WO2010055601A1 - ブロックコポリマーの自己組織化促進方法及びそれを用いたブロックコポリマーの自己組織化パターン形成方法 - Google Patents

ブロックコポリマーの自己組織化促進方法及びそれを用いたブロックコポリマーの自己組織化パターン形成方法 Download PDF

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WO2010055601A1
WO2010055601A1 PCT/JP2009/004217 JP2009004217W WO2010055601A1 WO 2010055601 A1 WO2010055601 A1 WO 2010055601A1 JP 2009004217 W JP2009004217 W JP 2009004217W WO 2010055601 A1 WO2010055601 A1 WO 2010055601A1
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block copolymer
self
film
pattern
forming
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Ceased
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English (en)
French (fr)
Japanese (ja)
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遠藤政孝
笹子勝
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Panasonic Corp
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Panasonic Corp
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B81—MICROSTRUCTURAL TECHNOLOGY
    • B81C—PROCESSES OR APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OR TREATMENT OF MICROSTRUCTURAL DEVICES OR SYSTEMS
    • B81C1/00—Manufacture or treatment of devices or systems in or on a substrate
    • B81C1/00015—Manufacture or treatment of devices or systems in or on a substrate for manufacturing microsystems
    • B81C1/00023—Manufacture or treatment of devices or systems in or on a substrate for manufacturing microsystems without movable or flexible elements
    • B81C1/00031—Regular or irregular arrays of nanoscale structures, e.g. etch mask layer
    • 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
    • B29C71/00—After-treatment of articles without altering their shape; Apparatus therefor
    • B29C71/02—Thermal after-treatment
    • G—PHYSICS
    • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03F—PHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00—Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/0002—Lithographic processes using patterning methods other than those involving the exposure to radiation, e.g. by stamping
    • 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
    • B29C71/00—After-treatment of articles without altering their shape; Apparatus therefor
    • B29C71/02—Thermal after-treatment
    • B29C2071/022—Annealing
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29K—INDEXING SCHEME ASSOCIATED WITH SUBCLASSES B29B, B29C OR B29D, RELATING TO MOULDING MATERIALS OR TO MATERIALS FOR MOULDS, REINFORCEMENTS, FILLERS OR PREFORMED PARTS, e.g. INSERTS
    • B29K2995/00—Properties of moulding materials, reinforcements, fillers, preformed parts or moulds
    • B29K2995/0037—Other properties
    • B29K2995/0093—Other properties hydrophobic

Definitions

  • the present invention relates to a method for promoting self-organization of a block copolymer used for pattern formation such as a manufacturing process of a semiconductor device and a method for forming a self-organized pattern of a block copolymer using the same.
  • Patent Document 1 a method of forming a pattern from the bottom up rather than from the bottom down has been proposed (see, for example, Patent Document 1). Specifically, an ultrafine pattern by self-organization using a block copolymer obtained by copolymerizing a polymer chain having one property with a monomer unit and another polymer chain (monomer unit) having different properties. It is a forming method. According to this method, by annealing the block copolymer film, the monomer units having different properties repel each other and the monomer units having the same properties are patterned in a self-aligned manner (directed self-assembly). ).
  • a block copolymer film 2 having the following composition and a film thickness of 0.07 ⁇ m is formed on a substrate 1.
  • the formed block copolymer film 2 is annealed in an oven at a temperature of 180 ° C. for 24 hours, and the line width shown in FIG. 7C is 16 nm.
  • the first pattern 2a and the second pattern 2b having a self-assembled lamellar structure (layer structure) are obtained.
  • the block copolymer film 2 is formed inside the guide pattern, but the guide pattern is omitted here.
  • the present invention has been made in view of the above-described conventional problems, and an object thereof is to improve the throughput of pattern formation by self-organization of a block copolymer.
  • the present inventors have conducted the following method during annealing of one of the monomer units constituting the block copolymer, for example, a hydrophilic or hydrophobic monomer unit. Has gained the knowledge that it is easier to self-assemble.
  • the outside (mainly upward) of the block copolymer film becomes non-polar, so that, for example, a monomer unit having hydrophobicity (hydrophobic unit) is formed in the film. Because it is strongly attracted to the outside, self-organization is promoted.
  • the block copolymer film when the block copolymer film is annealed under humidification, the outside of the block copolymer film (mainly upward) becomes hydrophilic.
  • a hydrophilic monomer unit hydrophilic unit
  • a method of applying humidification a method of introducing water vapor into the oven can be mentioned.
  • a water-soluble polymer film is formed on the block copolymer film
  • a water-soluble polymer is formed on the upper surface of the block copolymer film.
  • hydrophilic monomer units are strongly attracted to the outside (upper) of the film. So self-organization is promoted.
  • An exposure method in which a water-soluble polymer film is formed on a resist film and exposed is conventionally known, but the present invention is different from the conventional method in that a pattern can be formed without exposure.
  • the water-soluble polymer film is removed by water or the like after annealing, but when cured by annealing, it can be removed by ashing of oxygen-based plasma.
  • Annealing of the block copolymer film according to the present invention may be performed, for example, in an oven at a temperature of about 150 ° C. or higher. According to the present invention, the annealing time can be greatly shortened, for example, about 2 to 6 hours. However, the present invention is not limited to this range.
  • the present invention has been made based on the above findings, and when annealing the block copolymer film, the atmosphere mainly contacting the upper surface of the annealed block copolymer film is made hydrophilic or hydrophobic, or is in contact with the upper surface.
  • the other film is made hydrophilic or hydrophobic, and is specifically realized by the following method.
  • a method for promoting self-assembly of a first block copolymer according to the present invention includes a step of forming a first film made of a block copolymer on a substrate, and a step of annealing the first film in an inert gas atmosphere. It is characterized by having.
  • the method for promoting self-assembly of the first block copolymer since the first film made of the block copolymer is annealed in an inert gas atmosphere, the outside (mainly above) of the first film is in a state of no polarity. Become. Thereby, for example, the monomer unit having hydrophobicity is strongly attracted to the outside of the first film, and thus self-assembly is promoted. Therefore, the throughput of pattern formation by the self-assembly of the block copolymer is improved.
  • helium, neon, argon, krypton, or xenon can be used as the inert gas.
  • the second block copolymer self-assembly promotion method includes a step of forming a first film made of a block copolymer on a substrate, and a step of annealing the first film under humidification. It is characterized by.
  • the first film made of the block copolymer is annealed under humidification, so that the outside (mainly upper) of the first film is in a hydrophilic state. Accordingly, for example, the monomer unit having hydrophilicity is strongly attracted to the outside of the first film, so that self-organization is promoted. Therefore, the throughput of pattern formation by the self-assembly of the block copolymer is improved.
  • the annealing under humidification is preferably performed in a humidified atmosphere having a humidity of 30% or more.
  • the third method for promoting self-assembly of a block copolymer according to the present invention includes a step of forming a first film made of a block copolymer on a substrate, and a second process made of a water-soluble polymer on the first film. And a step of annealing the first film and the second film.
  • the second film made of the water-soluble polymer is formed on the first film made of the block copolymer, the upper surface of the first film is water-soluble. A polymer is formed. For this reason, for example, the monomer unit having hydrophilicity is strongly attracted above the first film, so that self-organization is promoted. Therefore, the throughput of pattern formation by the self-assembly of the block copolymer is improved.
  • polyvinyl alcohol polyvinyl pyrrolidone, polyacrylic acid or polystyrene sulfonic acid can be used as the water-soluble polymer.
  • the film thickness of the second film made of the water-soluble polymer is preferably about 50 nm or less.
  • the block copolymer is preferably composed of a hydrophilic unit and a hydrophobic unit.
  • methacrylate, butadiene, vinyl acetate, acrylate, acrylamide, acrylonitrile, acrylic acid, vinyl alcohol, ethylene glycol or propylene glycol can be used for the hydrophilic unit.
  • styrene, xylene or ethylene can be used for the hydrophobic unit.
  • the copolymerization ratio of the block copolymer containing two types of monomer units is about 50 to 50, the self-assembled pattern has a lamellar structure. As the ratio of any one of the monomer units decreases from this ratio, a cylinder structure and further a dot structure are obtained.
  • a first block copolymer self-assembly pattern forming method includes a step of forming a guide pattern having hydrophilicity or hydrophobicity and an opening on a substrate, and a guide pattern on the substrate.
  • the first film made of the block copolymer is formed in the opening of the guide pattern having hydrophilicity or hydrophobicity and having the opening, and then Since the first film is annealed in the inert gas atmosphere, the self-organization of the first film is promoted as described above. For this reason, it is possible to improve the throughput of the self-assembled pattern made of the block copolymer.
  • helium, neon, argon, krypton, or xenon can be used as the inert gas.
  • the second block copolymer self-organized pattern forming method includes a step of forming a hydrophilic or hydrophobic guide pattern having an opening on a substrate, and a guide pattern on the substrate. Forming a first film made of a block copolymer in the opening of the first film; annealing the first film under humidification to self-assemble the first film; and And a step of forming a self-assembled pattern from one film.
  • the first film made of the block copolymer is formed in the opening of the guide pattern having hydrophilicity or hydrophobicity and having the opening, Since the first film is annealed under humidification, self-organization of the first film is promoted as described above. For this reason, it is possible to improve the throughput of the self-assembled pattern made of the block copolymer.
  • the annealing under humidification is performed in a humidified atmosphere having a humidity of 30% or more.
  • the third method for forming a self-organized pattern of a block copolymer according to the present invention includes a step of forming a hydrophilic or hydrophobic guide pattern having an opening on a substrate, and a guide pattern on the substrate. Forming a first film made of a block copolymer in the opening, a step of forming a second film made of a water-soluble polymer on the first film, a first film and a second film A step of self-organizing the first film by annealing the film; and a step of forming a self-assembled pattern from the first film that has been self-assembled after removing the second film. It is characterized by.
  • the first film made of the block copolymer is formed in the opening of the guide pattern having hydrophilicity or hydrophobicity and having the opening, Since annealing is performed with the second film made of the water-soluble polymer formed on the first film, the second film made of the water-soluble polymer promotes self-organization of the first film as described above. Is done. For this reason, it is possible to improve the throughput of the self-assembled pattern made of the block copolymer.
  • polyvinyl alcohol polyvinyl pyrrolidone
  • polyacrylic acid polystyrene sulfonic acid
  • the block copolymer is preferably composed of a hydrophilic unit and a hydrophobic unit.
  • methacrylate, butadiene, vinyl acetate, acrylate, acrylamide, acrylonitrile, acrylic acid, vinyl alcohol, ethylene glycol or propylene glycol can be used for the hydrophilic unit.
  • styrene, xylene or ethylene can be used for the hydrophobic unit.
  • the self-assembled pattern may be formed by etching the first pattern including the hydrophilic unit or the second pattern including the hydrophobic unit. it can.
  • the block copolymer self-assembly promotion method and the block copolymer self-assembly pattern formation method using the block copolymer according to the present invention can improve the throughput in pattern formation by block copolymer self-assembly.
  • FIG. 1A to FIG. 1D are cross-sectional views showing respective steps of the pattern forming method according to the first embodiment of the present invention.
  • FIG. 2 is a cross-sectional view showing one step of the pattern forming method according to the first embodiment of the present invention.
  • FIG. 3A to FIG. 3D are cross-sectional views showing respective steps of the pattern forming method according to the second embodiment of the present invention.
  • FIG. 4 is a sectional view showing one step of the pattern forming method according to the second embodiment of the present invention.
  • FIG. 5A to FIG. 5D are cross-sectional views showing respective steps of the pattern forming method according to the third embodiment of the present invention.
  • FIG. 6A and FIG. 6B are cross-sectional views showing each step of the pattern forming method according to the third embodiment of the present invention.
  • FIG. 7A to FIG. 7C are cross-sectional views showing respective steps of a conventional pattern forming method using a block copolymer.
  • a solution obtained by dissolving hydrophilic hydrogenated silsesquioxane in methyl isobutyl ketone is spin-coated on a substrate 101, and subsequently the temperature is set to 110 by a hot plate.
  • a hydrogenated silsesquioxane film having a thickness of 40 nm is formed by baking at 60 ° C. for 60 seconds. Thereafter, the formed hydrogenated silsesquioxane film is selectively irradiated with an electron beam exposure having a voltage of 100 kV, and subsequently developed with an aqueous tetramethylammonium hydroxide solution having a concentration of 2.3 wt%.
  • a guide pattern 102 having an opening 102a having a width of 30 nm is formed from the hydrogenated silsesquioxane film.
  • a block copolymer film 103 having the following composition and a thickness of 30 nm is formed in the opening 102a of the guide pattern 102.
  • the block copolymer film 103 is annealed in an oven for about 3 hours at a temperature of 180 ° C. in an atmosphere of neon (Ne) as an inert gas.
  • Ne neon
  • a first pattern 103a and a second pattern 103b having a lamellar structure with a line width of 16 nm and self-organized perpendicularly to the substrate 101 are obtained.
  • the guide pattern 102 is made of hydrogenated silsesquioxane having hydrophilicity
  • the first pattern 103a in contact with the side surface of the guide pattern 102 is mainly composed of polymethylmethacrylate having hydrophilicity
  • the second pattern 103b inside the pattern 103a is mainly composed of polystyrene having hydrophobicity.
  • the first pattern 103a is formed with oxygen-based gas.
  • the second pattern 103b made of polystyrene can be formed by annealing for about 3 hours. Therefore, pattern formation using a block copolymer can be applied to a semiconductor device manufacturing process.
  • neon (Ne) is used as the inert gas, but instead of neon, helium (He), argon (Ar), krypton (Kr), xenon (Xe), or any of these Two or more gas mixtures can be used.
  • a solution in which hydrogenated silsesquioxane having hydrophilicity is dissolved in methyl isobutyl ketone is spin-coated on a substrate 201, and subsequently, the temperature is set to 110 by a hot plate.
  • a hydrogenated silsesquioxane film having a thickness of 40 nm is formed by baking at 60 ° C. for 60 seconds. Thereafter, the formed hydrogenated silsesquioxane film is selectively irradiated with an electron beam exposure having a voltage of 100 kV, and subsequently developed with an aqueous tetramethylammonium hydroxide solution having a concentration of 2.3 wt%.
  • a guide pattern 202 having an opening 202a having a width of 30 nm is formed from the hydrogenated silsesquioxane film.
  • a block copolymer film 203 having the following composition and a thickness of 30 nm is formed in the opening 202a of the guide pattern 202.
  • water vapor is introduced around the block copolymer film 203, the humidity is about 40% relative to the block copolymer film 203, the temperature is set to 190 ° C., and about 2%. Annealing with oven for hours. As a result, as shown in FIG.
  • a first pattern 203a and a second pattern 203b having a lamellar structure with a line width of 16 nm and self-organized perpendicularly to the substrate 201 are obtained.
  • the guide pattern 202 is made of hydrogenated silsesquioxane having hydrophilicity
  • the first pattern 203a in contact with the side surface of the guide pattern 202 is mainly composed of polymethylmethacrylate having hydrophilicity
  • the second pattern 203b inside the pattern 203a is mainly composed of polystyrene having hydrophobicity.
  • the first pattern 203a and the second pattern 203b are etched with an oxygen-based gas, as shown in FIG. 4, the first pattern 203a having a large etching rate is etched, and polystyrene is used.
  • the second pattern 203b can be formed by annealing for about 2 hours. Therefore, pattern formation using a block copolymer can be applied to a semiconductor device manufacturing process.
  • the humidity at the time of annealing is set to about 40%, but the humidity may be 30% or more.
  • FIGS. 5 (a) to 5 (d), FIG. 6 (a) and FIG. 6 (b). a pattern forming method using the block copolymer according to the third embodiment of the present invention will be described with reference to FIGS. 5 (a) to 5 (d), FIG. 6 (a) and FIG. 6 (b). .
  • a solution obtained by dissolving hydrophilic hydrogenated silsesquioxane in methyl isobutyl ketone is spin-coated on a substrate 301, and subsequently the temperature is set to 110 by a hot plate.
  • a hydrogenated silsesquioxane film having a thickness of 40 nm is formed by baking at 60 ° C. for 60 seconds. Thereafter, the formed hydrogenated silsesquioxane film is selectively irradiated with an electron beam exposure having a voltage of 100 kV, and subsequently developed with an aqueous tetramethylammonium hydroxide solution having a concentration of 2.3 wt%.
  • a guide pattern 302 having an opening 302a having a width of 30 nm is formed from the hydrogenated silsesquioxane film.
  • a block copolymer film 303 having the following composition and a thickness of 30 nm is formed in the opening 302a of the guide pattern 302.
  • a water-soluble polymer film 304 made of polyvinyl alcohol having a thickness of 20 nm is formed on the block copolymer film 303.
  • the water-soluble polymer film 304 and the block copolymer film 303 are annealed in an oven at a temperature of 180 ° C. for about 3 hours.
  • the water-soluble polymer film 304 is removed with water or the like, or ashed with an oxygen-based gas, and self-organized perpendicularly to the substrate 301 as shown in FIG.
  • a first pattern 303a and a second pattern 303b having a structure are obtained.
  • the guide pattern 302 is made of hydrogenated silsesquioxane having hydrophilicity
  • the first pattern 303a in contact with the side surface of the guide pattern 302 is mainly composed of polymethylmethacrylate having hydrophilicity
  • the second pattern 303b inside the pattern 303a has hydrophobic polystyrene as a main component.
  • the first pattern 303a and the second pattern 303b are etched with an oxygen-based gas, as shown in FIG. 6B, the first pattern 303a having a high etching rate is etched.
  • the second pattern 303b made of polystyrene can be formed by annealing for about 3 hours. Therefore, pattern formation using a block copolymer can be applied to a semiconductor device manufacturing process.
  • polyvinyl alcohol is used for the water-soluble polymer film 304, but polyvinyl pyrrolidone, polyacrylic acid, or polystyrene sulfonic acid can be used instead.
  • the water-soluble polymer film 304 is also formed on the guide pattern 302.
  • the guide pattern 302 It may be formed only on the block copolymer film 303 without covering the top of 302.
  • methacrylate is used as the hydrophilic unit constituting the block copolymer film and styrene is used as the hydrophobic unit.
  • the present invention is not limited to this.
  • butadiene, vinyl acetate, acrylate, acrylamide, acrylonitrile, acrylic acid, vinyl alcohol, ethylene glycol or propylene glycol can be used for the hydrophilic unit instead of methacrylate, and styrene is used for the hydrophobic unit.
  • xylene or ethylene can be used.
  • the monomer constituting the monomer unit does not have to be a single monomer, and a polymer chain obtained by mixing a plurality of monomers may be used as the monomer unit.
  • silsesquioxane hydride is used as a material constituting the guide pattern, tetraalkoxysilane or the like can be used instead.
  • a lamellar structure in a direction perpendicular to the substrate is formed by a hydrophilic guide pattern. Therefore, the inert gas atmosphere at the time of annealing in the first embodiment, the humidified atmosphere at the time of annealing in the second embodiment, and the use of the water-soluble polymer film in the third embodiment has a lamella structure perpendicular to the substrate. It is limited to the extent to promote and does not impair the lamellar structure.
  • the block copolymer self-assembly promotion method and the block copolymer self-assembly pattern formation method using the block copolymer self-assembly pattern formation method according to the present invention can improve the throughput in pattern formation by block copolymer self-assembly, and manufacture a semiconductor device. This is useful for forming a fine pattern in a process.

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PCT/JP2009/004217 2008-11-12 2009-08-28 ブロックコポリマーの自己組織化促進方法及びそれを用いたブロックコポリマーの自己組織化パターン形成方法 Ceased WO2010055601A1 (ja)

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JP2013227479A (ja) * 2011-09-15 2013-11-07 Wisconsin Alumni Research Foundation 化学的にパターン化された表面と第２の表面との間でのブロック共重合体薄膜の誘導集合
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JP6089298B2 (ja) * 2012-04-10 2017-03-08 裕司 清野 パターン形成方法、スチレン系ポリマー薄膜付き基材、表面撥水性材料、パスワード生成装置、培養器、パターン形成剤、及び反転パターン形成方法。
JP5752655B2 (ja) * 2012-09-10 2015-07-22 株式会社東芝 パターン形成方法
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