CN100463244C - Organic white light emitting diode in tiny cavity type - Google Patents
Organic white light emitting diode in tiny cavity type Download PDFInfo
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- CN100463244C CN100463244C CNB2004100113720A CN200410011372A CN100463244C CN 100463244 C CN100463244 C CN 100463244C CN B2004100113720 A CNB2004100113720 A CN B2004100113720A CN 200410011372 A CN200410011372 A CN 200410011372A CN 100463244 C CN100463244 C CN 100463244C
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Abstract
The invention solves issues of color purity of white color, stability of color and luminous efficiency. The disclosed diode includes substrate, Bragg reflection mirror, anode, hole transport layer, luminous layer, cavity barrier layer, electron transport layer, and cathode. Through structure of micro cavity, changing luminous characters of broadband of organic material, the invention realizes irradiance in two modes of resonance in visible range, making match of spectrum generate white light. Since luminous layer is positioned near to antinode of stationary field intensity in two modes of resonance in micro cavity, luminous intensities in two modes are enhanced, and luminous efficiency is increased. Under condition of not changing length of cavity, adjusting relative position of luminous layer changes relative luminous intensities between two modes to optimize color purity. Features are: stable white light and raised luminous efficiency.
Description
Technical field:
The invention belongs to luminous and the Display Technique field, relate to the structural design and the preparation method of organic white light-emitting diode.
Background technology:
Organic Light Emitting Diode is a kind of flat panel display that development in recent years is got up, and is with a wide range of applications.Such device is to add the electric driven for emitting lights device that top electrode constitutes by a plurality of organic layers.Utilize luminous organic material to realize red, blue, green and white OLED.Wherein white OLED has important use at the aspects such as backlight of green illumination, liquid crystal display screen.Most of organic molecules and high-molecular luminous material have very wide photoluminescent band (typical the about 100nm of half-breadth), so their glow color is neither pure monochrome, neither pure white.The main preparation methods of organic white light-emitting diode is to mix multiple organic fluorescent dyes such as red, blue, green in luminescent layer, or adopts methods red, blue, green a plurality of luminescent layers.Though these methods can realize white light, but exist some problems, not high as the colorimetric purity of white light, the color instability, can change along with the difference of operating voltage, and the luminosity of device and luminous efficiency will be starkly lower than the Organic Light Emitting Diode of other color.These phenomenons are all unfavorable for demonstration and illumination.
Organic tiny cavity light-emitting diode is to introduce plane optics micro resonant cavity (abbreviation microcavity) in the structure of common Organic Light Emitting Diode.Microcavity is by the plural layers between two speculums and two speculums, also is the plural layers formation of microcavity inside (being called for short in the chamber).The advantage of microcavity is the characteristics of luminescence of material in the control chamber effectively, can modulate and realize luminous enhancing to the material emission spectrum at the mode of resonance place, this is because the chamber of optical wavelength magnitude length has greatly changed the photon state density in the chamber, make electromagnetic field mode in the chamber no longer resemble in the free space continuous distribution, but present discrete distribution.Photon state density is enhanced at microcavity mode of resonance place, is suppressed at other disresonance pattern place.In addition, place the spontaneous emission rate of the radiation dipole in chamber not only to be determined, but also depend on the stiffness of coupling between radiation dipole and the limited electromagnetic field by the photon state density in the chamber.Be the radiation dipole in the chamber during diverse location, its spontaneous emission rate is also with difference.This is that the diverse location place has different intensity levels because the stationary field of planar micro cavity is SIN function to distribute.The place has maximum in antinode, and the place has minimum value at node.For most of materials, the raising of spontaneous emission rate promptly is the raising of luminous efficiency.
Organic tiny cavity light-emitting diode can realize having only the light emission of 1 mode of resonance, thereby obtains the luminous of pure monochromes such as pure red, ethereal blue or pure green.If can realize the light emission of a plurality of modes of resonance, so just may obtain white luminous.Though at present by increasing methods such as the microcavity chamber is long have realized a plurality of modes of resonance in organic tiny cavity light-emitting diode light emission, it is multicolor luminous that glow color still belongs to, also there be not ideal results aspect the acquisition of white light and the luminous efficiency.
Summary of the invention:
The objective of the invention is for problem such as the colorimetric purity, colour stability and the luminous efficiency that solve white light in the above-mentioned background technology be not high.The present invention utilizes the structure of microcavity and emission spectrum shape and the luminous intensity that principle is controlled organic material, the white light emission that implementation efficiency is high.The present invention will provide the structure and the method for the high organic microcavity white light-emitting diode of a kind of implementation efficiency.
The present invention includes: substrate, Bragg mirror, anode, hole transmission layer, luminescent layer, hole blocking layer, electron transfer layer, negative electrode, as shown in Figure 1;
The Bragg mirror preparation is on substrate; Bragg mirror and negative electrode are the speculums of microcavity; Structure in the chamber comprises: anode, hole transmission layer, luminescent layer, hole blocking layer, electron transfer layer; Anode preparation is on Bragg mirror; On anode, deposit hole transmission layer, luminescent layer, hole blocking layer, electron transfer layer successively; Deposition cathode on electron transfer layer;
Substrate is made of transparent material; The structure of Bragg mirror is [HL]
nOr [HL]
nH, it is the dielectric optical thin film in a plurality of cycles of constituting by two kinds of different optical materials of the first refractive index optical material H and the second refractive index optical material L, the first refractive index optical material H is identical with the optical thickness of the second refractive index optical material L, optical thickness is the product of material refractive index and material thickness, and the numerical value of optical thickness is chosen in 1/4th of the corresponding wavelength λ of high reflectance institute 0 of Bragg mirror; Anode is made of translucent conductive film; Hole transmission layer is made of organic film, and the anode injected holes is transferred in the luminescent layer by hole transmission layer; The band gap width of hole transmission layer makes the interface between hole transmission layer and the luminescent layer form effective electronics potential barrier greater than the band gap width of luminescent layer; Luminescent layer and hole blocking layer constitute by organic film; The band gap width of hole blocking layer makes the interface between hole blocking layer and the luminescent layer form effective hole barrier potential barrier greater than the band gap width of luminescent layer; Electron transfer layer is made of organic film, and the negative electrode injected electrons is transferred in the luminescent layer by electron transfer layer and hole blocking layer;
In order to realize white light, the luminescent layer material is chosen in the luminous organic material that the visible range has broad band; The mode of resonance of microcavity satisfies the Fabry-Perot equation, promptly
, n wherein
iAnd d
iThe refractive index and the thickness of each layer film in the expression chamber, n
iAnd d
iProduct be optics thickness of film, the ∑ n in the equation
id
iBe the total optical thickness of each layer film in the chamber, the chamber that is called as microcavity is long.
With
Be two reflection phase shift that speculum is Bragg mirror and negative electrode, m is a pattern progression, and λ is the wavelength of mode of resonance; From equation as can be known, change the chamber length of microcavity and the reflection phase shift of speculum, just can control the mode of resonance of microcavity; The organic microcavity white light-emitting diode of the present invention is selected two modes of resonance, its emission wavelength lays respectively at short wavelength 450nm-500nm zone and long wavelength 580nm-630nm zone, and the suitable coupling of the luminous spectrum of these two modes of resonance can produce the white light of different colorimetric puritys; In order to obtain two such modes of resonance, the chamber length of microcavity is controlled at about 3/2nds times, two times and 5/2nds times of long wavelength's mode of resonance, need select for use the first suitable refractive index optical material H and the second refractive index optical material L to control the reflection phase shift of Bragg mirror simultaneously, thereby adjust the peak wavelength distance between two modes of resonance of microcavity, make their emission spectrum be matched to white light; The structural design of microcavity makes anode and negative electrode respectively near the node position of the standing wave field intensity of two modes of resonance in the chamber, luminescent layer is near the anti-node location of standing wave field intensity of two modes of resonance in the chamber, the luminous intensity of such two modes of resonance all is enhanced, thereby the luminous efficiency of white light is improved; Keeping regulating the relative position of luminescent layer in microcavity inside under the long constant situation in microcavity chamber, the relative luminous intensity between two modes of resonance can change thereupon, and the colorimetric purity of white light is optimized; The structure of luminescent layer is one deck, and does not mix multiple organic fluorescent dyes such as red, blue, green, so the colorimetric purity of the white light of micro chamber device generation does not change with the variation of operating voltage; The high reflectance of Bragg mirror is less than the reflectivity of negative electrode, and white light is sent in substrate one side.
Organic microcavity white light-emitting diode of the present invention, anode is connected positive source, negative electrode connects power cathode, under forward voltage drives, from the anode injected holes and from the negative electrode injected electrons in luminescent layer, be combined into can be luminous exciton, the radiation recombination of exciton produces white light, sends in substrate one side.
Advantage of the present invention is:
The present invention changes the broad band luminescence feature of organic material by micro-cavity structure, be implemented in two modes of resonance luminous of visible range, as Fig. 8, shown in Figure 12, and make their Spectral matching produce white light, as Fig. 9, shown in Figure 13, thereby provide a kind of method that realizes organic microcavity white light-emitting diode.Luminescent layer of the present invention is near the anti-node location of the standing wave field intensity of two modes of resonance in the microcavity, as shown in Figure 7, the luminous intensity of two modes of resonance all is enhanced, and as shown in Figure 8, the luminous efficiency of white light is improved, as shown in figure 10.The present invention changes two relative luminous intensities between the mode of resonance keeping regulating the relative position of luminescent layer in microcavity inside under the long constant situation in microcavity chamber, can optimize the colorimetric purity of regulating white light, as shown in figure 11.White light parts colour stable of the present invention, the variation with operating voltage does not change.Problem such as the present invention has overcome common white organic light emitting diode glow color instability, colorimetric purity is not high and luminous efficiency is not high has not only realized stable white light emission, and has improved luminous efficiency significantly.
Description of drawings:
The structural representation of the organic microcavity white light-emitting diode of Fig. 1 the present invention
The molecular structure of hole transport layer material in Fig. 2 embodiment of the invention 1 and 2
The molecular structure of luminescent layer material in Fig. 3 embodiment of the invention 1 and 2
The molecular structure of hole barrier material in Fig. 4 embodiment of the invention 1
The molecular structure of electric transmission layer material in Fig. 5 embodiment of the invention 1
The refraction index profile of Fig. 6 embodiment of the invention 1 each layer of microcavity
The stationary field distribution situation of 1 two modes of resonance of Fig. 7 embodiment of the invention, wherein solid line is the stationary field of 601nm mode of resonance, and dotted line is the stationary field of 482nm mode of resonance, and dash area is the luminescent layer position.
Fig. 8 embodiment of the invention 1 white electroluminescence spectrum (solid line) and electroluminescence spectrum (dotted line) with the commonplace components of spline structure
Fig. 9 embodiment of the invention 1 white color coordinate (some A) and commonplace components chromaticity coordinates (some B)
The comparison of the luminous efficiency (solid line) of Figure 10 embodiment of the invention 1 white light and the luminous efficiency (dotted line) of commonplace components
Figure 11 embodiment of the invention 1 microcavity chamber appearance with and the electroluminescence spectrum of different five devices in luminescent layer position has provided the corresponding chromaticity coordinates value of each spectrum in the bracket on curve right side among the figure
The white electroluminescence spectrum of Figure 12 embodiment of the invention 2
The white color coordinate of Figure 13 embodiment of the invention 2
Embodiment:
Embodiment 1:
The structure of organic tiny cavity light-emitting diode is:
Glass substrate/Bragg mirror/ITO/NPB/Alq/F-TBB/OXD-7/MgAg, wherein substrate is an ordinary optical glass.The structure of Bragg mirror is HLH, and totally three layers, wherein the H layer material is TiO
2, thickness 57.3nm; The L layer material is LiF, thickness 97.5nm.The maximum reflectivity of Bragg mirror is about 70%.Transparent conductive film ITO makes anode, and thickness is 300nm.Hole transmission layer adopts NPB material, thick 83nm.Luminescent layer adopts Alq material, thickness 20nm.Luminescent layer materials A lq is the broad band luminescent material that a fluorescence peak is positioned at 510nm, line half-width 90nm.Hole blocking layer adopts the F-TBB material, and thickness is 20nm.Electron transfer layer adopts the OXD-7 material, and thickness is 40nm.What negative electrode adopted is the MgAg alloy electrode, and thickness is 150nm.Fig. 2,3,4 and 5 is respectively the molecular structure of organic material NPB, Alq, F-TBB and OXD-7.Fig. 6 is the refraction index profile of each layer, and wherein ordinate is a refractive index, and abscissa is for beginning the distance between each layer and the substrate from Bragg mirror, and dotted line separates each layer among the figure.The refractive index of the hole transmission layer NPB that is made of organic film, luminescent layer Alq, hole blocking layer F-TBB, electron transfer layer OXD-7 is respectively 1.81,1.72,1.65,1.71 as can be seen from Figure 6.Fig. 7 is the stationary field distribution situation of two modes of resonance, and wherein solid line is the stationary field of 601nm mode of resonance, and dotted line is the stationary field of 482nm mode of resonance, and dash area is the luminescent layer position.Fig. 7 shows that luminescent layer is in the stationary field anti-node location of 601nm mode of resonance, simultaneously also near the anti-node location of 482nm mode of resonance stationary field.Organic tiny cavity light-emitting diode in the present embodiment 1 is when applied voltage, and hole and electronics inject from anode and negative electrode respectively, and are combined into exciton (a kind of radiation dipole) in luminescent layer Alq, and the radiation recombination of exciton produces luminous.Play bright voltage 4V, glow color is a white.Electroluminescence spectrum when Figure 8 shows that applied voltage 12V (solid line) is made of two emission peaks, lays respectively at 482nm and 601nm, and they are modes of resonance of microcavity.The spectrum of this white light does not change with the difference of applied voltage, and 1931 luminous CIE chromaticity coordinatess are (0.345,0.331), shown in Fig. 9 mid point A.For the ease of relatively, when the dotted line of Fig. 8 has also provided applied voltage 12V with electroluminescence (EL) spectrum of the commonplace components (do not have Bragg mirror, remainder is identical) of spline structure.The EL peak position of commonplace components plays bright voltage 4V in 510nm, the about 90nm of line half-width, and glow color is a yellow green, and the 1931CIE chromaticity coordinates is (0.27,0.55), shown in Fig. 9 mid point B.Figure 10 has provided luminous efficiency (solid line) and the luminous efficiency (dotted line) of commonplace components and the relation of current density of micro chamber device white light.The luminous efficiency of organic microcavity white light-emitting diode exceeds 0.7 times of commonplace components.After Figure 11 has provided long constant and relative position luminescent layer in chamber and has changed, the relative variation of the luminous intensity of two modes of resonance of micro chamber device.The glass substrate of five micro chamber devices, Bragg mirror, ito anode and MgAg negative electrode are identical, and microcavity chamber length also is identical, and the structure of all the other each layers is respectively:
1：NPB(99nm)/Alq(20nm)/F-TBB(15.5nm)/OXD-7(28nm)
2：NPB(74nm)/Alq(20nm)/F-TBB(20nm)/OXD-7(49.5nm)
3：NPB(110nm)/Alq(20nm)/F-TBB(15nm)/OXD-7(16.5nm)
4：NPB(63nm)/Alq(20nm)/F-TBB(21nm)/OXD-7(61nm)
5：NPB(46nm)/Alq(20nm)/F-TBB(30nm)/OXD-7(69nm)
The curve right side has provided the chromaticity coordinates of each spectrum correspondence, and they are respectively (0.32,0.32), (0.36,0.34), (0.31,0.31), (0.39,0.35), (0.45,0.37).Figure 11 shows and keeping regulating the relative position of luminescent layer in microcavity inside under the long constant situation in microcavity chamber, and the relative luminous intensity between two modes of resonance can change, thereby can optimize the colorimetric purity of regulating white light.
Embodiment 2: the structure that micro chamber device adopted is: the structure of glass/Bragg mirror/ITO (156nm)/NPB (97nm)/Alq (72nm)/MgAg (150nm) Bragg mirror is three layers of HLH, and wherein the H layer material is ZrO
2/ TiO
2Mixture, refractive index 2.2, thickness 62nm; The L layer material is LiF, refractive index 1.41, thickness 98nm.The maximum reflectivity of Bragg mirror is 60%.As shown in Figure 12, the electroluminescence spectrum of micro chamber device has two glow peaks, distributes to be positioned at 467nm and 616nm.Glow color be white, its 1931CIE chromaticity coordinates be (0.357,0.30) as shown in figure 13.
Claims (4)
1. organic microcavity white light-emitting diode comprises: substrate (1), negative electrode (8); It is characterized in that also comprising: Bragg mirror (2), anode (3), hole transmission layer (4), luminescent layer (5), hole blocking layer (6), electron transfer layer (7); There are anode (3), hole transmission layer (4), luminescent layer (5), hole blocking layer (6), electron transfer layer (7) to constitute microcavity between Bragg mirror (2) and the negative electrode (8); Bragg mirror (2) preparation is on substrate (1); Anode (3) preparation is on Bragg mirror (2); On anode (3), deposit hole transmission layer (4), luminescent layer (5), hole blocking layer (6), electron transfer layer (7) successively; Go up deposition cathode (8) at electron transfer layer (7); The structure of Bragg mirror (2) is [HL]
nOr [HL]
nH is the dielectric optical thin film in a plurality of cycles of being made of two kinds of different optical materials of the first refractive index optical material H and the second refractive index optical material L; Anode (3) adopts translucent conductive film; Hole transmission layer (4), luminescent layer (5), hole blocking layer (6), electron transfer layer (7) adopt organic film, and the band gap width of hole transmission layer (4) and hole blocking layer (6) is greater than the band gap width of luminescent layer (5); Luminescent layer (5) material is chosen in the luminous organic material that the visible range has broad band; Microcavity selects two its emission wavelengths of mode of resonance to lay respectively at short wavelength 450nm-500nm zone and long wavelength 580nm-630nm zone, makes the luminous spectrum of two modes of resonance suitably mate the generation white light.
2. organic microcavity white light-emitting diode according to claim 1 is characterized in that: utilize Fabry-Perot equation principle to control the mode of resonance of microcavity by the chamber that changes microcavity reflection phase shift long and speculum; The chamber length of microcavity is that the total optical thickness of anode (3), hole transmission layer (4), luminescent layer (5), hole blocking layer (6), electron transfer layer (7) in the chamber is 3/2nds times or two times or 5/2nds times of long wavelength's mode of resonance; The first refractive index optical material H of Bragg mirror (2) is identical with the optical thickness of the second refractive index optical material L, and it is the corresponding wavelength λ of high reflectance institute of Bragg mirror (2) that the numerical value of optical thickness is selected
01/4th; The reflection phase shift that Bragg mirror (2) selects the first different refractive index optical material H and the second refractive index optical material L to control Bragg mirror, thereby adjust the peak wavelength distance between two modes of resonance of microcavity, make their emission spectrum be matched to white light.
3. organic microcavity white light-emitting diode according to claim 1 is characterized in that: anode (3) and negative electrode (8) lay respectively at the node position of two mode of resonance standing wave field intensity in the microcavity; Luminescent layer (5) is in the wave amplitude position of the standing wave field intensity of two modes of resonance in the microcavity, thereby the luminous efficiency of white light is improved.
4. organic microcavity white light-emitting diode according to claim 2, it is characterized in that: keeping under the long constant situation in microcavity chamber, regulate the relative position of luminescent layer (5) in microcavity inside, relative luminous intensity between two modes of resonance can change thereupon, and the colorimetric purity of white light is optimized; The high reflectance of Bragg mirror (2) is less than the reflectivity of negative electrode (8), and white light is sent in substrate (1) one side, and the colorimetric purity of white light does not change with the variation of operating voltage.
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