CN115498121A - Quantum dot sensitized up-conversion electroluminescent device - Google Patents
Quantum dot sensitized up-conversion electroluminescent device Download PDFInfo
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- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
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Abstract
The invention discloses a quantum dot sensitized up-conversion electroluminescent device, belongs to the technical field of luminescent devices, and can solve the problems of poor blue light stability, high starting voltage and low efficiency of the conventional electroluminescent device. The electroluminescent device comprises an anode, a cathode and a light-emitting active layer arranged between the anode and the cathode; the light-emitting active layer is made of quantum dot materials and organic molecular materials. The invention is used for electroluminescent devices.
Description
Technical Field
The invention relates to a quantum dot sensitized up-conversion electroluminescent device, and belongs to the technical field of luminescent devices.
Background
The electroluminescent device consists of a cathode, an anode, and a hole transport layer, a light emitting layer and an electron transport layer which are arranged between the anode and the cathode. When the voltage on the anode and the cathode is loaded to a proper value, holes generated by the anode and electrons generated by the cathode are combined in the luminescent layer through the hole transport layer and the electron transport layer respectively, so that the luminescent layer generates light, and light of three primary colors of red, green and blue RGB is generated according to different formulas of the luminescent layer to form basic colors for display. However, most of the existing electroluminescent devices have the problems of poor blue light stability, high turn-on voltage and low efficiency.
Disclosure of Invention
The invention provides a quantum dot sensitized up-conversion electroluminescent device which can solve the problems of poor blue light stability, high starting voltage and low efficiency of the conventional electroluminescent device.
The invention provides a quantum dot sensitized up-conversion electroluminescent device, which comprises an anode, a cathode and a luminous active layer arranged between the anode and the cathode;
the light-emitting active layer is made of quantum dot materials and organic molecule materials.
Optionally, the quantum dot material is used as a sensitizer in a TTA upconversion material system; the organic molecular material is used as an annihilator in a TTA up-conversion material system.
Optionally, the sensitizer is one or more of semiconductor quantum dot materials PbSe, cdSe, cdTe, znSe and InP.
Optionally, the organic molecular material serves as a sensitizer and an annihilator in the TTA upconversion material system;
the quantum dot material emits photons with energy greater than or equal to the singlet energy level of the sensitizer.
Optionally, the sensitizer is a transition metal-containing complex or an organic dye.
Optionally, the transition metal is one of ruthenium, platinum, iridium, and palladium.
Optionally, the organic molecular material serves as an energy transmission ligand and an annihilator in a TTA up-conversion material system;
the energy transmission ligand is one of anthracene formic acid (9-ACA) and tetracene derivative (4- (tetracen-5-yl) benzoic acid, CPT).
Optionally, the quantum dot material is one or more of PbSe, cdSe, cdTe, znSe, and InP.
Optionally, the annihilator is one or more of polycyclic aromatic hydrocarbons anthracene, pyrene, fluorene, tetracene, perylene and its derivatives, heterocyclic compound diimide and dye.
Optionally, an electron transport layer is disposed between the light-emitting active layer and the cathode;
a hole transport layer is arranged between the light-emitting active layer and the anode;
and a hole injection layer is arranged between the hole transport layer and the anode.
Optionally, the light-emitting active layer includes a quantum dot film and an organic molecular film stacked together;
the quantum dot film is made of a quantum dot material;
the organic molecular film is made of an organic molecular material.
The invention can produce the beneficial effects that:
according to the quantum dot sensitized up-conversion electroluminescent device provided by the invention, by adopting a photon up-conversion approach and according to a TTA up-conversion mechanism, based on energy transfer between quantum dots and organic molecules and a triplet state-triplet state annihilation energy up-conversion mechanism of the organic molecules, low-energy photons emitted by the quantum dots in the electroluminescent device are converted into high-energy photons through a quantum dot-organic molecule hybrid system, for example, near infrared emission of the quantum dots can be converted into visible light emission, or red and green light emission of the quantum dots can be converted into blue light emission, so that up-conversion electroluminescence is realized.
Drawings
Fig. 1 is a schematic structural diagram of a quantum dot sensitized up-conversion electroluminescent device and an up-conversion principle thereof according to an embodiment of the present invention;
fig. 2 is a material system of a quantum dot-annihilator up-conversion luminescence active layer represented by PbSe QDs-Rubrene and an up-conversion mechanism thereof provided by an embodiment of the present invention;
FIG. 3 is a material system of quantum dot-energy transfer ligand-annihilator up-conversion luminescence active layer represented by CdSe QDs-9-ACA-DPA and an up-conversion mechanism thereof, provided by an embodiment of the present invention;
fig. 4 is a material system of a quantum dot-sensitizer-annihilator up-conversion luminescence active layer represented by CdSe QDs-PtOEP-DPA and an up-conversion mechanism thereof provided by an embodiment of the invention.
List of parts and reference numerals:
11. an anode; 12. a cathode; 13. an electron transport layer; 14. a hole transport layer; 15. a hole injection layer.
Detailed Description
The present invention will be described in detail with reference to examples, but the present invention is not limited to these examples.
The light-emitting wavelength of the current electroluminescent device is directly determined by the band gap width of the material of the light-emitting active layer, and the realization way of the light-emitting wavelength of the device can be expanded by utilizing the photon up-conversion principle. Photon up-conversion is an anti-stokes process that absorbs two or more photons of low energy and emits photons of higher energy. Photon upconversion is typically achieved by three means: two-photon absorption up-conversion, rare earth doped material up-conversion and triplet-triplet annihilation (TTA) -based up-conversion. Two-photon absorption up-conversion requires up to 10 of the absorbed light intensity 6 W/cm 2 The rare earth doped material has small absorption cross section, low up-conversion efficiency and limited up-conversion spectrum coverage. The triplet state-triplet state annihilation up-conversion does not need coherent light, has low requirement on the intensity of exciting light, can combine the electroluminescence of quantum dots and the up-conversion mechanism of organic molecules in a light-emitting active layer through the structural design of a device, and realizes photon up-conversion in an electroluminescent device based on the TTA process.
The TTA upconverter system includes a sensitizer and an annihilator (emitter/receptor). Different types of heavy metal complexes or organic dyes can act as up-conversion sensitizers, such as MOEP (M = Pt, pd), znTPP, TIHF. The up-converting annihilator may be selected from conjugated organic compounds such as polycyclic aromatic hydrocarbons and heterocyclic compounds. During the TTA upconversion, the sensitizer gains energy to transition from a ground state to a singlet excited state, followed by intersystem crossing to a triplet excited state. Since the triplet excited state has a longer lifetime than the singlet excited state, a triplet-triplet energy transfer can occur, transferring the sensitizer triplet excited state energy to the annihilator triplet excited state. Two annihilators in a triplet excited state undergo triplet-triplet annihilation (TTA), producing one annihilator in a singlet excited state. Finally, annihilation electrons in the singlet excited state return to the ground state to emit photons with higher energy, so that photon up-conversion is realized. Effective TTA up-conversion at low light intensity conditions can be successfully achieved in quantum dot-organic molecule hybrid systems, in addition to occurring in mixed conjugated organisms. Therefore, the equivalent molecular point-organic molecule hybrid system is used as a light-emitting active layer of an electroluminescent device, and up-conversion electroluminescence can be realized.
The quantum dot light-emitting diode oriented to the display field has potential advantages in the aspects of cost, luminous efficiency, half-peak width, printing process and the like. The innovative design of the device structure and the regulation and control of emitted photons are effective ways for exerting the potential energy of the quantum dot light-emitting diode. For example, the current blue light device with low efficiency and poor stability can be realized by selecting an up-conversion path. For a blue device emitting light with a wavelength of 460nm, the turn-on voltage can be theoretically lowered from 2.69V to 1.35V. And thus the driving voltage of the device is expected to be reduced. And the device working under lower voltage can reduce the damage of the electric field to the structure of the device, and is beneficial to improving the stability of the device. The invention adopts a photon up-conversion approach, combines quantum dots and organic molecules by designing a luminescent active layer of a quantum dot electroluminescent device according to a TTA up-conversion mechanism, and realizes up-conversion electroluminescent.
An embodiment of the present invention provides a quantum dot sensitized up-conversion electroluminescent device, which is shown in fig. 1 and includes an anode 11 and a cathode 12, and a light emitting active layer disposed between the anode 11 and the cathode 12; the light-emitting active layer is made of quantum dot materials and organic molecular materials.
In practical application, an electron transport layer 13 is further arranged between the light-emitting active layer and the cathode 12; a hole transport layer 14 is also arranged between the light-emitting active layer and the anode 11; a hole injection layer 15 is also provided between the hole transport layer 14 and the anode 11.
In an embodiment of the present invention, the light emitting active layer is a single layer film structure including a quantum dot material and an organic molecular material; in other embodiments of the present invention, the light emitting active layer may also include a quantum dot film and an organic molecule film that are disposed in a stack; the quantum dot film is made of quantum dot materials; the organic molecular film is made of an organic molecular material.
The quantum dot electroluminescent device structure of the invention is introduced with a luminescent active layer capable of generating photon up-conversion, and the up-conversion electroluminescent device is designed with two paths:
one is that the quantum dots are directly used as sensitizers to be combined with the annihilators, wherein the ratio of the sensitizers to the annihilators is 1: 10 4 ～10 5 Forming a quantum dot-annihilator up-conversion luminescence active layer, wherein the difference between the conduction band bottom level of the semiconductor quantum dot and the triplet state energy level of the organic molecule is less than 0.1eV, so as to ensure an effective energy transfer process; the quantum dot system can select one or more of semiconductor quantum dot materials such as PbSe, cdSe, cdTe, znSe, inP and the like as a sensitizer; one or more of polycyclic aromatic hydrocarbon anthracene, pyrene, fluorene, tetracene, perylene and derivatives thereof can be selected as effective annihilator, such as 9, 10-Diphenylanthracene (DPA), 9, 10-Bisphenylethynylanthracene (BPEA), 5,6, 11, 12-tetraphenylnaphthalene (rubrene), 9, 10-Bisphenylethynylnaphthalene (BPEN), pyrene, poly-9, 9-bis 2-ethylhexylfluorene (PF 2/6), etc.; and one or more of heterocyclic compound diimide, dye and other materials as effective annihilator, such as BODIPY dye, PDI and other materials.
Secondly, the quantum dots emit photons, and combine sensitizers and annihilators to form a quantum dot-sensitizer-annihilator up-conversion luminescence active layer, wherein the ratio of the quantum dots, the sensitizers and the annihilators is 1: 10 2 -10 3 ∶10 2 The energy of the emitted photons of the semiconductor quantum dots is not less than the singlet energy level of the sensitizer organic molecules, so that the effective photon absorption process is ensured. The quantum dot system can be selected from one or more of semiconductor quantum dot materials such as PbSe, cdSe, cdTe, znSe, inP and the like as an emission photon source, and can be selected from transition metal complexes containing ruthenium, platinum, iridium, palladium and the like and organic dyes and the like as sensitizers in an up-conversion system, such as porphyrin/phthalocyanine complexes (PtOEP, pdOEP, znTPP, ptTPBP) and polyimine complexes ([ Ru (dmb) 3 ] 2+ 、[Pt(ttpy)(C≡CPh)]ClO 4 ) Cyclometallated complex (Ir (ppy) 3 ) Organic dyes (2, 4,5, 7-tetraiodo-6-hydroxy-3-fluorenone (TIHF), and the like. Can be selected from polycyclic aromatic hydrocarbons such as anthracene, pyrene, fluorene, tetracene, and peryleneAnd derivatives thereof, and one or more of materials such as heterocyclic compound diimide and dye as effective annihilator. The specific implementation case is as follows:
example 1: quantum dot-annihilator up-conversion photoluminescence.
The electroluminescent device is formed by a method such as sputtering, spin coating, or evaporation on a glass substrate to form a hole injection layer 15, a hole transport layer 14, a light-emitting active layer, an electron transport layer 13, and electrodes. The key to the up-conversion electroluminescence is the design of the light-emitting active layer. Fig. 2 shows the materials, energy level structures and the up-conversion mechanism of the quantum dot-annihilator up-conversion luminescence active layer, which is represented by a lead selenide quantum dot (PbSe QDs) -Rubrene (Rubrene) system, and can up-convert infrared light into visible light emission. The preparation method comprises the following steps: 10-100 μ L concentration about 10 -3 M magnitude PbSe QDs hexane solution is mixed with 500-1000. Mu.L Rubrene toluene solution with concentration of 1-10M to form up-conversion luminescence active layer in the device by spin coating. PEDOT, TFB, znO, al and other materials can be selected as other functional layers of the device to prepare the complete up-conversion electroluminescent device.
Example 2: quantum dot-energy transfer ligand-annihilator up-conversion photoluminescence
In order to improve the energy transfer efficiency and the up-conversion efficiency, an energy transmission ligand can be introduced between the quantum dot and the energy transfer path of the annihilator, so that the transition effect is realized in the energy transfer process, and the efficiency is improved. The device structure is the same as that of example 1, the materials, energy level structures and up-conversion mechanisms of the quantum dot-energy transfer ligand-annihilator up-conversion luminescence active layer are shown in fig. 3, and a cadmium selenide quantum dot (CdSe QDs) -9-anthracene carboxylic acid (9-ACA) -9, 10-Diphenylanthracene (DPA) system is taken as a representative, and can up-convert green light into blue light for emission. The preparation method comprises the following steps: 0.1-1mL concentration of about 10 -5 M-magnitude CdSe QDs toluene solution and 1-10mL of about 10-concentration -2 Mixing and stirring 9-ACA acetonitrile/toluene (volume ratio about 3/11) solution of M grade for 1-3 hr, adding equal volume of acetone, centrifuging, purifying, and dispersing in toluene. Then 10-50. Mu.L of a 0.05M DPA toluene solution was added and mixed. The upconversion emissive active layer is formed in the device by spin coating.
Example 3: quantum dot-sensitizer-annihilator up-conversion photoluminescence
Embodiments 1 and 2 both belong to quantum dots as sensitizers to transfer exciton energy directly to an annihilator or intermediate ligand without emitting a photon. Example 3 is characterized in that the quantum dots undergo exciton recombination, emit a photon, which is absorbed by the sensitizer and subsequently transfers energy to the annihilator, resulting in photon up-conversion. The materials, energy level structures and up-conversion mechanisms of the quantum dot-sensitizer-annihilator up-conversion luminescence active layer are shown in fig. 4, and are represented by cadmium selenide quantum dot (CbSe QDs) - (PtOEP) - (DPA) systems. The preparation method is similar to that of examples 1 and 2, a mixed solution of CbSe QDs, ptOEP and DPA with appropriate concentration and proportion is prepared, and an up-conversion luminescence active layer is formed in the device through spin coating.
Although the present application has been described with reference to a few embodiments, it should be understood that various changes, substitutions and alterations can be made herein without departing from the spirit and scope of the application as defined by the appended claims.
Claims (10)
1. A quantum dot sensitized up-conversion electroluminescent device is characterized by comprising an anode, a cathode and a light emitting active layer arranged between the anode and the cathode;
the light-emitting active layer is made of quantum dot materials and organic molecule materials.
2. The electroluminescent device of claim 1, wherein the quantum dot material acts as a sensitizer in a TTA up-conversion material system; the organic molecular material is used as an annihilator in a TTA up-conversion material system.
3. An electroluminescent device according to claim 2, characterized in that the sensitizer is one or more of the semiconductor quantum dot materials PbSe, cdSe, cdTe, znSe, inP.
4. An electroluminescent device according to claim 1, characterized in that the organic molecular material acts as a sensitizer and annihilator in the TTA up-conversion material system;
the quantum dot material emits photon energy greater than or equal to the sensitizer singlet energy level.
5. An electroluminescent device as claimed in claim 4, characterized in that the sensitizer is a complex containing a transition metal or an organic dye.
6. The device of claim 5, wherein the transition metal is one of ruthenium, platinum, iridium, and palladium.
7. The electroluminescent device of claim 1, wherein the organic molecular material acts as an energy-transporting ligand and annihilator in the TTA upconverter system;
the energy transmission ligand is anthracene formic acid or tetracene derivative.
8. An electroluminescent device according to claim 4 or 7, characterized in that the quantum dot material is one or more of PbSe, cdSe, cdTe, znSe, inP.
9. The electroluminescent device according to any of claims 1 to 7, characterized in that the annihilator is one or more of polycyclic aromatic hydrocarbons anthracene, pyrene, fluorene, tetracene, perylene and its derivatives, heterocyclic compounds diimide, dyes.
10. The electroluminescent device of claim 1, wherein the light-emitting active layer comprises a quantum dot film and an organic molecule film arranged in a stack;
the quantum dot film is made of a quantum dot material;
the organic molecular film is made of an organic molecular material.
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| US20160237343A1 (en) * | 2015-02-17 | 2016-08-18 | Massachusetts Institute Of Technology | Methods and compositions for the upconversion of light |
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| US20210036249A1 (en) * | 2019-08-02 | 2021-02-04 | The Florida State University Research Foundation, Incorporated | Systems and methods for bulk semiconductor sensitized solid state upconversion |
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| US20160237343A1 (en) * | 2015-02-17 | 2016-08-18 | Massachusetts Institute Of Technology | Methods and compositions for the upconversion of light |
| US20210036249A1 (en) * | 2019-08-02 | 2021-02-04 | The Florida State University Research Foundation, Incorporated | Systems and methods for bulk semiconductor sensitized solid state upconversion |
| CN111063680A (en) * | 2019-12-06 | 2020-04-24 | 北京大学深圳研究生院 | Up-conversion device based on alternating current driving planar display unit |
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| WAQAS AHMAD等: "Strategies for combining triplet–triple tannihilation upconversion sensitizers and acceptors in a host matrix", COORDINATION CHEMISTRY REVIEWS, vol. 439, 19 April 2021 (2021-04-19), pages 1 - 26 * |
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