JP3776606B2 - Method for producing transparent electrode substrate - Google Patents

Method for producing transparent electrode substrate Download PDF

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Publication number
JP3776606B2
JP3776606B2 JP31622398A JP31622398A JP3776606B2 JP 3776606 B2 JP3776606 B2 JP 3776606B2 JP 31622398 A JP31622398 A JP 31622398A JP 31622398 A JP31622398 A JP 31622398A JP 3776606 B2 JP3776606 B2 JP 3776606B2
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Prior art keywords
film
electrode substrate
transparent electrode
aluminum
conductive film
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JP2000150928A (en
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武志 山本
総一 酒井
伸 松見
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Sanyo Electric Co Ltd
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Sanyo Electric Co Ltd
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    • 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
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Description

【０００１】
【発明の属する技術分野】
本発明は、透光性基板に透明導電性膜を形成して構成される透明電極基板及びその作製方法、並びに、そのような透明電極基板を用いる光起電力素子に関する。
【０００２】
【従来の技術】
基板側から光を入射させて電気エネルギを取り出す構成の光起電力素子では、ガラス板等の透光性基板上に透明導電性膜を光入射側電極として積層してなる透明電極基板が利用される。この透明導電性膜の材料としては、酸化亜鉛（ＺｎＯ），酸化インジウム錫（ＩＴＯ），酸化錫（ＳｎＯ2 ）が一般的であり、これ以外に、高光透過率及び低抵抗率を実現するべく、酸化アルミニウム（Ａｌ2 Ｏ3 ）を含む酸化亜鉛（特開平５−２７５７２７号公報）も知られている。
【０００３】
そして、この透明電極基板の作製には、量産性に優れていて低コストである点を考慮して、一般的にスパッタリング法が検討されている。即ち、透光性基板を陽極とし、上記のような透明導電性膜の材料（ターゲット）を陰極として、１０-2Ｔｏｒｒ程度の不活性ガス（例えばＡｒガス）中で陰極に負の高周波電圧を印加することによってグロー放電を行い、放電で生じたイオン（例えばＡｒ+ ）をターゲットに当てて、その際に起こるスパッタリング作用を利用して透光性基板上にその材料を成膜して透明導電性膜を形成する。
【０００４】
ところで、光起電力素子にあっては、光入射側電極（透明導電性膜）の表面が凹凸化している構造（テクスチャ構造）を有していると大きな電流を出力できることが知られている。即ち、透光性基板側から入射してきた光が凹凸形状を有する光入射側電極（透明導電性膜）と光電変換層との界面で散乱された後に光電変換層に入射するので、光電変換層に斜めに光が入射して光路の実質的な距離が延びて光の吸収が増大し、この結果、光起電力素子の光電変換特性が向上して出力電流が増加する。
【０００５】
【発明が解決しようとする課題】
スパッタリング法を用いて透光性基板上に透明導電性膜を形成する方法は、処理工程が簡便であるが、光起電力素子の光入射側電極に期待されるような凹凸形状（テクスチャ構造）を実現することはできない。よって、スパッタリング法を用いて光入射側電極（透明導電性膜）を形成した光起電力素子の光電変換特性の向上が妨げられているという問題がある。
【０００６】
本発明は斯かる事情に鑑みてなされたものであり、スパッタリング法を用いて透明導電性膜を作製する場合にあっても、その表面を凹凸形状にできる透明電極基板及びその作製方法を提供することを目的とする。
【０００７】
本発明の他の目的は、スパッタリング法を用いて光入射側電極を形成する場合において、その光電変換特性の向上を図れる光起電力素子を提供することにある。
【００１４】
【課題を解決するための手段】
本発明に係る透明電極基板の作製方法は、スパッタリング法にて透明導電性膜を透光性基板に形成してなる透明電極基板を作製する方法において、前記透光性基板にアルミニウム膜を形成する工程と、形成したアルミニウム膜をエッチングして凹凸化する工程と、アルミニウム膜をアルミニウム化合物膜に変化させる工程と、アルミニウム化合物膜にスパッタリング法にて透明導電性膜を形成する工程とを有することを特徴とする。
【００１５】
エッチング処理により凹凸化されたアルミニウム化合物膜上にスパッタリング法にて透明導電性膜を形成することにより、スパッタリング法を用いても、アルミニウム化合物膜の凹凸形状に応じて透明導電性膜が凹凸化する。
【００１６】
【発明の実施の形態】
以下、本発明をその実施の形態を示す図面を参照して具体的に説明する。
【００１７】
図１は、本発明の透明電極基板の構成図である。図１において、１はガラス製の透光性基板である。透光性基板１上には、表面が凹凸形状をなす酸化アルミニウム（Ａｌ2 Ｏ3 ）または窒化アルミニウム（ＡｌＮ）からなるアルミニウム化合物膜２（厚さ：１０００Å）が形成され、その上には、表面が凹凸形状をなす、即ち表面にテクスチャ構造を有する酸化亜鉛（ＺｎＯ）または酸化錫（ＳｎＯ2 ）からなる透明導電性膜３（厚さ：６０００Å）が形成されている。
【００１８】
次に、このような構成を有する本発明の透明電極基板の作製手順を、その工程を示す図２を参照して説明する。まず、ガラス製の透光性基板１上に、スパッタリング法にて、厚さ１０００Åのアルミニウム（Ａｌ）膜２１を形成する（図２（ａ））。次に、塩酸：水＝１：１のエッチャントを用いてアルミニウム膜２１を部分的にエッチング除去してその表面を凹凸化する（図２（ｂ））。
【００１９】
次に、大気中または窒素雰囲気中で５０℃で加熱して、アルミニウム膜２１を酸化または窒化させて、結晶化された酸化アルミニウムまたは窒化アルミニウムのアルミニウム化合物膜２を形成する（図２（ｃ））。最後に、スパッタリング法にて、酸化亜鉛または酸化錫を厚さ６０００Åだけ成膜して、透明導電性膜３を形成する（図２（ｄ））。この際、下地となるアルミニウム化合物膜２の表面が凹凸形状をなすので、その上に形成される透明導電性膜３も凹凸化し、テクスチャ構造を有することになる。
【００２０】
ところで、スパッタリング法にて透光性基板１上に直接形成した酸化亜鉛または酸化錫の透明導電性膜を直接エッチングしてその表面を凹凸化するような手法も考えられるが、酸化亜鉛または酸化錫のエッチング加工は容易でないという問題がある。これに対して、アルミニウムは、これらの酸化亜鉛または酸化錫と比較してエッチング加工が容易であるので、本発明は簡単にテクスチャ構造の透明導電性膜を持った透明電極基板を作製できる。
【００２１】
図３は、上述したような透明電極基板を用いた本発明の光起電力素子の構成図である。図３において、１，２，３は、図１と同様のガラス製の透光性基板，アルミニウム化合物膜，透明導電性膜（光入射側電極）である。透明導電性膜３上には、ｐ型非晶質シリコン層４（厚さ：２００Å）、ｉ型非晶質シリコン層５（厚さ：７５０Å）、ｎ型微結晶シリコン層６（厚さ：２５０Å）、ｐ型非晶質シリコン層７（厚さ：２００Å）、ｉ型非晶質シリコン層８（厚さ：３０００Å）、ｎ型非晶質シリコン層９（厚さ：３００Å）、ＺｎＯまたはＩＴＯからなる拡散防止層１０（厚さ：１０００Å）、Ａｇからなる裏面電極膜１１（厚さ：２０００Å）がこの順に積層形成されている。
【００２２】
このようなアルミニウム化合物膜２は透光性を有するので、透光性基板１と透明導電性膜３との間のアルミニウム化合物膜２の存在が光電変換特性に悪影響を及ぼすことはなく、例えば酸化アルミニウムの屈折率（１．６２）が、ガラスの屈折率（１．５）とＺｎＯまたはＩＴＯの屈折率（２．０）との間であるので、このアルミニウム化合物膜２の存在によって反射防止効果が得られる。
【００２３】
このような構成の光起電力素子は、以下のようにして製造できる。まず、上述したような工程（図２参照）にて透明電極基板を作製し、その透明電極基板上に、プラズマＣＶＤ法にて各シリコン層４〜９を順次形成し、その上に、スパッタリング法にて、拡散防止層１０，裏面電極膜１１を形成する。
【００２４】
次に、本発明による透明電極基板及び光起電力素子の特性について説明する。
（実施例１）
図１，図３におけるアルミニウム化合物膜２として酸化アルミニウムを用いた透明電極基板，光起電力素子を製造し、夫々の特性を測定した。また、比較例として、酸化アルミニウムからなるアルミニウム化合物膜を設けない透明電極基板，光起電力素子を製造し、夫々の特性も測定した。これらの測定結果を表１（透明電極基板の特性），表２（１ｃｍセルの光起電力素子の特性）に示す。
【００２５】
【表１】

Figure 0003776606
【００２６】
【表２】
Figure 0003776606
【００２７】
比較例の透明電極基板にあっては、透明導電性膜の表面が平坦であって充分なヘイズ率が得られていない。これに対して、表面が凹凸のアルミニウム化合物膜（酸化アルミニウム膜）を設けた本発明の透明電極基板では、透明導電性膜の表面が凹凸化して充分なヘイズ率を達成できている。この結果、これを用いる本発明の光起電力素子では、特に短絡電流（ＩSC）及び最大起電力Ｐmax が大幅に向上している。
【００２８】
（実施例２）
図１，図３におけるアルミニウム化合物膜２として窒化アルミニウムを用いた透明電極基板，光起電力素子を製造し、夫々の特性を測定した。また、比較例として、窒化アルミニウムからなるアルミニウム化合物膜を設けない透明電極基板，光起電力素子を製造し、夫々の特性も測定した。これらの測定結果を表３（透明電極基板の特性），表４（１ｃｍセルの光起電力素子の特性）に示す。
【００２９】
【表３】
Figure 0003776606
【００３０】
【表４】
Figure 0003776606
【００３１】
比較例の透明電極基板にあっては、透明導電性膜の表面が平坦であって充分なヘイズ率が得られていない。これに対して、表面が凹凸のアルミニウム化合物膜（窒化アルミニウム膜）を設けた本発明の透明電極基板では、透明導電性膜の表面が凹凸化して充分なヘイズ率を達成できている。この結果、これを用いる本発明の光起電力素子では、特に短絡電流（ＩSC）及び最大起電力（Ｐmax ）が大幅に向上している。
【００３２】
なお、上述した例では、アルミニウム膜を形成し、それをエッチングした後に酸化または窒化するようにしたが、酸化アルミニウムの粉末を使用することも可能である。この場合には、酸化アルミニウムの粉末を溶媒に溶かしたペーストを透光性基板上に塗布し、その塗布した膜にエッチング処理を施して表面を凹凸化すれば、全く同様に、テクスチャ構造を有する透明導電性膜を形成することができる。
【００３３】
【発明の効果】
以上のように本発明では、スパッタリング法によって透明導電性膜を形成する場合にあっても、表面が凹凸形状をなす透明導電性膜を有する透明電極基板を得ることができ、高いヘイズ率を持つ透明電極基板を提供できる。
【００３４】
また、このような透明電極基板を用いるようにしたので、光の有効利用を図って優れた光電変換特性を持つ光電変換素子を提供できる。
【図面の簡単な説明】
【図１】本発明の透明電極基板の構成図である。
【図２】本発明の透明電極基板の作製方法の工程を示す図である。
【図３】本発明の光起電力素子の構成図である。
【符号の説明】
１ 透光性基板
２ アルミニウム化合物膜
３ 透明導電性膜
２１ アルミニウム膜[0001]
BACKGROUND OF THE INVENTION
The present invention relates to a transparent electrode substrate formed by forming a transparent conductive film on a translucent substrate, a method for manufacturing the same, and a photovoltaic device using such a transparent electrode substrate.
[0002]
[Prior art]
In a photovoltaic device having a configuration in which light is incident from the substrate side and electric energy is extracted, a transparent electrode substrate in which a transparent conductive film is laminated as a light incident side electrode on a translucent substrate such as a glass plate is used. The As a material of the transparent conductive film, zinc oxide (ZnO), indium tin oxide (ITO), and tin oxide (SnO 2 ) are generally used. In addition to this, in order to realize high light transmittance and low resistivity. In addition, zinc oxide containing aluminum oxide (Al 2 O 3 ) (Japanese Patent Laid-Open No. 5-275727) is also known.
[0003]
For the production of this transparent electrode substrate, a sputtering method is generally studied in view of its excellent mass productivity and low cost. That is, a negative high frequency voltage is applied to the cathode in an inert gas (for example, Ar gas) of about 10 −2 Torr using the light-transmitting substrate as the anode, the transparent conductive film material (target) as described above as the cathode. Applying a glow discharge, applying ions (for example, Ar + ) generated by the discharge to the target, and depositing the material on the translucent substrate by utilizing the sputtering action that occurs at that time, transparent conductive Forming a conductive film.
[0004]
Incidentally, it is known that a photovoltaic device can output a large current if it has a structure (texture structure) in which the surface of the light incident side electrode (transparent conductive film) is uneven. That is, the light incident from the translucent substrate side is scattered at the interface between the light incident side electrode (transparent conductive film) having a concavo-convex shape and the photoelectric conversion layer and then enters the photoelectric conversion layer. The light is incident obliquely and the substantial distance of the optical path is extended to increase the light absorption. As a result, the photoelectric conversion characteristics of the photovoltaic element are improved and the output current is increased.
[0005]
[Problems to be solved by the invention]
The method of forming a transparent conductive film on a light-transmitting substrate using a sputtering method has a simple processing step, but has an uneven shape (texture structure) that is expected for a light incident side electrode of a photovoltaic device. Cannot be realized. Therefore, there exists a problem that the improvement of the photoelectric conversion characteristic of the photovoltaic element which formed the light-incidence side electrode (transparent conductive film) using sputtering method is prevented.
[0006]
The present invention has been made in view of such circumstances, and provides a transparent electrode substrate whose surface can be formed into an uneven shape even when a transparent conductive film is produced using a sputtering method and a method for producing the same. For the purpose.
[0007]
Another object of the present invention is to provide a photovoltaic device capable of improving the photoelectric conversion characteristics when a light incident side electrode is formed by sputtering.
[0014]
[Means for Solving the Problems]
The method for producing a transparent electrode substrate according to the present invention is a method for producing a transparent electrode substrate in which a transparent conductive film is formed on a translucent substrate by a sputtering method, wherein an aluminum film is formed on the translucent substrate. A step of etching the formed aluminum film to make it uneven, a step of changing the aluminum film into an aluminum compound film, and a step of forming a transparent conductive film on the aluminum compound film by a sputtering method. Features.
[0015]
By forming a transparent conductive film on the aluminum compound film that has been roughened by the etching process by a sputtering method, the transparent conductive film becomes uneven depending on the uneven shape of the aluminum compound film even if the sputtering method is used. .
[0016]
DETAILED DESCRIPTION OF THE INVENTION
Hereinafter, the present invention will be described in detail with reference to the drawings showing embodiments thereof.
[0017]
FIG. 1 is a configuration diagram of a transparent electrode substrate of the present invention. In FIG. 1, 1 is a glass transparent substrate. On the translucent substrate 1, an aluminum compound film 2 (thickness: 1000 mm) made of aluminum oxide (Al 2 O 3 ) or aluminum nitride (AlN) having an uneven surface is formed. A transparent conductive film 3 (thickness: 6000 mm) made of zinc oxide (ZnO) or tin oxide (SnO 2 ) having an uneven surface, that is, having a textured structure on the surface is formed.
[0018]
Next, a manufacturing procedure of the transparent electrode substrate of the present invention having such a configuration will be described with reference to FIG. First, an aluminum (Al) film 21 having a thickness of 1000 mm is formed on a glass transparent substrate 1 by a sputtering method (FIG. 2A). Next, the aluminum film 21 is partially removed by etching using an etchant of hydrochloric acid: water = 1: 1 to make the surface uneven (FIG. 2B).
[0019]
Next, the aluminum film 21 is oxidized or nitrided by heating at 50 ° C. in air or nitrogen atmosphere to form the crystallized aluminum oxide or aluminum nitride aluminum compound film 2 (FIG. 2C). ). Finally, a transparent conductive film 3 is formed by sputtering to form a zinc oxide or tin oxide film having a thickness of 6000 mm (FIG. 2D). At this time, since the surface of the aluminum compound film 2 serving as a base has an uneven shape, the transparent conductive film 3 formed thereon is also uneven and has a texture structure.
[0020]
By the way, a method of directly etching a transparent conductive film of zinc oxide or tin oxide formed directly on the light-transmitting substrate 1 by a sputtering method to make the surface uneven may be considered. There is a problem that the etching process is not easy. On the other hand, aluminum is easier to etch than these zinc oxides or tin oxides. Therefore, the present invention can easily produce a transparent electrode substrate having a textured transparent conductive film.
[0021]
FIG. 3 is a configuration diagram of the photovoltaic element of the present invention using the transparent electrode substrate as described above. In FIG. 3, 1, 2 and 3 are the same glass transparent substrate, aluminum compound film, and transparent conductive film (light incident side electrode) as in FIG. On the transparent conductive film 3, a p-type amorphous silicon layer 4 (thickness: 200 mm), an i-type amorphous silicon layer 5 (thickness: 750 mm), and an n-type microcrystalline silicon layer 6 (thickness: 250 mm), p-type amorphous silicon layer 7 (thickness: 200 mm), i-type amorphous silicon layer 8 (thickness: 3000 mm), n-type amorphous silicon layer 9 (thickness: 300 mm), ZnO or A diffusion preventing layer 10 (thickness: 1000 mm) made of ITO and a back electrode film 11 (thickness: 2000 mm) made of Ag are laminated in this order.
[0022]
Since such an aluminum compound film 2 has translucency, the presence of the aluminum compound film 2 between the translucent substrate 1 and the transparent conductive film 3 does not adversely affect the photoelectric conversion characteristics. Since the refractive index of aluminum (1.62) is between the refractive index of glass (1.5) and the refractive index of ZnO or ITO (2.0), the presence of the aluminum compound film 2 prevents the reflection. Is obtained.
[0023]
The photovoltaic device having such a configuration can be manufactured as follows. First, a transparent electrode substrate is produced by the process as described above (see FIG. 2), and silicon layers 4 to 9 are sequentially formed on the transparent electrode substrate by a plasma CVD method, and a sputtering method is formed thereon. Then, the diffusion prevention layer 10 and the back electrode film 11 are formed.
[0024]
Next, characteristics of the transparent electrode substrate and the photovoltaic element according to the present invention will be described.
Example 1
A transparent electrode substrate and a photovoltaic device using aluminum oxide as the aluminum compound film 2 in FIGS. 1 and 3 were manufactured, and their characteristics were measured. In addition, as a comparative example, a transparent electrode substrate and a photovoltaic element not provided with an aluminum compound film made of aluminum oxide were manufactured, and their characteristics were also measured. These measurement results are shown in Table 1 (characteristics of the transparent electrode substrate) and Table 2 (characteristics of the photovoltaic element of 1 cm cell).
[0025]
[Table 1]
Figure 0003776606
[0026]
[Table 2]
Figure 0003776606
[0027]
In the transparent electrode substrate of the comparative example, the surface of the transparent conductive film is flat and a sufficient haze ratio is not obtained. On the other hand, in the transparent electrode substrate of the present invention provided with an aluminum compound film (aluminum oxide film) having an uneven surface, the surface of the transparent conductive film is made uneven to achieve a sufficient haze ratio. As a result, in the photovoltaic element of the present invention using this, particularly the short circuit current (I SC ) and the maximum electromotive force P max are greatly improved.
[0028]
(Example 2)
A transparent electrode substrate and a photovoltaic device using aluminum nitride as the aluminum compound film 2 in FIGS. 1 and 3 were manufactured, and their characteristics were measured. In addition, as a comparative example, a transparent electrode substrate and a photovoltaic element without an aluminum compound film made of aluminum nitride were manufactured, and their characteristics were also measured. The measurement results are shown in Table 3 (characteristics of the transparent electrode substrate) and Table 4 (characteristics of 1 cm cell photovoltaic elements).
[0029]
[Table 3]
Figure 0003776606
[0030]
[Table 4]
Figure 0003776606
[0031]
In the transparent electrode substrate of the comparative example, the surface of the transparent conductive film is flat and a sufficient haze ratio is not obtained. On the other hand, in the transparent electrode substrate of the present invention provided with an aluminum compound film (aluminum nitride film) having an uneven surface, the surface of the transparent conductive film is uneven and a sufficient haze ratio can be achieved. As a result, the short-circuit current (I SC ) and the maximum electromotive force (P max ) are greatly improved particularly in the photovoltaic device of the present invention using this.
[0032]
In the above-described example, an aluminum film is formed and then oxidized or nitrided after being etched, but aluminum oxide powder can also be used. In this case, if a paste in which aluminum oxide powder is dissolved in a solvent is applied on a light-transmitting substrate and the coated film is etched to make the surface uneven, the texture structure is exactly the same. A transparent conductive film can be formed.
[0033]
【The invention's effect】
As described above, in the present invention, even when a transparent conductive film is formed by a sputtering method, a transparent electrode substrate having a transparent conductive film having an uneven surface can be obtained and has a high haze ratio. A transparent electrode substrate can be provided.
[0034]
In addition, since such a transparent electrode substrate is used, it is possible to provide a photoelectric conversion element having excellent photoelectric conversion characteristics by effectively using light.
[Brief description of the drawings]
FIG. 1 is a configuration diagram of a transparent electrode substrate of the present invention.
FIG. 2 is a diagram showing a process of a method for producing a transparent electrode substrate according to the present invention.
FIG. 3 is a configuration diagram of a photovoltaic element of the present invention.
[Explanation of symbols]
DESCRIPTION OF SYMBOLS 1 Translucent substrate 2 Aluminum compound film 3 Transparent conductive film 21 Aluminum film

Claims (1)

スパッタリング法にて透明導電性膜を透光性基板に形成してなる透明電極基板を作製する方法において、前記透光性基板にアルミニウム膜を形成する工程と、形成したアルミニウム膜をエッチングして凹凸化する工程と、アルミニウム膜をアルミニウム化合物膜に変化させる工程と、アルミニウム化合物膜にスパッタリング法にて透明導電性膜を形成する工程とを有することを特徴とする透明電極基板の作製方法。  In a method for producing a transparent electrode substrate formed by forming a transparent conductive film on a light-transmitting substrate by a sputtering method, a step of forming an aluminum film on the light-transmitting substrate, and etching the formed aluminum film A method for producing a transparent electrode substrate, comprising: a step of converting the aluminum film into an aluminum compound film; and a step of forming a transparent conductive film on the aluminum compound film by a sputtering method.
JP31622398A 1998-11-06 1998-11-06 Method for producing transparent electrode substrate Expired - Fee Related JP3776606B2 (en)

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JP2002222975A (en) * 2001-01-29 2002-08-09 Kyocera Corp THIN FILM CRYSTALLINE Si SOLAR BATTERY AND ITS MANUFACTURING METHOD
JP4959127B2 (en) * 2004-10-29 2012-06-20 三菱重工業株式会社 Photoelectric conversion device and substrate for photoelectric conversion device
JP4634129B2 (en) 2004-12-10 2011-02-16 三菱重工業株式会社 Light scattering film and optical device using the same
FR2915834B1 (en) * 2007-05-04 2009-12-18 Saint Gobain TRANSPARENT SUBSTRATE WITH IMPROVED ELECTRODE LAYER
US20090173373A1 (en) * 2008-01-07 2009-07-09 Wladyslaw Walukiewicz Group III-Nitride Solar Cell with Graded Compositions
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