CN105845840B - It is inverted green light quantum point membrane electro luminescent device - Google Patents
It is inverted green light quantum point membrane electro luminescent device Download PDFInfo
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/14—Carrier transporting layers
- H10K50/15—Hole transporting layers
- H10K50/156—Hole transporting layers comprising a multilayered structure
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- H—ELECTRICITY
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
- H10K50/11—OLEDs or polymer light-emitting diodes [PLED] characterised by the electroluminescent [EL] layers
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- H—ELECTRICITY
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K2101/00—Properties of the organic materials covered by group H10K85/00
- H10K2101/40—Interrelation of parameters between multiple constituent active layers or sublayers, e.g. HOMO values in adjacent layers
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- H—ELECTRICITY
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- H10K2102/00—Constructional details relating to the organic devices covered by this subclass
- H10K2102/301—Details of OLEDs
- H10K2102/321—Inverted OLED, i.e. having cathode between substrate and anode
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K50/00—Organic light-emitting devices
- 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
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Abstract
The invention discloses one kind to be inverted green light quantum point membrane electro luminescent device, including substrate, negative electrode, electron transfer layer, green light quantum point luminescent layer, hole balance layer, hole transmission layer and the anode stacked gradually.Hole transmission layer includes the 3rd hole transmission layer, the second hole transmission layer and the first hole transmission layer stacked gradually.The thickness of hole balance layer is 5nm~10nm.The HOMO energy levels of 3rd hole transmission layer, the second hole transmission layer and the first hole transmission layer are sequentially reduced, so as to form steps potential barrier between green light quantum point luminescent layer and anode, reach the Hole injection capacity for stepping up hole transmission layer, meet the requirement of the hole injection of green light quantum point membrane electro luminescent device.Further, hole balance layer can prevent the first hole mobile material of high mobility and directly contacting for green light quantum point luminescent layer, avoid causing luminescence queenching.
Description
Technical field
The present invention relates to light emitting device technologies field, and green light quantum point TFEL device is inverted more particularly, to one kind
Part.
Background technology
Quantum dot (QDs, quantum dots) is semiconductor nano that some can not visually see, extremely small
Body, particle diameter are generally less than 10nm.Stimulated when by light or electricity, quantum dot can send coloured light, and the color of light is by measuring
The composition material and size shape of son point determine that this characteristic enables quantum dot to change the light color that light source is sent.By
In electronics, hole and exciton on three-dimensional space direction by quantum confinement so that QDs band structure by block continuous structure
Become the discrete energy level structure with molecular characterization.When the bohr of QDs particle diameters and ten thousand Neil excitons (Wannier exciton) half
Footpath (Bohr radius) is quite or more hour, the locality of electronics and coherence's enhancing, the absorption coefficient of exciton band increase, gone out
Existing exciton absorbs by force, can launch hyperfluorescence after being excited, and symmetrical emission spectrum, width and continuous absorption spectra etc. with narrow
Advantage.With QDs change in size, the effect of quantum effect enables it to gap width and changed therewith, so as to send different colours
Light.With light emitting diode with quantum dots made of QDs (QLEDs, quantum dot light emitting diodes) also by
This possesses the features such as high efficiency, rich in color, high stability.
However, the hole of traditional quantum dot film electroluminescent device (QLED) is not easy injection, it is necessary to high HOMO
The hole-injecting material of (Highest Occupied Molecular Orbital, highest occupied molecular orbital) energy level helps
The injection in hole.Especially for green light quantum point membrane electro luminescent device, the HOMO energy levels of green light quantum point are generally large,
About 6.5eV, and the work function of in general transparent anode is about less than 5.0eV, both differ farther out, cause in QLED devices
Hole injection barrier is universal higher, and the HOMO energy levels of conventional hole-injecting material are generally 5.0eV~5.5eV, Wu Faman
The requirement of sufficient hole injection.
The content of the invention
Based on this, it is necessary to provide a kind of inversion green light quantum point TFEL that can meet hole injection and require
Device.
One kind is inverted green light quantum point membrane electro luminescent device, including substrate, negative electrode, the electric transmission stacked gradually
Layer, green light quantum point luminescent layer, hole balance layer, hole transmission layer and anode；
The hole transmission layer includes the first hole transmission layer, the second hole transmission layer and the 3rd hole transport of stacking
Layer, the 3rd hole transmission layer directly contact with the hole balance layer, and the material of first hole transmission layer is first
The mixture that hole mobile material and the second hole mobile material are formed, the material of second hole transmission layer is the first hole
The mixture that transmission material and the 3rd hole mobile material are formed, the material of the 3rd hole transmission layer is the first hole transport
The mixture that material and the 4th hole mobile material are formed；
The material of the hole balance layer is the 4th hole mobile material, the thickness of the hole balance layer for 5nm~
10nm；
The HOMO energy levels of the hole balance layer are 6.04eV~6.5eV, the HOMO energy levels of the 3rd hole transmission layer
For 6.04eV~6.5eV, the HOMO energy levels of second hole transmission layer are 5.6eV~6.03eV, first hole transport
The HOMO energy levels of layer be 4.2eV~5.6eV, the 3rd hole transmission layer, second hole transmission layer and first sky
The HOMO energy levels of cave transport layer are sequentially reduced.
In one embodiment, the material of the green light quantum point luminescent layer is CdSe@ZnS core-shell structured quantum dots,
Wherein ,@represents cladding, and CdSe is the core of the nuclear shell structure quantum point, and ZnS is the shell of the nuclear shell structure quantum point.
In one embodiment, the thickness of the green light quantum point luminescent layer is 15nm~30nm.
In one embodiment, first hole mobile material, second hole mobile material, the 3rd sky
The HOMO energy levels of hole transport materials and the 4th hole mobile material increase successively.
In one embodiment, the first hole mobile material described in first hole transmission layer and the described second sky
The mass ratio of hole transport materials is 1:2~1:1, first hole mobile material is selected from molybdenum trioxide, tungstic acid, vanadium oxide
With one kind in titanium cyanines copper, second hole mobile material is selected from N, N '-two (1- naphthyls)-N, N '-diphenyl -1,1 '-connection
One kind in benzene -4-4 '-diamines and 2,2 ' two (3- dimethyl benzenes aminobenzene) 1,1' biphenyl.
In one embodiment, the first hole mobile material described in second hole transmission layer and the described 3rd sky
The mass ratio of hole transport materials is 1:3~1:2, first hole mobile material is selected from molybdenum trioxide, tungstic acid, vanadium oxide
With one kind in titanium cyanines copper, the 3rd hole mobile material is selected from 4,4'- double (9H- carbazole -9- bases) biphenyl, (4- of 8,8- bis-
(9 hydrogen-carbazole -9- bases) phenyl) -8 hydrogen-indoles [3,2,1-de] acridine and 3,5- bis- (9 hydrogen-carbazole -9- bases)-nitrogen, nitrogen-biphenyl
One kind in ammonia.
In one embodiment, the first hole mobile material described in the 3rd hole transmission layer and the described 4th sky
The mass ratio of hole transport materials is 1:3~1:2, first hole mobile material is selected from molybdenum trioxide, tungstic acid, vanadium oxide
With one kind in titanium cyanines copper, the 4th hole mobile material is selected from 2- hydroxy-3-methyl -2- cyclopentene-1-ones and 6,6- bis-
(4-9 hydrogen-carbazole -9- bases) phenyl) one kind in -6 hydrogen-pyrroles [3,2,1-de] acridine.
In one embodiment, the material of the hole balance layer is the 4th hole mobile material, the 4th hole
Transmission material is selected from 2- hydroxy-3-methyl -2- cyclopentene-1-ones and 6,6- bis- (4-9 hydrogen-carbazole -9- bases) phenyl) -6 hydrogen-pyrrole
Cough up one kind in [3,2,1-de] acridine.
In one embodiment, the thickness of the 3rd hole transmission layer is 10nm~20nm, and second hole passes
The thickness of defeated layer is 10nm~20nm, and the thickness of first hole transmission layer is 20nm~30nm.
In one embodiment, the one kind of the anode in aluminium, silver, gold and platinum.
Above-mentioned inversion green light quantum point membrane electro luminescent device, by setting hole balance layer, high migration can be prevented
First hole mobile material of rate directly contacts with green light quantum point luminescent layer, avoids causing luminescence queenching.First hole passes
Defeated layer, the second hole transmission layer and the 3rd hole transmission layer include the first hole mobile material, pass through the first hole transport material
Material adulterates with the second hole mobile material, the 3rd hole mobile material and the 4th hole mobile material respectively so that hole transport
Potential barrier change is gentle between layer, further reduces green glow QLED driving voltage.Hole balance layer and the 3rd hole transmission layer
HOMO energy levels are close with the HOMO energy levels of green light quantum point, the HOMO energy levels of the first hole transmission layer and the work function phase of anode
Closely, and the HOMO energy levels of the 3rd hole transmission layer, the second hole transmission layer and the first hole transmission layer are sequentially reduced, so as to
Steps potential barrier is formed between green light quantum point luminescent layer and anode, reaches the hole injection energy for stepping up hole transmission layer
Power, meet the requirement of the hole injection of green light quantum point membrane electro luminescent device.
Brief description of the drawings
Fig. 1 is the structural representation of the inversion green light quantum point membrane electro luminescent device of an embodiment；
Fig. 2 is the level structure principle schematic for being inverted green light quantum point membrane electro luminescent device；
Fig. 3 is the flow chart of the preparation method of the inversion green light quantum point membrane electro luminescent device of an embodiment；
Fig. 4 is respectively to the inversion green light quantum point thin-film electro in embodiment 1, embodiment 2, embodiment 3 and comparative example
Electroluminescence device carries out the result figure of luminance test.
Embodiment
It is described in further detail below mainly in combination with accompanying drawing to being inverted green light quantum point membrane electro luminescent device.
As shown in figure 1, the inversion green light quantum point membrane electro luminescent device 10 of an embodiment, including stack gradually
Substrate 100, negative electrode 200, electron transfer layer 300, green light quantum point luminescent layer 400, hole balance layer 500, hole transmission layer 600
And anode 700.
The material of substrate 100 can be glass, and glass transmission is good, and conveniently sputter or be deposited conducting film thereon.
The material of negative electrode 200 can be indium tin oxide (ITO), fluorine doped tin oxide (FTO), the zinc oxide (AZO) for mixing aluminium,
Indium-doped zinc oxide (IZO) etc..The thickness of negative electrode 200 can be 80nm~200nm.
Electron transfer layer 300 has preferable electron mobility, can be zinc oxide (ZnO) or titanium dioxide (TiO2) etc..
Specifically, the thickness of electron transfer layer 300 is 30nm~50nm.
The material of green light quantum point luminescent layer 400 is CdSe@ZnS core shell structure green light quantum points, wherein ,@represents cladding,
CdSe is the core of nuclear shell structure quantum point, and ZnS is the shell of nuclear shell structure quantum point.CdSe@ZnS core shell structure green light quantum points
Particle diameter is generally 6nm~15nm, and this nuclear shell structure quantum point, brightness is higher, and luminous efficiency is high.In present embodiment, CdSe@
The particle diameter of ZnS core shell structure green light quantum point is 12.5nm.
Specifically, the thickness of green light quantum point luminescent layer 400 is 15nm~30nm.
Hole transmission layer 600 includes the first hole transmission layer 610, the second hole transmission layer 620 and the 3rd hole transmission layer
630, the 3rd hole transmission layer 630 directly contacts with hole balance layer 500.The material of first hole transmission layer 610 is first empty
The mixture that hole transport materials (HTL1) and the second hole mobile material (HTL2) are formed, the material of the second hole transmission layer 620
The mixture formed for the first hole mobile material (HTL1) and the 3rd hole mobile material (HTL3), the 3rd hole transmission layer
630 material is the mixture that the first hole mobile material (HTL1) and the 4th hole mobile material (HTL4) are formed.
Specifically, the first hole mobile material (HTL1), the second hole mobile material (HTL2), the 3rd hole mobile material
(HTL3) and the HOMO energy levels of the 4th hole mobile material (HTL4) increase successively.First hole transmission layer 510, the second hole pass
The defeated hole transmission layer 530 of layer 520 and the 3rd forms doping system using two kinds of hole mobile material (HTL) doping.Compared to biography
A kind of only hole transmission layer of hole mobile material of system, doping system is formed by two kinds of hole mobile material (HTL) doping
Easily realize and obtain different HOMO energy levels, so as to form stair-stepping potential barrier.And the first hole transmission layer 610, second
The hole transmission layer 630 of hole transmission layer 620 and the 3rd includes the first hole mobile material (HTL1), passes through the first hole transport
Material (HTL1) respectively with the second hole mobile material (HTL2), the 3rd hole mobile material (HTL3) and the 4th hole transport material
Expect (HTL4) doping so that hole transmission layer 600 forms stair-stepping relationship between energy levels, and anode 700 arrives green light quantum point luminescent layer
Potential barrier change between 400 is gentle, reduces green glow QLED driving voltage.
Further, hole balance layer 500 is provided between hole transmission layer 600 and green light quantum point luminescent layer 400, it is empty
The material of cave balance layer 500 is the 4th hole mobile material (HTL4), and the thickness of hole balance layer 500 is 5nm~10nm.By
The relatively thin hole balance layer 500 that a layer thickness is 5nm~10nm is laminated on nearly green light quantum point luminescent layer 400, is ensureing foot
On the basis of enough hole injections, the leakage current of electroluminescent device can be effectively reduced, improves luminous efficiency.And hole is put down
Weighing apparatus layer 500 can prevent the first hole mobile material (HTL1) of high mobility and directly connecing for green light quantum point luminescent layer 400
Touch, avoid causing luminescence queenching.
The level structure principle schematic of green light quantum point membrane electro luminescent device 10 is inverted as shown in Fig. 2 first is empty
The material of cave transport layer 610 is the mixing that the first hole mobile material (HTL1) and the second hole mobile material (HTL2) are formed
Thing, the material of the second hole transmission layer 620 is the first hole mobile material (HTL1) and the 3rd hole mobile material (HTL3) shape
Into mixture, the material of the 3rd hole transmission layer 630 is the first hole mobile material (HTL1) and the 4th hole mobile material
(HTL4) mixture formed.The material of hole balance layer 500 is the 4th hole mobile material (HTL4).First hole transmission layer
610 HOMO energy levels are 4.2eV~5.6eV, and the HOMO energy levels of the second hole transmission layer 620 are 5.6eV~6.03eV, and the 3rd is empty
The HOMO energy levels of cave transport layer 630 are 6.04eV~6.5eV, and the HOMO energy levels of hole balance layer are 6.04eV~6.5eV, first
The HOMO energy levels of hole transmission layer 610, the second hole transmission layer 620 and the 3rd hole transmission layer 630 increase successively.Put down in hole
The HOMO energy levels of weighing apparatus layer 500 can be equal to or more than the HOMO energy levels of the 3rd hole transmission layer 630.First hole transmission layer 610
HOMO energy levels and anode work function number (for example, Al work function is 4.0eV or so) it is close, and the 3rd hole transmission layer 630
The HOMO energy levels (generally 6.5eV or so) of HOMO energy levels and green light quantum point luminescent layer 400 are close, pass through the first hole transport
Layer the 610, second hole transmission layer 620 and the 3rd hole transmission layer 630 form stair-stepping relationship between energy levels, when hole from anode to
When cathode direction migrates, hole injection barrier is small, reaches the Hole injection capacity for stepping up sub- hole transmission layer, meets green glow
The requirement of the hole injection of quantum dot film electroluminescent device.Further, it is the 4th by the material of hole balance layer 500
Hole mobile material (HTL4), with containing the 4th common hole mobile material (HTL4), a side in the 3rd hole transmission layer 630
Face is advantageous to hole and enters hole balance layer 500 from the 3rd hole transmission layer 630, and another aspect hole balance layer 500 can
The first hole mobile material (HTL1) of high mobility and directly contacting for green light quantum point luminescent layer 400 are prevented, avoids causing
Luminescence queenching.
Traditional quantum dot film electroluminescent device for just putting structure, because quantum dot light emitting layer (QDs luminescent layers) needs
To be prepared using solwution method, when preparing hole transmission layer 600, solwution method limits hole injection and hole mobile material
It is alternative.The green light quantum point membrane electro luminescent device 10 of the present invention uses inverted structure, anode 700 in the superiors, from
Substrate 100 is farthest.Hole transmission layer 600 can green light quantum point luminescent layer 400 preparation after the completion of with the mode of vacuum evaporation come
Prepare, therefore the high HOMO energy levels hole mobile material selectable range matched with green light quantum point luminescent layer 400 is wider.
Specifically, the first hole mobile material (HTL1) is selected from molybdenum oxide (MoO3), tungstic acid (WO3), vanadium oxide
(V2O5) and titanium cyanines copper (CuPc) in one kind.In general, HTL1 HOMO energy levels are typically relatively low, close to the work content of anode 700
Number so that hole easily enters in the first hole transmission layer 610 from the conduction of anode 700, improves luminous efficiency.
Second hole mobile material (HTL2) is selected from N, and N '-two (1- naphthyls)-N, N '-diphenyl -1,1 '-biphenyl -4-4 ' -
One kind in diamines (NPB) and 2,2 ' two (3- dimethyl benzenes aminobenzene) 1,1' biphenyl (BTPD).In general, HTL2 HOMO energy
Level is more than HTL1 HOMO energy levels.
3rd hole mobile material (HTL3) is selected from 4,4'- double (9H- carbazole -9- bases) biphenyl (CBP), (4- (9 of 8,8- bis-
Hydrogen-carbazole -9- bases) phenyl) -8 hydrogen-indoles [3,2,1-de] acridine (FPCC) and 3,5- bis- (9 hydrogen-carbazole -9- bases)-nitrogen, nitrogen -
One kind in biphenyl ammonia (DCDPA).In general, HTL3 HOMO energy levels are more than HTL2 HOMO energy levels.
4th hole mobile material (HTL4) is selected from 2- hydroxy-3-methyl -2- cyclopentene-1-ones (mCP) and (4- of 6,6- bis-
9 hydrogen-carbazole -9- bases) phenyl) one kind in -6 hydrogen-pyrroles [3,2,1-de] acridine (BCPPA).HTL4 HOMO energy levels one compared with
Height, close to the HOMO energy levels of green light quantum point luminescent layer 400 so that hole is easily conducted from the 3rd hole transmission layer 630 to be entered
In green light quantum point luminescent layer 400, luminous efficiency is improved.
Specifically, the first hole mobile material (HTL1) and the second hole mobile material in the first hole transmission layer 610
(HTL2) mass ratio is 1:2~1:1, the first hole mobile material (HTL1) is selected from molybdenum oxide (MoO3), tungstic acid (WO3)、
Vanadium oxide (V2O5) and titanium cyanines copper (CuPc) in one kind, the second hole mobile material (HTL2) is selected from N, N '-two (1- naphthyls)-
N, N '-diphenyl -1,1 '-biphenyl -4-4 '-diamines (NPB) and 2,2 ' two (3- dimethyl benzenes aminobenzene) 1,1' biphenyl (BTPD)
In one kind.
The matter of first hole mobile material (HTL1) and the 3rd hole mobile material (HTL3) in second hole transmission layer 620
Amount is than being 1:3~1:2.First hole mobile material (HTL1) is selected from molybdenum oxide (MoO3), tungstic acid (WO3), vanadium oxide
(V2O5) and titanium cyanines copper (CuPc) in one kind, the 3rd hole mobile material (HTL3) is selected from 4,4'- double (9H- carbazole -9- bases) connection
Benzene (CBP), (4- (9 hydrogen-carbazole -9- bases) phenyl) -8 hydrogen-indoles [3,2,1-de] acridines (FPCC) of 8,8- bis- and 3,5- bis- (9
Hydrogen-carbazole -9- bases)-nitrogen, one kind in nitrogen-biphenyl ammonia (DCDPA).
The matter of first hole mobile material (HTL1) and the 4th hole mobile material (HTL4) in 3rd hole transmission layer 630
Amount is than being 1:3~1:2, the first hole mobile material (HTL1) is selected from molybdenum oxide (MoO3), tungstic acid (WO3), vanadium oxide
(V2O5) and titanium cyanines copper (CuPc) in one kind, the 4th hole mobile material (HTL4) be selected from 2- hydroxy-3-methyl -2- cyclopentene -
1- ketone (mCP) and 6,6- bis- (4-9 hydrogen-carbazole -9- bases) phenyl) in -6 hydrogen-pyrroles [3,2,1-de] acridine (BCPPA) one
Kind.
The material of hole balance layer 500 is the 4th hole mobile material (HTL4), and the 4th hole mobile material (HTL4) selects
From 2- hydroxy-3-methyl -2- cyclopentene-1-ones (mCP) and 6,6- bis- (4-9 hydrogen-carbazole -9- bases) phenyl) -6 hydrogen-pyrroles [3,
2,1-de] one kind in acridine (BCPPA).
The material of first hole transmission layer 610, the second hole transmission layer 620 and the 3rd hole transmission layer 630 is two kinds
The mixture that hole mobile material (HTL) is formed, by the quality for adjusting HTL1 and HTL2 in the first hole transmission layer 610 respectively
HTL1 and HTL4 matter in mass ratio and the 3rd hole transmission layer 630 than HTL1 and HTL3 in, the second hole transmission layer 620
Ratio is measured, the first hole transmission layer 610 of multiple different HOMO energy levels, the second hole transmission layer 620 and the can be obtained respectively
Three hole transmission layers 630, so as to which the HOMO energy levels formed layer by layer successively decrease relation, the green light quantum point luminescent layer 400 and anode made
Potential barrier change between 600 is gentle, beneficial to the transmission in hole, improves luminous efficiency.And it is undoped in hole balance layer 500
Mode, it is made of the 4th hole mobile material (HTL4).Three layers of hole transmission layer 600 adulterated and one layer of undoped hole
Balance layer 500 coordinates so that and hole is very easily passed in hole transmission layer 600 by the potential barrier of step type from anode, then
The first hole mobile material (HTL1) and green light quantum point luminescent layer 400 of high mobility are prevented by hole balance layer 500
Directly contact, can avoid causing luminescence queenching.
Specifically, hole balance layer 500, the 3rd hole transmission layer 630, the second hole transmission layer 620 and the first hole pass
The thickness of defeated layer 610 increases successively.The thickness of the hole balance layer 500 directly contacted with green light quantum point luminescent layer 400 is
5nm~10nm, because balance layer 500 kinds of hole mobilities in hole are relatively low, 5nm~10nm relatively thin thickness is ensureing enough
On the basis of the injection of hole, the leakage current of electroluminescent device is effectively reduced, improves luminous efficiency.First hole transmission layer
610th, the thickness of the second hole transmission layer 620 and the 3rd hole transmission layer 630 determines according to the property of hole mobile material.
Specifically, the thickness of the 3rd hole transmission layer 630 is 10nm~20nm, the thickness of the second hole transmission layer 620 is
10nm~20nm, the thickness of the first hole transmission layer 610 is 20nm~30nm.
Traditional QLED only has the hole transmission layer 600 of individual layer, or has sandwich construction, is typically also to make identical thickness
Degree, due to hole, the mobility at each position is not quite similar in hole transmission layer 600 and hole balance layer 500, hole transport
Efficiency it is low.Hole balance layer 500, the 3rd hole transmission layer 630, the second hole transmission layer 620 and the first hole transmission layer 610
Thickness increase successively.According to the change of stair-stepping potential barrier and hole mobility, each layer of hole transmission layer is rationally designed
Thickness, the efficiency of transmission in hole is improved, and then improve QLED luminous efficiency.
The one kind of anode 600 in aluminium, silver, gold and platinum.Aluminium (Al), silver-colored (Ag), the work function of golden (Au) and platinum (Pt)
It is higher, be advantageous to reduce the barrier potential difference between anode 600 and green light quantum point luminescent layer 400.
Specifically, the thickness of anode 600 is 100nm~150nm.
Above-mentioned inversion green light quantum point membrane electro luminescent device 10, one layer is laminated on green light quantum point luminescent layer 400
Thickness is 5nm~10nm relatively thin hole balance layer 500, on the basis of enough hole injections are ensured, can effectively be dropped
The leakage current of low electroluminescent device, improve luminous efficiency.Hole balance layer 500 can prevent the first hole of high mobility from passing
Defeated material (HTL1) directly contacts with green light quantum point luminescent layer 400, avoids causing luminescence queenching.First hole transmission layer
610th, 630 layers of the second hole transmission layer 620 and the 3rd hole transport include the first hole mobile material (HTL1), pass through first
Hole mobile material (HTL1) is empty with the second hole mobile material (HTL2), the 3rd hole mobile material (HTL3) and the 4th respectively
Hole transport materials (HTL4) adulterate so that potential barrier change is gentle between hole transmission layer 600, further reduces green glow QLED drive
Dynamic voltage.The HOMO energy levels of the hole transmission layer 630 of hole balance layer 500 and the 3rd are close with the HOMO energy levels of green light quantum point,
The HOMO energy levels of first hole transmission layer 610 are close with the work function of anode 700, and hole balance layer 500, the 3rd hole pass
The HOMO energy levels of defeated layer 630, the second hole transmission layer 620 and the first hole transmission layer 610 are sequentially reduced, so as in green quantum
Steps potential barrier is formed between point luminescent layer 400 and anode 700, reaches the hole injection energy for stepping up hole transmission layer 600
Power, meet the requirement of the hole injection of green light quantum point membrane electro luminescent device 10.
In addition, the present invention also provides a kind of preparation method of above-mentioned inversion green light quantum point membrane electro luminescent device 10,
As shown in figure 3, this method comprises the following steps S110~S140.
S110, substrate is provided, negative electrode is formed in substrate.
The material of substrate can be glass, can respectively be ultrasonically treated substrate with detergent, acetone, ethanol and isopropanol successively
15min.Evaporation, spraying plating, sputtering or electrochemistry hydatogenesis form negative electrode in substrate afterwards.The material of negative electrode can be indium tin
Oxide (ITO), fluorine doped tin oxide (FTO), the zinc oxide (AZO) for mixing aluminium, indium-doped zinc oxide (IZO) etc., the thickness of negative electrode
For 80nm~200nm.
Preferably, indium tin oxide (ITO) is sputtered onto in substrate of glass using the method for sputtering.
In present embodiment, after forming negative electrode in substrate, include to formed the substrate of negative electrode use successively detergent,
Acetone, ethanol and isopropanol are respectively ultrasonically treated 15min, then carry out UV ozone (UV-ozone) processing 15min.
Electron transfer layer and green light quantum point luminescent layer are sequentially formed on S120, the negative electrode obtained in S110.
Electron transfer layer can be prepared on negative electrode conducting film using solution spin-coating method, electron transfer layer can be zinc oxide
Or titanium dioxide (TiO (ZnO)2) etc., thickness 30nm~50nm of electron transfer layer.
Equally, green light quantum point luminescent layer, green light quantum point hair can be formed on the electron transport layer using solution spin-coating method
The thickness of photosphere is 15nm~30nm.The material of green light quantum point luminescent layer can be CdSe ZnS core shell structure green quantums
Point.
Hole balance layer, hole transmission layer are formed on S130, the green light quantum point luminescent layer obtained in S120, hole passes
Defeated layer includes the 3rd hole transmission layer, the second hole transmission layer and the first hole transmission layer stacked gradually.
Hole balance layer can be formed on green light quantum point luminescent layer using vacuum vapour deposition, the material of hole balance layer is
4th hole mobile material (HTL4), the thickness of hole balance layer is 5nm~10nm.Then the 3rd is formed on the balance layer of hole
Hole transmission layer, the material of the 3rd hole transmission layer is the first hole mobile material (HTL1) and the 4th hole mobile material
(HTL4) mixture formed, the thickness of the 3rd hole transmission layer is 10nm~20nm.The vacuum on the 3rd hole transmission layer again
Evaporation forms the second hole transmission layer, and the material of the second hole transmission layer is the first hole mobile material (HTL1) and the 3rd hole
The mixture that transmission material (HTL3) is formed, the thickness of the second hole transmission layer can be 10nm~20nm.It is empty second afterwards
Vacuum evaporation forms the first hole transmission layer in the transport layer of cave, and the material of the first hole transmission layer is the first hole mobile material
(HTL1) and the mixture that is formed of the second hole mobile material (HTL2), the thickness of the first hole transmission layer can be 20nm~
30nm。
S140, obtain in S130 forming anode on the first hole transmission layer.
Anode can be formed on the first hole transmission layer using evaporation, spraying plating, sputtering or the method for electrochemistry hydatogenesis.
The material of anode may be selected from one kind in aluminium, silver, gold and platinum.
This preparation method for being inverted green light quantum point membrane electro luminescent device, technique are simple, easy to operate.It is prepared
Green light quantum point membrane electro luminescent device green light quantum point luminescent layer and anode between form steps potential barrier, hole passes
The Hole injection capacity of defeated layer is strong, meets the requirement of the hole injection of green light quantum point membrane electro luminescent device.Further set
Cave balance layer is empty, the first hole mobile material of high mobility can be prevented directly to be contacted with green light quantum point luminescent layer, kept away
Exempt to cause luminescence queenching.
It is embodiment part below.
In following examples, unless otherwise instructed, the experimental method of unreceipted actual conditions, generally according to normal condition,
Experiment material used is purchased from Sigma-Aldrich (Shanghai) trade Co., Ltd, lark prestige Science and Technology Ltd..
Embodiment 1
The structure for being inverted green light quantum point membrane electro luminescent device is substrate, negative electrode, electron transfer layer, green light quantum point
Luminescent layer, hole balance layer, hole transmission layer and anode.First hole transmission layer of its hole-transporting layer including stacking,
Second hole transmission layer and the 3rd hole transmission layer.3rd hole transmission layer directly contacts with hole transmission layer.Hole balance layer
Thickness be 8nm, the material of hole balance layer is the 4th hole mobile material (HTL4), and HTL4 is 2- hydroxy-3-methyl -2- rings
Amylene -1- ketone (mCP).The thickness of 3rd hole transmission layer is 15nm, and the material of the 3rd hole transmission layer is the first hole transport
The mixture that material (HTL1) and the 4th hole mobile material (HTL4) are formed, wherein HTL1 is molybdenum oxide (MoO3), HTL4 is
2- hydroxy-3-methyl -2- cyclopentene-1-ones (mCP), MoO3It is 1 with mCP mass ratioes:3.The thickness of second hole transmission layer is
15nm, the material of the second hole transmission layer is the first hole mobile material (HTL1) and the formation of the 3rd hole mobile material (HTL3)
Mixture, wherein HTL1 is molybdenum oxide (MoO3), double (9H- carbazole -9- bases) biphenyl (CBP) of HTL3 4,4'-, MoO3With CBP
Mass ratio is 1:2.The thickness of first hole transmission layer is 25nm, and the material of the first hole transmission layer is the first hole mobile material
(HTL1) and the second hole mobile material (HTL2) formed mixture, wherein HTL1 is molybdenum oxide (MoO3), HTL2 N, N '-
Two (1- naphthyls)-N, N '-diphenyl -1,1 '-biphenyl -4-4 '-diamines (NPB), MoO3It is 1 with NPB mass ratioes:1.
The specific preparation process for being inverted green light quantum point membrane electro luminescent device is as follows：
Substrate of glass is respectively ultrasonically treated 15min with detergent, acetone, ethanol and isopropanol successively.Then in glass base
A layer thickness is sputtered on bottom and is 150nm ITO conducting films, then carries out UV ozone (UV-ozone) processing 15min.Then use
Solution spin-coating method prepares ZnO electron transfer layers in full of nitrogen and the extremely low glove box of water oxygen content, using 20mg/ml's
ZnO nano particle ethanol solution, it is 1500 revs/min (Resolutions per minute, rpm) in rotating speed, temperature 150
Anneal 30min at DEG C, and the thickness of ZnO electron transfer layers is 40nm.Green light quantum point is prepared on the electron transport layer afterwards to light
Layer, using 20mg/ml green glow CdSe@ZnS quantum dot toluene solutions, in rotating speed 2000rpm, temperature is to be annealed at 150 DEG C
30min, green light quantum point light emitting layer thickness are 20nm.Device is transferred to pressure as 10 afterwards-4In high vacuum cavity under Pa,
MCP vacuum evaporations are formed to 8nm hole balance layer successively, are then 1 by mass ratio:3 MoO3Formed with mCP vacuum evaporations
3rd hole transmission layer, then by mass ratio be 1:2 MoO3The second hole transmission layer is formed with CBP vacuum evaporations, afterwards by matter
Amount is than being 1:1 MoO3The first hole transmission layer is formed with NPB vacuum evaporations.Last vacuum evaporation 100nm Al electrode conducts
Anode, obtain being inverted green light quantum point membrane electro luminescent device.
Hole balance layer, the 3rd hole transmission layer, the second hole transmission layer and the first hole transmission layer are surveyed respectively
Examination, the HOMO energy levels of hole balance layer are 6.1eV, and the HOMO energy levels of the 3rd hole transmission layer are 6.1eV, the second hole transmission layer
HOMO energy levels be 5.9eV, the HOMO energy levels of the first hole transmission layer are 5.4eV.
Luminance test is carried out to the inversion green light quantum point membrane electro luminescent device being prepared, as a result as shown in Figure 4.
From fig. 4, it can be seen that inversion green light quantum point membrane electro luminescent device brightness height in embodiment 1 is apparently higher than comparative example.
Embodiment 2
The thickness of hole balance layer is 5nm in the inversion green light quantum point membrane electro luminescent device of the present embodiment, hole
The material of balance layer is HTL4, HTL4 mCP.The thickness of 3rd hole transmission layer is 10nm, the material of the 3rd hole transmission layer
The mixture formed for HTL1 and HTL4, wherein HTL1 is MoO3, HTL4 mCP, MoO3It is 1 with mCP mass ratioes:2.Second is empty
The thickness of cave transport layer is 11nm, and the material of the second hole transmission layer is the mixture that HTL1 and HTL3 is formed, and wherein HTL1 is
MoO3, HTL3 CBP, MoO3It is 1 with CBP mass ratioes:3.The thickness of first hole transmission layer is 20nm, the first hole transmission layer
The mixture that is formed for HTL1 and HTL2 of material, wherein HTL1 is MoO3, HTL2 NPB, MoO3It is 1 with NPB mass ratioes:2.
Remaining is same as Example 1.
The specific preparation method for being inverted green light quantum point membrane electro luminescent device is same as Example 1.
Hole balance layer, the 3rd hole transmission layer, the second hole transmission layer and the first hole transmission layer are surveyed respectively
Examination, the HOMO energy levels of hole balance layer are 6.1eV, and the HOMO energy levels of the 3rd hole transmission layer are 6.1eV, the second hole transmission layer
HOMO energy levels be 5.9eV, the HOMO energy levels of the first hole transmission layer are 5.4eV.
Luminance test is carried out to the inversion green light quantum point membrane electro luminescent device being prepared, as a result as shown in Figure 4.
From fig. 4, it can be seen that inversion green light quantum point membrane electro luminescent device brightness height in embodiment 2 is apparently higher than comparative example.
Embodiment 3
The thickness of hole balance layer is 10nm in the inversion green light quantum point membrane electro luminescent device of the present embodiment, hole
The material of balance layer is HTL4, HTL4 mCP.The thickness of 3rd hole transmission layer is 18nm, the material of the 3rd hole transmission layer
The mixture formed for HTL1 and HTL4, wherein HTL1 is MoO3, HTL4 mCP, MoO3It is 1 with mCP mass ratioes:3.Second is empty
The thickness of cave transport layer is 20nm, and the material of the second hole transmission layer is the mixture that HTL1 and HTL3 is formed, and wherein HTL1 is
MoO3, HTL3 CBP, MoO3It is 1 with CBP mass ratioes:2.The thickness of first hole transmission layer is 30nm, the first hole transmission layer
The mixture that is formed for HTL1 and HTL2 of material, wherein HTL1 is MoO3, HTL2 NPB, MoO3It is 1 with NPB mass ratioes:1.
Remaining is same as Example 1.
The specific preparation method for being inverted green light quantum point membrane electro luminescent device is same as Example 1.
Hole balance layer, the 3rd hole transmission layer, the second hole transmission layer and the first hole transmission layer are surveyed respectively
Examination, the HOMO energy levels of hole balance layer are 6.1eV, and the HOMO energy levels of the 3rd hole transmission layer are 6.1eV, the second hole transmission layer
HOMO energy levels be 5.9eV, the HOMO energy levels of the first hole transmission layer are 5.4eV.
Luminance test is carried out to the inversion green light quantum point membrane electro luminescent device being prepared, as a result as shown in Figure 4.
From fig. 4, it can be seen that inversion green light quantum point membrane electro luminescent device brightness height in embodiment 2 is apparently higher than comparative example.
Embodiment 4
The thickness of hole balance layer is 6nm in the inversion green light quantum point membrane electro luminescent device of the present embodiment, hole
The material of balance layer is HTL4, HTL4 BCPPA.The thickness of 3rd hole transmission layer is 12nm, the material of the 3rd hole transmission layer
Expect the mixture for HTL1 and HTL4 formation, wherein HTL1 is WO3, HTL4 BCPPA, WO3It is 1 with BCPPA mass ratioes:3.The
The thickness of two hole transmission layers is 20nm, and the material of the second hole transmission layer is the mixture that HTL1 and HTL3 is formed, wherein
HTL1 is WO3, HTL3 FPCC, WO3It is 1 with FPCC mass ratioes:3.The thickness of first hole transmission layer is 25nm, the first hole
The material of transport layer is the mixture that HTL1 and HTL2 is formed, and wherein HTL1 is WO3, HTL2 BTPD, WO3With BTPD mass ratioes
For 1:1.Remaining is same as Example 1.
The specific preparation method for being inverted green light quantum point membrane electro luminescent device is same as Example 1.
Hole balance layer, the 3rd hole transmission layer, the second hole transmission layer and the first hole transmission layer are surveyed respectively
Examination, the HOMO energy levels of hole balance layer are 6.04eV, and the HOMO energy levels of the 3rd hole transmission layer are 6.04eV, the second hole transport
The HOMO energy levels of layer are 6.03eV, and the HOMO energy levels of the first hole transmission layer are 5.57eV.
Embodiment 5
The thickness of hole balance layer is 8nm in the inversion green light quantum point membrane electro luminescent device of the present embodiment, hole
The material of balance layer is HTL4, HTL4 BCPPA.The thickness of 3rd hole transmission layer is 10nm, the material of the 3rd hole transmission layer
Expect the mixture for HTL1 and HTL4 formation, wherein HTL1 is V2O5, HTL4 BCPPA, V2O5It is 2 with BCPPA mass ratioes:5.
The thickness of second hole transmission layer is 10nm, and the material of the second hole transmission layer is the mixture that HTL1 and HTL3 is formed, wherein
HTL1 is V2O5, HTL3 DCDPA, V2O5It is 2 with DCDPA mass ratioes:5.The thickness of first hole transmission layer is 20nm, first
The material of hole transmission layer is the mixture that HTL1 and HTL2 is formed, and wherein HTL1 is V2O5, HTL2 BTPD, V2O5With BTPD
Mass ratio is 3:4.Remaining is same as Example 1.
The specific preparation method for being inverted green light quantum point membrane electro luminescent device is same as Example 1.
Hole balance layer, the 3rd hole transmission layer, the second hole transmission layer and the first hole transmission layer are surveyed respectively
Examination, the HOMO energy levels of hole balance layer are 6.04eV, and the HOMO energy levels of the 3rd hole transmission layer are 6.04eV, the second hole transport
The HOMO energy levels of layer are 5.88eV, and the HOMO energy levels of the first hole transmission layer are 5.57eV.
Embodiment 6
The thickness of hole balance layer is 10nm in the inversion green light quantum point membrane electro luminescent device of the present embodiment, hole
The material of balance layer is HTL4, HTL4 mCP.The thickness of 3rd hole transmission layer is 15nm, the material of the 3rd hole transmission layer
The mixture formed for HTL1 and HTL4, wherein HTL1 are CuPc, and HTL4 mCP, CuPc and mCP mass ratio are 1:3.Second is empty
The thickness of cave transport layer is 16nm, and the material of the second hole transmission layer is the mixture that HTL1 and HTL3 is formed, and wherein HTL1 is
CuPc, HTL3 DCDPA, CuPc and DCDPA mass ratio are 1:1.The thickness of first hole transmission layer is 20nm, and the first hole passes
The material of defeated layer is the mixture that HTL1 and HTL2 are formed, and wherein HTL1 is CuPc, HTL2 BTPD, CuPc and BTPD mass ratioes
For 1:2.Remaining is same as Example 1.
The specific preparation method for being inverted green light quantum point membrane electro luminescent device is same as Example 1.
Hole balance layer, the 3rd hole transmission layer, the second hole transmission layer and the first hole transmission layer are surveyed respectively
Examination, the HOMO energy levels of hole balance layer are 6.1eV, and the HOMO energy levels of the 3rd hole transmission layer are 6.1eV, the second hole transmission layer
HOMO energy levels be 5.88eV, the HOMO energy levels of the first hole transmission layer are 5.57eV.
Comparative example
The structure of the green light quantum point membrane electro luminescent device of comparative example is substrate, negative electrode, electron transfer layer, green glow amount
Son point luminescent layer, hole transmission layer and anode.Cathode material is ITO, and electron transfer layer ZnO, luminescent layer is green quantum
Point, hole transmission layer are one layer of NPB and one layer of MoO3, anode Al.Luminance test is carried out to comparative example, as a result as shown in Figure 4.
From fig. 4, it can be seen that the brightness of comparative example is significantly less than the inversion green light quantum point in embodiment 1, embodiment 2 and embodiment 3
Membrane electro luminescent device.
Embodiment described above only expresses the several embodiments of the present invention, and its description is more specific and detailed, but simultaneously
Therefore the limitation to the scope of the claims of the present invention can not be interpreted as.It should be pointed out that for one of ordinary skill in the art
For, without departing from the inventive concept of the premise, various modifications and improvements can be made, these belong to the guarantor of the present invention
Protect scope.Therefore, the protection domain of patent of the present invention should be determined by the appended claims.
Claims (10)
1. one kind be inverted green light quantum point membrane electro luminescent device, it is characterised in that including stack gradually substrate, negative electrode,
Electron transfer layer, green light quantum point luminescent layer, hole balance layer, hole transmission layer and anode；
The hole transmission layer includes the first hole transmission layer, the second hole transmission layer and the 3rd hole transmission layer of stacking, institute
State the 3rd hole transmission layer directly to contact with the hole balance layer, the material of first hole transmission layer passes for the first hole
The mixture that defeated material and the second hole mobile material are formed, the material of second hole transmission layer is the first hole transport material
The mixture that material and the 3rd hole mobile material are formed, the material of the 3rd hole transmission layer for the first hole mobile material and
The mixture that 4th hole mobile material is formed；
The material of the hole balance layer is the 4th hole mobile material, and the thickness of the hole balance layer is 5nm~10nm；
The HOMO energy levels of the hole balance layer are 6.04eV~6.5eV, and the HOMO energy levels of the 3rd hole transmission layer are
6.04eV~6.5eV, the HOMO energy levels of second hole transmission layer are 5.6eV~6.03eV, first hole transmission layer
HOMO energy levels be 4.2eV~5.6eV, the 3rd hole transmission layer, second hole transmission layer and first hole
The HOMO energy levels of transport layer are sequentially reduced；
First hole transmission layer directly contacts with the anode；
The thickness of 3rd hole transmission layer, second hole transmission layer and first hole transmission layer increases successively.
2. inversion green light quantum point membrane electro luminescent device according to claim 1, it is characterised in that the green glow amount
The material of son point luminescent layer is CdSe@ZnS core-shell structured quantum dots, wherein ,@represents cladding, and CdSe is the core shell structure amount
The core of son point, ZnS are the shell of the nuclear shell structure quantum point.
3. inversion green light quantum point membrane electro luminescent device according to claim 1, it is characterised in that the green glow amount
The thickness of son point luminescent layer is 15nm~30nm.
4. inversion green light quantum point membrane electro luminescent device according to claim 1, it is characterised in that described first is empty
Hole transport materials, second hole mobile material, the 3rd hole mobile material and the 4th hole mobile material
HOMO energy levels increase successively.
5. inversion green light quantum point membrane electro luminescent device according to claim 1, it is characterised in that described first is empty
The mass ratio of first hole mobile material described in the transport layer of cave and second hole mobile material is 1:2~1:1, described
The one kind of one hole mobile material in molybdenum trioxide, tungstic acid, vanadium oxide and titanium cyanines copper, the second hole transport material
Material is selected from N, N '-two (1- naphthyls)-N, N '-diphenyl -1,1 '-biphenyl -4-4 '-diamines and 2,2 ' two (3- dimethyl benzene amino
Benzene) one kind in 1,1' biphenyl.
6. inversion green light quantum point membrane electro luminescent device according to claim 1, it is characterised in that described second is empty
The mass ratio of first hole mobile material described in the transport layer of cave and the 3rd hole mobile material is 1:3~1:2, described
The one kind of one hole mobile material in molybdenum trioxide, tungstic acid, vanadium oxide and titanium cyanines copper, the 3rd hole transport material
Material is selected from 4,4'- double (9H- carbazole -9- bases) biphenyl, 8,8- bis- (4- (9 hydrogen-carbazole -9- bases) phenyl) -8 hydrogen-indoles [3,2,1-
De] acridine and 3,5- bis- (9 hydrogen-carbazole -9- bases)-nitrogen, one kind in nitrogen-biphenyl ammonia.
7. inversion green light quantum point membrane electro luminescent device according to claim 1, it is characterised in that the described 3rd is empty
The mass ratio of first hole mobile material described in the transport layer of cave and the 4th hole mobile material is 1:3~1:2, described
The one kind of one hole mobile material in molybdenum trioxide, tungstic acid, vanadium oxide and titanium cyanines copper, the 4th hole transport material
Material is selected from 2- hydroxy-3-methyl -2- cyclopentene-1-ones and 6,6- bis- (4-9 hydrogen-carbazole -9- bases) phenyl) -6 hydrogen-pyrroles [3,2,
1-de] one kind in acridine.
8. inversion green light quantum point membrane electro luminescent device according to claim 1, it is characterised in that put down in the hole
The material of weighing apparatus layer be the 4th hole mobile material, the 4th hole mobile material selected from 2- hydroxy-3-methyl -2- cyclopentene -
1- ketone and 6,6- bis- (4-9 hydrogen-carbazole -9- bases) phenyl) one kind in -6 hydrogen-pyrroles [3,2,1-de] acridine.
9. inversion green light quantum point membrane electro luminescent device according to claim 1, it is characterised in that the described 3rd is empty
The thickness of cave transport layer is 10nm~20nm, and the thickness of second hole transmission layer is 10nm~20nm, first hole
The thickness of transport layer is 20nm~30nm.
10. inversion green light quantum point membrane electro luminescent device according to claim 1, it is characterised in that the anode
One kind in aluminium, silver, gold and platinum.
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