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EP4689796A1 - Composition - Google Patents

Composition

Info

Publication number
EP4689796A1
EP4689796A1 EP24713463.8A EP24713463A EP4689796A1 EP 4689796 A1 EP4689796 A1 EP 4689796A1 EP 24713463 A EP24713463 A EP 24713463A EP 4689796 A1 EP4689796 A1 EP 4689796A1
Authority
EP
European Patent Office
Prior art keywords
polysiloxane
composition
acrylic polymer
composite
scattering particle
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
EP24713463.8A
Other languages
German (de)
French (fr)
Inventor
Daishi Yokoyama
Atsuko Noya
Chi-Shun Huang
Yung-Cheng Chang
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Merck Patent GmbH
Original Assignee
Merck Patent GmbH
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Merck Patent GmbH filed Critical Merck Patent GmbH
Publication of EP4689796A1 publication Critical patent/EP4689796A1/en
Pending legal-status Critical Current

Links

Classifications

    • GPHYSICS
    • G02OPTICS
    • G02BOPTICAL ELEMENTS, SYSTEMS OR APPARATUS
    • G02B5/00Optical elements other than lenses
    • G02B5/02Diffusing elements; Afocal elements
    • G02B5/0205Diffusing elements; Afocal elements characterised by the diffusing properties
    • G02B5/0236Diffusing elements; Afocal elements characterised by the diffusing properties the diffusion taking place within the volume of the element
    • G02B5/0242Diffusing elements; Afocal elements characterised by the diffusing properties the diffusion taking place within the volume of the element by means of dispersed particles
    • GPHYSICS
    • G03PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03FPHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/0005Production of optical devices or components in so far as characterised by the lithographic processes or materials used therefor
    • G03F7/0007Filters, e.g. additive colour filters; Components for display devices
    • GPHYSICS
    • G03PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03FPHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/004Photosensitive materials
    • G03F7/0047Photosensitive materials characterised by additives for obtaining a metallic or ceramic pattern, e.g. by firing
    • GPHYSICS
    • G03PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03FPHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/004Photosensitive materials
    • G03F7/027Non-macromolecular photopolymerisable compounds having carbon-to-carbon double bonds, e.g. ethylenic compounds
    • GPHYSICS
    • G03PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03FPHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/004Photosensitive materials
    • G03F7/027Non-macromolecular photopolymerisable compounds having carbon-to-carbon double bonds, e.g. ethylenic compounds
    • G03F7/032Non-macromolecular photopolymerisable compounds having carbon-to-carbon double bonds, e.g. ethylenic compounds with binders
    • G03F7/033Non-macromolecular photopolymerisable compounds having carbon-to-carbon double bonds, e.g. ethylenic compounds with binders the binders being polymers obtained by reactions only involving carbon-to-carbon unsaturated bonds, e.g. vinyl polymers
    • GPHYSICS
    • G03PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03FPHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/004Photosensitive materials
    • G03F7/075Silicon-containing compounds
    • G03F7/0757Macromolecular compounds containing Si-O, Si-C or Si-N bonds
    • GPHYSICS
    • G03PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03FPHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/004Photosensitive materials
    • G03F7/075Silicon-containing compounds
    • G03F7/0757Macromolecular compounds containing Si-O, Si-C or Si-N bonds
    • G03F7/0758Macromolecular compounds containing Si-O, Si-C or Si-N bonds with silicon- containing groups in the side chains

Definitions

  • the present invention relates to a composite, preferably being a layered composite, preferably said layered composite is an optical layer, obtained or obtainable by the method of the present invention.
  • the present invention relates to a composite, preferably being a layered composite, preferably said layered composite is an optical layer, comprising at least, essentially consisting of or consisting of; i) a polymer (A) derived or derivable from at least (I) an alkaline soluble polymer, preferably said alkaline soluble polymer is a polysiloxane, an 20 acrylic polymer, or a combination of a polysiloxane and an acrylic polymer; and (III) a scattering particle.
  • the polysiloxane used in the present invention may further comprise a repeating unit represented 30 by formula (l b ): Foreignfiling_text P23-049 - 8 - 5 wherein R Ib is a group obtained by removing plural hydrogen from a nitrogen and/or oxygen-containing cycloaliphatic hydrocarbon compound having amino, imino and/or carbonyl. 10
  • R Ib is preferably a group obtained by removing plural hydrogen, preferably two or three hydrogen, from preferably a nitrogen- containing aliphatic hydrocarbon ring having imino and/or carbonyl, more preferably a 5-membered or 6-membered ring containing nitrogen as a 15 member.
  • the polysiloxane used 20 in the present invention may further comprise a repeating unit represented by the formula (I c ): 25
  • the mixing ratio of the repeating units represented by the formulae 30 (l b ) and (I c ) is high, compatibility with solvents and additives decreases, and the film stress increases so that cracks sometimes easily generate.
  • the polysiloxane used in the present invention may further comprise a repeating unit 5 represented by the formula (I d ): 10 wherein R Id each independently represents hydrogen, a C 1- 30 (preferably C 1-10 ) linear, C3-30 (preferably C3-10) branched or cyclic, saturated or unsaturated, 15 aliphatic hydrocarbon group or aromatic hydrocarbon group; the aliphatic hydrocarbon group and the aromatic hydrocarbon group are each unsubstituted or substituted with fluorine, hydroxy or alkoxy, and in the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is not replaced or replaced with oxy, imide or carbonyl.
  • R Id each independently represents hydrogen, a C 1- 30 (preferably C 1-10 ) linear, C3-30 (preferably C3-10) branched or cyclic, saturated or unsaturated, 15 aliphatic hydrocarbon group or aromatic hydrocarbon group; the aliphatic hydrocarbon group and the aromatic hydrocarbon group are each unsubstituted or substituted with
  • R Id includes, for example, (i) alkyl, such as methyl, ethyl, propyl, butyl, pentyl, hexyl, heptyl, octyl and decyl, (ii) aryl, such as phenyl, tolyl and benzyl, (iii) fluoroalkyl, such as trifluoromethyl, 2,2,2-trifluoroethyl and 3,3,3-trifluoropropyl, (iv) fluoroaryl, (v) cycloalkyl, such as cyclohexyl, (vi) a nitrogen-containing 25 group having an amino or imide structure, such as isocyanate and amino, and (vii) an oxygen-containing group having an epoxy structure, such as glycidyl, or an acryloyl structure or a methacryloyl structure.
  • alkyl such as methyl, ethyl, propyl, butyl,
  • R Id is methyl, ethyl, propyl, butyl, pentyl, hexyl and phenyl.
  • the compound wherein R Id is methyl is preferred, since raw material thereof is easily 30 obtained, its film hardness after curing is high and it has high chemical resistance. Further, the compound wherein R Id is phenyl is preferred since it Foreignfiling_text P23-049 - 10 - increases solubility of the polysiloxane in the solvent and the cured film becomes hardly crackable.
  • the repeating unit of the formula (I d ) is 10 preferably 30 mol % or less, more preferably 5 mol % or less, based on the total number of the repeating units of the polysiloxane. It is also one aspect of the present invention to have no repeating unit of the formula (I d ) (0 mol %).
  • the polysiloxane used in the present invention may contain two or more types of repeating units. For example, it can contain three types of repeating units having repeating units represented by the formula (la) in which R Ia is methyl or phenyl and a repeating unit represented by the formula (I c ).
  • the polysiloxane used in the composition according to the present invention preferably has silanol.
  • the silanol refers to one in which an OH group is directly bonded to the Si skeleton of polysiloxane and is one in which hydroxy is directly attached to a silicon atom in the 25 polysiloxane comprising repeating units such as the above formulae (l a ) to (I d ). That is, the silanol is composed by bonding -O0.5H to - O0.5- in the above formulae (l a ) to (I d ).
  • the content of the silanol in polysiloxane varies depending on the conditions for synthesizing polysiloxane, for example, the mixing ratio of the monomers, the type of the reaction catalyst and the like. 30
  • the content of this silanol can be evaluated by quantitative infrared absorption spectrum measurement.
  • the absorption band assigned to Foreignfiling_text P23-049 - 11 - silanol (SiOH) appears as an absorption band having a peak in the range of 900 ⁇ 100 cm -1 in the infrared absorption spectrum. When the content of the silanol is high, the intensity of this absorption band increases.
  • the intensity of the absorption band assigned to Si-0 is used as a reference.
  • An absorption band having a peak in the range of 1100 ⁇ 100 cm -1 is adopted as a peak assigned to Si-O.
  • the silanol content can be relatively evaluated by the ratio S2/S1, which is a ratio of the integrated 10 intensity S2 of the absorption band assigned to SiOH to the integrated intensity SI of the absorption band assigned to Si-O.
  • the ratio S2/S1 is preferably 0.003 to 0.15, more preferably 0.01 to 0.10. 15
  • the integrated intensity of the absorption band is determined in consideration of noise in the infrared absorption spectrum.
  • an absorption band assigned to Si-OH having a peak in the range of 900 ⁇ 100 cm -1 and an absorption band assigned to a Si-0 having a peak in the range of 1100 ⁇ 100 cm -1 are 20 confirmed.
  • the integrated intensity of these absorption bands can be measured as an area in consideration of a baseline in which noise and the like are considered.
  • the foot of the absorption band assigned to Si-OH and the foot of the absorption band assigned to Si-0 are overlapped; however, in such a case, the wavenumber 25 corresponding to the minimal point between the two absorption bands in the spectrum is set as their boundary.
  • the mass average molecular weight of the polysiloxane used in the present invention is not particularly limited. However, the higher the molecular weight, the more the coating properties tend to be improved. On the other Foreignfiling_text P23-049 - 12 - hand, the lower the molecular weight is, the less synthesis conditions are limited, so that the synthesis is easy, and the synthesis of polysiloxane having a remarkably high molecular weight is difficult.
  • the mass average molecular weight of polysiloxane is usually 500 to 5 25,000, and preferably 1,000 to 20,000 from the viewpoint of solubility in an organic solvent.
  • the mass average molecular weight means a mass average molecular weight in terms of polystyrene, which can be measured by the gel permeation chromatography based on polystyrene.
  • the synthesis method of the polysiloxane used in the present invention is not particularly limited. For example, it can be synthesized according to the method disclosed in JP 6639724 B. As stated above, publicly available polysiloxane falls under above 15 definitions can be used preferably for examples like described in WO2021/099236 A1, EP 3717966 B1.
  • acrylic polymer When acrylic polymer is used as an alkaline soluble polymer in the present invention, it can be selected from commonly used (meth)acrylic polymer, 25 preferably it is selected from acrylic polymer, such as polyacrylic acid, polymethacrylic acid, polyalkyl acrylate, polyalkyl methacrylate. It is believed that by using (meth)acrylic polymer, thicker layer, lowering process temperature and/or improving etching property, can be realized.
  • the acrylic polymer used in the present invention preferably comprises a repeating unit containing an acryloyl group. It is also preferable that the Foreignfiling_text P23-049 - 13 - acrylic polymer further comprises a repeating unit containing a carboxy group and/or a repeating unit containing an alkoxysilyl group.
  • the repeating unit containing a carboxy group is not particularly 5 limited as long as it is a repeating unit containing a carboxy group at its side chain, a repeating unit derived from an unsaturated carboxylic acid, an unsaturated carboxylic anhydride or a mixture thereof is preferable.
  • the repeating unit containing an alkoxysilyl group can be a 10 repeating unit containing an alkoxysilyl group at its side chain, it is preferably a repeating unit derived from a monomer represented by the following formula (B): X B -(CH2)a-Si(OR B )b(CH3)3-b (B) wherein, 15 X B is a vinyl group, a styryl group or a (meth)acryloyloxy group, and R B is a methyl group or an ethyl group, a is an integer of 0 to 3, and b is an integer of 1 to 3.
  • B X B -(CH2)a-Si(OR B )b(CH3)3-b
  • the above-described polymer contains a 20 repeating unit containing a hydroxy group derived from a hydroxy group- containing unsaturated monomer.
  • the mass average molecular weight of the acrylic polymer used in the present invention is not particularly limited, and is preferably 1,000 to 25 40,000, more preferably 2,000 to 30,000.
  • the mass average molecular weight is a mass average molecular weight in terms of polystyrene according to gel permeation chromatography.
  • the content of the acrylic polymer (II) is preferably 18.0 to 35.0 mass%, 30 and more preferably 20.0 to 32.0 mass%, based on the total mass of the composition.
  • the content of the acrylic polymer (II) is preferably 65.0 to 92.0 mass%, and more preferably 70.0 to 90.0 mass%, based on the total mass of the polysiloxane (I) and the acrylic polymer (II).
  • said alkali-soluble polymer is a polysiloxane, or a combination of a polysiloxane and an acrylic polymer, and the total amount of the polysiloxane is in the range from 1 to 40 mass% based on the total mass of the composition without solvent, preferably it is from 5 to 35 mass%, more preferably from 10 to 30 mass%.
  • said acrylic polymer is selected from one or more members of the group consisting of polyacrylic acid, polymethacrylic acid, polyalkyl acrylate, polyalkyl methacrylate.
  • the total amount of the acrylic polymer in the composition is in 15 the range from 65 to 99 mass%, more preferably from 70 to 90 mass%, based on the total mass of the composition without solvent.
  • (II) Polymerization initiator The composition according to the present invention comprises a 20 polymerization initiator.
  • the polymerization initiator includes a polymerization initiator that generates an acid, a base or a radical by radiation, and a polymerization initiator that generates an acid, a base or a radical by heat.
  • the former is preferable and the photo radical generator is more preferable, in terms of process shortening 25 and cost since the reaction is initiated immediately after the irradiation of radiation and the reheating process performed after the irradiation of radiation and before the development process can be eliminated.
  • the photo radical generator can improve the resolution by strengthening 30 the shaped pattern or increasing the contrast of development.
  • the photo radical generator used in the present invention is a photo radical generator that emits a radical when irradiated with radiation. Examples of the Foreignfiling_text P23-049 - 15 - radiation include visible light, ultraviolet light, infrared light, X-ray, electron beam, ⁇ -ray, and ⁇ -ray.
  • the content of the photo radical generator is preferably 0.001 to 30 mass%, 5 and more preferably 0.01 to 10 mass%, based on the total mass of the component (I) and the component (II), though the optimal amount thereof depends on the type and amount of active substance generated by decomposition of the photo radical generator, the required photosensitivity, and the required dissolution contrast between the exposed area and 10 unexposed area. If the content is less than 0.001 mass%, the dissolution contrast between the exposed area and unexposed portion is too low, and the addition effect is not sometimes exhibited. On the other hand, when the content of the photo radical generator is more than 30 mass%, cracks are generated in the coated film and colorless transparency of the coated film 15 sometimes degrades, because coloring becomes remarkable due to decomposition of the photo radical generator.
  • the photo radical generator include azo-based, peroxide- based, acylphosphine oxide-based, alkylphenone-based, oxime ester- based, and titanocene-based initiators.
  • alkylphenone-based, acylphosphine oxide-based and oxime ester-based initiators are preferred, and 2,2-dimethoxy-1,2-diphenylethan-1-one, 1-hydroxy-cyclohexylphenyl 30 ketone, 2-hydroxy-2-methyl-1-phenylpropan-1-one, 1-[4-(2- hydroxyethoxy)phenyl]-2-hydroxy-2-methyl-1-propan-1-one, 2-hydroxy-1- ⁇ 4- [4-(2-hydroxy-2-methylpropionyl)-benzyl]phenyl ⁇ -2-methylpropan-1-one, 2- Foreignfiling_text P23-049 - 16 - methyl-1-(4-methylthiophenyl)-2-morpholinopropan-1-one, 2-benzyl-2- dimethylamino-1-(4-morpholinophenyl)-1-butanone, 2-(dimethylamino)-2- [(4-methylphenyl)methyl]-1-[4-(4-(4-
  • the average particle size of the scattering particle is 200 nm or more and 10 ⁇ m or less, preferably from 230nm-5 ⁇ m, more preferably from 250nm to 2 ⁇ m.
  • the average particle size is in the range from 200nm to 1 ⁇ m, preferably from 230 to 800nm, more preferably 15 from 250 to 700nm, even more preferably from 300 to 600nm; and in case of the scattering particle is an organic particle, preferably the average particle size is in the range from 300nm to 10 ⁇ m, more preferably from 500nm to 5 ⁇ m, even more preferably from 700nm to 3 ⁇ m, furthermore preferably from 800nm to 2 ⁇ m.
  • the scattering particle has the refractive index greater than the refractive index of the mixture of the polysiloxane and the acrylic polymer, preferably the scattering particle is configured to have the refractive index greater than the 25 refractive index of a matrix polymer derived from the polysiloxane and an acrylic polymer by polymerization.
  • said refractive index of the scattering particle is 1.6 or more, preferably it is 1.7 or more, and 2.4 or less, preferably 2.2 or less. The most preferably from 1.8 to 2.0.
  • the 30 average refractive index of the scattering particles is 1.6 or more, preferably it is 1.7 or more, and 2.4 or less, preferably 2.2 or less. The most preferably from 1.8 to 2.0.
  • Foreignfiling_text P23-049 - 17 - It is believed that the above mentioned high refractive index of the scattering particle realizes increased scatter effect. Namely, when said scattering particle has the average particle size described above, and has 5 the refractive index value indicated above, said scattering effect becomes most optimal in the obtained optical layer.
  • the scattering particle is an organic particle and the difference X of the refractive index of the scattering particle 10 and the refractive index of the mixture of the polysiloxane and the acrylic polymer is in the range from -0.2 to +0.2.
  • the difference X’ of the refractive index of the scattering particle and the refractive index of a matrix polymer derived from the polysiloxane and an acrylic polymer by polymerization is in the range from -0.2 to +0.2.
  • the scattering particle is an organic particle and the difference X of 30 the refractive index of the scattering particle and the refractive index of the mixture of the polysiloxane and the acrylic polymer is in the range defined above, incident light may pass though said scattering particle well.
  • Foreignfiling_text P23-049 - 18 - When the organic scatter is used in the optical layer (composite), it is believed that the outermost surface of the obtained optical layer (composite) has surface roughness caused by the organic scatter, and on 5 the surface of said roughness, when the light goes out from the optical layer (composite), the direction of the light is changed. It generates scattering effect effectively, preferably without causing loss of light within the optical layer.
  • the composition further comprises a solvent from the viewpoint of improved handling, coating, coating of the composition when string it or when fabricating a layer.
  • said solvent is an organic solvent, more preferably said solvent is an organic solvent selected from one or more members of the group consisting of ethylene glycol monoalkyl ethers, preferably it is ethylene glycol monomethyl ether, ethylene glycol monoethyl ether, ethylene glycol monopropyl ether and/or ethylene glycol monobutyl ether; diethylene glycol 25 dialkyl ethers, preferably it is diethylene glycol dimethyl ether, diethylene glycol diethyl ether, diethylene glycol dipropyl ether and/or diethylene glycol dibutyl ether; propylene glycol monoalkyl ethers, preferably it is propylene glycol monomethyl ether(PGME), propylene glycol monoethyl ether and/or propylene glycol monopropyl ether; ethylene glycol alkyl ether acetates, 30 preferably it is methyl cellosolve acetate and/or ethyl cellosolve acetate; propylene glyco
  • the composition further comprises a compound containing two or more Foreignfiling_text P23-049 - 20 - (meth)acryloyloxy groups (hereinafter sometimes referred to as (meth)acryloyloxy group-containing compound), preferably the content of the compound is in the range from 10.0 to 25.0 mass% based on the total mass of the composition without solvent.
  • the (meth)acryloyloxy group is a general term for the acryloyloxy group and the methacryloyloxy group.
  • This compound is a compound that can form a crosslinked structure by reacting with the polysiloxane (I), acrylic polymer (II) and the like.
  • a compound 10 containing two or more (meth)acryloyloxy groups, which are reactive groups is needed.
  • it preferably contains three or more (meth)acryloyloxy groups.
  • 15 esters obtained by reacting ( ⁇ ) a polyol compound having two or more hydroxy groups with ( ⁇ ) two or more (meth)acrylic acids are preferably used.
  • polyol compound ( ⁇ ) compounds having, as a basic skeleton, a saturated or unsaturated aliphatic hydrocarbon, aromatic hydrocarbon, heterocyclic hydrocarbon, primary, secondary or tertiary amine, ether or the 20 like, and having, as substituents, two or more hydroxy groups are included.
  • the polyol compound can contain other substituents, for example, a carboxy group, a carbonyl group, an amino group, an ether bond, a thiol group, a thioether bond, and the like, as long as the effects of the present invention are not impaired.
  • Preferred polyol compounds include alkyl polyols, aryl polyols, polyalkanolamines, cyanuric acid, and dipentaerythritol.
  • the polyol compound ( ⁇ ) has three or more hydroxy groups, it is not necessary that all the hydroxy groups have reacted with (meth)acrylic acid, and they can be 30 partially esterified. This means that the esters can have unreacted hydroxy group(s).
  • the composition according to the present invention comprises a combination of two or more kinds of the (meth)acryloyloxy group-containing compounds, and preferably a combination of three or more kinds of the (meth)acryloyloxy group-containing compounds.
  • the composition according to the 15 present invention comprises a combination of three kinds of the (meth)acryloyloxy group-containing compounds.
  • At least one of two or more kinds of the (meth)acryloyloxy group-containing compounds is the compound containing three or more 25 (meth)acryloyloxy groups. More preferably, at least one is the compound containing three or more (preferably three) (meth)acryloyloxy groups, and at least one is the compound containing two (meth)acryloyloxy groups. Further preferably, in order to make the pattern surface smoother, the component (III) is a combination of one kind of the compound containing 30 three (meth)acryloyloxy groups and two kinds of the compounds containing two (meth)acryloyloxy groups.
  • the content of the compounds containing three or more (meth)acryloyloxy groups is preferably 20.0 to 50.0 mass%, and more preferably 30.0 to 40.0 mass%, based on 5 the total mass of the component (III).
  • the component (III) in order to improve alkali solubility during development and heat resistance of the cured film, preferably comprises the compound having an isocyanurate 10 structure.
  • such compounds include tris(2- acryloyloxyethyl)isocyanurate, bis(2-acryloyloxyethyl)isocyanurate, tris(3-acryloyloxypropyl)isocyanurate, bis(3-acryloyloxypropyl)isocyanurate, 15 tris(4-acryloyloxybutyl)isocyanurate, bis(4-acryloyloxybutyl)isocyanurate, and preferably tris(2- acryloyloxyethyl)isocyanurate.
  • the content of the component (III) is adjusted according to the type of the polymer or the (meth)acryloyloxy group-containing compound to 30 be used, it is preferably 10.0 to 25.0 mass%, and more preferably 10.0 to 20.0 mass%, based on the total mass of the polysiloxane (I) and the acrylic polymer (II) from the viewpoint of compatibility with polymers.
  • Foreignfiling_text P23-049 - 23 - - Additives may further comprise one or more of additives. However, in some case, the 5 amount of said additive can be zero.
  • Such additive may be selected from one or more members of the group consisting of, for examples, surfactants, adhesion promoter, silane coupling agent, thermal acid generators, thermal base generators, crosslinkable monomers and polymerization initiators. Publicly available ones can be used preferably, like described in EP 10 3717966 A1 or WO 2021/099236 A1. Since said additive is not mandatory for this invention, the amount of the additive in the composition or in the layer based on the total amount of polysiloxane is preferably 5wt% or less, more preferably 1wt% or less. The composition and/or a layer obtained from the composition may not contain any said additives.
  • present invention further relates to a method of preparing the composition of the present invention comprising at least, essentially consisting of or consisting of the following steps; (X) mixing at least 20 (I) an alkaline soluble polymer, preferably it is a polysiloxane, an acrylic polymer, or a combination of a polysiloxane and an acrylic polymer; (II) a polymerization initiator; and (III) a scattering particle.
  • said mixing step (X) is performed in the presence of a solvent, 25 more preferably in the presence of an organic solvent.
  • a compound containing two or more (meth)acryloyloxy groups is also mixed in the mixing step (X) to form the composition.
  • present invention further relates to a composition 30 obtained or obtainable by the method of fabricating the composition described above.
  • Foreignfiling_text P23-049 - 24 - present invention also relates to use of the composition of the present invention for preparing an optical layer containing a metal oxide, preferably for preparing a composite, more preferably for preparing a layered composite.
  • present invention further relates to a method of fabricating a composite of the present invention comprising at least, essentially consisting of or consisting of the following steps; (Xi) applying the composition of the present invention onto a layer or onto a 10 substrate to form a coated layer; and (Xii) baking a coated layer to obtain a composite (post baking process).
  • the energy of Foreignfiling_text P23-049 - 26 - the irradiation light is generally 5 to 2,000 mJ/cm 2 , preferably 10 to 1,000 mJ/cm 2 , although it depends on the light source and the film thickness of the coating film. If the irradiation light energy is lower than 5 mJ/cm 2 , sufficient resolution cannot be obtained in some cases. On the other hand, 5 when the irradiation light energy is higher than 2,000 mJ/cm 2 , the exposure becomes excess and halation sometimes occurs.
  • a general photomask can be used. Such a photomask can be freely selected from well-known ones.
  • the environment at the time of irradiation is not particularly limited and can generally be set as an ambient atmosphere (in the air) or nitrogen atmosphere. Further, in the case of forming a film on the entire surface of the substrate, light irradiation can be performed over the entire surface of the substrate. In the present invention, the pattern film also includes such a 15 case where a film is formed on the entire surface of the substrate.
  • Post exposure baking process After the exposure, to promote the reaction between the polymer in the film by the polymerization initiator, post exposure baking can be performed, as 20 necessary. Different from the heating process (6) to be described later, this heating treatment is performed not to completely cure the coating film but to leave only a desired pattern on the substrate after development and to make other areas capable of being removed by development.
  • the heating temperature should not be excessively high because it is not desirable for the acid, base or radical in the exposed area, which is generated by light irradiation, to diffuse to the 30 unexposed area.
  • the range of the heating temperature after exposure is preferably 40 to 150°C, and more preferably 60 to 120°C. Stepwise heating can be applied as needed to control the Foreignfiling_text P23-049 - 27 - curing rate of the composition.
  • the atmosphere during the heating is not particularly limited and can be selected from in an inert gas such as nitrogen, under a vacuum, under a reduced pressure, in an oxygen gas, and the like, for the purpose of controlling the curing rate of the 5 composition.
  • the heating time is preferably above a certain level in order to maintain higher the uniformity of temperature history in the wafer surface and is preferably not excessively long in order to suppress diffusion of the generated acid, base or radical. From such a viewpoint, the heating time is preferably 20 seconds to 500 seconds, and more preferably 40 10 seconds to 300 seconds. (5) Developing process After post-exposure baking is optionally performed after exposure, the coating film is developed.
  • any developer conventionally used for developing a photosensitive composition can be used.
  • the developer include an alkali developer which is an aqueous solution of an alkaline compound such as tetraalkylammonium hydroxide, choline, alkali metal hydroxide, alkali metal metasilicate (hydrate), alkali metal phosphate 20 (hydrate), ammonia, alkylamine, alkanolamine and heterocyclic amine, and a particularly preferable alkali developer is tetramethylammonium hydroxide (TMAH) aqueous solution, a potassium hydroxide aqueous solution, or a sodium hydroxide aqueous solution.
  • TMAH tetramethylammonium hydroxide
  • a water- soluble organic solvent such as methanol and ethanol, or a surfactant can 25 be further contained, if necessary.
  • the developing method can also be freely selected from conventionally known methods. Specifically, methods such as dipping in a developer (dip), paddle, shower, slit, cap coat, spray, and the like can be included.
  • rinsing with water is 30 carried out.
  • Post baking process After development, the obtained pattern film is cured by heating. As the heating apparatus used for the heating process, the same one as used for the above-described post-exposure baking can be used.
  • the heating 5 temperature in the heating process is not particularly limited as long as it is a temperature at which curing of the coating film can be performed and can be freely determined. However, if the silanol group of the polysiloxane remains, the chemical resistance of the cured film sometimes becomes insufficient, or dielectric constant of the cured film sometimes becomes 10 higher. From such a viewpoint, a relatively high temperature is generally selected as the heating temperature. In order to keep the remaining film ratio after curing high, the curing temperature is more preferably 350°C or lower, and particularly preferably 250°C or lower.
  • the curing temperature is preferably 70°C or higher, more preferably 80°C or higher, and particularly preferably 90°C or higher.
  • the heating time is not particularly limited and is generally 10 minutes to 24 hours, and preferably 30 minutes to 3 hours.
  • this heating time is a time from when the temperature of the pattern film reaches a desired heating 20 temperature. Usually, it takes about several minutes to several hours for the pattern film to reach a desired temperature from the temperature before heating.
  • present invention further relates to a composite, 25 preferably being a layered composite, preferably said layered composite is an optical layer, obtained or obtainable by the method of fabricating a composite, of the present invention explained above.
  • said photosensitive composition is a filling composition to be used for fabricating an electronic device, more preferably it is a filing composition for an LED or ⁇ LED.
  • said scattering particle is 15 selected from inorganic particles, organic particles and a mixture of inorganic particles and organic particles.
  • 3. The composition of embodiment 1 or 2, wherein the average particle size of the scattering particle is 200 nm or more and 10 ⁇ m or less, preferably 20 from 230nm-5 ⁇ m, more preferably from 250nm to 2 ⁇ m.
  • said refractive index of the scattering particle is 1.6 or more, preferably it is 1.7 or more, and 2.4 or less, preferably 2.2 or less. The most preferably from 1.8 to 2.0.
  • the average refractive index of the scattering particles is 1.6 or more, preferably it is 1.7 or more, and 2.4 or less, preferably 2.2 or less. The most preferably from 1.8 to 2.0. 10 5.
  • the composition of any one of embodiments 1 to 3, wherein the scattering particle is an organic particle and the difference X of the refractive index of the scattering particle and the refractive index of the mixture of the polysiloxane and the acrylic polymer is in the range from -0.2 to +0.2.
  • the difference X’ of the refractive index of the scattering 15 particle and the refractive index of a matrix polymer derived from the polysiloxane and an acrylic polymer by polymerization is in the range from -0.2 to +0.2.
  • R Ia is hydrogen, a C1-30 (preferably C1-10) linear, C3-30 (preferably C3-10) branched or cyclic, saturated or unsaturated, aliphatic hydrocarbon group or aromatic hydrocarbon group, the aliphatic hydrocarbon group and the aromatic hydrocarbon group are each unsubstituted or substituted with fluorine, hydroxy or alkoxy, and 15 in the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is not replaced, or one or more methylene is replaced by oxy, imino or carbonyl, provided that R Ia is neither hydroxy nor alkoxy. 7.
  • an alkali-soluble polymer is an acrylic polymer, or a combination of a polysiloxane and an acrylic polymer
  • said acrylic polymer is selected from one or more members of the group consisting of polyacrylic 20 acid, polymethacrylic acid, polyalkyl acrylate, polyalkyl methacrylate.
  • the total amount of the acrylic polymer in the composition is in the range from 65 to 99 mass%, more preferably from 70 to 90 mass%, based on the total mass of the composition without solvent. 25 10.
  • composition of any one of the preceding embodiments further comprises a solvent, preferably said solvent is an organic solvent, more preferably said solvent is an organic solvent selected from one or more members of the group consisting of ethylene glycol monoalkyl ethers, preferably it is ethylene glycol monomethyl ether, ethylene glycol monoethyl 30 ether, ethylene glycol monopropyl ether and/or ethylene glycol monobutyl ether; diethylene glycol dialkyl ethers, preferably it is diethylene glycol dimethyl ether, diethylene glycol diethyl ether, diethylene glycol dipropyl Foreignfiling_text P23-049 - 34 - ether and/or diethylene glycol dibutyl ether; propylene glycol monoalkyl ethers, preferably it is propylene glycol monomethyl ether(PGME), propylene glycol monoethyl ether and/or propylene glycol monopropyl ether; ethylene glycol alkyl ether acetates,
  • composition of any one of the preceding embodiments further comprises a compound containing two or more (meth)acryloyloxy groups, preferably the content of the compound is in the range from 10.0 to 25.0 30 mass% based on the total mass of the composition without solvent.
  • Method of preparing the composition of any one of the preceding embodiments containing at least the following step; (X) mixing at least (I) an alkaline soluble polymer, preferably it is a polysiloxane, an acrylic 5 polymer, or a combination of a polysiloxane and an acrylic polymer; (II) a polymerization initiator; and (III) a scattering particle.
  • said mixing step (X) is performed in the presence of a solvent, more preferably in the presence of an organic solvent.
  • a 10 compound containing two or more (meth)acryloyloxy groups is also mixed in the mixing step (X) to form the composition.
  • Method of fabricating a composite comprising steps of: (Xi) applying the composition of any one of the embodiments 1 to 11 onto a layer or onto a substrate to form a coated layer; and 20 (Xii) baking a coated layer to obtain a composite.
  • said polymer (A) is derived or derivable from at least (I) the alkaline soluble polymer, and (II) a polymerization initiator; more preferably it is derived or derivable from at least (I) the alkaline soluble polymer, (II) a 15 polymerization initiator and a compound containing two or more (meth)acryloyloxy groups.
  • the composite of embodiment 15 or 16 contains one or more organic particles as the scattering particle, and the outermost surface of the 20 composite has an uneven structure, preferably the surface of the composite has finely roughened structure, more preferably the whole surface of the composite has finely roughened structure, even more preferably said uneven structure and finely roughened structure are caused by said organic one or more organic particles. 25 18.
  • the composite of any one of embodiments 15 to 17, has the average layer thickness in the rage from 1 ⁇ m to 200 ⁇ m, preferably from 1.5 to 100 ⁇ m, more preferably from 2 to 100 ⁇ m. 30 19.
  • a display device comprising at least one functional medium configured to modulate a light or configured to emit light; and the composite of any one of embodiments 15 to 18.
  • Foreignfiling_text P23-049 - 37 - Working Examples The working examples below provide descriptions of the present invention, as well as an in-detail description of their fabrication. However, the present 5 invention is not limited to these working examples.
  • the mixed solution is added dropwise at 40°C, stirred at the same temperature for 2 hours, and neutralized by adding a 10 mass% aqueous solution of 15 HCl.
  • 400 ml of toluene and 600 ml of water are added to the neutralized solution to separate into two layers, and the aqueous layer is removed. Further, the resulting product is rinsed three times with 300 ml of water, the obtained organic layer is concentrated under reduced pressure to remove the solvent, and PGMEA is added to the concentrate to adjust the solid 20 content to be 35 mass%, thereby obtaining Polysiloxane A solution.
  • Mass average molecular weight (Mw) of the obtained Polysiloxane A is 1,700.
  • a mixture liquid of acrylic acid, ⁇ -methacryloxypropyltrimethoxysilane, 2-hydroxyethyl methacrylate 30 and methyl methacrylate at 10 : 20 : 20 : 50, azobisisobutyronitrile, and PGMEA is prepared, and the mixture liquid is dropped into the above- described solvent over 4 hours. Thereafter, the resulting product is reacted Foreignfiling_text P23-049 - 38 - for 3 hours to obtain Acrylic polymer A. Mw of the obtained Acrylic polymer A is 8,700.
  • the negative tone formulation mixture is prepared as mentioned below: alkaline soluble siloxane polymer (Polysiloxane A) from Merck represented 20 by the following chemical formula, alkaline soluble acrylic polymer A from synthesis example 2, alkaline soluble acrylic polymer B from synthesis example 3, photo initiator NCI-831E, IRGACURE OXE03, monomer A- 9300S, A-DCP, A-DOD-N and AKS-10 for additives are solved in PGMEA. The mixture is adjusted to 44wt% of solid content in PGMEA.
  • total transmittance in the wavelength range from 380 to 780nm
  • said Haze value is measured at room temperature in air using a haze measurement system with an integrating sphere (NDH-7000, Nippon Denshoku, Japan, Light source White LED 3W, 15 wavelength range 380 ⁇ 780nm).
  • the sample thickness is between 2 ⁇ m and 700 ⁇ m. Particularly it is 700 ⁇ m.
  • the degree of light scattering in the sample, i.e., 25 the haze (H), is defined as H TD/TT.
  • the transmittance and haze is measured.
  • Particle size is obtained from catalog published by the material suppliers.
  • RI (Refractive Index) value is not measured, but publicly available RI data 30 (Catalog Value) for the materials is used.

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Abstract

The present invention relates to a composition comprising a photosensitive composition comprising at least an alkaline soluble polymer.

Description

Foreignfiling_text P23-049 - 1 - Composition Field of the invention The present invention relates to a photosensitive composition comprising at 5 least an alkaline soluble polymer, method for preparing a photosensitive composition, use of a photosensitive composition, method for fabricating a composite, a composite and a display device. Background Art 10 US2010/0016488 A1 discloses a process for producing an organosiloxane polymer comprising hydrolyzing tri- and tetraalkoxysilane monomers in a hydrolysis step; and polymerizing said hydrolyzed monomers in a polymerization step by subjecting them to conditions conducive to polymerization to form an organosiloxane polymer; wherein the hydrolysis 15 step is conducted in a reaction medium comprising an organic compound with hydroxy groups. It also discloses use of a composition produced by a process for optical and electrical coatings. Patent Literature 20 1. US 2010/0016488 A1 Summary of the invention However, the inventors newly have found that there are still one or more of considerable problems for which improvement is desired, as listed below: 25 obtaining a photosensitive composition which can realize improved scattering effect, increase haze value, preferably with keeping constant transmittance; providing a photosensitive composition which can realize improved brightness from the side angle of a cured film, improved dispersion of scattering particles in an optical layer and/or in a 30 photosensitive composition, realizing said improved scattering effect and/or improved brightness from the sided angle with smaller amount of scattering particles. Foreignfiling_text P23-049 - 2 - The inventors aimed to solve one or more of the above-mentioned problems. Then it is found as claimed, a novel photosensitive composition comprising 5 at least, essentially consisting of or consisting of; (I) an alkaline soluble polymer, preferably it is a polysiloxane, an acrylic polymer, or a combination of a polysiloxane and an acrylic polymer; (II) a polymerization initiator; and (III) a scattering particle. 10 In another aspect, the present invention relates to a method of preparing the composition of the present invention, containing at least, essentially consisting of or consisting of, the following step; (X) mixing at least 15 (I) an alkaline soluble polymer, preferably it is a polysiloxane, an acrylic polymer, or a combination of a polysiloxane and an acrylic polymer; (II) a polymerization initiator; and (III) a scattering particle. 20 In another aspect, the present invention relates to use of the composition of the present invention for preparing an optical layer containing a metal oxide, preferably for preparing a composite, more preferably for preparing a layered composite. 25 In another aspect, the present invention relates to a method of fabricating a composite, comprising steps of: (Xi) applying the composition of the present invention onto a layer or onto a substrate to form a coated layer; and (Xii) baking a coated layer to obtain a composite. 30 Preferably the method further comprises one or more of the following steps after step (Xi) and before the step (Xii): Foreignfiling_text P23-049 - 3 - (Xiii) Applying a pre-baking (heat treatment) of the coating layer in order to dry the coated layer and reduce the residual amount of the solvent in the coated layer; (Xiv) irradiating the coated layer with light (applying light irradiation), 5 preferably with light having peak maximum wavelength in the range from 360 to 430 nm, preferably a patterning mask is used when light irradiation is conducted; (Xv) applying post exposure baking process; and/or (Xvi) applying developing process to form a patterned cured layer. 10 In another aspect, the present invention relates to a composite, preferably being a layered composite, preferably said layered composite is an optical layer, obtained or obtainable by the method of the present invention. 15 In another aspect, the present invention relates to a composite, preferably being a layered composite, preferably said layered composite is an optical layer, comprising at least, essentially consisting of or consisting of; i) a polymer (A) derived or derivable from at least (I) an alkaline soluble polymer, preferably said alkaline soluble polymer is a polysiloxane, an 20 acrylic polymer, or a combination of a polysiloxane and an acrylic polymer; and (III) a scattering particle. In another aspect, the present invention further relates to a display device 25 comprising at least one functional medium configured to modulate a light or configured to emit light; and the composite of the present invention. Further advantages of the present invention will become evident from the following detailed description. 30 Technical effects of the invention Foreignfiling_text P23-049 - 4 - The present invention provides one or more of the following technical effects: obtaining a photosensitive composition which can realize improved scattering effect, increase haze value, preferably with keeping constant 5 transmittance; providing a photosensitive composition which can realize improved brightness from the side angle of a cured film, improved dispersion of scattering particles in an optical layer and/or in a photosensitive composition, realizing said improved scattering effect and/or improved brightness from the sided angle with smaller amount of scattering 10 particles. Definition of the terms In the present specification, symbols, units, abbreviations, and terms have the following meanings unless otherwise specified. 15 In the present specification, unless otherwise specifically mentioned, the singular form includes the plural form and “one” or “that” means “at least one.” In the present specification, unless otherwise specifically mentioned, an element of a concept can be expressed by a plurality of species, and 20 when the amount (for example, mass % or mol %) is described, it means sum of the plurality of species. “and/or” includes a combination of all elements and also includes single use of the element. In the present specification, when a numerical range is indicated using “to” 25 or “ - ,” it includes both endpoints and units thereof are common. For example, 5 to 25 mol % means 5 mol % or more and 25 mol % or less. In the present specification, the hydrocarbon means one including carbon and hydrogen, and optionally including oxygen or nitrogen. The hydrocarbyl 30 group means a monovalent or divalent or higher valent hydrocarbon. In the present specification, the aliphatic hydrocarbon means a linear, branched or cyclic aliphatic hydrocarbon, and the aliphatic hydrocarbon group means Foreignfiling_text P23-049 - 5 - a monovalent or divalent or higher valent aliphatic hydrocarbon. The aromatic hydrocarbon means a hydrocarbon comprising an aromatic ring which may optionally not only comprise an aliphatic hydrocarbon group as a substituent but also be condensed with an alicycle. The aromatic 5 hydrocarbon group means a monovalent or divalent or higher valent aromatic hydrocarbon. Further, the aromatic ring means a hydrocarbon comprising a conjugated unsaturated ring structure, and the alicycle means a hydrocarbon having a ring structure but comprising no conjugated unsaturated ring structure. 10 In the present specification, the alkyl means a group obtained by removing any one hydrogen from a linear or branched, saturated hydrocarbon and includes a linear alkyl and branched alkyl, and the cycloalkyl means a group obtained by removing one hydrogen from a saturated hydrocarbon 15 comprising a cyclic structure and optionally includes a linear or branched alkyl in the cyclic structure as a side chain. In the present specification, the aryl means a group obtained by removing any one hydrogen from an aromatic hydrocarbon. The alkylene means a 20 group obtained by removing any two hydrogens from a linear or branched, saturated hydrocarbon. The arylene means a hydrocarbon group obtained by removing any two hydrogens from an aromatic hydrocarbon. In the present specification, when polymer has a plural types of repeating 25 units, these repeating units copolymerize. These copolymerization are any of alternating copolymerization, random copolymerization, block copolymerization, graft copolymerization, or a mixture of any of these. In the present specification, Celsius is used as the temperature unit. For 30 example, 20°C, 20 degrees means 20 degrees Celsius. Detailed description of the invention Foreignfiling_text P23-049 - 6 - According to the present invention, in one aspect, photosensitive composition comprises at least, essentially consisting of or consisting of; (I) an alkaline soluble polymer, preferably it is a polysiloxane, an acrylic polymer, or a combination of a polysiloxane and an acrylic polymer; 5 (II) a polymerization initiator; and (III) a scattering particle. Preferably said photosensitive composition is a negative type of photosensitive composition, preferably said photosensitive composition is to be used for fabricating a protection layer of an electronic device. Preferably 10 said photosensitive composition is a filling composition to be used for fabricating an electronic device, more preferably it is a filing composition for an LED or μLED. (I) Alkaline soluble polymer 15 - Polysiloxane According to the present invention, in a preferable embodiment, said alkali- soluble polymer is a polysiloxane, an (meth)acrylic polymer or a combination of a polysiloxane and an (meth)acrylic polymer. Any publicly available polysiloxane and/or (meth)acrylic polymer can be used. Preferably 20 said polysiloxane comprises a repeating unit of chemical formula (Ia). 25 wherein RIa is hydrogen, a C1-30 (preferably C1-10) linear, C3-30 (preferably C3-10) branched or cyclic, saturated or unsaturated, aliphatic hydrocarbon group or aromatic hydrocarbon group, the aliphatic hydrocarbon group and the aromatic hydrocarbon group are each unsubstituted or substituted with 30 fluorine, hydroxy or alkoxy, and Foreignfiling_text P23-049 - 7 - in the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is not replaced, or one or more methylene is replaced by oxy, imino or carbonyl, provided that RIa is neither hydroxy nor alkoxy. 5 Here, the above-described methylene also includes a terminal methyl. Further, the above-described "substituted with fluorine, hydroxy or alkoxy" means that a hydrogen atom directly bonded to a carbon atom in an aliphatic hydrocarbon group and aromatic hydrocarbon group is replaced with fluorine, hydroxy or alkoxy. In the present specification, the same 10 applies to other similar descriptions. In a more preferable embodiment of the present invention, in the repeating unit represented by the formula (la), RIa includes, for example, (i) alkyl, such as methyl, ethyl, propyl, butyl, pentyl, hexyl, heptyl, octyl and decyl, (ii) aryl, 15 such as phenyl, tolyl and benzyl, (iii) fluoroalkyl, such as trifluoromethyl, 2,2,2-trifluoroethyl and 3,3,3-trifluoropropyl, (iv) fluoroaryl, (v) cycloalkyl, such as cyclohexyl, (vi) a nitrogen-containing group having an amino or imide structure, such as isocyanate and amino, and (vii) an oxygen- containing group having an epoxy structure, such as glycidyl, or an acryloyl 20 structure or a methacryloyl structure. It is preferably methyl, ethyl, propyl, butyl, pentyl, hexyl and phenyl. The compound wherein RIa is methyl is preferred, since raw material thereof is easily obtained, its film hardness after curing is high and it has high chemical resistance. Further, the compound wherein RIa is phenyl is preferred since it increases solubility of 25 the polysiloxane in the solvent and the cured film becomes hardly crackable. In a preferred embodiment of the present inventions, the polysiloxane used in the present invention may further comprise a repeating unit represented 30 by formula (lb): Foreignfiling_text P23-049 - 8 - 5 wherein RIb is a group obtained by removing plural hydrogen from a nitrogen and/or oxygen-containing cycloaliphatic hydrocarbon compound having amino, imino and/or carbonyl. 10 In the formula (lb), RIb is preferably a group obtained by removing plural hydrogen, preferably two or three hydrogen, from preferably a nitrogen- containing aliphatic hydrocarbon ring having imino and/or carbonyl, more preferably a 5-membered or 6-membered ring containing nitrogen as a 15 member. For example, groups obtained by removing two or three hydrogen from piperidine, pyrrolidine or isocyanurate. RIb connects Si each other included in plural repeating units. In a preferable embodiment of the present invention, the polysiloxane used 20 in the present invention may further comprise a repeating unit represented by the formula (Ic): 25 When the mixing ratio of the repeating units represented by the formulae 30 (lb) and (Ic) is high, compatibility with solvents and additives decreases, and the film stress increases so that cracks sometimes easily generate. Therefore, it is preferably 40 mol % or less with, more preferably 20 mol % Foreignfiling_text P23-049 - 9 - or less, based on the total number of the repeating units of the polysiloxane. According to the present invention, in some embodiments, the polysiloxane used in the present invention may further comprise a repeating unit 5 represented by the formula (Id): 10 wherein RId each independently represents hydrogen, a C1- 30 (preferably C1-10) linear, C3-30 (preferably C3-10) branched or cyclic, saturated or unsaturated, 15 aliphatic hydrocarbon group or aromatic hydrocarbon group; the aliphatic hydrocarbon group and the aromatic hydrocarbon group are each unsubstituted or substituted with fluorine, hydroxy or alkoxy, and in the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is not replaced or replaced with oxy, imide or carbonyl. 20 In the repeating unit represented by the formula (Id), RId includes, for example, (i) alkyl, such as methyl, ethyl, propyl, butyl, pentyl, hexyl, heptyl, octyl and decyl, (ii) aryl, such as phenyl, tolyl and benzyl, (iii) fluoroalkyl, such as trifluoromethyl, 2,2,2-trifluoroethyl and 3,3,3-trifluoropropyl, (iv) fluoroaryl, (v) cycloalkyl, such as cyclohexyl, (vi) a nitrogen-containing 25 group having an amino or imide structure, such as isocyanate and amino, and (vii) an oxygen-containing group having an epoxy structure, such as glycidyl, or an acryloyl structure or a methacryloyl structure. It is preferably methyl, ethyl, propyl, butyl, pentyl, hexyl and phenyl. The compound wherein RId is methyl is preferred, since raw material thereof is easily 30 obtained, its film hardness after curing is high and it has high chemical resistance. Further, the compound wherein RId is phenyl is preferred since it Foreignfiling_text P23-049 - 10 - increases solubility of the polysiloxane in the solvent and the cured film becomes hardly crackable. By having the repeating unit of the above formula (Id), it is possible to make 5 the polysiloxane according to the present invention partially of a linear structure. However, since heat resistance is reduced, it is preferable that portions of linear structure are few. In particular, the repeating unit of the formula (Id) is 10 preferably 30 mol % or less, more preferably 5 mol % or less, based on the total number of the repeating units of the polysiloxane. It is also one aspect of the present invention to have no repeating unit of the formula (Id) (0 mol %). 15 The polysiloxane used in the present invention may contain two or more types of repeating units. For example, it can contain three types of repeating units having repeating units represented by the formula (la) in which RIa is methyl or phenyl and a repeating unit represented by the formula (Ic). 20 In addition, the polysiloxane used in the composition according to the present invention preferably has silanol. Here, the silanol refers to one in which an OH group is directly bonded to the Si skeleton of polysiloxane and is one in which hydroxy is directly attached to a silicon atom in the 25 polysiloxane comprising repeating units such as the above formulae (la) to (Id). That is, the silanol is composed by bonding -O0.5H to - O0.5- in the above formulae (la) to (Id). The content of the silanol in polysiloxane varies depending on the conditions for synthesizing polysiloxane, for example, the mixing ratio of the monomers, the type of the reaction catalyst and the like. 30 The content of this silanol can be evaluated by quantitative infrared absorption spectrum measurement. The absorption band assigned to Foreignfiling_text P23-049 - 11 - silanol (SiOH) appears as an absorption band having a peak in the range of 900 ± 100 cm-1 in the infrared absorption spectrum. When the content of the silanol is high, the intensity of this absorption band increases. 5 In the present invention, in order to quantitatively evaluate the silanol content, the intensity of the absorption band assigned to Si-0 is used as a reference. An absorption band having a peak in the range of 1100 ± 100 cm-1 is adopted as a peak assigned to Si-O. The silanol content can be relatively evaluated by the ratio S2/S1, which is a ratio of the integrated 10 intensity S2 of the absorption band assigned to SiOH to the integrated intensity SI of the absorption band assigned to Si-O. In the present invention, the ratio S2/S1 is preferably 0.003 to 0.15, more preferably 0.01 to 0.10. 15 The integrated intensity of the absorption band is determined in consideration of noise in the infrared absorption spectrum. In a typical infrared absorption spectrum of polysiloxane, an absorption band assigned to Si-OH having a peak in the range of 900 ± 100 cm-1 and an absorption band assigned to a Si-0 having a peak in the range of 1100 ± 100 cm-1 are 20 confirmed. The integrated intensity of these absorption bands can be measured as an area in consideration of a baseline in which noise and the like are considered. Incidentally, there is a possibility that the foot of the absorption band assigned to Si-OH and the foot of the absorption band assigned to Si-0 are overlapped; however, in such a case, the wavenumber 25 corresponding to the minimal point between the two absorption bands in the spectrum is set as their boundary. The same applies to the case where the foot of the other absorption band overlaps with the foot of the absorption band assigned to Si-OH or Si-O. 30 The mass average molecular weight of the polysiloxane used in the present invention is not particularly limited. However, the higher the molecular weight, the more the coating properties tend to be improved. On the other Foreignfiling_text P23-049 - 12 - hand, the lower the molecular weight is, the less synthesis conditions are limited, so that the synthesis is easy, and the synthesis of polysiloxane having a remarkably high molecular weight is difficult. For these reasons, the mass average molecular weight of polysiloxane is usually 500 to 5 25,000, and preferably 1,000 to 20,000 from the viewpoint of solubility in an organic solvent. Here, the mass average molecular weight means a mass average molecular weight in terms of polystyrene, which can be measured by the gel permeation chromatography based on polystyrene. 10 The synthesis method of the polysiloxane used in the present invention is not particularly limited. For example, it can be synthesized according to the method disclosed in JP 6639724 B. As stated above, publicly available polysiloxane falls under above 15 definitions can be used preferably for examples like described in WO2021/099236 A1, EP 3717966 B1. It is believed that photo-stability, chemical stability, color change because of degradation of a cured film and/or thermal stability of a cured film can be 20 improved by using / adding polysiloxane. - (Meth)acrylic polymer When acrylic polymer is used as an alkaline soluble polymer in the present invention, it can be selected from commonly used (meth)acrylic polymer, 25 preferably it is selected from acrylic polymer, such as polyacrylic acid, polymethacrylic acid, polyalkyl acrylate, polyalkyl methacrylate. It is believed that by using (meth)acrylic polymer, thicker layer, lowering process temperature and/or improving etching property, can be realized. 30 The acrylic polymer used in the present invention preferably comprises a repeating unit containing an acryloyl group. It is also preferable that the Foreignfiling_text P23-049 - 13 - acrylic polymer further comprises a repeating unit containing a carboxy group and/or a repeating unit containing an alkoxysilyl group. Although the repeating unit containing a carboxy group is not particularly 5 limited as long as it is a repeating unit containing a carboxy group at its side chain, a repeating unit derived from an unsaturated carboxylic acid, an unsaturated carboxylic anhydride or a mixture thereof is preferable. Although the repeating unit containing an alkoxysilyl group can be a 10 repeating unit containing an alkoxysilyl group at its side chain, it is preferably a repeating unit derived from a monomer represented by the following formula (B): XB-(CH2)a-Si(ORB)b(CH3)3-b (B) wherein, 15 XB is a vinyl group, a styryl group or a (meth)acryloyloxy group, and RB is a methyl group or an ethyl group, a is an integer of 0 to 3, and b is an integer of 1 to 3. Further, it is preferable that the above-described polymer contains a 20 repeating unit containing a hydroxy group derived from a hydroxy group- containing unsaturated monomer. The mass average molecular weight of the acrylic polymer used in the present invention is not particularly limited, and is preferably 1,000 to 25 40,000, more preferably 2,000 to 30,000. The mass average molecular weight is a mass average molecular weight in terms of polystyrene according to gel permeation chromatography. The content of the acrylic polymer (II) is preferably 18.0 to 35.0 mass%, 30 and more preferably 20.0 to 32.0 mass%, based on the total mass of the composition. Foreignfiling_text P23-049 - 14 - The content of the acrylic polymer (II) is preferably 65.0 to 92.0 mass%, and more preferably 70.0 to 90.0 mass%, based on the total mass of the polysiloxane (I) and the acrylic polymer (II). 5 In a preferable embodiment of the present invention, said alkali-soluble polymer is a polysiloxane, or a combination of a polysiloxane and an acrylic polymer, and the total amount of the polysiloxane is in the range from 1 to 40 mass% based on the total mass of the composition without solvent, preferably it is from 5 to 35 mass%, more preferably from 10 to 30 mass%. 10 In a preferable embodiment of the present invention, said acrylic polymer is selected from one or more members of the group consisting of polyacrylic acid, polymethacrylic acid, polyalkyl acrylate, polyalkyl methacrylate. Preferably the total amount of the acrylic polymer in the composition is in 15 the range from 65 to 99 mass%, more preferably from 70 to 90 mass%, based on the total mass of the composition without solvent. (II) Polymerization initiator The composition according to the present invention comprises a 20 polymerization initiator. The polymerization initiator includes a polymerization initiator that generates an acid, a base or a radical by radiation, and a polymerization initiator that generates an acid, a base or a radical by heat. In the present invention, the former is preferable and the photo radical generator is more preferable, in terms of process shortening 25 and cost since the reaction is initiated immediately after the irradiation of radiation and the reheating process performed after the irradiation of radiation and before the development process can be eliminated. The photo radical generator can improve the resolution by strengthening 30 the shaped pattern or increasing the contrast of development. The photo radical generator used in the present invention is a photo radical generator that emits a radical when irradiated with radiation. Examples of the Foreignfiling_text P23-049 - 15 - radiation include visible light, ultraviolet light, infrared light, X-ray, electron beam, α-ray, and γ-ray. The content of the photo radical generator is preferably 0.001 to 30 mass%, 5 and more preferably 0.01 to 10 mass%, based on the total mass of the component (I) and the component (II), though the optimal amount thereof depends on the type and amount of active substance generated by decomposition of the photo radical generator, the required photosensitivity, and the required dissolution contrast between the exposed area and 10 unexposed area. If the content is less than 0.001 mass%, the dissolution contrast between the exposed area and unexposed portion is too low, and the addition effect is not sometimes exhibited. On the other hand, when the content of the photo radical generator is more than 30 mass%, cracks are generated in the coated film and colorless transparency of the coated film 15 sometimes degrades, because coloring becomes remarkable due to decomposition of the photo radical generator. When the content becomes large, thermal decomposition may cause deterioration of the electrical insulation of the cured product and release of 20 gas, which sometimes becomes a problem in subsequent processes. Further, the resistance of the coated film to a photoresist stripper containing monoethanolamine or the like as a main component sometimes deteriorates. 25 Examples of the photo radical generator include azo-based, peroxide- based, acylphosphine oxide-based, alkylphenone-based, oxime ester- based, and titanocene-based initiators. Among them, alkylphenone-based, acylphosphine oxide-based and oxime ester-based initiators are preferred, and 2,2-dimethoxy-1,2-diphenylethan-1-one, 1-hydroxy-cyclohexylphenyl 30 ketone, 2-hydroxy-2-methyl-1-phenylpropan-1-one, 1-[4-(2- hydroxyethoxy)phenyl]-2-hydroxy-2-methyl-1-propan-1-one, 2-hydroxy-1-{4- [4-(2-hydroxy-2-methylpropionyl)-benzyl]phenyl}-2-methylpropan-1-one, 2- Foreignfiling_text P23-049 - 16 - methyl-1-(4-methylthiophenyl)-2-morpholinopropan-1-one, 2-benzyl-2- dimethylamino-1-(4-morpholinophenyl)-1-butanone, 2-(dimethylamino)-2- [(4-methylphenyl)methyl]-1-[4-(4-morpholinyl)- phenyl]-1-butanone, 2,4,6- trimethylbenzoyldiphenyl-phosphine oxide, bis(2,4,6-trimethylbenzoyl)- 5 phenylphosphine oxide, 1,2-octanedione-1-[4-(phenylthio)-2-(O- benzoyloxime)], 1-[9-ethyl-6-(2-methylbenzoyl)-9H-carbazol-3-yl]ethanone- 1-(O-acetyloxime) are included. (III) Scattering particles 10 According to the present invention, preferably the average particle size of the scattering particle is 200 nm or more and 10 μm or less, preferably from 230nm-5μm, more preferably from 250nm to 2μm. In case of the scattering particle is an inorganic particle, preferably the average particle size is in the range from 200nm to 1μm, preferably from 230 to 800nm, more preferably 15 from 250 to 700nm, even more preferably from 300 to 600nm; and in case of the scattering particle is an organic particle, preferably the average particle size is in the range from 300nm to 10μm, more preferably from 500nm to 5μm, even more preferably from 700nm to 3μm, furthermore preferably from 800nm to 2μm. 20 In one preferable embodiment of the present invention, the scattering particle has the refractive index greater than the refractive index of the mixture of the polysiloxane and the acrylic polymer, preferably the scattering particle is configured to have the refractive index greater than the 25 refractive index of a matrix polymer derived from the polysiloxane and an acrylic polymer by polymerization. Preferably said refractive index of the scattering particle is 1.6 or more, preferably it is 1.7 or more, and 2.4 or less, preferably 2.2 or less. The most preferably from 1.8 to 2.0. When 2 or more different scattering particles are used in the composition, then the 30 average refractive index of the scattering particles is 1.6 or more, preferably it is 1.7 or more, and 2.4 or less, preferably 2.2 or less. The most preferably from 1.8 to 2.0. Foreignfiling_text P23-049 - 17 - It is believed that the above mentioned high refractive index of the scattering particle realizes increased scatter effect. Namely, when said scattering particle has the average particle size described above, and has 5 the refractive index value indicated above, said scattering effect becomes most optimal in the obtained optical layer. In another preferred embodiment, the scattering particle is an organic particle and the difference X of the refractive index of the scattering particle 10 and the refractive index of the mixture of the polysiloxane and the acrylic polymer is in the range from -0.2 to +0.2. Preferably the difference X’ of the refractive index of the scattering particle and the refractive index of a matrix polymer derived from the polysiloxane and an acrylic polymer by polymerization, is in the range from -0.2 to +0.2. 15 X: the refractive index of the scattering particle – the refractive index of the mixture = -0.2 to +0.2, preferably -0.1 to +0.1 X’: the refractive index of the scattering particle - the refractive index of a matrix polymer derived from the polysiloxane and an acrylic polymer by 20 polymerization = from -0.2 to +0.2, preferably from -0.1 to +0.1 When a mixture of organic particles are used as the scattering particle, then the definition of X is: the average refractive index of the scattering particle – the refractive index of the mixture = -0.2 to +0.2, preferably -0.1 to +0.1 And the definition of X’ is: the average refractive index of the scattering 25 particle - the refractive index of a matrix polymer derived from the polysiloxane and an acrylic polymer by polymerization = in the range from - 0.2 to +0.2, preferably from -0.1 to +0.1. When the scattering particle is an organic particle and the difference X of 30 the refractive index of the scattering particle and the refractive index of the mixture of the polysiloxane and the acrylic polymer is in the range defined above, incident light may pass though said scattering particle well. Foreignfiling_text P23-049 - 18 - When the organic scatter is used in the optical layer (composite), it is believed that the outermost surface of the obtained optical layer (composite) has surface roughness caused by the organic scatter, and on 5 the surface of said roughness, when the light goes out from the optical layer (composite), the direction of the light is changed. It generates scattering effect effectively, preferably without causing loss of light within the optical layer. 10 As such scattering particles, any publicly known inorganic/organic scattering particles satisfying the above-mentioned conditions can be used preferably. Such as, the scattering particles used in the working examples can be used preferably. 15 - Solvent In a preferred embodiment of the present invention, the composition further comprises a solvent from the viewpoint of improved handling, coating, coating of the composition when string it or when fabricating a layer. 20 Preferably said solvent is an organic solvent, more preferably said solvent is an organic solvent selected from one or more members of the group consisting of ethylene glycol monoalkyl ethers, preferably it is ethylene glycol monomethyl ether, ethylene glycol monoethyl ether, ethylene glycol monopropyl ether and/or ethylene glycol monobutyl ether; diethylene glycol 25 dialkyl ethers, preferably it is diethylene glycol dimethyl ether, diethylene glycol diethyl ether, diethylene glycol dipropyl ether and/or diethylene glycol dibutyl ether; propylene glycol monoalkyl ethers, preferably it is propylene glycol monomethyl ether(PGME), propylene glycol monoethyl ether and/or propylene glycol monopropyl ether; ethylene glycol alkyl ether acetates, 30 preferably it is methyl cellosolve acetate and/or ethyl cellosolve acetate; propylene glycol alkyl ether acetates, preferably it is propylene glycol monomethyl ether acetate (PGMEA), propylene glycol monoethyl ether Foreignfiling_text P23-049 - 19 - acetate and/or propylene glycol monopropyl ether acetate; ketones, preferably it is methyl ethyl ketone, acetone, methyl amyl ketone, methyl isobutyl ketone and/or cyclohexanone; alcohols, preferably it is ethanol, propanol, butanol, hexanol, cyclo hexanol, ethylene glycol, propylene 5 glycol, triethylene glycol and/or glycerin; esters, preferably it is ethyl 3- ethoxypropionate, methyl 3-methoxypropionate and/or ethyl lactate; and cyclic esters, preferably it is gamma-butyro-lactone; chlorinated hydrocarbons, preferably it is chloroform, dichloromethane, chlorobenzene; trimethyl benzenes, preferably it is 1,3,5-trimethylbenzene, 1,2,4-trimethyl 10 benzene, 1,2,3-trimethyl benzene, docecylbenzene, cyclohexylbenzene, 1,2,3,4-tetramethylbenzene, 1,2,3,5-tetramethylbenzene, 3- isopropylbiphenyl, 3-methylbiphenyl, 4-methylbiphenyl; and dichlorobenzene; preferably said solvent is ethylene glycol monoalkyl ethers, diethylene glycol dialkyl ethers, propylene glycol, ethylene glycol, 15 propylene glycol monoalkyl ethers, ethylene glycol alkyl ether acetates, propylene glycol alkyl ether acetate, more preferably said solvent is selected from propylene glycol alkyl ether acetates, ethylene glycol monoalkyl ethers, propylene glycol and propylene glycol monoalkyl ethers. 20 It is believed that above selected solvents have good compatibility with the composition, boiling points, viscosity and/or vapor pressure, realizing better handling of the composition, suitable for lower temperature fabrication of the layer and/or realizing an easy fabrication. 25 In a preferred embodiment of the present invention, the total amount of the solvent based on the total amount of polysiloxane is 0 to 300 wt %. When the composition contains a solvent, preferably from 0.1 to 150wt%, more preferably from 50 to 90wt%. 30 - Compound containing two or more (meth)acryloxyloxy groups According to the present invention, in a preferable embodiment, the composition further comprises a compound containing two or more Foreignfiling_text P23-049 - 20 - (meth)acryloyloxy groups (hereinafter sometimes referred to as (meth)acryloyloxy group-containing compound), preferably the content of the compound is in the range from 10.0 to 25.0 mass% based on the total mass of the composition without solvent. 5 The (meth)acryloyloxy group is a general term for the acryloyloxy group and the methacryloyloxy group. This compound is a compound that can form a crosslinked structure by reacting with the polysiloxane (I), acrylic polymer (II) and the like. In order to form a crosslinked structure, a compound 10 containing two or more (meth)acryloyloxy groups, which are reactive groups, is needed. In order to form a higher-order crosslinked structure, it preferably contains three or more (meth)acryloyloxy groups. As such a compound containing two or more (meth)acryloyloxy groups, 15 esters obtained by reacting (α) a polyol compound having two or more hydroxy groups with (β) two or more (meth)acrylic acids are preferably used. As the polyol compound (α), compounds having, as a basic skeleton, a saturated or unsaturated aliphatic hydrocarbon, aromatic hydrocarbon, heterocyclic hydrocarbon, primary, secondary or tertiary amine, ether or the 20 like, and having, as substituents, two or more hydroxy groups are included. The polyol compound can contain other substituents, for example, a carboxy group, a carbonyl group, an amino group, an ether bond, a thiol group, a thioether bond, and the like, as long as the effects of the present invention are not impaired. 25 Preferred polyol compounds include alkyl polyols, aryl polyols, polyalkanolamines, cyanuric acid, and dipentaerythritol. When the polyol compound (α) has three or more hydroxy groups, it is not necessary that all the hydroxy groups have reacted with (meth)acrylic acid, and they can be 30 partially esterified. This means that the esters can have unreacted hydroxy group(s). Foreignfiling_text P23-049 - 21 - As such esters, tris(2-acryloxyethyl)isocyanurate, bis(2- acryloxyethyl)isocyanurate, dipentaerythritol hexa(meth)acrylate, tripentaerythritol octa(meth) acrylate, pentaerythritol tetra(meth)acrylate, dipropylene glycol diacrylate, tripropylene glycol diacrylate, 5 trimethylolpropane triacrylate, polytetramethylene glycol dimethacrylate, trimethylolpropane trimethacrylate, ditrimethylolpropane tetraacrylate, tricyclodecane dimethanol diacrylate, 1,9-nonanediol diacrylate, 1,6- hexanediol diacrylate, 1,10-decanediol diacrylate are included. 10 The composition according to the present invention comprises a combination of two or more kinds of the (meth)acryloyloxy group-containing compounds, and preferably a combination of three or more kinds of the (meth)acryloyloxy group-containing compounds. In one preferred embodiment of the present invention, the composition according to the 15 present invention comprises a combination of three kinds of the (meth)acryloyloxy group-containing compounds. Without wishing to be bound by theory, it is considered that the combination of the (meth)acryloyloxy group-containing compounds with different glass 20 transition temperatures can suppress rapid thermal reflow in the post baking process, which can lead to form a certain taper angle. Preferably, at least one of two or more kinds of the (meth)acryloyloxy group-containing compounds is the compound containing three or more 25 (meth)acryloyloxy groups. More preferably, at least one is the compound containing three or more (preferably three) (meth)acryloyloxy groups, and at least one is the compound containing two (meth)acryloyloxy groups. Further preferably, in order to make the pattern surface smoother, the component (III) is a combination of one kind of the compound containing 30 three (meth)acryloyloxy groups and two kinds of the compounds containing two (meth)acryloyloxy groups. Foreignfiling_text P23-049 - 22 - In the composition according to the present invention, the content of the compounds containing three or more (meth)acryloyloxy groups is preferably 20.0 to 50.0 mass%, and more preferably 30.0 to 40.0 mass%, based on 5 the total mass of the component (III). In another embodiment of the present invention, in order to improve alkali solubility during development and heat resistance of the cured film, the component (III) preferably comprises the compound having an isocyanurate 10 structure. In particular, such compounds include tris(2- acryloyloxyethyl)isocyanurate, bis(2-acryloyloxyethyl)isocyanurate, tris(3-acryloyloxypropyl)isocyanurate, bis(3-acryloyloxypropyl)isocyanurate, 15 tris(4-acryloyloxybutyl)isocyanurate, bis(4-acryloyloxybutyl)isocyanurate, and preferably tris(2- acryloyloxyethyl)isocyanurate. In the composition according to the present invention, the content of the 20 compound having an isocyanurate structure is preferably 10.0 to 50.0 mass%, and more preferably 10.0 to 40.0 mass%, based on the total mass of the component (III). From the viewpoint of the reactivity, the molecular weight of the compound 25 containing two or more (meth)acryloyloxy groups is preferably 200 to 2,000, and more preferably 200 to 1,500. Although the content of the component (III) is adjusted according to the type of the polymer or the (meth)acryloyloxy group-containing compound to 30 be used, it is preferably 10.0 to 25.0 mass%, and more preferably 10.0 to 20.0 mass%, based on the total mass of the polysiloxane (I) and the acrylic polymer (II) from the viewpoint of compatibility with polymers. Foreignfiling_text P23-049 - 23 - - Additives In some embodiments of the present invention, optionally, the composition may further comprise one or more of additives. However, in some case, the 5 amount of said additive can be zero. Such additive may be selected from one or more members of the group consisting of, for examples, surfactants, adhesion promoter, silane coupling agent, thermal acid generators, thermal base generators, crosslinkable monomers and polymerization initiators. Publicly available ones can be used preferably, like described in EP 10 3717966 A1 or WO 2021/099236 A1. Since said additive is not mandatory for this invention, the amount of the additive in the composition or in the layer based on the total amount of polysiloxane is preferably 5wt% or less, more preferably 1wt% or less. The composition and/or a layer obtained from the composition may not contain any said additives. 15 In another aspect, present invention further relates to a method of preparing the composition of the present invention comprising at least, essentially consisting of or consisting of the following steps; (X) mixing at least 20 (I) an alkaline soluble polymer, preferably it is a polysiloxane, an acrylic polymer, or a combination of a polysiloxane and an acrylic polymer; (II) a polymerization initiator; and (III) a scattering particle. Preferably said mixing step (X) is performed in the presence of a solvent, 25 more preferably in the presence of an organic solvent. Preferably a compound containing two or more (meth)acryloyloxy groups is also mixed in the mixing step (X) to form the composition. In another aspect, present invention further relates to a composition 30 obtained or obtainable by the method of fabricating the composition described above. Foreignfiling_text P23-049 - 24 - In another aspect, present invention also relates to use of the composition of the present invention for preparing an optical layer containing a metal oxide, preferably for preparing a composite, more preferably for preparing a layered composite. 5 In another aspect, present invention further relates to a method of fabricating a composite of the present invention comprising at least, essentially consisting of or consisting of the following steps; (Xi) applying the composition of the present invention onto a layer or onto a 10 substrate to form a coated layer; and (Xii) baking a coated layer to obtain a composite (post baking process). Preferably the method further comprises one or more of the following steps after step (Xi) and before the step (Xii): (Xiii) Applying a pre-baking (heat treatment) of the coating layer in order to 15 dry the coated layer and reduce the residual amount of the solvent in the coated layer; (Xiv) irradiating the coated layer with light (applying light irradiation), preferably with light having peak maximum wavelength in the range from 360 to 430 nm, preferably a patterning mask is used when light irradiation is 20 conducted; (Xv) applying post exposure baking process; and/or (Xvi) applying developing process to form a patterned cured layer. (1) Application process 25 First, the above-described composition is applied above a substrate. In the present invention, the "above a substrate” includes the case where the composition is applied directly on a substrate and the case where the composition is applied on a substrate via one or more intermediate layer. Formation of the coating film of the composition in the present invention can 30 be carried out by any method conventionally known as a method for applying a photosensitive composition. It can be freely selected from dip coating, roll coating, bar coating, brush coating, spray coating, doctor Foreignfiling_text P23-049 - 25 - coating, flow coating, spin coating, slit coating, and the like. As the substrate on which the composition is applied, a suitable substrate such as a silicon substrate, a glass substrate, a resin film, and the like can be used. Various semiconductor devices and the like can be formed on these 5 substrates as needed. When the substrate is a film, gravure coating can also be utilized. If desired, a drying process can be additionally provided after applying the film. Further, if necessary, the applying process can be repeated once, twice, or more to make the film thickness of the coating film to be formed as desired. 10 (2) Pre-baking process After forming the coating film of the composition by applying the composition, it is preferable to carry out pre-baking (heat treatment) of the coating film in order to dry the coating film and reduce the residual amount 15 of the solvent in the coating film. The pre-baking process can be carried out at a temperature of generally 50 to 150°C, preferably 90 to 120°C, in the case of a hot plate, for 10 to 300 seconds, preferably 30 to 120 seconds and in the case of a clean oven, for 1 to 30 minutes. 20 (3) Exposure process (light irradiation) After forming a coating film, the coating film surface is then irradiated with light. As the light source to be used for the light irradiation, any one conventionally used for a pattern forming method can be used. As such a light source, a high-pressure mercury lamp, a low-pressure mercury lamp, a 25 lamp such as metal halide and xenon, a laser diode, an LED, and the like can be included. As the irradiation light, ultraviolet ray such as g-line, h-line and i-line is usually used. Except ultrafine processing for semiconductors or the like, it is general to use light of 360 to 430 nm (high-pressure mercury lamp) for patterning of several μm to several dozen μm. Above all, in the 30 case of liquid crystal display devices, light of 430 nm is often used. In such a case, as described above, it is advantageous to combine a sensitizing dye with the composition according to the present invention. The energy of Foreignfiling_text P23-049 - 26 - the irradiation light is generally 5 to 2,000 mJ/cm2, preferably 10 to 1,000 mJ/cm2, although it depends on the light source and the film thickness of the coating film. If the irradiation light energy is lower than 5 mJ/cm2, sufficient resolution cannot be obtained in some cases. On the other hand, 5 when the irradiation light energy is higher than 2,000 mJ/cm2, the exposure becomes excess and halation sometimes occurs. In order to irradiate light in a pattern shape, a general photomask can be used. Such a photomask can be freely selected from well-known ones. 10 The environment at the time of irradiation is not particularly limited and can generally be set as an ambient atmosphere (in the air) or nitrogen atmosphere. Further, in the case of forming a film on the entire surface of the substrate, light irradiation can be performed over the entire surface of the substrate. In the present invention, the pattern film also includes such a 15 case where a film is formed on the entire surface of the substrate. (4) Post exposure baking process After the exposure, to promote the reaction between the polymer in the film by the polymerization initiator, post exposure baking can be performed, as 20 necessary. Different from the heating process (6) to be described later, this heating treatment is performed not to completely cure the coating film but to leave only a desired pattern on the substrate after development and to make other areas capable of being removed by development. Therefore, it is not essential in the present invention. 25 When the post exposure baking is performed, a hot plate, an oven, a furnace, and the like can be used. The heating temperature should not be excessively high because it is not desirable for the acid, base or radical in the exposed area, which is generated by light irradiation, to diffuse to the 30 unexposed area. From such a viewpoint, the range of the heating temperature after exposure is preferably 40 to 150°C, and more preferably 60 to 120°C. Stepwise heating can be applied as needed to control the Foreignfiling_text P23-049 - 27 - curing rate of the composition. Further, the atmosphere during the heating is not particularly limited and can be selected from in an inert gas such as nitrogen, under a vacuum, under a reduced pressure, in an oxygen gas, and the like, for the purpose of controlling the curing rate of the 5 composition. Further, the heating time is preferably above a certain level in order to maintain higher the uniformity of temperature history in the wafer surface and is preferably not excessively long in order to suppress diffusion of the generated acid, base or radical. From such a viewpoint, the heating time is preferably 20 seconds to 500 seconds, and more preferably 40 10 seconds to 300 seconds. (5) Developing process After post-exposure baking is optionally performed after exposure, the coating film is developed. As the developer to be used at the time of 15 development, any developer conventionally used for developing a photosensitive composition can be used. Preferable examples of the developer include an alkali developer which is an aqueous solution of an alkaline compound such as tetraalkylammonium hydroxide, choline, alkali metal hydroxide, alkali metal metasilicate (hydrate), alkali metal phosphate 20 (hydrate), ammonia, alkylamine, alkanolamine and heterocyclic amine, and a particularly preferable alkali developer is tetramethylammonium hydroxide (TMAH) aqueous solution, a potassium hydroxide aqueous solution, or a sodium hydroxide aqueous solution. In this alkali developer, a water- soluble organic solvent such as methanol and ethanol, or a surfactant can 25 be further contained, if necessary. The developing method can also be freely selected from conventionally known methods. Specifically, methods such as dipping in a developer (dip), paddle, shower, slit, cap coat, spray, and the like can be included. After the development with a developer, by which a pattern can be obtained, it is preferable that rinsing with water is 30 carried out. Foreignfiling_text P23-049 - 28 - (6) Post baking process After development, the obtained pattern film is cured by heating. As the heating apparatus used for the heating process, the same one as used for the above-described post-exposure baking can be used. The heating 5 temperature in the heating process is not particularly limited as long as it is a temperature at which curing of the coating film can be performed and can be freely determined. However, if the silanol group of the polysiloxane remains, the chemical resistance of the cured film sometimes becomes insufficient, or dielectric constant of the cured film sometimes becomes 10 higher. From such a viewpoint, a relatively high temperature is generally selected as the heating temperature. In order to keep the remaining film ratio after curing high, the curing temperature is more preferably 350°C or lower, and particularly preferably 250°C or lower. On the other hand, in order to accelerate the curing reaction and obtain a sufficiently cured film, 15 the curing temperature is preferably 70°C or higher, more preferably 80°C or higher, and particularly preferably 90°C or higher. The heating time is not particularly limited and is generally 10 minutes to 24 hours, and preferably 30 minutes to 3 hours. In addition, this heating time is a time from when the temperature of the pattern film reaches a desired heating 20 temperature. Usually, it takes about several minutes to several hours for the pattern film to reach a desired temperature from the temperature before heating. In another aspect, present invention further relates to a composite, 25 preferably being a layered composite, preferably said layered composite is an optical layer, obtained or obtainable by the method of fabricating a composite, of the present invention explained above. Preferably said layer is a protection layer of an electric device. Preferably said curing is a heat curing and/or UV light curing. 30 In another aspect, present invention further relates to a composite, preferably being a layered composite, preferably said layered composite is Foreignfiling_text P23-049 - 29 - an optical layer, comprising at least, essentially consisting of or consisting of; i) a polymer (A) derived or derivable from at least (I) an alkaline soluble polymer, preferably said alkaline soluble polymer is a polysiloxane, an 5 acrylic polymer, or a combination of a polysiloxane and an acrylic polymer; and (III) a scattering particle. Preferably said polymer (A) is derived or derivable from at least (I) the alkaline soluble polymer, and (II) a polymerization initiator; more preferably 10 it is derived or derivable from at least (I) the alkaline soluble polymer, (II) a polymerization initiator and a compound containing two or more (meth)acryloyloxy groups. In a preferable embodiment of the present invention, said composite 15 contains one or more organic particles as the scattering particle, and the outermost surface of the composite has an uneven structure, preferably the surface of the composite has finely roughened structure, more preferably the whole surface of the composite has finely roughened structure, even more preferably said uneven structure and finely roughened structure are 20 caused by said organic one or more organic particles. In a preferable embodiment of the present invention, the composite has the average layer thickness in the rage from 1μm to 200μm, preferably from 1.5 to 100μm, more preferably from 2 to 100μm. 25 In another aspect, present invention further relates to a display device comprising at least one functional medium configured to modulate a light or configured to emit light; and the composite of the present invention. 30 Preferably said display device is selected from the group consisting of OLED, LCD, LED and μLED. Thus, said functional medium is an OLED layer, LCD layer, LED array and/or μLED array. Foreignfiling_text P23-049 - 30 - Preferable embodiments 1. A photosensitive composition comprising at least; (I) an alkaline soluble polymer, preferably it is a polysiloxane, an acrylic polymer, or a combination of a polysiloxane and an acrylic polymer; 5 (II) a polymerization initiator; and (III) a scattering particle. Preferably said photosensitive composition is a negative type of photosensitive composition, preferably said photosensitive composition is to be used for fabricating a protection layer of an electronic device. Preferably 10 said photosensitive composition is a filling composition to be used for fabricating an electronic device, more preferably it is a filing composition for an LED or μLED. 2. The composition of embodiment 1, wherein said scattering particle is 15 selected from inorganic particles, organic particles and a mixture of inorganic particles and organic particles. 3. The composition of embodiment 1 or 2, wherein the average particle size of the scattering particle is 200 nm or more and 10 μm or less, preferably 20 from 230nm-5μm, more preferably from 250nm to 2μm. In case of the scattering particle is an inorganic particle, preferably the average particle size is in the range from 200nm to 1μm, preferably from 230 to 800nm, more preferably from 250 to 700nm, even more preferably from 300 to 600nm; and in case of the scattering particle is an organic particle, 25 preferably the average particle size is in the range from 300nm to 10μm, more preferably from 500nm to 5μm, even more preferably from 700nm to 3μm, furthermore preferably from 800nm to 2μm. 4. The composition of any one of the preceding embodiments, wherein said 30 scattering particle has the refractive index greater than the refractive index of the mixture of the polysiloxane and the acrylic polymer, preferably the scattering particle is configured to have the refractive index greater than the Foreignfiling_text P23-049 - 31 - refractive index of a matrix polymer derived from the polysiloxane and an acrylic polymer by polymerization. Preferably said refractive index of the scattering particle is 1.6 or more, preferably it is 1.7 or more, and 2.4 or less, preferably 2.2 or less. The most preferably from 1.8 to 2.0. When 2 or 5 more different scattering particles are used in the composition, then the average refractive index of the scattering particles is 1.6 or more, preferably it is 1.7 or more, and 2.4 or less, preferably 2.2 or less. The most preferably from 1.8 to 2.0. 10 5. The composition of any one of embodiments 1 to 3, wherein the scattering particle is an organic particle and the difference X of the refractive index of the scattering particle and the refractive index of the mixture of the polysiloxane and the acrylic polymer is in the range from -0.2 to +0.2. Preferably the difference X’ of the refractive index of the scattering 15 particle and the refractive index of a matrix polymer derived from the polysiloxane and an acrylic polymer by polymerization, is in the range from -0.2 to +0.2. X: the refractive index of the scattering particle – the refractive index of the 20 mixture = -0.2 to +0.2, preferably -0.1 to +0.1 X’: the refractive index of the scattering particle - the refractive index of a matrix polymer derived from the polysiloxane and an acrylic polymer by polymerization = from -0.2 to +0.2, preferably from -0.1 to +0.1 When a mixture of organic particles is used as the scattering particle, then 25 the definition of X is: the average refractive index of the scattering particle – the refractive index of the mixture = -0.2 to +0.2, preferably -0.1 to +0.1 And the definition of X’ is: the average refractive index of the scattering particle - the refractive index of a matrix polymer derived from the polysiloxane and an acrylic polymer by polymerization = from -0.2 to +0.2, 30 preferably from -0.1 to +0.1. Foreignfiling_text P23-049 - 32 - 6. The composition of any one of the preceding embodiments, wherein said alkali-soluble polymer is a polysiloxane, or a combination of a polysiloxane and an acrylic polymer, preferably the polysiloxane comprises a repeating unit of chemical formula (Ia). 5 wherein 10 RIa is hydrogen, a C1-30 (preferably C1-10) linear, C3-30 (preferably C3-10) branched or cyclic, saturated or unsaturated, aliphatic hydrocarbon group or aromatic hydrocarbon group, the aliphatic hydrocarbon group and the aromatic hydrocarbon group are each unsubstituted or substituted with fluorine, hydroxy or alkoxy, and 15 in the aliphatic hydrocarbon group and the aromatic hydrocarbon group, methylene is not replaced, or one or more methylene is replaced by oxy, imino or carbonyl, provided that RIa is neither hydroxy nor alkoxy. 7. The composition of any one of the preceding embodiments, wherein said 20 alkali-soluble polymer is a polysiloxane, or a combination of a polysiloxane and an acrylic polymer, and the polysiloxane comprises a repeating unit of chemical formula (Ib). 25 wherein 30 RIb is a group obtained by removing plural hydrogen from a nitrogen and/or oxygen-containing cycloaliphatic hydrocarbon compound having amino, imino and/or carbonyl. Foreignfiling_text P23-049 - 33 - RIb is preferably a group obtained by removing plural hydrogen, preferably two or three hydrogen, from preferably a nitrogen-containing aliphatic hydrocarbon ring having imino and/or carbonyl, more preferably a 5- membered or 6-membered ring containing nitrogen as a member. For 5 example, groups obtained by removing two or three hydrogen from piperidine, pyrrolidine or isocyanurate. RIb connects Si each other included in plural repeating units. 8. The composition of any one of the preceding embodiments, wherein said 10 alkali-soluble polymer is a polysiloxane, or a combination of a polysiloxane and an acrylic polymer, and the total amount of the polysiloxane is in the range from 1 to 40 mass% based on the total mass of the composition without solvent, preferably it is from 5 to 35 mass%, more preferably from 10 to 30 mass%. 15 9. The composition of any one of the preceding embodiments, wherein an alkali-soluble polymer is an acrylic polymer, or a combination of a polysiloxane and an acrylic polymer, preferably said acrylic polymer is selected from one or more members of the group consisting of polyacrylic 20 acid, polymethacrylic acid, polyalkyl acrylate, polyalkyl methacrylate. Preferably the total amount of the acrylic polymer in the composition is in the range from 65 to 99 mass%, more preferably from 70 to 90 mass%, based on the total mass of the composition without solvent. 25 10. The composition of any one of the preceding embodiments, further comprises a solvent, preferably said solvent is an organic solvent, more preferably said solvent is an organic solvent selected from one or more members of the group consisting of ethylene glycol monoalkyl ethers, preferably it is ethylene glycol monomethyl ether, ethylene glycol monoethyl 30 ether, ethylene glycol monopropyl ether and/or ethylene glycol monobutyl ether; diethylene glycol dialkyl ethers, preferably it is diethylene glycol dimethyl ether, diethylene glycol diethyl ether, diethylene glycol dipropyl Foreignfiling_text P23-049 - 34 - ether and/or diethylene glycol dibutyl ether; propylene glycol monoalkyl ethers, preferably it is propylene glycol monomethyl ether(PGME), propylene glycol monoethyl ether and/or propylene glycol monopropyl ether; ethylene glycol alkyl ether acetates, preferably it is methyl cellosolve 5 acetate and/or ethyl cellosolve acetate; propylene glycol alkyl ether acetates, preferably it is propylene glycol monomethyl ether acetate (PGMEA), propylene glycol monoethyl ether acetate and/or propylene glycol monopropyl ether acetate; ketones, preferably it is methyl ethyl ketone, acetone, methyl amyl ketone, methyl isobutyl ketone and/or 10 cyclohexanone; alcohols, preferably it is ethanol, propanol, butanol, hexanol, cyclo hexanol, ethylene glycol, propylene glycol, triethylene glycol and/or glycerin; esters, preferably it is ethyl 3-ethoxypropionate, methyl 3- methoxypropionate and/or ethyl lactate; and cyclic esters, preferably it is gamma-butyro-lactone; chlorinated hydrocarbons, preferably it is 15 chloroform, dichloromethane, chlorobenzene; trimethyl benzenes, preferably it is 1,3,5-trimethylbenzene, 1,2,4-trimethyl benzene, 1,2,3- trimethyl benzene, docecylbenzene, cyclohexylbenzene, 1,2,3,4- tetramethylbenzene, 1,2,3,5-tetramethylbenzene, 3-isopropylbiphenyl, 3- methylbiphenyl, 4-methylbiphenyl; and dichlorobenzene; preferably said 20 solvent is ethylene glycol monoalkyl ethers, diethylene glycol dialkyl ethers, propylene glycol, ethylene glycol, propylene glycol monoalkyl ethers, ethylene glycol alkyl ether acetates, propylene glycol alkyl ether acetate, more preferably said solvent is selected from propylene glycol alkyl ether acetates, ethylene glycol monoalkyl ethers, propylene glycol and propylene 25 glycol monoalkyl ethers. 11. The composition of any one of the preceding embodiments, further comprises a compound containing two or more (meth)acryloyloxy groups, preferably the content of the compound is in the range from 10.0 to 25.0 30 mass% based on the total mass of the composition without solvent. Foreignfiling_text P23-049 - 35 - 12. Method of preparing the composition of any one of the preceding embodiments, containing at least the following step; (X) mixing at least (I) an alkaline soluble polymer, preferably it is a polysiloxane, an acrylic 5 polymer, or a combination of a polysiloxane and an acrylic polymer; (II) a polymerization initiator; and (III) a scattering particle. Preferably said mixing step (X) is performed in the presence of a solvent, more preferably in the presence of an organic solvent. Preferably a 10 compound containing two or more (meth)acryloyloxy groups is also mixed in the mixing step (X) to form the composition. 13. Use of the composition of any one of embodiments 1 to 11 for preparing an optical layer containing a metal oxide, preferably for preparing a 15 composite, more preferably for preparing a layered composite. 14. Method of fabricating a composite, comprising steps of: (Xi) applying the composition of any one of the embodiments 1 to 11 onto a layer or onto a substrate to form a coated layer; and 20 (Xii) baking a coated layer to obtain a composite. Preferably the method further comprises one or more of the following steps after step (Xi) and before the step (Xii): (Xiii) Applying a pre-baking (heat treatment) of the coating layer in order to dry the coated layer and reduce the residual amount of the solvent in the 25 coated layer; (Xiv) irradiating the coated layer with light (applying light irradiation), preferably with light having peak maximum wavelength in the range from 360 to 430 nm, preferably a patterning mask is used when light irradiation is conducted; 30 (Xv) applying post exposure baking process; and/or (Xvi) applying developing process to form a patterned cured layer. Foreignfiling_text P23-049 - 36 - 15. A composite, preferably being a layered composite, preferably said layered composite is an optical layer, obtained or obtainable by the method of embodiment 14. 5 16. A composite, preferably being a layered composite, preferably said layered composite is an optical layer, comprising at least; i) a polymer (A) derived or derivable from at least (I) an alkaline soluble polymer, preferably said alkaline soluble polymer is a polysiloxane, an acrylic polymer, or a combination of a polysiloxane and an acrylic polymer; 10 and (III) a scattering particle. Preferably said polymer (A) is derived or derivable from at least (I) the alkaline soluble polymer, and (II) a polymerization initiator; more preferably it is derived or derivable from at least (I) the alkaline soluble polymer, (II) a 15 polymerization initiator and a compound containing two or more (meth)acryloyloxy groups. 17. The composite of embodiment 15 or 16, contains one or more organic particles as the scattering particle, and the outermost surface of the 20 composite has an uneven structure, preferably the surface of the composite has finely roughened structure, more preferably the whole surface of the composite has finely roughened structure, even more preferably said uneven structure and finely roughened structure are caused by said organic one or more organic particles. 25 18. The composite of any one of embodiments 15 to 17, has the average layer thickness in the rage from 1μm to 200μm, preferably from 1.5 to 100μm, more preferably from 2 to 100μm. 30 19. A display device comprising at least one functional medium configured to modulate a light or configured to emit light; and the composite of any one of embodiments 15 to 18. Foreignfiling_text P23-049 - 37 - Working Examples The working examples below provide descriptions of the present invention, as well as an in-detail description of their fabrication. However, the present 5 invention is not limited to these working examples. <Synthesis Example 1: Polysiloxane A> In a 2L flask equipped with a stirrer, a thermometer and a condenser, 49.0 g of a 25 mass% TMAH aqueous solution, 600 ml of isopropyl alcohol 10 (IPA), and 4.0 g of water are charged, and then in a dropping funnel, a mixed solution of 68.0 g of methyltrimethoxysilane, 79.2 g of phenyltrimethoxysilane, and 15.2 g of tetramethoxysilane is prepared. The mixed solution is added dropwise at 40°C, stirred at the same temperature for 2 hours, and neutralized by adding a 10 mass% aqueous solution of 15 HCl. 400 ml of toluene and 600 ml of water are added to the neutralized solution to separate into two layers, and the aqueous layer is removed. Further, the resulting product is rinsed three times with 300 ml of water, the obtained organic layer is concentrated under reduced pressure to remove the solvent, and PGMEA is added to the concentrate to adjust the solid 20 content to be 35 mass%, thereby obtaining Polysiloxane A solution. Mass average molecular weight (Mw) of the obtained Polysiloxane A is 1,700. <Synthesis Example 2: Acrylic polymer A> In a 2L flask equipped with a stirrer, a thermometer, a condenser and a 25 nitrogen gas introducing pipe, normal butanol and PGMEA solvent are charged, and under a nitrogen gas atmosphere, the temperature is raised to an appropriate temperature, while referring to the 10-hour half-life temperature of the initiator. Separately from that, a mixture liquid of acrylic acid, γ-methacryloxypropyltrimethoxysilane, 2-hydroxyethyl methacrylate 30 and methyl methacrylate at 10 : 20 : 20 : 50, azobisisobutyronitrile, and PGMEA is prepared, and the mixture liquid is dropped into the above- described solvent over 4 hours. Thereafter, the resulting product is reacted Foreignfiling_text P23-049 - 38 - for 3 hours to obtain Acrylic polymer A. Mw of the obtained Acrylic polymer A is 8,700. <Synthesis Example 3: Acrylic polymer B> 5 In a 1L flask equipped with a stirrer, a thermometer, a condenser and a nitrogen gas introducing pipe, 16.4 g of azobisisobutyronitrile and 120 g of butanol are charged, and under a nitrogen gas atmosphere, the temperature is raised to an appropriate temperature, while referring to the 10-hour half-life temperature of the initiator. Separately from that, a mixture 10 liquid of 5.16 g of methacrylic acid, 46.5 g of 3- methacryloxypropylmethyldimethoxysilane, 6.5 g of 2-hydroxyethyl methacrylate and 70.08 g of methyl methacrylate is prepared, and the mixture liquid is dropped into the above-described solvent over 4 hours. Thereafter, the resulting product is reacted for 3 hours to obtain Acrylic 15 polymer B. Mw of the obtained Acrylic polymer B is 7,350. Working example 1: Mixture sample preparation The negative tone formulation mixture is prepared as mentioned below: alkaline soluble siloxane polymer (Polysiloxane A) from Merck represented 20 by the following chemical formula, alkaline soluble acrylic polymer A from synthesis example 2, alkaline soluble acrylic polymer B from synthesis example 3, photo initiator NCI-831E, IRGACURE OXE03, monomer A- 9300S, A-DCP, A-DOD-N and AKS-10 for additives are solved in PGMEA. The mixture is adjusted to 44wt% of solid content in PGMEA. 25 30 n=0.5、m=0.4、l=0.1 Foreignfiling_text P23-049 - 39 - Then the obtained negative tone formulation and below nanoparticles mentioned in Table 1 are mixed to obtain efficient optical properties. - Preparation of substrate: The mixture is coated onto a non-alkali glass substrate. After coating by spin coater, the glass is baked at hotplate at 5 100deg.C for 90 seconds. Then the glass is exposed to i-line exposure. The coated glass is then dipped in 2.38% TMAH aqueous solution for 60sec. for development. After rinse by water, the glass is cured at 160deg.C for 30min. in an oven. 10 T.T. means “total transmittance” in the wavelength range from 380 to 780nm According to the present invention, said Haze value is measured at room temperature in air using a haze measurement system with an integrating sphere (NDH-7000, Nippon Denshoku, Japan, Light source White LED 3W, 15 wavelength range 380 ~ 780nm). The sample thickness is between 2μm and 700μm. Particularly it is 700μm. . Schematics of the integrating sphere for transmittance and haze measurement, the total transmittance (TT) TT = TP + TD, the haze (H) H =TD/TT. 20 The parallel transmittance (TP) is determined by measuring the light intensity at a position opposite to that of the sample in the sphere, and the total transmittance (TT), including the diffracted light transmittance (TD) and TP, is obtained by measuring the light passing through the sample, using the equation TT = TP + TD. The degree of light scattering in the sample, i.e., 25 the haze (H), is defined as H =TD/TT. The transmittance and haze is measured. Particle size is obtained from catalog published by the material suppliers. RI (Refractive Index) value is not measured, but publicly available RI data 30 (Catalog Value) for the materials is used. Reflection at 450nm: measured by CM-5, Konica Minolta, SCI mode Foreignfiling_text P23-049 - 40 - average Reflection Sample T.T HAZE particle size RI at 450nm (nm) Target 80 60 10 Non Alkali glass 92.01 0.35 8.34 DT-S1 98.94 -0.22 7.99 TiO2, supplied by Toyo-color 273 1.8 5 5% 79.41 55.21 19.83 TiO2, supplied by Toyo-color 145 1.8 3% 94.11 3.49 10.32 5% 91.6 6.53 12.19 8% 87.96 13.01 15.98 Surulia, hollow Silica, supplied by Nikki chem. 60 1.25 3% 98.39 0.02 8.33 10 5% 98.45 0.06 8.37 8% 98.65 0.05 8.32 silica, supplied by Chem-mat 135 1.5 3% 98.82 0.06 8.32 5% 98.92 0.04 8.3 8% 98.91 0.07 8.35 A2O3, supplied by Chem-mat 60 1.8 5% 98.71 -0.07 8.04 15 8% 98.61 -0.11 8.07 Al2O3, supplied by Chem-mat 51.5 1.8 5% 98.51 0.16 8.1 8% 98.26 0.18 8.15 TiO2, supplied by Toyo-color 488 1.8 3% 84.77 36.71 14.2 5% 79.67 51.65 18.39 20 8% 69.37 75.58 27.51 22% 38.31 99.45 53.09 ZnO2, supplied by Toyo-color 322 1.8 3% 94.22 25.44 9.43 5% 91.95 38.33 10.94 8% 88.27 46.82 12.69 12% 85.55 47.32 17.83 15% 79.58 56.65 18.75 25 ZrO2, supplied by Toyo-color 200 2 3wt% 91.8 16.39 11.02 5wt% 89.28 24.05 13.25 8wt% 86.36 32.74 15.89 Urethane particles, from Negami industry 150 1.5 3wt% 99.02 0.01 8.05 5wt% 98.96 0.43 8.01 8wt% 98.89 2.25 8.05 30 12wt% 98.45 2.81 7.94 20wt% 98.26 5.23 7.9 40wt% 98.13 3.16 7.89 80wt% 98.37 3.8 8.02 Foreignfiling_text P23-049 - 41 - average Reflection Sample T.T HAZE particle size RI at 450nm (nm) Urethane particles, from Negami industry 1000 1.5 5wt% 99.03 10.7 7.96 5 10wt% 98.38 38.16 7.86 15wt% 97.18 48.68 7.77 20wt% 97.49 52.2 7.81 30wt% 96.98 60.42 7.8 Scattering particles, from Toyo Color TiO2 92.84 59.52 9.42 488 ZnO 95.45 57.81 8.4 322 10 ZrO2 94.65 56.97 8.96 200 Urethane particles, from Negami industry 2000 1.5 30wt% 94.11 45.74 H-600T, hollow urethane, from Negami industry 10,000 below 1.5 30wt% 94.09 37 15 TE-812T, acryl- urethane, from Negami industry 6,000 1.5 30wt% 88.21 87.63 J-3PY, acryl beads, from Negami industry 1,200 1.5 30wt% 90.05 61.85 20 As shown above table, nanoparticle mixed formulation can provide higher haze value and high transmittance. And it is believed that it is effective for future display such as rollable, foldable and vendable flexible display. 25 30

Claims

Foreignfiling_text P23-049 - 42 - Claims 1. A photosensitive composition comprising at least; (I) an alkaline soluble polymer, preferably it is a polysiloxane, an acrylic 5 polymer, or a combination of a polysiloxane and an acrylic polymer; (II) a polymerization initiator; and (III) a scattering particle. 2. The composition of claim 1, wherein said scattering particle is selected 10 from inorganic particles, organic particles and a mixture of inorganic particles and organic particles. 3. The composition of claim 1 or 2, wherein the average particle size of the scattering particle is 200 nm or more and 10 μm or less. 15 4. The composition of any one of the preceding claims, wherein said scattering particle has the refractive index greater than the refractive index of the mixture of the polysiloxane and the acrylic polymer. 20 5. The composition of any one of claims 1 to 3, wherein the scattering particle is an organic particle and the difference X of the refractive index of the scattering particle and the refractive index of the mixture of the polysiloxane and the acrylic polymer is in the range from -0.2 to +0.2. X: the refractive index of the scattering particle – the refractive index of the 25 mixture = -0.2 to +0.2, preferably -0.1 to +0.1 When a mixture of organic particles is used as the scattering particle, then the definition of X is: the average refractive index of the scattering particle – the refractive index of the mixture = -0.2 to +0.2, preferably -0.1 to +0.1. 30 6. The composition of any one of the preceding claims, wherein said alkali- soluble polymer is a polysiloxane, or a combination of a polysiloxane and an acrylic polymer. Foreignfiling_text P23-049 - 43 - 7. The composition of any one of the preceding claims, wherein said alkali- soluble polymer is a polysiloxane, or a combination of a polysiloxane and an acrylic polymer, and the polysiloxane comprises a repeating unit of 5 chemical formula (Ib). 10 wherein RIb is a group obtained by removing plural hydrogen from a nitrogen and/or oxygen-containing cycloaliphatic hydrocarbon compound having amino, imino and/or carbonyl. 15 RIb is preferably a group obtained by removing plural hydrogen, preferably two or three hydrogen, from preferably a nitrogen-containing aliphatic hydrocarbon ring having imino and/or carbonyl, more preferably a 5- membered or 6-membered ring containing nitrogen as a member. For example, groups obtained by removing two or three hydrogen from 20 piperidine, pyrrolidine or isocyanurate. RIb connects Si each other included in plural repeating units. 8. The composition of any one of the preceding claims, wherein said alkali- soluble polymer is a polysiloxane, or a combination of a polysiloxane and 25 an acrylic polymer, and the total amount of the polysiloxane is in the range from 1 to 40 mass% based on the total mass of the composition without solvent, preferably it is from 5 to 35 mass%, more preferably from 10 to 30 mass%. 30 9. The composition of any one of the preceding claims, wherein an alkali- soluble polymer is an acrylic polymer, or a combination of a polysiloxane Foreignfiling_text P23-049 - 44 - and an acrylic polymer, preferably said acrylic polymer is selected from one or more members of the group consisting of polyacrylic acid, polymethacrylic acid, polyalkyl acrylate, polyalkyl methacrylate. Preferably the total amount of the acrylic polymer in the composition is in the range 5 from 65 to 99 mass%, more preferably from 70 to 90 mass%, based on the total mass of the composition without solvent. 10. The composition of any one of the preceding claims, further comprises a solvent. 10 11. The composition of any one of the preceding claims, further comprises a compound containing two or more (meth)acryloyloxy groups, preferably the content of the compound is in the range from 10.0 to 25.0 mass% based on the total mass of the composition without solvent. 15 12. Method of preparing the composition of any one of the preceding claims, containing at least the following step; (X) mixing at least (I) an alkaline soluble polymer, preferably it is a polysiloxane, an acrylic 20 polymer, or a combination of a polysiloxane and an acrylic polymer; (II) a polymerization initiator; and (III) a scattering particle. 13. Method of fabricating a composite, comprising steps of: 25 (Xi) applying the composition of any one of the claims 1 to 11 onto a layer or onto a substrate to form a coated layer; and (Xii) baking a coated layer to obtain a composite. 14. A composite, preferably being a layered composite, preferably said 30 layered composite is an optical layer, comprising at least; i) a polymer (A) derived or derivable from at least (I) an alkaline soluble polymer, preferably said alkaline soluble polymer is a polysiloxane, an Foreignfiling_text P23-049 - 45 - acrylic polymer, or a combination of a polysiloxane and an acrylic polymer; and (III) a scattering particle. 5 15. The composite of claim 14, contains one or more organic particles as the scattering particle, and the outermost surface of the composite has an uneven structure, preferably the surface of the composite has finely roughened structure, more preferably the whole surface of the composite has finely roughened structure, even more preferably said uneven structure 10 and finely roughened structure are caused by said organic one or more organic particles. 16. The composite of claim 14 or 15, has the average layer thickness in the rage from 1μm to 200μm. 15 17. A display device comprising at least one functional medium configured to modulate a light or configured to emit light; and the composite of any one of claims 14 to 16. 20 25 30
EP24713463.8A 2023-03-28 2024-03-25 Composition Pending EP4689796A1 (en)

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JP2019095695A (en) 2017-11-27 2019-06-20 メルク、パテント、ゲゼルシャフト、ミット、ベシュレンクテル、ハフツングMerck Patent GmbH Negative type photosensitive siloxane composition and methods for producing cured film and electronic device using the same
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