CN116322112A - Electron injection material, inverted organic electroluminescent device and display device - Google Patents
Electron injection material, inverted organic electroluminescent device and display device Download PDFInfo
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Abstract
The invention discloses an electron injection material, an inverted organic electroluminescent device and a display device. The injection material comprises the P-type material layer doped with the metal oxide, the bipolar material layer doped with the metal and the n-type material layer doped with the metal which are sequentially stacked, has very strong electron injection capability, can effectively reduce the driving voltage of the IBOLED, and improves the efficiency and the luminous intensity of the IBOLED.
Description
Technical Field
The invention relates to the technical field of display devices, in particular to the technical field of organic electroluminescent devices, and in particular relates to an electron injection material, an inverted organic electroluminescent device and a display device.
Background
The display industry is a basic stone of information industry, and is an important strategic and basic industry. The traditional backboard technology is difficult to realize real flexibility and large-area display, and has high production cost, complex preparation process and high energy consumption, and is difficult to meet the requirements of the development of the current display technology. Finding a low cost flexible backsheet technology that is efficient and can be manufactured in large areas is a strategic choice in many countries. In this context, organic light emitting diodes (Organic Light Emitting Diode, OLED), which are regarded as a new generation of display technology, have been developed, and are considered as the most flexible and bendable display implementation manner due to the all-solid-state thin film devices, and have become the leading edge and hot spot of research in the display field today and are also the strategic place of international high-new technology competition. The OLED not only has the advantages of active light emission, wide color gamut, wide viewing angle, high brightness, energy conservation and the like, but also has the unique properties of light weight, thinness, flexibility, high contrast and health to human eyes.
As a new generation of display technology, active Matrix OLED (AMOLED) has become one of the main developments of OLED displays, having many advantages such as active light emission, surface light source, fast response speed, high contrast ratio and flexibility. In AMOLED driving technology, mainstream oxide Thin Film Transistors (TFTs) and amorphous silicon (a-Si) TFTs are generally n-type semiconductor materials. In order to ensure stability of the OLED driving circuit, the device should be connected to the drain terminal of the n-type transistor, i.e., the cathode of the OLED is connected to the drain terminal of the n-type transistor, which requires the OLED to adopt an inverted structure with the cathode as the bottom electrode. However, the injection barrier for electrons is typically as high as 1.3 to 2.3eV, because ITO (indium tin oxide) having a work function of about 4.7eV is widely used as a transparent cathode in an inverted bottom-emitting OLED (IBOLED), and the Lowest Unoccupied Molecular Orbital (LUMO) of most electron transport materials is only 2.4 to 3.4eV. Thus, electron injection is very difficult, which severely limits the performance of IBOLED.
Fukagawa et al use high efficiency stable IBOLEDs to achieve long life flexible displays in which zinc oxide (ZnO) is interposed between ITO and various organic layers to reduce the drive voltage of the IBOLED, at 100 cd.m -2 A voltage of about 4V is generated and the maximum EQE (external quantum efficiency) is about 15.5%. Choi et al developed a bright, efficient and addressable optical fiber based on phosphorescent IBOLED, using ZnO nanoparticles as the material of the electron injection layer, at 1 cd.m -2 The maximum EQE is 16.04% with an on voltage of about 3.5V. Recently, xie and Lee et al reported air stable super bright IBOLEDs with metal ion chelating polymer injection layer at 1 cd.m -2 The starting voltage of 4.5V is realized, the maximum EQE is 16.5 percent, and the maximum PE is 25.8lm W -1 . Thus, it can be seen that the enhancement of electron injection is beneficial to improve the performance of the IBOLED. However, the further development of IBOLED is limited by several problems. First, the voltage of the most advanced IBOLEDs is too high, so far at 100 cd.m -2 Is rarely reported for voltages < 3V. Second, unsatisfactory electron injection in turn is detrimentalThe efficiency of the IBOLED, especially for power efficiency, is quantified. In fact, the power efficiency of the most advanced IBOLEDs is not yet sufficiently high.
Disclosure of Invention
The main object of the present invention is to provide an electron injection material, an inverted organic electroluminescent device and a display device, which can greatly enhance the electron injection capability of an IBOLED, reduce its driving voltage and improve its efficiency.
To achieve the above object, a first aspect of the present invention provides an electron injection material, comprising a p-type material layer, a bipolar material layer, and an n-type material layer, which are sequentially stacked, wherein the p-type material layer comprises a p-type host material and a metal oxide, the bipolar material layer comprises a bipolar host material and a first metal, and the n-type material layer comprises an n-type host material and a second metal.
Further, in the p-type material layer, the mass of the metal oxide is x% of the mass of the p-type main body material, and x is more than 0 and less than 10.
Further, in the n-type material layer, the mass of the second metal is z < 10 of the mass of the n-type main body material.
Further, the mass of the first metal of the bipolar material layer is y% of the mass of the bipolar material, and y is more than or equal to 1 and less than or equal to 90.
Further, the metal oxide includes MoO 3 、WO 3 、V 2 O 5 、Fe 2 O 3 、Na 2 O、Cu 2 O、CuO、Ag 2 O、Fe 3 O 4 、NiO、CrO 3 At least one of them.
Further, the first metal comprises at least one of Al, ag, au, pt, cu, mo, fe, co, zn.
Further, the second metal includes at least one of Li, na, K, rb, cs, be, mg, ca, sr, ba.
Further, at least one of the following conditions is satisfied:
(1) The p-type main material in the p-type material layer refers to a material with hole mobility being greater than electron mobility;
(2) The bipolar main material in the bipolar material layer refers to a single material with hole mobility equal to electron mobility, or a mixed material with hole mobility equal to electron mobility obtained by mixing p-type material and n-type material, wherein the p-type material refers to a material with hole mobility greater than electron mobility, and the n-type material refers to a material with hole mobility less than electron mobility;
(3) The n-type host material in the n-type material layer refers to a material having a hole mobility less than an electron mobility.
Further, the thickness of the p-type material layer is 0.1-100nm; the thickness of the bipolar material layer is 0.5-50nm; the thickness of the n-type material layer is 1-100nm.
The second aspect of the invention provides an inverted organic electroluminescent device or a display device, which comprises a substrate, a cathode, an electron injection layer, an electron transport layer, an organic light-emitting layer, a hole transport layer, a hole injection layer and an anode, wherein the substrate, the cathode, the electron injection layer, the electron transport layer, the hole injection layer and the anode are sequentially stacked from bottom to top, the electron injection layer is made of the electron injection material, and a p-type material layer, a bipolar material layer and an n-type material layer in the electron injection layer are sequentially stacked from bottom to top.
Compared with the prior art, the invention has the main beneficial effects that: under the combined action of the p-type material layer, the bipolar material layer and the n-type material layer which are sequentially stacked, the electron injection material has very strong electron injection capability, can effectively reduce the driving voltage of the IBOLED, and improves the efficiency (including power efficiency) and luminous intensity of the IBOLED.
Drawings
Fig. 1 is a schematic structural diagram of an inverted organic light emitting diode of embodiment 1;
fig. 2 is a schematic structural view of an inverted organic light emitting diode of comparative example 1.
Fig. 3 is a graph showing the comparison of the luminous intensities of the inverted organic light emitting diodes of example 1 and comparative example.
Detailed Description
For a better understanding of the objects, technical solutions and advantages of the present application, the present application will be further described with reference to specific examples and comparative examples, which are intended to be in detail, but are not to be construed as limiting the present application. All other embodiments, which can be made by those skilled in the art without the inventive effort, are intended to be within the scope of the present application. The experimental reagents and apparatus according to the present application are common reagents and apparatus unless otherwise specified.
According to a first aspect of the present invention, there is provided an electron injection material comprising a p-type material layer, a bipolar material layer and an n-type material layer, which are sequentially stacked, wherein the p-type material layer comprises a p-type host material and a metal oxide, the bipolar material layer comprises a bipolar host material and a first metal, and the n-type material layer comprises an n-type host material and a second metal.
Under the combined action of the p-type material layer, the bipolar material layer and the n-type material layer in a specific lamination sequence, the electron injection material has very strong electron injection capability, can effectively improve the luminous intensity of the IBOLED, reduce the driving voltage and improve the efficiency (including power efficiency) of the IBOLED.
In some embodiments, the mass of the metal oxide in the p-type material layer is x% of the mass of the p-type host material, 0 < x < 10. When x is more than 10, exciton quenching is easy to occur, and the device performance is reduced. Therefore, 0 < x < 10 is preferable, and 1.ltoreq.x < 10 is more preferable.
In some embodiments, the mass of the second metal in the n-type material layer is z < 10 of the mass of the n-type host material. When z is 10 or more, exciton quenching is liable to occur, degrading device performance. Therefore, z < 10 is preferable, and 1.ltoreq.z < 10 is more preferable.
In some embodiments, the mass of the first metal in the bipolar material layer is y% of the mass of the bipolar material, 1.ltoreq.y.ltoreq.90. Alternatively, y is 5, or 15, or 25, or 35, or 45, or 55, or 65, or 75, or 85, or a range of any two values.
In some embodiments, the metal oxide comprises MoO 3 、WO 3 、V 2 O 5 、Fe 2 O 3 、Na 2 At least one of O. But the choice of the metal oxide species is not limited thereto.
In some embodiments, the first metal comprises at least one of Al, ag, au, pt, cu, mo, fe, co, zn, etc. But the choice of the first metal species is not limited thereto.
In some embodiments, the second metal comprises at least one of Li, na, K, rb, cs, be, mg, ca, sr, ba, etc. But the choice of the second metal species is not limited thereto.
The p-type host material in the p-type material layer refers to a material having a hole mobility greater than an electron mobility. In some embodiments, the p-type host material in the p-type material layer includes at least one of F4-TCNQ (2, 3,5, 6-tetrafluoro-7, 8-tetracyanoquinoline dimethylmethane, CAS No. 29261-33-4), HAT-CN (CAS No. 105598-27-4), NPB (CAS No. 2247491-97-8), TAPC (CAS No. 1174006-36-0), TCTA (CAS No. 139092-78-7), PVK (CAS No. 25067-59-8), and the like. But the selection of the kind thereof is not limited thereto.
The bipolar host material in the bipolar material layer refers to a single material with hole mobility equal to electron mobility, or a mixed material with hole mobility equal to electron mobility obtained by mixing a p-type material and an n-type material, wherein the p-type material refers to a material with hole mobility greater than electron mobility, and the n-type material refers to a material with hole mobility less than electron mobility. As one example, a single material with hole mobility equal to electron mobility includes CBP (CAS No. 1662-01-7); the p-type material comprises at least one of F4-TCNQ and HAT-CN, NPB, TAPC, TCTA, PVK, and the n-type material comprises at least one of Bphen (4, 7-diphenyl-1, 10-phenanthroline, CAS No. 1662-01-7), TPBi (CAS No. 192198-85-9) and TmPyPB (CAS No. 921205-03-0). However, the choice of the type of bipolar host material is not limited thereto.
The n-type host material in the n-type material layer refers to a material having a hole mobility less than an electron mobility. In some embodiments, the n-type host material in the n-type material layer includes at least one of 4, 7-diphenyl-1, 10-phenanthroline, TPBi, tmpyreb. But the selection of the kind thereof is not limited thereto.
In some embodiments, the p-type material layer has a thickness of 0.1-100nm, the bipolar material layer has a thickness of 0.5-50nm, and the n-type material layer has a thickness of 0.5-50nm.
In one embodiment, the layers of the electron injecting material are formed by vacuum evaporation, spin coating, blade coating, ink jet printing, and the like, but are not limited thereto.
According to a second aspect of the present invention, there is provided an inverted organic electroluminescent device or display device, comprising a substrate, a cathode, an electron injection layer, an electron transport layer, an organic light emitting layer, a hole transport layer, a hole injection layer and an anode, which are sequentially stacked from bottom to top, wherein the electron injection layer is made of the above electron injection material, and a p-type material layer, a bipolar material layer and an n-type material layer in the electron injection layer are sequentially stacked from bottom to top.
In some embodiments, the cathode has a thickness of 10-300nm; the thickness of the electron injection layer is 10-100nm; the thickness of the electron transport layer is 10-100nm; the thickness of the organic light-emitting layer is 0.1-80nm; the thickness of the hole transport layer is 10-100nm; the thickness of the hole injection layer is 0.5-50nm; the thickness of the anode is 10-300nm.
The formation modes of the cathode, the electron injection layer, the electron transport layer, the organic light emitting layer, the hole transport layer, the hole injection layer and the anode are not particularly limited, and may be any common formation mode in the art. In some embodiments, the layers of the electron injection layer are formed by vacuum evaporation, spin coating, blade coating, ink jet printing, and the like, but are not limited thereto.
The types of the display device are not particularly limited, and examples thereof include an inverted organic electroluminescent green light device, an inverted organic electroluminescent red light device, an inverted organic electroluminescent blue light device, and an inverted organic electroluminescent white light device.
The invention will be further illustrated with reference to specific examples.
Example 1
The embodiment provides an inverted organic light emitting diode. Referring to fig. 1, it includes a substrate 10, a cathode 20, an electron injection layer 30, an electron transport layer 40, an organic light emitting layer 50, a hole transport layer 60, a hole injection layer 70, and an anode 80, which are sequentially stacked from bottom to top,
the electron injection layer 30 includes a p-type material layer 301, a bipolar material layer 302, and an n-type material layer 303, which are stacked in this order from bottom to top;
the p-type material layer 301 includes F4-TCNQ and MoO 3 ，MoO 3 The mass is 3% of the mass of F4-TCNQ;
the n-type material layer 303 includes Bphen and Li, the Li mass being 5% of the Bphen mass;
the organic light emitting layer includes an organic light emitting layer 501 and an organic light emitting layer 502 which are sequentially stacked from bottom to top.
The preparation method of the inverted organic light-emitting diode comprises the following steps:
a glass substrate is selected as a substrate 10, a cathode 20 with the thickness of 50nm is prepared on the upper surface of the substrate 10, and the cathode 20 is made of ITO;
using F4-TCNQ and MoO 3 Is a mixture of (MoO) 3 3% of the mass of F4-TCNQ) on the upper surface of the cathode 20 to form a p-type material layer 301 with a thickness of 10nm by vacuum evaporation;
a bipolar material layer 302 with the thickness of 5nm is formed on the upper surface of the p-type material layer 301 by adopting a mixture of CBP and Al (the mass of Al is 10% of that of CBP) through vacuum evaporation;
an n-type material layer 303 with the thickness of 20nm is formed on the upper surface of the bipolar material layer 302 by vacuum evaporation by adopting a mixture of Bphen and Li (the mass of Li is 5% of that of Bphen);
forming an electron transport layer 40 with the thickness of 25nm on the upper surface of the n-type material layer 303 by adopting TpPyPB through vacuum evaporation;
ir with CBP and (ppy) 3 Mixture (Ir (ppy) 3 15% of CBP mass) on the upper surface of the electron transport layer 40, an organic light emitting layer 501 having a thickness of 50nm was formed by vacuum evaporation;
by usingTCTA and Ir (ppy) 3 mixture (Ir (ppy) 3 10% of TCTA by mass) and evaporating an organic light-emitting layer 502 with a thickness of 50nm on the upper surface of the organic light-emitting layer 501, wherein the thickness is 50nm;
evaporating and forming a hole transport layer 6 with the thickness of 50nm on the upper surface of the organic light-emitting layer 502 by adopting TAPC;
the hole injection layer 70 having a thickness of 10nm was formed on the upper surface of the hole transport layer 60 by vapor deposition using HAT-CN.
An anode 80 having a thickness of 100nm was formed on the upper surface of the hole injection layer 70 by evaporation using Al.
Example 2
The embodiment provides an inverted organic light emitting diode. The only difference from example 1 is that: the mass of Al in bipolar material layer 302 is 1% of the mass of CBP;
the thickness of the cathode 20 is 10nm;
the thickness of the p-type material layer 301 is 0.1nm;
the bipolar material layer 302 has a thickness of 0.5nm;
the n-type material layer 303 has a thickness of 1nm;
the electron transport layer 40 has a thickness of 10nm;
the thickness of the organic light emitting layer 501 is 0.05nm;
the thickness of the organic light emitting layer 502 is 0.05nm;
the hole transport layer 600 has a thickness of 10nm;
the hole injection layer 700 has a thickness of 0.5nm;
the anode 800 has a thickness of 10nm.
Example 3
The embodiment provides an inverted organic light emitting diode. The only difference from example 1 is that: the mass of Al in bipolar material layer 302 is 90% of the mass of CBP;
the cathode 20 has a thickness of 300nm;
the thickness of the p-type material layer 301 is 100nm;
the bipolar material layer 302 has a thickness of 50nm;
the n-type material layer 303 has a thickness of 100nm;
the electron transport layer 40 has a thickness of 100nm;
the thickness of the organic light emitting layer 501 is 40nm;
the thickness of the organic light-emitting layer 502 is 40nm;
the hole transport layer 600 has a thickness of 100nm;
the hole injection layer 700 has a thickness of 50nm;
anode 800 has a thickness of 300nm.
Example 4
The embodiment provides an inverted organic light emitting diode. The only difference from example 1 is that: moO in the p-type material layer 301 3 The mass of the mixture is 0.5% of that of F4-TCNQ.
Example 5
The embodiment provides an inverted organic light emitting diode. The only difference from example 1 is that: moO in the p-type material layer 301 3 The mass is 9% of the mass of F4-TCNQ.
Example 6
The embodiment provides an inverted organic light emitting diode. The only difference from example 1 is that: the mass of Li in the n-type material layer 303 was 0.5% of the mass of Bphen.
Example 7
The embodiment provides an inverted organic light emitting diode. The only difference from example 1 is that: the mass of Li in the n-type material layer 303 was 9% of the mass of Bphen.
Comparative example 1
The present comparative example provides an inverted organic light emitting diode. Referring to fig. 2, the difference from example 1 is that the electron injection layer 30 has a single-layer structure, and is formed by vacuum evaporation of a mixture of Bphen and Li (the mass of Li is 5% of the mass of Bphen) on the upper surface of the cathode 20, and the thickness is 20nm.
Comparative example 2
The present comparative example provides an inverted organic light emitting diode. The difference from example 1 is that the electron injection layer 30 has a single-layer structure, and is formed by vacuum evaporation of LiF on the upper surface of the cathode 20, and the thickness is 1nm.
Comparative example 3
The present comparative example provides an inverted organic light emitting diode. The only difference from example 1 is that: the n-type material layer 303 is replaced with equal mass of lithium chloride.
The light emission intensity, driving voltage and power efficiency of the inverted organic light emitting diodes of each example and comparative example were measured as follows: the current density-voltage-luminance curve, spectrum and efficiency measurements of the organic light emitting diode were collected by an integrating sphere.
The test results are shown in Table 1 and FIG. 3.
TABLE 1
As can be seen from table 1, each example has higher maximum light emission luminance and maximum power efficiency, and lower driving on voltage due to the use of a specific electron injection material, compared to comparative example 1, comparative example 2, and comparative example 3.
The present invention has been described with respect to one or more embodiments. It will be apparent to those skilled in the art that various changes and modifications can be made without departing from the scope of the invention as defined in the following claims.
Although the invention has been described above with reference to some embodiments, various modifications may be made and equivalents may be substituted for elements thereof without departing from the scope of the invention. In particular, the features of the various embodiments disclosed herein may be combined with each other in any manner so long as there is no structural conflict, and the combination is not described in the present specification in an exhaustive manner for the sake of brevity and resource saving. Therefore, it is intended that the invention not be limited to the particular embodiment disclosed, but that the invention will include all embodiments falling within the scope of the appended claims.
Claims (10)
1. The electron injection material is characterized by comprising a p-type material layer, a bipolar material layer and an n-type material layer which are sequentially stacked, wherein the p-type material layer comprises a p-type main body material and a metal oxide, the bipolar material layer comprises a bipolar main body material and a first metal, and the n-type material layer comprises an n-type main body material and a second metal.
2. The electron injecting material according to claim 1, wherein the mass of the metal oxide in the p-type material layer is x% of the mass of the p-type host material, 0 < x < 10.
3. The electron injecting material according to claim 1, wherein in the n-type material layer, the mass of the second metal is z% of the mass of the n-type host material, and 0 < z < 10.
4. The electron injecting material according to claim 1, wherein the mass of the first metal in the bipolar material layer is y% of the mass of the bipolar material, and y is 1.ltoreq.y.ltoreq.90.
5. The electron injecting material according to claim 1, wherein the metal oxide comprises MoO 3 、WO 3 、V 2 O 5 、Fe 2 O 3 、Na 2 O、Cu 2 O、CuO、Ag 2 O、Fe 3 O 4 、NiO、CrO 3 At least one of them.
6. The electron injecting material according to claim 1, wherein the first metal comprises at least one of Al, ag, au, pt, cu, mo, fe, co, zn.
7. The electron injecting material according to claim 1, wherein the second metal comprises at least one of Li, na, K, rb, cs, be, mg, ca, sr, ba.
8. The electron injecting material as defined in claim 1, wherein at least one of the following conditions is satisfied:
(1) The p-type main material in the p-type material layer refers to a material with hole mobility being greater than electron mobility;
(2) The bipolar main material in the bipolar material layer refers to a single material with hole mobility equal to electron mobility, or a mixed material with hole mobility equal to electron mobility obtained by mixing p-type material and n-type material, wherein the p-type material refers to a material with hole mobility greater than electron mobility, and the n-type material refers to a material with hole mobility less than electron mobility;
(3) The n-type host material in the n-type material layer refers to a material with hole mobility less than electron mobility.
9. The electron injection material of claim 1, wherein the p-type material layer has a thickness of 0.1 to 100nm; the thickness of the bipolar material layer is 0.5-50nm; the thickness of the n-type material layer is 1-100nm.
10. An inverted organic electroluminescent device or display device, comprising a substrate, a cathode, an electron injection layer, an electron transport layer, an organic light emitting layer, a hole transport layer, a hole injection layer and an anode which are sequentially stacked from bottom to top, wherein the electron injection layer is made of an electron injection material according to any one of claims 1 to 9, and a p-type material layer, a bipolar material layer and an n-type material layer in the electron injection layer are sequentially stacked from bottom to top.
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