Title of Invention

A RADIATION SENSITIVE REFRACTIVE INDEX CHANGING COMPOSITION AND A REFRACTIVE INDEX CHANGING METHOD

Abstract A composition which can be changed in refractive index by a simple method to give a refractive-index pattern and an optical material in each of which the resultant difference in refractive index is significantly large and is stable regardless of conditions of use thereafter; and a method of forming the pattern or optical material. The composition comprises (A) a decomposable compound, (B) a hydrolyzate of an alkoxide such as tetrabutoxytitanium, tetramethoxyzirconium, tetramethoxygermanium, or tetramethoxysilane or of a halide such as tetrachlorosilane, and (C) a radiation-sensitive decomposer. The composition is sensitive to a radiation
Full Text DESCRIPTION
RADIATION SENSITIVE REFRACTIVE INDEX CHANGING COMPOSITION
AND USE THEREOF
Field of the Invention
The present invention relates to a radiation sensitive refractive index changing composition, a refractive index changing method, a refractive index pattern forming method, a refractive index pattern and an optical material. More specifically, it relates to a refractive index pattern forming method which provides a novel refractive index pattern and optical material for use in optoelectronic and display fields, a refractive index changing method and a radiation sensitive refractive index changing composition suitably used in these methods. Description of Prior Art
In the current society called 'multi-media society", refractive index distribution type optically molded products each consisting of different refractive index regions are in great demand. The products include not only optical fibers for transmitting information but also optical diffraction gratings having a periodical change in refractive index, optical memories in which information is written at sites having different refractive indices, optically coupled elements such as optical IC's having a fine refractive index pattern, optical control elements, optical modulation elements and optical transmission elements.
The refractive index distribution type optically molded products are divided into two types: one having a continuous refractive index distribution in a molded product, such as GI type optical fibers (to be referred to as "GRIN optically molded products" hereinafter) and the other having a discontinuous refractive index distribution, such as

optical diffraction gratings and SI type optical waveguides.
The GRIN optically molded products are attracting much attention as the next-generation optically molded products. For example, a GI type optical fiber whose refractive index is reduced from the center axis of the core of the optical fiber to the periphery in a parabolic form can transmit a great volume of information. A GRIN lens whose refractive index continuously changes therein is used as a reading lens for use in copiers, spherical lens for connecting fibers, or micro-lens, making use of its characteristic features that it has refractive power even on a flat surface and that it is free from spherical aberration.
A large number of methods of producing the above GRIN optically molded products have been proposed up till now. For example, JP-A 9-133813, JP-A 8-336911, JP-A 8-337609, JP-A 3-192310, JP-A 5-60931 (the term "JP-A" as used herein means an "unexamined published Japanese patent application") , WO93/19505 and WO94/04949 disclose a method of obtaining a GI type optical fiber by dispersing a low-molecular weight compound or a monomer into a polymer and continuously distributing its concentration. JP-A 62-25705 discloses that a rod-like GI type optically molded product or optical fiber is obtained by photo-copolymerizing two or more vinyl monomers having different refractive indices and reactivity ratios. Further, JP-A 7-56026 discloses a method of obtaining a refractive index distribution by forming a polymer A having a photo-reactive functional group, dispersing a compound B having a lower refractive index than the polymer A into the polymer A to form the concentration distribution of the compound B and photo-reacting the polymer A with the compound B.
Some methods of producing GRIN optically molded products of an inorganic material have also been proposed. One of them is, for example, a method of producing a GI type

rod by adding high refractive index thallium to rod-like glass essentially composed of silicon or lead, immersing the glass in a molten solution containing low refractive index potassium, and forming a potassium concentration ; distribution by ion exchange.
A GRIN lens can be obtained likewise by applying the above method to a short rod, that is, lens-like optically molded product. Alternatively, the GI type rod produced by the above method may be sliced.
As one of the methods of producing an optically molded product having a fine refractive index pattern, such as the above optical diffraction grating or optical IC, there is known a technology for obtaining a change in refractive index by causing a photochemical reaction in a molded product through exposure to light. For instance, in the case of an inorganic material, glass doped with germanium is exposed to light to change its refractive index so as to produce an optical diffraction grating. In the case of an organic material, the above technology is known as a photochromic reaction or photobleaching. JP-A 7-92313 discloses a technology for obtaining an optical diffraction grating by causing a change in refractive index through the exposure of a material containing a low-molecular weight compound having photochemical reactivity dispersed in a polymer to a laser beam. Further, JP-A 9-178901 has recently proposed the application of this technology to the production of a GRIN optically molded product. This method provides a continuous refractive index distribution in a depth direction with respect to irradiation, making use of the fact that light irradiated onto a molded product is absorbed and weakened in intensity.
However, in the refractive index distributions obtained with the above conventional materials, the maximum refractive index difference is only about 0.001 to 0.02 and

it is difficult to provide a wider refractive index distribution for preventing an optical loss and suppressing the malfunction of a circuit.
When the above conventional materials are used under the condition that light having a wavelength close to the wavelength used for changing the refractive index passes therethrough after a refractive index distribution is formed, it is impossible to prevent a phenomenon that a gradual change in refractive index occurs, thereby deteriorating the materials. Summary of the Invention
The present invention has been made in view of the above situation of the prior art.
That is, it is an object of the present invention to provide a refractive index pattern and an optical material whose refractive indices are changed by a simple method, which have a sufficiently large refractive index difference and which are stable irrespective of their use conditions, and a novel method of forming these.
Other objects and advantages of the present invention will become apparent from the following description.
According to the present invention, firstly, the above objects and advantages of the present invention are attained by a composition comprising:
(A) a decomposable compound,
(B) a hydrolyzate of at least one compound selected from
j» —
the group consisting of an alkoxide represented by the
following formula (1'):
M(OR)mYn (1')
wherein M is a positive divalent to pentavalent atom, R is an alkyl group or aryl group, Y is a hydrogen atom, alkyl group, aryl group, hydroxyl group, alkoxyl group or aryloxy group, and m and n are each independently an integer of 0 or more, with the proviso that (m + n) is equal to the valence

of M,
and a halogen compound represented by the following formula
(2'):
MXmYn (2')
wherein M, Y, m and n are as defined in the formula (!'), and X is a halogen atom, and (C) a radiation sensitive decomposer.
Secondly, the above objects and advantages of the present invention are attained by a refractive index changing method comprising the step of exposing the radiation sensitive refractive index changing composition of the present invention to radiation.
Thirdly, the above objects and advantages of the present invention are attained by a refractive index pattern forming method comprising the step of exposing part of the above radiation sensitive refractive index changing composition to radiation.
In the fourth place, the above objects and advantages of the present invention are attained by a refractive index pattern formed by the above refractive index pattern forming method.
In the fifth place, the above objects and advantages of the present invention are attained by an optical material formed by the above refractive index pattern forming method. Detailed Description of the Preferred Embodiments
In the present invention, the term "refractive index pattern" means a refractive index distribution type material consisting of regions having different refractive indices.
A detailed description is subsequently given of each component of a refractive index changing composition used in the present invention. (A) decomposable compound
The decomposable compound (A) used in the present invention can be an acid decomposable compound or a base

decomposable compound. The weight average molecular weight of the decomposable compound (A) is preferably 100 to 500 , 000 , more preferably 100 to 300,000.
The acid decomposable compound is selected from compounds having at least one of structures represented by the following formulas (1) to (6) and (7). These compounds may be used alone or in combination of two or more.

(In the formula (1), R1 is an alkylene group, perfluoroalkylene group, alkylsilylene group, alkylene-arylene-alkylene group or arylene group, and R^ is an alkylene group, perfluoroalkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group or alkylgermylene group, with the proviso that the above alkylene group or perfluoroalkylene group may contain a -O-, -CO-, -COO- or -OCOO- bond.)

(In the formula (2), M is Si or Ge, R3 is an alkylene group, perfluoroalkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group, alkylgermylene group or single bond, R4 is an oxygen atom, alkylene group, perfluoroalkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group or single bond, R5, R6, R7 and R8 are each independently a hydrogen atom, alkyl group, aryl group, alkoxyl group, thioalkyl group, alkoxyester group, perfluoroalkyl group, perfluoroalkoxyl group, perf luoroalkoxyester group or perfluoroaryl group, and m is an integer of 0 to 2, with the proviso that the above alkylene group or perfluoroalkylene group may contain a -0-, -CO-, -COO- or -OCOO- bond.)


(In the formula (3), R9 and R10 are each independently an alkylene group, perfluoroalkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group or alkylgermylene group, with the proviso that the above alkylene group or perfluoroalkylene group may contain a -0-, -CO-, -COO- or -OCOO- bond.)

(In the formula (4), R11 is an oxyalkylene group or single bond, and R12 is a hydrogen atom, alkyl group, alkoxyl group, alkoxyester group, perfluoroalkyl group, perfluoroalkoxyester group, perfluoroaryl group, alkylene-arylene-alkylene group or aryl group.)

(In the formula (5), R13 is a hydrogen atom, alkyl group, alkoxyl group, alkoxyester group, perfluoroalkyl group, perfluoroalkoxyl group, perfluoroalkoxyester group, perfluoroaryl group or aryl group.)

(In the formula (6) , R14 is an alkylene group or a structure represented by the following formula (6)-l, (6)-2or(6)-3.)


independently a hydrogen atom, chain alkyl group having 1 to 6 carbon atoms, chlorine atom, bromine atom, iodine atom, hydroxyl group, mercapto group, carboxyl group, alkoxyl group having 1 to 6 carbon atoms, alkylthio group having 1 to 6 carbon atoms, haloalkyl group having 1 to 6 carbon atoms, haloalkoxyl group having 1 to 6 carbon atoms, haloalkylthio group having 1 to 6 carbon atoms, hydroxyalkyl group having 1 to 6 carbon atoms, mercaptoalkyl group having 1 to 6 carbon atoms, hydroxyalkoxyl group having 1 to 6 carbon atoms, mercaptoalkylthio group having 1 to 6 carbon atoms, aryl group having 6 to 10 carbon atoms or aralkyl group having 7 to 11 carbon atoms.)



atom, chain alkyl group having 1 to 6 carbon atoms or aryl group having 6 to 10 carbon atoms, and R38, R39, R40 and R41 are each independently a hydrogen atom, chlorine atom, bromine atom, hydroxyl group, mercapto group, alkoxyl group.

thioalkyl group, alkylester group, alkylthioester group, aryl group, cyano group or nitro group.


atom, chain alkyl group having 1 to 6 carbon atoms or aryl group having 6 to 10 carbon atoms, A3 is -0-, alkylene group or arylene group, and a is an integer of 0 or 1.
All the above alkylgermylene groups each independently have a structure represented by the following formula (16):
wherein R68, R39, R70 and R71 are each independently a hydrogen atom, chain alkyl group having 1 to 6 carbon atoms or aryl group having 6 to 10 carbon atoms, A4 is -0-, alkylene group or arylene group, and b is an integer of 0 or 1.
All the above alkylene groups can be a linear, branched or cyclic alkylene group having 1 to 10 carbon atoms, and some of the hydrogen atoms contained in the above groups may be substituted by a fluorine atom, or some or all of the hydrogen atoms contained in the above groups may be substituted by a chlorine atom, bromine atom, perf luoroalkyl group, hydroxyl group, mercapto group, thioalkyl group, alkoxyl group, perfluoroalkoxyl group, alkylester group, alkylthioester group, perfluoroalkylester group, cyano group or nitro group.
All the above alkyl groups and alkyl groups contained in the above alkoxyl groups, thioalkyl groups, alkylester groups and alkylthioester groups can be a linear, branched or cyclic alkyl group having 1 to 10 carbon atoms, and some of the hydrogen atoms contained in the above groups may be substituted by a fluorine atom, or some or all of the hydrogen atoms contained in the above groups may be substituted by a chlorine atom, bromine atom, perfluoroalkyl group, hydroxyl group, mercapto group, thioalkyl group, alkoxyl group, perfluoroalkoxyl group, alkylester group, alkylthioester group, perfluoroalkylester group, cyano group, nitro group or aryl group.

All the above perfluoroaryl groups are each independently a perfluorophenyl group, perfluoronaphthyl group, perfluoroanthracenyl group or perfluorobiphenyl group, and a fluorine atom contained in these groups may be substituted by a hydroxyl group, perfluoroalkoxyl group, perfluoroalkyl group, perfluoroalkylester group, cyano group or nitro group.
All the above aryl groups are each independently a phenyl group, naphthyl group, anthracenyl group or biphenyl group, and a hydrogen atom contained in the above groups may be substituted by a chlorine atom, bromine atom, hydroxyl group, mercapto group, alkoxyl group, thioalkyl group, alkylester group, alkylthioester group, cyano group or nitro group.
Methods of producing acid decomposable compounds having structures represented by the above formulas (1) to (7) as a recurring unit, for example, in the present invention are already known.
Methods of producing a compound having a structure represented by the above formula (1) are disclosed by Polymer Bull. , 1. 199 (1978), JP-A 62-136638, EP 225,454, US 806,5 97, JP-A 4-303843, JP-A 7-56354 and the like.
Methods of producing a compound having a structure represented by the above formula (2) are disclosed by Macromolecules 29, 5529 (1996), Polymer 17, 1086 (1976), JP-A 60-37549 and the like.
Methods of producing a compound having a structure represented by the above formula (3) are disclosed by Electrochem. Soc, Solid State Sci. Technol., 133(1) 181 (1986), J. Imaging Sci., 30(2)59 (1986), Macromol. Chem., Rapid Commun., 7, 121(1986) and the like.
Methods of producing a compound having a structure represented by the above formula (4) are disclosed by USP 3,894,253, JP-A 62-190211, JP-A 2-146544, Macromol. Chem.,

23, 16 (1957), JP-A 63-97945, Polymer Sci., A-1, 8, 2375 (1970) , USP 4,247,611, EP 41,657, JP-A 57-31674, JP-A 64-36 47, JP-A 56-17345 and the like.
Methods of producing a compound having a structure represented by the above formula (5) are disclosed by Prepr. Eur, Disc Meet. Polymer Sci., Strasbourg, p.106 (1978), Macromol. Chem., 179, 1689 (1978) and the like.
Methods of producing a compound having a structure represented by the above formula (6) are disclosed by USP 3,894,253, USP 3,940,507, JP-A 62-190211 and the like.
Methods of producing a compound having a structure represented by the above formula (7) are disclosed by J. Am. Chem. Soc, 54, 1579 (1932), J. Polym. Sci., 29, 343 (1958), J. Polym. Sci., Part A, Polym. Chem., 25, 3373 (1958), Macromolecules, 25, 12, (1992), Macromolecules, 20, 705, (1997), Macromolecules, 21, 1925, (1998), Macromol. Chem,, Rapid Commun., 11, 83 (1990) and the like.
The weight average molecular weight of the decomposable compound (A) is preferably 100 to 500,000, more preferably 100 to 300,000.
Methods of producing base decomposable compounds having structures represented by the above formulas (8) to (11) as a recurring unit are also known.
Methods of producing a compound having a structure represented by the above formula (8) are disclosed by Macromol. Chem., Rapid Commun., 5, 151 (1984), Macromol. Chem., 189, 2229 (1988), Macromol. Chem., 187, 2525 (1986), Polym, J., 22, 803 (1990) and the like.
Methods of producing a compound having a structure represented by the above formula (9) are disclosed by J. Polym. Sci., 47, 1523 (1993), J. Appl. Polym. Sci., 35, 85 (1985), J. Polym. Sci., Polym. Chem. Ed., 22, 1579 (1984), J. Polym. Sci., Polym. Chem. Ed., 14, 655 (1976), J. Polym. Sci., Polym. Chem. Ed,, 17, 2429 (1979) and the like.

Methods of producing a compound having a structure represented by the above formula (10) are disclosed by J. Macromol, Sci. -Chem., A9, 1265 (1975) and the like.
Methods of producing a compound having a structure represented by the above formula (11) are disclosed by Polym, Bull., 14, 85 (1985), Macromol. Chem., 189, 1323 (1988) and the like.
The weight average molecular weight of the decomposable compound (A) is preferably 100 to 500,000, more preferably 100 to 300,000.
When the above decomposable compounds (A) are classified according to refractive index for the convenience' sake, a compound having at least one of the following structures (i) to (vii) is preferred as a compound having a refractive index of 1.5 or less, (i) The structure of the formula (1) in which R^ and R^ are each independently an alkylene group, perfluoroalkylene group or alkylsilylene group, with the proviso that the above alkylene group or perfluoroalkylene group may contain a -0-, -CO-, -COO- or -OCOO- bond.
(ii) The structure of the formula (2) in which M is Si or Ge, R3 is an alkylene group or perfluoroalkylene group, R4 is an alkylene group, perfluoroalkylene group, alkylsilylene group or single bond, R5, R6, R7 and R8 are each independently a hydrogen atom, alkyl group, alkoxyl group, alkoxyester
group, perfluoroalkyl group, perfluoroalkoxyl group,
^ —-
perf luoroalkoxyester group or perfluoroaryl group, and m is an integer of 0 to 2, with the proviso that the above alkylene group or perfluoroalkylene group may contain a -0-, -CO-, -COO- or -OCOO- bond.
(iii) The structure of the formula (3) in which R9 and R10 are each independently an alkylene group or perfluoroalkylene group, with the proviso that the above alkylene group or perfluoroalkylene group may contain a -0-, -CO-, -COO- or

-OCOO- bond.
(iv) The structure of the formula (4) in which R11 is an oxyalkylene group or single bond, and R12 is a hydrogen atom, alkyl group, alkoxyl group, alkoxyester group, perfluoroalkyl group, perfluoroalkoxyester group or perfluoroaryl group.
(v) The structure of the formula (5) in which R13 is a hydrogen atom, alkyl group, alkoxyl group, alkoxyester group, perfluoroalkyl group, perfluoroalkoxyl group, perfluoroalkoxyester group or perfluoroaryl group, (vi) The structure represented by the formula (6). (vii) The structure of the formula (7) in which R21 is an alkylene group.
A compound having at least one of the following structures (viii) to (xiv) is preferred as a compound having a refractive index of more than 1.5.
(viii) The structure of the formula (1) in which R1 is an alkylene group, alkylene-arylene-alkylene group or arylene group, and R2 is an alkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group or alkylgermylene group.
(ix) The structure of the formula (2) in which M is Si or Ge, R3 is an alkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group or alkylgermylene group, R* is an oxygen atom, alkylene group,
alkylene-arylene-alkylene group, arylene group or single bond, R5, R6, R7 and R8 are each independently a hydrogen atom, alkyl group, aryl group, alkoxyl group or thioalkyl group, and m is an integer of 0 to 2.
(x) The structure of the formula (3) in which R9 and R10 are each independently an alkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group or alkylgermylene group. (xi) The structure of the formula (4) in which R11 is an

oxyalkylene group or single bond, and R12 is a hydrogen atom, alkyl group, alkylene-arylene-alkylene group or aryl group, (xii) The structure of the formula (5) in which R13 is a hydrogen atom, alkyl group or aryl group, (xiii) The structure represented by the formula (7) (xiv) The structures represented by the formulas (8) to (11). (B) hydrolyzate
The component (B) used in the present invention is a hydrolyzate of at least one compound selected from the group consisting of a metal alkoxide represented by the following formula (1') and a metal halide represented by the following formula (2'):
M{OR)mmYn (1')
MXmYn (2')
wherein M is a positive divalent to pentavalent atom, R is an alkyl group or aryl group, Y is a hydrogen atom, alkyl group, aryl group, hydroxyl group, alkoxyl group or aryloxy group, X is a halogen atom, and m and n are each independently an integer of 0 or more, with the proviso that (m + n) is equal to the valence of M.
It should be understood that the above hydrolyzate includes what is obtained by hydrolyzing all the hydrolyzable portions contained in a raw material and also what is obtained by hydrolyzing some and not all of the hydrolyzable portions.
The positive divalent to pentavalent atom M in the above formulas (1') and (2') is, for example, B, Si, P or metal atom. The metal atom is preferably a group 2A or 3B metal atom of the periodic table or a transition metal atom.
All the above alkyl groups and alkyl group contained in the above alkoxyl group may be a linear, branched or cyclic alkyl group having 1 to 10 carbon atoms, and some of the hydrogen atoms contained in the above groups may be substituted by a fluorine atom, or some or all of the hydrogen atoms contained in the above groups may be substituted by

a chlorine atom, bromine atom, perfluoroalkyl group, hydroxyl group, mercapto group, thioalkyl group, alkoxyl group, perfluoroalkoxyl group, alkylester group, alkylthioester group, perfluoroalkylester group, cyano group, nitro group or aryl group.
All the above aryl groups and aryl group contained in the above aryloxy group are each independently a phenyl group, naphthyl group, anthracenyl group or biphenyl group, and a hydrogen atom contained in the above groups may be substituted by a chlorine atom, bromine atom, hydroxyl group, mercapto group, alkoxyl group, thioalkyl group, alkylester group, alkylthioester group, cyano group or nitro group.
The halogen atom is preferably fluorine, chlorine or bromine.
Excimples of the silicon compound as the compound represented by the above formula (1') include tetraalkoxysilanes such as tetreimethoxysilane, tetraethoxysilane (generally called TEOS), tetra-n-propyloxysilane, tetraisopropyloxysilane and tetra-n-butoxysilane; monoalkyltrialkoxysilanes such as methyltrimethoxysilane, methyltriethoxysilane, methyltri-n-propyloxysilane, ethyltriethoxysilane and cyclohexyltriethoxysilane; monoaryltrialkoxysilanes such as phenyltriethoxysilane, naphthyltriethoxysilane, 4-chlorophenyltriethoxysilane, 4-cyanophenyltriethoxysilane, 4-aminophenyltriethoxysilane, 4-nitrophenyltriethoxysilane, 4-methylphenyltriethoxysilane and 4-hydroxyphenyltriethoxysilane;
monoaryloxytrialkoxysilanes such as phenoxytriethoxysilane, naphthyloxytriethoxysilane, 4-chlorophenyloxytriethoxysilane, 4-cyanophenyltrioxyethoxysilane,

4-aminophenyloxytriethoxysilane,
4-nitrophenyloxytriethoxysilane,
4-methylphenyloxytriethoxysilane and
4-hydroxyphenyloxytriethoxysilane;
monohydroxytrialkoxysilanes such as
monohydroxytrimethoxysilane, monohydroxytriethoxysilane
and monohydroxytri-n-propyloxysilane;
dialkyldialkoxysilanes such as dimethyldimethoxysilane,
dimethyldiethoxysilane, dimethyldi-n-propyloxysilane,
methyl(ethyl)diethoxysilane and
methyl(cyclohexyl)diethoxysilane;
monoalkylmonoaryldialkoxysilanes such as
methyl{phenyl)diethoxysilane; diaryldialkoxysilanes such
as diphenyldiethoxysilane; diaryloxydialkoxysilanes such as
diphenoxydiethoxysilane;
monoalkylraonoaryloxydialkoxysilanes such as
methyl(phenoxy)diethoxysilane;
monoarylmonoaryloxydialkoxysilanes such as
phenyl(phenoxy)diethoxysilane; dihydroxydialkoxysilanes
such as dihydroxydimethoxysilane, dihydroxydiethoxysilane
and dihydroxydi-n-propyloxysilane:
monoalkylmonohydroxydialkoxysilanes such as
methyl(hydroxy)dimethoxysilane;
monoarylmonohydoxydialkoxysilanes such as
phenyl(hydroxy)dimethoxysilane; trialkylmonoalkoxysilanes
such as trimethylmethoxysilane, trimethylethoxysilane,
trimethyl-n-propyloxysilane, dimethyl{ethyl)ethoxysilane
and dimethyl(cyclohexyl)ethoxysilane;
dialkylmonoarylmonoalkoxysilanes such as
dimethyl(phenyl)ethoxysilane;
monoalkyldiarylmonoalkoxysilanes such as
methyl(diphenyl)ethoxysilane; triaryloxymonoalkoxysilanes
such as triphenoxyethoxysilane;
monoalkyldiaryloxymonoalkoxysilanes such as

methyl(diphenoxy)ethoxysilane;
monoaryldiaryloxymonoalkoxysilanes such as
phenyl(diphenoxy)ethoxysilane;
dialkylmonoaryloxymonoalkoxysilanes such as
dimethyl(phenoxy)ethoxysilane;
diaryImonoaryloxymonoalkoxysilanes such as
diphenyl(phenoxy)ethoxysilane;
monoalkylmonoaryImonoaryloxymonoalkoxysilanes such as
methyl(phenyl)(phenoxy)ethoxysilane;
trihydroxymonoalkoxysilanes such as
trihydroxymethoxysilane, trihydroxyethoxysilane and
trihydroxy-n-propyloxysilane; and oligomers of the above
compounds such as dimmers to pentamers of
tetramethoxysilane.
Examples of the silicon compound as the compound represented by the above formula (2') include tetrahalogenosilanes such as tetrachlorosilane, tetrabromosilane, tetraiodosilane, trichlorobromosilane and dichlorodibromosilane; monoalkyltrihalogenosilanes such as methyltrichlorosilane, methyldichlorobromosilane, cyclohexyltrichlorosilane; monoaryltrihalogenosilanes such as phenyltrichlorosilane, naphthyltrichlorosilane, 4-chlorophenyltrichlorosilane and
phenyldichlorobromosilane; monoaryloxytrihalogenosilanes such as phenoxytrichlorosilane and
phenoxydichlorobromosilane; monoalkoxytrihalogenosilanes such as methoxytrichlorosilane and ethoxytrichlorosilane; dialkyldihalogenosilanes such as dimethyldichlorosilane, methyl(ethyl)dichlorosilane and methyl(cyclohexyl)dichlorosilane; monoalkylmonoaryldihalogenosilanes such as methyl(phenyl)dichlorosilane; diaryldihalogenosilanes such as diphenyldichlorosilane; diaryloxydihalogenosilanes such as diphenoxydichlorosilane;

monoalkylmonoaryloxydihalogenosilanes such as methyl(phenoxy)dichlorosilane; monoarylmonoaryloxydihalogenosilanes such as phenyl(phenoxy)dichlorosilane; dialkoxydihalogenosilanes such as diethoxydichlorosilane; monoalkylmonoalkoxydichlorosilanes such as methyl(ethoxy)dichlorosilane; monoarylmonoethoxydichlorosilanes such as phenyl(ethoxy)dichlorosilane; trialkylmonohalogenosilanes such as trimethylchlorosilane, dimethyl(ethyl)chlorosilane and dimethyl(cyclohexyl)chlorosilane; dialkylmonoarylmonohalogenosilanes such as dimethyl(phenyl)chloros ilane; monoalkyldiarylmonohalogenosilanes such as methyl(diphenyl)chlorosilane; triaryloxymonohalogenosilanes such as triphenoxychlorosilane;
monoalkyldiaryloxymonohalogenosilanes such as methyl(diphenoxy)chlorosilane; monoaryldiaryloxymonohalogenosilanes such as phenyl(diphenoxy)chlorosilane; dialkylmonoaryloxymonohalogenosilanes such as dimethyl(phenoxy)chlorosilane; diarylmonoaryloxymonohalogenosilanes such as diphenyl(phenoxy)chlorosilane;
monoalkylmonoarylmonoaryloxymonohalogenosilanes such as methyl(phenyl)(phenoxy)chlorosilane; triethoxymonohalogenosilanes such as
triethoxychlorosilane; and oligomers of the above compounds such as dimmers to pentamers of tetrachlorosilane.
Other examples of the compounds represented by the above formula (1') and (2') include alkoxides and halides such as diethoxyberyIlium, dichloroberyllium, triethoxyboron, trichloroboron, diethoxymagnesium,

dichloromagnes ium, triethoxyaluminum, trichloroaluminum, triethoxyphosphorus, trichlorophosphorus, pentaethoxyphosphorus, pentachlorophosphorus, diethoxycalcium, dichlorocalcium, triethoxyscandium, trichloroscandium, tetraethoxytItanium, tetrabutoxytitanium, tetrachlorotitanium, diethoxymanganese, dichloromanganese, diethoxyiron, dichloroiron, triethoxyiron, trichloroiron, diethoxycobalt, dichlorocobalt, diethoxynickel, dichloronickel, diethoxyzinc, dichlorozinc, triethoxygallium, trichlorogallium tetramethoxygermanium, tetraethoxygermanium, tetrachlorogermanium, diethoxystrontium, dichlorostrontium triethoxyyttrium, trichloroyttrium, tetramethoxyzirconium, tetraethoxyzirconium, tetrachlorozirconium, diethoxycadmium, dichlorocadmium, triethoxyindium, trichloroindium, tetraethoxytellurium, tetrachlorotellurium, diethoxybarium, dichlorobarium, triethoxylanthanum, trichlorolanthanum, triethoxyneodymium, trichloroneodymium, triethoxyytterbium, trichloroytterbium, hexaethoxytungsten, hexachlorotungsten, pentaethoxytantalum, pentachlorotantalum, diethoxylead, dichlorolead, triethoxybismuth, trichlorobismuth, tetraethoxythorium and tetrachlorothorium.
Out of these, tetraalkoxysilanes such as tetramethoxysilane and tetraethoxysilane; trialkoxyaluminums such as triethoxyaluminum; tetraalkoxytitaniums such as tetraethoxytitaniun; tetrahalogenosilanes such as tetrachlorosilane; trihalogenoaluminums such as trichloroaluminum; and tetrahalogenotitaniums such as tetrachlorotitanium are preferred. More preferred are tetraalkoxysilanes such as tetramethoxysilane and tetraethoxysilane; trialkoxyaluminums such as triethoxyaluminum; and

tetrahalogenosilanes such as tetrachlorosilane and the most preferred are tetraalkoxysilanes such as tetraethoxysilane. Any number of compounds out of the above compounds may be used in combination in any ratio.
The component (B) used in the present invention can be produced by subjecting the above compound to a hydrolytic reaction. The hydrolytic reaction is preferably carried out in a suitable solvent. Examples of the solvent include water-soluble solvents such as methanol, ethanol, n-propanol, isopropyl alcohol, n-butanol, isobutyl alcohol, t-butyl alcohol, acetone, tetrahydrofuran, dioxane and acetonitrile and aqueous solutions thereof.
Since these water-soluble solvents may be removed in the subsequent step, methanol, ethanol, n-propanol, isopropyl alcohol, acetone and tetrahydrofuran having a relatively low boiling point are preferred, and alcohols such as methanol, ethanol, n-propanol and isopropyl alcohol are more preferred from the view point of solubility for the raw material. The most preferred is ethanol.
The hydrolytic reaction for synthesizing the component
(B) is preferably carried out in the presence of an acid
catalyst (for example, hydrochloric acid, sulfuric acid,
nitric acid, formic acid, acetic acid, trifluoroacetic acid,
trif luoromethanesulfonic acid, acidic ion exchange resin or
Lewis acid) or basic catalyst (for example, ammonia, primary
amine, secondary amine, tertiary amine, nitrogen-containing
I"
aromatic compound such as pyridine, basic ion exchange resin,
hydroxide such as sodium hydroxide, carbonate such as
potassium carbonate, carboxylate such as sodium acetate or
Lewis base). The content of water, reaction temperature and
reaction time are suitably determined. For example, the
following conditions may be adopted.
Content of water; 2 mols or less, preferably 1.5 mols
or less, more preferably 1 mol or less based on 1 mol of the

total of alkoxyl groups and halogen atoms contained in the compound represented by the above formula (1') or (2')
Reaction temperature; preferably 40 to 200°C, more preferably 50 to 150°C
Reaction time; preferably 30 minutes to 24 hours, more preferably 1 to 12 hours
In the present invention, inorganic oxide particles can be used together with the above hydrolyzate. The inorganic oxide particles are preferably stable to an acid or base formed from the radiation sensitive decomposer (C) to be described hereinafter, do not absorb light having a wavelength range used when it passes therethrough and has optically high transparency. Oxide particles having a preferred refractive index value are selected according to application purpose.
Preferred examples of the oxide particles include oxides containing an atom such as Be, Mg, Ca, Sr, Ba, Sc, Y, La, Ce, Gd, Tb, Dy, Yb, Lu, Ti, Zr, Hf, Nb, Mo, W, Zn, B, Al, Si, Ge, Sn, Pb, Bi or Te. More preferred examples of the oxide particles include oxides such as BeO, MgO, CaO, SrO, BaO, SC2O3, Y2O3, La203, Ce203, Gd203, Tb203, Dy203, Yb203, LU2O3, Ti02, Zr02, Hf02, Nb205, M0O3, WO3, ZnO, B2O3, AI2O3, Si02, Ge02, SnOa, PbO, Bi203 and Te02, and composite oxides containing these, such as Al203-MgO, Al203-Si02, ZnO-Y203, Zr02-Ce203, Zr02-Ti02-Sn02, Te02-BaO-ZnO, Te02-W03-Ta205, Te02-W03-Bi203, Te02-Ba07PbG, CaO-Al203, CaO-Al203.BaO, CaO-Al203-Na20, CaO-Al203-K20 CaO-Al203-Si02, PbO-Bi203-BaO, PbO-Bi203-ZnO, PbO-Bi203, PbO-Bi203"BaO-ZnO, PbO-Bi203-CdO-Al203,PbO-Bi203-Ge02, PbO-BizOs-GeOz-TlzO, BaO-PbO-Bi203, BaO-PbO-Bi203-ZnO, Bi203-Ga203-PbO, Bi203-Ga203-CdO and Bi203-Ga203-(Pb, Cd)0.
The particle diameters of the oxide particles are preferably smaller than the wavelength of light used by the refractive index changing composition of the present

invention and can be, for example, 2 µm or less, preferably 0.2 pm or less, particularly preferably 0 .1 µm or less • When the particle diameters are larger than 2 µm, the transparency of the obtained refractive index changing composition may lower or a film obtained therefrom may have a problem with its surface state.
The shapes of the oxide particles are not particularly limited but preferably substantially spherical because the scattering of input light is rare.
The above oxide particles may be contacted to a silane coupling agent, surfactant or coordinating compound having coordination capability to a metal atom constituting the oxide to modify their surfaces before use.
The inorganic oxide particles are used in an amount of preferably 500 parts or less by weight, more preferably 300 parts or less by weight based on 100 parts by weight of the hydrolyzate.
Particularly preferably, the refractive index ns of the component (B) and the refractive index nA of the component (A) have one of the following relationships (1) and (2).
ns - nA > 0.05 (1)
nA - HB > 0.05 (2)
The amount of the component (B) is preferably 10 to 90 parts by weight, more preferably 20 to 70 parts by weight based on 100 parts by weight of the total of the components (A) and (B) . When the amount of the component (B) is smaller than 10 parts by weight, the refractive index changing composition may become brittle and when the amount is larger than 90 parts by weight, the obtained refractive index difference may become small. (C) radiation sensitive decomposer
The radiation sensitive decomposer (C) used in the present invention can be a radiation sensitive acid generator or a radiation sensitive base generator.

The above radiation sensitive acid generator is, for example, a trichloromethyl-s-triazine, diaryl iodonium salt, triaryl sulfonium salt, quaternary ammonium salt or sulfonic acid ester.
Examples of the above trichloromethyl-s-triazine include 2,4,6-tris(trichloromethyl)-s-triazine, 2-phenyl-4,6-bis(trichloromethyl)-s-triazine, 2-{4-chlorophenyl)-4,6-bis(trichloromethyl)-s-triazine, 2 -(3 -chlorophenyl)-4,6-bis(trichloromethyl)-s-triaz ine, 2-(2-chlorophenyl)-4,6-bis(trichloromethyl)-s-triaz ine, 2-(4-methoxyphenyl)-4,6-bis(trichloromethyl)-s-triazine, 2 -(3-methoxyphenyl)-4,6-bis(trichloromethyl)-s-triazine, 2 -(2-methoxyphenyl)-4,6-bis(trichloromethyl)-s-triazine, 2 -{4-methylthiophenyl)-4,6-bis(trichloromethyl)-s-triazine,
2 -{3-methylthiophenyl)-4,6-bis(trichloromethyl)-s-triazine,
2-(2-methylthiophenyl)-4,6-bis{trichloromethyl)-s-triazine,
2-(4-methoxynaphthyl)-4,6-bis(trichloromethyl)-s-triazine,
2-(3-methoxynaphthyl)-4,6-bis(trichloromethyl)-s-triazine,
2-(2-methoxynaphthyl)-4,6-bis(trichloromethyl)-s-triazine,
2 -(4-methoxy-p-styryl)-4,6-bis(trichloromethyl)-s-triazine,
2-(3-methoxy-p-styryl)- 4,6-bis(trichloromethyl)-s-triazine,
2 -(2-methoxy-p-styryl)-4,6-bis(trichloromethyl)-s-triazine,
2 -(3,4,5-trimethoxy-p-styryl)-4,6-bis(trichloromethyl) -s-triazine,
2 -(4-methylthio-p-styryl)- 4,6-bis(trichloromethyl)-s-

triazine,
2- (3-methylthio-|3-styryl) -4, 6-bis(trichloromethyl) -s-triazine,
2 -{3-methylthio-p-styryl)-4,6-bis(trichloromethyl)-s-
triazine, 2-piperonyl-4,6-bis(trichloromethyl)-s-triazine,
2-[2-(furan-2-yl)ethenyl]-4,6-bis(trichloromethyl)-s-
triazine, 2-[2-(5-methylfuran-2-yl)ethenyl]-4,6-bis
(trichloromethyl)-s-triazine and
2-[2-(4-diethylamino-2-methylphenyl)ethenyl]-4,6 -
bis(trichloromethyl)-s-triazine.
Examples of the above diaryl iodonium salt include diphenyliodonium tetrafluoroborate, diphenyliodonium hexafluorophosphonate, diphenyliodonium hexafluoroarsenate, diphenyliodonium trifluoromethane sulfonate, diphenyliodonium trifluoroacetate,
diphenyliodonium-p-toluene sulfonate, diphenyliodonium butyltris(2,6-difluorophenyl)borate, diphenyliodonium hexyltris(p-chlorophenyl)borate, diphenyliodonium hexyltris(3-trifluoromethylphenyl)borate, 4 -methoxyphenylphenyliodoniiom tetraf luoroborate, 4-methoxyphenylphenyliodonium hexafluorophosphonate, 4-methoxyphenylphenyliodonium hexafluoroarsenate, 4-methoxyphenylphenyliodonium trifluoromethane sulfonate, 4-methoxyphenylphenyliodonium trifluoroacetate, 4-methoxyphenylphenyliodonium-p-toluene sulfonate, 4-methoxyphenylphenyliodonium butyltris(2,6-difluorophenyl)borate, 4-methoxyphenylphenyliodonium hexyltris(p-chlorophenyl)borate, 4-methoxyphenylphenyliodonium hexyltris(3-trifluoromethylphenyl)borate, bis(4-tert-butylphenyl)iodonium tetrafluoroborate, bis(4 -tert-butylphenyl)iodonium hexafluoroarsenate, bis (4 - tert -butylphenyl) iodonium trifluoromethane sulfonate,

triazine,
2-(3-methylthio-p-styryl)-4,6-bis(trichloromethyl)-s-triazine,
2-(3-methylthio-p-styryl)-4,6-bis(trichloromethyl)-s-
triazine, 2-piperonyl-4,6-bis{trichloromethyl)-s-triazine,
2-[2-(furan-2-yl)ethenyl]-4,6-bis(trichloromethyl)-s-
triazine, 2-[2-(5-methylfuran-2-yl)ethenyl]-4,6-bis
(trichloromethyl)-s-triazine and
2-[2-(4-diethylamino-2-methylphenyl)ethenyl]-4,6-
bis(trichloromethyl)-s-triazine•
Examples of the above diaryl iodonium salt include diphenyliodonium tetrafluoroborate, diphenyliodonium hexafluorophosphonate, diphenyliodonium hexafluoroarsenate, diphenyliodonium trifluoromethane sulfonate, diphenyliodonium trifluoroacetate,
diphenyliodonium-p-toluene sulfonate, diphenyliodonium butyltris(2,6-difluorophenyl)borate, diphenyliodonium hexyltris(p-chlorophenyl)borate, diphenyliodonium hexyltris(3-trifluoromethylphenyl)borate, 4-methoxyphenylphenyliodonium tetrafluoroborate, 4-methoxyphenylphenyliodonium hexafluorophosphonate, 4-methoxyphenylphenyliodonium hexafluoroarsenate, 4-methoxyphenylphenyliodonium trifluoromethane sulfonate, 4-methoxyphenylphenyliodonium trifluoroacetate, 4-methoxyphenylphenyliodonium-p-toluene sulfonate, 4-methoxyphenylphenyliodonium butyltris(2,6-difluorophenyl)borate, 4-methoxyphenylphenyliodonium hexyltris(p-chlorophenyl)borate, 4-methoxyphenylphenyliodonium hexyltris(3-trifluoromethylphenyl)borate, bis(4-tert-butylphenyl)iodonium tetrafluoroborate, bis(4-tert-butylphenyl)iodonium hexafluoroarsenate, bis ( 4 - tert -butylphenyl) iodonium trif luoromethane sulfonate,

bis(4 -tert-butylphenyl)iodonium trifluoroacetate, bis(4-tert-butylphenyl)iodonium-p-toluene sulfonate, bis(4-tert-butylphenyl)iodonium butyltris(2,6-difluorophenyl)borate, bis{4-tert-butylphenyl)iodonium hexyltris(p-chlorophenyl)borate and bis(4-tert-butylphenyl)iodonium hexyltris{3 -trifluoromethylphenyl)borate.
Examples of the above triaryl sulfonium salt include triphenylsulfonium tetrafluoroborate, triphenylsulfonium hexafluorophosphonate, triphenylsulfonium hexafluoroarsenate. triphenylsulfonium trifluoromethane sulfonate, triphenylsulfonium trifluoroacetate, triphenylsulf onium-p-toluene sulfonate, triphenylsulf onium butyltris(2,6-difluorophenyl)borate, triphenylsulfonium hexyltris(p-chlorophenyl)borate, triphenylsulfonium hexyltris{3-trifluoromethylphenyl)borate, 4-methoxyphenyldiphenylsulfonium tetrafluoroborate, 4-methoxyphenyldiphenylsulfonium hexafluorophosphonate, 4-methoxyphenyldiphenylsulfonium hexafluoroarsenate, 4-methoxyphenyldiphenylsulfonium trifluoromethane sulfonate, 4-methoxyphenyldiphenylsulfonium trifluoroacetate,
4-methoxyphenyldiphenylsulfonium-p-toluene sulfonate, 4-methoxyphenyldiphenylsulfonium butyltris(2,6-difluorophenyl)borate, 4-methoxyphenyldiphenylsulfonium hexyltris{p-chlorophenyl)borate, 4-methoxyphenyldiphenylsulfonium hexyltris(3-trifluoromethylphenyl)borate, 4-phenylthiophenyldiphenylsulfonium tetrafluoroborate, 4-phenylthiophenyldiphenylsulfonium hexafluorophosphonate, 4-phenylthiophenyldiphenylsulfonium hexafluoroarsenate, 4-phenylthiophenyldiphenylsulfonium trifluoromethane

sulfonate, 4-phenylthiophenyldiphenylsulfonium
trifluoroacetate,
4-phenylthiophenyldiphenylsulfonium-p-toluene sulfonate,
4-phenylthiophenyldiphenylsulfonium
butyltris(2,6-difluorophenyl)borate,
4-phenylthiophenyldiphenylsulfonium
hexyltris(p-chlorophenyl)borate,
4-phenylthiophenyldiphenylsulfonium
hexyltris(3-trifluoromethylphenyl)borate,
4-hydroxy-1-naphthalenyldimethylsulfonium
tetrafluoroborate,
4-hydroxy-1-naphthalenyldimethylsulfonium
hexafluorophosphonate,
4-hydroxy-1-naphthalenyldimethylsulfonium
hexafluoroarsenate,
4-hydroxy-1-naphthalenyldimethylsulfonium
trifluoromethane sulfonate,
4-hydroxy-1-naphthalenyldimethylsulfonium
trifluoroacetate,
4-hydroxy-1-naphthalenyldimethylsulfonium-p-toluene
sulfonate, 4-hydroxy-1-naphthalenyldimethylsulfonium
butyltris(2,6-difluorophenyl)borate,
4-hydroxy-1-naphthalenyldimethylsulfonium
hexyltris(p-chlorophenyl)borate and
4-hydroxy-1-naphthalenyldimethylsulfonium
hexyltris(3-trifluoromethylphenyl)borate.
Examples of the above quaternary ammonium salt include tetramethylammonium tetraf luoroborate, tetramethylammonium hexafluorophosphonate, tetramethylammonium hexafluoroarsenate, tetramethylammonium trifluoromethane sulfonate, tetramethylammonium trifluoroacetate, tetramethylammonium-p-toluene sulfonate,
tetramethylammonium butyltris(2,6-difluorophenyl)borate, tetramethylammonium hexyltris(p-chlorophenyl)borate.

tetramethylammonium
hexyltris(3-trifluoromethylphenyl)borate,
tetrabutylaminonium tetrafluoroborate. tetrabutylammuonium
hexaf luorophosphonate, tetrabutylaminonium
hexafluoroarsenate, tetrabutylammonium trifluoromethane
sulfonate, tetrabutylammonium trifluoroacetate,
tetrabutylammonium-p-toluene sulfonate, tetrabutylammonium
butyltris(2,6-difluorophenyl)borate, tetrabutylammonium
hexyltris(p-chlorophenyl)borate, tetrabutylammonium
hexyltris(3-trifluoromethylpheny1)borate,
benzyltrimethylammonium tetrafluoroborate,
benzyltrimethylammonium hexafluorophosphonate,
benzyltrimethylammonium hexafluoroarsenate,
benzyltrimethylammonium trifluoromethane sulfonate,
benzyltrimethylammonium trifluoroacetate,
benzyltrimethylammonium-p-toluene sulfonate,
benzyltrimethylammonium
butyltris(2,6-difluorophenyl)borate,
benzyltrimethylammonium hexyltris(p-chlorophenyl)borate,
benzyltrimethylammonium
hexyltris{3-trifluoromethylphenyl)borate,
benzyldimethylphenylammonium tetrafluoroborate,
benzyldimethylphenylammonium hexafluorophosphonate,
benzyldimethylphenylammonium hexafluoroarsenate,
benzyldimethylphenylammonium trifluoromethane sulfonate,
benzyldimethylphenylammonium trifluoroacetate,
benzyldimethylphenylammonium-p-toluene sulfonate,
benzyldimethylphenylammonium
butyltris(2,6-difluorophenyl)borate,
benzyldimethylphenylammonium
hexyltris(p-chlorophenyl)borate,
benzyldimethylphenylammonium
hexyltris(3-trifluoromethylphenyl)borate,
N-cinnamylideneethylphenylammonium tetrafluoroborate,

N-cinnamylideneethylphenylanunonium hexafluorophosphonate, N-cinnamylideneethylphenylammonium hexafluoroarsenate, N-cinnamylideneethylphenylammoniuxn trifluoromethane sulfonate, N-cinnamylideneethylphenylammonium trifluoroacetate,
N-cinnamylideneethylphenylammonium-p-toluene sulfonate, N-cinnamylideneethylphenylammonium butyltris(2,6-difluorophenyl)borate, N-cinnamylideneethylphenylcunmonium hexyltris(p--chlorophenyl)borate and N-cinnamylideneethylphenylammoniuin hexyltris(3-trifluoromethylphenyl)borate•
Examples of the above sulfonic acid ester include
a-hydroxymethylbenzoin-p-toluenesulfonic acid ester,
a-hydroxymethylbenzoin-trifluoromethanesulfonic acid
ester, a-hydroxymethylbenzoin-methanesulfonic acid ester,
pyrogallol-tri(p"toluenesulfonic acid)ester,
pyrogallol-tri(trifluoromethanesulfonic acid)ester,
pyrogallol-trimethanesulfonic acid ester,
2,4-dinitrobenzyl-p-toluenesulfonic acid ester,
2,4-dinitrobenzyl-trifluoromethanesulfonic acid ester,
2,4-dinitrobenzyl-methanesulfonic acid ester,
2,4-dinitrobenzyl-l,2-naphthoquinonediazido-5-sulfonic
acid ester, 2,6-dinitroben2yl-p-toluenesulfonic acid ester,
2,S-dinitrobenzyl-trifluoromethanesulfonic acid ester,
2,6-dinitrobenzyl-methanesulfonic acid ester,
2,6-dinitrobenzyl-l,2-naphthoquinonediazido-5-sulfonic
acid ester, 2-nitrobenzyl-p-toluenesulfonic acid ester,
2-nitrobenzyl-trifluoromethanesulfonic acid ester,
2-nitrobenzyl-methanesulfonic acid ester,
2-nitrobenzyl-l,2-naphthoquinonediazido-5-sulfonic acid
ester, 4-nitrobenzyl-p-toluenesulfonic acid ester,
4-nitrobenzyl-trifluoromethanesulfonic acid ester,
4-nitrobenzyl-methanesulfonic acid ester.

4-nitrobenzyl-l,2-naphthoquinonediazido-5-sulfonic acid ester, N-hydroxynaphthalimide-p-toluenesulfonic acid ester, N-hydroxynaphthalimide-trifluoromethanesulfonic acid ester, N-hydroxynaphthalimide-methanesulfonic acid ester,
N-hydroxy-5-norbornene-2,3-dicarboxyimide-p-
toluenesulfonic acid ester,
N-hydroxy-5-norbornene-2,3-dicarboxyimide-
trifluoromethanesulfonic acid ester,
N-hydroxy-5-norbornene-2,3-dicarboxyimide-
methanesulfonic acid ester,
2,4,6,3',4',5'-hexahydroxybenzophenone-1,2-
naphthoquinonediazido-4-sulfonic acid ester and
1,1,l-tri{p-hydroxyphenyl)ethane-1,2-
naphthoquinonediazido-4-sulfonic acid ester.
Out of these compounds, 2-(3-chlorophenyl)-4,6-bis(trichloromethyl)-s-triazine, 2-(4-methoxyphenyl)-4,6-bis(trichloromethyl)-s-triazine, 2-(4-methylthiophenyl)-4,6-bis(trichloromethyl)-s-triazine,
2 -(4-methoxy-P-styryl)- 4,6-bis(trichloromethyl)-s-
triazine, 2-piperonyl-4,6-bis(trichloromethyl)-s-triazine,
2 -[2 -(furan-2-yl)ethenyl]- 4,6-bis(trichloromethyl)-s-
triazine, 2-[2-(5-methylfuran-2-yl)ethenyl]-4,6-bis
(trichloromethyl)-s-triazine,
2-[2-(4-diethylamino-2-methylphenyl)ethenyl]-4,6-bis
(trichloromethyl)-s-triazine and
2-(4-methoxynaphthyl)-4,6-bis(trichloromethyl)-s-
triazine are preferred as trichloromethyl-s-triazines;
diphenyliodonium trifluoroacetate, diphenyliodonium
trifluoromethane sulfonate, 4-methoxyphenylphenyliodonium
trifluoromethane sulfonate and
4-methoxyphenylphenyliodonium trifluoroacetate are
preferred as diaryliodonium salts; triphenylsulfonium
trifluoromethane sulfonate, triphenylsulfonium

trifluoroacetate, 4-methoxyphenyldiphenylsulfonium
trifluoromethane sulfonate,
4-methoxyphenyldiphenylsulfonium trifluoroacetate,
4-phenylthiophenyldiphenylsulfonium trifluoromethane
sulfonate and 4-phenylthiophenyldiphenylsulfonium
trifluoroacetate are preferred as triarylsulfonium salts;
tetramethylammonium butyltris(2,6-difluorophenyl)borate,
tetramethylammonium hexyltris(p-chlorophenyl)borate,
tetramethylammonium
hexyltris(3-trifluoromethylphenyl)borate,
benzyldimethylphenylammonium
butyltris(2,6-difluorophenyl)borate,
benzyldimethylphenylammonium
hexyltris(p-chlorophenyl)borate and
benzyldimethylphenylammonium
hexyltris(3-trifluoromethylphenyl)borate are preferred as
quaternary ammonium salts; and
2,6-dinitrobenzyl-p-toluenesulfonic acid ester,
2,6-dinitrobenzyl-trifluoromethanesulfonic acid ester,
N-hydroxynaphthalimide-p-toluenesulfonic acid ester and
N-hydroxynaphthalimide-trifluoromethanesulfonic acid ester
are preferred as sulfonic acid esters.
What are disclosed by JP-A 4-330444, "Polymer", pp, 242-248, vol. 46, No. 6 (1997) and USP 5,627,010 are advantageously used as the above radiation sensitive base generator. However, any radiation sensitive base generator is acceptable if it forms a base upon exposure to radiation.
The radiation sensitive base generator in the present invention is preferably a photoactive carbamate such as triphenyl methanol, benzyl carbamate or benzoin carbamate; amide such as o-carbamoyl hydroxylamide, o-carbamoyloxime, aromatic sulfonamide, alpha-lactam or N-(2-allylethynyl)amide, or other amide; oxime ester,
a-aminoacetophenone or cobalt complex.
1

Examples of the radiation sensitive base generator include compounds represented by the following general formulas (17) to (27):

wherein R72 is an alkyl group having 1 to 6 carbon atoms, alkoxyl group having 1 to 6 carbon atoms, thioalkyl group having 1 to 6 carbon atoms, dialkylamino group having 1 to 6 carbon atoms, piperidyl group, nitro group, hydroxy group, mercapto group, alkenyl group or alkynyl group having 2 to 6 carbon atoms, aryl group having 6 to 20 carbon atoms, fluorine atom, chlorine atom or bromine atom, k is an integer of 0 to 3, R73 is a hydrogen atom, alkyl grorp having 1 to 6 carbon atoms, alkenyl group or alkynyl group having 2 to 6 carbon atoms or aryl group having 6 to 20 carbon atoms, and R74 and R75 are each independently a hydrogen atom, alkyl group having 1 to 6 carbon atoms, alkenyl group or alkynyl group having 2 to 6 carbon atoms, or aryl group or benzyl group having 6 to 20 carbon atoms, or R74 and R75 may be bonded together to form a cyclic structure having 5 to 6 carbon atoms,

wherein R76 is an alkyl group having 1 to 6 carbon atoms, alkoxyl group having 1 to 6 carbon atoms, thioalkyl group having 1 to 6 carbon atoms, dialkylamino group having 1 to 6 carbon atoms, piperidyl group, nitro group, hydroxy group, mercapto group or aryl group, R77 is a hydrogen atom, alkyl group or aryl group having 1 to 6 carbon atoms, and R78 and R79 are each independently a hydrogen atom, alkyl group having 1 to 6 carbon atoms, aryl group or benzyl group, or R78 and R79 may be bonded together to form a cyclic structure having


wherein R93 is an alkyl group having 1 to 6 carbon atoms, alkoxyl group having 1 to 6 carbon atoms, thioalkyl group

having 1 to 6 carbon atoms, dialkylamino group having 1 to 6 carbon atoms, piperidyl group, nitro group, hydroxy group, mercapto group or aryl group, R94 and R95 are each independently a hydrogen atom, hydroxyl group, mercapto group, cyano group, phenoxy group, alkyl group having 1 to 6 carbon atoms, fluorine atom, chlorine atom, bromine atom or aryl group, and R96 and R97 are each independently a hydrogen atom, alkyl group having 1 to 6 carbon atoms, aryl group or benzyl group, or R96 and R97 may be bonded together to form a cyclic structure having 5 to 6 carbon atoms.


R106 and R107 are each independently a hydrogen atom, hydroxyl group, mercapto group, cyano group, phenoxy group, alkyl group having 1 to 6 carbon atoms, fluorine atom, chlorine atom, bromine atom or aryl group, R108 to R111 are each independently a hydrogen atom, alkyl group having 1 to 6 carbon atoms, aryl group or benzyl group, or R108 and R109, or R110 and R111 may be bonded together to form a cyclic structure having 5 to 6 carbon atoms, and A6 is an alkylene group having 1 to 6 carbon atoms, cyclohexylene group, phenylene group or single bond.


obtained by substituting a hydrogen atom contained in the above groups by a fluorine atom, chlorine atom, bromine atom, haloalkyl group, 'hydroxyl group, carboxyl group, mercapto group, cyano group, nitro group, azido group, dialkylamino group, alkoxyl group or thioalkyl group.
Out of these radiation sensitive base generators, preferred are 2-nitrobenzylcyclohexyl carbamate, triphenyl methanol, o-carbamoylhydroxylamide, o-carbamoyloxime, [[(2,6-dinitrobenzyl)oxy]carbonyl]cyclohexylamine, bis[[{2-nitrobenzyl)oxy]carbonyl]hexane 1,6-diamine, 4-(methylthiobenzoyl)-1-methyl-1-morpholinoethane, {4-morpholinobenzoyl)-1-benzyl-1-dimethylaminopropane, N-(2-nitrobenzyloxycarbonyl)pyrrolidine, hexaamminecobalt(III) tris(triphenylmethylborate) and 2-benzyl-2-dimethylamino-1-(4-morpholinophenyl)-butanone.
The above radiation sensitive decomposer (C) is used in an amount of preferably 0.01 part or more by weight, more preferably 0.05 part or more by weight based on 100 parts by weight of the total of the decomposable compound (A) and the hydrolyzate (B), When the amount of the component (C) is smaller than 0.01 part by weight, sensitivity to radiation may lower. The upper limit value is preferably 30 parts by weight, more preferably 20 parts by weight. (D) stabilizer
The refractive index changing composition of the present invention may contain (D) a stabilizer as an optional component in addition to the above components (A), (B) and (C).
The stabilizer (D) used in the present invention has
the function of stabilizing the residual decomposable

compound (A) contained in the refractive index changing composition after exposure to radiation to provide stability to an acid or base. This stabilization prevents a change in refractive index and hence the deterioration of a refractive

index pattern formed by the method of the present invention even when it is used under the condition that light having a wavelength close to the wavelength used to change the refractive index passes therethrough.
The above stabilizer (D) is selected from an amino compound, epoxy compound, thiirane compound, oxetane compound, alkoxymethyl melamine compound, alkoxymethyl glycoluril compound, alkoxymethyl benzoguanamine compound, alkoxymethyl urea compound, isocyanate compound, cyanate compound, oxazoline compound, oxazine compound and silyl compound (halogenated silyl compound and other silyl compound).
Examples of the above amino compound include triethylamine, tripropylamine, tributylamine, tripentylamine, trihexylamine, tricyclohexylamine, triphenylamine, tribenzylamine, aniline, ethylenediamine, diethylenetriamine, triethylenetetramine, tetraethylenepentamine, 1,3-diaminopropane, 1,4-diaminobutane, 1,5-diaminopentane, 1,6-diaminohexane, 1,7-diaminoheptane, 1,8-diaminooctane, 1,9-diaminononane, 1,10-diaminodecane, 1,11-diaminoundecane, 1,12-diaminododecane, 1,4-diaminocyclohexane, 1,3-cyclohexanebis(methylamine), 1,3-propane-2-ol, 2,2', 2'-triaminotriethylamine, 1,4-diamino-2,2,3,3-tetrafluoropentane, 1,5-diamino-2,2,3,3,4,4-hexafluoropentane, melamine, benzoguanamine, acetoguanamine, acryloguanamine, paramine, amidol, m-phenylenediamine, p-phenylenediamine, p,p'-diaminodiphenylmethane, diaminodiphenylsulfone, 1,8-diaminonaphthalene, 3,5-diamino-l,2,4-triazole, 2-chloro-4,6-diamino-S-triazine, 2,6-diaminopyridine, 3,3'-diaminobenzidine, bis(4-aminophenyl)ether, m-xylylenedieunine, p-xylylenediamine, 1,2,4,5-benzenetetramine, 2,4-diamine-1,3,5-triazine,

4,4'-diaminobenzophenone,
3,3',4,4'-tetraaminobenzophenone, triaminobenzene,
4,4' -thiodianiline, 2,3,5,6-tetrabromo-p-xylylenediamine,
2,3,5, 6-tetrachloro-p-xylylenediainine,
4,5-methylenedioxy-1,2-phenylenediamine and
2,2'-bis(5-aminopyridyl)sulfide.
Examples of the above epoxy compound include bisphenol A epoxy resin, bisphenol F epoxy resin, phenol novolak epoxy resin, cresol novolak epoxy resin, cyclic aliphatic epoxy resin, bisphenol A epoxy compound and aliphatic polyglycidyl ether.
Examples of commercially available products of the above compounds are given below. Commercially available products of the bisphenol A epoxy resin include Epicoat 1001, 1002, 1003, 1004, 1007, 1009, 1010 and 828 (of Yuka Shell Epoxy Co. , Ltd. ) , those of the bisphenol F epoxy resin include Epicoat 807 (of Yuka Shell Epoxy Co., Ltd.), those of the phenol novolak epoxy resin include Epicoat 152 and 154 (of Yuka Shell Epoxy Co., Ltd.) and EPPN201 and 202 (of Nippon Kayaku Co., Ltd.), those of the cresol novolak epoxy resin include EOCN-102, EOCN-103S, EOCN-104S, EOCN-1020, EOCN-1025 and EOCN-1027 (of Nippon Kayaku Co., Ltd.) and Epicoat 180S75 (of Yuka Shell Epoxy Co. , Ltd.), those of the cyclic aliphatic epoxy resin include CY175, CY177 and CY179 (of CIBA-GEIGY A.G.), ERL-4234, ERL-4299, ERL-4221 and ERL-4206 (of U.C.C. Co., Ltd.), Showdyne 509 (of Showa Denko K.K.), Araldyte CY-182, CY-192 and CY-184 (of CIBA-GEIGY A.G. ) , Epichlon 200 and 400 (of Dainippon Ink and Chemicals, Inc.), Epicoat 871 and 872 (of Yuka Shell Epoxy Co., Ltd.) and ED-5661 and ED-5662 (of Celanees Coating Co. , Ltd. ) , and those of the aliphatic polyglycidyl ether include Epolite lOOMF (of Kyoeisha Kagaku Co., Ltd.) and Epiol TMP (of NOF Corporation).
Besides the above compounds, phenylglycidyl ether.

butylglycidyl ether, 3,3,3-trifluoromethylpropylene oxide,
styrene oxide, hexafluoropropylene oxide, cyclohexene_oxide,
N-glycidylphthalimide, (nonafluoro-N-butyl)epoxide,
perfluoroethylglycidyl ether, epichlorohydrin,
epibromohydrin, N,N-diglycidylaniline and
3-[2-{perfluorohexyl)ethoxy]-1,2-epoxypropane may be
advantageously used as an epoxy compound.
Examples of the above thiirane compound include what are obtained by substituting the epoxy groups of the above epoxy compounds with an ethylene sulfide group as shown in J, Org. Chem., 28, 229 (1963), for example.
Examples of the above oxetane compound include bis[(3-ethyl-3-oxetanylmethoxy)methyl]benzene (trade name of XDO, manufactured by Toagosei Chemical Industry Co., Ltd.),.
bis[(3-ethyl-3-oxetanylmethoxy)methyl-phenyl]methane, bis[(3-ethyl- 3-oxetanylmethoxy)methyl-phenyl]ether, bis[(3-ethyl-3-oxetanylmethoxy)methyl-phenyl]propane, bis[(3-ethyl-3-oxetanylmethoxy)methyl-phenyl]sulfone, bis[(3-ethyl-3-oxetanylmethoxy)methyl-phenyl]ketone, bis[(3-ethyl-3-oxetanylmethoxy)methyl-phenyl] hexafluoropropane,
tri[(3-ethyl-3-oxetanylmethoxy)methyl]benzene and tetra[(3-ethyl-3-oxetanylmethoxy)methyl]benzene.
The above alkoxymethyl melamine compound, alkoxymethyl benzoguanamine compound, alkoxymethyl glycoluril compound and alkoxymethyl urea compound are obtained by substituting the methylol groups of a methylol melamine compound, methylol benzoguanamine compound, methylol glycoluril compound and methylol urea compound with an alkoxymethyl group, respectively. The type of the alkoxymethyl group is not particularly limited, as exemplified by methoxymethyl group, ethoxymethyl group, propoxymethyl group and butoxymethyl group.

commercially available products of the above compounds include Cymel 300, 301, 303, 370, 325, 327, 701, 266, 267, 238, 1141, 272, 202, 1156, 1158, 1123, 1170 and 1174, and UFR65 and 300 (of Mitsui Cyanamid Co., Ltd.). and Nicalak Mx-750, Mx-032, Mx-706, Mx-708, Mx-40, Mx-31, Ms-11 and Mw-30 (of Sanwa Chemical Co., Ltd.).
Examples of the above isocyanate compound include phenylene-1,3-diisocyanate, phenylene-1,4-diisocyanate, l-methoxyphenylene-2,4-diisocyanate, l-methylphenylene-2,4-diisocyanate, 2,4-tolylene diisocyanate, 2,6-tolylene diisocyanate, 1,3-xylylene diisocyanate, 1,4-xylylene diisocyanate, biphenylene-4,4'-diisocyanate, 3,3'-dimethoxybiphenylene-4,4'-diisocyanate, 3,3'-dimethylbiphenylene-4,4'-diisocyanate, diphenylmethane-2,4'-diisocyanate, diphenylmethane-4,4'-diisocyanate, 3,3'-dimethoxydiphenylmethane-4,4'-diisocyanate, 3,3'-dimethyldiphenylmethane-4,4'-diisocyanate, naphthylene-1,5-diisocyanate, cyclobutylene-1,3-diisocyanate, cyclopentylene-1,3-diisocyanate, cyclohexylene-1,3-diisocyanate, cyclohexylene-1,4-diisocyanate, l-methylcyclohexylene-2,4-diisocyanate, 1-methylcyclohexylene-2,6-diisocyanate, l-isocyanate-3,3,5-trimethyl-5-isocyanate methylcyclohexane, cyclohexane-1,3-bis(methylisocyanate), cyclohexane-1,4-bis(methylisocyanate), isophorone diisocyanate, dicyclohexylmethane-2,4'-diisocyanate, dicyclohexylmethane-4,4'-diisocyanate, ethylene diisocyanate, tetramethylene-1,4-diisocyanate, hexamethylene-1,6-diisocyanate, dodecamethylene-1,12-diisocyanate, lysine diisocyanate

methyl ester and prepolymers having an isocyanate group at both terminals obtained from a reaction between a stoichiometrically excessive amount of one of the above organic diisocyanates and a bifunctional active hydrogen-containing compound.
The above diisocyanate may be used in combination with an organic polyisocyanate having 3 or more isocyanate groups , such as phenyl-1,3,5-triisocyanate, diphenylmethane-2,4,4'-triisocyanate, diphenylmethane-2,5,4'-triisocyanate, triphenylmethane-2,4',4"-triisocyanate, triphenylmethane-4,4',4"-triisocyanate, diphenylmethane-2,4,2',4'-tetraisocyanate, diphenylmethane-2,5,2',5'-tetraisocyanate, cyclohexane-1,3,5-triisocyanate, cyclohexane-1,3,5-tris(methylisocyanate), 3,5-dimethylcyclohexane-l,3,5-tris(methylisocyanate), 1,3,5-trimethylcyclohexane-l,3,5-tris{methylisocyanate), dicyclohexylmethane-2,4,2'-triisocyanate, dicyclohexylmethane~2,4,4'-triisocyanate or a prepolymer having an isocyanate group at a terminal obtained from a reaction between a stoichiometrically excessive amount of one of the above organic polyisocyanates having 3 or more isocyanate groups and a polyfunctional active hydrogen-containing compound having 2 or more hydrogen atoms.
Examples of the above cyanate compound include 1,3-dicyanatobenzene, 1,4-dicyanatobenzene, 1,3,5-tricyanatobenzene, 1,3-, 1,4-, 1,6-, 1,8-, 2,6- or 2,7-dicyanatonaphthalene, 1,3,6-tricyanatonaphthalene, 2,2'- or 4,4'-dicyanatobiphenyl, bis(4-cyanatophenyl)methane, 2,2-bis(4-cyanatophenyl)propane, 2,2'-bis(3,5-dichloro-4-cyanatophenyl)propane.

2,2-bis(4-cyanatophenyl)ethane, bis(4-cyanatophenyl)ether, bis(4-cyanatophenyl)thioether, bis(4-cyanatophenyl)sulfone,
1,1,1,3,3,3-hexafluoro-2,2-bis(4-cyanatophenyl)propane, tris(4-cyanatophenyl)phosphite,
tris(4-cyanatophenyl)phosphate and benzene polynuclear polyisocyanate compounds obtained from a reaction between a phenol resin and halogenated cyan (for example, JP-B 45-11712 and JP-B 55-9433) (the term "JP-B" as used herein means an "examined Japanese patent publication"). A divalent cyanic acid ester compound derived from a bisphenol such as 2,2-bis(4-cyanatophenyl)propane is particularly preferred because it is easily acquired and provides excellent moldability and favorable properties to the final cured product. A polycyanate obtained by reacting an initial condensate of a phenol and formaldehyde with halogenated cyan is also useful.
Examples of the above oxazoline compound include 2,2'-bis(2-oxazoline),
4-furan-2-ylmethylene-2-phenyl-4H-oxazol-5-one, 1,4-bis(4,5-dihydro-2-oxazolyl)benzene, 1,3-bis(4,5-dihydro-2-oxazolyl)benzene, 2,3-bis(4-isopropenyl-2-oxazoline-2-yl)butane, 2,2'-bis-4-benzyl"2-oxazoline, 2,6-bis(isopropyl-2-oxazoline-2-yl)pyridine, 2,2'-isopropylidenebis(4-tert-butyl-2-oxazoline), 2,2'-isopropylidenebis(4-phenyl-2-oxazoline), 2,2'-methylenebis(4-tert-butyl-2-oxazoline) and 2,2'-methylenebis(4-phenyl-2-oxazoline).
Examples of the above oxazine compound include 2,2'-bis(2-oxazine),
4-furan-2-ylmethylene-2-phenyl-4H-oxazyl-5-one, 1,4-bis(4,5-dihydro-2-oxazyl)benzene, 1,3-bis(4,5-dihydro- 2-oxazyl)benz ene,

2,3-bis(4-isopropenyl-2-oxazine-2-yl)butane, 2,2'-bis-4-benzyl-2-oxazine, 2,6-bis(isopropyl-2-oxazine-2-yl)pyridine, 2,2'-isopropylidenebis(4-tert-butyl-2-oxazine), 2,2'-isopropylidenebis(4-phenyl-2-oxazine), 2,2'-methylenebis{4-tert-butyl-2-oxazine) and 2,2'-methylenebis{4-phenyl-2-oxazine).
Examples of the above halogenated silyl compound include tetrahalogenosilanes such as tetrachlorosilane, tetrabromosilane, tetraiodosilane, trichlorobromosilane and dichlorodibromosilane; monoalkyltrihalogenosilanes such as methyltrichlorosilane, methyldichlorobromosilane and cyclohexyltrichlorosilane; monoaryltrihalogenosilanes such as phenyltrichlorosilane, naphthyltrichlorosilane, 4-chlorophenyltrichlorosilane and
phenyldichlorobromosilane; monoaryloxytrihalogenosilanes such as phenoxytrichlorosilane and phenoxydichlorobromosilane; monoalkoxytrihalogenosilanes
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such as methoxytrichlorosilane and ethoxytrichlorosilane; dialkyldihalogenosilanes such as dimethyldichlorosilane, methyl(ethyl)dichlorosilane and methyl(cyclohexyl)dichlorosilane; monoalkylmonoaryldihalogenosilanes such as methyl(phenyl)dichlorosilane; diaryldihalogenosilanes such as diphenyldichlorosilane; diaryloxydihalogenosilanes such as diphenoxydichlorosilane;
monoalkylmonoaryloxydihalogenosilanes such as methyl(phenoxy)dichlorosilane; monoarylmonoaryloxydihalogenosilanes such as phenyl(phenoxy)dichlorosilane; dialkoxydihalogenosilanes such as diethoxydichlorosilane; monoalkylmonoalkoxydichlorosilanes such as methyl(ethoxy)dichlorosilane; monoarylmonoethoxydichlorosilanes such as

phenyl(ethoxy)dichlorosilane; trialkylmonohalogenosilanes such as trimethylchlorosilane, dimethyl(ethyl)chlorosilane and dimethyl(cyclohexyl)chlorosilane; dialkylmonoarylmonohalogenosilanes such as dimethyl(phenyl)chlorosilane; monoalkyldiarylmonohalogenosilanes such as methyl(diphenyl)chlorosilane; triaryloxymonohalogenosilanes such as triphenoxychlorosilane;
monoalkyldiaryloxymonohalogenosilanes such as methyl(diphenoxy)chlorosilane; monoaryldiaryloxymonohalogenosilanes such as phenyl(diphenoxy)chlorosilane; dialkylmonoaryloxymonohalogenosilanes such as dimethyl(phenoxy)chlorosilane; diaryImonoaryloxymonohalogenosilanes such as diphenyl(phenoxy)chlorosilane;
monoalkylmonoarylmonoaryloxymonohalgenosilanes such as methyl(phenyl)(phenoxy)chlorosilane; triethoxymonohalogenosilanes such as
triethoxychlorosilane; and oligomers thereof such as dimer, trimer, tetramer and pentamer of tetrachlorosilane.
Examples of the above other silyl compound include hexamethyldisilazane, t-butyldimethylchlorosilane, bis(trimethylsilyl)trifluoroacetamide, diethylciminotrimethylsilane, trimethylsilanol, hexamethyldisiloxane, chloromethyldimethylethoxysilane, acetyltriphenylsilane, ethoxytriphenylsilane, triphenylsilanol, triethylsilanol, tripropylsilanol, tributylsilanol, hexaethyldisiloxane, trimethylmethoxysilane, trimethylethoxysilane, triethylmethoxysilane, triethylethoxysilane, acetoxyethyldimethylchlorosilane, l,3-bis(hydroxybutyl)tetramethyldisiloxane.

1,3-bis(hydroxypropyl)tetramethyldisiloxane, Y-aminqpropylmethoxysilane, y-apiinoprapylathoxysilan-e, N-p(aminoethyl) -γ-aminopropyltrimethoxysilane, N-p(aminoethyl) -γ-aminopeopylmethyldimethoxysilane, N-phenyl-y-aminopropyltrimethoxysilane, y-anilinopropyltrimethoxysilane, y-dibutylaminopropyltrimethoxysilane, y-ureidopropyltriethoxysilane, N-p(N-vinylbenzylaminoethyl)-y-aminopropyltrimethoxysilane•hydrochlorate,
y-methacryloxypropyltrimethoxysilane, y-methacryloxypropyltriethoxysilane, vinyltrimethoxysilane, vinyltriethoxysilane,
vinyltrichlorosilane, vinyltris(p-methoxyethoxy)silane, y-glycidoxypropylmethyldiethoxysilane, y-glycidoxypropyltriethoxysilane, y-(3,4-epoxycyclohexyl)ethyltrimethoxysilane, y-glycidoxypropyltrimethoxysilane, y-mercaptopropyltrimethoxysilane,
y-chloropropyltrimethoxysilane, trimethylchlorosilane, hexamethyldisilazane, N-trimethylsilylimidazole, bis(trimethylsilyl)urea, trimethylsilylacetamide, bistrimethylsilylacetamide, trimethylsilylisocyanate, trimethylmethoxysilane, trimethylethoxysilane, methyltrimethoxysilane, methyltriethoxysilane, dimethyldimethoxysilane, dimethyldiethoxysilane, t-butyldimethylchlorosilane, t-butyldiphenylchlorosilane, triisopropylchlorosilane, n-propyltrimethoxysilane, isobutyltrimethoxysilane, n-hexyltrimethoxysilane, n-decyltrimethoxysilane, n-hexadecyltrimethoxysilane, l,6-bis(trimethoxysilyl)hexane, dimethylsilyldiisocyanate, methylsilyltriisocyanate, phenyltrimethoxysilane, diphenyldimethoxysilane and phenylsilyltriisocyanate.
Out of these, the stabilizer (D) used in the present

invention is preferably an amino compound, epoxy compound, thiirane compound, oxetane compound, oxazoline compound, oxazine compound, silyl compound, isocyanate compound or cyanate compound, more preferably an amino compound, epoxy compound, thiirane compound, oxetane compound, oxazoline compound or oxazine compound. It is particularly preferably ethylenediamine, phenylglycidyl ether, 3-phenoxypropylene sulfide, 3,3,3-trifluoropropylene oxide,
hexamethyldisilazane, γ-aminopropylmethoxysilane, Y-glycidoxypropyltrimethoxysilane or methylsilyltriisocyanate•
These stabilizers (D) may be used alone or in combination of two or more. The amount of the component (D) may be excessive so that the residual decomposable compound (A) can react to the full but it is generally 10 parts or more by weight, preferably 30 parts or more by weight based on 100 parts by weight of the component (A) . When the amount of the component (D) is smaller than 10 parts by weight, the stability of the refractive index changing composition may become unsatisfactory due to an incomplete reaction.
A catalyst may be used in combination with the stabilizer (D). Use of the catalyst promotes a reaction between the component (D) and the residual decomposable compound (A).
The catalyst is, for example, an acid catalyst, basic catalyst or quaternary onium salt.
Examples of the above acid catalyst include organic acids such as acetic acid, methanesulfonic acid, p-toluenesulfonic acid, trifluoroacetic acid and trifluoromethanesulfonic acid; and inorganic acids such as hydrochloric acid, sulfuric acid and nitric acid. Examples of the above basic catalyst include alkali metal carbonates such as sodium carbonate, potassium carbonate and lithium carbonate; alkali metal bicarbonates such as sodium

bicarbonate, potassium bicarbonate and lithium bicarbonate; alkali metal acetates such as sodium acetate; alkali metal hydrides such as lithium hydride, sodium hydride and potassium hydride; alkali metal hydroxides such as sodium hydroxide, potassium hydroxide and lithium hydroxide; alkali metal alkoxides such as sodium methoxide, sodium ethoxide, potassium t-butoxide and lithium methoxide; mercaptan alkali metals such as methyl mercaptan sodium and ethyl mercaptan sodium; organic amines such as triethylamine, tributylamine, diisopropylethylamine, N-methylmorpholine, pyridine, 4-(N,N-dimethylamino)pyridine, N,N-dimethylaniline, N,N-diethylaniline, 1,5-diazabicyclo[4.3.0]non-5-ene, 1,4-diazabicyclo[2,2.2]octane (DABCO) and l,8-diazabicyclo[5. 4 .0]undec-7-ene (DBU) ; alkyl lithitims such as methyl lithium, ethyl lithium and butyl lithium; and lithium alkyl amides such as lithium diisopropylamide and lithium dicyclohexylamide. Examples of the above quaternary onium salt include tetrabutylammonium chloride, tetrabutylammonium bromide, tetrabutylammonium iodide, tetrabutylammonium acetate, tetrabutylphosphonixim chloride, tetrabutylphosphonium bromide, cetyltrimethylammonixim bromide, tetrapropylammonium bromide and benzyltriethylammonium chloride. A combination of 18-crown-6-ether and a salt such as potassium chloride, potassium bromide, potassium iodide, cesium chloride, potassium phenoxide, sodium phenoxide or potassium benzoate may also be used as a catalyst.
Out of these, p-toluenesulfonic acid, hydrochloric acid, sulfuric acid, sodium hydroxide, potassium t-butoxide, triethylamine, DBU, tetrabutylammonium bromide, tetrabutylphosphonium bromide and
18-crown-6-ether/potassium phenoxide are preferred as a catalyst.
The amount of the catalyst is preferably 2 mols or less

based on 1 equivalent of the component (D) when an amino compound, alkoxymethyl melamine compound, alkoxymethyl glycoluril compound, alkoxymethyl benzoguanamine compound, alkoxymethyl urea compound or halogenated silyl compound is used as the component (D).
When an epoxy compound, thiirane compound, oxetane compound, isocyanate compound, cyanate compound, oxazoline compound, oxazine compound or other silyl compound is used as the component (D), it is preferably 0.2 mol or less based on 1 equivalent of the component (D).
The number of equivalents of the component (D) is obtained by multiplying the number of reactive groups contained in the component (D) by the amount (mol) of the component (D), and the number of reactive groups is defined as follows according to the type of the component (D). amino compound: number of nitrogen atoms epoxy compound: number of epoxy groups thiirane compound: number of ethylene sulfide groups oxetane compound: number of oxetanyl groups alkoxymethyl melamine compound, alkoxymethyl glycoluril compound, alkoxymethyl benzoguanamine compound and alkoxymethyl urea compound: number of alkoxymethyl groups isocyanate compound: number of isocyanate groups cyanate compound: number of cyanate groups oxazoline compound: number of oxazolyl groups oxazine compound: number of oxazyl groups
halogenated silyl compound: number of halogen atoms bonded to silicon atoms
other silyl compound: number of silicon atoms
The refractive index changing composition of the present invention may contain other additives in limit not prejudicial to the object of the present invention. The additives include an ultraviolet light absorber, sensitizer.

surfactant, antioxidant, heat resistance improving agent and adhesive aid.
The above urtravidlet light absorber" is, for example, a benzotriazole, salicylate, benzophenone, substituted acrylonitrile, xanthene, coumarin, flavone or chalcone. Specific examples of the ultraviolet light absorber include Tinubin 234
(2-(2-hydroxy-3,5-bis(α,α-dimethylbenzyl)phenyl)-2H-benzotriazole), Tinubin 571 (hydroxyphenylbenzotriazole derivative) and Tinubin 1130 (condensate of methyl-3-(3-t-butyl-5-(2H-benzotriazol-2-yl)-4-hydroxyphenyl)propionate and polyethylene glycol (molecular weight of 300)) (of Ciba Specialty Chemicals Co., Ltd.), 1,7-bis(4-hydroxy-3-methoxyphenyl)-1,6-heptadiene-3,5-dione and dibenzylidene acetone.
By adding an ultraviolet light absorber, the amount of an acid or base formed from the component (C) can be made gradually smaller as the depth from the surface of an exposed
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portion of the refractive index changing composition of the present invention increases, which is useful as means of forming GRIN. The amount of the ultraviolet light absorber is preferably 30 parts or less by weight, more preferably 20 parts or less by weight based on 100 parts by weight of the total of the components (A) and (B).
The above sensitizer is, for example, a coumarin having a substituent at the 3-position and/or 7-position, flavone, dibenzalacetone, dibenzalcyclohexane, chalcone, xanthene, thioxanthene, porphyrin, phthalocyanine, acridine or anthracene.
The amount of the sensitizer is preferably 30 parts or less by weight, more preferably 20 parts or less by weight based on 100 parts by weight of the total of the components (A) and (B).
The above surfactant may be added to improve

coatability, for example, prevent striation or improve developability.
"Examples of the surfactant include nonionic surfactants such as polyoxyethylene alkyl ethers including polyoxyethylene lauryl ether, polyoxyethylene stearyl ether and polyoxyethylene oleyl ether; polyoxyethylene aryl ethers including polyoxyethylene octylphenyl ether and polyoxyethylene nonylphenyl ether; and polyethylene glycol dialkyl esters including polyethylene glycol dilaurate and polyethylene glycol distearate; fluorinated surfactants which are commercially available under the trade names of F Top EF301, EF303 and EF352 (of Shin Akita Kasei Co. , Ltd. ) , Megafac F171, F172 and F173 (of Dainippon Ink and Chemicals, Inc. ) , Florade FC430 and FC431 (of Sumitomo 3M Limited) , and Asahi Guard AG710, Surflon S-382, SC-101, SC-102, SC-103, SC-104, SC-105 and SC-106 (of Asahi Glass Co., Ltd.); and other surfactants which are commercially available under the trade names of organosiloxane polymer KP341 (of Shin-Etsu Chemical Co., Ltd.) and acrylic or methacrylic acid-based (co)polymer Polyflow No. 57 and No. 95 (of Kyoeisha Kagaku Co., Ltd.).
The amount of the surfactant is preferably 2 parts or less by weight, more preferably 1 part or less by weight based on 100 parts by weight of the total of the components (A) and (B).
The above antioxidant is, for example, a phenol-based (such as hindered phenol), amine-based, phosphorus-based, sulfur-based, hydroquinone-based or quinoline-based antioxidant.
Examples of the phenol-based antioxidant include hindered phenols such as
2,2'-methylenebis(4-methyl-6-t-butylphenol), 4,4'-methylenebis(2,6-di-t-butylphenol), 4,4'-butylidenebis(3-methyl-6-t-butylphenol),

2,6-di-t-butyl-p-cresol, l,3,5-trimethyl-2 4,6-tris(3,5-di-t-butyl-4-hydroxybenzyl )benzene,
1,6-hexanediol-bis[3-(3,5-di-t-butyl-4-hydroxyphenyl) propionate], pentaerythritol
tetrakis[3-{3,5-di-t-butyl-4-hydroxyphenyl)propionate], triethylene
glycol-bis[3-(3 -1-butyl-5-methyl-4-hydroxyphenyl) propionate],
n-octadecyl-3-(4',5'-di-t-butylphenol)propionate, n-octadecyl-3-(4'-hydroxy-3',5'-di-t-butylphenol) propionate,
stearyl-2-(3,5-di-t-butyl-4-hydroxyphenol)propionate, distearyl-3,5 -di-1-butyl-4-hydroxybenzylphosphonate, 2-t-butyl-6-(3-t-butyl-5-methyl-2-hydroxybenzyl)-4-methylphenyl acrylate,
N,N'-hexamethylenebis(3,5-di-t-butyl-4-hydroxy-hydrocinnamide),
3,9-bis{2-[3-(3 -1-butyl-4-hydroxy-5-methylphenyl) propionyloxy]-1,l-dimethylethyl}-2,4,8,10-tetraoxaspiro [5,5]undecane, 4,4'-thiobis(3-methyl-6-t-butylphenol) and l,l,3-tris(2-methyl-4-hydroxy-5-t-butylphenol)butane. Examples of the amine-based antioxidant include phenyl-1-naphthylamine, phenyl-2-naphthylamine, I N,N'-diphenyl-1,4-phenylenediamine,
N-phenyl-N' -cyclohexyl-.l, 4-phenylenediamine and
4,4'-di(a,a-dimethylbenzyl)diphenylamine.
Examples of the phosphorus-based antioxidant include phosphite compounds such as triisodecyl phosphite, triphenyl ) phosphite, trisnonylphenyl phosphite, diphenylisodecyl phosphite, phenyldiisodecyl phosphite, 2,2-methylenebis(4,6-di-t-butylphenyl)octyl phosphite, 4,4'-butylidenebis(3-methyl-6-t-butylphenyl)ditridecyl phosphite, tris(2,4-di-t-butylphenyl)phosphite.

tris(2-t-butyl-4-methylphenyl)phosphite,
tris(2,4-di-t-amylphenyl)phosphite,
tris(2-t-butylphenyl)phosphite,
bis(2-t-butylphenyl)phenyl phosphite,
tris[2-(1,1-dimethylpropyl)-phenyl]phosphite,
tris[2,4-(1,1-dimethylpropyl)-phenyl]phosphite,
tris(2-cyclohexylphenyl)phosphite and
tris(2-t-butyl-4-phenylphenyl)phosphite; and phosphine
compounds such as triethyl phosphine, tripropyl phosphine,
tributyl phosphine, tricyclohexyl phosphine, diphenylvinyl
phosphine, allyldiphenyl phosphine, triphenyl phosphine,
methylphenyl-p-anisyl phosphine, p-anisyldiphenyl
phosphine, p-tolyldiphenyl phosphine, di-p-anisylphenyl
phosphine, di-p-tolylphenyl phosphine, tri-m-aminophenyl
phosphine, tri-2,4-dimethylphenyl phosphine,
tri-2,4, 6-trimethylphenyl phosphine, tri-o-tolylphosphine,
tri-m-tolylphosphine, tri-p-tolylphosphine,
tri,-o-anisylphosphine, tri-p-anisylphosphine and
1,4-bis(diphenylphosphino)butane.
Examples of the hydroquinone-based antioxidant include 2, 5-di-t-butylhydroquinone, examples of the quinoline-based antioxidant include
6 -ethoxy-2,2,4-trimethyl-1,2-dihydroquinoline, and examples of the sulfur-based antioxidant include dilauryl thiodipropionate and distearyl thiodipropionate.
Out of these antioxidants, phenol-based antioxidants (particularly hindered phenol-based antioxidants) are preferred, and polyol-poly[branched alkyl group or hydroxyl group-substituted phenyl having 3 to 6 carbon atoms]propionate] such as
alkylenediol-bis[3-(3,5-di-branched alkyl having 3 to 6 carbon atoms-4-hydroxyphenyl)propionate] having 2 to 10 carbon atoms including l,6-hexanediol-bis[3-(3,5-di-t-butyl-4-hydroxyphenyl)

propionate]; di- or tri-oxy-alkylene diol having 2 to 4 carbon
atoms-bis[3-(3,5-di-branched alkyl having 3 to 6 carbon
atoms - 4 -hydroxyphenyl) propionate ] including triethyiene
glycol-bis[3-(3-t-butyl-5-methyl-4-hydroxyphenyl)
propionate]; alkane triol having 3 to 8 carbon
atoms-bis[3-(3,5-di-branched alkyl having 3 to 6 carbon
atoms-4-hydroxyphenyl)propionate] including glycerin
tris[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate]; and
alkane tetraol having 4 to 8 carbon atoms
tetrakis[3-(3,5-di-branched alkyl having 3 to 6 carbon
atoms-4-hydroxyphenyl)propionate] including
pentaerythritol
tetrakis[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate]
are particularly preferred among hindered phenols.
These antioxidants may be used alone or in combination of two or more. The amount of the antioxidant is preferably 5 parts or less by weight, more preferably 0.05 to 2.5 parts by weight, particularly preferably 0.1 to 1 part by weight based on 100 parts by weight of the component (A).
The above adhesive aid may be added to improve adhesion to a substrate and is preferably a silane coupling agent.
The above heat resistance improving agent is an unsaturated compound such as a polyacrylate.
An antistatic agent, keeping stabilizer, halation inhibitor, anti-foaming agent, pigment and acid thermal generator may be further added to the refractive index changing composition used in the present invention as required.
In the present invention, a refractive index pattern can be formed from the above refractive index changing composition as follows, for example.
First, the refractive index changing composition is dissolved or dispersed in a solvent to prepare a composition

solution having a solid content of 5 to 70 wt%. The composition solution may be filtered with a filter having an opening-diameter of about 0.+ to lOµm as reiquired before use.
Thereafter, this composition solution is applied to the surface of a substrate such as a silicon wafer and prebaked to remove the solvent so as to form the coating film of the refractive index changing composition. Part of the formed coating film is then exposed to radiation through a pattern mask and baked after exposure (PEB) to produce a refractive index difference between exposed and unexposed portions of the refractive index changing composition.
An acid or base is formed from the radiation sensitive decomposer (C) by the above exposure to act on the component (A) to decompose it. This decomposed product dissipates at the time of baking after exposure. As a result, there is produced a difference in refractive index between exposed and unexposed portions.
The solvent used to prepare a solution containing the refractive index changing composition used in the present invention uniformly dissolves or disperses the above components (A), (B) and (C), the optionally added component (D) and other additives and does not react with these components.
Examples of the solvent include alcohols such as methanol, ethanol, propanol, iso-propanol, butanol, ethylene glycol and propylene glycol; ethers such as tetrahydrofuran; glycol ethers such as ethylene glycol monomethyl ether and ethylene glycol monoethyl ether; ethylene glycol alkylether acetates such as methyl cellosolve acetate and ethyl cellosolve acetate; diethylene glycols such as diethylene glycol monomethyl ether, diethylene glycol monoethyl ether, diethylene glycol dimethyl ether, diethylene glycol ethyl methyl ether and

solution having a solid content of 5 to 70 wt%. The composition solution may be filtered with a filter having -an opening drameter'of about 0.1 to 10 µm as required brfore use.
Thereafter, this composition solution is applied to the surface of a substrate such as a silicon wafer and prebaked to remove the solvent so as to form the coating film of the refractive index changing composition. Part of the formed coating film is then exposed to radiation through a pattern mask and baked after exposure (PEB) to produce a refractive index difference between exposed and unexposed portions of the refractive index changing composition.
An acid or base is formed from the radiation sensitive decomposer (C) by the above exposure to act on the component (A) to decompose it. This decomposed product dissipates at the time of baking after exposure. As a result, there is produced a difference in refractive index between exposed and unexposed portions.
The solvent used to prepare a solution containing the refractive index changing composition used in the present invention uniformly dissolves or disperses the above components (A), (B) and (C), the optionally added component (D) and other additives and does not react with these components.
Examples of the solvent include alcohols such as methanol, ethanol, propanol, iso-propanol, butanol, ethylene glycol and propylene glycol; ethers such as tetrahydrofuran; glycol ethers such as ethylene glycol monomethyl ether and ethylene glycol monoethyl ether; ethylene glycol alkylether acetates such as methyl cellosolve acetate and ethyl cellosolve acetate; diethylene glycols such as diethylene glycol monomethyl ether, diethylene glycol monoethyl ether, diethylene glycol dimethyl ether, diethylene glycol ethyl methyl ether and

diethylene glycol diethyl ether; propylene glycol monoalkyl ethers such as propylene glycol methyl ether, propylene glycol-ethyl ether, propylene glycol propyl ether and propylene glycol butyl ether; propylene glycol alkyl ether acetates such as propylene glycol methyl ether acetate, propylene glycol ethyl ether acetate, propylene glycol propyl ether acetate and propylene glycol butyl ether acetate; propylene glycol alkyl ether acetates such as propylene glycol methyl ether propionate, propylene glycol ethyl ether propionate, propylene glycol propyl ether propionate and propylene glycol butyl ether propionate; aromatic hydrocarbons such as toluene and xylene; ketones such as methyl ethyl ketone, cyclohexanone and 4-hydroxy-4-methyl-2-pentanone; esters such as methyl acetate, ethyl acetate, propyl acetate, butyl acetate, ethyl 2-hydroxypropionate, methyl 2-hydroxy-2-methylpropionate, ethyl 2-hydroxy-2-methylpropionate, methyl hydroxyacetate, ethyl hydroxyacetate, butyl hydroxyacetate, methyl lactate, ethyl lactate, propyl lactate, butyl lactate, methyl 3-hydroxypropionate, ethyl 3-hydroxypropionate, propyl 3-hydroxypropionate, butyl 3-hydroxypropionate, methyl 2-hydroxy-3-methylbutanoate, methyl methoxyacetate, ethyl methoxyacetate, propyl methoxyacetate, butyl methoxyacetate, methyl ethoxyacetate, ethyl ethoxyacetate, propyl ethoxyacetate, butyl ethoxyacetate, methyl propoxyacetate, ethyl propoxyacetate, propyl propoxyacetate, butyl propoxyacetate, methyl butoxyacetate, ethyl butoxyacetate, propyl butoxyacetate, butyl butoxyacetate, methyl 2-methoxypropionate, ethyl 2-methoxypropionate, propyl 2-methoxypropionate, butyl 2-methoxypropionate, methyl 2-ethoxypropionate, ethyl 2-ethoxypropionate, propyl 2-ethoxypropionate, butyl 2-ethoxypropionate, methyl 2-butoxypropionate, ethyl 2-butoxypropionate, propyl 2-butoxypropionate, butyl 2-butoxypropionate, methyl

3-methoxypropionate, ethyl 3-methoxypropionate, propyl
3-methoxypropionate, butyl 3-methoxypropionate, methyl
3-ethoxypropionate ethyl 3-ethoxyproplonate, propyl
3-ethoxypropionate, butyl 3-ethoxypropionate, methyl
3-propoxypropionate, ethyl 3-propoxypropionate, propyl
3-propoxypropionate, butyl 3-propoxypropionate, methyl
3-butoxypropionate, ethyl 3-butoxypropionate, propyl
3-butoxypropionate and butyl 3-butoxypropionate; and
fluorine atom-containing solvents such as
trifluoromethylbenzene, 1,3-bis(trifluoromethyl)benzene,
hexafluorobenzene, hexafluorocyclohexane,
perfluorodimethylcyclohexane, perfluoromethylcyclohexane,
octafluorodecalin and
1,1,2-trichloro-l,2,2-trifluoroethane.
Out of these solvents, alcohols, glycol ethers, ethylene glycol alkyl ether acetates, propylene glycol alkyl ether acetates, ketones, esters and diethylene glycols are preferred from the viewpoints of solubility, reactivity with . each component and ease of forming a coating film.
Further, a high-boiling solvent may be used in combination with the above solvent. Examples of the high-boiling solvent include N-methylformaimide, N,N-dimethylformamide, N-methylformanilide, N-methylacetamide, N,N-dimethylacetamide,
N-methylpyrrolidone, dimethyl sulfoxide, benzyl ethyl ether, dihexyl ether, acetonyl acetone, isophorone, caproic acid, caprylic acid, 1-octanol, 1-nonanol, benzyl alcohol, benzyl acetate, ethyl benzoate, diethyl oxalate, diethyl maleate,
y-butyrolactone, ethylene carbonate, propylene carbonate and phenyl cellosolve acetate.
The refractive index changfing composition used in the present invention is molded into various shapes in consideration of application purpose before exposure to radiation. For example, it is molded like a rod, fiber, long

board, sphere, film or lens to which the present invention is not limited. A commonly used method may be used to mold the refractive in'dex changing composition of the present"" invention. For example, injection molding, compression molding, blow molding, extrusion, in-case frame polymerization, shaving, drawing, heating/cooling, CVD, sintering or scanning may be employed. According to the application purpose of an optically molded product, spin coating, slitting, bar coating, solvent casting, LB, spraying, roll coating, relief-printing or screen printing may also be used.
In this molding process, heating (to be referred to as "prebaking" hereinafter) is preferably carried out. The heating condition which changes according to the composition of the material of the present invention and the type of each additive is preferably 30 to 200°C, more preferably 40 to 150°C. A hot plate or oven, or infrared radiation may be used for heating.
The radiation used for exposure is an i-ray having a wavelength of 365 nm, h-ray having a wavelength of 404 nm, g-ray having a wavelength of 436 nm, ultraviolet radiation from a wide wavelength light source such as a xenon lamp, far ultraviolet radiation such as a KrF excimer laser beam having a wavelength of 248 nm or an ArF excimer laser beam having a wavelength of 193 nm, X-radiation such as synchrotron radiation, charged corpuscular beam such as electron beam, visible radiation or a mixture thereof. Out of these, ultraviolet radiation and visible radiation are preferred. The illuminance which depends on the wavelength of the radiation is preferably 0.1 to 100 mW/cm2 because the highest reaction efficiency is obtained. Exposure to the above radiation through a pattern mask makes possible the patterning of the radiation sensitive refractive index changing composition. As for patterning accuracy which is

affected by a light source used, an optical part having a refractive index changing distribution with a resolution of about'0.2 µm can be produted".
In the present invention, heating (to be referred to as "post-exposure baking (PEB)") is preferably carried out after exposure. A similar device to the above prebaking device may be used for PEB and PEB conditions may be arbitrary. The heating temperature is preferably 30 to 150°C, more preferably 30 to 130°C.
When the refractive index changing composition of the present invention does not contain the optional component (D), stabilization with the stabilizer (D) is then preferably carried out.
The stabilizer (D) used in the present invention has the function of stabilizing the residual decomposable compound (A) contained in the refractive index changing composition after exposure to provide stability to an acid or base. This stabilization prevents a change in refractive index and hence the deterioration of a refractive index pattern formed by the method of the present invention even when it is used under the condition that light having a wavelength close to the wavelength used to change the refractive index passes therethrough.
Examples of the above stabilizer (D) include an amino compound, epoxy compound, thiirane compound, oxetane compound, alkoxymethyl melamine compound, alkoxymethyl glycoluril compound, alkoxymethyl benzoguanamine compound, alkoxymethyl urea compound, isocyanate compound, cyanate compound, oxazoline compound, oxazine compound, halogenated silyl compound and other silyl compound.
Specific examples of these compounds are the same as those listed as the stabilizer (D) . Besides the above amino compounds, a low-boiling compound such as ammonia or trimethylamine may be used as the amino compound.

These stabilizers (D) may be used alone or in combination of two or more. The amount of the component (D) may be excessive so that the residual decomposable°Compound (A) can react to the full but it is generally 10 parts or more by weight, preferably 15 parts or more by weight based on 100 parts by weight of the component (A). When the amount of the component (D) is smaller than 10 parts by weight, the stability of the refractive index changing composition may become unsatisfactory due to an incomplete reaction.
A catalyst may be used in combination with the stabilizer (D). Use of the catalyst promotes a reaction between the component (D) and the residual decomposable compound (A).
Examples of the catalyst are the same as those listed as the catalyst for the stabilizer (D).
For contact between the refractive index changing composition after exposure to radiation and the stabilizer (D) for stabilization, a suitable method may be employed. For instance, the component (D) and optionally a catalyst are dissolved in a suitable solvent to be contacted to the refractive index changing composition as a solution. Alternatively, when the component (D) is liquid or gas under contact conditions, it may be 100 % directly contacted to the refractive index changing composition.
When a solvent is used in the reaction between the above stabilizer (D) and the component (A) , the solvent preferably dissolves the component '(D) and an optionally added catalyst and does not dissolve the component (A) . If the above solvent is selected, the surface of the obtained refractive index pattern will not be roughened.
Examples of the solvent include water; alcohols such as methanol, ethanol, iso-propanol, n-propanol, n-butanol, iso-butanol, tert-butanol, cyclohexanol, ethylene glycol, propylene glycol and diethylene glycol; ethers such as

diethyl ether and tetrahydrofuran; glycol ethers such as ethylene glycol monomethyl ether and ethylene glycol -monoethyl ether; ethylene glycol alkyl -ether acetates such -as methyl cellosolve acetate and ethyl cellosolve acetate; diethylene glycols such as diethylene glycol monomethyl ether, diethylene glycol monoethyl ether and diethylene glycol dimethyl ether; propylene glycol monoalkyl ethers such as propylene glycol methyl ether and propylene glycol ethyl ether; propylene glycol alkyl ether acetates such as propylene glycol methyl ether acetate and propylene glycol ethyl ether acetate; propylene glycol alkyl ether acetates such as propylene glycol methyl ether propionate, propylene glycol ethyl ether propionate, propylene glycol propyl ether propionate and propylene glycol butyl ether propionate; aromatic hydrocarbons such as toluene and xylene; aliphatic hydrocarbons such as n-hexane, n-heptane and n-octane; ketones such as methyl ethyl ketone, cyclohexanone, methyl isobutyl ketone, methylamyl ketone and 4-hydroxy-4-methyl-2-pentanone; esters such as ethyl acetate, propyl acetate, butyl acetate, ethyl 2-hydroxypropionate, methyl 2-hydroxy-2-methylpropionate, ethyl hydroxyacetate, butyl hydroxyacetate, ethyl lactate, propyl lactate, butyl lactate, methyl 3-hydroxypropionate, methyl 2-hydroxy-3-methylbutanoate, ethyl methoxyacetate, butyl methoxyacetate, ethyl 2-methoxypropionate, butyl 2-methoxypropionate, butyl 2-ethoxypropionate, butyl 2-butoxypropionate, butyl 3-methoxypropionate, butyl 3-ethoxypropionate, butyl 3-propoxypropionate and butyl 3-butoxypropionate; aprotic polar solvents such as dimethylformamide, dimethyl sulfoxide, dimethylacetamide and N-methylpyrrolidone; and fluorine atom-containing solvents such as trifluoromethylbenzene, 1,3-bis(trifluoromethyl)benzene, hexafluorobenzene, hexafluorocyclohexane, perfluorodimethylcyclohexane,

perfluoromethylcyclohexane, octafluorodecalin and 1,1,2-trichloro-l,2,2-trifluoroethane.
Out of these solvents, water, alcohols, glycol ethers, ethylene glycol alkyl ether acetates and fluorine atom-containing solvents are preferred.
The reaction temperature for carrying out a reaction between the stabilizer (D) and the residual decomposable compound (A) is generally 0 to 130** C, and the reaction time is generally 10 seconds to 1 hour.
When the refractive index changing composition of the present invention contains the stabilizer (D) as an optional component, heating is preferably carried out for stabilization, that is, a reaction between the residual component (A) and the component (D) successively after post-exposure baking or separately. The heating temperature for stabilization is preferably 35 to 200°C, more preferably a temperature 10°C or more higher than the PEB temperature, much more preferably a temperature 20°C or more higher than the PEB temperature.
Further, re-exposure may be carried out to decompose the residual component (C) existent in the unexposed portion and further improve the stability of the material.
For example, the re-exposure may be carried out by applying radiation having the Same wavelength as the radiation used to change the refractive index to the entire surface of the pattern in the same amount.
Optionally, heating may be further carried out to further improve the stability of the material. A similar device to the prebaking device used at the time of forming the material may be used for heating and the heating conditions may be arbitrary.
In the refractive index pattern formed as described above of the present invention, the refractive index of the exposed portion is higher than that of the unexposed portion.

This difference can be adjusted to a desired value by controlling the types and contents of the components (A) and (B) in the refractive index changing composition u'sed in the present invention. For example, the maximum value of refractive index difference can be adjusted to a value larger than 0.02.
The refractive index pattern of the present invention does not deteriorate as there occurs no change in refractive index even when it is used under the condition that light having a wavelength close to the wavelength used to change the refractive index passes therethrough as described above. Therefore, it is extremely useful as an optical material for use in optoelectronic and display fields.
Examples
The following examples are provided for the purpose of further illustrating the present invention but are in no way to be taken as limiting.
«
The weight average molecular weight in terms of polystyrene of each polymer was measured using the' GPC CHROMATOGRAPH SYSTEM-21 of Showa Denko K.K. Synthesis Examples of component (A) Synthesis Example 1 of component (A)
63.62 g of 3,3,4,4,5,5,5-heptafluoropentanaldehyde and 500 g of tetrahydrofuran were fed to a 1-liter flask whose inside had been substituted with nitrogen and cooled to -78°C. 0.64 g of a boron triflubride ether complex was added to the resulting solution and stirred in a nitrogen atmosphere at -78°C for 48 hours.
0.8 g of acetic anhydride and 0.6 g of pyridine were added to the obtained reaction solution while they were cooled and then stirred at -78°C for 2 hours. The reaction solution was wholly concentrated to 100 ml by heating at 60°C under reduced pressure and injected into 5 liters of ion exchange

water continuously in 10 minutes. The precipitate was re-dissolved in 50 parts by weight of tetrahydrofuran, purified by re-precipitation with 5- liters of fon exchange water and vacuum dried at 50°C to obtain 43.31 g of a polymer (A-1) • The weight average molecular weight of the obtained polymer was 2,700. Synthesis Example 2 of component (A)
A solution prepared by dissolving 83.08 g of hexafluoroglutaric acid dichloride in 400 ml of chloroform was fed to a 1-liter three-necked flask in an argon atmosphere, and a solution prepared by dissolving 18.62 g of ethylene glycol and 33.66 g of potassium hydroxide in 200 ml of ion exchange water was added to the above solution and stirred to carry out interfacial polycondensation. After 6 hours of the reaction, the reaction product was purified twice by re-precipitation with tetrahydrofuran-methanol.
The precipitated polymer was separated by filtration and vacuum dried at 50* C to obtain 59 .87 g of a polymer (A-2) . The weight average molecular weight of the obtained polymer was 16,700. Synthesis Example 3 of component (A)
50 parts by weight of o-phthalaldehyde and 500 parts by weight of tetrahydrofuran were fed as monomers to a 1-liter flask whose inside had been substituted with nitrogen and cooled to -78°C. 1.0 part by weight of an n-hexane solution of n-butyl lithium (1.5 mols/1) was added to this flask and stirred in a nitrogen atmosphere under cooling at -78°C for 48 hours.
0.8 part by weight of acetic anhydride and 0.6 part by weight of pyridine were added to the obtained reaction solution while they were cooled and then stirred at -78°C for 2 hours. The reaction solution was concentrated to 100 ml by heating at 60°C under reduced pressure and injected into 5 liters of ion exchange water in 10 minutes. The

precipitate was re-dissolved in 50 parts by weight of tetrahydrofuran, purified by re-precipitation with 5 liters of ion exchange warter and vacuum-dried at 50°C to obtain 45 parts by weight of a polymer (A-3). The weight average molecular weight of the obtained polymer was 26,000. Synthesis Example 4 of component (A)
61.51 g of terephthalic acid chloride was dissolved in 150 ml of chloroform in a 500-ml three-necked flask in an argon atmosphere. A solution prepared by dissolving 33.05 g of 1,4-benzenethiol and 33.66 g of potassium hydroxide in 150 ml of ion exchange water was added to the resulting solution and stirred to carry out interfacial polycondensation. After 6 hours of the reaction, the reaction product was purified twice by re-precipitation with tetrahydrofuran-methanol.
The precipitated polymer was separated by filtration and vacuum dried at 50°C to obtain 75 .98 g of a polymer {A-4) . The weight average molecular weight.of the obtained polymer was 33,600.
Synthesis Examples of Component (B) Synthesis Example 1 of component (B)
200 g of tetrabutoxytitanium was dissolved in 100 g of anhydrous toluene to prepare a solution which was then heated at 85°C. A mixed solution of 20.1 g of ion exchange water and 400 g of n-butyl alcohol was added dropwise to this solution at 85" C over 1 hour. After the end of addition, the resulting solution was 'further heated at 85°C for 3 hours under agitation. The thus obtained reaction solution was heated at 150" C under reduced pressure (0.1 mmHg) to distill off a volatile component. The weight average molecular weight of the obtained polymer (B-1) was 1,870. Synthesis Example 2 of component (B)
100 g of tetramethoxyzirconium was dissolved in 300 g of ethanol to prepare a solution which was then heated at

70°C, A mixed solution of 7 . 5 g of ion exchange water and 200 g of ethanol was added dropwise to this solution at 70" C over 1 hour. After the end of addition, the resulting solution was further heated at 70°C for 3 hours under agitation. The thus obtained reaction solution was heated at 150°C under reduced pressure (0.1 mmHg) to distill off a volatile component. The weight average molecular weight of the obtained polymer (B-2) was 1,360. Synthesis Example 3 of component (B)
100 g of tetramethoxygermanium was dissolved in 100 g of anhydrous toluene to prepare a solution which was then heated at 85°C. A mixed solution of 8.7 g of ion exchange water and 400 g of ethanol was added dropwise to this solution at 70°C over 1 hour. After the end of addition, the resulting solution was further heated at 70°C for 3 hours under agitation. The thus obtained reaction solution was heated at 150°C under reduced pressure (0.1 mmHg) to distill off a volatile component. The weight average molecular weight of the obtained polymer (B-3) was 1,510. Synthesis Example 4 of component (B)
15.22 g of tetramethoxysilane and 27.24 g of methyltrimethoxysilane were placed in a 1-liter three-necked flask, 100 g of ethylene glycol ethyl methyl ether was added to the flask to dissolve them, and the obtained mixed solution was heated at 60°C under agitation with a magnetic stirrer. 5.20 g of ion exchange water was continuously added to the mixed solution over 1 hour. After 4 hours of a reaction at 60°C, the obtained reaction solution was cooled to room temperature. Thereafter, 9.20 g of methanol which was a reaction by-product was distilled off from the reaction solution under reduced pressure. The weight average molecular weight of the obtained polymer (B-4) was 1,600. Example 1
50 parts by weight of the polymer (A-1) as the component

(A) , 50 parts by weight of the polymer (B-1) as the component
(B) and 1 part by weight of
2 - (4 -methoxyphenyl) -bis R , 6 - trichloromethyl) - s -friazine as the component (C) were dissolved in diethylene glycol ethy] methyl ether to a total solids content of 20 wt%, and the resulting solution was filtered with a membrane filter having an opening diameter of 0.2 µm to prepare a refractive index changing composition.
(1) formation of a coating film
The above solution was applied to a silicon substrate with a spinner and prebaked on a hot plate at 90°C for 2 minutes to form a 1.0 pm-thick coating film.
(2) formation of a refractive index pattern
The coating film obtained as described above was exposed to 100 mJ/cm2 of radiation with the NSR1505i6A reduction projection exposure device (of Nikon Corporation,
NA = 0.45, X = 365 nm) at the optimum focusing depth through a pattern mask. The coating film was then baked at 130°C for 2 minutes after exposure to form a refractive index pattern having a refractive index difference between exposed and unexposed portions. The exposed portion of the refractive index pattern formed herein will be referred to as "refractive index changed portion" and the unexposed portion will be referred to as "refractive index unchanged portion" hereinafter.
(3) measurement of refractive index
The refractive indices of the refractive index changed portion and the refraction index unchanged portion of the refractive index pattern formed above were measured at 633 nmwith the Auto EL IV NIR III ellipsometer (of Rudolf Research Co., Ltd.). The results are shown in Table 1.
(4) evaluation of transparency
A refractive index pattern was formed on a glass substrate in the same manner as in (1) and (2) except that

the Corning 1737 glass substrate (of Corning Co., Ltd.) was used in place of the silicon substrate. The exposed portion of the refractive index pattern formed on the glass substrate will be referred to as "refractive index changed portion" and the unexposed portion will be referred to as "refractive index unchanged portion" hereinafter as well.
Thereafter, the transmittances of the refractive index changed portion and the refractive index unchanged portion of the refractive index pattern formed on the glass substrate were measured at a wavelength of 400 to 800 nm with the 150-20 Double Beam spectrophotometer (of Hitachi, Ltd. ). When the minimum transmittance is higher than 95 %, the transmittance is satisfactory and when the minimum transmittance is 95 % or less, the transmittance is unsatisfactory. The results are shown in Table 1.
(5) stabilization
A 20 % dimethylformamide solution of 2,2,3,3,4,4,4-heptafluorobutyloxysilane (containing 10 mol% of tetrabutylammonium bromide) as the component (D) was heated at 100°C, and the refractive index patterns formed on the silicon substrate and the glass substrate as described above were immersed in the solution at 100°C for 2 minutes and then washed in super pure water for 1 minute.
Then, the entire surfaces of the patterns were re-exposed to 4 . 5 mW/cm2 of radiation using the Canon PLA-501F without a filter for 1 minute and heated in an oven at 200°C for 10 minutes to stabilize the refractive index patterns.
(6) evaluation of refractive index and transparency
The refractive indices of the refractive index changed portion and the refractive index unchanged portion of the above stabilized refractive index pattern formed on the silicon substrate were measured in the same manner as in (3) above. The results are shown in Table 2.
The transparencies of the refractive index changed

portion and the refractive index unchanged portion of the above stabilized refractive index pattern formed on the glass Substrate were measured in the same'manner" as in' (4) above. The results are shown in Table 2. (7) evaluation of stability of refractive index pattern
The entire surface of the above stabilized refractive index pattern formed on the silicon substrate and the entire surface of the above stabilized refractive index pattern formed on the glass substrate were exposed to 4.5 mW/cm2 of radiation for 30 minutes using the Canon PLA-50IF without a filter to carry out the acceleration of exposure to radiation.
The refractive indices of the refractive index changed portion and the refractive index unchanged portion of the thus treated refractive index pattern formed on the silicon substrate were measured in the same manner as in (3) above. The results are shown in Table 2.
The transparencies of the refractive index changed portion and the refractive index unchanged portion of the stabilized refractive index pattern formed on the glass substrate were measured in the same manner as in (4) above. The results are shown in Table 2, Example 2
Evaluations were carried out in the same manner as in Example 1 except that 50 parts by weight of the polymer (B-2) was used as the component (B), The results are shown in Table 1 and Table 2. Example 3
Evaluations were carried out in the same manner as in Example 1 except that 50 parts by weight of the polymer (A-2) was used as the component (A), 50 parts by weight of the polymer (B-3) was used as the component (B), 5 parts by weight of N-(2-nitrobenzyloxycarbonyl)pyrrolidine was used as the component (C) , the dose of radiation and the PEB temperature

in the step (2) (formation of a refractive index pattern) were changed as shown in Table 1, and the type of the component (D) and'the stabilization temperature in the step (5) (stabilization) were changed as shown in Table 2. The results are shown in Table 1 and Table 2. Example 4
Evaluations were carried out in the same manner as in Example 1 except that 50 parts by weight of the polymer (A-3) was used as the component (A), 50 parts by weight of the polymer (B-4) was used as the component (B), the dose of radiation and the PEE temperature in the step (2) (formation of a refractive index pattern) were changed as shown in Table 1, and the type of the component (D) in the step (5) (stabilization) was changed as shown in Table 2. The results are shown in Table 1 and Table 2. Example 5
Evaluations were carried out in the same manner as in Example 1 except that 50 parts by weight of the polymer (A-4) was used as the component (A), 50 parts by weight of the polymer (B-4) was used as the component (B), 5 parts by weight of N-(2-nitrobenzyloxycarbonyl)pyrrolidine was used as the component (C), the dose of radiation and the PEB temperature in the step (2) (formation of a refractive index pattern) were changed as shown in Table 1, and the type of the component (D) in the step (5) (stabilization) was changed as shown in Table 2. The results are shown in Table 1 and Table 2.





In Table 2, symbols for the component (D) denote the following.
D-1: 20 % dimethylformamide solution of 2,2,3,3,4,4,4-heptafluorobutyloxysilane (containing 10 mol% of tetrabutylammonium bromide) D-2: 1 % aqueous solution of ethylenediamine D-3: 20 % dimethylformamide solution of bisphenol A diglycidyl ether (containing 10 mol% of tetrabutylammonium bromide)
Since the refractive index pattern formed by the method of the present invention has a sufficiently large refractive index difference and the obtained refractive index difference is stable to light and heat, it is extremely useful as an optical material for use in optoelectronic and display fields. The refractive index pattern of the present invention is also used as an optical material for photoarrays, lenses, photocouplers, photointerruptors, polarization beam splitters, holograms, single-mode and- multi-mode optical fibers, bundled fibers, light guides, single-core, multi-core and photoelectrically coupling optical connectors, optical isolators, polarizers, optical sensors such as photodiodes, phototransistors, photo-ICs, CCD image sensors, CMOS image sensors, optical fiber sensors and optical fiber gyros, optical disks such as CD, LD, PD and DVD, optical switches, waveguides, optical touch panels, diffraction gratings, optical guide plates, optical diffusers, anti-reflectors and optical sealers.



CLAIMS
1. A composition comprising:
(A) a decomposable compound,
(B) a hydrolyzate of at least one compound selected from the group consisting of an alkoxide represented by the following formula (1'):
M(OR)n.Yn (1')
wherein M is a positive divalent to pentavalent atom, R is an alkyl group or aryl group, Y is a hydrogen atom, alkyl group, aryl group, hydroxyl group, alkoxyl group or aryloxy group, and m and n are each independently an integer of 0 or more, with the proviso that (m + n) is equal to the valence of M,
and a halogen compound represented by the following formula (2'):
MXmYn (2' )
wherein M, Y, m and n are as defined in the above formula (1'), and X is a halogen atom, and
(C) a radiation sensitive decomposer.
2. The composition of claim 1 which is a radiation sensitive refractive index changing composition.
3- The composition of claim 1 which further comprises (D) a stabilizer.
4. The composition of any one of claims 1 to 3, wherein
the refractive index nA of the component (A) and the refractive
index nB of the component (B) have the following relationship
(1):
ns - nA > 0.05 (1).
5. The composition of any one of claims 1 to 3, wherein

the refractive index HA of the component (A) and the refractive index nb of the component (B) have the following relationship (2):

6. The composition of any one of claims 1 to 5, wherein the decomposable compound (A) is a polymer having at least one of structures represented by the following formulas (1) to (7) and (8) to (11):

wherein R1 is an alkylene group, perfluoroalkylene group, alkylsilylene group, alkylene-arylene-alkylene group or arylene group, and R2 is an alkylene group, perf luoroalkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group or alkylgermylene group, with the proviso that the above alkylene group or perfluoroalylene group may contain a -0-, -CO-, -COO- or -OCOO- bond,

wherein M is Si or Ge, R3 is an alkylene group, perfluoroalkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group, alkylgermylene group or single bond, R4 is an oxygen atom, alkylene group, perf luoroalkylene group', alkylene-arylene-alkylene group, arylene group, alkylsilylene group or single bond, R5, R6, R7 and R8 are each independently a hydrogen atom, alkyl group, aryl group, alkoxyl group, thioalkyl group, alkoxyester group, perfluoroalkyl group, perfluoroalkoxyl group, perfluoroalkoxyester group or perfluoroaryl group, and m is an integer of 0 to 2, with the proviso that the above alkylene group or perfluoroalkylene group may contain a -0-, -CO-,


wherein M is Si or Ge, R3 is an alkylene group, perfluoroalkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group, alkylgermylene group or single bond, R4 is an oxygen atom, alkylene group, perfluoroalkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group or single bond, R5, R6, R7 and R8 are each independently a hydrogen atom, alkyl group, aryl group, alkoxyl group, thioalkyl group, alkoxyester group, perfluoroalkyl group, perfluoroalkoxyl group, perfluoroalkoxyester group or perfluoroaryl group, and m is an integer of 0 to 2, with the proviso that the above alkylene group or perfluoroalkylene group may contain a -0-, -CO-,


wherein R9 and R10 are each independently an alkylene group, perfluoroalkylene group, alkylene-arylene-alkylene group, arylene group, alkylsilylene group or alkylgermylene group, with the proviso that the above alkylene group or perfluoroalkylene group may contain a -0-, -CO-, -COO- or -OCOO- bond,

wherein R11 is an oxyalkylene group or single bond, and R12 is a hydrogen atom, alkyl group, alkoxyl group, alkoxyester group, perfluoroalkyl group, perfluoroalkoxyester group, perfluoroaryl group, alkylene-arylene-alkylene group or aryl group.


wherein R15, R16, R17 and R18 are each independently a hydrogen atom, chain alkyl group having 1 to 6 carbon atoms, chlorine atom,- bromine-atom, dodine. a-tom, hydroxyl group," mercapto ' group, carboxyl group, alkoxyl group having 1 to 6 carbon atoms, alkylthio group having 1 to 6 carbon atoms, haloalkyl group having 1 to 6 carbon atoms, haloalkoxyl group having 1 to 6 carbon atoms, haloalkylthio group having 1 to 6 carbon atoms, hydroxyalkyl group having 1 to 6 carbon atoms, mercaptoalkyl group having 1 to 6 carbon atoms, hydroxyalkoxyl group having 1 to 6 carbon atoms, mercaptoalkylthio group having 1 to 6 carbon atoms, aryl group having 6 to 10 carbon atoms or aralkyl group having 7 to 11


wherein R15, R16, R17 and R18 are each independently a hydrogen atom, chain alkyl group having 1 to 6 carbon atoms, chlorine atom, bromine-atom, iodi-ne atom,-hydroxyl group, mercapto group, carboxyl group, alkoxyl group having 1 to 6 carbon atoms, alkylthio group having 1 to 6 carbon atoms, haloalkyl group having 1 to 6 carbon atoms, haloalkoxyl group having 1 to 6 carbon atoms, haloalkylthio group having 1 to 6 carbon atoms, hydroxyalkyl group having 1 to 6 carbon atoms, mercaptoalkyl group having. 1 to 6 carbon atoms, hydroxyalkoxyl group having 1 to 6 carbon atoms, mercaptoalkylthio group having 1 to 6 carbon atoms, aryl group having 6 to 10 carbon atoms or aralkyl group having 7 to 11


wherein R28 is an alkylene group, aralkylene group or arylene group, and R29 is an alkylene group, aralkylene group, arylene group, alkylene-arylene-alkylene groups alkylsilylene group or alkylgermylene group,

wherein R32 and R33 are each independently an alkylene group, aralkylene group, arylene group, alkylene-arylene-alkylene group, alkylsilylene group or alkylgermylene group.
7. The composition of any one of claims 1 to 6, wherein
. the component (B) contains inorganic oxide particles in
addition to the above hydrolyzate.
8. A refractive index changing method comprising the step
of exposing the composition of any one of claims 1 to 3 to
radiation.
9. A refractive index pattern forming method comprising
the step of exposing part of the composition of any one of
claims 1 to 3 to radiation.
10. A refractive index pattern forming method comprising
the steps of exposing part of the composition of claim 1 or
2 to radiation and treating it with (D) a stabilizer.
11. A refractive index pattern forming method comprising

the steps of exposing part of the composition of claim 3 to radiation and treating it with (D) the stabilizer at a temperature at which the stabilizer can react with the decomposable compound (A).
12. The refractive index pattern forming method of any one of claims 9 to 11, wherein the maximum difference in refractive index between an exposed portion and an unexposed portion is 0.02 or more.
13. A refractive index pattern formed by the method of any one of claims 9 to 12,
14. An optical material formed by the method of any one of claims 9 to 12.

15. A composition substantially as herein described and exemplified.
16. An optical material substantially as herein described and exemplified.


Documents:

in-pct-2002-1858-che-abstract.pdf

in-pct-2002-1858-che-claims filed.pdf

in-pct-2002-1858-che-claims grand.pdf

in-pct-2002-1858-che-correspondnece-others.pdf

in-pct-2002-1858-che-correspondnece-po.pdf

in-pct-2002-1858-che-description(complete) filed.pdf

in-pct-2002-1858-che-description(complete) grand.pdf

in-pct-2002-1858-che-form 1.pdf

in-pct-2002-1858-che-form 18.pdf

in-pct-2002-1858-che-form 26.pdf

in-pct-2002-1858-che-form 3.pdf

in-pct-2002-1858-che-form 5.pdf

in-pct-2002-1858-che-other documents.pdf

in-pct-2002-1858-che-pct.pdf


Patent Number 208985
Indian Patent Application Number IN/PCT/2002/1858/CHE
PG Journal Number 38/2007
Publication Date 21-Sep-2007
Grant Date 16-Aug-2007
Date of Filing 13-Nov-2002
Name of Patentee JSR CORPORATION
Applicant Address 11-24, Tsukiji 2-chome Chuo-ku, Tokyo 104-0045
Inventors:
# Inventor's Name Inventor's Address
1 NISHIMURA, Isao c/o JSR Corporation 11-24, Tsukiji 2-chome Chuo-ku, Tokyo 104-0045
2 KUMANO ATSUSHI C/O JSR CORPORATION 11-24, TSUKIJI 2 CHOME, CHUO-KU, TOKYO 104-0045
3 BESSHO NOBUO C/O JSR CORPORATION 11-24, TSUKIJI 2 CHOME, CHUO-KU, TOKYO 104-0045
4 YAMANDA KENJI RESIDENCE SANKYO 501, 8-122-1, FUKAKUSANISHIURA-CHO, FUSHIMI-KU, KYOTO-SHI, KYOTO 612-0029
PCT International Classification Number C08L101/00
PCT International Application Number PCT/JP02/02178
PCT International Filing date 2002-03-08
PCT Conventions:
# PCT Application Number Date of Convention Priority Country
1 2001-70151 2001-03-13 Japan