CN108054287A - A kind of efficient organic monolayer light emitting diode and preparation method thereof - Google Patents
A kind of efficient organic monolayer light emitting diode and preparation method thereof Download PDFInfo
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- CN108054287A CN108054287A CN201711250383.8A CN201711250383A CN108054287A CN 108054287 A CN108054287 A CN 108054287A CN 201711250383 A CN201711250383 A CN 201711250383A CN 108054287 A CN108054287 A CN 108054287A
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- light emitting
- emitting diode
- ito
- organic monolayer
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/80—Constructional details
- H10K50/805—Electrodes
- H10K50/81—Anodes
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- 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
- H10K71/60—Forming conductive regions or layers, e.g. electrodes
Abstract
The present invention relates to a kind of efficient organic monolayer light emitting diodes and preparation method thereof.The structure of the diode is sequentially arranged to from bottom to top：Glass substrate, tin indium oxide, luminescent layer, electron injecting layer and the metallic cathode of chlorination processing.The organic monolayer light emitting diode does not have hole transmission layer and electron transfer layer, and luminescent layer is unique organic material of device.Chlorinated solvent used in the present invention is respectively chloroform, chlorobenzene and dichloro-benzenes.After the ultraviolet processing of chlorinated solvent, work function is increased tin indium oxide, improves the injectability in hole.Performance with the device of dichloro-benzenes chlorination processing tin indium oxide is optimal, and maximum current efficiency is 33.48 every ampere of candelas, and maximum power efficiency is 27.51 lumen per Watts.
Description
Technical field
The present invention relates to organic electroluminescence device (OLED) fields.It is more particularly related to a kind of organic list
Layer electroluminescent device and its method simply prepared.
Background technology
With the promotion of scientific and technological level, display technology from traditional mode such as cathode-ray tube, liquid crystal display,
Gradually develop to the technologies such as large area, flexible, ultra-thin, ultralight.Organic electroluminescence device (OLED) is developed recently
A kind of solidification flat panel display to attract people's attention, compared with other display technologies, OLED have low dc voltage driving,
The advantages that low in energy consumption, self-luminous, simple in structure, ultra-thin, fast response time, wide viewing angle and realization flexible, thus become
One of most promising technology in opto-electronic device and flat display field.(Nature,459234(2009))
In order to promote the efficiency of organic electroluminescence device and service life, high performance device usually contains hole injection
The functional layers such as layer, hole transmission layer, luminescent layer, electron transfer layer, electron injecting layer.(adv.Funct.Mater.11310
(2010)) however, the device architecture of so Multifunctional layered adds the complexity of preparation and the cost of production.Therefore, it is necessary to
Simplify organic electroluminescence device structure, particularly develop organic monolayer electroluminescent device.However organic function layer can be very well
Regulation and control hole current and electronic current, the recombination region of carrier is adjusted, so as to promote the luminescent properties of device, so with having
Machine multilayer electroluminescent device is compared, and under the premise of not reducing external quantum efficiency and keeping efficient in high brightness, is simplified
There is certain challenges for the structure of organic multilayer electroluminescent device.
For organic luminescent device, current efficiency is one of important criterion for characterizing OLED.Have in double-deck
In organic electroluminescence devices, recombination region is in the interface of hole transmission layer and electron transfer layer, (Appl.Phys.Lett.51913
(1987)) but in single layer device, due to the presence of no heterogeneous interface, hole and the compound of electronics will be during transmission
It completes, the hole otherwise transmitted and electronics will form dark current, so as to reduce the efficiency of device.Therefore in the electroluminescent hair of organic monolayer
During the design and preparation of optical device, the injection and transmission of equilbrium carrier are answered, recombination region is made to reduce away from anode and cathode
Exciton is quenched.
The content of the invention
Technical problem：The present invention addresses the above problem propose a kind of efficient organic monolayer light emitting diode and its
Preparation method, devising the high efficiency that a kind of chlorinated solvent and the ITO electrode Cl-ITO that ultraviolet processing is formed jointly do anode has
Machine monolayer luminescence diode and preparation method thereof.The organic monolayer light emitting diode of the present invention uses chlorinated solvent and ITO electrode
The method of common ultraviolet processing modifies ITO electrode, the injection and transmission of equilbrium carrier, promotes the efficiency of device.With with oxygen
Change molybdenum modification ITO devices to compare, Cl-ITO reduces the process being once vapor-deposited, and effectively simplifies manufacturing process.
Technical solution：There are high work function, the characteristics such as work function is adjustable, preparation method is simple using Cl-ITO, drawn
The anode of organic monolayer light emitting diode is used as, the Hole injection capacity of organic monolayer light emitting diode is significantly carried
Height, while also improve the current efficiency of device.Under the irradiation of ultraviolet rays, chlorine (Cl) base easily from chlorinated solvent (chloroform,
Chlorobenzene, dichloro-benzenes) in release, the O on substitution ITO surfaces forms chloro- indium key.It composes and tests through ultraviolet photoelectron, Cl-ITO and ITO
It compares, Cl-ITO has higher work function.How much related, work(of Cl-ITO that the work function of Cl-ITO is formed with chloro- indium key
Function reaches as high as 6.1 electron-volts (eV).It is related with chlorinated solvent ultraviolet processing time using the work function of Cl-ITO, variation
The work function (4.7eV -6.1eV) of Cl-ITO is adjusted in ITO and chlorinated solvent ultraviolet processing time.
In organic monolayer light emitting diode, the interface between electrode and luminescent material is relatively important part, electrode with
Energy level between luminescent material mismatches, and the injection for causing carrier is difficult, and light emitting diode opens bright voltage height, current efficiency
It is low, the shortcomings of device easily deteriorates.The present invention has the property of high work function and the adjustable grade of work function using Cl-ITO, uses it
As the anode of organic monolayer light emitting diode, the injectability of hole and electronics is balanced, improves the performance of entire device.
A kind of order of the layer structure of high efficiency organic monolayer light emitting diode of the present invention from bottom to top is arranged to：Thoroughly
Bright substrate, transparent anode, luminescent layer, electron injecting layer and metallic cathode.
Wherein,
The transparent substrates are transparent glass.
The transparent anode is tin indium oxide ITO.
The luminous layer main body be 1,3,5- tri- (N- phenylbenzimidazol -2- bases) benzene, abbreviation TPBi；Luminescent layer object
For three (2- phenylpyridines) iridium, abbreviation Ir (ppy)3。
The electron injecting layer is lithium fluoride LiF.
The metallic cathode is aluminium Al.
The preparation method of the high efficiency organic monolayer light emitting diode of the present invention comprises the following steps：
1) ito glass is pre-processed：The ITO electro-conductive glass for etching and cleaning up with nitrogen is dried up and to carry out ultraviolet light smelly
Oxygen processing；
2) ito glass and chlorinated solvent that have pre-processed are put into together in the glass reaction kettle of closing again, then it is common purple
Then outer processing is fitted into the complete ito glass of chlorination, that is, Cl-ITO anodes in vacuum coating system；
3) it is 5 × 10 in a vacuum degree-4The method that vacuum thermal evaporation is used in vacuum coating system below Pascal,
80-100 nanometers luminescent layer TPBi, Ir (ppy) is deposited on the Cl-ITO glass successively3, Ir (ppy)3Mass fraction
Account for the 30-35% of entire luminescent layer quality, the metallic cathode Al of 0.7-1 nanometers of LiF and 120-150 nanometers of electron injecting layer；
The part that intersects of wherein Cl-ITO anodes and metallic cathode forms the luminous zone of device.
Wherein,
The chlorinated solvent is one kind in chloroform, chlorobenzene or dichloro-benzenes.
The evaporation rate of the TPBi controls, Ir (ppy) per second at 0.05-0.1 nanometers3Evaporation rate control exist
0.015-0.033 nanometers per second, and the evaporation rate control of LiF is per second at 0.005-0.01 nanometers, the evaporation speed of thick metallic cathode
Rate control is per second at 0.3-0.5 nanometers.The thickness and growth rate of Material growth are monitored in real time by film thickness gauge.
The organic monolayer light emitting diode of the present invention is repaiied using the method for chlorinated solvent and ITO electrode ultraviolet processing jointly
ITO electrode is adornd, the injection and transmission of equilbrium carrier promote the efficiency of device.Compared with modifying ITO devices with molybdenum oxide, Cl-
ITO reduces the process being once vapor-deposited, and effectively simplifies manufacturing process.
Advantageous effect：The above-mentioned technical proposal of the present invention has the following advantages compared with the prior art：
It, can be by adjusting time of the ultraviolet processing of chlorinated solvent 1. high efficiency organic monolayer luminescent device of the present invention
Change the work function of ITO, so as to the injection and transmission of equilbrium carrier, promote the efficiency of device.
2. high efficiency organic monolayer luminescent device of the present invention, Cl-ITO need not be vapor-deposited in the preparation, only
By the ultraviolet processing jointly of ITO surfaces and chlorinated solvent, manufacturing process can be effectively simplified.
3. high efficiency organic monolayer luminescent device of the present invention, the species of workable chlorinated solvent is more, such as chloroform,
Chlorobenzene, dichloro-benzenes etc..
4. the present invention uses material：TPBi、Ir(ppy)3, LiF and Al be commercialized material, convenient material drawing.
Description of the drawings
Fig. 1 is the organic monolayer EL device structure figure made by case study on implementation one.
Fig. 2 is the organic monolayer EL device structure figure made by case study on implementation two, three, four.
Fig. 3 gives current efficiency-luminosity response of four groups of devices.
Fig. 4 gives the spectrogram of four groups of devices.
Specific embodiment
Embodiment one:
By the ITO electro-conductive glass etched successively with washing lotion solution, deionized water, acetone, each ultrasonic 15 minutes two of ethyl alcohol
Time.After the ITO electro-conductive glass cleaned up is dried up with nitrogen, placed in UV ozone instrument and handled 5 minutes, finally this
Glass substrate is put into vacuum coating system.Organic material is placed on to different evaporation sources, the temperature of each evaporation source can be with
Individually control.When vacuum coating system vacuum degree reaches 5 × 10-4When below Pascal, 1 nanometer of sky is deposited on anode
Cave implanted layer MoO3, 100 nanometers of luminescent layer TPBi：Ir(ppy)3,Ir(ppy)3Mass fraction account for entire luminescent layer quality
33%th, 0.7 nanometer of electron injecting layer LiF and 150 nanometers of thick metallic cathode Al, the cross one another part of two of which electrode
The luminous zone of device is formed, luminous zone effective area is 16 square millimeters.The thickness and growth rate of Material growth are by film thickness gauge
Real time monitoring.MoO3Evaporation rate control it is per second at 0.005 nanometer, the evaporation rate of TPBi is controlled in 0.1 nanometer of per second, Ir
(ppy)3Evaporation rate control it is per second at 0.033 nanometer, the control of the evaporation rate of LiF is per second at 0.005 nanometer, and thick metal is cloudy
The evaporation rate control of pole is per second per second to 0.5 nanometer at 0.3 nanometer.After vapor deposition is completed, device is taken in atmospheric environment
Carry out the test of Current density-voltage-brightness relationship and the test of spectrum.Finally being prepared into structure is:Glass/ITO/MoO3
(1nm)/TPBi：Ir(ppy)3(100nm, 33wt%)/LiF (0.7nm)/Al (150nm) organic monolayer light emitting diode.Its device
Part structure chart is Figure of description figure (1), and Current density-voltage-brightness relationship curve figure of device is Figure of description figure
(3), the spectrogram of device is Figure of description figure (4).
Embodiment two:
By the ITO electro-conductive glass etched successively with washing lotion solution, deionized water, acetone, each ultrasonic 15 minutes two of ethyl alcohol
Time.After the ITO electro-conductive glass cleaned up is dried up with nitrogen, placed in UV ozone instrument and handled 5 minutes, then pre-
The ito glass and chloroform solvent handled well are put into together in the glass reaction kettle of closing, then ultraviolet processing 2 minutes jointly.Finally
The glass substrate is put into vacuum coating system.Organic material is placed on to different evaporation sources, the temperature of each evaporation source
It can individually control.When vacuum coating system vacuum degree reaches 5 × 10-4When below Pascal, on anode, 90 nanometers
Luminescent layer TPBi：Ir(ppy)3,Ir(ppy)3Mass fraction account for 33%, 0.7 nanometer of electron injection of entire luminescent layer quality
The thick metallic cathode Al of LiF and 150 nanometer of layer, the cross one another part of two of which electrode form the luminous zone of device, shine
Area's effective area is 16 square millimeters.The thickness and growth rate of Material growth are monitored in real time by film thickness gauge.The evaporation speed of TPBi
Rate controls, Ir (ppy) per second at 0.1 nanometer3Evaporation rate control it is per second at 0.033 nanometer, the control of the evaporation rate of LiF exists
0.005 nanometer per second, and the evaporation rate control of thick metallic cathode is per second per second to 0.5 nanometer at 0.3 nanometer.In vapor deposition completion
Afterwards, test and the spectrum that Current density-voltage-brightness relationship is carried out in atmospheric environment are taken.Finally being prepared into structure is:
Glass/Cl-ITO/TPBi：Ir(ppy)3(90nm, 33wt%)/LiF (0.7nm)/Al (150nm) organic monolayer light-emitting diodes
Pipe.Its device junction is patterned into Figure of description figure (2), and Current density-voltage-brightness relationship curve figure of device is specification
Attached drawing figure (3), the spectrogram of device is Figure of description figure (4).
Embodiment three:
By the ITO electro-conductive glass etched successively with washing lotion solution, deionized water, acetone, each ultrasonic 15 minutes two of ethyl alcohol
Time.After the ITO electro-conductive glass cleaned up is dried up with nitrogen, placed in UV ozone instrument and handled 5 minutes, then pre-
The ito glass and chlorobenzene solvent handled well are put into together in the glass reaction kettle of closing, then ultraviolet processing 5 minutes jointly.Finally
The glass substrate is put into vacuum coating system.Organic material is placed on to different evaporation sources, the temperature of each evaporation source
It can individually control.When vacuum coating system vacuum degree reaches 5 × 10-4When below Pascal, on anode, 90 nanometers
Luminescent layer TPBi：Ir(ppy)3,Ir(ppy)3Mass fraction account for 33%, 0.7 nanometer of electron injection of entire luminescent layer quality
The thick metallic cathode Al of LiF and 150 nanometer of layer, the cross one another part of two of which electrode form the luminous zone of device, shine
Area's effective area is 16 square millimeters.The thickness and growth rate of Material growth are monitored in real time by film thickness gauge.The evaporation speed of TPBi
Rate controls, Ir (ppy) per second at 0.1 nanometer3Evaporation rate control it is per second at 0.033 nanometer, the control of the evaporation rate of LiF exists
0.005 nanometer per second, and the evaporation rate control of thick metallic cathode is per second per second to 0.5 nanometer at 0.3 nanometer.In vapor deposition completion
Afterwards, test and the spectrum that Current density-voltage-brightness relationship is carried out in atmospheric environment are taken.Finally being prepared into structure is:
Glass/Cl-ITO/TPBi：Ir(ppy)3(90nm, 33wt%)/LiF (0.7nm)/Al (150nm) organic monolayer light-emitting diodes
Pipe.Its device junction is patterned into Figure of description figure (2), and Current density-voltage-brightness relationship curve figure of device is specification
Attached drawing figure (3), the spectrogram of device is Figure of description figure (4).
Example IV:
By the ITO electro-conductive glass etched successively with washing lotion solution, deionized water, acetone, each ultrasonic 15 minutes two of ethyl alcohol
Time.After the ITO electro-conductive glass cleaned up is dried up with nitrogen, placed in UV ozone instrument and handled 5 minutes, then pre-
The ito glass and dichloro benzene solvent handled well are put into together in the glass reaction kettle of closing, then ultraviolet processing 5 minutes jointly.Most
The glass substrate is put into vacuum coating system afterwards.Organic material is placed on to different evaporation sources, the temperature of each evaporation source
Degree can be controlled individually.When vacuum coating system vacuum degree reaches 5 × 10-4When below Pascal, on anode, 90 nanometers
Luminescent layer TPBi：Ir(ppy)3,Ir(ppy)3Mass fraction account for entire luminescent layer quality 33%, 0.7 nanometer of electronics note
Enter layer LiF and 150 nanometer of thick metallic cathode Al, the cross one another part of two of which electrode forms the luminous zone of device, hair
Light area effective area is 16 square millimeters.The thickness and growth rate of Material growth are monitored in real time by film thickness gauge.The evaporation of TPBi
Speed control is per second at 0.1 nanometer, Ir (ppy)3Evaporation rate control it is per second at 0.033 nanometer, the control of the evaporation rate of LiF
Per second at 0.005 nanometer, the evaporation rate control of thick metallic cathode is per second per second to 0.5 nanometer at 0.3 nanometer.It is completed in vapor deposition
Afterwards, test and the spectrum that Current density-voltage-brightness relationship is carried out in atmospheric environment are taken.Finally being prepared into structure is:
Glass/Cl-ITO/TPBi：Ir(ppy)3(90nm, 33wt%)/LiF (0.7nm)/Al (150nm) organic monolayer light-emitting diodes
Pipe.Its device junction is patterned into Figure of description figure (2), and Current density-voltage-brightness relationship curve figure of device is specification
Attached drawing figure (3), the spectrogram of device is Figure of description figure (4).
As can be seen from Figure 3 the current efficiency of embodiment two, three, four is above embodiment one in monolayer luminescence device,
The current efficiency highest of example IV reaches 33.48 every ampere of candelas, and the current efficiency of embodiment one is 28.40 candelas
Every ampere, the current efficiency of embodiment two is 31.39 every ampere of candelas, and the current efficiency of embodiment three is 32.50 candelas
Every ampere.Illustrate that Cl-ITO electrodes can prepare organic monolayer electroluminescent device well.And as can be seen from Figure 4 own
Single layer device spectrum be almost be overlapped, illustrate using chlorinated solvent modification ITO electrode to device spectral, there is no shadows
It rings.
Claims (9)
1. a kind of high efficiency organic monolayer light emitting diode, which is characterized in that the layer structure of the light emitting diode is from bottom to top
Order be arranged to：Transparent substrates, transparent anode, luminescent layer, electron injecting layer and metallic cathode.
A kind of 2. high efficiency organic monolayer light emitting diode according to claim 1, which is characterized in that the transparent lining
Bottom is transparent glass.
A kind of 3. high efficiency organic monolayer light emitting diode according to claim 1, which is characterized in that the transparent sun
Extremely tin indium oxide ITO.
A kind of 4. high efficiency organic monolayer light emitting diode according to claim 1, which is characterized in that the luminescent layer
Main body is 1,3,5- tri- (N- phenylbenzimidazol -2- bases) benzene, abbreviation TPBi；Luminescent layer object is three (2- phenylpyridines) iridium,
Abbreviation Ir (ppy)3。
A kind of 5. high efficiency organic monolayer light emitting diode according to claim 1, which is characterized in that the electronics note
It is lithium fluoride LiF to enter layer.
6. a kind of high efficiency organic monolayer light emitting diode according to claim 1, which is characterized in that the metal is cloudy
Extremely aluminium Al.
A kind of 7. preparation method of high efficiency organic monolayer light emitting diode as described in claim 1, which is characterized in that the system
Preparation Method comprises the following steps：
1) ito glass is pre-processed：The ITO electro-conductive glass for etching and cleaning up with nitrogen is dried up and is carried out at ultraviolet and ozone
Reason；
2) ito glass and chlorinated solvent that have pre-processed are put into together in the glass reaction kettle of closing again, then common ultraviolet place
Reason, is then fitted into the complete ito glass of chlorination, that is, Cl-ITO anodes in vacuum coating system；
3) it is 5 × 10 in a vacuum degree-4The method that vacuum thermal evaporation is used in vacuum coating system below Pascal, successively
80-100 nanometers luminescent layer TPBi, Ir (ppy) are deposited on the Cl-ITO glass3, Ir (ppy)3Mass fraction account for it is whole
The 30-35% of a luminescent layer quality, the metallic cathode Al of 0.7-1 nanometers of LiF and 120-150 nanometers of electron injecting layer；
The part that intersects of wherein Cl-ITO anodes and metallic cathode forms the luminous zone of device.
A kind of 8. preparation method of high efficiency organic monolayer light emitting diode according to claim 7, which is characterized in that institute
The chlorinated solvent stated is one kind in chloroform, chlorobenzene or dichloro-benzenes.
A kind of 9. preparation method of high efficiency organic monolayer light emitting diode according to claim 7, which is characterized in that institute
The evaporation rate of the TPBi stated controls, Ir (ppy) per second at 0.05-0.1 nanometers3Evaporation rate control in 0.015-0.033
Nanometer is per second, and the evaporation rate control of LiF is per second at 0.005-0.01 nanometers, and the evaporation rate of thick metallic cathode is controlled in 0.3-
0.5 nanometer per second.
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Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102945693A (en) * | 2012-10-31 | 2013-02-27 | 清华大学 | Method for improving surface work function of ITO transparent conducting thin film and application of ITO transparent conducting thin film |
| CN104051637A (en) * | 2013-03-11 | 2014-09-17 | 海洋王照明科技股份有限公司 | Organic light-emitting device and preparation method thereof |
| CN106920856A (en) * | 2017-03-14 | 2017-07-04 | 芜湖乐知智能科技有限公司 | A kind of electroluminescent and photovoltaic double-function device and preparation method thereof |
-
2017
- 2017-12-01 CN CN201711250383.8A patent/CN108054287A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102945693A (en) * | 2012-10-31 | 2013-02-27 | 清华大学 | Method for improving surface work function of ITO transparent conducting thin film and application of ITO transparent conducting thin film |
| CN104051637A (en) * | 2013-03-11 | 2014-09-17 | 海洋王照明科技股份有限公司 | Organic light-emitting device and preparation method thereof |
| CN106920856A (en) * | 2017-03-14 | 2017-07-04 | 芜湖乐知智能科技有限公司 | A kind of electroluminescent and photovoltaic double-function device and preparation method thereof |
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Application publication date: 20180518 |