CN106098958B - White light organic electroluminescent device and preparation method thereof - Google Patents
White light organic electroluminescent device and preparation method thereof Download PDFInfo
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Abstract
The present invention relates to a kind of white light organic electroluminescent device and preparation method thereof.Above-mentioned white light organic electroluminescent device includes anode layer, cathode layer and the organic function layer between anode layer and cathode layer, and organic function layer includes luminescent layer, and luminescent layer includes red and green luminous layer；Red and green luminous layer includes material of main part and the red dye and green glow dyestuff that are doped in material of main part；Direction of the doping concentration of red dye along anode layer to cathode layer reduces, and direction of the doping concentration of green glow dyestuff along anode layer to cathode layer is constant.In above-mentioned white light organic electroluminescent device, red dye and green glow dyestuff can be located at the position that its respective optimal light takes out, and so as to add the light extraction efficiency of white light organic electroluminescent device, while extend the service life of white light organic electroluminescent device.Moreover, it relates to the preparation method of above-mentioned white light organic electroluminescent device.
Description
Technical field
The present invention relates to organic electroluminescence device technical field, more particularly to a kind of white light organic electroluminescent device
And preparation method thereof.
Background technology
Organic electroluminescent refers to the phenomenon that luminous organic material lights under the excitation of electric current or electric field.It is organic
When electroluminescent device (OLED, Organic Light-Emitting Diode) has luminous active, luminous efficiency height, reaction
Between fast (1 μ s magnitudes), operating voltage low (3v~10v), wide viewing angle (more than 175 ° of ＞), plate thickness thin (＜ 1mm), power consumption
Low, operating temperature range wide (85 DEG C of 40 DEG C~﹢ of ﹣) and many advantages, such as Flexible Displays can be realized, therefore cause extensively
Concern.
White light organic electroluminescent device (WOLED, White Organic Light-Emitting Diode) is OLED
Important branch, FPD with illumination application there are huge potentiality, over nearly more than 10 year always people study focus.
Wherein, red-green glow dyestuff codope be in WOLED commonly use a kind of technology, however, due to the centre wavelength of two kinds of light have it is larger
Gap, traditional method by red-green glow dyestuff codope can only make a kind of light be located at the position that optimal light takes out, and now
Another light has deflected away from optimal light extracting position, causes WOLED light extraction efficiency not high.
The content of the invention
Based on this, it is necessary to for traditional white light organic electroluminescent device light extraction efficiency it is not high the problem of, there is provided
A kind of white light organic electroluminescent device that can improve light extraction efficiency.
A kind of white light organic electroluminescent device, including anode layer, cathode layer and positioned at the anode layer and described the moon
Organic function layer between the layer of pole,
The organic function layer includes luminescent layer, and the luminescent layer includes red and green luminous layer；
The red and green luminous layer includes material of main part and the red dye and green glow that are doped in the material of main part dye
Material；
Direction of the doping concentration of the red dye along the anode layer to the cathode layer reduces, and the green glow contaminates
Direction of the doping concentration of material along the anode layer to the cathode layer is constant.
In above-mentioned white light organic electroluminescent device, due to side of the doping concentration along anode layer to cathode layer of red dye
To reduction, and direction of the doping concentration of green glow dyestuff along anode layer to cathode layer is constant, then, red dye and green glow dyestuff
The position that its respective optimal light takes out can be located at, so as to add the light extraction efficiency of white light organic electroluminescent device, together
When extend the service life of white light organic electroluminescent device.
In one of the embodiments, the doping concentration of the red dye is 0.1wt%~3wt%.
In one of the embodiments, the doping concentration of the green glow dyestuff is 5wt%~20wt%.
In one of the embodiments, the doping concentration of the red dye is along the anode layer to the side of the cathode layer
To first keep it is constant, afterwards monotone decreasing, finally keep constant.
In one of the embodiments, the doping concentration of the red dye is along the anode layer to the side of the cathode layer
To monotone decreasing.
In addition, also providing a kind of preparation method of white light organic electroluminescent device, including form the anode layer of stacking, have
The step of machine functional layer and cathode layer, the organic function layer include luminescent layer, and the luminescent layer includes red and green luminous layer, described
Red and green luminous layer includes material of main part and the red dye and green glow dyestuff that are doped in the material of main part, is formed red green
The step of luminescent layer is：
It is as follows that the material of main part, the red dye and the green glow dyestuff, evaporation rate is deposited simultaneously：
The evaporation rate of the material of main part and the green glow dyestuff keeps constant；
The red dye is decreased to the second evaporation rate by the first evaporation rate.
In the preparation method of above-mentioned white light organic electroluminescent device, because red dye is decreased to by the first evaporation rate
Second evaporation rate, direction of the doping concentration of red dye along anode layer to cathode layer reduces in obtained luminescent layer, and green
Direction of the doping concentration of photoinitiator dye along anode layer to cathode layer is constant, then, red dye and green glow dyestuff can be located at it
The position that respective optimal light takes out, so as to add the light extraction efficiency of white light organic electroluminescent device, while is extended white
The service life of light organic electroluminescence device.
In one of the embodiments, the step of forming red and green luminous layer be：
The material of main part, the red dye and the green glow dyestuff is deposited simultaneously, evaporation time is 120s~720s,
Evaporation rate is as follows：
The evaporation rate of the material of main part and the green glow dyestuff remain respectively 0.04nm/s~0.24nm/s and 6 ×
10-3Nm/s~3.6 × 10-2nm/s；
First evaporation rate of the red dye remains 3 × 10-4Nm/s~2 × 10-3Nm/s, evaporation time 40s
~240s；It is described afterwards by the first evaporation rate monotone decreasing to the second evaporation rate, second evaporation rate is 5 × 10- 5Nm/s~6 × 10-4Nm/s, evaporation time are 40s~240s；Finally keep second evaporation rate, evaporation time 40s
~240s.
In one of the embodiments, the step of forming red and green luminous layer be：
The material of main part, the red dye and the green glow dyestuff, evaporation time 300s, evaporation speed are deposited simultaneously
Rate is as follows：
The evaporation rate of the material of main part and the green glow dyestuff remains 0.1nm/s and 1.5 × 10 respectively-2nm/s；
First evaporation rate of the red dye remains 8 × 10-4Nm/s, evaporation time 100s；Afterwards by described
First evaporation rate monotone decreasing to the second evaporation rate, second evaporation rate are 2 × 10-4Nm/s, evaporation time are
100s；Finally keep second evaporation rate, evaporation time 100s.
In one of the embodiments, the step of forming red and green luminous layer be：
The material of main part, the red dye and the green glow dyestuff is deposited simultaneously, evaporation time is 120s~720s,
Evaporation rate is as follows：
The evaporation rate of the material of main part and the green glow dyestuff remain respectively 0.04nm/s~0.24nm/s and 6 ×
10-3Nm/s~3.6 × 10-2nm/s；
The red dye is by the first evaporation rate monotone decreasing to second evaporation rate, first evaporation
Speed is 3 × 10-4Nm/s~2 × 10-3Nm/s, second evaporation rate are 5 × 10-5Nm/s~6 × 10-4nm/s。
In one of the embodiments, the step of forming red and green luminous layer be：
The material of main part, the red dye and the green glow dyestuff, evaporation time 300s, evaporation speed are deposited simultaneously
Rate is as follows：
The evaporation rate of the material of main part and the green glow dyestuff remains 0.1nm/s and 1.5 × 10 respectively-2nm/s；
The red dye is by the first evaporation rate monotone decreasing to second evaporation rate, first evaporation
Speed is 8 × 10-4Nm/s, second evaporation rate are 2 × 10-4nm/s。
Brief description of the drawings
Fig. 1 is the structural representation of the white light organic electroluminescent device of an embodiment；
Fig. 2 is the flow chart of the preparation method of the white light organic electroluminescent device of an embodiment；
M- evaporation rate curve when Fig. 3 is in the preparation process of the white light organic electroluminescent device of embodiment 1；
M- evaporation rate curve when Fig. 4 is in the preparation process of the white light organic electroluminescent device of embodiment 2.
Embodiment
In order to facilitate the understanding of the purposes, features and advantages of the present invention, below in conjunction with the accompanying drawings to the present invention
Embodiment be described in detail.Many details are elaborated in the following description in order to fully understand this hair
It is bright.But the invention can be embodied in many other ways as described herein, those skilled in the art can be not
Similar improvement is done in the case of running counter to intension of the present invention, therefore the present invention is not limited by following public specific embodiment.
Fig. 1 is referred to, the white light organic electroluminescent device 100 of an embodiment includes substrate 110, the sun stacked gradually
Pole layer 120, organic function layer 130 and cathode layer 140.Wherein, the position of anode layer 120 and cathode layer 140 can exchange.It is organic
Functional layer 130 includes hole transmission layer 131 (HTL), luminescent layer 132 and electron transfer layer 133 (ETL).White light organic electroluminescence is sent out
Optical device 100 lights under the driving of additional power source 200.
Substrate 110 is glass either flexible substrate or metal foil in the white light organic electroluminescent device 100 of the present invention
Piece, wherein flexible substrate are a kind of materials in ultra-thin solid-state thin slice, polyesters or poly- peptide imine compound.
The generally use inorganic, metal oxide of 100 Anodic layer of white light organic electroluminescent device 120 of the present invention is (such as
ITO, ZnO etc.), organic conductive polymer (such as PEDOT:PSS, PANI etc.) or high-work-function metal material (as gold, copper, silver,
Platinum etc.).
The hole-transporting layer 131 of white light organic electroluminescent device 100 of the present invention for aromatic diamines compound or
One kind in person's aromatic triamine class compound, such as NPB, TPD, α-NPD, TAPC materials.
The present invention white light organic electroluminescent device 100 in luminescent layer 132 include blue light-emitting 1321 (B-EML),
Charge generation layer 1322 (CGL) and red and green luminous layer 1323 (R/G-EML).
Wherein, red and green luminous layer 1323 includes material of main part and the red dye and green glow that are doped in material of main part
Dyestuff.Material of main part has higher triplet, can effectively transfer energy to dopant material, send out dopant material
Light.Material of main part typically uses a kind of material of carbazole compound (such as CBP, CDBP, TCTA, mCP).Dopant material includes red
Photoinitiator dye and green glow dyestuff.Red dye is selected from the phosphor material of the atom centered on heavy metal iridium (Ir), such as Ir (piq)2
(acac)、Ir(m-piq)2(acac)、Ir(DPQ)2(acac) etc..Green glow dyestuff is selected from the atom centered on heavy metal (Ir)
Phosphor material, such as Ir (ppy)3、Ir(pbi)2(acac)、Ir(nbi)2(acac)、Ir(pybi)2(acac) etc..
The doping concentration edge of red dye in the red and green luminous layer 1323 of the white light organic electroluminescent device 100 of the present invention
Anode layer 120 reduces to the direction of cathode layer 140, and the doping concentration of green glow dyestuff is along anode layer 120 to the side of cathode layer 140
To constant.Wherein, the doping concentration of red dye refers to doping concentration of the red dye relative to material of main part, green glow dyestuff
Doping concentration refer to doping concentration of the green glow dyestuff relative to material of main part.In one preferably embodiment, feux rouges dye
The doping concentration of material is 0.1wt%~3wt%.The doping concentration of green glow dyestuff is 5wt%~20wt%.Certainly, red dye
With the doping concentration not limited to this of green glow dyestuff.
In one preferably embodiment, the direction of the doping concentration of red dye along anode layer to cathode layer is first kept not
Change, afterwards monotone decreasing, finally keep constant.In another preferably embodiment, the doping concentration of red dye is along anode
Direction monotone decreasing of the layer to cathode layer.Both embodiments can make red dye and green glow dyestuff be respectively positioned on its each
The position taken out of optimal light, so as to add the light extraction efficiency of white light organic electroluminescent device, while extend white light and have
The service life of organic electroluminescence devices.
The present invention white light organic electroluminescent device 100 in electron transfer layer 133 be metal organic complex (such as
Alq3, BAlq), arsenic pyridine class (such as 3TPYMB), o-phenanthroline class (such as BCP, BPhen), oxadiazoles classes (such as PBD, OXD-7) or miaow
A kind of material in azole (such as TPBI) compound-material.
Cathode layer 140 can be the work(such as lithium, magnesium, calcium, strontium, aluminium, indium in the white light organic electroluminescent device 100 of the present invention
The relatively low metallic film of function or they with copper, the alloy firm of gold, silver.The present invention is preferably Mg successively:Ag alloy-layers,
Ag layers or LiF layers, Al layers successively.
In addition, the white light organic electroluminescent device 100 of the present invention can also include being arranged at substrate 110 and anode layer
Cushion (not shown) between 120.Cushion is promoting the levelness of substrate and prevent the intrusion of impurity.Cushion can be with
Use SiNxAnd/or SiOxPass through such as plasma enhanced chemical vapor deposition (PECVD) technology, atmospheric pressure cvd (APCVD) skill
The various deposition techniques of art and low pressure chemical vapor deposition (LPCVD) technology etc carry out buffer layer 110.Further, it is also possible in anode layer
Anode buffer layer (not shown) is set between 120 and hole transmission layer 131, typically using phthalocyanines, polyacrylate, polyamides
A kind of material in imines, fluoropolymer, inorganic fluorine salt dissolving, inorganic oxide or diamond, such as CuPc.
Fig. 2 is referred to, the preparation method of the white light organic electroluminescent device of an embodiment, is comprised the following steps：
S100, anode layer 120 is formed on a substrate 110.
The method of such as wet etching can be used to form anode layer 120 on a substrate 110.
S200, organic function layer 130 is formed on anode layer 120, organic function layer 130 includes luminescent layer 132, luminescent layer
132 include red and green luminous layer 1323, and red and green luminous layer 1323 includes material of main part and the feux rouges being doped in material of main part dye
Material and green glow dyestuff, the step of forming red and green luminous layer 1323 be：
It is as follows that material of main part, red dye and green glow dyestuff, evaporation rate is deposited simultaneously：
The evaporation rate of material of main part and green glow dyestuff keeps constant；
Red dye is decreased to the second evaporation rate by the first evaporation rate.
The method of three sources evaporation can be used to carry out grade doping, respectively by material of main part, red dye and green glow dyestuff
It is placed in different evaporation sources, by controlling the evaporation rate of three evaporation sources, to make the evaporation of material of main part and green glow dyestuff
Speed keeps constant, while red dye is decreased to the second evaporation rate by the first evaporation rate.
It should be noted that the first evaporation rate can directly monotone decreasing to the second evaporation rate；Also can be first by first
Evaporation rate is kept for a period of time, and monotone decreasing to the second evaporation rate, finally continues the second evaporation rate keeping one again afterwards
The section time, complete whole evaporation process；It can also be deposited by the first evaporation rate monotone decreasing to the first evaporation rate and second
A certain numerical value between speed, repeats said process several times afterwards, until being decreased to the second evaporation rate, completes whole steam
Plating process.
In one preferably embodiment, the step of forming red and green luminous layer 1323, is：
Material of main part, red dye and green glow dyestuff is deposited simultaneously, evaporation time is 120s~720s, and evaporation rate is such as
Under：
The evaporation rate of material of main part and green glow dyestuff remains 0.04nm/s~0.24nm/s and 6 × 10 respectively-3nm/s
~3.6 × 10-2nm/s；
First evaporation rate of red dye remains 3 × 10-4Nm/s~2 × 10-3Nm/s, evaporation time be 40s~
240s；Afterwards by the first evaporation rate monotone decreasing to the second evaporation rate, the second evaporation rate is 5 × 10-5Nm/s~6 ×
10-4Nm/s, evaporation time are 40s~240s；The second evaporation rate is finally kept, evaporation time is 40s~240s.
In the red and green luminous layer 1323 being prepared by the present embodiment, the doping concentration of red dye is along anode layer 120
To the direction of cathode layer 140 first keep it is constant, afterwards monotone decreasing, finally keep constant.
In another preferably embodiment, the step of forming red and green luminous layer 1323, is：
Material of main part, red dye and green glow dyestuff is deposited simultaneously, evaporation time is 120s~720s, and evaporation rate is such as
Under：
The evaporation rate of material of main part and green glow dyestuff remains 0.04nm/s~0.24nm/s and 6 × 10 respectively-3nm/s
~3.6 × 10-2nm/s；
For red dye by the first evaporation rate monotone decreasing to the second evaporation rate, the first evaporation rate is 3 × 10-4nm/s
~2 × 10-3Nm/s, the second evaporation rate are 5 × 10-5Nm/s~6 × 10-4nm/s。
In the red and green luminous layer 1323 being prepared by the present embodiment, the doping concentration of red dye is along anode layer 120
To the direction monotone decreasing of cathode layer 140.
S300, cathode layer 140 is formed on organic function layer 130, obtain white light organic electroluminescent device 100.
The method of evaporation can be used to form cathode layer 140 on organic function layer 130.
In the preparation method of above-mentioned white light organic electroluminescent device, because red dye is decreased to by the first evaporation rate
Second evaporation rate, direction of the doping concentration of red dye along anode layer to cathode layer reduces in obtained luminescent layer, and green
Direction of the doping concentration of photoinitiator dye along anode layer to cathode layer is constant, then, red dye and green glow dyestuff can be located at it
The position that respective optimal light takes out, so as to add the light extraction efficiency of white light organic electroluminescent device, while is extended white
The service life of light organic electroluminescence device.
The white light organic electroluminescent device of the present invention is carried out further with reference to specific embodiments and the drawings
It is bright.
Embodiment 1
Fig. 3 is referred to, is the step of the red and green luminous layer for forming the present embodiment：
It is deposited material of main part, red dye and green glow dyestuff simultaneously, evaporation time 300s, evaporation rate is as follows：
The evaporation rate of material of main part and green glow dyestuff remains 0.1nm/s and 1.5 × 10 respectively-2nm/s。
First evaporation rate of red dye remains 8 × 10-4Nm/s, evaporation time 100s；Afterwards by the first evaporation
Rate monotonic is decremented to the second evaporation rate, and the second evaporation rate is 2 × 10-4Nm/s, evaporation time 100s；Finally keep
Two evaporation rates, evaporation time 100s.
Light extraction efficiency (the outer quantum effect of the white light organic electroluminescent device obtained by the preparation method of the present embodiment
Rate) about 2% can be improved.
Embodiment 2
Fig. 4 is referred to, is the step of the red and green luminous layer for forming the present embodiment：
It is deposited material of main part, red dye and green glow dyestuff simultaneously, evaporation time 300s, evaporation rate is as follows：
The evaporation rate of material of main part and green glow dyestuff remains 0.1nm/s and 1.5 × 10 respectively-2nm/s。
For red dye by the first evaporation rate monotone decreasing to the second evaporation rate, the first evaporation rate is 8 × 10-4nm/
S, the second evaporation rate are 2 × 10-4nm/s。
Light extraction efficiency (the outer quantum effect of the white light organic electroluminescent device obtained by the preparation method of the present embodiment
Rate) about 3% can be improved.
Each technical characteristic of embodiment described above can be combined arbitrarily, to make description succinct, not to above-mentioned reality
Apply all possible combination of each technical characteristic in example to be all described, as long as however, the combination of these technical characteristics is not deposited
In contradiction, the scope that this specification is recorded all is considered to be.
Embodiment described above only expresses the several embodiments of the present invention, and its description is more specific and detailed, but simultaneously
Can not therefore it be construed as limiting the scope of the patent.It should be pointed out that come for one of ordinary skill in the art
Say, without departing from the inventive concept of the premise, various modifications and improvements can be made, these belong to the protection of the present invention
Scope.Therefore, the protection domain of patent of the present invention should be determined by the appended claims.
Claims (10)
1. a kind of white light organic electroluminescent device, including anode layer, cathode layer and positioned at the anode layer and the negative electrode
Organic function layer between layer, it is characterised in that
The organic function layer includes luminescent layer, and the luminescent layer includes red and green luminous layer；
The red and green luminous layer includes material of main part and the red dye and green glow dyestuff that are doped in the material of main part；
Direction of the doping concentration of the red dye along the anode layer to the cathode layer reduces, and the green glow dyestuff
Direction of the doping concentration along the anode layer to the cathode layer is constant.
2. white light organic electroluminescent device according to claim 1, it is characterised in that the doping of the red dye is dense
Spend for 0.1wt%~3wt%.
3. white light organic electroluminescent device according to claim 1, it is characterised in that the doping of the green glow dyestuff is dense
Spend for 5wt%~20wt%.
4. white light organic electroluminescent device according to claim 1, it is characterised in that the doping of the red dye is dense
Degree along the anode layer to the direction of the cathode layer first keep it is constant, afterwards monotone decreasing, finally keep constant.
5. white light organic electroluminescent device according to claim 1, it is characterised in that the doping of the red dye is dense
Spend the direction monotone decreasing along the anode layer to the cathode layer.
6. a kind of preparation method of white light organic electroluminescent device, including form anode layer, organic function layer and the moon of stacking
The step of pole layer, the organic function layer include luminescent layer, and the luminescent layer includes red and green luminous layer, it is characterised in that described
Red and green luminous layer includes material of main part and the red dye and green glow dyestuff that are doped in the material of main part, is formed red green
The step of luminescent layer is：
It is as follows that the material of main part, the red dye and the green glow dyestuff, evaporation rate is deposited simultaneously：
The evaporation rate of the material of main part and the green glow dyestuff keeps constant；
The red dye is decreased to the second evaporation rate by the first evaporation rate.
7. the preparation method of white light organic electroluminescent device according to claim 6, it is characterised in that form red green hair
The step of photosphere is：
The material of main part, the red dye and the green glow dyestuff is deposited simultaneously, evaporation time is 120s~720s, evaporation
Speed is as follows：
The evaporation rate of the material of main part and the green glow dyestuff remains 0.04nm/s~0.24nm/s and 6 × 10 respectively- 3Nm/s~3.6 × 10-2nm/s；
First evaporation rate of the red dye remains 3 × 10-4Nm/s~2 × 10-3Nm/s, evaporation time be 40s~
240s；It is described afterwards by the first evaporation rate monotone decreasing to the second evaporation rate, second evaporation rate is 5 × 10-5nm/
S~6 × 10-4Nm/s, evaporation time are 40s~240s；Finally keep second evaporation rate, evaporation time be 40s~
240s。
8. the preparation method of white light organic electroluminescent device according to claim 7, it is characterised in that form red green hair
The step of photosphere is：
The material of main part, the red dye and the green glow dyestuff is deposited simultaneously, evaporation time 300s, evaporation rate is such as
Under：
The evaporation rate of the material of main part and the green glow dyestuff remains 0.1nm/s and 1.5 × 10 respectively-2nm/s；
First evaporation rate of the red dye remains 8 × 10-4Nm/s, evaporation time 100s；Afterwards by described first
For evaporation rate monotone decreasing to the second evaporation rate, second evaporation rate is 2 × 10-4Nm/s, evaporation time 100s；Most
After keep second evaporation rate, evaporation time 100s.
9. the preparation method of white light organic electroluminescent device according to claim 6, it is characterised in that form red green hair
The step of photosphere is：
The material of main part, the red dye and the green glow dyestuff is deposited simultaneously, evaporation time is 120s~720s, evaporation
Speed is as follows：
The evaporation rate of the material of main part and the green glow dyestuff remains 0.04nm/s~0.24nm/s and 6 × 10 respectively- 3Nm/s~3.6 × 10-2nm/s；
The red dye is by the first evaporation rate monotone decreasing to second evaporation rate, first evaporation rate
For 3 × 10-4Nm/s~2 × 10-3Nm/s, second evaporation rate are 5 × 10-5Nm/s~6 × 10-4nm/s。
10. the preparation method of white light organic electroluminescent device according to claim 9, it is characterised in that formed red green
The step of luminescent layer is：
The material of main part, the red dye and the green glow dyestuff is deposited simultaneously, evaporation time 300s, evaporation rate is such as
Under：
The evaporation rate of the material of main part and the green glow dyestuff remains 0.1nm/s and 1.5 × 10 respectively-2nm/s；
The red dye is by the first evaporation rate monotone decreasing to second evaporation rate, first evaporation rate
For 8 × 10-4Nm/s, second evaporation rate are 2 × 10-4nm/s。
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