CN117334801A - Graphene nanoribbon light-emitting diode and preparation method thereof - Google Patents
Graphene nanoribbon light-emitting diode and preparation method thereof Download PDFInfo
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- CN117334801A CN117334801A CN202311390647.5A CN202311390647A CN117334801A CN 117334801 A CN117334801 A CN 117334801A CN 202311390647 A CN202311390647 A CN 202311390647A CN 117334801 A CN117334801 A CN 117334801A
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 67
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 66
- 239000002074 nanoribbon Substances 0.000 title claims abstract description 58
- 238000002360 preparation method Methods 0.000 title abstract description 14
- 238000002347 injection Methods 0.000 claims abstract description 73
- 239000007924 injection Substances 0.000 claims abstract description 73
- 239000000758 substrate Substances 0.000 claims abstract description 17
- 238000000034 method Methods 0.000 claims abstract description 12
- 239000000463 material Substances 0.000 claims abstract description 11
- 238000004544 sputter deposition Methods 0.000 claims description 13
- 238000001548 drop coating Methods 0.000 claims description 4
- 239000011521 glass Substances 0.000 claims description 4
- 238000004528 spin coating Methods 0.000 claims description 4
- 239000004065 semiconductor Substances 0.000 abstract description 8
- 230000006798 recombination Effects 0.000 abstract description 2
- 238000005215 recombination Methods 0.000 abstract description 2
- 239000010410 layer Substances 0.000 description 68
- 239000010408 film Substances 0.000 description 6
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 4
- 239000000969 carrier Substances 0.000 description 4
- 238000004020 luminiscence type Methods 0.000 description 4
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000005669 field effect Effects 0.000 description 2
- 229910052733 gallium Inorganic materials 0.000 description 2
- 229910052738 indium Inorganic materials 0.000 description 2
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 2
- 238000001755 magnetron sputter deposition Methods 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 239000000243 solution Substances 0.000 description 2
- 239000010409 thin film Substances 0.000 description 2
- 230000007704 transition Effects 0.000 description 2
- 239000011787 zinc oxide Substances 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000002041 carbon nanotube Substances 0.000 description 1
- 229910021393 carbon nanotube Inorganic materials 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 230000005684 electric field Effects 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 230000005672 electromagnetic field Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
- 239000011147 inorganic material Substances 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 230000005693 optoelectronics Effects 0.000 description 1
- 239000002096 quantum dot Substances 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 238000002834 transmittance Methods 0.000 description 1
Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/02—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies
- H01L33/26—Materials of the light emitting region
- H01L33/34—Materials of the light emitting region containing only elements of Group IV of the Periodic Table
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/005—Processes
- H01L33/0054—Processes for devices with an active region comprising only group IV elements
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/02—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies
- H01L33/14—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor bodies with a carrier transport control structure, e.g. highly-doped semiconductor layer or current-blocking structure
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- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Computer Hardware Design (AREA)
- Microelectronics & Electronic Packaging (AREA)
- Power Engineering (AREA)
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Abstract
The invention relates to a graphene nanoribbon light-emitting diode and a preparation method thereof, wherein the graphene nanoribbon light-emitting diode comprises a substrate, an anode, a hole injection layer, a light-emitting layer, an electron injection layer and a cathode which are sequentially arranged from bottom to top; the material of the luminous layer is GNR; the hole injection layer is made of NiO; the electron injection layer is made of IGZO. According to the invention, the graphene nanoribbon is innovatively used as a light-emitting layer of the light-emitting diode, and IGZO and NiO are used as electron and hole injection layers, and because the energy band structures of the two semiconductor materials can be matched with the energy band structures of the graphene nanoribbon, the processes of carrier injection, recombination and the like can be realized in theory, when energy is transferred to valence band electrons of the graphene nanoribbon, the valence band electrons of the graphene nanoribbon can be excited to conduction bands, and thus, in the process that electrons return to the valence band from an unstable conduction band, the energy can be released in a visible light form.
Description
Technical Field
The invention relates to a graphene nanoribbon light-emitting diode (GNRLED) and a preparation method thereof, and belongs to the technical field of photoelectric devices.
Background
Graphene (Graphene) has been found to be of great interest since 2004 because of its high strength, hardness, thermal conductivity, electrical conductivity, and excellent light transmittance, and its excellent optical and electrical characteristics, showing great potential for application. However, since graphene is a zero bandgap material, it cannot be used as a semiconductor material, which limits its application in field effect transistors and other optoelectronic devices. In order to expand the forbidden band width thereof and thus give the semiconductor characteristics thereof, a learner expands a single-layer graphene into a quasi-one-dimensional graphene strip with a width of approximately less than 50nm according to a certain shape, and finds that the electronic characteristics thereof can be changed by changing the width and the edge geometry of the graphene nanoribbon (Graphene Nanoribbons, GNR), thereby realizing the adjustable band gap of the graphene nanoribbon. Currently, graphene nanoribbons have been widely used in the fields of sensor elements, field effect transistors, high-speed electrical switches, and the like. In addition, as a new class of semiconductor materials, their use in the photovoltaic field has attracted attention.
In 2018, the Italy and French research groups first observed through experiments that the high-intensity luminescence phenomenon of 7-atom-wide graphene nanoribbons, the intensity was comparable to that of a luminescent device made of carbon nanotubes, and the color could be changed by adjusting the voltage. These observations made a good bedding for further exploring the potential mechanism of graphene nanoribbons luminescence. However, achieving visible luminescence of graphene nanoribbons remains a recognized problem.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a graphene nanoribbon light-emitting diode and a preparation method thereof;
according to the invention, a vertical light-emitting diode structure is adopted, the materials of the electron injection layer and the hole injection layer, which are matched with the energy band of the graphene nanoribbon, are selected, the graphene nanoribbon is used as a light-emitting layer, and the red light emission of the graphene nanoribbon is realized, so that a solution idea is provided for solving the problem of light emission of the graphene nanoribbon. And secondly, by adopting an all-inorganic device structure, the device can be prepared by only coating by using magnetron sputtering in the preparation process, the preparation process is simple, and the device is stable in structure and is not easy to degrade.
Term interpretation:
IGZO, indium gallium zinc oxide, abbreviation for indium gallium zinc oxide;
GNR, graphene Nanoribbons, graphene nanoribbons;
the technical scheme of the invention is as follows:
a graphene nanoribbon light-emitting diode comprises a substrate, an anode, a hole injection layer, a light-emitting layer, an electron injection layer and a cathode which are sequentially arranged from bottom to top;
the material of the luminous layer is GNR; the hole injection layer is made of NiO; the electron injection layer is made of IGZO.
According to the present invention, preferably, the hole injection layer has a thickness of 30 to 200nm; the thickness of the electron injection layer is 50-200nm;
most preferably, the thickness of the hole injection layer is 30nm; the thickness of the electron injection layer was 50nm.
According to the invention, preferably, the anode is made of ITO; the cathode is made of Al; the substrate is a glass substrate.
According to the invention, the anode has a thickness of 100-150nm;
most preferably, the anode has a thickness of 180nm; the thickness of the cathode is 100nm.
The preparation method of the graphene nanoribbon light-emitting diode comprises the following steps:
growing an anode on the cleaned substrate;
growing a hole injection layer on the anode;
transferring the prepared luminescent layer to a hole injection layer by adopting a spin coating or drop coating mode;
growing an electron injection layer on the light emitting layer;
a cathode is grown on the electron injection layer.
Further preferably, growing an anode on the cleaned substrate comprises:
the parameters of growth are: at a vacuum level of less than 10 -6 Growing for 28min in pure Ar atmosphere with sputtering power of 60W to obtain ITO thin filmThe membrane acts as an anode.
Further preferably, growing a hole injection layer on the anode includes:
the parameters of growth are: at a vacuum level of less than 10 -6 Under Torr, in the presence of 2.5% O 2 In Ar atmosphere of (2), adopting sputtering power of 150W, and growing for 18min to obtain the NiO film as a hole injection layer.
Further preferably, growing an electron injection layer on the light emitting layer includes:
the parameters of growth are: at a vacuum level of less than 10 -6 And growing for 26 minutes and 40 seconds in a pure Ar atmosphere by adopting sputtering power of 90W to obtain the IGZO film serving as an electron injection layer.
Further preferably, growing a cathode on the electron injection layer includes:
the parameters of growth are: at a vacuum level of less than 10 -6 And growing for 8 minutes and 20 seconds in a pure Ar atmosphere by adopting sputtering power of 200W, thereby obtaining the Al film serving as a cathode.
The beneficial effects of the invention are as follows:
according to the invention, the graphene nanoribbon is innovatively used as a light-emitting layer of the light-emitting diode, and IGZO and NiO are used as electron and hole injection layers, and because the energy band structures of the two semiconductor materials can be matched with the energy band structures of the graphene nanoribbon, the processes of carrier injection, recombination and the like can be realized in theory, when energy is transferred to valence band electrons of the graphene nanoribbon, the valence band electrons of the graphene nanoribbon can be excited to conduction bands, and thus, in the process that electrons return to the valence band from an unstable conduction band, the energy can be released in a visible light form.
Drawings
Fig. 1 is a schematic structural diagram of a graphene nanoribbon light emitting diode;
FIG. 2 is a schematic illustration of a armchair graphene nanoribbon;
FIG. 3 is a schematic diagram of the working principle of a graphene nanoribbon light emitting diode;
FIG. 4 is a schematic flow chart of a method for preparing a graphene nanoribbon light emitting diode;
10. glass substrate, 11, anode, 12, hole injection layer, 13, light emitting layer, 14, electron injection layer, 15, cathode, 36, electron, 37, hole, 38, photon.
Detailed Description
The invention is further defined by, but is not limited to, the following drawings and examples in conjunction with the specification.
Example 1
A graphene nanoribbon light-emitting diode, as shown in figure 1, comprises a substrate, an anode 11, a hole injection layer 12, a light-emitting layer 13, an electron injection layer 14 and a cathode 15 which are sequentially arranged from bottom to top;
the material of the light-emitting layer 13 is GNR; the hole injection layer 12 is made of NiO; the electron injection layer 14 is made of IGZO.
By adopting a vertical light-emitting diode structure, IGZO and NiO are respectively selected as an electron injection layer 14 and a hole injection layer 12, and the energy band structures of the two materials are matched with the energy band of a Graphene Nanoribbon (GNR). After a voltage is applied to the electrodes, electrons 36 and holes 37 in IGZO and NiO are injected into the graphene nanoribbon light-emitting layer 13, respectively, and the electrons 36 and holes 37 recombine, causing electrons 36 in the graphene nanoribbons to transition from the valence band to the conduction band, and when the conduction band electrons 36 return to the valence band again, energy is released in the form of light 38. The emission wavelength corresponding to the forbidden bandwidth of the semiconductor graphene nanoribbon is in the red light range, so that the red light is emitted.
As shown in fig. 2, the graphene nanoribbon light emitting diode operates as follows: when a voltage in the voltage direction shown in fig. 1 is applied across the device, the electrons 36 of the electron injection layer 14 and the holes 37 of the hole injection layer 12 move towards the light emitting layer 13 under the action of an electric field, the electrons 36 and the holes 37 are recombined in the light emitting layer 13, the released energy makes the electrons 36 of the light emitting layer 13 transition from the valence band to the conduction band, the energy is released in the form of light during the process of recovering the electrons 36 from the conduction band to the valence band, visible red light emission is realized, and the diode emits red light.
Example 2
A graphene nanoribbon light emitting diode according to embodiment 1, which is different in that:
the thickness of the hole injection layer 12 is 30-200nm; the thickness of the electron injection layer 14 is 50-200nm;
the anode 11 is made of ITO; the thickness of the anode 11 is 100-150nm; the cathode 15 is made of Al; the substrate is a glass substrate 10.
Example 3
A graphene nanoribbon light emitting diode according to embodiment 1, which is different in that:
the thickness of the hole injection layer 12 is 30nm; the thickness of the electron injection layer 14 was 50nm.
For the hole injection layer 12 and the electron injection layer 14, the greater the thickness of the injection layer, the longer the time for which carriers are transferred in the injection layer, the greater the probability that carriers undergo scattering and reflection, and the greater the probability that energy is transferred away by vibration, i.e., the smaller the probability that carriers reach the light emitting layer 13, resulting in a decrease in light emitting efficiency.
The thickness of the anode 11 is 180nm; the thickness of the cathode 15 is 100nm.
From the dispersion relation of energy, it is shown that Graphene (Graphene) is free of band gap, shows strong metal, the energy in the internal energy band is basically continuous, so that the electron energy can be continuously changed, and the energy is easily changed by absorbing heat, kinetic energy or electromagnetic field energy, so that Graphene has the capability of being easily conductive to heat and electricity like metal, but is difficult to release new photons to a semiconductor, and therefore the luminescence phenomenon is difficult to realize.
According to the preparation method, the graphene band gap can be opened by preparing the quasi-one-dimensional Graphene Nanoribbon (GNR), and the size of the band gap is directly related to the width and the boundary crystal orientation of the nanoribbon. The graphene nanoribbon with the unique quasi-one-dimensional structure has electronic and magnetic properties which are diametrically opposite to those of two-dimensional graphene. z-type graphene nanoribbons (zGNRs) are more prone to semi-metallic properties. The carriers can be directly transmitted through the z-shaped graphene nanoribbons, and light emission is also difficult to realize. However, such armchair-type graphene nanoribbons (aGNRs) are a non-magnetic semiconductor with energy gaps, and as shown in fig. 2, the energy gaps gradually decrease with increasing nanoribbon bandwidth according to the first principle of properties, and when the width increases to a certain extent, the graphene nanoribbons have electronic properties approaching two dimensions indefinitely. However, when the bandwidth is gradually reduced, properties similar to those of quantum dots are exhibited. By estimating the band gap, it is expected that red light emission with a wavelength of around 700nm can be achieved.
Example 4
The preparation method of the graphene nanoribbon light-emitting diode according to any one of embodiments 1 to 3, as shown in fig. 4, includes:
growing an anode 11 on the cleaned substrate;
growing a hole injection layer 12 on the anode 11;
transferring the prepared luminescent layer 13 to the hole injection layer 12 by adopting a spin coating or drop coating mode;
growing an electron injection layer 14 on the light emitting layer 13;
a cathode 15 is grown on the electron injection layer 14.
Example 5
The preparation method of the graphene nanoribbon light-emitting diode according to embodiment 4 is different in that:
growing an anode 11 on the cleaned substrate, comprising:
the parameters of growth are: at a vacuum level of less than 10 -6 Under Torr, in a pure Ar (gas flow rate: 20 sccm) atmosphere, an ITO thin film was obtained as the anode 11 by growing for 28 minutes with a sputtering power of 60W.
Growing a hole injection layer 12 on the anode 11, comprising:
the parameters of growth are: at a vacuum level of less than 10 -6 Under Torr, in the presence of 2.5% O 2 In Ar atmosphere of (2), a sputtering power of 150W was used, and the film was grown for 18 minutes, to obtain a NiO film as the hole injection layer 12.
Growing an electron injection layer 14 on the light emitting layer 13 includes:
the parameters of growth are: at a vacuum level of less than 10 -6 Growing for 26 minutes and 40 seconds in a pure Ar atmosphere by adopting sputtering power of 90W under the condition of Torr to obtainThe IGZO thin film serves as the electron injection layer 14.
Growing a cathode 15 on the electron injection layer 14 includes:
the parameters of growth are: at a vacuum level of less than 10 -6 And growing for 8 minutes and 20 seconds in a pure Ar atmosphere by adopting sputtering power of 200W under the Torr, thereby obtaining an Al film as a cathode 15.
The full inorganic device structure is adopted, the preparation process mainly adopts a common sputtering coating mode, for example, the electron injection layer 14, the hole injection layer 12 and the electrode material are all stable inorganic materials, the preparation is carried out by adopting a simple magnetron sputtering method, the luminescent layer 13GNR is prepared by adopting a solution spin coating or drop coating mode, the preparation process is simple, the cost is lower, and the industrialization is easier to realize. And the components of the device are inorganic matters, so that the degradation problem possibly existing in an organic device does not exist, and the device has good stability, good repeatability and environmental friendliness.
Claims (10)
1. The graphene nanoribbon light-emitting diode is characterized by comprising a substrate, an anode, a hole injection layer, a light-emitting layer, an electron injection layer and a cathode which are sequentially arranged from bottom to top;
the material of the luminous layer is GNR; the hole injection layer is made of NiO; the electron injection layer is made of IGZO.
2. The graphene nanoribbon light-emitting diode according to claim 1, wherein the thickness of the hole injection layer is 30-200nm; the thickness of the electron injection layer is 50-200nm.
3. The graphene nanoribbon light emitting diode according to claim 1, wherein the thickness of the hole injection layer is 30nm; the thickness of the electron injection layer was 50nm.
4. The graphene nanoribbon light-emitting diode according to claim 1, wherein the anode is made of ITO; the cathode is made of Al; the substrate is a glass substrate.
5. The graphene nanoribbon light-emitting diode according to any one of claims 1 to 4, wherein the thickness of the anode is 100 to 150nm;
most preferably, the anode has a thickness of 180nm; the thickness of the cathode is 100nm.
6. The method for preparing the graphene nanoribbon light-emitting diode according to any one of claims 1 to 5, which is characterized by comprising the following steps:
growing an anode on the cleaned substrate;
growing a hole injection layer on the anode;
transferring the prepared luminescent layer to a hole injection layer by adopting a spin coating or drop coating mode;
growing an electron injection layer on the light emitting layer;
a cathode is grown on the electron injection layer.
7. The method of claim 6, wherein growing an anode on the cleaned substrate comprises:
the parameters of growth are: at a vacuum level of less than 10 -6 And growing for 28min in a pure Ar atmosphere by adopting sputtering power of 60W to obtain the ITO film serving as an anode.
8. The method of claim 6, wherein growing a hole injection layer on the anode comprises:
the parameters of growth are: at a vacuum level of less than 10 -6 Under Torr, in the presence of 2.5% O 2 In Ar atmosphere of (2), adopting sputtering power of 150W, and growing for 18min to obtain the NiO film as a hole injection layer.
9. The method of claim 6, wherein growing an electron injection layer on the light emitting layer comprises:
the parameters of growth are: at a vacuum level of less than 10 -6 And growing for 26 minutes and 40 seconds in a pure Ar atmosphere by adopting sputtering power of 90W to obtain the IGZO film serving as an electron injection layer.
10. The method for preparing a graphene nanoribbon light emitting diode according to any one of claims 6 to 9, wherein growing a cathode on the electron injection layer comprises:
the parameters of growth are: at a vacuum level of less than 10 -6 And growing for 8 minutes and 20 seconds in a pure Ar atmosphere by adopting sputtering power of 200W, thereby obtaining the Al film serving as a cathode.
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| CN202311390647.5A CN117334801A (en) | 2023-10-25 | 2023-10-25 | Graphene nanoribbon light-emitting diode and preparation method thereof |
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