JPH08176512A - Coating liquid for silica-based film formation, its production, silica-based film and semiconductor device - Google Patents

Coating liquid for silica-based film formation, its production, silica-based film and semiconductor device

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Publication number
JPH08176512A
JPH08176512A JP32222994A JP32222994A JPH08176512A JP H08176512 A JPH08176512 A JP H08176512A JP 32222994 A JP32222994 A JP 32222994A JP 32222994 A JP32222994 A JP 32222994A JP H08176512 A JPH08176512 A JP H08176512A
Authority
JP
Japan
Prior art keywords
silica
coating
integer
coating liquid
general formula
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
Application number
JP32222994A
Other languages
Japanese (ja)
Inventor
Shigeru Nobe
茂 野部
Yasuhiro Yamamoto
靖浩 山本
Hiroyuki Morishima
浩之 森嶋
Yasuo Shimamura
泰夫 島村
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Showa Denko Materials Co Ltd
Original Assignee
Hitachi Chemical Co Ltd
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Hitachi Chemical Co Ltd filed Critical Hitachi Chemical Co Ltd
Priority to JP32222994A priority Critical patent/JPH08176512A/en
Publication of JPH08176512A publication Critical patent/JPH08176512A/en
Pending legal-status Critical Current

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Abstract

PURPOSE: To obtain the subject coating liquid containing a specific polysilazane compound and a diamine compound, capable of reducing coating unevenness or the unevenness of the resultant silica-based film and improving the flatness of a wiring interlayer film, thus useful for e.g. improving the reliability of the semiconductor devices using this coating liquid. CONSTITUTION: This coating liquid contains (A) a polysilazane compound of formula I (R<1> -R<3> are each H or a 1-3C alkyl; (n) is an integer) and (B) a diamine compound of formula II ((m) is 0, 1 or 2; (q) is an integer of 1-10; R<4> is a 1-10C aliphatic group) or formula III ((p) is an integer of 1-10; R<5> is methly or phenyl). The diamine compound of formula II of the component B is e.g. N,N,N',N'- tetramethyldiaminomethane, N,N,N',N'-tetramethylethylenediamine, and the diamine compound of formula III is a e.g. α, ω-bis(3-aminopropyl) polydimethylsiloxane.

Description

【発明の詳細な説明】Detailed Description of the Invention

【0001】[0001]

【産業上の利用分野】本発明はシリカ系被膜形成用塗布
液、この塗布液の製造法、シリカ系被膜および半導体装
置に関する。
BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a coating liquid for forming a silica coating, a method for producing the coating, a silica coating and a semiconductor device.

【0002】[0002]

【従来の技術】近年、半導体装置の高集積化にともない
配線幅が細くなり、かつその間隙は狭くなり、配線は多
層化が進んでいる。このため、上層の配線に断線が生じ
たり、またリソグラフィ工程においてフォーカスマージ
ンの確保が困難になってきている。これらの問題を解決
するため、配線の層間絶縁膜による平坦化が重要な技術
になってきている。層間絶縁膜による平坦化法として
は、バイアススパッタ法、CVD(Chemical Vaper Dep
osition)法、CMP(Chemical Mechanical Polishin
g)法などが検討されている。しかし、量産性、平坦性
などの観点から、SOG(Spin On Glass)と呼ばれる
シリカ系被膜形成用塗布液をウエハ上に回転塗布し、加
熱硬化させることによりシリカ系被膜を形成するSOG
法が広く用いられている。このシリカ系被膜形成用塗布
液は、アルコキシシラン化合物を溶媒中、触媒の存在
下、水を添加してアルコキシ基を加水分解し、縮重合さ
せて製造されたポリシロキサン溶液が多く用いられる。
このシリカ系被膜形成用塗布液により形成されたシリカ
系被膜を層間絶縁膜に適用する場合、エッチバック処理
を行い、膜の上下をCVDによる酸化ケイ素系膜で挟ん
だ3層構造で用いられる。これは、半導体素子の信頼性
を向上させるためで、配線間をつなぐために形成された
層間絶縁膜のスルーホール側壁にシリカ系被膜を露出さ
せないためである。しかし、半導体素子は配線の多層化
が進んでおり、工程数低減のためエッチバックを行わず
に使用できるSOG材料が求められている。この要求に
応えるため、各種の材料、プロセスが検討されてきた。
エッチバックを行わずに使用できるSOG材料としては
ポリシラザンが検討されており、例えば特開平4−34
1705号公報に示されるように、ポリシラザン溶液を
半導体装置形成基板に塗布後、非水条件下で加熱硬化し
シリカ系被膜を形成する方法がある。しかし、ポリシラ
ザン化合物溶液を半導体装置形成基板に回転塗布し、加
熱硬化させてシリカ系被膜を形成すると膜表面に細かい
凹凸や色の濃淡として観察される塗布ムラが現れる。こ
のような膜表面の凹凸や塗布ムラは半導体装置の層間絶
縁膜に適用した場合、層間絶縁膜の平坦性を損ない、半
導体装置の信頼性を低下させることになる。
2. Description of the Related Art In recent years, with the high integration of semiconductor devices, the wiring width has become narrower and the gap between them has become narrower, and the wiring has become multi-layered. For this reason, disconnection occurs in the upper wiring, and it is becoming difficult to secure the focus margin in the lithography process. In order to solve these problems, planarization of wiring by an interlayer insulating film has become an important technique. Bias sputtering method, CVD (Chemical Vapor Dep
osition) method, CMP (Chemical Mechanical Polishin)
g) Laws are being studied. However, from the viewpoints of mass productivity, flatness, etc., SOG (Spin On Glass) is a SOG that forms a silica-based coating by spin-coating a coating liquid for forming a silica-based coating on a wafer and curing it by heating.
The method is widely used. As the silica-based coating solution for forming a coating film, a polysiloxane solution produced by polycondensing an alkoxysilane compound in a solvent in the presence of a catalyst to add water to hydrolyze an alkoxy group and polycondensate is often used.
When the silica-based coating formed by this coating liquid for forming a silica-based coating is applied to the interlayer insulating film, it is used in a three-layer structure in which an etchback process is performed and the upper and lower portions of the film are sandwiched by a silicon oxide-based film formed by CVD. This is to improve the reliability of the semiconductor element and not to expose the silica-based coating on the side wall of the through hole of the interlayer insulating film formed to connect the wirings. However, in the semiconductor device, the number of wirings is increasing, and there is a demand for an SOG material that can be used without etching back in order to reduce the number of steps. In order to meet this demand, various materials and processes have been studied.
Polysilazane has been studied as an SOG material that can be used without etching back, and is disclosed in, for example, JP-A-4-34.
As disclosed in Japanese Patent No. 1705, there is a method in which a polysilazane solution is applied to a semiconductor device forming substrate and then heat-cured under non-aqueous conditions to form a silica-based film. However, when the polysilazane compound solution is spin-coated on a semiconductor device forming substrate and heat-cured to form a silica-based coating, fine irregularities and uneven coating, which are observed as light and shade of color, appear on the surface of the film. When applied to the interlayer insulating film of the semiconductor device, such unevenness of the film surface or coating unevenness impairs the flatness of the interlayer insulating film and reduces the reliability of the semiconductor device.

【0003】[0003]

【発明が解決しようとする課題】本発明は、このような
シリカ系被膜表面の凹凸や塗布ムラを低減して配線層間
膜の平坦性を高め、半導体装置の信頼性を向上させるこ
とのできるシリカ系被膜形成用塗布液、この塗布液の製
造法、シリカ系被膜およびこのシリカ系被膜を用いた半
導体装置を提供するものである。
SUMMARY OF THE INVENTION According to the present invention, silica which can improve the reliability of a semiconductor device by reducing the unevenness and coating unevenness on the surface of a silica-based coating to improve the flatness of a wiring interlayer film. The present invention provides a coating liquid for forming a coating film, a method for producing the coating liquid, a silica coating film, and a semiconductor device using the silica coating film.

【0004】[0004]

【課題を解決するための手段】本発明者らは前記の課題
に鑑み、鋭意研究を重ねた結果、下記の一般式(I)で
示されるポリシラザン化合物および特定のジアミン化合
物を含むシリカ系被膜形成用塗布液を加熱硬化させて形
成したシリカ系被膜の表面の凹凸や塗布ムラが低減でき
ることを見いだし、本発明に到達した。
Means for Solving the Problems The inventors of the present invention have conducted extensive studies in view of the above problems, and as a result, formed a silica-based coating film containing a polysilazane compound represented by the following general formula (I) and a specific diamine compound. The inventors have found that it is possible to reduce surface irregularities and coating unevenness of a silica-based coating film formed by heating and curing a coating solution for use in the present invention, and arrived at the present invention.

【0005】本発明は、一般式(I)The present invention has the general formula (I)

【化5】 (式中R1、R2及びR3は水素または炭素数1〜3のア
ルキル基を示し、nは整数を示す)で表されるポリシラ
ザン化合物および一般式(II)
Embedded image (Wherein R 1 , R 2 and R 3 represent hydrogen or an alkyl group having 1 to 3 carbon atoms, and n represents an integer) and the general formula (II)

【化6】 (式中mは0、1または2の整数、qは1〜10の整数
を示し、R4は炭素数1〜10の脂肪族基を示す)で表
されるジアミン化合物または一般式(III)
[Chemical 6] (In the formula, m is an integer of 0, 1 or 2, q is an integer of 1 to 10, and R 4 is an aliphatic group having 1 to 10 carbon atoms) or a general formula (III).

【化7】 (式中pは1〜10の整数を示し、R5はメチル基また
はフェニル基を示す)で表されるジアミン化合物を含有
してなるシリカ系被膜形成用塗布液に関する。ポリシラ
ザン化合物は、例えば特公昭63−16325号公報に
記載されているハロゲノシラン、オルガノハロゲノシラ
ン等とアンモニア、アミン化合物等とを有機溶媒中で反
応させ、重合させることにより得られる。ハロゲノシラ
ンとしては例えば
[Chemical 7] (In the formula, p represents an integer of 1 to 10 and R 5 represents a methyl group or a phenyl group) A coating solution for forming a silica-based coating film, which comprises a diamine compound. The polysilazane compound can be obtained, for example, by reacting a halogenosilane, an organohalogenosilane, etc. described in JP-B-63-16325 with ammonia, an amine compound, etc. in an organic solvent to polymerize them. Examples of halogenosilane include

【化8】 などがある。オルガノハロゲノシランとしては例えばEmbedded image and so on. Examples of the organohalogenosilane include

【化9】 などがある。また、アミン化合物としては[Chemical 9] and so on. Also, as the amine compound

【化10】 などがある。ハロゲノシラン、オルガノハロゲノシラン
等を反応溶媒中に溶解し、ハロゲノシラン1モルに対
し、4モル以上10モル以下のアンモニア、アミン化合
物等を導入する。アンモニア、アミン化合物等中で窒
素、アルゴンなどの不活性ガスをキャリアガスとしてバ
ブリングし、気化したアンモニア、アミン化合物等をハ
ロゲノシラン溶液中に1時間以上かけてゆっくり導入す
る。また、反応中、液温は0℃以下に保持する。反応溶
媒としては、ピリジン、トルエン、キシレンなどが用い
られる。反応後、反応液を濾過し、エバポレータ等によ
り反応溶媒を除去することにより、ポリシラザン化合物
を得ることができる。この反応は水の存在により阻害さ
れるので、一連の操作は乾燥窒素雰囲気下で行う。ポリ
シラザン化合物は、通常GPCを用いて測定されるポリ
スチレン換算分子量で、数平均分子量が600〜500
0、重量平均分子量が1000〜20000の範囲とさ
れ、一般式(I)における整数、nの値は10〜120
の範囲とされる。ポリシラザン化合物は、有機溶媒に溶
解して塗布液とされるが、有機溶媒としとは、例えばト
ルエン、キシレン、ジエチルエーテルなどがあげられ
る。
[Chemical 10] and so on. A halogenosilane, an organohalogenosilane, etc. are dissolved in a reaction solvent, and 4 mol or more and 10 mol or less of ammonia, an amine compound or the like is introduced to 1 mol of the halogenosilane. Bubbling is performed by using an inert gas such as nitrogen or argon as a carrier gas in ammonia, an amine compound or the like, and the vaporized ammonia, amine compound or the like is slowly introduced into the halogenosilane solution over 1 hour or more. The liquid temperature is maintained at 0 ° C. or lower during the reaction. As the reaction solvent, pyridine, toluene, xylene and the like are used. After the reaction, the reaction solution is filtered and the reaction solvent is removed by an evaporator or the like to obtain a polysilazane compound. Since this reaction is hindered by the presence of water, a series of operations are performed under a dry nitrogen atmosphere. The polysilazane compound has a number average molecular weight of 600 to 500 in terms of polystyrene-equivalent molecular weight usually measured using GPC.
0, the weight average molecular weight is in the range of 1000 to 20000, the integer in the general formula (I), the value of n is 10 to 120.
Range. The polysilazane compound is dissolved in an organic solvent to prepare a coating solution, and examples of the organic solvent include toluene, xylene, diethyl ether and the like.

【0006】本発明で用いられるジアミン化合物として
は、一般式(II)
The diamine compound used in the present invention has the general formula (II)

【化11】 (式中mは0、1または2の整数、qは1〜10の整数
を示し、R4は炭素数1〜10の脂肪族基を示す)で表
されるジアミン化合物または一般式(III)
[Chemical 11] (In the formula, m is an integer of 0, 1 or 2, q is an integer of 1 to 10, and R 4 is an aliphatic group having 1 to 10 carbon atoms) or a general formula (III).

【化12】 (式中pは1〜10の整数を示し、R5はメチル基また
はフェニル基を示す)で表されるジアミン化合物が用い
られる。
[Chemical 12] A diamine compound represented by the formula (p represents an integer of 1 to 10 and R 5 represents a methyl group or a phenyl group) is used.

【0007】一般式(II)で示されるジアミン化合物と
しては例えば、N,N,N′,N′−テトラメチルジア
ミノメタン、N,N,N′,N′−テトラメチルエチレ
ンジアミン、N,N,N′,N′−テトラメチルトリメ
チレンジアミン、N,N,N′,N′−テトラメチル−
1,6−ヘキサンジアミンなどがある。一般式(III)
で示されるジアミンの化合物としては例えば、α,ω−
ビス(3−アミノプロピル)ポリジメチルシロキサン、
α,ω−ビス(3−アミノプロピル)ポリジフェニルシ
ロキサンなどがある。
Examples of the diamine compound represented by the general formula (II) include N, N, N ', N'-tetramethyldiaminomethane, N, N, N', N'-tetramethylethylenediamine, N, N, N ', N'-tetramethyltrimethylene diamine, N, N, N', N'-tetramethyl-
1,6-hexanediamine and the like. General formula (III)
Examples of the diamine compound represented by α, ω-
Bis (3-aminopropyl) polydimethylsiloxane,
Examples include α, ω-bis (3-aminopropyl) polydiphenylsiloxane.

【0008】また、本発明は、上記のポリシラザン化合
物の上記の有機溶媒を用いた溶液に上記のジアミン化合
物を添加するシリカ系被膜形成用塗布液の製造方法に関
するが、このような方法により製造されたシリカ系被膜
形成用塗布液は、主に回転塗布によりウエハなどの基板
上に塗布される。塗布方法としては、この他に、ディッ
プ、スプレーなどがある。また、塗布基板としてはガラ
ス、セラミック、金属などを用いることもできる。これ
らの方法で塗布した後、大気中で100〜200℃で予
備硬化し、硬化炉中で300〜500℃で本硬化させる
ことによりシリカ系被膜が形成される。予備硬化は、ホ
ットプレート上で30秒〜3分間、本硬化は10〜30
分間行うことが好ましい。本発明のシリカ系被膜は半導
体装置の層間絶縁膜として用いることが好ましい。半導
体装置の層間絶縁膜は半導体装置上の配線間に本発明の
シリカ系被膜を形成して得られる。
The present invention also relates to a method for producing a coating liquid for forming a silica-based coating film, which comprises adding the above diamine compound to a solution of the above polysilazane compound using the above organic solvent. The coating liquid for forming a silica-based film is applied onto a substrate such as a wafer mainly by spin coating. In addition to this, as a coating method, there is dip, spray, or the like. Moreover, glass, ceramics, metal, etc. can also be used as a coating substrate. After applying by these methods, pre-curing is performed at 100 to 200 ° C. in the atmosphere, and main curing is performed at 300 to 500 ° C. in a curing furnace to form a silica-based coating. Pre-cure 30 seconds to 3 minutes on the hot plate, main cure 10-30
It is preferable to perform it for a minute. The silica-based coating film of the present invention is preferably used as an interlayer insulating film of a semiconductor device. The interlayer insulating film of a semiconductor device is obtained by forming the silica-based film of the present invention between wirings on the semiconductor device.

【0009】以下本発明を実施例及び比較例により説明
するが、本発明はこれらの実施例に限定されるものでは
ない。 実施例1 特公昭63−16325号公報に記載の製造法に準じて
ポリシラザン溶液を製造した。500mlの4口フラスコ
中に乾燥ピリジン150mlを入れ、氷冷した。これにH
2SiCl2 16.1gを1時間かけて徐々に加えたと
ころ、白色のアダクツが生成した。これにアンモニア1
0.9gを乾燥した窒素ガスと共に80分かけて導入し
た。反応終了後、濾過した。濾液から溶媒を減圧除去
し、ポリシラザン化合物を得た。50mlのなす型フラス
コ中でポリシラザン化合物2gにキシレン8gを加えて
溶解し、これにN,N,N′,N′−テトラメチルエチ
レンジアミン0.129gを添加し塗布液を作製した。
これをウエハの上に回転塗布し、大気中、ホットプレー
トで150℃で30秒ついで250℃で30秒予備硬化
した。次に石英炉の中に入れ、300℃で10分ついで
400℃で20分硬化した。金属顕微鏡を用い、倍率2
00倍でシリカ系被膜表面を観察したところ表面の凹凸
や塗布ムラは認められなかった。
The present invention will be described below with reference to examples and comparative examples, but the present invention is not limited to these examples. Example 1 A polysilazane solution was produced according to the production method described in JP-B-63-16325. 150 ml of dry pyridine was placed in a 500-ml four-necked flask and cooled with ice. H to this
When 16.1 g of 2 SiCl 2 was gradually added over 1 hour, a white adduct was formed. Ammonia 1
0.9 g was introduced over 80 minutes with dry nitrogen gas. After the reaction was completed, it was filtered. The solvent was removed from the filtrate under reduced pressure to obtain a polysilazane compound. In a 50 ml eggplant-shaped flask, 8 g of xylene was added to 2 g of the polysilazane compound and dissolved, and 0.129 g of N, N, N ', N'-tetramethylethylenediamine was added to this to prepare a coating solution.
This was spin-coated on a wafer and pre-cured at 150 ° C. for 30 seconds and then at 250 ° C. for 30 seconds in a hot plate in the atmosphere. Then, it was placed in a quartz furnace and cured at 300 ° C. for 10 minutes and then at 400 ° C. for 20 minutes. Magnification 2 using a metallurgical microscope
When the surface of the silica coating was observed at 00 times, no surface irregularities or coating unevenness was observed.

【0010】実施例2 実施例1と同様にして作製したポリシラザン化合物2g
にキシレン8gを加えて溶解し、これにN,N,N′,
N′−テトラメチル−1,6−ヘキサンジアミン0.1
78gを添加し塗布液を作製した。この塗布液を実施例
1と同様にしてウエハの上に回転塗布し、大気中、ホッ
トプレートで150℃で30秒ついで250℃で30秒
予備硬化した。実施例1で用いた石英炉の中に入れ、3
00℃で10分ついで400℃で20分硬化した。金属
顕微鏡を用い、倍率200倍でシリカ系被膜表面を観察
したところ表面の凹凸や塗布ムラは認められなかった。
Example 2 2 g of polysilazane compound prepared in the same manner as in Example 1
Xylene 8 g was added to and dissolved in N, N, N ',
N'-tetramethyl-1,6-hexanediamine 0.1
78 g was added to prepare a coating solution. This coating solution was spin-coated on a wafer in the same manner as in Example 1, and preliminarily cured at 150 ° C. for 30 seconds and then at 250 ° C. for 30 seconds in the air using a hot plate. It was placed in the quartz furnace used in Example 1 and 3
Curing was carried out at 00 ° C. for 10 minutes and then at 400 ° C. for 20 minutes. When the surface of the silica-based coating film was observed with a metallurgical microscope at a magnification of 200 times, no surface irregularity or coating unevenness was observed.

【0011】実施例3 実施例1と同様にして作製したポリシラザン化合物2g
にキシレン8gを加えて溶解し、これにα,ω−ビス
(3−アミノプロピル)ポリジメチルシロキサン(重合
度p=4、R5=CH3)0.125gを添加し塗布液を
作製した。この塗布液を実施例1と同様にしてウエハの
上に回転塗布し、大気中、ホットプレートで150℃で
30秒ついで250℃で30秒予備硬化した。実施例1
で用いた石英炉の中に入れ、300℃で10分ついで4
00℃で20分硬化した。金属顕微鏡を用い、倍率20
0倍でシリカ系被膜表面を観察したところ表面の凹凸や
塗布ムラは認められなかった。
Example 3 2 g of polysilazane compound prepared in the same manner as in Example 1
8 g of xylene was added to and dissolved therein, and 0.125 g of α, ω-bis (3-aminopropyl) polydimethylsiloxane (polymerization degree p = 4, R 5 = CH 3 ) was added to this to prepare a coating solution. This coating solution was spin-coated on a wafer in the same manner as in Example 1, and preliminarily cured at 150 ° C. for 30 seconds and then at 250 ° C. for 30 seconds in the air using a hot plate. Example 1
Place it in the quartz furnace used in step 10 at 300 ° C for 10 minutes, and then
Cured at 00 ° C. for 20 minutes. Magnification 20 using a metallurgical microscope
When the surface of the silica coating was observed at 0 times, no surface irregularities or coating unevenness was observed.

【0012】実施例4 実施例1と同様にして作製したポリシラザン化合物2g
にキシレン8gを加えて溶解し、これにα,ω−ビス
(3−アミノプロピル)ポリジメチルシロキサン(重合
度p=8、R5=CH3)0.125gを添加し塗布液を
作製した。この塗布液を実施例1と同様にしてウエハの
上に回転塗布し、大気中、ホットプレートで150℃で
30秒ついで250℃で30秒予備硬化した。実施例1
で用いた石英炉の中に入れ、300℃で10分ついで4
00℃で20分硬化した。金属顕微鏡を用い、倍率20
0倍でシリカ系被膜表面を観察したところ表面の凹凸や
塗布ムラは認められなかった。
Example 4 2 g of polysilazane compound prepared in the same manner as in Example 1
8 g of xylene was added to and dissolved therein, and 0.125 g of α, ω-bis (3-aminopropyl) polydimethylsiloxane (polymerization degree p = 8, R 5 = CH 3 ) was added thereto to prepare a coating solution. This coating solution was spin-coated on a wafer in the same manner as in Example 1, and preliminarily cured at 150 ° C. for 30 seconds and then at 250 ° C. for 30 seconds in the air using a hot plate. Example 1
Place it in the quartz furnace used in step 10 at 300 ° C for 10 minutes, and then
Cured at 00 ° C. for 20 minutes. Magnification 20 using a metallurgical microscope
When the surface of the silica coating was observed at 0 times, no surface irregularities or coating unevenness was observed.

【0013】比較例1 実施例1と同様にして作製したポリシラザン化合物2g
にキシレン8gを加えて溶解し、塗布液を作製した。こ
の塗布液を実施例1と同様にウエハの上に回転塗布し、
大気中、ホットプレートで150℃で30秒ついで25
0℃で30秒予備硬化した。実施例1で用いた石英炉の
中に入れ、300℃で10分ついで400℃で20分硬
化した。金属顕微鏡を用い、倍率200倍でシリカ系被
膜表面を観察したところ表面の凹凸や塗布ムラが無数に
発生した。一部、大きなものは肉眼でも確認された。
Comparative Example 1 2 g of polysilazane compound prepared in the same manner as in Example 1
8 g of xylene was added to and dissolved to prepare a coating solution. This coating solution was spin coated on the wafer in the same manner as in Example 1,
In the air, on a hot plate at 150 ° C for 30 seconds, then 25
It was pre-cured at 0 ° C. for 30 seconds. It was placed in the quartz furnace used in Example 1 and cured at 300 ° C. for 10 minutes and then at 400 ° C. for 20 minutes. When the surface of the silica-based coating film was observed with a metallurgical microscope at a magnification of 200 times, numerous surface irregularities and coating unevenness occurred. Some large ones were also confirmed by the naked eye.

【0014】[0014]

【発明の効果】本発明により、ポリシラザンから形成さ
れたシリカ系被膜の表面の凹凸や塗布ムラを低減して配
線層間膜の平坦性を高めることが可能になる。
According to the present invention, it is possible to improve the flatness of the wiring interlayer film by reducing the unevenness of the surface and the coating unevenness of the silica coating formed of polysilazane.

───────────────────────────────────────────────────── フロントページの続き (51)Int.Cl.6 識別記号 庁内整理番号 FI 技術表示箇所 C08L 83/16 LRM H01L 21/768 (72)発明者 島村 泰夫 茨城県日立市東町四丁目13番1号 日立化 成工業株式会社山崎工場内─────────────────────────────────────────────────── ─── Continuation of the front page (51) Int.Cl. 6 Identification number Internal reference number FI Technical indication C08L 83/16 LRM H01L 21/768 (72) Inventor Yasio Shimamura 4-13 Higashimachi, Hitachi City, Ibaraki Prefecture No. 1 Hitachi Chemical Co., Ltd. Yamazaki Factory

Claims (4)

【特許請求の範囲】[Claims] 【請求項1】 一般式(I) 【化1】 (式中R1、R2及びR3は水素または炭素数1〜3のア
ルキル基を示し、nは整数を示す)で表されるポリシラ
ザン化合物および一般式(II) 【化2】 (式中mは0、1または2の整数、qは1〜10の整数
を示し、R4は炭素数1〜10の脂肪族基を示す)で表
されるジアミン化合物または一般式(III) 【化3】 (式中pは1〜10の整数を示し、R5はメチル基また
はフェニル基を示す)で表されるジアミン化合物を含有
してなるシリカ系被膜形成用塗布液。
1. A compound of the general formula (I) (Wherein R 1 , R 2 and R 3 represent hydrogen or an alkyl group having 1 to 3 carbon atoms, and n represents an integer) and a polysilazane compound represented by the general formula (II): (In the formula, m is an integer of 0, 1 or 2, q is an integer of 1 to 10, and R 4 is an aliphatic group having 1 to 10 carbon atoms) or a general formula (III). [Chemical 3] (In the formula, p represents an integer of 1 to 10 and R 5 represents a methyl group or a phenyl group) A coating solution for forming a silica-based coating film containing a diamine compound.
【請求項2】 一般式(I) 【化4】 (式中R1、R2及びR3は水素または炭素数1〜3のア
ルキル基を示し、nは整数を示す)で表されるポリシラ
ザン化合物の溶液に請求項1記載の一般式(II)で表さ
れるジアミン化合物または請求項1記載の一般式(II
I)で表されるジアミン化合物を添加することを特徴と
するシリカ系被膜形成用塗布液の製造法。
2. A compound represented by the general formula (I): (Wherein R 1 , R 2 and R 3 represent hydrogen or an alkyl group having 1 to 3 carbon atoms, and n represents an integer) in a solution of a polysilazane compound represented by the general formula (II) according to claim 1. Or a diamine compound represented by the general formula (II
A method for producing a coating liquid for forming a silica-based coating, which comprises adding a diamine compound represented by I).
【請求項3】 請求項1〜3のいずれかに記載のシリカ
系被膜形成用塗布液を用いて形成されたシリカ系被膜。
3. A silica-based coating film formed by using the coating liquid for forming a silica-based coating film according to claim 1.
【請求項4】 請求項3記載のシリカ系被膜を層間絶縁
膜とした半導体装置。
4. A semiconductor device in which the silica-based coating according to claim 3 is used as an interlayer insulating film.
JP32222994A 1994-12-26 1994-12-26 Coating liquid for silica-based film formation, its production, silica-based film and semiconductor device Pending JPH08176512A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP32222994A JPH08176512A (en) 1994-12-26 1994-12-26 Coating liquid for silica-based film formation, its production, silica-based film and semiconductor device

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP32222994A JPH08176512A (en) 1994-12-26 1994-12-26 Coating liquid for silica-based film formation, its production, silica-based film and semiconductor device

Publications (1)

Publication Number Publication Date
JPH08176512A true JPH08176512A (en) 1996-07-09

Family

ID=18141379

Family Applications (1)

Application Number Title Priority Date Filing Date
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Country Status (1)

Country Link
JP (1) JPH08176512A (en)

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