# Patent

## Title
Paste composition for light guide and light guide utilizing the same

## Abstract

The present invention is an optical waveguide-forming paste composition including (A) barium sulfate particles with a mean particle diameter of 1 nm or more to 50 nm or less, (B) a compound having a polymerizable group and a carboxyl group, or a phosphoric ester compound having a polymerizable group, and (C) an organic solvent.

## Background
This application is a 371 of international application PCT/JP2007/071510, filed Nov. 6, 2007, which claims priority based on Japanese patent application Nos. 2006-304942 and 2007-116469 filed Nov. 10, 2006, and Apr. 26, 2007, respectively, which are incorporated herein by reference.
BACKGROUND OF THE INVENTION
1. Field of the Invention
The present invention relates to an optical waveguide-forming paste composition. More specifically, the present invention relates to an optical waveguide-forming paste composition including an organic material and barium sulfate particles dispersed therein and to an optical waveguide using the composition.
2. Description of the Related Art
Paste compositions including organic materials such as resins and inorganic particles dispersed therein and cured materials obtained by curing such paste compositions are widely used for printing paints, lubricants, cosmetics, adhesives, release agents, components of displays or circuit boards, and so on. The purposes of dispersing inorganic particles in resins include imparting excellent properties such as thermo-mechanical properties, electromagnetic properties, and optical properties, which are not achievable only with resins, and reducing the content of resins and making the manufacturing cost low in a case where the resins used are expensive. In recent years, there have been attempts to use very small inorganic particles with particle diameters of several tens to several nanometers for dispersions for the purpose of improving the surface flatness or transparency of materials or meeting requirements for micro-machining of semiconductors or the like in various technical fields. Particularly in the field of optical interconnection technology, there have been investigations to develop techniques for dispersing inorganic particles with particle diameters of several tens to several nanometers into resins so that temperature-dependent changes in the refractive index or the dimension of optical waveguide materials can be suppressed, while the transparency of the materials can be ensured.
A method for dispersing inorganic particles into a resin includes first preparing a dispersion solution containing an organic solvent and inorganic particles well dispersed therein and then mixing the dispersion solution with a resin. Commercially available inorganic particles with a mean particle diameter of several tens to several nanometers are often provided in the form of agglomerates (secondary particles) with a mean particle diameter of several tens μm in which individual particles (primary particles) are moderately agglomerated. In order to prepare a dispersion solution of inorganic particles with a mean particle diameter of several tens to several nanometers, therefore, the secondary particles should be deagglomerated in an organic solvent and a dispersion solution containing stably dispersed primary particles should be prepared. However, in such a case where primary particles have a mean particle diameter of less than 50 nm, once dispersed particles may be frequently agglomerated to make a further dispersion process difficult in many cases, because the ratio of the surface area to the volume of the particles is significantly high.
Therefore, there is disclosed a method that includes adding an organic material having a certain functional group or the like at its end, called a dispersant, so that the functional group of the dispersant is located on the surface of the inorganic particles to inhibit the contact between the inorganic particles, which can suppress reagglomeration of primary particles and improve the dispersibility. As an example of this technique, there is proposed a nickel colloid solution containing nickel colloid particles with a mean particle diameter of 20 to 40 nm, a non-polar high-molecular pigment dispersant, and an organic solvent (see for example Patent Literature 1). There is also disclosed a method of using a dispersant to disperse barium sulfate particles into an organic solvent (see for example Patent Literature 2).
However, when a cured material is produced by a method including mixing a resin and a dispersion solution of inorganic particles prepared with conventionally known dispersants to form a paste composition and then curing the paste composition to form a cured material in which the inorganic particles are dispersed, the curing reaction of the resin by photoirradiation or heating is more likely to be insufficient, than when no inorganic particles are used. Therefore, the resulting cured material may have low thermo-mechanical properties. In addition, when photolithographic patterning is performed on a film produced with a paste composition containing inorganic particles and an optically curable resin, the exposed area may be insufficiently cured so that the composition may be eluted during development to form an unclearly patterned portion, or the non-exposed area may have low solubility so that a paste composition residue may be produced during development. Therefore, photolithographically produced optical waveguides may have large optical propagation loss.
It is also known that addition of a polymerizable group-containing phosphoric ester monomer in the process of curing a resin can produce an advantageous effect such as an improvement in the antistatic performance or flame retardancy of the cured material or an improvement in the dispersibility of pigments (particles) dispersed in the resin (see Patent Literature 3).
In general, the dispersibility of pigments (particles) significantly depends on whether the pigment used is an organic or inorganic material. Even among the inorganic pigments, however, for example, barium sulfate particles significantly differ in surface potential, surface smoothness or the like from alumina particles, and, therefore, a certain additive effective in improving the dispersibility of one may reduce the dispersibility of the other. Patent Literature 3 only discloses that inorganic pigments may be used and does not specifically disclose the type of inorganic pigments that can influence the dispersibility as mentioned above.

    Patent Literature 1: Japanese Patent Application Laid-Open (JP-A) No. 2004-124237 (Claims and Examples)
    Patent Literature 2: JP-A No. 2006-106708 (page 18)
    Patent Literature 3: JP-A No. 2003-146992 (page 2)


SUMMARY OF THE INVENTION
Problems to be Solved by the Invention
When barium sulfate particles with a mean particle diameter of 1 nm or more to 50 nm or less are used as a component in an optical waveguide-forming paste composition, addition of conventionally known dispersants to disperse the particles may cause an insufficient curing reaction of the paste composition upon photoirradiation or heating or may cause a difficulty in performing development when photolithographic patterning is performed on a film produced with the paste composition, as mentioned above.
In view of the problems with the conventional art, an object of the present invention is to provide an optical waveguide-forming paste composition that allows reliable curing and provides excellent developability.
Means for Solving the Problems
The present invention is directed to an optical waveguide-forming paste composition including (A) barium sulfate particles with a mean particle diameter of 1 nm or more to 50 nm or less, (B) a compound having a polymerizable group and a carboxyl group, or a phosphoric ester compound having a polymerizable group, and (C) an organic solvent. The present invention is also directed to an optical waveguide including a cured material produced by curing the optical waveguide-forming paste composition.
EFFECTS OF THE INVENTION
The optical waveguide-forming paste composition of the present invention is reliably cured by photoirradiation or heating. When photolithographic patterning is performed, the optical waveguide-forming paste composition of the present invention provides very good curability for the exposed area and very good developability for the non-exposed area. The use of the optical waveguide-forming paste composition of the present invention allows production of optical waveguides having low temperature-dependent change rate of refractive index, small coefficient of linear expansion, and low optical propagation loss.



BRIEF DESCRIPTION OF THE DRAWINGS
FIG. 1 is a schematic diagram showing a channel optical waveguide structure; and
FIG. 2 is a schematic diagram showing a slab optical waveguide structure.



DESCRIPTION OF REFERENCE SYMBOLS
In the drawings, reference numeral 1 represents a core, 2 a cladding, and 3 an optical signal.
BEST MODE FOR CARRYING OUT THE INVENTION
The optical waveguide-forming paste composition of the present invention (hereinafter referred to as “the paste composition”) includes (A) barium sulfate particles, (B) a compound having a polymerizable group and a carboxyl group, or a phosphoric ester compound having a polymerizable group, and (C) an organic solvent. Hereinafter, unless otherwise stated, the term “compound A” refers to the compound having a polymerizable group and a carboxyl group, or the phosphoric ester compound having a polymerizable group.
In the paste composition of the present invention, the compound A has the function of dispersing barium sulfate particles. The carboxyl group or the phosphoric ester bond moiety of the compound A interacts with barium sulfate particles so that the surface of the barium sulfate particles can be covered with the compound A. It is considered that the polymerizable group of the compound A placed over the surface of the barium sulfate particles can face outward and be compatible with the organic solvent and other compounds in the paste composition to allow the barium sulfate particles to form a stable dispersion.
The polymerizable group of the compound A is an organic group capable of allowing polymerization to proceed through a polyaddition reaction, a radical reaction, or the like caused by light or heat. In the paste composition of the present invention, the compound A is involved in polymerization so that curing can be allowed to proceed rapidly and reliably.
In the present invention, the compound A itself is optically or thermally polymerized to form a matrix resin in a cured material. Therefore, the compound A used in the present invention can function not only to serve as a dispersant for the barium sulfate particles but also to form a matrix resin. If a dispersant having no polymerizable group is used to disperse barium sulfate into a matrix-forming resin having a polymerizable group, barium sulfate particles may migrate and gather in the process of polymerization of the matrix resin so that their dispersibility can be reduced. In contrast, when the paste composition of the present invention is used, the dispersibility of barium sulfate particles can be kept high even in the cured material, because polymerization proceeds while the barium sulfate particles are captured by the compound A. Therefore, the cured material has a high level of transparency and surface flatness.
In addition, the compound A in the paste composition may be cured by light so that photolithographic patterning may be performed. In this case, polymerization proceeds, while the barium sulfate particles are captured by the compound A in the exposed area, so that a strong network can be formed with the barium sulfate particles serving as starting points and that swelling or dissolution of the exposed area can be prevented during development, which leads to the formation of a clear pattern.
In order to well disperse the barium sulfate particles, the polymerizable group of the compound A preferably has a high affinity for the organic solvent and other compounds in the paste composition. Examples of such a polymerizable group include vinyl, acrylate, methacrylate, epoxyacrylate, epoxymethacrylate, and epoxy groups.
Besides the polymerizable group, the compound A has a carboxyl group. The carboxyl group of the compound A interacts with the barium sulfate particles so that the surface of the barium sulfate particles can be covered with the compound A and that the barium sulfate particles can be dispersed. When the compound A in the paste composition of the present invention is cured by light in photolithographic patterning, the non-exposed area can be rapidly dissolved in a developing solution, because the compound A has a carboxyl group, whose polarity is high, and, therefore, the residue left in the non-exposed area during development can be reduced.
The compound A used in the present invention is preferably represented by the following formula (1):




In the formula (1), R1 represents a hydrogen atom or a methyl group, and R2 represents a bivalent group represented by any one of the following formulae (2) to (4):




In the formulae (2) to (4), n and m are each an integer of 1 to 3.
In the formula (1), the polymerizable group is an acrylate group when R1 is a hydrogen atom, or a methacrylate group when R1 is a methyl group. The acrylate or methacrylate group has an unsaturated bond and therefore is capable of undergoing radical polymerization upon photoirradiation or heating. In the process of radical polymerization using light, a photolithographic method including exposure to light through a photomask may be performed to form patterned wirings or the like. The acrylate group having a hydrogen atom for R1 is preferred because of its higher polymerizing ability.
The smaller the n and m values in the formulae (2) to (4), the larger the number of the polymerizable groups and the carboxyl groups per unit weight, which means better polymerizing ability and better dispersibility of the barium sulfate particles. On the other hand, as the n and m values increase, the steric hindrance effect produced by the compound A located on the barium sulfate particles increases so that the dispersibility can increase. Therefore, n and m are each preferably 2, which means an ethylene group having two carbon atoms.
In the compound represented by the formula (1), R1 is preferably a hydrogen atom, and R2 is preferably a bivalent group represented by the formula (4). In this case, n is preferably 2 for the reason described above. When such a compound is used, higher polymerizing ability and higher developability can be provided, and better dispersibility of the barium sulfate particles can also be provided, which allows a reduction in the mean particle diameter of the dispersed barium sulfate particles so that a cured material with improved transparency can be produced from the paste composition. In this case, therefore, an optical waveguide with low optical propagation loss can be obtained.
Examples of the compound A represented by the formula (1) used in the present invention include HOA-MS (trade name) in which R1 in the formula (1) is a hydrogen atom, R2 is represented by the formula (2), and n and m are each 2, HOA-HH (trade name) in which R1 in the formula (1) is a hydrogen atom, R2 is represented by the formula (3), and n is 2, and HOA-MPL (trade name) in which R1 in the formula (1) is a hydrogen atom, R2 is represented by the formula (4), and n is 2, each manufactured by KYOEISHA CHEMICAL Co., LTD.
On the other hand, the compound A represented by the formula (5) below is also preferably used.




In the formula (5), R3 to R5 each represent a monovalent group represented by any one of the following formulae (6) to (10), or a hydrogen atom, and R3 to R5 may be the same or different, provided that not all of R3 to R5 are hydrogen atoms.




In the formulae (6) to (10), R6 to R9 each represent a hydrogen atom or a methyl group, R10 and R11 each represent a bivalent group of 1 to 10 carbon atoms, preferably a bivalent hydrocarbon group of 1 to 10 carbon atoms, more preferably an alkyl group of two carbon atoms, and R12 represents a bivalent group of 1 to 10 carbon atoms having a hydroxyl group, preferably an organic group represented by any one of the following formulae (13) to (15):




As the compound A represented by the formula (5), a phosphoric monoester in which any two of R3 to R5 are each a hydrogen atom is preferred to a phosphoric diester in which any one of R3 to R5 is a hydrogen atom, because the former can further increase the dispersibility of the barium sulfate particles than the latter. The phosphoric diester is preferred to a phosphoric triester in which none of R3 to R5 is a hydrogen atom, because the former can further increase the dispersibility of the barium sulfate particles than the latter.
The monovalent group represented by any one of the formulae (6) to (9) has an acrylate or methacrylate group and is capable of undergoing radical polymerization upon photoirradiation or heating. The monovalent group represented by the formula (10) is capable of undergoing ionic polymerization upon photoirradiation or heating. The acrylate group in which R6 to R9 are each a hydrogen atom is preferred because of its higher polymerizing ability.
The smaller the number of carbon atoms in each of R10 to R12 in the formulae (8) to (10), the larger the number of the polymerizable groups and the phosphoric ester bond moieties per unit weight, which means better polymerizing ability and better dispersibility of the barium sulfate particles. As the number of carbon atoms in each of R10 to R12 increase, the steric hindrance effect produced by the compound A located on the barium sulfate particles increases so that the dispersibility can increase. Therefore, the number of carbon atoms in each of R10 to R12 is preferably from 1 to 4.
In the compound represented by the formula (5), at least one of R3 to R5 is particularly preferably a monovalent group represented by the formula (8) in which R10 is more preferably a bivalent hydrocarbon group of 1 to 3 carbon atoms. In addition, at least one of R3 to R5 in the formula (5) is preferably a monovalent group represented by the formula (9), and R12 in the formula (9) is preferably a bivalent hydrocarbon group of 2 to 3 carbon atoms having a hydroxyl group.
Examples of the compound A represented by the formula (5) used in the present invention include LIGHT-ACRYLATE P-1A (trade name) manufactured by KYOEISHA CHEMICAL Co., LTD. (a phosphoric monoester having an acrylate group), LIGHT-ESTER P-1M (trade name) manufactured by KYOEISHA CHEMICAL Co., LTD. (a phosphoric monoester having a methacrylate group), LIGHT-ESTER P-2M (trade name) manufactured by KYOEISHA CHEMICAL Co., LTD. (a phosphoric diester having a methacrylate group), and RDX 63182 manufactured by DAICEL-CYTEC COMPANY LTD. (a phosphoric diester having an epoxyacrylate group). One or more types of the compound A may be used in the present invention.
The temperature-dependent change in the physical properties of the cured material produced from the paste composition of the present invention is very small, and, for example, the temperature-dependent refractive-index change rate or linear expansion coefficient is small. Dispersants used to increase the dispersibility of inorganic particles may inhibit a curing reaction of a resin in a paste composition or increase the temperature-dependent refractive-index change rate or linear expansion coefficient of a cured material produced from a paste composition so that the properties of the cured material may be degraded. It has been therefore preferred that the dispersant content should be as low as possible. In the present invention, the compound A itself, which contributes to the dispersibility of the barium sulfate particles, is polymerizable or curable or can be involved in the polymerization with a resin as described later, so that degradation of the properties of the cured material, such as an increase in the temperature-dependent refractive-index change rate or linear expansion coefficient, can be prevented.
The paste composition of the present invention may also contain any other matrix-forming resin, although the compound A can be polymerized to form a matrix in a cured material as described above. Examples of such a resin that may be used to form a matrix include heat or UV curing resins having a polymerizable group, such as polyamic acid, vinyl resins, norbornene resins, epoxy resins, acrylate resins, methacrylate resins, epoxyacrylate resins, epoxymethacrylate resins, cyanate resins, bismaleimide-triazine resins, benzocyclobutene resins, and siloxane resins; and thermoplastic resins such as aramid resins, polystyrene, polyether imide, polyphenylene ether, and thermoplastic polyimide. One or more of these resins may be used alone or in any appropriate mixture ratio.
For applications requiring heat resistance or the like in the process, polymerizable group-containing resins such as heat or UV curing resins are preferred among the resins listed above. When the cured material produced from the paste composition is used for optical waveguide-forming materials which require transparency, epoxy resins, acrylate resins, methacrylate resins, epoxyacrylate resins, epoxymethacrylate resins, siloxane resins, or the like are preferably used. In particular, UV curing resins are preferably selected, because patterned optical waveguides can be formed by photolithographic method using them.
In the present invention, the polymerizable groups of the heat or UV curing resin may be polymerized with one another, or the polymerizable group of the heat or UV curing resin may be polymerized with the polymerizable group of the compound A. The polymers formed in the cured material according to the present invention may include various types of polymers such as (a) a polymer of the compound A, (b) a polymer of the compound A and the resin, and (c) a polymer of only the resin, and the barium sulfate particles may be dispersed in these polymers. Unless otherwise stated, each of the polymers (a) to (c) in the cured material produced from the paste composition will be simply referred to as the “polymer.”
In the cured material obtained from the paste composition, one or more of the polymers (a) to (c) may exist alone or in combination depending on the components of the paste composition, such as the compound A, the resin, and a polymerization initiator.
For example, when the polymerizable group of the compound A and the polymerizable group of the resin are each an acrylate group, a relatively large amount of the compound A exists in the vicinity of the barium sulfate particles, and, therefore, a relatively large amount of the polymer (a) exists in the vicinity of the barium sulfate particles, a relatively large amount of the polymer (c) exists in a region distant from the barium sulfate particles, and the polymer (b) exists in an intermediate region between them. In another example, a cured material including the polymers (a) and (c) may be produced from the paste composition containing the compound A having an acrylate group as the polymerizable group and a resin having an epoxy group as the polymerizable group. Alternatively, different resins may be used. In such a case, for example, the compound A having an acrylate group as the polymerizable group, a resin having an epoxyacrylate group as the polymerizable group, and another resin having an epoxy group as the polymerizable group may be used, and the three components may be copolymerized to form the polymer (b).
When the polymer in the cured material according to the present invention has a refractive index close to that of the barium sulfate particles, the Rayleigh scattering of light in the cured material is low so that the cured material can have high transparency. For transparency requiring applications such as optical materials, the types and mixing ratio of the compound A and the resin are preferably determined so that a polymer having the desired refractive index can be produced. Since barium sulfate has a refractive index of 1.6, the resulting polymer preferably has a refractive index close to 1.6, more preferably a refractive index of 1.6, in order to provide high transparency.
The polymer is produced from components of the paste composition other than the barium sulfate particles, such as a dispersant and the resin. Therefore, the type and amount of each material to be mixed are preferably determined so that the resulting polymer can have a refractive index close to 1.6. When different materials having different refractive indices are mixed to form a polymer having a certain refractive index, it is preferred that each material should have a refractive index close to the desired refractive index so that a polymer with small variations in refractive index can be easily produced.
The examples of the compound A listed above, HOA-MS, HOA-HH, HOA-MPL, LIGHT-ACRYLATE P-1A, LIGHT-ESTER P-1M, LIGHT-ESTER P-2M, and RDX 63182, have refractive indices of 1.46, 1.48, 1.52, 1.47, 1.47, 1.47, and 1.54, respectively. For optical material applications such as optical waveguides, HOA-MPL or RDX 63182, of which refractive index is close to that of barium sulfate, is preferably used, because a cured material with good transparency can be easily produced from the paste composition containing it.
When the cured material produced from the paste composition of the present invention is used for optical waveguide materials requiring heat resistance and transparency, the polymerizable group of the heat or UV curing resin is preferably an epoxy, acrylate, methacrylate, epoxyacrylate, or epoxymethacrylate group. When an epoxy resin or the like is cationically polymerized, the activated cations may adsorb to the barium sulfate particles to slow down the polymerization reaction. Therefore, acrylate resins, methacrylate resins, epoxyacrylate resins, or epoxymethacrylate resins are preferred, because they are suitable for radical polymerization. Optical interconnection materials should preferably have a refractive index close to that of the barium sulfate particles as described above. Examples of such materials include an acrylate resin represented by the formula (11) below (1.55 in refractive index) and an epoxyacrylate resin represented by the formula (12) below (1.56 in refractive index). When photolithographic patterning is performed using the paste composition, the resin represented by the formula (11) below is preferably selected so that the residue in the non-exposed area can be reduced during development. The resin represented by the formula (12) below is also preferably selected so that a cured material with low temperature-dependent change rate of refractive index and small coefficient of linear expansion can be produced from the paste composition.




The amount of the compound A in the paste composition of the present invention is preferably from 5 parts by weight or more to 20 parts by weight or less, based on 100 parts by weight of the barium sulfate particles. The compound A in an amount of 5 parts by weight or more based on the amount of the barium sulfate particles can increase the dispersibility of the barium sulfate particles and reduce the size of the dispersed barium sulfate particles so that a cured material with improved transparency can be produced from the paste composition of the present invention. In this case, optical waveguides with low optical propagation loss can be obtained. Considering the difference between the refractive indices of the compound A and barium sulfate, a cured material with improved transparency can be produced from the paste composition containing the compound A in an amount of 20 parts by weight or less based on the amount of the barium sulfate particles. In this case, optical waveguides with low optical propagation loss can be obtained.
The preferred content of the compound A in paste composition of the present invention (based on the total amount of the paste composition) may differ between the case where a polymer of only the compound A is produced by curing and the case where a polymer of the compound A and a resin is produced by curing. For example, when the compound A alone is polymerized to form a cured material in the mode (a), the content of the compound A is preferably, but not limited to, from 20% by weight or more to 70% by weight or less, based on the amount of the solid components in the paste composition, exclusive of volatile components such as the organic solvent. When the content of the compound A is 20% by weight or more based on the amount of the solid components in the paste composition, exclusive of volatile components such as the organic solvent, the resulting cured material can have improved cracking resistance and adhesion to substrates and high resistance to cohesive fracture. The content of the compound A is more preferably 30% by weight or more based on the amount of the solid components in the paste composition, exclusive of volatile components such as the organic solvent, so that the effects can be enhanced. When the content of the compound A is 70% by weight or less based on the amount of the solid components in the paste composition, exclusive of volatile components such as the organic solvent, the resulting cured material can have low temperature-dependent change rate of refractive index and small coefficient of linear expansion. The content of the compound A is more preferably 50% by weight or more based on the amount of the solid components in the paste composition, exclusive of volatile components such as the organic solvent, so that the effects can be enhanced.
On the other hand, when the polymer (b) or (c) is produced to form a cured material, the total content of the compound A and the resin is preferably 20% by weight or more, more preferably 30% by weight or more, based on the amount of the solid components in the paste composition, exclusive of volatile components such as the organic solvent. The total content of the compound A and the resin is preferably 70% by weight or less, more preferably 50% by weight or less, based on the amount of the solid components in the paste composition, exclusive of volatile components such as the organic solvent. The reason why the range is preferred is the same as described above for the mode (a). The mixing ratio of the compound A and the resin may be determined as needed depending on the composition ratio of the polymer of the compound A and the resin to be produced. In this case, the content of the compound A is preferably 1% by weight or more based on the amount of the barium sulfate particles so that the dispersibility of the barium sulfate particles can be improved.
When the polymerizable group-containing resin is used, the polymerization properties of the compound A and the resin should preferably be taken into account when the mixing ratio between them is determined. Specifically, the mixing ratio of the compound A and the resin may differ between the case (b1) where the compound A and the polymerizable group-containing resin are each independently polymerized, the case (b2) where the polymerizable group-containing resin is polymerized from a molecule of the compound A as a starting point into a chain, and the case (b3) where the compound A and the polymerizable group-containing resin are alternately polymerized. In an example of the case (b3), the compound A having an epoxyacrylate group as the polymerizable group and an epoxy resin may be alternately polymerized. In this case, the number of the polymerizable groups should preferably be the same between both materials.
In order to accelerate the polymerization of the compound A and the resin, the paste composition of the present invention may also contain a polymerization initiator capable of producing an active species such as a radical, cation or anion. There are different polymerization initiators capable of being activated by photoirradiation or heat treatment, and they may be selected and used depending on the intended use. When the paste composition is formed into a film and then subjected to photolithographic patterning, a polymerization initiator capable of being activated by photoirradiation should be used. For example, oxime, benzophenone, triazine, or benzotriazole polymerization initiators can produce radicals upon UV irradiation. Phosphonium, sulfonium, or iodonium polymerization initiators can produce cations upon UV irradiation.
The paste composition of the present invention contains barium sulfate with a mean particle diameter of 1 nm or more to 50 nm or less. As used herein, the term “mean particle diameter” indicates number average particle diameter. In the paste composition, the barium sulfate particles may exist in the form of primary particles, which are completely deagglomerated, and in the form of agglomerates of a plurality of primary particles. Therefore, the particle diameter of the barium sulfate particles in the paste composition is intended to include the particle diameter of the non-agglomerated primary particles and the particle diameter of agglomerates of the primary particles. In order to produce a paste composition containing dispersed barium sulfate particles with a mean particle diameter of 50 nm or less, it is necessary to use barium sulfate particles in which primary particles have a mean particle diameter of 50 nm or less. For example, BF-40 manufactured by SAKAI CHEMICAL INDUSTRY CO., LTD. (10 nm in mean primary particle diameter) satisfies the requirement. The mean particle diameter of the barium sulfate particles in the paste composition may be measured by a method that includes directly observing the particles with a SEM (scanning electron microscope) or a TEM (transmission electron microscope) and calculating the number average of particle diameters. When the mean particle diameter of the barium sulfate particles in the paste composition is 50 nm or less, improved uniformity can be provided for each of the paste composition and the cured material, and Rayleigh scattering of light caused by the barium sulfate particles can be small so that high transparency can be provided. Optical waveguides with low optical propagation loss can be produced using such a paste composition. When the mean particle diameter of the barium sulfate particles dispersed in the paste composition is 30 nm or less, Rayleigh scattering of light caused by the barium sulfate particles in the cured material produced from the paste composition can be very small so that the cured material can exhibit transparency as high as that of a cured material produced from a barium sulfate particle-free composition. Optical waveguides with very low optical propagation loss can be produced using such a material. On the other hand, when the barium sulfate particles have a particle diameter of 1 nm or more, the specific surface area of the particles is small relative to their volume so that the particles can have high dispersibility.
In the present invention, the content of the barium sulfate particles in the paste composition is preferably from 30% by weight or more to 80% by weight or less based on the amount of the solid components in the paste composition, exclusive of volatile components such as the organic solvent. When the content of the barium sulfate particles is 30% by weight or more based on the amount of the solid components in the paste composition, a cured material with reduced temperature-dependent change rate of refractive index and reduced coefficient of linear expansion can be produced from the paste composition. The content of the barium sulfate particles is preferably 50% by weight or more based on the amount of the solid components in the paste composition. When the content of the barium sulfate particles is 80% by weight or less based on the amount of the solid components in the paste composition, cracking resistance and adhesion to substrates can be improved, and high resistance to cohesive fracture can be provided. When such a material is used, a cured material with high transparency can be obtained, and, therefore, optical waveguides with low optical propagation loss can be obtained. The content of the barium sulfated particles is preferably 70% by weight or less based on the amount of the solid components in the paste composition so that the residue left in the non-exposed area during development can be reduced in the process of photolithographic patterning.
The paste composition of the present invention contains an organic solvent. Examples of the organic solvent include N,N-dimethylacetamide, N-methyl-2-pyrrolidone, dimethylimidazolidinone, dimethylsulfoxide, γ-butyrolactone, ethyl lactate, 1-methoxy-2-propanol, 1-ethoxy-2-propanol, ethylene glycol mono-n-propyl ether, diacetone alcohol, and tetrahydrofurfuryl alcohol.
The paste composition of the present invention preferably contains a silane coupling agent. When a silane coupling agent is used, thinning or peeling of a patterned portion in an exposed area and cracking can be reduced and suppressed in the process of photolithographic patterning so that clear patterns can be formed and that the residue left in the non-exposed area can be further reduced. In general, silane coupling agents are known to be effective in improving adhesion between inorganic and organic materials. In the present invention, the silane coupling agent is expected to be effective in improving adhesion between the resin component and the inorganic component in the composition or adhesion between the resin component in the composition and an inorganic substrate such as a silicon wafer and effective in reducing cracking and thinning or peeling of a patterned portion in an exposed area in the process of photolithographic patterning. It is also considered that the residue in the non-exposed area can be effectively reduced in the process of photolithographic patterning, for the reason described below. When a developing solution is brought into contact with the non-exposed area, the resin and the compound A are eluted, and the barium sulfate particles captured by the compound A are also eluted. As the compound A is dissociated from the barium sulfate particles during the development process, the barium sulfate particles with exposed surfaces can agglomerate with each other along with the resin or the like in the vicinity to form a development residue. In the presence of a silane coupling agent, however, the binding force between the compound A (an organic component) and the barium sulfate particles (an inorganic component) is made stronger by the silane coupling agent so that the dispersibility of the barium sulfate particles can be maintained during the development, while the composition can be rapidly dissolved, and as a result, the residue is less likely to form.
Preferred examples of the silane coupling agent include 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropyltriethoxysilane, 3-methacryloxypropyltrimethoxysilane, 3-methacryloxypropyltriethoxysilane, N-2(aminoethyl)-3-aminopropyltrimethoxysilane, N-2(aminoethyl)-3-aminopropyltriethoxysilane, 3-isocyanatopropyltrimethoxysilane, and 3-isocyanatopropyltriethoxysilane. The content of the silane coupling agent in the paste composition is preferably from 0.1% by weight or more to 10% by weight or less based on the amount of the solid components in the paste composition, exclusive of volatile components such as the organic solvent. When the content of the silane coupling agent is 0.1% by weight or more based on the amount of the solid components in the paste component, the silane coupling agent can sufficiently produce the above effect. Common silane coupling agents including those listed above have refractive indices of 1.45 or less, which are significantly different from that of the barium sulfate particles. Therefore, the content of the silane coupling agent should preferably be 10% by weight or less based on the amount of the solid components in the paste composition so that Rayleigh scattering can be reduced and that transparency can be improved.
The paste composition of the present invention may also contain a dispersant other than the compound A. The amount of the dispersant other than the compound A is preferably from 5 parts by weight or more to 20 parts by weight or less based on 100 parts by weight of the barium sulfate particles. At least 5 parts by weight of the dispersant other than the compound A can be significantly effective in improving the dispersibility of the barium sulfate particles. When the amount of the dispersant is 20 parts by weight or less, a cured material with low temperature-dependent change rate of refractive index and small coefficient of linear expansion can be produced from the paste composition.
Next, methods for producing the paste composition of the present invention are described in detail below. First, a description is given of methods for producing a dispersion solution of barium sulfate particles in an organic solvent.
Barium sulfate particles (containing secondary particles and agglomerates) with a mean primary particle diameter of 50 nm or less, the compound A, and an organic solvent, and optionally an additional resin, a pH adjusting agent, a polymerization inhibitor, or the like are mixed in a specific proportion and stirred. Immediately after the mixing, the surface of the barium sulfate particles may be covered with an air layer so that the barium sulfate particles may be insufficiently wetted with the organic solvent to increase the viscosity. In such a case, the mixture is preferably stirred with a rotating blade or the like for a relatively long time until the barium sulfate particles are completely wetted with the organic solvent.
In the process of mixing the barium sulfate particles, the whole amount of the resin necessary for the production of the desired cured material or a partial amount thereof may be added. The resin and the barium sulfate particles can be more uniformly mixed when the resin is added before a dispersion process than when the resin is added after a dispersion process. When the resin is added before the dispersion process, however, the viscosity of the dispersion solution may increase to reduce the efficiency of the dispersion process, or after the dispersion process, the dispersion solution may have low storage stability. All the necessary amount of the compound A may be added before the dispersion process, or part of the necessary amount may be added before the dispersion process, and the remainder may be added after the dispersion process. Alternatively, the compound A and other materials may be added gradually, while the viscosity and any other state of the dispersion solution are measured during the dispersion process.
A polymerization initiator, a defoaming agent, an antioxidant, a polymerization inhibitor, a plasticizer, a silane coupling agent, or any other material necessary for the production of the desired cured material may also be added. In view of the storage stability of the dispersion solution, a polymerization initiator or the like should preferably be added immediately before the preparation of the paste composition is completed.
The barium sulfate particles (including secondary particles and agglomerates), the compound A, the organic solvent, and other necessary materials may be mixed and stirred, and then the barium sulfate particles may be subjected to the dispersion process using a dispersing device.
For example, the dispersing device may be a bead mill such as ULTRA APEX MILL (trade name) manufactured by KOTOBUKI INDUSTRIES CO., LTD. or STAR MILL (trade name) manufactured by ASHIZAWA FINETECH LTD. The beads used in the bead mill preferably have a mean particle diameter of 0.01 mm or more to 0.5 mm or less. When the beads have a mean particle diameter of 0.5 mm or less, the barium sulfate particles can be frequently brought into contact with the beads in the bead mill so that a sufficient dispersing effect can be obtained. When the beads have a mean particle diameter of 0.01 mm or more, each bead can have large momentum so that sufficient shearing stress can be obtained for dispersion of the agglomerated barium sulfate particles.
Ceramic beads, glass beads, metal beads, or the like may be used. Examples of the material of beads include soda glass, quartz, titania, silicon nitride, silicon carbide, alumina, zirconia, zirconium silicate, steel, and stainless steel. In particular, zirconia beads are preferably used, because of their high hardness.
Dispersion with a bead mill may be performed in a single process using small beads or performed while the size of beads is changed stepwise. For example, a dispersion process using beads with a particle diameter of 0.5 mm may be performed first until the particle diameter of the dispersed barium sulfate particles reaches about 100 nm, and then another dispersion process using much smaller beads may be performed.
The time to be spent for the dispersion process may be appropriately determined depending on the type and composition ratio of the components of the dispersion solution, such as the barium sulfate particles, the compound A, and the organic solvent. A sample may preferably be taken from the dispersion solution at regular intervals to determine the mean particle diameter of the barium sulfate particles in the dispersion solution so that changes in the dispersion state can be monitored over time and the time to end the dispersion process can be determined. The particle diameter of the barium sulfate particles in the dispersion solution may be measured with a dynamic light scattering meter such as Zetasizer Nano ZS (trade name) manufactured by Sysmex Corporation. Next, a description is given of methods of producing the paste composition by mixing the dispersion solution obtained as described above with the resin and so on. However, when all the materials necessary for the production of the cured material are mixed to form the dispersion solution, the dispersion solution obtained by the method described above corresponds to the paste composition of the present invention.
When the resin is added to a dispersion solution of the barium sulfate particles, the type and the amount of the resin to be mixed should be selected depending on the components of the dispersion solution, such as the compound A. When the paste composition containing dispersed barium sulfate particles according to the present invention is used for the production of an optical waveguide, the polymer produced from the compound A and the resin preferably has a refractive index close to that of the barium sulfate particles (1.6) so that an optical waveguide with low optical propagation loss can be produced. In the process of mixing the dispersion solution and the resin, the dispersion solution may be added to the resin until a specific amount is reached, or the resin may be added to the dispersion solution until a specific amount is reached. The compound A may be further added to adjust the composition while the paste composition is prepared.
The paste composition produced by mixing specific amounts of the dispersion solution and the resin may be subjected to a process using a ball mill or a roll mill so that it can be more homogeneous. When air bubbles are incorporated into the paste composition in the mixing process, the air bubbles should be removed by standing, placing under reduced pressure, or using a mixing defoamer so that incorporation of air bubbles into a cured material produced from the paste composition can be avoided.
In order to adjust the viscosity of the paste composition, the organic solvent may be further added, or an adequate amount of the organic solvent may be removed by heating or under reduced pressure. The polymerization reaction of the compound A or the resin may also be allowed to moderately proceed by heating or photoirradiation.
The paste composition produced as described above may be cured to form a cured material containing the barium sulfate particles dispersed in a polymer.
Next, a description is given of some examples of the method for curing the paste composition of the present invention. First, the paste composition may be applied to a substrate and spread into a film or strings, poured into a mold, or subjected to any other forming process, and then the organic solvent may be removed from the paste composition by heat treatment. Examples of methods for removing the organic solvent include heating and drying in an oven or on a hot plate, vacuum drying, and heating by electromagnetic waves such as infrared rays or microwaves. If the organic solvent is insufficiently removed in this process, the next curing process may produce a composition in an uncured state or with poor thermo-mechanical properties.
After the organic solvent is removed, a curing reaction of the paste composition is allowed to proceed by heat treatment, photoirradiation or the like, according to the mechanism of curing of the compound A or the resin in the paste composition used. In this case, different processes may be combined in order to allow the curing to completely proceed, for example, heat treatment may be performed after photoirradiation. In an environment at 100° C. or higher, heat treatment is preferably performed under an inert atmosphere such as nitrogen so that oxidation of the polymer can be inhibited. Also when the composition is cured by photoirradiation using a polymerization initiator capable of producing radicals, whose activity may be quenched by oxygen, the treatment is preferably performed under an inert atmosphere such as nitrogen, so that the polymerization is not inhibited.
When photolithographic patterning is performed, the process may include first applying the paste composition to a substrate, removing the organic solvent, and then applying light corresponding to the curing wavelength band of the paste composition through a mask that is designed to allow light to pass through a necessary portion corresponding to a certain pattern. The light source may be an ultra-high pressure mercury vapor lamp, a metal halide lamp, a halogen lamp, a helium-neon laser, a YAG laser, or the like. An exposure system such as an ultra-high pressure mercury vapor lamp exposure system PEM-6M (manufactured by UNION OPTICAL CO., LTD.) may be used. When the mechanism of curing of the paste composition is radical polymerization, exposure to light is preferably performed under a nitrogen atmosphere so that radical reaction species can be prevented from being deactivated by oxidation. In order to increase the resolution of the pattern, light applied in the exposure system should preferably have a high degree of parallelization. Also, in order to reduce the influence of diffracted light caused by the mask, the mask should preferably be in contact with the substrate, or the gap between the mask and the substrate should preferably be reduced.
During exposure, applied light can be scattered inside the paste composition after drying so that the pattern edge can be distorted. For this case, a UV absorber is preferably added to the paste composition so that the UV absorber can absorb faint light leaking from the exposed area to prevent scattering, which can keep the pattern edge sharp. After drying, scattering inside the paste composition is mainly caused by Rayleigh scattering from the barium sulfate particles. The shorter the wavelength of light, the larger the scattering. Therefore, a UV absorber capable of selectively absorbing short-wavelength light is also preferably used. A filter to cut short-wavelength light may also be placed between the light source and the mask so that scattering can be prevented.
In order to allow the curing reaction to further proceed after the exposure, the substrate may be stored at room temperature for a certain period of time, or heat treatment may be performed.
After the exposure process, the substrate may be immersed in a developing solution so that the paste composition can be removed from the non-exposed area. The substrate on which the patterned cured material is formed may be washed and dried. Heat treatment may be further performed to allow the curing reaction to proceed.
The paste composition or the cured material according to the present invention is preferably used to form optical waveguides. Optical waveguides are formed on circuit boards for electrical appliances and so on and have the function of transmitting optical signals between ICs mounted on the boards. An optical waveguide includes a core to transmit optical signals and a cladding surrounding the core and having a refractive index lower than that of the core. FIGS. 1 and 2 show a channel optical waveguide structure and a slab optical waveguide structure, respectively. The channel optical waveguide has a structure including a linear core 1 and a cladding 2 surrounding the periphery of the core 1. The slab optical waveguide has a structure including a layer core 1 and layer claddings 2 with which the upper and lower sides of the core 1 are covered. The paste composition of the present invention may be used to form both or one of the core and the cladding.
Patterning by photoirradiation is possible with the paste composition of the present invention. Therefore, the paste composition of the present invention is preferably used as a core-forming material so that various shapes of optical waveguides can be easily produced. There is preferably a large difference between the refractive indices of the core and the cladding, so that the transmitted light-trapping effect can be high.
The refractive indices and the thicknesses of the cladding and the core in an optical waveguide may be arbitrarily selected depending on the design of the optical waveguide. In the case of a multimode optical waveguide, it is appropriate that the difference between the refractive indices of the core and the cladding should be large and that the core should be made thick. In the case of a single mode optical waveguide, the difference between the refractive indices of the core and the cladding should be small, and the core should be made thin so that single mode transmission can be achieved.
For example, the channel optical waveguide may be manufactured by the method described below. The paste composition for forming an under-cladding is applied to a substrate such as a glass substrate, a silicon wafer, a glass epoxy substrate, or a plastic film. The coating is dried and cured to form an under-cladding. The paste composition for forming a core is then applied to the under-cladding, and the coating is dried to form a film-shaped core. The film-shaped core is then patterned into a waveguide. When the paste composition for forming the core is polymerized by photoirradiation, the patterning may be performed by photolithographic method. Alternatively, when the paste composition for forming the core is polymerized by heat, the patterning may be performed by reactive ion etching or the like. The paste composition for forming an over-cladding is then applied to the core, and the coating is dried and cured to form an over-cladding.
Examples of the method for forming the coating film include, but are not limited to, methods using a spinner, screen printing, a blade coater, a die coater, or any other coating devices.
EXAMPLES
The present invention is more specifically described with some examples below which are not intended to limit the scope of the invention. Some chemical compounds used in the examples are abbreviated as follows: DMAc, N,N-dimethylacetamide; THFA, tetrahydrofurfuryl alcohol.
The properties of each of dispersion solutions of barium sulfate particles, cured materials produced from paste compositions, and optical waveguides were measured by the methods described below.
Method for Measuring the Refractive Index of Cured Materials Produced from Paste Compositions
The refractive index of a film-shaped cured material produced from a paste composition was determined using Prism Coupler 2010 manufactured by Metricon Corporation at a wavelength of 850 nm and a temperature of 25° C. The refractive index was also measured with this equipment at 40° C., 60° C., 80° C., and 100° C. The slope of the four points was obtained by a least-squares method, and a temperature-dependent change in the refractive index (temperature dependency of the refractive index) was calculated.
Method for Measuring Optical Propagation Loss of Optical Waveguide
The measurement was performed by the cut-back method according to the JPCA standard (JPCA-PE02-05-01S-2004). Multimode optical fibers each with a core diameter of 50 μm and a numerical aperture of 0.28 were used on the input and output sides. The measurement temperature was 23° C., and the wavelength of the measurement light source was 850 nm.
Method for Measuring Mean Particle Diameter of Raw Barium Sulfate Particles Agglomerated Before Dispersion Solution Preparation
The measurement was performed using an optical microscope as shown below. The particles were placed on a transparent plate such as a glass plate, and the transparent plate on which the particles were placed was mounted on the observation stage of the optical microscope. Light was applied from beneath the transparent plate. The transmitted light images of the particles captured through a CCD camera ADP-240M (manufactured by FLOVEL CO., LTD.) attached instead of an eye lens to an optical microscope were stored as digital images in a computer. The spherically approximated particle diameters of any observed 100 particles were determined using an image processing software FlvFs (manufactured by FLOVEL CO., LTD.), and the number average particle diameter was calculated therefrom.
Method for Measuring Mean Particle Diameter of Barium Sulfate Particles in Dispersion Solution
A drop of the dispersion solution was put on a carbon-evaporated collodion film. After the solvent was removed by drying, the barium sulfate particles were observed using a transmission electron microscope H-7100FA (manufactured by Hitachi Ltd.) at an accelerating voltage of 100 kV. The observed images were stored as digital images in a computer. The spherically approximated particle diameters of any observed 100 particles were determined using an image processing software FlvFs (manufactured by FLOVEL CO., LTD.), and the number average particle diameter was calculated therefrom. When primary particles were agglomerated, the particle diameters of the agglomerates were measured.
Method for Measuring Mean Particle Diameter of Barium Sulfate Particles in Paste Composition
A drop of the paste composition was put on a carbon-evaporated collodion film. After the solvent was removed by drying, the barium sulfate particles were observed using a transmission electron microscope H-7100FA (manufactured by Hitachi Ltd.) at an accelerating voltage of 100 kV. The observed images were stored as digital images in a computer. The spherically approximated particle diameters of any observed 100 particles were determined using an image processing software FlvFs (manufactured by FLOVEL CO., LTD.), and the number average particle diameter was calculated therefrom. When primary particles were agglomerated, the particle diameters of the agglomerates were measured.
Method for Measuring Coefficient of Linear Expansion of Cured Material Produced from Paste Composition
The cured material produced from the paste composition was measured for dimensional change under an indentation load of 50 mN using a TMA meter TMA/SS6100 manufactured by SSI Nano Technology Inc. in the process of heating it from room temperature to 120° C. and then cooling it to room temperature in a nitrogen atmosphere. The average coefficient of linear expansion during heating and cooling between 50° C. and 70° C. was calculated. In order to eliminate the temperature history of the coefficient of linear expansion, the heating and cooling process was sequentially repeated twice, and the result of the second measurement was used as the displacement value.
Preparation of Dispersion Solutions
Dispersion solutions A to P were prepared as described below. Barium sulfate secondary particles BF-40 (15 μm in mean secondary particle diameter, 10 nm in mean primary particle diameter, manufactured by SAKAI CHEMICAL INDUSTRY CO., LTD.), a dispersant, and an organic solvent were mixed in the respective amounts shown in Table 1, and the mixture was processed in a homogenizer EXCEL AUTOTM manufactured by NIHONSEIKI KAISHA LTD. at a rotary blade end peripheral speed of 5 m/second for 1 hour, so that the barium sulfate particles were dispersed.
The homogenized dispersion solution was subjected to a dispersion process using a bead mill ULTRA APEX MILL UAM-015 (trade name) manufactured by KOTOBUKI INDUSTRIES CO., LTD. The beads were made of zirconia and had a mean particle diameter of 0.05 mm (YTZ Ball manufactured by NIKKATO CORPORATION). The beads were charged in an amount of 400 g. The peripheral speed of the rotor of the bead mill was 9.5 m/second, and the feeding pressure was 0.1 MPa. The dispersion process time was 10 hours for dispersions A to 0 and 1 hour for dispersion P. After the dispersion process was completed, the liquid was collected so that the dispersion solution of the barium sulfate particles was obtained. Table 1 also shows the mean particle diameter of the barium sulfate particles in the dispersion solution at the end of the dispersion process.
In Table 1, HOA-MPL (trade name) and HOA-HH (trade name) manufactured by KYOEISHA CHEMICAL Co., LTD. each used as a dispersant are compounds each having a polymerizable group and a carboxyl group, LIGHT-ESTER P-1M (trade name) manufactured by KYOEISHA CHEMICAL Co., LTD. and RDX 63182 (trade name) manufactured by DAICEL-CYTEC COMPANY LTD. are phosphoric ester compounds each having a polymerizable group, and Disperbyk-111 (trade name) manufactured by BYK-Chemie Japan KK is a phosphoric ester compound having no polymerizable group.









TABLE 1








Components of Dispersion Solution
















Dispersant








*HOA-MPL and HOA-HH








are compounds each having








a polymerizable group and a








carboxyl group, LIGHT-ESTER








P-1M and RDX 63182 are








phosphoric ester

Amount of






compounds each

Dispersant based





Amount of
having a polymerizable

on 100 parts by
Time for




Barium
group. (Compound A)
Organic Solvent
weight of Barium
Dispersion
Mean Particle
















Sulfate

Amount

Amount
Sulfate
Process
Diameter



(g)
Material
(g)
Material
(g)
(parts by weight)
(h)
(nm)


















Dispersion Solution A
200
HOA-MPL
30
THFA
270
15
10
22


Dispersion Solution B
200
HOA-MPL
8
THFA
292
4
10
33


Dispersion Solution C
200
HOA-MPL
14
THFA
286
7
10
24


Dispersion Solution D
200
HDA-MPL
60
THFA
240
30
10
26


Dispersion Solution E
200
HOA-HH
30
THFA
270
15
10
26


Dispersion Solution F
200
HOA-HH
8
THFA
292
4
10
37


Dispersion Solution G
200
HOA-HH
14
THFA
286
7
10
25


Dispersion Solution H
200
HOA-HH
60
THFA
240
30
10
26


Dispersion Solution I
200
LIGHT-ESTER P-1M
30
DMAc
270
15
10
19


Dispersion Solution J
200
LIGHT-ESTER P-1M
8
DMAc
292
4
10
31


Dispersion Solution K
200
LIGHT-ESTER P-1M
14
DMAc
286
7
10
20


Dispersion Solution L
200
LIGHT-ESTER P-1M
60
DMAc
240
30
10
21


Dispersion Solution M
200
RDX 63182
30
DMAc
270
15
10
29


Dispersion Solution N
200
Disperbyk-111
30
DMAc
270
15
10
31


Dispersion Solution O
200
Disperbyk-111
10
DMAc
290
5
10
40


Dispersion Solution P
200
HOA-MPL
30
THFA
270
15
1
49









Example 1
A paste composition was prepared by mixing 9.8 g of the dispersion solution A, 5 g of a resin represented by the formula (11), 0.1 g of a UV-activatable oxime-type polymerization initiator OXE02 (manufactured by Chiba Specialty Chemicals K.K.), and 0.2 g of a silane coupling agent KBM403 (trade name, manufactured by Shin-Etsu Chemical Co., Ltd., chemical name: 3-glycidoxypropyltrimethoxysilane) in a ball mill. The content of the barium sulfate particles in the paste composition was 40% by weight based on the amount of the solid components in the paste composition, exclusive of the organic solvent. The barium sulfate particles in the paste composition had a mean particle diameter of 26 nm. The paste composition was applied to a quartz substrate with a spin coater. The coating was dried in air at 80° C. for 1 hour using an oven and then exposed to 50 mJ/cm2 of ultraviolet light using an ultra-high pressure mercury vapor lamp exposure system (PEM-6M, manufactured by UNION OPTICAL CO., LTD.) so that the paste composition was cured to form a 10 μm-thick film-shaped cured material. At a wavelength of 850 nm and a temperature of 25° C., the film-shaped cured material had a refractive index of 1.556 and a temperature-dependent change rate of refractive index of 51 ppm/° C.
On the other hand, a cured material for use in evaluation of linear expansion coefficient was produced using the paste composition as described below. A Teflon (registered trademark) tape of 10 mm×10 mm was attached to a 94 inch silicon wafer, and a 5 mm-long cut piece of a Teflon (registered trademark) tube with an inner diameter of 8 mm was placed thereon. The paste composition obtained as described above was charged into the Teflon (registered trademark) tube in such a manner that the liquid level reached 1 mm. Thereafter, the paste composition was dried in air at 80° C. for 1 hour using an oven and then exposed to 50 mJ/cm2 of ultraviolet light using an ultra-high pressure mercury vapor lamp exposure system (PEM-6M, manufactured by UNION OPTICAL CO., LTD.) so that the paste composition was cured to form a cured material with a bottom diameter of 8 mm and a thickness of 1 mm. The resulting cured material was removed from the Teflon (registered trademark) tube, and the linear expansion coefficient of the cured material was measured in the thickness direction to be 44 ppm/° C.
In addition, an optical waveguide was produced using the paste composition as described below. A liquid epoxy resin (#314, manufactured by EPOXY TECHNOLOGY, INC.) was applied to a φ4 inch silicon wafer with a spin coater. The coating was dried in air at 80° C. for 1 hour using an oven and then cured by heating in nitrogen at 150° C. for 1 hour to form a 5 μm-thick under-cladding. The refractive index of the under-cladding was measured at a wavelength of 850 nm and a temperature of 25° C. to be 1.502. Thereafter, the paste composition was applied with a spin coater to the under-cladding formed on the quartz substrate, and then dried in air at 80° C. for 1 hour to form a 50 μm-thick dried paste composition film. The resulting film was exposed to 50 mJ/cm2 of ultraviolet light through a quartz mask using an ultra-high pressure mercury vapor lamp exposure system (PEM-6M, manufactured by UNION OPTICAL CO., LTD.). The quartz mask had a 50 μm-wide, 9 cm-long slit, and the portion other than the slit was for blocking light. After the exposure, the substrate was immersed in a developing solution P-7G (manufactured by TOKYO OHKA KOGYO CO., LTD.) for 5 minutes so that the non-exposed film was removed. As a result, a 50 μm-wide 9 cm-long core was formed. After the development, the patterned portion had a clear rectangle shape with no cracking. No residue was observed in the non-exposed area, and the developability was good.
The same material as for the under-cladding was further applied thereto with a spin coater. The coating was dried at 80° C. for 1 hour and then cured by heating in nitrogen at 150° C. for 1 hour to form a 5 μm-thick over-cladding, so that an optical waveguide was obtained.
Both ends of the optical waveguide together with the substrate were cut using a dicing machine, and its optical propagation loss was measured to be 0.3 dB/cm.
Examples 2 to 290
Each of the paste compositions of the formulations shown in Tables 2 to 31 was prepared by the same method as that in Example 1 and then used to form a cured material for use in evaluation of physical properties and to form an optical waveguide, except that the compound A used to form the dispersion solution was further added in place of the resin in the process of preparing the paste composition in each of Examples 209 to 226. The results of the evaluation are shown in Tables 2 to 31, in which the resins A and B are represented by the formulae (11) and (12), respectively, and the chemical name of the silane coupling agent KBM503 (trade name) manufactured by Shin-Etsu Chemical Co., Ltd. is 3-methacryloxypropyltrimethoxysilane.
In some examples, a thin film-like residue was present on the surface of the substrate in the non-exposed area after the development in the process of forming the optical waveguide. In such cases, the comment “residue present in non-exposed area” is entered in the section of Developability in Tables 2 to 31. In some examples, a cracked portion or portions were observed in the core after the development in the process of forming the optical waveguide. In such cases, the comment “cracking of core” is entered in the section of Developability in Tables 2 to 31.








TABLE 2








Components of Paste Compositon



















Content of






Silane
Content of Barium
Compoound A and





Polymerization
Coupling
Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)




















Example 1
Dispersion Solution A
9.8
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 2
Dispersion Solution A
2.4
Resin A
5
OXE02
0.1
KBM403
0.2
15
80


Example 3
Dispersion Solution A
3.4
Resin A
5
OXE02
0.1
KBM403
0.2
20
76


Example 4
Dispersion Solution A
15.4
Resin A
3
OXE02
0.06
KBM403
0.12
60
38


Example 5
Dispersion Solution A
26.5
Resin A
1
OXE02
0.02
KBM403
0.04
80
20


Example 6
Dispersion Solution A
50.1
Resin A
0.5
OXE02
0.01
KBM403
0.02
85
15


Example 7
Dispersion Solution B
9.1
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 8
Dispersion Solution B
2.3
Resin A
5
OXE02
0.1
KBM403
0.2
15
81


Example 9
Dispersion Solution B
3.3
Resin A
5
OXE02
0.1
KBM403
0.2
20
76


Example 10
Dispersion Solution B
12.7
Resin A
3
OXE02
0.06
KBM403
0.12
60
37


Example 11
Dispersion Solution B
12.6
Resin A
1
OXE02
0.02
KBM403
0.04
80
18


Example 12
Dispersion Solution B
9.7
Resin A
0.5
OXE02
0.01
KBM403
0.02
85
14


Example 13
Dispersion Solution C
9.3
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 14
Dispersion Solution C
2.4
Resin A
5
OXE02
0.1
KBM403
0.2
15
80


Example 15
Dispersion Solution C
3.4
Resin A
5
OXE02
0.1
KBM403
0.2
20
75


Example 16
Dispersion Solution C
13.3
Resin A
3
OXE02
0.06
KBM403
0.12
60
38


Example 17
Dispersion Solution C
14.7
Resin A
1
OXE02
0.02
KBM403
0.04
80
20


Example 18
Dispersion Solution C
12.4
Resin A
0.5
OXE02
0.01
KBM403
0.02
85
15


Example 19
Dispersion Solution D
11.0
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 20
Dispersion Solution D
2.5
Resin A
5
OXE02
0.1
KBM403
0.2
15
81


Example 21
Dispersion Solution D
3.6
Resin A
5
OXE02
0.1
KBM403
0.2
20
76


Example 22
Dispersion Solution D
21.7
Resin A
3
OXE02
0.06
KBM403
0.12
60
39

















TABLE 3








Results














Mean








Particle

Temperature






Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)
















Example 1
26
1.556
51
44
good
0.3


Example 2
23
1.552
56
52
good
0.3


Example 3
25
1.553
55
51
good
0.3


Example 4
27
1.562
44
37
good
0.3


Example 5
29
1.572
31
24
good
0.4


Example 6
32
1.575
25
18
Residue present in
0.5







non-exposed area,








Cracking of core



Example 7
37
1.558
52
46
good
0.6


Example 8
35
1.552
57
52
good
0.5


Example 9
35
1.553
56
50
good
0.6


Example 10
36
1.566
44
36
good
0.6


Example 11
39
1.578
33
25
good
0.7


Example 12
42
1.583
26
17
Residue present in
0.8







non-exposed area,








Cracking of core



Example 13
25
1.558
49
44
good
0.3


Example 14
24
1.552
55
51
good
0.3


Example 15
25
1.553
56
51
good
0.3


Example 16
27
1.565
44
37
good
0.3


Example 17
29
1.577
30
23
good
0.4


Example 18
31
1.581
24
18
Residue present in
0.5







non-exposed area,








Cracking of core



Example 19
27
1.554
52
43
good
0.5


Example 20
25
1.551
55
51
good
0.4


Example 21
25
1.552
55
51
good
0.5


Example 22
27
1.557
43
37
good
0.6

















TABLE 4








Components of Paste Compositon



















Content of






Silane
Content of Barium
Compoound A and





Polymerization
Coupling
Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)




















Example 23
Dispersion Solution A
9.8
Resin A
5
OXE02
0.1
KBM503
0.2
40
57


Example 24
Dispersion Solution A
2.4
Resin A
5
OXE02
0.1
KBM503
0.2
15
80


Example 25
Dispersion Solution A
3.4
Resin A
5
OXE02
0.1
KBM503
0.2
20
76


Example 26
Dispersion Solution A
15.4
Resin A
3
OXE02
0.06
KBM503
0.12
60
38


Example 27
Dispersion Solution A
26.5
Resin A
1
OXE02
0.02
KBM503
0.04
80
20


Example 28
Dispersion Solution A
50.1
Resin A
0.5
OXE02
0.01
KBM503
0.02
85
15


Example 29
Dispersion Solution B
9.1
Resin A
5
OXE02
0.1
KBM503
0.2
40
57


Example 30
Dispersion Solution C
9.3
Resin A
5
OXE02
0.1
KBM503
0.2
40
57


Example 31
Dispersion Solution D
11.0
Resin A
5
OXE02
0.1
KBM503
0.2
40
57


Example 32
Dispersion Solution A
9.4
Resin A
5
OXE02
0.1
none
none
40
59


Example 33
Dispersion Solution A
2.3
Resin A
5
OXE02
0.1
none
none
15
83


Example 34
Dispersion Solution A
3.3
Resin A
5
OXE02
0.1
none
none
20
79


Example 35
Dispersion Solution A
14.8
Resin A
3
OXE02
0.06
none
none
60
39


Example 36
Dispersion Solution A
25.5
Resin A
1
OXE02
0.02
none
none
80
20


Example 37
Dispersion Solution A
48.2
Resin A
0.5
OXE02
0.01
none
none
85
15


Example 38
Dispersion Solution B
8.7
Resin A
5
OXE02
0.1
none
none
40
59


Example 39
Dispersion Solution B
2.2
Resin A
5
OXE02
0.1
none
none
15
84


Example 40
Dispersion Solution B
3.2
Resin A
5
OXE02
0.1
none
none
20
79


Example 41
Dispersion Solution B
12.2
Resin A
3
OXE02
0.06
none
none
60
39


Example 42
Dispersion Solution B
12.1
Resin A
1
OXE02
0.02
none
none
80
20


Example 43
Dispersion Solution B
9.3
Resin A
0.5
OXE02
0.01
none
none
85
14


Example 44
Dispersion Solution C
8.9
Resin A
5
OXE02
0.1
none
none
40
59


Example 45
Dispersion Solution C
2.3
Resin A
5
OXE02
0.1
none
none
15
83


Example 46
Dispersion Solution C
3.3
Resin A
5
OXE02
0.1
none
none
20
78


Example 47
Dispersion Solution C
12.8
Resin A
3
OXE02
0.06
none
none
60
39


Example 48
Dispersion Solution C
14.2
Resin A
1
OXE02
0.02
none
none
80
20


Example 49
Dispersion Solution C
12.0
Resin A
0.5
OXE02
0.01
none
none
85
15

















TABLE 5








Results














Mean








Particle

Temperature






Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)
















Example 23
27
1.556
50
42
good
0.3


Example 24
24
1.552
55
52
good
0.3


Example 25
26
1.553
55
52
good
0.3


Example 26
27
1.562
43
38
good
0.3


Example 27
29
1.572
31
25
good
0.4


Example 28
33
1.578
24
19
Residue present in
0.5







non-exposed area,








Cracking of core



Example 29
35
1.558
51
44
good
0.6


Example 30
25
1.558
53
41
good
0.3


Example 31
25
1.554
53
42
good
0.5


Example 32
25
1.556
51
42
good
0.4


Example 33
22
1.552
55
51
good
0.3


Example 34
25
1.553
54
50
good
0.3


Example 35
26
1.562
44
37
good
0.4


Example 36
30
1.572
32
24
Cracking of core
0.4


Example 37
31
1.578
24
18
Residue present in
0.5







non-exposed area,








Cracking of core



Example 38
36
1.558
51
43
good
0.6


Example 39
35
1.552
56
52
good
0.5


Example 40
36
1.553
56
51
good
0.6


Example 41
36
1.566
43
36
good
0.6


Example 42
36
1.578
31
22
Cracking of core
0.7


Example 43
41
1.583
25
17
Residue present in
0.8







non-exposed area,








Cracking of core



Example 44
25
1.558
52
43
good
0.4


Example 45
25
1.552
56
51
good
0.3


Example 46
24
1.553
55
51
good
0.3


Example 47
26
1.565
43
37
good
0.4


Example 48
29
1.577
31
24
Cracking of core
0.4


Example 49
33
1.581
24
18
Residue present in
0.5







non-exposed area,








Cracking of core


















TABLE 6









Components of Paste Composition



















Content of







Content of
Compoound







Barium
A and





Polymerization

Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Silane Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 50
Dispersion Solution D
10.6
Resin A
5
OXE02
0.1
none
none
40
59


Example 51
Dispersion Solution D
2.4
Resin A
5
OXE02
0.1
none
none
15
84


Example 52
Dispersion Solution D
3.5
Resin A
5
OXE02
0.1
none
none
20
78


Example 53
Dispersion Solution D
20.9
Resin A
3
OXE02
0.06
none
none
60
40


Example 54
Dispersion Solution E
9.8
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 55
Dispersion Solution E
2.4
Resin A
5
OXE02
0.1
KBM403
0.2
15
80


Example 56
Dispersion Solution E
3.4
Resin A
5
OXE02
0.1
KBM403
0.2
20
76


Example 57
Dispersion Solution E
15.4
Resin A
3
OXE02
0.06
KBM403
0.12
60
38


Example 58
Dispersion Solution E
26.5
Resin A
1
OXE02
0.02
KBM403
0.04
80
20


Example 59
Dispersion Solution E
50.1
Resin A
0.5
OXE02
0.01
KBM403
0.02
85
15


Example 60
Dispersion Solution F
9.1
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 61
Dispersion Solution G
9.3
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 62
Dispersion Solution H
11.0
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 63
Dispersion Solution E
9.4
Resin A
5
OXE02
0.1
none
none
40
59


Example 64
Dispersion Solution E
2.3
Resin A
5
OXE02
0.1
none
none
15
83


Example 65
Dispersion Solution E
3.3
Resin A
5
OXE02
0.1
none
none
20
79


Example 66
Dispersion Solution E
14.8
Resin A
3
OXE02
0.06
none
none
60
39


Example 67
Dispersion Solution E
25.5
Resin A
1
OXE02
0.02
none
none
80
20


Example 68
Dispersion Solution E
48.2
Resin A
0.5
OXE02
0.01
none
none
85
15


Example 69
Dispersion Solution F
8.7
Resin A
5
OXE02
0.1
none
none
40
59


Example 70
Dispersion Solution G
8.9
Resin A
5
OXE02
0.1
none
none
40
59


Example 71
Dispersion Solution H
10.6
Resin A
5
OXE02
0.1
none
none
40
59


















TABLE 7









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 50
24
1.554
51
43
good
0.5


Example 51
23
1.551
56
51
good
0.4


Example 52
24
1.552
55
51
good
0.5


Example 53
26
1.557
43
37
good
0.6


Example 54
30
1.553
52
44
good
0.5


Example 55
29
1.551
56
51
good
0.3


Example 56
30
1.551
55
51
good
0.4


Example 57
31
1.555
43
38
good
0.5


Example 58
34
1.560
33
25
good
0.5


Example 59
39
1.561
27
20
Residue present in
0.6







non-exposed area,







Cracking of core


Example 60
42
1.557
51
43
good
0.7


Example 61
33
1.556
51
44
good
0.5


Example 62
32
1.547
50
44
good
0.6


Example 63
29
1.553
52
43
good
0.5


Example 64
30
1.551
55
52
good
0.3


Example 65
29
1.551
54
51
good
0.4


Example 66
30
1.555
44
36
good
0.5


Example 67
33
1.560
31
24
Cracking of core
0.5


Example 68
40
1.561
25
18
Residue present in
0.6







non-exposed area,







Cracking of core


Example 69
43
1.557
51
43
good
0.7


Example 70
31
1.556
51
43
good
0.5


Example 71
31
1.547
52
44
good
0.6


















TABLE 8









Components of Paste Composition


















Content of
Content of







Barium
Compoound A and





Polymerization

Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Silane Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 72
Dispersion Solution A
9.8
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 73
Dispersion Solution A
2.4
Resin B
5
OXE02
0.1
KBM403
0.2
15
80


Example 74
Dispersion Solution A
3.4
Resin B
5
OXE02
0.1
KBM403
0.2
20
76


Example 75
Dispersion Solution A
15.4
Resin B
3
OXE02
0.06
KBM403
0.12
60
38


Example 76
Dispersion Solution A
26.5
Resin B
1
OXE02
0.02
KBM403
0.04
80
20


Example 77
Dispersion Solution A
50.1
Resin B
0.5
OXE02
0.01
KBM403
0.02
85
15


Example 78
Dispersion Solution B
9.1
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 79
Dispersion Solution C
9.3
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 80
Dispersion Solution D
11.0
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 81
Dispersion Solution A
9.4
Resin B
5
OXE02
0.1
none
none
40
59


Example 82
Dispersion Solution A
2.3
Resin B
5
OXE02
0.1
none
none
15
83


Example 83
Dispersion Solution A
3.3
Resin B
5
OXE02
0.1
none
none
20
79


Example 84
Dispersion Solution A
14.8
Resin B
3
OXE02
0.06
none
none
60
39


Example 85
Dispersion Solution A
25.5
Resin B
1
OXE02
0.02
none
none
80
20


Example 86
Dispersion Solution A
48.2
Resin B
0.5
OXE02
0.01
none
none
85
15


Example 87
Dispersion Solution B
8.7
Resin B
5
OXE02
0.1
none
none
40
59


Example 88
Dispersion Solution C
8.9
Resin B
5
OXE02
0.1
none
none
40
59


Example 89
Dispersion Solution D
10.6
Resin B
5
OXE02
0.1
none
none
40
59


















TABLE 9









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 72
25
1.566
50
37
good
0.4


Example 73
23
1.563
54
45
good
0.3


Example 74
24
1.563
53
43
good
0.3


Example 75
25
1.566
44
27
Residue present in
0.4







non-exposed area


Example 76
29
1.574
32
16
Residue present in
0.4







non-exposed area


Example 77
33
1.576
24
12
Residue present in
0.5







non-exposed area,







Cracking of core


Example 78
36
1.568
48
32
good
0.6


Example 79
25
1.568
49
35
good
0.4


Example 80
27
1.562
52
35
good
0.5


Example 81
23
1.566
51
35
Residue present in
0.4







non-exposed area


Example 82
23
1.563
53
43
good
0.3


Example 83
24
1.563
53
43
good
0.3


Example 84
25
1.566
43
28
Residue present in
0.5







non-exposed area


Example 85
28
1.574
32
16
Residue present in
0.5







non-exposed area,







Cracking of core


Example 86
32
1.576
23
12
Residue present in
0.6







non-exposed area,







Cracking of core


Example 87
34
1.568
49
31
Residue present in
0.7







non-exposed area


Example 88
25
1.568
50
35
Residue present in
0.4







non-exposed area


Example 89
27
1.562
51
33
Residue present in
0.5







non-exposed area


















TABLE 10









Components of Paste Compositon


















Content of
Content of







Barium
Compoound A and





Polymerization

Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Silane Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 90
Dispersion Solution E
9.8
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 91
Dispersion Solution E
2.4
Resin B
5
OXE02
0.1
KBM403
0.2
15
80


Example 92
Dispersion Solution E
3.4
Resin B
5
OXE02
0.1
KBM403
0.2
20
76


Example 93
Dispersion Solution E
26.5
Resin B
1
OXE02
0.02
KBM403
0.04
80
20


Example 94
Dispersion Solution E
50.1
Resin B
0.5
OXE02
0.01
KBM403
0.02
85
15


Example 95
Dispersion Solution F
9.1
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 96
Dispersion Solution G
9.3
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 97
Dispersion Solution H
11.0
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 98
Dispersion Solution E
9.4
Resin B
5
OXE02
0.1
none
none
40
59


Example 99
Dispersion Solution E
2.3
Resin B
5
OXE02
0.1
none
none
15
83


Example 100
Dispersion Solution E
3.3
Resin B
5
OXE02
0.1
none
none
20
79


Example 101
Dispersion Solution E
25.5
Resin B
1
OXE02
0.02
none
none
80
20


Example 102
Dispersion Solution E
48.2
Resin B
0.5
OXE02
0.01
none
none
85
15


Example 103
Dispersion Solution F
8.7
Resin B
5
OXE02
0.1
none
none
40
59


Example 104
Dispersion Solution G
8.9
Resin B
5
OXE02
0.1
none
none
40
59


Example 105
Dispersion Solution H
10.6
Resin B
5
OXE02
0.1
none
none
40
59


















TABLE 11









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 90
30
1.555
52
38
good
0.5


Example 91
30
1.562
54
44
good
0.3


Example 92
29
1.562
53
41
good
0.4


Example 93
35
1.562
34
18
Residue present in
0.5







non-exposed area


Example 94
40
1.562
26
13
Residue present in
0.6







non-exposed area,







Cracking of core


Example 95
42
1.567
51
36
good
0.7


Example 96
32
1.566
51
38
good
0.5


Example 97
33
1.555
53
39
good
0.6


Example 98
29
1.555
53
37
Residue present in
0.5







non-exposed area


Example 99
29
1.562
55
44
good
0.3


Example 100
30
1.562
54
42
good
0.4


Example 101
34
1.562
33
15
Residue present in
0.6







non-exposed area,







Cracking of core


Example 102
39
1.562
24
12
Residue present in
0.7







non-exposed area,







Cracking of core


Example 103
43
1.567
48
35
Residue present in
0.8







non-exposed area


Example 104
33
1.566
49
37
Residue present in
0.5







non-exposed area


Example 105
31
1.555
51
37
Residue present in
0.6







non-exposed area


















TABLE 12









Components of Paste Compositon


















Content of
Content of







Barium
Compoound A and





Polymerization

Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Silane Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 106
Dispersion Solution A
9.8
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 107
Dispersion Solution A
2.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
15
80





Resin B
2.5


Example 108
Dispersion Solution A
3.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
20
76





Resin B
2.5


Example 109
Dispersion Solution A
15.4
Resin A
1.5
OXE02
0.06
KBM403
0.12
60
38





Resin B
1.5


Example 110
Dispersion Solution A
26.5
Resin A
0.5
OXE02
0.02
KBM403
0.04
80
20





Resin B
0.5


Example 111
Dispersion Solution A
50.1
Resin A
0.25
OXE02
0.01
KBM403
0.02
85
15





Resin B
0.25


Example 112
Dispersion Solution B
9.1
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 113
Dispersion Solution B
2.3
Resin A
2.5
OXE02
0.1
KBM403
0.2
15
81





Resin B
2.5


Example 114
Dispersion Solution B
3.3
Resin A
2.5
OXE02
0.1
KBM403
0.2
20
76





Resin B
2.5


Example 115
Dispersion Solution B
12.7
Resin A
1.5
OXE02
0.06
KBM403
0.12
60
37





Resin B
1.5


Example 116
Dispersion Solution B
12.6
Resin A
0.5
OXE02
0.02
KBM403
0.04
80
18





Resin B
0.5


Example 117
Dispersion Solution B
9.7
Resin A
0.25
OXE02
0.01
KBM403
0.02
85
14





Resin B
0.25


Example 118
Dispersion Solution C
9.3
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 119
Dispersion Solution C
2.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
15
80





Resin B
2.5


Example 120
Dispersion Solution C
3.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
20
75





Resin B
2.5


Example 121
Dispersion Solution C
13.3
Resin A
1.5
OXE02
0.06
KBM403
0.12
60
38





Resin B
1.5


Example 122
Dispersion Solution C
14.7
Resin A
0.5
OXE02
0.02
KBM403
0.04
80
20





Resin B
0.5


Example 123
Dispersion Solution C
12.4
Resin A
0.25
OXE02
0.01
KBM403
0.02
85
15





Resin B
0.25


















TABLE 13









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 106
25
1.561
50
40
good
0.3


Example 107
24
1.557
55
48
good
0.3


Example 108
26
1.558
54
47
good
0.3


Example 109
26
1.565
42
33
good
0.3


Example 110
27
1.573
32
21
good
0.4


Example 111
31
1.576
25
16
Residue present in
0.5







non-exposed area,







Cracking of core


Example 112
37
1.563
51
41
good
0.6


Example 113
36
1.558
56
48
good
0.5


Example 114
35
1.559
53
46
good
0.6


Example 115
36
1.570
42
33
good
0.6


Example 116
39
1.581
30
20
good
0.7


Example 117
41
1.585
24
15
Residue present in
0.8







non-exposed area,







Cracking of core


Example 118
26
1.563
51
40
good
0.3


Example 119
24
1.558
55
47
good
0.3


Example 120
24
1.559
55
47
good
0.3


Example 121
26
1.569
43
33
good
0.3


Example 122
28
1.579
31
21
good
0.4


Example 123
30
1.582
25
16
Residue present in
0.5







non-exposed area,







Cracking of core


















TABLE 14









Components of Paste Compositon


















Content of
Content of







Barium
Compoound A and





Polymerization

Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Silane Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 124
Dispersion Solution D
11.0
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 125
Dispersion Solution D
2.5
Resin A
2.5
OXE02
0.1
KBM403
0.2
15
81





Resin B
2.5


Example 126
Dispersion Solution D
3.6
Resin A
2.5
OXE02
0.1
KBM403
0.2
20
76





Resin B
2.5


Example 127
Dispersion Solution D
21.7
Resin A
1.5
OXE02
0.06
KBM403
0.12
60
39





Resin B
1.5


Example 128
Dispersion Solution A
9.4
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 129
Dispersion Solution A
2.3
Resin A
2.5
OXE02
0.1
none
none
15
83





Resin B
2.5


Example 130
Dispersion Solution A
3.3
Resin A
2.5
OXE02
0.1
none
none
20
79





Resin B
2.5


Example 131
Dispersion Solution A
14.8
Resin A
1.5
OXE02
0.06
none
none
60
39





Resin B
1.5


Example 132
Dispersion Solution A
25.5
Resin A
0.5
OXE02
0.02
none
none
80
20





Resin B
0.5


Example 133
Dispersion Solution A
48.2
Resin A
0.25
OXE02
0.01
none
none
85
15





Resin B
0.25


Example 134
Dispersion Solution B
8.7
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 135
Dispersion Solution C
8.9
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 136
Dispersion Solution D
10.6
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 137
Dispersion Solution E
9.8
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 138
Dispersion Solution E
2.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
15
80





Resin B
2.5


Example 139
Dispersion Solution E
3.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
20
76





Resin B
2.5


Example 140
Dispersion Solution E
26.5
Resin A
0.5
OXE02
0.02
KBM403
0.04
80
20





Resin B
0.5


Example 141
Dispersion Solution E
50.1
Resin A
0.25
OXE02
0.01
KBM403
0.02
85
15





Resin B
0.25


















TABLE 15









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 124
26
1.558
52
39
good
0.5


Example 125
25
1.557
55
48
good
0.4


Example 126
26
1.557
54
47
good
0.5


Example 127
27
1.559
42
33
good
0.6


Example 128
24
1.561
51
40
good
0.4


Example 129
23
1.557
56
47
good
0.3


Example 130
25
1.558
55
46
good
0.3


Example 131
26
1.565
43
32
good
0.4


Example 132
28
1.573
32
21
Cracking of core
0.4


Example 133
31
1.576
24
17
Residue present in
0.5







non-exposed area,







Cracking of core


Example 134
26
1.563
50
40
good
0.6


Example 135
25
1.563
51
39
good
0.4


Example 136
25
1.558
52
40
good
0.5


Example 137
29
1.557
52
40
good
0.5


Example 138
30
1.556
56
48
good
0.3


Example 139
30
1.557
55
47
good
0.4


Example 140
35
1.561
31
21
good
0.5


Example 141
40
1.562
25
16
Residue present in
0.6







non-exposed area,







Cracking of core


















TABLE 16









Components of Paste Compositon


















Content of
Content of







Barium
Compoound A and





Polymerization

Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Silane Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 142
Dispersion Solution F
9.1
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 143
Dispersion Solution G
9.3
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 144
Dispersion Solution H
11.0
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 145
Dispersion Solution E
9.4
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 146
Dispersion Solution E
2.3
Resin A
2.5
OXE02
0.1
none
none
15
83





Resin B
2.5


Example 147
Dispersion Solution E
3.3
Resin A
2.5
OXE02
0.1
none
none
20
79





Resin B
2.5


Example 148
Dispersion Solution E
25.5
Resin A
0.5
OXE02
0.02
none
none
80
20





Resin B
0.5


Example 149
Dispersion Solution E
48.2
Resin A
0.25
OXE02
0.01
none
none
85
15





Resin B
0.25


Example 150
Dispersion Solution F
8.7
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 151
Dispersion Solution G
8.9
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 152
Dispersion Solution H
10.6
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


















TABLE 17









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 142
44
1.562
50
41
good
0.7


Example 143
32
1.561
49
41
good
0.5


Example 144
30
1.551
52
40
good
0.6


Example 145
30
1.557
50
40
good
0.5


Example 146
28
1.556
54
47
good
0.3


Example 147
29
1.557
55
46
good
0.4


Example 148
36
1.561
30
20
Cracking of core
0.5


Example 149
39
1.562
24
15
Residue present in
0.6







non-exposed area,







Cracking of core


Example 150
42
1.562
50
41
good
0.7


Example 151
29
1.561
51
39
good
0.5


Example 152
31
1.551
50
39
good
0.6


















TABLE 18









Components of Paste Compositon


















Content of
Content of







Barium
Compoound A and





Polymerization

Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Silane Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 153
Dispersion Solution I
9.8
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 154
Dispersion Solution I
2.4
Resin A
5
OXE02
0.1
KBM403
0.2
15
80


Example 155
Dispersion Solution I
3.4
Resin A
5
OXE02
0.1
KBM403
0.2
20
76


Example 156
Dispersion Solution I
15.4
Resin A
3
OXE02
0.06
KBM403
0.12
60
38


Example 157
Dispersion Solution I
26.5
Resin A
1
OXE02
0.02
KBM403
0.04
80
20


Example 158
Dispersion Solution I
50.1
Resin A
0.5
OXE02
0.01
KBM403
0.02
85
15


Example 159
Dispersion Solution J
9.1
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 160
Dispersion Solution J
2.3
Resin A
5
OXE02
0.1
KBM403
0.2
15
81


Example 161
Dispersion Solution J
3.3
Resin A
5
OXE02
0.1
KBM403
0.2
20
76


Example 162
Dispersion Solution J
12.7
Resin A
3
OXE02
0.06
KBM403
0.12
60
37


Example 163
Dispersion Solution J
12.6
Resin A
1
OXE02
0.02
KBM403
0.04
80
18


Example 164
Dispersion Solution J
9.7
Resin A
0.5
OXE02
0.01
KBM403
0.02
85
14


Example 165
Dispersion Solution K
9.3
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 166
Dispersion Solution K
2.4
Resin A
5
OXE02
0.1
KBM403
0.2
15
80


Example 167
Dispersion Solution K
3.4
Resin A
5
OXE02
0.1
KBM403
0.2
20
75


Example 168
Dispersion Solution K
13.3
Resin A
3
OXE02
0.06
KBM403
0.12
60
38


Example 169
Dispersion Solution K
14.7
Resin A
1
OXE02
0.02
KBM403
0.04
80
20


Example 170
Dispersion Solution K
12.4
Resin A
0.5
OXE02
0.01
KBM403
0.02
85
15


Example 171
Dispersion Solution L
11.0
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 172
Dispersion Solution L
2.5
Resin A
5
OXE02
0.1
KBM403
0.2
15
81


Example 173
Dispersion Solution L
3.6
Resin A
5
OXE02
0.1
KBM403
0.2
20
76


Example 174
Dispersion Solution L
21.7
Resin A
3
OXE02
0.06
KBM403
0.12
60
39


















TABLE 19









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Composition
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 153
21
1.552
51
44
good
0.4


Example 154
20
1.550
55
52
good
0.3


Example 155
21
1.551
54
51
good
0.3


Example 156
23
1.553
44
38
good
0.4


Example 157
26
1.556
31
24
Residue present in
0.4







non-exposed area


Example 158
28
1.557
26
19
Residue present in
0.5







non-exposed area,







Cracking of core


Example 159
35
1.557
51
46
good
0.6


Example 160
33
1.552
56
53
good
0.5


Example 161
33
1.553
55
51
good
0.6


Example 162
36
1.563
43
36
good
0.7


Example 163
37
1.574
33
25
Residue present in
0.7







non-exposed area


Example 164
38
1.578
25
16
Residue present in
0.8







non-exposed area,







Cracking of core


Example 165
22
1.556
49
44
good
0.4


Example 166
21
1.552
55
50
good
0.3


Example 167
22
1.552
55
49
good
0.3


Example 168
24
1.561
43
38
good
0.4


Example 169
26
1.569
30
23
Residue present in
0.4







non-exposed area


Example 170
29
1.572
24
18
Residue present in
0.5







non-exposed area,







Cracking of core


Example 171
22
1.544
53
43
good
0.5


Example 172
21
1.548
55
51
good
0.4


Example 173
22
1.548
55
51
good
0.4


Example 174
23
1.539
43
37
good
0.6


















TABLE 20









Components of Paste Composition



















Content of







Content of Barium
Compoound A and





Polymerization
Silane
Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 175
Dispersion Solution I
9.4
Resin A
5
OXE02
0.1
none
none
40
59


Example 176
Dispersion Solution I
2.3
Resin A
5
OXE02
0.1
none
none
15
83


Example 177
Dispersion Solution I
3.3
Resin A
5
OXE02
0.1
none
none
20
79


Example 178
Dispersion Solution I
14.8
Resin A
3
OXE02
0.06
none
none
60
39


Example 179
Dispersion Solution I
25.5
Resin A
1
OXE02
0.02
none
none
80
20


Example 180
Dispersion Solution I
48.2
Resin A
0.5
OXE02
0.01
none
none
85
15


Example 181
Dispersion Solution J
8.7
Resin A
5
OXE02
0.1
none
none
40
59


Example 182
Dispersion Solution J
2.2
Resin A
5
OXE02
0.1
none
none
15
84


Exampte 183
Dispersion Solution J
3.2
Resin A
5
OXE02
0.1
none
none
20
79


Example 184
Dispersion Solution J
12.2
Resin A
3
OXE02
0.06
none
none
60
39


Example 185
Dispersion Solution J
12.1
Resin A
1
OXE02
0.02
none
none
80
20


Example 186
Dispersion Solution J
9.3
Resin A
0.5
OXE02
0.01
none
none
85
14


Example 187
Dispersion Solution K
8.9
Resin A
5
OXE02
0.1
none
none
40
59


Example 188
Dispersion Solution K
2.3
Resin A
5
OXE02
0.1
none
none
15
83


Example 189
Dispersion Solution K
3.3
Resin A
5
OXE02
0.1
none
none
20
78


Example 190
Dispersion Solution K
12.8
Resin A
3
OXE02
0.06
none
none
60
39


Example 191
Dispersion Solution K
14.2
Resin A
1
OXE02
0.02
none
none
80
20


Example 192
Dispersion Solution K
12.0
Resin A
0.5
OXE02
0.01
none
none
85
15


Example 193
Dispersion Solution L
10.6
Resin A
5
OXE02
0.1
none
none
40
59


Example 194
Dispersion Solution L
2.4
Resin A
5
OXE02
0.1
none
none
15
84


Example 195
Dispersion Solution L
3.5
Resin A
5
OXE02
0.1
none
none
20
78


Example 196
Dispersion Solution L
20.9
Resin A
3
OXE02
0.06
none
none
60
40


















TABLE 21









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Composition
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 175
23
1.552
51
43
good
0.4


Example 176
21
1.550
56
52
good
0.3


Example 177
21
1.551
55
51
good
0.3


Example 178
24
1.553
44
37
Residue present in
0.5







non-exposed area


Example 179
27
1.556
30
25
Residue present in
0.5







non-exposed area,







Cracking of core


Example 180
28
1.557
25
18
Residue present in
0.6







non-exposed area,







Cracking of core


Example 181
35
1.557
53
46
good
0.7


Example 182
33
1.552
56
51
good
0.5


Example 183
34
1.553
56
50
good
0.6


Example 184
37
1.563
45
37
Residue present in
0.7







non-exposed area


Example 185
38
1.574
33
25
Residue present in
0.8







non-exposed area,







Cracking of core


Example 186
40
1.578
26
17
Residue present in
0.9







non-exposed area,







Cracking of core


Example 187
22
1.556
49
44
good
0.4


Example 188
20
1.552
56
51
good
0.3


Example 189
20
1.552
55
50
good
0.3


Example 190
22
1.561
44
37
Residue present in
0.5







non-exposed area


Example 191
26
1.569
31
22
Residue present in
0.5







non-exposed area,







Cracking of core


Example 192
28
1.572
25
19
Residue present in
0.6







non-exposed area,







Cracking of core


Example 193
21
1.544
53
44
good
0.5


Example 194
20
1.548
54
51
good
0.4


Example 195
21
1.548
54
50
good
0.4


Example 196
22
1.539
43
36
Residue present in
0.6







non-exposed area


















TABLE 22









Components of Paste Composition



















Content of







Content of Barium
Compoound A and





Polymerization
Silane
Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 197
Dispersion Solution M
9.8
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 198
Dispersion Solution M
2.4
Resin A
5
OXE02
0.1
KBM403
0.2
15
80


Example 199
Dispersion Solution M
3.4
Resin A
5
OXE02
0.1
KBM403
0.2
20
76


Example 200
Dispersion Solution M
15.4
Resin A
3
OXE02
0.06
KBM403
0.12
60
38


Example 201
Dispersion Solution M
26.5
Resin A
1
OXE02
0.02
KBM403
0.04
80
20


Example 202
Dispersion Solution M
50.1
Resin A
0.5
OXE02
0.01
KBM403
0.02
85
15


Example 203
Dispersion Solution M
9.4
Resin A
5
OXE02
0.1
none
none
40
59


Example 204
Dispersion Solution M
2.3
Resin A
5
OXE02
0.1
none
none
15
83


Example 205
Dispersion Solution M
3.3
Resin A
5
OXE02
0.1
none
none
20
79


Example 206
Dispersion Solution M
14.8
Resin A
3
OXE02
0.06
none
none
60
39


Example 207
Dispersion Solution M
25.5
Resin A
1
OXE02
0.02
none
none
80
20


Example 208
Dispersion Solution M
48.2
Resin A
0.5
OXE02
0.01
none
none
85
15


















TABLE 23









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Composition
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 197
35
1.558
51
43
good
0.6


Example 198
34
1.552
54
52
good
0.5


Example 199
34
1.553
54
51
good
0.6


Example 200
37
1.565
45
37
good
0.6


Example 201
39
1.578
32
24
Residue present in
0.7







non-exposed area


Example 202
40
1.582
26
20
Residue present in
0.8







non-exposed area,







Cracking of core


Example 203
36
1.558
52
44
good
0.6


Example 204
33
1.552
55
51
good
0.5


Example 205
34
1.553
55
49
good
0.6


Example 206
38
1.565
45
37
Residue present in
0.7







non-exposed area


Example 207
39
1.578
31
25
Residue present in
0.8







non-exposed area,







Cracking of core


Example 208
41
1.582
26
19
Residue present in
0.9







non-exposed area,







Cracking of core


















TABLE 24









Components of Paste Composition



















Content of







Content of Barium
Compoound A and





Polymerization
Silane
Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 209
Dispersion Solution I
9.8
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 210
Dispersion Solution I
2.4
Resin B
5
OXE02
0.1
KBM403
0.2
15
80


Example 211
Dispersion Solution I
3.4
Resin B
5
OXE02
0.1
KBM403
0.2
20
76


Example 212
Dispersion Solution I
15.4
Resin B
3
OXE02
0.06
KBM403
0.12
60
38


Example 213
Dispersion Solution I
26.5
Resin B
1
OXE02
0.02
KBM403
0.04
80
20


Example 214
Dispersion Solution I
50.1
Resin B
0.5
OXE02
0.01
KBM403
0.02
85
15


Example 215
Dispersion Solution J
9.1
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 216
Dispersion Solution K
9.3
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 217
Dispersion Solution L
11.0
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 218
Dispersion Solution I
9.4
Resin B
5
OXE02
0.1
none
none
40
59


Example 219
Dispersion Solution I
2.3
Resin B
5
OXE02
0.1
none
none
15
83


Example 220
Dispersion Solution I
3.3
Resin B
5
OXE02
0.1
none
none
20
79


Example 221
Dispersion Solution I
14.8
Resin B
3
OXE02
0.06
none
none
60
39


Example 222
Dispersion Solution I
25.5
Resin B
1
OXE02
0.02
none
none
80
20


Example 223
Dispersion Solution I
48.2
Resin B
0.5
OXE02
0.01
none
none
85
15


Example 224
Dispersion Solution J
8.7
Resin B
5
OXE02
0.1
none
none
40
59


Example 225
Dispersion Solution K
8.9
Resin B
5
OXE02
0.1
none
none
40
59


Example 226
Dispersion Solution L
10.6
Resin B
5
OXE02
0.1
none
none
40
59


Example 227
Dispersion Solution M
9.8
Resin B
5
OXE02
0.1
KBM403
0.2
40
57


Example 228
Dispersion Solution M
2.4
Resin B
5
OXE02
0.1
KBM403
0.2
15
80


Example 229
Dispersion Solution M
3.4
Resin B
5
OXE02
0.1
KBM403
0.2
20
76


Example 230
Dispersion Solution M
26.5
Resin B
1
OXE02
0.02
KBM403
0.04
80
20


Example 231
Dispersion Solution M
50.1
Resin B
0.5
OXE02
0.01
KBM403
0.02
85
15


















TABLE 25









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 209
24
1.560
50
37
good
0.4


Example 210
23
1.560
53
44
good
0.3


Example 211
23
1.560
53
43
good
0.3


Example 212
25
1.559
44
26
Residue present in
0.4







non-exposed area


Example 213
28
1.559
31
16
Residue present in
0.4







non-exposed area


Example 214
31
1.559
24
13
Residue present in
0.5







non-exposed area,







Cracking of core


Example 215
34
1.565
49
32
good
0.6


Example 216
22
1.564
49
35
good
0.4


Example 217
24
1.552
51
35
good
0.5


Example 218
21
1.560
51
36
Residue present in
0.4







non-exposed area


Example 219
22
1.560
54
44
good
0.3


Example 220
23
1.560
53
43
good
0.3


Example 221
23
1.559
42
28
Residue present in
0.5







non-exposed area


Example 222
27
1.559
32
17
Residue present in
0.5







non-exposed area,







Cracking of core


Example 223
32
1.559
22
12
Residue present in
0.6







non-exposed area,







Cracking of core


Example 224
34
1.565
49
30
Residue present in
0.7







non-exposed area


Example 225
25
1.564
50
35
Residue present in
0.4







non-exposed area


Example 226
26
1.552
52
33
Residue present in
0.5







non-exposed area


Example 227
34
1.566
53
37
good
0.6


Example 228
33
1.562
54
44
good
0.5


Example 229
35
1.562
53
41
good
0.6


Example 230
38
1.580
34
18
Residue present in
0.8







non-exposed area


Example 231
41
1.583
25
12
Residue present in
0.9







non-exposed area,







Cracking of core


















TABLE 26









Components of Paste Composition



















Content of







Content of Barium
Compoound A and





Polymerization
Silane
Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 232
Dispersion Solution I
9.8
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 233
Dispersion Solution I
2.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
15
80





Resin B
2.5


Example 234
Dispersion Solution I
3.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
20
76





Resin B
2.5


Example 235
Dispersion Solution I
15.4
Resin A
1.5
OXE02
0.06
KBM403
0.12
60
38





Resin B
1.5


Example 236
Dispersion Solution I
26.5
Resin A
0.5
OXE02
0.02
KBM403
0.04
80
20





Resin B
0.5


Example 237
Dispersion Solution I
50.1
Resin A
0.25
OXE02
0.01
KBM403
0.02
85
15





Resin B
0.25


Example 238
Dispersion Solution J
9.1
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 239
Dispersion Solution J
2.3
Resin A
2.5
OXE02
0.1
KBM403
0.2
15
81





Resin B
2.5


Example 240
Dispersion Solution J
3.3
Resin A
2.5
OXE02
0.1
KBM403
0.2
20
76





Resin B
2.5


Example 241
Dispersion Solution J
12.7
Resin A
1.5
OXE02
0.06
KBM403
0.12
60
37





Resin B
1.5


Example 242
Dispersion Solution J
12.6
Resin A
0.5
OXE02
0.02
KBM403
0.04
80
18





Resin B
0.5


Example 243
Dispersion Solution J
9.7
Resin A
0.25
OXE02
0.01
KBM403
0.02
85
14





Resin B
0.25


Example 244
Dispersion Solution K
9.3
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 245
Dispersion Solution K
2.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
15
80





Resin B
2.5


Example 246
Dispersion Solution K
3.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
20
75





Resin B
2.5


Example 247
Dispersion Solution K
13.3
Resin A
1.5
OXE02
0.06
KBM403
0.12
60
38





Resin B
1.5


Example 248
Dispersion Solution K
14.7
Resin A
0.5
OXE02
0.02
KBM403
0.04
80
20





Resin B
0.5


Example 249
Dispersion Solution K
12.4
Resin A
0.25
OXE02
0.01
KBM403
0.02
85
15





Resin B
0.25


















TABLE 27









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 232
22
1.556
50
41
good
0.3


Example 233
21
1.555
54
49
good
0.3


Example 234
23
1.555
53
47
good
0.3


Example 235
25
1.557
40
33
good
0.3


Example 236
27
1.558
31
20
good
0.4


Example 237
32
1.558
24
16
Residue present in
0.5







non-exposed area,







Cracking of core


Example 238
36
1.561
51
41
good
0.6


Example 239
37
1.557
55
47
good
0.5


Example 240
34
1.558
53
46
good
0.6


Example 241
38
1.567
42
33
good
0.6


Example 242
39
1.577
29
21
good
0.7


Example 243
41
1.580
25
15
Residue present in
0.8







non-exposed area,







Cracking of core


Example 244
25
1.560
51
41
good
0.3


Example 245
23
1.556
56
48
good
0.3


Example 246
23
1.557
55
47
good
0.3


Example 247
25
1.564
44
34
good
0.3


Example 248
28
1.571
31
22
good
0.4


Example 249
30
1.574
24
17
Residue present in
0.5







non-exposed area,







Cracking of core


















TABLE 28









Components of Paste Composition



















Content of







Content of Barium
Compoound A and





Polymerization
Silane
Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 250
Dispersion Solution L
11.0
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 251
Dispersion Solution L
2.5
Resin A
2.5
OXE02
0.1
KBM403
0.2
15
81





Resin B
2.5


Example 252
Dispersion Solution L
3.6
Resin A
2.5
OXE02
0.1
KBM403
0.2
20
76





Resin B
2.5


Example 253
Dispersion Solution L
21.7
Resin A
1.5
OXE02
0.06
KBM403
0.12
60
39





Resin B
1.5


Example 254
Dispersion Solution I
9.4
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 255
Dispersion Solution I
2.3
Resin A
2.5
OXE02
0.1
none
none
15
83





Resin B
2.5


Example 256
Dispersion Solution I
3.3
Resin A
2.5
OXE02
0.1
none
none
20
79





Resin B
2.5


Example 257
Dispersion Solution I
14.8
Resin A
1.5
OXE02
0.06
none
none
60
39





Resin B
1.5


Example 258
Dispersion Solution I
25.5
Resin A
0.5
OXE02
0.02
none
none
80
20





Resin B
0.5


Example 259
Dispersion Solution I
48.2
Resin A
0.25
OXE02
0.01
none
none
85
15





Resin B
0.25


Example 260
Dispersion Solution J
8.7
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 261
Dispersion Solution K
8.9
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 262
Dispersion Solution L
10.6
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 263
Dispersion Solution M
9.8
Resin A
2.5
OXE02
0.1
KBM403
0.2
40
57





Resin B
2.5


Example 264
Dispersion Solution M
2.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
15
80





Resin B
2.5


Example 265
Dispersion Solution M
3.4
Resin A
2.5
OXE02
0.1
KBM403
0.2
20
76





Resin B
2.5


Example 266
Dispersion Solution M
26.5
Resin A
0.5
OXE02
0.02
KBM403
0.04
80
20





Resin B
0.5


Example 267
Dispersion Solution M
50.1
Resin A
0.25
OXE02
0.01
KBM403
0.02
85
15





Resin B
0.25


















TABLE 29









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 250
25
1.548
51
39
good
0.5


Example 251
24
1.553
55
48
good
0.4


Example 252
24
1.552
54
46
good
0.5


Example 253
27
1.543
42
33
good
0.6


Example 254
23
1.556
50
41
good
0.4


Example 255
21
1.555
55
47
good
0.3


Example 256
24
1.555
55
45
good
0.3


Example 257
25
1.557
42
32
good
0.4


Example 258
27
1.558
32
22
Cracking of core
0.4


Example 259
30
1.558
23
18
Residue present in
0.5







non-exposed area,







Cracking of core


Example 260
25
1.561
50
40
good
0.6


Example 261
24
1.560
51
39
good
0.4


Example 262
24
1.548
52
41
good
0.5


Example 263
34
1.562
52
40
good
0.5


Example 264
33
1.557
55
48
good
0.3


Example 265
34
1.558
55
47
good
0.4


Example 266
38
1.579
31
22
good
0.5


Example 267
41
1.583
24
16
Residue present in
0.6







non-exposed area,







Cracking of core


















TABLE 30









Components of Paste Compositon



















Content of







Content of
Compoound A







Barium Sulfate
and





Polymerization
Silane
based on
Resin based on



Dispersion Solution
Compound A
Initiator
Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Example 268
Dispersion Solution M
9.4
Resin A
2.5
OXE02
0.1
none
none
40
59





Resin B
2.5


Example 269
Dispersion Solution M
2.3
Resin A
2.5
OXE02
0.1
none
none
15
83





Resin B
2.5


Example 270
Dispersion Solution M
3.3
Resin A
2.5
OXE02
0.1
none
none
20
79





Resin B
2.5


Example 271
Dispersion Solution M
25.5
Resin A
0.5
OXE02
0.02
none
none
80
20





Resin B
0.5


Example 272
Dispersion Solution M
48.2
Resin A
0.25
OXE02
0.01
none
none
85
15





Resin B
0.25


Example 273
Dispersion Solution A
9.8
HOA-MPL
5
OXE02
0.1
KBM403
0.2
40
57


Example 274
Dispersion Solution A
2.4
HOA-MPL
5
OXE02
0.1
KBM403
0.2
15
80


Example 275
Dispersion Solution A
3.4
HOA-MPL
5
OXE02
0.1
KBM403
0.2
20
76


Example 276
Dispersion Solution A
15.4
HOA-MPL
3
OXE02
0.06
KBM403
0.12
60
38


Example 277
Dispersion Solution A
26.5
HOA-MPL
1
OXE02
0.02
KBM403
0.04
80
20


Example 278
Dispersion Solution A
50.1
HOA-MPL
0.5
OXE02
0.01
KBM403
0.02
85
15


Example 279
Dispersion Solution B
9.1
HOA-MPL
5
OXE02
0.1
KBM403
0.2
40
57


Example 280
Dispersion Solution C
9.3
HOA-MPL
5
OXE02
0.1
KBM403
0.2
40
57


Example 281
Dispersion Solution D
11.0
HOA-MPL
5
OXE02
0.1
KBM403
0.2
40
57


Example 282
Dispersion Solution A
9.4
HOA-MPL
5
OXE02
0.1
none
none
40
59


Example 283
Dispersion Solution A
2.3
HOA-MPL
5
OXE02
0.1
none
none
15
83


Example 284
Dispersion Solution A
3.3
HOA-MPL
5
OXE02
0.1
none
none
20
79


Example 285
Dispersion Solution A
14.8
HOA-MPL
3
OXE02
0.06
none
none
60
39


Example 286
Dispersion Solution A
25.5
HOA-MPL
1
OXE02
0.02
none
none
80
20


Example 287
Dispersion Solution A
48.2
HOA-MPL
0.5
OXE02
0.01
none
none
85
15


Example 288
Dispersion Solution B
8.7
HOA-MPL
5
OXE02
0.1
none
none
40
59


Example 289
Dispersion Solution C
8.9
HOA-MPL
5
OXE02
0.1
none
none
40
59


Example 290
Dispersion Solution D
10.6
HOA-MPL
5
OXE02
0.1
none
none
40
59


















TABLE 31









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)

















Example 268
34
1.562
51
40
good
0.6


Example 269
32
1.557
54
47
good
0.5


Example 270
33
1.558
54
46
good
0.6


Example 271
38
1.579
30
22
Cracking of core
0.7


Example 272
40
1.583
24
16
Residue present in
0.8







non-exposed area,







Cracking of core


Example 273
23
1.531
53
43
good
0.6


Example 274
24
1.521
56
51
good
0.5


Example 275
24
1.523
55
52
good
0.5


Example 276
26
1.543
44
37
good
0.6


Example 277
29
1.565
30
23
Residue present in
0.7







non-exposed area


Example 278
32
1.572
24
18
Residue present in
0.8







non-exposed area,







Cracking of core


Example 279
36
1.531
52
42
good
0.8


Example 280
26
1.531
52
43
good
0.6


Example 281
26
1.531
52
42
good
0.6


Example 282
25
1.531
54
42
good
0.6


Example 283
24
1.521
56
51
good
0.5


Example 284
25
1.523
55
51
good
0.5


Example 285
25
1.543
43
36
good
0.7


Example 286
28
1.565
31
24
Residue present in
0.8







non-exposed area,







Cracking of core


Example 287
31
1.572
24
17
Residue present in
0.9







non-exposed area,







Cracking of core


Example 288
35
1.531
51
42
good
0.8


Example 289
25
1.531
51
41
good
0.6


Example 290
27
1.531
52
40
good
0.6









Comparative Examples 1 and 2
Each of the paste compositions of the formulations shown in Tables 32 and 33 was prepared by the same method as that in Example 1 and then used to form a cured material for use in evaluation of physical properties and to form an optical waveguide. The results of the evaluation are shown in Tables 32 and 33. The resulting cured materials were soft because of insufficient polymerization, and it was impossible to evaluate the refractive index and the linear expansion coefficient. In addition, the non-exposed area was whitened during the development in the process of forming the optical waveguide. The non-exposed area was not removed by the immersion for 5 minutes, and it was removed by shaking the substrate for 20 minutes in the immersion process. A thin film-like residue was present on the surface of the substrate in the non-exposed area. The patterned optical waveguide in the exposed area had a gentle convex shape. The measurement of optical propagation loss was attempted but failed, because the loss was so large that the propagated light intensity was below the detection limit.
Comparative Examples 3 and 4
Each of the paste compositions of the formulations shown in Tables 32 and 33 was prepared by the same method as that in Example 1 and then used to form a cured material for use in evaluation of physical properties and to form an optical waveguide. The results of the evaluation are shown in Tables 32 and 33. The temperature-dependency of the refractive index and the linear expansion coefficient were both relatively large. The non-exposed area was whitened during the development in the process of forming the optical waveguide. A several μm-thick film was left in the non-exposed area even after the shaking for 20 minutes in the developing solution. The measurement of optical propagation loss was attempted but failed, because the loss was so large that the propagated light intensity was below the detection limit.
Comparative Examples 5 to 10
Each of the paste compositions of the formulations shown in Tables 32 and 33 was prepared by the same method as that in Example 1 and then used to form a cured material for use in evaluation of physical properties and to form an optical waveguide. The results of the evaluation are shown in Tables 32 and 33.









TABLE 32









Components of Paste Composition



















Content of







Content of Barium
Compoound A and





Polymerization
Silane
Sulfate based on
Resin based on



Dispersion Solution
Resin
Initiator
Coupling Agent
Amount of Solid
Amount of Solid



















Amount

Amount

Amount

Amount
Components
Components



Sample
(g)
Material
(g)
Material
(g)
Material
(g)
(% by weight)
(% by weight)





















Comparative
Dispersion Solution N
9.8
Resin A
5
OXE02
0.1
KBM403
0.2
40
51


Example 1


Comparative
Dispersion Solution N
9.4
Resin A
5
OXE02
0.1
none
none
40
53


Example 2


Comparative
Dispersion Solution O
9.1
Resin A
5
OXE02
0.1
KBM403
0.2
40
55


Example 3


Comparative
Dispersion Solution O
8.8
Resin A
5
OXE02
0.1
none
none
40
57


Example 4


Comparative
Dispersion Solution P
9.8
Resin A
5
OXE02
0.1
KBM403
0.2
40
57


Example 5


Comparative
Dispersion Solution P
2.4
Resin A
5
OXE02
0.1
KBM403
0.2
15
80


Example 6


Comparative
Dispersion Solution P
3.4
Resin A
5
OXE02
0.1
KBM403
0.2
20
76


Example 7


Comparative
Dispersion Solution P
15.4
Resin A
3
OXE02
0.06
KBM403
0.12
60
38


Example 8


Comparative
Dispersion Solution P
26.5
Resin A
1
OXE02
0.02
KBM403
0.04
80
20


Example 9


Comparative
Dispersion Solution P
50.1
Resin A
0.5
OXE02
0.01
KBM403
0.02
85
15


Example 10


















TABLE 33









Results














Mean








Particle

Temperature



Diameter in

Dependency of
Coefficient of

Optical



Paste

the Refractive
Linear

Propagation



Compositon
Refractive
Index
Expansion

Loss



(nm)
Index
(ppm/° C.)
(ppm/° C.)
Developability
(dB/cm)














Comparative Example 1
35
Impossible to evaluate because of
Unclear pattern,




insufficient polymerization
Residue present in non-exposed





area


Comparative Example 2
34
Impossible to evaluate because of
Unclear pattern,




insufficient polymerization
Residue present in non-exposed





area












Comparative Example 3
52
1.557
74
67
Difficult to remove non-exposed area


Comparative Example 4
50
1.557
74
68
Difficult to remove non-exposed area













Comparative Example 5
54
1.556
53
44
good
1.0


Comparative Example 6
55
1.552
58
53
good
0.8


Comparative Example 7
54
1.553
57
51
good
0.9


Comparative Example 8
56
1.562
46
38
good
1.2


Comparative Example 9
61
1.572
33
24
good
1.5


Comparative Example 10
62
1.575
26
19
Residue present in
2.3







non-exposed area,







Cracking of core









INDUSTRIAL APPLICABILITY
The optical waveguide-forming paste composition of the present invention is suitable for use in forming optical interconnections and other components to transmit information between LSIs on circuit boards which may be used in information-processing devices to make high-speed signal transmission, such as personal computers, hard-disc recorders, DVD recorders, game machines, and cellular phones.

## Claims

1. An optical waveguide-forming paste composition, comprising:
(A) barium sulfate particles with a mean particle diameter of 1 nm or more to 50 nm or less;
(B) a compound having a polymerizable group and a carboxyl group, or a phosphoric ester compound having a polymerizable group; and
(C) an organic solvent.

2. The optical waveguide-forming paste composition according to claim 1, wherein the compound having a polymerizable group and a carboxyl group comprises a compound represented by the formula (1):




in the formula (1), R1 represents a hydrogen atom or a methyl group, and R2 represents a bivalent group represented by any one of the following formulae (2) to (4):




in the formulae (2) to (4), n and m each represent an integer of 1 to 3.

3. The optical waveguide-forming paste composition according to claim 2, wherein R1 in the formula (1) is a hydrogen atom, R2 is a bivalent group represented by the formula (4), and n is 2.

4. The optical waveguide-forming paste composition according to claim 1, wherein the phosphoric ester compound having a polymerizable group comprises a compound represented by the formula (5):




in the formula (5), R3 to R5 each represent a monovalent group represented by any one of the following formulae (6) to (10) or a hydrogen atom, and R3 to R5 may be the same or different, provided that not all of R3 to R5 are hydrogen atoms:




in the formulae (6) to (10) R6 to R9 each represent a hydrogen atom or a methyl group. R10 and R11 each represent a bivalent group of 1 to 10 carbon atoms, and R12 represents a bivalent group of 1 to 10 carbon atoms having a hydroxyl group.

5. The optical waveguide-forming paste composition according to claim 4, wherein at least one of R3, R4 and R5 in the formula (5) is a monovalent group represented by the formula (8).

6. The optical waveguide-forming paste composition according to claim 1, further comprising a resin having a polymerizable group.

7. The optical waveguide-forming paste composition according to claim 6, wherein the resin having a polymerizable group comprises a resin represented by the formula (11) or (12):

8. The optical waveguide-forming paste composition according to claim 1, further comprising a silane coupling agent.

9. An optical waveguide, comprising a cured material produced by curing the optical waveguide-forming composition according to claim 1.