KR20100091277A - Zinc oxide doping method using a dual dopant - Google Patents
Zinc oxide doping method using a dual dopant Download PDFInfo
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- KR20100091277A KR20100091277A KR1020090010393A KR20090010393A KR20100091277A KR 20100091277 A KR20100091277 A KR 20100091277A KR 1020090010393 A KR1020090010393 A KR 1020090010393A KR 20090010393 A KR20090010393 A KR 20090010393A KR 20100091277 A KR20100091277 A KR 20100091277A
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- Prior art keywords
- zinc oxide
- doping
- group
- group iiia
- transparent conductive
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- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 title claims abstract description 123
- 238000000034 method Methods 0.000 title claims abstract description 34
- 239000011787 zinc oxide Substances 0.000 title claims description 58
- 239000002019 doping agent Substances 0.000 title description 12
- 230000009977 dual effect Effects 0.000 title description 2
- 239000010409 thin film Substances 0.000 claims description 25
- 239000011701 zinc Substances 0.000 claims description 15
- 229910052760 oxygen Inorganic materials 0.000 claims description 13
- 239000002243 precursor Substances 0.000 claims description 13
- 239000013078 crystal Substances 0.000 claims description 11
- 229910052731 fluorine Inorganic materials 0.000 claims description 11
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical group [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 9
- 239000001301 oxygen Substances 0.000 claims description 9
- JBQYATWDVHIOAR-UHFFFAOYSA-N tellanylidenegermanium Chemical group [Te]=[Ge] JBQYATWDVHIOAR-UHFFFAOYSA-N 0.000 claims description 3
- 239000012535 impurity Substances 0.000 abstract description 11
- 238000002834 transmittance Methods 0.000 abstract description 8
- 238000004519 manufacturing process Methods 0.000 abstract description 4
- 229910052733 gallium Inorganic materials 0.000 description 8
- 239000011261 inert gas Substances 0.000 description 8
- 229910052725 zinc Inorganic materials 0.000 description 7
- 230000007547 defect Effects 0.000 description 6
- 230000003287 optical effect Effects 0.000 description 6
- 229910005269 GaF 3 Inorganic materials 0.000 description 5
- 229910052782 aluminium Inorganic materials 0.000 description 5
- XOYLJNJLGBYDTH-UHFFFAOYSA-M chlorogallium Chemical compound [Ga]Cl XOYLJNJLGBYDTH-UHFFFAOYSA-M 0.000 description 4
- 229910052738 indium Inorganic materials 0.000 description 4
- 150000002500 ions Chemical class 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 239000004065 semiconductor Substances 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 229910007541 Zn O Inorganic materials 0.000 description 3
- 239000004020 conductor Substances 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 239000000758 substrate Substances 0.000 description 3
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- 125000004429 atom Chemical group 0.000 description 2
- 230000015556 catabolic process Effects 0.000 description 2
- 238000006731 degradation reaction Methods 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- HQWPLXHWEZZGKY-UHFFFAOYSA-N diethylzinc Chemical compound CC[Zn]CC HQWPLXHWEZZGKY-UHFFFAOYSA-N 0.000 description 2
- AXAZMDOAUQTMOW-UHFFFAOYSA-N dimethylzinc Chemical compound C[Zn]C AXAZMDOAUQTMOW-UHFFFAOYSA-N 0.000 description 2
- 238000002844 melting Methods 0.000 description 2
- 230000008018 melting Effects 0.000 description 2
- 230000009257 reactivity Effects 0.000 description 2
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910052796 boron Inorganic materials 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 125000001309 chloro group Chemical group Cl* 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- UPWPDUACHOATKO-UHFFFAOYSA-K gallium trichloride Chemical compound Cl[Ga](Cl)Cl UPWPDUACHOATKO-UHFFFAOYSA-K 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 1
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000000197 pyrolysis Methods 0.000 description 1
- 238000010405 reoxidation reaction Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 238000010897 surface acoustic wave method Methods 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- VTDQBKLDBJKTMS-UHFFFAOYSA-N trihydrate;hydrofluoride Chemical compound O.O.O.F VTDQBKLDBJKTMS-UHFFFAOYSA-N 0.000 description 1
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/02—Details
- H01L31/0224—Electrodes
- H01L31/022466—Electrodes made of transparent conductive layers, e.g. TCO, ITO layers
- H01L31/022483—Electrodes made of transparent conductive layers, e.g. TCO, ITO layers composed of zinc oxide [ZnO]
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/18—Processes or apparatus specially adapted for the manufacture or treatment of these devices or of parts thereof
- H01L31/1884—Manufacture of transparent electrodes, e.g. TCO, ITO
-
- 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
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- Engineering & Computer Science (AREA)
- Physics & Mathematics (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- Electromagnetism (AREA)
- General Physics & Mathematics (AREA)
- Computer Hardware Design (AREA)
- Microelectronics & Electronic Packaging (AREA)
- Power Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Non-Insulated Conductors (AREA)
- Physical Vapour Deposition (AREA)
- Crystals, And After-Treatments Of Crystals (AREA)
Abstract
The present invention is a method of doping zinc oxide (ZnO) for the production of transparent conducting oxide (TCO), an improved method of obtaining a transparent conductive electrode by doping the existing single species of impurities, The present invention relates to a method for producing a transparent conductive oxide capable of obtaining high electrical conductivity and light transmittance by simultaneously doping with impurities.
The doping method according to the present invention has a constitutive feature in double doping a group IIIA element and a group IIIA element.
Description
The present invention is a doping method for producing a transparent conducting oxide (TCO), more specifically a method of doping a single type of impurities in zinc oxide, rather than doping by using two kinds of impurities simultaneously, The present invention relates to a doping method for obtaining electrical conductivity and light transmittance.
Zinc Oxide (ZnO) is a typical transparent oxide direct transition semiconductor material with a wide band gap of 3.37 eV. The exciton binding energy is 60 meV, and light gum including light emitting devices such as LEDs and LDs in blue and UV regions using excitons at room temperature. It is expected to be applied to next-generation photovoltaic materials to replace III-V compound semiconductors such as photo sensors.
Ultraviolet and blue light blockers, gas sensors, surface acoustic wave devices, UV-based optical sensors, active layers of transparent transistors in next-generation displays, and lean magnetic semiconductors doped with transition metals Semiconductor, DMS), active layer of the dye-sensitized solar cell (Dye Sensitized solar cell) has been widely studied.
The most promising field for such industrial application of zinc oxide is transparent conductive oxide. Transparent conductive oxides have been studied in many fields such as solar cells, flat panel displays, and functional coatings because they can control electrical properties from insulation to high conductivity as well as transparent optical properties in the visible region.
On the other hand, indium tin oxide (ITO), which is widely used in displays and solar cells, has problems such as environmental problems, human hazards, limited resources, and low economy due to high price. Zinc oxide thin films doped with Group IIIA elements, such as Group IIIA elements such as F and Cl, are transparent for displays and solar cells due to their high electrical conductivity, environmentally friendly harmlessness to humans, stability to hydrogen plasma, and economical efficiency due to abundant reserves. It is attracting attention as an electrode.
Summarizing the research reports of zinc oxide TCO to date, the direction of the study can be summarized as an effort to obtain a thin film having a low resistivity and a high visible light transmittance.
In the case of zinc oxide TCO for display, it aims to realize a zinc oxide thin film having a transmittance of 80% or more and a resistivity of 10 −5 Ωcm or less. The lower the specific resistivity, the lower the power consumption, which can increase the use time of battery power, which is limited in applications such as portable display devices. In addition, the higher the transparency, the higher the power generation efficiency.
In the case of TCO for solar cells, it aims at a light transmittance of more than 80% and a resistivity of 10 -5 Ωcm as in the display. In order to satisfy the required characteristics of the zinc oxide thin film, a process of depositing a transparent conductive oxide and a dopant Efficient selection of
On the other hand, the dopants of zinc oxide include group IIIA elements B, Al, Ga, and In, which have more electrons than zinc, and F, Cl, Br, etc. of Group VIIIA which have one electron more than oxygen (O). have.
However, in the case of aluminum (Al) and indium (In), which are considered as dopants of zinc oxide, the lattice defects are not only prone to occur due to a large difference in atomic radius between zinc to be substituted, but also have high reactivity with oxygen and thus resistivity of the thin film. There is a disadvantage that the transmittance is changed. Moreover, the high reactivity with oxygen also affects the reliability of the formed thin film. In the high temperature and high humidity environment, the increase in the specific resistance of zinc oxide is due to the absorption of water molecules, mostly oxygen incomplete oxygen vacancy or dopant. The theory is that it is due to the reoxidation of.
In addition, in the case of zinc oxide doped with aluminum or a conventional single dopant, when the dopant content is increased in order to increase the electrical conductivity of the formed thin film, the specific resistance increases due to the decrease in mobility due to the increase in the density of the carrier, thereby increasing the target electrical conductivity. Problems are difficult to obtain.
The present invention has been made to improve the conventional problems caused by the change in the electrical conductivity or transparency due to the above-described crystal lattice defects and the increase in the resistivity according to the increase of the carrier density, and to control the cause of the crystal lattice defects and The problem to be solved by providing a doping method of zinc oxide that can implement a transparent conductive thin film with improved electrical conductivity compared to the prior art by improving the problem of mobility decrease with increasing concentration.
Another object of the present invention is to provide a method for doping a transparent conductive zinc oxide that can exhibit a high optical transmittance to be used for the transparent electrode of the solar cell.
It is another object of the present invention to provide a method for doping transparent conductive zinc oxide, which is structurally stable, simple in manufacturing, and non-toxic.
As a means for solving the above problems, the present invention provides a doping method for zinc oxide, characterized in that the group IIIA element and the Group VIIA element is doped in a double.
According to the conventional method of doping with only Group IIIA elements, when the concentration of the carrier is increased to increase the electrical conductivity of the formed transparent conductive oxide, the density of the positively charged donor level increases simultaneously. The effect of lattice scattering of the carriers is increased, which leads to a decrease in carrier mobility, which makes it difficult to obtain sufficient electrical conductivity.
However, according to the zinc oxide doping method according to the present invention, the group IIIA element supplies electrons by substituting Zn atoms in the crystal structure of zinc oxide (ZnO), as shown in FIG. Supplying electrons is characterized by its configuration.
This constitutional feature is that as the dopant used for ZnO, the group IIIA element occupies the position of substitution of Zn and the electrons are in local perturbation state in the conduction band of zinc oxide. While it causes a decrease in mobility due to the scattering effect, if the dopant is substituted for oxygen (O) rather than the zinc (Zn) position, the dopants are disturbed in the valence band and the relative mobility of electrons It is based on the concept that it can be increased.
In other words, excessive doping of the group IIIA element increases the density of the donor level, thereby increasing the electrical resistivity relatively, while the group IIIA element dopes only a certain amount, and the energy level inside the valence band. When doping the Group VIIA element is distributed, as shown in Figure 2 can increase the concentration of the carrier while maintaining its mobility can be sufficiently improved the electrical conductivity.
Further, in the doping method according to the present invention, the group IIIA element is preferably Ga and the group XVIIA element is F.
Ga not only reduces the lattice defect than Al because its atomic radius is similar to the atomic radius of Zn among group IIIA elements, but Ga is less reactive with oxygen than Al and In, so the specific resistance of Al and In The disadvantage of changing transmittance can be compensated for. In this respect, Ga improves the reliability of the formed transparent conductive thin film. Similarly, in the case of the Group VIIA element, F is preferable in terms of reducing lattice defects because its ion radius is similar to that of O.
In addition, in the doping method according to the present invention, the group IIIA element is Ga and the VIIA element is Cl.
When Ga atoms are structurally substituted at the Zn atomic position in zinc oxide, the atomic radius of Ga (r = 0.062 kV) is smaller than that of Zn, as shown in FIG. 1A. , The distance between Zn-O becomes short as compared with the case where Zn exists. This acts as a compressive force in the whole crystal structure, causing deformation of the whole crystalline and changing its structural and optical properties. On the contrary, when the Cl atom is substituted at the O atom position, since the atomic radius of Cl (r = 0.180) is larger than the ion radius of O (r = 0.140), as shown in FIG. 1B due to doping, O is present. The distance between Zn-O is far greater than that of Zn-O, which acts as a tensile force in the entire crystal structure, causing deformation of the entire crystalline, thereby changing the structural and optical properties. Therefore, by double doping the compressive force generating element and the tensile force generating element as in the present invention to be mutually offset, it is possible to minimize the internal deformation of the doped zinc oxide, it is possible to prevent the degradation of the optical properties due to the internal deformation.
In addition, in the doping method according to the present invention, the doping is characterized in that the doping using a single precursor containing both a Group IIIA element and Group VIIA element.
For example, it can be simpler than the doping process when using a single precursor such as GaCl 3 containing GaF 3 and H 2 O or a precursor, Ga and Cl containing Ga and F.
In addition, the present invention provides a doping method characterized by controlling the lattice scattering (lattice scattering) of the formed transparent conductive zinc oxide thin film through the double doping of the group IIIA element and Group VIIA element.
In addition, the present invention provides a doping method of zinc oxide, characterized in that the double doping of the Group IIIA element and Group VIIA element, and controlling the crystal structure through the difference in the ion radius of the Group IIIA element and Group VIIA element to be doped. do.
According to the doping method according to the present invention, a compressive force or tensile force that can be formed in the crystal lattice through the difference in the ion radius of Zn or O and the element substituted at the Zn or O site of zinc oxide (ZnO) By controlling the content of the doped group IIIA element and group VIIA element in consideration of the force), the degree of deformation in the crystal structure can be controlled to a desired shape.
In addition, the present invention is a transparent conductive zinc oxide thin film, at least one of the group IIIA element in the zinc oxide (ZnO) is a zinc (Zn) position and at least one of the group VIIA element in the position of oxygen (O) Provided is a transparent conductive zinc oxide, which is doped.
In addition, the present invention provides a transparent conductive zinc oxide thin film, characterized in that consisting of the following formula 1, when the upper limit of the doping amount exceeds 0.01, since the scattering effect is increased and the electrical conductivity is sharply dropped, it is maintained at 0.01 or less It is preferable.
Zn 1 - x O 1 -y : xGa, yA
[Where 0 <x ≦ 0.01 0 <y ≦ 0.01 and A is F or Cl]
According to the doping method according to the present invention, by double doping ZnO group IIIA element and Group VIIA element, it is possible to increase the concentration of the carrier while maintaining the mobility of the carrier, it is possible to improve the electrical conductivity.
In addition, according to the doping method according to the present invention, by double doping Ga and F having a similar atomic radius to Zn and O substituted in ZnO, lattice defects can be reduced to prevent the degradation of reliability such as increase in specific resistance over time have.
Further, according to the doping method according to the present invention, since ZnO is doped with two or more kinds of impurities, it is determined by controlling the stress state inside the crystal through the difference between the atomic radius of the impurity and the atomic radius of the element constituting the host lattice. You can adjust the structure.
Further, according to the doping method according to the present invention, the doping process can be simplified by using a single species of a material simultaneously containing a double doped Ga and impurities such as F or Cl as a precursor.
Hereinafter, a double doping method of zinc oxide according to a preferred embodiment of the present invention will be described with reference to the accompanying drawings, but the present invention is not limited to the following examples.
In an embodiment of the present invention, as a precursor for doping zinc oxide, GaF 3 ㆍ H 2 O (gallium fluoride trihydrate) is used as a precursor when double doping of Ga and F, GaF 3 · H 2 O is dissolved in water Therefore, it is a material that can overcome the disadvantages of GaF 3 , which shows high melting point and low solubility in water.
In the case of double doping of Ga and Cl, GaCl 3 (gallium chloride) may be used as a precursor. GaCl 3 has a low melting point of 77.9 ° C. and a high solubility in water, which is advantageous for doping.
In an embodiment of the present invention, a device configured as shown in FIG. 4 is used as a device for forming a double doped zinc oxide thin film using the precursor as described above.
As shown in FIG. 4, the thin film forming apparatus according to the exemplary embodiment of the present invention includes a zinc
The zinc
Like the zinc
When using the thin film forming apparatus configured as described above, the formation and doping of the zinc oxide thin film is performed as follows.
Ar and the like is controlled from the first inert gas tank 12 through the
In addition, Ar and the like from the second
As described above, the zinc oxide and the double doping precursor reached on the substrate are formed into a thin film by a known method such as drying and pyrolysis.
1A and 1B are conceptual views illustrating a form in which an impurity is substituted at the Zn position and an impurity in the O position of the ZnO oxide transparent conductive material, respectively.
2A and 2B are graphs showing the change in specific resistance according to the concentration of impurities during single doping and double doping, respectively.
3 is a conceptual diagram of a doping type in which impurities are simultaneously substituted at Zn and O positions in a ZnO oxide transparent conductive material.
Figure 4 is a schematic diagram of a ZnO transparent oxide thin film growth apparatus according to an embodiment of the present invention for double doping the ZnO oxide transparent conductive material.
Claims (10)
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| KR1020090010393A KR20100091277A (en) | 2009-02-10 | 2009-02-10 | Zinc oxide doping method using a dual dopant |
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| Application Number | Priority Date | Filing Date | Title |
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| KR1020090010393A KR20100091277A (en) | 2009-02-10 | 2009-02-10 | Zinc oxide doping method using a dual dopant |
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| Publication Number | Publication Date |
|---|---|
| KR20100091277A true KR20100091277A (en) | 2010-08-19 |
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| KR1020090010393A KR20100091277A (en) | 2009-02-10 | 2009-02-10 | Zinc oxide doping method using a dual dopant |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2015023137A1 (en) * | 2013-08-14 | 2015-02-19 | 코닝정밀소재 주식회사 | Deposition method for zinc oxide-based thin film |
-
2009
- 2009-02-10 KR KR1020090010393A patent/KR20100091277A/en not_active Application Discontinuation
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2015023137A1 (en) * | 2013-08-14 | 2015-02-19 | 코닝정밀소재 주식회사 | Deposition method for zinc oxide-based thin film |
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