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.

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。

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， 。

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。

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。

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。

公开(公告)号：US6011123A

公开(公告)日：2000-01-04

申请号：US974916

申请日：1997-11-20

申请人： Takahiko Kurosawa ,  Kinji Yamada ,  Minoru Matsubara ,  Yasutake Inoue ,  Tomotaka Shinoda ,  Kouhei Gotou

发明人： Takahiko Kurosawa ,  Kinji Yamada ,  Minoru Matsubara ,  Yasutake Inoue ,  Tomotaka Shinoda ,  Kouhei Gotou

IPC分类号： C08G77/455 ,  C08K5/5415 ,  C08L79/08 ,  C09D183/10 ,  H01L21/312 ,  C08L77/00

CPC分类号： H01L21/312 ,  C08G77/455 ,  C08K5/5415 ,  C08L79/08 ,  C09D183/10

摘要： A curable resin composition comprising (A) a hydrolyzate or a partial condensate of an organosilane compound, or both; (B) at least one compound selected from the group consisting of polyamic acids having a hydrolyzable silyl group or carboxylic acid anhydride group, or both, and polyimides having a hydrolyzable silyl group or carboxylic acid anhydride group, or both; and (C) a chelate compound or an alkoxide compound with a metal selected from the group consisting of zirconium, titanium, and aluminum, or both the chelate compound and the alkoxide compound. The resin composition can be cured and fabricated without producing no cracks into a cured product such as a semiconductor device having a low dielectric constant, high heat resistance and moisture resistance, superior adhesion to various substrate materials, superb electrical insulation properties, and low moisture absorption. Semiconductor devices using this curable resin composition as an insulating film exhibit a low electricity consumption, work at a high speed, and have excellent reliability.

摘要翻译： 一种可固化树脂组合物，其包含（A）有机硅烷化合物的水解产物或部分缩合物，或两者; （B）至少一种选自具有水解性甲硅烷基或羧酸酐基团的聚酰胺酸或二者的化合物和具有可水解甲硅烷基或羧酸酐基团的聚酰亚胺或两者; 和（C）螯合化合物或选自锆，钛和铝的金属的醇盐化合物，或螯合化合物和醇盐化合物两者。 可以固化和制造树脂组合物，而不会在诸如具有低介电常数，高耐热性和耐湿性，优异的各种基材的粘合性，优异的电绝缘性能和低吸湿性的半导体装置等固化产物中不产生裂纹 。 使用该固化性树脂组合物作为绝缘膜的半导体装置的电耗低，高速工作，可靠性优异。

公开(公告)号：US06313233B1

公开(公告)日：2001-11-06

申请号：US09447952

申请日：1999-11-29

申请人： Takahiko Kurosawa ,  Kinji Yamada ,  Minoru Matsubara ,  Yasutake Inoue ,  Tomotaka Shinoda ,  Kouhei Gotou

发明人： Takahiko Kurosawa ,  Kinji Yamada ,  Minoru Matsubara ,  Yasutake Inoue ,  Tomotaka Shinoda ,  Kouhei Gotou

IPC分类号： C08G6548

CPC分类号： H01L21/02126 ,  C08G77/455 ,  C08K5/5415 ,  C08L79/08 ,  C09D183/10 ,  H01L21/312 ,  C08L2666/52

摘要： A curable resin composition comprising (A) a hydrolyzate or a partial condensate of an organosilane compound, or both; (B) at least one compound selected from the group consisting of polyamic acids having a hydrolyzable silyl group or carboxylic acid anhydride group, or both, and polyimides having a hydrolyzable silyl group or carboxylic acid anhydride group, or both; and (C) a chelate compound or an alkoxide compound with a metal selected from the group consisting of zirconium, titanium, and aluminum, or both the chelate compound and the alkoxide compound. The resin composition can be cured and fabricated without producing no cracks into a cured product such as a semiconductor device having a low dielectric constant, high heat resistance and moisture resistance, superior adhesion to various substrate materials, superb electrical insulation properties, and low moisture absorption. Semiconductor devices using this curable resin composition as an insulating film exhibit a low electricity consumption, work at a high speed, and have excellent reliability.

摘要翻译： 一种可固化树脂组合物，其包含（A）有机硅烷化合物的水解产物或部分缩合物，或两者; （B）至少一种选自具有水解性甲硅烷基或羧酸酐基团的聚酰胺酸或二者的化合物和具有可水解甲硅烷基或羧酸酐基团的聚酰亚胺或两者; 和（C）螯合化合物或选自锆，钛和铝的金属的醇盐化合物，或螯合化合物和醇盐化合物两者。 可以固化和制造树脂组合物，而不会在诸如具有低介电常数，高耐热性和耐湿性，优异的各种基材的粘合性，优异的电绝缘性能和低吸湿性的半导体装置等固化产物中不产生裂纹 。 使用该固化性树脂组合物作为绝缘膜的半导体装置的电耗低，高速工作，可靠性优异。

公开(公告)号：US06235101B1

公开(公告)日：2001-05-22

申请号：US09203534

申请日：1998-12-01

申请人： Takahiko Kurosawa ,  Kinji Yamada ,  Tomotaka Shinoda ,  Minoru Matsubara ,  Satoko Hakamatsuka

发明人： Takahiko Kurosawa ,  Kinji Yamada ,  Tomotaka Shinoda ,  Minoru Matsubara ,  Satoko Hakamatsuka

IPC分类号： C09D525

CPC分类号： H01L21/02126 ,  C08G77/58 ,  C09D183/14 ,  H01L21/02282 ,  H01L21/3121

摘要： A composition for film formation and a film obtained by heating the composition. The composition comprises: (A) a hydrolyzate and/or partial condensate of a compound represented by the following formula (1) R1nSi(OR2)4-n  (1) wherein R1 and R2 may be the same or different and each represent an alkyl group having 1 to 5 carbon atoms or an aryl group having 6 to 20 carbon atoms, and n is an integer of 1 or 2; (B) a metal chelate compound represented by the following formula (2) R3tM(OR4)s-t  (2) wherein R3 represents a chelating agent, M represents a metal atom, R4 represents an alkyl group having 2 to 5 carbon atoms or an aryl group having 6 to 20 carbon atoms, s represents a valence of the metal M, and t is an integer of 1 to s; (C) an organic solvent having a boiling point of 110 to 180° C.; and (D) &bgr;-diketone.

摘要翻译： 用于成膜的组合物和通过加热组合物获得的膜。组合物包含：（A）由下式（1）表示的化合物的水解产物和/或部分缩合物，其中R 1和R 2可以相同或不同， 各自表示碳原子数1〜5的烷基或碳原子数6〜20的芳基，n表示1或2的整数，（B）由下式（2）表示的金属螯合物，其中，R3表示 螯合剂，M表示金属原子，R4表示碳原子数2〜5的烷基或碳原子数6〜20的芳基，s表示金属M的化合价，t表示1〜s的整数。 ;（C）沸点为110〜180℃的有机溶剂。 和（D）β-二酮。

公开(公告)号：US06749944B2

公开(公告)日：2004-06-15

申请号：US10252606

申请日：2002-09-24

申请人： Michinori Nishikawa ,  Manabu Sekiguchi ,  Atsushi Shiota ,  Kinji Yamada

发明人： Michinori Nishikawa ,  Manabu Sekiguchi ,  Atsushi Shiota ,  Kinji Yamada

IPC分类号： B32B904

CPC分类号： B05D1/60 ,  B05D7/52 ,  C09D183/04 ,  C09D183/14 ,  H01L21/02126 ,  H01L21/0214 ,  H01L21/022 ,  H01L21/02211 ,  H01L21/02216 ,  H01L21/02271 ,  H01L21/02282 ,  H01L21/3122 ,  Y10T428/24942 ,  Y10T428/31663

摘要： A stacked film, a method for the production of the stacked film, an insulating film comprising the stacked film, and a substrate for semiconductor, using the insulating film. The stacked film comprises films of two or more kinds of alkoxysilane hydrolysis condensates having 5 nm or more difference in a mean radius of gyration, or films of alkoxysilane hydrolysis condensate having 0.3 or more difference in the dielectric constant. The stacked film is obtained by applying a coating solution comprising (B) a compound having a mean radius of gyration of less than 10 nm, and then applying a coating solution comprising (A) a compound having a mean radius of gyration of from 10 to 30 nm, followed by heating. The stacked film provides a dielectric film (substrate for semiconductor) having superior adhesion to a CVD film.

摘要翻译： 叠层膜，制造层叠膜的方法，包括层叠膜的绝缘膜和使用绝缘膜的半导体用基板。 叠层膜包含两个或更多种平均回转半径的差异为5nm以上的烷氧基硅烷水解缩合物的膜或介电常数为0.3以上的烷氧基硅烷水解缩合物的膜。 通过涂布包含（B）平均回转半径为10nm以下的化合物的涂布溶液，然后涂布包含（A）平均半径为10的化合物的涂布溶液， 30nm，然后加热。 叠层膜提供对CVD膜具有优异粘合性的电介质膜（半导体用基板）。