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1. 发明授权

US06558747B2 Method of forming insulating film and process for producing semiconductor device 有权
公开(公告)号：US06558747B2
公开(公告)日：2003-05-06
申请号：US10014593
申请日：2001-12-14
申请人： Rempei Nakata , Nobuhide Yamada , Hideshi Miyajima , Akihiro Kojima , Takahiko Kurosawa , Eiji Hayashi , Youngsoon Seo , Atsushi Shiota , Kinji Yamada
发明人： Rempei Nakata , Nobuhide Yamada , Hideshi Miyajima , Akihiro Kojima , Takahiko Kurosawa , Eiji Hayashi , Youngsoon Seo , Atsushi Shiota , Kinji Yamada
IPC分类号： B05D379397
CPC分类号： C08G77/16 , C09D183/06 , H01L21/02126 , H01L21/02216 , H01L21/02282 , H01L21/3122 , Y10T428/31663
摘要： A method of forming an insulating film which includes the steps of: dissolving in a solvent a first and second polymer which each comprise methylpolysiloxane as the main component and one of which has a weight average molecular weight at least 10 times that of the other to thereby prepare a chemical solution; applying the chemical solution to a semiconductor substrate to form a coating film; and heat-treating the coating film to thereby form an organosilicon oxide film. The weight-average molecular weight of the first polymer is preferably at least 100 times that of the second polymer. Thus, an insulating organosilicon oxide film having a low dielectric constant and high cracking resistance is formed from a coating fluid.

2. 发明授权

US06410151B1 Composition for film formation, method of film formation, and insulating film 有权
标题翻译：用于成膜的成分，成膜方法和绝缘膜
公开(公告)号：US06410151B1
公开(公告)日：2002-06-25
申请号：US09670547
申请日：2000-09-27
申请人： Takahiko Kurosawa , Eiji Hayashi , Seo Youngsoon , Atsushi Shiota , Kinji Yamada
发明人： Takahiko Kurosawa , Eiji Hayashi , Seo Youngsoon , Atsushi Shiota , Kinji Yamada
IPC分类号： B32B904
CPC分类号： H01L21/3122 , C09D183/04 , C09D183/14 , H01L21/02126 , H01L21/02216 , H01L21/02282 , Y10T428/31663 , C08L83/00
摘要： A polyorganosiloxane-based composition for film formation which gives a film having low dielectric constant and high modulus of elasticity and useful as an interlayer insulating film in semiconductor devices and the like. The composition for film formation comprises: (A) a product of hydrolysis and condensation obtained by hydrolyzing and condensing, in the presence of an alkali catalyst, at least one member selected from the group consisting of compounds (1) represented by RaSi (OR1)4−a (wherein R represents hydrogen, fluorine, or a monovalent organic group; R1 represents a monovalent organic group; and a Is an integer of 1 or 2), compounds (2) represented by Si(OR2)4 (wherein R2 represents a monovalent organic group), and compounds (3) represented by R3b(R4O)3−bSi—(R7)d—Si(OR5)3−cR6c [wherein R3 to R6 may be the same or different and each represent a monovalent organic group; b and c may be the same or different and each are an integer of 0 to 2; R7 represents oxygen, phenylene, or a group represented by —(CH2)n—, wherein n is an integer of 1 to 6; and d is 0 or 1]; and (B) a product of hydrolysis and condensation obtained by hydrolyzing and condensing, in the presence of a metal chelate compound catalyst, at least one member selected from the group consisting of the compounds (1), (2), and (3).
摘要翻译：一种用于成膜的聚有机硅氧烷基组合物，其具有低介电常数和高弹性模量的膜，并且可用作半导体器件等中的层间绝缘膜。用于成膜的组合物包括：（A）水解和在碱催化剂存在下，通过水解和缩合得到的缩合物，所述缩合物选自由RaSi（OR 1）4-a（其中R表示氢，氟或一价有机物）表示的化合物（1）中的至少一种基团; R1表示一价有机基团，Is表示1或2的整数），由Si（OR 2）4表示的化合物（2）（其中，R2表示一价有机基团），R3b（ R4O）3-bSi-（R7）d-Si（OR5）3-cR6c [其中R3至R6可以相同或不同，各自表示一价有机基团; b和c可以相同或不同，各自为0〜2的整数; R7表示氧，亚苯基或由 - （CH2）n-表示的基团，其中n为1至6的整数; 和d为0或1]; 和（B）在金属螯合化合物催化剂存在下，通过水解和缩合得到的水解和缩合产物，选自化合物（1），（2）和（3）中的至少一种，。

3. 发明授权

US06410150B1 Composition for film formation, method of film formation, and insulating film 有权
标题翻译：用于成膜的成分，成膜方法和绝缘膜
公开(公告)号：US06410150B1
公开(公告)日：2002-06-25
申请号：US09669859
申请日：2000-09-27
申请人： Takahiko Kurosawa , Eiji Hayashi , Seo Youngsoon , Keiji Konno , Atsushi Shiota , Kinji Yamada
发明人： Takahiko Kurosawa , Eiji Hayashi , Seo Youngsoon , Keiji Konno , Atsushi Shiota , Kinji Yamada
IPC分类号： B32B904
CPC分类号： H01L21/3122 , C09D183/04 , C09D183/14 , H01L21/02126 , H01L21/02216 , H01L21/02282 , Y10T428/31663 , C08L83/00
摘要： A polyorganosiloxane-based composition for film formation which gives a film having low dielectric constant and high modulus of elasticity and useful as an interlayer insulating film in semiconductor devices and the like. The composition for film formation comprises: (A) a product of hydrolysis and condensation obtained by hydrolyzing and condensing, in the presence of an alkali catalyst, at least one member selected from the group consisting of compounds (1) represented by RaSi(OR1)4−a (wherein R represents hydrogen, fluorine, or a monovalent organic group; R1 represents a monovalent organic group; and a Is an integer of 1 or 2), compounds (2) represented by Si(OR2)4 (wherein R2 represents a monovalent organic group), and compounds (3) represented by R3b(R4O)3−bSi—(R7)d—Si(OR5)3−cR6c [wherein R3 to R6 may be the same or different and each represent a monovalent organic group; b and c may be the same or different and each are an integer of 0 to 2; R7 represents oxygen, phenylene, or a group represented by —(CH2)n—, wherein n is an integer of 1 to 6; and d is 0 or 1]; and (B) a product of hydrolysis and condensation obtained by hydrolyzing and condensing, in the presence of an acid catalyst, at least one member selected from the group consisting of the compounds (1), (2), and (3).
摘要翻译：一种用于成膜的聚有机硅氧烷类组合物，其具有低介电常数和高弹性模量的膜，并且可用作半导体器件等中的层间绝缘膜。用于成膜的组合物包括：（A）在碱催化剂存在下，通过水解和缩合获得的水解和缩合产物，选自由RaSi（OR1）表示的化合物（1）中的至少一种，（其中R表示氢，氟或一价有机基团; R1表示一价有机基团，Is表示1或2的整数）表示的化合物（2），由Si（OR 2）4表示的化合物（2）一价有机基团）和由R3b（R4O）3-bSi-（R7）d-Si（OR5）3-cR6c表示的化合物（3）[其中R3至R6可以相同或不同，各自表示一价有机基团组; b和c可以相同或不同，各自为0〜2的整数; R7表示氧，亚苯基或由 - （CH2）n-表示的基团，其中n为1至6的整数; 和d为0或1]; 和（B）在酸催化剂存在下，通过水解和缩合获得的至少一种选自化合物（1），（2）和（3）的水解和缩合的产物。

4. 发明授权

US06406794B1 Film-forming composition 有权
标题翻译：成膜组合物
公开(公告)号：US06406794B1
公开(公告)日：2002-06-18
申请号：US09778822
申请日：2001-02-08
申请人： Atsushi Shiota , Takahiko Kurosawa , Eiji Hayashi , Makoto Sugiura , Toshiyuki Akiike , Keiji Konno , Tadahiro Shiba , Kohei Goto , Kinji Yamada
发明人： Atsushi Shiota , Takahiko Kurosawa , Eiji Hayashi , Makoto Sugiura , Toshiyuki Akiike , Keiji Konno , Tadahiro Shiba , Kohei Goto , Kinji Yamada
IPC分类号： B32B904
CPC分类号： C08J5/18 , C08G2650/58 , C08J2371/00 , C08L71/00 , C08L71/02 , C09D171/02 , C09D183/04 , H01L21/02126 , H01L21/02216 , H01L21/02282 , H01L21/3122 , Y10T428/31663 , C08L83/00 , C08L2666/14
摘要： A film-forming composition comprising: (A) at least one silane compound selected from the group consisting of a compound shown by the following formula (1), a compound shown by the following formula (2), and a compound shown by the following formula (3) and a hydrolysis condensate of these compounds: R2R3Si(OR1)2 (1) R2Si(OR1)3 (2) Si(OR1)4 (3) wherein R1, R2, and R3 individually represent a monovalent organic group, (B) a polyether shown by the formula (PEO)p—(PPO)q—(PEO)r, wherein PEO represents a polyethylene oxide unit, PPO represents a polypropylene oxide unit, p is a number of 2-200, q is a number of 20-80, and r is a number of 2-200, and (C) an organic solvent. The composition exhibits superior storage stability, is capable of producing a low-density film having a small relative dielectric constant, low water absorption properties, and small vacant space size, and is thus suitable as an interlayer dielectric material in the manufacture of semiconductor devices.
摘要翻译：一种成膜组合物，其包含：（A）至少一种选自由下式（1）表示的化合物，下式（2）所示的化合物和下述化合物的硅烷化合物式（3）和这些化合物的水解缩合物：其中R1，R2和R3各自表示一价有机基团，（B）由式（PEO）p-（PPO）q-（PEO）r表示的聚醚，其中PEO表示聚环氧乙烷单元，PPO表示聚环氧丙烷单元，p为2〜200的数，q为20〜80的数，r为2〜200的数，（C）有机溶剂。该组合物表现出优异的储存稳定性，能够生产具有小的相对介电常数，低吸水性和小的空间空间尺寸的低密度膜，因此适合作为制造半导体器件的层间绝缘材料。

5. 发明授权

US06800330B2 Composition for film formation, method of film formation, and silica-based film 失效
标题翻译：用于成膜的成分，成膜方法和二氧化硅基膜
公开(公告)号：US06800330B2
公开(公告)日：2004-10-05
申请号：US10103996
申请日：2002-03-25
申请人： Eiji Hayashi , Michinori Nishikawa , Atsushi Shiota , Kinji Yamada
发明人： Eiji Hayashi , Michinori Nishikawa , Atsushi Shiota , Kinji Yamada
IPC分类号： B05D512
CPC分类号： H01L21/02126 , C09D183/04 , C09D183/14 , H01L21/02216 , H01L21/02282 , H01L21/3122
摘要： A composition for film formation capable of forming a silica-based coating film having low water absorption and dielectric constant of 2.1 or lower and useful as an interlayer insulating film material in semiconductor devices, etc. The composition contains: (A) a product of hydrolysis and condensation obtained by hydrolyzing and condensing at least one silane compound selected from the group consisting of compounds represented by formula (1), compounds represented by formula (2), and compounds represented by formula (3) in the presence of a basic catalyst and water, RaSi(OR1)4−a (1) wherein R represents a hydrogen atom, a fluorine atom, or a monovalent organic group, R1 represents a monovalent organic group, and a is an integer of 1 or 2, Si(OR2)4 (2) wherein R2 represents a monovalent organic group, R3b(R4O)3−bSi—(R7)d—Si(OR5)3−cR6c (3) wherein R3 to R6 may be the same or different and each represents a monovalent organic group, b and c may be the same or different and each is a number of 0 to 2, R7 represents an oxygen atom, a phenylene group, or a group represented by —(CH2)n—, wherein n is an integer of 1 to 6, and d is 0 or 1; (B) a compound compatible with or dispersible in ingredient (A) and having a boiling point or decomposition temperature of from 250 to 450° C.; and (C) an organic solvent.
摘要翻译：用于形成能够形成低吸水性和介电常数为2.1以下并且用作半导体装置中的层间绝缘膜材料的二氧化硅系涂膜的成膜用组合物等。该组合物含有：（A）水解产物和通过水解和缩合在式（1）表示的化合物，式（2）表示的化合物和式（3）表示的化合物中的至少一种硅烷化合物在碱性催化剂存在下水解和缩合得到的缩合物，和水，其中R表示氢原子，氟原子或一价有机基团，R 1表示一价有机基团，a为1或2的整数，其中R 2表示一价有机基团，其中R 3至R 6可以相同或不同，并且各自表示一价有机基团，b和c可以相同或不同，并且各自为0至2的数，R 7表示氧原子，亚苯基，或由 - （CH 2）n - 表示的基团，其中n为1至6的整数，d为0或1; （B）与成分（A）相容或分散且沸点或分解温度为250-450℃的化合物; 和（C）有机溶剂。

6. 发明授权

US06787193B2 Method for the formation of silica film, silica film, insulating film, and semiconductor device 失效
标题翻译：形成二氧化硅膜，二氧化硅膜，绝缘膜和半导体器件的方法
公开(公告)号：US06787193B2
公开(公告)日：2004-09-07
申请号：US10165324
申请日：2002-06-10
申请人： Eiji Hayashi , Atsushi Shiota , Michinori Nishikawa , Kinji Yamada
发明人： Eiji Hayashi , Atsushi Shiota , Michinori Nishikawa , Kinji Yamada
IPC分类号： B32B1800
CPC分类号： H01L21/02126 , C09D183/04 , H01L21/02216 , H01L21/02282 , H01L21/02343 , H01L21/31133 , H01L21/31138 , H01L21/3122 , H01L21/31695 , Y02P20/544 , Y10T428/31663
摘要： A method for the formation of a silica film which comprises treating a film in a supercritical medium, the film comprising (A) a siloxane compound and (B) at least one member selected from the group consisting of (B-1) a compound compatible with or dispersible in ingredient (A) and having a boiling or decomposition temperature of from 150 to 500° C. and (B-2) a surfactant. The silica film has excellent mechanical strength showing a dielectric constant of generally 2.2 or lower, and hence is useful as a dielectric film in semiconductor devices and the like.
摘要翻译：一种形成二氧化硅膜的方法，其包括在超临界介质中处理膜，所述膜包含（A）硅氧烷化合物和（B）选自（B-1）中的至少一种，与具有或分散在成分（A）中，沸点或分解温度为150-500℃，和（B-2）表面活性剂。该二氧化硅膜的机械强度优异，介电常数为2.2以下，因此可用作半导体装置等的电介质膜。

7. 发明授权

US06472079B2 Composition for film formation, method of film formation, and silica-based film 有权
标题翻译：用于成膜的成分，成膜方法和二氧化硅基膜
公开(公告)号：US06472079B2
公开(公告)日：2002-10-29
申请号：US09829954
申请日：2001-04-11
申请人： Eiji Hayashi , Michinori Nishikawa , Kinji Yamada
发明人： Eiji Hayashi , Michinori Nishikawa , Kinji Yamada
IPC分类号： B32B9041
CPC分类号： H01L21/02126 , C08G77/06 , C08G77/08 , C08G77/50 , C09D183/04 , C09D183/14 , H01L21/02282 , H01L21/312 , Y10T428/31663
摘要： A composition for film formation which comprises: (A) a product of hydrolysis and condensation obtained by hydrolyzing and condensing at least one compound selected from the group consisting of (A-1) compounds represented by the following formula (1) RaSi(OR1)4-a (1) (A-2) compounds represented by the following formula (2) Si(OR2)4 (2) and (A-3) compounds represented by the following formula (3) R3b(R4O)3-bSi—(R7)d—Si(OR5)3-cR6c (3) (B) at least one member selected from the group consisting of compounds of the metals in Groups IA and IIA of the periodic table; and (C) an organic solvent. A method for film formation using the composition and a silica-based film obtained by the method are also disclosed.
摘要翻译：一种成膜用组合物，其特征在于，含有：（A）水解缩合产物，其通过水解和缩合选自（A-1）由下式（1）表示的化合物（A-2））由下式（2）和（A-3）表示的化合物，由下式（3）（B）表示的化合物中的至少一种选自由周期表中第IA和IIA族中的金属的化合物组成的组中的至少一种表; 和（C）有机溶剂。还公开了使用该组合物和通过该方法获得的二氧化硅基膜的成膜方法。

8. 发明授权

US07128976B2 Composition for film formation, method of film formation, and silica-based film 有权
公开(公告)号：US07128976B2
公开(公告)日：2006-10-31
申请号：US10269967
申请日：2002-10-15
申请人： Eiji Hayashi , Kouichi Hasegawa , Youngsoo Seo , Michinori Nishikawa , Kinji Yamada
发明人： Eiji Hayashi , Kouichi Hasegawa , Youngsoo Seo , Michinori Nishikawa , Kinji Yamada
IPC分类号： B32B25/20
CPC分类号： H01L21/02126 , C08G77/08 , C08G77/50 , C09D183/04 , C09D183/14 , H01L21/02216 , H01L21/02282 , H01L21/3122 , Y10T428/31663
摘要： A composition for film formation which comprises: (A) a product of hydrolysis and condensation obtained by hydrolyzing and condensing at least one silane compound selected from the group consisting of compounds represented by the formula (1), compounds represented by the formula (2), and compounds represented by the formula (3) in the presence of water and an ammonium compound, and (B) an organic solvent.

9. 发明授权

US06503633B2 Composition for film formation, process for producing composition for film formation, method of film formation, and silica-based film 有权
标题翻译：用于成膜的组合物，用于制备成膜用组合物的方法，成膜方法和二氧化硅基膜
公开(公告)号：US06503633B2
公开(公告)日：2003-01-07
申请号：US09860914
申请日：2001-05-21
申请人： Michinori Nishikawa , Kouichi Hasegawa , Eiji Hayashi , Kinji Yamada
发明人： Michinori Nishikawa , Kouichi Hasegawa , Eiji Hayashi , Kinji Yamada
IPC分类号： C08G7716
CPC分类号： H01L21/02126 , H01L21/02216 , H01L21/02282 , H01L21/3122 , H01L21/316 , Y10T428/31663
摘要： A composition for film formation which, when used in the production of semiconductor devices and the like, can give interlayer insulating films which differ little in dielectric constant even when obtained through curing under different conditions and have excellent adhesion to substrates, a process for producing the composition, and a silica-based film obtained from the composition. The composition for film formation comprises: (A) a product of hydrolysis and condensation obtained by hydrolyzing and condensing (A-1) at least one compound selected from the group consisting of compounds represented by the following formula (1), compounds represented by the following formula (2), and compounds represented by the following formula (3), and (A-2) at least one compound represented by the following formula (4), in the presence of a catalyst and water; and (B) an organic solvent.
摘要翻译：一种成膜用组合物，当用于半导体装置等的制造中时，即使在不同条件下固化而获得的介电常数几乎不相等且对基材的附着性优异，也可以制造出组合物和由该组合物获得的二氧化硅基膜。用于成膜的组合物包括：（A）通过水解和缩合获得的水解和缩合产物（A-1）至少一种选自由下式（1）表示的化合物的化合物，由下述式（2）表示的化合物和下述式（3）所示的化合物和（A-2）至少一种下述式（4）所示的化合物在催化剂和水的存在下反应; 和（B）有机溶剂。

10. 发明授权

US07297360B2 Insulation film 有权
标题翻译：绝缘膜
公开(公告)号：US07297360B2
公开(公告)日：2007-11-20
申请号：US10726666
申请日：2003-12-04
申请人： Mutsuhiko Yoshioka , Eiji Hayashi , Kouji Sumiya , Atsushi Shiota
发明人： Mutsuhiko Yoshioka , Eiji Hayashi , Kouji Sumiya , Atsushi Shiota
IPC分类号： B05D5/12 , H01L21/31 , H01L21/469 , C08G77/20
CPC分类号： C09D183/16 , H01L21/02123 , H01L21/02282 , H01L21/31116 , H01L21/31144 , H01L21/3121
摘要： An insulation film comprising an organosilicon polymer and an organic polymer such as polyarylene, polyarylene ether, polyimide, and fluororesin is disclosed, wherein the organosilicon polymer has a relative dielectric constant of 4 or less and has a dry etching selection ratio of 1/3 or less to silicon oxide, fluorine-doped silicon oxide, organosilicate glass, carbon-doped silicon oxide, methyl silsesquioxane, hydrogen silsesquioxane, a spin-on-glass, or polyorganosiloxane. The insulation film is used as an etching stopper or a hard mask in a dry etching process of interlayer dielectric films for semiconductors and can produce semiconductors having excellent precision with minimal damages.
摘要翻译：公开了一种包含有机硅聚合物和有机聚合物如聚亚芳基，聚亚芳基醚，聚酰亚胺和氟树脂的绝缘膜，其中有机硅聚合物的相对介电常数为4以下，干蚀刻选择比为1/3或硅掺杂氧化硅，有机硅酸盐玻璃，碳掺杂氧化硅，甲基硅倍半氧烷，氢倍半硅氧烷，旋涂玻璃或聚有机硅氧烷。在半导体层间绝缘膜的干式蚀刻工艺中，绝缘膜用作蚀刻阻挡层或硬掩模，并且可以以最小的损伤产生具有优异精度的半导体。

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