WO2022252525A1 - 集发光、开关、颜色控制的电致发光四极管及其控制方法 - Google Patents

集发光、开关、颜色控制的电致发光四极管及其控制方法 Download PDF

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WO2022252525A1
WO2022252525A1 PCT/CN2021/134464 CN2021134464W WO2022252525A1 WO 2022252525 A1 WO2022252525 A1 WO 2022252525A1 CN 2021134464 W CN2021134464 W CN 2021134464W WO 2022252525 A1 WO2022252525 A1 WO 2022252525A1
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layer
light
tetrode
electroluminescent
emitting
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French (fr)
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孟鸿
纪君朋
杨标
张超红
赵长斌
陈经伟
蔡雨露
孟智敏
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Peking University Shenzhen Graduate School
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    • G—PHYSICS
    • G06—COMPUTING OR CALCULATING; COUNTING
    • G06F—ELECTRIC DIGITAL DATA PROCESSING
    • G06F3/00—Input arrangements for transferring data to be processed into a form capable of being handled by the computer; Output arrangements for transferring data from processing unit to output unit, e.g. interface arrangements
    • G06F3/14—Digital output to display device ; Cooperation and interconnection of the display device with other functional units
    • G06F3/1407—General aspects irrespective of display type, e.g. determination of decimal point position, display with fixed or driving decimal point, suppression of non-significant zeros
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
    • H05B33/00—Electroluminescent light sources
    • H05B33/02—Details
    • H05B33/06—Electrode terminals
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02B—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO BUILDINGS, e.g. HOUSING, HOUSE APPLIANCES OR RELATED END-USER APPLICATIONS
    • Y02B20/00—Energy efficient lighting technologies, e.g. halogen lamps or gas discharge lamps
    • Y02B20/30—Semiconductor lamps, e.g. solid state lamps [SSL] light emitting diodes [LED] or organic LED [OLED]

Definitions

  • the invention relates to the technical field of electroluminescence, in particular to an electroluminescent tetrode integrating light emission, switching and color control and a control method thereof.
  • the full-color display unit is an important part of intelligent electronic devices, so the display unit, like other electronic components, is facing the needs of miniaturization, integration and intelligence. With the introduction of the concept of system-level integration of electronic devices, more and more multifunctional electronic devices have aroused people's interest.
  • organic electronics is considered to be the development direction of flexible electronics in the future.
  • OFTs organic transistors
  • OLED active-matrix organic light-emitting diode
  • A-OLED active matrix organic light-emitting diode
  • the entire screen of full-color display is composed of multiple pixels, and each pixel must include three sub-pixels that emit red, green, and blue light respectively.
  • the pixels of the screen display colors by adjusting the color ratio of red, green, and blue sub-pixels.
  • the switch control of each sub-pixel needs to be completed by at least one transistor.
  • OLET organic light-emitting transistor
  • the pixel color control logic is complicated, and the red, green, and blue light-emitting sub-pixels need to be controlled separately, and integrated control cannot be performed through one signal.
  • the technical problem to be solved by the present invention is to provide a mold, a crucible and a crystal growth device aiming at solving the problem in the prior art that integrated control cannot be performed through one signal, aiming at the above-mentioned defects of the prior art.
  • An electroluminescent tetrode integrating light emission, switching, and color control including: an electrode layer, a light emitting layer, and a modulation layer arranged in sequence;
  • the light-emitting layer includes: at least two sub-light-emitting layers;
  • the electrode layer includes: at least two electrodes, two adjacent electrodes are spaced apart from each other;
  • the electrodes are provided in one-to-one correspondence with the sub-light-emitting layers, and the modulation layer is used to control each sub-light-emitting layer.
  • the electroluminescent tetrode that integrates lighting, switching, and color control, wherein the electroluminescent tetrode further includes:
  • a first DC blocking layer located between the electrode layer and the light emitting layer;
  • the second DC blocking layer is located between the light emitting layer and the modulation layer.
  • the first direct current blocking layer adopts a dielectric layer
  • the second direct current blocking layer adopts a dielectric layer
  • the electroluminescent tetrode that integrates lighting, switching, and color control, wherein the electroluminescent tetrode further includes:
  • the hole generating layer is connected with the light emitting layer.
  • the hole generation layer is a stacked or doped structure.
  • the electroluminescent tetrode that integrates lighting, switching, and color control, wherein the electroluminescent tetrode further includes:
  • the electron transport layer and the hole generation layer are respectively located on two sides of the light emitting layer.
  • the electroluminescent tetrode that integrates lighting, switching, and color control, wherein the electroluminescent tetrode further includes:
  • the emission colors of each sub-emission layer are different; and/or
  • Each sub-light-emitting layer is in a spiral shape, and each electrode is in a spiral shape;
  • the modulation layer is an electronic conductor layer or an ion conductor layer.
  • a control method for an electroluminescent tetrode that integrates light emission, switch, and color control as described in any one of the above, wherein, it includes the steps of:
  • control method of the electroluminescent tetrode that integrates light emission, switch, and color control, wherein the control signal includes: high level and low level, and the voltage of the high level is greater than the voltage of the multi-phase alternating current peak voltage.
  • each sub-light-emitting layer can be controlled separately through the modulation layer, these The sub-light-emitting layers can form a pixel, that is, each sub-light-emitting layer can be integratedly controlled by giving a control signal to the modulation layer.
  • FIG. 1 is a schematic structural diagram of a device with an adjustment electrode at the bottom and a DC blocking layer at the bottom provided by an embodiment of the present invention.
  • FIG. 2 is a schematic structural diagram of a device with an adjustable electrode at the bottom and a DC blocking layer at the top provided by an embodiment of the present invention.
  • FIG. 3 is a schematic structural diagram of a device with an adjustment electrode on top and a DC blocking layer on the bottom provided by an embodiment of the present invention.
  • FIG. 4 is a schematic structural diagram of a device with an adjustable electrode on top DC blocking layer on top structure provided by an embodiment of the present invention.
  • FIG. 5 is a schematic structural diagram of an inversion structure device with an adjustment electrode at the bottom and a DC blocking layer at the bottom provided by an embodiment of the present invention.
  • Fig. 6 is a schematic structural diagram of an inverted structure device with an adjustment electrode at the bottom and a DC blocking layer at the top provided by an embodiment of the present invention.
  • FIG. 7 is a schematic structural diagram of an inversion structure device with an adjustment electrode on top and a DC blocking layer on the bottom provided by an embodiment of the present invention.
  • FIG. 8 is a schematic structural diagram of a device with an inversion electrode on top DC blocking layer on top provided by an embodiment of the present invention.
  • FIG. 9 is a schematic structural diagram of a device with an upright structure provided by an embodiment of the present invention, in which the adjustment electrodes are arranged at the bottom and the top of the DC blocking layer.
  • FIG. 10 is a schematic structural diagram of a device with an upright structure with an adjustment electrode at the bottom without a DC blocking layer provided by an embodiment of the present invention.
  • FIG. 11 is a schematic diagram of interdigitated electrodes suitable for electrodes of three-phase electronic devices in Embodiment 1 of the present invention.
  • 12A-12J are structural diagrams of organic materials used in the device preparation process in Example 1 of the present invention.
  • FIG. 13 is a schematic diagram of the device structure of the electroluminescent tetrode in Embodiment 1 of the present invention.
  • FIG. 14 is a schematic diagram of control signals represented by eight representative control codes and their corresponding driving signals in Embodiment 1 of the present invention.
  • FIG. 15 shows the distribution of the emission color states of the device represented by all 64 kinds of control codes in the CIE coordinates in Embodiment 1 of the present invention.
  • the present invention provides some embodiments of an electroluminescent tetrode integrating light emission, switching and color control.
  • OLET organic light-emitting transistor
  • the luminous color cannot be adjusted, or can only be adjusted within a small range.
  • the current OLET technology can only realize the emission and control of monochromatic light.
  • the desired technology should be able to satisfy a device that emits red, green, and blue colors at the same time without the need for pixels.
  • the dot is further divided into three sub-pixels of red, green and blue.
  • the drive circuit and control circuit are complex. Most of the existing technologies use direct current or single-phase alternating current to drive the light-emitting unit.
  • the driving circuit requires complex back-end equipment to realize AC-DC (AD) conversion, which increases static power loss, increases the complexity of integrated circuits, and may reduce the aperture ratio. .
  • AD AC-DC
  • the pixel color control logic is complicated, and integrated control cannot be performed through one signal, and the red, green, and blue light-emitting sub-pixels need to be controlled separately, which is not convenient for color storage and extraction.
  • the light-emitting layer is divided into at least two sub-light-emitting layers, and the electrode layer is divided into at least two electrodes arranged at intervals.
  • the electrodes correspond to the sub-light-emitting layers one by one. Therefore, each sub-light-emitting layer can be controlled separately through the modulation layer.
  • the light-emitting layer can form a pixel, that is, each sub-light-emitting layer can be integratedly controlled by giving a control signal to the modulation layer.
  • a kind of electroluminescence tetrode of the present invention that integrates lighting, switching, and color control includes:
  • the electrode layer 8 the light emitting layer 5 and the modulation layer 2 arranged in sequence;
  • the light-emitting layer 5 includes: at least two sub-light-emitting layers (5-1, 5-2, 5-3);
  • the electrode layer 8 includes: at least two electrodes (8-1, 8-2, 8-3), and two adjacent electrodes (8-1, 8-2, 8-3) are spaced apart from each other;
  • the electrodes (8-1, 8-2, 8-3) are provided in one-to-one correspondence with the sub-light emitting layers, and the modulation layer 2 is used to control the sub-light-emitting layers (5-1, 5-2, 5-3).
  • each sub-light-emitting layer can emit the same light or different lights.
  • the pixel in order to enable the pixel to emit white light, the pixel generally includes at least three sub-pixels, and the light emitted by the three sub-pixels is different and can be mixed to form white light. Therefore, in order to make the light-emitting layer emit white light, the light-emitting layer includes at least three sub-light-emitting layers, and the light emitted by the three sub-light-emitting layers is mixed to form white light.
  • the modulation signal By connecting the modulation signal to the modulation layer, the overall switch and color change of the light-emitting device including sub-light-emitting layers of different colors can be controlled. switch, color.
  • the electroluminescent tetrode (i.e. the device) is driven by a three-phase alternating current, and the three phase differences of the three-phase alternating current applied to the electrode 8-1, the electrode 8-2 and the electrode 8-3 in the electrode layer 8 of the device are mutually 120 degree sine wave output voltage with proper amplitude. At this time, if no control signal is applied to the modulation layer, the red, green and blue light emitting units all emit light.
  • the red, green and blue light-emitting units of the device can be controlled in an integrated manner to have different light-emitting states, such as only red light, only green light, only blue light, red light and green light at the same time, red light Light and blue light are on at the same time, green light and blue light are on at the same time, neither red, green, and blue light-emitting units are on, or both red, green, and blue light-emitting units are lighted but the ratio of light-emitting brightness is different.
  • the adjustment of the outgoing light between red light, green light, and blue light can be realized, and the adjustment range can cover a plane area of CIE coordinates.
  • an organic electroluminescent tetrode with adjustable color is prepared by arranging three light emitting units with different colors side by side.
  • This device can be driven by three-phase AC to emit three colors of light, which can be directly connected to the power grid to achieve "plug and play", and not only control the luminous intensity of the three light-emitting units, but also control three different colors through a control signal
  • the light ratio can be adjusted to realize the color.
  • the device integrates light emitting, switching and three-dimensional color control functions at the system level, which is expected to simplify the fabrication process and cost of the pixel structure, miniaturize the pixel unit, reduce the use of TFT switching devices, and increase the aperture ratio.
  • the organic electroluminescent tetrode in the present invention is prepared using materials that are easy to commercialize, has a simple manufacturing process, and is easy to form pixels in a display.
  • the electroluminescent tetrode of the present application can adopt materials related to LEDs (including inorganic LEDs, organic LEDs, polymer LEDs, quantum dot LEDs, perovskite LEDs, etc.), that is to say, all existing LED light-emitting layers can be As the light-emitting layer of the electroluminescent tetrode of the present application, the electrode layers of existing LEDs can be used as the electrode layer of the electroluminescent tetrode of the present application. Of course, other functional layers of LED, such as hole transport layer, hole injection layer, electron transport layer, electron injection layer, etc., can also be applied to the electroluminescent tetrode of this application. Certainly, the material of the electroluminescent tetrode of the present application is not limited to the materials listed below in the present application,
  • the same or different light-emitting materials can be selected for each sub-light-emitting layer, which can be independently selected from the following materials, including polymer organic light-emitting materials, small molecule organic fluorescent materials, small molecule phosphorescent light-emitting materials, TADF thermally delayed luminescence Material.
  • Polymer organic light-emitting materials include but are not limited to Super yellow (super yellow, poly[ ⁇ 2,5-bis(3',7'-dimethyloctyloxy)-1,4-phenylacetylene ⁇ -co- ⁇ 3 -(4'-(3",7"-Dimethyloctyloxy)phenyl)-1,4-phenylacetylene ⁇ -co- ⁇ 3-(3'-(3",7"-dimethyl octyloxy)phenyl)-1,4-phenylacetylene ⁇ ]), Bu-PPP (poly(2,5-dibutoxybenzene-1,4-diyl)), PFO (poly(9,9 -Di-n-octylfluorenyl-2,7-diyl)), PVK (poly(9-vinylcarbazole)), F8BT (poly[(9,9-dioctylfluorenyl-2,7-diy
  • small molecule organic fluorescent or phosphorescent luminescent materials include but are not limited to CBP (4,4-bis (9-carbazole) biphenyl), Alq3 (tris (8-hydroxyquinoline) aluminum), TBCPF (9, 9-di-4,4'-(3,6-di-tert-butylcarbazolyl)-phenylfluorene), mCP(1,3-di-9-carbazolylbenzene), 26DCzPPY(2,6- Bis((9H-carbazol-9-yl)-3,1-phenylene)pyridine), Ir(mppy)3, Ir(piq)2(acac), Ir(hpiq)3, Ir(ppy)3 , Ir(bt)2(acac), Ir(pbi)2(acac), Ir(ppy)2(acac), FCNIrPic, PhFIrPic, FirPic, PO-01-TB (acetylacetonate
  • Thermally activated delayed fluorescence (TADF) materials are the third-generation organic light-emitting materials developed after organic fluorescent materials and organic phosphorescent materials. Such materials generally have a small singlet-triplet energy level difference (DEST), and the triplet excitons can be transformed into singlet excitons to emit light through anti-intersystem crossing. This can make full use of the singlet excitons and triplet excitons formed under electrical excitation, and the internal quantum efficiency of the device can reach 100%.
  • the structure of the material is controllable, the properties are stable, the price is cheap and no precious metals are required, and the application prospects in the field of OLEDs are broad.
  • TADF thermally delayed luminescent materials include but are not limited to BCPO (bis-4(N-carbazolylphenyl)phenylphosphine oxide), 2CzPN(4,5-bis(9-carbazolyl)-o-phenyl Dinitrile), 4CzPN (3,4,5,6-tetrakis(9-carbazolyl)-phthalonitrile), 4CzIPN (2,4,5,6-tetrakis(9-carbazolyl)-isophthalonitrile dinitrile), 4CzTPN (2,3,5,6-tetrakis(9-carbazolyl)-terephthalonitrile), 4CzTPN-Bu(2,3,5,6-tetrakis(3,6-di-tert-butyl Base-9-carbazolyl)-terephthalonitrile), 4CzPN-Ph(3,4,5,6-tetrakis(3,6-diphenyl-9-carbazolyl)-
  • Inorganic luminescent materials or organic-inorganic hybrid luminescent materials that are well known to those skilled in the art and have a similar luminescent principle to organic electroluminescent materials may also be within the selection range of luminescent materials.
  • the perovskite material itself can absorb in the spectral range of 390-790nm, and has the characteristics of super large light absorption coefficient, ultra-low volume defect density, slow Auger recombination and balanced bipolar transmission, making perovskite materials Significant advantages have been achieved in terms of high luminous efficiency.
  • the characteristics of perovskite materials such as solution processing and flexible device preparation, make it possible to prepare large-area devices with simple process and low price, making them have broad application prospects in display, lighting and optical communication.
  • Quantum dot materials are nanoparticles composed of II-VI or III-V elements.
  • the particle size of quantum dots is generally between 1 and 10 nm. Since electrons and holes are quantum-confined, the continuous energy band structure becomes a discrete energy level structure with molecular characteristics, and can emit fluorescence after being excited.
  • the quantum dot material includes 3D or 2D perovskite quantum dots, carbon quantum dots and ZnS, ZnSe, ZnO, ZnTe, CdSe, CdS, CdTe, CaS, SrS based on the above perovskite materials.
  • the above-mentioned quantum dots can be single-component, multi-component, core-shell structure, etc. At the same time, its morphology can be nanoparticles, nanobelts, nanowires and the like.
  • Inorganic semiconductor LED light-emitting materials are made of compounds containing gallium (Ga), arsenic (As), phosphorus (P), nitrogen (N) and the like. Its light-emitting principle is roughly the same as that of OLED, which can radiate visible light when electrons and holes recombine, so it can also be used to make light-emitting diodes and electroluminescent quadruples that integrate light-emitting, switching, and color control functions in this application. polar tube.
  • the inorganic semiconductor LED luminescent material can be made of one or more of the following doped or non-doped materials: aluminum gallium arsenide, gallium arsenide, gallium arsenide phosphide, indium phosphide Gallium, aluminum gallium phosphide (doped zinc oxide), aluminum gallium phosphide, indium gallium nitride/gallium nitride, gallium phosphide, aluminum indium gallium phosphide, aluminum gallium phosphide, aluminum indium phosphide, gallium arsenide Gallium, phosphide, indium gallium aluminum phosphide, gallium phosphide, gallium arsenide phosphide, gallium phosphide, zinc selenide, indium gallium nitride, silicon carbide, gallium nitride, indium gallium nitride, zinc selenide, sapphire , silicon, silicon, silicon,
  • the size of the device made of the above-mentioned inorganic semiconductor LED light-emitting material as the material of the light-emitting layer can be nanoscale, micron-scale or millimeter-scale. More preferably, the light-emitting layer is composed of a PN junction formed by doping one or more of the above-mentioned inorganic semiconductor LED light-emitting materials.
  • the light-emitting layer involved in the present invention can be further doped with materials such as carbon nanotubes, nano-silver wires, and metal oxides to improve its light-emitting properties.
  • each electrode is selected from any type of conductive material, including but not limited to various metals, such as silver, aluminum, gold, copper, platinum, nickel, palladium, iron, magnesium-aluminum alloy, copper-silver alloy, aluminum-copper alloy, iron-copper Silver alloy, etc., or metal carbon/nitride (MXene), graphene, graphite, carbon black, carbon fiber, single-walled carbon nanotubes, multi-walled carbon nanotubes with a two-dimensional layered structure, or containing PEDOT, PANi , Ppy and other conductive polymer materials, conductive elastomers, conductive oxides, or one or more composites.
  • various metals such as silver, aluminum, gold, copper, platinum, nickel, palladium, iron, magnesium-aluminum alloy, copper-silver alloy, aluminum-copper alloy, iron-copper Silver alloy, etc.
  • metal carbon/nitride MXene
  • graphene graphite
  • carbon black carbon fiber
  • the modulation layer 2 is an electronic conductor layer or an ion conductor layer.
  • the modulation layer can be made of any electronic conductor or ion conductor material, including various metals, such as silver, aluminum, gold, copper, platinum, nickel, palladium, iron, magnesium aluminum alloy, copper silver alloy, aluminum copper alloy, iron copper silver Alloys, etc., or metal carbon/nitride (MXene), graphene, graphite, carbon black, carbon fiber, single-walled carbon nanotubes, multi-walled carbon nanotubes with a two-dimensional layered structure, or containing PEDOT, PANi, One or several composites of conductive polymer materials such as Ppy, conductive elastomers, and conductive oxides.
  • various metals such as silver, aluminum, gold, copper, platinum, nickel, palladium, iron, magnesium aluminum alloy, copper silver alloy, aluminum copper alloy, iron copper silver Alloys, etc.
  • MXene metal carbon/nitride
  • the electrodes are placed in the same plane of the device structure and are separated from each other, respectively connected to three output ends of the driving voltage, and correspond to each sub-light-emitting layer in vertical space.
  • the electroluminescent tetrode further includes:
  • a first DC blocking layer located between the electrode layer and the light emitting layer;
  • the second DC blocking layer is located between the light emitting layer and the modulation layer.
  • the DC blocking layer 3 refers to a layer that blocks the passage of DC current.
  • the DC blocking layer (as shown in FIG. 10 ) may not be provided, or only one DC blocking layer 3 (such as 1-8), or two DC blocking layers 3 (as shown in FIG. 9 ), or multiple DC blocking layers. Setting one DC blocking layer can block the passage of DC current, and setting two or more DC blocking layers can more fully block the passing of DC current.
  • the first DC blocking layer is a dielectric layer; the second DC blocking layer is a dielectric layer.
  • the DC barrier layer is made of a dielectric material with a high dielectric constant, such as ceramic alumina, corundum, barium titanate, mullite, forsterite, magnesia, zirconia, zircon, boron nitride , aluminum nitride, beryllium oxide, spodumene and various glass ceramics, or polyvinylidene fluoride, polytetrafluoroethylene, polyvinylidene fluoride-trifluoroethylene copolymer (P(VDF- TrFE), P(VDF-TrFE-CTFE), P(VDF-TrFE-CFE)), polystyrene, polyvinyl alcohol, polyvinylpyrrolidone, polymethyl methacrylate, tetrafluoroethylene hexafluoropropyl copolymer , poly 4-methyl-1-pentene, polypropylene, polyethylene, polychlorotrifluoroethylene, polyphenylene oxide
  • the electroluminescent tetrode further includes:
  • the hole generating layer 4 is connected to the light emitting layer 5 .
  • the hole-generating layer refers to a layer that can generate holes. By generating holes through the hole-generating layer and increasing the concentration of holes, more holes and electrons can recombine and emit light on the light-emitting layer, which increases luminous efficiency.
  • One side of the hole-generating layer is connected to the light-emitting layer, and the other side of the hole-generating layer is connected to the electrode layer (or modulation layer).
  • a DC blocking layer can be set between the hole-generating layer and the electrode layer.
  • a DC blocking layer may also be provided between the layer and the modulation layer.
  • the DC blocking layer can also be arranged between the hole generating layer and the light emitting layer.
  • the hole generating layer is a stacked layer or a doped structure.
  • the carrier generation layer can generally be used as the hole generation layer, for example, the structure and material of the carrier generation layer widely used in stacked OLED devices is generally a stacked or doped structure. It can be roughly divided into the following types: N-type doped organic matter/inorganic metal oxide, N-type doped organic matter/organic matter, N-type doped organic matter/P-type doped organic matter, N-type organic matter/P-type organic matter .
  • the electroluminescent tetrode further includes:
  • the electron transport layer and the hole generation layer are respectively located on two sides of the light emitting layer.
  • an electron transport layer and an electron injection layer may be provided.
  • the electron transport layer and the electron injection layer are located between the electrode layer (or modulation layer) and the light-emitting layer.
  • the electron transport layer and the electron injection layer are arranged at the same time, the electron transport layer is located on the side close to the light-emitting layer, and the electron injection layer is located on the side close to the electrode.
  • the electron transport layer is connected to the light emitting layer, and the electron injection layer is connected to the electron transport layer.
  • a DC blocking layer may be provided between the electron injection layer and the electrode layer.
  • the DC blocking layer can also be arranged between the light emitting layer and the electron transport layer, or between the electron transport layer and the electron injection layer.
  • the material of the electron transport layer can be 1,3,5-tris(2-N-benzene-benzimidazole)benzene (TPBi), 1,3,5-tris[(3-pyridyl)-3-phenyl] Benzene (TmPyPB), 1,3-bis(3,5-dipyridin-3-ylphenyl)benzene (BmPyPhB) or 4,7-diphenyl-1,10-phenanthroline (Bphen), etc. are not limited to this.
  • TPBi 1,3,5-tris(2-N-benzene-benzimidazole)benzene
  • TmPyPB 1,3,5-tris[(3-pyridyl)-3-phenyl] Benzene
  • BmPyPhB 1,3-bis(3,5-dipyridin-3-ylphenyl)benzene
  • Bphen 4,7-diphenyl-1,10-phenanthroline
  • the material of the electron injection layer may be LiF, Cs 2 CO 3 or (8-hydroxyquinoline)lithium (Liq), but is not limited thereto.
  • the electroluminescent tetrode further includes:
  • the substrate 1 is connected with the modulation layer 2 or the electrode layer 8 .
  • each functional layer is usually prepared on the basis of a substrate, and finally the substrate can be removed or retained.
  • the modulation layer can be prepared on the substrate first, and the electrode layer can also be prepared on the substrate first, so the substrate is connected to the modulation layer, or the substrate is connected to the electrode layer.
  • the substrate can be any non-conductive solid material that can play a supporting role, including plastic, cloth, stone, cement board, ceramics, glass, leather, polymer resin board, wood, or metal material protected by an insulator such as plated plastic, glass Or ceramic metal plates, etc.
  • the shape of the substrate is also not limited, and it can be a substrate of any shape and any size.
  • the substrate is selected from but not limited to at least one of glass, quartz, sapphire or flexible organic materials (such as PET).
  • the light emitting colors of the sub-light emitting layers are different.
  • each sub-light emitting layer is different. It should be noted that at least two sub-light emitting layers may also have the same light emission color.
  • each sub-light-emitting layer is in a spiral shape, and each electrode is in a spiral shape.
  • each sub-light-emitting layer can be set as required, for example, a square, a circle, a rhombus, etc.
  • each sub-light-emitting layer is arranged in a spiral shape, specifically a planar spiral shape.
  • the sub-light-emitting layers are arranged in sequence.
  • the electrode layer is circular, and the electrode layer is divided into several parts by using line segments from the center of the electrode layer, that is to say, one end of several line segments is located at the center of the circle, and then Connect the other end of each line segment to the helix respectively, and an electrode is between the other two adjacent helixes.
  • the light-emitting layer is circular, and the center of the self-luminous layer uses line segments to divide the light-emitting layer into several parts. line, between the other two adjacent helixes is a sub-luminescent layer.
  • Figure 1 shows the structure of an organic electroluminescence tetrode (OLETe) in one embodiment designed according to the teachings of the present invention.
  • the device structure includes a substrate 1 , a modulation layer 2 , a DC blocking layer 3 , a hole generating layer 4 , a light emitting layer 5 , an electron transport layer 6 , an electron injection layer 7 and an electrode layer 8 from top to bottom.
  • the electrode layer 8 includes three coplanar electrodes (8-1, 8-2, 8-3) arranged at intervals, and each electrode is not in contact with each other.
  • the light-emitting layer includes three sub-light-emitting layers (5-1, 5-2, 5-3) that correspond one-to-one to the electrode layer in vertical space, and each light-emitting layer uses red, green, and blue organic light-emitting materials respectively. It is also possible to add an encapsulation layer on the top layer to isolate the influence of the external environment, or not to add it.
  • the DC blocking layer 3 can also be arranged on the surface of the electron injection layer 7, such that the electrodes 8-1, 8-2 and electrodes 8-3 are arranged at intervals on the surface of the DC blocking layer 3, as shown in FIG. 2.
  • the positions of the modulation layer 2 and the electrode layer 8 can be interchanged, such that the DC blocking layer 3 is disposed on the surface of the electrode layer 8 and the uncovered surface of the electrode layer 8 on the substrate 1, and the modulation layer 2 is disposed on the surface of the electron injection layer 7, as shown in FIG. 3 .
  • the DC blocking layer 3 is disposed on the surface of the electron injection layer 7 and the positions of the modulation layer 2 and the electrode layer 8 are exchanged, the device structure is shown in FIG. 4 .
  • the entire device can also adopt an inverted structure, placing the electron transport layer and the electron injection layer below the light-emitting layer, and placing the hole generation layer above the light-emitting layer, as shown in FIG. 5 .
  • the DC blocking layer 3 can also be arranged on the surface of the hole generating layer 4, such that electrodes, electrodes and electrodes are arranged at intervals on the surface of the DC blocking layer 3, as shown in FIG. 6 Show.
  • the positions of the modulation layer 2 and the electrode layer 8 can be interchanged, such that the DC blocking layer 3 is arranged on the surface of the electrode layer 8 and the uncovered surface of the electrode layer 8 on the substrate 1, while the modulation layer 2 is placed in the empty space.
  • the surface of the hole generating layer 4 is as shown in FIG. 7 . Wherein, when the DC blocking layer 3 is disposed on the surface of the hole generating layer 4 and the positions of the modulation layer 2 and the electrode layer 8 are exchanged, the device structure is shown in FIG. 8 .
  • the DC blocking layer can also be disposed on the surface of the modulation layer and the surface of the electron injection layer at the same time, as shown in FIG. 9 .
  • no direct current blocking layer may be applied, as shown in FIG. 10 .
  • the present invention also provides a preferred implementation of a preparation method for an electroluminescent tetrode that integrates light emission, switching, and color control. example:
  • the preparation method of the present invention comprises steps:
  • An electrode layer, a light-emitting layer and a modulation layer are sequentially prepared on the substrate, or a modulation layer, a light-emitting layer and an electrode layer are sequentially prepared on the substrate to obtain an electroluminescence tetrode.
  • the preparation method may further include the steps of:
  • the resulting electroluminescent tetrode then does not contain the substrate, and if the substrate is not removed, the resulting electroluminescent tetrode contains the substrate.
  • the electroluminescent tetrode may also include other functional layers, such as a DC blocking layer, a hole generating layer, an electron transport layer or an electron injection layer, and the preparation sequence of each functional layer may be set or not set according to requirements.
  • the present invention also provides a better implementation of a control method for an electroluminescent tetrode that integrates light emission, switching, and color control. example:
  • Control method of the present invention comprises steps:
  • the sub-light-emitting layer is made to emit light through the electrodes and the modulation layer.
  • the control signal includes: a high level and a low level, and the voltage of the high level may be greater than the peak voltage of the multi-phase alternating current.
  • the control signal includes a high level and a low level, the voltage of the high level is greater than the peak voltage of the polyphase alternating current, and the voltage of the low level may be 0V.
  • the sub-luminescent layer 5-1 adopts red luminescent material
  • the sub-luminescent layer 5-2 adopts green luminescent material
  • the sub-luminescent layer 5-3 adopts blue luminescent material.
  • Figure 12A- Figure 12J The chemical structural formulas and corresponding abbreviations of the organic materials used in this example are shown in Figure 12A- Figure 12J, and Figure 12A is HATCN (2,3,6,7,10,11-hexacyano-1,4,5,8 , 9,12-hexaazatriphenylene), Figure 12B is HTM (1-[4-(10-[1,1'-biphenyl]-4-yl-9-anthracenyl)phenyl]-2 -Ethyl-1H-benzimidazole), Figure 2C is H1(5-[3-(4,6-diphenyl-1,3,5-triazin-2-yl)phenyl]-5, 7-dihydro-7,7-dimethylindeno[2,1-b]carbazole), Figure 12D is H2(5,7-dihydro-7,7-dimethyl-5-phenyl- 2-(9-phenyl-9H-carbazol-3-yl)indeno[2,
  • EML-R is the light-emitting layer of the red light-emitting unit, which is composed of 65%H1:32.5%H2:2.5%RD;
  • EML-G is the light-emitting layer of the green light-emitting unit, consisting of 48.8%H1:48.8%H2:2.4%GD;
  • EML-B is the light-emitting layer of the blue light-emitting unit, which is composed of 90%H3:10%BD (50nm).
  • the ITO conductive thin film is the modulation layer material
  • the PVDF material is the DC blocking layer, which plays the role of blocking DC current
  • HATCN (10nm)/HTM (30nm) together constitute the hole generation layer
  • EML-R/G/B is the light emitting layer layer
  • ETM is the electron transport layer material
  • Liq is the electron injection layer material
  • aluminum is the electrode layer material.
  • the light-emitting units emit red, green, and blue lights respectively. Due to the small distance between the interdigitated electrodes, the three colors are mixed to display white in macroscopic view.
  • a digital signal is applied on top of the adjustment electrode layer for color adjustment.
  • the code bit of the control signal is 111111
  • the potential of the modulation layer is always higher than the potential of the electrode layer, and the direction of the electric field on both sides of the light-emitting layer in the three light-emitting units does not change, which is equivalent to applying a DC voltage, while Direct current cannot pass through the DC blocking layer, so the red, green and blue light emitting units do not emit light.
  • the control code is 101111, that is, the second time period of each driving voltage cycle is low level, and the rest of the time period is high level, only for the red light-emitting unit, in the second time period, the two sides of the light-emitting layer
  • the electric field has changed, and the alternating electric field can generate an AC signal through the DC blocking layer to drive the red light-emitting unit to emit light; while the control signal voltage of the blue and green light-emitting units is 0V even in the second time period, but because the blue light-emitting unit at this time
  • the driving voltage of the color and green light-emitting units is less than 0V, the potential of the modulation layer is still higher than the potential of the electrode layer, and the value of the potential difference is always greater than 0, always in the same direction.
  • the light-emitting brightness of the three light-emitting units can be controlled by adjusting the high-level amplitude of the control signal.
  • the following table shows the changes in the brightness of the red, green, and blue light-emitting units by changing the high-level amplitude of different control signals when the codes of the red, green, and blue light-emitting units are 101111, 111011, and 111110, respectively, when the effective value of the driving voltage is constant at 53V.

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Abstract

本发明公开了一种集发光、开关、颜色控制的电致发光四极管及其控制方法，电致发光四极管包括：依次设置的电极层，发光层以及调制层；所述发光层包括：至少两个子发光层；所述电极层包括：至少两个电极，相邻两个电极相互间隔设置；其中，所述电极与所述子发光层一一对应设置，所述调制层用于控制各子发光层。通过将发光层分成至少两个子发光层，并将电极层分成至少两个间隔设置的电极，电极与子发光层一一对应，因此，可以通过调制层分别控制各子发光层，这些子发光层可以形成一个像素，也就是说，给调制层一个控制信号，就可以集成化控制各子发光层。

Description

集发光、开关、颜色控制的电致发光四极管及其控制方法 技术领域
本发明涉及电致发光技术领域，尤其涉及的是一种集发光、开关、颜色控制的电致发光四极管及其控制方法。
背景技术
全彩显示单元是智能电子器件的重要组成部分，因此显示单元也和其他电子元器件一样，面临着小型化、集成化、智能化的需求。随着电子器件系统级集成概念的提出，越来越多的多功能电子器件引起了人们的兴趣。
另一方面，有机电子被认为是未来柔性电子的发展方向。近年来，有机晶体管(OTFT)的研究取得了显著的进展，利用有机晶体管的有源矩阵有机发光二极管(OLED)显示也有很多报道。在被广泛应用的主动矩阵OLED(AM-OLED)技术中，全彩显示的整个屏幕由多个像素点组成，每一个像素点都要包含分别发射红、绿、蓝色光的三个子像素，整个屏幕的像素点通过调整红、绿、蓝子像素的颜色配比来显示颜色。而每个子像素点的开关控制都需要通过至少一个晶体管来完成。
为了简化发光器件的结构，结合了OLED的发光功能和OTFT的电路调制功能的有机发光晶体管(OLET)被提出。该技术被认为有望实现简化的有机有源矩阵显示器，还有望提高像素孔径比、降低功耗等，受到了广泛的关注。
现有技术中，像素颜色控制逻辑复杂，需要分别对红色、绿色、蓝色发光子像素进行控制，无法通过一个信号进行集成化控制。
因此，现有技术还有待于改进和发展。
发明内容
本发明要解决的技术问题在于，针对现有技术的上述缺陷，提供一种模具、坩埚及晶体生长装置，旨在解决现有技术中无法通过一个信号进行集成化控制的问题。
本发明解决技术问题所采用的技术方案如下：
一种集发光、开关、颜色控制的电致发光四极管，其中，包括：依次设置的电极层，发光层以及调制层；
所述发光层包括：至少两个子发光层；
所述电极层包括：至少两个电极，相邻两个电极相互间隔设置；
其中，所述电极与所述子发光层一一对应设置，所述调制层用于控制各子发光层。
所述的集发光、开关、颜色控制的电致发光四极管，其中，所述电致发光四极管还包括：
第一直流阻挡层，位于所述电极层与所述发光层之间；和/或
第二直流阻挡层，位于所述发光层与所述调制层之间。
所述的集发光、开关、颜色控制的电致发光四极管，其中，所述第一直流阻挡层采用介电层；所述第二直流阻挡层采用介电层。
所述的集发光、开关、颜色控制的电致发光四极管，其中，所述电致发光四极管还包括：
空穴产生层，与所述发光层连接。
所述的集发光、开关、颜色控制的电致发光四极管，其中，所述空穴产生层为叠层或掺杂结构。
所述的集发光、开关、颜色控制的电致发光四极管，其中，所述电致发光四极管还包括：
电子传输层，与所述发光层连接；
电子注入层，与所述电子传输层连接；
其中，所述电子传输层与所述空穴产生层分别位于所述发光层的两侧。
所述的集发光、开关、颜色控制的电致发光四极管，其中，所述电致发光四极管还包括：
基底，与所述调制层或所述电极层连接。
所述的集发光、开关、颜色控制的电致发光四极管，其中，
各子发光层的发光颜色不相同；和/或
各子发光层呈螺旋状，各电极呈螺旋状；和/或
所述调制层采用电子导体层或离子导体层。
一种如上述任一项所述的集发光、开关、颜色控制的电致发光四极管的控制方法，其中，包括步骤：
对各电极分别施加多相交流电，并对所述调制层施加控制信号，以控制各电极各自分别对应的子发光层发光；其中，所述多相交流电的相数与所述电极的数量一致。
所述的集发光、开关、颜色控制的电致发光四极管的控制方法，其中，所述控制信号包括：高电平和低电平，所述高电平的电压大于所述多相交流电的峰值电压。
有益效果：通过将发光层分成至少两个子发光层，并将电极层分成至少两个间隔设置的电极，电极与子发光层一一对应，因此，可以通过调制层分别控制各子发光层，这些子发光层可以形成一个像素，也就是说，给调制层一个控制信号，就可以集成化控制各子发光层。
附图说明
图1为本发明实施例提供的调节电极在底直流阻挡层在底正置结构器件的结构示意图。
图2为本发明实施例提供的调节电极在底直流阻挡层在顶正置结构器件的结构示意图。
图3为本发明实施例提供的调节电极在顶直流阻挡层在底正置结构器件的结构示意图。
图4为本发明实施例提供的调节电极在顶直流阻挡层在顶正置结构器件的结构示意图。
图5为本发明实施例提供的调节电极在底直流阻挡层在底倒置结构器件的结构示意图。
图6为本发明实施例提供的调节电极在底直流阻挡层在顶倒置结构器件的结构示意 图。
图7为本发明实施例提供的调节电极在顶直流阻挡层在底倒置结构器件的结构示意图。
图8为本发明实施例提供的调节电极在顶直流阻挡层在顶倒置结构器件的结构示意图。
图9为本发明实施例提供的调节电极在底直流阻挡层在底部顶部均设置的正置结构器件的结构示意图。
图10为本发明实施例提供的调节电极在底无直流阻挡层的正置结构器件的结构示意图。
图11为本发明实施例1中的适用于三相电子器件电极的叉指电极示意图。
图12A-图12J为本发明实施例1中器件制备过程中使用的有机材料的结构式图。
图13为本发明实施例1中电致发光四极管的器件结构示意图。
图14为本发明实施例1中具有代表性的8各控制编码所表示的控制信号及其对应的驱动信号示意图。
图15为本发明实施例1中所有64种控制编码所表示的器件发光颜色状态在CIE坐标中的分布情况。
附图标记说明：
1、基底；2、调制层；3、直流阻挡层；4、空穴产生层；5、发光层；5-1、子发光层；5-2、子发光层；5-3、子发光层；6、电子传输层；7、电子注入层；8、电极层；8-1、电极；8-2、电极；8-3、电极。
具体实施方式
为使本发明的目的、技术方案及优点更加清楚、明确，以下参照附图并举实施例对本发明进一步详细说明。应当理解，此处所描述的具体实施例仅仅用以解释本发明，并不用于限定本发明。
请同时参阅图1-图15，本发明提供了一种集发光、开关、颜色控制的电致发光四 极管的一些实施例。
发明人经过研究发现，有机发光晶体管(OLET)目前依然至少具有以下一个或多个可改进之处：
(1)发光颜色无法调节，或只能在小范围内调节。目前的OLET技术只能实现单色光的发射和控制，为了实现进一步的系统化集成，所希望的技术应当可以满足一个器件同时发射红色、绿色、蓝色三种颜色的光，而无需将像素点再分为红、绿、蓝三个子像素。
(2)无法独立调节发光颜色和发光亮度。
(3)驱动电路和控制电路复杂。现有技术大多采用直流电或单相交流电来驱动发光单元，驱动电路需要复杂的后端设备实现交流-直流(AD)转换，增大静态功率损耗，增加集成电路的复杂程度并可能减小开口率。
(4)像素颜色控制逻辑复杂，无法通过一个信号进行集成化控制，需要分别对红色、绿色、蓝色发光子像素进行控制，不便于颜色的储存和提取。
本发明通过将发光层分成至少两个子发光层，并将电极层分成至少两个间隔设置的电极，电极与子发光层一一对应，因此，可以通过调制层分别控制各子发光层，这些子发光层可以形成一个像素，也就是说，给调制层一个控制信号，就可以集成化控制各子发光层。
如图1-图10所示，本发明的一种集发光、开关、颜色控制的电致发光四极管，包括：
依次设置的电极层8，发光层5以及调制层2；
所述发光层5包括：至少两个子发光层(5-1，5-2，5-3)；
所述电极层8包括：至少两个电极(8-1，8-2，8-3)，相邻两个电极(8-1，8-2，8-3)相互间隔设置；
其中，所述电极(8-1，8-2，8-3)与所述子发光层一一对应设置，所述调制层2用于控制各子发光层(5-1，5-2，5-3)。
值得说明的是，各子发光层可以采用相同或不相同的发光材料，也就是说，各子发 光层可以发出相同的光或不同的光。对于单个像素而言，为了使像素可以发出白光，通常像素至少包括三个子像素，三个子像素发出的光不同且可以混合形成白光。因此，为了使发光层发出白光，发光层包括至少三个子发光层，三个子发光层发出的光混合形成白光，举例说明，发光层至少有红色子发光层，蓝色子发光层以及绿色子发光层。通过在调制层连接调制信号，可以控制包含不同颜色子发光层的发光器件整体的开关和颜色变化，也就是说，调制层可以控制各子发光层的开关、发光亮度，从而调整整个发光层的开关、颜色。
具体地，以三个子发光层为例进行工作原理说明：
电致发光四极管(即器件)由三相交流电驱动，在器件的电极层8中的电极8-1、电极8-2和电极8-3分别施加三相交流电的三个相位差互为120度的具有适当幅值的正弦波输出电压。此时如果不在调制层施加控制信号，红、绿、蓝发光单元均发光。而如果在调制层施加控制信号，可以集成化地控制该器件红绿蓝发光单元分别具有不同的发光状态，如只有红光亮、只有绿光亮、只有蓝光亮、红光和绿光同时亮、红光和蓝光同时亮、绿光和蓝光同时亮、红绿蓝发光单元均不亮、或红绿蓝发光单元均发光但发光亮度比例不同等。利用上述原理制备叉指电极器件，如果叉指电极间距小于人眼分辨率，可以实现出射光在红光、绿光、蓝光之间的调节，调节范围可覆盖CIE坐标的一个平面区域。
本实施例具有如下优点：本实施例通过三种不同颜色发光单元横向并排列的方式，制备了颜色可调控的有机电致发光四极管。本器件可以实现三相交流电驱动发出三种颜色光，满足直接连接到电网中实现“即插即用”，并通过一个控制信号不仅控制三个发光单元的发光强度，还可以控制三种不同颜色光比例，实现颜色可调控。该器件系统级地集成了发光、开关和三维颜色控制功能，有望简化像素结构的制备工艺和成本，并使像素单元小型化，减少TFT开关器件的使用，增加开口率。
本发明中的有机电致发光四极管，使用易于商业化的材料制备，制备工艺简单，易于构成显示器中的像素点。
本申请的电致发光四极管可以采用LED(包括无机LED，有机LED，聚合物LED， 量子点LED，钙钛矿LED等)相关的材料，也就是说，现有的LED发光层均可以作为本申请电致发光四极管的发光层，现有的LED的电极层均可以作为本申请电致发光四极管的电极层。当然，LED的其它功能层，如空穴传输层，空穴注入层，电子传输层，电子注入层等，也可以应用于本申请电致发光四极管。当然，本申请的电致发光四极管的材料，并不限于本申请如下所罗列的材料，
具体地，各子发光层可以选择使用相同或不同的发光材料，分别可以独立地从以下材料中选择，包括聚合物有机发光材料、小分子有机荧光材料、小分子磷光发光材料、TADF热延迟发光材料。
聚合物有机发光材料包括但不限于Super yellow(超级黄，聚[{2,5-二(3',7'-二甲基辛氧基)-1,4-苯乙炔}-co-{3-(4'-(3”,7”-二甲基辛氧基)苯基)-1,4-苯乙炔}-co-{3-(3'-(3”,7”-二甲基辛氧基)苯基)-1,4-苯乙炔}])、Bu-PPP(聚(2,5-二丁氧基苯-1,4-二基))、PFO(聚(9,9-二正辛基芴基-2,7-二基))、PVK(聚(9-乙烯基咔唑))、F8BT(聚[(9,9-二辛基芴基-2,7-二基)-alt-(苯并[2,1,3]噻二唑-4,8-二基)])、MEH-PPV(聚[2-甲氧基-5-(2-乙基己氧基)-1,4-苯乙炔])、PFO(DMP end capped)(聚(9,9-二正辛基芴基-2,7-二基)，间二甲苯封端)、PFOPV(聚[(9,9-二正辛基芴基-2,7-亚苯基乙撑)-alt-(2-甲氧基-5-(2-乙基己氧基)-1,4二基)])、TFB(聚[(9,9-二正辛基芴基-2,7-二基)-alt-(4,4'-(N-(4-正丁基)苯基)-二苯胺)])、PFOBPA(聚(9,9-二辛基芴-2,7-二基)-alt-(N,N’-二苯基联苯胺-N,N’-二基))、PFB(聚[(N,N’-(4-正丁基苯基)-N,N’-二苯基-1,4-苯二胺)-alt-(9,9-二正辛基芴基-2,7-二基)])、MDMO-PPV(聚[2-甲氧基-5-[(3,7-二甲基辛氧基)-1,4-苯]-1,2-乙烯二基])、PCz(聚[9-(1-辛基壬基)-9H-咔唑])中的一种或者几种。
更优选的，小分子有机荧光或者磷光发光材料包括但不限于CBP(4,4-二(9-咔唑)联苯)、Alq3(三(8-羟基喹啉)铝)、TBCPF(9,9-二-4,4’-(3,6-二叔丁基咔唑基)-苯基芴)、mCP(1,3-二-9-咔唑基苯)、26DCzPPY(2,6-双((9H-咔唑-9-基)-3,1-亚苯基)吡啶)、Ir(mppy)3、Ir(piq)2(acac)、Ir(hpiq)3、Ir(ppy)3、Ir(bt)2(acac)、Ir(pbi)2(acac)、Ir(ppy)2(acac)、FCNIrPic、PhFIrPic、FirPic、PO-01-TB(乙酰丙酮酸二(4-(4-叔丁基-苯基)-噻吩[3,2-c]吡啶-C2,N)合铱(III))、PO-01(乙酰丙酮酸二(4-苯基-噻吩[3,2-c]吡啶-C2,N)合铱(III))、 6,12-dobenzylchrysene和α,β-AND系列中的一种或几种。
热激活延迟荧光(TADF)材料是继有机荧光材料和有机磷光材料之后发展的第三代有机发光材料。该类材料一般具有小的单线态-三线态能级差(DEST)，三线态激子可以通过反系间穿越转变成单线态激子发光。这可以充分利用电激发下形成的单线态激子和三线态激子，器件的内量子效率可以达到100％。同时，材料结构可控，性质稳定，价格便宜无需贵重金属，在OLEDs领域的应用前景广阔。更优选的，TADF热延迟发光材料包括但不限于BCPO(双-4(N-咔唑基苯基)苯基氧化膦)、2CzPN(4,5-二(9-咔唑基)-邻苯二腈)、4CzPN(3,4,5,6-四(9-咔唑基)-邻苯二腈)、4CzIPN(2,4,5,6-四(9-咔唑基)-间苯二腈)、4CzTPN(2,3,5,6-四(9-咔唑基)-对苯二腈)、4CzTPN-Bu(2,3,5,6-四(3,6-二叔丁基-9-咔唑基)-对苯二腈)、4CzPN-Ph(3,4,5,6-四(3,6-二苯基-9-咔唑基)-对苯二腈)、4CzTPN-Ph(2,3,5,6-四(3,6-二苯基-9-咔唑基)-对苯二腈)、4CzPN-Bu(3,4,5,6-四(3,6-二叔丁基-9-咔唑基)-对苯二腈)、DMAC-DPS(双[4-(9,9-二甲基-9,10-二氢吖啶)苯基]硫砜)、DPEPO(二[2-((氧代)二苯基膦基)苯基]醚)、2,6-双[4-二苯胺基苯基]-9,10-蒽醌中的一种或者几种。
TADF发光材料参考文献请见：
Scientific Reports,2015,5,8429；
Advanced Functional Materials,2014,24,6178-6186；
Nature Photonics,2014,8,326-332；
Advanced Materials,2014,26,5198-5204。
而本领域技术人员所熟知的与有机电致发光材料发光原理类似的无机发光材料或有机-无机杂化发光材料也可以在发光材料的选择范围之内。如钙钛矿发光材料、量子点发光材料、无机半导体LED材料等。
钙钛矿材料本身在390－790nm光谱范围内均可吸收，具备超大的光吸收系数，超低的体积缺陷密度，缓慢的俄歇复合以及平衡的双极性传输等特性，使得钙钛矿材料在高发光效率方面取得显著优势。同时，钙钛矿材料的可溶液加工、柔性器件制备等特性，使得工艺简单、价格低廉的大面积器件制备成为可能，使其在显示、照明和光通信方面 都有广泛的应用前景。更优选的，无机或者有机无机杂化钙钛矿发光材料为CsPbX 3,CH 3NH 3PbX 3、二维钙钛矿如(PMA) 2PbX 4或者(NMA) 2PbX 4中的一种或者几种(其中X＝Cl,Br or I，PMA为苯甲胺基团，NMA为萘甲胺基团)。
钙钛矿发光材料参考文献请见：
Advanced Functional Materials,2016,26,4797-4802；
Nature Photonics,2016,10,699-704；
Science,2015,350,1222-1225；
Advanced materials,2015,27,2311-2316；
Angewandte Chemie International Edition,2016,55,8328-8。
量子点材料，又可称为纳米晶，是一种由II－VI族或III－V族元素组成的纳米颗粒。量子点的粒径一般介于1～10nm之间，由于电子和空穴被量子限域，连续的能带结构变成具有分子特性的分立能级结构，受激后可以发射荧光。更优选的，量子点材料包括基于上述钙钛矿材料的3D或者2D钙钛矿量子点、碳量子点以及ZnS、ZnSe、ZnO、ZnTe、CdSe、CdS、CdTe、CaS、SrS。需要说明的是，上述量子点可为单组份、多组分、核壳结构等。同时其形貌可为纳米粒子、纳米带、纳米线等。
量子点发光材料相关参考文献请见：
Nature Photonics,2008,2,247-250；
Nano letters,2009,9,2532-2536；
Nature photonics,2013,7,407-412；
Organic Electronics,2003,4,123-130；
Advanced Materials,2010,22,3076-3080。
无机半导体LED发光材料由含镓(Ga)、砷(As)、磷(P)、氮(N)等的化合物制成。其发光原理与OLED大致相同，都是当电子与空穴复合时能辐射出可见光，因而也可以用来制成发光二极管和本申请中集发光、开关、颜色控制功能于一体的电致发光四极管。优选的，所述无机半导体LED发光材料可以由以下掺杂或非掺杂的材料中的其中一种或多种制成：铝砷化镓、砷化镓、砷化镓磷化物、磷化铟镓、铝磷化镓(掺杂氧化锌)、 铝磷化镓、铟氮化镓/氮化镓、磷化镓、磷化铟镓铝、铝磷化镓、磷化铝铟、镓砷化镓、磷化物、磷化铟镓铝、磷化镓、磷砷化镓、磷化镓、硒化锌、铟氮化镓、碳化硅、氮化镓、铟氮化镓、硒化锌、蓝宝石、硅、碳化硅、钻石、氮化铝、氮化铝镓等。优选的，由上述无机半导体LED发光材料作为发光层材料所制成的器件尺寸可以是纳米级，微米级或毫米级。更优选的，发光层由上述无机半导体LED发光材料中的一种或多种经过掺杂后形成的PN结组成。
需要说明的是。本发明所涉及发光层可进一步掺杂碳纳米管、纳米银线、金属氧化物等材料来提高其发光特性。
各电极的材料选择任意类型的导电材料，包括但不限于各种金属，如银、铝、金、铜、铂、镍、钯、铁、镁铝合金、铜银合金、铝铜合金、铁铜银合金等，或者为具有二维层状结构的金属碳/氮化物(MXene)、石墨烯、石墨、炭黑、碳纤维、单壁碳纳米管、多壁碳纳米管，或者为含有PEDOT、PANi、Ppy等的导电高分子材料、导电弹性体、导电氧化物中的一种或者几种复合。
在本发明实施例的一个较佳实现方式中，如图1-图10所示，所述调制层2采用电子导体层或离子导体层。
调制层可以是使用任意电子导体或离子导体材料，包括各种金属，如银、铝、金、铜、铂、镍、钯、铁、镁铝合金、铜银合金、铝铜合金、铁铜银合金等，或者为具有二维层状结构的金属碳/氮化物(MXene)、石墨烯、石墨、炭黑、碳纤维、单壁碳纳米管、多壁碳纳米管，或者为含有PEDOT、PANi、Ppy等的导电高分子材料、导电弹性体、导电氧化物中的一种或者几种复合。
在一种实施例中，各电极置于器件结构的同一平面内且相互分离，分别连接驱动电压的三个输出端，且与各子发光层在垂直空间上相互对应。
在本发明实施例的一个较佳实现方式中，如图1-图10所示，所述电致发光四极管还包括：
第一直流阻挡层，位于所述电极层与所述发光层之间；和/或
第二直流阻挡层，位于所述发光层与所述调制层之间。
具体地，直流阻挡层3是指阻挡直流电流通过的层，在电致发光四极管中，可以不设置直流阻挡层(如图10所示)，也可以只设置一个直流阻挡层3(如图1-8所示)，或两个直流阻挡层3(如图9所示)，或者多个直流阻挡层。设置一个直流阻挡层可以阻挡直流电流通过，设置两个或多个直流阻挡层可以更充分地阻挡直流电流通过。
在本发明实施例的一个较佳实现方式中，所述第一直流阻挡层采用介电层；所述第二直流阻挡层采用介电层。
具体地，直流阻挡层选用具有高介电常数的电介质材料，如陶瓷类的氧化铝、刚玉、钛酸钡、莫来石、镁橄榄石、氧化镁、氧化锆、锆英石、氮化硼、氮化铝、氧化铍、锂辉石及各种玻璃陶瓷等，或高分子塑料类的聚偏氟乙烯、聚四氟乙烯、聚偏二氟乙烯－三氟乙烯共聚物(P(VDF-TrFE)、P(VDF-TrFE-CTFE),P(VDF-TrFE-CFE))、聚苯乙烯、聚乙烯醇、聚乙烯吡咯烷酮、聚甲基丙烯酸甲酯、四氟乙烯六氟丙基共聚物、聚4-甲基-1-戊烯、聚丙烯、聚乙烯、聚三氟氯乙烯、聚苯醚、聚碳酸酯、乙基纤维素、CYTOP、聚对苯二甲酸乙二醇酯、派瑞林(对二甲苯聚合物)等。
在本发明实施例的一个较佳实现方式中，如图1-图10所示，所述电致发光四极管还包括：
空穴产生层4，与所述发光层5连接。
具体地，空穴产生层是指可以产生空穴的层，通过空穴产生层产生空穴，提高空穴的浓度，那么更多的空穴和电子可以在发光层上复合发光，也就提高了发光效率。空穴产生层的一侧与发光层连接，空穴产生层的另一侧与电极层(或调制层)连接，在空穴产生层与电极层之间可以设置直流阻挡层，在空穴产生层与调制层之间也可以设置直流阻挡层。当然直流阻挡层也可以设置在空穴产生层与发光层之间。
在本发明实施例的一个较佳实现方式中，所述空穴产生层为叠层或掺杂结构。
具体地，通常可以采用载流子产生层作为空穴产生层，例如，叠层OLED器件中被广泛使用的载流子产生层的结构和材料，一般为叠层或掺杂结构。大体分为以下几种类型：N型掺杂的有机物/无机金属氧化物，N型掺杂的有机物/有机物，N型掺杂的有机物/P型掺杂的有机物，N型有机物/P型有机物。
空穴产生层相关参考文献请见：
Advanced Functional Materials，2012，22(4)：855-860；
Advanced Materials，2006，18(3)：339—342；
Nanoscale,2020,12(32):17020-17028；
AIP Advances,2020,10(7):075316；
Organic Electronics,2020,83:105745；
Advanced Materials,2015,24(40):5408-5427。
在本发明实施例的一个较佳实现方式中，如图1-图10所示，所述电致发光四极管还包括：
电子传输层6，与所述发光层5连接；
电子注入层7，与所述电子传输层6连接；
其中，所述电子传输层与所述空穴产生层分别位于所述发光层的两侧。
具体地，为了提高电子的传输效率和注入效率，可以设置电子传输层和电子注入层。当然也可以仅设置电子传输层或电子注入层，也可以同时设置电子传输层和电子注入层(如图1-10所示)。电子传输层和电子注入层位于电极层(或调制层)与发光层之间，在同时设置电子传输层和电子注入层时，电子传输层位于靠近发光层的一侧，电子注入层位于靠近电极层(或调制层)的一侧，例如，电子传输层与发光层连接，电子注入层与电子传输层连接。电子注入层和电极层之间可以设置直流阻挡层。当然直流阻挡层还可以设置在发光层与电子传输层之间，或设置在电子传输层与电子注入层之间。
电子传输层的材料可以为1,3,5-三(2-N-苯-苯并咪唑)苯(TPBi)、1,3,5-三[(3-吡啶基)-3-苯基]苯(TmPyPB)、1,3-双(3,5-二吡啶-3-基苯基)苯(BmPyPhB)或4,7-二苯基-1,10-菲罗啉(Bphen)等不限于此。
电子注入层的材料可以为LiF、Cs 2CO 3或(8-羟基喹啉)锂(Liq)等不限于此。
在本发明实施例的一个较佳实现方式中，如图1-图10所示，所述电致发光四极管还包括：
基底1，与所述调制层2或所述电极层8连接。
具体地，在制备电致发光四极管时，通常在基底的基础上制备各功能层，最后可以去除基底，也可以保留基底。在制备电致发光四极管时，可以先在基底上制备调制层，也可以先在基底上制备电极层，因此，基底与调制层连接，或者基底与电极层连接。
基底可以是任何能起到支撑作用的非导体固体材料，包括塑料，布，石头，水泥板，陶瓷，玻璃，皮革，高分子树脂板，木材，或者是金属材料被绝缘体保护如镀塑料，玻璃或陶瓷的金属板材等。基底形状也不限，可以是任何形状任何尺寸大小基材。
优选的，基底选自但不仅限于玻璃、石英、蓝宝石或具有柔性有机材料(例如PET)中的至少一种。
在本发明实施例的一个较佳实现方式中，各子发光层的发光颜色不相同。
具体地，为了使电致发光四极管发出不同颜色的光，各子发光层发出光的颜色不同，需要说明的是，也可以有至少两个子发光层的发光颜色相同。
在本发明实施例的一个较佳实现方式中，如图1和图13所示，各子发光层呈螺旋状，各电极呈螺旋状。
各子发光层的形状可以根据需要设定，例如，采用正方形，圆形，菱形等，为了提高发光层的发光均匀性，将各子发光层设置成螺旋状，具体为平面螺旋状。各子发光层依次排列，例如，如图11所示，电极层呈圆形，自电极层的圆心采用线段先将电极层分成若干份，也就是说，若干个线段的一端位于圆心处，然后将各线段的另一端分别连接螺旋线，相邻另两个螺旋线之间即为一个电极。如图13所示，发光层呈圆形，自发光层的圆心采用线段先将发光层分成若干份，也就是说，若干个线段的一端位于圆心处，然后将各线段的另一端分别连接螺旋线，相邻另两个螺旋线之间即为一个子发光层。
图1显示了根据本发明内容设计的一个实施方案中有机电致发光四极管(OLETe)的结构。在此具体实施方案中，器件结构自上而下包括基底1、调制层2、直流阻挡层3、空穴产生层4、发光层5、电子传输层6、电子注入层7和电极层8。所述电极层8包括三个间隔排列的共平面电极(8-1，8-2，8-3)，各个电极之间互不接触。所述发光层包括在垂直空间上与电极层一一对应的三个子发光层(5-1，5-2，5-3)，各发光层分别使用红色、绿色、蓝色有机发光材料。还可以在最上层增设封装层，用于隔绝外界环境的影响， 也可以不增设。所述直流阻挡层3也可设置于电子注入层7的表面，如此所述电极8-1、电极8-2和电极8-3间隔排列的设置于所述直流阻挡层3的表面，如图2所示。其中，所述调制层2和电极层8的位置可以互换，如此所述直流阻挡层3设置于所述电极层8的表面以及基底1上电极层8未覆盖的表面，而调制层2置于电子注入层7的表面，如图3所示。其中，当所述直流阻挡层3设置于电子注入层7的表面，同时所述调制层2和电极层8的位置互换时，器件结构如图4所示。
整个器件还可以采用倒置结构，将电子传输层和电子注入层置于发光层下方，而将空穴产生层置于发光层上方，如图5所示。在此器件结构的基础上，所述直流阻挡层3也可设置于空穴产生层4的表面，如此电极、电极和电极间隔排列的设置于所述直流阻挡层3的表面，如图6所示。所述调制层2和电极层8的位置可以互换，如此所述直流阻挡层3设置于所述电极层8的表面以及基底1上电极层8未覆盖的表面，而调制层2置于空穴产生层4的表面，如图7所示。其中，当所述直流阻挡层3设置于空穴产生层4的表面，同时所述调制层2和电极层8的位置互换时，器件结构如图8所示。
根据器件控制需要，所述直流阻挡层也可以同时设置于调制层表面和电子注入层表面，如图9所示。或者也可以不施加直流阻挡层，如图10所示。
基于上述任一实施例的集发光、开关、颜色控制的电致发光四极管，本发明还提供了一种集发光、开关、颜色控制的电致发光四极管的制备方法的较佳实施例：
本发明制备方法包括步骤：
提供一基底；
在基底上依次制备电极层、发光层以及调制层，或者在基底上依次制备调制层、发光层以及电极层，得到电致发光四极管。
当然，在基底上依次制备电极层、发光层以及调制层，或者在基底上依次制备调制层、发光层以及电极层之后，制备方法还可以包括步骤：
去除基底。
那么得到的电致发光四极管中不含有基底，如果不去除基底，则得到的电致发光四极管含有基底。
在制备调制层、发光层以及电极层时，可以采用沉积的方式得到。当然，电致发光四极管还可以包括其它功能层，如，直流阻挡层、空穴产生层、电子传输层或电子注入层，根据需求，设置各功能层的制备顺序或不设置。
基于上述任一实施例的集发光、开关、颜色控制的电致发光四极管，本发明还提供了一种集发光、开关、颜色控制的电致发光四极管的控制方法的较佳实施例：
本发明控制方法包括步骤：
对各电极分别施加多相交流电，并对所述调制层施加控制信号，以控制各电极各自分别对应的子发光层发光；其中，所述多相交流电的相数与所述电极的数量一致。
通过对各电极分别施加多相交流电，并对调制层施加控制信号，从而通过电极和调制层使得子发光层发光。
所述控制信号包括：高电平和低电平，所述高电平的电压可以大于所述多相交流电的峰值电压。
控制信号包括高电平和低电平，高电平的电压大于多相交流电的峰值电压，低电平的电压可以是0V。
实施例1
本实施例中，子发光层5-1采用红色发光材料，子发光层5-2采用绿色发光材料，子发光层5-3采用蓝色发光材料，使用真空热蒸镀法制备了红、绿、蓝三色可调的电致发光晶体管，三种发光单元以叉指电极形状排列。三相叉指电极的形状如图11所示。本实施例中所用有机材料的化学结构式和对应简称如图12A-图12J所示，图12A为HATCN(2,3,6,7,10,11-六氰基-1,4,5,8,9,12-六氮杂苯并菲)，图12B为HTM(1-[4-(10-[1,1'-联苯]-4-基-9-蒽基)苯基]-2-乙基-1H-苯并咪唑)，图是2C为H1(5-[3-(4,6-二苯基-1,3,5-三嗪-2-基)苯基]-5,7-二氢-7,7-二甲基茚并[2,1-b]咔唑)，图12D为H2(5,7-二氢-7,7-二甲基-5-苯基-2-(9-苯基-9H-咔唑-3-基)茚并[2,1-b]咔唑)，图12E为H3(9-(1-萘基)-10-[4-(2-萘基)苯基]蒽)，图12F为RD(双[2,4-二甲基-6-[5-(2-甲基丙基)-2-喹啉基-κN]苯基-κC](2,4-戊二酮-κO2,κO4)铱)，图12G为GD(双[2-(2-吡啶基-N)苯基-C](2,4-戊二酮-O2,O4)铱(III))，图12H为BD(N,N'-双(2-甲基苯基)-N,N'-双(6-叔丁基二苯并呋喃-4- 基)芘-3,8-二胺)，图12I为ETM(1-[4-[10-(1,1'-联苯-4-基)蒽-9-基]苯基]-2-乙基-1H-苯并咪唑)，图12J为Liq(8-羟基喹啉锂)。用有机材料简称表达的具体器件结构和各层厚度为：
玻璃/ITO(120nm)/PVDF(700nm)/HATCN(10nm)/HTM(30nm)/EML-R/G/B(50nm)/ETM(30nm)/Liq(2.5nm)/铝(100nm)；器件结构如图11所示。
其中，EML-R为红色发光单元的发光层，由65％H1:32.5％H2:2.5％RD组成；
EML-G为绿色发光单元的发光层，由48.8％H1:48.8％H2:2.4％GD组成；
EML-B为蓝色发光单元的发光层，由90％H3:10％BD(50nm)组成。
其中，ITO导电薄膜为调制层材料；PVDF材料为直流阻挡层，起到阻挡直流电流的作用；HATCN(10nm)/HTM(30nm)共同构成空穴产生层；EML-R/G/B为发光层；ETM为电子传输层材料；Liq为电子注入层材料；铝为电极层材料。
在制备好的器件的电极层上对分离的三个电极分别施加峰值位V D的三相交流电的三个相位差互为120度的驱动电压时，发光单元分别发出红色、绿色、蓝色光，由于叉指电极间距小，宏观看到三种颜色混合而显示白色。在调节电极层上面施加数字信号，用于颜色调节。具体调节逻辑如下：
将三相电的一个周期分为6个均等的时间段，对6个时间段分别编码为高电平和低电平，高电平记为1，电压值为V C，低电平记为0，电压值为0V。其中V C>V D。图14的(a)-(h)显示了具有代表性的几个编码，编码内容随驱动电压周期的循环而循环。对于三相电驱动OLED的每个发光单元，尽管在交流电的反向周期不产生发光，但反向电压对于发光来说不可或缺。因此当控制信号编码位111111时，对于三个发光单元，调制层电位始终高于电极层电位，三个发光单元中发光层两侧的电场方向均不发生改变，相当于施加了直流电压，而直流电无法通过直流阻挡层，因此红绿蓝发光单元均不发光。而控制编码为101111时，即每个驱动电压周期的第二个时间段为低电平，其余时间段为高电平时，仅对于红色发光单元，在第二个时间段时发光层两侧的电场发生了改变，交变电场可以通过直流阻挡层产生交流信号，驱动红色发光单元发光；而蓝色和绿色发光单元即使在第二个时间段内，控制信号电压为0V，但由于此时蓝色和绿色发光单元 的驱动电压小于0V，调制层电位依然始终高于电极层电位，电势差的值始终大于0，始终是同一方向。因此只有红色发光单元正常工作，蓝色和绿色发光单元不工作。同理，控制编码为111011时只有绿色发光单元发光，控制编码为111110时只有蓝色发光单元发光。而六位数字进行编码，每个编码所控制的发光状态均不相同，因此共有2 6即64种发光状态。将所有发光状态收集到的的CIE坐标汇总如图15所示。黑色点代表各状态的CIE坐标点，可见颜色覆盖了CIE坐标的大面积区域，集中在白色三角形范围内，可在蓝色、绿色、红色之间调节。
进一步地，通过调节控制信号高电平幅值可以控制三个发光单元的发光亮度。下表展示了在驱动电压有效值恒定为53V时，红色、绿色、蓝色发光单元在编码分别为101111、111011、111110时，通过改变不同的控制信号高电平幅值亮度的变化。
表1
Figure PCTCN2021134464-appb-000001
应当理解的是，本发明的应用不限于上述的举例，对本领域普通技术人员来说，可以根据上述说明加以改进或变换，所有这些改进和变换都应属于本发明所附权利要求的保护范围。

Claims (10)

  1. 一种集发光、开关、颜色控制的电致发光四极管，其特征在于，包括：依次设置的电极层，发光层以及调制层；
    所述发光层包括：至少两个子发光层；
    所述电极层包括：至少两个电极，相邻两个电极相互间隔设置；
    其中，所述电极与所述子发光层一一对应设置，所述调制层用于控制各子发光层。
  2. 根据权利要求1所述的集发光、开关、颜色控制的电致发光四极管，其特征在于，所述电致发光四极管还包括：
    第一直流阻挡层，位于所述电极层与所述发光层之间；和/或
    第二直流阻挡层，位于所述发光层与所述调制层之间。
  3. 根据权利要求2所述的集发光、开关、颜色控制的电致发光四极管，其特征在于，所述第一直流阻挡层采用介电层；所述第二直流阻挡层采用介电层。
  4. 根据权利要求2所述的集发光、开关、颜色控制的电致发光四极管，其特征在于，所述电致发光四极管还包括：
    空穴产生层，与所述发光层连接。
  5. 根据权利要求4所述的集发光、开关、颜色控制的电致发光四极管，其特征在于，所述空穴产生层为叠层或掺杂结构。
  6. 根据权利要求4所述的集发光、开关、颜色控制的电致发光四极管，其特征在于，所述电致发光四极管还包括：
    电子传输层，与所述发光层连接；
    电子注入层，与所述电子传输层连接；
    其中，所述电子传输层与所述空穴产生层分别位于所述发光层的两侧。
  7. 根据权利要求1所述的集发光、开关、颜色控制的电致发光四极管，其特征在于，所述电致发光四极管还包括：
    基底，与所述调制层或所述电极层连接。
  8. 根据权利要求1-7任一项所述的集发光、开关、颜色控制的电致发光四极管，其特征在于，
    各子发光层的发光颜色不相同；和/或
    各子发光层呈螺旋状，各电极呈螺旋状；和/或
    所述调制层采用电子导体层或离子导体层。
  9. 一种如权利要求1-8任一项所述的集发光、开关、颜色控制的电致发光四极管的控制方法，其特征在于，包括步骤：
    对各电极分别施加多相交流电，并对所述调制层施加控制信号，以控制各电极各自分别对应的子发光层发光；其中，所述多相交流电的相数与所述电极的数量一致。
  10. 根据权利要求9所述的集发光、开关、颜色控制的电致发光四极管的控制方法，其特征在于，所述控制信号包括：高电平和低电平，所述高电平的电压大于所述多相交流电的峰值电压。
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