JP5019742B2 - Cyclic siloxane compound, Si-containing film forming material, and use thereof - Google Patents

Description

  The present invention relates to a Si-containing film forming material and the like, and more particularly to a low dielectric constant interlayer insulating film material used in a multilayer wiring technique in logic ULSI. In particular, the present invention relates to a Si-containing film-forming material containing a cyclic siloxane compound for plasma polymerization and its use.

  In the manufacturing technology of the integrated circuit field of the electronics industry, there is an increasing demand for high integration and high speed. In silicon ULSIs, especially logic ULSIs, the performance of wiring connecting them is a problem rather than the performance due to miniaturization of MOSFETs. That is, in order to solve the wiring delay problem associated with the multilayer wiring, it is required to reduce the wiring resistance and between the wirings and the interlayer capacitance.

  For these reasons, it is essential to introduce copper wiring with lower electrical resistance and migration resistance instead of aluminum wiring, which is currently used in most integrated circuits. Sputtering or chemical vapor deposition A process of performing copper plating after seed formation by a method (hereinafter abbreviated as CVD) is being put into practical use.

There are various proposals for low dielectric constant interlayer insulating film materials. As the prior art, silicon dioxide (SiO ₂ ), silicon nitride, phosphosilicate glass has been used for inorganic systems, and polyimide has been used for organic systems. Recently, however, a tetralayer has been previously prepared for the purpose of obtaining a more uniform interlayer insulating film. Hydrolysis of ethoxysilane monomer, that is, polycondensation to obtain SiO ₂ and proposal to use it as a coating material called inorganic spin on glass (inorganic SOG), or polysiloxane obtained by polycondensation of organic alkoxysilane monomer to organic There are proposals for use as SOG.

  Further, as an insulating film forming method, an insulating film polymer solution is applied by a spin coating method or the like, and a coating type in which a film is formed and a plasma in a plasma enhanced chemical vapor deposition (PECVD) apparatus. There are two methods, a CVD method in which a film is formed by polymerization.

  As a proposal of the PECVD method, for example, in Patent Document 1, a method of forming a trimethylsilane oxide thin film from trimethylsilane and oxygen by PECVD is used, and in Patent Document 2, straight lines such as methyl, ethyl, and n-propyl are used. There has been proposed a method for forming an alkyl oxide silane thin film by PECVD from an alkoxysilane having an alkynyl and aryl group such as chain alkyl and vinylphenyl. These conventional PECVD process materials have good adhesion to barrier metal and copper wiring material, but the uniformity of the film is a problem, film formation speed, relative dielectric constant There were cases where there was insufficient.

  As a proposal of PECVD using cyclic siloxane, for example, in Patent Document 3, a method using tetramethylcyclotetrasiloxane is used, and in Patent Document 4, tetraalkylcyclotetrasiloxane, tetraaminocyclotetrasiloxane, octaalkylcyclotetra. A method using siloxane or octaaminocyclotetrasiloxane has been proposed. In these methods, cyclic siloxane is used as a raw material compound, and while maintaining the cyclic structure in the generated thin film, it is intended to form vacancies in the generated thin film and lower the relative dielectric constant. However, according to the knowledge of the present inventor, when a PECVD film is formed using these substituted cyclic siloxanes, a thin film having a relative dielectric constant of less than 2.7 cannot be obtained. This is presumably because the cyclic siloxane compound easily breaks the cyclic structure in plasma to form a chain structure and does not contribute to the formation of a thin film.

  Patent Document 5 proposes a hexamembered cyclosiloxane such as hexamethylcyclotrisiloxane and 1,3,5-trimethyl-1,3,5-trivinylcyclotrisiloxane, and Patent Document 6 discloses bisbenzocyclobutene. There is a proposal to copolymerize a substituted disiloxane compound and an 8-membered cyclic siloxane 1,3,5,7-tetramethyl-1,3,5,7-tetravinylcyclotetrasiloxane in a plasma atmosphere. However, according to the knowledge of the present inventor, a thin film having a relative dielectric constant of less than 2.5 cannot be obtained by the method using a cyclic siloxane substituted with vinyl and / or methyl according to these proposals.

In Patent Document 7 and Patent Document 8, a PECVD method low dielectric constant thin film forming method using a porous agent is proposed. In the former, triethoxysilane, diethoxymethylsilane, and α-terpinene as a porous agent are supplied into the PECVD apparatus chamber, and after PECVD film formation,
A method for reducing the dielectric constant is proposed by annealing at a temperature of 400 ° C. or more and volatilizing the component derived from α-terpinene in the thin film. In the latter, cyclo-1,3,5,7-tetrasilylene-2,6-dioxy-4,8-dimethylene, a vinyl furyl ether as a porous agent, and nitrous oxide as an oxidizing agent are supplied into a PECVD apparatus chamber. Then, after PECVD film formation, a method of annealing is performed at a temperature of 400 ° C. or higher to volatilize a component derived from vinyl furyl ether in the thin film to reduce the dielectric constant is proposed. Although these methods can be expected to reduce the dielectric constant due to porosity, the matrix of the thin film is destroyed because the porous material is removed from the thin film by post-processing from the thin film once formed. The composition inside the film becomes non-uniform, the mechanical strength such as rigidity and Young's modulus decreases, and the formed holes become continuous open holes, preventing the diffusion of metal components into the film. It has no problem.

  On the other hand, as a coating type proposal, although the uniformity of the film is good, three steps of coating, solvent removal, and heat treatment are necessary, which is economically disadvantageous than CVD materials, and barrier metal, wiring In many cases, adhesion to a copper wiring material, which is a material, and uniform application of a coating liquid to a miniaturized substrate structure itself are problems.

Moreover, in the coating type material, the method of using a porous material in order to implement | achieve the Ultra Low-k material whose relative dielectric constant is 2.5 or less and also 2.0 or less is proposed. Organic or inorganic material matrix readily disperse the thermally decomposed organic component particles in the method of heat treating and pore formation, silicon and oxygen by evaporating SiO ₂ ultrafine particles formed by evaporation in a gas, SiO ₂ than There is a method of forming a fine particle thin film. However, although these porous methods are effective for lowering the dielectric constant, the mechanical strength decreases, chemical mechanical polishing (CMP) becomes difficult, and the dielectric constant increases due to moisture absorption. And wiring corrosion could be caused.

  Therefore, the market is further seeking a well-balanced material that meets all the required performance such as low dielectric constant, sufficient mechanical strength, adhesion to barrier metal, copper diffusion prevention, plasma ashing resistance, moisture resistance, etc. As a method of satisfying these required performances with a certain degree of balance, a material having an intermediate characteristic between an organic polymer and an inorganic polymer has been proposed in an organic silane material by increasing the carbon ratio of the organic substituent to silane. . For example, in Patent Document 9, a coating solution obtained by hydrolyzing and condensing a silicon compound having an adamantyl group in the presence of an acidic aqueous solution by a sol-gel method is used, and an interlayer having a relative dielectric constant of 2.4 or less without being made porous. A method for obtaining an insulating film is proposed. However, this material is a coating type material, and still has the problem of the film forming method using the coating type as described above.

JP 2002-110670 A JP-A-11-288931 Japanese Patent No. 20678801 JP-A-5-279856 International Publication No. 03/019645 Pamphlet JP 2004-47873 A Japanese Patent Laid-Open No. 2005-19980 JP 2001-298023 A JP 2000-302791 A

  The present invention has been made in view of the above problems, and its object is to provide a novel Si-containing film forming material, particularly a low dielectric constant insulating film material containing a cyclic siloxane compound suitable for a PECVD apparatus. It is another object of the present invention to provide a Si-containing film using the same and a semiconductor device including these films.

  The present inventors have found that a cyclic siloxane compound having a substituent containing a hetero atom is suitable as an insulating film, particularly as a low dielectric constant interlayer insulating film material for a semiconductor device, and has completed the present invention. It was.

  That is, the present invention provides the following general formula (1)

（式中、Ａは、酸素原子、ホウ素原子、及び窒素原子からなる群から選ばれた少なくとも一種を含む基を表し、Ｒ^１は、水素原子または炭化水素基を表す。ｎは、１または２を表し、ｘは、２乃至１０の整数を表す。）で示される環状シロキサン化合物を含有することを特徴とする、
Ｓｉ含有膜形成材料である。

(In the formula, A represents a group containing at least one selected from the group consisting of an oxygen atom, a boron atom, and a nitrogen atom, R ¹ represents a hydrogen atom or a hydrocarbon group, and n represents 1 or 2) Wherein x represents an integer of 2 to 10.), and a cyclic siloxane compound represented by
Si-containing film forming material.

  Moreover, this invention is a manufacturing method of Si containing film characterized by using the above-mentioned Si containing film forming material as a raw material. Moreover, this invention is a Si containing film characterized by the above-mentioned manufacturing method. The present invention is also a method for producing a Si-containing film, characterized by subjecting the above-mentioned Si-containing film to heat treatment, ultraviolet irradiation treatment, or electron beam treatment. Moreover, this invention is a Si containing film characterized by the above-mentioned manufacturing method. Moreover, this invention is a semiconductor device characterized by using the above-mentioned Si containing film as an insulating film.

  Furthermore, the present invention provides the following general formula (20)

（式中、Ｒ^１８は炭化水素基を表し、Ｒ^１９は水素原子又は炭化水素基を表す。ｇは２乃至１０の整数を表し、ｈは１乃至３の整数を表す。）で示されることを特徴とする環状シロキサン化合物である。

(Wherein R ¹⁸ represents a hydrocarbon group, R ¹⁹ represents a hydrogen atom or a hydrocarbon group, g represents an integer of 2 to 10, and h represents an integer of 1 to 3). Is a cyclic siloxane compound characterized by

  Details of the present invention will be described below.

In the present invention, R ¹ and R ² , R ⁴ , R ⁶ , R ⁸ , R ⁹ , R ¹⁰ , R ¹¹ , R ¹² , R ¹³ , R ¹⁴ , R ¹⁵ , R ¹⁶ , R ¹⁷ , R described below ^The hydrocarbon group represented by ¹⁸ or R ¹⁹ is preferably a saturated or unsaturated hydrocarbon group having 1 to 20 carbon atoms, and may have any of a linear, branched or cyclic structure. In the following general formulas (3), (5), and (7), when p, q, or r is 2 or more, they may be bonded to each other to form a cyclic structure. When the number of carbon atoms exceeds 20, it may be difficult to procure the corresponding raw material such as organic halide, or even if it can be procured, the purity may be low. In consideration of stable use in a CVD apparatus, a hydrocarbon group having 1 to 6 carbon atoms is particularly preferable in that the vapor pressure of the organosilane compound does not become too low.

R ¹ and R ² , R ⁴ , R ⁶ , R ⁸ , R ⁹ , R ¹⁰ , R ¹¹ , R ¹² , R ¹³ , R ¹⁴ , R ¹⁵ , R ¹⁶ , R ¹⁷ , R ¹⁸ , R ¹⁹ described below The hydrocarbon group represented by is not particularly limited, but is preferably an alkyl group having 1 to 6 carbon atoms, an aryl group, an arylalkyl group, an alkylaryl group, an alkenyl group, an arylalkenyl group, an alkenylaryl group, an alkynyl group. Group, an arylalkynyl group and an alkynylaryl group, more preferably an alkyl group having 1 to 6 carbon atoms and an aryl group.

  Specific examples include methyl, ethyl, n-propyl, i-propyl, cyclopropyl, n-butyl, i-butyl, sec-butyl, tert. -Butyl, cyclobutyl, n-pentyl, tert. -Alkyl groups such as amyl, cyclopentyl, n-hexyl, cyclohexyl, 2-ethylhexyl, aryl groups such as phenyl, diphenyl, naphthyl, arylalkyl groups such as benzyl, methylbenzyl, o-toluyl, m-toluyl, p-toluyl 2,3-dimethylphenyl, 2,4-dimethylphenyl, 2,5-dimethylphenyl, 2,6-dimethylphenyl, 3,4-dimethylphenyl, 3,5-dimethylphenyl, 2,4,6-trimethyl Examples thereof include alkylaryl groups such as phenyl, o-ethylphenyl, m-ethylphenyl, and p-ethylphenyl.

  Also vinyl, allyl, 1-propenyl, 1-butenyl, 1,3-butadienyl, 1-pentenyl, 1-cyclopentenyl, 2-cyclopentenyl, cyclopentadienyl, methylcyclopentadienyl, ethylcyclopentadienyl, Alkenyl groups such as 1-hexenyl, 1-cyclohexenyl, 2,4-cyclohexadienyl, 2,5-cyclohexadienyl, 2,4,6-cycloheptatrienyl, 5-norbornen-2-yl, 2- Arylalkenyl groups such as phenyl-1-ethenyl, alkenylaryl groups such as o-styryl, m-styryl, p-styryl, ethynyl, 1-propynyl, 2-propynyl, 1-butynyl, 2-butynyl, 3-butynyl, 1-pentynyl, 2-pentynyl, 3-pentynyl, 4-pentynyl, 1-hexini , 3-hexynyl, 5-alkynyl group hexynyl, etc., 2-phenyl-1-arylalkynyl group ethynyl etc., and 2-ethynyl -2 alkynyl aryl groups such as phenyl and the like.

  Among these, an alkyl group having 1 to 4 carbon atoms and a phenyl group are particularly preferable.

  In the general formula (1), A represents a group containing at least one selected from the group consisting of an oxygen atom, a boron atom, and a nitrogen atom, and has a linear, branched, or cyclic structure. It's okay.

  Among them, A containing oxygen is preferable, for example, the following general formula (2)

（式中、Ｒ^２は、上記に同じ。）又は、下記一般式（３）

(Wherein R ² is the same as above) or the following general formula (3)

（式中、Ｒ^２は、上記に同じ。Ｒ^３は、炭化水素残基を表す。ｐは、Ｒ^３に置換するＯＲ^２の数であり、１以上の整数である。）で示される酸素含有基を挙げることができる。

(In the formula, R ² is the same as above. R ³ represents a hydrocarbon residue. P is the number of OR ² substituted for R ³ and is an integer of 1 or more.) A containing group can be mentioned.

R ^{3 in the} general formula (3) and R ⁵ and R ⁷ shown below are R ¹ , R ² , R ⁴ , R ⁶ , R ⁸ , R ⁹ , R ¹⁰ , R ¹¹ , R ¹² , R ¹³ , A hydrocarbon residue having a structure in which p, q, or r hydrogen atoms are removed from the structure of the hydrocarbon group shown as an example of R ¹⁴ , R ¹⁵ , R ¹⁶ , R ¹⁷ , R ¹⁸ , R ¹⁹ , respectively. The group can be shown by way of example, and is preferably a saturated or unsaturated hydrocarbon residue having 1 to 20 carbon atoms, and may have any of a linear, branched, or cyclic structure.

When the number of carbon atoms exceeds 20, the vapor pressure of the produced organosilane becomes low, and it may be difficult to use in the PECVD apparatus, which may be undesirable. A containing oxygen is preferably an alkoxy group, a silanoxy group, an alkoxyaryl group, or an alkoxyalkyl group, more preferably an alkoxy group having 1 to 4 carbon atoms or an alkoxy group having 1 to 4 carbon atoms substituted. It is a C1-C4 alkyl group which the phenyl group or the C1-C4 alkoxy group substituted. R ^{1 at} this time is preferably an alkyl group having 1 to 6 carbon atoms, more preferably an alkyl group having 1 to 4 carbon atoms.

  As A containing nitrogen, for example, the following general formula (4)

（式中、Ｒ^４は、上記に同じ。）、又は、下記一般式（５）

(Wherein R ⁴ is the same as above) or the following general formula (5)

（式中、Ｒ^４は、上記に同じ。Ｒ^５は、炭化水素残基を表す。ｑは、Ｒ^５に置換するＮＲ^４ _２の数であり、１以上の整数である。）で示される窒素含有基を挙げることができる。上式においてＲ^４どうしは、同一であっても異なっても良い。窒素を含むＡとしては、アルキルアミノ基、ジアルキルアミノ素基、アリールアミノ基、又はジアリールアミノ基が好ましい。

(Wherein, R ⁴ is the same as above. R ⁵ represents a hydrocarbon residue. Q is the number of NR ⁴ ₂ substituted for R ⁵ and is an integer of 1 or more). Mention may be made of nitrogen-containing groups. In the above formula, R ⁴ may be the same or different. As A containing nitrogen, an alkylamino group, a dialkylamino group, an arylamino group, or a diarylamino group is preferable.

  As A containing boron, for example, the following general formula (6)

（式中、Ｒ^６は、上記に同じ。）、又は、下記一般式（７）

(Wherein R ⁶ is the same as above) or the following general formula (7)

（式中、Ｒ^６は、上記に同じ。Ｒ^７は、炭化水素残基を表す。ｒは、Ｒ^７に置換するＢＲ^６ _２の数であり、１以上の整数である。）で示されるホウ素含有基を挙げることができる。上式においてＲ^６どうしは、同一であっても異なっても良い。ホウ素を含むＡとしては、アルキルホウ素残基、アルコキシホウ素残基が好ましい。

(Wherein, ^{R 6} is the same .R ⁷ above are, .r representing a hydrocarbon residue, the number of ^BR _{6 2} replacing the ^{R 7,} 1 or more is an integer.) Represented by Mention may be made of boron-containing groups. In the above formula, R ⁶ may be the same or different. As A containing boron, an alkylboron residue and an alkoxyboron residue are preferable.

  A Si-containing film-forming material comprising the cyclic siloxane compound represented by the general formula (1) having a structure in which the substituents of the general formulas (2) to (7) are mixed is also included in the present invention. Enter the range.

In the general formula (1), when R ¹ is a secondary hydrocarbon group or a tertiary hydrocarbon group directly bonded to an Si atom, the cyclic siloxane compound represented by the general formula (1) is stabilized in plasma, A thin film having a low relative dielectric constant and high mechanical properties is obtained, which is preferable. Further, n is 1 and x is preferably 3 to 4, and the molecular weight of the cyclic siloxane compound represented by the general formula (1) is preferably less than 1000.

  Specific examples of the cyclic siloxane compound represented by the general formula (1) include 2,4,6-tritert. -Butyl-2,4,6-trimethoxycyclotrisiloxane, 2,4,6-trisec-butyl-2,4,6-trimethoxycyclotrisiloxane, 2,4,6-triisobutyl-2,4 , 6-trimethoxycyclotrisiloxane, 2,4,6-tri-n-butyl-2,4,6-trimethoxycyclotrisiloxane, 2,4,6-tricyclobutyl-2,4,6-trimethoxy Cyclotrisiloxane, 2,4,6-triisopropyl-2,4,6-trimethoxycyclotrisiloxane, 2,4,6-tri-n-propyl-2,4,6-trimethoxycyclotrisiloxane, 2, 4,6-tricyclopropyl-2,4,6-trimethoxycyclotrisiloxane, 2,4,6-triethyl-2,4,6-trimethoxycyclotrisiloxane, 2,4, - trimethyl-2,4,6-trimethoxy cyclotrisiloxane and the like.

  In addition, 2,4,6-tri tert. -Butyl-2,4,6-triethoxycyclotrisiloxane, 2,4,6-trisec-butyl-2,4,6-triethoxycyclotrisiloxane, 2,4,6-triisobutyl-2,4 , 6-triethoxycyclotrisiloxane, 2,4,6-tri-n-butyl-2,4,6-triethoxycyclotrisiloxane, 2,4,6-tricyclobutyl-2,4,6-triethoxy Cyclotrisiloxane, 2,4,6-triisopropyl-2,4,6-triethoxycyclotrisiloxane, 2,4,6-tri-n-propyl-2,4,6-triethoxycyclotrisiloxane, 2, 4,6-tricyclopropyl-2,4,6-triethoxycyclotrisiloxane, 2,4,6-triethyl-2,4,6-triethoxycyclotrisiloxane, 2,4, - trimethyl-2,4,6-triethoxy cyclotrisiloxane and the like.

  In addition, 2,4,6-tri tert. -Butyl-2,4,6-tri-n-propoxycyclotrisiloxane, 2,4,6-trisec-butyl-2,4,6-tri-n-propoxycyclotrisiloxane, 2,4,6-triisobutyl -2,4,6-tri-n-propoxycyclotrisiloxane, 2,4,6-tri-n-butyl-2,4,6-tri-n-propoxycyclotrisiloxane, 2,4,6-tricyclobutyl- 2,4,6-tri-n-propoxycyclotrisiloxane, 2,4,6-triisopropyl-2,4,6-tri-n-propoxycyclotrisiloxane, 2,4,6-tri-n-propyl-2, 4,6-tri-n-propoxycyclotrisiloxane, 2,4,6-tricyclopropyl-2,4,6-tri-n-propoxycyclotrisiloxane, 1,3,5-triethyl-1,3 5-tri-n- propoxy cyclotrisiloxane, 2,4,6-trimethyl-2,4,6-n- propoxy cyclotrisiloxane and the like.

  In addition, 2,4,6-tri tert. -Butyl-2,4,6-triisopropoxycyclotrisiloxane, 2,4,6-trisec-butyl-2,4,6-triisopropoxycyclotrisiloxane, 2,4,6-triisobutyl-2 , 4,6-triisopropoxycyclotrisiloxane, 2,4,6-tri-n-butyl-2,4,6-triisopropoxycyclotrisiloxane, 2,4,6-tricyclobutyl-2,4 6-triisopropoxycyclotrisiloxane, 2,4,6-triisopropyl-2,4,6-triisopropoxycyclotrisiloxane, 2,4,6-tri-n-propyl-2,4,6-triiso Propoxycyclotrisiloxane, 2,4,6-tricyclopropyl-2,4,6-triisopropoxycyclotrisiloxane, 2,4,6-triethyl-2,4 6- triisopropoxy cyclotrisiloxane, 2,4,6-trimethyl-2,4,6-isopropoxyphenyl cyclotrisiloxane and the like.

  In addition, 2,4,6,8-tetra tert. -Butyl-2,4,6,8-tetramethoxycyclotetrasiloxane, 2,4,6,8-tetrasec-butyl-2,4,6,8-tetramethoxycyclotetrasiloxane, 2,4,6, 8-tetraisobutyl-2,4,6,8-tetramethoxycyclotetrasiloxane, 2,4,6,8-tetran-butyl-2,4,6,8-tetramethoxycyclotetrasiloxane, 2,4, 6,8-tetracyclobutyl-2,4,6,8-tetramethoxycyclotetrasiloxane, 2,4,6,8-tetraisopropyl-2,4,6,8-tetramethoxycyclotetrasiloxane, 2,4 , 6,8-tetran-propyl-2,4,6,8-tetramethoxycyclotetrasiloxane, 2,4,6,8-tetracyclopropyl-2,4,6,8-tetrameth Cycyclotetrasiloxane, 2,4,6,8-tetraethyl-2,4,6,8-tetramethoxycyclotetrasiloxane, 2,4,6,8-tetramethyl-2,4,6,8-tetramethoxy And cyclotetrasiloxane.

  In addition, 2,4,6,8-tetra tert. -Butyl-2,4,6,8-tetraethoxycyclotetrasiloxane, 2,4,6,8-tetrasec-butyl-2,4,6,8-tetraethoxycyclotetrasiloxane, 2,4,6, 8-tetraisobutyl-2,4,6,8-tetraethoxycyclotetrasiloxane, 2,4,6,8-tetran-butyl-2,4,6,8-tetraethoxycyclotetrasiloxane, 2,4, 6,8-tetracyclobutyl-2,4,6,8-tetraethoxycyclotetrasiloxane, 2,4,6,8-tetraisopropyl-2,4,6,8-tetraethoxycyclotetrasiloxane, 2,4 , 6,8-tetran-propyl-2,4,6,8-tetraethoxycyclotetrasiloxane, 2,4,6,8-tetracyclopropyl-2,4,6,8-tetraeth Cycyclotetrasiloxane, 2,4,6,8-tetraethyl-2,4,6,8-tetraethoxycyclotetrasiloxane, 2,4,6,8-tetramethyl-2,4,6,8-tetraethoxy And cyclotetrasiloxane.

  In addition, 2,4,6,8-tetra tert. -Butyl-2,4,6,8-tetra n-propoxycyclotetrasiloxane, 2,4,6,8-tetrasec-butyl-2,4,6,8-tetra n-propoxycyclotetrasiloxane, 2, 4,6,8-tetraisobutyl-2,4,6,8-tetra n-propoxycyclotetrasiloxane, 2,4,6,8-tetra n-butyl-2,4,6,8-tetra n-propoxy Cyclotetrasiloxane, 2,4,6,8-tetracyclobutyl-2,4,6,8-tetra n-propoxycyclotetrasiloxane, 2,4,6,8-tetraisopropyl-2,4,6,8 -Tetra n-propoxycyclotetrasiloxane, 2,4,6,8-tetra n-propyl-2,4,6,8-tetra n-propoxycyclotetrasiloxane, 2,4,6,8-tetra Chlopropyl-2,4,6,8-tetra n-propoxycyclotetrasiloxane, 2,4,6,8-tetraethyl-2,4,6,8-tetra n-propoxycyclotetrasiloxane, 2,4,6 , 8-tetramethyl-2,4,6,8-tetra n-propoxycyclotetrasiloxane and the like.

  In addition, 2,4,6,8-tetra tert. -Butyl-2,4,6,8-tetraisopropoxycyclotetrasiloxane, 2,4,6,8-tetrasec-butyl-2,4,6,8-tetraisopropoxycyclotetrasiloxane, 2,4, 6,8-tetraisobutyl-2,4,6,8-tetraisopropoxycyclotetrasiloxane, 2,4,6,8-tetran-butyl-2,4,6,8-tetraisopropoxycyclotetrasiloxane, 2,4,6,8-tetracyclobutyl-2,4,6,8-tetraisopropoxycyclotetrasiloxane, 2,4,6,8-tetraisopropyl-2,4,6,8-tetraisopropoxycyclo Tetrasiloxane, 2,4,6,8-tetran-propyl-2,4,6,8-tetraisopropoxycyclotetrasiloxane, 2,4,6,8-tetra Chloropropyl-2,4,6,8-tetraisopropoxycyclotetrasiloxane, 2,4,6,8-tetraethyl-2,4,6,8-tetraisopropoxycyclotetrasiloxane, 2,4,6,8 -Tetramethyl-2,4,6,8-tetraisopropoxycyclotetrasiloxane and the like.

  Also 2,4,6,8,10-penta tert. -Butyl-2,4,6,8,10-pentamethoxycyclopentasiloxane, 2,4,6,8,10-pentasec-butyl-2,4,6,8,10-pentamethoxycyclopentasiloxane, 2,4,6,8,10-pentaisobutyl-2,4,6,8,10-pentamethoxycyclopentasiloxane, 2,4,6,8,10-penta n-butyl-2,4,6, 8,10-pentamethoxycyclopentasiloxane, 2,4,6,8,10-pentacyclobutyl-2,4,6,8,10-pentamethoxycyclotetrasiloxane, 2,4,6,8,10- Pentaisopropyl-2,4,6,8,10-pentamethoxycyclopentasiloxane, 2,4,6,8,10-penta n-propyl-2,4,6,8,10-pentamethoxycyclopent Siloxane, 2,4,6,8,10-pentacyclopropyl-2,4,6,8,10-pentamethoxycyclopentasiloxane, 2,4,6,8,10-pentaethyl-2,4,6, Examples include 8,10-pentamethoxycyclopentasiloxane and 2,4,6,8,10-pentamethyl-2,4,6,8,10-pentamethoxycyclopentasiloxane.

  Also 2,4,6,8,10-penta tert. -Butyl-2,4,6,8,10-pentaethoxycyclopentasiloxane, 2,4,6,8,10-pentasec-butyl-2,4,6,8,10-pentaethoxycyclopentasiloxane, 2,4,6,8,10-pentaisobutyl-2,4,6,8,10-pentaethoxycyclopentasiloxane, 2,4,6,8,10-penta n-butyl-2,4,6, 8,10-pentaethoxycyclopentasiloxane, 2,4,6,8,10-pentacyclobutyl-2,4,6,8,10-pentaethoxycyclotetrasiloxane, 2,4,6,8,10- Pentaisopropyl-2,4,6,8,10-pentaethoxycyclopentasiloxane, 2,4,6,8,10-penta-n-propyl-2,4,6,8,10-pentaethoxycyclopent Siloxane, 2,4,6,8,10-pentacyclopropyl-2,4,6,8,10-pentaethoxycyclopentasiloxane, 2,4,6,8,10-pentaethyl-2,4,6, Examples include 8,10-pentaethoxycyclopentasiloxane, 2,4,6,8,10-pentamethyl-2,4,6,8,10-pentaethoxycyclopentasiloxane.

  Also 2,4,6,8,10-penta tert. -Butyl-2,4,6,8,10-penta n-propoxycyclopentasiloxane, 2,4,6,8,10-pentasec-butyl-2,4,6,8,10-penta n-propoxy Cyclopentasiloxane, 2,4,6,8,10-pentaisobutyl-2,4,6,8,10-penta n-propoxycyclopentasiloxane, 2,4,6,8,10-penta n-butyl- 2,4,6,8,10-penta n-propoxycyclopentasiloxane, 2,4,6,8,10-pentacyclobutyl-2,4,6,8,10-penta n-propoxycyclotetrasiloxane, 2,4,6,8,10-pentaisopropyl-2,4,6,8,10-penta n-propoxycyclopentasiloxane, 2,4,6,8,10-penta n-propyl-2,4 6 8,10-penta n-propoxycyclopentasiloxane, 2,4,6,8,10-pentacyclopropyl-2,4,6,8,10-penta n-propoxycyclopentasiloxane, 2,4,6, 8,10-pentaethyl-2,4,6,8,10-penta n-propoxycyclopentasiloxane, 2,4,6,8,10-pentamethyl-2,4,6,8,10-penta n-propoxy And cyclopentasiloxane.

  Also 2,4,6,8,10-penta tert. -Butyl-2,4,6,8,10-pentaisopropoxycyclopentasiloxane, 2,4,6,8,10-pentasec-butyl-2,4,6,8,10-pentaisopropoxycyclopenta Siloxane, 2,4,6,8,10-pentaisobutyl-2,4,6,8,10-pentaisopropoxycyclopentasiloxane, 2,4,6,8,10-penta-n-butyl-2,4 , 6,8,10-pentaisopropoxycyclopentasiloxane, 2,4,6,8,10-pentacyclobutyl-2,4,6,8,10-pentaisopropoxycyclotetrasiloxane, 2,4,6 , 8,10-pentaisopropyl-2,4,6,8,10-pentaisopropoxycyclopentasiloxane, 2,4,6,8,10-penta-n-propyl-2,4,6 8,10-pentaisopropoxycyclopentasiloxane, 2,4,6,8,10-pentacyclopropyl-2,4,6,8,10-pentaisopropoxycyclopentasiloxane, 2,4,6,8, 10-pentaethyl-2,4,6,8,10-pentaisopropoxycyclopentasiloxane, 2,4,6,8,10-pentamethyl-2,4,6,8,10-pentaisopropoxycyclopentasiloxane Is mentioned.

  2,2,4,4,6,6-hexamethoxycyclotrisiloxane, 2,2,4,4,6,6-hexaethoxycyclotrisiloxane, 2,2,4,4,6,6-hexa n-propoxycyclotrisiloxane, 2,2,4,4,6,6-hexaisopropoxycyclotrisiloxane, 2,2,4,4,6,6-hexacyclopropoxycyclotrisiloxane, 2,2,4 4,6,6-hexa tert. -Butoxycyclotrisiloxane, 2,2,4,4,6,6-hexasec-butoxycyclotrisiloxane, 2,2,4,4,6,6-hexaisobutoxycyclotrisiloxane, 2,2,4 4,6,6-hexa n-butoxycyclotrisiloxane, 2,2,4,4,6,6-hexacyclobutoxycyclotrisiloxane, and the like.

  2,2,4,4,6,6,8,8-octamethoxycyclotetrasiloxane, 2,2,4,4,6,6,8,8-octaethoxycyclotetrasiloxane, 2,2,4 , 4,6,6,8,8-octane-propoxycyclotetrasiloxane, 2,2,4,4,6,6,8,8-octaisopropoxycyclotetrasiloxane, 2,2,4,4 6,6,8,8-octacyclopropoxycyclotetrasiloxane, 2,2,4,4,6,6,8,8-octa tert. -Butoxycyclotetrasiloxane, 2,2,4,4,6,6,8,8-octasec-butoxycyclotetrasiloxane, 2,2,4,4,6,6,8,8-octaisobutoxycyclo Tetrasiloxane, 2,2,4,4,6,6,8,8-octane n-butoxycyclotetrasiloxane, 2,2,4,4,6,6,8,8-octacyclobutoxycyclotetrasiloxane Etc.

  2,2,4,4,6,6,8,8,10,10-decamethoxycyclopentasiloxane, 2,2,4,4,6,6,8,8,10,10-decaethoxycyclo Pentasiloxane, 2,2,4,4,6,6,8,8,10,10-decane-propoxycyclopentasiloxane, 2,2,4,4,6,6,8,8,10,10 -Decaisopropoxycyclopentasiloxane, 2,2,4,4,6,6,8,8,10,10-decacyclopropoxycyclopentasiloxane, 2,2,4,4,6,6,8,8 , 10, 10-deca tert. -Butoxycyclopentasiloxane, 2,2,4,4,6,6,8,8,10,10-decasec-butoxycyclopentasiloxane, 2,2,4,4,6,6,8,8, 10,10-decapentaisobutoxycyclopentasiloxane, 2,2,4,4,6,6,8,8,10,10-decane-butoxycyclopentasiloxane, 2,2,4,4,6 Examples include 6,8,8,10,10-decacyclobutoxycyclopentasiloxane.

  2,4,6-tris (2-methoxyethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (2-tert.-butoxyethyl) -2,4,6-trimethyl Cyclotrisiloxane, 2,4,6,8-tetrakis (2-methoxyethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (2-tert.-butoxy Ethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8,10-pentakis (2-methoxyethyl) -2,4,6,8,10-pentamethylcyclopentasiloxane 2,4,6,8,10-pentakis (2-tert.-butoxyethyl) -2,4,6,8,10-pentamethylcyclotetrasiloxane.

  2,4,6-tris (4-methoxyphenyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (4-tert.-butoxyphenyl) -2,4,6- Trimethylcyclotrisiloxane, 2,4,6,8-tetrakis (4-methoxyphenyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (4-tert.- Butoxyphenyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8,10-pentakis (4-methoxyphenyl) -2,4,6,8,10-pentamethylcyclopenta Examples include siloxane, 2,4,6,8,10-pentakis (4-tert.-butoxyphenyl) -2,4,6,8,10-pentamethylcyclopentasiloxane. That.

  2,4,6-tris (methoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (ethoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 4,6-tris (n-propoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (isopropoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4 , 6-tris (n-butoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (iso.-butoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 2, Examples include 4,6-tris (tret.-butoxymethyl) -2,4,6-trimethylcyclotrisiloxane.

  2,4,6-tris (methoxymethyl) -2,4,6-triethylcyclotrisiloxane, 2,4,6-tris (ethoxymethyl) -2,4,6-triethylcyclotrisiloxane, 2,4 , 6-Tris (n-propoxymethyl) -2,4,6-triethylcyclotrisiloxane, 2,4,6-tris (isopropoxymethyl) -2,4,6-triethylcyclotrisiloxane, 2,4, 6-tris (n-butoxymethyl) -2,4,6-triethylcyclotrisiloxane, 2,4,6-tris (iso.-butoxymethyl) -2,4,6-triethylcyclotrisiloxane, 2,4 , 6-tris (tret.-butoxymethyl) -2,4,6-triethylcyclotrisiloxane.

  2,4,6-tris (methoxymethyl) -2,4,6-triisopropylcyclotrisiloxane, 2,4,6-tris (ethoxymethyl) -2,4,6-triisopropylcyclotrisiloxane, , 4,6-tris (n-propoxymethyl) -2,4,6-triisopropylcyclotrisiloxane, 2,4,6-tris (isopropoxymethyl) -2,4,6-triisopropylcyclotrisiloxane, 2,4,6-tris (n-butoxymethyl) -2,4,6-triisopropylcyclotrisiloxane, 2,4,6-tris (iso.-butoxymethyl) -2,4,6-triisopropylcyclo Trisiloxane, 2,4,6-tris (tret.-butoxymethyl) -2,4,6-triisopropylcyclotrisiloxane That.

  2,4,6-tris (methoxymethyl) -2,4,6-tri n-propylcyclotrisiloxane, 2,4,6-tris (ethoxymethyl) -2,4,6-tri n-propylcyclo Trisiloxane, 2,4,6-tris (n-propoxymethyl) -2,4,6-tri-n-propylcyclotrisiloxane, 2,4,6-tris (isopropoxymethyl) -2,4,6- Tri-n-propylcyclotrisiloxane, 2,4,6-tris (n-butoxymethyl) -2,4,6-tri-n-propylcyclotrisiloxane, 2,4,6-tris (iso.-butoxymethyl) -2,4,6-tri-n-propylcyclotrisiloxane, 2,4,6-tris (tret.-butoxymethyl) -2,4,6-tri-n-propylcyclotrisiloxane and the like. That.

  In addition, 2,4,6-tris (methoxymethyl) -2,4,6-tritert. -Butylcyclotrisiloxane, 2,4,6-tris (ethoxymethyl) -2,4,6-tri tert. -Butylcyclotrisiloxane, 2,4,6-tris (n-propoxymethyl) -2,4,6-tritert. -Butylcyclotrisiloxane, 2,4,6-tris (isopropoxymethyl) -2,4,6-tritert. -Butylcyclotrisiloxane, 2,4,6-tris (n-butoxymethyl) -2,4,6-tritert. -Butylcyclotrisiloxane, 2,4,6-tris (iso.-butoxymethyl) -2,4,6-tritert. -Butylcyclotrisiloxane, 2,4,6-tris (tret.-butoxymethyl) -2,4,6-tritert. -Butylcyclotrisiloxane and the like.

  2,4,6-tris (methoxymethyl) -2,4,6-tricyclopentylcyclotrisiloxane, 2,4,6-tris (ethoxymethyl) -2,4,6-tricyclopentylcyclotrisiloxane, , 4,6-tris (n-propoxymethyl) -2,4,6-tricyclopentylcyclotrisiloxane, 2,4,6-tris (isopropoxymethyl) -2,4,6-tricyclopentylcyclotrisiloxane, 2,4,6-tris (n-butoxymethyl) -2,4,6-tricyclopentylcyclotrisiloxane, 2,4,6-tris (iso.-butoxymethyl) -2,4,6-tricyclopentylcyclo Trisiloxane, 2,4,6-tris (tret.-butoxymethyl) -2,4,6-tricyclopentylcyclotrisiloxy Emissions, and the like.

  2,4,6-tris (methoxymethyl) -2,4,6-tricyclohexylcyclotrisiloxane, 2,4,6-tris (ethoxymethyl) -2,4,6-tricyclohexylcyclotrisiloxane, , 4,6-tris (n-propoxymethyl) -2,4,6-tricyclohexylcyclotrisiloxane, 2,4,6-tris (isopropoxymethyl) -2,4,6-tricyclohexylcyclotrisiloxane, 2,4,6-tris (n-butoxymethyl) -2,4,6-tricyclohexylcyclotrisiloxane, 2,4,6-tris (iso.-butoxymethyl) -2,4,6-tricyclohexylcyclo Trisiloxane, 2,4,6-tris (tret.-butoxymethyl) -2,4,6-tricyclohexylcyclotrisiloxy Emissions, and the like.

  2,4,6-tris (methoxyethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (ethoxyethyl) -2,4,6-trimethylcyclotrisiloxane, 4,6-tris (n-propoxyethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (isopropoxyethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4 , 6-tris (n-butoxyethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (iso.-butoxyethyl) -2,4,6-trimethylcyclotrisiloxane, Examples include 4,6-tris (tret.-butoxyethyl) -2,4,6-trimethylcyclotrisiloxane.

  2,4,6-tris (methoxyethyl) -2,4,6-triethylcyclotrisiloxane, 2,4,6-tris (ethoxyethyl) -2,4,6-triethylcyclotrisiloxane, 2,4 , 6-Tris (n-propoxyethyl) -2,4,6-triethylcyclotrisiloxane, 2,4,6-tris (isopropoxyethyl) -2,4,6-triethylcyclotrisiloxane, 2,4, 6-tris (n-butoxyethyl) -2,4,6-triethylcyclotrisiloxane, 2,4,6-tris (iso.-butoxyethyl) -2,4,6-triethylcyclotrisiloxane, 2,4 , 6-tris (tret.-butoxyethyl) -2,4,6-triethylcyclotrisiloxane and the like.

  2,4,6-tris (methoxyethyl) -2,4,6-triisopropylcyclotrisiloxane, 2,4,6-tris (ethoxyethyl) -2,4,6-triisopropylcyclotrisiloxane, , 4,6-tris (n-propoxyethyl) -2,4,6-triisopropylcyclotrisiloxane, 2,4,6-tris (isopropoxyethyl) -2,4,6-triisopropylcyclotrisiloxane, 2,4,6-tris (n-butoxyethyl) -2,4,6-triisopropylcyclotrisiloxane, 2,4,6-tris (iso.-butoxyethyl) -2,4,6-triisopropylcyclo Trisiloxane, 2,4,6-tris (tret.-butoxyethyl) -2,4,6-triisopropylcyclotrisiloxane That.

  2,4,6-tris (methoxyethyl) -2,4,6-tri n-propylcyclotrisiloxane, 2,4,6-tris (ethoxyethyl) -2,4,6-tri n-propylcyclo Trisiloxane, 2,4,6-tris (n-propoxyethyl) -2,4,6-tri-n-propylcyclotrisiloxane, 2,4,6-tris (isopropoxyethyl) -2,4,6- Tri-n-propylcyclotrisiloxane, 2,4,6-tris (n-butoxyethyl) -2,4,6-tri-n-propylcyclotrisiloxane, 2,4,6-tris (iso.-butoxyethyl) -2,4,6-tri-n-propylcyclotrisiloxane, 2,4,6-tris (tret.-butoxyethyl) -2,4,6-tri-n-propylcyclotrisiloxane and the like. That.

  In addition, 2,4,6-tris (methoxyethyl) -2,4,6-tritert. -Butylcyclotrisiloxane, 2,4,6-tris (ethoxyethyl) -2,4,6-tri tert. -Butylcyclotrisiloxane, 2,4,6-tris (n-propoxyethyl) -2,4,6-tritert. -Butylcyclotrisiloxane, 2,4,6-tris (isopropoxyethyl) -2,4,6-tri tert. -Butylcyclotrisiloxane, 2,4,6-tris (n-butoxyethyl) -2,4,6-tritert. -Butylcyclotrisiloxane, 2,4,6-tris (iso.-butoxyethyl) -2,4,6-tritert. -Butylcyclotrisiloxane, 2,4,6-tris (tret.-butoxyethyl) -2,4,6-tritert. -Butylcyclotrisiloxane and the like.

  2,4,6-tris (methoxyethyl) -2,4,6-tricyclopentylcyclotrisiloxane, 2,4,6-tris (ethoxyethyl) -2,4,6-tricyclopentylcyclotrisiloxane, , 4,6-tris (n-propoxyethyl) -2,4,6-tricyclopentylcyclotrisiloxane, 2,4,6-tris (isopropoxyethyl) -2,4,6-tricyclopentylcyclotrisiloxane, 2,4,6-tris (n-butoxyethyl) -2,4,6-tricyclopentylcyclotrisiloxane, 2,4,6-tris (iso.-butoxyethyl) -2,4,6-tricyclopentylcyclo Trisiloxane, 2,4,6-tris (tret.-butoxyethyl) -2,4,6-tricyclopentylcyclotrisiloxy Emissions, and the like.

  2,4,6-tris (methoxyethyl) -2,4,6-tricyclohexylcyclotrisiloxane, 2,4,6-tris (ethoxyethyl) -2,4,6-tricyclohexylcyclotrisiloxane, , 4,6-tris (n-propoxyethyl) -2,4,6-tricyclohexylcyclotrisiloxane, 2,4,6-tris (isopropoxyethyl) -2,4,6-tricyclohexylcyclotrisiloxane, 2,4,6-tris (n-butoxyethyl) -2,4,6-tricyclohexylcyclotrisiloxane, 2,4,6-tris (iso.-butoxyethyl) -2,4,6-tricyclohexylcyclo Trisiloxane, 2,4,6-tris (tret.-butoxyethyl) -2,4,6-tricyclohexylcyclotrisiloxy Emissions, and the like.

  2,4,6-tris (methoxypropyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (methoxypropyl) -2,4,6-triethylcyclotrisiloxane, 2,4 , 6-Tris (methoxypropyl) -2,4,6-triisopropylcyclotrisiloxane, 2,4,6-tris (methoxybutyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6- And tris (methoxypentyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (methoxyhexyl) -2,4,6-trimethylcyclotrisiloxane, and the like.

  2,4,6,8-tetrakis (methoxymethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxymethyl) -2,4,6,8 -Tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxymethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxymethyl) ) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxymethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4, 6,8-tetrakis (isobutoxymethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (tert.-butoxymethyl) 2,4,6,8-tetramethyl cyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxymethyl) -2,4,6,8-tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxymethyl) -2,4,6,8- Tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxymethyl) -2,4,6,8-tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxymethyl) -2 , 4,6,8-tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxymethyl) -2,4,6,8-tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (Isobutoxymethyl) -2,4,6,8-tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (tert.-butoxymethyl) 2,4,6,8-tetraethyl cyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxymethyl) -2,4,6,8-tetran-propylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxymethyl) -2,4,6 , 8-tetra n-propylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxymethyl) -2,4,6,8-tetra n-propylcyclotetrasiloxane, 2,4,6,8 -Tetrakis (isopropoxymethyl) -2,4,6,8-tetran-propylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxymethyl) -2,4,6,8-tetran -Propylcyclotetrasiloxane, 2,4,6,8-tetrakis (isobutoxymethyl) -2,4,6,8-tetran-propylcyclotetrasiloxane, 2,4,6,8-te Rakisu (tert.-butoxymethyl) -2,4,6,8-tetra n- propyl cyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxymethyl) -2,4,6,8-tetraisopropylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxymethyl) -2,4,6,8 -Tetraisopropylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxymethyl) -2,4,6,8-tetraisopropylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxymethyl) ) -2,4,6,8-tetraisopropylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxymethyl) -2,4,6,8-tetraisopropylcyclotetrasiloxane, 2,4, 6,8-tetrakis (isobutoxymethyl) -2,4,6,8-tetraisopropylcyclotetrasiloxane, 2,4,6,8-te Rakisu (tert.-butoxymethyl) -2,4,6,8-tetra isopropyl cyclotetrasiloxane and the like.

  In addition, 2,4,6,8-tetrakis (methoxymethyl) -2,4,6,8-tetratert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxymethyl) -2,4,6,8-tetratert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxymethyl) -2,4,6,8-tetra tert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxymethyl) -2,4,6,8-tetra tert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxymethyl) -2,4,6,8-tetra tert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (isobutoxymethyl) -2,4,6,8-tetra tert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (tert.-butoxymethyl) -2,4,6,8-tetratert. -Butylcyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxymethyl) -2,4,6,8-tetracyclopentylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxymethyl) -2,4,6,8 -Tetracyclopentylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxymethyl) -2,4,6,8-tetracyclopentylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxymethyl) ) -2,4,6,8-tetracyclopentylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxymethyl) -2,4,6,8-tetracyclopentylcyclotetrasiloxane, 2,4, 6,8-tetrakis (isobutoxymethyl) -2,4,6,8-tetracyclopentylcyclotetrasiloxane, 2,4 6,8-tetrakis (tert.-butoxymethyl) -2,4,6,8-tetra cyclopentyl cyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxymethyl) -2,4,6,8-tetracyclohexylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxymethyl) -2,4,6,8 -Tetracyclohexylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxymethyl) -2,4,6,8-tetracyclohexylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxymethyl) ) -2,4,6,8-tetracyclohexylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxymethyl) -2,4,6,8-tetracyclohexylcyclotetrasiloxane, 2,4, 6,8-tetrakis (isobutoxymethyl) -2,4,6,8-tetracyclohexylcyclotetrasiloxane, 2,4 6,8-tetrakis (tert.-butoxymethyl) -2,4,6,8-tetramethyl cyclohexyl cyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxyethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxyethyl) -2,4,6,8 -Tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxyethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxyethyl) ) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxyethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4, 6,8-tetrakis (isobutoxyethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (tert.-butoxyethyl) 2,4,6,8-tetramethyl cyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxyethyl) -2,4,6,8-tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxyethyl) -2,4,6,8- Tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxyethyl) -2,4,6,8-tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxyethyl) -2 , 4,6,8-tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxyethyl) -2,4,6,8-tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (Isobutoxyethyl) -2,4,6,8-tetraethylcyclotetrasiloxane, 2,4,6,8-tetrakis (tert.-butoxyethyl) 2,4,6,8-tetraethyl cyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxyethyl) -2,4,6,8-tetran-propylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxyethyl) -2,4,6 , 8-tetran-propylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxyethyl) -2,4,6,8-tetran-propylcyclotetrasiloxane, 2,4,6,8 -Tetrakis (isopropoxyethyl) -2,4,6,8-tetran-propylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxyethyl) -2,4,6,8-tetran -Propylcyclotetrasiloxane, 2,4,6,8-tetrakis (isobutoxyethyl) -2,4,6,8-tetran-propylcyclotetrasiloxane, 2,4,6,8-te Rakisu (tert.-butoxyethyl) -2,4,6,8-tetra n- propyl cyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxyethyl) -2,4,6,8-tetraisopropylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxyethyl) -2,4,6,8 -Tetraisopropylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxyethyl) -2,4,6,8-tetraisopropylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxyethyl) ) -2,4,6,8-tetraisopropylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxyethyl) -2,4,6,8-tetraisopropylcyclotetrasiloxane, 2,4 6,8-tetrakis (isobutoxyethyl) -2,4,6,8-tetraisopropylcyclotetrasiloxane, 2,4,6,8-te Rakisu (tert.-butoxyethyl) -2,4,6,8-tetra isopropyl cyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxyethyl) -2,4,6,8-tetratert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxyethyl) -2,4,6,8-tetratert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxyethyl) -2,4,6,8-tetra tert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxyethyl) -2,4,6,8-tetra tert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxyethyl) -2,4,6,8-tetra tert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (isobutoxyethyl) -2,4,6,8-tetra tert. -Butylcyclotetrasiloxane, 2,4,6,8-tetrakis (tert.-butoxyethyl) -2,4,6,8-tetratert. -Butylcyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxyethyl) -2,4,6,8-tetracyclopentylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxyethyl) -2,4,6,8 -Tetracyclopentylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxyethyl) -2,4,6,8-tetracyclopentylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxyethyl) ) -2,4,6,8-tetracyclopentylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxyethyl) -2,4,6,8-tetracyclopentylcyclotetrasiloxane, 2,4 6,8-tetrakis (isobutoxyethyl) -2,4,6,8-tetracyclopentylcyclotetrasiloxane, 2,4 6,8-tetrakis (tert.-butoxyethyl) -2,4,6,8-tetra cyclopentyl cyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxyethyl) -2,4,6,8-tetracyclohexylcyclotetrasiloxane, 2,4,6,8-tetrakis (ethoxyethyl) -2,4,6,8 -Tetracyclohexylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-propoxyethyl) -2,4,6,8-tetracyclohexylcyclotetrasiloxane, 2,4,6,8-tetrakis (isopropoxyethyl) ) -2,4,6,8-tetracyclohexylcyclotetrasiloxane, 2,4,6,8-tetrakis (n-butoxyethyl) -2,4,6,8-tetracyclohexylcyclotetrasiloxane, 2,4, 6,8-tetrakis (isobutoxyethyl) -2,4,6,8-tetracyclohexylcyclotetrasiloxane, 2,4 6,8-tetrakis (tert.-butoxyethyl) -2,4,6,8-tetramethyl cyclohexyl cyclotetrasiloxane and the like.

  2,4,6,8-tetrakis (methoxypropyl) -2,4,6,8-tetramethylcyclotrisiloxane, 2,4,6,8-tetrakis (methoxypropyl) -2,4,6,8 Tetraethylcyclotrisiloxane, 2,4,6,8-tetrakis (methoxypropyl) -2,4,6,8-tetraisopropylcyclotrisiloxane, 2,4,6,8-tetrakis (methoxybutyl) -2, 4,6,8-tetramethylcyclotrisiloxane, 2,4,6,8-tetrakis (methoxypentyl) -2,4,6,8-tetramethylcyclotrisiloxane, 2,4,6,8-tetrakismethoxy Hexyl) -2,4,6,8-tetramethylcyclotrisiloxane and the like.

  2,4,6,8,10-pentakis (methoxymethyl) -2,4,6,8,10-pentamethylcyclopentasiloxane, 2,4,6,8,10-pentakis (methoxymethyl) -2 4,6,8,10-pentaethylcyclopentasiloxane, 2,4,6,8,10-pentakis (methoxymethyl) -2,4,6,8,10-pentaisopropylcyclopentasiloxane and the like. .

  2,4,6,8,10-pentakis (methoxyethyl) -2,4,6,8,10-pentamethylcyclopentasiloxane, 2,4,6,8,10-pentakis (methoxyethyl) -2 4,6,8,10-pentaethylcyclopentasiloxane, 2,4,6,8,10-pentakis (methoxyethyl) -2,4,6,8,10-pentaisopropylcyclopentasiloxane and the like. .

  In addition, 2,4,6-tri tert. -Butyl-2,4,6-tris (dimethylamino) cyclotrisiloxane, 2,4,6-tri tert. -Butyl-2,4,6-tris (diethylamino) cyclotrisiloxane, 2,4,6,8-tetra tert. -Butyl-2,4,6,8-tetrakis (dimethylamino) cyclotetrasiloxane, 2,4,6,8-tetratert. -Butyl-2,4,6,8-tetrakis (diethylamino) cyclotetrasiloxane, 2,4,6,8,10-penta tert. -Butyl-2,4,6,8,10-pentakis (dimethylamino) cyclopentasiloxane, 2,4,6,8,10-penta tert. -Butyl-2,4,6,8,10-pentakis (diethylamino) cyclopentasiloxane and the like.

  2,4,6-triisopropyl-2,4,6-tris (dimethylamino) cyclotrisiloxane, 2,4,6-triisopropyl-2,4,6-tris (diethylamino) cyclotrisiloxane, 4,6,8-tetraisopropyl-2,4,6,8-tetrakis (dimethylamino) cyclotetrasiloxane, 2,4,6,8-tetraisopropyl-2,4,6,8-tetrakis (diethylamino) cyclo Tetrasiloxane, 2,4,6,8,10-pentaisopropyl-2,4,6,8,10-pentakis (dimethylamino) cyclopentasiloxane, 2,4,6,8,10-pentaisopropyl-2, Examples include 4,6,8,10-pentakis (diethylamino) cyclopentasiloxane.

  2,4,6-trimethyl-2,4,6-tris (dimethylamino) cyclotrisiloxane, 2,4,6-trimethyl-2,4,6-tris (diethylamino) cyclotrisiloxane, 6,8-tetramethyl-2,4,6,8-tetrakis (dimethylamino) cyclotetrasiloxane, 2,4,6,8-tetramethyl-2,4,6,8-tetrakis (diethylamino) cyclotetrasiloxane 2,4,6,8,10-pentamethyl-2,4,6,8,10-pentakis (dimethylamino) cyclopentasiloxane, 2,4,6,8,10-pentamethyl-2,4,6, Examples include 8,10-pentakis (diethylamino) cyclopentasiloxane.

  2,4,6-tris (4-dimethylaminophenyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (4-diethylaminophenyl) -2,4,6-trimethylcyclotrisiloxane Siloxane, 2,4,6,8-tetrakis (4-dimethylaminophenyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (4-diethylaminophenyl) -2 , 4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8,10-pentakis (4-dimethylaminophenyl) -2,4,6,8,10-pentamethylcyclopentasiloxane, 2, 4,6,8,10-pentakis (4-diethylaminophenyl) -2,4,6,8,10-pentamethylcyclopentasiloxane .

  In addition, 2,4,6-tri tert. -Butyl-2,4,6-tris (dimethylboro) cyclotrisiloxane, 2,4,6-tri tert. -Butyl-2,4,6-tris (diethylboro) cyclotrisiloxane, 2,4,6,8-tetra tert. -Butyl-2,4,6,8-tetrakis (dimethylboro) cyclotetrasiloxane, 2,4,6,8-tetratert. -Butyl-2,4,6,8-tetrakis (diethylboro) cyclotetrasiloxane, 2,4,6,8,10-penta tert. -Butyl-2,4,6,8,10-pentakis (dimethylboro) cyclopentasiloxane, 2,4,6,8,10-penta tert. -Butyl-2,4,6,8,10-pentakis (diethylboro) cyclopentasiloxane and the like.

  2,4,6-triisopropyl-2,4,6-tris (dimethylboro) cyclotrisiloxane, 2,4,6-triisopropyl-2,4,6-tris (diethylboro) cyclotrisiloxane, 2,4 , 6,8-tetraisopropyl-2,4,6,8-tetrakis (dimethylboro) cyclotetrasiloxane, 2,4,6,8-tetraisopropyl-2,4,6,8-tetrakis (diethylboro) cyclotetrasiloxane 2,4,6,8,10-pentaisopropyl-2,4,6,8,10-pentakis (dimethylboro) cyclopentasiloxane, 2,4,6,8,10-pentaisopropyl-2,4,6 , 8,10-pentakis (diethylboro) cyclopentasiloxane.

  2,4,6-trimethyl-2,4,6-tris (dimethylboro) cyclotrisiloxane, 2,4,6-trimethyl-2,4,6-tris (diethylboro) cyclotrisiloxane, 2,4,6 , 8-tetramethyl-2,4,6,8-tetrakis (dimethylboro) cyclotetrasiloxane, 2,4,6,8-tetramethyl-2,4,6,8-tetrakis (diethylboro) cyclotetrasiloxane, 2, , 4,6,8,10-pentamethyl-2,4,6,8,10-pentakis (dimethylboro) cyclopentasiloxane, 2,4,6,8,10-pentamethyl-2,4,6,8,10 -Pentakis (diethylboro) cyclopentasiloxane and the like.

  2,4,6-tris (4-dimethylborophenyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6-tris (4-diethylborophenyl) -2,4,6-trimethylcyclo Trisiloxane, 2,4,6,8-tetrakis (4-dimethylborophenyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8-tetrakis (4-diethylborophenyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6,8,10-pentakis (4-dimethylborophenyl) -2,4,6,8,10-pentamethylcyclopentasiloxane, Examples include 2,4,6,8,10-pentakis (diethylborophenyl) -2,4,6,8,10-pentamethylcyclopentasiloxane.

  The Si-containing film-forming material of the present invention contains a cyclic siloxane compound represented by the general formula (1), but for use as an insulating film material, other than silicon, carbon, oxygen, hydrogen, nitrogen and boron The amount of impurities is preferably less than 10 ppb and the water content is less than 50 ppm.

  The production method of the cyclic siloxane compound represented by the general formula (1) is not particularly limited. For example, the method for producing the cyclic siloxane compound having the structure of the general formula (2) includes the following general formula: (8)

（式中、Ｒ^１、Ｒ^８は、上記に同じ。）で示される酸素含有シラン化合物を酸もしくは塩基の共存または非共存下で加水分解する方法や、下記一般式（９）

(Wherein R ¹ and R ⁸ are the same as above), a method of hydrolyzing the oxygen-containing silane compound in the presence or absence of an acid or a base, or the following general formula (9)

（式中、Ｒ^１、ｎ、ｘは、上式と同じ。）で示される環状シロキサンとアルコール類をＰｄ，Ｎｉ，又はＲｈ触媒下に反応させ、製造する方法を用いることができる。

(Wherein R ¹ , n, and x are the same as those in the above formula) can be used by reacting a cyclic siloxane with an alcohol in the presence of a Pd, Ni, or Rh catalyst.

  As a method for producing a cyclic siloxane compound having the structure of the general formula (3), for example, the following general formula (10) obtained by reacting a corresponding Grignard reagent or an organolithium compound with an organosilane compound

（式中、Ｒ^１、Ｒ^２、Ｒ^３、Ｒ^９、ｐは、上記に同じ。ｓは、１または２を表し、ｔは、０または１を表し、ｓ＋ｔは、１乃至２である。）で示される酸素含有シラン化合物を酸もしくは塩基の共存または非共存下で加水分解する方法や、上記一般式（９）で示される環状シロキサンとＲ^２Ｏ基を有するアルキン化合物をＰｔ触媒下に反応させ、製造する方法を用いることができる。

(Wherein R ¹ , R ² , R ³ , R ⁹ and p are the same as above. S represents 1 or 2, t represents 0 or 1, and s + t is 1 to 2). The oxygen-containing silane compound represented by formula (9) is hydrolyzed in the presence or absence of an acid or a base, or the alkyne compound having the cyclic siloxane represented by the general formula (9) and the R ² O group is prepared under a Pt catalyst. A method of reacting and producing can be used.

  As a method for producing a cyclic siloxane having the structure of the general formula (4), for example, the following general formula (11)

（式中、Ｒ^１、Ｒ^４、Ｒ^１０は、上記に同じ。ｕは、１または２を表し、ｖは、０または１を表し、ｕ＋ｖは、１乃至２である。）で示される窒素及び酸素含有シラン化合物を酸もしくは塩基の共存または非共存下で加水分解する方法を用いることができる。

(Wherein R ¹ , R ⁴ , and R ¹⁰ are the same as above. U represents 1 or 2, v represents 0 or 1, and u + v is 1 to 2). And a method of hydrolyzing the oxygen-containing silane compound in the presence or absence of an acid or a base.

  As a method for producing a cyclic siloxane compound having the structure of the general formula (5), for example, the following general formula (12)

（式中、Ｒ^１、Ｒ^４、Ｒ^５、Ｒ^１１、ｑは、上記に同じ。ｙは、１または２を表し、ｚは、０または１を表し、ｙ＋ｚは、１乃至２である。）で示される窒素及び酸素含有シラン化合物を酸もしくは塩基の共存または非共存下で加水分解する方法を用いることができる。

(Wherein R ¹ , R ⁴ , R ⁵ , R ¹¹ , q are the same as above. Y represents 1 or 2, z represents 0 or 1, and y + z is 1 to 2.) And a method of hydrolyzing the nitrogen- and oxygen-containing silane compound represented by (3) in the presence or absence of an acid or a base.

  As a method for producing a cyclic siloxane having the structure of the general formula (6), for example, the following general formula (13)

（式中、Ｒ^１、Ｒ^６、Ｒ^１２は、上記に同じ。ａは、１または２を表し、ｂは、０または１を表し、ａ＋ｂは、１乃至２である。）で示されるホウ素及び酸素含有シラン化合物を酸もしくは塩基の共存または非共存下で加水分解する方法を用いることができる。

(Wherein R ¹ , R ⁶ and R ¹² are the same as above. A represents 1 or 2, b represents 0 or 1, and a + b represents 1 to 2). And a method of hydrolyzing the oxygen-containing silane compound in the presence or absence of an acid or a base.

  As a method for producing a cyclic siloxane having the structure of the general formula (7), for example, the following general formula (14)

（式中、Ｒ^１、Ｒ^６、Ｒ^７、Ｒ^１３、ｒは、上記に同じ。ｃは、１または２を表し、ｄは、０または１を表し、ｃ＋ｄは、１乃至２である。）で示されるホウ素及び酸素含有シラン化合物を酸もしくは塩基の共存または非共存下で加水分解する方法用いることができる。

(Wherein R ¹ , R ⁶ , R ⁷ , R ¹³ and r are the same as above. C represents 1 or 2, d represents 0 or 1, and c + d is 1 to 2. And a method of hydrolyzing the oxygen-containing silane compound represented by (3) in the presence or absence of an acid or a base.

  In the reaction, for example, inorganic acids such as hydrochloric acid, nitric acid and sulfuric acid, and organic acids such as toluenesulfonic acid can be used as the coexisting acid. In addition, as the base to be coexisted in the reaction, for example, sodium hydroxide, potassium hydroxide, sodium methoxide, potassium methoxide, sodium ethoxide, potassium ethoxide, sodium tertiary butoxide, potassium tertiary butoxide and the like can be used. it can.

  As Pd, Ni, or Rh catalyst that can be used when the cyclic siloxane compound of the general formula (9) and alcohols are reacted, Pd (0), Ni (0) supported on high surface area activated carbon, or Rh (0) catalyst and the following general formula (15)

（式中、Ｍは、Ｐｄ、Ｎｉ、又はＲｈを表し、Ｘは、弗素、塩素、臭素、又は沃素を表し、Ｌは、電子供与性化合物を表す。ｅ及びｆは，０以上の数を表し、ｅ＋ｆは、Ｍの価数及
び配位数を満たす数である。）で示される不均一又は均一系触媒を用いることができる。

(In the formula, M represents Pd, Ni, or Rh, X represents fluorine, chlorine, bromine, or iodine, L represents an electron-donating compound, and e and f each represent a number of 0 or more. E + f is a number satisfying the valence and coordination number of M).

  As the electron donating compound represented by L in the general formula (15), for example, phosphine compounds, amine compounds and the like can be used. Specifically, for example, the following general formula (16) or the following general formula (17)

（式中、Ｒ^１４は、上記に同じ。Ｒ^１４どうしは、同一であっても、異なってもよい。）

(In the formula, R ¹⁴ is the same as above. R ¹⁴ may be the same or different.)

（式中、Ｒ^１５は、上記に同じ。Ｒ^１５どうしは、同一であっても、異なってもよい。）
で示されるホスフィン化合物、又は、一般式（１８）もしくは（１９）

(In the formula, R ¹⁵ is the same as above. R ¹⁵ may be the same or different.)
A phosphine compound represented by the general formula (18) or (19)

（式中、Ｒ^１６は、前述と同様を表す。Ｒ^１６どうしは、同一であっても、異なってもよい。）

^{(Wherein, R 16} is is what ^{.R 16} represent the same manner as described above, may be the same or different.)

（式中、Ｒ^１７は、前述と同様を表す。Ｒ^１７どうしは、同一であっても、異なってもよい。）で示されるアミン化合物を用いることができる。

(Wherein, R ¹⁷ is and what .R ¹⁷ represent the same as described above, may be the same or different.) Can be used an amine compound represented by.

  The reaction solvent that can be used in the production of the cyclic siloxane compound represented by the general formula (1) is not particularly limited as long as it is used in the technical field. For example, n-pentane, i-pentane. , Saturated hydrocarbons such as n-hexane, cyclohexane, n-heptane and n-decane, unsaturated hydrocarbons such as toluene, xylene and decene-1, diethyl ether, dipropyl ether, tert. -Ethers such as butyl methyl ether, dibutyl ether, cyclopentyl methyl ether, tetrahydrofuran, methanol, ethanol, isopropanol, n-butanol, tert. Alcohols such as butanol and 2-ethylhexanol can be used. Moreover, these mixed solvents can also be used. In particular, when ethers or alcohols are used, the cyclic siloxane compound represented by the general formula (1) having a specific molecular weight may be produced in a high yield.

  Regarding the reaction temperature in the production of the cyclic siloxane compound represented by the general formula (1), it is usually in the range of −100 to 200 ° C., preferably −85 to 150 ° C., which is an industrially used temperature. It is preferable to carry out within a range. The pressure conditions for the reaction can be any of under pressure, normal pressure, and reduced pressure.

  About the purification method of the produced cyclic siloxane compound represented by the general formula (1), the moisture content useful for use as an insulating film material is less than 50 ppm, impurities other than silicon, carbon, oxygen and hydrogen, for example, metal impurities In order to make the amount less than 10 ppb, a purification method such as atmospheric pressure or vacuum distillation or column separation using silica, alumina, or polymer gel can be used. At this time, these means may be used in combination as necessary.

  When the cyclic siloxane compound represented by the general formula (1) finally obtained contains a high amount of moisture, elemental impurities other than silicon, carbon, oxygen, and hydrogen, especially metal impurity residues, it is not suitable as an insulating film material. Become.

  In the production, it is preferable that other conditions follow the method in the organic synthesis and organometallic compound synthesis fields. That is, the dehydration and deoxygenation is performed in a nitrogen or argon atmosphere, and the solvent to be used and the column filler for purification are preferably subjected to a dehydration operation in advance. Further, it is preferable to remove impurities such as metal residues and particles.

  The cyclic siloxane compound represented by the general formula (1) of the present invention is used as a Si-containing film-forming material, and a Si-containing film can be produced using it as a raw material. The film formation method at this time is not limited, but is preferably performed by CVD, and particularly preferably by PECVD.

  At this time, the type of PECVD and the apparatus to be used are not particularly limited. For example, the PECVD used is generally used in the technical field such as the semiconductor manufacturing field and the liquid crystal display manufacturing field.

  In the PECVD apparatus, the Si-containing film forming material of the present invention is vaporized by a vaporizer, introduced into a film forming chamber, applied to an electrode in the film forming chamber by a high frequency power source, and plasma is generated to form a film forming chamber. A plasma CVD thin film can be formed on the inner silicon substrate or the like. At this time, a gas such as argon or helium, or an oxidant such as oxygen or nitrous oxide may be introduced for the purpose of generating plasma. Also, it is within the scope of the present invention to simultaneously introduce an organic peroxide or an epoxy compound for the purpose of making the thin film porous. When a film is formed using the Si-containing film forming material of the present invention by a PECVD apparatus, a thin film suitable as a low dielectric constant material (Low-k material) for semiconductor devices can be formed.

  The plasma generation method of the PECVD apparatus is not particularly limited, and inductively coupled plasma, capacitively coupled plasma, ECR plasma, microwave plasma, or the like used in the art can be used. Inductively coupled plasma and capacitively coupled plasma are preferable. As the plasma generation source, various types such as a parallel plate type and an antenna type can be used. As the inert gas supplied to the chamber of the PECVD apparatus, helium, argon, krypton, neon used in the technical field. Xenon, etc. can be used.

  As an example of the PECVD apparatus, FIG. 1 shows a parallel plate capacitively coupled PECVD apparatus. A parallel plate capacitively coupled PECVD apparatus 1 shown in FIG. 1 includes a showerhead upper electrode and a lower electrode capable of controlling the temperature of a substrate in a PECVD apparatus chamber, and a vaporizer apparatus that vaporizes and supplies the general formula (1) to the chamber. It consists of a plasma generator consisting of a high-frequency power source and a matching circuit, and an exhaust system consisting of a vacuum pump.

  Specifically, the PECVD apparatus 1 includes a PECVD chamber 2, an upper electrode 3 having a shower head for uniformly supplying the compound of the general formula (1) into the chamber, and a thin film forming substrate 5 such as a Si substrate. A lower electrode 4 having a temperature control device 8 for installation, vaporization devices 9 to 15 for vaporizing the compound of the general formula (1), a matching circuit 6 and an RF power source 7 which are plasma generation sources, and unreacted in the chamber It consists of an exhaust device 16 for exhausting objects and by-products. Reference numerals 17 and 18 denote grounds.

  The matching circuit 6 and the RF power source 7 which are plasma generation sources are connected to the upper electrode 3 and generate plasma by discharge. The standard of the RF power source 7 is not particularly limited, but the power used in the technical field is 1 W to 2000 W, preferably 10 W to 1000 W, the frequency is 50 kHz to 2.5 GHz, preferably 100 kHz to 100 MHz, particularly preferably 200 kHz. An RF power source of ˜50 MHz can be used.

  The control of the substrate temperature is not particularly limited, but is in the range of −90 to 1,000 ° C., preferably 0 ° C. to 500 ° C.

  The vaporizer is filled with a compound 13 of the general formula (1) that is liquid at normal temperature and pressure, and is equipped with a dip pipe and a pipe 15 that is pressurized with the inert gas, and a general formula (1) that is liquid. A liquid flow rate control device 10 for controlling the flow rate of the compound 13; a vaporizer 9 for vaporizing the compound 13 of the general formula (1) which is a liquid; and for supplying the inert gas into the PECVD apparatus chamber via the vaporizer. It comprises a pipe 14 and a gas flow rate control device 11 for controlling the flow rate thereof. This vaporizer is connected by piping from the vaporizer 9 to the upper electrode 3 having a shower head.

  As an example of a PECVD apparatus, FIG. 2 shows an inductively coupled remote PECVD apparatus. The inductively coupled remote PECVD apparatus 19 shown in FIG. 2 is expressed by the above-described general formula (1), a plasma generating part wound in a coil shape around quartz at the upper part of the PECVD apparatus chamber, a substrate setting part capable of temperature control. It consists of a vaporizer device that vaporizes the compound to be supplied to the chamber, a plasma generator comprising a high frequency power source and a matching circuit, and an exhaust system comprising a vacuum pump.

  Specifically, the PECVD apparatus 19 includes a PECVD chamber 20, a coil 21 that is a plasma generation unit and a quartz tube 22, a heater unit 23 for installing a thin film forming substrate 24 such as a Si substrate, and a temperature control unit 27, It comprises vaporizing devices 28 to 35 for vaporizing the compound of the general formula (1), a matching circuit 25 and an RF power source 26 which are plasma generation sources, and an exhaust device 36 for exhausting unreacted substances and by-products in the chamber. . 37 is a ground.

  A coil around quartz, which is a plasma generation unit, is connected to the matching circuit 25 and is discharged in the quartz tube by an antenna current magnetic field by RF current to generate plasma. Although it does not specifically limit about the specification of RF power supply 26, The electric power used in the said technical field is 1W-2000W, Preferably it is 10W-1000W, A frequency is 50 kHz-2.5 GHz, Preferably it is 100 kHz-100 MHz, Most preferably, it is 200 kHz- A 50 MHz RF power supply can be used.

  The control of the substrate temperature is not particularly limited, but is in the range of −90 to 1,000 ° C., preferably 0 ° C. to 500 ° C.

  The vaporizer is filled with a compound 33 of the general formula (1) that is liquid at normal temperature and pressure, and is provided with a container 32 having a dip pipe and a pipe 35 that is pressurized with the inert gas, and a general formula (1) that is liquid. A liquid flow rate control device 29 for controlling the flow rate of the compound 33, a vaporizer 28 for vaporizing the compound 33 of the general formula (1) as a liquid, and for supplying the inert gas into the PECVD apparatus chamber via the vaporizer. It comprises a pipe 34, a gas flow rate control device 30 for controlling the flow rate thereof, and a shower head 31 for uniformly supplying an inert gas and gasified compound 33 of the general formula (1) into the chamber.

  The compound represented by the general formula (1) is gasified using the above-described PECVD apparatus or the like, supplied into the chamber together with an inert gas as necessary, and formed into a film by PECVD. The pressure in the chamber at this time is not particularly limited, but is 0.1 Pa to 10000 Pa, preferably 1 Pa to 5000 Pa.

  Although a Si-containing film is obtained in this way, this film has a low relative dielectric constant, and depending on conditions, a film having a relative dielectric constant of 2.0 or less can be obtained. Therefore, it can be used as a low dielectric constant film. it can. Further, this film preferably has a cyclic siloxane structure, and the cyclic siloxane structure may be one in which the cyclic siloxane structure in the cyclic siloxane compound represented by the general formula (1) remains, or is newly formed by plasma. It may be generated. As a result, the film having a cyclic siloxane structure is a porous film having a main pore diameter of 1 nm or less, and the pores are not continuous, there is no metal diffusion into the film, and high mechanical properties are obtained. Since it has high heat conductivity, it is a thin film particularly suitable as a low dielectric constant material (low-k material) for semiconductor devices. That is, it is more preferable to form a film under PECVD conditions that do not destroy the cyclic siloxane structure in the cyclic siloxane compound represented by the general formula (1).

  Further, a thin film with increased porosity or mechanical strength can be obtained by subjecting the above-described Si-containing film to heat treatment, ultraviolet irradiation treatment, or electron beam treatment. A Si-containing film that has been subjected to a combination of these treatments also falls within the scope of the present invention. The thin film obtained by this treatment is suitable as a low dielectric constant insulating material.

  All of the Si-containing films according to the present invention are suitable as low dielectric constant materials, and these can be used for semiconductor devices as insulating films. It is particularly suitable for the manufacture of ULSI using multilayer wiring.

Among the compounds represented by the general formula (1) of the present invention, the compound represented by the general formula (20) is a novel compound. Here, R ¹⁸ , R ¹⁹ , g and h are as described above. Preferably, R ¹⁸ is an alkyl group having 1 to 6 carbon atoms, R ¹⁹ is an alkyl group having 1 to 6 carbon atoms, and g is 3 or 4, h is 1 or 2, more preferably R ¹⁸ is an alkyl group having 1 to 4 carbon atoms, and R ¹⁹ is an alkyl group having 1 to 4 carbon atoms.

  Specific examples of the compound represented by the general formula (20) include 2,4,6-triisopropyl-2,4,6-trimethoxycyclotrisiloxane, 2,4,6-triisopropyl-2,4, 6-triethoxycyclotrisiloxane, 2,4,6-triisopropyl-2,4,6-tri-n-propoxycyclotrisiloxane, 2,4,6-triisopropyl-2,4,6-triisopropoxycyclo Trisiloxane, 2,4,6-tris (methoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6,8-tetrakis (methoxymethyl) -2,4,6,8-tetramethyl Cyclotetrasiloxane, 2,4,6-tris (ethoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6,8-tetrakis (ethoxymethyl) ) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6-tris (isopropoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6,8-tetrakis ( Isopropoxymethyl) -2,4,6,8-tetramethylcyclotetrasiloxane and the like.

  2,4,6-tris (methoxyethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6,8-tetrakis (methoxyethyl) -2,4,6,8-tetramethylcyclotetra Siloxane, 2,4,6-tris (ethoxyethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6,8-tetrakis (ethoxyethyl) -2,4,6,8-tetramethylcyclo Tetrasiloxane, 2,4,6-tris (isopropoxyethyl) -2,4,6-trimethylcyclotrisiloxane, or 2,4,6,8-tetrakis (isopropoxyethyl) -2,4,6,8 -Tetramethylcyclotetrasiloxane and the like.

  According to the present invention, the following remarkable effects are exhibited. That is, as a first effect of the present invention, the use of the cyclic siloxane compound represented by the general formula (1) as the Si-containing film forming material allows the low dielectric constant as a low dielectric constant material in the semiconductor device interlayer insulating film. In addition, a material having high mechanical strength can be provided. Moreover, in this invention, the cyclic siloxane compound represented by General formula (1) useful as a PECVD method interlayer insulation film material can be efficiently manufactured with high purity.

  Examples are shown below, but the present invention is not limited to these Examples. The film thickness was measured using an interference type film thickness measuring device manufactured by Horiba. In addition, the measurement of relative permittivity (k value) was measured by Four Dimensions Inc. The stiffness and Young's modulus were measured using a mercury probe manufactured by Hystron Inc. It measured using the nano indentator by a company.

Example 1 [Production of organosilane compound represented by general formula (10)]
Under a nitrogen stream, 26.7 g (2.20 mol) of metallic magnesium and 0.53 L of dry tetrahydrofuran were charged into a 1 L four-necked flask equipped with a dropping funnel and a stirrer, and cooled to 0 ° C. While stirring, 187 g (1.00 mol) of 4-bromoanisole was added dropwise over 5 hours and reacted at room temperature for 3 hours to obtain a tetrahydrofuran solution of 4-methoxyphenylmagnesium bromide. Under a nitrogen stream, 130 g (0.952 mol) of methyltrimethoxylane and 52.0 ml of dry tetrahydrofuran were charged into a 2 L four-necked flask equipped with a dropping funnel and a stirrer and cooled to 0 ° C. While stirring this, 1.00 mol of the tetrahydrofuran solution of 4-methoxyphenylmagnesium bromide prepared above was added dropwise over 1 hour and reacted at room temperature for 4 hours. After completion of the reaction, the by-product magnesium methoxide residue was removed by filtration, and the obtained filtrate was distilled under reduced pressure to obtain 106 g (0.501 mol) of methyl (4-methoxyphenyl) dimethoxysilane as the target product. The yield was 52.6%.

The results of analyzing the isolated methyl (4-methoxyphenyl) dimethoxysilane by ¹ H-NMR, ¹³ C-NMR, and GC-MS were as follows.
¹ H-NMR; δ 0.33 ppm (s, 3H, C H ₃ —Si), δ 3.55 ppm (s, 6H, 2C H ₃ —O—Si), δ 3.81 ppm (s, 3H, C H ₃ —O) -Ph), [delta] 6.93-6.94 ppm (m, 2H, Ph- H ), [delta] 7.55-7.56 ppm (m, 2H, Ph- H ),
¹³ C-NMR; δ 4.8 ppm ( C H ₃ —Si), 50.7 ppm ( C H ₃ —O—Si), 55.2 ppms ( C H ₃ —O—Ph), δ 113.9 ppm (Ph), δ 125 0.0 ppm (Ph), δ 135.8 ppm (Ph), δ 161.5 ppm (Ph)
_{GC-MS; Mw = 212,} C 10 H 16 О 3 Si.

[Production of cyclic siloxane compound represented by general formula (1)]
A 100 ml Schlenk tube was charged with 21.2 g (100 mmol) of methyl (4-methoxyphenyl) dimethoxysilane, 1.80 g (100 mmol) of pure water, 9.81 g (100 mmol) of sulfuric acid, and 20 ml of tetrahydrofuran. Reacted for hours. After completion of the reaction, THF and water were distilled off, and the resulting organic layer was dried with molecular sieves. After distillation under reduced pressure, the desired product 2,4,6-tris (4-methoxyphenyl) -2,4 , 6-Trimethylcyclotrisiloxane was obtained. The yield was 11.3%, and the conversion rate of methyl (4-methoxyphenyl) dimethoxysilane was 33.8%.

  The results of analyzing the isolated 2,4,6-tris (4-methoxyphenyl) -2,4,6-trimethylcyclotrisiloxane by GC-MS were as follows.

_{GC-MS; Mw = 498,} C 24 H 30 О 6 Si 3.

Example 2 [Production of cyclic siloxane compound represented by general formula (1)]
In a 50 ml Schlenk tube equipped with a stirrer and a dropping funnel, 0.0141 g (0.0800 mmol) of palladium chloride and 20.5 g (640 mmol) of methanol were charged and stirred. From the dropping funnel, 4.81 g (20.0 mmol) of 2,4,6,8-tetramethylcyclotetrasiloxane was added dropwise at room temperature over 30 minutes. After completion of dropping, the mixture was further stirred at room temperature for 15 hours. After completion of the reaction, methanol was distilled off and the Pd residue was filtered off with a glass filter to obtain the desired product 2,4,6,8-tetramethyl-2,4,6,8-tetramethoxycyclotetrasiloxane. . The yield by gas chromatograph was 1.5%.
The result of analyzing the isolated 2,4,6,8-tetramethyl-2,4,6,8-tetramethoxycyclotetrasiloxane by GC-MS was as follows.

_{GC-MS; Mw = 360,} C 8 H 24 О 8 Si 4.

Example 3 [Production of Cyclic Siloxane Compound Represented by General Formula (1)]
A 200 ml Schlenk tube equipped with a stirrer and a dropping funnel was charged with 13.62 g (0.100 mol) of methyltrimethoxysilane and 100 ml of toluene and stirred to 80 ° C. From the dropping funnel, 1.35 g of pure water was added dropwise at 80 ° C. over 10 minutes. After completion of the dropwise addition, the mixture was further stirred for 2 hours under reflux conditions. After completion of the reaction, toluene was distilled off, and 2,4,6,8-tetramethyl-2,4,6,8-tetramethoxycyclotetrasiloxane was obtained as a target product by distillation under reduced pressure. The yield was 4.6%, and the conversion rate of methyltrimethoxysilane was 13.8%.
The result of analyzing the isolated 2,4,6,8-tetramethyl-2,4,6,8-tetramethoxycyclotetrasiloxane by GC-MS was as follows.

_{GC-MS; Mw = 360,} C 8 H 24 О 8 Si 4.

Example 4 [Production of Cyclic Siloxane Compound Represented by General Formula (1)]
A 200 ml Schlenk tube equipped with a stirrer and a dropping funnel was charged with 96.2 g (1.60 mol) of isopropanol and 0.740 g (0.80 mmol) of chlorotris (triphenylphosphine) rhodium (I), stirred and added dropwise. From the funnel, 48.1 g (0.20 mol) of 2,4,6,8-tetramethylcyclotetrasiloxane was added dropwise at room temperature over 20 minutes. After completion of dropping, the mixture was stirred for 4 hours under refluxing isopropanol. After completion of the reaction, isopropanol was distilled off, and 2,4,6,8-tetramethyl-2,4,6,8-tetraisopropoxycyclotetrasiloxane, which was the target product, was obtained by distillation under reduced pressure. The yield was 54.9%.

  The result of analyzing the isolated 2,4,6,8-tetramethyl-2,4,6,8-tetraisopropoxycyclotetrasiloxane by GC-MS was as follows.

_{GC-MS; Mw = 472,} C 16 H 40 О 8 Si 4.

Example 5 [Production of cyclic siloxane compound represented by general formula (1)]
A 200 ml Schlenk tube equipped with a stirrer and a dropping funnel was charged with 2.4 g of 0.01N sulfuric acid solution in 20.0 g (0.217 mol) of toluene and stirred. From the dropping funnel, 20.0 g (0.133 mol) of methyl (methoxymethyl) dimethoxysilane was added dropwise at room temperature over 5 minutes. After completion of dropping, the mixture was stirred at room temperature for 7 hours. After completion of the reaction, toluene was distilled off, and 2,4,6,8-tetrakis (methoxymethyl) -2,4,6,8-tetramethylcyclotetrasiloxane was obtained as a target product by distillation under reduced pressure. The yield was 15.3%, and the conversion rate of methyl (methoxymethyl) dimethoxysilane was 61.2%.

The isolated 2,4,6,8-tetrakis (methoxymethyl) -2,4,6,8-tetramethylcyclotetrasiloxane was analyzed by ¹ H-NMR, ¹³ C-NMR, and GC-MS. It was as follows.
^{1 H-NMR; δ0.17~0.19ppm (m} , 12H, 4C H 3 -Si),
δ 3.04-3.07 ppm (m, 8H, 4CH ₃ —O—C H ₂ Si),
δ 3.34 to 3.36 ppm (m, 12H, 4C H ₃ —O—CH ₂ Si)
¹³ C-NMR; δ-2.2 ppm ( C H ₃ -Si),
_{δ62.9ppm (CH 3 -O- C H 2} Si),
δ 65.8 ppm ( C H ₃ —O—CH ₂ Si)
_{GC-MS; Mw = 416,} C 12 H 32 О 8 Si 4.

Example 6 [PECVD Film Formation Using Cyclic Siloxane Compound Represented by General Formula (1)]
The 2,4,6-tris (4-methoxyphenyl) -2,4,6-trimethylcyclotrisiloxane synthesized in Example 1 was formed on a silicon substrate using the capacitively coupled PECVD apparatus shown in FIG. did. The film forming conditions were as follows: argon gas as an inert gas was supplied at 10 sccm, and vaporized 2,4,6-tris (4-methoxyphenyl) -2,4,6-trimethylcyclotrisiloxane was set at a chamber internal pressure of 10 Pa. The film was formed under the conditions of a substrate temperature of 150 ° C., an RF power supply power of 30 W, and an RF power supply frequency of 13.56 MHz. As a result, the deposition rate was 4.3 nm / min. The relative dielectric constant (k value) was 2.7. Regarding mechanical properties, the rigidity was 1.3 GPa and the Young's modulus was 13.9 GPa.

Example 7 [PECVD film formation using cyclic siloxane compound represented by general formula (1)]
2,4,6,8-tetramethyl-2,4,6 synthesized in Example 3 instead of 2,4,6-tris (4-methoxyphenyl) -2,4,6-trimethylcyclotrisiloxane A PECVD thin film was obtained in the same manner as in Example 6 except that, 8-tetramethoxycyclotetrasiloxane was used. As a result, the film formation rate was 12.8 nm / min. The relative dielectric constant (k value) was 2.6. Regarding mechanical properties, the stiffness was 1.36 GPa and the Young's modulus was 15.2 GPa.

Example 8 [PECVD film formation using cyclic siloxane compound represented by general formula (1)]
2,4,6,8-tetramethyl-2,4,6 synthesized in Example 4 instead of 2,4,6-tris (4-methoxyphenyl) -2,4,6-trimethylcyclotrisiloxane A PECVD thin film was obtained in the same manner as in Example 6 except that, 8-tetraisopropoxycyclotetrasiloxane was used. As a result, the film formation rate was 11.2 nm / min. The relative dielectric constant (k value) was 2.4. As for mechanical properties, the rigidity was 1.1 GPa and the Young's modulus was 17.1 GPa.

Example 9 [PECVD film formation using cyclic siloxane compound represented by general formula (1)]
2,4,6,8-tetrakis (methoxymethyl) -2 synthesized in Example 5 instead of 2,4,6-tris (4-methoxyphenyl) -2,4,6-trimethylcyclotrisiloxane A PECVD thin film was obtained in the same manner as in Example 6 except that 4,6,8-tetramethylcyclotetrasiloxane was used. As a result, the film formation rate was 6.8 nm / min. The relative dielectric constant (k value) was 1.8. Regarding mechanical properties, the rigidity was 1.6 GPa and the Young's modulus was 22.1 GPa.

Comparative Example 1
Example 6 except that 2,4,6,8-tetramethylcyclotetrasiloxane was used instead of 2,4,6-tris (4-methoxyphenyl) -2,4,6-trimethylcyclotrisiloxane. In the same manner, a PECVD thin film was obtained. The result is a film formation rate of 10.4 nm / min. The relative dielectric constant (k value) was 2.9. As for mechanical properties, the rigidity was 1.1 GPa and the Young's modulus was 10.7 GPa.

It is a figure which shows a parallel plate capacitive coupling type PECVD apparatus. It is a figure which shows an inductively coupled remote PECVD apparatus.

Explanation of symbols

1. PECVD apparatus 2. PECVD chamber Upper electrode 4. Lower electrode 5. 5. Substrate for thin film formation 6. Matching circuit RF power supply 8. Temperature controller 9. Vaporizer 10. Liquid flow controller 11. Gas flow control device 12. Container 13. Compound represented by general formula (1) 14. Piping 15. Piping 16. Exhaust device 17. Earth 18. Earth 19. PECVD apparatus 20. PECVD chamber 21. Coil 22. Quartz tube 23. Heater section 24. Thin film forming substrate 25. Matching circuit 26. RF power supply 27. Temperature controller 28. Vaporizer 29. Liquid flow control device 30. Gas flow control device 31. Shower head 32. Container 33. Compound represented by formula (1) 34. Piping 35. Piping 36. Exhaust device 37. Earth

Claims (9)

The following general formula (20)

(Wherein R ¹⁸ represents an alkyl group having 1 to 6 carbon atoms, R ¹⁹ represents an alkyl group having 1 to 6 carbon atoms, g represents 3 or 4, and h represents 1 or 2). A Si-containing film-forming material for chemical vapor deposition, comprising the cyclic siloxane compound shown. The cyclic siloxane compound represented by the general formula (20) is 2,4,6-tris (methoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6,8-tetrakis (methoxymethyl). -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6-tris (ethoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6,8-tetrakis (ethoxymethyl) ) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6-tris (isopropoxymethyl) -2,4,6-trimethylcyclotrisiloxane, 2,4,6,8-tetrakis ( Isopropoxymethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6-tris (methoxyethyl) -2,4,6-trimethylcyclo Lisiloxane, 2,4,6,8-tetrakis (methoxyethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6-tris (ethoxyethyl) -2,4,6-trimethyl Cyclotrisiloxane, 2,4,6,8-tetrakis (ethoxyethyl) -2,4,6,8-tetramethylcyclotetrasiloxane, 2,4,6-tris (isopropoxyethyl) -2,4,6 Si according to claim 1, characterized in that it is trimethylcyclotrisiloxane or 2,4,6,8-tetrakis (isopropoxyethyl) -2,4,6,8-tetramethylcyclotetrasiloxane. Containing film forming material. The Si-containing film-forming material according to claim 1 or 2, wherein the cyclic siloxane compound represented by the general formula (20) has a molecular weight of less than 1000. 4. The Si-containing film formation according to claim 1, wherein the amount of impurities other than silicon, carbon, oxygen, hydrogen, nitrogen, and boron is less than 10 ppb, and the water content is less than 50 ppm. material. A method for producing a Si-containing film, wherein the Si-containing film forming material according to any one of claims 1 to 4 is used as a raw material to form a film by chemical vapor deposition. 6. The method according to claim 5, wherein the chemical vapor deposition method is a plasma enhanced chemical vapor deposition method. A Si-containing film obtained by the production method according to claim 5. The Si-containing film according to claim 7, comprising a cyclic siloxane structure in the cyclic siloxane compound represented by the general formula (20). A semiconductor device using the film according to claim 7 as an insulating film.

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