JP2001002990A - Composition for forming film, formation of film and low- density film - Google Patents

Abstract

PROBLEM TO BE SOLVED: To obtain a composition for forming a film having excellent dielectric constant characteristics, mechanical strength, etc. SOLUTION: This composition for forming a film comprises (A) a silane compound which is a hydrolyzate and a condensate or either of the hydrolyzate and the condensate of at least one compound selected from the group consisting of a compound of the formula, R1aSi(OR2)4-a (R1 is a hydrogen atom, a fluorine atom or a monofunctional organic group; R2 is a monofunctional organic group; and (a) is an integer of 0-2) and a compound of the formula, R3b(R4O)3-bSi-(R7)d- Si(OR5)3-cR6c (R3, R4, R5 and R6 are each the same or different and a monofunctional organic group; (b) and (c) are each the same or different and an integer of 0-2; R7 is an oxygen atom or a group of -(CH2)n; (n) is 1-6; and (d) is 0 or 1), (B) a latent basic catalyst and (C) a compound which is compatible or dispersible in the component A and has 250-450 deg.C decomposition temperature.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a film-forming composition, and more particularly, to a film-forming composition excellent in dielectric properties, mechanical properties, storage stability and the like, and obtained by curing the composition. Membrane to be used.

[0002]

Conventionally, as an interlayer insulating film in semiconductor devices and the like, silica is formed Te than by a vacuum process such as CVD (SiO ₂₎ film is often used. And in recent years,
In order to form a more uniform interlayer insulating film, S
A coating-type insulating film called a OG (Spin on Glass) film, which is mainly composed of a hydrolysis product of tetraalkoxylan, has also been used. Also, with the high integration of semiconductor elements and the like, an interlayer insulating film having a low dielectric constant, which is mainly composed of organopolysiloxane and is called organic SOG, has been developed. However, with higher integration of semiconductor devices and the like, better electrical insulation between conductors is required, and therefore, an interlayer insulating film material having a lower dielectric constant has been required.

[0003] Japanese Patent Application Laid-Open No. 6-181201 discloses a coating composition for forming an insulating film having a lower dielectric constant as an interlayer insulating film material. Such a coating composition has a low water absorption and is intended to provide an insulating film of a semiconductor device having excellent crack resistance, and the constitution is
Titanium, zirconium, niobium and tantalum; an organometallic compound containing at least one element selected from the group consisting of polycondensation of an organosilicon compound having at least one alkoxy group in the molecule; It is a coating type composition for forming an insulating film mainly comprising an oligomer. However, the dielectric constant of the conventional inorganic interlayer insulating film material is 3.0 or more, which is insufficient for high integration.

[0004] It is an object of the present invention to provide a material for an interlayer insulating film which is excellent in balance among dielectric constant characteristics, mechanical characteristics, storage stability and the like. Hereinafter, the present invention will be described in detail.

According to the present invention, (A) a silane compound represented by the following general formula (1): R ¹ _a Si (OR ² ) _4-a (1) wherein R ¹ is a hydrogen atom; A fluorine atom or a monovalent organic group, R ² represents a monovalent organic group, a represents an integer of 0 to 2) and a compound represented by the following general formula (2): R ³ _b (R _{^{4 O) 3-b Si- (}} R 7) d -Si (oR 5) 3-c R 6 c ····· (2) (R 3, R 4, R 5 and R ⁶ be the same or different Each represents a monovalent organic group; b and c may be the same or different and each represents a number of 0 to 2; and R ⁷ is represented by an oxygen atom or — (CH 2) _n —. And n
Represents 1 to 6, and d represents 0 or 1. Or at least one of a hydrolyzate and a condensate of at least one compound selected from the group consisting of (B) a latent base catalyst and (C) a component which is compatible or dispersed with the component (A), and has a boiling point or decomposition. It is intended to provide a film-forming composition containing a compound having a temperature of 250 to 450 ° C., a method for producing a film using the film, and a film.

Component (A) In the general formula (1), examples of the monovalent organic group include an alkyl group, an aryl group, an allyl group, and a glycidyl group. Here, examples of the alkyl group include a methyl group, an ethyl group, a propyl group, a butyl group and the like, preferably having 1 to 5 carbon atoms, and these alkyl groups may be chain-like or branched, Further, a hydrogen atom may be substituted with a fluorine atom or the like. General formula (1)
Examples of the aryl group include a phenyl group and a naphthyl group. Specific examples of the compound represented by the general formula (1) include n = 0 in the general formula (1).
Examples of the compound include tetramethoxysilane, tetraethoxysilane, tetra-n-propoxysilane, tetra-
iso-propoxysilane, tetra-n-butoxysilane, tetra-sec-butoxysilane, tetra-ter
Examples thereof include t-butoxysilane and tetraphenoxysilane. Specific examples of the compound where n = 1 in the general formula (1) include methyltrimethoxysilane, methyltriethoxysilane, methyltri-n-propoxysilane, methyltri-iso-propoxysilane, methyltri-n-butoxysilane, methyltrimethoxysilane. -Sec-butoxysilane, methyltri-tert-butoxysilane, methyltriphenoxysilane, ethyltrimethoxysilane, ethyltriethoxysilane, ethyltri-n-
Propoxysilane, ethyltri-iso-propoxysilane, ethyltri-n-butoxysilane, ethyltri-
sec-butoxysilane, ethyltri-tert-butoxysilane, ethyltriphenoxysilane, n-propyltrimethoxysilane, n-propyltriethoxysilane, n-propyltri-n-propoxysilane, n-propyltri-iso-propoxysilane , N-propyltri-n-butoxysilane, n-propyltri-sec
-Butoxysilane, n-propyltri-tert-butoxysilane, n-propyltriphenoxysilane, i-
Propyltrimethoxysilane, i-propyltriethoxysilane, i-propyltri-n-propoxysilane,
i-propyltri-iso-propoxysilane, i-propyltri-n-butoxysilane, i-propyltri-
sec-butoxysilane, i-propyltri-tert
-Butoxysilane, i-propyltriphenoxysilane, n-butyltrimethoxysilane, n-butyltriethoxysilane, n-butyltri-n-propoxysilane, n-butyltri-iso-propoxysilane, n-
Butyltri-n-butoxysilane, n-butyltri-s
ec-butoxysilane, n-butyltri-tert-butoxysilane, n-butyltriphenoxysilane, se
c-butyltrimethoxysilane, sec-butyl-i-
Triethoxysilane, sec-butyl-tri-n-propoxysilane, sec-butyl-tri-iso-propoxysilane, sec-butyl-tri-n-butoxysilane, sec-butyl-tri-sec-butoxysilane,
sec-butyl-tri-tert-butoxysilane, s
ec-butyl-triphenoxysilane, t-butyltrimethoxysilane, t-butyltriethoxysilane, t-butyl
Butyl tri-n-propoxy silane, t-butyl tri-iso-propoxy silane, t-butyl tri-n-butoxy silane, t-butyl tri sec-butoxy silane, t-butyl tri-tert-butoxy silane, t-butyl
Butyltriphenoxysilane, phenyltrimethoxysilane, phenyltriethoxysilane, phenyltri-n
-Propoxysilane, phenyltri-iso-propoxysilane, phenyltri-n-butoxysilane, phenyltri-sec-butoxysilane, phenyltri-te
Specific examples of the compound in which n = 2 in the general formula (1) include rt-butoxysilane, phenyltriphenoxysilane, and the like; dimethyldimethoxysilane, dimethyldiethoxysilane, dimethyl-di-n-propoxysilane,
Dimethyl-di-iso-propoxysilane, dimethyl-
Di-n-butoxysilane, dimethyl-di-sec-butoxysilane, dimethyl-di-tert-butoxysilane, dimethyldiphenoxysilane, diethyldimethoxysilane, diethyldiethoxysilane, diethyl-di-n
-Propoxysilane, diethyl-di-iso-propoxysilane, diethyl-di-n-butoxysilane, diethyl-di-sec-butoxysilane, diethyl-di-te
rt-butoxysilane, diethyldiphenoxysilane,
Di-n-propyldimethoxysilane, di-n-propyldiethoxysilane, di-n-propyl-di-n-propoxysilane, di-n-propyl-di-iso-propoxysilane, di-n-propyl-di -N-butoxysilane, di-n-propyl-di-sec-butoxysilane,
Di-n-propyl-di-tert-butoxysilane, di-n-propyl-di-phenoxysilane, di-iso-
Propyldimethoxysilane, di-iso-propyldiethoxysilane, di-iso-propyl-di-n-propoxysilane, di-iso-propyl-di-iso-propoxysilane, di-iso-propyl-di-n-butoxy Silane, di-iso-propyl-di-sec-butoxysilane, di-iso-propyl-di-tert-butoxysilane, di-iso-propyl-di-phenoxysilane, di-n-butyldimethoxysilane, di-n -Butyldiethoxysilane, di-n-butyl-di-n-propoxysilane, di-n-butyl-di-iso-propoxysilane, di-n-butyl-di-n-butoxysilane, di-n-butyl -Di-sec-butoxysilane, di-n-
Butyl-di-tert-butoxysilane, di-n-butyl-di-phenoxysilane, di-sec-butyldimethoxysilane, di-sec-butyldiethoxysilane, di-sec-butyl-di-n-propoxysilane, Di-s
ec-butyl-di-iso-propoxysilane, di-s
ec-butyl-di-n-butoxysilane, di-sec-
Butyl-di-sec-butoxysilane, di-sec-butyl-di-tert-butoxysilane, di-sec-butyl-di-phenoxysilane, di-tert-butyldimethoxysilane, di-tert-butyldiethoxysilane, Di-tert-butyl-di-n-propoxysilane, di-tert-butyl-di-iso-propoxysilane, di-tert-butyl-di-n-butoxysilane, di-tert-butyl-di-sec-butoxy Silane, di-tert-butyl-di-tert-butoxysilane, di-tert-butyl-di-phenoxysilane,
Diphenyldimethoxysilane, diphenyl-di-ethoxysilane, diphenyl-di-n-propoxysilane, diphenyl-di-iso-propoxysilane, diphenyl-di-n-butoxysilane, diphenyl-di-sec-
Butoxysilane, diphenyl-di-tert-butoxysilane, diphenyldiphenoxysilane, divinyltrimethoxysilane, γ-aminopropyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ-glycidoxypropyltrimethoxysilane, γ- Glycidoxypropyltriethoxysilane, γ-trifluoropropyltrimethoxysilane, γ-trifluoropropyltriethoxysilane and the like can be mentioned. These may be used alone or in combination of two or more.

Among the compounds represented by the general formula (1), tetraalkoxysilanes such as tetramethoxysilane and tetraethoxysilane; alkyltrialkoxysilanes such as methyltrimethoxysilane and methyltriethoxysilane; Dialkyldialkoxysilanes such as ethoxysilane and dimethyldimethoxysilane are preferred. In the general formula (2), examples of the monovalent organic group include the same organic groups as those in the general formula (1). Examples of the divalent organic group represented by R ⁷ in the general formula (2) include a methylene group and an alkylene group having 2 to 6 carbon atoms. In the general formula (2), R
Compounds in which ⁷ is an oxygen atom include hexamethoxydisiloxane, hexaethoxydisiloxane, hexaphenoxydisiloxane, 1,1,1,3,3-pentamethoxy-3-methyldisiloxane, 1,1,1,3 , 3-pentaethoxy-3-methyldisiloxane, 1,1,1,
3,3-pentamethoxy-3-phenyldisiloxane,
1,1,1,3,3-pentaethoxy-3-phenyldisiloxane, 1,1,3,3-tetramethoxy-1,3
-Dimethyldisiloxane, 1,1,3,3-tetraethoxy-1,3-dimethyldisiloxane, 1,1,3,3
-Tetramethoxy-1,3-diphenyldisiloxane,
1,1,3,3-tetraethoxy-1,3-diphenyldisiloxane, 1,1,3-trimethoxy-1,3,3
-Trimethyldisiloxane, 1,1,3-triethoxy-1,3,3-trimethyldisiloxane, 1,1,3-
Trimethoxy-1,3,3-triphenyldisiloxane, 1,1,3-triethoxy-1,3,3-triphenyldisiloxane, 1,3-dimethoxy-1,1,3,3
3-tetramethyldisiloxane, 1,3-diethoxy-
1,1,3,3-tetramethyldisiloxane, 1,3-
Examples thereof include dimethoxy-1,1,3,3-tetraphenyldisiloxane and 1,3-diethoxy-1,1,3,3-tetraphenyldisiloxane. Of these, hexamethoxydisiloxane, hexaethoxydisiloxane, 1,1,3,3-tetramethoxy-1,1
3-dimethyldisiloxane, 1,1,3,3-tetraethoxy-1,3-dimethyldisiloxane, 1,1,3,
3-tetramethoxy-1,3-diphenyldisiloxane, 1,3-dimethoxy-1,1,3,3-tetramethyldisiloxane, 1,3-diethoxy-1,1,3,3
-Tetramethyldisiloxane, 1,3-dimethoxy-
1,1,3,3-tetraphenyldisiloxane, 1,3
-Diethoxy-1,1,3,3-tetraphenyldisiloxane and the like can be mentioned as preferred examples.
In the general formula (2), examples of the compound in which d is 0 include hexamethoxydisilane, hexaethoxydisilane, hexaphenixidisilane, 1,1,1,2,2-pentamethoxy-2-methyldisilane, 1,1,1 , 2,2-pentaethoxy-2-methyldisilane, 1,1,1,2,2-
Pentamethoxy-2-phenyldisilane, 1,1,1,
2,2-pentaethoxy-2-phenyldisilane, 1,
1,2,2-tetramethoxy-1,2-dimethyldisilane, 1,1,2,2-tetraethoxy-1,2-dimethyldisilane, 1,1,2,2-tetramethoxy-1,2
-Diphenyldisilane, 1,1,2,2-tetraethoxy-1,2-diphenyldisilane, 1,1,2-trimethoxy-1,2,2-trimethyldisilane, 1,1,2
-Triethoxy-1,2,2-trimethyldisilane,
1,1,2-trimethoxy-1,2,2-triphenyldisilane, 1,1,2-triethoxy-1,2,2-triphenyldisilane, 1,2-dimethoxy-1,1,1
2,2-tetramethyldisilane, 1,2-diethoxy-
1,1,2,2-tetramethyldisilane, 1,2-dimethoxy-1,1,2,2-tetraphenyldisilane,
And 1,2-diethoxy-1,1,2,2-tetraphenyldisilane, R ⁷ in the general formula (2) is - (CH
2) As compounds of the group represented by n-, bis (hexamethoxysilyl) methane, bis (hexaethoxysilyl)
Methane, bis (hexaphenoxysilyl) methane, bis (dimethoxymethylsilyl) methane, bis (diethoxymethylsilyl) methane, bis (dimethoxyphenylsilyl) methane, bis (diethoxyphenylsilyl) methane, bis (methoxydimethylsilyl) Methane, bis (ethoxydimethylsilyl) methane, bis (methoxydiphenylsilyl) methane, bis (ethoxydiphenylsilyl) methane, bis (hexamethoxysilyl) ethane, bis (hexaethoxysilyl) ethane, bis (hexaphenoxysilyl) ethane, Bis (dimethoxymethylsilyl) ethane, bis (diethoxymethylsilyl) ethane,
Bis (dimethoxyphenylsilyl) ethane, bis (diethoxyphenylsilyl) ethane, bis (methoxydimethylsilyl) ethane, bis (ethoxydimethylsilyl) ethane, bis (methoxydiphenylsilyl) ethane, bis (ethoxydiphenylsilyl) ethane, 1 1,3-bis (hexamethoxysilyl) propane, 1,3-bis (hexaethoxysilyl) propane, 1,3-bis (hexaphenoxysilyl) propane, 1,3-bis (dimethoxymethylsilyl) propane, 1,3 -Bis (diethoxymethylsilyl) propane, 1,3-bis (dimethoxyphenylsilyl) propane, 1,3-bis (diethoxyphenylsilyl) propane, 1,3-bis (methoxydimethylsilyl) propane, 1,3 -Bis (ethoxydimethylsilyl) propane 1,3-bis (methoxydiphenylsilyl) propane, 1,3-bis (ethoxydiphenylsilyl) propane can be cited. Of these, hexamethoxydisilane, hexaethoxydisilane, hexaphenixidisilane, 1,1,2,2-tetramethoxy-1,2-dimethyldisilane, 1,1,
2,2-tetraethoxy-1,2-dimethyldisilane,
1,1,2,2-tetramethoxy-1,2-diphenyldisilane, 1,1,2,2-tetraethoxy-1,2-
Diphenyldisilane, 1,2-dimethoxy-1,1,1
2,2-tetramethyldisilane, 1,2-diethoxy-
1,1,2,2-tetramethyldisilane, 1,2-dimethoxy-1,1,2,2-tetraphenyldisilane,
1,2-diethoxy-1,1,2,2-tetraphenyldisilane, bis (hexamethoxysilyl) methane, bis (hexaethoxysilyl) methane, bis (dimethoxymethylsilyl) methane, bis (diethoxymethylsilyl)
Methane, bis (dimethoxyphenylsilyl) methane, bis (diethoxyphenylsilyl) methane, bis (methoxydimethylsilyl) methane, bis (ethoxydimethylsilyl) methane, bis (methoxydiphenylsilyl) methane, bis (ethoxydiphenylsilyl) methane Can be mentioned as a preferable example.

In the film-forming composition of the present invention, the compound represented by the general formula (1) and the compound represented by the general formula (2) are preferably used in combination of two or more, and particularly, tetraalkoxy. It is particularly preferable to use a combination of three kinds of silane, alkyl trialkoxy silane and dialkyl dialkoxy silane in view of heat resistance, dielectric properties and mechanical properties. In the present invention, the use ratio of tetraalkoxysilane / alkyl trialkoxysilane / dialkylalkoxysilane is 10 to 70/100.
~ 0/0 ~ 30 is preferred. When the compound represented by the general formula (1) and the compound represented by the general formula (2) are hydrolyzed and partially condensed, the compounds represented by R ² O—, R ⁴ O— and R ⁵ O— 0.3 to 5.0 per mole of the group
It is preferable to use moles of water, and it is particularly preferable to add 0.5 to 2.0 moles of water. When the amount of water to be added is within the range of 0.3 to 5.0 mol, there is no possibility that the uniformity of the coating film is reduced, and the storage stability of the film-forming composition is reduced. Is also less. When the component (A) is a partial condensate of a compound selected from the group consisting of the compound represented by the general formula (1) and the compound represented by the general formula (2), the polystyrene equivalent weight average molecular weight is 500 It is preferably from 100,000 to 100,000.

Component (B) The latent base catalyst that can be used in the present invention is capable of generating a base upon external stimulus. As the external stimulus, ultraviolet rays and heat are preferred. As latent base catalysts, orthonitrobenzyl carbamates, α,
α-dimethyl-3,5-dimethoxybenzyl carbamates, acyloxyiminos and the like can be exemplified. In addition, hydrazine as a base generated by light,
Tetramethylenediamine, toluenediamine, diaminodiphenylmethane, hexamethyltetraamine, ammonia, methylamine, ethylamine, propylamine,
Butylamine, hexylamine, cyclohexylamine, decylamine, cetylamine, piperidine, piperazine and the like. More specifically, [[(2-nitrobenzyl) oxy] carbonyl] methylamine,
[[(2-nitrobenzyl) oxy] carbonyl] propylamine, [[(2-nitrobenzyl) oxy] carbonyl] hexylamine, [[(2-nitrobenzyl)
Oxy] carbonyl] cyclohexylamine, [[(2
-Nitrobenzyl) oxy] carbonyl] aniline,
[[(2-nitrobenzyl) oxy] carbonyl] piperidine, [[(2-nitrobenzyl) oxy] carbonyl] hexamethylenediamine, [[(2-nitrobenzyl) oxy] carbonyl] phenylenediamine,
[[(2-nitrobenzyl) oxy] carbonyl] toluenediamine, [[(2-nitrobenzyl) oxy] carbonyl] diaminodiphenylmethane, [[(2-nitrobenzyl) oxy] carbonyl] piperazine,
[[(2,6-dinitrobenzyl) oxy] carbonyl] methylamine, [[(2,6-dinitrobenzyl) oxy
Oxy] carbonyl] propylamine, [[(2,6-
[Dinitrobenzyl) oxy] carbonyl] hexylamine, [[(2,6-dinitrobenzyl) oxy] carbonyl] cyclohexylamine, [[(2,6-dinitrobenzyl) oxy] carbonyl] aniline, [[(2,
6-dinitrobenzyl) oxy] carbonyl] piperidine, [[(2,6-dinitrobenzyl) oxy] carbonyl] hexamethylenediamine, [[(2,6-dinitrobenzyl) oxy] carbonyl] phenylenediamine, [[(2 , 6-dinitrobenzyl) oxy] carbonyl] toluenediamine, [[(2,6-dinitrobenzyl) oxy] carbonyl] diaminodiphenylmethane, [[(2,6-dinitrobenzyl) oxy] carbonyl] piperazine, [[(α , Α-dimethyl-3,5-
[Dimethoxybenzyl) oxy] carbonylmethylamine, [[(α, α-dimethyl-3,5-dimethoxybenzyl) oxy] carbonylpropylamine, [[(α,
α-dimethyl-3,5-dimethoxybenzyl) oxy]
Carbonylhexylamine, [[(α, α-dimethyl-
3,5-dimethoxybenzyl) oxy] carbonylcyclohexylamine, [[(α, α-dimethyl-3,5-
Dimethoxybenzyl) oxy] carbonylaniline,
[[(Α, α-dimethyl-3,5-dimethoxybenzyl) oxy] carbonylpiperidine, [[(α, α-dimethyl-3,5-dimethoxybenzyl) oxy] carbonylhexamethylenediamine, [[(α, α -Dimethyl-3,5-dimethoxybenzyl) oxy] carbonylphenylenediamine, [[(α, α-dimethyl-3,5-
[Dimethoxybenzyl) oxy] carbonyltoluenediamine, [[(α, α-dimethyl-3,5-dimethoxybenzyl) oxy] carbonyldiaminodiphenylmethane, [[(α, α-dimethyl-3,5-dimethoxybenzyl) oxy] carbonyl Piperazine, propionyl acetophenone oxime, propionyl benzophenone oxime, propionyl acetone oxime, butyryl acetophenone oxime, butyryl benzophenone oxime, butyryl acetone oxime, adipoyl acetophenone oxime, adipoyl benzophenone oxime, adipoyl acetone oxime, acroyl acetophenone Oxime, acroylbenzophenone oxime, acroylacetone oxime and the like. Among them, [[(2-nitrobenzyl) oxy] carbonyl] cyclohexylamine, [[(2-nitrobenzyl) oxy] carbonyl] hexamethylenediamine, [(α, α
-Dimethyl-3,5-dimethoxybenzyl) oxy] carbonylhexamethylenediamine. Also,
A sensitizer can be added as needed. The amount of the component (B) used is the component (A) (in terms of a completely hydrolyzed condensate).
For 100 parts by weight, usually 0.001 to 50 parts by weight,
Preferably it is 0.01 to 20 parts by weight. In the present invention, the completely hydrolyzed condensate is defined as -O in component (A).
A group represented by R ² , —OR ⁴ , or —OR ⁵ is hydrolyzed to 100% to form an OH group, which is completely condensed.

Component (C) In the present invention, the compound having a boiling point or decomposition temperature of 250 to 450 ° C., which is compatible or dispersed with the component (A), has a polyalkylene oxide structure,
(Meth) acrylate polymers, polyesters,
Examples thereof include polycarbonate and polyanhydride. In the present invention, the boiling point and the decomposition temperature refer to the temperature at 1 atm. Compound having a polyalkylene oxide structure Here, examples of the polyalkylene oxide structure include a polyethylene oxide structure, a polypropylene oxide structure, a polytetramethylene oxide structure, and a polybutylene oxide structure. Specifically, polyoxyethylene alkyl ether, polyoxyethylene alkylphenyl ether, polyoxyethylene sterol ether, polyoxyethylene lanolin derivative, ethylene oxide derivative of alkylphenol formalin condensate, polyoxyethylene polyoxypropylene block copolymer, polyoxyethylene polyoxypropylene block copolymer Ether-type compounds such as oxyethylene polyoxypropylene alkyl ether, ether-type compounds such as polyoxyethylene glycerin fatty acid ester, polyoxyethylene sorbitan fatty acid ester, polyoxyethylene sorbitol fatty acid ester, polyoxyethylene fatty acid alkanolamide sulfate, polyethylene Glycol fatty acid esters, ethylene glycol fatty acid esters, fatty acid monoglycerides, It can be mentioned Li glycerol fatty acid esters, sorbitan fatty acid esters, propylene glycol fatty acid esters, ether-ester type compounds such as sucrose fatty acid esters and the like. As the component (C), a polyoxyalkylene block copolymer such as a polyoxyethylene polyoxypropylene block copolymer is preferable. Examples of the polyoxyethylene polyoxypropylene block copolymer include compounds having the following block structures. -(A) n- (B) m--(A) n- (B) m- (A) l- (where A is a group represented by -CH2CH2O-, and B is-
A group represented by CH2CH (CH3) O-, wherein n is 1 to
90, m is a number from 10 to 99, and l is a number from 0 to 90)

(Meth) acrylate polymer In the present invention, the acrylate and methacrylate constituting the acrylic polymer include alkyl acrylate, alkyl methacrylate, alkoxyalkyl acrylate, alkyl methacrylate. And methacrylic acid alkoxyalkyl esters. Examples of the alkyl acrylate include methyl acrylate, ethyl acrylate, n-propyl acrylate, isopropyl acrylate, n-butyl acrylate, isobutyl acrylate,
Examples of alkyl esters having 1 to 6 carbon atoms, such as pentyl acrylate and hexyl acrylate, and alkyl methacrylates include methyl methacrylate, ethyl methacrylate, n-propyl methacrylate, isopropyl methacrylate, n-butyl methacrylate, and methacrylic acid. Isobutyl acid,
C1-6 alkyl esters such as butyl methacrylate, pentyl methacrylate, hexyl methacrylate,
Examples of the alkoxyalkyl acrylate include methoxymethyl acrylate and ethoxyethyl acrylate, and examples of the alkoxyalkyl methacrylate include methoxymethyl methacrylate and ethoxyethyl methacrylate. Among these, it is preferable to use alkyl methacrylate, and particularly preferable to use ethyl methacrylate, isobutyl methacrylate, and the like.

In the present invention, the acrylic polymer is preferably formed by copolymerizing a monomer having an alkoxysilyl group with the above monomer. Examples of the monomer having an alkoxysyl group include 3- (trimethoxysilyl) propyl methacrylate, 3- (triethoxysilyl) propyl methacrylate, 3- [tri (methoxyethoxy) silyl] propyl methacrylate, and 3- (methacrylic acid). Methyldimethoxysilyl) propyl, 3- (methyldiethoxysilyl) propyl methacrylate and the like can be mentioned. The monomer having an alkoxysilyl group is usually contained in a proportion of 0.5 to 10 mol%, preferably 1 to 7 mol%, in all the monomers constituting the acrylic polymer. In the present invention, the acrylic polymer may be copolymerized with not more than 40 mol% of a radical polymerizable monomer other than the above-mentioned acrylate, methacrylate and monomer having an alkoxysilyl group. Examples of the radical polymerizable monomer include unsaturated carboxylic acids such as acrylic acid and methacrylic acid, N, N-dimethylacrylamide, N, N-
Examples include unsaturated amides such as dimethyl methacrylamide, unsaturated nitriles such as acrylonitrile, unsaturated ketones such as methyl vinyl ketone, and aromatic compounds such as styrene and α-methylstyrene. In the present invention, the number average molecular weight in terms of polystyrene of the acrylic polymer is 1,000 to 100,000, preferably 1,000 to 100,000.
20,000. Polycondensates of polyester hydroxycarboxylic acids, ring-opening polymers of lactones, polycondensates of aliphatic polyols and aliphatic polycarboxylic acids and the like can be mentioned. Polycarbonate Polycondensates of carbonic acid and alkylene glycol, such as polyethylene carbonate, polypropylene carbonate, polytrimethylene carbonate, polytetramethylene carbonate, polypentamethylene carbonate, and polyhexamethylene carbonate, can be given. Examples include polycondensates of dicarboxylic acids such as polyanhydride polymalonyl oxide, polyadipoyl oxide, polypimeloyl oxide, polysuberoyl oxide, polyazelayl oxide, and polysebacoil oxide. Also,
As the component (B), poly (N-vinylacetamide), poly (N-vinylpyrrolidone), poly (2-vinylacetamide)
Examples thereof include vinylamide polymers such as methyl-2-oxazoline) and poly (N, N-dimethylacrylamide), and styrene polymers such as polystyrene, polymethylstyrene, and polyα-methylstyrene.

In the present invention, as the component (C), it is preferable to use a compound having an alkylene oxide structure or an acrylate polymer, and it is particularly preferable to use a compound having an alkylene oxide structure. The amount of the component (C) to be used is generally 1 to 80% by weight, preferably 5 to 65% by weight, based on the component (A). When the use ratio of the component (C) is 1% by weight or less, the effect of lowering the dielectric constant is small, and when it is 80% by weight or more, the mechanical strength decreases.

Component (D) In the present invention, the above components are usually used by dissolving them in an organic solvent. As the organic solvent used in the present invention, examples of the organic solvent used in the present invention include n-pentane, i-pentane, n-hexane, i-hexane, n-heptane,
i-heptane, 2,2,4-trimethylpentane, n-
Aliphatic hydrocarbon solvents such as octane, i-octane, cyclohexane, and methylcyclohexane; benzene, toluene, xylene, ethylbenzene, trimethylbenzene, methylethylbenzene, n-propylbenzene, i
Aromatic hydrocarbon solvents such as -propylbenzene, diethylbenzene, i-butylbenzene, triethylbenzene, di-i-propylbenzene, n-amylnaphthalene, trimethylbenzene; methanol, ethanol, n-propanol, i-propanol, n -Butanol, i-
Butanol, sec-butanol, t-butanol, n
-Pentanol, i-pentanol, 2-methylbutanol, sec-pentanol, t-pentanol, 3-
Methoxybutanol, n-hexanol, 2-methylpentanol, sec-hexanol, 2-ethylbutanol, sec-heptanol, heptanol-3, n-
Octanol, 2-ethylhexanol, sec-octanol, n-nonyl alcohol, 2,6-dimethylheptanol-4, n-decanol, sec-undecyl alcohol, trimethylnonyl alcohol, sec-tetradecyl alcohol, sec-heptadecyl Monoalcohol solvents such as alcohol, phenol, cyclohexanol, methylcyclohexanol, 3,3,5-trimethylcyclohexanol, benzyl alcohol, phenylmethylcarbinol, diacetone alcohol, cresol; ethylene glycol, 1,2-propylene glycol , 1,3-butylene glycol, pentanediol-2,4,2-methylpentanediol-2,
4, hexanediol-2,5, heptanediol-
Polyhydric alcohol solvents such as 2,4,2-ethylhexanediol-1,3, diethylene glycol, dipropylene glycol, triethylene glycol, tripropylene glycol, glycerin; acetone, methyl ethyl ketone, methyl-n-propyl ketone, methyl- n-butyl ketone, diethyl ketone, methyl-i-butyl ketone, methyl-n-pentyl ketone, ethyl-n-butyl ketone, methyl-n-hexyl ketone, di-i-butyl ketone, trimethylnonanone, cyclohexanone, methylcyclohexanone, 2, Ketone solvents such as 4-pentanedione, acetonylacetone, diacetone alcohol, acetophenone, fenchone; ethyl ether;
i-propyl ether, n-butyl ether, n-hexyl ether, 2-ethylhexyl ether, ethylene oxide, 1,2-propylene oxide, dioxolan, 4-methyldioxolan, dioxane, dimethyldioxane, ethylene glycol monomethyl ether, ethylene glycol monoethyl ether , Ethylene glycol diethyl ether, ethylene glycol mono-n-
Butyl ether, ethylene glycol mono-n-hexyl ether, ethylene glycol monophenyl ether, ethylene glycol mono-2-ethyl butyl ether, ethylene glycol dibutyl ether, diethylene glycol monomethyl ether, diethylene glycol monoethyl ether, diethylene glycol diethyl ether, diethylene glycol mono-n-butyl ether , Diethylene glycol di-n-butyl ether, diethylene glycol mono-n-hexyl ether, ethoxytriglycol, tetraethylene glycol di-n
-Butyl ether, propylene glycol monomethyl ether, propylene glycol monoethyl ether, propylene glycol monopropyl ether, propylene glycol monobutyl ether, dipropylene glycol monomethyl ether, dipropylene glycol monoethyl ether, tripropylene glycol monomethyl ether, tetrahydrofuran, 2-methyltetrahydrofuran Ether solvents such as diethyl carbonate, methyl acetate, ethyl acetate, γ-butyrolactone, γ-valerolactone, n-propyl acetate, i-propyl acetate, n-butyl acetate, i-butyl acetate, sec-butyl acetate;
N-pentyl acetate, sec-pentyl acetate, 3-methoxybutyl acetate, methylpentyl acetate, 2-ethylbutyl acetate, 2-ethylhexyl acetate, benzyl acetate, cyclohexyl acetate, methylcyclohexyl acetate, n-nonyl acetate, methyl acetoacetate, acetoacetate Ethyl acetate, ethylene glycol monomethyl ether acetate, ethylene glycol monoethyl ether acetate, diethylene glycol monomethyl ether acetate, diethylene glycol monoethyl ether acetate, diethylene glycol mono-n-butyl ether, propylene glycol monomethyl ether acetate, propylene glycol monoethyl ether acetate, propylene acetate Glycol monopropyl ether,
Propylene glycol monobutyl ether acetate, dipropylene glycol monomethyl acetate acetate, dipropylene glycol monoethyl ether acetate, glycol diacetate, methoxytriglycol acetate, ethyl propionate, n-butyl propionate, i-amyl propionate, diethyl oxalate, Ester solvents such as di-n-butyl oxalate, methyl lactate, ethyl lactate, n-butyl lactate, n-amyl lactate, diethyl malonate, dimethyl phthalate, diethyl phthalate; N-methylformamide;
N, N-dimethylformamide, N, N-diethylformamide, acetamide, N-methylacetamide,
Nitrogen-containing solvents such as N, N-dimethylacetamide, N-methylpropionamide, N-methylpyrrolidone; dimethyl sulfide, diethyl sulfide, thiophene, tetrahydrothiophene, dimethyl sulfoxide, sulfolane, 1,3
-Sulfur-containing solvents such as propane sultone. These can be used alone or in combination of two or more. In the present invention, the boiling point is 250 ° C.
It is particularly preferable to use less than an organic solvent, specifically, methanol, ethanol, alcohols such as isopropanol, ethylene glycol, polyhydric alcohols such as glycerin, ethylene glycol monomethyl ether, ethylene glycol monobutyl ether, diethylene glycol monoethyl ether, Glycol ether solvents such as diethylene glycol diethyl ether, propylene glycol monopropyl ether and dipropylene glycol monoethyl ether; glycol acetate ether solvents such as ethylene glycol monomethyl acetate, diethylene glycol monobutyl ether acetate, ethylene glycol diacetate and propylene glycol methyl ether acetate; N , N-dimethylacetamide, N, N- Methylformamide, N- methyl -
Amide solvents such as 2-pyrrolidone, ketone solvents such as acetone, methyl ethyl ketone, methyl isobutyl ketone, acetylacetone and methyl amyl ketone; carboxylic acid ester solvents such as ethyl lactate, methoxymethyl propionate and ethoxyethyl propionate; May be used alone or in combination of two or more.

In the present invention, the amount of the organic solvent used is
It is in the range of 0.3 to 25 times (by weight) the total amount of the components (A), (B) and (C).

Component (E) In the present invention, a catalyst can be used in addition to the components (A) to (D). Examples of the catalyst include organic acids, inorganic acids, organic salts, inorganic salts, and metal chelates. Examples of the organic acid include acetic acid, propionic acid,
Butanoic acid, pentanoic acid, hexanoic acid, heptanoic acid, octanoic acid, nonanoic acid, decanoic acid, oxalic acid, maleic acid,
Methylmalonic acid, adipic acid, sebacic acid, gallic acid,
Butyric acid, melitic acid, arachidonic acid, mykimic acid, 2-ethylhexanoic acid, oleic acid, stearic acid, linoleic acid, linoleic acid, salicylic acid, benzoic acid, p-aminobenzoic acid, p-toluenesulfonic acid, benzenesulfonic acid, Monochloroacetic acid, dichloroacetic acid, trichloroacetic acid,
Examples include trifluoroacetic acid, formic acid, malonic acid, sulfonic acid, phthalic acid, fumaric acid, citric acid, tartaric acid and the like. Examples of the inorganic acid include hydrochloric acid, nitric acid, sulfuric acid, hydrofluoric acid, phosphoric acid and the like. As organic salts,
For example, pyridine, pyrrole, piperazine, pyrrolidine,
Piperidine, picoline, trimethylamine, triethylamine, monoethanolamine, diethanolamine,
Examples thereof include dimethylmonoethanolamine, monomethyldiethanolamine, triethanolamine, diazabicyclooctane, diazabicyclononane, diazabicycloundecene, and tetramethylammonium hydroxide. Examples of the inorganic salt include ammonia, sodium hydroxide, potassium hydroxide, barium hydroxide, calcium hydroxide and the like. Also,
Metal chelates can also be used in the compositions of the present invention. Examples of metal chelate compounds include triethoxy mono (acetylacetonate) titanium,
n-propoxy mono (acetylacetonate) titanium, tri-i-propoxy mono (acetylacetonate) titanium, tri-n-butoxy mono (acetylacetonate) titanium, tri-sec-butoxy mono (acetylacetate) (Nato) titanium, tri-t-butoxy mono (acetylacetonate) titanium, diethoxy bis (acetylacetonate) titanium, di-n-propoxy bis (acetylacetonate) titanium, di-i-propoxy bis ( Acetylacetonate) titanium, di-n
-Butoxybis (acetylacetonato) titanium, di-sec-butoxybis (acetylacetonato) titanium, di-t-butoxybis (acetylacetonato) titanium, monoethoxytris (acetylacetonato) titanium, Mono-n-propoxy tris (acetylacetonate) titanium, mono-i-propoxy tris (acetylacetonate) titanium, mono-n-butoxy tris (acetylacetonate) titanium, mono-s
ec-butoxy tris (acetylacetonate) titanium, mono-t-butoxy tris (acetylacetonate) titanium, tetrakis (acetylacetonate) titanium, triethoxy mono (ethylacetoacetate) titanium, tri-n-propoxy. Mono (ethyl acetoacetate) titanium, tri-i-propoxy mono (ethyl acetoacetate) titanium, tri-n-butoxy mono (ethyl acetoacetate) titanium, tri-sec-butoxy mono (ethyl acetoacetate) titanium, Tri-t-butoxy mono (ethyl acetoacetate) titanium, diethoxy bis (ethyl acetoacetate) titanium, di-n-propoxy bis (ethyl acetoacetate) titanium, di-i-propoxy bis (ethyl acetoacetate) Chita , Di-n-butoxybis (ethylacetoacetate) titanium, di-sec-butoxybis (ethylacetoacetate) titanium, di-t-butoxybis (ethylacetoacetate) titanium, monoethoxy tris (ethylacetoacetate) Acetate) titanium, mono-n-propoxy tris (ethyl acetoacetate)
Titanium, mono-i-propoxy tris (ethyl acetoacetate) titanium, mono-n-butoxy tris (ethyl acetoacetate) titanium, mono-sec-butoxy tris (ethyl acetoacetate) titanium, mono-
t-butoxy-tris (ethylacetoacetate) titanium, tetrakis (ethylacetoacetate) titanium, mono (acetylacetonate) tris (ethylacetoacetate) titanium, bis (acetylacetonate) bis (ethylacetoacetate) titanium, tris ( Titanium chelate compounds such as acetylacetonate) mono (ethylacetoacetate) titanium; triethoxymono (acetylacetonato) zirconium, tri-n-propoxymono (acetylacetonato) zirconium, tri-i-propoxymono ( (Acetylacetonato) zirconium, tri-n-butoxy mono (acetylacetonato) zirconium, tri-sec-butoxy mono (acetylacetonato) zirconium, tri-t-butoxy mono (A Tilacetonate) zirconium, diethoxybis (acetylacetonato) zirconium, di-n-propoxybis (acetylacetonato) zirconium, di-i-propoxybis (acetylacetonato) zirconium, di-n-butoxy. Bis (acetylacetonato) zirconium, di-sec-butoxybis (acetylacetonato) zirconium, di-t-butoxybis (acetylacetonato) zirconium, monoethoxy tris (acetylacetonato) zirconium, mono-n -Propoxy-tris (acetylacetonato) zirconium, mono-i-propoxy-tris (acetylacetonato) zirconium, mono-n-butoxytris (acetylacetonato) zirconium, mono-sec-butyl Carboxymethyl -
Tris (acetylacetonate) zirconium, mono-
t-butoxy tris (acetylacetonate) zirconium, tetrakis (acetylacetonate) zirconium, triethoxy mono (ethylacetoacetate)
Zirconium, tri-n-propoxy mono (ethyl acetoacetate) zirconium, tri-i-propoxy mono (ethyl acetoacetate) zirconium, tri-n-butoxy mono (ethyl acetoacetate) zirconium, tri-sec-butoxy. Mono (ethyl acetoacetate) zirconium, tri-t-butoxy mono (ethyl acetoacetate) zirconium, diethoxy bis (ethyl acetoacetate) zirconium, di-n-propoxy bis (ethyl acetoacetate) zirconium, di-i- Propoxy bis (ethyl acetoacetate) zirconium, di-n-butoxy bis (ethyl acetoacetate) zirconium, di-sec
-Butoxy bis (ethyl acetoacetate) zirconium, di-t-butoxy bis (ethyl acetoacetate) zirconium, monoethoxy tris (ethyl acetoacetate) zirconium, mono-n-propoxy.
Tris (ethylacetoacetate) zirconium, mono-i-propoxy tris (ethylacetoacetate)
Zirconium, mono-n-butoxy tris (ethyl acetoacetate) zirconium, mono-sec-butoxy tris (ethyl acetoacetate) zirconium,
Mono-t-butoxy tris (ethylacetoacetate) zirconium, tetrakis (ethylacetoacetate) zirconium, mono (acetylacetonate) tris (ethylacetoacetate) zirconium, bis (acetylacetonate) bis (ethylacetoacetate)
Zirconium chelate compounds such as zirconium, tris (acetylacetonate) mono (ethylacetoacetate) zirconium; tris (acetylacetonate) aluminum, tris (ethylacetoacetate)
Aluminum chelate compounds such as aluminum; and the like.

The composition of the present invention can be produced by mixing the above components (A) to (C) and, if necessary, other components. In order to form a film of the component (B) using the composition of the present invention, first, the composition of the present invention is applied to a substrate to form a coating film. Here, examples of the substrate on which the composition of the present invention can be applied include semiconductors, glass, ceramics, and metals, and examples of the application method include spin coating, dipping, and roller blades. The thickness of the coating film to be formed is usually 0.2 to 20 μm in the case of an interlayer insulating film. Then, the formed coating film is heated to remove the solvent, but at 50 to 150 ° C. for 30 seconds.
It is preferably performed in 10 minutes. Subsequently, light having a wavelength of 200 to 400 nm and 50 to 2000 mJ may be irradiated using an exposure machine, and if necessary, post exposure at 50 to 200 ° C. for 30 seconds to 10 minutes as long as the component (C) is not decomposed. Baking may be added. In the present invention, it is necessary to select the heating conditions of the coating film so that the cured film of the component (A) has pores. As the heating method, the formed coating film is heated at a temperature lower than the decomposition temperature of the component (C).
A method in which a component is partially cured, and then heated from a temperature equal to or higher than the decomposition temperature of the component (C) to a final curing temperature to obtain a porous cured product, may be mentioned. Further, in order to control the curing rate of the component (A) and the decomposition rate of the component (C),
If necessary, heating can be performed stepwise, or an atmosphere such as nitrogen, air, oxygen, or reduced pressure can be selected. Normal,
Since the decomposition temperature of the component (C) is 250 to 450 ° C,
The coating includes a step of being finally heated to this temperature or higher. This step is preferably performed under reduced pressure or under an inert gas. The film obtained by heating the composition of the present invention by the method of the present invention has a film density of 0.3 to 1.2 g / cm.
³ , and the hole diameter is 10 nm or less in the case of having pores. The dielectric constant of the film is usually from 2.6 to 1.2. The film of the present invention is suitable as an insulating film, and is particularly suitable as an interlayer insulating film for highly integrated circuits.

[0018]

DESCRIPTION OF THE PREFERRED EMBODIMENTS Embodiments of the present invention will be described below based on examples. However, the following description generally shows an example of the embodiment of the present invention, and the present invention is not limited by the description without any particular reason. Parts and% in Examples and Comparative Examples indicate parts by weight and% by weight, respectively, unless otherwise specified.

Example 1 (1) Maleic acid 10.0 was added to a mixed solution of 140.5 g of tetramethoxysilane, 182.7 g of methyltrimethoxysilane, 56.0 g of dimethyldimethoxysilane, and 394.0 g of propylene glycol monopropyl ether.
g was dissolved in 116.8 g of water at room temperature over 1 hour. After the addition of the mixture was completed, the mixture was further reacted at 60 ° C. for 1 hour, and the produced methanol was distilled off under reduced pressure to obtain a polysiloxane sol. (2) 100 g of the polysiloxane sol obtained in the above (1),
8.9 g of a polyethylene oxide block-polypropylene oxide block-polyethylene oxide block copolymer (Newport PE61 manufactured by Sanyo Chemical Co., Ltd.), 3.0 g of propionyl acetophenone oxime and 0.75 g of N-phenylglycine were added, and the resulting mixture was added to 8 parts.
Coating on an inch silicon wafer by a spin coating method, and then applying ultraviolet light of 365 nm for 30 minutes at 80 ° C. for 30 minutes.
After irradiating with 0 mJ / cm ^{2 and} heating at 200 ° C. under nitrogen for 5 minutes, it was further heated at 425 ° C. for 1 hour to form a colorless and transparent film. Further, the obtained film was evaluated as follows. Table 1 shows the results. (Evaluation of composition for film formation)

1. Dielectric constant An aluminum electrode pattern was formed on the obtained film by a vapor deposition method to prepare a sample for dielectric constant measurement. Using the sample at a frequency of 100 kHz, the dielectric constant of the coating film was measured by a CV method using an HP16451B electrode manufactured by Yokogawa Hewlett-Packard Co., Ltd. and an HP4284A precision LCR meter. Table 1 shows the results
Shown in 2. Storage stability A film-forming composition stored at 25 ° C. for 3 months was formed into a film by the method of Example 1. The film thickness of the coating film thus obtained is measured by an optical film thickness meter (Rudolph Technology).
gies, SpectraLaser200). In addition, similarly, the film thickness of the coating film before storage was measured, and the storage stability was evaluated based on the film thickness increase rate determined by the following equation. Film thickness increase rate (%) = ((film thickness after storage) − (film thickness before storage)) ÷ (film thickness before storage) × 100 〇: film thickness change rate ≦ 10% △: 10% <film Thickness change rate ≦ 20% ×: 20% <Thickness change rate

3. Film density The composition sample is applied on an 8-inch Si wafer by using a spin coating method, and is placed on a hot plate at 80 ° C. for 5 minutes.
The substrate was dried at 200 ° C. for 5 minutes, and baked at 450 ° C. for 60 minutes in a vacuum oven at 450 ° C. The film density was calculated from the thickness and area of the coating film and the weight of the coating film. 4. Elastic Modulus The obtained film was measured by a continuous stiffness measuring method using a nano indenter XP (manufactured by Nano Instruments). 5. CMP resistance The obtained film was polished under the following conditions. Slurry: silica-hydrogen peroxide polishing pressure: 300 g / cm ² polishing time: 60 seconds The evaluation was performed according to the following criteria. ：: No change Δ: Partly peeling or flaws ×: All peeling Also, the polishing rate was calculated as follows. Polishing rate (angstrom / min) = (initial film thickness)-
(Film thickness after polishing for 60 seconds)

Synthesis Example Synthesis of Acrylic Polymer Isobutyl methacrylate 18.32 in a 100 ml flask.
g, 3- (trimethoxysilyl) propyl methacrylate 1.68 g, azoisobutyronitrile (AIBN) 0.
33 g, 0.20 g of 2-mercaptoethanol and 3
30 g of -methoxymethyl propionate was added and dissolved. After the inside of the reaction system was replaced with nitrogen gas, the mixture was stirred for 7 hours while heating in an oil bath at 80 ° C. to obtain a viscous polymer solution. When the average molecular weight in terms of polystyrene was measured by GPC, the number average molecular weight was 4,830 and the weight average molecular weight was 8,900.

Example 2 (1) In a mixed solution of 91.2 g of tetramethoxysilane and 292.3 g of methyltrimethoxysilane and 387.0 g of propylene glycol monopropyl ether, 10.0 g of maleic acid was dissolved in 119.4 g of water. The aqueous solution was added dropwise at room temperature over 1 hour. After addition of the mixture, 6
After reacting at 0 ° C. for 1 hour, the produced methanol was distilled off under reduced pressure to obtain a polysiloxane sol. (2) 21.2 g (solid content 8.5 g) of the acrylic polymer solution obtained in the synthesis example was added to 100 g of the silica sol obtained in (1), and the mixture was stirred at 60 ° C. for 1 hour. 3.0 g of [[α, α-dimethyl-3,5-dimethoxybenzyl] oxy] carbonyl] propylamine was added to the obtained solution.
, And spin-coated on an 8-inch wafer, and heated on a hot plate at 80 ° C. for 5 minutes and at 200 ° C. for 5 minutes.
After drying for a minute, the mixture was fired at 425 ° C. for 1 hour under vacuum to obtain a transparent coating film. Evaluation was performed in the same manner as in Example 1. Table 1 shows the results.

[0024]

[Table 1]

[0025]

The film obtained by curing the composition of the present invention is excellent in dielectric properties, storage stability and mechanical strength.

Continued on the front page (51) Int.Cl. ⁷ Identification symbol FI Theme coat II (Reference) H01L 21/312 H01L 21/312 C 21/316 21/316 H F term (Reference) 4J038 CG142 DD002 DE002 DF022 DL021 DL031 JC32 KA04 KA06 NA26 PA19 5F058 AA10 AC03 AC06 AF04 AG01 AH01 AH02 BA20 BC02 BC04 BC05 BF46 BH01 BJ01 BJ02

Claims (8)

[Claims] (1) A silane compound represented by the following general formula (1):
R ¹ _a Si (OR ² ) _4-a ... (1) (R ¹ represents a hydrogen atom, a fluorine atom or a monovalent organic group, and R ² represents a monovalent organic group. And a represents an integer of 0 to 2) and a compound represented by the following general formula (2): R ³ _b (R ⁴ O) _3-b Si— (R ⁷ ) _d —Si (OR ⁵ ) _3-c R ⁶ _c (2) (R ³ , R ⁴ , R ⁵ and R ⁶ may be the same or different and each represents a monovalent organic group, and b and c are May be the same or different, and represent a number of 0 to 2; R ⁷ represents an oxygen atom or a group represented by — (CH 2) _n —;
Represents 1 to 6, and d represents 0 or 1. Or at least one of a hydrolyzate and a condensate of at least one compound selected from the group consisting of (B) a latent base catalyst and (C) a component which is compatible or dispersed with the component (A), and has a boiling point or decomposition. A film-forming composition comprising a compound having a temperature of 250 to 450 ° C. 2. The film-forming composition according to claim 1, wherein (A) two or more compounds represented by the general formula (1) are used. 3. A compound wherein the component (C) has a polyalkylene oxide structure, an acrylic polymer, a polyester,
The film forming composition according to claim 1, wherein the composition is at least one selected from the group consisting of polycarbonate and polyanhydride. 4. The film-forming composition according to claim 1, further comprising (D) an organic solvent having a boiling point of less than 250 ° C. 5. A method for producing a film, comprising applying the composition according to claim 1 to a substrate and heating the substrate. 6. Applying the composition according to claim 1 to a substrate,
(A) by heating at a temperature lower than the decomposition temperature of the component (D)
A method for forming a film, comprising partially curing the components and then heating and curing at a temperature equal to or higher than the decomposition temperature of the component (D). 7. Applying the composition according to claim 1 to a substrate,
A method of forming a film, comprising curing the component (A) at a temperature equal to or higher than the decomposition temperature of the component (D). 8. A low-density film obtained by the method according to claim 6.