CN111092159A - Organic semiconductor device and connection structure thereof - Google Patents
Organic semiconductor device and connection structure thereof Download PDFInfo
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Abstract
The application discloses organic semiconductor device and connection structure thereof, connection structure is including the n type electron transport material layer and the p type hole transport material layer that the stack set up, be equipped with interface modification layer between n type electron transport material layer and the p type hole transport material layer for combine cumulative charge in the connection structure. The interface modification layer effectively reduces the high cross voltage of the organic semiconductor device at the connecting structure, and improves the anti-irradiation capability and the service life of the OLED device.
Description
Technical Field
The present disclosure relates generally to the field of organic optoelectronic technologies, and more particularly to organic semiconductor devices and connection structures therefor.
Background
Organic light-emitting diodes (OLEDs) and organic photovoltaic devices (OPVs) are the main application directions of organic semiconductors, wherein OLEDs are electroluminescent devices and are mainly applied in the fields of display and illumination; the OPV is a way to convert an external light source into electric energy, and is a green energy source with great potential. With the development of many years, the materials required for the OLED and OPV manufacturing process are not limited to pure organic semiconductor materials, and organic materials, inorganic materials, and organic-inorganic composite materials can effectively improve the device performance and the service life.
One type of device in the OLED and the OPV is called a tandem structure (also called a "tandem structure"), and the purpose of the OLED is to increase the luminance per unit area or reduce the operating current, so as to effectively increase the operating luminous intensity and the lifetime of the device; the OPV uses more than two luminescent layers connected in series, so that the photoelectric conversion ratio can be effectively increased or the conversion efficiency of different wave bands can be increased. In terms of charge conduction characteristics, a metal conductive material is most suitable for a connection structure in a stacked device, but since optical properties need to be considered at the same time, a transparent connection structure is an important research subject.
The connection structure in the OLED is collectively called a Charge Generation Layer (CGL), and the connection structure in the OPV is collectively called connection units (connecting units); the electric charge generating layer and the connecting layer have the same composition structure and basically the same requirements on electric charge transmission characteristics, and need to have high-efficiency electric charge transmission capability including the transmission capability of electrons and holes; the CGL in a stacked OLED allows electrons and holes to be provided to the light emitting active layers connected up and down, respectively (the connecting structure can provide electrons and holes to different structures with different requirements, so the stacked OLED is called a charge generation layer); in a stacked OPV, the light absorbing active layers generate a separation of electrons and holes, and the connecting structure is connected between two different light absorbing active layers and is to receive the electrons and holes respectively to combine in the connecting structure. The connection structure of both types (OLED and OPV) maintains the charge balance in the device, so that the device can be maintained in a normal and efficient operation state.
The charge generation layer and the connecting layer are developed into at least two structural combinations, and basically, the charge generation layer and the connecting layer are combined by a layer of electron transport material (n-type material) and a layer of hole transport material (p-type material); the n-type material is usually an electron transport type material and is matched with specific doping to further improve the electron mobility, and the p-type material is usually a hole transport type material and is matched with specific doping to further improve the hole mobility; the above materialsMaterials are not limited to all organic or all inorganic materials, and existing charge generation layers or tie layers such as: alq3:Mg/WO3、Bphen:Li/MoO3、BCP:Li/V2O5、Alq3:Li/HAT-CN、CuPc/F16-CuPc、Alq3:Li./NPB:F4-TCNQ、Alq3:Li./NPB:FeCl3、Bphen:Li/m-TDATA:F4-TCNQ、Alq3:Li./NPB:MoO3、A/WO3/Ag、C60A plurality of combinations of Al/Au, etc. However, it is indicated by calculation and analysis that a certain voltage is applied to the charge generation layer and the connection layer, i.e. the charge generation layer and the connection layer must consume a certain voltage although the stacked device can operate normally.
Disclosure of Invention
In view of the above-mentioned drawbacks or deficiencies in the prior art, it is desirable to provide an organic semiconductor device and a connection structure thereof.
In a first aspect, the present application provides an organic semiconductor device connection structure, where the connection structure includes an n-type electron transport material layer and a p-type hole transport material layer that are stacked, and an interface modification layer is disposed between the n-type electron transport material layer and the p-type hole transport material layer, and is used for combining with accumulated charges in the connection structure.
According to the technical scheme provided by the embodiment of the application, the interface modification layer is made of an organic-inorganic hybrid perovskite material with an energy gap larger than 2.3 electron volts.
According to the technical scheme provided by the embodiment of the application, the structural general formula of the organic-inorganic hybrid perovskite material is AmBnXkWherein A is organic amine group, B is fourth main group metal ion or transition metal ion, X is one or more halogen element combination, and m, n and k are integers more than or equal to 1.
According to the technical scheme provided by the embodiment of the application, the organic-inorganic hybrid perovskite material is CH3NH3PbCl3、(C10H21NH3)2PbI4、((CH3)2NH2)3BiI6、CH3NH3SnI3At least one of (1).
According to the technical scheme provided by the embodiment of the application, the thickness range of the interface modification layer is 0.1nm-200 nm.
According to the technical scheme provided by the embodiment of the application, the thickness of the interface modification layer ranges from 0.5nm to 20 nm.
According to the technical scheme provided by the embodiment of the application, the optical transmittance of the interface modification layer is more than 70%.
In a second aspect, the present application provides an organic semiconductor device comprising any one of the above-described connection structures.
According to the technical scheme, an interface modification layer is arranged between an n-type electron transport material layer and a p-type hole transport material layer of a connection structure of an organic semiconductor device; for combining with accumulated charge within the connection structure; when the OLED device works normally, a large amount of surplus electrons are generated at the connecting structure to form accumulated charges, so that high voltage is formed at the connecting structure, the driving voltage of the device is continuously increased due to the continuous accumulation of the charges, and the service life of the device is influenced.
According to the technical scheme provided by the embodiment of the application, the interface modification layer is made of an organic-inorganic hybrid perovskite material with an energy gap larger than 2.3 electron volts, so that light rays larger than 2.3 electron volts can be absorbed, the intensity of the light rays larger than 2.3 electron volts in the device is reduced, and the radiation resistance of the screen body is improved. Therefore, the material can solve the problem of charge accumulation of the organic semiconductor device, effectively reduce the high voltage-spanning phenomenon of the organic semiconductor device at the charge connection structure by absorbing the accumulated charges, avoid the rise of the driving voltage of the device, have the capability of absorbing ultraviolet rays, and further improve the ultraviolet resistance and the service life of the OLED device. ,
in the prior art, there is a technical scheme of applying an organic-inorganic hybrid perovskite material to a connection structure of an OLED screen, but at this time, the organic-inorganic hybrid perovskite material is directly used as a material of an n-type electron transport material layer and a p-type hole transport material layer, or is doped in the n-type electron transport material layer and the p-type hole transport material layer, and is used for improving the carrier transport capability or improving the brightness of visible light; the absorption range of the organic-inorganic hybrid perovskite with the energy gap of more than 2.3eV leaves a visible light region, and the organic-inorganic hybrid perovskite does not have the capability of emitting light in a visible light range; the energy gap is too narrow, so that the charge separation capability of the device is too poor, and a charge trap is easily formed, so that the energy gap is applied to the light-emitting device and does not have the capability of improving the drivable current; it is therefore not within the general knowledge of the person skilled in the art to select perovskite materials with a band gap above 2.3eV for use as the material of the charge connection structure.
In the application, the characteristics that the energy gap of the organic-inorganic hybrid perovskite with the energy gap of more than 2.3eV is narrow and a charge trap is easily formed are just utilized to combine the charges accumulated at the connecting structure, so that the problem of high cross pressure at the connecting structure is solved on the premise that the transmission capability of current carriers at the connecting structure is sacrificed, the radiation resistance is improved, the overall performance of the OLED screen body is effectively improved, and particularly the service life of an OLED device is effectively prolonged.
Drawings
Other features, objects and advantages of the present application will become more apparent upon reading of the following detailed description of non-limiting embodiments thereof, made with reference to the accompanying drawings in which:
FIG. 1 is a schematic structural diagram of example 1 of the present application;
FIG. 2 is a schematic structural diagram of embodiment 2 of the present application;
FIG. 3 is a schematic voltage cross-over diagram of a prior art OLED device at a charge generation layer;
FIG. 4 is a schematic voltage-spanning diagram of an OPV device at a charge generation layer in the prior art;
FIG. 5 is a schematic diagram of the voltage across the charge generation layer of the OLED device in example 2 of the present application;
fig. 6 is a schematic voltage-cross diagram of an OPV device at a charge generation layer in example 2 of the present application;
reference numbers in the figures:
61. a layer of n-type electron transporting material; 62. an interface modification layer; 63. a p-type hole transport material layer; 10. a substrate; 20. a first electrode; 31. a first hole transport functional layer; 41. a first light-emitting layer; 51. a first electron transport functional layer; 60. a connecting structure; 32. a second hole transport functional layer; 42. a second light emitting layer; 52. a second electron transport functional layer; 70. a second electrode; 80. electrons; 90. a cavity.
Detailed Description
The present application will be described in further detail with reference to the following drawings and examples. It is to be understood that the specific embodiments described herein are merely illustrative of the relevant invention and not restrictive of the invention. It should be noted that, for convenience of description, only the portions related to the present invention are shown in the drawings.
It should be noted that the embodiments and features of the embodiments in the present application may be combined with each other without conflict. The present application will be described in detail below with reference to the embodiments with reference to the attached drawings.
Example 1
Referring to fig. 1, a schematic structural diagram of a connection structure 60 of an organic semiconductor device according to the present application is provided, in which the connection structure 60 is a charge generation layer applied in an OLED device; the charge generation layer comprises an n-type electron transport material layer 61 and a p-type hole transport material layer 63 which are stacked, and an interface modification layer 62 is arranged between the n-type electron transport material layer 61 and the p-type hole transport material layer 63.
The interface modifying layer 62 is made of organic-inorganic hybrid perovskite material with energy gap larger than 2.3 electron volts, and the structural general formula of the organic-inorganic hybrid perovskite material is AmBnXkWherein A is an organic amine group, B is a fourth main group metal ion or a transition metal ion, and X is one or more halogen element combinations; m, n and k are integers of 1 or more.
For example, the materials of the layers of the connecting structure are respectively:
Alq3mg (10 nm)/interface modification layer/NPB F4-TCNQ (25 nm); wherein the n-type electron transport material layer 61 is composed of magnesium (Mg) -doped 8-hydroxyquinoline and aluminum (Alq)3) The thickness of the film is 10 nm; the p-type hole transport material layer 63 is formed by doping with tetracyanoquinodimethane (F)4-TCNQ) hole transport material.
The specific implementation of the interface modification layer can optionally adopt the following ways, and the specific material, thickness and visible light transmittance of the interface modification layer are shown in table 1 below corresponding to various implementations of the interface modification layer:
TABLE 1
In embodiment 1-1, interface modification layer 62 is made of perovskite material (CH)3NH3PbCl3) The thickness is 0.5nm, and the visible light transmittance is 88%; whereas in embodiment mode 1-2 the interface modification layer 62 is made of a perovskite material (CH)3NH3PbCl3) The thickness is 3nm, and the visible light transmittance is 85%; in embodiments 1 to 3, the interface modification layer 62 is also made of a perovskite material (CH)3NH3PbCl3) The thickness is 20nm, and the visible light transmittance is 75%; finally, in embodiments 1 to 4, interface modification layer 62 is made of a perovskite material (((CH)3)2NH2)3BiI6) The film had a thickness of 3nm and a visible light transmittance of 84%.
In various embodiments of the interface modifying layer described above, the perovskite material (CH)3NH3PbCl3) Has an energy gap of 2.4 electron volts, a perovskite material (((CH)3)2NH2)3BiI6) The energy gap of the interface modification layer is 2.6 eV, so that the interface modification layer can effectively absorb light with an absorption rate higher than 2.3The high-energy light of electron volt effectively absorbs accumulated charges when the OLED screen body works, so that the phenomenon that the OLED screen body has overhigh driving voltage is avoided, and the service life of the OLED screen body is effectively prolonged.
In other embodiments, the perovskite material may also be CH3NH3SnI3、(C10H21NH3)2PbI4Other perovskite materials with energy gaps larger than 2.3 ev.
Example 2
As shown in fig. 2, the present embodiment provides an organic semiconductor device, and the organic semiconductor device in the present embodiment includes any one of the connection structures described above. For example, the organic semiconductor device includes a substrate 10, a first electrode 20, a first hole transport functional layer 31, a first light emitting layer 41, a first electron transport functional layer 51, a connection structure 60, a second hole transport functional layer 32, a second light emitting layer 42, a second electron transport functional layer 52, and a second electrode 70 in this order. The connecting structure 60 includes an n-type electron transporting material layer 61, an interface modification layer 62, and a p-type hole transporting material layer 63.
As shown in fig. 3, which is a schematic view of carrier movement of each layer in an OLED device in the prior art, electrons 80 and holes 90 in the OLED are separated at a connecting structure (charge generation layer CGL), and when the quantity of the electrons and holes at the CGL is unequal as the device ages, one carrier is excessively accumulated at the CGL, and the accumulation inhibits the separation of the electrons and holes, so that a higher voltage is required at the CGL to further separate the electrons and holes, and thus the voltage across the device is larger, for example, as indicated by H1;
as shown in fig. 4, which is a schematic view of carrier movement of each layer in the OPV device in the prior art, when the electrons 80 and the holes 90 in the OPV are combined at the connection structure (connection layer), and as the device ages, the number of the electrons and the holes at the connection layer is unequal, one carrier is excessively accumulated at the connection layer, and during accumulation, an accumulation of electrons 80 is generally formed, and when the accumulation of electrons is excessive, the voltage across the device is also increased, for example, as indicated by H2;
the principle isIn an embodiment, as shown in FIG. 5, a charge generation layer of perovskite material (CH) is disposed in an OLED device3NH3PbCl3) After the interface modification layer is manufactured, redundant electrons can be combined in the perovskite material so as to reduce the cross voltage, for example, the required cross voltage drop is H3 and is obviously smaller than H1;
in the present embodiment, as shown in fig. 6, a perovskite material (CH) is provided in the connection layer of the OPV device3NH3PbCl3) After the interface modification layer is manufactured, redundant electrons can be combined in the perovskite material so as to reduce the cross voltage, for example, the required cross voltage drop is H4 and is obviously smaller than H2;
as can be seen from the comparative example, in the connection structure provided in the present embodiment, the interface modification layer formed by the perovskite material is provided, so that the cross-voltage of the stacked organic semiconductor device at the connection structure is effectively reduced.
In this embodiment, the device structure of the organic semiconductor device is formed by sequentially forming NPB (40nm)/CPB Ir (ppy) on the ITO conductive glass3(30nm)/Bphen/CGL2/NPB(40nm)/CPB:Ir(ppy)3(30nm)/Bphen/LiF/Al。
Wherein NPB is a hole transport layer; CPB Ir (ppy)3The material is a luminescent layer doped with green phosphorescent dye, Bphen is an electron transport layer, and LiF is an electron injection functional layer; the CGL2 is a charge generation layer, i.e. a connection structure, the charge generation layer CGL2 optionally takes the following embodiments, comprising the following structural layers in order: embodiments 2-1 to 2-4 of the following CGL2 correspond to embodiments 1-1 to 1-4 of the interface modification layer in example 1, respectively;
TABLE 2
Corresponding to the 4 embodiments of the CGL2 layer described above, the organic semiconductor device provided in this example had the following comparison of the photoelectric performance results at the same luminance:
TABLE 3
As can be seen from Table 3, CGL2 in embodiment 2-2, i.e., the interface modification layer, was made of 3nm thick perovskite material (CH)3NH3PbCl3) The photoelectric performance is optimal under the same brightness.
For comparative illustration, the present example also provides the following comparative examples to illustrate: the following OLED device structures provided by the comparative examples were sequentially formed on ITO conductive glass: NPB (40nm)/CPB Ir (ppy)3(30nm)/Bphen/CGL1/NPB(40nm)/CPB:Ir(ppy)3(30nm)/Bphen/LiF/Al。
Wherein CGL1 is a charge generation layer, i.e., a connecting structure, CGL1 comprises the following layered structure in each of the following comparative examples: as shown in table 4:
comparative example 1 described above is a conventional connection structure in the prior art, i.e., CGL1 has only an n-type electron transport material layer [ Alq ]3Mg (10nm) and a p-type hole transport material layer [ NPB: F4-TCNQ (25nm) ];
comparative example 2 in n-type electron transport material layer [ Alq ]3An interface modification layer (NH) is arranged between Mg (10nm) and the p-type hole transport material layer (NPB: F4-TCNQ (25 nm))2CH＝NH2PbI3) (3nm) wherein the interface modifying layer [ NH ]2CH＝NH2PbI3) (3nm) the energy gap is less than 2.3 ev;
comparative example 3 n-type electron transport material layer [ Alq ] in comparative example 13Mg (10nm) ] in Alq3Replacing with organic-inorganic perovskite material [ NH ] with energy gap less than 2.3ev2CH＝NH2PbI3】；
Comparative example 4 the p-type hole transport material layer [ NPB: F4-TCNQ (25nm) ] of comparative example 1 was replaced with an organic-inorganic perovskite material [ NH ] having an energy gap of less than 2.3eV2CH＝NH2PbI3】；
Comparative example 5n in comparative example 1Type electron transport material layer [ Alq3Mg (10nm) ] in Alq3Replaced by an organic-inorganic perovskite material [ CH ] with an energy gap larger than 2.3ev3NH3PbCl3】；
Comparative example 6 the p-type hole transport material layer [ NPB: F4-TCNQ (25nm) ] of comparative example 1 was replaced with an organic-inorganic perovskite material [ CH ] having an energy gap of more than 2.3eV3NH3PbCl3】；
TABLE 4
The photovoltaic performance results of the devices at the same luminance are shown in table 5 below:
| comparative example | Voltage (V) | Efficiency (cd/A) | Life LT90(h) |
| 1 | 10.3 | 91 | 1000 |
| 2 | 10.8 | 86 | 800 |
| 3 | 9.6 | 94 | 1200 |
| 4 | 11.7 | 75 | 600 |
| 5 | 11.9 | 60 | 400 |
| 6 | 13.2 | 24 | 200 |
TABLE 5
Perovskite materials (NH) provided in comparative examples 2, 3 and 42CH＝NH2PbI3) The energy gap of the perovskite material is 1.48 electron volts, the performance of doping the perovskite material with high mobility in the n-type electron transport material layer and the p-type hole transport material layer and serving as an interface modification layer is verified in comparative examples 3 and 4, and the influence of doping the perovskite material with the electron voltage of more than 2.3 on the performance of the device is verified in comparative examples 5 and 6.
According to tables 3 and 5, the OLED device of the present example and the OLED device of the comparative example were compared, and the current efficiency using comparative example 1 at the same luminance was 91cd/a, the corresponding voltage was 10.3V, and the time for which the lifetime decayed to 90% of the initial value under irradiation of sunlight was 1000 h; comparative example 2 has a current efficiency of 86cd/A, corresponding to a voltage of 10.8V, and a time for the lifetime to decay to 90% of the initial value of 800 h; comparative example 3, which has the best performance, has a current efficiency of 94cd/A, a corresponding voltage of 9.6V, and a lifetime decay time of 1200h to 90% of the initial value; in the embodiment 2, the current efficiency of the device in the embodiment 2-2 adopting the CGL2 is 98cd/a, the corresponding voltage is 7.9V, and the time for the lifetime to decay to 90% of the initial value is 2000 h; therefore, the OLED device of this embodiment 2 effectively improves the voltage-crossing phenomenon caused by the charge generation layer by using the connection structure in embodiment 1, and simultaneously protects the organic material from being damaged due to the improvement of the radiation resistance, thereby prolonging the service life of the device.
The above description is only a preferred embodiment of the application and is illustrative of the principles of the technology employed. It will be appreciated by a person skilled in the art that the scope of the invention as referred to in the present application is not limited to the embodiments with a specific combination of the above-mentioned features, but also covers other embodiments with any combination of the above-mentioned features or their equivalents without departing from the inventive concept. For example, the above features may be replaced with (but not limited to) features having similar functions disclosed in the present application.
Claims (8)
1. The organic semiconductor device connecting structure comprises an n-type electron transport material layer and a p-type hole transport material layer which are arranged in a stacked mode, and is characterized in that an interface modification layer is arranged between the n-type electron transport material layer and the p-type hole transport material layer and used for being combined with accumulated charges in the connecting structure.
2. The organic semiconductor device connection structure according to claim 1, wherein the interface modification layer is made of an organic-inorganic hybrid perovskite material having an energy gap greater than 2.3 ev.
3. The organic semiconductor device connection structure according to claim 2, wherein the organic-inorganic hybrid perovskite material has a general structural formula of AmBnXkWherein A is organic amine group, B is fourth main group metal ion or transition metal ion, X is one or more halogen element combination, and m, n and k are integers more than or equal to 1.
4. The method of claim 1Characterized in that the organic-inorganic hybrid perovskite material is CH3NH3PbCl3、(C10H21NH3)2PbI4、((CH3)2NH2)3BiI6、CH3NH3SnI3At least one of (1).
5. The organic semiconductor device connecting structure according to any one of claims 1 to 3, wherein the interface modification layer has a thickness in the range of 0.1nm to 200 nm.
6. The organic semiconductor device connecting structure according to any one of claims 1 to 3, wherein the interface modification layer has a thickness in a range of 0.5nm to 20 nm.
7. The organic semiconductor device connecting structure according to any one of claims 1 to 3, wherein the interface modification layer has an optical transmittance of more than 70%.
8. An organic semiconductor device, characterized by comprising the connection structure of any one of claims 1 to 6.
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