Main > ELECTRICAL > Insulation > Poly(ImidoSiloxane). Film. > PhotoCurable Compn.

Product Japan. U

PATENT ASSIGNEE'S COUNTRY Japan
UPDATE 08.00
PATENT NUMBER This data is not available for free
PATENT GRANT DATE 01.08.00
PATENT TITLE Photosensitive polyimidosiloxane compositions and insulating films made thereof

PATENT ABSTRACT A photosensitive polyimidosiloxane composition comprising a polyimidosiloxane comprising 15-80 mole percent of the units, ##STR1## wherein X represents CO, O or a direct bond and R.sub.3 represents an aromatic residue containing a photosensitive group with an unsaturated hydrocarbon group, and 85-20 mole percent of the units, ##STR2## wherein X is as defined above, each R.sub.4 independently represents a divalent hydrocarbon residue, each R.sub.5 independently represents an alkyl group of 1-3 carbon atoms and 1 represents an integer of 3-30, a finely divided inorganic filler, and an organic solvent. The composition provides films having excellent light transmittance.

PATENT INVENTORS This data is not available for free
PATENT ASSIGNEE This data is not available for free
PATENT FILE DATE 05.12.97
PATENT FOREIGN APPLICATION PRIORITY DATA This data is not available for free
PATENT REFERENCES CITED English Transaction of Japanese Kokai Patent Application 3-71633, by United States Patent and Trademark Office, Jul. 1997 (PT097-4442), Mar. 27, 1991.
European Patent Application No. 0,459,809 to Nakajima et al. dated Dec. 4, 1991.
Japanese Laid Open Patent Publication No. 8-76376 to Shinetsu Kagaku Kogyo K.K. dated Mar. 22, 1996 (including an English language description).
Japanese Laid Open Patent Publication No. 57-131227 to Sugihara dated Aug. 14, 1982 (including an English language abstract).
Japanese Laid Open Patent Publication No. 2-50161 to Nobuyuki et al. dated Feb. 20, 1990 (including an English language abstract).
Japanese Laid Open Patent Publication No. 4-252227 to Eguchi dated Sep. 8, 1992 (including an English language abstract).
Patent Abstracts of Japan, vol. 14, No. 219, p. 1045, Sumitomo Bakelite Co., Ltd., "Photosensitive Resin Composition," Publication No. 2-50161, Feb. 20, 1990.
Japanese Laid Open Patent Publication No. 3-71633 to Takeuchi et al., dated Mar. 27, 1991.
Japanese Laid Open Patent Publication No. 6-11832 to Okunoyama dated Jan. 21, 1994.
Takeuchi et al. 115:172528, Chemical Abstracts, on line from Columbis, Ohio of JP 6-11832, published Jan. 21, 1994 with Registry No. 26374-94-4, 535-87-5, and 1823-59-2, on line, cited in Abstract.
Takeuchi et al., 03-71633, Patent Abstract of Japan, Abstract Group No. E1078, vol. 15, No. 236, Abstract published Jun. 18, 1991 of JP 3-71633.
Takeuchi et al., AN 91-135616, Derwent Information Ltd., on line English Abstract of JP 3-761633A.

PATENT PARENT CASE TEXT This data is not available for free
PATENT CLAIMS What is claimed is:

1. A photosensitive polyimidosiloxane composition comprising:

a polyimidosiloxane comprising 15-80 mole percent of the units, ##STR6## wherein X represents a direct bond and R.sub.3 represents an aromatic residue containing a photosensitive group with an unsaturated hydrocarbon group, and 85-20 mole percent of the units, ##STR7## wherein X is as defined above, each R.sub.4 independently represents a divalent hydrocarbon residue, each R.sub.5 independently represents an alkyl group of 1-3 carbon atoms or a phenyl group and 1 represents an integer of 3-30,

a finely divided inorganic filler, and

an organic solvent

wherein an insulating film of a thickness of 2-50 .mu.m obtained from said photosensitive polyimidosiloxane composition has a resolution of at least 10 .mu.m after photocuring by irradiation with a superhigh-pressure mercury lamp (2 kW) on a dried film prepared from said photosensitive polyimidosiloxane composition, immersing the photocured film in a triglyme solvent and washing off the uncured portions, and then washing the surface with methanol to obtain a relief pattern adhering to the polyimide film which is then heat treated at 160.degree. C. for 120 minutes.

2. A photosensitive polyimidosiloxane composition according to claim 1, wherein the finely divided inorganic filler is selected from the group consisting of silica, talc, Wallastonite and calcium carbonate powders.

3. A photosensitive polyimidosiloxane composition according to claim 1, wherein the finely divided inorganic filler is contained in an amount of 10-100 parts by weight per 100 parts by weight of the polyimidosiloxane.

4. A photosensitive polyimidosiloxane composition according to claim 1, wherein the solid concentration consisting of the polyimidosiloxane is 20 to 50 wt %.

5. A photosensitive polyimidosiloxane composition according to claim 1, wherein at least one of a sensibilizer, photopolymerization initiator, adhesion-improving agent and air-shutting agent is added in a total amount of 1-50 wt % with respect to the photosensitive polyimidosiloxane.

6. A photosensitive polyimidosiloxane composition according to claim 1, wherein the polyimidosiloxane is prepared by polymerization and imidation of substantially equimolar amounts of:

an aromatic tetracarboxylic dianhydride component represented by the following general formula (1)

R.sub.1 --X--R.sub.2 ( 1)

wherein R.sub.1 and R.sub.2 each represent mononuclear aromatic residues with acid anhydride groups and X represents a direct bond, and

a diamine component consisting of 15-80 mole percent of an aromatic diamine compound containing a photosensitive group, represented by the following general formula (2)

H.sub.2 N--R.sub.3 --NH.sub.2 ( 2)

wherein R.sub.3 represents an aromatic residue containing a photosensitive group with an unsaturated hydrocarbon group, and 85-20 mole percent of a diaminopolysiloxane represented by the following general formula (3) ##STR8## wherein each R.sub.4 independently represents a divalent hydrocarbon residue, each R.sub.5 independently represents an alkyl group of 1-3 carbon atoms or a phenyl group and l represents an integer of 3-30.

7. A photosensitive polyimidosiloxane composition according to claim 6, wherein the aromatic tetracarboxylic dianhydride component is 2,3,3',4'-biphenyltetracarboxylic dianhydride.

8. A photosensitive polyimidosiloxane composition according to claim 1, wherein the polyimidosiloxane is prepared by polymerization and imidation of an aromatic tetracarboxylic dianhydride component represented by the general formula (1)

R.sub.1 --X--R.sub.2 ( 1)

wherein R.sub.1 and R.sub.2 each represent mononuclear aromatic residues with acid anhydride groups an X represents a direct bond, an aromatic diamine component having a --OH or --COOH group and diaminopolysiloxane represented by the general formula (3) ##STR9## wherein each R.sub.4 independently represents a divalent hydrocarbon residue, each R.sub.5 independently represents an alkyl group of 1-3 carbon atoms or a phenyl group and l represents an integer of 3 -30 to form a polyimidosiloxane having a --OH or --COOH group, and reaction of the resulting polyimidosiloxane with a (meth)acryloyl compound.

9. A photosensitive polyimidosiloxane composition according to claim 8, wherein the aromatic diamine component having a --OH or --COOH group is 3,3'-dihydroxy-4,4'-diaminodiphenyl ether or 5,5'-methylene-bis[2-aminobenzoic acid].

10. A photosensitive polyimidosiloxane composition according to claim 8, where the (meth)acryloyl compound is glycidyl methacrylate, glycidyl acrylate or a half-epoxy (meth)acrylate.

11. A photosensitive polyimidosiloxane composition according to claim 1, wherein the insulating film is formed on a circuit board.

12. A photosensitive polyimidosiloxane composition according to claim 1, wherein the insulating film has a soldering heat resistance of 250-300.degree. C.
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PATENT DESCRIPTION BACKGROUND OF THE INVENTION

1. Field of the Invention

The present invention relates to novel aromatic polyimidosiloxanes with excellent solubility in organic solvents and containing photosensitive groups in their main polymer chains. More specifically, the present invention relates to organic solvent-soluble photosensitive polyimidosiloxanes providing photocured products with excellent heat resistance, electrical properties and mechanical properties including flexibility, which are suitable as overcoat materials for flexible wiring boards, interlayer insulating materials, or materials for forming insulating films on solid elements and passivation films for industrial semiconductors.

2. Description of the Related Art

Overcoat materials for flexible wiring boards, interlayer insulating films for multilayer boards, materials for forming insulating films on solid elements and passivation films for industrial semiconductors, as well as interlayer insulating materials for semiconductor integrated circuits and multilayer printed wiring boards, require excellent heat resistance and insulating properties, and photosensitive heat resistant materials are being sought to meet the demand for high density and high integration.

A number of ideas have been devised for forming such insulating films of polyimides, due to their high heat resistance and insulating properties.

However, commonly used polyimides are either insoluble in solvents and have no photosensitive groups, or the polymers containing photosensitive groups are all in the form of polyimide precursors, i.e. polyamic acids, modified by amidation or esterification of the carboxylic acid, and must have the polyamic acids converted into polyimides during photocuring, or be post-baked into polyimides after photocuring.

There also exist heat-resistant photoresist compositions prepared by mixing organic solvent-soluble polyimides (without photosensitive groups) with monomers which contain a photocurable group and subjecting the mixture to photocuring (see, for example, Japanese Unexamined Patent Publication No. 54-109828), but such compositions have inferior photocuring properties, while the heat resistance of the polyimides after photocuring is insufficient. In addition, since aromatic polyimides with superior heat resistance generally have inferior solubility in solvents, they are not suitable for the formation of relief patterns which involves a step of dissolving the unexposed parts after photocuring.

Ideas have also been proposed for obtaining polyimides with excellent photosensitivity and heat resistance by reacting a tetracarboxylic dianhyride with a diamine compound containing a photocrosslinkable unsaturated double bond, such as diaminochalcone (see, for example, Japanese Unexamined Patent Publication No. 57-131227).

However, although polyimides obtained in this manner have excellent photosensitivity, their inferior solubility in organic solvents results in longer times required for dissolution, thus constituting a practicality problem for the formation of relief patterns.

Polyimidosiloxanes have also been proposed in order to obtain flexible photosensitive polyimides (Japanese Unexamined Patent Publication Nos. 2-50161, 4-252227), but since polyamic acids are used as the polymer components, high-temperature heating is necessary after patterning to accomplish imidation, thus constituting a practicality problem in that thermal damage can occur in the board.

SUMMARY OF THE INVENTION

It is an object of the present invention to provide a photosensitive polyimidosiloxane composition having substantially no practicality problems.

It is another object of the present invention to provide an electrical insulating film with satisfactory resolution, which can be formed to a large thickness and requires no high-temperature heating (250-400.degree. C.) for imidation after patterning.

The present invention provides a photosensitive polyimidosiloxane composition comprising:

a polyimidosiloxane comprising 15-80 mole percent of the units, ##STR3## wherein X represents CO, O or a direct bond and R.sub.3 represents an aromatic residue containing a photosensitive group with an unsaturated hydrocarbon group, and 85-20 mole percent of the units, ##STR4## wherein X is as defined above, each R.sub.4 independently represents a divalent hydrocarbon residue, each R.sub.5 independently represents an alkyl group of 1-3 carbon atoms and l represents an integer of 3-30,

a finely divided inorganic filler, and

an organic solvent,

the photocured product of said photosensitive polyimidosiloxane composition exhibiting excellent light transmittance.

The present invention also provides an insulating film obtained from the photosensitive polyimidosiloxane composition according to the present invention, which has a thickness of 2-50 .mu.m and a resolution of at least 10 .mu.m after photocuring by irradiation with a superhigh-pressure mercury lamp (2 kW) on a dried film prepared from the photosensitive polyimidosiloxane composition.

DESCRIPTION OF THE PREFERRED EMBODIMENTS

The polyimidosiloxane usable for the photosensitive polyimidosiloxane composition according to the present invention may be prepared by polymerization and imidation of substantially equimolar amounts of:

an aromatic tetracarboxylic dianhydride component represented by the following general formula (1)

R.sub.1 --X--R.sub.2 (1)

wherein R.sub.1 and R.sub.2 each represent mononuclear aromatic residues with acid anhydride groups and X is as defined above,

and a diamine component consisting of 15-80 mole percent of an aromatic diamine compound containing a photosensitive group, represented by the following general formula (2)

H.sub.2 N--R.sub.3 --NH.sub.2 (2)

wherein R.sub.3 is as defined above, and 85-20 mole percent of a diaminopolysiloxane represented by the following general formula (3) ##STR5## wherein R.sub.4, R.sub.5 and l are as defined above.

The polyimidosiloxanes may be produced by random or block polymerization of substantially equimolar amounts of an aromatic tetracarboxylic dianhydride and two types of diamine components, represented by the general formulas given above, in an organic solvent, followed by chemical imidation of the resulting polyamic acid.

The aromatic tetracarboxylic dianhydride represented by general formula (1) above may be a biphenyltetracarboxylic dianhydride, benzophenonetetracarboxylic dianhydride or oxydiphthalic anhydride, preferred among which are 3,3',4,4'-benzophenonetetracarboxylic dianhydride and 2,3,3',4'-biphenyltetracarboxylic dianhydride (a-BPDA).

The photosensitive group-containing aromatic diamine represented by general formula (2) above may be any aromatic diamine with a photosensitive unsaturated hydrocarbon group, examples of which include unsaturated benzoic acid esters such as 3,5-diaminobenzoic ethylacrylic acid ester, 2,4-diaminobenzoic ethylacrylic acid ester, 3,5-diaminobenzoic ethylmethacrylic acid ester, 2,4-diaminobenzoic ethylmethacrylic acid ester, 3,5-diaminobenzoic glycidylacrylate ester, 2,4-diaminobenzoic glycidylacrylate ester, 3,5-diaminobenzoic glycidylmethacrylate ester, 2,4-diaminobenzoic glycidylmethacrylate ester, 3,5-diaminobenzoic cinnamyl ester and 2,4-diaminobenzoic cinnamyl ester; benzyl (meth)acrylates such as 3,5-diaminobenzyl acrylate and 3,5-diaminobenzyl methacrylate; unsaturated diphenylether esters such as 4-acrylamido-3,4'-diaminodiphenyl ether, 2-acrylamido-3,4'-diaminodiphenyl ether, 2-acrylamido-3,4'-diaminodiphenyl ether, 4-cinnamamido-3,4'-diaminodiphenyl ether, 3,4'-diacrylamido-3',4-diaminodiphenyl ether, 3,4'-dicinnamamido-3',4-diaminodiphenyl ether, 4-methyl-2'-carboxyethylmethacrylic acid ester-3,4'-diaminodiphenyl ether [carboxyethylmethacrylic acid ester: CH.sub.2 .dbd.C(CH.sub.3)COOCH.sub.2 CH.sub.2 OOC--], and 4-methyl-2'-carboxyethylacrylic acid ester-3,4'-diaminodiphenyl ether [carboxyethylacrylic acid ester: CH.sub.2 .dbd.CHCOOCH.sub.2 CH.sub.2 OOC--]; and substituted or unsubstituted diaminochalcones such as 4,4'-diaminochalcone, 3,3'-diaminochalcone, 3,4'-diaminochalcone, 3',4-diaminochalcone, 4'-methyl-3',4-diaminochalcone, 4'-methoxy-3',4-diaminochalcone and 3'-methyl-3,5-diaminochalcone.

A single photosensitive group-containing aromatic diamine represented by general formula (2) above may be used, or 2 or more thereof may be used in combination.

The diaminopolysiloxane represented by general formula (3) above preferably is one wherein R.sub.4 in general formula (3) is a divalent hydrocarbon residue, preferably a "polymethylene" group of 2-6 carbon atoms, particularly 3-5 carbon atoms, or a phenylene group, R.sub.5 is independently an alkyl group of 1-3 carbon atoms such as a methyl, ethyl, propyl or a phenyl group, and l is 3-30, especially 5-20. So long as l is in the aforementioned range (3-30), the diaminopolysiloxane represented by general formula (3) may be a homogeneous compound, or it may be a mixture of compounds with different values for l. In the case of a mixture, the average value for l is preferably in the range of 5-20, as calculated based on amino equivalents.

According to the present invention, the diamine components may be a photosensitive group-containing aromatic diamine represented by general formula (2) above and a diaminopolysiloxane represented by general formula (3) above, and the aromatic diamine represented by general formula (2) may be used in a proportion of 15-80 mole percent, preferably 20-70 mole percent, and the diaminopolysiloxane represented by general formula (3) in a proportion of 85-20 mole percent, preferably 80-30 mole percent.

If the proportion of the photosensitive group-containing aromatic diamine represented by general formula (2) is less than the minimum given above, then the photosensitivity of the resulting photosensitive polyimidosiloxane may be reduced, a high resolution electrical insulating film may not be obtained after photocuring, and the thermal decomposition temperature of the photosensitive polyimidosiloxane may be lowered. If the proportion of the photosensitive group-containing aromatic diamine represented by general formula (2) is greater than the maximum given above, then the organic solubility of the resulting photosensitive polyimidosiloxane may be reduced.

Other aromatic diamines may also be used in addition to the diamines represented by general formulas (2) and (3). These are preferably used at not more than 65 mole percent, more preferably not more than 30 mole percent of the diamine component. Other suitable aromatic diamines include, for example, aromatic diamines with two benzene rings such as 4,4'-diaminodiphenyl ether, 4,4'-diaminodiphenylmethane, 4,4'-diaminodiphenylsulfone and o-tolidine; aromatic diamines with 3 benzene rings such as 1,4-bis(4-aminophenoxy)benzene and 1,4-bis(4-aminophenyl)benzene; and aromatic diamines with 4 benzene rings such as bis[4-(4-aminophenoxy)phenyl]sulfone and 2,2-bis[4-(4-aminophenoxy)phenyl]propane.

The photosensitive polyimidosiloxane may preferably be obtained by first subjecting an aromatic tetracarboxylic dianhyride component and a substantially equimolar amount of a diamine component to a random or block polymerization reaction, preferably a random polymerization reaction, for about 1-48 hours in an organic solvent at a reaction temperature of 100.degree. C. or lower, preferably at a reaction temperature of 10-80.degree. C., and then diluting the polyamic acid solution resulting from the polymerization reaction with an organic solvent, and adding a chemical imidating agent, for example a carboxylic anhydride such as acetic anhydride or a tertiary amine such as pyridine, at a temperature of 100.degree. C. or lower, preferably at a reaction temperature of 10-50.degree. C., for imidation reaction for about 0.1 to 5 hours.

The organic solvent used for the above-mentioned polymerization reaction and imidation reaction may be, for example, N,N-dimethylsulfoxide, N,N-dimethylformamide, N,N-diethylformamide, N,N-dimethylacetoamide, N,N-diethylacetoamide, N-methyl-2-pyrrolidone (NMP) or hexamethylenephosphoamide.

Alternatively, the photosensitive polyimidosiloxane may be prepared by polymerization and imidation of an aromatic tetracarboxylic dianhydride component represented by the above-mentioned general formula (1), an aromatic diamine component having a --OH or --COOH group such as 3,3'-dihydroxy-4,4'-diaminodiphenyl ether or 5,5'-methylene-bis[2-aminobenzoic acid] and a diaminopolysiloxane represented by the above-mentioned general formula (3) to form a polyimide, and reaction of the resulting polyimide with a (meth)acryloyl compound such as glycidyl methacrylate, glycidyl acrylate or, preferably, a half-epoxy (meth)acrylate (the half number of epoxy groups of an epoxy compound having about 10 epoxy groups are replaced by (meth)acrylate groups) under an inert gas atmosphere such as N.sub.2 at a low temperature.

The photosensitive polyimidosiloxane may be used without modification, or depending on the use, for example when used as a pattern-forming material, it is preferably used as a solution in an organic solvent.

The aforementioned organic solvent used for the photosensitive polyimidosiloxane composition according to the present invention may be a sulfoxide-based solvent such as dimethylsulfoxide or diethylsulfoxide, a formamide-based solvent such as N,N-dimethylformamide or N,N-diethylformamide, an acetoamide-based solvent such as N,N-dimethylacetoamide or N,N-diethylacetoamide, a pyrrolidone-based solvent such as N-methyl-2-pyrrolidone, N-ethyl-2-pyrrolidone or N-vinyl-2-pyrrolidone, a glyme-based solvent such as methyldiglyme or methyltriglyme, or hexamethylphosphoric triamide, .gamma.-butyllactone or cyclohexanone.

The polymer solid concentration in the photosensitive polyimidosiloxane composition of the invention is preferably 20-50 wt %.

A sensitizer and photopolymerization initiator as well as an adhesion-improving agent such as a thermosetting resin or melamine resin and an air-shutting agent such as vaseline or paraffin wax are preferably also added to the photosensitive polyimidosiloxane composition.

A photopolymerizable compound with an ethylenic unsaturated group may also be added within a range which does not impair the properties of the insulating film after photocuring.

The aforementioned sensibilizer or photopolymerization initiator may be Michler's ketone, benzoin, benzoin methyl ether, benzoin ethyl ether, benzoin isopropyl ether, 2-t-butylanthraquinone, 1,2-benzo-9,10-anthraquinone, 4,4'-bis(diethylamino)benzophenone, acetophenone, benzophenone, thioxanthone, 1,5-acenaphthene, 1-hydroxy-cyclohexylphenyl ketone, 2-benzyl-1,2-dimethylamino-1-(4-morpholinophenyl)butane-1,1-hydroxy-cycloh exylphenyl ketone, etc., and these are preferably added in a total of 1-50 parts by weight, and especially 10-50 parts by weight, with respect to 100 parts by weight of the polyimidosiloxane.

The above-mentioned photopolymerizable compound having an ethylenic unsaturated group may be ethyleneglycol di(meth)acrylate, propyleneglycol di(meth)acrylate, trimethylolpropane tri(meth)acrylate, tetramethylolmethane tetra(meth)acrylate, N,N'-methylene bis(meth)acrylate, diethylaminoethyl (meth)acrylate, 1,3,5-triacryloylhexahydro-s-triazine, tris(hydroxyethylacryloyl) isocyanate, (meth)acryloxyethyl phosphate or bis[(meth)acryloxyethyl]phosphate.

The photosensitive polyimidosiloxane composition of the invention contains a finely divided inorganic filler such as Wallastonite, silica, talc or calcium carbonate powder preferably in an amount of 10-100 parts by weight per 100 parts by weight of the photosensitive polyimidosiloxane.

A pattern may be formed by using the photosensitive polyimidosiloxane composition as mentioned above.

For example, the above-mentioned photosensitive polyimidosiloxane composition may be first applied onto a board and then dried to remove the organic solvent. The application onto the board may be accomplished by screen printing, a curtain roll, a reverse roll, or the like. The applied film (preferably with a thickness of 5-100 .mu.m, and especially 10-100 .mu.m) is dried at 90.degree. C. or lower, and preferably 40-80.degree. C. After drying, a negative photomask is placed on the dried applied film which is then irradiated with activating light rays such as ultraviolet rays, visible light rays or electron rays. A polyimidosiloxane pattern may then be obtained by washing the unexposed portions with a developing agent using a shower or ultrasonic waves. The thickness of the cured film is preferably about 2-50 .mu.m.

The developing agent may be an organic solvent such as N,N-dimethylformamide, N,N-dimethylacetoamide, dimethylsulfoxide, N-methyl-2-pyrrolidone, hexamethylenephosphoamide, diglyme, triglyme, or a mixture thereof with methanol, ethanol or the like.

The photosensitive polyimidosiloxane as mentioned above is very readily soluble, and thus the polyimidosiloxane in the unexposed portions is easily removed to allow ready formation of a pattern.

Many other excellent effects are provided, in that since the photosensitive polyimidosiloxane composition of the invention have high photosensitivity and excellent light transmittance and photocrosslinkability, there is no need for a separate resist for image formation as with non-photosensitive polyimides of the prior art, and since there is no need for high-temperature heating (250-400.degree. C.) for imidation after image formation as with photosensitive polyamic acids, an after-heating step at 150-200.degree. C. being sufficient, not only are high reliability and lower cost afforded, but thermal damage to the boards is also avoided. The photosensitive polyimidosiloxane composition of the invention may therefore be suitably used for the formation of both negative patterns and positive patterns.

Furthermore, patterns made with cured films formed from photosensitive polyimidosiloxane compositions of the invention have excellent heat resistance and electrical and mechanical properties, and especially excellent flexibility. For example, an insulating film according to the invention, suitably with a thickness of about 2-50 .mu.m, has a post-photocuring resolving power of at least 10 .mu.m, and usually about 10-1000 .mu.m. Thus, the insulating film according to the invention is particularly suited as an insulating material for high-density flexible boards.

Examples of the present invention will now be provided.

Evaluation of the following examples was conducted in the following manner.

(Property tests)

1. Inherent viscosity

The inherent viscosity (In .eta./c) was measured at 30.degree. C. in a solution containing 0.5 g of a polymer in 100 ml of N-methyl-2-pyrrolidone.

2. Polyimidosiloxane film formability

A solution of 20 g polyimidosiloxane dissolved in 100 ml N-methyl-2-pyrrolidone was applied onto a Teflon plate (1.0 mm) to a polyimidosiloxane film thickness of approximately 20 .mu.m and dried at 70.degree. C. for 30 minutes, and the occurrence of cracks upon heating at 160.degree. C. for 60 minutes and 180.degree. bending was observed. Absence of cracking was indicated by ".largecircle.", and cracking was indicated by ".times.".

3. Solubility of polyimidosiloxane in NMP

A 0.2 g portion of polyimidosiloxane was added to 0.8 g of N-methyl-2-pyrrolidone, and the state of dissolution of the polyimidosiloxane was observed, indicating dissolution for up to 1 hour by "*", dissolution for up to one day by ".largecircle.", swelling alone by ".DELTA.", and no dissolution by ".times.".

4. Thermal decomposition temperature

This was measured using a thermogravimetric analyzer.

5. Evaluation of photocuring property

A dam was constructed using a polyimide film as the spacer, a bar coater was used for uniform casting of ink on copper foil (35 .mu.m), and the dried film obtained from drying at 70.degree. C. for 30 minutes was subjected to the photosensitivity and resolving power tests described below.

Photosensitivity

The dried film was irradiated using a superhigh-pressure mercury lamp (2 kW) at an illuminance of 7 mW/cm.sup.2, and the amount of light irradiation required for photocuring was recorded.

Resolution

A negative film (a test pattern containing an equally-spaced figure pattern having a line width and spacing of 0.075-2.0 mm) was placed on the dried film, and a superhigh-pressure mercury lamp (2 kW) was used to produce a prescribed degree of irradiation for photocuring, after which it was immersed in a triglyme solvent and the uncured portions were washed off, the surface was washed with methanol to obtain a relief pattern adhering to the polyimide film which was then heat treated at 160.degree. C. for 120 minutes, and the resolution of the pattern was measured.

6. Measurement of mechanical properties

The photosensitive polyimidosiloxane composition was coated onto a polytetrafluoroethylene film and dried at 70.degree. C. for 30 minutes, and after subsequent 1 J/cm.sup.2 ultraviolet light exposure and heating at 200.degree. C. for one hour, the film was peeled off, a dumbbell-shaped test piece was cut out, and a tension tester was used for measurement according to ASTM D882 to determine the tensile strength, elongation rate and initial elastic modulus.

7. Electrical properties

The photosensitive polyimidosiloxane composition was applied onto a 0.3 mm-thick copper plate and dried at 70.degree. C. for 30 minutes, and the sample obtained by subsequent 1 J/cm.sup.2 ultraviolet light exposure and heating at 200.degree. C. for one hour was subjected to testing based on JIS C 2103 (electrical insulation varnish test method).

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