CN111092159B - Organic semiconductor device and connection structure thereof - Google Patents
Organic semiconductor device and connection structure thereof Download PDFInfo
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- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
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- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/19—Tandem OLEDs
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- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/549—Organic PV cells
Abstract
The application discloses an organic semiconductor device and a connecting structure thereof, wherein the connecting structure comprises an n-type electron transmission material layer and a p-type hole transmission material layer which are overlapped, and an interface modification layer is arranged between the n-type electron transmission material layer and the p-type hole transmission material layer and is used for combining accumulated charges in the connecting structure. The interface modification layer effectively reduces the high cross voltage of the organic semiconductor device at the connecting structure, and improves the irradiation resistance and the service life of the OLED device.
Description
Technical Field
The present disclosure relates generally to the field of organic photovoltaics, and in particular to organic semiconductor devices and connection structures thereof.
Background
Organic light-emitting diode (OLED) and organic photovoltaic device (organic photovoltaic device, OPV) are main application directions of organic semiconductors, wherein OLED is an electroluminescent device, and the main application is in the fields of display and illumination; the OPV is a mode for converting an external light source into electric energy, and is a green energy source with great potential. The materials required in the OLED and OPV manufacturing process are not limited to pure organic semiconductor materials, the organic materials, inorganic materials and organic-inorganic composite materials can effectively improve the performance and service life of the device, and the semiconductor materials can be synthesized in a large amount through a laboratory, so that the cost and the development of the semiconductor materials have irreplaceable advantages, and the important point of the current development is how to further improve the performance and service life of the device.
One type of device is called a tandem structure (also called a structure (stacking structure)) among OLED and OPV, and the OLED aims to increase the brightness per unit area or reduce the operating current, so that the operating luminous intensity and the service life of the device can be effectively increased; the OPV uses more than two light-emitting 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 the connection structure in the stacked device, but since optical properties are required to be considered at the same time, a transparent connection structure becomes an important study subject.
The connection structures in the OLED are collectively referred to as charge generation layers (charge generation layer, CGL), and the connection structures in the OPV are collectively referred to as connection layers (connection units); the charge generation layer and the connection layer have substantially the same architecture and charge transport characteristics, and require efficient charge transport capabilities, including electron and hole transport capabilities; the CGL in the stacked OLED allows electrons and holes to be provided for the light-emitting active layers connected up and down respectively (the formal connection structure can provide electrons and holes for different requirement structures at the same time, so that the stacked OLED is called a charge generation layer); in the stacked OPV, the light-absorbing active layers generate separation of electrons and holes, and the connection structure is connected between two different light-absorbing active layers, so that the electrons and holes are respectively accepted to be combined in the connection structure. Both types of connection structures (OLED and OPV) maintain charge balance in the device, so that the device can be maintained in a normal and efficient operation.
The charge generation layer and the connecting layer are developed into at least two structural combinations, and basically are formed by combining 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 material and matched with specific doping to further improve the electron mobility, and the p-type material is usually a hole transport material and matched with specific doping to further improve the hole mobility; the above materials are not limited to all organic or all inorganic materials, and existing charge generation layers or connection layers such as: alq 3 :Mg / WO 3 、Bphen:Li / MoO 3 、BCP:L i/ V 2 O 5 、Alq 3 :Li / HAT-CN、CuPc / F 16 - CuPc、Alq 3 :Li. / NPB:F4-TCNQ、Alq 3 :Li ./ NPB:FeCl 3 、Bphen:Li / m - TDATA:F4-TCNQ、Alq 3 :Li. / NPB:MoO 3 、A / WO 3 / Ag、C 60 Numerous combinations of/Al/Au, etc. However, it is indicated by calculation and analysis that a certain voltage crossing phenomenon exists between the charge generation layer and the connection layer, that is, the stacked device can normally operate, but the charge generation layer and the connection layer must consume a certain voltage.
Disclosure of Invention
In view of the above-described drawbacks or shortcomings 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 a connection structure of an organic semiconductor device, 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 the interface modification layer 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 the 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 hybridization perovskite material is A m B n X k Wherein A is an organic amine group, B is a fourth main group metal ion or a transition metal ion, X is one or a combination of a plurality of halogen elements, and m, n and k are integers of 1 or more.
According to the technical scheme provided by the embodiment of the application, the organic-inorganic hybrid perovskite material is CH 3 NH 3 PbCl 3 、（C 10 H 21 NH 3 ） 2 PbI 4 、（（CH 3 ） 2 NH 2 ） 3 BiI 6 、CH 3 NH 3 SnI 3 At least one of them.
According to the technical scheme provided by the embodiment of the application, the thickness range of the interface modification layer is 0.1nm-200nm.
According to the technical scheme provided by the embodiment of the application, the thickness of the interface modification layer ranges from 0.5nm to 20nm.
According to the technical scheme provided by the embodiment of the application, the visible light 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 connection structures described above.
In the technical scheme of the application, 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 binding with accumulated charges within the connection structure; because the OLED device can generate a large amount of surplus electrons at the connecting structure to form accumulated charges when normally working, high cross voltage is formed at the connecting structure, and continuous accumulation of charges can cause continuous rising of device driving voltage and influence the service life of the device, after the surplus electrons (namely accumulated charges) are combined by the interface modification layer, the high cross voltage of the organic semiconductor device at the connecting structure can be effectively reduced, and the irradiation resistance and the service life of the OLED device are improved.
According to the technical scheme provided by the embodiment of the application, the material of the interface modification layer is the organic-inorganic hybridization perovskite material with the energy gap larger than 2.3 electron volts, so that the 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 irradiation 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 phenomenon of the organic semiconductor device at the charge connection structure by absorbing the accumulated charges, avoid the rise of the device driving voltage, and further has the capability of absorbing ultraviolet rays, thereby further improving the ultraviolet resistance and the service life of the OLED device.
In the prior art, the organic-inorganic hybrid perovskite material is applied to the connecting structure of the OLED screen body, but the organic-inorganic hybrid perovskite material is directly used as the material of the n-type electron transport material layer and the p-type hole transport material layer or doped in the n-type electron transport material layer and the p-type hole transport material layer, so as to improve the carrier transport capacity or the brightness of visible light; the light absorption range of the organic-inorganic hybridization perovskite with the energy gap of more than 2.3eV is separated from the visible light region, so that the capability of emitting light in the visible light range is not provided; the energy gap is too narrow, so that the charge separation capability of the device is too poor, and charge traps are easy to form, so that the device is applied to a light-emitting device and does not have the capability of improving the drivable current; therefore, perovskite materials with energy gaps of 2.3eV or more are not selected as materials for the charge connection structure within the common general knowledge of the person skilled in the art.
In the application, the characteristics of narrow energy gap and easiness in forming charge traps of the organic-inorganic hybridization perovskite with the energy gap of more than 2.3eV are just utilized to combine charges accumulated at the connecting structure, so that the problem of high voltage crossing at the connecting structure is solved on the premise of sacrificing the carrier transmission capacity at the connecting structure, and meanwhile, the irradiation resistance is improved, the overall performance of the OLED screen is effectively improved, and particularly the service life of the OLED device is effectively prolonged.
Drawings
Other features, objects and advantages of the present application will become more apparent upon reading of the detailed description of non-limiting embodiments, made with reference to the accompanying drawings in which:
FIG. 1 is a schematic structural diagram of embodiment 1 of the present application;
FIG. 2 is a schematic structural diagram of embodiment 2 of the present application;
FIG. 3 is a schematic cross-voltage diagram of a prior art OLED device at a charge-generating layer;
FIG. 4 is a schematic cross-voltage diagram of an OPV device at a charge generation layer in the prior art;
FIG. 5 is a schematic cross-voltage diagram of an OLED device at the charge-generating layer according to example 2 of the present application;
FIG. 6 is a schematic cross-voltage diagram of an OPV device at a charge generation layer in example 2 of the application;
reference numerals in the drawings:
61. an n-type electron transport material layer; 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 connection 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. an electron; 90. a cavity.
Detailed Description
The application is described in further detail below with reference to the drawings and examples. It is to be understood that the specific embodiments described herein are merely illustrative of the application and are not limiting of the application. It should be noted that, for convenience of description, only the portions related to the application are shown in the drawings.
It should be noted that, without conflict, the embodiments of the present application and features of the embodiments may be combined with each other. The application will be described in detail below with reference to the drawings in connection with embodiments.
Example 1
Referring to fig. 1, the present application provides a schematic structure diagram of an organic semiconductor device connection structure 60, wherein the connection structure 60 in the present embodiment 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 overlapped, 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 modification layer 62 is made of organic-inorganic hybrid perovskite material with the following material energy gap larger than 2.3 electron volts, and the structural general formula of the organic-inorganic hybrid perovskite material is A m B n X k Wherein A is an organic amine group, B is a fourth main group metal ion or a transition metal ion, and X is one or a combination of a plurality of halogen elements; m, n and k are integers greater than or equal to 1.
For example, the materials of each layer of the connection structure are respectively:
Alq 3 mg (10 nm)/interfacial modification layer/NPB: F 4 -TCNQ (25 nm); wherein the n-type electron transport material layer 61 is composed of 8-hydroxyquinoline doped with magnesium (Mg) and aluminum (Alq 3 ) Thickness of it10nm; the p-type hole transport material layer 63 is formed of a material doped with tetracyanodimethyl p-benzoquinone (F 4 -TCNQ).
The following manner is optionally adopted for the specific embodiments of the interface modification layer, and the specific materials, thicknesses and visible light transmittance of the interface modification layer are shown in the following table 1 under the corresponding various embodiments of the interface modification layer:
TABLE 1
In embodiment 1-1, the interface modification layer 62 is made of a perovskite material (CH 3 NH 3 PbCl 3 ) Forming, wherein the thickness is 0.5nm, and the transmittance of visible light is 88%; while in embodiments 1-2 the interface modification layer 62 is formed of a perovskite material (CH 3 NH 3 PbCl 3 ) Forming, wherein the thickness is 3nm, and the visible light transmittance is 85%; the interface modification layer 62 in embodiments 1-3 is also made of a perovskite material (CH 3 NH 3 PbCl 3 ) Forming, wherein the thickness is 20nm, and the visible light transmittance is 75%; finally in embodiments 1-4 the interface modification layer 62 is formed from a perovskite material (((CH) 3 ） 2 NH 2 ） 3 BiI 6 ) The thickness was 3nm, and the transmittance of visible light was 84%.
In various embodiments of the interface modification layer described above, the perovskite material (CH 3 NH 3 PbCl 3 ) Is 2.4 ev, perovskite material (((CH) 3 ） 2 NH 2 ） 3 BiI 6 ) The energy gap of the interface modification layer is 2.6 electron volts, so that the interface modification layer can effectively absorb high-energy light rays higher than 2.3 electron volts, and can effectively absorb accumulated charges when the OLED screen body works, so that the over-high driving voltage of the OLED screen body is avoided, and the service life of the OLED screen body is effectively prolonged.
In other embodiments, the perovskite material may also be CH 3 NH 3 SnI 3 、（C 10 H 21 NH 3 ） 2 PbI 4 Etc. other energyPerovskite material with a gap greater than 2.3 ev.
Example 2
As shown in fig. 2, the present embodiment provides an organic semiconductor device, which includes any one of the connection structures described above. For example, the organic semiconductor device includes, in order, 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. Wherein the connection structure 60 includes an n-type electron transport material layer 61, an interface modification layer 62, and a p-type hole transport material layer 63.
As shown in fig. 3, which is a schematic diagram illustrating carrier movement of each layer in the OLED device in the prior art, electrons 80 and holes 90 in the OLED are separated at a connection structure (charge generation layer CGL), when the number of electrons and holes at the CGL is unequal as the device ages, excessive accumulation of one carrier at the CGL is caused, the accumulation inhibits separation of electrons and holes, and thus a higher voltage is required at the CGL to further separate electrons and holes, so that the cross voltage of the device is larger, for example, denoted by H1;
as shown in fig. 4, which is a schematic diagram illustrating carrier movement of each layer in the OPV device in the prior art, electrons 80 and holes 90 in the OPV are combined at a connection structure (connection layer), and when the number of electrons and holes at the connection layer is unequal as the device ages, one carrier is accumulated at the connection layer too much, while during accumulation, electrons 80 are generally formed, and when electrons are accumulated too much, the cross voltage of the device is larger, for example, denoted by H2;
in the present embodiment, however, as shown in fig. 5, a charge generation layer made of perovskite material (CH 3 NH 3 PbCl 3 ) After the interface modification layer is manufactured, redundant electrons can be combined in the perovskite material so as to reduce the cross-pressure, for example, the required cross-pressure drop is H3, which is obviously smaller than H1;
in this embodiment, as shown in FIG. 6, a connection layer of the OPV device is providedIs composed of perovskite material (CH 3 NH 3 PbCl 3 ) After the interface modification layer is manufactured, redundant electrons can be combined in the perovskite material so as to reduce the cross-pressure, for example, the required cross-pressure drop is H4 and is obviously smaller than H2;
as can be seen from the above comparative examples, in the connection structure provided in this embodiment, by providing the interface modification layer formed of the perovskite material, 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 NPB (40 nm)/CPB:Ir (ppy) sequentially on the ITO conductive glass 3 (30nm)/ Bphen/CGL2/ NPB(40nm)/CPB:Ir (ppy) 3 (30nm)/Bphen/LiF/Al。
Wherein NPB is a hole transport layer; CPB Ir (ppy) 3 The light-emitting layer is 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, and the charge generation layer CGL2 may alternatively adopt the following embodiments, and sequentially includes the following structural layers: embodiments 2-1 to 2-4 of CGL2 described below correspond to embodiments 1-1 to 1-4 of the interface modification layer in example 1, respectively;
TABLE 2
Corresponding to the above 4 embodiments of the CGL2 layer, the results of the photoelectric performance of the organic semiconductor device provided in this example under the same brightness are compared as follows:
TABLE 3 Table 3
As can be seen from Table 3 above, in embodiment 2-2, CGL2, i.e., the interface modification layer was made of perovskite material (CH) having a thickness of 3nm 3 NH 3 PbCl 3 ) The photoelectric performance is optimal under the same brightness.
For comparison and explanation, the present embodimentThe examples also provide the following comparative examples for illustration: the OLED device structures provided in the following respective comparative examples were sequentially on ITO conductive glass: NPB (40 nm)/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 connection structure, in each of the following comparative examples, CGL1 comprises the following layered structure: as shown in table 4:
the above comparative example 1 is a conventional connection structure in the prior art, i.e., CGL1 has only n-type electron transport material layer [ Alq ] 3 Mg (10 nm) and a p-type hole transport material layer [ NPB: F4-TCNQ (25 nm) ];
comparative example 2 in n-type electron transport material layer [ Alq ] 3 An interface modification layer (NH) is arranged between Mg (10 nm) and a p-type hole transport material layer (NPB: F4-TCNQ (25 nm)) 2 CH= NH 2 PbI 3 ) (3 nm) wherein the interface modification layer [ NH ] 2 CH= NH 2 PbI 3 ) The energy gap of (3 nm) is less than 2.3ev;
comparative example 3 the n-type electron transport material layer [ Alq ] in comparative example 1 3 Alq in Mg (10 nm) 3 Replacement with an organic-inorganic perovskite material with an energy gap of less than 2.3ev [ NH ] 2 CH = NH 2 PbI 3 】；
Comparative example 4 NPB in the p-type hole transport material layer [ NPB: F4-TCNQ (25 nm) ] in comparative example 1 was replaced with an organic-inorganic perovskite material [ NH ] having an energy gap of less than 2.3ev 2 CH =NH 2 PbI 3 】；
Comparative example 5 the n-type electron transport material layer [ Alq ] in comparative example 1 3 Alq in Mg (10 nm) 3 Replaced by an organic-inorganic perovskite material with an energy gap greater than 2.3ev [ CH ] 3 NH 3 PbCl 3 】；
Comparative example 6 NPB in the p-type hole transport material layer [ NPB: F4-TCNQ (25 nm) ] in comparative example 1 was replaced with an organic-inorganic perovskite material [ CH ] having an energy gap of more than 2.3ev 3 NH 3 PbCl 3 】；
TABLE 4 Table 4
The results of the photovoltaic performance of the device at the same brightness are shown in table 5 below:
TABLE 5
Perovskite materials (NH 2 CH=NH 2 PbI 3 ) Comparative examples 3 and 4 verify the performance of the high mobility perovskite material doped in the n-type electron transport material layer, the p-type hole transport material layer, and as an interface modification layer, and comparative examples 5 and 6 verify the effect of perovskite material doped above 2.3 electron volts on device performance when doped in the n-type electron transport material layer, the p-type hole transport material layer.
According to tables 3 and 5, the OLED device of this example was compared with the OLED device of the comparative example, and the current efficiency of 91 cd/a, corresponding to a voltage of 10.3V, using comparative example 1 at the same luminance was 1000 hours for which the lifetime decayed to 90% of the initial value under irradiation with sunlight; the current efficiency of comparative example 2 was 86cd/A, the corresponding voltage was 10.8V, and the time for the lifetime to decay to 90% of the initial value was 800h; the best current efficiency of comparative example 3 was 94cd/A, the corresponding voltage was 9.6V, and the time for lifetime decay to 90% of the initial value was 1200h; in the embodiment 2, the current efficiency of the device of the embodiment 2-2 using CGL2 is 98cd/A, the corresponding voltage is 7.9V, and the time for the life to decay to the initial value of 90% is 2000h; therefore, the OLED device of this embodiment 2 effectively improves the voltage-crossing phenomenon caused by the charge generating layer by adopting the connection structure of embodiment 1, and also protects the organic material from being damaged due to the improvement of the radiation resistance, thereby improving the service life of the device.
The above description is only illustrative of the preferred embodiments of the present application and of the principles of the technology employed. It will be appreciated by persons skilled in the art that the scope of the application referred to in the present application is not limited to the specific combinations of the technical features described above, but also covers other technical features formed by any combination of the technical features described above or their equivalents without departing from the inventive concept. Such as the above-mentioned features and the technical features disclosed in the present application (but not limited to) having similar functions are replaced with each other.
Claims (7)
1. The connecting structure of the organic semiconductor device comprises an n-type electron transport material layer and a p-type hole transport material layer which are overlapped, 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 is used for being combined with accumulated charges in the connecting structure, and the interface modification layer is made of an organic-inorganic hybridization perovskite material with an energy gap of more than 2.3 electron volts.
2. An organic semiconductor device connection structure according to claim 1, wherein the organic-inorganic hybrid perovskite material has a general structural formula a m B n X k Wherein A is an organic amine group, B is a fourth main group metal ion or a transition metal ion, X is one or a combination of a plurality of halogen elements, and m, n and k are integers of 1 or more.
3. An organic semiconductor device connection structure according to claim 2, wherein the organic-inorganic hybrid perovskite material is CH 3 NH 3 PbCl 3、 （C 10 H 21 NH 3 ） 2 PbI 4 、
（（CH 3 ） 2 NH 2 ） 3 BiI 6 、CH 3 NH 3 SnI 3 At least one of them.
4. An organic semiconductor device connection structure according to any one of claims 1 to 3, wherein the thickness of the interface modification layer is in the range of 0.1nm to 200nm.
5. An organic semiconductor device connection structure according to any one of claims 1 to 3, wherein the thickness of the interface modification layer is in the range of 0.5nm to 20nm.
6. The organic semiconductor device connection structure according to any one of claims 1 to 3, wherein the interface modification layer has a visible light transmittance of 70% or more.
7. An organic semiconductor device comprising the connection structure of any one of claims 1 to 6.
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