CN105244447B - A kind of planar heterojunction Organic Light Emitting Diode and preparation method thereof - Google Patents

A kind of planar heterojunction Organic Light Emitting Diode and preparation method thereof Download PDF

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Publication number
CN105244447B
CN105244447B CN201510553459.9A CN201510553459A CN105244447B CN 105244447 B CN105244447 B CN 105244447B CN 201510553459 A CN201510553459 A CN 201510553459A CN 105244447 B CN105244447 B CN 105244447B
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light emitting
emitting diode
type
semiconductor layer
layer
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CN201510553459.9A
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CN105244447A (en
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苏仕健
陈东成
曹镛
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华南理工大学
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Abstract

The invention belongs to organic photoelectrical material technical field, a kind of planar heterojunction Organic Light Emitting Diode and preparation method thereof is disclosed.The light emitting diode includes the substrate stacked gradually, anode, p-type organic semiconductor layer, n-type organic semiconductor layer and cathode.P-type organic semiconductor layer is made of the organic semiconducting materials for capableing of preferably conduction hole, and n-type organic semiconductor layer is made of the organic semiconducting materials that can preferably conduct electronics.The photochromic interaction from PN hetero-junctions of light emitting diode of the present invention, luminescent spectrum is different from the luminescent spectrum of independent p-type or N-type semiconductor, and the light emitting diode of the present invention is that P-type material and n type material are constituted in a manner of being layered on top of each other, there is no the luminescent layers of traditional OLED, have lower driving voltage and higher luminous efficiency, application prospect are good.

Description

A kind of planar heterojunction Organic Light Emitting Diode and preparation method thereof

Technical field

The invention belongs to organic photoelectrical material technical fields, and in particular to a kind of planar heterojunction Organic Light Emitting Diode and Preparation method.

Background technology

Currently, the research of Organic Light Emitting Diode (OLED) has been introduced into the commercial application stage, scientific research institutions are high School, enterprise has all put into a large amount of human and material resources, financial resources carry out relevant research and applies work.The research starts from 1987, The equal OLED device developed using sandwich device architecture in patent US4356429 of doctor Deng Qingyun of Kodak Light emission luminance reaches 1000cd/m under 10V direct voltage drives2, OLED is made to obtain epoch-making development.It is rich in Deng Qingyun In the device architecture that scholar puts forward, two kinds of organic functional materials of hole transport and electron-transport are only existed, wherein electron-transport material Material has functioned simultaneously as carrier (electronics) transmission and luminous function.From after last century the nineties, more organic layer Multiple heterostructures OLED device be increasingly becoming the mainstream of research.At least there are an individual luminescent layer and two inside this device architecture Carrier blocking layers, shine in device and the function of carrier transport is respectively by the luminescent layer and high mobility of relatively low mobility Carrier blocking layers undertake.In order to which carrier and blocking exciton, the OLED devices of more organic layer Multiple heterostructures is better balanced Often there is also the barrier layers of the implanted layer of carrier and exciton inside part so that device architecture further complicates.

Come from the point of view of business application, the OLED device of more organic layer Multiple heterostructures has the following disadvantages:(1) more Layer organic layer makes device preparation flow cumbersome, is unfavorable for the reduction of time cost;(2) material of multilayer multiple types makes device Preparation needs the cost of material also to increase significantly;(3) it is easy to there is a problem of mutually stablizing between different organic phases, so as to shadow Ring device lifetime;(4) it is easy Presence of an interface pressure drop between different organic layers so that the more difficult reduction of driving voltage of device increases Power consumption when device work.

Based on considerations above, a kind of OLED for the planar heterojunction structure that novel structure is simple is developed, to reducing device Manufacturing cost, while obtaining high device efficiency and be just particularly important.

Invention content

In order to solve the disadvantage that the above prior art and shortcoming, the primary purpose of the present invention is that providing a kind of plane Hetero-junctions Organic Light Emitting Diode.

Another object of the present invention is to provide a kind of preparation methods of above-mentioned planar heterojunction Organic Light Emitting Diode.

The object of the invention is achieved through the following technical solutions:

A kind of planar heterojunction Organic Light Emitting Diode, including stack gradually substrate, anode, p-type organic semiconductor layer, N-type organic semiconductor layer and cathode, stratose structural schematic diagram are as shown in Figure 1;

The material for preparing of the p-type organic semiconductor layer includes but not limited to following material:

The material for preparing of the n-type organic semiconductor layer includes but not limited to following material:

The p-type organic semiconductor layer and n-type organic semiconductor layer can be single-layer or multi-layer;P-type organic semiconductor Layer prepares the blending that material is one-component material or multi-component material with n-type organic semiconductor layer.

One layer of anode buffer layer can also be added between the anode and p-type organic semiconducting materials;Cathode is organic with N-type One layer of cathode buffer layer can also be added between semi-conducting material.

The substrate be rigid substrate such as glass, quartz, sapphire etc. and flexible substrate such as polyimides, poly- pair Ethylene terephthalate, mylar's fat, polyethylene naphthalate or other polyester materials and metal, Alloy or stainless steel film etc..

The anode and cathode is metal or metal oxide;The preferred tin indium oxide of the metal oxide (ITO), the group of one or more of fluorine-doped tin dioxide (FTO), zinc oxide (ZnO) and indium gallium zinc oxide (IGZO) It closes.

The luminescent spectrum of the planar heterojunction Organic Light Emitting Diode is organic from p-type organic semiconductor layer and N-type The PN hetero-junctions that semiconductor layer is constituted, spectral position are different from independent p-type organic semiconductor layer material or N-type organic semiconductor The luminescent spectrum of layer material.

The preparation method of above-mentioned planar heterojunction Organic Light Emitting Diode, includes the following steps:

The substrate material with anode layer is taken, it is organic to be then sequentially prepared p-type organic semiconductor layer, N-type on the anode layer Semiconductor layer and cathode layer obtain planar heterojunction Organic Light Emitting Diode.

The method of the preparation includes hot evaporation, spin coating, brushing, spraying, dip-coating, roller coating, printing or inkjet printing.

The present invention preparation method and obtained product has the following advantages that and advantageous effect:

(1) device architecture according to the present invention is simple, and preparation flow is few, while low driving voltage and height may be implemented External quantum efficiency;

(2) device organic layer according to the present invention does not contain precious metal element, is conducive to reduce the material cost of device;

(3) device according to the present invention is without traditional so-called luminescent layer with preferable fluorescence capability of OLED device, Only constituted using charge transport materials;

(4) device according to the present invention can carry out radioluminescence using singlet and triplet excitons simultaneously, theoretical Internal quantum efficiency reaches 100%, and can only achieve using conventional fluorescent material as the device of luminescent layer, theoretical internal quantum efficiency 25%.

Description of the drawings

Fig. 1 is the stratose structural schematic diagram of the planar heterojunction Organic Light Emitting Diode of the present invention;

Fig. 2 is the Current density-voltage-brightness curve figure for the planar heterojunction Organic Light Emitting Diode that embodiment 1 obtains (a), current efficiency-power efficiency-current density plot figure (b), external quantum efficiency-current density plot figure (c) and 1 milli Electroluminescent light spectrogram (d) under peace/square centimeter current density;

Fig. 3 is the Current density-voltage-brightness curve figure for the planar heterojunction Organic Light Emitting Diode that embodiment 2 obtains (a), current efficiency-external quantum efficiency-brightness curve figure (b) and the electroluminescent light under 1 milliamps per square centimeter of current density It composes (c).

Specific implementation mode

Present invention will now be described in further detail with reference to the embodiments and the accompanying drawings, but embodiments of the present invention are unlimited In this.

Embodiment 1

Take same lot number ITO Conducting Glass several, specification is 30 millimeters × 30 millimeters, and ITO thickness is about 90 nanometers, Square resistance is about 20 ohms/squares.Acetone, micron level semiconductor special purpose detergent, deionized water, isopropanol ultrasound are used successively Cleaning 15 minutes, to remove the dirt of substrate surface.It is for use to be subsequently placed into 80 degrees Celsius of drying in insulating box.ITO after drying Substrate is handled 4 minutes with plasma glow start equipment, further removes the organic pollution of surface attachment.Then ITO substrates It is transferred to anhydrous and oxygen-free, the glove box full of high pure nitrogen.In this glove box, device is fitted into Vacuum Deposition chamber.Unlatching machine Tool pumps and molecular pump, when plating intracavitary reaches 4 × 10-4High vacuum after start hot evaporation film.Using specific mask plate, successively P-type organic semiconducting materials TAPC, N-type organic semiconducting materials TmPyTZ, cathode cushioning layer material lithium fluoride, cathode material is deposited Expect metallic aluminium.The thickness of vapor deposition layer is monitored in real time by quartz crystal oscillator film thickness detector, controls p-type organic semiconducting materials respectively TAPC layers of thickness is 20nm, 30nm, 40nm, 50nm, 65nm, 75nm, 85nm and 95nm;Control N-type organic semiconducting materials TmPyTZ layers of thickness is 85nm.Obtain planar heterojunction Organic Light Emitting Diode:Ito glass substrate/TAPC (x)/TmPyTZ (85nm)/lithium fluoride/aluminium.

The light emitting diode for the different-thickness N-type organic semiconductor material that the present embodiment obtains carries out photoelectric properties survey Examination:

After the completion of prepared by device, device is taken out from vapor deposition cavity, using glass cover-plate, passes through epoxy resin Packaging plastic carries out simplified package in glove box.It then takes out in air and is tested, test equipment is that Konica-Minolta is public The CS200 luminance meters generated are taken charge of, device current information of voltage is measured by the 2400 source tables that Keithley company generates.By brightness, The information such as electric current, voltage can extrapolate current efficiency, the power efficiency of device respectively.Under the supposed premise of lambertian distribution, root According to brightness, the external quantum efficiency of current density, electroluminescent spectrum calculating device.The electroluminescent spectrum of device by The PR705 equipment that PhotoResearch companies generate is tested and is obtained.Test result is as shown in table 1.

1 embodiment of table, 1 light emitting diode light electric performance test result

The planar heterojunction Organic Light Emitting Diode that this implementation obtains:Ito glass substrate/TAPC (85nm)/TmPyTZ The Current density-voltage of (85nm)/lithium fluoride/aluminium-brightness curve figure, current efficiency-power efficiency-current density plot figure, Electroluminescent light spectrogram difference of the external quantum efficiency-current density plot figure and device under 1 milliamps per square centimeter of current density As shown in (a), (b), (c) and (d) in Fig. 2.

The plane PN heterojunction device simple in structure by the present embodiment it can be seen from the result of table 1 and Fig. 2 realizes highest 12.02% external quantum efficiency breaches limitation (the light extraction efficiency of maximum 5% external quantum efficiency of conventional fluorescent OLED device For 20%).Device has low-down driving voltage, opens bright voltage voltage more corresponding than the peak photon energies of emission spectrum also Want low.The device is the planar heterojunction OLED device of yellow light.

Embodiment 2

Preparation process is such as embodiment 1, and p-type organic semiconducting materials are selected as TCTA, N-type organic semiconducting materials are TmPyTZ.The thickness for controlling TmPyTZ layers of TCTA layers of p-type organic semiconducting materials and N-type organic semiconducting materials is 85nm, Obtain planar heterojunction Organic Light Emitting Diode:Ito glass substrate/TCTA (85nm)/TmPyTZ (85nm)/lithium fluoride/aluminium.

The ito glass substrate that the present embodiment obtains/TCTA (85nm)/TmPyTZ (85nm)/lithium fluoride/aluminium light emitting diode Current density-voltage-brightness curve figure, current efficiency-external quantum efficiency-brightness curve figure and device in 1 milliampere/square li Electroluminescent spectrum under rice current density is as respectively as (a), (b) and (c) in Fig. 3 is shown.The device is the plane of green light Hetero-junctions OLED device.

Embodiment 3

For preparation process such as embodiment 1, p-type organic semiconducting materials are selected as m-MTDATA, N-type organic semiconducting materials For TmPyTZ.M-MTDATA layer of p-type organic semiconducting materials of control and the thickness of TmPyTZ layers of N-type organic semiconducting materials are 85nm obtains planar heterojunction Organic Light Emitting Diode:Ito glass substrate/m-MTDATA (85nm)/TmPyTZ (85nm)/fluorine Change lithium/aluminium.

The ito glass substrate that the present embodiment obtains/m-MTDATA (85nm)/TmPyTZ (85nm)/lithium fluoride/aluminium luminous two Pole pipe carries out photoelectric properties test, and the results are shown in Table 2.The device is the device class of red plane PN heterojunction types OLED Type.

2 embodiment of table, 3 light emitting diode light electric performance test result

The above embodiment is a preferred embodiment of the present invention, but embodiments of the present invention are not by above-described embodiment Limitation, it is other it is any without departing from the spirit and principles of the present invention made by changes, modifications, substitutions, combinations, simplifications, Equivalent substitute mode is should be, is included within the scope of the present invention.

Claims (7)

1. a kind of planar heterojunction Organic Light Emitting Diode, it is characterised in that:Substrate, anode, p-type including stacking gradually are organic Semiconductor layer, n-type organic semiconductor layer and cathode;
The material for preparing of the p-type organic semiconductor layer is one or more of TAPC, TCTA and m-MTDATA It is blended:
The material for preparing of the n-type organic semiconductor layer is TmPyTZ:
The luminescent spectrum of the planar heterojunction Organic Light Emitting Diode is from p-type organic semiconductor layer and N-type is organic partly leads The PN hetero-junctions that body layer is constituted, spectral position are different from independent p-type organic semiconductor layer material or n-type organic semiconductor layer material The luminescent spectrum of material.
2. a kind of planar heterojunction Organic Light Emitting Diode according to claim 1, it is characterised in that:The p-type has Machine semiconductor layer and n-type organic semiconductor layer are single-layer or multi-layer.
3. a kind of planar heterojunction Organic Light Emitting Diode according to claim 1, it is characterised in that:The anode with One layer of buffer layer is individually or simultaneously added between p-type organic semiconductor layer, between cathode and n-type organic semiconductor layer.
4. a kind of planar heterojunction Organic Light Emitting Diode according to claim 1, it is characterised in that:The substrate is Glass, quartz, sapphire, polyimides, polyethylene terephthalate, mylar's fat, poly- naphthalenedicarboxylic acid second Diol ester, metal, alloy or stainless steel film.
5. a kind of planar heterojunction Organic Light Emitting Diode according to claim 1, it is characterised in that:The anode and Cathode is metal or metal oxide;The metal oxide refers to tin indium oxide, fluorine-doped tin dioxide, zinc oxide and indium The combination of one or more of gallium zinc oxide.
6. a kind of preparation method of planar heterojunction Organic Light Emitting Diode of Claims 1 to 5 any one of them, feature exist In including the following steps:
The substrate material with anode layer is taken, is then sequentially prepared that p-type organic semiconductor layer, N-type are organic partly to be led on the anode layer Body layer and cathode layer obtain planar heterojunction Organic Light Emitting Diode.
7. a kind of preparation method of planar heterojunction Organic Light Emitting Diode according to claim 6, it is characterised in that:Institute The method for stating preparation includes hot evaporation, spin coating, brushing, spraying, dip-coating, roller coating, printing or inkjet printing.
CN201510553459.9A 2015-09-01 2015-09-01 A kind of planar heterojunction Organic Light Emitting Diode and preparation method thereof CN105244447B (en)

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CN107026238A (en) * 2016-01-30 2017-08-08 兰州大学 Organic near-infrared upconversion device with planar heterojunction as photosensitive layer
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CN109244255A (en) * 2018-07-31 2019-01-18 华南理工大学 Organic planar heterojunction white light parts and its dimmer application suitable for pulsed drive

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