Molecule
Δ ESTRegulated and controled, realizes lesser Δ EST, so that triplet excitons are easier to convert to singlet exciton, and then utilize
The delayed fluorescence of doping fluorescent emitter promotes the efficiency of organic electroluminescence device in wall.In addition, this embodiment party
Control is not necessarily to for phosphor bodies and receptor master for for phosphor bodies 51 and the way separated by phosphor bodies 52 by wall 53 in formula
The doping ratio of body can repeat to realize, be easy to realization industrially.
In addition, in the present embodiment, being capable of forming exciplex for phosphor bodies 51 and by between phosphor bodies 52, base is swashed
The singlet energy level of compound is lower than for phosphor bodies 51 and by the triplet of phosphor bodies 52.
It is illustrated in figure 3 for phosphor bodies 51 and by the schematic illustration for being capable of forming exciplex between phosphor bodies 52,
Hole on the lowest unoccupied molecular orbital track of m-MTDATA on electronics and HOMO highest occupied molecular orbital is acted on by coulomb directly to be occurred occasionally
It closes, and forms exciton on some m-MTDATA molecule, the exciton formed in this way is since bond energy is big, so very stable, referred to as
Localised exciton.
M-MTDATA is electron donor, and T2T is electron acceptor, there is electronics from the donor molecule (m-MTDATA) of excitation
Effect is transferred in the ground state of acceptor molecule (T2T) to forming charge transfer state, it is necessary to assure donor and acceptor molecule are physics
Adjacent, the effect of wall mCBP is the delocalization for occurring that hole and electronics spatially, while also needing to control suitable thickness
Degree guarantees that there are still coulombs to act between m-MTDATA and T2T, to form exciplex.
In addition, the die-away time of exciton is also extended, so exciplex is made to have the property similar to TADF material,
The triplet excitons that can only be dissipated originally by heat radiation are utilized, so improving device efficiency.
Specifically, in the present embodiment, the triplet of exciplex and the triplet for phosphor bodies 51
Between energy gap be greater than or equal to 0.4eV, between the triplet of exciplex and triplet by phosphor bodies 52
Energy gap be greater than or equal to 0.4eV.
Preferably, in the present embodiment, it is less than or equal to for the absolute value of the HOMO highest occupied molecular orbital energy level of phosphor bodies 51
5.5eV is greater than or equal to 2.5eV by the minimum absolute value for having accounted for orbital energy level of phosphor bodies 52.
More preferably, in the present embodiment, wall 53 and the triplet state energy gap for phosphor bodies 51 are greater than or equal to
0.2eV, wall 53 and by phosphor bodies 52 triplet state energy gap be greater than or equal to 0.2eV.
In addition, in the present embodiment, the HOMO highest occupied molecular orbital energy level of wall 53 and accounted for for the highest of phosphor bodies 51
The energy gap of orbital energy level is greater than or equal to 0.4eV, and the wall is greater than with the minimum track energy gap that accounted for by phosphor bodies
Or it is equal to 0.4eV.
Specifically, being 20nm~40nm for phosphor bodies 51 and by the thickness range of phosphor bodies 52 in the present embodiment.
It is understood that also including 20nm and 40nm for phosphor bodies 51 and by the thickness range of phosphor bodies 52 in the present embodiment.
More specifically, the thickness range of wall 53 is 5nm~12nm.In the present embodiment, the thickness of wall 53
Degree is also possible to be equal to 5nm and 12nm.It is understood that the thickness range of above-mentioned wall 53 is only that present embodiment provides
A value range for example, not constitute limit.The effect of wall 53 is to guarantee for phosphor bodies and by phosphor bodies
Between under the premise of electric charge transfer, electrons and holes are subjected to delocalization, if 53 thickness of wall is excessively thin, electronics and sky can not be made
The complete delocalization in cave can be such that the coulomb active force between electrons and holes completely disappears, lead to not produce if wall 53 is blocked up
Raw charge transfer state, can specifically be configured according to the actual situation.
Further, the singlet energy level of fluorescent emitter be lower than wall 53 singlet energy level, fluorescent emitter with
Singlet energy gap between wall 53 is less than or equal to 0.3eV.
Further, doping concentration of the fluorescent emitter in wall 53 is 2%~10%.It is understood that
In the present embodiment, the doping concentration of fluorescent emitter is also possible to be equal to 2% and 10%.
In the following, by joining to the preparation method and performance of organic electroluminescence device 100 provided by embodiment of the present invention
Number is illustrated, it is to be understood that and following is only a kind of specific embodiment of the invention, does not constitute and limits,
Specific production step is as shown in Figure 4, comprising the following steps:
Step S401: cleaning substrate using detergent, deionized water, acetone, ethyl alcohol etc., by the substrate after cleaning
It is placed in baking 1 hour in 110 DEG C of baking oven.
Specifically, in this step, anode layer is provided on substrate.
Step S402: it is handled after substrate is cooled to room temperature using plasma (plasma) cavity, to improve anode
The work function of layer.
Step S403: will by plasma chamber, treated that substrate is placed in vacuum chamber, vacuum chamber is evacuated to 5 ×
10-7Pa。
Step S404: on the anode layer successively be deposited hole injection layer, hole transmission layer, luminescent layer, electron transfer layer and
Electron injecting layer.
Specifically, in this step, in vapor deposition hole injection layer, hole transmission layer, luminescent layer, electron transfer layer and electronics
When implanted layer, plating rate and film thickness are monitored by crystal-vibration-chip.
Further, in this step, luminescent layer uses the form steamed altogether of double source, wherein the plating rate of wall is
0.98A/s, the plating rate of fluorescent emitter are 0.02A/s, hole injection layer, hole transmission layer, electron transfer layer and electron injection
The plating rate of layer is 1A/s.
Step S405: lithium fluoride (LiF) layer and aluminium (Al) layer is successively deposited as cathode layer on the surface of electron injecting layer.
Specifically, in this step, LiF layers of evaporation rate is 0.1A/s, and with a thickness of 1nm, Al layers of evaporation rate is
1.5A/s, with a thickness of 120nm.
In this example, the specific structure of the organic electroluminescence device 100 to complete through the above steps is as follows:
ITO/HATCN (10nm)/m-MTDATA (50nm)/mCBP:2%DBP (8nm)/T2T (20nm)/Alq3 (20nm)/
LiF(1nm)/Al.It (is in the present embodiment tin indium oxide ITO material, it is to be understood that anode layer in anode layer
Can be other materials, herein without enumerating) on set gradually the hole injection layer (HATCN) of 10nm, 50nm
M-MTDATA layers, the mCBP layer of 8nm, the T2T layer of 20nm, three (8-hydroxyquinoline) aluminium (Alq3) layers of 20nm, 1nm LiF layer
And Al layers.Wherein, doped with fluorescent emitter in wall, doping concentration 2%, the unit of doping concentration is weight percent
Than (wt%).
In addition, also providing a kind of organic electroluminescence device 200 of prior art, specific structure in this example are as follows:
ITO/HATCN (10nm)/m-MTDATA (40nm)/m-MTDATA:T2T:DBP (4:6:2%, 25nm)/T2T
(10nm)/Alq3(20nm)/LiF(1nm)/Al.I.e. anode layer (be in the present embodiment tin indium oxide ITO material, can be with
Understand, anode layer is also possible to other materials, herein without enumerating) on set gradually 10nm hole injection
(HATCN) T2T of layer, the m-MTDATA layer of 40nm, the luminescent layer (m-MTDATA:T2T:DBP, 4:6:2%) of 25nm, 10nm
Layer, the Alq3 layer of 20nm, the LiF layer of 1nm and Al layers.
The performance of organic electroluminescence device 100 and organic electroluminescence device 200 is indicated in the following table:
| Device | Bright voltage | EQE | Efficiency roll-off |
| Organic electroluminescence device 100 | 3.2V | 14.5 | 6.2% |
| Organic electroluminescence device 200 | 3.0V | 12.8 | 26.5% |
As seen from the above table, it in organic electroluminescence device 200, is co-doped with using m-MTDATA, T2T and DBP three as hair
Photosphere, maximum external quantum efficiency (EQE) be 12.8%, due to exciton concentration in luminescent layer Relatively centralized, be easy to happen three lines
State-triplet state buries in oblivion (TTA) and (TPA) is quenched in triplet state-polaron, so efficiency is relatively low, efficiency roll-off is also larger.Fig. 1 is
The energy diagram of organic luminescent device 100 inserts one layer mCBP layers, the triplet energy state ratio of mCBP between m-MTDATA and T2T
M-MTDATA and T2T will be high, so hole can be limited in the interface of m-MTDATA layers He mCBP layers, and electronics is limited
In T2T layers and mCBP layers of interface, to generate space delocalization.Further, effective by the adjustment to mCBP thickness degree
The Δ E of exciplex is regulated and controled to be formed between m-MTDATA layers and T2T layersST(wherein S1=2.56eV, T1=2.22eV, Δ
EST=0.04eV), break triplet energy state and the unborn forbidden transition of singlet energy.Therefore, exciplex
Triplet energy state can quickly be converted to singlet energy by anti-intersystem crossing (RISC) process, the singlet energy after conversion
It can be by being transferred to the DBP being entrained in mCBP layers to radioluminescence.Due to being utilized cannot be used to shine originally three
Line state energy, so the theoretical upper limit of luminous efficiency can be more than 25%.It can also be seen that organic electroluminescence from table 1
Part 100 greatly reduces efficiency roll-off with respect to organic electroluminescence device 200, is further conducive to improve device lifetime.
It will be understood by those skilled in the art that the respective embodiments described above are to realize specific embodiments of the present invention,
And in practical applications, can to it, various changes can be made in the form and details, without departing from the spirit and scope of the present invention.
Claims (10)
1. a kind of organic electroluminescence device, including substrate and the anode being successively set on substrate, electron injecting layer, electronics
Transport layer, luminescent layer, hole transmission layer, hole injection layer and cathode, which is characterized in that the luminescent layer includes at least one confession
Phosphor bodies, at least one described being arranged in pairs for phosphor bodies by phosphor bodies and be set to it is each pair of it is described for phosphor bodies and
Described at least one wall by between phosphor bodies and doped with fluorescent emitter.
2. organic electroluminescence device according to claim 1, which is characterized in that described for phosphor bodies and the receptor master
Exciplex is capable of forming between body, the triplet of the exciplex is lower than described for phosphor bodies and the receptor
The triplet of main body.
3. organic electroluminescence device according to claim 2, which is characterized in that the singlet energy of the exciplex
Energy gap between grade and the triplet for phosphor bodies is greater than or equal to 0.4eV, the singlet of the exciplex
Energy gap between energy level and the triplet by phosphor bodies is greater than or equal to 0.4eV.
4. organic electroluminescence device according to claim 2, which is characterized in that the highest for phosphor bodies has accounted for rail
The absolute value of road energy level is less than or equal to 5.5eV, and the absolute value of the lowest unoccupied molecular orbital energy level by phosphor bodies is greater than or waits
In 2.5eV.
5. organic electroluminescence device according to claim 1, which is characterized in that the wall and described for phosphor bodies
Triplet state energy gap be greater than or equal to 0.1eV, the wall and the triplet state energy gap by phosphor bodies are greater than or equal to
0.1eV。
6. organic electroluminescence device according to claim 1, which is characterized in that the wall and described for phosphor bodies
HOMO highest occupied molecular orbital energy gap be greater than or equal to 0.4eV, the wall and the lowest unoccupied molecular orbital energy gap by phosphor bodies
More than or equal to 0.4eV.
7. organic electroluminescence device according to claim 1, which is characterized in that described for phosphor bodies and the receptor master
The thickness range of body is 20nm~40nm.
8. organic electroluminescence device according to claim 1, which is characterized in that the thickness range of the wall is
5nm~12nm.
9. organic electroluminescence device according to claim 1, which is characterized in that the singlet energy of the fluorescent emitter
Grade be lower than the wall singlet energy level, the singlet energy gap between the fluorescent emitter and the wall be less than or
Equal to 0.3eV.
10. organic electroluminescence device according to claim 9, which is characterized in that the fluorescent emitter is between described
Doping concentration in interlayer is 2%~10%.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112271262A (en) * | 2020-10-26 | 2021-01-26 | 京东方科技集团股份有限公司 | Organic light-emitting device, preparation method and display panel |
| CN112701231A (en) * | 2020-12-31 | 2021-04-23 | 昆山国显光电有限公司 | Organic electroluminescent device and display device |
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| CN102655222A (en) * | 2011-02-28 | 2012-09-05 | 株式会社半导体能源研究所 | Light-emitting device |
| WO2018047853A1 (en) * | 2016-09-06 | 2018-03-15 | 株式会社Ｋｙｕｌｕｘ | Organic light-emitting device |
| CN108463895A (en) * | 2016-01-14 | 2018-08-28 | 国立大学法人九州大学 | Organic electroluminescent device, element group, the manufacturing method of organic electroluminescent device, the emission wavelength control method of organic electroluminescent device |
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| CN102655222A (en) * | 2011-02-28 | 2012-09-05 | 株式会社半导体能源研究所 | Light-emitting device |
| CN108463895A (en) * | 2016-01-14 | 2018-08-28 | 国立大学法人九州大学 | Organic electroluminescent device, element group, the manufacturing method of organic electroluminescent device, the emission wavelength control method of organic electroluminescent device |
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| CN112271262A (en) * | 2020-10-26 | 2021-01-26 | 京东方科技集团股份有限公司 | Organic light-emitting device, preparation method and display panel |
| CN112271262B (en) * | 2020-10-26 | 2024-01-23 | 京东方科技集团股份有限公司 | Organic light-emitting device, preparation method and display panel |
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