CN110718636A - Quantum dot light-emitting diode and preparation method thereof - Google Patents
Quantum dot light-emitting diode and preparation method thereof Download PDFInfo
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- CN110718636A CN110718636A CN201810758133.3A CN201810758133A CN110718636A CN 110718636 A CN110718636 A CN 110718636A CN 201810758133 A CN201810758133 A CN 201810758133A CN 110718636 A CN110718636 A CN 110718636A
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- H10K50/00—Organic light-emitting devices
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- H10K50/16—Electron transporting layers
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- H10K50/166—Electron transporting layers comprising a multilayered structure
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- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/11—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers
- H10K50/115—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers comprising active inorganic nanostructures, e.g. luminescent quantum dots
Abstract
The invention relates to a quantum dot light-emitting diode and a preparation method thereof. The quantum dot light-emitting diode comprises an anode, a cathode and a quantum dot light-emitting layer arranged between the anode and the cathode, wherein a composite electron transmission layer containing a doped material is stacked between the cathode and the quantum dot light-emitting layer, the composite electron transmission layer comprises N layers of electron transmission layers, the first layer of electron transmission layer is adjacent to the quantum dot light-emitting layer, and the Nth layer of electron transmission layer is adjacent to the cathode; the doping material is used for improving the carrier transmission rate in the quantum dot light-emitting diode, and the doping concentration of the doping material is sequentially increased from the first layer of the electron transmission layer to the Nth layer of the electron transmission layer; wherein N is an integer greater than or equal to 2. The N-layer electron transport layer is beneficial to balancing electrons and holes in the quantum dot light-emitting layer, so that the recombination efficiency of the quantum dots is improved, and the problem of unbalanced carrier injection is solved.
Description
Technical Field
The invention belongs to the technical field of display, and particularly relates to a quantum dot light-emitting diode and a preparation method thereof.
Background
The quantum dot light emitting diode (QLED) has the advantages of high light color purity, high light emitting quantum efficiency, adjustable light emitting color, long service life and the like, and has wide application prospect in the fields of illumination and flat panel display. The QLED can be structurally divided into a positive QLED and an inverse QLED, and most of research is focused on the structure of a positive QLED device, but the inverse device structure can be integrated with a low-cost n-type metal oxide or amorphous silicon thin film transistor, so that the on-voltage is lower than that of a positive device, and the inverse device has a more practical potential application value in the display field, however, the light emitting efficiency and the service life of the inverse device are different from those of a positive device.
The energy level structure of the conventional QLED device is more beneficial to the injection of electrons, so that the injection of the electrons and the injection of the holes are unbalanced. The excessive electron injection causes self-luminescence of device functional layers such as a hole transport layer, thereby affecting the luminous purity and recombination efficiency of the quantum dot light emitting device. In addition, if the transport of excessively injected electrons in the quantum dot light emitting layer is hindered, electric charges may be accumulated in the quantum dot light emitting layer, seriously affecting the light emitting characteristics of the quantum dot.
Disclosure of Invention
The invention aims to overcome the defects in the prior art, provides a quantum dot light-emitting diode and a preparation method thereof, and aims to solve the technical problem that excessive electron injection in the conventional quantum dot light-emitting diode causes unbalance of electrons and holes.
In order to achieve the purpose, the invention adopts the following technical scheme:
the invention provides a quantum dot light-emitting diode, which comprises an anode, a cathode and a quantum dot light-emitting layer arranged between the anode and the cathode, wherein a composite electron transmission layer containing a doped material is stacked between the cathode and the quantum dot light-emitting layer, the composite electron transmission layer comprises N layers of electron transmission layers, the first layer of the electron transmission layer is adjacent to the quantum dot light-emitting layer, and the Nth layer of the electron transmission layer is adjacent to the cathode;
the doping material is used for improving the carrier transmission rate in the quantum dot light-emitting diode, and the doping concentration of the doping material is sequentially increased from the first layer of the electron transmission layer to the Nth layer of the electron transmission layer; wherein N is an integer greater than or equal to 2.
The invention also provides a preparation method of the quantum dot light-emitting diode, which comprises the following steps:
preparing a composite electron transport layer containing a doped material on the cathode or the quantum dot light-emitting layer, wherein the composite electron transport layer comprises N laminated electron transport layers;
the electron transport layer of the first layer is adjacent to the quantum dot light emitting layer, the electron transport layer of the Nth layer is adjacent to the cathode, the doping concentration of the doping material is increased from the electron transport layer of the first layer to the electron transport layer of the Nth layer in sequence, and N is an integer greater than or equal to 2.
In the quantum dot light-emitting diode provided by the invention, a composite electron transmission layer (comprising N electron transmission layers) containing a doping material is stacked between a cathode and a quantum dot light-emitting layer, the doping concentrations of the first electron transmission layer to the Nth electron transmission layer are sequentially increased, and the N electron transmission layers form N-type doping with concentration gradient, namely the doping concentrations are sequentially distributed in a step-down manner from the high concentration close to the cathode to the light-emitting layer close to the quantum dot; the doping material can improve the carrier transmission rate, the electron transmission layers with different doping concentrations can form carrier concentration difference, carriers can move from a high concentration position to a low concentration position for uniform distribution to form diffusion, ionized impurities cannot move when the carriers leave the original positions, the local electric neutrality inside the doped electron transmission layers is damaged, a built-in electric field is generated, the existence of the built-in electric field enables the doped main body material to have different electric potentials of electrons at each position, so that the energy of each electron is different, an upward energy band bending from high doping to low doping is formed, therefore, the built-in electric field can obstruct the migration of electrons from the electron transmission layers to the luminous layers, the electron transmission efficiency is reduced, the carrier balance inside the device is promoted, the N-layer electron transmission layer is beneficial to balancing the electrons and holes in the quantum dot luminous layers, and the recombination efficiency of the quantum dots is improved, the problem of carrier injection imbalance is alleviated.
The preparation method of the quantum dot light-emitting diode provided by the invention has a simple process, and the composite electron transport layer (comprising N laminated electron transport layers) containing the doping material is prepared on the cathode or the quantum dot light-emitting layer, so that the N electron transport layers form N-type doping with concentration gradient, namely, the doping concentration is sequentially reduced from the high concentration close to the cathode to the light-emitting layer close to the quantum dot in a sequential step-down distribution, thereby forming a built-in electric field, the built-in electric field can obstruct the migration of electrons from the electron transport layer to the light-emitting layer, reduce the electron transport efficiency and promote the balance of carriers in the device, and the N electron transport layers are beneficial to balancing electrons and holes in the quantum dot light-emitting layer, thereby improving the recombination efficiency of the quantum dots and relieving the problem of unbalanced carrier injection.
Drawings
Fig. 1 is a schematic structural diagram of a QLED according to an embodiment of the present invention.
Detailed Description
In order to make the technical problems, technical solutions and advantageous effects to be solved by the present invention more clearly apparent, the present invention is further described in detail below with reference to the following embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
In one aspect, an embodiment of the present invention provides a quantum dot light emitting diode, including an anode, a cathode, and a quantum dot light emitting layer disposed between the anode and the cathode, where a composite electron transport layer containing a doped material is stacked between the cathode and the quantum dot light emitting layer, the composite electron transport layer includes N electron transport layers, a first electron transport layer is adjacent to the quantum dot light emitting layer, and an N-th electron transport layer is adjacent to the cathode;
the doping material is used for improving the carrier transmission rate in the quantum dot light-emitting diode, and the doping concentration of the doping material is sequentially increased from the first layer of the electron transmission layer to the Nth layer of the electron transmission layer; wherein N is an integer greater than or equal to 2.
In the quantum dot light-emitting diode provided by the embodiment of the invention, a composite electron transport layer (comprising N electron transport layers) containing a doping material is stacked between a cathode and a quantum dot light-emitting layer, and the doping concentrations of the first electron transport layer to the Nth electron transport layer are sequentially increased, so that the N electron transport layers form N-type doping with concentration gradient, namely the doping concentrations sequentially decrease from the high concentration close to the cathode to the quantum dot light-emitting layer and are sequentially distributed in a step-down manner; the doping material can improve the carrier transmission rate, the electron transmission layers with different doping concentrations can form carrier concentration difference, carriers can move from a high concentration position to a low concentration position in order to be uniformly distributed, the formed and diffused different doping concentrations enable the carriers to be diffused in the electron transmission layers, the carriers tend to be uniformly distributed, ionized impurities cannot move when the carriers leave the original positions, the local electric neutrality in the doped electron transmission layers is damaged, a built-in electric field appears, the existence of the built-in electric field enables the doped main body material to have different electric potentials of electrons at each position, so that the energy of the electrons at each position is different, an upward energy band bending from high doping to low doping is formed, and thus the built-in electric field can obstruct the migration of the electrons from the electron transmission layers to the light emitting layers, the electron transmission efficiency is reduced, and the carrier balance in the device is promoted, the N-layer electron transport layer is beneficial to balancing electrons and holes in the quantum dot light-emitting layer, so that the recombination efficiency of the quantum dots is improved, and the problem of unbalanced carrier injection is solved.
It should be emphasized that, in the above-mentioned quantum dot light emitting diode according to the embodiment of the present invention, the sequentially increasing doping concentration of the doping material from the first layer to the N-th layer of the electron transport layer may be understood as: the doping concentration of the first electron transport layer is zero (i.e. the first electron transport layer is undoped), or the doping concentration of the first electron transport layer is lowest (i.e. the doping concentration of the first electron transport layer is lowest in the N-layer electron transport layers); in both cases, the case described in the embodiment of the present invention that the doping concentration of the doping material is sequentially increased from the electron transport layer of the first layer to the electron transport layer of the nth layer can be realized, and both cases are within the protection scope of the present invention.
The quantum dot light-emitting diode of the embodiment of the invention can be a positive type QLED or an inverse type QLED; the positive device has better luminous efficiency and service life, and the inversion device can be integrated with a low-cost n-type metal oxide or amorphous silicon thin film transistor and has lower starting voltage.
Further, in the quantum dot light emitting diode provided by the embodiment of the invention, N is an integer of 2 to 5.
Further, in the quantum dot light-emitting diode provided by the embodiment of the invention, the host material of the electron transport layer is selected from ZnO and SnO2And TiO2At least one of (1). And the doping material is selected from at least one of V and Nb. The doping material is used for improving the carrier transmission rate in the quantum dot light-emitting diode, and the main material of the electron transmission layer is TiO2For example, the doping element is Nb or V, and the doping method is magnetron sputtering or ion implantation. Doped V5+Or Nb+5By substituting Ti by doping4 +Present as donor level in TiO2The electron mobility of the N-th layer is gradually increased as the doping concentration of the N-th layer increases, and the main purpose of the N-th layer is to diffuse carriers, form a built-in electric field, block electron transmission, and promote carrier balance.
Further, the first layer of the electron transport layer is undoped TiO2And (3) a layer. That is, in the quantum dot light emitting diode according to the embodiment of the present invention, the doping concentrations of the electron transport layer from the first layer to the nth layer are sequentially increased, and it can be understood that the electron transport layer of the first layer is a low-doped or undoped electron transport layer. For undoped TiO2And the quantum dot light-emitting layer has a lower valence band energy level, so that holes can be blocked, and carriers are limited in the quantum dot light-emitting layer. The N-layer electron transport layer can reduce the electron transport efficiency, block holes, further improve the luminous efficiency of the QLED device and prolong the service life of the device.
Further, in the quantum dot light emitting diode provided by the embodiment of the invention, the doping concentration of the electron transport layer of the nth layer is 0.5-2 wt%; and the doping concentration of the electron transport layer of the first layer is 0 to 0.1 wt%. Meanwhile, the thickness of the electron transmission layer of the Nth layer is 10-30 nm; and the thickness of the electron transport layer of the first layer is 2-10 nm.
For example, in a preferred embodiment, the quantum dot light emitting diode comprises 2 electron transport layers, wherein the first electron transport layer (near the quantum dot light emitting layer) is undoped TiO2The thickness is 2-10 nm; and the second electron transport layer (near the bottom electrode) contains TiO with a doping concentration of 0.1-0.5 wt%2The thickness is 10-30 nm.
In another preferred embodiment, the quantum dot light emitting diode comprises 3 electron transport layers, wherein the first electron transport layer (close to the quantum dot light emitting layer) is undoped TiO2The thickness is 2-10 nm; the second electron transport layer (between the first and third electron transport layers) comprises TiO with a doping concentration of 0.1-0.5 wt%2The thickness is 20-30 nm; and a third electron transport layer (near the bottom electrode) comprising TiO with a doping concentration of 0.5-2 wt%2The thickness is 20-30 nm.
Further, in the quantum dot light-emitting diode provided by the embodiment of the invention, a hole function layer is further stacked between the anode and the quantum dot light-emitting layer; an electron injection layer is further stacked between the cathode and the Nth layer of the electron transport layer. The hole function layer can be at least one of a hole transport layer and a hole injection layer; namely, the light emitting layer from the anode to the quantum dot can be sequentially as follows: the anode, the hole transport layer and the quantum dot light emitting layer are adopted as the anode, the hole injection layer and the quantum dot light emitting layer, or the anode, the hole injection layer, the hole transport layer and the quantum dot light emitting layer are adopted as the anode. It should be noted that the hole injection layer, the hole transport layer, and the electron injection layer are not essential and may be increased or decreased according to actual circumstances.
On the other hand, the embodiment of the invention also provides a preparation method of the quantum dot light-emitting diode, which comprises the following steps:
preparing a composite electron transport layer containing a doped material on the cathode or the quantum dot light-emitting layer, wherein the composite electron transport layer comprises N laminated electron transport layers;
the electron transport layer of the first layer is adjacent to the quantum dot light emitting layer, the electron transport layer of the Nth layer is adjacent to the cathode, the doping concentration of the doping material is increased from the electron transport layer of the first layer to the electron transport layer of the Nth layer in sequence, and N is an integer greater than or equal to 2.
The preparation method of the quantum dot light-emitting diode provided by the embodiment of the invention has a simple process, and the composite electron transport layer (comprising N laminated electron transport layers) containing the doping material is prepared on the cathode or the quantum dot light-emitting layer, so that the N electron transport layers form N-type doping with concentration gradient, namely, the doping concentration is sequentially reduced from the high concentration close to the cathode to the light-emitting layer close to the quantum dot and is distributed in a sequential step-down manner, and thus, an electric field is built in, the built-in electric field can block the migration of electrons from the electron transport layer to the light-emitting layer, the electron transport efficiency is reduced, the carrier balance in the device is promoted, and the N electron transport layers are beneficial to balancing electrons and holes in the quantum dot light-emitting layer, so that the composite efficiency of the quantum dot is improved, and the problem of.
Further, N is an integer of 2 to 5. The main material of the electron transport layer is selected from ZnO and SnO2And TiO2At least one of; the doping material is at least one selected from V and Nb.
As shown in fig. 1: the structure of an inversion type QLED device sequentially comprises: substrate (glass), bottom electrode (ITO), N-layer electron transport layer (TiO)2Doped materials), quantum dot light emitting layers (QDs), hole transport layers (PVK), hole injection layers (PEDOT: PSS), and top electrodes (Al).
The method for preparing the inversion type QLED device comprises the following steps:
1. pretreating the substrate and depositing a layer of bottom electrode material on the surface of the substrate;
2. forming an N-layer electron transport layer on the bottom electrode;
3. forming a quantum dot light emitting layer on a layer of a material capable of transporting electrons
4. Forming a hole transport layer on the quantum dot light emitting layer;
5. forming a hole injection layer on the hole transport layer;
6. and forming a top electrode on the hole injection layer to encapsulate the device.
In the preparation method of the quantum dot light-emitting diode provided by the embodiment of the invention, the quantum dot light-emitting layer material can be a quantum dot with a CdSe/CdSnS core-shell structure; the hole transport layer material may be PVK; the material of the hole injection layer can be PEDOT: PSS; the top electrode material is metal Al or Ag. The above functional layer materials can be deposited by known methods such as vacuum vapor deposition, ion plating, sputtering, ink-jet printing, sol-gel, etc.
The invention is described in further detail with reference to a part of the test results, which are described in detail below with reference to specific examples.
Example 1
A QLED device comprises ITO/0.5% wtV doped TiO2Undoped TiO2PSS/Al, CdSe/CdSN core-shell structured quantum dots/PVK/PEDOT.
(1) The ITO glass with the patterning on one surface is cleaned and sequentially placed in ultrapure water, acetone water and isopropanol for ultrasonic cleaning, and the time of each step of ultrasonic cleaning is 15 minutes. After the sonication was completed, the mica was irradiated under ultraviolet ozone for 20 minutes.
(2) Then depositing TiO with a layered structure with two different doping concentrations on the ITO surface2First, a 20nm layer of 0.5% wtV doped TiO was deposited2Subsequently, a layer of 5nm undoped TiO is deposited thereon2。
(3) Then the substrate is transferred to a nitrogen environment, and a quantum dot light-emitting layer with a CdSe/CdSnS core-shell structure is prepared by a spin coating method, wherein the thickness of the light-emitting layer is 10 nm.
(4) The hole transporting material PVK was then spin coated onto the quantum dot emissive layer at 3000RPM in the same ambient atmosphere to a thickness of 40 nm.
(5) The hole injection layer material PEDOT: PSS was spin coated onto the PVK surface at 5000RPM to a thickness of about 40nm and then heated on an 80 degree hot plate for 15 minutes to dry the PEDOT: PSS.
(6) Finally, the dried device is transferred to a chamber deposition chamber, which is evacuated to 10 deg.f-6After torr or lower, a 100nm layer of metallic Al is deposited as the top electrode and the necessary encapsulation of the device is performed.
Example 2
The QLED device structurally comprises ITO/1 wt% Nb-doped TiO20.5% wt Nb-doped TiO2Undoped TiO2PSS/Al, CdSe/CdSN core-shell structured quantum dots/PVK/PEDOT.
The preparation method of the QLED device comprises the following steps:
(1) the ITO glass with the patterning on one surface is cleaned and sequentially placed in ultrapure water, acetone water and isopropanol for ultrasonic cleaning, and the time of each step of ultrasonic cleaning is 15 minutes. After the sonication was completed, the mica was irradiated under ultraviolet ozone for 20 minutes.
(2) Then depositing TiO with a layered structure with three different doping concentrations on the ITO surface2First, a layer of 15nm TiO doped with 1% by weight of Nb is deposited2Layer, then depositing thereon a layer of 0.5% by weight Nb doped TiO2Layer, and finally depositing a layer of 5nm undoped TiO on the layer2。
(3) Then the substrate is transferred to a nitrogen environment, and a quantum dot light-emitting layer with a CdSe/CdSnS core-shell structure is prepared by a spin coating method, wherein the thickness of the light-emitting layer is 10 nm.
(4) The hole transporting material PVK was then spin coated onto the quantum dot emissive layer at 3000RPM in the same ambient atmosphere to a thickness of 40 nm.
(5) The hole injection layer material PEDOT: PSS was spin coated onto the PVK surface at 5000RPM to a thickness of about 40nm and then heated on an 80 degree hot plate for 15 minutes to dry the PEDOT: PSS.
(6) Finally, the dried device is transferred to a chamber deposition chamber, which is evacuated to 10 deg.f-6After torr or lower, a 100nm layer of metallic Al is deposited as the top electrode and the necessary encapsulation of the device is performed.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.
Claims (10)
1. A quantum dot light-emitting diode comprises an anode, a cathode and a quantum dot light-emitting layer arranged between the anode and the cathode, and is characterized in that a composite electron transmission layer containing a doped material is arranged between the cathode and the quantum dot light-emitting layer in a stacking manner, the composite electron transmission layer comprises N layers of electron transmission layers, the first layer of the electron transmission layer is adjacent to the quantum dot light-emitting layer, and the Nth layer of the electron transmission layer is adjacent to the cathode;
the doping material is used for improving the carrier transmission rate in the quantum dot light-emitting diode, and the doping concentration of the doping material is sequentially increased from the first layer of the electron transmission layer to the Nth layer of the electron transmission layer; wherein N is an integer greater than or equal to 2.
2. The quantum dot light-emitting diode of claim 1, wherein N is an integer from 2 to 5.
3. The quantum dot light-emitting diode of claim 1, wherein the host material of the electron transport layer is selected from ZnO, SnO2And TiO2At least one of; and/or
The doping material is selected from at least one of V and Nb.
4. The quantum dot light-emitting diode of claim 1, wherein the first layer of the electron transport layer is undopedTiO2And (3) a layer.
5. The quantum dot light-emitting diode of claim 1, wherein the electron transport layer of the nth layer has a doping concentration of 0.5 to 2 wt%; and/or
The doping concentration of the electron transport layer of the first layer is 0 to 0.1 wt%.
6. The quantum dot light-emitting diode of claim 1, wherein the electron transport layer of the nth layer has a thickness of 10 to 30 nm; and/or
The thickness of the electron transport layer of the first layer is 2-10 nm.
7. The quantum dot light emitting diode of any one of claims 1 to 6, wherein a hole function layer is further stacked between the anode and the quantum dot light emitting layer; and/or
An electron injection layer is further stacked between the cathode and the Nth layer of the electron transport layer.
8. A preparation method of a quantum dot light-emitting diode is characterized by comprising the following steps:
preparing a composite electron transport layer containing a doped material on the cathode or the quantum dot light-emitting layer, wherein the composite electron transport layer comprises N laminated electron transport layers;
the electron transport layer of the first layer is adjacent to the quantum dot light emitting layer, the electron transport layer of the Nth layer is adjacent to the cathode, the doping concentration of the doping material is increased from the electron transport layer of the first layer to the electron transport layer of the Nth layer in sequence, and N is an integer greater than or equal to 2.
9. The method of claim 8, wherein N is an integer from 2 to 5.
10. The production method according to claim 8, wherein the host material of the electron transport layer is selected from ZnO and SnO2And TiO2At least one of; and/or
The doping material is selected from at least one of V and Nb.
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| CN112151648B (en) * | 2020-10-27 | 2022-08-12 | 合肥福纳科技有限公司 | Quantum dot light-emitting diode and preparation method thereof |
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