JP2018060878A - Manufacturing method of pattern structure and manufacturing method of mold for imprint - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a manufacturing method of pattern structure capable of forming a pattern structure on a transfer substrate with high precision, and to provide a manufacturing method of a mold for imprint using this manufacturing method of pattern structure.SOLUTION: A manufacturing method of pattern structure uses a transfer substrate 21 having unit imprint regions 23A, 23B on one face, and having a recess 27 of wider plan view area than that of the unit imprint region on the opposite side so as to include the unit imprint regions. In a contact process, the area of the transfer substrate 21 where the recess 27 of the transfer substrate 21 exists is bent to the mold 11 side in convex, and the normal in the center of the unit imprint region was matched to the normal in the center of the irregular structure region 16 of the mold 11, thus bringing the mold and the transfer substrate close to each other.SELECTED DRAWING: Figure 5

Description

  The present invention relates to a pattern structure manufacturing method for forming a pattern structure on a transfer substrate by imprinting, and an imprint mold manufacturing method using the pattern structure manufacturing method.

  In recent years, a pattern forming technique using an imprint method has attracted attention as a fine pattern forming technique that replaces the photolithography technique. The imprint method is a pattern forming technique in which a fine structure is transferred at an equal magnification by using a mold member (mold) having a fine concavo-convex structure and transferring the concavo-convex structure to a molding resin layer. For example, in an imprint method using a photocurable resin composition as a molding resin composition, a mold having a desired concavo-convex structure and a transfer substrate by supplying droplets of the photocurable resin composition to the surface of the transfer substrate The photo-curable resin composition is filled in the concavo-convex structure with a distance close to a predetermined distance, and in this state, the photo-curable resin composition is cured by irradiating light from the mold side. A pattern structure having a concavo-convex structure (concavo-convex pattern) in which the concavo-convex provided in the mold is inverted is formed.

  In such an imprint method, when the mold and the transfer substrate are brought close to a predetermined distance and the photocurable resin composition is filled in the concavo-convex structure of the mold, pattern defects may occur due to residual bubbles. . In order to prevent such bubbles from remaining, the mold and the transfer substrate are bonded with the transfer substrate convexly curved toward the mold side and / or with the mold curved convexly toward the transfer substrate side. Closely contact with the photocurable resin composition at the center of the uneven structure area of the mold and the center of the imprint area of the transfer substrate, and then gradually contact the outer peripheral side of the uneven structure area to form the photocurable resin. Elimination of bubbles with filling of the composition is performed (for example, Patent Document 1).

Special table 2011-512019 gazette

  However, in the case where the mold and the transfer substrate are brought close to each other in a state where the transfer substrate is convexly curved toward the mold side, the portion of the imprint area where the transfer substrate is curved and is most convex toward the mold side When the center does not match, for example, when an imprint region exists on the inclined surface of the curved transfer substrate, there are the following problems. That is, the position where the droplet of the photocurable resin composition supplied to the imprint area of the transfer substrate and the mold first come out of the center of the imprint area. For this reason, the development of the photocurable resin composition in the imprint region becomes non-uniform, and the amount of protrusion of the photocurable resin composition at the end of the imprint region near the position where the droplet and the mold first contact each other There is a risk that unfilling of the photocurable resin composition may occur at the end portion on the opposite side of the imprint region. In addition, the uniformity of the thickness distribution of the remaining film (film portion formed in the gap between the mold and the transfer substrate) in the formed pattern structure may be impaired.

Further, when the imprint is performed a plurality of times to form a pattern with multiple surfaces on the transfer substrate, the imprint region is inevitably present on the inclined surface of the curved transfer substrate, and the above-described problem occurs. For example, in the case of producing a replica mold having multiple concavo-convex structure regions by imprinting using a master mold, as a transfer substrate for the replica mold, a recess is formed on the surface opposite to the surface on which the concavo-convex structure region is formed. The above-described problem occurs when imprinting is performed a plurality of times by using a transfer substrate having the mold and the transfer substrate in a state where the transfer substrate is convexly curved toward the mold.
The present invention has been made in view of the above-described actual situation, and uses a method for manufacturing a pattern structure that can form a pattern structure on a transfer substrate with high accuracy, and a method for manufacturing this pattern structure. It is an object of the present invention to provide a method for manufacturing an imprint mold.

  In order to achieve such an object, the pattern structure manufacturing method of the present invention has a unit imprint region on one surface and is wider than the planar view shape of the unit imprint region on the opposite surface. A supply step of supplying a molding resin composition to the unit imprint region of the transfer substrate, using a transfer substrate having a depression having an area in plan view so as to include the unit imprint region; Contacting the mold having a concavo-convex structure in the concavo-convex structure region with the transfer substrate to unfold the molded resin composition between the mold and the transfer substrate to form a molded resin layer; A curing step of curing the molded resin layer to form a transfer resin layer, and separating the transfer resin layer and the mold to separate the pattern structure, which is the transfer resin layer, from the transfer resin layer. A mold release step that is positioned on the substrate, and in the contact step, the region where the depression portion of the transfer substrate exists is curved so as to have a convex shape on the mold side, The mold and the transfer substrate are arranged such that the normal line at the center of the unit imprint region supplied with the molding resin composition matches the normal line at the center of the uneven structure region of the mold. It was set as the structure made to adjoin.

As another aspect of the present invention, the transfer substrate has an imprint region composed of a plurality of the unit imprint regions, and the area of the recessed portion in a plan view shape is an area of the imprint region in a plan view shape. The configuration is such that the supply step, the contact step, the curing step, and the release step are executed on each unit imprint region.
As another aspect of the present invention, in the contact step, after contacting the mold and the resin composition to be molded, the normal line at the center of the unit imprint region and the center of the concavo-convex structure region of the mold The region where the depression portion of the transfer substrate is present is flattened while keeping the normal line coincident.

As another aspect of the present invention, in the mold release step, the normal line at the center of the unit imprint region and the normal line at the center of the concavo-convex structure region of the mold are made to coincide with each other. The region where the depression is present is curved so as to have a convex shape toward the mold, and then the transfer resin layer and the mold are separated.
As another aspect of the present invention, the mold has the concavo-convex structure region in which the concavo-convex structure is located on one surface, and a plan view having a larger area than the plan view shape of the concavo-convex structure region on the opposite surface. A concave portion having a shape is included so as to include the concavo-convex structure region, and in the contact step, a region where the concave portion of the mold is present is curved so as to have a convex shape on the transfer substrate side, The mold and the transfer substrate are brought close to each other so that the normal line at the center of the concavo-convex structure region matches the normal line at the center of the unit imprint region supplied with the molding resin composition. The configuration was

As another aspect of the present invention, in the contacting step, after contacting the mold and the resin composition to be molded, a normal line at the center of the concavo-convex structure region of the mold and a center of the unit imprint region While keeping the normal line coincident, the region where the hollow portion of the mold is present is flattened and the imprint region of the transfer substrate is flattened.
As another aspect of the present invention, in the mold release step, the dent of the mold is maintained while the normal line at the center of the concavo-convex structure region of the mold matches the normal line at the center of the unit imprint region. Curving the region where the portion is present in a convex shape toward the transfer substrate side, and curving the region where the recess portion of the transfer substrate is present in a convex shape toward the mold side, Thereafter, the transfer resin layer and the mold were separated.

As another aspect of the present invention, in the mold, the concavo-convex structure region where the concavo-convex structure is located is present on the surface of the convex structure portion protruding from the periphery, and the area of the convex structure portion in plan view Is configured to be smaller than the area of the shape of the recess in plan view.
As another aspect of the present invention, in the transfer substrate, the imprint region is present on a surface of a convex structure portion protruding from the periphery, and an area of the convex structure portion in a plan view is an area of the depression portion. It was set as the structure smaller than the area of a planar view shape.
As another aspect of the present invention, the mold has a plurality of alignment marks around the concavo-convex structure region, the transfer substrate has a plurality of alignment marks around the unit imprint region, and the contact In the process, the alignment is performed using the plurality of alignment marks included in the transfer substrate and the plurality of alignment marks included in the mold.

  The imprint mold manufacturing method of the present invention has a concavo-convex structure region composed of a plurality of unit concavo-convex structure regions in which the concavo-convex structure is located on one surface, and the opposite surface has a plan view shape of the concavo-convex structure region. A method of manufacturing an imprint mold having a recess having a wide area in plan view so as to include the concavo-convex structure region, wherein the unit imprint region is defined on one surface. The imprint includes a region having a hard mask material layer positioned at least in the imprint region, and a recess having a plan view shape having a larger area than the plan view shape of the imprint region on the opposite surface. Manufacturing of the above-described pattern structure on the hard mask material layer in each unit imprint region using a mold manufacturing substrate having a region included A pattern structure which is a resist pattern layer is formed by a method, a hard mask is formed by etching the hard mask material layer through the pattern structure, and then the mold manufacturing substrate through the hard mask. Is configured to be etched.

  As another aspect of the present invention, in the mold manufacturing substrate, the imprint region is present on the surface of a convex structure portion protruding from the periphery, and the area of the convex structure portion in plan view is the depression. It was set as the structure smaller than the area of the planar view shape of a part.

  In the present invention, a highly accurate pattern structure can be stably produced on a transfer substrate having a depression on the surface opposite to the surface on which the pattern is formed. In addition, an imprint mold having a multi-sided uneven structure can be manufactured with high accuracy.

FIG. 1 is a plan view showing an example of a mold used in the method for producing a patterned structure of the present invention. 2 is a cross-sectional view taken along line II of the transfer substrate shown in FIG. FIG. 3 is a plan view showing an example of a transfer substrate used in the method for producing a patterned structure of the present invention. 4 is a cross-sectional view taken along the line II-II of the transfer substrate shown in FIG. FIG. 5 is a process diagram for explaining an embodiment of a method for producing a patterned structure according to the present invention. FIG. 6 is a process diagram for explaining an embodiment of a method for producing a patterned structure according to the present invention. FIG. 7 is a process diagram for explaining an embodiment of a method for producing a patterned structure according to the present invention. FIG. 8 is a process diagram for explaining an embodiment of a method for producing a patterned structure according to the present invention. FIG. 9 is a diagram illustrating the center of the unit imprint region. FIG. 10 is a plan view showing another example of a mold used in the method for producing a patterned structure of the present invention. FIG. 11 is a plan view showing another example of a transfer substrate used in the method for producing a patterned structure of the present invention. FIG. 12 is a view for explaining a contact process using a mold that does not have a recess, and corresponds to FIG. 6 (A). FIG. 13 is a plan view showing an example of a mold manufactured by the method for manufacturing an imprint mold of the present invention. 14 is a cross-sectional view of the mold shown in FIG. 13 taken along line III-III. FIG. 15 is a process diagram showing an embodiment of a method for producing an imprint mold of the present invention.

Hereinafter, embodiments of the present invention will be described with reference to the drawings.
Note that the drawings are schematic or conceptual, and the dimensions of each member, the ratio of sizes between the members, etc. are not necessarily the same as the actual ones, and represent the same members. However, in some cases, the dimensions and ratios may be different depending on the drawing.

[Pattern Structure Manufacturing Method]
The manufacturing method of the pattern structure of this invention has a supply process, a contact process, a hardening process, and a mold release process.
FIG. 1 is a plan view showing an example of a mold used in the method for producing a patterned structure of the present invention, and FIG. 2 is a cross-sectional view taken along the line II of the transfer substrate shown in FIG. 1 and 2, the mold 11 includes a so-called mesa structure having a base 12 and a convex structure portion 14 protruding from the periphery on one surface 12 a of the base 12. A concavo-convex structure region 15 is defined on the surface 14 a of the convex structure portion 14, and the concavo-convex structure 16 is located in the concavo-convex structure region 15. Further, the surface 12 b on the opposite side of the base portion 12 has a recess portion 17 having a planar view shape with a larger area than that of the convex structure portion 14 so as to include the convex structure portion 14. Therefore, a portion around the convex structure portion 14 of the base portion 12 and where the hollow portion 17 is located is a thin portion 18. In FIG. 1, the periphery of the hollow part 17 is shown with the dashed-dotted line.

  The material of such a mold 11 can be selected as appropriate. For example, when the molding resin composition to be used is photo-curable, it can be formed using a transparent substrate that can transmit irradiation light, such as quartz glass, silicate glass, calcium fluoride, magnesium fluoride, acrylic Glass etc. or these arbitrary laminated materials can be used. The thickness of the mold 11 can be set so that the thin-walled portion 18 can be bent in a convex shape by applying pressure from the recessed portion 17 side in consideration of the shape of the concavo-convex structure, material strength, handling suitability, etc. The thickness of the base portion 12 can be appropriately set in the range of about 300 μm to 10 mm, and the thickness of the thin portion 18 can be appropriately set in the range of about 300 μm to 2 mm. Note that the mold 11 may not have the convex structure portion 14 protruding from the periphery on the one surface 12 a of the base portion 12.

  FIG. 3 is a plan view showing an example of a transfer substrate used in the pattern structure manufacturing method of the present invention, and FIG. 4 is a cross-sectional view taken along the line II-II of the transfer substrate shown in FIG. . 3 and 4, the transfer substrate 21 has a so-called mesa structure having a base portion 22 and a convex structure portion 24 protruding from the periphery on one surface 22 a of the base portion 22. The surface 24a of the convex structure 24 has an imprint region 23 in which a plurality of unit imprint regions 23A, 23B, 23C, and 23D are defined. In addition, the surface 22 b on the opposite side of the base portion 22 has a depression 27 having a planar view shape with a larger area than the planar view shape of the convex structure portion 24 so as to include the convex structure portion 24. In FIG. 4, the periphery of the recessed portion 27 is indicated by a one-dot chain line, and the portion around the convex structure portion 24 of the base portion 22 where the recessed portion 27 is located is a thin portion 28. In FIG. 4, the unit imprint regions 23A, 23B, 23C, and 23D are shown surrounded by chain lines. In the illustrated example, the imprint area 23 includes four unit imprint areas 23A, 23B, 23C, and 23D. However, the number and arrangement of the unit imprint areas are not particularly limited. Further, only one unit imprint area may be defined in the imprint area 23.

As the transfer substrate 21, for example, glass such as quartz glass, silicate glass, calcium fluoride, magnesium fluoride, and acrylic glass, sapphire and gallium nitride, and resin substrates such as polycarbonate, polystyrene, acrylic, and polypropylene, or These arbitrary laminated materials can be used. These materials are light transmissive, and are suitable when the light transmissive property is required for the transfer substrate 21 after the pattern structure is formed according to the present invention. Further, it may be a semiconductor such as silicon, gallium arsenide, or gallium nitride, a metal substrate, or a composite material substrate made of any combination of these materials. Further, for example, a desired pattern structure such as a fine wiring used in a semiconductor or a display, a photonic crystal structure, an optical waveguide, or an optical structure such as holography may be formed.
In addition, the transfer substrate 21 may have a hard mask material layer on the surface 22 a of the base portion 22 and on the surface 24 a of the convex structure portion 24. Further, the transfer substrate 21 may not have the convex structure portion 24 protruding from the periphery on the one surface 22 a of the base portion 22.
Next, an embodiment of the pattern structure manufacturing method of the present invention will be described as an example using the mold 11 and the transfer substrate 21 as described above.
5, FIG. 6, FIG. 7 and FIG. 8 are process diagrams for explaining an embodiment of the method for producing a patterned structure of the present invention, and are shown in cross-sections corresponding to FIG. 2 and FIG. Hereinafter, a method for producing a pattern structure according to the present invention will be described with reference to FIGS.

<Supply process>
First, the transfer substrate 21 is mounted on the substrate holding member 121, and a fluid such as air is press-fitted into a space S formed by the substrate holding member 121 and the recess 27 of the transfer substrate 21 by a fluid supply / discharge mechanism (not shown). By applying pressure, the thin portion 28 of the transfer substrate 21 is bent so that the convex structure 24 side has a convex shape (FIG. 5A).
The substrate holding member 121 is not particularly limited, and the transfer substrate 21 can be held by means such as a suction holding method, a machine holding method, and an electrostatic adsorption holding method. The substrate holding member 121 and the recess 27 of the transfer substrate 21 What is necessary is just to be able to make the space S formed in a liquid-tight state and an air-tight state. Further, the fluid supply / exhaust mechanism supplies a fluid to the space S formed by the substrate holding member 121 and the recessed portion 27 of the transfer substrate 21 to bend the thin-walled portion 28 of the transfer substrate 21. Any material can be used as long as it can discharge the fluid from the substrate and flatten the thin portion 28 of the transfer substrate 21 to the original state.

In the supplying step, the droplet 31 of the resin composition to be molded is supplied to a desired unit imprint region of the transfer substrate 21 (FIG. 5B). In the illustrated example, droplets 31 of the molding resin composition are supplied to the unit imprint region 23A. The supply of the droplet 31 can be performed by discharging a droplet from the inkjet head, supplying from a dispenser, or the like.
The molding resin composition only needs to have fluidity that can be supplied from a supply means such as an inkjet head or a dispenser, and examples thereof include a photocurable resin composition and a thermosetting resin composition. . For example, the photocurable resin composition is composed of a main agent, an initiator, and a crosslinking agent, and if necessary, a mold release agent for suppressing adhesion to the mold 11 or adhesion to the transfer substrate 21. It may contain an adhesive for improving the properties. And the to-be-molded resin composition to be used can be suitably selected according to the use of the pattern structure to manufacture, a required characteristic, a physical property, etc. For example, if the use of the pattern structure is a lithography application, it is required to have etching resistance, a low viscosity and a small residual film thickness, and if the use of the pattern structure is an optical member, a specific refractive index, Light transmittance is required, and a resin composition to be molded can be appropriately selected according to these requirements. However, in any application, it is required to have characteristics (viscosity, surface tension, etc.) that satisfy the compatibility with the supply means such as the inkjet head to be used. Note that the viscosity, surface tension, and the like of a compatible liquid differ depending on the structure and material of the inkjet head. For this reason, it is preferable to appropriately adjust the viscosity, surface tension and the like of the molding resin composition to be used, or to appropriately select an ink jet head suitable for the molding resin composition to be used.

Further, the number of droplets 31 of the molding resin composition to be supplied onto the unit imprint region 23A of the transfer substrate 21, the distance between adjacent droplets, the dropping amount of each droplet, and the molding resin required The total amount of the composition, the wettability of the molding resin composition with respect to the transfer substrate 21, the size of the gap between the transfer substrate 21 and the mold 11 in the subsequent contact step, and the like can be set as appropriate.
In addition, after supplying the droplet 31 of the molding resin composition to the unit imprint region 23A, the thin portion 28 of the transfer substrate 21 may be curved so that the convex structure 24 side has a convex shape.

<Contact process>
The mold 11 is mounted on the mold holding member 111, and a fluid such as air is press-fitted and pressurized into a space S ′ formed by the mold holding member 111 and the recessed portion 17 of the mold 11 by a fluid supply / discharge mechanism (not shown). Thus, the thin portion 18 of the mold 11 is bent so that the convex structure 14 side has a convex shape (FIG. 5C).
The mold holding member 111 is not particularly limited, and the mold 11 can be held by means such as a suction holding method, a machine holding method, and an electrostatic adsorption holding method, and is formed by the mold holding member 111 and the recessed portion 17 of the mold 11. Any space can be used as long as the space S ′ can be made liquid-tight or air-tight. Further, the fluid supply / exhaust mechanism supplies a fluid to a space S ′ formed by the mold holding member 111 and the hollow portion 17 of the mold 11 to bend the thin-walled portion 18 of the mold 11, and this space S ′. Any fluid can be used as long as the fluid can be discharged from the mold 11 and the thin portion 18 of the mold 11 can be flattened to the original state.

In the contact step, the transfer substrate 21 in which the thin portion 28 is curved so that the convex structure 24 side has a convex shape as described above, and the thin portion 18 has a convex shape on the convex structure 14 side as described above. The mold 11 curved so as to be In the present invention, the proximity between the transfer substrate 21 and the mold 11 is as shown in FIG. 6A at the center C of the unit imprint region 23A to which the molding resin composition of the transfer substrate 21 is supplied. The mold 11 and the transfer substrate 21 are brought close to each other so that the normal line N and the normal line N ′ at the center C ′ of the uneven structure region 15 of the mold 11 coincide with each other. In FIG. 6A, the normal line N is indicated by a solid line, and the normal line N ′ is indicated by a two-dot chain line. Here, the normal line N at the center C of the unit imprint region 23A to which the resin composition to be molded of the transfer substrate 21 is supplied is matched with the normal line N ′ at the center C ′ of the uneven structure region 15 of the mold 11. Means the case where there is a difference of 0.002 ° or less between the direction of the normal line N and the direction of the normal line N ′ in addition to the case where the normal line N and the normal line N ′ completely coincide. It is a concept to include.
FIG. 9 is a partial plan view showing the imprint region 23 of the transfer substrate 21. In FIG. 9, in the imprint area 23 in which the four unit imprint areas 23A, 23B, 23C, and 23D are defined, the droplets 31 of the resin composition to be molded are supplied and the mold 11 is close to the target. The center C of the unit imprint areas 23A, 23B, 23C, and 23D is shown. The center C of the unit imprint areas 23A, 23B, 23C, and 23D can be the center of gravity of the figure determined by the outline of each unit imprint area. Similarly, the center C ′ of the concavo-convex structure region 15 of the mold 11 can also be the center of gravity of the figure determined by the outline of the concavo-convex structure region 15.

  As described above, in order to make the normal line N at the center C of the unit imprint area 23A of the transfer substrate 21 coincide with the normal line N ′ at the center C ′ of the uneven structure area 15 of the mold 11, for example, Such a method can be used. First, the normal N at the center C of the unit imprint region 23A when the thin portion 28 of the transfer substrate 21 changes between a flat state and a curved state in which the convex structure 24 side has a convex shape. The change is grasped in advance by measurement or simulation. Further, the change in the normal N when the orientation of the transfer substrate 21 is changed by operating the substrate holding member 121 is also grasped in advance by measurement or simulation. Similarly, changes in the normal line N are grasped for the other unit imprint areas 23B, 23C, and 23D. Similarly, with respect to the mold 11, the normal line at the center C ′ of the concavo-convex structure region 15 when the thin-walled portion 18 changes between a flat state and a curved state such that the convex structure 14 side has a convex shape. The change of N ′ is grasped in advance by measurement or simulation. Further, the change of the normal line N ′ when the mold holding member 111 is operated to change the direction of the mold 1 is also grasped in advance by measurement or simulation. The mold holding member 111 and / or the substrate holding member 121 are operated on the basis of the change prediction data of the normal line N and the normal line N ′ thus grasped, so that the direction of the mold 11 and the direction of the transfer substrate 21 are relative to each other. By adjusting to the normal line N, the normal line N and the normal line N ′ can be matched.

In the example shown in FIG. 6A, the direction of the normal N at the center C of the unit imprint region 23A of the transfer substrate 21 is deviated from the vertical direction, so the direction of the normal N and the normal N ′ The mold holding member 111 is operated so that the directions match. Further, for example, by operating the substrate holding member 121, the normal line N at the center C of the unit imprint region 23 </ b> A of the transfer substrate 21 in which the thin portion 28 is curved is set to the vertical direction, and then the center C of the concavo-convex structure region 15. The mold holding member 111 holding the mold 11 is operated so that the normal line N ′ in the vertical direction is in the vertical direction, and the mold 11 is brought close to the transfer substrate 21 so that the normal line N and the normal line N ′ coincide with each other. You may let them.
In this way, by bringing the transfer substrate 21 and the mold 11 close to each other, the molded resin composition is developed between the mold 11 and the unit imprint region 23A of the transfer substrate 21 to form the molded resin layer 32 ( FIG. 6 (B)). In the proximity of the transfer substrate 21 and the mold 11, the first contact position between the mold 11 and the droplet 31 of the molding resin composition supplied to the unit imprint area 23 </ b> A is the center of the unit imprint area 23 </ b> A. Thus, the development of the molding resin composition in the unit imprint region 23A becomes uniform, and the thickness of the remaining film portion (the portion existing in the gap between the mold 11 and the transfer substrate 21) in the molding resin layer 32 to be formed. The distribution is uniform.

  In the present embodiment, in the contact step, after forming the resin layer 32 to be molded by bringing the transfer substrate 21 and the mold 11 close to each other as described above, the normal line N at the center C of the unit imprint region 23A, While the normal line N ′ at the center C ′ of the concavo-convex structure region 15 of the mold 11 is made coincident, the thin-walled portion 28 in the region where the recessed portion 27 of the transfer substrate 21 exists is flattened. The thin portion 18 in the existing region is flattened (FIG. 7A). The flattening of the thin portion 18 of the mold 11 is performed by discharging the fluid from the space S ′ formed by the mold holding member 111 and the recess portion 17 of the mold 11 by a fluid supply / discharge mechanism (not shown). Can do. Similarly, the thin portion 28 of the transfer substrate 21 is flattened by discharging the fluid from the space S formed by the substrate holding member 121 and the recessed portion 27 of the transfer substrate 21 by a fluid supply / discharge mechanism (not shown). be able to. In the example shown in FIG. 6B, the direction of the normal line N at the center C of the unit imprint region 23A of the transfer substrate 21 is deviated from the vertical direction, and thus the progress of the flattening of the thin portion 28 of the transfer substrate 21 is performed. Along with this, the direction of the normal N changes so as to be the vertical direction. Therefore, the mold holding member 111 is made flat so that the thin portion 18 of the mold 11 is flattened and the normal line N ′ at the center C ′ of the mold 11 coincides with the normal line N at the center C of the unit imprint region 23A. To operate.

Before the curing step described later, the thin portion 18 of the mold 11 is flattened as described above, and the thin portion 28 of the transfer substrate 21 is flattened to thereby form a remaining film portion (mold 11) in the resin layer 32 to be molded. The thickness distribution of the portion existing in the gap between the transfer substrate 21 and the transfer substrate 21 becomes more uniform.
As described above, when only one unit imprint area is defined in the imprint area 23, the same operation as that of the unit imprint area 23A is performed for the one unit imprint area. be able to.

<Curing process>
Next, light irradiation is performed from the mold 11 side, and the resin layer 32 to be molded is cured to form a transfer resin layer 33 to which the concavo-convex structure 16 of the mold 11 is transferred (FIG. 7B). In this curing step, when the transfer substrate 21 is made of a light-transmitting material, light irradiation may be performed from the transfer substrate 21 side, or light irradiation may be performed from both sides of the transfer substrate 21 and the mold 11.
Further, when the molding resin composition is a thermosetting resin, the molding resin layer 32 can be cured by heat treatment.

<Release process>
Next, in the mold release process, the normal line N at the center C of the unit imprint region 23A and the normal line N ′ at the center C ′ of the uneven structure region 15 of the mold 11 are made to coincide with each other. The thin-walled portion 28 in the region where the hollow portion 27 exists is curved, and the thin-walled portion 18 in the region where the hollow portion 17 of the mold 11 exists is curved (FIG. 8A). Such bending of the thin portion 18 of the mold 11 is caused by pressurizing and pressurizing a fluid into a space S ′ formed by the mold holding member 111 and the recess portion 17 of the mold 11 by a fluid supply / discharge mechanism (not shown). It can be carried out. Similarly, the thin portion 28 of the transfer substrate 21 is curved by pressurizing and pressurizing the fluid into the space S formed by the substrate holding member 121 and the recess portion 27 of the transfer substrate 21 by a fluid supply / discharge mechanism (not shown). Can be performed. In the example shown in FIG. 8A, the direction of the normal N at the center C of the unit imprint region 23A of the transfer substrate 21 deviates from the vertical direction as the thin portion 28 curves. Therefore, the mold holding member 111 is moved so that the thin portion 18 of the mold 11 is curved and the normal line N ′ at the center C ′ of the mold 11 coincides with the normal line N at the center C of the unit imprint region 23A. Manipulate.

Next, the transfer resin layer 31 and the mold 11 are separated from each other, so that the pattern structure 35 as the transfer resin layer 33 is positioned on the unit imprint region 23A of the transfer substrate 21 (FIG. 8B). As described above, the thin portion 18 of the mold 11 is bent and the thin portion 28 of the transfer substrate 21 is bent, and then the transfer resin layer 31 and the mold 11 are separated, whereby the transfer resin layer 31 and the mold 11 are separated. It is easy to separate the region in contact with the outer periphery from the outer peripheral side, and it is possible to prevent occurrence of defects in the formed pattern structure 35 and damage to the mold 11.
Thereafter, the pattern structure 35 is sequentially formed in the other unit imprint regions 23B, 23C, and 23D constituting the imprint region 23 by repeating the above-described supply process, contact process, curing process, and mold release process.
In such a method for manufacturing a pattern structure, a highly accurate pattern structure can be stably formed on a transfer substrate having a depression by multi-faceting.

In the present invention, when the transfer substrate 21 has a hard mask material layer on the surface 22a of the base portion 22 and on the surface 24a of the convex structure portion 24, all the units constituting the imprint region 23 as described above. In the imprint regions 23A, 23B, 23C, and 23D, after the pattern structure 35 is formed on the hard mask material layer, the four unit imprint regions 23A, 23B, 23C, and 23D are formed using the pattern structure as an etching mask. At the same time, the hard mask material layer can be etched. Alternatively, the pattern structure 35 may be formed for each unit imprint region, and the hard mask material layer may be etched using the pattern structure as an etching mask.
In the present invention, for example, the mold 11 used in the above embodiment is provided with alignment marks 51 at the four corners around the convex structure portion 14 as shown in FIG. As shown in FIG. 11, an alignment mark 55 corresponding to each unit imprint region 23A, 23B, 23C, 23D may be provided around the convex structure portion 24. In the contact process, in the imprint using the mold 11 for a desired unit imprint region, for example, the unit imprint region 23A shown in FIG. 11, the circle is enclosed in the alignment mark 55 of the transfer substrate 21. The alignment may be performed using the three alignment marks 55 and the four alignment marks 51 of the mold 11.

  The above-described embodiment is an exemplification, and the present invention is not limited to such an embodiment. For example, the mold 11 may not have the recess 17. FIG. 12 is a view for explaining a contact process using such a mold 11 ′ that does not have the depression 17, and corresponds to FIG. 6 (A). As shown in FIG. 12, the mold 11 ′ held by the mold holding member 111 does not require the operation of bending and flattening the mold 11 in the above-described embodiment, but the uneven structure region 15 of the mold 11 ′ is not necessary. The operation of making the normal line N ′ at the center C ′ coincide with the normal line N at the center C of the unit imprint region 23A of the transfer substrate 21 needs to be performed in the same manner. Thereby, the position where the droplet 31 of the molding resin composition supplied to the unit imprint region 23A and the mold 11 ′ first come into contact is the center of the unit imprint region 23A. Therefore, the development of the molding resin composition in the unit imprint region 23A becomes uniform, and the thickness distribution of the remaining film portion (the portion existing in the gap between the mold 11 ′ and the transfer substrate 21) in the molding resin layer to be formed. It will be uniform.

  Further, in the contacting step, after the transfer substrate 21 and the mold 11 are brought close to each other and the molding resin layer 32 is formed, the thinned portion 28 in the region where the recess portion 27 of the transfer substrate 21 exists, the depression of the mold 11 is formed. Even in the case where the thin portion 18 in the region where the portion 17 exists is flattened, the thinning portion 18 of the mold 11 and the thin portion 28 of the transfer substrate 21 are not curved in the mold release process. The resin layer 31 and the mold 11 may be pulled apart.

[Method for producing imprint mold]
FIG. 13 is a plan view showing an example of a mold manufactured by the method for manufacturing an imprint mold of the present invention, and FIG. 14 is a cross-sectional view taken along line III-III of the mold shown in FIG. A mold 41 shown in FIGS. 13 and 14 has a base 42 and a convex structure 44 protruding from the periphery on one surface 42a of the base 42. On the surface 44a of the convex structure portion 44, a concave / convex structure region 43 including four unit concave / convex structure regions 43A, 43B, 43C, and 43D is defined, and the four unit concave / convex structure regions 43A, 43B, 43C, The uneven structure 46 is located at 43D. Further, the surface 42 b on the opposite side of the base portion 42 has a recess 47 having a planar view shape with a larger area than the planar view shape of the uneven structure region 43 so as to include the uneven structure region 43. In FIG. 13, the periphery of the recess 47 is indicated by a one-dot chain line, and the concavo-convex structure 46 is omitted. In the illustrated example, the concavo-convex structure region 43 includes four unit concavo-convex structure regions 43A, 43B, 43C, and 43D. However, the number and arrangement of the unit concavo-convex structure regions are not particularly limited.

Next, an example of the method for producing an imprint mold of the present invention will be described by taking the production of the mold 41 as an example. FIG. 15 is a process diagram showing an embodiment of a method for producing an imprint mold of the present invention, and shows a cross section corresponding to FIG.
In the present embodiment, a substrate provided with a hard mask material layer 29 on the surface 22a of the base portion 22 of the transfer substrate 21 and the surface 24a of the convex structure portion 24 is used as the mold manufacturing substrate 21 ′. For this reason, in the mold manufacturing substrate 21 ′, the same members as those of the transfer substrate 21 are denoted by the same member numbers. The four unit imprint regions 23A, 23B, 23C, and 23D in the mold manufacturing substrate 21 ′ become the four unit uneven structure regions 43A, 43B, 43C, and 43D in the imprint mold 41. Further, the recess 27 in the mold manufacturing substrate 21 ′ becomes a recess 47 in the imprint mold 41.
In the imprint mold manufacturing method of the present invention, the four unit imprint regions 23A, 23B, 23C, and the like on the hard mask material layer 29 of the mold manufacturing substrate 21 ′ are manufactured by the pattern structure manufacturing method of the present invention. A pattern structure 35 which is a resist pattern layer is formed on 23D (FIG. 15A).

Next, the hard mask material layer 29 is etched through the pattern structure 35 to form a hard mask 29 '(FIG. 15B).
Next, the mold manufacturing substrate 21 ′ is etched through the hard mask 29 ′ to form the concavo-convex structure 46, whereby an imprint mold 41 as shown in FIGS. 13 and 14 can be obtained. Since the mold manufacturing substrate 21 ′ is etched simultaneously in the four unit imprint regions 23A, 23B, 23C, and 23D using the hard mask 29 ′ thus formed as a mask, the four unit uneven structure regions 43A are etched. , 43B, 43C, 43D, the concave-convex structure 46 has a uniform recess depth.
In such a method for producing an imprint mold of the present invention, an imprint mold having a multi-sided unit concavo-convex structure region where the concavo-convex structure is located can be produced with high accuracy.
The above-described embodiment is an exemplification, and the present invention is not limited to such an embodiment. For example, the mold manufacturing substrate 21 ′ may not include the convex structure portion 24.

  The present invention can be used for various processes that require the formation of a pattern structure having a multi-sided fine concavo-convex structure, such as a replica mold used in the imprint method.

DESCRIPTION OF SYMBOLS 11 ... Mold 14 ... Convex structure part 15 ... Uneven structure area 16 ... Uneven structure 17 ... Indentation part 21 ... Transfer substrate 23 ... Imprint area 23A, 23B, 23C, 23D ... Unit imprint area 24 ... Convex structure part 27 ... Indentation Part 31: Droplet 32 ... Molded resin layer 33 ... Transfer resin layer 35 ... Pattern structure 21 '... Mold manufacturing substrate 29 ... Hard mask material layer 29' ... Hard mask 41 ... Imprint mold 43 ... Uneven structure region 43A, 43B, 43C, 43D ... Unit uneven structure region 46 ... Uneven structure 47 ... Depression

Claims (12)

A depression having a unit imprint area on one surface and having a planar view shape having a larger area than the planar view shape of the unit imprint area on the opposite surface is included to include the unit imprint area. A supply step of supplying a molding resin composition to the unit imprint region of the transfer substrate using a transfer substrate having
A contact step of forming the molded resin layer by unfolding the molded resin composition between the mold and the transfer substrate by bringing the mold having the concavo-convex structure in the concavo-convex structure region close to the transfer substrate;
A curing step of curing the molded resin layer to form a transfer resin layer;
A mold release step in which the pattern structure that is the transfer resin layer is positioned on the transfer substrate by separating the transfer resin layer and the mold;
In the contacting step, a region where the depression portion of the transfer substrate is present is curved so as to have a convex shape on the mold side, and at the center of the unit imprint region to which the molding resin composition is supplied. A method of manufacturing a pattern structure, wherein the mold and the transfer substrate are brought close to each other so that a normal line and a normal line at the center of the concavo-convex structure region of the mold coincide with each other.   The transfer substrate has an imprint region composed of a plurality of unit imprint regions, and the area of the recessed portion in plan view is larger than the area of the imprint region in plan view, and each unit imprint The method for manufacturing a pattern structure according to claim 1, wherein the supplying step, the contacting step, the curing step, and the releasing step are performed on a region.   In the contact step, after the mold and the resin composition to be molded are contacted, the normal line at the center of the unit imprint region and the normal line at the center of the uneven structure region of the mold remain matched. The method for producing a pattern structure according to claim 1, wherein a region where the depression portion of the transfer substrate is present is flattened.   In the mold release step, the region where the depression portion of the transfer substrate is present remains while the normal line at the center of the unit imprint region and the normal line at the center of the uneven structure region of the mold are matched. 4. The method of manufacturing a pattern structure according to claim 3, wherein the pattern resin is curved so as to have a convex shape on the mold side, and then the transfer resin layer and the mold are separated from each other. The mold has the concavo-convex structure region in which the concavo-convex structure is located on one surface, and a concave portion having a planar view shape having a larger area than the plan view shape of the concavo-convex structure region on the opposite surface. Having a structural region,
In the contacting step, a region where the hollow portion of the mold is present is curved so as to form a convex shape toward the transfer substrate, and a normal line at the center of the concavo-convex structure region and the resin composition to be molded are 5. The pattern according to claim 1, wherein the mold and the transfer substrate are brought close to each other so as to coincide with a normal line at a center of the supplied unit imprint region. Manufacturing method of structure.   In the contact step, after contacting the mold and the resin composition to be molded, the normal line at the center of the uneven structure region of the mold and the normal line at the center of the unit imprint region remain matched. The method for producing a pattern structure according to claim 5, wherein the area where the hollow portion of the mold is present is flattened and the imprint area of the transfer substrate is flattened.   In the mold release step, a region where the depression portion of the mold exists is transferred while keeping a normal line at the center of the uneven structure region of the mold and a normal line at the center of the unit imprint region. The substrate is curved so as to have a convex shape on the substrate side, and the region of the transfer substrate where the depression is present is curved so as to have a convex shape on the mold side, and then the transfer resin layer and the The pattern structure manufacturing method according to claim 6, wherein the mold is pulled apart.   In the mold, the concavo-convex structure region where the concavo-convex structure is located is present on the surface of the convex structure portion protruding from the periphery, and the area of the convex structure portion in plan view is the plan view shape of the recess portion The method of manufacturing a pattern structure according to claim 5, wherein the pattern structure is smaller than the area of the pattern structure.   In the transfer substrate, the imprint region is present on the surface of the convex structure portion protruding from the periphery, and the area of the convex structure portion in plan view is smaller than the area of the recess portion in plan view The method for manufacturing a pattern structure according to any one of claims 1 to 8, wherein In the mold, a plurality of alignment marks are located around the concavo-convex structure region,
The transfer substrate has a plurality of alignment marks around the unit imprint region,
10. The alignment according to claim 1, wherein in the contacting step, alignment is performed using the plurality of alignment marks included in the transfer substrate and the plurality of alignment marks included in the mold. The manufacturing method of the pattern structure as described in any one of. A concave-convex portion having a concavo-convex structure region composed of a plurality of unit concavo-convex structure regions where the concavo-convex structure is located on one surface, and having a planar view shape with a larger area than the planar view shape of the concavo-convex structure region on the opposite surface In the method for producing an imprint mold having the concavo-convex structure region,
It has an imprint area in which a plurality of unit imprint areas are defined on one surface, and has a hard mask material layer positioned at least in the imprint area, and a plan view of the imprint area on the opposite surface A mold manufacturing substrate having a depression having a plan view shape with a larger area than the shape so as to include the imprint region, and on the hard mask material layer of each unit imprint region, A pattern structure that is a resist pattern layer is formed by the method for manufacturing a pattern structure according to claim 10,
Etching the hard mask material layer through the pattern structure to form a hard mask, and then etching the mold manufacturing substrate through the hard mask. .   In the mold manufacturing substrate, the imprint region is present on the surface of the convex structure portion protruding from the periphery, and the area of the convex structure portion in plan view is larger than the area of the recess portion in plan view shape. The method for producing an imprint mold according to claim 11, wherein the mold is small.

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