Radiation-sensitive composition with variable refraction coefficient

FIELD: optical materials.

SUBSTANCE: invention relates to radiation-sensitive compositions with variable refraction coefficients allowing novel model with refraction coefficient distribution to be obtained, in particular optical material used in optical electronics and information representation devices. Invention discloses emission-sensitive composition with variable dielectric permittivity containing decomposable compound (A), non-decomposable component (B) including inorganic oxide particles resistant to acid or base originated from acid or base source (C), and radiation-sensitive degradable substance (C), wherein refraction coefficient nA of decomposable compound A and refraction coefficient nB of non-decomposable compound B lie in one of following relationships: nB-nA ≥ 0.05 (1) and nA-nB ≥ 0.05 (2), amount of component B ranges from 10 to 90 wt parts based on 100 wt parts of summary amount of components A and B, and amount of component C ranges from 0.01 to 30 wt parts based on 100 wt parts of summary amount of components A and B. Model obtained from indicated composition allows one to vary in a simple way refraction coefficients thereby achieving sufficiently large difference between them and their stability irrespective of application conditions.

EFFECT: expanded possibilities in optical representation of information.

12 cl, 3 tbl, 7 ex

 

The technical field

The present invention relates to sensitive to irradiation of the composition, changing the refractive index, the method of changing the refractive index, to a method of forming a model of the distribution of the refractive index with respect to the model distribution of the refractive index and the optical material. In particular, this invention relates to a method of forming a model of the distribution of refractive index, allowing to obtain a new model of distribution of refractive index, and optical material intended for use in the field of optoelectronics and display devices, the method of changing the refractive index and sensitive to the irradiation of the composition, changing the refractive index, which is designed for use in the above methods.

Background of the invention

In modern society, referred to as "media society", there is a great need in the molded optical products with the distribution of values of the refractive index, having areas with different refractive indices. These products are not only optical fibers used to transmit information, but also the optical diffraction grating with a periodic change of refractive index, optical device stored the I information in which information is stored in areas with different refractive indices, the elements with optical connection, such as optical IC having the fine structure of the distribution of refractive index, optical control elements of the optical modulation element and the optical transmission elements.

Optical molded products with the distribution of refractive indices fall into two types: the first type are molded products with a continuous distribution of refractive indices, such as optical fiber GI-type (hereinafter referred to as "optical molded products GRIN"), and the second type consists of products with intermittent distribution of refractive indices, such as optical diffraction gratings and optical waveguides SI-type.

Optical molded products are particularly attractive GRIN optical molded products of the next generation. For example, optical fiber GI-type, in which the refractive index decreases from the Central axis of the core of the optical fiber to the periphery according to the parabolic law, can transfer a large amount of information. The GRIN lens with a continuous change in the refractive index is used as a reading lens in copiers, spherical lens for connection of the fibers or of the microlenses is, the basis of its application are such distinctive features as the presence of refractive ability even on a flat surface and the absence of spherical aberration.

By this time developed many ways of obtaining optically molded products GRIN. For example, in patent applications JP-A 9-133813, JP-A 8-336911, JP-A 8-337609, JP-A 3-192310, JP-A 5-60931 (the term "JP-A" used herein the value means "unexamined published patent application of Japan"), WO 93/19505 and WO 94/04949 described method of obtaining an optical fiber GI-type dispersing a low-molecular compound or monomer in the polymer with a continuous distribution of concentrations. In the application JP-A 62-25705 describes a method for prochorenko optically molded product of the GI-type optical fiber photodepolymerization two or more vinyl monomers with different refractive indices and constants copolymerization. Further, in the application JP-A 7-56026 describes how the distribution of refractive indices, which includes obtaining a polymer And having photoreactivation functional group, the dispersion connection with a lower refractive index than the polymer A, the polymer And the concentration distribution connection and implementation of photochemical vzaimodeystviya polymer And compound Century

In addition to the CSO, proposed some methods for obtaining optically molded products GRIN from inorganic materials. One of such methods is, for example, a method of producing rod GI-type, which includes an introduction providing a high refractive index of thallium in prodiamesinae glass, consisting mainly of silicon or lead, immersing the glass in a molten solution containing potassium with low refractive index, and education distribution of the concentrations of potassium by means of ion exchange.

The GRIN lens can be obtained similarly to the above described method, using a short rod, that is, the lens is optically molded product. Alternatively, the rod GI-type, obtained as described above, can be cut into pieces.

One way of obtaining optically molded product with a microstructured model the distribution of the refractive index, such as the above-mentioned optical diffraction grating or optical IP is a known technology changes the refractive index by means of photochemical reactions in the molded product under the action of light irradiation. For example, in the case of inorganic material is glass doped with germanium, is exposed to light, resulting in a change in the refractive index of washes the VA with the formation of the optical diffraction grating. The above technology is applied to an organic substance known as photochromic reaction or whitening. In the application JP-A 7-92313 described the technology of optical diffraction grating as a result of changes of the refractive index under the action of the laser beam in the material containing dispersed in a polymer of low molecular weight compound which has a photochemical reactivity. Further, in the application JP-A 9-178901 recently it was proposed to apply the above technique for obtaining optically molded product GRIN. This method provides a continuous distribution of refractive indices inside the product relative to the direction of irradiation, by using the fact that is the absorption of light radiated on the molded product, and the weakening of its intensity.

However, in the distribution of refractive indices, and it does so in the above known materials, the maximum difference in refractive indices is only about 0,001-0,02, and it is difficult to achieve a wider distribution of refractive indices to prevent optical loss and suppress malfunction of the schema.

If, after the distribution of the refractive indices of the above known materials are used in conditions responsive the Oia through them the light wave, the length of which is close to the wavelength used to change the refractive index, there is a gradual change in the refractive index, which cannot be prevented, which leads to deterioration of the quality of materials.

The problem solved by this invention

The present invention is made considering the above situation, existing in this field of technology.

That is the purpose of the present invention is to create a model of the distribution of refractive index and optical material, which can be a simple way to change the refractive index, thus achieving a large enough difference between them and their stability regardless of the conditions after the formation of the model of the distribution of refractive index, and a new way of distribution of refractive indices.

Other objectives and advantages of the present invention will be apparent from the following description.

Tools solve this problem

The above objectives and advantages of the present invention are achieved, first, by creating sensitive to the irradiation of the composition, changing the refractive index, which contains (A) degradable compound, (B) non-biodegradable component containing particles of inorganic oxide, and (C) sensitive to radiation corrosive substance./p>

Secondly, the above objectives and advantages of the present invention are achieved by changing the refractive index, which is sensitive to the irradiation of the composition of the present invention, changing the refractive index, are irradiated.

Thirdly, the above objectives and advantages of the present invention are achieved by means of the method of forming a model of the distribution of refractive index, which is that the exposure is subjected to some of the listed sensitive to the irradiation of the composition, changing the refractive index.

Fourthly, the above-mentioned objectives and advantages of the present invention are achieved through a model of the distribution of refractive index is formed using the above-mentioned method of forming a model of the distribution of refractive index.

Fifth, the above-mentioned objectives and advantages of the present invention are achieved through optical material formed by using the above-mentioned method of forming a model of the distribution of refractive index.

In the present invention, the term "model of distribution of refractive index" means a material with a distribution of refractive index, which consists of areas that differ from each other in refractive index.

All of the components changes the refractive index of the composition of the present invention are described in detail below.

(A) Degradable connection

Degradable compound (A)used in the present invention may be acidic or basic degradable compound whose refractive index is preferably equal to 1.7 or less. Srednevekovaja molecular weight degradable compounds (A) preferably equal 100-500000, more preferably 100-300000.

Acid degradable compound selected from compounds having at least one structure selected from the group comprising the structure represented by the following formulas (1)to(6) and (10). These compounds can be used individually or in combination of two or more compounds.

(In the formula (1) R1means alkylenes group, performancelevel group, alkylsilane group, alkylenediamines group or Allenova group, and R2means alkylenes group, performancelevel group, alkylenediamines group, Allenova group, alkylsilane group or alkylamino group, provided that the above Allenova group or performanceheavy group can have link-O-, -CO-, -COO - or-LLC-).

p> (In the formula (2) M stands for Si or Ge, R3means alkylenes group, performancelevel group, alkylenediamines group, Allenova group, alkylsilane group, alkylamino group or a simple bond, R4means an oxygen atom, alkylenes group, performancelevel group, alkylenediamines group, Allenova group, alkylsilane group or a simple bond, R5, R6, R7and R8independently mean a hydrogen atom, alkyl group, aryl group, CNS group, thioalkyl group, alkoxyimino group, performanceline group, performanceline group, performancevery group or bertorello group, and m means an integer from 0 to 2, provided that the above Allenova group or performanceheavy group can have link-O-, -CO-, -COO - or-LLC-).

(In the formula (3) R9and R10independently mean alkylenes group, performancelevel group, alkylenediamines group, Allenova group, alkylsilane group or alkylamino group, provided that the above Allenova group or performanceheavy group can have link-O-, -CO-, -COO - or-LLC-).

(In the formula (4) R11means oxyalkylene groups is or a simple link, and R12means a hydrogen atom, alkyl group, CNS group, alkoxyimino group, performanceline group, performancevery group, bertorello group, alkylenediamines group or aryl group).

(In the formula (5) R13means a hydrogen atom, alkyl group, CNS group, alkoxyimino group, performanceline group, performanceline group, performancevery group, bertorello group or aryl group).

(In the formula (6) R14means alkylenes group or a structure represented by the following formula (7), (8) or (9)).

(In the formula (7) R15, R16, R17and R18independently mean a hydrogen atom, chain alkyl group with 1-6 carbon atoms, chlorine atom, bromine or iodine, hydroxyl group, mercaptopropyl, carboxyl group, CNS group with 1-6 carbon atoms, alkylthiols with 1-6 carbon atoms, halogenation group with 1-6 carbon atoms, halogenalkyls group with 1-6 carbon atoms, halogenation with 1-6 carbon atoms, hydroxyalkyl group with 1-6 carbon atoms, mercaptoethanol group with 1-6 carbon atoms, hydroxyalkoxy group with 1-6 carbon atoms, markup is oakerthorpe with 1-6 carbon atoms, aryl group with 6-10 carbon atoms or aracelio group with 7 to 11 carbon atoms).

(In the formula (8) R19means alkylenes group).

(In the formula (9) R20means alkylenes group).

(In the formula (10) R21means alkylenes group, alkylenediamines group or Allenova group).

The main degradable compound selected from the group of compounds having at least one structure selected from the group comprising the structure represented by the following formulas (11)-(14). These compounds can be used individually or in combination of two or more compounds.

(In the formula (11) R22means alkylenes group, Aracinovo group or Allenova group, R23means alkylenes group, Aracinovo group, Allenova group, alkylenediamines group, alkylsilane group or alkylamino group, R24, R25, R26and R27independently mean a hydrogen atom, alkyl group, aryl group, CNS group or thioalkyl group, i and j independently denote 0 or 1).

(In the formula (12) R28means alkylenes group, alkylenes group or Allenova group, and R29means alkylenes group, Aracinovo group, Allenova group, alkylenediamines group, alkylsilane group or alkylamino group).

(In the formula (13) R30and R31independently mean akiyanova group, Aracinovo group, Allenova group, alkylenediamines group, alkylsilane group or alkylamino group).

(In the formula (14) R32and R33independently mean alkylenes group, Aracinovo group, Allenova group, alkylenediamines group, alkylsilane group or alkylamino group).

All of the above alkylenediamines groups have the structure represented by the following formula (15) or (16):

(In the formula (15) R34, R35, R36and R37independently mean a hydrogen atom, chain alkyl group with 1-6 carbon atoms or aryl group with 6-10 carbon atoms, R38, R39, R40and R41independently mean a hydrogen atom, chlorine or bromine, a hydroxyl group, mercaptopropyl, CNS group, thioalkyl group, alkylamino group, alkylthiomethyl group, aryl group, cyano, or nitro-group).

<> (In the formula (16) R42, R43, R44and R45independently mean a hydrogen atom, chain alkyl group with 1-6 carbon atoms or aryl group with 6-10 carbon atoms, R46, R47, R48, R49, R50, R51, R52and R53independently mean a hydrogen atom, chlorine or bromine, a hydroxyl group, mercaptopropyl, CNS group, thioalkyl group, alkylamino group, alkylthiomethyl group, aryl group, cyano, or nitro-group, and A1means-S-, -O-, -SO2-, -CO-, -COO-, -OCOO-, -CH2- or-C(R54)2- (R54means chain alkyl group with 1-6 carbon atoms)).

All of the above allenbyi groups independently have a structure represented by the following formula (17):

where R55-R62independently mean a hydrogen atom, a chlorine atom or bromine, a hydroxyl group, mercaptopropyl, CNS group, thioalkyl group, alkylamino group, alkylthiomethyl group, aryl group, cyano, or nitro-group, and2means-S-, -O-, -SO2-, -CO-, -COO-, -OCOO-, -CH2- or-C(R63)2- (R63means chain alkyl group with 1-6 carbon atoms).

All of the above alkylsilane groups independently have a structure represented by the following formula (18):

where R64, R65, R66and R67independently mean a hydrogen atom, chain alkyl group with 1-6 carbon atoms or aryl group with 6-10 carbon atoms, And3means, alkylenes group or Allenova group, and a represents an integer of 0 or 1.

All of the above alkylamino groups independently have a structure represented by the following formula (19):

where R68, R69, R70and R71independently mean a hydrogen atom, chain alkyl group with 1-6 carbon atoms or aryl group with 6-10 carbon atoms, And4means, alkylenes group or Allenova group, and b denotes an integer of 0 or 1.

All of the above alkylene group can be linear, branched or cyclic alkionovymi groups with 1-10 carbon atoms, and some of the hydrogen atoms in these groups may be substituted by a fluorine atom or some or all of the hydrogen atoms in these groups may be substituted by a chlorine atom or bromine, perforaciones group, a hydroxyl group, mercaptopropyl, thioalkyl group, CNS group, performanceline group, alkylamino group, alkylthiophenes group, performancereview group, a cyano or a nitro-group.

Alkyl g is the UPP all the above alkyl groups, CNS groups, thioalkyl groups, alkylamine groups and alkylthiophene groups may be linear, branched or cyclic alkyl group with 1-10 carbon atoms, and some of the hydrogen atoms in these groups may be substituted by a fluorine atom or some or all of the hydrogen atoms in these groups may be substituted by a chlorine atom or bromine, perforaciones group, a hydroxyl group, mercaptopropyl, thioalkyl group, CNS group, performanceline group, alkylamino group, alkylthiophenes group, performancereview group, a cyano, a nitro-group or aryl group.

All of the above perforazione group independently represent performancenow group, perforation group, performancesailing group or performatively group, and the fluorine atom in these groups may be substituted by a hydroxyl group, performanceline group, perforaciones group, performancereview group, a cyano or a nitro-group.

All of the above aryl groups independently are phenyl group, naftalina group, antarctilyne group or biphenylene group, and the hydrogen atom in these groups may be substituted by a chlorine atom or bromine, a hydroxyl group, mercaptopropyl, CNS GRU is sing, thioalkyl group, alkylamino group, alkylthiophenes group, a cyano or a nitro-group.

Ways to get acidic or basic degradable compounds having structures represented in the present invention by the above formulas (1)to(6) and (10), for example, in the form of repeating units, is already known.

Methods for obtaining compounds having a structure represented by the above formula (1)described in journal of Polymer Bull., 1, 199 (1978), application JP-A 62-136638, European patent EP 225545, U.S. patent No. 806597, applications JP-A 4-303843, JP-A 7-56354 and other sources.

Methods for obtaining compounds having a structure represented by the above formula (2)described in magazines Macromolecules 29, 5529 (1996), Polymer 17, 1086 (1976), application JP-A 60-37549 and other sources.

Methods for obtaining compounds having a structure represented by the above formula (3)described in magazines 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 other sources.

Methods for obtaining compounds having a structure represented by the above formula (4)described in U.S. patent No. 3894253, applications JP-A 62-190211, JP-A 2-146544, Macromol. Chem., 23, 16 (1957), the application JP-A 63-97945, journal of Polymer Sci., A-1, 8, 2375 (1970), U.S. patent No. 4247611, European patent EP 41657, applications JP-A 57-31674, JP-A 64-3647, JP-A 56-17345 and other sources.

Methods of obtaining joint is, having a structure represented by the above formula (5)described in magazines Prepr. Eur. Disc Meet. Polymer Sci., Strasbourg, p.106 (1978), Macromol. Chem., 179, 1689 (1978) and other sources.

Methods for obtaining compounds having a structure represented by the above formula (6)described in U.S. patent No. 3894253, 3940507, application JP-A 62-190211 and other sources.

Methods for obtaining compounds having a structure represented by the above formula (10)described in the journals 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, (997), Macromolecules, 21, 1925, (1998), Macromol. Chem. Rapid Commun., 11, 83 (1990) and other sources.

There are also known methods of obtaining basic degradable compounds having structures represented by these formulas (11)-(14), for example, in the form of duplicate links.

Methods for obtaining compounds having a structure represented by the above formula (11)described in magazines Macromol. Chem. Rapid Commun., 5, 151 (1984), Macromol. Chem., 189, 2229 (1988), Macromol. Chem., 187, 2525 (1986), Polym. J., 22, 803 (1990) and other sources.

Methods for obtaining compounds having a structure represented by the above formula (12)described in magazines 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 other sources.

Methods for obtaining compounds having a structure represented by the above formula (13), described in the journal J. Macromol. Sci. Chem., A9, 1265 (1975) and other sources.

Methods for obtaining compounds having a structure represented by the above formula (14)described in magazines Polym. Bull., 14, 85 (1985), Macromol. Chem., 189, 1323 (1988) and other sources.

Srednevekovaja molecular weight degradable compounds (A) preferably equal 100-500000, more preferably 100-300000.

The above degradable compounds (A) can be conveniently classified according to the magnitude of the refractive index, while the compound with at least one of the following structures (i)to(vii)is preferred as compounds with a refractive index of 1.5 or less.

(i) the Structure of formula (1)in which R1and R2independently mean alkylenes group, performancelevel group or alkylsilane group, provided that the above Allenova group or performanceheavy group can have link-O-, -CO-, -COO - or-LLC-.

(ii) the Structure of the formula (2), in which M stands for Si or Ge, R3means alkylenes group or performancelevel group, R4means alkylenes group, performancelevel group, alkylsilane group or a simple bond, R5, R6, R7and R8independently mean a hydrogen atom, alkyl group, CNS group, alkoxyamino g is the SCP, performanceline group, performanceline group, performancevery group or bertorello group, and m means an integer from 0 to 2, provided that the above Allenova group or performanceheavy group can have link-O-, -CO-, -COO - or-LLC-.

(iii) the Structure of the formula (3), in which R9and R10independently mean alkylenes group or performancelevel group, provided that the above Allenova group or performanceheavy group can have link-O-, -CO-, -COO - or-LLC-.

(iv) the Structure of the formula (4), in which R11means oxyalkylene group or a simple bond, and R12means a hydrogen atom, alkyl group, CNS group, alkoxyimino group, performanceline group, performancevery group or bertorello group.

(v) the Structure of the formula (5), in which R13means a hydrogen atom, alkyl group, CNS group, alkoxyimino group, performanceline group, performanceline group, performancevery group or bertorello group.

(vi) the Structure represented by formula (6).

(vii) the Structure of the formula (10), in which R21means alkylenes group.

Connection with at least one of the following structures (viii)to(xiv), is preferred as compounds with pok is an indicator of refraction greater than 1.5.

(viii) the Structure of formula (1)in which R1means alkylenes group, alkylenediamines group or Allenova group, and R2means alkylenes group, alkylenediamines group, Allenova group, alkylsilane group or alkylamino group.

(ix) the Structure of the formula (2), in which M stands for Si or Ge, R3means alkylenes group, alkylenediamines group, Allenova group, alkylsilane group or alkylamino group, R4means an oxygen atom, alkylenes group, alkylenediamines group, Allenova group or a simple bond, R5, R6, R7and R8independently mean a hydrogen atom, alkyl group, aryl group, CNS group or thioalkyl group, and m means an integer from 0 to 2.

(x) the Structure of the formula (3), in which R9and R10independently mean alkylenes group, alkylenediamines group, Allenova group, alkylsilane group or alkylamino group.

(xi) the Structure of the formula (4), in which R11means oxyalkylene group or a simple bond, and R12means a hydrogen atom, alkyl group, alkylenediamines group or aryl group.

(xii) the Structure of the formula (5), in which R13means a hydrogen atom, alkyl group or aryl which ing group.

(xiii) the Structure represented by formula (10).

(xiv) the Structure represented by the formula(11)-(14).

(B) non-biodegradable component comprising particles of an inorganic oxide

Non-biodegradable component (C) is the particles of the above-mentioned oxide or a combination of oxide particles and a binder. As the oxide particles can be used particles of conventional inorganic oxide. Non-biodegradable component is preferably resistant to acids or bases formed from sensitive to radiation present and degrades substance (S), which will be described below, does not absorb light in the wavelength range passing through the composition, and is characterized by high optical transparency. Oxide particles with a preferred value of refractive index is selected depending on the application.

Preferred examples of the oxide particles are oxides containing such an atom, 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 are oxides such as BeO, MgO, CaO, SrO, BaO, Sc2O3, Y2O3La2O3Ce2O3, Gd2O3, Tb2O3, Dy2O3, Yb2O3, Lu2O3, TiO2, ZrO2, HfO2, Nb2O5, MoO3WO3, ZnO, B2O3, Al O3, SiO2, GeO2, SnO2, PbO, Bi2O3or TeO2and complex oxides, including Al2O3-MgO, Al2O3-SiO2, ZnO-Y2O3, ZrO2-Ce2O3, ZrO2-TiO2-SnO2, TeO2-BaO-ZnO, TeO2-WO3Ta2O5, TeO2-WO3-Bi2O3, TeO2-BaO-PbO, CaO-Al2O3, CaO-Al2O3-BaO, CaO-Al2O3-Na2O, CaO-Al2O3-K2O, CaO-Al2O3-SiO2, PbO-Bi2O3-BaO, PbO-Bi2O3-ZnO, PbO-Bi2O3, PbO-Bi2O3-BaO-ZnO, PbO-Bi2O3-CdO-Al2O3, PbO-Bi2O3-GeO2, PbO-Bi2O3-GeO2-Tl2O, BaO-PbO-Bi2O3, BaO-PbO-Bi2O3-ZnO, Bi2O3-Ga2O3-PbO, Bi2O3-Ga2O3-CdO and Bi2O3-Ga2O3-(Pb,Cd)O.

The diameters of the particles of oxide, preferably, should be less than the wavelength of light passing through altering the refractive index of the composition of the present invention, and may be equal to, for example, 2 μm or less, preferably 0.2 μm or less, particularly preferably of 0.1 μm or less. When the particle diameter of more than 2 μm may deteriorate the transparency changes the refractive index of a composition or film obtained from such a composition can be characterized wrong with the standing surface.

Form oxide particles has no specific limitation, but it is preferable to essentially spherical shape, as in this case, the scattering of incident light is small.

Particles of the above oxides can be entered in contact with celanova binding agent, surface-active substance or a coordination compound, providing a coordinating effect on the metal atom forming the oxide, with the aim of changing their surfaces before using.

The binder is non-biodegradable compound that is resistant to acid or base and preferably has a high optical transparency.

Such non-biodegradable compound is an acrylic resin, resin-based, urethane resin-based complex polyester, resin-based polycarbonate, resin-based norbornene resin based on styrene, easy polyester-based sulfone, silicone resin, polyamide resin, polyimide resin, resin-based polysiloxane resin-based fluorine resin-based polybutadiene resin on the basis of simple vinyl ether resin based on vinyl ester or the like. Any preferred non-biodegradable compound can be selected depending on the refractive index used degradable connected to the I (A). To increase the difference between the refractive indices are non-biodegradable compounds and degradable compounds (A) can preferably be used non-biodegradable compound with an aromatic group, a halogen atom or a sulfur atom.

Typical examples of non-biodegradable compounds include the following compounds (values given in parentheses represent the values of the refractive indices measured with a directional radiation): polyvinylidene fluoride (1,42), polydimethylsiloxane (1,43), politicomilitary (1,44), polyoxypropylene (1,45), polivinilbutilovy ether (1,45), polivinilbutilovy ether (1,45), polyoxyethylene (1,46), polyvinylbutyral ether (1,46), polivinilbutilovy ether (1,46), polyvinilcelates ether (1,46), poly(4-methyl-1-penten) (of 1.46 to 1.47), butyrate cellulose acetate (1,46-1,49), poly(4-fluoro-2-trifloromethyl) (1,46), polivinilbutilovy ether (1,46), poly(vinyl-2-ethylhexyloxy ether) (1,46), polivinilbutilovy ether (1,46), poly(2-methoxyethylamine) (1,46), polymethylacrylate (1,46), polymethylacrylate (1,47), poly(tert-butylmethacrylate) (1,46), polivinilbutilovy ether (1,46), poly(3-ethoxypropylamine) (1,47), policycombinerparameters (1,47), polyvinylpyridine (1,47)the polyvinyl acetate (1,47), polivinilbutilovy ether (1,47), politicalit (1,47), a copolymer of ethylene and vinyl acetate (1,47-1,50), propionate (80-20% vinyl acetate) cellulose (1,47-1,49, propionate, cellulose acetate (1,47), benzyltoluene (1,47-1,58), phenol-formaldehyde resin (1,47 is 1.70), triacetate cellulose (about 1.47 to 1.48), polivinilbutilovy ether (isotactic) (1,47), poly(3-methoxypropylacetate) (1,47), poly(2-ethoxyethylacetate) (1,47), polymethylacrylate (about 1.47 to 1.48), polyisopropylene (1,47), poly(1-mission) (1,47), polypropylene (atactic, density 0,8575 g/cm3) (1,47), poly(vinyl sec-butyl ether) (isotactic) (1,47), politicallegal (1,47), polyoxyethyleneglycol (1,47), polytetramethylene of poliatilenaksidna (1,47), a copolymer of ethylene and propylene (EPR rubber) (about 1.47 to 1.48), polyhexamethylene (1,48), polyvinylformal (1,48), poly(2-foraminotomies) (1,48), polyisobutylcyanoacrylate (1,48), ethylcellulose (1,48), polyvinylacetal (1,48-1,50), cellulose acetate (1,48-1,50), tripropionin cellulose (1,48-1,49), Polyoxymethylene (1,48), polyvinyl butyral (1,48-1,49), poly(n-hexyllithium) (1,48), poly(n-butylmethacrylate) (1,48), polietilentireftalat (1,48), poly(2-ethoxyethylacetate) (1,48), polyoxyethyleneglycol (1,48), poly(n-propylbetaine) poliatilenglikola (1,48), poly(3,3,5-trimethylcyclohexylidene) (1,49), polimetilmetakrilat (1,49), poly(2-nitro-2-methylpropionitrile) (1,49), politicalinstability (1,49), poly(1,1-diarylpropionitrile) (1,49), polymethylmethacrylate (1,49), poly(2-decyl-1,3-butadiene) (1,49), polyvinyl alcohol (1,49-1,53), IU the acrylate of polietilenglikolya (1,49), poly(3-methylcyclohexylamine) (1,49), poly(cyclohexyl-α-ethoxyacrylate) (1,50), methyl cellulose (low viscosity) (1,50), poly(4-methylcyclohexylamine) (1,50), polydimethyldiallylammonium (1,50), polyurethane (1,50-1,60), poly(1,2-butadiene) (1,50), polyvinylformal (1,50), poly(2-bromo-4-trifloromethyl) (1,50), cellulose nitrate (1,50-1,51), poly(sec-butylα-chloroacrylate) (1,50), poly(2-heptyl-1,3-butadiene) (1,50), poly(ethyl-α-chloroacrylate) (1,50), poly(2-isopropyl-1,3-butadiene) (1,50), poly(2-methylcyclohexylamine) (1,50), polypropylene (density 0,9075 g/cm3) (1,50), polyisobutene (1,51), polybutylmethacrylate (1,51), poly(2-tert-butyl-1,3-butadiene) (1,51), polietilenglikolmonostearat (1,51), polycyclohexylene (1,51), poly(cyclohexanediol-1,4-dimethacrylate) (1,51), butyl rubber (unvulcanized) (1,51), polytetrahydrofuran (1,51), gutta-percha (β) (1,51), polyethylene ion meter (1,51), polyoxyethylene (molecular) (1,51-1,54), polyethylene (density 0,914 g/cm3) (1,51), (density of 0.94-0,945 g/cm3) (1,52-1,53), (density 0,965 g/cm3) (1,55), poly(1-methylcyclohexylamine) (1,51), poly(2-hydroxyethylmethacrylate) (1,51), polivinilacetat (1,51), polybutene (isotactic) (1,51), polivinilatsetat (1,51), poly(N-butylmethacrylate) (1,51), gutta-percha (α) (1,51), terpene resin (1,52), poly(1,3-butadiene) (1,52), shellac (1,51-1,53), poly(methyl-α-Chloraka ilat) (1.52m), poly(2-claritromicina) (1,52), poly-(2-diethylaminoethylmethacrylate) (1,52), poly(2-chlorocyclohexanone) (1,52), poly(1,3-butadiene) (35% CIS-form; 56% TRANS-form 1,5180; 7% of 1,2-configuration), natural rubber (1,52), polyalkylacrylate (1,52), polyvinyl chloride +40% dioctylphthalate (1,52), polyacrylonitrile (1,52), polymethacrylamide (1,52), poly(1,3-butadiene) (high content of CIS-configuration) (1,52), a copolymer of butadiene and Acrylonitrile (1,52), polyethylenepropylene (1,52), polyisoprene (1,52), hard polyester resin (50% styrene) (1,52-1,54), poly(N-(2-methoxyethyl)methacrylamide) (1,52), poly(2,3-dimethylbutadiene)metilius (1,53), a copolymer of vinyl chloride and vinyl acetate (95/5-90/10) (1,53-1,54), polyacrylic acid (1,53), poly(1,3-dichloropropionitrile) (1,53), poly(2-chloro-1-(chloromethyl)ethyl methacrylate) (1,53), polyacrolein (1,53), poly(1-vinyl-2-pyrrolidone) (1,53), hydrochloridebuy rubber (1,53-1.55V), nylon 6; nylon 6,6; nylon 6,10 (molded product) (1,53), a copolymer of butadiene and styrene (30% styrene) (1,53), a block copolymer of poly(cyclohexyl-α-chloroacrylate) (1,53), poly(2-chloroethyl-α-chloroacrylate) (1,53), a copolymer of butadiene and styrene (about 75/25) (1,54), poly(2-aminoheterocycles) (1,54), polyfurfuryl (1,54), polimetilmetakrilat (1,54), poly(1-phenyl-n-amylmetacresol) (1,54), poly(N-methylmethacrylate) (1,54), cellulose (1,54), polyvinyl chloride (1,54-1.55V), carbamidoformaldegid the Naya resin (1,54-1,56), poly(sec-butyl-α-bromacil) (1,54), poly(cyclohexyl-α-bromacil) (1,54), poly(2-bromatological) (1,54), policyidreference acid (1,54), Polubarinova acid (1,546), polyethylenepolyamines (1,55), poly(N-allylmethylamine) (1,55), poly(1-fenilatilmalonamid) (1,55), polyvinylformal (1,55), poly(2-vinyltetrahydrofuran) (1,55), poly(vinyl chloride) +40% tricresylphosphate (1,55), poly(p-methoxybenzylthio) (1,55), polyisopropylene (1,55), poly(p-isopropylthio) (1,55), polychloroprene (1,55-1,56), poly(oksietilenom-α-benzoate-ω-methacrylate) (1,56), poly(p,p'-xylylenediamine) (1,56), poly(1-federalmileagerate) (1,56), poly(p-cyclohexenylmethyl) (1,56), poly(2-fenilatilmalonamid) (1,56), poly(oxycarbonyl-1,4-phenylene-1-propyl) (1,56), poly(1-(o-chlorophenyl)ethyl methacrylate) (1,56), a copolymer of styrene and maleic anhydride (1,56), poly(1-phenylcyclohexylamine) (1,56), poly(oxycarbonyl-1,4-phenylene-1,3-dimethylbutylamine-1,4-phenylene) (1,57), poly(methyl-α-bromacil) (1,57), polybenzimidazole (1,57), poly(2-(phenylsulfonyl)the ethyl methacrylate) (1,57), poly(m-kizilmescit) (1,57), a copolymer of styrene and Acrylonitrile (about 75/25) (1,57), poly(oxycarbonyl-1,4-phenyleneisopropylidene-1,4-phenylene) (1,57), poly(o-methoxyphenylacetyl) (1,57), polyphenylmethyl (1,57), poly(o-kizilmescit) (1,57), polivalente (1,57), poly(2,3-dibromopropyl acrylat) (1,57), poly(oxycarbonyl-hydroxy-1,4-phenylene-1-methylethylidene-1,4-phenylene) (1,57), poly(oxy-2,6-dimethylphenyl) (1,58), polyoxyethylenesorbitan (amorphous) (1,58), polyethylene terephthalate (1,51-1,64), polyvinylether (1,58), poly(oxycarbonyl-1,4-familienbetrieben-1,4-phenylene) (1,58), poly(1,2-diphenyl-ethyl methacrylate) (1,58), poly(o-chlorobenzonitrile) (1,58), poly(oxycarbonyl-1,4-phenylene-second-butylidene-1,4-phenylene) (1,58), polyoxyethyleneglycol (1,58), poly(m-nitrobenzonitrile) (1,58), poly(oxycarbonyl-1,4-phenyleneisopropylidene-1,4-phenylene) (1,59), poly(N-phenylethyl)methacrylamide) (1,59), poly(4-methoxy-2-methylsterol) (1,59), poly(o-methylsterol) (1,59), polystyrene (1,59), poly(oxycarbonyl-1,4-phenyltrichlorosilane-1,4-phenylene) (1,59), poly(o-mitoxantron) (1,59), polydiphenylsiloxane (1,59), poly(oxycarbonyl-hydroxy-1,4-phenylaniline-1,4-phenylene) (1,59), poly(p-bromophenylacetate) (1,60), poly(N-benzylacrylamide) (1,60), poly(p-mitoxantron) (1,60), grades (1,60-1,63), polysulfide ("Thiokol") (1,6-1,7), poly-(o-chlorodiphenylmethane) (1,60), poly(oxycarbonyl-1,4-(2,6-dichloro)phenyleneisopropylidene-1,4-(2,6-dichloro)phenylene) (1,61), poly(oxycarboxylic(1,4-(3,5-dichloraniline)))polymethacrylates (1,61), poly(o-chloresterol) (1,61), poly(phenyl-α-bromacil) (1,61), poly(p-divinylbenzene) (1,62), poly(N-vinylphthalimide) (1,62), poly(2,6-dichlorostyrene) (1,62), poly(&x003B2; -naphthylmethyl) (1,63), poly(α-nattermannallee) (1,63), polysulfone (1,63), poly(2-venitien) (1,64), poly(α-naphthylmethyl) (1,64), poly(oxycarbonyl-1,4-phenylendiamin-methylene-1,4-phenylene) (1,65), polyphenylenesulfide (1,66), butylbenzaldehyde resin (1,66), carbamidomethylation resin (1,66), polivinildeftorid (1,68), polyvinylcarbazole (1,68), naphthaleneformaldehyde resin (1,70), phenol-formaldehyde resin (1,70) and polypentaerythritols (1,71).

Non-biodegradable compound may be a copolymer of two or more monomers forming the above connection.

Srednevekovaja molecular mass of non-biodegradable compounds preferably equal 100-500000, more preferably 100-200000.

The above non-biodegradable compounds can be used individually or in combination of two or more compounds.

Non-biodegradable compound is used in a quantity of preferably 300 wt. parts or less, more preferably 150 wt. parts or less per 100 wt. parts of particles of inorganic oxide.

Particularly preferably, if the refractive index of nBcomponent (b) and the refractive index nAnddegradable compounds (A) are in one of the following relations (1) and (2).

The amount of component (C) is preferably 10-90 wt. parts, more preferably 20-70 wt. parts per 100 wt. parts of the total quantity of components (a) and (B). If the amount of component (C) is less than 10 wt. parts that change the refractive index of the material can become brittle, and if the specified number is greater than 90 wt. parts, the difference between the refractive indices may be insignificant.

(C) Sensitive to radiation corrosive substance

Sensitive to irradiation corrosive substance (S)used in the present invention, may be sensitive to radiation substance, giving acid, or sensitive to radiation substance, giving rise.

The above sensitive to radiation by a substance that produces acid is, for example, trichloromethyl-s-triazine, salt diarylethene, salt triarylsulfonium, Quaternary ammonium salt or an ester of sulfonic acid.

Examples of 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-triazine,

2-(2-chlorophenyl)-4,6-bis(trichloromethyl)-s-triazine,

2-(4-methoxyphenyl)-4,6-bis(trichloromethyl)-s-triazine,

2-(3-methoxyphenyl)-4,6-bis(trichloromethyl)-s-triazine,

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-methoxyethyl)-4,6-bis(trichloromethyl)-s-triazine,

2-(3-methoxyethyl)-4,6-bis(trichloromethyl)-s-triazine,

2-(2-methoxyethyl)-4,6-bis(trichloromethyl)-s-triazine,

2-(4-methoxy-β-styryl)-4,6-bis(trichloromethyl)-s-triazine,

2-(3-methoxy-β-styryl)-4,6-bis(trichloromethyl)-s-triazine,

2-(2-methoxy-β-styryl)-4,6-bis(trichloromethyl)-s-triazine,

2-(3,4,5-trimetoksi-β-styryl)-4,6-bis(trichloromethyl)-s-triazine,

2-(4-methylthio-β-styryl)-4,6-bis(trichloromethyl)-s-triazine,

2-(3-methylthio-β-styryl)-4,6-bis(trichloromethyl)-s-triazine,

2-(3-methylthio-β-styryl)-4,6-bis(trichloromethyl)-s-triazine,

2 piperonyl-4,6-bis(trichloromethyl)-s-triazine,

2-[2-(furan-2-yl)ethynyl]-4,6-bis(trichloromethyl)-s-triazine,

2-[2-(5-methylfuran-2-yl)ethynyl]-4,6-bis(trichloromethyl)-s-triazine and

2-[2-(4-diethylamino-2-were)ethynyl]-4,6-bis(trichloromethyl)-s-triazine.

Examples of the above salt diarylethene include

tetrafluoroborate diphenylethane,

hexaphosphate diphenylethane,

hexafluoroarsenate diphenylethane,

triftorbyenzola diphenylethane,

triptorelin diphenylethane,

p-toluensulfonate diphenylethane,

butyltin(2,6-differenl)borate diphenylethane,

p> exillis(p-chlorophenyl)borate diphenylethane,

exillis(3-triptoreline)borate diphenylethane,

tetrafluoroborate 4-methoxyphenylacetone,

hexaphosphate 4-methoxyphenylacetone,

hexafluoroarsenate 4-methoxyphenylacetone,

triftorbyenzola 4-methoxyphenylacetone,

triptorelin 4-methoxyphenylacetone,

p-toluensulfonate 4-methoxyphenylacetone,

butyltin(2,6-differenl)borate, 4-methoxyphenylacetone,

exillis(p-chlorophenyl)borate, 4-methoxyphenylacetone,

exillis(3-triptoreline)borate, 4-methoxyphenylacetone,

tetrafluoroborate bis(4-tert-butylphenyl)iodone,

hexafluoroarsenate bis(4-tert-butylphenyl)iodone,

triftorbyenzola bis(4-tert-butylphenyl)iodone,

triptorelin bis(4-tert-butylphenyl)iodone,

p-toluensulfonate bis(4-tert-butylphenyl)iodone,

butyltin(2,6-differenl)borate, bis(4-tert-butylphenyl)iodone,

exillis(p-chlorophenyl)borate, bis(4-tert-butylphenyl)iodone and

exillis(3-triptoreline)borate, bis(4-tert-butylphenyl)iodone.

Examples of the above salt triarylsulfonium include

tetrafluoroborate triphenylsulfonium,

hexaphosphate triphenylsulfonium,

hexafluoroarsenate triphenylsulfonium,

triftorbyenzola triphenylsulfonium,

triftoratsetata triphenylsulfonium,

p-toluensulfonate triphenylsulfonium,

butyltin(2,6-differenl)borate triphenylsulfonium,

exillis(p-chlorophenyl)borate triphenylsulfonium,

exillis(3-triptoreline)borate triphenylsulfonium,

tetrafluoroborate 4-methoxybenzenesulfonyl,

hexaphosphate 4-methoxybenzenesulfonyl,

hexafluoroarsenate 4-methoxybenzenesulfonyl,

triftorbyenzola 4-methoxybenzenesulfonyl,

triptorelin 4-methoxybenzenesulfonyl,

p-toluensulfonate 4-methoxybenzenesulfonyl,

butyltin(2,6-differenl)borate, 4-methoxybenzenesulfonyl,

exillis(p-chlorophenyl)borate, 4-methoxybenzenesulfonyl,

exillis(3-triptoreline)borate, 4-methoxybenzenesulfonyl,

tetrafluoroborate 4-phenyldiethanolamine,

hexaphosphate 4-phenyldiethanolamine,

hexafluoroarsenate 4-phenyldiethanolamine,

triftorbyenzola 4-phenyldiethanolamine,

triptorelin 4-phenyldiethanolamine,

p-toluensulfonate 4-phenyldiethanolamine,

butyltin(2,6-differenl)borate, 4-phenyldiethanolamine,

exillis(p-chlorophenyl)borate, 4-phenyldiethanolamine,

exillis(3-triptoreline)borate, 4-phenyldiethanolamine,

trattoria 4-hydroxy-1-naphthalenemethylamine,

hexaphosphate 4-hydroxy-1-naphthalenemethylamine,

hexafluoroarsenate 4-hydroxy-1-naphthalenemethylamine,

triftorbyenzola 4-hydroxy-1-naphthalenemethylamine,

triptorelin 4-hydroxy-1-naphthalenemethylamine,

p-toluensulfonate 4-hydroxy-1-naphthalenemethylamine,

butyltin(2,6-differenl)borate, 4-hydroxy-1-naphthalenemethylamine,

exillis(p-chlorophenyl)borate, 4-hydroxy-1-naphthalenemethylamine and

exillis(3-triptoreline)borate, 4-hydroxy-1-naphthalenemethylamine.

Examples of the above-mentioned Quaternary ammonium salt include

tetrafluoroborate of Tetramethylammonium,

hexaphosphate of Tetramethylammonium,

hexafluoroarsenate of Tetramethylammonium,

triftorbyenzola of Tetramethylammonium,

triptorelin of Tetramethylammonium,

p-toluensulfonate of Tetramethylammonium,

butyltin(2,6-differenl)borate of Tetramethylammonium,

exillis(p-chlorophenyl)borate of Tetramethylammonium,

exillis(3-triptoreline)borate of Tetramethylammonium,

tetrafluoroborate tetrabutylammonium,

hexaphosphate tetrabutylammonium,

hexafluoroarsenate tetrabutylammonium,

triftorbyenzola tetrabutylammonium,

triptorelin tetrabutylammonium,

p-toluensulfonate tetrabutylammonium,

butelli is(2,6-differenl)borate tetrabutylammonium,

exillis(p-chlorophenyl)borate tetrabutylammonium,

exillis(3-triptoreline)borate tetrabutylammonium,

tetrafluoroborate designed,

hexaphosphate designed,

hexafluoroarsenate designed,

triftorbyenzola designed,

triptorelin designed,

p-toluensulfonate designed,

butyltin(2,6-differenl)borate designed,

exillis(p-chlorophenyl)borate designed,

exillis(3-triptoreline)borate designed,

tetrafluoroborate of benzyldimethylamine,

hexaphosphate of benzyldimethylamine,

hexafluoroarsenate of benzyldimethylamine,

triftorbyenzola of benzyldimethylamine,

triptorelin of benzyldimethylamine,

p-toluensulfonate of benzyldimethylamine,

butyltin(2,6-differenl)borate of benzyldimethylamine,

exillis(p-chlorophenyl)borate of benzyldimethylamine,

exillis(3-triptoreline)borate of benzyldimethylamine,

tetrafluoroborate N-cinnamylpiperazine,

hexaphosphate N-cinnamylpiperazine,

hexafluoroarsenate N-cinnamylpiperazine,

triftorbyenzola N-cinnamylpiperazine,

t is itterated N-cinnamylpiperazine,

p-toluensulfonate N-cinnamylpiperazine,

butyltin(2,6-differenl)borate and N-cinnamylpiperazine,

exillis(p-chlorophenyl)borate and N-cinnamylpiperazine and

exillis(3-triptoreline)borate and N-cinnamylpiperazine.

Examples of the above complex ether sulfonic acids include

ether α-hydroxymethylbenzene-p-toluensulfonate acid,

ether α-hydroxyethylidenediphosphonic acid,

ether α-hydroxyethylmethylcellulose acid,

ether pyrogallol(p-toluensulfonate acid),

ether pyrogallol(triftormetilfullerenov acid),

ether piagetaltiplano.html acid,

ether 2,4-dinitrobenzyl-p-toluensulfonate acid,

ether 2,4-dinitrobenzenesulfonic acid,

ether 2,4-dinitrobenzenesulfonic acid,

ether 2,4-dinitrobenzyl-1,2-nattokinase-5-sulfonic acid,

ether 2,6-dinitrobenzyl-p-toluensulfonate acid,

ether 2,6-dinitrobenzenesulfonic acid,

ether 2,6-dinitrobenzenesulfonic acid,

ether 2,6-dinitrobenzyl-1,2-nattokinase-5-sulfonic acid,

ether 2-nitrobenzyl-p-toluensulfonate acid,

ether 2-nitrobenzenesulfonic acid,

ether 2-nitrobenzyl econsultancy acid,

ether 2-nitrobenzyl-1,2-nattokinase-5-sulfonic acid,

ether 4-nitrobenzyl-p-toluensulfonate acid,

ether 4-nitrobenzenesulfonic acid,

ether 4-nitrobenzenesulfonic acid,

ether 4-nitrobenzyl-1,2-nattokinase-5-sulfonic acid,

ether N-hydroxyphthalimide p-toluensulfonate acid,

ether N-hydroxyphthalimide triftormetilfullerenov acid,

ether N-hydroxyphthalimide methanesulfonic acid,

ester of N-hydroxy-5-norbornene-2,3-dicarboximide p-toluensulfonate acid,

ester of N-hydroxy-5-norbornene-2,3-dicarboximide triftormetilfullerenov acid,

ester of N-hydroxy-5-norbornene-2,3-dicarboximide methanesulfonic acid,

ether 2,4,6,3',4',5'-hexahydroxybenzene-1,2-nattokinase-4-sulfonic acid and

ether 1,1,1-three(p-hydroxyphenyl)ethane-1,2-nattokinase-4-sulfonic acid.

Of the above compounds are preferred trichloromethyl-s-triazine are the following connections:

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-β-styryl)-4,6-bis(trichloromethyl)-s-triazine,

2 piperonyl-4,6-bis(trasmital)-s-triazine,

2-[2-(furan-2-yl)ethynyl]-4,6-bis(trichloromethyl)-s-triazine

2-[2-(5-methylfuran-2-yl)ethynyl]-4,6-bis(trichloromethyl)-s-triazine,

2-[2-(4-diethylamino-2-were)ethynyl]-4,6-bis(trichloromethyl)-s-triazine and

2-(4-methoxyethyl)-4,6-bis(trichloromethyl)-s-triazine;

preferred salts diarylethene are the following connections:

triptorelin diphenylethane,

triftorbyenzola diphenylethane,

triftorbyenzola 4-methoxyphenylacetone and

triptorelin 4-methoxyphenylacetone;

preferred salts triarylsulfonium are the following connections:

triftorbyenzola triphenylsulfonium,

triptorelin triphenylsulfonium,

triftorbyenzola 4-methoxybenzenesulfonyl,

triptorelin 4-methoxybenzenesulfonyl,

triftorbyenzola 4-phenyldiethanolamine and

triptorelin 4-phenyldiethanolamine;

the preferred Quaternary ammonium salts are the following connections:

butyltin(2,6-differenl)borate of Tetramethylammonium,

exillis(p-chlorophenyl)borate of Tetramethylammonium,

exillis(3-triptoreline)borate of Tetramethylammonium,

butyltin(2,6-differenl)borate of benzyldimethylamine,

exillis(p-chlorophenyl)borate of benzyldimethylamine and

exillis(3-triptoreline)borate of benzyldimethylamine;

<> preferred esters of sulfonic acids are the following connections:

ether 2,6-dinitrobenzyl-p-toluensulfonate acid,

ether 2,6-dinitrobenzenesulfonic acid,

ether N-hydroxyphthalimide p-toluensulfonate acid and

ether N-hydroxyphthalimide triftormetilfullerenov acid.

As the above sensitive to radiation of a substance producing base, mainly used compounds described in application JP-A 4-330444, the journal "Polymer", pp.242-248, vol.46, No.6 (1997), and U.S. patent No. 627010. However, you can use any sensitive to radiation substance, giving rise, if this substance forms the base exposed.

Sensitive to radiation substance, forming the basis of the present invention is preferably optically active carbamate, such as triphenylmethanol, benzylcarbamoyl or antinormal; amide such as O-carbamoyltransferase, carbamoyloximes, aromatic sulfonamide, alpha-lactam, N-(2-allylamine)amide or other amide; ester of oxime, α-aminoacetophenone or the complex compound of cobalt.

Examples of sensitive to radiation substances forming the base include compounds represented by the following formulas(20)-(30):

where R72means an alkyl group with 1-6 carbon atoms, CNS group with 1-6 carbon atoms, thioalkyl group with 1-6 carbon atoms, dialkylamino with 1-6 carbon atoms, piperidino group, a nitrogroup, a hydroxyl group, mercaptopropyl, alkenylphenol or alkenylphenol group with 2-6 carbon atoms, aryl group with 6-20 carbon atoms, fluorine atom, chlorine or bromine, k is an integer from 0 to 3, R73means a hydrogen atom, alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms, R74and R75independently mean a hydrogen atom, alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms, aryl or benzyl group with 6-20 carbon atoms, or R74and R75can be connected to each other to form a cyclic structure having 5-6 carbon atoms;

where R76means an alkyl group with 1-6 carbon atoms, CNS group with 1-6 carbon atoms, thioalkyl group with 1-6 carbon atoms, dialkylamino with 1-6 carbon atoms, piperidino group, a nitrogroup, a hydroxyl group, mercaptopropyl, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or the aryl grupos 6-20 carbon atoms, R77means a hydrogen atom, alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms, R78and R79independently mean a hydrogen atom, alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms, aryl or benzyl group with 6-20 carbon atoms, or R78and R79can be connected to each other to form a cyclic structure having 5-6 carbon atoms;

where R80means an alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms, R81and R82independently mean a hydrogen atom, alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms, aryl or benzyl group with 6-20 carbon atoms, or R81and R82can be connected to each other to form a cyclic structure having 5-6 carbon atoms;

where R83and R84independently denote an alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms;

where R85 , R86and R87independently denote an alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms;

where R88means an alkyl group with 1-6 carbon atoms, CNS group with 1-6 carbon atoms, thioalkyl group with 1-6 carbon atoms, dialkylamino with 1-6 carbon atoms, piperidino group, a nitrogroup, a hydroxyl group, mercaptopropyl, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 atomania carbon, R89means a hydrogen atom, alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms, R90, R91and R92independently mean a hydrogen atom, alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms, aryl or benzyl group with 6-20 carbon atoms;

where R93means an alkyl group with 1-6 carbon atoms, CNS group with 1-6 carbon atoms, thioalkyl group with 1-6 carbon atoms, dialkylamino with 1-6 carbon atoms, piperidino group, a nitrogroup, a hydroxyl group, mercaptopropyl, alkenylphenol or alkenylphenol GRU is PU with 2-6 carbon atoms or aryl group with 6-20 carbon atoms, R94and R95independently mean a hydrogen atom, a hydroxyl group, mercaptopropyl, cyano, fenoxaprop, alkyl group with 1-6 carbon atoms, fluorine atom, chlorine or bromine, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms, R96and R97independently mean a hydrogen atom, alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms, aryl or benzyl group with 6-20 atomania carbon, or R96and R97can be connected to each other to form a cyclic structure having 5-6 carbon atoms;

where R98and R99independently denote an alkyl group with 1-6 carbon atoms, CNS group with 1-6 carbon atoms, thioalkyl group with 1-6 carbon atoms, dialkylamino with 1-6 carbon atoms, piperidino group, a nitrogroup, a hydroxyl group, mercaptopropyl, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms, R100-R103independently mean a hydrogen atom, a hydroxyl group, mercaptopropyl, cyano, fenoxaprop, alkyl group with 1-6 carbon atoms, fluorine atom, chlorine or bromine, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl GRU is PU with 6-20 carbon atoms, And5means a divalent aromatic, resulting from the removal of two hydrogen atoms attached to one or two nitrogen atoms of monoalkylamines, piperazine, aromatic diamine or aliphatic diamine;

where R104and R105independently denote an alkyl group with 1-6 carbon atoms, CNS group with 1-6 carbon atoms, thioalkyl group with 1-6 carbon atoms, dialkylamino with 1-6 carbon atoms, piperidino group, a nitrogroup, a hydroxyl group, mercaptopropyl, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms, R106and R107independently mean a hydrogen atom, a hydroxyl group, mercaptopropyl, cyano, fenoxaprop, alkyl group with 1-6 carbon atoms, fluorine atom, chlorine or bromine, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms, R108-R111independently mean a hydrogen atom, alkyl group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms, aryl or benzyl group with 6-20 carbon atoms, or R108and R109or R110and R111can be connected to each other to form a cyclic structure having 5-6 carbon atoms, and sup> 6means alkylenes group with 1-6 carbon atoms, cyclohexylamino group, fenelonov group or a simple bond;

where R112-R114independently mean a hydrogen atom, fluorine atom, chlorine or bromine, alkyl group with 1-6 carbon atoms, alkenylphenol group with 1-6 carbon atoms, alkylamino group with 1-6 carbon atoms, CNS group with 1-6 carbon atoms, alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms;

where L is at least one ligand selected from the group comprising ammonia, pyridine, imidazole, Ethylenediamine, trimethylenediamine, tetramethylaniline, hexamethylenediamine were, Propylenediamine, 1,2-cyclohexanediamine, N,N-diethylethylenediamine and Diethylenetriamine, n means an integer from 2 to 6, R115means alkenylphenol or alkenylphenol group with 2-6 carbon atoms or aryl group with 6-20 carbon atoms, and R116means an alkyl group with 1-18 carbon atoms.

In all the above formulas (20)-(30) alkyl group may be linear, branched or cyclic. Examples alkenylphenol group include vinyl group, and propylaniline group, and examples alkenylphenol groups include acetylenyl group. Examples of aryl groups include f is niloy group, naftalina group and antarctilyne group, and groups containing a fluorine atom, chlorine or bromine, halogenation group, hydroxyl group, carboxyl group, mercaptopropyl, a cyano, a nitro-group, asiagraph, dialkylamino, CNS group or thioalkyl group substituted by hydrogen atom present in the above groups.

From the above sensitive to radiation substances that form the basis of, preferred are 2-nitrobenzenesulfonate, triphenylmethanol, o-carbamoyltransferase, carbamoyloximes, [[(2,6-dinitrobenzyl)oxy]carbonyl]cyclohexylamine, bis[[(2-nitrobenzyl)oxy]carbonyl]hexane-1,6-diamine, 4-(methylthiomethyl)-1-methyl-1-morpholinoethyl, (4-morpholinomethyl)-1-benzyl-1-dimethylaminopropane, N-(2-nitro-benzyloxycarbonyl)pyrrolidin, Tris(triphenylmethyl) hexamine cobalt(III) and 2-benzyl-2-dimethylamino-1-(4-morpholinomethyl)butanone.

The above sensitive to radiation corrosive substance (C) is preferably used in an amount of 0.01 wt. part or more, more preferably in amounts of 0.05 wt. parts or more per 100 wt. parts of the total quantity of degradable compounds (A) and non-biodegradable compounds, including particles of inorganic oxide (B). If the amount of component (C) is less than 0.01 wt. part, is sensitive is to be irradiated may be insufficient. The upper limit is preferably 30 wt. parts, more preferably 20 wt. parts.

(D) a Stabilizer

Changing the refractive index of the composition according to 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, performs the function of stabilizing the residual degradable compound (A)contained in altering the refractive index of the material after exposure to him resistance to acid or base. This stabilization prevents the change of the refractive index and, consequently, deterioration of the model distribution of the refractive index obtained by the method according to the present invention, even when used in conditions of light with a wavelength close to the wavelength used to change the refractive index.

The above stabilisator (D) selected from the group including aminosilane, epoxy connection, the connection Tirana, the connection of oxetane, the connection of alkoxysilanes, the connection of alkoxyglycerols, the connection of alkoxybenzenes, the connection alkoxylation, the connection isocyanate compound cyanate, soedineniya oxazoline, with the Association of oxazine and silyl compound (halogenated silyl compound and other silyl connection).

Examples of the above amino compounds include triethylamine, Tripropylamine, tributylamine, triphenylamine, tridecylamine, tricyclohexyltin, triphenylamine, tribenzylamine, aniline, ethylendiamin, 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-diaminodecane, 1,12-diaminododecane, 1,4-diaminocyclohexane, 1,3-cyclohexanebis(methylamine), 1,3-propane-2-ol, 2,2',2"-trigeminothalamic, 1,4-diamino-2,2,3,3-tetraterpene, 1,5-diamino-2,2,3,3,4,4-hexafluoropentane, melamine, benzoguanamine, acetogenin, akilahanahid, paramin, amidol, m-phenylenediamine, p-phenylenediamine, p,p'-diaminodiphenylmethane, diaminodiphenylsulfone, 1,8-diaminonaphthalene, 3,5-diamino-1,2,4-triazole, 2-chloro-4,6-diamino-S-triazine, 2,6-diaminopyridine, 3,3'-diaminobenzidin, bis(4-aminophenoxy) ether, m-xylylenediamine, p-xylylenediamine, 1,2,4,5-benzylamine, 2,4-diamino-1,3,5-triazine, 4,4'-diaminobenzophenone, 3,3',4,4'-tetraaminobiphenyl, triaminobenzene, 4,4'-thiodianiline, 2,3,5,6-tetrabromo-p-xylylenediamine, 2,3,5,6-tetrachloro-p-xylylenediamine, 4,5-methylenedioxy-1,2-phenylenediamine and 2,2'-bis-(5-aminopyridin)sulfide.

Examples of the above epoxy compounds are bisphenol a epoxy resin, bisphenol F-epoxy resin, epoxyphenol bolacha resin, amoxicillinlavulanate resin, cyclic aliphatic epoxy resin, bisphenol a epoxy compound and aliphatic polyglycidyl ether.

Below are examples of commercial products, including the above compounds. Commercially produced products of bisphenol a-epoxy resin include Epicoat 1001, 1002, 1003, 1004, 1007, 1009, 1010 and 828 (Yuka Shell Epoxy Co., Ltd.), similar products bisphenol F-epoxy resin include Epicoat 807 (Yuka Shell Co., Ltd.), similar products epoxyphenolic resin include Epicoat 152 and 154 (Yuka Shell Epoxy Co., Ltd.) and EPPN201 and 202 (Nippon Kayaku Co., Ltd.), similar products amoxicillinlavulanate resin include EOCN-102, EOCN-103S, EOCN-104S, EOCN-1020, EOCN-1025 and EOCN-1027 (Nippon Kayaku Co., Ltd.) and Epicoat 180S75 (Yuka Shell Epoxy Co., Ltd.), similar products cyclic aliphatic epoxy resin include CY175, CY177 and CY179 (CIBA-GEIGY A.G.), ERL-4234, ERL-4299, ERL-4221 and ERL-4206 (U.C.C. Co., Ltd.), Showdyne 509 (a company Showa Denko K.K.), Araldyte CY-182, CY-192 and CY-184 (CIBA-GEIGY A.G.), Epichlon 200 and 400 (Dainippon Ink and Chemicals, Inc.), Epicoat 871 and 872 (Yuka Shell Epoxy Co., Ltd.), ED-5661 and ED-5662 (company Celanees Coating Co., Ltd.), and similar products of aliphatic polyglycidyl ether include Epolite 100MF (Kyoeisha Depending Co., Ltd.) and Epiol TMP (NOF Corporation).

In addition to the above compounds as epoxy compounds can be successfully used phenylglycyl levy ether, butespecially ether, 3,3,3-triftormetilfullerenov, stimulated, geksaftorpropilenom, cyclohexanone, N-gilderfluke, (nonfor-N-butyl)epoxide, performatively ether, epichlorohydrin, epibromohydrin, N,N-diglycidylether and 3-[2-(perferences)ethoxy]-1,2-epoxypropane.

Examples of the above compounds Tirana include compounds obtained by substitution epoxying groups in the above epoxy compounds group tylenchida, as described, for example, in the journal J. Org. Chem., 28, 229 (1963).

Examples of the above compounds oxetane include

bis[(3-ethyl-3-oxetanemethanol)methyl]benzene (trade name XDO, the production company Toagosei Chemical Industry Co., Ltd.),

bis[(3-ethyl-3-oxetanemethanol)were]methane,

bis[(3-ethyl-3-oxetanemethanol)methylphenylamine] ether

bis[(3-ethyl-3-oxetanemethanol)were]propane,

bis[(3-ethyl-3-oxetanemethanol)were]sulfon,

bis[(3-ethyl-3-oxetanemethanol)were]ketone,

bis[(3-ethyl-3-oxetanemethanol)were]hexaferrite,

three[(3-ethyl-3-oxetanemethanol)methyl]benzene and

Tetra[(3-ethyl-3-oxetanemethanol)methyl]benzene.

The above link alkoxysilanes, the connection of alkoxybenzenes, the connection of alkoxyglycerols and connection alkoxylation receive, replacing matilal the e group compounds methylaniline, connection methylolmethacrylamide, connection Meterological and connection metrologiya alkoxymethyl group. Type alkoxymethyl group has no specific limitation, and as an example of such a group can lead methoxymethyl group, ethoxymethyl group, propoxymethyl group and butoxymethyl group.

Commercially produced products of the above compounds include Simel 300, 301, 303, 370, 325, 327, 701, 266, 267, 238, 1141, 272, 202, 1156, 1158, 1123, 1170 and 1174, UFR65 and 300 (of Mitsui Cyanamid Co., Ltd.), Nicalak Mx-750, Mx-032, Mx-706, Mx-708, Mx-40, Mx-31, Ms-11 and Mw-30 (a company Sanwa Chemical Co., Ltd.).

Examples of the above isocyanate compounds include phenylene-1,3-diisocyanate, phenylene-1,4-diisocyanate, 1-methoxyphenyl-2,4-diisocyanate, 1-methylphenylene-2,4-diisocyanate, 2,4-tolylenediisocyanate, 2,6-tolylenediisocyanate, 1,3-xylylenediisocyanate, 1,4-xylylenediisocyanate, biphenylene-4,4'-diisocyanate, 3,3'-dimethoxybiphenyl-4,4'-diisocyanate, 3,3'-dimethylbiphenyl-4,4'-diisocyanate, difenilmetana-2,4'-diisocyanate, difenilmetana-4,4'-diisocyanate, 3,3'-dimethoxybiphenyl-4,4'-diisocyanate, 3,3'-dimethyldiphenyl-4,4'-diisocyanate, naphthalene-1,5-diisocyanate, CYCLOBUTANE-1,3-diisocyanate, cyclopentane-1,3-diisocyanate, cyclohexyl-1,3-diisocyanate, cyclohexyl-1,4-diisocyanate, 1-methylcyclohexane-2,4-diisocyanate, 1-methylcyclohexane-2,6-diisocyanate, 1-isocyanate-3,3,5-trimet is l-5-isocyanate, methylcyclohexane, cyclohexane-1,3-bis(methyl isocyanate), cyclohexane-1,4-bis(methyl isocyanate), isophorondiisocyanate, dicyclohexylmethane-2,4'-diisocyanate, dicyclohexylmethane-4,4'-diisocyanate, atlantaatlanta, tetramethylene 1,4-diisocyanate, hexamethylene-1,6-diisocyanate, dodecamethyl-1,12-diisocyanate, methyl ester lizenzierte and prepolymers having isocyanate groups at both ends, which are the result of the interaction of a stoichiometric excess of an organic diisocyanate and a bifunctional active hydrogen-containing compounds.

The above diisocyanate optional can be used in combination with an organic polyisocyanate having 3 or more isocyanate groups, such as phenyl-1,3,5-triisocyanate, difenilmetana-2,4,4'-triisocyanate, difenilmetana-2,5,4'-triisocyanate, triphenylmethane-2,4',4"-triisocyanate, triphenylmethane-4,4',4"-triisocyanate, difenilmetana-2,4,2',4'-tetrazocine, difenilmetana-2,5,2',5'-tetrazocine, cyclohexane-1,3,5-triisocyanate, cyclohexane-1,3,5-Tris(methyl isocyanate), 3,5-dimethylcyclohexane-1,3,5-Tris(methyl isocyanate), 1,3,5-trimethylcyclohex-hexane-1,3,5-Tris(methyl isocyanate), dicyclohexylmethane-2,4,2'-triisocyanate, dicyclohexylmethane-2,4,4'-triisocyanate or a prepolymer having a terminal isocyanate group, which is produced by the interaction of stechiometric the excessive amounts of organic MDI, containing 3 or more isocyanate groups, and a polyfunctional active hydrogen-containing compound having 2 or more hydrogen atom.

Examples of the above sanatoga compounds include 1,3-dicyanobenzene, 1,4-dicyanobenzene, 1,3,5-tricentrol, 1,3-, 1,4-, 1,6- 1,8-, 2,6- or 2,7-dilantinaugmentin, 1,3,6-tricentennial, 2,2'- or 4,4'-ditionality, bis(4-centopani)methane, 2,2-bis(4-centopani)propane, 2,2'-bis(3,5-dichloro-4-centopani)propane, 2,2-bis(4-centopani)ethane, bis(4-canadianguy) ether, BISM(4-canadianguy) thioether, bis(4-centopani)sulfon, 1,1,1,3,3,3-hexaplar-2,2-bis(4-centopani)propane, Tris(4-centopani)FOSFA, Tris(4-centopani)phosphonate and benzene multicore connection MDI obtained by the interaction of phenolic resins and halogenated cyanide (see, for example, application JP-B 45-11712 and JP-B 55-9433) (the term "JP-B" used here in the meaning means "the publication is considered Japan patent"). Especially preferred is a divalent connecting ether cyanic acid derived from a bisphenol such as 2,2-bis(4-centopani)propane, as this connection can easily be bought, it has excellent formability and reports required properties of the final otverzhdennom product. Policenet obtained as a result of interaction between the Oia initial condensate of phenol and formaldehyde with a halogen-containing CYANOGEN, also a useful connection.

Examples of the above compounds of oxazoline include

2,2'-bis(2-oxazoline),

4-furan-2-ylmethylene-2-phenyl-4H-oxazol-5-he,

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-(isopropyl-2-oxazoline-2-yl)pyridine,

2,2'-isopropylidenebis(4-tert-butyl-2-oxazoline),

2,2'-isopropylidenebis(4-phenyl-2-oxazoline),

2,2'-methylenbis(4-tert-butyl-2-oxazoline), and

2,2'-Methylenebis(4-phenyl-2-oxazoline).

Examples of the above compounds oxazine include

2,2'-bis(2-oxazin),

4-furan-2-ylmethylene-2-phenyl-4H-oksazil-5-he,

1,4-bis(4,5-dihydro-2-oxalyl)benzene,

1,3-bis(4,5-dihydro-2-oxalyl)benzene,

2,3-bis(4-Isopropenyl-2-oxazin-2-yl)butane,

2,2'-bis-4-benzyl-2-oxazin,

2,6-bis(isopropyl-2-oxazin-2-yl)pyridine,

2,2'-isopropylidenebis(4-tert-butyl-2-oxazin),

2,2'-isopropylidenebis(4-phenyl-2-oxazin),

2,2'-methylenbis(4-tert-butyl-2-oxazin) and

2,2'-Methylenebis(4-phenyl-2-oxazin).

Examples of the above halogenated silyl compounds include tetrachlorosilane, such as tetrachlorosilane, tetrabromide, tetraiodide, trichlorosilane and dichloropropylene; monoalkylammonium, such as methyltrichlorosilane, methyldichlorosilane and cycle hexyltrichlorosilane; monoacrylated, such as phenyltrichlorosilane, naphthylthiourea, 4-chlorophenyltrichlorosilane and phenyldichloroarsine; monohalomethanes, such as panaxytriol and PEROXYDICARBONATE; monoalkylation, such as metaxytherium and amoxicillan; dialkyldiphenyl, such as a clear, methyl(ethyl)DICHLOROSILANE and methyl(cyclohexyl)dichlorsilane; monoalkylammonium, such as methyl(phenyl)DICHLOROSILANE; diarylethylenes, such as diphenyldichlorosilane; dialogtitleversion, such as Diphenoxylate; monoaminooxidase, such as methyl(phenoxy)dichlorsilane; monoaminooxidase, such as phenyl(phenoxy)dichlorsilane; dialkoxybenzene, such as diethoxymethylsilane; monoaminooxidase, such as methyl(ethoxy)dichlorsilane; monoaminooxidase, such as phenyl(ethoxy)dichlorsilane; trialkylaluminium, such as trimethylchlorosilane, dimethyl(ethyl)chlorosilane and dimethyl(cyclohexyl)chlorosilane; dialkylaminoalkyl, such as dimethyl(phenyl)chlorosilane; monoalkylammonium, such as methyl(diphenyl)chlorosilane; triaminotrinitrobenzene, such as trigonometrician; monoacylglycerols the Ana, such as methyl(diphenoxy)chlorosilane; monocrystallization, such as phenyl(diphenoxy)chlorosilane; dialkylmonothiophosphinate, such as dimethyl(phenoxy)chlorosilane; diarylaminochloroquinones, such as diphenyl(phenoxy)chlorosilane; monoaminodinitrotoluenes, such as methyl(phenyl)(phenoxy)chlorosilane; triethoxyoctylsilane, such as triethoxysilane; and their oligomers, such as dimer, trimer, tetramer and pentamer of tetrachlorosilane.

Examples of the above other silyl compounds include hexamethyldisilazane, tert-butyldimethylchlorosilane, bis(trimethylsilyl)triptorelin, diethylaminocoumarin, trimethylsilanol, hexamethyldisiloxane, chlorotrimethylsilane, acetyltryptamine, ethoxytrimethylsilane, triphenylsilanol, triethylsilanol, Tripropylamine, tributyltin, hexaethyldisiloxane, trimethylboroxine, trimethylaluminium, triethylammonium, triethylaluminium, acetoxyisobutyryl, 1,3-bis(hydroxybutyl)tetramethyldisiloxane, 1,3-bis-(hydroxypropyl)tetramethyldisiloxane, γ-aminopropyltriethoxysilane, γ-aminopropyltriethoxysilane, N-β-(aminoethyl)-γ-aminopropyltrimethoxysilane, N-β-(aminoethyl)-γ-aminopropyltrimethoxysilane, N-phenyl-γ-aminopropyltrimethoxysilane, 3 -anilinopyrimidines, γ-dibutylaminoethanol, γ-ureidopropionic, hydrochloric N-β-(N-vinylbenzoate)-γ-aminopropyltrimethoxysilane, γ-methacryloxypropyltrimethoxysilane, γ-methacryloxypropyltrimethoxysilane, VINYLTRIMETHOXYSILANE, vinyltriethoxysilane, vinyltrichlorosilane, vinyltris(β-methoxyethoxy)silane, γ-glycidoxypropyltrimethoxysilane, γ-glycidoxypropyltrimethoxysilane, γ-(3,4-epoxycyclohexyl)ethyltrimethoxysilane, γ-glycidoxypropyltrimethoxysilane, γ-mercaptopropionylglycine, γ-chloropropionitrile, trimethylchlorosilane, hexamethyldisilazane, N-trimethylsilylimidazole, bis(trimethylsilyl)urea, trimethylsilylacetamide, bestemmelsessted, trimethylsilyltriflate, trimethyloxonium, trimethylaluminium, methyltrimethoxysilane, methyltriethoxysilane, dimethyldiethoxysilane, dimethyldiethoxysilane, tert-butyldimethylchlorosilane, tert-butyldiphenylchlorosilane, triisopropylchlorosilane, n-propyltrimethoxysilane, isobutyltrimethoxysilane, n-hexyltrimethoxysilane, n-decyltrimethoxysilane, n-hexadecyltrimethylammonium, 1,6-bis(trimethoxysilyl)hexane, dimethylimidazolidin, methicillinresistant, phenyltrimethoxysilane, diphenylimidazole and penicillinresistant.

The stabilizer is a torus (D) of the present invention preferably is aminosidine, epoxy connection, the connection Tirana, the connection of oxetane, the connection oxazoline, the connection of oxazine, silyl connection, the connection isocyanate or cyanate, more preferably aminosilane, epoxy connection, the connection Tirana, the connection of oxetane, the connection oxazoline or connection oxazine. Particularly preferred compounds are Ethylenediamine, phenylglycidyl ether, 3-phenoxypropionate, 3,3,3-triphosphorylated, hexamethyldisilazane, γ-aminopropyltriethoxysilane, γ-glycidoxypropyltrimethoxysilane or methicillinresistant.

These Stalinization (D) can be used individually or in combination of two or more compounds. The amount of component (D) may be redundant to ensure full interaction residual degradable compounds (A), but usually this amount is 10 wt. parts or more, preferably 30 wt. parts or more per 100 wt. parts component (A). If the amount of component (D) is less than 10 wt. parts, stability, altering the refractive index of the material may be unsatisfactory to sustainability due to incomplete interaction.

The stabilizer (D) can be used in combination with a catalyst. The catalyst promotes the interaction between the component (D) and the residual is m degradable compound (A).

The catalyst may be, for example, an acid catalyst, basic catalyst or Quaternary oneway salt.

Examples of the acid catalyst include organic acids such as acetic acid, methanesulfonate acid, p-toluensulfonate acid, triperoxonane acid and triftormetilfullerenov acid; and inorganic acids such as hydrochloric acid, sulfuric acid and nitric acid. Examples of the basic catalyst include carbonates of alkali metals such as sodium carbonate, potassium carbonate and lithium carbonate; bicarbonates of alkali metals such as sodium bicarbonate, potassium bicarbonate and lithium bicarbonate; acetates of alkali metals such as sodium acetate; hydrides of alkali metals such as lithium hydride, sodium hydride and potassium hydride; hydroxides of alkali metals such as sodium hydroxide, potassium hydroxide and lithium hydroxide; alkoxides of alkali metals such as sodium methoxide, ethoxide sodium tert-piperonyl potassium and lithium methoxide; mercaptomenthone metals, such as methylmercaptane and ethylmercaptan; 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]Nona-5-ene, 1,4-diazabicyclo[2.2.2]octane (DABCO) and 1,8-diaza icicle[5.4.0]undec-7-ene (DBU); connection alkylate, such as motility, utility and utility; and alkylamide lithium, such as diisopropylamide lithium and dicyclohexylamine lithium. Examples of the above-mentioned Quaternary oneway salts include tetrabutylammonium chloride, tetrabutylammonium bromide, tetrabutylammonium iodide, tetrabutylammonium acetate, chloride tetrabutylphosphonium, bromide tetrabutylphosphonium, bromide, cetyltrimethylammonium, bromide of tetrapropylammonium and chloride of benzyltriethylammonium. As the catalyst can also use a combination of 18-crown-6-ether and salts, such as potassium chloride, potassium bromide, potassium iodide, cesium chloride, phenoxide potassium, phenoxide sodium or potassium benzoate.

Of the above compounds, the preferred catalysts are p-toluensulfonate acid, hydrochloric acid, sulfuric acid, sodium hydroxide, tert-piperonyl potassium, triethylamine, DBU, tetrabutylammonium bromide, bromide tetrabutylphosphonium and 18-crown-6-ether/phenoxide potassium.

The amount of catalyst is preferably 2 mol or less per 1 equivalent of the compound (D)as component (D) use aminosidine, the connection of alkoxysilanes, the connection of alkoxyglycerols, the connection of alkoxybenzenes, the connection alkoxylation or halogenated silyl compounds is used.

Epoxy connection, the connection Tirana, the connection of oxetane, the connection isocyanate compound cyanate, connection oxazoline, the connection of oxazine or more silyl compound which is the component (D)is preferably used in an amount of 0.2 mol or less per 1 equivalent of the compound (D).

The number of equivalents of component (D) are obtained by multiplying the number of reactive groups present in component (D)amount (mol) of the component (D), and the number of reactive groups determined in the following way depending on the type of component (D).

aminosidine: the number of nitrogen atoms;

epoxy compound: number epoxying groups;

connection Tirana: number ethylenesulphonic groups;

connection oxetane: number oxetanyl groups;

connection alkoxysilanes, the connection of alkoxyglycerols, the connection of alkoxybenzenes and connection alkoxylation: number alkoxymethyl groups;

the isocyanate compound: number of isocyanate groups;

connection cyanate: number cyanotic groups;

connection oxazoline: number oxazolidine groups;

soedineniya of oxazine: number oxazoline groups;

connection sirgalahad: the number of atoms of halogen, associated with cu atoms is mnia;

other silyl compound: number of silicon atoms.

<Other components>

Changing the refractive index of the composition according to the present invention may contain other additives in amounts which do not prejudice the purposes of the invention. These additives include an absorber of ultraviolet rays, a sensitizer, a surfactant, a substance that improves the heat resistance and the adhesive.

The above absorber of ultraviolet rays is, for example, benzotriazole, salicylate, benzophenone, substituted Acrylonitrile, xanthene, coumarin, flavone or Halcon. Typical examples of the absorber of ultraviolet rays include Tinubin 234 (2-(2-hydroxy-3,5-bis-(α,α-dimethylbenzyl)phenyl)-2H-benzotriazole), Tinubin 571 (derived hydroxyphenylacetate) and Tinubin 1130 (the condensation product of methyl-3-(3-tert-butyl-5-(2H-benzotriazol-2-yl)-4-hydroxyphenyl)propionate and polyethylene glycol (molecular weight 300)) (Ciba Specialty Chemicals), 1,7-bis(4-hydroxy-3-methoxyphenyl)-1,6-heptadien-3,5-dione and dibenzylideneacetone.

Adding an absorber of ultraviolet rays, the amount of acid or base generated from the component (C)can be done gradually decreasing with increasing depth from the surface of the exposed part of changing the refractive index of the material on this is the invention, that allows you to effectively form a GRIN. The number of the absorber of ultraviolet rays is preferably 30 wt. parts or less, more preferably 20 wt. parts or less per 100 wt. parts of the total quantity of components (a) and (B).

The above sensitizer is, for example, coumarin, substituted in position 3 and/or position 7, Flavon, dibenzalacetone, dibenzyltoluene, Halcon, Xanten, thioxanthen, porphyrin, phthalocyanine, acridine or anthracene.

The amount of the sensitizer is preferably 30 wt. parts or less, more preferably 20 wt. parts or less per 100 wt. parts of the total quantity of components (a) and (B).

The above surfactant can be added to improve the covering ability, for example, to prevent banding or improve the ability to manifest.

Examples of surfactants include nonionic surfactants, such as polyoxyethylenesorbitan esters, including polyoxyethyleneglycol ether, polyoxyethyleneglycol ether and polyoxyethyleneglycol ether; polyoxyethylenesorbitan esters, including polyoxyethyleneglycol ether and polyoxyethyleneglycol ether; and dialkyl ethers of polyethylene glycol, including polietilenglikolmonostearat polietilenglikolmonostearat; fluorinated surfactant available commercially under the trade names F Top EF301, EF303 and EF352 (of Shin Akita Kasei Co., Ltd.), Megafac F171, F172 and F173 (Dainippon Ink and Chemicals, Inc.), Florade FC430 and FC431 (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 company Col., Ltd.); other surfactants that can be purchased commercially under the trade names: celexaorganon polymer KR (the company Shin-Etsu Chemical Co., Ltd.) and (co)polymer based on acrylic or methacrylic acid Polyflow No.57 and No.95 (Kyoeisha Depending Co., Ltd.).

The amount of surfactant is preferably 2 wt. parts or less, more preferably 1 wt. part or less per 100 wt. parts of the total quantity of components (a) and (B).

The above adhesive, which preferably is celanova binder, can be added to improve adhesion with the substrate.

The above substance, which improves the heat resistance, is an unsaturated compound, such as polyacrylate.

In changing the refractive index of the composition of the present invention can optionally also add an antistatic agent, protivookislitelnoj, inhibitor of halo, defoamer, pigment and thermosetting acid-forming substance.

<Formation of the s model of the distribution of refractive index>

In accordance with the present invention model the distribution of refractive index can be obtained, for example, as described below, of the above composition, altering the refractive index.

Changing the refractive index of the composition is first dissolved or dispersed in the solvent, thus obtaining a solution of a composition with a solids content of from 5 to 70 wt.%. The solution of the composition before application can optionally be filtered through a filter with a hole diameter of about 0.1-10 microns.

This solution composition is then applied to the surface of a substrate such as a silicon wafer, and subjected to preliminary hot drying to remove the solvent, thus obtaining the covering film material that changes refractive index. Part of the obtained coating film is then subjected to exposure through a template to build the model and fail drying after irradiation (ROAR), resulting in the difference between the refractive index in the irradiated and non-irradiated parts of the material, altering the refractive index.

Under the action of irradiation of sensitive to radiation present and degrades substance (S) formed by the acid or base, which have a corrosive impact on component (A). Subjected to decomposition product is removed in BP the two drying after irradiation. This results in a difference between the refractive index in the irradiated and non-irradiated parts.

The solvent used to obtain the solution containing altering the refractive index of the composition of the present invention, uniformly dissolves or disperses the above components (A), (b) and (C)optionally adding component (D) and other additives and does not interact with these components.

Examples of the solvent include alcohols such as methanol, ethanol, propanol, isopropanol, butanol, ethylene glycol and propylene glycol; ethers such as tetrahydrofuran; ethers of glycol, such as onomatology ether of ethylene glycol and monotropy ether of ethylene glycol; acetates Olkiluoto ether of ethylene glycol, such as methylcellosolve and ethylcellosolve; diethylenglycol, such as onomatology ether of diethylene glycol, monotropy ether of diethylene glycol, dimethyl ether of diethylene glycol, utilmately ether of diethylene glycol and diethyl ether of diethylene glycol; monoalkyl ethers of propylene glycol, such as methyl ether of propylene glycol, ethyl ether of propylene glycol, propyl ether of propylene glycol and butyl ether of propylene glycol; acetates Olkiluoto ether of propylene glycol, such as the acetate methyl ether of propylene glycol, ethyl acetate E. the Ira propylene glycol, acetate propyl ether of propylene glycol and acetate butyl ether of propylene glycol; acetates Olkiluoto ether of propylene glycol, such as propionate, methyl ether of propylene glycol, ethyl propionate ester of propylene glycol, propyl propionate ester of propylene glycol and propionate butyl ether of propylene glycol; 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, butyl acetate, ethyl-2-hydroxypropionate, methyl-2-hydroxy-2-methylpropionate, ethyl-2-hydroxy-2-methylpropionate, methylhydroxylamine, ethylhydroxylamine, butylhydroxyanisole, mutilated, ethyllactate, prophylactic, butylacetate, methyl-3-hydroxypropionate, ethyl-3-hydroxypropionate, propyl-3-hydroxypropionate, butyl-3-hydroxypropionate, methyl-2-hydroxy-3-methylbutanoate, methylmethacrylat, utilitarianist, propylenoxide, butylmethacrylate, methylationspecific, utilitarianist, populationsize, butylacetate, methylpropionate, ethylbromoacetate, profileproperties, buypropeciait, methylbutoxy, tivoconnect, papillomacular, butylmethacrylate, methyl-2-methoxypropionate, ethyl-2-methoxypropionate, propyl-2-methoxypropionate, butyl-2-methoxypropyl the NAT, methyl-2-ethoxypropionate, ethyl-2-ethoxypropionate, propyl-2-ethoxypropionate, butyl-2-ethoxypropionate, methyl-2-butoxypropyl, ethyl-2-butoxypropyl, propyl-2-butoxypropyl, butyl-2-butoxypropyl, methyl-3-methoxypropionate, ethyl-3-methoxypropionate, propyl-3-ethoxypropionate, butyl-3-methoxypropionate, methyl-3-ethoxypropionate, ethyl-3-ethoxypropionate, propyl-3-ethoxypropionate, butyl-3-ethoxypropionate, methyl-3-propoxyphene, ethyl-3-propoxyphenol, propyl-3-propoxyphenol, butyl-3-propoxyphenol, methyl-3-butoxypropan, ethyl-3-butoxypropan, propyl-3-butoxypropan and butyl-3-butoxypropan; and fluorine-containing solvents, such as triptoreline, 1,3-bis(trifluoromethyl)benzene, phenyl, hexaferrites, performatilicious, performatilicious, acceptancein and 1,1,2-trichloro-1,2,2-trifluoroethane.

Alcohols, ethers, glycol acetates Olkiluoto ether of ethylene glycol, acetates Olkiluoto ether of propylene glycol, ketones, esters and diethylenglycol preferably selected from the above solvents with regard to solubility, reactivity, in respect of each component, and ease of formation of a coating film.

In addition, in combination with the above solvent can be used a solvent with a high boiling point. PR is the measure of the solvent with a high boiling point include N-methylformamide, N,N-dimethylformamide, N-methylformamide, N-methylacetamide, N,N-dimethylacetamide, N-organic, dimethylsulfoxide, benzylation ether, directroy ether, acetonylacetone, isophorone, Caproic acid, Caprylic acid, 1-octanol, 1-nonanol, benzyl alcohol, benzoylacetate, ethylbenzoic, diethyloxalate, diethylmaleate, γ-butyrolactone, ethylene carbonate resulting, propylene carbonate and penisclotrimazole.

Changing the refractive index of the composition used in the present invention, molded, giving it a different shape depending on the purpose, and then subjected to irradiation. For example, such a composition is formed into a rod, fiber, long plate, sphere, film or lens, and the present invention is not limited to these forms. Changing the refractive index of the composition of the present invention can be molded by usual method. For example, for this purpose you can use injection molding, press-moulding, blow moulding, extrusion, polymerization in the form, stamping, stretching, heating/cooling, chemical deposition in the vapour phase (CVD), sintering or scanning. Depending on the destination optically molded product can also be used methods such as coating, deposition, longitudinal cutting, coating on the bar, forming dipping in rest the R, laser processing (LB), sputtering, coating roller, high printing or stencil printing.

While performing the above methods of forming the composition is preferably heated (this step is hereinafter referred to as "pre-drying"). The heating temperature, which varies depending on the composition of the present invention and the type of additives, is preferably 30-200°S, more preferably 40-150°C. For heating, you can use a hot stove, microwave or infrared radiation.

The composition is exposed to infrared rays with a wavelength of 365 nm, thermal rays with a wavelength of 404 nm, gamma-rays with a wavelength of 436 nm, ultraviolet rays from the light source with a broad wavelength range, such as a xenon lamp, short wave ultraviolet radiation such as a laser beam of KrF excimer with a wavelength of 248 nm or a laser beam of the excimer ArF with a wavelength of 193 nm, x-rays such as synchrotron radiation, charged particle beam such as an electron beam, visible light, or combinations thereof. Of the above impacts are preferred ultraviolet radiation and visible radiation. Illumination, which depends on the wavelength of the radiation, preferably 0.1-100 mW/cm2because when the uke is Anna illumination maximizes the efficiency of the reaction. The impact of the above-mentioned irradiation through the template to build the model allows to model the distribution of the refractive index is sensitive to the irradiation of the material, altering the refractive index. With regard to exactly model the distribution of the refractive index of the effect of light source used, the optical part with the distribution of different refractive indices can be obtained with a resolution of about 0.2 μm.

In accordance with the present invention, the heating (hereinafter referred to as "drying after irradiation (ROAR)") is preferably performed after irradiation. ROAR can be performed using a device similar to the device for predvaritelnoe drying, and randomly choose its execution environment. The heating temperature is preferably equal 30-150°S, more preferably 30-130°C.

If changing the refractive index of the composition according to the present invention does not contain an optional component (D), then preferably perform the stabilization of stabilization (D).

The stabilizer (D)used in the present invention, performs the function of stabilizing the residual degradable compound (A)contained in altering the refractive index of the composition after exposure to resistance to acid or base. Podobn what I stabilization prevents the change of the refractive index and, therefore, the deterioration model the distribution of the refractive index obtained by the method according to the present invention, even when in conditions of light with a wavelength close to the wavelength used to change the refractive index.

Examples of the above stabilizer (D) include aminosilane, epoxy connection, the connection Tirana, the connection of oxetane, the connection of alkoxysilanes, the connection of alkoxyglycerols, the connection of alkoxybenzenes, the connection alkoxylation, the connection isocyanate compound cyanate, soedineniya oxazoline, the connection of oxazine, halogenated silyl compound and other silyl connection.

Typical examples of such compounds similar to the above stabilizer (D). In addition to the above amino compounds can also be used aminosidine with a low boiling point, such as ammonia or triethylamine.

These stabilizers (D) can be used individually or in combination of two or more compounds. The amount of component (D) may be redundant to provide full interaction residual degradable compounds (A), but usually this amount is 10 wt. parts or more, preferably 15 wt. parts or more in the calculation is 100 wt. parts component (A). If the amount of component (D) is less than 10 wt. parts that change the refractive index of the material can be unstable due to incomplete interaction.

The stabilizer (D) can be used in combination with a catalyst. The catalyst promotes the interaction between the component (D) and residual degradable compound (A).

Examples of the catalyst is similar to the above for the catalyst described in connection with the stabilizer (D).

Changing the refractive index of the composition that has been subjected to irradiation, it is possible to enter into contact with the stabilizer (D) to stabilize any way you see fit. For example, the component (D) and optional catalyst are dissolved in an acceptable solvent for contact with changes the refractive index of the composition is in the form of a solution. Alternatively, if the component (D) is liquid or gas in terms of contact, it is possible to provide 100% direct contact with changes the refractive index composition.

When using a solvent in the process of interaction of the above stabilizer (D) and component (a) such a solvent should preferably dissolve the component (D) and optionally adding a catalyst and does not dissolve the component (A). If you select the above races is varicela surface of the resulting model of the distribution of refractive index is not rough.

Examples of the solvent include water; alcohols such as methanol, ethanol, isopropanol, n-propanol, n-butanol, Isobutanol, tert-butanol, cyclohexanol, ethylene glycol, propylene glycol and diethylene glycol; ethers, such as diethyl ether and tetrahydrofuran; ethers of glycol, such as onomatology ether of ethylene glycol and monotropy ether of ethylene glycol; acetates Olkiluoto ether of ethylene glycol, such as methylcellosolve and ethylcellosolve; diethylenglycol, such as onomatology ether of diethylene glycol, monotropy ether of diethylene glycol, and dimethyl ether of diethylene glycol; monoalkyl ethers of propylene glycol, such as methyl ether of propylene glycol, and ethyl ether propylene glycol; acetates Olkiluoto ether of propylene glycol, such as the acetate methyl ester of propylene glycol and acetate ethyl ether of propylene glycol; acetates Olkiluoto ether of propylene glycol, such as propionate, methyl ether of propylene glycol, ethyl propionate ester of propylene glycol, propyl propionate ester of propylene glycol and propionate butyl ether of propylene glycol; 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, methylmercaptan and 4-hydroxy-4-methyl-pentane; esters, such as ethyl acetate, propyl, butyl acetate, ethyl-2-hydroxypropionate, methyl-2-hydroxy-2-methylpropionate, ethylhydroxylamine, butylhydroxyanisole, ethyllactate, prophylactic, butylacetate, methyl-3-hydroxypropionate, methyl-2-hydroxy-3-methylbutanoate, utilitarianist, butylmethacrylate, ethyl-2-methoxypropionate, butyl-2-methoxypropionate, butyl-2-ethoxypropionate, butyl-2-butoxypropyl, butyl-3-ethoxypropionate, butyl-3-ethoxypropionate, butyl-3-propoxyphene and butyl-3-butoxypropan; fluorine-containing solvents, such as triptoreline, 1,3-bis(trifluoromethyl)benzene, phenyl, hexaferrites, performatilicious, performatilicious, acceptancein and 1,1,2-trichloro-1,2,2-triptorelin; and aprotic polar solvents such as dimethylformamide, dimethylsulfoxide, dimethylacetamide and N-organic.

Of the above preferred solvents are water, alcohols, ethers, glycol acetates Olkiluoto ether of ethylene glycol and fluorinated solvents.

The stabilizer (D) and residual razlogova compound (A) is subjected to interaction at the reaction temperature from 0 to 130°C, and the reaction time is usually from 10 seconds to 1 hour.

If changing the refractive index of the composition according to the present invention soda is incorporated stabilizer (D) as an optional component, the reaction mixture is preferably heated to stabilize the reaction between the residual component (a) and component (D), followed by drying after exposure or as a separate process. The temperature of the heating for stabilization is preferably 35-200°more preferably this temperature for 10°or more greater than the temperature ROAR, still preferable to the specified temperature at 20°or more greater than the temperature of the ROAR.

In addition, you can re-irradiation to decompose the residual component (S)not present in exposed parts, and further improve the stability of the material.

Re-irradiation can be performed at the same wavelength used for exposure, in order to change the refractive index, on the entire surface of the model and in the same amount.

To further enhance the stability of the material can be made optional heating. For heating, you can use a device similar to the device for pre-drying, used during molding material, and the heating conditions can be arbitrary. In this model, the distribution of refractive index according to the present invention, the refractive index of the exposed part of the above, h is m a refractive index portion, not subjected to irradiation. The specified difference can be increased to the required value by adjusting the types and content of the components (a) and (b) change in the refractive index of the material of the present invention. For example, the maximum value of the difference between the refractive index can be increased to a value of more than 0.02.

Since the model of the distribution of refractive index according to the present invention does not deteriorate as a result of changes in the refractive index even when in conditions of light with a wavelength close to the wavelength used to change the refractive index, as described above, the resulting material is extremely useful as an optical material intended for use in the field of optoelectronics and display data.

Examples

The following examples are given to further illustrate the present invention and do not limit its scope.

Srednevekovoy the molecular weight of all connections in the calculation of polystyrene measured by GPC chromatograph system-21 company Showa Denko K.K.

Examples of the synthesis of component (A)

Example 1 synthesis of the component (A)

63,62 g 3,3,4,4,5,5,5-getattributeid and 500 g of tetrahydrofuran is introduced into one litre flask filled with nitrogen and cooled to -78°C. To the resulting solution to relax the Ute 0.64 g of a complex of boron TRIFLUORIDE and an ether and stirred under nitrogen atmosphere at -78° With in 48 hours.

To the resulting reaction solution while cooling add 0.8 g of acetic anhydride and 0.6 g of pyridine and stirred at -78°C for 2 hours. The reaction solution is completely concentrated to 100 ml by heating at 60°With under reduced pressure, and continuously injected in 5 liters of ion exchange water for 10 minutes. The residue re-dissolved in 50 wt. parts of tetrahydrofuran, clean, making repeated sedimentation of 5 liters of ion-exchange water, and dried in vacuum at 50°thus 43,31 g of compound (a-1). Srednevekovaja molecular weight of the obtained compound of 2,700.

Example 2 synthesis of component (A)

The solution 83,08 g of the dichloride hexafluoro acid in 400 ml of chloroform administered in one litre three-neck flask in an argon atmosphere, the resulting solution was added a solution of 18,62 g of ethylene glycol and 33,66 g of potassium hydroxide in 200 ml of ion-exchange water and stirred for implementation of interfacial polycondensation. The reaction solution is subjected to interaction within 6 hours, and then double-cleanse, re-producing the deposition of a tetrahydrofuran-methanol.

The precipitated polymer is separated by filtration and dried in vacuum at 50°thus 59,87 g of compound (a-2). Srednevekovaja molecular mass of the obtained compound is 16700.

Example 3 synthesis of whom is Ananta (A)

50 wt. parts o-phthalaldehyde monomer and 500 wt. parts of tetrahydrofuran is introduced into one litre flask filled with nitrogen and cooled to -78°C. specified In the flask add 1.0 wt. part of the solution n-utility (1.5 mol/l) in n-hexane and stirred in a nitrogen atmosphere, cooling at -78°within 48 hours.

To the resulting reaction solution while cooling add to 0.8 wt. parts of acetic anhydride and 0.6. parts of pyridine and stirred at -78°C for 2 hours. The reaction solution is concentrated to 100 ml by heating at 60°With under reduced pressure, and injected in 5 liters of ion exchange water for 10 minutes. The residue re-dissolved in 50 wt. parts of tetrahydrofuran, clean, making repeated sedimentation of 5 liters of ion-exchange water, and dried in vacuum at 50°receiving, by weight, 45. parts of the compound (a-3). Srednevekovaja molecular mass of the obtained compound is 26000.

Example 4 synthesis of component (A)

61,51 g of the chloride of terephthalic acid is dissolved in 150 ml of chloroform in a 500 ml three-neck flask in an argon atmosphere. To the resulting solution was added a solution of 33,05 g of 1,4-bentolila and 33,66 g of potassium hydroxide in 150 ml of ion exchange water and stirred for implementation of interfacial polycondensation. The reaction solution is subjected to interaction within 6 hours, after which cleanse, p is Ozoda re-deposition of a tetrahydrofuran-methanol.

The precipitated compound is separated by filtration and dried in vacuum at 50°thus 75,98 g of compound (a-4). Srednevekovaja molecular weight of the obtained compound is equal to 33600.

Examples of the synthesis of the component (C)

Example 1 synthesis of the component (C)

39,66 g phenyltrimethoxysilane and 24,44 g diphenylmethylsilane dissolved in 100 g ethylmethylamino ether of ethylene glycol in one litre three-neck flask and the resulting solution was heated at 70°, stirring with magnetic stir bar. Within 1 hour the solution is continuously added 5.20 g of ion exchange water. The interaction is carried out at 70°C for 4 hours, after which the resulting reaction solution was cooled to room temperature. From the reaction solution under reduced pressure, distilled 9,20 g of methanol, which is a byproduct of the reaction. Srednevekovaja molecular weight of the obtained polymer (B-1) is equal to 1600. For a given polymer type 54,90 g of a solution of zirconium dioxide in methylethylketone (average particle diameter of 0.01 to 0.05 μm, the concentration of the zirconium dioxide is 30%). The solid content in the obtained mixed solution of particles of inorganic oxide (Bmix-1) is equal to 31.3 percent.

Example 2 synthesis of the component (C)

To the compound (B-1)obtained in synthesis example 1, add 54,90 g of the solution of titanium oxide in methyl ethyl ketone (medium is iameter particles is 0.01 to 0.5 μm, the concentration of titanium oxide is 30%). The solid content in the obtained mixed solution of particles of inorganic oxide (Bmix-2) is equal to 31.3 percent.

Example 3 synthesis of the component (C)

To the compound (B-1)obtained in synthesis example 1, add 54,90 g of the solution of tin oxide in methyl ethyl ketone (average particle diameter of 0.01 to 0.05 μm, the concentration by surimi is 30%). The solid content in the obtained mixed solution of particles of inorganic oxide (Bmix-3) is equal to 31.3 percent.

Example 4 synthesis of the component (C)

To the compound (B-1)obtained in synthesis example 1, add 54,90 g dispersed in methanol solution of aluminum oxide (average particle diameter equal 0,0015 is 0.003 μm, solid content is 30%, the water content is 5.6%). The solid content in the obtained mixed solution of particles of inorganic oxide (Bmix-4) is equal to 31.3 percent.

Example 5 synthesis of the component (C)

15,22 g tetramethoxysilane and 27,24 g methyltrimethoxysilane injected into one litre three-neck flask, dissolve these substances by adding 100 g ethylmethylamino ether of ethylene glycol, and the resulting mixed solution is heated at 60°, stirring with magnetic stir bar. In for 1 hour in a mixed solution is continuously added 5.20 g of ion exchange water. The interaction is carried out at 60°C for 4 h the owls, then the resulting reaction solution was cooled to room temperature. Then from the reaction solution under reduced pressure, distilled 9,20 g of methanol, which is a byproduct of the reaction. Srednevekovaja molecular weight of the obtained compound (b-2) is equal to 1600. To the obtained connection type 54,90 g of the solution of silica in methyl ethyl ketone (average particle diameter of 0.01 to 0.05 μm, the concentration of silicon dioxide is 30%). The solid content in the obtained mixed solution of particles of inorganic oxide (Bmix-5) is equal to 31.3 percent.

Example 1

50 wt. parts of the compound (a-1)used as component (A), 50 wt. parts of solids in the mixed solution of the particles of inorganic oxide (Bmix-1)used as component (B), and 1 wt. part 2-(4-methoxyphenyl)bis(4,6-trichloromethyl)-s-triazine used as component (C)is dissolved in utilityroom ether of diethylene glycol to the total solids content of 20 wt.%, and the resulting solution was filtered through a membrane filter with a diameter of overstay 0.2 μm, thus changing the refractive index composition.

(1) the Formation of surface films

The above composition is applied to the silicon substrate using a roller and is subjected to preliminary drying on a hot plate at 90°With those who tell 2 minutes with the formation of a coating film thickness of 1.0 μm.

(2) Forming a model of the distribution of the refractive index of

The above coating film is subjected to irradiation of 100 MJ/cm2through the template to build the model with the optimal depth-of-focus device for display in the reduction projection (Nikon Corporation, NA=0.45, and λ=365 nm). The coating film is dried after irradiation at 130°C for 2 minutes to form a model of the distribution of the refractive index difference between the refractive index in the exposed and not exposed portions of the material. Exposed part formed model of the distribution of refractive index hereinafter referred to as "part with a changed refractive index, and is not exposed part referred to as "part with constant refractive index".

(3) Measurement of refractive index of

The refractive indices in part with a modified refractive index and in part with constant refractive index formed above model, the distribution of refractive index is measured at 633 nm in the ellipsometer Auto EL IV NIR III (the company Rudolf Research Co., Ltd.). The results are shown in table 1.

(4) Evaluation of transparency

The model distribution of refractive index is formed on the glass substrate similar to paragraphs (1) and (2) except that instead of the on silicon substrate using a glass substrate of Corning 1737 (Corning Co., Ltd.). Exposed part of the model distribution of the refractive index, formed on the glass substrate, hereinafter referred to as "part with a changed refractive index, and is not exposed part referred to as "part with constant refractive index".

Then measure the transparency part with a modified refractive index and part with constant refractive index distribution model of the refractive index, formed on the glass substrate, at a wavelength of 400-800 nm in the spectrophotometer with two rays (Hitachi, Ltd.). It can be noted that the minimum transparency, greater than 95%is considered satisfactory and minimal transparency, equal to 95% or less is considered to be unsatisfactory. The results are shown in table 1.

(5) Stabilization

a 20% solution 2,2,3,3,4,4,4-getattributeasboolean in dimethylformamide (containing 10 mol.% of tetrabutylammonium bromide)used as component (D), heated at 100°C, after which the silicon and glass substrates formed with them models of the distribution of refractive index is dipped in this solution at 100°With 2 minutes, and then washed with ultrapure water for 1 minute.

Then all surface models re-exposed to radiation, equal to 4.5 mW/cm2in the device Canon PLA-50F without filter for 1 minute and heated in an oven at 200° C for 10 minutes to stabilize patterns of distribution of refractive index.

(6) Evaluation of the refractive index and transparency

The refractive indices in part with a modified refractive index and in part with constant refractive index of a stable distribution model of the refractive index, formed on a silicon substrate, measured similarly, paragraph (3). The results are shown in table 2.

The transparent part with a modified refractive index and part with constant refractive index of a stable distribution model of the refractive index, formed on the glass substrate, measured similarly, paragraph (4). The results are shown in table 2.

(7) evaluation of the stability of the model distribution of the refractive index of

The entire surface of the stable models of the distribution of refractive index, formed on a silicon substrate, and the entire surface of the stable models of the distribution of refractive index, formed on the glass substrate, is subjected to irradiation equal to 4.5 mW/cm2within 30 minutes the device Canon PLA-501F without a filter in order to accelerate the effects of exposure to radiation.

The refractive indices in part with a modified refractive index and in part with constant refractive index subjected to the data processing model of the distribution of refractive index, formed on a silicon substrate, measured similarly, paragraph (3). The results are shown in table 2.

The transparent part with a modified refractive index and part with constant refractive index of a stable distribution model of the refractive index, formed on the glass substrate, measured similarly, paragraph (4). The results are shown in table 2.

Example 2

Evaluation performed analogously to example 1 except that as component (B) use 50 wt. parts of solids in the mixed solution of the particles of inorganic oxide (Bmix-2), temperature ROAR on stage (2) (formation of a model of the distribution of refractive index) changes, as shown in table 1, the type of component (D) and temperature stabilization stage (5) (stabilization) change as shown in table 2. The results are shown in table 1 and table 2.

Example 3

Evaluation performed analogously to example 1 except that as component (A) used 50 wt. parts of the compound (a-2), as component (B) use 50 wt. parts of solids in the mixed solution of the particles of inorganic oxide (Bmix-3), as component (C) using 5 wt. parts N-(2-nitrobenzenesulfonyl)-pyrrolidine, temperature ROAR on stage (2) (formation model the distribution of the indicator prelola the Oia) change, as shown in table 1, the type of component (D) and temperature stabilization stage (5) (stabilization) change as shown in table 2. The results are shown in table 1 and table 2.

Example 4

Evaluation performed analogously to example 1 except that as component (A) used 50 wt. parts of the compound (a-2), as component (B) use 50 wt. parts of solids in the mixed solution of the particles of inorganic oxide (Bmix-4), as component (C) using 5 wt. parts N-(2-nitrobenzenesulfonyl)-pyrrolidine, temperature ROAR on stage (2) (formation of a model of the distribution of refractive index) changes, as shown in table 1, the type of component (D) and temperature stabilization stage (5) (stabilization) change as shown in table 2. The results are shown in table 1 and table 2.

Example 5

Evaluation performed analogously to example 1 except that as component (A) used 50 wt. parts of the compound (a-3), as component (B) use 50 wt. parts of solids in the mixed solution of the particles of inorganic oxide (Bmix-5), the degree of exposure at the stage (2) (formation of a model of the distribution of refractive index) changes, as shown in table 1, the type of component (D) at stage (5) (stabilization) change as shown in table 2. The results are shown the table 1 and table 2.

Example 6

Evaluation performed analogously to example 1 except that as component (A) used 50 wt. parts of the compound (a-4), as component (B) use 50 wt. parts of solids in the mixed solution of the particles of inorganic oxide (Bmix-5), as component (C) using 5 wt. parts N-(2-nitrobenzenesulfonyl)-pyrrolidine, the degree of exposure at the stage (2) (formation of a model of the distribution of refractive index) changes, as shown in table 1, the type of component (D) at stage (5) (stabilization) change as shown in table 2. The results are shown in table 1 and table 2.

Table 1
Conditions of forming a model of the distribution of refractive indexOptical properties to stabilize
The degree of exposure (MJ/cm2)Temperature ROAR (°)Refractive indexTransparency
The part with the modified refractive indexThe part with constant refractive indexThe part with the modified p is the index of refraction The part with constant refractive index
Example 1401101,751,5696,6%96,3%
Example 2401101,741,5695,8%95,4%
Example 3401101,701,5496,6%96,3%
Example 490901,621,5095,8%95,4%
Example 5301301,431,5198,7%98,4%
Example 6801301,431,5599,0%98,6%
Table 2
Conditions stabilizationOptical properties after stabilization
The type of component (D)Temperature, °Refractive indexTransparency
The part with the modified refractive indexThe part with constant refractive indexThe part with the modified refractive indexThe part with constant refractive index
Example 1D-1100°1,76of 1.5796,7%96,4%
Example 2D-1100°1,75of 1.5796,0%95.6%of
Example 3D-220°1,701,5496,6%96,3%
Example 4D-2 20°1,621,5095,8%95,4%
Example 5D-3100°1,431,5198,7%98,4%
Example 6D-3100°1,431,5599,0%98,6%
Optical properties after accelerated exposure
Refractive indexTransparency
The part with the modified refractive indexThe part with constant refractive indexThe part with the modified refractive indexThe part with constant refractive index
Example 11,76of 1.5796,7%96,4%
Example 21,75of 1.5796,0%95.6%of
Example 31,701,5496,6%96,3%
Example 41,621,5095,8%95,4%
Example 51,431,5198,7%98,4%
Example 61,431,5599,0%98,6%

In table 2, the symbols denoting the component (D), shall have the following meanings.

D-1: a 20% solution 2,2,3,3,4,4,4-getattributeasboolean in dimethylformamide (containing 10 mol.% of tetrabutylammonium bromide).

D-2: 1% aqueous solution of Ethylenediamine.

D-3: 20% solution diglycidylether ether of bisphenol a in dimethylformamide (containing 10 mol.% of tetrabutylammonium bromide).

Example 7

Changing the refractive index composition was prepared as in example 1 except that the added 15 wt. parts of diglycidyl the CSOs ether of glycerol (D). Top film get a similar stage (1) of example 1, using the above composition, and subjecting it to irradiation, as described in stage (2). After irradiation, the film is heated at 110°C for 2 minutes and then stabilize at 130°C for 10 minutes. Exposed part formed above model, the distribution of refractive index is referred to as "part with a changed refractive index, and is not exposed part referred to as "part with constant refractive index".

The refractive index and transparency of the model distribution of the refractive index, formed in accordance with the above description, evaluate similar stage (3) stage (4) of example 1, respectively. The results are shown in table 3. The stability of the formed model of the distribution of refractive index estimate is similar stage (7) of example 1. The results are shown in table 3.

Table 3
Optical properties after stabilization
Refractive indexTransparency
The part with the modified refractive indexThe part with the unmodified indicator prelo the population The part with the modified refractive indexThe part with constant refractive index
Example 71,761,5896,7%96,2%
Optical properties after accelerated exposure
Refractive indexTransparency
The part with the modified refractive indexThe part with constant refractive indexThe part with the modified refractive indexThe part with constant refractive index
Example 71,76of 1.5796,7%96,4%

Industrial applicability

Since the model of the distribution of refractive index, formed by the method according to the present invention, is characterized by a rather large difference between the refractive indices, which is stable to light and heat, this model is extremely useful for applications in the field of optoelectronics and display the data. The model distribution of the refractive index of the present invention, in addition, use of the AC is este optical material for photometric, lenses, optocouplers fotoprimaverili, polarized beam splitting elements, holograms, single-mode and multimode optical fibers, optical fiber bundles, fiber optic cable, single conductor, multi-conductor and fiber optic connectors and fiber optic connectors, photovoltaic communication, optical isolators, polarizers, optical sensors such as photodiodes, photointerrupter, photo-IP shapers of image signals based on charge-coupled devices (CCD), the shapers of the image signal based on CMOS, fiber-optic sensors and fiber-optic gyroscopes, optical disks such as CD, LD, PD and DVD, optical switches, waveguides, optical touch panels, diffraction gratings, optical guiding devices, optical diffusers, antitreaty and optical seals.

1. Sensitive to the irradiation of the composition, changing the refractive index, which contains (a) a biodegradable compound and a compound having at least one structure selected from the group comprising the structure represented by the following formula(1)-(6), (10) and(11)-(14):

where R1means alkylenes group, performancelevel group, alkylsilane group, alkylenediamines Elenovo group or Allenova group, and R2means alkylenes group, performancelevel group, alkylenediamines group, Allenova group, alkylsilane group or alkylamino group, provided that the above Allenova group or performanceheavy group can have link-O-, -CO-, -COO - or-OCOO-;

where M stands for Si or Ge, R3means alkylenes group, performancelevel group, alkylenediamines group, Allenova group, alkylsilane group, alkylamino group or a simple bond, R4means an oxygen atom, alkylenes group, performancelevel group, alkylenediamines group, Allenova group, alkylsilane group or a simple bond, R5, R6, R7and R8independently mean a hydrogen atom, alkyl group, aryl group, CNS group, thioalkyl group, alkoxy(difficult)ester group, performanceline group, performanceline group, performace(difficult)ester group or bertorello group, and m means an integer from 0 to 2, provided that the above Allenova group or performanceheavy group can have link-O-, -CO-, -COO - or-LLC-;

where R9and R10independently mean alkylenes group is, performancelevel group, alkylenediamines group, Allenova group, alkylsilane group or alkylamino group, provided that the above Allenova group or performanceheavy group can have link-O-, -CO-, -COO - or-LLC-;

where R11means oxyalkylene group or a simple bond, and R12means a hydrogen atom, alkyl group, CNS group, alkoxy(difficult)ester group, performanceline group, performace(difficult)ester group, bertorello group, alkylenediamines group or aryl group;

where R13means a hydrogen atom, alkyl group, CNS group, alkoxy(difficult)ester group, performanceline group, performanceline group, performace(difficult)ester group, bertorello group or aryl group;

where R14means alkylenes group or a structure represented by the following formula (7), (8) or (9):

where R15, R16, R17and R18independently mean a hydrogen atom, chain alkyl group with 1-6 carbon atoms, chlorine atom, bromine or iodine, hydroxyl group, Merck is progroup, carboxyl group, CNS group with 1-6 carbon atoms, alkylthiols with 1-6 carbon atoms, halogenation group with 1-6 carbon atoms, halogenalkyls group with 1-6 carbon atoms, halogenation with 1-6 carbon atoms, hydroxyalkyl group with 1-6 carbon atoms, mercaptoethanol group with 1-6 carbon atoms, hydroxyalkoxy group with 1-6 carbon atoms, mercaptoacetic with 1-6 carbon atoms, aryl group with 6-10 carbon atoms, or aracelio group with 7 to 11 carbon atoms;

where R19means alkylenes group;

where R20means alkylenes group;

where R21means alkylenes group, alkylenediamines group or Allenova group;

where R22means alkylenes group, Aracinovo group or Allenova group, R23means alkylenes group, Aracinovo group, Allenova group, alkylenediamines group, alkylsilane group or alkylamino group, R24, R25, R26and R27independently mean a hydrogen atom, alkyl group, aryl group, CNS group or tilki is inuu group, i and j independently denote 0 or 1;

where R28means alkylenes group, Aracinovo group or Allenova group, and R29means alkylenes group, Aracinovo group, Allenova group, alkylenediamines group, alkylsilane group or alkylamino group;

where R30and R31independently mean alkylenes group, Aracinovo group, Allenova group, alkylenediamines group, alkylsilane group or alkylamino group;

where R32and R33independently mean alkylenes group, Aracinovo group, Allenova group, alkylenediamines group, alkylsilane group or alkylamino group,

(B) non-biodegradable component comprising particles of an inorganic oxide, resistant to acid or base formed from sensitive to radiation present and degrades substances, (C) defined below,

and (C) sensitive to radiation corrosive substance,

and in which the ratio between the refractive index of nAnddegradable compounds (A) and refractive index of ninnon-biodegradable component (C) satisfies one is the two following expressions (1) or (2):

and the quantity of the component (b) is 10-90 parts by weight per 100 parts by weight of the total quantity of components (a) and (B), and the quantity of the component (C) is 0.01-30 parts by weight per 100 parts by weight of the total quantity of components (a) and (B).

2. The composition according to claim 1, which further comprises (D) a stabilizer.

3. The composition according to claim 1 or 2, in which the ratio between the refractive index of nAcomponent (A) and refractive index of nIncomponent (C) satisfies the expression (1):

4. The composition according to claim 1 or 2, in which the ratio between the refractive index of nAcomponent (A) and refractive index of nIncomponent (C) satisfies the expression (2):

5. Composition according to any one of claims 1 to 4, in which component (B) includes binder with the particles of the inorganic oxide.

6. How to change the refractive index, which is sensitive to radiation a composition according to claims 1 or 2, changing the index of refraction, are irradiated.

7. The method of forming a model of the distribution of refractive index, which is that part sensitive to the irradiation of the composition according to claim 1 or 2, varies the overall refractive index, are irradiated.

8. The method of forming a model of the distribution of refractive index, which is that part sensitive to the irradiation of the composition according to claim 1, changes the refractive index, are irradiated and treated with (D) a stabilizer.

9. The method of forming a model of the distribution of refractive index, which is that part sensitive to the irradiation of the composition according to claim 2, changing the refractive index, are irradiated and then treated with (D) a stabilizer at a temperature at which the stabilizer may interact with degradable compound (A).

10. The method of forming a model of the distribution of refractive index according to any one of claims 7 to 9, in which the maximum difference between the refractive index in the exposed part and not exposed part is 0.02 or more.

11. The model distribution of the refractive index, formed by the method according to any of claims 7 to 10.

12. The optical material obtained by the method according to any of claims 7 to 10.



 

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