JP2002069375A - Composition for forming film and material for forming insulating film - Google Patents

Abstract

PROBLEM TO BE SOLVED: To exhibit a low dielectric constant as a material for an interlayer insulating film in a semiconductor device, etc.
(Chemical Mechanical Polis
hing) A film forming composition and a material for forming an insulating film having excellent resistance are obtained. (A) The following general formulas (1), (2),
At least one selected from the group of compounds represented by (3)
A film-forming composition comprising a condensate obtained by hydrolyzing and condensing a kind compound in the presence of a catalyst, (B) silicon carbide and (C) an organic solvent. ^{_{R a Si (OR 1) 4}} -a ····· (1) Si (OR 2) 4 ····· (2) R 3 b (R 4 O) 3-b Si- (R 7) d -Si (OR
⁵ ) _3-c R ⁶ _c (3) (wherein R is a hydrogen atom, a fluorine atom, or a monovalent organic group,
R ^{1 to} R ⁶ are a monovalent organic group, R 7 is an oxygen atom, a phenylene group or — (CH ₂ ) _n —, a is an integer of 1 to 2, b, c
Represents a number of 0 to 2, d represents 0 or 1, and n represents an integer of 1 to 6. )

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a composition for forming a film, and more particularly, to a material for an interlayer insulating film in a semiconductor device or the like, which exhibits a low dielectric constant, a mechanical strength of a coating film, and a CMP (Chemical Mechanical). P
The present invention relates to a film-forming composition and a material for forming an insulating film having excellent resistance.

[0002]

2. Description of the Related Art Conventionally, CVD (Chemical Vapor Deposit) has been used as an interlayer insulating film in a semiconductor device or the like.
A silica (SiO ₂ ) film formed by a vacuum process such as a position method is frequently used. In recent years, for the purpose of forming a more uniform interlayer insulating film, a coating-type insulating film mainly composed of a hydrolysis product of tetraalkoxylan, which is called an SOG (Spin on Glass) film, may be used. It has become. Further, with the increase in integration of semiconductor elements and the like, an interlayer insulating film having a low relative dielectric constant and mainly containing polyorganosiloxane called organic SOG has been developed. In particular, with higher integration and multi-layering of semiconductor devices and the like, better electrical insulation between conductors is required, and therefore a lower dielectric constant is exhibited, and the mechanical strength and CMP resistance of the coating film are reduced. An excellent interlayer insulating film material has been demanded.

As a material having a low relative dielectric constant, a composition comprising a mixture of particles obtained by condensing alkoxysilane in the presence of ammonia and a basic partial hydrolyzate of alkoxysilane (JP-A-5-263045, 5-3-1153
19) and a coating solution obtained by condensing a basic hydrolyzate of polyalkoxysilane in the presence of ammonia (JP-A-11-340219 and JP-A-11-340220).
However, the materials obtained by these methods are:
The nature of the reaction product was not stable, and the dispersion of the dielectric constant, the mechanical strength of the coating film, and the CMP resistance was large, so that it was not suitable for industrial production.

[0004]

The present invention relates to a film-forming composition for solving the above problems, and more particularly, to a film having a low relative dielectric constant as an interlayer insulating film in a semiconductor device or the like. It is an object of the present invention to provide a film-forming composition having excellent mechanical strength and CMP resistance, and a material for forming an insulating film obtained from the composition.

[0005]

The present invention SUMMARY OF] is (hereinafter also referred to as "Compound (1)") (A) (A-1) a compound represented by the following general formula (1), R _a Si (OR ¹ _4-a ··· (1) (wherein, R represents a hydrogen atom, a fluorine atom or a monovalent organic group, R ¹ represents a monovalent organic group, and a represents an integer of 1 or 2.) (A-2) a compound represented by the following general formula (2) (hereinafter, referred to as
(Also referred to as “compound (2)”) and Si (OR ² ) ₄ ... (2) (wherein R ² represents a monovalent organic group.) (A-3) The following general formula (3) ) (Hereinafter, a compound represented by
"Compound (3)" is also referred to ^{_{as) R 3 b (R 4 O}} ) 3-b Si- (R 7) d -Si (OR 5) 3-c R 6 c ··· ·· (3) wherein , R ^{3 to} R ⁶ are the same or different, each is a monovalent organic group, b to c are the same or different, an integer of 0 to 2,
R ⁷ is an oxygen atom, a phenylene group or — (CH ₂ ) _n —
(Where n is an integer of 1 to 6), d
Represents 0 or 1. At least one selected from the group of
The present invention relates to a film-forming composition comprising: a hydrolyzed condensate obtained by hydrolyzing and condensing a kind compound in the presence of a catalyst; (B) silicon carbide particles; and (C) an organic solvent. Next, the present invention relates to a material for forming an insulating film comprising the above-described composition for forming a film.

[0006]

BEST MODE FOR CARRYING OUT THE INVENTION In the present invention, the (A) hydrolyzed condensate is a hydrolyzate or condensate of at least one silane compound selected from the above-mentioned compounds (1) to (3). is there. Here, in the hydrolysis of the component (A), the R ¹ O—, R ² O—, R ⁴ O— and R ⁴ O-groups contained in the compounds (1) to (3) constituting the component (A) are included. ⁵ O-
Not all of the groups need be hydrolyzed, for example,
It may be one in which only one is hydrolyzed, one in which two or more are hydrolyzed, or a mixture thereof. Further, the condensation in the component (A) means that the silanol groups of the hydrolyzates of the compounds (1) to (3) constituting the component (A) condense to form a Si—O—Si bond. In the present invention, it is not necessary that all of the silanol groups are condensed, but the concept encompasses a mixture of a small amount of silanol groups condensed and a mixture of those having different degrees of condensation.

(A) Hydrolysis condensate (A) The hydrolysis condensate is obtained by hydrolyzing at least one silane compound selected from the group of compounds (1) to (3) in the presence of a catalyst. Obtained by condensation. Compound (1): In the above general formula (1), R and R
The ¹ monovalent organic group, an alkyl group, an aryl group,
Examples include an allyl group and a glycidyl group. In the general formula (1), R is preferably a monovalent organic group, particularly an alkyl group or a phenyl group. Here, examples of the alkyl group include a methyl group, an ethyl group, a propyl group, and a butyl group, and preferably have 1 to 1 carbon atoms.
5, these alkyl groups may be chain-like or branched, and a hydrogen atom may be substituted by a fluorine atom or the like. In the general formula (1), examples of the aryl group include a phenyl group, a naphthyl group, a methylphenyl group, an ethylphenyl group, a chlorophenyl group, a bromophenyl group, and a fluorophenyl group.

Specific examples of the compound represented by the general formula (1) include trimethoxysilane, triethoxysilane, tri-n-propoxysilane, tri-iso-propoxysilane, tri-n-butoxysilane, tri- sec-butoxysilane, tri-tert-butoxysilane, triphenoxysilane, fluorotrimethoxysilane, fluorotriethoxysilane, fluorotri-n-propoxysilane, fluorotri-iso-propoxysilane,
Fluorotri-n-butoxysilane, fluorotri-s
ec-butoxysilane, fluorotri-tert-butoxysilane, fluorotriphenoxysilane and the like;

[0009] Methyltrimethoxysilane, methyltriethoxysilane, methyltri-n-propoxysilane, methyltri-iso-propoxysilane, methyltri-n
-Butoxysilane, methyltri-sec-butoxysilane, methyltri-tert-butoxysilane, methyltriphenoxysilane, ethyltrimethoxysilane, ethyltriethoxysilane, ethyltri-n-propoxysilane, ethyltri-iso-propoxysilane, ethyltri-n -Butoxysilane, ethyltri-sec-butoxysilane, ethyltri-tert-butoxysilane,
Ethyl triphenoxy silane, vinyl trimethoxy silane, vinyl triethoxy silane, vinyl tri-n-propoxy silane, vinyl tri-iso-propoxy silane, vinyl tri-n-butoxy silane, vinyl tri-s
ec-butoxysilane, vinyltri-tert-butoxysilane, vinyltriphenoxysilane, 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-butyltriethoxysilane, sec-butyl-tri-n-propoxysilane, sec-butyl-tri-iso-propoxysilane, sec-butyl-tri-n-butoxysilane, s
ec-butyl-tri-sec-butoxysilane, sec
-Butyl-tri-tert-butoxysilane, sec-
Butyl-triphenoxysilane, t-butyltrimethoxysilane, t-butyltriethoxysilane, t-butyltri-n-propoxysilane, t-butyltri-iso
-Propoxysilane, t-butyltri-n-butoxysilane, t-butyltri-sec-butoxysilane, t-
Butyltri-tert-butoxysilane, t-butyltriphenoxysilane, phenyltrimethoxysilane, phenyltriethoxysilane, phenyltri-n-propoxysilane, phenyltri-iso-propoxysilane, phenyltri-n-butoxysilane, phenyltri -Sec-butoxysilane, phenyltri-tert-
Butoxysilane, phenyltriphenoxysilane, vinyltrimethoxysilane, vinyltriethoxysilane, γ
-Aminopropyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ-glycidoxypropyltrimethoxysilane, γ-glycidoxypropyltriethoxysilane, γ-trifluoropropyltrimethoxysilane, γ-trifluoropropyltrimethoxysilane Ethoxysilane 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 and the like.

Preferred compounds as compound (1) are methyltrimethoxysilane, methyltriethoxysilane,
Methyltri-n-propoxysilane, methyltri-is
o-propoxysilane, ethyltrimethoxysilane, ethyltriethoxysilane, vinyltrimethoxysilane,
Vinyl triethoxysilane, phenyltrimethoxysilane, phenyltriethoxysilane, dimethyldimethoxysilane, dimethyldiethoxysilane, diethyldimethoxysilane, diethyldiethoxysilane, diphenyldimethoxysilane, diphenyldiethoxysilane, and the like. These may be used alone or in combination of two or more.

Compound (2): In the above formula (2), examples of the monovalent organic group represented by R ² include the same organic groups as in the above formula (1). Specific examples of the compound represented by the general formula (2) include tetramethoxysilane, tetraethoxysilane, tetra-n-propoxysilane, tetra-iso-propoxysilane, tetra-n-butoxysilane, and tetra-sec-butoxysilane. , Tetra-tert-butoxysilane, tetraphenoxysilane and the like.

Compound (3): In the above formula (3), examples of the monovalent organic group represented by R ^{3 to} R ⁶ include the same organic groups as in the above formula (1). . In the general formula (3), as a compound in which R ⁷ is an oxygen atom,
Hexamethoxydisiloxane, hexaethoxydisiloxane, hexaphenoxydisiloxane, 1,1,1,
3,3-pentamethoxy-3-methyldisiloxane,
1,1,1,3,3-pentaethoxy-3-methyldisiloxane, 1,1,1,3,3-pentaphenoxy-3
-Methyldisiloxane, 1,1,1,3,3-pentamethoxy-3-ethyldisiloxane, 1,1,1,3,3
-Pentaethoxy-3-ethyldisiloxane, 1,1,
1,3,3-pentaphenoxy-3-ethyldisiloxane, 1,1,1,3,3-pentamethoxy-3-phenyldisiloxane, 1,1,1,3,3-pentaethoxy-3-phenyl Disiloxane, 1,1,1,3,3-pentaphenoxy-3-phenyldisiloxane, 1,1,
3,3-tetramethoxy-1,3-dimethyldisiloxane, 1,1,3,3-tetraethoxy-1,3-dimethyldisiloxane, 1,1,3,3-tetraphenoxy-
1,3-dimethyldisiloxane, 1,1,3,3-tetramethoxy-1,3-diethyldisiloxane, 1,1,
3,3-tetraethoxy-1,3-diethyldisiloxane, 1,1,3,3-tetraphenoxy-1,3-diethyldisiloxane, 1,1,3,3-tetramethoxy-
1,3-diphenyldisiloxane, 1,1,3,3-tetraethoxy-1,3-diphenyldisiloxane, 1,
1,3,3-tetraphenoxy-1,3-diphenyldisiloxane, 1,1,3-trimethoxy-1,3,3-
Trimethyldisiloxane, 1,1,3-triethoxy-
1,3,3-trimethyldisiloxane, 1,1,3-triphenoxy-1,3,3-trimethyldisiloxane,
1,1,3-trimethoxy-1,3,3-triethyldisiloxane, 1,1,3-triethoxy-1,3,3
Triethyldisiloxane, 1,1,3-triphenoxy-1,3,3-triethyldisiloxane, 1,
1,3-trimethoxy-1,3,3-triphenyldisiloxane, 1,1,3-triethoxy-1,3,3-triphenyldisiloxane, 1,1,3-triphenoxy-1,3,3 -Triphenyldisiloxane, 1,3-dimethoxy-1,1,3,3-tetramethyldisiloxane, 1,3-diethoxy-1,1,3,3-tetramethyldisiloxane, 1,3-diphenoxy- 1,1,3
3-tetramethyldisiloxane, 1,3-dimethoxy-
1,1,3,3-tetraethyldisiloxane, 1,3-
Diethoxy-1,1,3,3-tetraethyldisiloxane, 1,3-diphenoxy-1,1,3,3-tetraethyldisiloxane, 1,3-dimethoxy-1,1,3,3
3-tetraphenyldisiloxane, 1,3-diethoxy-1,1,3,3-tetraphenyldisiloxane, 1,
Examples thereof include 3-diphenoxy-1,1,3,3-tetraphenyldisiloxane.

Among them, hexamethoxydisiloxane, hexaethoxydisiloxane, 1,1,3,3-tetramethoxy-1,3-dimethyldisiloxane,
1,3,3-tetraethoxy-1,3-dimethyldisiloxane, 1,1,3,3-tetramethoxy-1,3-diphenyldisiloxane, 1,3-dimethoxy-1,1,1
3,3-tetramethyldisiloxane, 1,3-diethoxy-1,1,3,3-tetramethyldisiloxane, 1,
Preferred examples include 3-dimethoxy-1,1,3,3-tetraphenyldisiloxane and 1,3-diethoxy-1,1,3,3-tetraphenyldisiloxane.

In the general formula (3), the compound in which d is 0 includes hexamethoxydisilane, hexaethoxydisilane, hexaphenoxydisilane, 1,1,1,1
2,2-pentamethoxy-2-methyldisilane, 1,
1,1,2,2-pentaethoxy-2-methyldisilane, 1,1,1,2,2-pentaphenoxy-2-methyldisilane, 1,1,1,2,2-pentamethoxy-2
-Ethyldisilane, 1,1,1,2,2-pentaethoxy-2-ethyldisilane, 1,1,1,2,2-pentaphenoxy-2-ethyldisilane, 1,1,1,2,2
-Pentamethoxy-2-phenyldisilane, 1,1,
1,2,2-pentaethoxy-2-phenyldisilane,
1,1,1,2,2-pentaphenoxy-2-phenyldisilane, 1,1,2,2-tetramethoxy-1,2-
Dimethyldisilane, 1,1,2,2-tetraethoxy-
1,2-dimethyldisilane, 1,1,2,2-tetraphenoxy-1,2-dimethyldisilane, 1,1,2,2
-Tetramethoxy-1,2-diethyldisilane, 1,
1,2,2-tetraethoxy-1,2-diethyldisilane, 1,1,2,2-tetraphenoxy-1,2-diethyldisilane, 1,1,2,2-tetramethoxy-1,
2-diphenyldisilane, 1,1,2,2-tetraethoxy-1,2-diphenyldisilane, 1,1,2,2-
Tetraphenoxy-1,2-diphenyldisilane, 1,
1,2-trimethoxy-1,2,2-trimethyldisilane, 1,1,2-triethoxy-1,2,2-trimethyldisilane, 1,1,2-triphenoxy-1,2,2
-Trimethyldisilane, 1,1,2-trimethoxy-
1,2,2-triethyldisilane, 1,1,2-triethoxy-1,2,2-triethyldisilane, 1,
1,2-triphenoxy-1,2,2-triethyldisilane, 1,1,2-trimethoxy-1,2,2-triphenyldisilane, 1,1,2-triethoxy-1,
2,2-triphenyldisilane, 1,1,2-triphenoxy-1,2,2-triphenyldisilane, 1,2
-Dimethoxy-1,1,2,2-tetramethyldisilane, 1,2-diethoxy-1,1,2,2-tetramethyldisilane, 1,2-diphenoxy-1,1,2,2-
Tetramethyldisilane, 1,2-dimethoxy-1,1,1
2,2-tetraethyldisilane, 1,2-diethoxy-
1,1,2,2-tetraethyldisilane, 1,2-diphenoxy-1,1,2,2-tetraethyldisilane,
1,2-dimethoxy-1,1,2,2-tetraphenyldisilane, 1,2-diethoxy-1,1,2,2-tetraphenyldisilane, 1,2-diphenoxy-1,1,1
2,2-tetraphenyldisilane and the like can be mentioned.

Of these, hexamethoxydisilane,
Hexaethoxydisilane, 1,1,2,2-tetramethoxy-1,2-dimethyldisilane, 1,1,2,2-tetraethoxy-1,2-dimethyldisilane, 1,1,
2,2-tetramethoxy-1,2-diphenyldisilane, 1,2-dimethoxy-1,1,2,2-tetramethyldisilane, 1,2-diethoxy-1,1,2,2-tetramethyldisilane, 1,2-dimethoxy-1,1,1,
Preferred examples include 2,2-tetraphenyldisilane and 1,2-diethoxy-1,1,2,2-tetraphenyldisilane.

Further, in the general formula (3), R ⁷ is-
Examples of the compound represented by the group represented by (CH ₂ ) _n- include bis (trimethoxysilyl) methane, bis (triethoxysilyl) methane, bis (tri-n-propoxysilyl) methane, and bis (tri-i-propoxy). Silyl) methane, bis (tri-n-butoxysilyl) methane, bis (tri-
sec-butoxysilyl) methane, bis (tri-t-butoxysilyl) methane, 1,2-bis (trimethoxysilyl) ethane, 1,2-bis (triethoxysilyl) ethane, 1,2-bis (tri- n-propoxysilyl) ethane, 1,2-bis (tri-i-propoxysilyl) ethane, 1,2-bis (tri-n-butoxysilyl) ethane, 1,2-bis (tri-sec-butoxysilyl) Ethane, 1,2-bis (tri-t-butoxysilyl) ethane, 1- (dimethoxymethylsilyl) -1- (trimethoxysilyl) methane, 1- (diethoxymethylsilyl)
-1- (triethoxysilyl) methane, 1- (di-n-
Propoxymethylsilyl) -1- (tri-n-propoxysilyl) methane, 1- (di-i-propoxymethylsilyl) -1- (tri-i-propoxysilyl) methane,
1- (di-n-butoxymethylsilyl) -1- (tri-
n-butoxysilyl) methane, 1- (di-sec-butoxymethylsilyl) -1- (tri-sec-butoxysilyl) methane, 1- (di-t-butoxymethylsilyl)
-1- (tri-t-butoxysilyl) methane, 1- (dimethoxymethylsilyl) -2- (trimethoxysilyl)
Ethane, 1- (diethoxymethylsilyl) -2- (triethoxysilyl) ethane, 1- (di-n-propoxymethylsilyl) -2- (tri-n-propoxysilyl) ethane, 1- (di-i -Propoxymethylsilyl) -2-
(Tri-i-propoxysilyl) ethane, 1- (di-n
-Butoxymethylsilyl) -2- (tri-n-butoxysilyl) ethane, 1- (di-sec-butoxymethylsilyl) -2- (tri-sec-butoxysilyl) ethane, 1- (di-t-butoxy) Methylsilyl) -2- (tri-t-butoxysilyl) ethane, bis (dimethoxymethylsilyl) methane, bis (diethoxymethylsilyl)
Methane, bis (di-n-propoxymethylsilyl) methane, bis (di-i-propoxymethylsilyl) methane,
Bis (di-n-butoxymethylsilyl) methane, bis (di-sec-butoxymethylsilyl) methane, bis (di-tert-butoxymethylsilyl) methane, 1,2-bis (dimethoxymethylsilyl) ethane, 1, 2-bis (diethoxymethylsilyl) ethane, 1,2-bis (di-n-propoxymethylsilyl) ethane, 1,2-bis (di-i-propoxymethylsilyl) ethane, 1,2-
Bis (di-n-butoxymethylsilyl) ethane, 1,2
-Bis (di-sec-butoxymethylsilyl) ethane,
1,2-bis (di-t-butoxymethylsilyl) ethane, 1,2-bis (trimethoxysilyl) benzene,
1,2-bis (triethoxysilyl) benzene, 1,2
-Bis (tri-n-propoxysilyl) benzene, 1,
2-bis (tri-i-propoxysilyl) benzene,
1,2-bis (tri-n-butoxysilyl) benzene,
1,2-bis (tri-sec-butoxysilyl) benzene, 1,2-bis (tri-t-butoxysilyl) benzene, 1,3-bis (trimethoxysilyl) benzene,
1,3-bis (triethoxysilyl) benzene, 1,3
-Bis (tri-n-propoxysilyl) benzene, 1,
3-bis (tri-i-propoxysilyl) benzene,
1,3-bis (tri-n-butoxysilyl) benzene,
1,3-bis (tri-sec-butoxysilyl) benzene, 1,3-bis (tri-t-butoxysilyl) benzene, 1,4-bis (trimethoxysilyl) benzene,
1,4-bis (triethoxysilyl) benzene, 1,4
-Bis (tri-n-propoxysilyl) benzene, 1,
4-bis (tri-i-propoxysilyl) benzene,
1,4-bis (tri-n-butoxysilyl) benzene,
Examples thereof include 1,4-bis (tri-sec-butoxysilyl) benzene and 1,4-bis (tri-t-butoxysilyl) benzene.

Of these, bis (trimethoxysilyl) methane, bis (triethoxysilyl) methane,
2-bis (trimethoxysilyl) ethane, 1,2-bis (triethoxysilyl) ethane, 1- (dimethoxymethylsilyl) -1- (trimethoxysilyl) methane, 1-
(Diethoxymethylsilyl) -1- (triethoxysilyl) methane, 1- (dimethoxymethylsilyl) -2-
(Trimethoxysilyl) ethane, 1- (diethoxymethylsilyl) -2- (triethoxysilyl) ethane, bis (dimethoxymethylsilyl) methane, bis (diethoxymethylsilyl) methane, 1,2-bis (dimethoxymethyl) (Silyl) ethane, 1,2-bis (diethoxymethylsilyl) ethane, 1,2-bis (trimethoxysilyl) benzene, 1,2-bis (triethoxysilyl) benzene, 1,3-bis (trimethoxysilyl) )benzene,
1,3-bis (triethoxysilyl) benzene, 1,4
Preferred examples include -bis (trimethoxysilyl) benzene and 1,4-bis (triethoxysilyl) benzene. In the present invention, compound (1)
As (1) to (3), one or more kinds can be used.

When hydrolyzing and condensing at least one silane compound selected from the group consisting of the compounds (1) to (3), 0.1 mol / mol of the compounds (1) to (3) is used.
It is preferred to use more than 5 mol and up to 150 mol of water, particularly preferred to add more than 0.5 mol and 130 mol of water.

In producing the hydrolyzed condensate (A) of the present invention, a catalyst is used for hydrolyzing and condensing at least one silane compound selected from the group of the compounds (1) to (3). It is characterized by using. Examples of the catalyst that can be used at this time include a metal chelate compound, an acidic catalyst, and a basic catalyst.

Examples of the metal chelate compound include triethoxy mono (acetylacetonate) titanium, tri-n-propoxy mono (acetylacetonate) titanium, tri-i-propoxy mono (acetylacetonate) titanium, -N-butoxy mono (acetylacetonate) titanium, tri-sec-butoxy mono (acetylacetonate) titanium, tri-t-butoxy mono (acetylacetonate) titanium, diethoxy.
Bis (acetylacetonato) titanium, di-n-propoxybis (acetylacetonato) titanium, di-i-
Propoxy bis (acetylacetonate) titanium, di-n-butoxybis (acetylacetonate) titanium, di-sec-butoxybis (acetylacetonato) titanium, di-t-butoxybis (acetylacetonate) Titanium, monoethoxy-tris (acetylacetonato) titanium, mono-n-propoxy-tris (acetylacetonato) titanium, mono-i-propoxy.
Tris (acetylacetonate) titanium, mono-n-butoxytris (acetylacetonate) titanium, mono-sec-butoxytris (acetylacetonate)
Titanium, mono-t-butoxy tris (acetylacetonate) titanium, tetrakis (acetylacetonate)
Titanium, triethoxy mono (ethyl acetoacetate) titanium, tri-n-propoxy mono (ethyl acetoacetate) titanium, tri-i-propoxy mono (ethyl acetoacetate) titanium, tri-n-butoxy mono (ethyl acetoacetate) Acetate) titanium, tri-s
ec-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) titanium, di-n-butoxy bis (ethyl acetoacetate) titanium, di-sec-butoxy bis (ethyl acetoacetate) titanium, di-t
-Butoxy bis (ethyl acetoacetate) titanium,
Monoethoxy tris (ethyl acetoacetate) 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 (ethylacetoacetate) titanium, mono-t-butoxytris (ethylacetoacetate) titanium, tetrakis (ethylacetoacetate)
Titanium chelating compounds such as titanium, mono (acetylacetonate) tris (ethylacetoacetate) titanium, bis (acetylacetonate) bis (ethylacetoacetate) titanium, tris (acetylacetonate) mono (ethylacetoacetate) titanium; triethoxy・ Mono (acetylacetonate) zirconium, tri-
n-propoxy mono (acetylacetonato) zirconium, tri-i-propoxy mono (acetylacetonato) zirconium, tri-n-butoxy mono (acetylacetonato) zirconium, tri-sec-butoxy mono (acetylacetonate) Nart) zirconium,
Tri-t-butoxy mono (acetylacetonate) zirconium, diethoxybis (acetylacetonato) zirconium, di-n-propoxybis (acetylacetonato) zirconium, di-i-propoxy.
Bis (acetylacetonate) zirconium, di-n-
Butoxy bis (acetylacetonate) zirconium, di-sec-butoxy bis (acetylacetonate) zirconium, di-t-butoxybis (acetylacetonate) zirconium, monoethoxy tris (acetylacetonate) zirconium, mono -N-propoxy tris (acetylacetonate) zirconium, mono-i-propoxy tris (acetylacetonate) zirconium, mono-n-butoxy tris (acetylacetonate) zirconium, mono-sec-butoxy tris (acetyl) (Acetonate) zirconium, mono-t-butoxy tris (acetylacetonate) zirconium, tetrakis (acetylacetonate) zirconium, triethoxy mono (ethylacetoacetate) zirconium Tri -n- propoxy mono (ethylacetoacetate) 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 (ethylacetoacetate) zirconium, diethoxybis (ethylacetoacetate) zirconium, di-n-propoxybis (ethylacetoacetate) zirconium, di-i-propoxybis (ethylacetoacetate) zirconium, di- n-butoxybis (ethylacetoacetate) zirconium, di-sec-butoxybis (ethylacetoacetate) zirconium, di-t-butoxybis (ethylacetoacetate) zirconium, monoethoxytris (ethylacetoacetate) zirconium , Mono-n
-Propoxy tris (ethyl acetoacetate) zirconium, mono-i-propoxy tris (ethyl acetoacetate) 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 and tris (acetylacetonate) mono (ethylacetoacetate) zirconium; aluminum chelate compounds such as tris (acetylacetonate) aluminum and tris (ethylacetoacetate) aluminum; Is a chelate compound of titanium or aluminum, particularly preferably a chelate compound of titanium. These metal chelate compounds may be used alone or in combination of two or more.

Examples of the acidic catalyst include inorganic acids such as hydrochloric acid, nitric acid, sulfuric acid, hydrofluoric acid, phosphoric acid, boric acid and oxalic acid; 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, shikimic 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,
Of dichloroacetic acid, trichloroacetic acid, trifluoroacetic acid, formic acid, malonic acid, sulfonic acid, phthalic acid, fumaric acid, citric acid, tartaric acid, succinic acid, fumaric acid, itaconic acid, mesaconic acid, citraconic acid, malic acid, glutaric acid Organic acids such as hydrolysates, hydrolysates of maleic anhydride and hydrolysates of phthalic anhydride can be mentioned, and organic acids can be mentioned as more preferred examples. One or more of these acidic catalysts may be used simultaneously.

Examples of the basic catalyst include sodium hydroxide, potassium hydroxide, lithium hydroxide, pyridine,
Pyrrole, piperazine, pyrrolidine, piperidine, picoline, monoethanolamine, diethanolamine, dimethylmonoethanolamine, monomethyldiethanolamine, triethanolamine, diazabicyclooctane, diazabicyclononane, diazabicycloundecene, tetramethylammonium hydroxide, Tetraethylammonium hydroxide, tetrapropylammonium hydroxide, tetrabutylammonium hydroxide, ammonia, methylamine, ethylamine, propylamine, butylamine, pentylamine, hexylamine, pentylamine, octylamine, nonylamine, decylamine,
N, N-dimethylamine, N, N-diethylamine,
N, N-dipropylamine, N, N-dibutylamine,
Trimethylamine, triethylamine, tripropylamine, tributylamine, cyclohexylamine, trimethylimidine, 1-amino-3-methylbutane, dimethylglycine, 3-amino-3-methylamine, and the like, more preferably an organic amine Yes, ammonia, alkylamine and tetramethylammonium hydroxide are particularly preferred in view of the adhesion of the silica-based film to the substrate. One or two or more of these basic catalysts may be used simultaneously.

The amount of the above-mentioned catalyst to be used is as follows:
R in (3)¹ O-group, R^Two O-group, R ^Four An O-group and
R^Five Usually, based on 1 mol of the total amount of the group represented by the O- group,
0.00001 to 10 mol, preferably 0.00005
５5 mol. If the amount of catalyst used is within the above range,
There is little risk of polymer precipitation or gelation during the reaction. Ma
In the present invention, when the component (A) is hydrolyzed,
The temperature is usually 0 to 100 ° C, preferably 15 to 80 ° C.
You.

In the component (A), when each component is converted into a complete hydrolysis condensate, the compound (2) is 5 to 75% by weight, preferably 5 to 75% by weight, based on the total amount of the compounds (1) to (3). Is 10 to 70% by weight, more preferably 15 to 70% by weight
It is. Compounds (1) and / or (3)
95 to 25% by weight, preferably 90 to 30% by weight, more preferably 85 to 3% by weight, based on the total amount of the compounds (1) to (3)
0% by weight. Compound (2) is a compound (1)-
When the amount is 5 to 75% by weight based on the total amount of (3), the resulting coating film has a high elastic modulus and is particularly excellent in low dielectric properties. Here, in the present invention, the completely hydrolyzed condensate refers to R ¹ O—, R ² O—, R ⁴ O in compounds (1) to (3).
- group and R ⁵ O-group 100% hydrolyzed to the SiOH
It is a group that becomes a group and is further completely condensed to form a siloxane structure. In addition, the component (A) is preferably a hydrolyzed condensate of the compound (1) and the compound (2) because the composition obtained is more excellent in storage stability.

Component (B) The component (B) used in the present invention is silicon carbide particles. At this time, as a method of producing silicon carbide,
A method of heating silicon and carbon at a high temperature, a method of heating SiO ₂ and carbon at a high temperature, a method of heating SiH ₄ and C ₃ H ₈ at a high temperature in a hydrogen atmosphere, a method of heating SiCl ₄ and CH ₄ at a high temperature in a hydrogen atmosphere , -CH ₃ SiH-CH ₂ -
Can be heated in a vacuum or under an argon atmosphere at a high temperature. Examples of the method for forming particles from these materials include a method of mechanically pulverizing silicon carbide with a ball mill or the like, and a method of controlling the growth rate of particles by a CVD method to obtain particles. The average particle size of the silicon carbide particles obtained by these methods is 2 to 1
00 nm, more preferably 2 to 80 nm. When the average particle size exceeds 100 nm, the unevenness of the coating film becomes large, which is not preferable when used as an interlayer insulating film.

In the present invention, the proportion of the component (B) to the component (A) is from 0.1 to 100 parts by weight of the component (A) (in terms of a completely hydrolyzed condensate).
It is 30 parts by weight, more preferably 0.5 to 20 parts by weight. If the amount of the component (B) is less than 0.1 part by weight, the coating film will have poor resistance to CMP treatment, and if it exceeds 30 parts by weight, the uniformity of the coating film may be poor.

In the present invention, the silicon carbide particles include:
If desired, the particle surface can be used after being modified with a polymer. Examples of the polymer that modifies the surface of the silicon carbide particles include polymers described in JP-A-8-259876 and various commercially available polymers or oligomers for dispersion. The silicon carbide particles in the present invention can be made into a dispersion by using a dispersant in a solvent, if desired. Such dispersants include, for example, cationic, anionic,
Nonionic, amphoteric, silicone-based, and fluorine-based dispersants can be exemplified. As a specific example of the dispersant,
Polyoxyethylene alkyl ethers such as polyoxyethylene lauryl ether, polyoxyethylene stearyl ether and polyoxyethylene oleyl ether;
Polyoxyethylene alkyl phenyl ethers such as polyoxyethylene n-octyl phenyl ether and polyoxyethylene n-nonyl phenyl ether; polyethylene glycol diesters such as polyethylene glycol dilaurate and polyethylene glycol distearate; sorbitan fatty acid esters; Polyesters; tertiary amine-modified polyurethanes; polyethylene imines, etc., as well as KP (manufactured by Shin-Etsu Chemical Co., Ltd.), Polyflow (manufactured by Kyoeisha Chemical Co., Ltd.), F-top (Tochem Products Co., Ltd.) ), Megafac (Dainippon Ink and Chemicals, Inc.), Florard (Sumitomo 3M Ltd.), Asahi Guard, Surflon (above,
Asahi Glass Co., Ltd.), Disperbyk (Big Chemie Japan Co., Ltd.), Solsperse (Zeneca Corp.)
Manufactured). These dispersants can be used alone or in combination of two or more. The amount of the dispersant to be used is generally 50 parts by weight or less, preferably 30 parts by weight or less, based on 100 parts by weight of the silicon carbide particles.

(C) Organic Solvent The film forming composition of the present invention is obtained by dissolving or dispersing the component (A) and the component (B) in the organic solvent (C). Examples of the solvent that can be used at this time include at least one selected from the group consisting of alcohol solvents, ketone solvents, amide solvents, ester solvents, and aprotic solvents. Here, as the alcohol solvent, methanol, ethanol, n-propanol, i-
Propanol, n-butanol, i-butanol, se
c-butanol, t-butanol, n-pentanol,
i-pentanol, 2-methylbutanol, sec-pentanol, t-pentanol, 3-methoxybutanol, n-hexanol, 2-methylpentanol, se
c-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 alcohol, phenol,
Cyclohexanol, methylcyclohexanol, 3,
Monoalcohol solvents such as 3,5-trimethylcyclohexanol, benzyl alcohol, diacetone alcohol;

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, and tripropylene glycol; ethylene glycol monomethyl ether, ethylene glycol monoethyl ether, ethylene glycol monopropyl Ether, ethylene glycol monobutyl ether, ethylene glycol monohexyl ether, ethylene glycol monophenyl ether,
Ethylene glycol mono-2-ethyl butyl ether,
Diethylene glycol monomethyl ether, diethylene glycol monoethyl ether, diethylene glycol monopropyl ether, diethylene glycol monobutyl ether, diethylene glycol monohexyl 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,
Polyhydric alcohol partial ether solvents such as dipropylene glycol monopropyl ether; and the like. One or two of these alcohol solvents are used.
More than one species may be used simultaneously.

Examples of the ketone solvent include 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, 2-hexanone, methylcyclohexanone, 2,4
-In addition to pentanedione, acetonylacetone, acetophenone, fenchone, etc., acetylacetone, 2,
4-hexanedione, 2,4-heptanedione, 3,5
-Heptanedione, 2,4-octanedione, 3,5-
Octanedione, 2,4-nonanedione, 3,5-nonanedione, 5-methyl-2,4-hexanedione, 2,
2,6,6-tetramethyl-3,5-heptanedione,
Β-diketones such as 1,1,1,5,5,5-hexafluoro-2,4-heptanedione and the like can be mentioned.
These ketone solvents may be used alone or in combination of two or more.

As amide solvents, formamide, N
-Methylformamide, N, N-dimethylformamide, N-ethylformamide, N, N-diethylformamide, acetamide, N-methylacetamide,
N-dimethylacetamide, N-ethylacetamide,
N, N-diethylacetamide, N-methylpropionamide, N-methylpyrrolidone, N-formylmorpholine, N-formylpiperidine, N-formylpyrrolidine, N-acetylmorpholine, N-acetylpiperidine, N-acetylpyrrolidine and the like. Can be One or two or more of these amide solvents may be used simultaneously.

Examples of the ester solvents include diethyl carbonate, ethylene carbonate, propylene carbonate, 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, acetic acid 2-ethylbutyl, 2-ethylhexyl acetate, benzyl acetate,
Cyclohexyl acetate, methyl cyclohexyl acetate, n-nonyl acetate, methyl acetoacetate, ethyl acetoacetate, ethylene glycol monomethyl ether acetate, ethylene glycol monoethyl ether, diethylene glycol monomethyl ether acetate, diethylene glycol monoethyl acetate, diethylene glycol mono-acetate
n-butyl ether, propylene glycol monomethyl ether acetate, propylene glycol monoethyl ether acetate, propylene glycol monopropyl ether acetate, propylene glycol monobutyl ether acetate, dipropylene glycol monomethyl ether acetate, dipropylene glycol monoethyl ether acetate, glycol diacetate, acetic acid Methoxy triglycol, ethyl propionate, n-butyl propionate, i-amyl propionate, diethyl oxalate, di-n-butyl oxalate, methyl lactate, ethyl lactate, n-butyl lactate, n-amyl lactate, malonic acid Examples thereof include diethyl, dimethyl phthalate, and diethyl phthalate. These ester solvents include 1
Species or two or more species may be used simultaneously. Examples of aprotic solvents include acetonitrile, dimethyl sulfoxide, N, N, N ', N'-tetraethylsulfamide, hexamethylphosphoric triamide, N-methylmorpholone, N-methylpyrrole, N-ethylpyrrole, −
Methyl-Δ3-pyrroline, N-methylpiperidine, N-
Ethyl piperidine, N, N-dimethylpiperazine, N-
Methylimidazole, N-methyl-4-piperidone, N
-Methyl-2-piperidone, N-methyl-2-pyrrolidone, 1,3-dimethyl-2-imidazolidinone, 1,3
-Dimethyltetrahydro-2 (1H) -pyrimidinone. These solvents may be used alone or in combination.
More than one species may be used simultaneously.

The hydrolytic condensate used in the present invention is produced, for example, by dissolving the component (A) in a solvent, adding a catalyst and water, and performing hydrolysis. When the component (A) is hydrolyzed and condensed, the alkoxyl group 1 in the component (A)
It is preferable to use 0.8 to 20 moles of water per mole, and it is particularly preferable to add 0.8 to 15 moles of water. When the amount of water to be added is less than 0.8 mol, the crack resistance of the coating film is poor, and when it exceeds 20 mol, the coating uniformity of the coating film may be poor. In the present invention, the temperature at which the components (A) and (B) are hydrolyzed is usually from 0 to 100.
° C, preferably 15 to 80 ° C. The total solid content concentration of the hydrolysis condensate used in the present invention is preferably 2 to 3
It is 0% by weight and is appropriately adjusted depending on the purpose of use. When the total solid content of the composition is 2 to 30% by weight, the thickness of the coating film is in an appropriate range, and the storage stability is more excellent. The hydrolysis condensate used in the present invention may further contain the following components.

Other Additives The hydrolytic condensate used in the present invention further comprises colloidal silica, colloidal alumina, an organic polymer, a surfactant, a silane coupling agent, a triazene compound, a radical generator, Components such as a heavy bond-containing compound and a reactive triple bond-containing compound may be added. The colloidal silica is, for example, a dispersion liquid in which high-purity silicic anhydride is dispersed in the hydrophilic organic solvent.
-30 μm, preferably 10-20 μm, and a solid content concentration of about 10-40% by weight. Examples of such colloidal silica include, for example, Nissan Chemical Industries, Ltd.
And methanol sol and isopropanol silica sol; Examples of the colloidal alumina include alumina sols 520, 100, and 200 manufactured by Nissan Chemical Industries, Ltd .;
Alumina clear sol, alumina sol 10, and 132, manufactured by Kawaken Fine Chemical Co., Ltd., and the like. Examples of the organic polymer include a compound having a sugar chain structure, a vinylamide polymer, a (meth) acrylic polymer, an aromatic vinyl compound, a dendrimer, a polyimide,
Polyamic acid, polyarylene, polyamide, polyquinoxaline, polyoxadiazole, fluoropolymer,
Examples thereof include compounds having a polyalkylene oxide structure.

Examples of the compound having a polyalkylene oxide structure include a polymethylene oxide structure, a polyethylene oxide structure, a polypropylene oxide structure,
Examples include a polytetramethylene oxide structure and a polybutylene oxide structure. Specifically, polyoxymethylene alkyl ether, polyoxyethylene alkyl ether, polyoxyethylene alkylphenyl ether, polyoxyethylene sterol ether, polyoxyethylene lanolin derivative, ethylene oxide derivative of alkylphenol formalin condensate, polyoxyethylene polyether Oxypropylene block copolymers, ether compounds such as polyoxyethylene polyoxypropylene alkyl ethers, polyoxyethylene glycerin fatty acid esters, polyoxyethylene sorbitan fatty acid esters, polyoxyethylene sorbitol fatty acid esters, polyoxyethylene fatty acid alkanolamide sulfates and the like Ether ester type compound, polyethylene glycol fatty acid ester, ethylene glycol fat Esters, fatty acid monoglycerides, polyglycerol fatty acid esters, sorbitan fatty acid esters, propylene glycol fatty acid esters, and the like ether ester type compounds such as sucrose fatty acid esters. Examples of the polyoxyethylene polyoxypropylene block copolymer include compounds having the following block structures. - (A) j- (B) k- - (A) j- (B) k- (A) l- ( In the formula, A a group represented by -CH ₂ CH ₂ O-, the B -
And represents a group represented by CH ₂ CH (CH ₃ ) O—, wherein j is 1 to
90, k is a number from 10 to 99, and l is a number from 0 to 90) Among these, polyoxyethylene alkyl ether,
Polyoxyethylene polyoxypropylene block copolymer, polyoxyethylene polyoxypropylene alkyl ether, polyoxyethylene glycerin fatty acid ester, polyoxyethylene sorbitan fatty acid ester, polyoxyethylene sorbitol fatty acid ester,
And ether-type compounds such as those described above as more preferable examples. These may be used alone or in combination of two or more.

Examples of the surfactant include a nonionic surfactant, an anionic surfactant, a cationic surfactant, an amphoteric surfactant, and the like. Further, a fluorine-based surfactant, a silicone-based surfactant, and the like. Examples of the surfactant include a surfactant, a polyalkylene oxide-based surfactant, and a poly (meth) acrylate-based surfactant, and preferably a fluorine-based surfactant and a silicone-based surfactant.

As the fluorine-based surfactant, for example, 1,
1,2,2-tetrafluorooctyl (1,1,2,2-
Tetrafluoropropyl) ether, 1,1,2,2-tetrafluorooctylhexyl ether, octaethylene glycol di (1,1,2,2-tetrafluorobutyl)
Ether, hexaethylene glycol (1, 1, 2,
2,3,3-hexafluoropentyl) ether, octapropylene glycol di (1,1,2,2-tetrafluorobutyl) ether, hexapropylene glycol di (1,1,2,2,3,3-hexafluoro) Pentyl) ether, sodium perfluorododecyl sulfonate,
1,1,2,2,8,8,9,9,10,10-decafluorododecane, 1,1,2,2,3,3-hexafluorodecane, N- [3- (perfluorooctanesulfone Amido) propyl] -N, N′-dimethyl-N-carboxymethyleneammonium betaine, perfluoroalkylsulfonamidopropyltrimethylammonium salt,
At least one of terminal, main chain and side chain of perfluoroalkyl-N-ethylsulfonylglycine salt, bis (N-perfluorooctylsulfonyl-N-ethylaminoethyl) phosphate, monoperfluoroalkylethyl phosphate, etc. And a fluorine-based surfactant composed of a compound having a fluoroalkyl or fluoroalkylene group at the position (1). Commercially available products are MegaFac F142D, F172, F173, F1
83 (manufactured by Dainippon Ink and Chemicals, Inc.), F-Top EF301, 303, and 352 (manufactured by Shin-Akita Chemical Co., Ltd.), Florad FC-430, and FC-431
(Manufactured by Sumitomo 3M Limited), Asahi Guard AG71
0, Surflon S-382, SC-101, SC-
102, SC-103, SC-104, SC-1
05, SC-106 (manufactured by Asahi Glass Co., Ltd.), BM-10
00, BM-1100 (manufactured by Yusho Co., Ltd.), NBX-15
(Neos Co., Ltd.) and other commercially available fluorosurfactants. Among them, the above MegaFac F172, BM-1000, BM-11
00, NBX-15 is particularly preferred.

Examples of the silicone-based surfactant include SH7PA, SH21PA, SH30PA, and ST94P.
A (All are Dow Corning Toray Silicone Co., Ltd.)
And the like can be used. The amount of surfactant used is
It is usually 0.0001 to 10 parts by weight based on 100 parts by weight (completely hydrolyzed condensate) of the components (A) and (B). These may be used alone or in combination of two or more.

As the silane coupling agent, for example, 3
-Glycidyloxypropyltrimethoxysilane, 3-aminoglycidyloxypropyltriethoxysilane, 3-
Methacryloxypropyltrimethoxysilane, 3-glycidyloxypropylmethyldimethoxysilane, 1-methacryloxypropylmethyldimethoxysilane, 3-aminopropyltrimethoxysilane, 3-aminopropyltriethoxysilane, 2-aminopropyltrimethoxysilane, 2-aminopropyltriethoxysilane, N-
(2-aminoethyl) -3-aminopropyltrimethoxysilane, N- (2-aminoethyl) -3-aminopropylmethyldimethoxysilane, 3-ureidopropyltrimethoxysilane, 3-ureidopropyltriethoxysilane, N- Ethoxycarbonyl-3-aminopropyltrimethoxysilane, N-ethoxycarbonyl-3-aminopropyltriethoxysilane, N-triethoxysilylpropyltriethylenetriamine, N-triethoxysilylpropyltriethylenetriamine, 10-trimethoxysilyl- 1,4,7-triazadecane, 10-
Triethoxysilyl-1,4,7-triazadecane, 9
-Trimethoxysilyl-3,6-diazanonyl acetate, 9-triethoxysilyl-3,6-diazanonyl acetate, N-benzyl-3-aminopropyltrimethoxysilane, N-benzyl-3-aminopropyltriacetate Ethoxysilane, N-phenyl-3-aminopropyltrimethoxysilane, N-phenyl-3-aminopropyltriethoxysilane, N-bis (oxyethylene) -3-
Aminopropyltrimethoxysilane, N-bis (oxyethylene) -3-aminopropyltriethoxysilane and the like can be mentioned. These may be used alone or in combination of two or more.

As the triazene compound, for example, 1,
2-bis (3,3-dimethyltriazenyl) benzene,
1,3-bis (3,3-dimethyltriazenyl) benzene, 1,4-bis (3,3-dimethyltriazenyl) benzene, bis (3,3-dimethyltriazenylphenyl) ether, bis ( 3,3-dimethyltriazenylphenyl) methane, bis (3,3-dimethyltriazenylphenyl) sulfone, bis (3,3-dimethyltriazenylphenyl) sulfide, 2,2-bis [4- (3 ,
3-dimethyltriazenylphenoxy) phenyl]-
1,1,1,3,3,3-hexafluoropropane,
2,2-bis [4- (3,3-dimethyltriazenylphenoxy) phenyl] propane, 1,3,5-tris (3,3-dimethyltriazenyl) benzene, 2,7-
Bis (3,3-dimethyltriazenyl) -9,9-bis [4- (3,3-dimethyltriazenyl) phenyl] fluorene, 2,7-bis (3,3-dimethyltriazenyl)- 9,9-bis [3-methyl-4- (3,3-dimethyltriazenyl) phenyl] fluorene, 2,7-bis (3,3-dimethyltriazenyl) -9,9-bis [3- Phenyl-4- (3,3-dimethyltriazenyl) phenyl] fluorene, 2,7-bis (3,3-dimethyltriazenyl) -9,9-bis [3-propenyl-4- (3,3 -Dimethyltriazenyl) phenyl] fluorene, 2,7-bis (3,3-dimethyltriazenyl) -9,9-bis [3-fluoro-4- (3,3-dimethyltriazenyl) phenyl] Fluorene, 2,7-
Bis (3,3-dimethyltriazenyl) -9,9-bis [3,5-difluoro-4- (3,3-dimethyltriazenyl) phenyl] fluorene, 2,7-bis (3,3
-Dimethyltriazenyl) -9,9-bis [3-trifluoromethyl-4- (3,3-dimethyltriazenyl)
Phenyl] fluorene and the like. These may be used alone or in combination of two or more.

Examples of the radical generator include isobutyryl peroxide, α, α'bis (neodecanoylperoxy) diisopropylbenzene, cumylperoxyneodecanoate, di-n-propylperoxydicarbonate and diisopropylperoxy. Dicarbonate,
1,1,3,3-tetramethylbutyl peroxy neodecanoate, bis (4-t-butylcyclohexyl) peroxy dicarbonate, 1-cyclohexyl-1-methylethyl peroxy neodecanoate, di-2 -Ethoxyethyl peroxydicarbonate, di (2-ethylhexylperoxy) dicarbonate, t-hexylperoxyneodecanoate, dimethoxybutylperoxydicarbonate, di (3-methyl-3-methoxybutylperoxy) Dicarbonate, t-butylperoxy neodecanoate, 2,4-dichlorobenzoyl peroxide, t-hexylperoxypivalate, t-butylperoxypivalate, 3,5,5-trimethylhexanoyl peroxide, Octanoyl peroxide, lauroyl par Oxide, stearoyl peroxide, 1,1,3,3-tetramethylbutylperoxy 2-ethylhexanoate, succinic peroxide, 2,5-dimethyl-2,5-di (2-ethylhexanoylperoxy ) Hexane, 1-cyclohexyl-
1-methylethyl peroxy 2-ethylhexanoate, t-hexylperoxy 2-ethylhexanoate, t-butylperoxy 2-ethylhexanoate,
m-toluoyl and benzoyl peroxide, benzoyl peroxide, t-butylperoxyisobutyrate, di-t-butylperoxy-2-methylcyclohexane, 1,1-bis (t-hexylperoxy)-
3,3,5-trimethylcyclohexane, 1,1-bis (t-hexylperoxy) cyclohexane, 1,1-
Bis (t-butylperoxy) -3,3,5-trimethylcyclohexane, 1,1-bis (t-butylperoxy) cyclohexane, 2,2-bis (4,4-di-t-
Butylperoxycyclohexyl) propane, 1,1-
Bis (t-butylperoxy) cyclodecane, t-hexylperoxyisopropyl monocarbonate, t-butylperoxymaleic acid, t-butylperoxy-
3,3,5-trimethylhexanoate, t-butylperoxylaurate, 2,5-dimethyl-2,5-di (m-toluoylperoxy) hexane, t-butylperoxyisopropyl monocarbonate, t -Butylperoxy 2-ethylhexyl monocarbonate, t-hexylperoxybenzoate, 2,5-dimethyl-
2,5-di (benzoylperoxy) hexane, t-butylperoxyacetate, 2,2-bis (t-butylperoxy) butane, t-butylperoxybenzoate, n-butyl-4,4-bis ( t-butylperoxy) valerate, di-t-butylperoxyisophthalate, α, α′-bis (t-butylperoxy) diisopropylbenzene, dicumyl peroxide, 2,5-
Dimethyl-2,5-di (t-butylperoxy) hexane, t-butylcumyl peroxide, di-t-butyl peroxide, p-menthane hydroperoxide,
2,5-dimethyl-2,5-di (t-butylperoxy) hexyne-3, diisopropylbenzene hydroperoxide, t-butyltrimethylsilyl peroxide, 1,1,3,3-tetramethylbutyl hydroperoxide, Cumene hydroperoxide, t-hexyl hydroperoxide, t-butyl hydroperoxide, dibenzyl, 2,3-dimethyl-2,3-diphenylbutane, α, α′-dimethoxy-α, α′-diphenylbibenzyl, α, α′-diphenyl-α-methoxybibenzyl, α, α′-diphenyl-α, α′-dimethoxybibenzyl, α, α′-dimethoxy-α, α′-dimethylbibenzyl, α, α′- Dimethoxybibenzyl,
Examples thereof include 3,4-dimethyl-3,4-diphenyl-n-hexane and 2,2,3,3-tetraphenylsuccinic nitrile. These are one or two
More than one species may be used simultaneously.

Examples of the compound containing a reactive double bond include allylbenzene, diallylbenzene, triallylbenzene, allyloxybenzene, diallyloxybenzene, triallyloxybenzene, α, w-diallyloxyalkanes, α, w- Diallyl alkenes, α, w-diallyl alkenes, allylamine, diallylamine, triallylamine, N-allylphthalimide, N-allylpyromellitimide, N, N′-diallylurea, triallyl isocyanurate, 2,2′-diallylbisphenol Allyl compounds such as A; styrene, divinylbenzene, trivinylbenzene, stilbene, propenylbenzene, dipropenylbenzene, tripropenylbenzene, phenylvinylketone, methylstyrylketone,
α, w-divinylalkanes, α, w-divinylalkenes, α, w-divinylalkynes, α, w-divinyloxyalkanes, α, w-divinylalkenes, α, w-divinylalkynes, α , W-diacryloxyalkanes, α, w-diacrylalkenes, α, w-diacrylalkenes, α, w-dimethacryloxyalkanes,
α, w-dimethacrylalkenes, α, w-dimethacrylalkenes, bisacryloxybenzene, trisacryloxybenzene, bismethacryloxybenzene,
Vinyl compounds such as tris methacryloxybenzene, N-vinylphthalimide, and N-vinylpyromellitimide; polyarylene ethers containing 2,2′-diallyl-4,4′-biphenol, 2,2′-diallyl-4
Polyarylene containing 4'-biphenol can be exemplified. These may be used alone or in combination of two or more.

Examples of the reactive triple bond-containing compound include ethynylbenzene, diethynylbenzene, triethynylbenzene, trantrimethylsilylethynylbenzene, trimethylsilylethynylbenzene, bis (trimethylsilylethynyl) benzene, tris (trimethylsilylethynyl) benzene, phenylethynyl benzene,
Bis (phenylethynyl) benzene, tris (phenylethynyl) benzene, bis (ethynylphenyl) ether, bis (trimethylsilylethynylphenyl) ether, bis (phenylethynylphenyl) ether, and the like can be given. These may be used alone or in combination of two or more.

In the present invention, the content of the alcohol having a boiling point of 100 ° C. or less in the composition for film formation is 20% by weight or less,
In particular, it is preferably at most 5% by weight. Boiling point 100 ° C
The following alcohols may be generated during the hydrolysis of the component (A) and / or its condensation, and should be removed by distillation or the like so that the content is 20% by weight or less, preferably 5% by weight or less. Is preferred.

The total solid content of the composition of the present invention thus obtained is preferably 2 to 30% by weight.
It is adjusted appropriately according to the purpose of use. When the total solid content of the composition is 2 to 30% by weight, the thickness of the coating film is in an appropriate range, and the storage stability is more excellent. The adjustment of the total solid concentration is performed by concentration and dilution with the above (C) organic solvent, if necessary.

When the composition of the present invention is applied to a silicon wafer, Si
When applying to a substrate such as an O ₂ wafer or a SiN wafer, a coating method such as spin coating, dipping, roll coating, or spraying is used. The film thickness at this time is about 0.05 to 2.5 μm in a single coating as a dry film thickness, and a coating film of about 0.1 to 5.0 μm in a double coating can be formed. . Then, it is dried at room temperature, or at a temperature of about 80 to 600 ° C., usually for 5 to 240 ° C.
By heating and drying for about a minute, a glassy or macromolecular insulating film can be formed. As a heating method at this time, a hot plate, an oven, a furnace, or the like can be used. As a heating atmosphere, the heating is performed in the atmosphere, a nitrogen atmosphere, an argon atmosphere, a vacuum, a reduced pressure in which the oxygen concentration is controlled, or the like. Can be. Further, the coating film can be formed by irradiating an electron beam or an ultraviolet ray. Further, in order to control the curing speed of the coating film, if necessary, heating may be performed stepwise, or an atmosphere such as nitrogen, air, oxygen, or reduced pressure may be selected. Furthermore, the relative permittivity of the silica-based film of the present invention is usually 3.0 to 1.2, preferably 3.0 to 1.8, and more preferably 3.0 to 2.0.

The interlayer insulating film thus obtained exhibits a lower relative dielectric constant, and is superior in mechanical strength and CMP resistance of the coating film.
Interlayer insulating film for semiconductor devices such as SDRAM, RDRAM, D-RDRAM, etc., etching stopper film, protective film such as surface coat film of semiconductor device, intermediate layer in semiconductor manufacturing process using multilayer resist, interlayer insulating film for multilayer wiring board ,
It is useful for applications such as protective films and insulating films for liquid crystal display elements.

[0049]

EXAMPLES Hereinafter, the present invention will be described more specifically with reference to examples. However, the following description generally shows an 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 are parts by weight and% by weight, respectively, unless otherwise specified. Also,
Various evaluations were performed as follows.

The weight average molecular weight (Mw) was measured by gel permeation chromatography (GPC) under the following conditions. Sample: Prepared by dissolving 1 g of a hydrolyzed condensate in 100 cc of tetrahydrofuran using tetrahydrofuran as a solvent. Standard polystyrene: Standard polystyrene manufactured by Pressure Chemical Co., USA was used. Apparatus: High-temperature, high-speed gel permeation chromatogram (model 150-C ALC / GPC) manufactured by Waters, Inc. Column: SHOdex A-80M manufactured by Showa Denko KK
(Length 50cm) Measurement temperature: 40 ° C Flow rate: 1cc / min

A composition sample was applied on a silicon wafer having a relative dielectric constant of 8 inches by a spin coating method, and the substrate was dried on a hot plate at 90 ° C. for 3 minutes and in a nitrogen atmosphere at 200 ° C. for 3 minutes. The substrate was baked on a hot plate in a nitrogen atmosphere at 45 ° C. for 45 minutes. An aluminum electrode pattern was formed on the obtained film by a vapor deposition method to prepare a sample for relative dielectric constant measurement. The sample is taken at a frequency of 100 kHz,
HP1645, manufactured by Yokogawa Hewlett-Packard Co., Ltd.
The relative dielectric constant of the coating film was measured by a CV method using a 1B electrode and an HP4284A precision LCR meter.

Mechanical strength (elastic modulus) A composition sample is applied on an 8-inch silicon wafer by spin coating, and the substrate is dried on a hot plate at 90 ° C. for 3 minutes and in a nitrogen atmosphere at 200 ° C. for 3 minutes. Then, the substrate was baked on a nitrogen atmosphere hot plate at 420 ° C. for 45 minutes. The modulus of elasticity of the obtained film was measured using Nanoindenter X.
Using P (manufactured by Nano Instruments), it was measured by a continuous rigidity measurement method.

A composition sample is applied on a CMP resistant 8-inch silicon wafer by using a spin coating method, and the substrate is dried on a hot plate at 90 ° C. for 3 minutes and in a nitrogen atmosphere at 200 ° C. for 3 minutes. The substrate was baked for 45 minutes on a hot plate in a nitrogen atmosphere. The obtained coating film was polished under the following conditions. Slurry: silica-hydrogen peroxide polishing pressure: 300 g / cm ² polishing time: 180 seconds The appearance of the coating film after CMP was measured with a defect inspection device (KLA Tencor, KLA2132) and evaluated according to the following criteria. ：: 100 or less scratches with a size of 0.2 μm or more on the wafer ×: 100 or more scratches with a size of 0.2 μm or more on the wafer

Synthesis Example 1 In a quartz separable flask, 276.01 g of methyltrimethoxysilane and 86.14 of tetramethoxysilane were used.
g and 0.0092 g of tetrakis (acetylacetonato) titanium were dissolved in 101 g of propylene glycol monoethyl ether, and then stirred with a three-one motor to stabilize the solution temperature at 55 ° C. Next, a mixed solution of 225.52 g of ion-exchanged water and 263.00 g of propylene glycol monoethyl ether was added to the solution over 1 hour. Then, after reacting at 55 ° C. for 4 hours, 48.12 g of acetylacetone was added, the reaction was further performed for 30 minutes, and the reaction solution was cooled to room temperature. 50 ℃
227 g of a solution containing methanol and water was removed from the reaction solution by evaporation to obtain a reaction solution. The weight average molecular weight of the condensate and the like thus obtained was 1,230.

Synthesis Example 2 In a quartz separable flask, 205.50 g of methyltrimethoxysilane and 85.51 of tetramethoxysilane were used.
g of propylene glycol monoethyl ether 426
g, then stirred with a three-one motor,
The solution temperature was stabilized at 50 ° C. Next, succinic acid 0.63
182 g of ion-exchanged water in which g was dissolved was added to the solution over 1 hour. Then, after reacting at 50 ° C. for 3 hours, the reaction solution was cooled to room temperature. At 50 ° C., 360 g of a solution containing methanol was removed from the reaction solution by evaporation to obtain a reaction solution. The weight average molecular weight of the condensate and the like thus obtained was 1,400.

Synthesis Example 3 Distilled ethanol 370 was placed in a quartz separable flask.
g, distilled propylene glycol monopropyl ether 2
00 g, 160 g of ion-exchanged water and 90 g of a 10% aqueous solution of methylamine were added and stirred uniformly. 136 g of methyltrimethoxysilane and tetraethoxysilane 2 were added to this solution.
09 g of the mixture were added. The reaction was performed for 2 hours while keeping the solution at 52 ° C. 300 g of propylene glycol monopropyl ether was added to this solution, and then 5 g
The solution was concentrated using an evaporator at 0 ° C. until the solution became 10% (in terms of a completely hydrolyzed condensate).
0% propylene glycol monopropyl ether solution 1
0 g was added to obtain a reaction solution. The weight average molecular weight of the condensate and the like thus obtained was 904,00.

Synthesis Example 4 Distilled ethanol 428 was placed in a quartz separable flask.
g, 215 g of ion-exchanged water and 15.6 g of a 25% aqueous solution of tetramethylammonium hydroxide were uniformly stirred. To this solution, add methyltrimethoxysilane 4
A mixture of 0.8 g and 61.4 g of tetraethoxysilane was added. The reaction was performed for 2 hours while keeping the solution at 57 ° C. 300 g of propylene glycol monopropyl ether was added to this solution, and then the solution was concentrated to 10% (complete hydrolyzed condensate) using an evaporator at 50 ° C., and then 10% propylene glycol monopropyl maleate was added. 20 g of an ether solution was added to obtain a reaction solution. The weight average molecular weight of the condensate and the like thus obtained was 1,600,00.

Dispersion Example 1 SiCl ₄ and CH ₄ gas were subjected to CV at 1300 ° C. in a hydrogen atmosphere.
By using Method D, silicon carbide particles having an average particle size of 50 nm were obtained. 100 g of the obtained silicon carbide particles, 10 g of polyoxyethylene stearyl ether, and 890 g of propylene glycol monopropyl ether were mixed and sufficiently dispersed using a paint shaker to obtain a dispersion.

Example 1 10 g of the dispersion was added to 100 g of the reaction solution obtained in Synthesis Example 1.
Was added, and the mixture was sufficiently stirred. This solution was filtered through a Teflon (registered trademark) filter having a pore size of 0.2 μm to obtain a film-forming composition of the present invention. The obtained composition was applied on a silicon wafer by a spin coating method. The relative dielectric constant of the coating film at room temperature was a low value of 2.77. In addition, when the elastic modulus of the coating film was measured, it was 10.3 GPa, which was excellent in mechanical strength. Furthermore, when the coating film was subjected to a defect inspection after the CMP treatment, the number of scratches was 100 or less.

Examples 2 to 8 Evaluations were made in the same manner as in Example 1 except that the reaction solution shown in Table 1 and the component (B) were used. The evaluation results are also shown in Table 1.

[0061]

[Table 1]

Comparative Example 1 A coating film was evaluated in the same manner as in Example 1 except that only the reaction solution obtained in Synthesis Example 1 was used. The relative dielectric constant of the coating film at room temperature was as low as 2.71, but the elastic modulus of the coating film was as low as 5.6 Gpa. In addition, CMP
When a defect inspection was performed after the treatment, 340 scratches were found.

Comparative Example 2 A coating film was evaluated in the same manner as in Example 1 except that only the reaction solution obtained in Synthesis Example 3 was used. The relative dielectric constant of the coating film at room temperature was a low value of 2.29, but the elastic modulus of the coating film was a low value of 4.1 Gpa. In addition, CMP
When a defect inspection was performed after the treatment, 690 scratches were found.

[0064]

According to the present invention, by using a film-forming composition containing an alkoxysilane hydrolyzed polymer, silicon carbide particles and an organic solvent, a low dielectric constant is exhibited and the mechanical properties of the coating film are reduced. It is possible to provide a film-forming composition (material for an interlayer insulating film) having excellent strength and CMP resistance.

──────────────────────────────────────────────────続 き Continued on the front page (51) Int.Cl. ⁷ Identification symbol FI Theme coat ゛ (Reference) C09D 183/14 C09D 183/14 H01B 3/46 H01B 3/46 DE H01L 21/312 H01L 21/312 C F-term (reference) 4J002 CP031 DJ006 GQ01 4J038 DL021 DL031 DL041 DL071 DL161 GA01 GA07 HA096 HA176 HA336 HA376 HA416 HA436 HA476 JA37 JA38 JA39 JA42 JB01 JB03 JB09 JB27 JB29 JB30 JC13 JC38 KA04 MA07 AC05 MA05 AC07 AD06 AD07 AH02 5G305 AA07 AA11 AB10 AB15 AB18 BA09 CA26 CC05 CD01 CD12

Claims (5)

[Claims] (A) (A-1) a compound represented by the following general formula (1): R _a Si (OR ¹ ) _4-a (1) wherein R is hydrogen An atom, a fluorine atom or a monovalent organic group, R ¹ is a monovalent organic group, and a is an integer of 1 to 2.) (A-2) a compound represented by the following general formula (2); (OR ² ) ₄ (2) (wherein, R ² represents a monovalent organic group.) (A-3) Compound represented by the following general formula (3) R ³ _b (R _{^{4 O) 3-b Si- (}} R 7) d -Si (oR 5) 3-c R 6 c ····· (3) wherein, R ³ to R ⁶ are same or different and each represents a monovalent Organic groups, b to c are the same or different, and an integer of 0 to 2,
R ⁷ is an oxygen atom, a phenylene group or — (CH ₂ ) _n —
(Where n is an integer of 1 to 6), d
Represents 0 or 1. At least one selected from the group of
A film forming composition comprising: a hydrolyzed condensate obtained by hydrolyzing and condensing a kind compound in the presence of a catalyst; (B) silicon carbide particles; and (C) an organic solvent. 2. The content of the component (B) relative to the component (A) is 0.1 to 30 parts by weight of the component (B) based on 100 parts by weight of the component (A) (in terms of a completely hydrolyzed condensate). The composition for forming a film according to claim 1, wherein: 3. The component (B) has an average particle size of 2 to 100 nm.
The composition for forming a film according to claim 1, wherein 4. The catalyst for hydrolysis of the component (A) is at least one selected from the group consisting of a metal chelate compound, an acidic catalyst and a basic catalyst.
The composition for forming a film according to the above. 5. An insulating film forming material comprising the film forming composition according to claim 1. Description: