WO2021060283A1 - Composition de formation de pellicule de sous-couche, stratifié, procédé de production de motif et procédé de production de dispositif à semi-conducteur - Google Patents

Composition de formation de pellicule de sous-couche, stratifié, procédé de production de motif et procédé de production de dispositif à semi-conducteur Download PDF

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WO2021060283A1
WO2021060283A1 PCT/JP2020/035814 JP2020035814W WO2021060283A1 WO 2021060283 A1 WO2021060283 A1 WO 2021060283A1 JP 2020035814 W JP2020035814 W JP 2020035814W WO 2021060283 A1 WO2021060283 A1 WO 2021060283A1
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ring
composition
group
forming
polymer compound
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PCT/JP2020/035814
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English (en)
Japanese (ja)
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旺弘 袴田
直也 下重
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富士フイルム株式会社
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Priority to JP2021548935A priority Critical patent/JP7303891B2/ja
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C59/00—Surface shaping of articles, e.g. embossing; Apparatus therefor
    • B29C59/02—Surface shaping of articles, e.g. embossing; Apparatus therefor by mechanical means, e.g. pressing
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/30—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08F—MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
    • C08F299/00—Macromolecular compounds obtained by interreacting polymers involving only carbon-to-carbon unsaturated bond reactions, in the absence of non-macromolecular monomers
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
    • C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
    • C08G59/20—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the epoxy compounds used
    • C08G59/32—Epoxy compounds containing three or more epoxy groups
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09D—COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR
    • C09D201/00—Coating compositions based on unspecified macromolecular compounds
    • C09D201/02—Coating compositions based on unspecified macromolecular compounds characterised by the presence of specified groups, e.g. terminal or pendant functional groups
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
    • H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
    • H01L21/027—Making masks on semiconductor bodies for further photolithographic processing not provided for in group H01L21/18 or H01L21/34

Definitions

  • the present invention relates to a composition for forming an underlayer film.
  • the present invention also relates to a method for producing a laminate and a pattern and a method for producing a semiconductor element to which the composition for forming an underlayer film is applied.
  • the imprint method is a technique for transferring a fine pattern to a plastic material by pressing a mold (generally also called a mold or stamper) on which a pattern is formed. Since it is possible to easily produce a precise fine pattern by using the imprint method, it is expected to be applied in various fields in recent years, such as the precision processing field for semiconductor integrated circuits. In particular, nanoimprint technology for forming nano-order level fine patterns is drawing attention.
  • the imprint method is roughly classified into a thermal imprint method and an optical imprint method according to the transfer method.
  • a mold is pressed against a thermoplastic resin heated to a temperature equal to or higher than the glass transition temperature (hereinafter, also referred to as “Tg”), and after cooling, the mold is peeled off from the resin to form a fine pattern on the resin.
  • Tg glass transition temperature
  • This method has advantages such as being able to select various materials, but also has problems such as high pressure being required during pressing and the finer the pattern size, the more easily the dimensional accuracy is lowered due to heat shrinkage or the like. ..
  • the composition is photocured while the mold is pressed against the photocurable pattern-forming composition, and then the mold is peeled off from the composition (Patent Document 1).
  • This method does not require high-pressure application or high-temperature heating, and has the advantage that fine patterns can be formed with high accuracy because dimensional fluctuations are small before and after curing.
  • nanocasting method that combines the advantages of both the thermal imprint method and the optical imprint method and a reversal imprint method for producing a three-dimensional laminated structure have been reported.
  • one of the issues is to improve the adhesion between the base material and the pattern-forming composition as the pattern becomes finer. That is, in the step of peeling the mold from the cured product of the pattern forming composition, in order to prevent the cured product from peeling from the base material and adhering to the mold, the base material and the pattern forming composition are separated from each other. Sufficient adhesion is required. Therefore, for example, as shown in Patent Documents 2 to 5, a technique for providing an underlayer film for improving the adhesion between the base material and the pattern-forming composition has been proposed.
  • the technique of providing the underlayer film has brought about a certain improvement in the pattern formation by the imprint method.
  • the conventional underlayer film forming composition when the underlayer film forming composition is applied on the base material, the underlayer film forming composition becomes a sea-island state on the base material and a uniform underlayer film cannot be formed. It turns out that there are cases. If the underlayer film cannot be formed uniformly in this way, there is a risk that a region having low adhesion may be partially generated, or the wet spread of the pattern forming composition applied to the surface of the underlayer film may be hindered.
  • the present invention has been made in view of the above problems, and an object of the present invention is to provide a composition for forming an underlayer film that can suppress the composition for forming an underlayer film from becoming a sea-island state on a substrate in an imprint method. .. Another object of the present invention is to provide a method for producing a laminate and a pattern and a method for producing a semiconductor element to which the composition for forming an underlayer film is applied.
  • the above problems are the polymer compound A having a polymerizable functional group and a relatively low ring content, and the polymer compound A having a polymerizable functional group and a relatively high ring content in the composition for forming an underlayer film.
  • the solution was solved by sufficiently increasing the content of one of the polymer compounds B.
  • the above problem was solved by the following means ⁇ 1>, preferably by the means after ⁇ 2>.
  • ⁇ 1> A composition for forming an underlayer film containing a polymer compound A having a polymerizable functional group, a polymer compound B having a polymerizable functional group, and a solvent.
  • Ring content Rc a representative of the number of moles of ring per unit mass of the polymer compound A is not more than 0.0010 mol / g
  • the ring content Rc b which represents the number of moles of the ring per unit mass of the polymer compound B, is 0.0015 mol / g or more.
  • the content of either the polymer compound A or the polymer compound B in the composition for forming the underlayer film is 100 parts by mass, the other content is 1 to 30 parts by mass.
  • the ring content Rc b is 0.002 mol / g or more.
  • the difference between the ring-containing rate Rc a ring with content Rc b is 0.7 mol / g or more,
  • ⁇ 5> When the content of the polymer compound A in the composition for forming the lower layer film is 100 parts by mass, the content of the polymer compound B in the composition for forming the lower layer film is 1 to 20 parts by mass.
  • the ring content Rc b is 0.002 to 0.02 mol / g.
  • the content of the polymer compound B in the composition for forming the lower layer film is 100 parts by mass
  • the content of the polymer compound A in the composition for forming the lower layer film is 1 to 20 parts by mass.
  • the ring content Rc b is 0.002 to 0.02 mol / g.
  • Ring content Rc all representing the number of moles of ring per unit mass of the entire polymer compound is 0.0005 to 0.03 mol / g
  • the polymer compound B contains the above ring in the side chain of the polymer compound B.
  • the ring is linked to the main chain of the polymer compound B via a single bond or a linking group having a linking length of 1 to 10 atoms.
  • the polymer compound B has an aromatic ring as the above ring.
  • the aromatic ring is a benzene ring,
  • At least one of the weight average molecular weight of the polymer compound A and the weight average molecular weight of the polymer compound B is 4000 or more.
  • the polymerizable functional group is a group containing an ethylenically unsaturated bond.
  • Polymer compounds A and B are acrylic resins, The composition for forming an underlayer film according to any one of ⁇ 1> to ⁇ 15>.
  • the content of the solvent in the composition for forming the underlayer film is 99.5 to 99.9% by mass.
  • ⁇ 18> Applied between a substrate and a pattern-forming composition comprising a polymerizable compound and a photopolymerization initiator.
  • a laminate comprising a base material and a lower layer film formed from the lower layer film forming composition according to any one of ⁇ 1> to ⁇ 16> on the base material.
  • a pattern-forming composition is applied to the surface of the underlayer film in the laminate according to ⁇ 19>.
  • the pattern-forming composition is cured with the molds in contact with each other.
  • a method for producing a pattern which comprises peeling a mold from a pattern-forming composition.
  • a method for manufacturing a semiconductor device which comprises the method for manufacturing a pattern according to ⁇ 20> as part of a process.
  • the composition for forming a lower layer film of the present invention can prevent the composition for forming a lower layer film from becoming a sea-island state on a substrate in the imprint method.
  • the numerical range represented by the symbol "-" in the present specification means a range including the numerical values before and after "-" as the lower limit value and the upper limit value, respectively.
  • process means not only an independent process but also a process that cannot be clearly distinguished from other processes as long as the intended action of the process can be achieved.
  • the notation that does not describe substitution and non-substituent with respect to a group (atomic group) means that a group having a substituent (atomic group) is included as well as a group having no substituent (atomic group). is there.
  • alkyl group when simply described as "alkyl group", this includes both an alkyl group having no substituent (unsubstituted alkyl group) and an alkyl group having a substituent (substituted alkyl group).
  • exposure means not only drawing using light but also drawing using particle beams such as an electron beam and an ion beam, unless otherwise specified.
  • energy rays used for drawing include emission line spectra of mercury lamps, far ultraviolet rays typified by excimer lasers, active rays such as extreme ultraviolet rays (EUV light) and X-rays, and particle beams such as electron beams and ion beams. Be done.
  • (meth) acrylate means both “acrylate” and “methacrylate”, or either
  • (meth) acrylic means both “acrylic” and “methacrylic", or , Either
  • (meth) acryloyl means both “acryloyl” and “methacryloyl”, or either.
  • the solid content in the composition means other components other than the solvent, and the content (concentration) of the solid content in the composition is, unless otherwise specified, based on the total mass of the composition. It is represented by the mass percentage of other components excluding the solvent.
  • the temperature is 23 ° C. and the atmospheric pressure is 101325 Pa (1 atm).
  • the weight average molecular weight (Mw) and the number average molecular weight (Mn) are shown as polystyrene-equivalent values according to gel permeation chromatography (GPC measurement) unless otherwise specified.
  • GPC measurement gel permeation chromatography
  • Mw and Mn for example, HLC-8220 (manufactured by Tosoh Corporation) is used, and guard columns HZ-L, TSKgel Super HZM-M, TSKgel Super HZ4000, TSKgel are used as columns. It can be obtained by using Super HZ3000 and TSKgel Super HZ2000 (manufactured by Tosoh Corporation).
  • the measurement is carried out using THF (tetrahydrofuran) as the eluent.
  • a UV ray (ultraviolet) wavelength 254 nm detector is used for detection in GPC measurement.
  • each layer constituting the laminated body when the positional relationship of each layer constituting the laminated body is described as "upper” or “lower", the other layer is above or below the reference layer among the plurality of layers of interest. All you need is. That is, a third layer or element may be further interposed between the reference layer and the other layer, and the reference layer and the other layer need not be in contact with each other.
  • the direction in which the layers are stacked on the base material is referred to as "upper", or if there is a photosensitive layer, the direction from the base material to the photosensitive layer is referred to as "upper”.
  • the opposite direction is referred to as "down”. It should be noted that such a vertical setting is for convenience in the present specification, and in an actual embodiment, the "upward" direction in the present specification may be different from the vertical upward direction.
  • imprint preferably refers to a pattern transfer having a size of 1 nm to 10 mm, and more preferably refers to a pattern transfer (nanoimprint) having a size of about 10 nm to 100 ⁇ m.
  • the composition for forming a lower layer film of the present invention in the imprint method contains a polymer compound A having a polymerizable functional group, a polymer compound B having a polymerizable functional group, and a solvent.
  • the ring content Rc a representative of the number of moles of ring per unit mass of the polymer compound A or less 0.0010 mol / g, ring-containing representing the number of moles of ring per unit mass of the polymer compound B
  • the ratio Rc b was 0.0015 mol / g or more, and the content of either the polymer compound A or the polymer compound B in the composition for forming the lower layer film was 100 parts by mass. Occasionally, the content of the other is 1-30 parts by mass.
  • composition for forming a lower layer film of the present invention can prevent the composition for forming a lower layer film from becoming a sea-island state on a substrate in the imprint method. The reason for this is not clear, but it is presumed to be as follows.
  • the composition for forming a lower layer film of the present invention since one of the polymer compounds A and B is sufficiently large in quantity with respect to the other, many parts of the polymer compounds have relatively similar compatibility. It is presumed that it became composed of compounds and phase separation was less likely to occur. Further, from the viewpoint of a small amount of the components of the polymer compounds A and B, it is presumed that the small amount of the components makes it difficult to aggregate and the dispersed state is easily maintained in the large amount of components. From these facts, it is considered that in the imprint method, it was possible to prevent the composition for forming the underlayer film from becoming a sea-island state on the base material.
  • the composition for forming an underlayer film of the present invention since the polymer compound has a polymerizable group, the polymerizable group reacts with the constituent material of the composition for forming a pattern to form a crosslink, so that the composition is formed with the underlayer film. It is considered that the adhesion with the pattern-forming composition is improved. Further, when the composition for forming an underlayer film of the present invention contains the polymer compound B having a relatively high ring content, the interaction between the underlayer film and the base material (for example, ⁇ - ⁇ interaction) increases. Conceivable.
  • the polymer compound A having a relatively low ring content may have a low glass transition temperature due to the small amount of aromatic rings, thereby performing a function of imparting flexibility to the underlayer film.
  • the lower layer film has flexibility, it is considered that the force for peeling the lower layer film is relaxed and the destruction of the lower layer film is suppressed. That is, it is considered that the adhesion between the lower layer film and the base material is improved by the total effect of the effect of increasing the interaction between the lower layer film and the base material and the effect of imparting flexibility to the lower layer film as described above. Be done. As a result, in the imprint method, the quality and production efficiency of the cured product having a pattern are improved.
  • Polymer Compound A As described above, a polymer compound having a polymerizable group, ring content Rc a representative of the number of moles of ring per unit mass of the polymer compound is less than or equal to 0.0010 mol / g It is a polymer compound.
  • a "polymer compound” means a compound having a weight average molecular weight of 2000 or more.
  • the polymer compound A is not particularly limited, but is preferably, for example, an acrylic resin, a vinyl resin, a styrene resin, a novolak resin, or the like.
  • the lower limit of the weight average molecular weight is preferably 4000 or more, more preferably 6000 or more, further preferably 10000 or more, and particularly preferably 15000 or more.
  • the upper limit is preferably 70,000 or less, more preferably 60,000 or less, and may be 50,000 or less.
  • the method for measuring the weight average molecular weight is as described above.
  • the weight average molecular weight is 4000 or more, the film stability at the time of heat treatment is further improved, which leads to the improvement of the surface shape at the time of forming the lower layer film.
  • the weight average molecular weight is 70,000 or less, the solubility in a solvent is improved, and spin coating and the like can be easily applied.
  • the upper limit of the ring-containing rate Rc a is preferably less 0.0008 mol / g, more preferably at most 0.0006 mol / g, more preferably not more than 0.0005 mol / g.
  • the ring content is zero, that is, the polymer compound A preferably does not contain a ring in the molecule, but may be about 0.0001 mol / g.
  • the lower the ring content of the polymer compound A the greater the degree of freedom of the polymer compound A in the composition for forming the underlayer film, and the formation of crosslinks with the constituent materials of the composition for pattern formation applied on the underlayer film. Is promoted.
  • Ring content Rc a are prepared, for example, by increasing or decreasing the proportion of the repeating unit containing no repeating units and ring containing a ring in the polymer compound A.
  • the ring content of the polymer compound can be obtained by dividing the number of rings converted into moles by the mass of the polymer compound.
  • the ring content of the polymer compound is ⁇ [(the number of rings in the repeating unit) ⁇ (molar ratio in the polymer compound of the repeating unit)] / ⁇ [( It can also be calculated by the formula (amount of formula for repeating units) x (molar ratio of repeating unit in polymer compound)].
  • ⁇ represents the sum of all the repeating units constituting the polymer.
  • the ring content of the polymer compound is calculated as [0 ⁇ 0.4 + 1 ⁇ 0.6] / [214 ⁇ 0.4 + 348 ⁇ 0.6]. From about 0.0020 mol / g.
  • the number of rings shall be counted in units of a single ring. Therefore, in the case of a fused ring, the individual monocycles constituting the fused ring are counted separately. For example, in the case of naphthalene ring and norbornene ring, the number of rings is 2.
  • the ring is preferably in the side chain of the polymer compound A.
  • the “side chain” refers to a main chain (an atomic chain having the maximum number of atoms; when an atom having two or more single or condensed rings shares an atom with such an atomic chain. Means an atomic group branched from the main chain as a whole.).
  • the number of rings in one repeating unit in the polymer compound A is preferably 1 to 5, more preferably 1 to 3, further preferably 1 or 2, and preferably 1. Especially preferable.
  • they may be the same kind or different from each other.
  • rings in the polymer compound A when there are a plurality of rings in the polymer compound A, they may be in the same repeating unit or may be in different repeating units. Further, when multiple rings are in the same repeating unit, they may be present in series on a common side chain or in parallel on a branched side chain.
  • the ring that the polymer compound A can have may be a monocyclic ring or a condensed ring, but it is preferably a monocyclic ring.
  • the number of monocyclic rings constituting the condensed ring is preferably 2 to 5, more preferably 2 to 4. It is more preferably 2 or 3, and particularly preferably 2.
  • the ring that the polymer compound A can have is not particularly limited and may be an alicyclic ring or an aromatic ring, but an aromatic ring is preferable.
  • the alicyclic has preferably 30 or less carbon atoms, more preferably 25 or less, further preferably 15 or less, and particularly preferably 10 or less. Further, the alicyclic is preferably a cycloalkane ring having 10 or less carbon atoms or a cycloalkane ring having 10 or less carbon atoms, more preferably a cycloalkane ring having 10 or less carbon atoms, and having 4 to 6 carbon atoms. It is more preferably a cycloalkane ring.
  • the alicyclic ring is, for example, a cyclopropane ring, a cyclobutane ring, a cyclopentane ring, a cyclohexane ring, a cycloheptane ring, a cyclooctane ring, a cyclopropene ring, a cyclobutene ring, a cyclopentene ring, a cyclohexene ring, a cycloheptene ring or a cyclooctene ring.
  • the aromatic ring may be an aromatic hydrocarbon ring or an aromatic heterocycle.
  • the number of carbon atoms in one aromatic ring is preferably 30 or less, more preferably 25 or less, further preferably 15 or less, and 10 or less. It is particularly preferable to have.
  • the aromatic hydrocarbon ring is preferably a benzene ring, a naphthalene ring, an anthracene ring, a phenanthrene ring, a tetracene ring, a tetraphen ring, a triphenylene ring or a pyrene ring, and is preferably a benzene ring, a naphthalene ring, an anthracene ring or a phenanthrene ring. It is more preferable that it is a benzene ring or a naphthalene ring.
  • the number of atoms (number of ring members) forming a ring in one aromatic ring is preferably 30 or less, more preferably 25 or less, and preferably 15 or less. It is more preferably 10 or less, and particularly preferably 10 or less.
  • aromatic heterocycles include pyrrole ring, furan ring, thiophene ring, imidazole ring, pyrazole ring, oxazole ring, thiazole ring, indole ring, benzofuran ring, benzothiophene ring, benzimidazole ring, benzoxazole ring, benzothiazole ring.
  • the ring that the polymer compound A can have is an unsubstituted aromatic ring, or an aromatic ring having one or more substituents and having an expression amount of one or more substituents of 1000 or less, respectively. It may be a ring.
  • the ring that the polymer compound A can have is preferably an unsubstituted aromatic ring.
  • the linking group that connects the ring that the polymer compound A can have and the main chain of the polymer compound A is not treated as a substituent of the ring.
  • the number of substituents is preferably 5 or less, more preferably 3 or less, further preferably 2 or less, and 1 It is particularly preferable to have.
  • the formula amount of each of the substituents is preferably 500 or less, more preferably 300 or less, further preferably 250 or less, and particularly preferably 200 or less.
  • the substituent contained in the ring that the polymer compound A can have is not particularly limited, but is preferably the following substituent T, for example.
  • Substituent T is halogen atom, cyano group, nitro group, hydrocarbon group, heterocyclic group, -ORt 1 , -CORt 1 , -COORt 1 , -OCORt 1 , -NRt 1 Rt 2 , -NHCORt 1 , -CONRT. 1 Rt 2 , -NHCONRT 1 Rt 2 , -NHCOORt 1 , -SRt 1 , -SO 2 Rt 1 , -SO 2 ORt 1 , -NHSO 2 Rt 1 and -SO 2 NRt 1 Rt 2 is there.
  • Rt 1 and Rt 2 independently represent a hydrogen atom, a hydrocarbon group, or a heterocyclic group, respectively. When Rt 1 and Rt 2 are hydrocarbon groups, they may be bonded to each other to form a ring.
  • examples of the halogen atom include a fluorine atom, a chlorine atom, a bromine atom and an iodine atom.
  • examples of the hydrocarbon group include an alkyl group, an alkenyl group, an alkynyl group, and an aryl group.
  • the number of carbon atoms of the alkyl group is preferably 1 to 10, more preferably 1 to 5, and even more preferably 1 or 2.
  • the alkyl group may be linear, branched or cyclic, preferably linear or branched.
  • the alkenyl group preferably has 2 to 10 carbon atoms, more preferably 2 to 5 carbon atoms, and particularly preferably 2 or 3 carbon atoms.
  • the alkenyl group may be linear, branched or cyclic, preferably linear or branched.
  • the alkynyl group preferably has 2 to 10 carbon atoms, and more preferably 2 to 5 carbon atoms.
  • the alkynyl group may be linear or branched.
  • the aryl group preferably has 6 to 10 carbon atoms, more preferably 6 to 8 carbon atoms, and even more preferably 6 to 7 carbon atoms.
  • the heterocyclic group may be monocyclic or polycyclic.
  • the heterocyclic group is preferably a monocyclic ring or a polycyclic ring having 2 to 4 rings.
  • the number of heteroatoms constituting the ring of the heterocyclic group is preferably 1 to 3.
  • the hetero atom constituting the ring of the heterocyclic group is preferably a nitrogen atom, an oxygen atom or a sulfur atom.
  • the number of carbon atoms constituting the ring of the heterocyclic group is preferably 3 to 10, more preferably 3 to 8, and even more preferably 3 to 5.
  • the hydrocarbon group and the heterocyclic group as the substituent T may have yet another substituent or may be unsubstituted.
  • the above-mentioned Substituent T can be mentioned.
  • the substituent T as described above includes, for example, a halogen atom (particularly a fluorine atom, a chlorine atom and a bromine atom), an alkyl group having 1 to 5 carbon atoms (particularly a methyl group, an ethyl group and a propyl group).
  • a halogen atom particularly a fluorine atom, a chlorine atom and a bromine atom
  • an alkyl group having 1 to 5 carbon atoms particularly a methyl group, an ethyl group and a propyl group.
  • Alkenyl groups with 2 to 5 carbon atoms (particularly ethenyl groups (vinyl groups) and propenyl groups), alkoxy groups with 1 to 5 carbon atoms (particularly methoxy groups, ethoxy groups and propoxy groups), hydroxyl groups, thiol groups, carbonyl groups, thio
  • These include a carbonyl group, a carboxyl group, an amino group, a nitro group and a phenyl group.
  • the substituent T is preferably a fluorine atom, a methyl group, an ethyl group, a methoxy group, an ethoxy group, a hydroxyl group, a carbonyl group and a carboxyl group.
  • These substituents may have yet another substituent or may be unsubstituted.
  • the ring that the polymer compound A can have is preferably linked to the main chain of the polymer compound A via a single bond or a linking group having a link length of 1 to 10 atoms.
  • the linking length of the linking group is the shortest path among the atomic chains that connect the ring and the main chain of the polymer compound to each other (at both ends, the atoms contained in the ring and the main chain of the polymer compound are not included). It refers to the number of atoms in the atomic chain that constitutes.
  • the polymer compound when it can be grasped that the polymer compound has a phenyl group in the side chain, it is between the branch point A1 and the ring B1 of the main chain and the side chain of the polymer compound.
  • the number of constituent atoms is counted for the shortest atomic chain (the part of the thick line from positions X1 to Y1 in the equation).
  • the linking length of the linking group is 7.
  • an asterisk "*" in a chemical formula indicates a bond with another atom which is not specified.
  • the ring that the polymer compound A can have is preferably linked to the main chain of the polymer compound A via a single bond.
  • the upper limit of the linking length of the linking group is preferably 8 or less, preferably 6 or less. Is more preferable.
  • the lower limit of the linking length of the linking group is not particularly limited, but may be 2 or more or 3 or more.
  • the alkylene group preferably has 1 to 3 carbon atoms, and more preferably 1 or 2 carbon atoms.
  • the number of carbon atoms of the alkenylene group is more preferably 2 or 3, and even more preferably 2.
  • the arylene group may be monocyclic or polycyclic, preferably monocyclic or bicyclic, and more preferably monocyclic.
  • One ring constituting the arylene group is preferably a 6-membered ring.
  • the linking group may have a substituent such as the substituent T, but preferably does not contain a polymerizable group as the substituent, and more preferably unsubstituted.
  • the substituent is preferably, for example, a fluorine atom, a methyl group, an ethyl group, a methoxy group, an ethoxy group, a hydroxyl group, a carbonyl group and a carboxyl group.
  • a plurality of the same constituent elements may be selected within the same group.
  • the polymerizable group of the polymer compound A is selected so that it can react with the material in the pattern-forming composition described later to form a crosslink.
  • the polymerizable group may be at least one in the side chain of some repeating units of the polymer compound A.
  • the number of polymerizable groups in one repeating unit is not particularly limited, but is preferably 1 to 5, more preferably 1 to 3, further preferably 1 or 2, and may be 1. ..
  • the polymer compound A has a plurality of the polymerizable groups, they may be the same kind or different from each other.
  • there are a plurality of polymerizable groups in the polymer compound A they may be in the same repeating unit or in different repeating units.
  • multiple polymerizable groups are in the same repeating unit, they may be present in series on a common side chain or in parallel on a branched side chain.
  • the polymerizable group of the polymer compound A is not particularly limited as long as it can form a crosslink as described above, but is preferably a group having an ethylenically unsaturated bond. Further, some polymerizable groups may be polymerizable groups containing a heterocycle as long as the effects of the present invention are not impaired.
  • the group having an ethylenically unsaturated bond is preferably a group having a vinyl group or an ethynyl group, and more preferably a group having a vinyl group.
  • These groups may have substituents.
  • the polymerizable group having a substituent include a methacryloyl group and a methacryloyloxy group.
  • the group having an ethylenically unsaturated bond is particularly preferably a (meth) acryloyloxy group.
  • the polymerizable group containing a heterocycle is, for example, a group containing a cyclic ether.
  • the cyclic ether group is, for example, a cyclic alkyleneoxy group having 2 to 6 carbon atoms, and specifically, an epoxy group or an oxetane group. Therefore, the polymerizable group containing the cyclic ether group is, for example, an epoxy group or an oxetane group itself, a glycidyl group or a glycidyl ether group, and the like.
  • the proportion of the polymerizable groups containing a heterocycle is preferably less than 3 mol%.
  • This ratio is preferably less than 2 mol%, more preferably less than 1.5 mol%, and even more preferably less than 1 mol%.
  • the polymerizable group preferably does not contain a polymerizable group containing a heterocycle, but may be 0.1 mol% or more.
  • the linking group linking between the main chain and the polymerizable group of the polymer compound A has an alkylene group having 1 to 5 carbon atoms and a carbon number of carbon atoms, as in the case of the linking group related to the ring that the polymer compound A can have.
  • the content of the specific linking group is the same as that of the linking group related to the ring that the polymer compound A can have.
  • the number of atoms (distance at the polymerization point) of the atomic chain constituting the shortest path between the polymerization point in the polymerizable group and the main chain of the polymer compound A is preferably 6 or more.
  • the upper limit of the polymerization point distance is preferably 50 or less, more preferably 35 or less, and even more preferably 20 or less.
  • the lower limit of the polymerization point distance is preferably 7 or more, more preferably 8 or more, and further preferably 9 or more.
  • the polymerization point distance is derived by identifying the polymerization point from the polymerizable group and counting the number of atoms in the shortest atomic chain connecting the polymerization point and the main chain of the polymer compound.
  • the "polymerization point” means an atomic group whose bonding state changes before and after a reaction with another atomic group among the polymerizable groups.
  • This "change in bond state” includes the change of unsaturated bond to saturated bond, opening of the ring, increase / decrease in the number of atoms of the bond partner, change of the atomic type of the bond partner, and some atoms. It includes being removed as small molecules (eg water).
  • the following formula (L-3) shows the relationship between a typical polymerizable group and a polymerization point.
  • the atomic group surrounded by the dotted line in the chemical formula is the polymerization point.
  • the ring and the polymerizable group may be contained in the same repeating unit, may be contained in different repeating units, or may be contained in different repeating units. It is preferable to have.
  • the degree of freedom of the polymerizable group is increased by including the ring and the polymerizable group in different repeating units. This promotes the interaction between the polymerizable group and the constituent materials in the pattern-forming composition.
  • the polymerization point distance is preferably 3 to 50 from the viewpoint of reducing the formula amount of the substituent of the ring and from the viewpoint of securing a polymerization point distance of a certain length.
  • the upper limit of this numerical range is more preferably 40 or less, and further preferably 20 or less. Further, the lower limit of this numerical range is more preferably 4 or more, and further preferably 5 or more.
  • the ratio of the repeating unit containing the ring is preferably 0.01 to 50 mol% of all the repeating units.
  • the upper limit of this numerical range is preferably 30 mol% or less, more preferably 10 mol% or less, and further preferably 5 mol% or less.
  • the lower limit of this numerical value range is preferably 0.1 mol% or more, more preferably 1 mol% or more, and further preferably 3 mol% or more.
  • the ratio of the repeating unit containing a polymerizable group is preferably 50 to 99.99% of all the repeating units.
  • the upper limit of this numerical range is preferably 99.9 mol% or less, more preferably 95 mol% or less, and further preferably 90 mol% or less.
  • the lower limit of this numerical value range is preferably 70 mol% or more, more preferably 80 mol% or more, and further preferably 85 mol% or more.
  • the content of the polymer compound A is preferably 0.01 to 10% by mass.
  • the upper limit of the above numerical range is preferably 5% by mass or less, more preferably 3% by mass or less, and further preferably 1% by mass or less.
  • the lower limit of the above numerical range is preferably 0.03% by mass or more, more preferably 0.05% by mass or more, and further preferably 0.1% by mass or more.
  • the content of the polymer compound A in the composition for forming an underlayer film is preferably 70% by mass or more with respect to the total solid content in the composition.
  • the lower limit of the above numerical range is more preferably 80% by mass or more, and further preferably 90% by mass or more.
  • the polymer compound A may be a single compound or a mixture of two or more. When the polymer compound A is a mixture, it is preferable that the total amount thereof is in the above range.
  • Polymer Compound B is a polymer compound having a polymerizable group, and has a ring content Rc b of 0.0015 mol / g or more, which represents the number of moles of rings per unit mass of the polymer compound. It is a polymer compound.
  • the polymer compound B is not particularly limited, but is preferably, for example, an acrylic resin, a vinyl resin, a styrene resin, a novolak resin, or the like.
  • the lower limit of the weight average molecular weight is preferably 4000 or more, more preferably 6000 or more, further preferably 10000 or more, and particularly preferably 15000 or more.
  • the upper limit is preferably 70,000 or less, more preferably 60,000 or less, and may be 50,000 or less.
  • the method for measuring the weight average molecular weight is as described above.
  • the weight average molecular weight is 4000 or more, the film stability at the time of heat treatment is further improved, which leads to the improvement of the surface shape at the time of forming the lower layer film.
  • the weight average molecular weight is 70,000 or less, the solubility in a solvent is improved, and spin coating and the like can be easily applied.
  • the lower limit of the ring content Rc b is preferably 0.0020 mol / g or more, more preferably 0.0025 mol / g or more, further preferably 0.0030 mol / g or more, and 0. It is particularly preferable that it is .0040 mol / g or more.
  • the upper limit of the ring content Rc b is not particularly limited, but is practically 0.015 mol / g or less, and may be 0.010 mol / g or less.
  • the ring content Rc b is prepared, for example, by increasing or decreasing the ratio of the ring-containing repeating unit and the ring-free repeating unit in the polymer compound B.
  • the ring of the polymer compound B is preferably located in the side chain of the polymer compound B.
  • the number of rings in one repeating unit in the polymer compound B is preferably 1 to 5, more preferably 1 to 3, further preferably 1 or 2, and preferably 1. Especially preferable.
  • they may be the same kind or different from each other.
  • they may be in the same repeating unit or may be in different repeating units.
  • multiple rings are in the same repeating unit, they may be present in series on a common side chain or in parallel on a branched side chain.
  • the ring of the polymer compound B may be a monocyclic ring or a condensed ring, but is preferably a monocyclic ring.
  • the number of monocyclic rings constituting the condensed ring is preferably 2 to 5, more preferably 2 to 4, 2 or 3. Is more preferable, and 2 is particularly preferable.
  • the ring contained in the polymer compound B is not particularly limited and may be an alicyclic ring or an aromatic ring, but an aromatic ring is preferable.
  • the alicyclic has preferably 30 or less carbon atoms, more preferably 25 or less, further preferably 15 or less, and particularly preferably 10 or less. Further, the alicyclic is preferably a cycloalkane ring having 10 or less carbon atoms or a cycloalkane ring having 10 or less carbon atoms, more preferably a cycloalkane ring having 10 or less carbon atoms, and having 4 to 6 carbon atoms. It is more preferably a cycloalkane ring.
  • the alicyclic ring is, for example, a cyclopropane ring, a cyclobutane ring, a cyclopentane ring, a cyclohexane ring, a cycloheptane ring, a cyclooctane ring, a cyclopropene ring, a cyclobutene ring, a cyclopentene ring, a cyclohexene ring, a cycloheptene ring or a cyclooctene ring.
  • the aromatic ring may be an aromatic hydrocarbon ring or an aromatic heterocycle.
  • the number of carbon atoms in one aromatic ring is preferably 30 or less, more preferably 25 or less, further preferably 15 or less, and 10 or less. It is particularly preferable to have.
  • the aromatic hydrocarbon ring is preferably a benzene ring, a naphthalene ring, an anthracene ring, a phenanthrene ring, a tetracene ring, a tetraphen ring, a triphenylene ring or a pyrene ring, and is preferably a benzene ring, a naphthalene ring, an anthracene ring or a phenanthrene ring. It is more preferable that it is a benzene ring or a naphthalene ring.
  • the number of atoms (number of ring members) forming a ring in one aromatic ring is preferably 30 or less, more preferably 25 or less, and preferably 15 or less. It is more preferably 10 or less, and particularly preferably 10 or less.
  • aromatic heterocycles include pyrrole ring, furan ring, thiophene ring, imidazole ring, pyrazole ring, oxazole ring, thiazole ring, indole ring, benzofuran ring, benzothiophene ring, benzimidazole ring, benzoxazole ring, benzothiazole ring.
  • the ring contained in the polymer compound B is an unsubstituted aromatic ring, or an aromatic ring having one or more substituents and having an expression amount of one or more substituents of 1000 or less, respectively. Is preferable.
  • the ring contained in the polymer compound B is preferably an unsubstituted aromatic ring.
  • the linking group that connects the ring of the polymer compound B and the main chain of the polymer compound B is not treated as a substituent of the ring.
  • the number of substituents is preferably 5 or less, more preferably 3 or less, further preferably 2 or less, and preferably 1. Especially preferable.
  • the formula amount of each of the substituents is preferably 500 or less, more preferably 300 or less, further preferably 250 or less, and particularly preferably 200 or less.
  • the substituent contained in the ring of the polymer compound B is not particularly limited, but is preferably the above-mentioned substituent T, for example.
  • the substituent T as described above includes, for example, a halogen atom (particularly a fluorine atom, a chlorine atom and a bromine atom), an alkyl group having 1 to 5 carbon atoms (particularly a methyl group, an ethyl group and a propyl group).
  • a halogen atom particularly a fluorine atom, a chlorine atom and a bromine atom
  • an alkyl group having 1 to 5 carbon atoms particularly a methyl group, an ethyl group and a propyl group.
  • Alkenyl groups with 2 to 5 carbon atoms (particularly ethenyl groups (vinyl groups) and propenyl groups), alkoxy groups with 1 to 5 carbon atoms (particularly methoxy groups, ethoxy groups and propoxy groups), hydroxyl groups, thiol groups, carbonyl groups, thio
  • These include a carbonyl group, a carboxyl group, an amino group, a nitro group and a phenyl group.
  • the substituent T is preferably a fluorine atom, a methyl group, an ethyl group, a methoxy group, an ethoxy group, a hydroxyl group, a carbonyl group and a carboxyl group.
  • These substituents may have yet another substituent or may be unsubstituted.
  • the ring of the polymer compound B is preferably linked to the main chain of the polymer compound B via a single bond or a linking group having a link length of 1 to 10 atoms. This has the effect of further improving the adhesion between the underlayer film and the base material.
  • the method for deriving the linking length of the linking group is the same as in the case of the polymer compound A.
  • the upper limit of the linking length of the linking group is preferably 8 or less, preferably 6 or less. Is more preferable.
  • the lower limit of the linking length of the linking group is not particularly limited, but may be 2 or more or 3 or more.
  • the alkylene group preferably has 1 to 3 carbon atoms, and more preferably 1 or 2 carbon atoms.
  • the number of carbon atoms of the alkenylene group is more preferably 2 or 3, and even more preferably 2.
  • the arylene group may be monocyclic or polycyclic, preferably monocyclic or bicyclic, and more preferably monocyclic.
  • One ring constituting the arylene group is preferably a 6-membered ring.
  • the linking group may have a substituent such as the substituent T, but preferably does not contain a polymerizable group as the substituent, and more preferably unsubstituted.
  • the substituent is preferably, for example, a fluorine atom, a methyl group, an ethyl group, a methoxy group, an ethoxy group, a hydroxyl group, a carbonyl group and a carboxyl group.
  • a plurality of the same constituent elements may be selected within the same group.
  • the polymerizable group of the polymer compound B is selected so that it can react with the material in the pattern-forming composition described later to form a crosslink.
  • the polymerizable group may be at least one in the side chain of some repeating units of the polymer compound B.
  • the number of polymerizable groups in one repeating unit is not particularly limited, but is preferably 1 to 5, more preferably 1 to 3, further preferably 1 or 2, and may be 1. ..
  • the polymer compound B has a plurality of the polymerizable groups, they may be the same kind or different from each other. Further, when there are a plurality of polymerizable groups in the polymer compound B, they may be in the same repeating unit or in different repeating units. Furthermore, when multiple polymerizable groups are in the same repeating unit, they may be present in series on a common side chain or in parallel on a branched side chain.
  • the polymerizable group of the polymer compound B is not particularly limited as long as it can form a crosslink as described above, but is preferably a group having an ethylenically unsaturated bond. Further, some polymerizable groups may be polymerizable groups containing a heterocycle as long as the effects of the present invention are not impaired.
  • the group having an ethylenically unsaturated bond is preferably a group having a vinyl group or an ethynyl group, and more preferably a group having a vinyl group.
  • Specific examples of the group having an ethylenically unsaturated bond are the same as in the case of the polymer compound A.
  • specific examples of the polymerizable group containing a heterocycle are the same as in the case of the polymer compound A.
  • the proportion of the polymerizable groups containing a heterocycle is preferably less than 3 mol%.
  • This ratio is preferably less than 2 mol%, more preferably less than 1.5 mol%, and even more preferably less than 1 mol%.
  • the polymerizable group preferably does not contain a polymerizable group containing a heterocycle, but may be 0.1 mol% or more.
  • the linking group linking between the main chain and the polymerizable group of the polymer compound B is an alkylene group having 1 to 5 carbon atoms and 2 to 5 carbon atoms, as in the case of the linking group related to the ring of the polymer compound B.
  • the specific content of the linking group is the same as that of the linking group related to the ring of the polymer compound B.
  • the polymerization point distance between the polymerization point in the polymerizable group and the main chain of the polymer compound B is preferably 6 or more.
  • the upper limit of the polymerization point distance is preferably 50 or less, more preferably 35 or less, and even more preferably 20 or less.
  • the lower limit of the polymerization point distance is preferably 7 or more, more preferably 8 or more, and further preferably 9 or more.
  • the ring and the polymerizable group of the polymer compound B may be contained in the same repeating unit or in different repeating units, and are preferably contained in different repeating units.
  • the degree of freedom of each of the ring and the polymerizable group is increased.
  • the interaction between the ring and the surface of the base material is promoted, and the interaction between the polymerizable group and the constituent material in the pattern-forming composition is promoted.
  • the polymerization point distance is preferably 3 to 50 from the viewpoint of reducing the formula amount of the substituent of the ring and from the viewpoint of securing a polymerization point distance of a certain length.
  • the upper limit of this numerical range is more preferably 40 or less, and further preferably 20 or less. Further, the lower limit of this numerical range is more preferably 4 or more, and further preferably 5 or more.
  • the ratio of the repeating unit containing the above ring is preferably 50 to 99.99% of all the repeating units.
  • the upper limit of this numerical range is preferably 99.90% or less, more preferably 95% or less, and further preferably 90% or less.
  • the lower limit of this numerical range is preferably 70% or more, more preferably 80% or more, and further preferably 85% or more.
  • the ratio of the repeating unit containing a polymerizable group is preferably 0.01 to 50% of all the repeating units.
  • the upper limit of this numerical range is preferably 30% or less, more preferably 10% or less, and further preferably 5% or less.
  • the lower limit of this numerical value range is preferably 0.1% or more, more preferably 1% or more, and further preferably 3% or more.
  • the content of the polymer compound B is preferably 0.01 to 10% by mass.
  • the upper limit of the above numerical range is preferably 5% by mass or less, more preferably 3% by mass or less, and further preferably 1% by mass or less.
  • the lower limit of the above numerical range is preferably 0.03% by mass or more, more preferably 0.05% by mass or more, and further preferably 0.1% by mass or more.
  • the content of the polymer compound B in the composition for forming the lower layer film is preferably 70% by mass or more with respect to the total solid content in the composition.
  • the lower limit of the above numerical range is more preferably 80% by mass or more, and further preferably 90% by mass or more.
  • the polymer compound B may be a single compound or a mixture of two or more. When the polymer compound B is a mixture, it is preferable that the total amount thereof is in the above range.
  • the polymer compounds A and B have a repeating unit represented by the following formula (AD-1), a repeating unit represented by the following formula (AD-2), and the following formula, respectively, within the range satisfying the requirements for the ring content. It is preferable to contain at least one of the repeating units represented by (AD-3).
  • X 1 represents a trivalent linking group
  • L 1 represents a single bond or a divalent linking group.
  • Ar 1 represents a group containing a ring and a polymerizable functional group;
  • X 2 and X 3 each independently represent a trivalent linking group.
  • L 2 and L 3 independently represent a single bond or a divalent linking group, respectively.
  • Ar 2 represents a group containing a ring and no polymerizable functional group.
  • Y represents a polymerizable functional group and represents * Represents the connection with the main chain.
  • the formula amount of each repeating unit is preferably 50 to 1500 independently.
  • the upper limit of this numerical range is more preferably 800 or less, and further preferably 600 or less. Further, the lower limit of this numerical range is more preferably 80 or more, and further preferably 100 or more.
  • X 1 , X 2 and X 3 are independently linear, branched or cyclic hydrocarbon groups and are substituted or unsubstituted hydrocarbon groups.
  • the number of carbon atoms of the hydrocarbon group is preferably 2 to 20, more preferably 2 to 15, and even more preferably 2 to 10.
  • X 1 , X 2 and X 3 are preferably groups represented by any one of the following formulas (AD-X1) to (AD-X3) independently of each other, and are preferably formulas (AD). More preferably, it is a group represented by ⁇ X1).
  • R 1 to R 3 independently represent a hydrogen atom or a monovalent substituent, respectively.
  • R 4 and R 5 each independently represent a monovalent substituent.
  • m and n independently represent integers of 0 to 3, respectively.
  • * 1 represents the bond with the main chain of the above polymer compound.
  • * 2 represents a connecting portion between one of the linking group L 1, L 2 and L 3.
  • the monovalent substituent as R 1 to R 5 is preferably an alkyl group, a halogen atom, a hydroxyl group or an alkoxy group.
  • the alkyl moiety in the alkyl group and the alkoxy group is more preferably a linear or branched alkyl group having 1 to 10 carbon atoms, and the linear or branched alkyl group having 1 to 5 carbon atoms. Is more preferable, an alkyl group having 1 to 3 carbon atoms is particularly preferable, and a methyl group is most preferable.
  • the halogen atom is preferably a fluorine atom, a chlorine atom and a bromine atom, more preferably a fluorine atom and a chlorine atom, and further preferably a fluorine atom.
  • m and n are preferably 0 to 2 independently of each other, more preferably 0 or 1, and may be 0.
  • a plurality of R 4 which brackets is attached may be the same as each other or may be different. Also, a plurality of R 5 parentheses is attached, it may be the same or may be different from one another.
  • R 1 to R 3 are independently hydrogen atom, halogen atom, methyl group, ethyl group, propyl group, hydroxyl group, methoxy group, ethoxy group or propoxy group. It is more preferably a hydrogen atom, a fluorine atom, a methyl group, a hydroxyl group or a methoxy group, and even more preferably a hydrogen atom, a fluorine atom or a methyl group.
  • R 4 and R 5 are each independently a halogen atom, a methyl group, an ethyl group, a propyl group, a hydroxyl group, a methoxy group, an ethoxy group or propoxy It is preferably a group, more preferably a fluorine atom, a methyl group, a hydroxyl group or a methoxy group, and even more preferably a fluorine atom or a methyl group.
  • the divalent linking groups as L 1 , L 2 and L 3 are independently alkylene groups having 1 to 5 carbon atoms and 2 to 2 carbon atoms.
  • It is preferably a group of the above combination, and is a group of one or more combinations selected from an alkylene group having 1 to 5 carbon atoms, an arylene group, -O- and -C ( O)-. Is more preferable.
  • the alkylene group preferably has 1 to 3 carbon atoms, and more preferably 1 or 2 carbon atoms.
  • the number of carbon atoms of the alkenylene group is more preferably 2 or 3, and even more preferably 2.
  • the arylene group may be monocyclic or polycyclic, preferably monocyclic or bicyclic, and more preferably monocyclic.
  • One ring constituting the arylene group is preferably a 6-membered ring.
  • the linking group may have a substituent such as the substituent T, but preferably does not contain a polymerizable group as the substituent, and more preferably unsubstituted.
  • the substituent is preferably, for example, a fluorine atom, a methyl group, an ethyl group, a methoxy group, an ethoxy group, a hydroxyl group, a carbonyl group and a carboxyl group.
  • a plurality of the same constituent elements may be selected within the same group.
  • L 1 , L 2 and L 3 have an arylene group such as a phenylene group, that is, an aromatic ring.
  • an aromatic ring such as a phenylene group
  • the interaction between the aromatic ring and the base material may occur, and the adhesion between the lower layer film and the base material may be further improved.
  • the aromatic rings contained in L 1 , L 2 and L 3 are also unsubstituted or the formula amount of the substituent is 1000 or less, respectively. As a result, the adhesion is further improved.
  • the rings in Ar 1 and Ar 2 are not particularly limited as long as they interact with the substrate in close contact with each other as described above, and are aromatic hydrocarbon rings. However, it may be an aromatic heterocycle, preferably an aromatic hydrocarbon ring. In addition, the preferred embodiment of the aromatic ring is also as described above.
  • the aromatic ring is preferably, for example, a benzene ring, a naphthalene ring, an anthracene ring, a phenanthrene ring, a tetracene ring, a tetraphen ring, a triphenylene ring or a pyrene ring, and is a benzene ring, a naphthalene ring, an anthracene ring or a phenanthrene ring. Is more preferable, and a benzene ring or a naphthalene ring is further preferable.
  • the polymerizable group and Y in Ar 1 are particularly capable of forming crosslinks by reacting with the materials in the pattern-forming composition described later, as described above.
  • it is preferably a group having an ethylenically unsaturated bond, and may be a group containing a cyclic ether group.
  • the preferred embodiment of the polymerizable group is also as described above.
  • R represents a hydrogen atom or a substituent.
  • substituents may have substituents.
  • the substituent is preferably, for example, a fluorine atom, a methyl group, an ethyl group, a methoxy group, an ethoxy group, a hydroxyl group, a carbonyl group and a carboxyl group.
  • the polymerizable group having a substituent include a methacryloyl group and a methacryloyloxy group.
  • the group having an ethylenically unsaturated bond is particularly preferably a (meth) acryloyloxy group.
  • the polymer compounds A and B preferably contain at least one of the following six types of resins.
  • R 1 ⁇ R 3 has the same meaning as R 1 ⁇ R 3 in the formula (AD-X1), R 4 and m are as defined and R 4 and m in the formula (AD-X2), L 4 to L 6 represent a single bond or a divalent linking group.
  • Ar 1 is synonymous with Ar 1 in equation (AD-1).
  • Ar 2 is synonymous with Ar 2 in equation (AD-2).
  • Y is synonymous with Y in equation (AD-3). Each element is independent unless otherwise specified.
  • the alkylene group preferably has 1 to 3 carbon atoms, and more preferably 1 or 2 carbon atoms.
  • the number of carbon atoms of the alkenylene group is more preferably 2 or 3, and even more preferably 2.
  • the arylene group may be monocyclic or polycyclic, preferably monocyclic or bicyclic, and more preferably monocyclic.
  • One ring constituting the arylene group is preferably a 6-membered ring.
  • the linking group may have a substituent such as the substituent T, but preferably does not contain a polymerizable group as the substituent, and more preferably unsubstituted.
  • the substituent is preferably, for example, a fluorine atom, a methyl group, an ethyl group, a methoxy group, an ethoxy group, a hydroxyl group, a carbonyl group and a carboxyl group.
  • a plurality of the same constituent elements may be selected within the same group.
  • the repeating unit is the formula (AD-4b), the formula (AD-6b), the formula (AD-7b), the formula (AD-9b), the formula (AD-10b), and the formula (AD-12b), respectively. It is also preferable that it is a repeating unit represented. These examples are examples in which each repeating unit contains a group having an ethylenically unsaturated bond as a polymerizable group.
  • Ar 5 independently represents a divalent group containing a ring
  • R 6 independently represents a hydrogen atom or an unsubstituted or substituted methyl group, and the other symbols are described above. That's right.
  • Ar 5 preferably has a benzene ring.
  • a preferable specific example of the repeating unit represented by the above formula (AD-1) is the following structure.
  • R 6 independently represents a hydrogen atom or an unsubstituted or substituted methyl group
  • -Or -S-) is represented.
  • a preferable specific example of the repeating unit represented by the above formula (AD-2) is the following structure.
  • R 6 independently represents a hydrogen atom or an unsubstituted or substituted methyl group
  • R 6 independently represents a hydrogen atom or an unsubstituted or substituted methyl group.
  • the polymer compounds A and B refer to repeating units other than the repeating units represented by any of the above formulas (AD-1) to (AD-3) (hereinafter, also simply referred to as “other repeating units”). It can also be included. Such other repeating units are, for example, repeating units that do not contain an aromatic ring or a polymerizable group.
  • the ratio of other repeating units is preferably 15% by mass or less with respect to all the repeating units in the polymer compounds A and B.
  • the upper limit of the above numerical range is more preferably 10% by mass or less, further preferably 5% by mass or less, and particularly preferably not substantially contained.
  • substantially free means that the ratio of the other repeating units is less than 1% by mass with respect to all the repeating units in the resin.
  • the content of either the polymer compound A or the content of the polymer compound B in the composition for forming a lower layer film is set to 100 parts by mass.
  • the content of the other is 1 to 30 parts by mass.
  • the composition for forming the lower layer film when the content of the polymer compound A in the composition for forming the lower layer film is 100 parts by mass, the composition for forming the lower layer film
  • the content of the polymer compound B is 1 to 30 parts by mass.
  • the lower limit of the above numerical range is preferably 2 parts by mass or more, more preferably 4 parts by mass or more, and further preferably 5 parts by mass or more.
  • the ring content Rc b of the polymer compound B is preferably 0.002 to 0.02 mol / g.
  • the upper limit of the above numerical range is preferably 0.0050 mol / g or less, more preferably 0.0045 mol / g or less, further preferably 0.0035 mol / g or less, and 0.
  • the lower limit of the above numerical range is preferably 0.0022 mol / g or more, more preferably 0.0023 mol / g or more, and further preferably 0.0025 mol / g or more.
  • the composition for forming the lower layer film when the content of the polymer compound B in the composition for forming the lower layer film is 100 parts by mass, the composition for forming the lower layer film
  • the content of the polymer compound A is 1 to 30 parts by mass.
  • the lower limit of the above numerical range is preferably 2 parts by mass or more, more preferably 4 parts by mass or more, and further preferably 5 parts by mass or more.
  • the ring content Rc b of the polymer compound B is preferably 0.002 to 0.02 mol / g.
  • the upper limit of the above numerical range is preferably 0.0050 mol / g or less, more preferably 0.0045 mol / g or less, further preferably 0.0035 mol / g or less, and 0.
  • the lower limit of the above numerical range is preferably 0.0022 mol / g or more, more preferably 0.0023 mol / g or more, and further preferably 0.0025 mol / g or more.
  • the underlayer film forming composition of the present invention it is preferred that the ring content Rc all representing the number of moles of ring per unit mass of the entire polymer compound is from 0.0005 to 0.030 mol / g.
  • the ring content Rc all is obtained by dividing the number of molar-converted rings in the total polymer compound by the mass of the total polymer compound.
  • the ring content of the entire polymer compound is ⁇ [(the number of rings in the repeating unit) ⁇ (molar ratio in the entire polymer compound of the repeating unit)] / ⁇ [( It can also be calculated by the formula (amount of formula for repeating units) x (molar ratio of repeating units in the entire polymer compound)].
  • ⁇ represents the sum of all the repeating units constituting each polymer in the entire polymer compound.
  • the ring content Rc all can be adjusted by the respective contents of the polymer compounds A and B and the ring content.
  • the upper limit of the above numerical range is preferably 0.020 mol / g or less, more preferably 0.015 mol / g or less, and further preferably 0.010 mol / g or less.
  • the lower limit of the above numerical range is preferably 0.0006 mol / g or more, more preferably 0.0007 mol / g or more, and further preferably 0.0008 mol / g or more.
  • the underlayer film forming composition of the present invention it is preferred that a difference between the ring-containing rate Rc b ring content Rc a high molecular compound B of the polymer compound A is 0.0006 mol / g or more ..
  • the upper limit of the above numerical range is preferably 0.01 mol / g or less, more preferably 0.005 mol / g or less, and further preferably 0.003 mol / g or less.
  • the lower limit of the above numerical range is preferably 0.0008 mol / g or more, more preferably 0.0010 mol / g or more, and further preferably 0.0015 mol / g or more.
  • the composition for forming a lower layer film of the present invention may also contain a polymer compound other than the above-mentioned polymer compounds A and B (hereinafter, also simply referred to as “polymer compound C”).
  • the polymer compound C has, for example, a polymer compound containing no polymerizable group and a ring content Rc c representing the number of moles of rings in the unit mass of the polymer compound, which is more than 0.0010 mol / g and 0.0015. It is a polymer compound having a molarity of less than mol / g.
  • the proportion of the polymer compound C is preferably 5% by mass or less with respect to the total polymer compounds in the composition for forming the lower layer film.
  • the upper limit of the above numerical range is more preferably 3% by mass or less, and further preferably 2% by mass or less.
  • the composition for forming an underlayer film does not substantially contain the polymer compound C.
  • substantially free means that the proportion of the polymer compound C is less than 1% by mass with respect to the total polymer compounds.
  • the composition for forming an underlayer film contains a solvent (hereinafter, may be referred to as "solvent for underlayer film”).
  • the solvent is, for example, a compound that is liquid at 23 ° C. and has a boiling point of 250 ° C. or lower.
  • solids other than the solvent finally form the underlayer film.
  • the composition for forming the lower layer film preferably contains 99.0% by mass or more of the solvent for the lower layer film, more preferably 99.5% by mass or more, and may contain 99.6% by mass or more.
  • the solvent for forming the underlayer film may contain only one type or two or more types of the solvent. When two or more kinds are contained, it is preferable that the total amount thereof is in the above range.
  • the boiling point of the solvent for the underlayer film is preferably 230 ° C. or lower, more preferably 200 ° C. or lower, further preferably 180 ° C. or lower, further preferably 160 ° C. or lower, and 130 ° C. or lower. Is even more preferable. It is practical that the lower limit is 23 ° C, but it is more practical that it is 60 ° C or higher. By setting the boiling point in the above range, the solvent can be easily removed from the underlayer film, which is preferable.
  • the solvent for the underlayer film is preferably an organic solvent.
  • the solvent is preferably a solvent having at least one of an alkylcarbonyl group, a carbonyl group, a hydroxyl group and an ether group. Of these, it is preferable to use an aprotic polar solvent.
  • alkoxy alcohols propylene glycol monoalkyl ether carboxylates, propylene glycol monoalkyl ethers, lactic acid esters, acetate esters, alkoxypropionic acid esters, chain ketones, cyclic ketones, lactones, and alkylene carbonates are selected.
  • alkoxy alcohol examples include methoxyethanol, ethoxyethanol, methoxypropanol (for example, 1-methoxy-2-propanol), ethoxypropanol (for example, 1-ethoxy-2-propanol), and propoxypropanol (for example, 1-propanol-2-).
  • methoxyethanol for example, 1-methoxy-2-propanol
  • ethoxypropanol for example, 1-ethoxy-2-propanol
  • propoxypropanol for example, 1-propanol-2-.
  • methoxybutanol eg 1-methoxy-2-butanol, 1-methoxy-3-butanol
  • ethoxybutanol eg 1-ethoxy-2-butanol, 1-ethoxy-3-butanol
  • methylpentanol for example, 4-methyl-2-pentanol
  • propylene glycol monoalkyl ether carboxylate at least one selected from the group consisting of propylene glycol monomethyl ether acetate, propylene glycol monomethyl ether propionate, and propylene glycol monoethyl ether acetate is preferable, and propylene glycol monomethyl ether acetate (propylene glycol monomethyl ether acetate).
  • PGMEA propylene glycol monomethyl ether acetate
  • propylene glycol monoalkyl ether propylene glycol monomethyl ether (PGME) or propylene glycol monoethyl ether is preferable.
  • lactic acid ester ethyl lactate, butyl lactate, or propyl lactate is preferable.
  • acetic acid ester methyl acetate, ethyl acetate, butyl acetate, isobutyl acetate, propyl acetate, isoamyl acetate, methyl formate, ethyl acetate, butyl formate, propyl acetate, or 3-methoxybutyl acetate are preferable.
  • MMP methyl 3-methoxypropionate
  • EEP ethyl 3-ethoxypropionate
  • Chain ketones include 1-octanone, 2-octanone, 1-nonanonone, 2-nonanonone, acetone, 4-heptanone, 1-hexanone, 2-hexanone, diisobutylketone, phenylacetone, methylethylketone, methylisobutylketone, acetylacetone, Acetylacetone, ionone, diacetonyl alcohol, acetylcarbinol, acetophenone, methylnaphthyl ketone or methyl amyl ketone are preferred.
  • cyclic ketone methylcyclohexanone, isophorone or cyclohexanone is preferable.
  • ⁇ -butyrolactone ⁇ BL
  • propylene carbonate is preferable.
  • an ester solvent having 7 or more carbon atoms (preferably 7 to 14, more preferably 7 to 12 and even more preferably 7 to 10) and having a heteroatom number of 2 or less.
  • ester-based solvents having 7 or more carbon atoms and 2 or less heteroatomic atoms include amyl acetate, 2-methylbutyl acetate, 1-methylbutyl acetate, hexyl acetate, pentyl propionate, hexyl propionate, and butyl propionate.
  • Examples thereof include isobutyl isobutyrate, heptyl propionate, butyl butanoate and the like, and isoamyl acetate is particularly preferable.
  • alkoxyalcohol propylene glycol monoalkyl ether carboxylate
  • propylene glycol monoalkyl ether lactic acid ester, acetate ester
  • alkoxypropionic acid ester chain ketone, cyclic ketone, lactone, and alkylene.
  • Examples include carbonates.
  • composition for forming an underlayer film includes one or more alkylene glycol compounds, polymerizable compounds, polymerization initiators, polymerization inhibitors, antioxidants, leveling agents, thickeners, surfactants and the like. It may be included.
  • the composition for forming an underlayer film may contain an alkylene glycol compound.
  • the alkylene glycol compound preferably has 3 to 1000 alkylene glycol repeating units, more preferably 4 to 500, and even more preferably 5 to 100. It is more preferable to have 50 of them.
  • the weight average molecular weight (Mw) of the alkylene glycol compound is preferably 150 to 10000, more preferably 200 to 5000, further preferably 300 to 3000, and even more preferably 300 to 1000.
  • the alkylene glycol compounds are polyethylene glycol, polypropylene glycol, these mono or dimethyl ethers, mono or dioctyl ethers, mono or dinonyl ethers, mono or didecyl ethers, monostearate esters, monooleic acid esters, monoadiponic acid esters, monosuccinates. Acid esters are exemplified, and polyethylene glycol and polypropylene glycol are preferable.
  • the surface tension of the alkylene glycol compound at 23 ° C. is preferably 38.0 mN / m or more, and more preferably 40.0 mN / m or more.
  • the upper limit of the surface tension is not particularly specified, but is, for example, 48.0 mN / m or less.
  • the surface tension is measured at 23 ° C. using a surface tension meter SURFACE TENS-IOMETER CBVP-A3 manufactured by Kyowa Interface Science Co., Ltd. and a glass plate.
  • the unit is mN / m. Two samples are prepared for each level and measured three times each. The arithmetic mean value of a total of 6 times is adopted as the evaluation value.
  • the content of the alkylene glycol compound is 40% by mass or less, preferably 30% by mass or less, more preferably 20% by mass or less, and 1 to 1 to 2% by mass, based on the total solid content in the composition for forming the underlayer film. It is more preferably 15% by mass. Only one kind of alkylene glycol compound may be used, or two or more kinds may be used. When two or more kinds are used, it is preferable that the total amount thereof is within the above range.
  • the polymerizable compound may be monofunctional, but is preferably polyfunctional.
  • the functional number is preferably 2 to 5, more preferably 2 to 4, and even more preferably 2 or 3.
  • the polymerizable group of the polymerizable compound is an ethylenically unsaturated bond-containing group such as a vinyl group, an allyl group, a vinylphenyl group, a (meth) acryloyl group, a (meth) acryloyloxy group, and a (meth) acryloylamino group. Is preferable. Further, the polymerizable group is more preferably a (meth) acryloyl group or a (meth) acryloyloxy group.
  • the molecular weight of the polymerizable compound is preferably less than 2000, more preferably 1500 or less, further preferably 1000 or less, and may be 800 or less.
  • the lower limit is preferably 100 or more.
  • the polymerizable compound contains a ring. Thereby, the strength of the underlayer film can be further improved.
  • the ring is preferably, for example, a benzene ring or a naphthalene ring.
  • the content of the polymerizable compound used in the underlayer film forming composition is, for example, 0.0001 to 5% by mass, preferably 0.0005 to 3% by mass, based on the total solid content in the underlayer film forming composition. %, More preferably 0.01 to 1% by mass.
  • the polymerizable compound may be used alone or in combination of two or more. When two or more kinds of polymerizable compounds are used, the total amount thereof is preferably in the above range.
  • the composition for forming a lower layer film may contain a polymerization initiator, and preferably contains at least one of a thermal polymerization initiator and a photopolymerization initiator.
  • a polymerization initiator By including the polymerization initiator, the reaction of the polymerizable group contained in the composition for forming the underlayer film is promoted, and the adhesion is improved.
  • a photopolymerization initiator is preferable from the viewpoint of improving the cross-linking reactivity with the pattern-forming composition.
  • the photopolymerization initiator a radical polymerization initiator and a cationic polymerization initiator are preferable, and a radical polymerization initiator is more preferable.
  • a plurality of types of photopolymerization initiators may be used in combination.
  • thermal polymerization initiator each component described in JP-A-2013-036027, JP-A-2014-090133, and JP-A-2013-189537 can be used. Regarding the content and the like, the description in the above publication can be taken into consideration.
  • a known compound can be arbitrarily used as the radical polymerization initiator.
  • halogenated hydrocarbon derivatives for example, compounds having a triazine skeleton, compounds having an oxadiazole skeleton, compounds having a trihalomethyl group, etc.
  • acylphosphine compounds such as acylphosphine oxide, hexaarylbiimidazole, oxime derivatives and the like.
  • the description in paragraphs 0165 to 0182 of JP-A-2016-0273557 can be referred to, and the contents thereof are incorporated in the present specification.
  • acylphosphine compound examples include 2,4,6-trimethylbenzoyl-diphenyl-phosphine oxide. Further, commercially available products such as IRGACURE-819, IRGACURE1173, and IRGACURE-TPO (trade names: all manufactured by BASF) can be used.
  • the content of the photopolymerization initiator used in the underlayer film forming composition is, for example, 0.0001 to 5% by mass, preferably 0.0005 to 3%, based on the total solid content in the underlayer film forming composition. It is by mass, more preferably 0.01 to 1% by mass. When two or more kinds of photopolymerization initiators are used, the total amount thereof is preferably in the above range.
  • the composition for forming an underlayer film of the present invention is prepared by blending raw materials in a predetermined ratio.
  • the raw material refers to a component that is positively blended in the composition for forming an underlayer film, and is intended to exclude components that are unintentionally contained such as impurities.
  • a curable component and a solvent are exemplified.
  • the raw material may be a commercially available product or a synthetic product. Both raw materials may contain impurities such as metal particles.
  • the method for producing a composition for forming an underlayer film of the present invention there is a production method including filtering at least one of the raw materials contained in the composition for forming an underlayer film by using a filter. Be done. It is also preferable to mix two or more kinds of raw materials, filter them with a filter, and mix them with other raw materials (which may or may not be filtered). As a more preferable embodiment, an embodiment in which raw materials (preferably all raw materials) contained in the underlayer film forming composition are mixed and then filtered using a filter is exemplified.
  • the laminate of the present invention includes a base material and a lower layer film formed from the above-mentioned composition for forming a lower layer film and provided in contact with the base material.
  • This laminate may contain other layers on the underlayer film.
  • Such another layer is, for example, a pattern-forming composition layer formed by applying a pattern-forming composition on an underlayer film.
  • the method for producing a laminate of the present invention includes applying the above-mentioned composition for forming an underlayer film on a base material to form an underlayer film. The method of forming the lower layer film will be described later.
  • the above ratio of carbon atoms in the depth region of 10 nm from the surface is 60%. It is preferably 70% or more, more preferably 80% or more, and particularly preferably 90% or more.
  • the upper limit of the carbon content is not particularly limited, but is practically 99% or less, and may be 95% or less or 90% or less.
  • the carbon-containing base material as described above is formed by forming a carbon film such as a spin-on carbon (SOC) film, a diamond-like carbon (DLC) film, or another amorphous carbon film on a semiconductor substrate, for example. Can be made.
  • a carbon film such as a spin-on carbon (SOC) film, a diamond-like carbon (DLC) film, or another amorphous carbon film on a semiconductor substrate, for example.
  • SOC spin-on carbon
  • DLC diamond-like carbon
  • the SOC film can be formed, for example, by applying a composition base material in which a carbonaceous material is dissolved in an organic solvent by a spin coating method or the like and drying the coating.
  • a carbonaceous material for example, a carbon-rich compound containing 80% by mass or more of carbon with respect to the total molecular weight of the compound can be used.
  • Examples of such a carbon-rich compound include a copolymer having a nortricylene skeleton, a copolymer of phenol and dicyclopentadiene, a copolymer of naphthol and dicyclopentadiene, and a polymerizable monomer having acenaphthylene and a hydroxyl group (for example).
  • bisphenol compounds eg, fluorene bisphenol
  • JP-A-2005-128509, JP-A-2005-250434, JP-A-2006-227391, and JP-A-2007-199653 can be referred to.
  • JP-A-2005-250434, JP-A-2006-227391, and JP-A-2007-199653 can be referred to.
  • JP-A-2007-199653 can be referred to.
  • SOC film the description in paragraph 0126 of JP2011-164345A can also be referred to. The contents of these documents are incorporated herein.
  • the DLC film and other amorphous carbon films are classified into, for example, a physical vapor deposition (PVD) method using a carbon raw material such as graphite, and a chemical vapor deposition (CVD) using a hydrocarbon gas such as acetylene. It can be formed by law.
  • PVD physical vapor deposition
  • CVD chemical vapor deposition
  • the ratio of the number of carbon atoms to the total atoms excluding hydrogen is preferably 50% or more.
  • the lower limit of this ratio is more preferably 60% or more, further preferably 70% or more, and particularly preferably 80% or more.
  • the upper limit of this ratio is not particularly limited, but it is practically 99% or less, and may be 95% or less or 90% or less.
  • the carbon content in the carbon film is preferably 60% by mass or more, more preferably 70% by mass or more, and further preferably 80% by mass or more.
  • the upper limit of the carbon content is not particularly limited, but is practically 99% by mass or less, and may be 95% by mass or less or 90% by mass or less.
  • the thickness of the carbon film is preferably 50 to 300 nm.
  • the upper limit of the above numerical range is preferably 290 nm or less, more preferably 275 nm or less, and further preferably 200 nm or less. Further, the lower limit of the above numerical range is preferably 60 nm or more, more preferably 75 nm or more, and further preferably 100 nm or more.
  • the material of the semiconductor substrate is not particularly limited, but for example, silicon, glass, quartz, sapphire, silicon carbide, gallium nitride, aluminum, amorphous aluminum oxide, polycrystalline aluminum oxide, silicon nitride, silicon oxynitride, GaAsP, GaP, etc. AlGaAs, InGaN, GaN, AlGaN, ZnSe, AlGa, InP, ZnO and the like.
  • Specific examples of glass materials include aluminosilicate glass, aluminoborosilicate glass, and barium borosilicate glass.
  • the underlayer film forming composition of the present invention is usually used as a composition for forming an underlayer film applied between a base material and a pattern forming composition.
  • the composition of the pattern-forming composition and the like are not particularly specified, but preferably contain a polymerizable compound and a photopolymerization initiator.
  • the pattern-forming composition preferably contains a polymerizable compound, and it is more preferable that the polymerizable compound constitutes the maximum amount of the component.
  • the polymerizable compound may have one polymerizable group in one molecule or may have two or more polymerizable groups. At least one of the polymerizable compounds contained in the pattern-forming composition preferably contains 2 to 5 polymerizable groups in one molecule, more preferably 2 to 4, and 2 or 3 polymerizable groups. Is more preferable, and it is more preferable to include three.
  • the polymerizable compound in the pattern-forming composition preferably has the same type of polymerizable group as the polymerizable group contained in the polymer compound in the underlayer film-forming composition. As a result, the crosslinkable monomer can be bonded to the polymerizable compound in the pattern-forming composition, and the effect of further improving the adhesion at the interface can be obtained by the bond across the interface between the compositions.
  • At least one of the polymerizable compounds contained in the pattern-forming composition has a cyclic structure.
  • this cyclic structure include an aliphatic hydrocarbon ring Cf and an aromatic hydrocarbon ring Cr.
  • the polymerizable compound preferably has an aromatic hydrocarbon ring Cr, and more preferably has a benzene ring.
  • the molecular weight of the polymerizable compound is preferably 100 to 900.
  • At least one of the above polymerizable compounds is preferably represented by the following formula (I-1).
  • L 20 is a 1 + q2 valent linking group, and examples thereof include a cyclic structure linking group.
  • the cyclic structure include ring Cf, ring Cr, ring Cn, ring Co, and ring Cs.
  • R 21 and R 22 independently represent a hydrogen atom or a methyl group, respectively.
  • L 21 and L 22 independently represent a single bond or the linking group L, respectively.
  • L 20 and L 21 or L 22 may be combined with or without the linking group L to form a ring.
  • L 20 , L 21 and L 22 may have the above-mentioned substituent T.
  • a plurality of substituents T may be bonded to form a ring. When there are a plurality of substituents T, they may be the same or different from each other.
  • q2 is an integer of 0 to 5, preferably an integer of 0 to 3, more preferably an integer of 0 to 2, and even more preferably 0 or 1.
  • Examples of the polymerizable compound include the compounds used in the following examples, paragraphs 0017 to 0024 of JP2014-090133A and the compounds described in Examples, and paragraphs 0024 to 0089 of JP2015-009171.
  • Examples of the compound, the compound described in paragraphs 0023 to 0037 of JP2015-070145A, and the compound described in paragraphs 0012 to 0039 of International Publication No. 2016/152597 can be mentioned, but the present invention is limited thereto. It is not interpreted.
  • the polymerizable compound is preferably contained in the pattern-forming composition in an amount of 30% by mass or more, more preferably 45% by mass or more, further preferably 50% by mass or more, further preferably 55% by mass or more, and 60% by mass or more. It may be 70% by mass or more. Further, the upper limit value is preferably less than 99% by mass, more preferably 98% by mass or less, and may be 97% by mass or less.
  • the boiling point of the polymerizable compound is set and designed in relation to the polymer compound contained in the above-mentioned composition for forming an underlayer film.
  • the boiling point of the polymerizable compound is preferably 500 ° C. or lower, more preferably 450 ° C. or lower, and even more preferably 400 ° C. or lower.
  • the lower limit value is preferably 200 ° C. or higher, more preferably 220 ° C. or higher, and even more preferably 240 ° C. or higher.
  • the pattern-forming composition may contain additives other than the polymerizable compound.
  • additives may include a polymerization initiator, a solvent, a surfactant, a sensitizer, a mold release agent, an antioxidant, a polymerization inhibitor and the like.
  • the content of the solvent in the pattern-forming composition is preferably 5% by mass or less, more preferably 3% by mass or less, and 1% by mass or less. Is even more preferable.
  • the pattern-forming composition may also be in a manner substantially free of a polymer (preferably having a weight average molecular weight of more than 1000, more preferably having a weight average molecular weight of more than 2000).
  • substantially free of polymer means, for example, that the content of the polymer is 0.01% by mass or less of the pattern-forming composition, preferably 0.005% by mass or less, and more preferably not contained at all. preferable.
  • the compositions described in the above are exemplified, and these contents are incorporated in the present specification. Further, the description of the above-mentioned publication can be referred to with respect to the preparation of the composition for pattern formation and the method for producing the pattern, and these contents are incorporated in the present specification.
  • the viscosity of the pattern-forming composition is preferably 20.0 mPa ⁇ s or less, more preferably 15.0 mPa ⁇ s or less, further preferably 11.0 mPa ⁇ s or less, and 9.0 mPa ⁇ s or less. -It is more preferable that it is s or less.
  • the lower limit of the viscosity is not particularly limited, but can be, for example, 5.0 mPa ⁇ s or more. Viscosity is measured according to the method below.
  • the viscosity is measured by adjusting the temperature of the sample cup to 23 ° C. using an E-type rotational viscometer RE85L manufactured by Toki Sangyo Co., Ltd. and a standard cone rotor (1 ° 34'x R24). The unit is mPa ⁇ s. Other details regarding the measurement are in accordance with JISZ8803: 2011. Two samples are prepared for each level and measured three times each. The arithmetic mean value of a total of 6 times is adopted as the evaluation value.
  • the surface tension ( ⁇ Resist) of the pattern-forming composition is preferably 28.0 mN / m or more, more preferably 30.0 mN / m or more, and may be 32.0 mN / m or more.
  • the upper limit of the surface tension is not particularly limited, but is preferably 40.0 mN / m or less, preferably 38.0 mN / m, from the viewpoint of imparting the relationship with the underlying film and inkjet suitability. It is more preferably 36.0 mN / m or less, and may be 36.0 mN / m or less.
  • the surface tension of the pattern-forming composition is measured according to the same method as that for the alkylene glycol compound described above.
  • the Onishi parameter of the pattern-forming composition is preferably 5.0 or less, more preferably 4.0 or less, and even more preferably 3.7 or less.
  • the lower limit of the Onishi parameter of the pattern-forming composition is not particularly defined, but may be, for example, 1.0 or more, and further may be 2.0 or more.
  • the storage container for the underlayer film forming composition and the pattern forming composition used in the present invention.
  • the inner wall of the container is made of a multi-layer bottle composed of 6 kinds of 6 layers of resin, and 6 kinds of resins are made into a 7 layer structure. It is also preferable to use a bottle of resin. Examples of such a container include the container described in Japanese Patent Application Laid-Open No. 2015-123351.
  • the imprint kit includes a combination of the above-mentioned pattern-forming composition for forming a pattern (pattern-transferred cured film) by the imprint method and a lower-layer film-forming composition for forming a lower-layer film. ..
  • the pattern-forming composition and the underlayer film-forming composition are each housed in a separate container and combined.
  • the method for producing a pattern of the present invention is a pattern-forming composition is applied on an underlayer film obtained by the above-mentioned method for producing a laminate, and the pattern-forming composition is cured in a state where the mold is in contact with the pattern. Includes peeling the mold from the forming composition.
  • the method for producing a pattern (pattern-transferred cured film) according to a preferred embodiment of the present invention is a method for producing a pattern (pattern-transferred cured film) on the surface of a base material (hereinafter, also simply referred to as “substrate”).
  • a step of forming a lower layer film using the forming composition (lower layer film forming step), a pattern forming composition is applied on the lower layer film (preferably the surface of the lower layer film) to form a pattern forming composition layer.
  • a step of forming (pattern forming composition layer forming step), a mold contacting step of bringing the mold into contact with the pattern forming composition layer, and light irradiation for exposing the pattern forming composition layer with the mold in contact.
  • the step includes a step of peeling the mold from the exposed pattern-forming composition layer.
  • the lower layer film 2 is formed on the surface of the substrate 1.
  • the lower layer film is preferably formed by applying the lower layer film forming composition on the substrate in a layered manner.
  • the method of applying the composition for forming an underlayer film to the surface of the substrate is not particularly specified, and a generally well-known application method can be adopted.
  • a dip coating method for example, a dip coating method, an air knife coating method, a curtain coating method, a wire bar coating method, a gravure coating method, an extrusion coating method, a spin coating method, a slit scan method, or an inkjet method. Is exemplified, and the spin coating method is preferable.
  • the solvent is volatilized (dried) by heat to form an underlayer film which is a thin film.
  • the thickness of the underlayer film 2 is preferably 2 nm or more, more preferably 3 nm or more, and further preferably 4 nm or more.
  • the thickness of the underlayer film is preferably 20 nm or less, more preferably 10 nm or less, and further preferably 7 nm or less.
  • composition layer forming step for pattern formation >> In this step, for example, as shown in FIG. 1 (3), the pattern forming composition 3 is applied to the surface of the underlayer film 2.
  • the method of applying the pattern-forming composition is not particularly specified, and the description in paragraph 0102 of JP-A-2010-109092 (the publication number of the corresponding US application is US2011 / 183127) can be referred to. Incorporated into the specification.
  • the pattern-forming composition is preferably applied to the surface of the underlayer film by an inkjet method. Further, the pattern-forming composition may be applied by multiple coating.
  • the amount of the droplets is preferably about 1 to 20 pL, and it is preferable to arrange the droplets on the surface of the lower layer film at intervals.
  • the droplet spacing is preferably 10 to 1000 ⁇ m. In the case of the inkjet method, the droplet interval is the arrangement interval of the inkjet nozzles.
  • the volume ratio of the lower layer film 2 and the film-like pattern forming composition 3 applied on the lower layer film is preferably 1: 1 to 500, more preferably 1:10 to 300. It is more preferably 1:50 to 200.
  • the method for producing the laminate is a method for producing the laminate using the above kit, and includes applying the pattern forming composition to the surface of the underlayer film formed from the underlayer film forming composition. Good. Further, the method for producing the laminate includes a step of applying the underlayer film forming composition on the substrate in a layered manner, and the underlayer film forming composition applied in the layered form is preferably applied at 100 to 300 ° C. It is preferable to include heating (baking) at 130 to 260 ° C., more preferably 150 to 230 ° C. The heating time is preferably 30 seconds to 5 minutes.
  • a liquid film may be formed on the substrate.
  • the formation of the liquid film may be performed by a conventional method. For example, it may be formed by applying a composition containing a crosslinkable monomer that is liquid at 23 ° C. (for example, a polymerizable compound) onto a substrate.
  • Mold contact process For example, as shown in FIG. 1 (4), the pattern forming composition 3 and the mold 4 having a pattern for transferring the pattern shape are brought into contact with each other. By going through such a process, a desired pattern (imprint pattern) can be obtained.
  • the mold 4 is pressed against the surface of the film-shaped pattern-forming composition 3.
  • the mold may be a light-transmitting mold or a light-impermeable mold.
  • a light-transmitting mold it is preferable to irradiate the pattern-forming composition 3 with light from the mold side.
  • the mold that can be used in the present invention is a mold having a pattern to be transferred.
  • the pattern possessed by the mold can be formed according to a desired processing accuracy by, for example, photolithography or an electron beam drawing method, but in the present invention, the method for forming the mold pattern is not particularly limited. Further, the pattern formed by the method for producing a pattern according to a preferred embodiment of the present invention can also be used as a mold.
  • the material constituting the light-transmitting mold used in the present invention is not particularly limited, but is limited to glass, quartz, polymethylmethacrylate (PMMA), light-transmitting resin such as polycarbonate resin, transparent metal vapor-deposited film, polydimethylsiloxane, and the like.
  • PMMA polymethylmethacrylate
  • a flexible film, a photocurable film, a metal film and the like are exemplified, and quartz is preferable.
  • the non-light-transmitting mold material used when the light-transmitting substrate is used in the present invention is not particularly limited, but may be any material having a predetermined strength. Specific examples include ceramic materials, vapor-deposited films, magnetic films, reflective films, metal substrates such as Ni, Cu, Cr, and Fe, and substrates such as SiC, silicon, silicon nitride, polysilicon, silicon oxide, and amorphous silicon. It is not particularly restricted.
  • the mold pressure is preferably 10 atm or less.
  • the mold pressure is preferably selected from a range in which the uniformity of mold transfer can be ensured while the residual film of the pattern forming composition corresponding to the convex portion of the mold is reduced. It is also preferable that the pattern-forming composition and the mold are brought into contact with each other in an atmosphere containing helium gas or condensable gas, or both helium gas and condensable gas.
  • the pattern-forming composition is exposed to light by irradiating it with light to form a cured product.
  • the irradiation amount of light irradiation in the light irradiation step may be sufficiently larger than the minimum irradiation amount required for curing.
  • the irradiation amount required for curing is appropriately determined by examining the consumption amount of unsaturated bonds of the pattern-forming composition.
  • the type of light to be irradiated is not particularly specified, but ultraviolet light is exemplified.
  • the substrate temperature at the time of light irradiation is usually room temperature, but light irradiation may be performed while heating in order to enhance the reactivity.
  • a vacuum state is used as a pre-stage of light irradiation, it is effective in preventing air bubbles from being mixed in, suppressing a decrease in reactivity due to oxygen mixing, and improving the adhesion between the mold and the pattern-forming composition. Therefore, light irradiation is performed in a vacuum state. You may.
  • the preferable degree of vacuum at the time of light irradiation is in the range of 10 -1 Pa to normal pressure.
  • the exposure illuminance is preferably in the range of 1 to 500 mW / cm 2 , and more preferably in the range of 10 to 400 mW / cm 2.
  • the exposure time is not particularly limited, but is preferably 0.01 to 10 seconds, more preferably 0.5 to 1 second.
  • Exposure amount is preferably in a range of 5 ⁇ 1000mJ / cm 2, and more preferably in the range of 10 ⁇ 500mJ / cm 2.
  • the film-shaped pattern-forming composition (pattern-forming composition layer) is cured by light irradiation, and then, if necessary, heat is applied to the cured pattern to further cure the cured pattern.
  • the process may be included.
  • the temperature for heat-curing the pattern-forming composition after light irradiation is preferably 150 to 280 ° C, more preferably 200 to 250 ° C.
  • the time for applying heat is preferably 5 to 60 minutes, more preferably 15 to 45 minutes.
  • the composition for forming a lower layer film of the present invention When the composition for forming a lower layer film of the present invention is used, the polymerizable group contained in the polymer compound in the lower layer film and the crosslinkable group contained in the crosslinkable monomer due to the above-mentioned light irradiation and heating. Cross-linking reaction is promoted. In addition, some of the crosslinkable groups of the crosslinkable monomer may also undergo a crosslink reaction with the polymerizable compound in the pattern-forming composition on the underlayer film, and the present invention is said to improve the film strength of the underlayer film. In addition to the effect, it is also possible to obtain the effect that the adhesion at the interface is further improved by the bond across the interface between the compositions.
  • the substrate temperature at the time of light irradiation is usually room temperature, but light irradiation may be performed while heating in order to enhance reactivity. If a vacuum state is used as a pre-stage of light irradiation, it is effective in preventing air bubbles from being mixed in, suppressing a decrease in reactivity due to oxygen mixing, and improving the adhesion between the mold and the pattern-forming composition. Therefore, light irradiation is performed in a vacuum state. You may. Further, in the method for producing the above pattern, the preferable degree of vacuum at the time of light irradiation is in the range of 10 -1 Pa to normal pressure.
  • the present invention discloses a laminate having a pattern formed from the pattern-forming composition on the surface of the underlayer film.
  • the film thickness of the pattern-forming composition layer made of the pattern-forming composition used in the present invention varies depending on the intended use, but is about 0.01 ⁇ m to 30 ⁇ m. Further, as will be described later, etching or the like can also be performed.
  • the pattern formed by the above pattern manufacturing method can be used as a permanent film used in a liquid crystal display (LCD) or the like, or as an etching resist (lithography mask) for manufacturing a semiconductor element.
  • the present specification discloses a method for manufacturing a semiconductor device, which manufactures the semiconductor device using the pattern according to the preferred embodiment of the present invention.
  • a step of etching or ion-implanting a substrate using the pattern obtained by the above pattern manufacturing method as a mask and a step of forming an electronic member are performed. You may have.
  • the semiconductor element is preferably a semiconductor element.
  • this specification discloses a method for manufacturing a semiconductor device including the above-mentioned pattern manufacturing method. Further, the present specification discloses a manufacturing method of an electronic device having a step of obtaining a semiconductor element by the method of manufacturing the semiconductor element and a step of connecting the semiconductor element and a control mechanism for controlling the semiconductor element. ..
  • a grid pattern is formed on the glass substrate of the liquid crystal display device by using the pattern formed by the above pattern manufacturing method, and the reflection and absorption are small, and the large screen size (for example, 55 inches, 60 inches, (1 inch)). It is possible to inexpensively manufacture a polarizing plate of (2.54 cm))).
  • the polarizing plates described in JP-A-2015-132825 and International Publication No. 2011/132649 can be manufactured.
  • the pattern formed in the present invention is also useful as an etching resist (mask for lithography).
  • a fine pattern on the order of nano or micron is formed on the substrate by the method for producing the pattern.
  • the present invention is particularly advantageous in that a nano-order fine pattern can be formed, and a pattern having a size of 50 nm or less, particularly 30 nm or less can be formed.
  • the lower limit of the size of the pattern formed by the above pattern manufacturing method is not particularly specified, but can be, for example, 1 nm or more.
  • the pattern manufacturing method of the present invention can also be applied to a manufacturing method of an imprint mold.
  • the method for manufacturing the imprint mold includes, for example, a step of manufacturing a pattern on a substrate (for example, a substrate made of a transparent material such as quartz) which is a material of the mold by the above-mentioned pattern manufacturing method, and this pattern. It has a step of etching the substrate using the above-mentioned substrate.
  • a desired pattern is formed on the substrate by etching with an etching solution such as hydrogen fluoride when wet etching is used as the etching method and an etching gas such as CF 4 when dry etching is used. be able to.
  • the pattern has particularly good etching resistance to dry etching. That is, the pattern formed by the above pattern manufacturing method is preferably used as a mask for lithography.
  • the pattern formed in the present invention includes a recording medium such as a magnetic disk, a light receiving element such as a solid-state imaging element, a light emitting element such as an LED (light emission diode) or an organic EL (organic electroluminescence), and a liquid crystal display.
  • a recording medium such as a magnetic disk
  • a light receiving element such as a solid-state imaging element
  • a light emitting element such as an LED (light emission diode) or an organic EL (organic electroluminescence)
  • a liquid crystal display such as a liquid crystal display.
  • Optical devices such as liquid crystals (LCDs), diffraction grids, relief holograms, optical waveguides, optical filters, optical components such as microlens arrays, thin film transistors, organic transistors, color filters, antireflection films, polarizing plates, polarizing elements, optical films, Flat panel display members such as pillars, nanobiodevices, immunoanalytical chips, deoxyribonucleic acid (DNA) separation chips, microreactors, photonic liquid crystals, and fine pattern formation (directed self-assembury) using self-assembly of block copolymers, It can be preferably used for producing a guide pattern or the like for DSA).
  • composition for forming underlayer film Each material was blended and mixed at the blending ratios (parts by mass) shown in Tables 1 to 5 below, and the mixture was thoroughly stirred. After stirring, this was filtered through a nylon filter having a pore size of 0.02 ⁇ m and an ultra-high molecular weight polyethylene (UPE) filter having a pore size of 0.001 ⁇ m to prepare a composition for forming an underlayer film shown in Examples and Comparative Examples.
  • UPE ultra-high molecular weight polyethylene
  • Mw 20,000. -Pb-5: A compound having the following structure.
  • Mw 20,000. -Pb-6: A compound having the following structure.
  • Mw 20,000. -Pb-7: A compound having the following structure.
  • Mw 20,000. -Pc-1: A compound having the following structure.
  • Mw 20,000. -Pc-2: A compound having the following structure.
  • Mw 20,000. -Pc-3: A compound having the following structure.
  • Mw 20,000.
  • Ad-1 A polymerizable compound having the following structure.
  • -Ad-2 A compound having the following structure.
  • -Ad-3 A polymerization initiator having the following structure.
  • -Ad-4 A polymerization initiator having the following structure.
  • -Ad-5 A polymerization initiator having the following structure.
  • -Ad-6 A polymerization initiator having the following structure.
  • -Ad-7 A polymerization initiator having the following structure.
  • -Ad-8 A polymerization inhibitor having the following structure.
  • -Ad-9 A polymerization inhibitor having the following structure.
  • composition for pattern formation The compounds shown in Table 9 below are blended in the blending ratio (parts by mass) shown in the table below, and 4-hydroxy-2,2,6,6-tetramethylpiperidin-1-oxylfree radical (Tokyo) is further blended as a polymerization inhibitor.
  • a product manufactured by Kasei Co., Ltd. was added so as to be 200 mass ppm (0.02 mass%) with respect to the total amount of the polymerizable compounds (Nos. 1 to 3 in the table). This was filtered through a nylon filter having a pore size of 0.02 ⁇ m and an UPE filter having a pore size of 0.001 ⁇ m to prepare patterns V-1 and V-2 for pattern formation.
  • k + m + n 10.
  • underlayer film forming compositions of each Example and Comparative Example were spin-coated on a silicon wafer having a contact angle with water of 50 ° or more, and a hot plate was used under the temperature conditions shown in Tables 1 to 5 above. It was heated to form an underlayer film on a silicon wafer.
  • the film thickness of the underlayer was measured by an ellipsometer and an atomic force microscope.
  • the surface roughness Ra (arithmetic mean roughness. JIS B 0601-2001) of the surface of the underlayer film was measured using an atomic force microscope (AFM-ICON, manufactured by Bruker) and evaluated according to the following criteria. The measurement area was 10 ⁇ m square and the measurement frequency was 0.5 Hz. It can be said that the smaller the surface roughness of the lower layer film, the less likely it is that the composition for forming the lower layer film will be in a sea-island state on the substrate.
  • the evaluation of A to C is a level suitable for practical use.
  • a pattern-forming composition V-1 or V-2 whose temperature has been adjusted to 23 ° C. is discharged onto the surface of the underlayer film at a droplet amount of 6 pL per nozzle using an inkjet printer DMP-2831 manufactured by Fujifilm Dimatics. Then, the droplets were applied on the lower film so as to form a square arrangement at intervals of about 100 ⁇ m to form a pattern forming layer. Next, under a He atmosphere (substitution rate of 90% by volume or more), a quartz wafer spin-coated with the composition for forming an adhesion layer shown in Example 6 of JP2014-024322A was pressed against the pattern forming layer.
  • a pattern-forming composition V-1 whose temperature was adjusted to 23 ° C. was discharged onto the surface of the lower layer film using an inkjet printer DMP-2831 manufactured by Fujifilm Dimatics at a droplet amount of 1 pL per nozzle to form the lower layer film. Above, the droplets were applied in a square arrangement at intervals of about 100 ⁇ m. Next, a quartz substrate having a flat surface was pressed against the pattern-forming composition to flatten the pattern-forming composition. Then, the quartz substrate was exposed from the quartz substrate side using a high-pressure mercury lamp under the condition of 300 mJ / cm 2 , and then the quartz substrate was peeled off to obtain a flat film of the pattern-forming composition.
  • A is a level suitable for practical use.
  • -A In the imprint area, an unfilled region (a region in which a cured product of the pattern forming composition does not exist) was not generated.
  • -B An unfilled area was confirmed in a part of the imprint area.
  • a lower layer film is formed on a silicon wafer using the lower layer film forming composition according to each example, and a semiconductor is used on the silicon wafer with the lower layer film using the pattern forming composition according to each example.
  • a predetermined pattern corresponding to the circuit was formed. Then, using this pattern as an etching mask, each silicon wafer was dry-etched, and each of the semiconductor elements was manufactured using the silicon wafer. There was no problem in performance of any of the semiconductor elements.
  • using the underlayer film forming composition and the pattern forming composition of Example 1 a semiconductor device was produced on the SOC substrate by the same procedure as described above. There was no problem in performance of this semiconductor element as well.

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Abstract

L'invention concerne une composition qui est destinée à former une pellicule de sous-couche et comprend un composé polymère A ayant un groupe fonctionnel polymérisable, un composé polymère B ayant un groupe fonctionnel polymérisable, et un solvant. Le composé polymère A a un pourcentage de teneur en cycle Rca, représentant le nombre de moles de cycles par unité de masse, d'au plus 0,0010 mol/g et le composé polymère B a un pourcentage de teneur en cycle Rcb, représentant le nombre de moles de cycles par unité de masse, d'au plus 0,0015 mol/g ; et lorsque l'une parmi la teneur du composé polymère A et la teneur du composé polymère B dans la composition pour former une pellicule de sous-couche est de 100 parties en masse, l'autre est de 1 à 30 parties en masse. L'invention concerne également : un stratifié dans lequel la composition pour former une pellicule de sous-couche est utilisée ; un procédé de production d'un motif ; et un procédé de production d'un dispositif à semi-conducteur.
PCT/JP2020/035814 2019-09-27 2020-09-23 Composition de formation de pellicule de sous-couche, stratifié, procédé de production de motif et procédé de production de dispositif à semi-conducteur WO2021060283A1 (fr)

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2013093552A (ja) * 2011-10-07 2013-05-16 Fujifilm Corp インプリント用下層膜組成物およびこれを用いたパターン形成方法
WO2016031879A1 (fr) * 2014-08-27 2016-03-03 富士フイルム株式会社 Composition de résine formant sous-couche, stratifié, procédé de formation de motif, trousse de formation d'empreinte et procédé de fabrication de dispositif
WO2018190337A1 (fr) * 2017-04-11 2018-10-18 富士フイルム株式会社 Composition, film adhérant étroitement, stratifié, procédé de production d'un motif de produit durci, et procédé de production de carte de circuit imprimé

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2013093552A (ja) * 2011-10-07 2013-05-16 Fujifilm Corp インプリント用下層膜組成物およびこれを用いたパターン形成方法
WO2016031879A1 (fr) * 2014-08-27 2016-03-03 富士フイルム株式会社 Composition de résine formant sous-couche, stratifié, procédé de formation de motif, trousse de formation d'empreinte et procédé de fabrication de dispositif
WO2018190337A1 (fr) * 2017-04-11 2018-10-18 富士フイルム株式会社 Composition, film adhérant étroitement, stratifié, procédé de production d'un motif de produit durci, et procédé de production de carte de circuit imprimé

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