公开(公告)号：US08227028B2

公开(公告)日：2012-07-24

申请号：US12310486

申请日：2007-07-11

申请人： Miki Egami ,  Akira Nakashima ,  Michio Komatsu

发明人： Miki Egami ,  Akira Nakashima ,  Michio Komatsu

IPC分类号： B05D3/02 ,  B05D3/04 ,  H01L29/00

CPC分类号： C09D1/00 ,  C09D4/00 ,  H01L21/316 ,  C08G77/04

摘要： A method of forming on a substrate an amorphous silica-based coating film having a low dielectric constant of 3.0 or below and a film strength (Young's modulus) of 3.0 GPa or more, which comprises, as a typical one, the steps of; (a) coating on the substrate a liquid composition containing hydrolysate of an organic silicon compound or compounds hydrolyzed in the presence of tetraalkylammonium hydroxide (TAAOH); (b) setting the substrate in a chamber and then drying a coating film formed on the substrate at a temperature in the range from 25 to 340° C.; (c) heating the coating film at a temperature in the range from 105 to 450° C. with introduction of a superheated steam having such a temperature into the chamber, and (d) curing the coating film at a temperature in the range from 350 to 450° C. with introduction of a nitrogen gas into the chamber.

摘要翻译： 一种在基板上形成介电常数低于3.0或更低的无定形二氧化硅基涂层以及3.0GPa或更高的膜强度（杨氏模量）的方法，其中典型的步骤包括： （a）在基材上涂覆含有有机硅化合物的水解产物或在四烷基氢氧化铵（TAAOH））存在下水解的化合物的液体组合物; （b）将基板设置在室中，然后在25至340℃的温度范围内干燥形成在基板上的涂膜。 （c）在105至450℃的温度范围内加热涂膜，并将具有这种温度的过热蒸汽引入室中，和（d）在350℃的温度下固化涂膜 至450℃，同时将氮气引入室中。

公开(公告)号：US20060084277A1

公开(公告)日：2006-04-20

申请号：US10533238

申请日：2003-10-27

申请人： Akira Nakashima ,  Miki Egami ,  Michio Komatsu ,  Yoshihiro Nakata ,  Ei Yano ,  Katsumi Suzuki

发明人： Akira Nakashima ,  Miki Egami ,  Michio Komatsu ,  Yoshihiro Nakata ,  Ei Yano ,  Katsumi Suzuki

IPC分类号： H01L21/31 ,  H01L21/469

CPC分类号： C09D183/02 ,  C08G77/08 ,  H01L21/02126 ,  H01L21/02203 ,  H01L21/02216 ,  H01L21/02282 ,  H01L21/02337 ,  H01L21/316 ,  H01L21/31695

摘要： The present invention relates to an amorphous silica-based coating film with a low specific dielectric constant of 2.5 or below and the Young's modulus of 6.0 GPa or more and having excellent hydrophobic property, and to a method of forming the same. A liquid composition containing a silicon compound obtained by hydrolyzing tetraalkyl ortho silicate (TAOS) and specific alkoxysilane (AS) in the presence of tetraalkyl ammonium hydroxide (TAAOH) is prepared. The liquid composition is then applied on a substrate, heated and cured to obtain a coating film. The coating film obtained as described has a smooth surface and also has specific micropores therein.

摘要翻译： 本发明涉及具有2.5以下的比介电常数低，6.0GPa以上的杨氏模量和疏水性优异的无定形二氧化硅系涂膜及其形成方法。 制备含有在四烷基氢氧化铵（TAAOH）存在下水解四烷基原硅酸盐（TAOS）和特定烷氧基硅烷（AS））得到的硅化合物的液体组合物。 然后将液体组合物涂布在基材上，加热固化，得到涂膜。 如上所述获得的涂膜具有光滑表面，并且其中也具有特定的微孔。

公开(公告)号：US20080011987A1

公开(公告)日：2008-01-17

申请号：US11665746

申请日：2005-10-11

申请人： Hiroki Arao ,  Miki Egami ,  Akira Nakashima ,  Michio Komatsu

发明人： Hiroki Arao ,  Miki Egami ,  Akira Nakashima ,  Michio Komatsu

IPC分类号： H01B3/20 ,  C04B41/50

CPC分类号： H01L21/02216 ,  C08L83/08 ,  C09C1/30 ,  C09C1/3081 ,  C09D183/02 ,  C09D183/04 ,  C23C18/1212 ,  C23C18/1295 ,  C23C18/14 ,  H01L21/02126 ,  H01L21/02282 ,  H01L21/316 ,  C08L2666/02

摘要： Disclosed is a coating liquid for forming an amorphous silica-based coating film having a low dielectric constant of 3.0 or below and low leakage current, and a method for preparing the coating liquid. The coating liquid is a liquid composition comprising (a) silicon compound obtained by hydrolyzing tetraalkyl orthosilicate (TAOS) and alkoxysilane (AS) in the presence of tetraalkyl ammonium hydroxide (TAAOH) and water, or a silicon compound obtained by hydrolyzing or partially hydrolyzing tetraalkyl orthosilicate (TAOS) in the presence of tetraalkyl ammonium hydroxide (TAAOH) and water, mixing the hydrolyzed or partially hydrolyzed product with alkoxysilane (AS) or a hydrolyzed or partially hydrolyzed product thereof, and hydrolyzing all or a portion of the mixture, (b) an organic solvent, and (c) water. The coating liquid is characterized in that a quantity of water contained in the liquid composition is in the range from 30 to 60% by weight.

摘要翻译： 公开了一种形成低介电常数为3.0以下，低漏电流的无定形二氧化硅系涂膜的涂布液及其制备方法。 涂布液是一种液体组合物，其包含（a）在四烷基氢氧化铵（TAAOH）和水的存在下水解四烷基原硅酸酯（TAOS）和烷氧基硅烷（AS）而获得的硅化合物，或通过水解或部分水解四烷基 在四烷基氢氧化铵（TAAOH）和水的存在下，将水解或部分水解的产物与烷氧基硅烷（AS）或其水解或部分水解产物混合，并水解所有或部分混合物，（b） ）有机溶剂，和（c）水。 涂布液的特征在于，液体组合物中所含的水的量为30〜60重量％。

公开(公告)号：US08062414B2

公开(公告)日：2011-11-22

申请号：US10533302

申请日：2003-10-27

申请人： Akira Nakashima ,  Miki Egami ,  Michio Komatsu ,  Yoshihiro Nakata ,  Ei Yano ,  Katsumi Suzuki

发明人： Akira Nakashima ,  Miki Egami ,  Michio Komatsu ,  Yoshihiro Nakata ,  Ei Yano ,  Katsumi Suzuki

IPC分类号： C04B41/50 ,  D06M15/643 ,  C09D183/04

CPC分类号： H01L21/02126 ,  C08G77/08 ,  C09D183/04 ,  H01L21/02216 ,  H01L21/02282 ,  H01L21/3122 ,  H01L21/316

摘要： The present invention relates to a coating liquid for forming an amorphous silica-based coating film with a low dielectric constant of 2.5 or below and the Young's modulus of 6.0 GPa or more and having excellent hydrophobic property, and to a method of preparing the same. The coating liquid may contain a silicon compound obtained by hydrolyzing tetraalkyl ortho silicate (TAOS) and specific alkoxysilane (AS) in the presence of tetraalkyl ammonium hydroxide (TAAOH), or may contain a silicon compound obtained by hydrolyzing or partially hydrolyzing tetraalkyl ortho silicate (TAOS) in the presence of tetraalkyl ammonium hydroxide (TAAOH), mixing the reaction product with specific alkoxysilane or a hydrolysate or a partial hydrolysate thereof, and hydrolyzing all or a portion of the mixture according to the necessity. In addition, the coating liquid is prepared by mixing components described above at a specific ratio and under specific process conditions.

摘要翻译： 本发明涉及一种低介电常数为2.5以下，杨氏模量为6.0GPa以上，疏水性优异的无定形二氧化硅系涂膜用涂布液及其制备方法。 涂布液可以含有通过在四烷基氢氧化铵（TAAOH）的存在下水解四烷基原硅酸盐（TAOS）和特定烷氧基硅烷（AS））而获得的硅化合物，或者可以含有通过水解或部分水解原硅酸四烷基酯 TAOS）在四烷基氢氧化铵（TAAOH）的存在下，将反应产物与特定的烷氧基硅烷或其水解产物或其部分水解产物混合，并根据需要水解全部或一部分混合物。 此外，通过以特定比例和特定工艺条件混合上述组分来制备涂布液。

公开(公告)号：US20100003181A1

公开(公告)日：2010-01-07

申请号：US12310486

申请日：2007-07-11

申请人： Miki Egami ,  Akira Nakashima ,  Michio Komatsu

发明人： Miki Egami ,  Akira Nakashima ,  Michio Komatsu

IPC分类号： C01B33/12 ,  H01L21/316

CPC分类号： C09D1/00 ,  C09D4/00 ,  H01L21/316 ,  C08G77/04

摘要： A method of forming on a substrate an amorphous silica-based coating film having a low dielectric constant of 3.0 or below and a film strength (Young's modulus) of 3.0 GPa or more, which comprises, as a typical one, the steps of; (a) coating on the substrate a liquid composition containing hydrolysate of an organic silicon compound or compounds hydrolyzed in the presence of tetraalkylammonium hydroxide (TAAOH); (b) setting the substrate in a chamber and then drying a coating film formed on the substrate at a temperature in the range from 25 to 340° C.; (c) heating the coating film at a temperature in the range from 105 to 450° C. with introduction of a superheated steam having such a temperature into the chamber, and (d) curing the coating film at a temperature in the range from 350 to 450° C. with introduction of a nitrogen gas into the chamber.

摘要翻译： 一种在基板上形成介电常数低于3.0或更低的无定形二氧化硅基涂层以及3.0GPa或更高的膜强度（杨氏模量）的方法，其中典型的步骤包括： （a）在基材上涂覆含有有机硅化合物的水解产物或在四烷基氢氧化铵（TAAOH））存在下水解的化合物的液体组合物; （b）将基板设置在室中，然后在25至340℃的温度范围内干燥形成在基板上的涂膜。 （c）在105至450℃的温度范围内加热涂膜，并将具有这种温度的过热蒸汽引入室中，和（d）在350℃的温度下固化涂膜 至450℃，同时将氮气引入室中。

公开(公告)号：US08686101B2

公开(公告)日：2014-04-01

申请号：US12086745

申请日：2006-12-15

申请人： Miki Egami ,  Hiroki Arao ,  Akira Nakashima ,  Michio Komatsu

发明人： Miki Egami ,  Hiroki Arao ,  Akira Nakashima ,  Michio Komatsu

IPC分类号： C08G77/08

CPC分类号： H01L21/316 ,  C01B33/12 ,  C08G77/50 ,  C09D183/14 ,  H01B3/08 ,  H01L21/02126 ,  H01L21/02216 ,  H01L21/02282 ,  H01L21/3122

摘要： A coating liquid for forming a low dielectric constant amorphous silica-based coating film with a dielectric constant of 3.0 or below and a film strength (Young's modulus) of 3.0 GPa or more, and also having a smooth surface with an excellent hydrophobicity. The coating liquid contains (1) a silicon compound obtained by hydrolyzing bis(trialkoxysilyl)alkane (BTASA) and alkoxysilane (AS) in the presence of tetraalkylammoniumhydroxide (TAAOH), or (2) a silicon compound obtained by hydrolyzing bis(trialkoxysilyl)alkane (BTASA), alkoxysilane (AS) and tetraalkylorthosilicate (TAOS) in the presence of tetraalkylammoniumhydroxide (TAAOH).

摘要翻译： 一种用于形成介电常数为3.0以下，膜强度（杨氏模量）为3.0GPa以上的低介电常数无定形二氧化硅系涂膜的涂布液，并且还具有疏水性优异的光滑表面。 涂布液含有（1）在四烷基氢氧化铵（TAAOH）存在下水解双（三烷氧基甲硅烷基）烷烃（BTASA）和烷氧基硅烷（AS））得到的硅化合物，或（2）通过水解双（三烷氧基甲硅烷基）烷烃获得的硅化合物 （BTASA），烷氧基硅烷（AS）和四烷基原硅酸盐（TAOS）在四烷基氢氧化铵（TAAOH）存在下。

公开(公告)号：US07998567B2

公开(公告)日：2011-08-16

申请号：US11665747

申请日：2005-10-11

申请人： Miki Egami ,  Hiroki Arao ,  Akira Nakashima ,  Michio Komatsu

发明人： Miki Egami ,  Hiroki Arao ,  Akira Nakashima ,  Michio Komatsu

IPC分类号： B32B3/26

CPC分类号： H01L21/02126 ,  C09D183/02 ,  C09D183/04 ,  H01L21/02203 ,  H01L21/02282 ,  H01L21/02351 ,  H01L21/3121 ,  Y10T428/249953

摘要： Disclosed is a coating liquid for forming a protective film having high film strength and a low specific dielectric constant for semiconductor processing, and a method for preparing the coating liquid. The coating liquid is a liquid composition comprising (a) silicon compound obtained by hydrolyzing tetraalkyl orthosilicate (TAOS) and alkoxysilane (AS) in the presence of tetraalkyl ammonium hydroxide (TAAOH) and water, or a silicon compound obtained by hydrolyzing or partially hydrolyzing tetraalkyl orthosilicate (TAOS) in the presence of tetraalkyl ammonium hydroxide (TAAOH) and water, mixing the hydrolyzed or partially hydrolyzed product with alkoxysilane (AS) or a hydrolyzed or partially hydrolyzed product thereof, and hydrolyzing all or a portion of the mixture, (b) an organic solvent, and (c) water. The coating liquid is characterized in that a quantity of water contained in the liquid composition is in the range from 35 to 65% by weight.

摘要翻译： 公开了一种用于形成用于半导体加工的具有高膜强度和低比介电常数的保护膜的涂布液，以及一种制备涂布液的方法。 涂布液是一种液体组合物，其包含（a）在四烷基氢氧化铵（TAAOH）和水的存在下水解四烷基原硅酸酯（TAOS）和烷氧基硅烷（AS）而获得的硅化合物，或通过水解或部分水解四烷基 在四烷基氢氧化铵（TAAOH）和水的存在下，将水解或部分水解的产物与烷氧基硅烷（AS）或其水解或部分水解产物混合，并水解所有或部分混合物，（b） ）有机溶剂，和（c）水。 涂布液的特征在于，液体组合物中含有的水的量在35至65重量％的范围内。

公开(公告)号：US20090061199A1

公开(公告)日：2009-03-05

申请号：US11665747

申请日：2005-10-11

申请人： Miki Egami ,  Hiroki Arao ,  Akira Nakashima ,  Michio Komatsu

发明人： Miki Egami ,  Hiroki Arao ,  Akira Nakashima ,  Michio Komatsu

IPC分类号： B32B3/26 ,  C09D7/12

CPC分类号： H01L21/02126 ,  C09D183/02 ,  C09D183/04 ,  H01L21/02203 ,  H01L21/02282 ,  H01L21/02351 ,  H01L21/3121 ,  Y10T428/249953

摘要： Disclosed is a coating liquid for forming a protective film having high film strength and a low specific dielectric constant for semiconductor processing, and a method for preparing the coating liquid. The coating liquid is a liquid composition comprising (a) silicon compound obtained by hydrolyzing tetraalkyl orthosilicate (TAOS) and alkoxysilane (AS) in the presence of tetraalkyl ammonium hydroxide (TAAOH) and water, or a silicon compound obtained by hydrolyzing or partially hydrolyzing tetraalkyl orthosilicate (TAOS) in the presence of tetraalkyl ammonium hydroxide (TAAOH) and water, mixing the hydrolyzed or partially hydrolyzed product with alkoxysilane (AS) or a hydrolyzed or partially hydrolyzed product thereof, and hydrolyzing all or a portion of the mixture, (b) an organic solvent, and (c) water. The coating liquid is characterized in that a quantity of water contained in the liquid composition is in the range from 35 to 65% by weight.

摘要翻译： 公开了一种用于形成用于半导体加工的具有高膜强度和低比介电常数的保护膜的涂布液，以及一种制备涂布液的方法。 涂布液是一种液体组合物，其包含（a）在四烷基氢氧化铵（TAAOH）和水的存在下水解四烷基原硅酸酯（TAOS）和烷氧基硅烷（AS）而获得的硅化合物，或通过水解或部分水解四烷基 在四烷基氢氧化铵（TAAOH）和水的存在下，将水解或部分水解的产物与烷氧基硅烷（AS）或其水解或部分水解产物混合，并水解所有或部分混合物，（b） ）有机溶剂，和（c）水。 涂布液的特征在于，液体组合物中含有的水的量在35至65重量％的范围内。

公开(公告)号：US20090025609A1

公开(公告)日：2009-01-29

申请号：US12086745

申请日：2006-12-15

申请人： Miki Egami ,  Hiroki Arao ,  Akira Nakashima ,  Michio Komatsu

发明人： Miki Egami ,  Hiroki Arao ,  Akira Nakashima ,  Michio Komatsu

IPC分类号： C09D7/12 ,  C07F7/18

CPC分类号： H01L21/316 ,  C01B33/12 ,  C08G77/50 ,  C09D183/14 ,  H01B3/08 ,  H01L21/02126 ,  H01L21/02216 ,  H01L21/02282 ,  H01L21/3122

摘要： A coating liquid for forming a low dielectric constant amorphous silica-based coating film with a dielectric constant of 3.0 or below and a film strength (Young's modulus) of 3.0 GPa or more, and also having a smooth surface with an excellent hydrophobicity. The coating liquid contains (1) a silicon compound obtained by hydrolyzing bis(trialcoxysilyl)alkane (BTASA) and alcoxysilane (AS) in the presence of tetraalkylammoniumhydroxide (TAAOH), or (2) a silicon compound obtained by hydrolyzing bis(trialcoxysilyl)alkane (BTASA), alcoxysilane (AS) and tetraalkylorthosilicate (TAOS) in the presence of tetraalkylammoniumhydroxide (TAAOH).

摘要翻译： 一种用于形成介电常数为3.0以下，膜强度（杨氏模量）为3.0GPa以上的低介电常数无定形二氧化硅系涂膜的涂布液，并且还具有疏水性优异的光滑表面。 涂布液含有（1）在四烷基氢氧化铵（TAAOH）存在下水解双（试剂 - 甲硅烷基）烷烃（BTASA）和烷氧基硅烷（AS））得到的硅化合物，或（2）通过水解双（试剂 - 甲硅烷基）烷烃获得的硅化合物 （BTASA），烷氧基硅烷（AS）和四烷基原硅酸盐（TAOS）在四烷基氢氧化铵（TAAOH）存在下。

公开(公告)号：US06599846B2

公开(公告)日：2003-07-29

申请号：US09914418

申请日：2001-08-28

申请人： Michio Komatsu ,  Akira Nakashima ,  Miki Egami ,  Ryo Muraguchi

发明人： Michio Komatsu ,  Akira Nakashima ,  Miki Egami ,  Ryo Muraguchi

IPC分类号： H01L2131

CPC分类号： H01L21/316

摘要： The present invention provides a method for forming a silica-containing film with a low-dielectric constant of 3 or less on a semiconductor substrate steadily, which comprises steps of (a) applying a coating liquid for forming the silica-containing film with the low-dielectric constant onto the semiconductor substrate, (b) heating the thus coated film at 50 to 350° C., and then (c) curing the thus treated film at 350 to 450° C. in an inert-gas atmosphere containing 500 to 15,000 ppm by volume of oxygen, and also provides a semiconductor substrate having a silica-containing film formed by the above method. The above step (b) for the thermal treatment is preferably conducted at 150 to 350° C. for 1 to 3 minutes in an air atmosphere. Also, the above curing step (c) is preferably conducted by placing the semiconductor substrate on a hot plate kept at 350 to 450° C. According to the present invention, a semiconductor substrate coated with a silica-containing film having characteristics of a low-dielectric constant of 3 or less, a low moisture adsorptivity and high film strength without causing any damage to the metal wiring arranged on the substrate, can be obtained steadily.

摘要翻译： 本发明提供一种在半导体基板上稳定地形成具有3以下的低介电常数的含二氧化硅的膜的方法，该方法包括以下步骤：（a）将形成含二氧化硅的膜的涂布液涂布到低 （b）在50至350℃下加热涂覆的膜，然后（c）在350至450℃下在含有500至500℃的惰性气体气氛中固化如此处理的膜 15000体积ppm的氧，并且还提供具有通过上述方法形成的含二氧化硅的半导体衬底。用于热处理的上述步骤（b）优选在150-350℃下进行1至3分钟 在空气气氛中。 此外，上述固化步骤（c）优选通过将半导体衬底放置在保持在350至450℃的热板上来进行。根据本发明，涂覆了具有低特性的含二氧化硅的膜的半导体衬底 - 可以稳定地获得3或更小的吸湿性和低膜强度，而不会对布置在基底上的金属布线造成任何损坏。