JPH1129743A - Coating solution for formation of silica-based film, its preparation and silica-based film - Google Patents
Coating solution for formation of silica-based film, its preparation and silica-based filmInfo
- Publication number
- JPH1129743A JPH1129743A JP18375497A JP18375497A JPH1129743A JP H1129743 A JPH1129743 A JP H1129743A JP 18375497 A JP18375497 A JP 18375497A JP 18375497 A JP18375497 A JP 18375497A JP H1129743 A JPH1129743 A JP H1129743A
- Authority
- JP
- Japan
- Prior art keywords
- silica
- based film
- film
- coating solution
- coating
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
Landscapes
- Paints Or Removers (AREA)
- Silicon Polymers (AREA)
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、シリカ系被膜形成
用塗布液、その製造法及びシリカ系被膜に関し、更に詳
しくは熱的に安定でかつ成膜性の良好なシリカ系被膜を
調整することができるシリカ系被膜形成用塗布液、その
製造法及びシリカ系被膜に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a coating solution for forming a silica-based film, a method for producing the same, and a silica-based film, and more particularly, to preparing a silica-based film which is thermally stable and has good film-forming properties. The present invention relates to a coating solution for forming a silica-based film, a method for producing the same, and a silica-based film.
【０００２】[0002]
【従来の技術】従来、ＩＣ、ＬＳＩ等の半導体素子の層
間絶縁膜の平坦化方法として、パターン形成された配線
層を有する基盤上に真空蒸着、ＣＶＤ等の気相成長法に
よりＳｉＯ2、ＳｉＮ等からなる１層目の層間絶縁膜を
形成し、２層目にＳＯＧ液（オルガノシロキサンのオリ
ゴマー液）を回転塗布し、その後熱処理することにより
オルガノシロキサン系被膜を形成する。次に１層目と同
様の方法により３層目の層間絶縁膜を形成する３層層間
膜によるＳＯＧ平坦化プロセスが広く用いられている。2. Description of the Related Art Conventionally, as a method of flattening an interlayer insulating film of a semiconductor element such as an IC or an LSI, SiO 2 , SiN is formed on a substrate having a patterned wiring layer by a vapor deposition method such as a vacuum deposition or a CVD. The first layer of an interlayer insulating film is formed, and the second layer is spin-coated with an SOG solution (organosiloxane oligomer solution), followed by heat treatment to form an organosiloxane-based film. Next, an SOG planarization process using a three-layer interlayer film in which a third interlayer insulating film is formed in the same manner as the first layer is widely used.
【０００３】近年、益々、配線の多層化の要求が高ま
り、また、微細配線加工プロセスでのフォーカスマージ
ン向上の要求から従来のシリカ系被膜形成用塗布液を用
いた平坦化技術に替わるより広域平坦化に優れた新たな
平坦化技術が不可欠となってきた。この要求に応えるた
め、近年、ＣＶＤ等の気相成長法により形成したＳｉＯ
2のＣＭＰ法による平坦化が提唱されている。しかし、
スループットの向上、コストの低減、研磨後の洗浄技術
の確立などの問題がある。In recent years, there has been an increasing demand for multilayer wiring, and a demand for an improvement in a focus margin in a fine wiring processing process has led to a flattening technique that can replace a conventional flattening technique using a silica-based coating liquid. A new flattening technology that is excellent in lithography has become indispensable. In order to meet this demand, in recent years, SiO formed by a vapor phase growth method such as CVD has been used.
Planarization by the CMP method 2 has been proposed. But,
There are problems such as improvement in throughput, reduction in cost, and establishment of a cleaning technique after polishing.
【０００４】現在、これらの問題を解決するため、シロ
キサンオリゴマー（ＳＯＧ）を基板上に回転塗布したあ
と、硬化し、その後ＣＭＰ法を用いて平坦化することに
よりスループットを向上させることができ、また、コス
トの低減が可能であると考えられている。しかし、ＳＯ
Ｇから作製された被膜をＣＭＰ法により平坦化させるた
めには、例えば、配線段差に対してシリカ系被膜の膜厚
を同様かそれ以上形成しないと、研磨後の平坦性が不十
分であり、配線段差が１μｍ以上の場合は、シリカ系被
膜形成用塗布液に厚膜成膜性が要求される。シリカ系被
膜を１μｍ以上形成するためには、塗布回転数の制御だ
けでなくシリカ系被膜形成用塗布液の樹脂分濃度を上げ
なくては、厚膜成膜性、塗布性の良好な被膜が形成され
にくい。ところが、樹脂分濃度を高濃度にするとシリカ
系被膜形成用塗布液の保存安定性が低下するという問題
がある。At present, in order to solve these problems, a siloxane oligomer (SOG) is spin-coated on a substrate, cured, and then flattened by a CMP method to improve throughput. It is considered that the cost can be reduced. However, SO
In order to flatten the film formed from G by the CMP method, for example, the flatness after polishing is insufficient unless the thickness of the silica-based film is equal to or greater than the wiring step. When the wiring step is 1 μm or more, the coating liquid for forming a silica-based film is required to have a thick film forming property. In order to form a silica-based coating of 1 μm or more, it is necessary to not only control the number of coating revolutions but also increase the resin component concentration of the coating liquid for forming a silica-based coating. Hard to form. However, when the concentration of the resin component is increased, there is a problem that the storage stability of the coating solution for forming a silica-based film decreases.
【０００５】[0005]
【発明が解決しようとする課題】請求項１又は２に記載
の発明は、保存安定性、厚膜成膜性に優れ、耐クラック
性に優れる被膜を形成することができるシリカ系被膜形
成用塗布液を提供するものである。請求項３又は４に記
載の発明は、保存安定性、厚膜成膜性に優れ、耐クラッ
ク性に優れる被膜を形成することができるシリカ系被膜
形成用塗布液の製造法を提供するものである。請求項５
に記載の発明は、耐クラック性に優れ成膜性の良好なシ
リカ系被膜を提供するものである。According to the first or second aspect of the present invention, there is provided a coating for forming a silica-based film capable of forming a film having excellent storage stability, excellent film-forming properties, and excellent crack resistance. A liquid is provided. The invention according to claim 3 or 4 provides a method for producing a coating solution for forming a silica-based film, which is capable of forming a film having excellent storage stability, excellent film-forming properties, and excellent crack resistance. is there. Claim 5
The invention described in (1) provides a silica-based film having excellent crack resistance and good film-forming properties.
【０００６】[0006]
【課題を解決するための手段】本発明は、（Ａ）一般式
（Ｉ）According to the present invention, there is provided (A) a compound represented by the following general formula (I):
【化３】 （式中Ｒは、炭素数１〜４のアルキル基、ｎは０〜２の
整数を意味し、複数個のＲは同一でも異なっていてもよ
い）で表されるアルコキシシラン化合物を加水分解、重
縮合させて得られるシロキサンポリマー並びにアンモニ
ア、アルキルアミン、ジアルキルアミン、トリアルキル
アミン及びアリールアミンからなる群から選ばれる少な
くとも一種の塩基性化合物を含有してなるシリカ系被膜
形成用塗布液に関する。また、本発明は、塩基性化合物
をpHが５〜７になるように含む前記シリカ系被膜形成用
塗布液に関する。Embedded image (Wherein R is an alkyl group having 1 to 4 carbon atoms, n is an integer of 0 to 2, and a plurality of Rs may be the same or different), The present invention relates to a coating solution for forming a silica-based film, comprising a siloxane polymer obtained by polycondensation and at least one basic compound selected from the group consisting of ammonia, alkylamine, dialkylamine, trialkylamine and arylamine. In addition, the present invention relates to the coating solution for forming a silica-based film, which contains a basic compound so as to have a pH of 5 to 7.
【０００７】また、本発明は、（Ａ）一般式（Ｉ）The present invention also relates to (A) a compound represented by the general formula (I):
【化４】 （式中Ｒは、炭素数１〜４のアルキル基、ｎは０〜２の
整数を意味し、複数個のＲは同一でも異なっていてもよ
い）で表されるアルコキシシラン化合物を加水分解、重
縮合させて得られるシロキサンポリマーを製造するに際
して、アンモニア、アルキルアミン、ジアルキルアミ
ン、トリアルキルアミン及びアリールアミンからなる群
から選ばれる少なくとも一種の塩基性化合物を存在させ
ることを特徴とするシリカ系被膜形成用塗布液の製造法
に関する。また、本発明は、塩基性化合物をpHが５〜７
になるように存在させる前記シリカ系被膜形成用塗布液
の製造法に関する。また、本発明は、前記シリカ系被膜
形成用塗布液を用いて形成されてなるシリカ系被膜に関
する。Embedded image (Wherein R is an alkyl group having 1 to 4 carbon atoms, n is an integer of 0 to 2, and a plurality of Rs may be the same or different), A step of producing a siloxane polymer obtained by polycondensation, wherein at least one basic compound selected from the group consisting of ammonia, alkylamine, dialkylamine, trialkylamine and arylamine is present; The present invention relates to a method for producing a coating liquid for formation. Further, the present invention provides a method for preparing a basic compound having a pH of 5 to 7;
The present invention relates to a method for producing the coating solution for forming a silica-based film, which is present in such a manner as to be present. The present invention also relates to a silica-based coating formed using the silica-based coating liquid.
【０００８】[0008]
【発明の実施の形態】前記一般式（Ｉ）で表されるアル
コキシシラン化合物は、具体的にはBEST MODE FOR CARRYING OUT THE INVENTION The alkoxysilane compound represented by the general formula (I) is specifically described below.
【化５】 等のテトラアルコキシシラン、Embedded image Such as tetraalkoxysilane,
【化６】 等のモノアルキルトリアルコキシシラン、Embedded image Monoalkyl trialkoxysilane such as,
【化７】 等のジアルキルジアルコキシシランがあげられ、これら
は１種または２種以上が用いられる。Embedded image And the like, and one or more of these may be used.
【０００９】本発明に用いられる前記一般式（Ｉ）で表
されるアルコキシシランオリゴマーとしてはテトラアル
コキシシラン、モノアルキルトリアルコキシシラン、ジ
アルキルジアルコキシシランの割合に制限はないが、良
質なシリカ系被膜を形成するためにジアルキルジアルコ
キシシランは使用するアルコキシシラン化合物の総量に
対し５０モル％以下であることが好ましい。The alkoxysilane oligomer represented by the general formula (I) used in the present invention is not limited in the proportion of tetraalkoxysilane, monoalkyltrialkoxysilane and dialkyldialkoxysilane, but it has good silica coating. The dialkyldialkoxysilane is preferably used in an amount of 50 mol% or less based on the total amount of the alkoxysilane compound to be used.
【００１０】本発明におけるシリカ系被膜形成用塗布液
には溶媒として、有機溶媒を使用することが好ましい。
有機溶媒としては、メタノール、エタノール、プロパノ
ール、ブタノール等のアルコール系、酢酸メチル、酢酸
エチル、酢酸プロピル、酢酸ブチル等の酢酸エステル
系、エチレングリコールモノメチルアセテート、エチレ
ングリコールジアセテート等のグリコールアセテート系
溶媒、Ｎ，Ｎ−メチル−２ピロリドン等のアミド系溶
媒、グリコールエーテル系溶媒等種々の溶媒があげら
れ、これらは１種または２種以上が用いられる。溶媒
は、上記の反応で得られるシロキサンポリマー樹脂の量
が１５〜５０重量％となるような量で使用されることが
好ましい。In the present invention, an organic solvent is preferably used as a solvent in the coating solution for forming a silica-based film.
Examples of the organic solvent include alcohols such as methanol, ethanol, propanol and butanol; acetates such as methyl acetate, ethyl acetate, propyl acetate and butyl acetate; glycol acetate solvents such as ethylene glycol monomethyl acetate and ethylene glycol diacetate; Various solvents such as amide solvents such as N, N-methyl-2-pyrrolidone and glycol ether solvents are used, and one or more of these solvents are used. The solvent is preferably used in an amount such that the amount of the siloxane polymer resin obtained by the above reaction is 15 to 50% by weight.
【００１１】本発明におけるシロキサンポリマーは、前
記した一般式（Ｉ）で表されるアルコキシシラン化合物
を加水分解、重縮合して製造されるが、このとき、触媒
としては、塩酸、硫酸、リン酸、硝酸、フッ酸等の無機
酸、シュウ酸、マレイン酸、スルホン酸、ギ酸等の有機
酸を使用することが好ましく、アンモニア、トリメチル
アンモニウムなどの塩基性触媒を用いることもできる。
これら触媒は、一般式（Ｉ）で表されるアルコキシシラ
ン化合物の量に応じて適当量用いられるが、好適には一
般式（Ｉ）で表されるアルコキシシラン化合物１モルに
対し０．００１〜０．５モルの範囲で用いられる。The siloxane polymer of the present invention is produced by hydrolyzing and polycondensing the alkoxysilane compound represented by the above general formula (I). At this time, as a catalyst, hydrochloric acid, sulfuric acid, phosphoric acid It is preferable to use inorganic acids such as nitric acid and hydrofluoric acid, and organic acids such as oxalic acid, maleic acid, sulfonic acid and formic acid, and basic catalysts such as ammonia and trimethylammonium.
These catalysts are used in an appropriate amount in accordance with the amount of the alkoxysilane compound represented by the general formula (I), and preferably from 0.001 to 1 mol per mol of the alkoxysilane compound represented by the general formula (I). It is used in a range of 0.5 mol.
【００１２】また、上記の加水分解・重縮合は、前記の
溶媒中で行うことが好ましい。また、この反応に際し
て、水が存在させられる。水の量も適宜決められるが、
余り少ない場合や多すぎる場合には塗布液の保存安定性
が低下するなどの問題があるので、水の量は、一般式
（Ｉ）で表されるアルコキシシラン化合物１モルに対し
て０．５〜４モルの範囲とすることが好ましい。以上の
ようにして得られる加水分解・重縮合生成物の反応液
（シロキサンポリマー液）は、シリカ系被膜形成用塗布
液としてそのまま使用することができる。また、溶媒を
除去後、改めて前記溶媒に溶解してシリカ系被膜形成用
塗布液（シロキサンポリマー液）としてから使用され
る。The above-mentioned hydrolysis / polycondensation is preferably carried out in the above-mentioned solvent. In this reaction, water is present. The amount of water is determined as appropriate,
If the amount is too small or too large, there is a problem that the storage stability of the coating solution is lowered. Therefore, the amount of water is 0.5 It is preferably in the range of 4 to 4 mol. The reaction solution (siloxane polymer solution) of the hydrolysis / polycondensation product obtained as described above can be used as it is as a coating solution for forming a silica-based film. After the solvent is removed, it is again dissolved in the solvent and used as a silica-based coating liquid (siloxane polymer liquid).
【００１３】本発明に使用される塩基性化合物として
は、アンモニア（アンモニア水として使用してもよ
い）、オクチルアミン、Ｎ，Ｎ−ジメチルベンジルアミ
ン等のフェニル基等の芳香族基で置換されていてもよい
アルキル基（置換基を除いて炭素数１〜９であることが
好ましい）を有するアルキルアミン、ジアルキルアミン
若しくはトリアルキルアミン並びにアニリン等のアリー
ルアミン（芳香族基を有するアミン化合物）がある。塩
基性化合物は得られたシロキサンポリマー液の安定化に
必要である。上記塩基性化合物がない場合、安定性が損
なわれ、ゲル化しやすくなる。上記塩基性化合物は、シ
ロキサンポリマー液のpHを５〜７とするように使用され
ることが好ましく、特にpHが５〜６となるように使用さ
れることが好ましい。pHは、必須の要件ではないが、大
きすぎたり小さすぎてもシロキサンポリマー液の保存安
定性が低下する傾向がある。The basic compound used in the present invention is substituted with an aromatic group such as a phenyl group such as ammonia (which may be used as aqueous ammonia), octylamine, N, N-dimethylbenzylamine and the like. Alkylamines (preferably having 1 to 9 carbon atoms, excluding substituents), dialkylamines or trialkylamines, and arylamines (amine compounds having an aromatic group) such as aniline. . The basic compound is necessary for stabilizing the obtained siloxane polymer solution. In the absence of the above basic compound, the stability is impaired, and the gel is easily formed. The basic compound is preferably used so that the pH of the siloxane polymer liquid is 5 to 7, particularly preferably 5 to 6. The pH is not an essential requirement, but if it is too high or too low, the storage stability of the siloxane polymer solution tends to decrease.
【００１４】このようにして得られた塗布液を用いて酸
化物被膜を形成するには、該塗布液をシリコンウエハ
ー、アルミニウム等の金属板、表面に金属を形成したシ
リコンウエハー、回路の形成されたシリコンウエハー等
の基体上に、浸漬法、回転塗布法などの方法で塗布した
後、５０〜２００℃、好ましくは、１００〜１５０℃で
乾燥し、ついで、窒素雰囲気中で３００〜５００℃、好
ましくは３００〜４５０℃で焼成する。このシリカ系被
膜を多層配線構造の層間膜（絶縁層間膜）として半導体
装置を得ることができる。In order to form an oxide film using the coating solution thus obtained, a silicon wafer, a metal plate such as aluminum, a silicon wafer having a metal formed on the surface, and a circuit are formed. After coating on a substrate such as a silicon wafer by a dipping method, a spin coating method, or the like, drying is performed at 50 to 200 ° C., preferably 100 to 150 ° C., and then 300 to 500 ° C. in a nitrogen atmosphere. Preferably, firing is performed at 300 to 450 ° C. A semiconductor device can be obtained by using this silica-based coating as an interlayer film (insulating interlayer film) having a multilayer wiring structure.
【００１５】本発明の塗布液を用いて得られる酸化物被
膜は、従来のアルコキシシランの加水分解縮合物を用い
て得られる酸化物被膜と比較して、金属との接着性が向
上しており、また熱的安定性、成膜性は従来のアルコキ
シシランの加水分解縮合物を用いて得られる酸化物被膜
と同等の酸化膜が形成される。The oxide film obtained by using the coating solution of the present invention has improved adhesion to metal as compared with an oxide film obtained by using a conventional hydrolysis condensate of alkoxysilane. In addition, an oxide film having the same thermal stability and film formability as an oxide film obtained by using a conventional hydrolysis condensate of alkoxysilane is formed.
【００１６】[0016]
【実施例】以下、本発明を実施例により詳しく説明す
る。 実施例１ テトラメトキシシラン ５１．０ｇ、ジメチルジメトキ
シシラン ４５．０ｇ、トリメチルトリメトキシシラン
４０．０ｇをイソプロピルアルコール１００．０ｇに
溶解し、この溶液に水５０．０ｇにリン酸２．０ｇを溶
解した液を撹拌下で１時間かけて滴下した。滴下終了後
５時間撹拌した後、アニリン１．３ｇを添加し、更に１
時間撹拌してシリカ系被膜形成用塗布液を得た。この塗
布液のｐＨは５．２であった。この塗布液は、１カ月室
温で放置してもゲル化せず、安定であった。The present invention will be described below in more detail with reference to examples. Example 1 51.0 g of tetramethoxysilane, 45.0 g of dimethyldimethoxysilane, and 40.0 g of trimethyltrimethoxysilane were dissolved in 100.0 g of isopropyl alcohol, and 2.0 g of phosphoric acid was dissolved in 50.0 g of water in this solution. The liquid was added dropwise over 1 hour under stirring. After completion of the dropwise addition, the mixture was stirred for 5 hours, and 1.3 g of aniline was added.
After stirring for an hour, a coating solution for forming a silica-based film was obtained. The pH of this coating solution was 5.2. This coating solution was stable without being gelled even when left at room temperature for one month.
【００１７】上記の塗布液をスピナーを用いて２０００
回転／分でシリコンウエハー上にアルミニウムを形成し
た基体に塗布した後１５０℃に制御されたホットプレー
ト上で１分聞乾燥し、４００℃で窒素雰囲気の電気炉中
で１時間焼成したところ無色透明でクラックのない被膜
が得られた。この被膜の膜厚を測定したところ１．２μ
ｍであった。[0017] The above coating solution was 2,000
After applying to a substrate on which aluminum was formed on a silicon wafer at a rate of rev / min, it was dried on a hot plate controlled at 150 ° C. for 1 minute and baked at 400 ° C. for 1 hour in an electric furnace under a nitrogen atmosphere. A film without cracks was obtained. When the film thickness of this film was measured, it was 1.2 μm.
m.
【００１８】実施例２ テトラメトキシシラン ７５．０ｇ、ジメチルジメトキ
シシラン ７０．０ｇ、をイソプロピルアルコール５
０．０ｇに溶解し、この溶液に水５５．０ｇにマレイン
酸０．５ｇを溶解した液を撹拌下で１時間かけて滴下し
た。滴下終了後５時間撹拌した後、オクチルアミン０．
４ｇを添加し、更に１時間撹拌してシリカ系被膜形成用
塗布液を得た。この塗布液のｐＨは５．８であった。こ
の塗布液は、１カ月室温で放置してもゲル化せず、安定
であった。Example 2 75.0 g of tetramethoxysilane and 70.0 g of dimethyldimethoxysilane were added to isopropyl alcohol 5
A solution of 0.5 g of maleic acid in 55.0 g of water was added dropwise to this solution over 1 hour with stirring. After the dropwise addition, the mixture was stirred for 5 hours, and then octylamine was added.
4 g was added, and the mixture was further stirred for 1 hour to obtain a coating solution for forming a silica-based film. The pH of this coating solution was 5.8. This coating solution was stable without being gelled even when left at room temperature for one month.
【００１９】上記の塗布液た。をスピナーを用いて２０
００回転／分でシリコンウエハー上にアルミニウムを形
成した基体に塗布した後１５０℃に制御されたホットプ
レート上で１分聞乾燥し、４００℃で窒素雰囲気の電気
炉中で１時間焼成したところ無色透明でクラックのない
被膜が得られた。この被膜の膜厚を測定したところ１．
０μｍであった。The above coating solution was used. 20 using a spinner
It was applied to a substrate on which aluminum was formed on a silicon wafer at 00 revolutions / minute, then dried on a hot plate controlled at 150 ° C. for 1 minute, and baked at 400 ° C. for 1 hour in an electric furnace under a nitrogen atmosphere to be colorless. A transparent and crack-free coating was obtained. When the film thickness of this coating was measured,
It was 0 μm.
【００２０】比較例１ テトラメトキシシラン ５１．０ｇ、ジメチルジメトキ
シシラン ４５．０ｇ、トリメチルトリメトキシシラン
４０．０ｇをイソプロピルアルコール１００．０ｇに
溶解し、この溶液に水５０．０ｇにリン酸２．０ｇを溶
解した液を撹拌下で１時間かけて滴下し、滴下終了後５
時間撹拌してシリカ系被膜形成用塗布液を得た。この塗
布液を室温で放置したところ、２週間でゲル化した。Comparative Example 1 51.0 g of tetramethoxysilane, 45.0 g of dimethyldimethoxysilane and 40.0 g of trimethyltrimethoxysilane were dissolved in 100.0 g of isopropyl alcohol, and 2.0 g of phosphoric acid was added to 50.0 g of water in this solution. Was added dropwise over 1 hour with stirring, and 5 hours after the addition was completed.
After stirring for an hour, a coating solution for forming a silica-based film was obtained. When this coating solution was left at room temperature, it gelled in two weeks.
【００２１】比較例２ テトラメトキシシラン ７５．０ｇ、ジメチルジメトキ
シシラン ７０．０ｇをイソプロピルアルコール５０．
０ｇに溶解し、この溶液に水５５．０ｇにマレイン酸
０．５ｇを溶解した液を撹拌下で１時間かけて滴下し
た。滴下終了後５時間撹拌した後、オクチルアミン０．
８ｇを添加し、更に１時間撹拌してシリカ系被膜形成用
塗布液を得た。この塗布液のｐＨは７．３であった。こ
の塗布液は、１カ月室温で放置したところ、ゲル化し
た。Comparative Example 2 75.0 g of tetramethoxysilane and 70.0 g of dimethyldimethoxysilane were added to 50.50 g of isopropyl alcohol.
0 g, and a solution prepared by dissolving 0.5 g of maleic acid in 55.0 g of water was added dropwise to this solution over 1 hour with stirring. After the dropwise addition, the mixture was stirred for 5 hours, and then octylamine was added.
8 g was added, and the mixture was further stirred for 1 hour to obtain a coating solution for forming a silica-based film. The pH of this coating solution was 7.3. This coating solution gelled when left at room temperature for one month.
【００２２】[0022]
【発明の効果】請求項１又は２におけるシリカ系被膜形
成用塗布液は、保存安定性に優れ、厚膜成膜性にも優
れ、耐クラック性優れる被膜を形成することができる。
請求項３又は４における方法により、保存安定性に優
れ、厚膜成膜性にも優れ、耐クラック性優れる被膜を形
成することができるシリカ系被膜形成用塗布液が得られ
る。請求項５におけるシリカ系被膜は、耐クラック性に
優れる。According to the first or second aspect of the present invention, the coating solution for forming a silica-based film can form a film having excellent storage stability, excellent film-forming properties, and excellent crack resistance.
According to the method of claim 3 or 4, a coating liquid for forming a silica-based film, which can form a film having excellent storage stability, excellent film-forming properties, and excellent crack resistance, can be obtained. The silica-based coating according to claim 5 is excellent in crack resistance.
【手続補正書】[Procedure amendment]
【提出日】平成９年８月５日[Submission date] August 5, 1997
【手続補正２】[Procedure amendment 2]
【補正対象書類名】明細書[Document name to be amended] Statement
【補正対象項目名】発明の名称[Correction target item name] Name of invention
【補正方法】変更[Correction method] Change
【補正内容】[Correction contents]
【発明の名称】 シリカ系被膜形成用塗布液、その製造
法及びシリカ系被膜Patent application title: Coating solution for forming silica-based film, method for producing the same, and silica-based film
───────────────────────────────────────────────────── フロントページの続き (72)発明者 成田 武憲 茨城県日立市東町四丁目13番１号 日立化 成工業株式会社半導体・液晶材料事業部開 発センタ内 (72)発明者 野部 茂 茨城県日立市東町四丁目13番１号 日立化 成工業株式会社半導体・液晶材料事業部開 発センタ内 ──────────────────────────────────────────────────続 き Continued on the front page (72) Inventor Takenori Narita 4-3-1-1, Higashicho, Hitachi City, Ibaraki Pref. Hitachi Chemical Co., Ltd. Semiconductor & Liquid Crystal Materials Division Development Center (72) Inventor Shigeru Nobe Ibaraki 3-1 Higashi-cho, Hitachi, Japan Hitachi Chemical Co., Ltd. Semiconductor & LCD Materials Division Development Center
Claims (5)
整数を意味し、複数個のＲは同一でも異なっていてもよ
い）で表されるアルコキシシラン化合物を加水分解、重
縮合させて得られるシロキサンポリマー並びにアンモニ
ア、アルキルアミン、ジアルキルアミン、トリアルキル
アミン及びアリールアミンからなる群から選ばれる少な
くとも一種の塩基性化合物を含有してなるシリカ系被膜
形成用塗布液。(A) General formula (I) (Wherein R is an alkyl group having 1 to 4 carbon atoms, n is an integer of 0 to 2, and a plurality of Rs may be the same or different), A coating liquid for forming a silica-based film, comprising a siloxane polymer obtained by polycondensation and at least one basic compound selected from the group consisting of ammonia, alkylamine, dialkylamine, trialkylamine and arylamine.
含む請求項１記載のシリカ系被膜形成用塗布液。2. The coating solution for forming a silica-based film according to claim 1, wherein the coating solution contains a basic compound so as to have a pH of 5 to 7.
整数を意味し、複数個のＲは同一でも異なっていてもよ
い）で表されるアルコキシシラン化合物を加水分解、重
縮合させて得られるシロキサンポリマーを製造するに際
して、アンモニア、アルキルアミン、ジアルキルアミ
ン、トリアルキルアミン及びアリールアミンからなる群
から選ばれる少なくとも一種の塩基性化合物を存在させ
ることを特徴とするシリカ系被膜形成用塗布液の製造
法。(A) General formula (I) (Wherein R is an alkyl group having 1 to 4 carbon atoms, n is an integer of 0 to 2, and a plurality of Rs may be the same or different), A step of producing a siloxane polymer obtained by polycondensation, wherein at least one basic compound selected from the group consisting of ammonia, alkylamine, dialkylamine, trialkylamine and arylamine is present; Manufacturing method of coating liquid for formation.
存在させる請求項３記載のシリカ系被膜形成用塗布液の
製造法。4. The method according to claim 3, wherein the basic compound is present at a pH of 5 to 7.
用塗布液を用いて形成されてなるシリカ系被膜。5. A silica-based coating formed by using the coating solution for forming a silica-based coating according to claim 1 or 2.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP18375497A JPH1129743A (en) | 1997-07-09 | 1997-07-09 | Coating solution for formation of silica-based film, its preparation and silica-based film |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP18375497A JPH1129743A (en) | 1997-07-09 | 1997-07-09 | Coating solution for formation of silica-based film, its preparation and silica-based film |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH1129743A true JPH1129743A (en) | 1999-02-02 |
Family
ID=16141400
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP18375497A Pending JPH1129743A (en) | 1997-07-09 | 1997-07-09 | Coating solution for formation of silica-based film, its preparation and silica-based film |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH1129743A (en) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2009114277A (en) * | 2007-11-05 | 2009-05-28 | Nippon Paint Co Ltd | Inorganic/organic composite coating composition containing basic poly-silanol |
| JP2012136563A (en) * | 2010-12-24 | 2012-07-19 | Asahi Kasei E-Materials Corp | Method for producing polysiloxane condensation reaction product varnish |
| KR101300150B1 (en) * | 2011-11-29 | 2013-08-26 | 한토이앤씨 주식회사 | Method of maufacturing resin composite with anti-pollution property and the composite thereof |
| US9685840B2 (en) | 2012-12-21 | 2017-06-20 | Fisher & Paykel Appliances Limited | Motor |
-
1997
- 1997-07-09 JP JP18375497A patent/JPH1129743A/en active Pending
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2009114277A (en) * | 2007-11-05 | 2009-05-28 | Nippon Paint Co Ltd | Inorganic/organic composite coating composition containing basic poly-silanol |
| JP2012136563A (en) * | 2010-12-24 | 2012-07-19 | Asahi Kasei E-Materials Corp | Method for producing polysiloxane condensation reaction product varnish |
| KR101300150B1 (en) * | 2011-11-29 | 2013-08-26 | 한토이앤씨 주식회사 | Method of maufacturing resin composite with anti-pollution property and the composite thereof |
| US9685840B2 (en) | 2012-12-21 | 2017-06-20 | Fisher & Paykel Appliances Limited | Motor |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| EP0992556B1 (en) | Coating liquid for forming silica-based film having low dielectric constant and substrate having film of low dielectric constant coated thereon | |
| US20060289849A1 (en) | Composition for forming porous film, porous film and method for forming the same, interlevel insulator film, and semiconductor device | |
| WO1997035939A1 (en) | Coating fluid for low-permittivity silica coating and substrate provided with low-permittivity coating | |
| JP4473352B2 (en) | Low dielectric constant silica-based coating, coating liquid for forming the same, and method for preparing the coating liquid | |
| TWI234787B (en) | Silica-based coating film on substrate and coating solution therefor | |
| JPH1129743A (en) | Coating solution for formation of silica-based film, its preparation and silica-based film | |
| JPH11340220A (en) | Coating liquid for forming silica film and its manufacture | |
| JPH11302595A (en) | Coating solution for forming silica-based film having low permittivity and substrate provided with film having low permittivity | |
| JP4079383B2 (en) | Silica-based coating solution | |
| JP3062040B2 (en) | Heat stable composition | |
| JP2004307693A (en) | Composition for forming porous film, method for producing porous film, porous film, interlayer dielectric film and semiconductor device | |
| JPH1129744A (en) | Coating solution for formation of silica-based film, its preparation and silica-based film | |
| JPH07173434A (en) | Coating fluid for forming oxide film and production of oxide film | |
| JPH06293879A (en) | Coating liquid for forming oxide coating film and production of oxide coating film | |
| JPH05214296A (en) | Coating fluid for forming oxide film and formation of oxide film | |
| JP2000049155A (en) | Semiconductor device | |
| JP2000336312A (en) | Coating solution for forming silica-based coating film, production of silica-based coating film and semiconductor device | |
| KR100444650B1 (en) | Substrate with a low dielectric constant coating film and low dielectric constant coating | |
| JPH10226767A (en) | Coating liquid for forming silica film | |
| KR101940171B1 (en) | Method for manufacturing silica layer, silica layer, and electronic device | |
| JPH10313002A (en) | Formation of sio2 coatings | |
| JP3227359B2 (en) | Semiconductor device | |
| JPH06172709A (en) | Coating fluid for formation of oxide coating film and formation of oxide coating film | |
| JP2006182811A (en) | Coating liquid for forming silica-based film | |
| JPH1112542A (en) | Coating liquid for forming silica-based coating film, silica-based coating film and semiconductor device using the same |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| A621 | Written request for application examination |
Effective date: 20040629 Free format text: JAPANESE INTERMEDIATE CODE: A621 |
|
| A977 | Report on retrieval |
Effective date: 20060818 Free format text: JAPANESE INTERMEDIATE CODE: A971007 |
|
| A131 | Notification of reasons for refusal |
Free format text: JAPANESE INTERMEDIATE CODE: A131 Effective date: 20060824 |
|
| A02 | Decision of refusal |
Free format text: JAPANESE INTERMEDIATE CODE: A02 Effective date: 20061214 |