JP3518682B2 - Organic electroluminescence device - Google Patents

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to an electroluminescence device having a light emitting layer formed by layering such a substance by utilizing the electroluminescence of a substance which emits light when an electric current is injected. The present invention relates to an organic electroluminescence device configured as a light emitting body.

[0002]

2. Description of the Related Art As an organic electroluminescence device of this type, as shown in FIG.
2 and an organic phosphor thin film (light emitting layer) 3 and an organic hole transport layer 4 which are laminated on each other, are disposed between the transparent electrode 2 and an anode transparent electrode 2 made of indium tin oxide (hereinafter, also referred to as ITO). Layered structures are known. In addition, as shown in FIG. 2, an organic electron transport layer 5, a light emitting layer 3 and an organic hole transport layer 4 which are laminated on each other between the metal electrode 1 and the transparent electrode 2.
A three-layer structure in which is arranged is also known. Here, the organic hole transport layer 4 has a function of facilitating injection of holes from the anode 2 and a function of blocking electrons, and the organic electron transport layer 5 has a function of facilitating injection of electrons from the cathode 1. is doing. In these organic electroluminescence elements, a glass substrate 6 is arranged outside the transparent electrode 2 of the anode. The recombination of the electrons injected from the metal electrode 1 and the holes injected from the transparent electrode 2 produces excitons,
The excitons emit light in the process of radiation deactivation, and the light passes through the transparent electrode 2 and the glass plate 6 and is emitted to the outside.
By using a transparent electrode with a large work function and a metal electrode with a small work function,
It is known that the efficiency of injecting charges is increased and the emission efficiency is improved.

For example, in the two-layered organic electroluminescent device shown in FIG. 1, as shown in FIG.
There are X and Y matrix types. A part of the cross section along the line AA 'in FIG. 3 is shown in FIG. The organic electroluminescence device comprises a plurality of transparent electrodes 2 such as ITO, a hole transport layer 4, a light emitting layer 3, and a transparent electrode 2 on a glass transparent substrate 6.
It is formed by sequentially stacking a plurality of metal cathodes 1 intersecting with each other. A light emitting portion to be an organic electroluminescence device is formed by the transparent anode 2 and the metal cathode 1 which sandwich the hole transport layer 4 and the light emitting layer 3 and face each other, and each of the transparent anode 2 and the metal cathode 1 is formed. One pixel is formed with the light emitting portions in the intersecting region portion that face each other and intersect each other as one unit.

By driving a panel in which a plurality of such organic electroluminescent elements are formed on one element substrate according to the number of pixels through a transparent anode 2 and a metal cathode 1 protruding from the periphery thereof, A flat display device is constructed.

[0005]

However, even an organic electroluminescence device capable of emitting light with a relatively high luminance is still insufficient in light emission efficiency.
Further, in a display device using this organic electroluminescence element, there is a problem that the resistance value of the transparent electrode line becomes very large as the substrate provided with a large number of transparent electrodes becomes larger and finer. .

The present invention has been made to meet the above-mentioned conventional demands, and provides an organic electroluminescence device capable of suppressing the increase in the resistance value of a transparent electrode line and allowing an organic phosphor to emit light with high luminous efficiency. The purpose is to do.

[0007]

The organic electroluminescence device of the present invention is an organic electroluminescence device in which an anode, a hole transport layer made of an organic compound, a light emitting layer made of an organic compound and a cathode are laminated in this order, It is characterized by having an insulating film for reducing a current flowing through a part of the light emitting layer.

[0008]

According to the present invention, in the organic electroluminescence device, by providing an insulating film on the anode, the efficiency of injecting hole charges is partially reduced, and the device does not participate in light emission emitted to the outside. Since the current value is reduced and the resistance value of all the anodes in which the metal film and the anode are integrated is reduced, it is possible to obtain an organic electroluminescence device having high luminous efficiency.

[0009]

Embodiments of the organic electroluminescent device according to the present invention will be described below with reference to the drawings. As shown in FIG. 4, the organic electroluminescent element of this example comprises a transparent anode 2, a transparent anode 2, a metal film 7 having a work function lower than that of the anode, an organic hole transport layer 4, and an organic compound, as shown in FIG. In the two-layer structure in which the light emitting layer 3 and the metal cathode 1 are sequentially stacked, the metal film 7 is stacked in a part between the anode 2 and the hole transport layer 4. Alternatively, as shown in FIG. 5, the organic electroluminescent element of the present embodiment is
A transparent anode 2, a metal film 7 having a work function lower than that of the anode 2, an organic hole transport layer 4, a light emitting layer 3 made of an organic compound, an electron transport layer 5, and a metal cathode 1 were sequentially laminated on a glass transparent substrate 6. In the three-layer structure, the metal film 7 may be laminated on a part between the anode 2 and the hole transport layer 4.

For the cathode 1, a metal having a small work function such as aluminum, magnesium, indium, silver, or an alloy of each (for example, the work function of an Al--Li alloy = about 3.0).
eV) having a thickness of about 100 to 5000 Å can be used. For the anode 2, a conductive material having a large work function such as ITO (ITO work function = about 5.0e
V) and has a thickness of about 1000 to 3000 Å, or gold (work function of Au = about 5.1 eV) and a thickness of 800 to
About 1500Å can be used. When gold is used as the electrode material, the electrode becomes semitransparent.

The metal film 7 laminated on a part between the anode 2 and the hole transport layer 4 includes aluminum used for the cathode 1,
A metal having a small work function such as magnesium, indium, silver, or an alloy of each is used. When ITO having a large work function is used for the anode 2, the metal film 7 has a small work function, for example, Al-Li, In-Li, Mg-Sr, Al-S.
r alloys may be used. The work function showing the energy (eV) required to extract one electron from the surface of a metal or the like to the outside of the vacuum is sensitively changed depending on the surface state such as impurities or adsorption even with the same metal. The work functions of the components are In = about 4.12 eV and Li = about 2.9 e.
V, Mg = about 3.66 eV, Sr = about 2.59 eV, A
1 = about 4.28 eV and Ag = about 4.26 eV.

FIG. 6 shows an exemplary embodiment of the metal film 7 laminated on a part between the anode 2 and the hole transport layer 4. Figure 6 (a)
4 shows the case where the metal film 7 is laminated along the edge of the anode 2 so as to partially cover the surface of the anode 2 as shown in FIGS. FIG. 6B shows a case where the metal film 7 is laminated so as to partially cover the surface of the anode 2 over the edge of the anode 2 and the transparent substrate 6. FIG. 6C shows a case where the metal film 7 is laminated so as to partially cover the surface of the anode 2 at the central portion on the anode 2. Further, the partially formed metal film 7 may be laminated continuously or intermittently on the anode 2 along the extension direction thereof. 6 (a) to 6 (c)
As shown in FIG. 6, the side surface of the anode 2 may be formed on the transparent substrate 6 at a substantially right angle by anisotropic etching or the like. Further, as shown in FIG. When formed as an inclined surface, the metal film 7 is laminated so as to cover the surface of the inclined side surface and be adjacent to each other. In addition,
The metal film 7 may be a single metal or an alloy composed of a plurality of metals, and one having a work function as low as possible is more effective.

The metal film 7 suppresses the injection of holes from the transparent electrode 2 side into the hole transport layer 4 and the light emitting layer 3 in the Q portion shown in FIG. The flowing current can be reduced and the anode 2
Also, the resistance value of the metal film 7 in the extending direction decreases. By the way, a substrate with a transparent electrode is also used in a general flat display device such as a liquid crystal display or an inorganic electroluminescence display, and there is a problem that the resistance value of the transparent electrode line increases with the increase in size and definition of the substrate. In order to solve this, a method of partially inserting the metal film 15 between the transparent substrate 11 and the ITO transparent electrode 12 as shown in FIG. 7 can be considered.

Based on this technique, as shown in FIG. 8, a metal film 15, a transparent anode 12,
When an organic electroluminescence device in which the organic hole transport layer 4, the light emitting layer 3 and the metal cathode 1 are laminated in this order is made, the light emission of the P portion in FIG. 8 is blocked by the metal film 15 and flows through this P portion. Current is wasted and efficiency is poor. Therefore, as shown in FIG. 9, the insulating film 1 is partially formed on the transparent electrode 12.
A method of preventing light emission from the P section and eliminating the current flowing through this section by stacking 6 is considered. However, in this method, the number of steps of photolithography increases, mask alignment becomes complicated, and its manufacturing becomes complicated.

In the present invention, as shown in FIGS. 4 to 6, by laminating the metal film 7 having a work function lower than that of the transparent electrode 2 on a part of the transparent electrode, the complexity is eliminated. That is, according to the present invention, the same effect can be achieved with a simple structure without using the complicated structure shown in FIG. Example 1 First, ITO (work function =
After forming about 5.0 eV) with a thickness of about 1000 Å to a width of 2 mm to form a transparent anode, an Al-Li alloy (work function = about 3.
0 eV) to about 500 by a vacuum deposition method of 10 ⁻⁵ Torr or less.
A film having a thickness of Å was formed, and a metal film was formed by patterning by photolithography on the edge of the transparent electrode so as to have a width of 0.5 mm along the ITO extension direction. N, N'-diphenyl- was formed on the substrate on which the transparent electrode and the metal film were laminated.
Organic hole-transporting layer made of N, N'-bis (3methylphenyl) -1,1'-biphenyl-4,4'-diamine (TPD) and organic layer made of tris (8-quinolinol) aluminum (Alq3) About 500Å for each light emitting layer
After being formed with a film thickness, an Al-Li alloy having a film thickness of about 1000 Å was formed with a width of 2 mm in a direction orthogonal to the ITO transparent electrode line to serve as a metal cathode, and an organic electroluminescence device having an area of 2 mm x 2 mm was produced.

A solid line A in FIG. 10 shows a graph of current-luminance characteristics of the manufactured device. Also, the broken line B shown in this graph
Example 1 except that a metal having a work function higher than that of ITO, for example, Pt (work function = about 5.65 eV) was used for the metal film.
The current-luminance characteristic of the organic electroluminescent element of the comparative example produced similarly to is shown. As shown in the graph,
The efficiency of Example 1 was higher than that of the device of Comparative Example using a metal film having a work function higher than that of ITO. (Embodiment 2) The following is an embodiment in which the present invention is applied to a transparent electrode having a double matrix structure.

As shown in FIG. 11A, the ITO transparent electrode 2 is formed on the glass substrate 6 and patterned by photolithography, and then the Al--Li alloy metal film 7 is ITO.
The transparent electrode 2 was intermittently formed in an intermediate portion S between the island-shaped light emitting portion electrode regions R with a film thickness of about 500 Å by vacuum deposition of 10 ^-5 Torr or less and photolithography. After forming an organic hole transport layer of TPD and an organic light emitting layer of Alq3 on this substrate with a film thickness of about 500Å over the entire surface, I
11B in a direction orthogonal to the TO transparent electrode line 2.
As shown in, Al-Li alloy metal cathode 1 (two-dot chain line)
Was formed with a thickness of 1000Å to prepare an organic electroluminescence device. FIG. 12 shows a part of the cross section taken along line BB ′ of FIG. 11.

First, the ITO transparent electrode line 2 of this substrate
The resistance value of was measured to be about 0.5 KΩ. IT
The resistance value of the ITO transparent electrode line 2 of the comparative example in which the Al—Li alloy metal film 7 is not laminated on the O transparent electrode line 2 is about 4.4 KΩ, and the line resistance value is significantly reduced in Example 2. I was able to. When the element of Example 2 was driven at about 10 V, the island-shaped light emitting portion electrode region R portion shown in FIG. 11B emitted bright green light. Also, FIG. 11 (b)
The intermediate portion S portion shown in (1) did not emit light, and the current flowing through the portion S in the film thickness direction was about 1/1000 of that of the R portion, which was very small.

[0019]

As described above, according to the present invention,
An organic electroluminescence device in which an anode, a hole transport layer made of an organic compound, a light emitting layer made of an organic compound, and a cathode are sequentially laminated, and the work function of the anode and the hole transport layer is partially laminated between the anode and the anode. Since it has a low metal film, it is possible to obtain an organic electroluminescence element having a high luminous efficiency, which is easy to manufacture and has a transparent electrode substrate having a low resistance value.

[Brief description of drawings]

FIG. 1 is a schematic partial cross-sectional view of an organic electroluminescence element.

FIG. 2 is a schematic partial sectional view of an organic electroluminescence element.

FIG. 3 is a schematic partially cutaway perspective view of the organic electroluminescent element shown in FIG.

FIG. 4 is a schematic partial cutaway perspective view of an organic electroluminescence device of an example according to the present invention.

FIG. 5 is a schematic partial cross-sectional view of an organic electroluminescent element of an example according to the present invention.

FIG. 6 is a schematic partial cross-sectional view showing an exemplary embodiment in which the metal film in the organic electroluminescence element of the present invention is laminated on a part of the anode and the hole transport layer.

FIG. 7 is a schematic partial cross-sectional view of a substrate with a transparent electrode in a flat display device.

FIG. 8 is a schematic partial cross-sectional view of an organic electroluminescence element.

FIG. 9 is a schematic partial cross-sectional view of an organic electroluminescence element.

FIG. 10 is a graph showing current-luminance characteristics of organic electroluminescent elements of Examples and Comparative Examples according to the present invention.

FIG. 11 is a schematic plan view showing constituent members during a manufacturing process of an organic electroluminescent element having a transparent electrode having a double matrix structure according to an example of the present invention.

FIG. 12 is a schematic partial cross-sectional view showing a part of the cross section taken along the line BB ′ of FIG. 11.

[Explanation of symbols for main parts]

1 Cathode, metal electrode 2 Anode, transparent electrode 3 Organic light emitting layer 4 Organic hole transport layer 5 Organic electron transport layer 6 substrate 7 Metal film with a lower work function than the anode

─────────────────────────────────────────────────── ─── Continuation of the front page (72) Inventor Teruichi Watanabe 6-1, 1-1 Fujimi, Tsurugashima City, Saitama Pioneer Co., Ltd. Research Institute (56) Reference JP-A-5-307997 (JP, A) Japanese Patent Application Laid-Open No. 4-82197 (JP, A) Japanese Patent Application Laid-Open No. 4-67596 (JP, A) Japanese Patent Application Laid-Open No. 4-51494 (JP, A) Japanese Patent Application Laid-Open No. 3-274694 (JP, A) Japanese Patent Application Laid-Open No. 3-250583 (JP , A) JP-A-1-134895 (JP, A) (58) Fields investigated (Int.Cl. ⁷ , DB name) H05B 33/00-33/28

Claims (2)

(57) [Claims] 1. A positive electrode, a hole transport layer comprising an organic compound,
An organic electroluminescence device in which a light emitting layer made of an organic compound and a cathode are sequentially stacked, and having an insulating film laminated on a part of an anode on an auxiliary electrode and reducing a current flowing through a part of the light emitting layer. An organic electroluminescence device characterized by the above. 2. The organic electroluminescent device according to claim 1, further comprising an organic electron transport layer disposed between the cathode and the light emitting layer.