KR101838043B1 - Transparent electronic device and method for manufacturing the same - Google Patents

Transparent electronic device and method for manufacturing the same Download PDF

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KR101838043B1
KR101838043B1 KR1020150149549A KR20150149549A KR101838043B1 KR 101838043 B1 KR101838043 B1 KR 101838043B1 KR 1020150149549 A KR1020150149549 A KR 1020150149549A KR 20150149549 A KR20150149549 A KR 20150149549A KR 101838043 B1 KR101838043 B1 KR 101838043B1
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layer
forming
electrode
ultra
thin metal
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KR20170049691A (en
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조관현
임중혁
강경태
이상호
강희석
황준영
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한국생산기술연구원
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    • H01L51/5203—
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L29/00—Semiconductor devices adapted for rectifying, amplifying, oscillating or switching, or capacitors or resistors with at least one potential-jump barrier or surface barrier, e.g. PN junction depletion layer or carrier concentration layer; Details of semiconductor bodies or of electrodes thereof  ; Multistep manufacturing processes therefor
    • H01L29/40—Electrodes ; Multistep manufacturing processes therefor
    • H01L29/41—Electrodes ; Multistep manufacturing processes therefor characterised by their shape, relative sizes or dispositions
    • H01L29/413—Nanosized electrodes, e.g. nanowire electrodes comprising one or a plurality of nanowires
    • H01L51/424—
    • H01L51/5088—
    • H01L51/5262—
    • H01L51/56—
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
    • H01L2924/10—Details of semiconductor or other solid state devices to be connected
    • H01L2924/11—Device type
    • H01L2924/12—Passive devices, e.g. 2 terminal devices
    • H01L2924/1204—Optical Diode
    • H01L2924/12044—OLED
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E10/00—Energy generation through renewable energy sources
    • Y02E10/50—Photovoltaic [PV] energy
    • Y02E10/549—Organic PV cells

Abstract

The present invention provides a semiconductor device comprising: a substrate; A stripe-shaped nano-auxiliary electrode repeatedly formed on the upper surface of the substrate at a predetermined distance; An ultra-thin metal electrode formed on an upper surface of the substrate and the nano-assist electrode; An organic layer formed on the upper surface of the ultra thin metal electrode; And a cathode layer formed on an upper surface of the organic layer, wherein the ultra-thin metal electrode includes a seed layer and a metal layer, and a method of manufacturing the same.

Description

[0001] TRANSPARENT ELECTRONIC DEVICE AND METHOD FOR MANUFACTURING THE SAME [0002]

The present invention relates to a transparent electronic device and a method of manufacturing the same. More particularly, the present invention relates to a transparent electronic device and a manufacturing method thereof. More particularly, the present invention relates to a transparent electronic device and a method of manufacturing the same. The present invention relates to a transparent electronic device which can be easily used in a flexible substrate and can maximize a light extraction effect by inducing a surface plasmon mode due to an ultra-thin metal film, and a manufacturing method thereof.

Transparent electronic devices are devices that have the purpose of eliminating the spatial / visual constraints of existing electronic devices using transparent characteristics. Transparent electronic devices are used in transparent devices that can be manufactured by actively utilizing transparency. They are used in a wide range of industries including optical and electronic products (displays, solar cells, smart windows, other, wearable devices) And so on. Accordingly, studies on transparent electronic devices have been actively conducted.

In the organic light emitting diode (OLED), one of the transparent electronic devices, only 20% of the emitted light is emitted to the outside, and 80% of the light is emitted from the glass or the transparent conductive substrate (ITO) constituting the organic light emitting diode and the organic layer, The efficiency of the diode is low.

In order to improve the light extraction efficiency of organic light emitting diodes (OLED), a microlens array is attached to the outside of the glass substrate, a scattering layer is coated, or a glass substrate mode light is extracted using a high refractive index glass substrate In order to improve light extraction efficiency of a waveguide mode between a transparent electrode such as ITO (Indium Tin Oxide) and an organic layer in which more light is trapped, a scattering layer may be interposed between the transparent electrode and the glass substrate, A method of introducing a photonic crystal structure having a size and an arrangement interval has been attempted. Also, a method of making the device itself into a corrugated structure or a wrinkled structure has been proposed. Also, a technique for forming an auxiliary electrode for improving a voltage drop phenomenon of an organic light emitting diode has been proposed.

Korean Patent Publication No. 10-2014-0090070 Korean Patent Publication No. 10-2006-0081190

Disclosure of the Invention The present invention has been made to solve the above problems of the prior art, and it is an object of the present invention to provide an ultra-thin metal film as a transparent electrode in order to maximize a light extraction effect by inducing a surface plasmon mode, And an object of the present invention is to provide a transparent electronic device and a manufacturing method thereof.

According to an aspect of the present invention, there is provided a transparent electronic device comprising: a substrate; A stripe-shaped nano-auxiliary electrode repeatedly formed on the upper surface of the substrate at a predetermined distance; An ultra-thin metal electrode formed on an upper surface of the substrate and the nano-assist electrode; An organic layer formed on the upper surface of the ultra thin metal electrode; And a cathode layer formed on an upper surface of the organic layer, wherein the ultra-thin metal electrode includes a seed layer and a metal layer.

At this time, the nano-auxiliary electrode may be formed at a period of 100 to 1000 nm.

The seed layer may be formed of at least one selected from the group consisting of Al, Ca, and Au.

The metal layer may be formed of a metal including Ag.

Further, a hole injection layer formed between the ultra-thin metal electrode and the organic layer may be further included.

Meanwhile, the hole injection layer may be formed of at least one selected from the group consisting of molybdenum oxide, zinc oxide, silver oxide, nickel oxide, and tungsten oxide.

The organic layer may have a structure in which a hole transporting layer, a light emitting layer, an electron transporting layer, and an electron injecting layer are sequentially stacked.

The organic layer may be composed of an organic material for a solar cell including a hole transport layer, a photoactive layer, an electron transport layer, and an electron injection layer.

According to another aspect of the present invention, there is provided a method of manufacturing a transparent electronic device, comprising: forming a nano-auxiliary electrode by patterning a high-conductive material on a substrate (step a); Forming an ultra-thin metal electrode on an upper surface of the substrate and the nano-assist electrode (step b); Forming an organic layer on the upper surface of the ultra-thin metal electrode (step c); And forming a cathode layer on an upper surface of the organic layer (step d), wherein the ultra-thin metal electrode forming step includes a seed layer forming step and a metal layer forming step.

The step a may be performed by a method of forming a stripe-shaped nano-auxiliary electrode at a period of 100 to 1000 nm.

The step b may be performed by a vacuum thermal deposition method.

The seed layer forming step may be performed by forming a thin film of at least one selected from the group consisting of Al, Ca and Au.

The metal layer forming step may be performed by forming a thin film using Ag.

And forming a hole injection layer between the step b and the step c.

The hole injection layer forming step may be performed by forming a thin film of at least one selected from the group consisting of molybdenum oxide, zinc oxide, silver oxide, nickel oxide, and tungsten oxide.

 The step c may be performed by sequentially laminating a hole transporting layer, a light emitting layer, an electron transporting layer, and an electron injecting layer.

The step c may be performed by a method of forming an organic layer using an organic material for a solar cell including a hole transport layer, a photoactive layer, an electron transport layer, and an electron injection layer.

According to the present invention, the problem of the conventional ITO electrode can be solved by realizing an ultra-thin metal film as a transparent electrode. Specifically, since the conventional ITO electrode has a weak mechanical strength and is easily broken, there is a problem that the surface resistance of the electrode increases as the electrode substrate for a flexible display is warped. However, the ultra-thin metal film has a very strong mechanical strength, The flexible substrate can be easily used. Also, by realizing an ultra-thin metal film as a transparent electrode, light extraction efficiency can be remarkably improved.

In addition, the transparent electronic device according to the present invention can be widely used in electronic fields such as LCD front electrodes, OLED electrodes, displays, touch screens, solar cells, and optoelectronic devices.

1 is a schematic view showing a cross-sectional structure of a transparent electronic device according to an embodiment of the present invention.
2A to 2E are cross-sectional views illustrating a method of manufacturing a transparent electronic device according to an embodiment of the present invention.
3 is an SEM image of an Al (1 nm) / Ag structure and an Ag single structure thin film.
FIG. 4 is a graph of light transmittance of Al (1 nm) / Ag structure and Ag single structure thin film.

Hereinafter, preferred embodiments of the present invention will be described with reference to the accompanying drawings. However, the embodiments of the present invention can be modified into various other forms, and the scope of the present invention is not limited to the embodiments described below. The shape and the size of the elements in the drawings may be exaggerated for clarity and the same elements are denoted by the same reference numerals in the drawings.

And throughout the specification, when a part is referred to as being "connected" to another part, it includes not only "directly connected" but also "electrically connected" with another part in between. Also, when a component is referred to as " comprising "or" comprising ", it does not exclude other components unless specifically stated to the contrary .

FIG. 1 is a cross-sectional view of a transparent electronic device according to an embodiment of the present invention, and FIGS. 2A to 2E are views illustrating a method of manufacturing a transparent electronic device according to an embodiment of the present invention. The transparent electronic device 100 according to an embodiment of the present invention as shown in FIGS. 1 to 2E includes a substrate 110, a nano-auxiliary electrode 120, an ultra-thin metal electrode 130, an organic layer 140, Layer 160, and the ultra-thin metal electrode 130 comprises a seed layer and a metal layer.

First, referring to FIGS. 1 and 2A, the nano-auxiliary electrode 120 can be repeatedly formed on the upper surface of the substrate 110 with a predetermined distance therebetween. At this time, the substrate 110 may be made of a material selected from the group consisting of polycarbonate, polyether sulfone (PES), polyethylene terephthalate (PET), polyethylene naphthalate (PEN), polyimide (PI), polyarylate But is not limited thereto.

The nano-assist electrode 120 may be formed of a highly conductive material such as aluminum (Al), silver (Ag), copper (Cu), magnesium (Mg), nickel (Ni) By forming the nano-auxiliary electrode 120, the voltage drop problem due to the conductive limit of the transparent electrode can be improved. In addition, the nano-auxiliary electrode 120 may be formed in a stripe shape having a period of 100 nm or more and 1000 nm or less. The light extraction can be easily performed by the nano-auxiliary electrode formed at the period of the above range. The width of the stripe-shaped nano pattern can be defined as a fill factor (FF) = (width of auxiliary electrode / period of auxiliary electrode), and the fill factor (FF) can be 0 or more and 50 or less. In addition to the stripe structure, the shape of the auxiliary electrode may be a rectangle structure or a square-delta structure.

Figure 112015104376977-pat00001

As shown in FIGS. 1, 2B and 2C, an ultra-thin metal electrode 130 may be formed on the upper surface of the substrate 110 and the nano-assist electrode 120. The ultra-thin metal electrode 130 may be formed by a vacuum thermal deposition method. The vacuum thermal deposition method may be performed in a vacuum chamber at a pressure ranging from 1 × 10 -3 to 10 -10 Torr and a temperature ranging from 20 ° C. to 500 ° C. The step of forming the ultra-thin metal electrode 130 may include a step of forming the seed layer 132 and a step of forming the metal layer 131. The ultra-thin metal electrode 130 is composed of a seed layer 132 and a metal layer 131, and the ultra-thin metal film is implemented as a transparent electrode. The ultra thin metal film has an advantage of maximizing the light extraction effect by inducing the surface plasmon mode to the anode. Specifically, the ultra-thin metal film is combined with a nano-assisted electrode grating to facilitate light extraction by the surface plasmon mode by a Bragg scattering effect. In the case of an electronic device using an ITO electrode, a waveguide mode is induced in the organic layer and the ITO electrode, so that only light extraction by the waveguide mode is possible by the auxiliary electrode and light extraction by the surface plasmon mode is not possible. According to the invention, the surface plasmon mode is additionally induced in the silver (Ag) layer, so that the light of the guided mode as well as the light of the waveguide mode induced by the nano-auxiliary electrode is further extracted. According to the present invention, it is possible to extract light by the surface plasmon mode, and ultimately the emission efficiency of a transparent electronic device such as an OLED can be remarkably improved.

 The thickness of the seed layer 132 of the ultra-thin metal electrode 130 may be 0.5 nm to 2 nm, and more preferably 1 nm. The thickness of the metal layer 131 may be 4 to 16 nm, and more preferably 4 to 10 nm.

The seed layer may include at least one selected from the group consisting of Al, Ca, and Au. By including a seed layer in the ultra-thin metal electrode, excellent smoothness and continuity of the thin film can be realized, and ultimately the light transmittance can be dramatically increased.

The metal layer may be made of silver (Ag).

1 and 2D, the transparent electronic device 100 may further include a hole injection layer 140 formed between the ultra-thin metal electrode 130 and the organic layer 150. Referring to FIG. Hole injection layer 140 may be formed of one or more selected from the group consisting of molybdenum oxide (MoO 3), zinc oxide (ZnO), silver oxide (AgO x), nickel oxide (NiO), and tungsten oxide (WO 3) .

On the other hand, as shown in FIGS. 1 and 2E, the organic layer 150 may be formed on the upper surface of the hole injection layer 140. The organic layer 150 may have a structure in which a hole transport layer, a light emitting layer, an electron transport layer, and an electron injection layer are sequentially stacked.

The hole transporting layer may be formed of at least one selected from the group consisting of poly (9,9-dioctylfluorene-co-bis-N, N '- (4-butylphenyl) (9,9-dioctylfluorene-co-bis-N, N'- (4-butylphenyl) -bis-N, N'-phenyl-1,4-phenylenediamine), PEDOT: poly (styrenesulfonate) -doped poly 3,4-ethylenedioxythiophene) or a p-type metal oxide (NiO, WO 3, etc.), but the present invention is not limited thereto.

The light emitting layer may be composed of a spirofluorene-based light emitting polymer or the like. However, the present invention is not limited thereto.

The electron transporting layer may include oxadiazole or the like. However, the present invention is not limited thereto.

The electron injection layer may include BaF 2 or the like. However, the present invention is not limited thereto.

The organic layer 150 may be formed by sequentially stacking a hole transport layer, a photoactive layer, an electron transport layer, and an electron injection layer. That is, an organic material for a solar cell. The photoactive layer consists of an electron donor poly (3-hexylthiophene), P3HT and an Acceptor 1- (3-methoxycarbonyl) propyl-1-phenyl [6, 6] C61, PCBM), and the like. The hole transporting layer, the electron transporting layer and the electron injecting layer are the same as those described above.

On the other hand, the cathode layer 160 may be formed on the organic layer 150. The cathode layer 160 may be made of at least one selected from the group consisting of Li, Ca, Ba, Cs, Na, Mg, Al and Ag. However, the present invention is not limited thereto.

Hereinafter, a method of manufacturing a transparent electronic device according to an embodiment of the present invention will be described in detail.

Example: Fabrication of transparent electronic device for OLED

A PC (Polycarbonate) substrate was used as the substrate. Aluminum, which is a highly conductive material, was patterned on the substrate to form stripe-shaped nano-auxiliary electrodes at intervals of 500 nm. At this time, the thickness of the nano-auxiliary electrode was set to 200 nm. The patterning can be made using laser interference lithography (a technique of forming a pattern by exposing an interference fringe created by two or more lasers to a photoresist layer as a photosensitive material). Then, an ultra-thin metal electrode was formed on the upper surface including the substrate and the nano auxiliary electrode by a thermal deposition method. As the ultra-thin metal electrode, a seed layer having a thickness of 1 nm was formed by Al, and a metal layer (thickness of 4 to 16 nm) was formed. Then, a hole injection layer of 40 nm in thickness of MoO 3 was formed on the upper surface of the ultra-thin metal electrode. N, N'-phenyl-1,4-phenylenediamine) (poly (9,9-dioctylfluorene-co-bis- N, N'-phenyl-1,4-phenylenediamine (PFB, a hole transport material manufactured by Dow Chemical) was spin-coated to form 50 nm A light emitting layer having a thickness of 70 nm was formed on the hole transporting layer by using a spirofluorene-based light emitting polymer as a blue light emitting material, and oxadiazole was deposited on the light emitting layer to form a 40 nm thick electron transporting layer Then, BaF 2 was deposited to form an electron injection layer having a thickness of 4 nm. A cathode layer having a thickness of 2.7 nm and Al having a thickness of 150 nm was formed on the electron injection layer. A transparent electronic device was manufactured.

Experimental Example 1: SEM analysis

A thin film prepared by thermally depositing an Al layer of 1 nm on a polycarbonate substrate and then thermally vapor-depositing an Ag layer of 4 to 10 nm and an Ag layer of 4 to 10 nm deposited on a polycarbonate substrate were subjected to SEM (scanning electron microscope). The results are shown in Fig. It was confirmed that the Al (1 nm) / Ag structure was superior in smoothness and continuity as compared with the Ag single structure.

Experimental Example 2: Analysis of light transmittance

A thin film prepared by thermally depositing an Al layer of 1 nm on a polycarbonate substrate and then thermally depositing an Ag layer of 4 to 16 nm and a thin film formed by thermally depositing an Ag layer of 4 to 16 nm on a polycarbonate substrate, And the results are shown in FIG. The light transmittance of the thin film was measured using a UV-Vis spectrophotometer (Varian, Cary 5000). The incident beam was measured in the region of 200 to 800 nm by adjusting the incident angle of the incident light to 90 degrees on the thin film surface. As shown in FIG. 3, it was confirmed that the Al (1 nm) / Ag structure exhibits a higher transmittance than the Ag single structure.

While the invention has been shown and described with reference to certain preferred embodiments thereof, it will be understood by those of ordinary skill in the art that various changes in form and details may be made therein without departing from the spirit and scope of the invention as defined by the appended claims. Therefore, the technical scope of the present invention should be defined by the appended claims.

100: transparent electronic device
110: substrate
120: Nano-auxiliary electrode
130: ultra-thin metal electrode
131: metal layer
132: Seed layer
140: Hole injection layer
150: organic layer
160: cathode electrode

Claims (17)

Board;
A stripe-shaped nano-auxiliary electrode repeatedly formed on the upper surface of the substrate at a predetermined distance;
An ultra-thin metal electrode formed on an upper surface of the substrate and the nano-assist electrode;
An organic layer formed on the upper surface of the ultra thin metal electrode; And
And a cathode layer formed on an upper surface of the organic layer,
Wherein the ultra-thin metal electrode comprises a seed layer formed of Al and a metal layer formed of Ag,
And the metal layer formed of Ag is formed to a thickness of 4 to 10 nm.
The method according to claim 1,
Wherein the nano-assist electrode is formed at a period of 100 to 1000 nm.
delete delete The method according to claim 1,
And a hole injection layer formed between the ultra-thin metal electrode and the organic layer.
The method of claim 5,
Wherein the hole injection layer is formed of at least one selected from the group consisting of molybdenum oxide, zinc oxide, silver oxide, nickel oxide, and tungsten oxide.
The method according to claim 1,
Wherein the organic layer is a structure in which a hole transporting layer, a light emitting layer, an electron transporting layer, and an electron injecting layer are stacked in this order.
The method according to claim 1,
Wherein the organic layer is composed of an organic material for a solar cell, the hole transport layer, the photoactive layer, the electron transport layer, and the electron injection layer.
Patterning a highly conductive material on the substrate to form a nano-assist electrode (step a);
Forming an ultra-thin metal electrode on an upper surface of the substrate and the nano-assist electrode (step b);
Forming an organic layer on the upper surface of the ultra-thin metal electrode (step c); And
And forming a cathode layer on an upper surface of the organic layer (step d)
The ultra-thin metal electrode forming step includes a seed layer forming step and a metal layer forming step,
The seed layer forming step is performed by forming a thin film using Al,
Wherein the metal layer forming step is performed by forming a thin film having a thickness of 4 to 10 nm using Ag.
The method of claim 9,
Wherein the step (a) is performed by forming a stripe-shaped nano-auxiliary electrode at a period of 100 to 1000 nm.
The method of claim 9,
Wherein the step (b) is performed by a vacuum thermal deposition method.
delete delete The method of claim 9,
And forming a hole injection layer between the step (b) and the step (c).
15. The method of claim 14,
Wherein the step of forming the hole injection layer is performed by a method of forming a thin film of at least one selected from the group consisting of molybdenum oxide, zinc oxide, silver oxide, nickel oxide and tungsten oxide.
The method of claim 9,
Wherein the step c) is performed by sequentially laminating a hole transport layer, a light emitting layer, an electron transport layer, and an electron injection layer.
The method of claim 9,
Wherein the step c is performed by a method of forming an organic layer using an organic material for a solar cell including a hole transport layer, a photoactive layer, an electron transport layer, and an electron injection layer.
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