JP6801349B2 - Manufacturing method of pattern structure and manufacturing method of imprint mold - Google Patents

Description

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

In recent years, a pattern forming technique using an imprint method has attracted attention as a fine pattern forming technique in place of the photolithography technique. The imprint method is a pattern forming technique in which a mold member (mold) having a fine concavo-convex structure is used and the concavo-convex structure is transferred to a resin layer to be molded to transfer the fine structure to the same size. For example, in the imprint method using a photocurable resin composition as the resin composition to be molded, droplets of the photocurable resin composition are supplied to the surface of the transfer substrate, and the mold and the transfer substrate have a desired uneven structure. The photocurable resin composition is filled in the concavo-convex structure by bringing the and the case close to each other to a predetermined distance, and in this state, light is irradiated from the mold side to cure the photocurable resin composition, and then the mold is molded into a resin layer. By pulling away from the mold, a pattern structure having a concavo-convex structure (concave-convex pattern) in which the concavo-convex features of the mold are inverted is formed.

In such an imprint method, when the mold and the transfer substrate are brought close to each other to a predetermined distance to fill the concave-convex structure of the mold with the photocurable resin composition, pattern defects may occur due to residual air bubbles. .. In order to prevent such residual air bubbles, the mold and the transfer substrate are placed in a state where the transfer substrate is convexly curved toward the mold side and / or when the mold is convexly curved toward the transfer substrate side. The photocurable resin is brought into close contact with the photocurable resin composition at the center of the concave-convex structure region of the mold and the center of the imprint region of the transfer substrate, and then gradually brought into contact with the outer peripheral side of the concave-convex structure region. Bubbles are eliminated as the composition is filled (for example, Patent Document 1).

Japanese Patent Publication No. 2011-512019

However, when the mold and the transfer substrate are brought close to each other in a state where the transfer substrate is curved convexly toward the mold side, the portion where the transfer substrate is curved and is most convex toward the mold side and the imprint region. When the center does not match, for example, when the imprint region exists on the inclined surface of the curved transfer board, there are the following problems. That is, the position where the droplet of the photocurable resin composition supplied to the imprint region of the transfer substrate and the mold first come into contact with each other is off the center of the imprint region. Therefore, 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 come into contact with each other. There is a possibility that the photocurable resin composition may not be filled at the opposite end of the imprinted area. In addition, the uniformity of the thickness distribution of the residual film (the film portion formed in the gap between the mold and the transfer substrate) in the formed pattern structure may be impaired.

Further, when imprinting is performed a plurality of times to form a pattern on the transfer substrate on multiple surfaces, a state in which an imprint region exists on the inclined surface of the curved transfer substrate inevitably occurs, and the above-mentioned problems occur. For example, in the case of producing a replica mold having a concavo-convex structure region on multiple surfaces by imprinting using a master mold, a recessed portion is provided on a surface opposite to the surface on which the concavo-convex structure region is formed as a transfer substrate for the replica mold. The above-mentioned problems occur when imprinting in which the mold and the transfer substrate are brought close to each other in a state where the transfer substrate is curved convexly toward the mold side is performed a plurality of times using the transfer substrate.
The present invention has been made in view of the above-mentioned actual conditions, and uses a method for manufacturing a pattern structure capable of forming 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 method for manufacturing a pattern structure of the present invention has a unit imprint area on one surface and is wider than the plan view shape of the unit imprint area on the opposite surface. A supply step of supplying the resin composition to be molded to the unit imprint region of the transfer substrate using a transfer substrate having a recess portion having a plan view shape of the area so as to include the unit imprint region. A contact step of developing the resin composition to be molded between the mold and the transfer substrate by bringing the mold having the concave-convex structure and the transfer substrate close to each other in the concave-convex structure region to form a resin layer to be molded, and the above-mentioned. A curing step of curing the resin layer to be molded to form a transfer resin layer, and a state in which the pattern structure, which is the transfer resin layer, is positioned on the transfer substrate by separating the transfer resin layer from the mold. In a plan view from one surface side of the transfer substrate, the center of the unit imprint region coincides with the center of the region where the recess portion of the transfer substrate exists. Orazu, in the contacting step, the area where recess is present is curved in a convex form on the mold side, the unit imprint area where the object to be molded resin composition is supplied in the transfer substrate The transfer substrate and / or the mold is tilted so that the normal line at the center of the mold and the normal line at the center of the concave-convex structure region of the mold are brought close to each other. The configuration was as follows.

As another aspect of the present invention, the transfer substrate has an imprint area composed of a plurality of the unit imprint areas, and the center of at least one unit imprint area of the plurality of unit imprint areas is set. does not coincide in the center of the area where the recess portion of the transfer substrate is present, the area of the plan view shape of the recess is wider than the area of the plan view shape of the imprint area, the said transfer substrate The supply step, the contact step, the curing step, and the mold release step are executed for each unit imprint region having the center that does not coincide with the center of the region where the recess portion exists .
As another aspect of the present invention, in the contact step, after the mold and the resin composition to be molded are brought into contact with each other, at the normal at the center of the unit imprint region and at the center of the uneven structure region of the mold. The configuration is such that the region where the recessed portion of the transfer substrate exists is flattened while keeping the normal line aligned.

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 concave-convex structure region of the mold are kept aligned, and the transfer substrate is described. The region where the recessed portion exists is curved toward the mold side so as to have a convex shape, and then the transfer resin layer and the mold are separated from each other.
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 the concavo-convex structure region has a wider area than the plan view shape of the concavo-convex structure region on the opposite surface. A recess having a shape is provided so as to include the concave-convex structure region, and in the contact step, the region where the recess of the mold exists is curved toward the transfer substrate so as to have a convex shape. The mold and the transfer substrate are brought close to each other so that the normal at the center of the concave-convex structure region and the normal at the center of the unit imprint region to which the resin composition to be molded is supplied match. The configuration was as follows.

As another aspect of the present invention, in the contact step, after the mold and the resin composition to be molded are brought into contact with each other, at the normal at the center of the uneven structure region of the mold and at the center of the unit imprint region. The structure is such that the region where the recessed portion of the mold exists is flattened and the imprint region of the transfer substrate is flattened while keeping the normal line aligned.
As another aspect of the present invention, in the mold release step, the depression of the mold while keeping the normal at the center of the uneven structure region of the mold and the normal at the center of the unit imprint region coincide with each other. The region where the portion exists is curved so as to have a convex shape toward the transfer substrate side, and the region where the recess portion of the transfer substrate exists is curved so as to have a convex shape toward the mold side. After that, the transfer resin layer and the mold were separated from each other.

As another aspect of the present invention, in the mold, the concave-convex structure region where the concave-convex structure is located exists on the surface of the convex structure portion protruding from the periphery, and the area of the convex structure portion in a plan view shape. Is smaller than the area of the recessed portion in a plan view.
As another aspect of the present invention, in the transfer substrate, the imprint region exists on the surface of the convex structure portion protruding from the periphery, and the area of the convex structure portion in a plan view is the recessed portion. The configuration is such that it is smaller than the area of the plan view shape.
As another aspect of the present invention, the mold has a plurality of alignment marks located around the uneven structure region, and the transfer substrate has a plurality of alignment marks around the unit imprint region, and the contact thereof. In the step, the plurality of alignment marks of the transfer substrate and the plurality of alignment marks of the mold are used for alignment.

The method for manufacturing an imprint mold of the present invention has a concavo-convex structure region composed of a plurality of unit concavo-convex structure regions in which a concavo-convex structure is located on one surface, and has a concavo-convex structure region on the opposite surface from a plan view shape of the concavo-convex structure region. Is a method for manufacturing an imprint mold having a recess having a wide area in plan view so as to include the uneven structure region, and an imprint in which a plurality of unit imprint regions are defined on one surface. The imprint has a recess having a region, at least a hard mask material layer located in the imprint region, and a plan view shape having an area wider than the plan view shape of the imprint region on the opposite surface. A pattern structure, which is a resist pattern layer, is formed on the hard mask material layer of each unit imprint region by the above-mentioned method for producing a pattern structure, using a mold manufacturing substrate having a region so as to include the region. The hard mask material layer was etched through the pattern structure to form a hard mask, and then the mold manufacturing substrate was etched through the hard mask.

As another aspect of the present invention, in the mold manufacturing substrate, the imprint region exists on the surface of the convex structure portion protruding from the periphery, and the area of the convex structure portion in the plan view shape is the recess. The configuration is such that it is smaller than the area of the plan view shape of the portion.

In the present invention, a highly accurate pattern structure can be stably produced on a transfer substrate having a recessed portion on the surface opposite to the surface on which the pattern is formed. In addition, it is possible to manufacture an imprint mold having a concavo-convex structure on multiple surfaces with high accuracy.

FIG. 1 is a plan view showing an example of a mold used in the method for manufacturing a pattern structure of the present invention. FIG. 2 is a cross-sectional view taken along the 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 manufacturing a pattern structure of the present invention. FIG. 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 the method for manufacturing a pattern structure of the present invention. FIG. 6 is a process diagram for explaining an embodiment of the method for manufacturing a pattern structure of the present invention. FIG. 7 is a process diagram for explaining an embodiment of the method for manufacturing a pattern structure of the present invention. FIG. 8 is a process diagram for explaining an embodiment of the method for manufacturing a pattern structure of the present invention. FIG. 9 is a diagram showing the center of the unit imprint area. FIG. 10 is a plan view showing another example of the mold used in the method for manufacturing the pattern structure of the present invention. FIG. 11 is a plan view showing another example of the transfer substrate used in the method for manufacturing the pattern structure of the present invention. FIG. 12 is a diagram for explaining a contact process using a mold having no recessed portion, and is a diagram corresponding 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. FIG. 14 is a cross-sectional view taken along the line III-III of the mold shown in FIG. FIG. 15 is a process diagram showing an embodiment of the method for manufacturing an imprint mold of the present invention.

Hereinafter, embodiments of the present invention will be described with reference to the drawings.
It should be noted that the drawings are schematic or conceptual, and the dimensions of each member, the ratio of the sizes between the members, etc. are not necessarily the same as the actual ones, and may represent the same members, etc. However, the dimensions and ratios may differ from each other depending on the drawing.

[Manufacturing method of pattern structure]
The method for producing a pattern structure of the present invention includes a supply step, a contact step, a curing step, and a mold release step.
FIG. 1 is a plan view showing an example of a mold used in the method for manufacturing a pattern structure of the present invention, and FIG. 2 is a cross-sectional view taken along line I-I of the transfer substrate shown in FIG. In FIGS. 1 and 2, the mold 11 has a so-called mesa structure having a base portion 12 and a convex structure portion 14 projecting from the periphery on one surface 12a of the base portion 12. A concave-convex structure region 15 is defined on the surface 14a of the convex structure portion 14, and the concave-convex structure 16 is located in the concave-convex structure region 15. Further, the surface 12b on the opposite side of the base portion 12 has a recessed portion 17 having a plan view shape having a wider area than the plan view shape of the convex structure portion 14 so as to include the convex structure portion 14. Therefore, the portion around the convex structure portion 14 of the base portion 12 where the recessed portion 17 is located is the thin-walled portion 18. In FIG. 1, the peripheral edge of the recessed portion 17 is indicated by a alternate long and short dash line.

The material of such a mold 11 can be appropriately selected. For example, when the resin composition to be used is photocurable, it can be formed using a transparent substrate that can transmit irradiation light, and can be formed of quartz glass, siliceous glass, calcium fluoride, magnesium fluoride, acrylic. Glass or the like, or any laminated material thereof can be used. The thickness of the mold 11 can be set so that the thin portion 18 can be curved in a convex shape by applying pressure from the recessed portion 17, while considering the shape of the uneven structure, the material strength, the handling suitability, and the like. 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-walled portion 18 can be appropriately set in the range of about 300 μm to 2 mm. The mold 11 may not have a convex structure portion 14 protruding from the periphery on one surface 12a of the base portion 12.

Further, FIG. 3 is a plan view showing an example of a transfer substrate used in the method for manufacturing a pattern structure of the present invention, and FIG. 4 is a cross-sectional view of the transfer substrate shown in FIG. 3 in lines II-II. .. In FIGS. 3 and 4, the transfer substrate 21 has a so-called mesa structure having a base portion 22 and a convex structure portion 24 projecting from the periphery on one surface 22a of the base portion 22. The surface 24a of the convex structure portion 24 has an imprint region 23 in which a plurality of unit imprint regions 23A, 23B, 23C, and 23D are defined. Further, the surface 22b on the opposite side of the base portion 22 has a recessed portion 27 having a plan view shape having a wider area than the plan view shape of the convex structure portion 24 so as to include the convex structure portion 24. In FIG. 4, the peripheral edge of the recessed portion 27 is shown by a 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-walled portion 28. Further, in FIG. 4, the unit imprint areas 23A, 23B, 23C, and 23D are shown surrounded by chain lines, respectively. In the illustrated example, the imprint area 23 is composed of four unit imprint areas 23A, 23B, 23C, and 23D, but 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.

The transfer substrate 21 includes, for example, quartz glass, silicic acid-based glass, glass such as calcium fluoride, magnesium fluoride, and acrylic glass, sapphire and gallium nitride, and resin substrates such as polycarbonate, polystyrene, acrylic, and polypropylene, or Any of these laminated materials can be used. These materials have light transmission property, and are suitable when the transfer substrate 21 after forming the pattern structure according to the present invention is required to have light transmission property. Further, it may be a semiconductor such as silicon, gallium arsenide, 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 for a semiconductor or a display, a photonic crystal structure, an optical waveguide, or an optical structure such as holography may be formed.
Further, the transfer substrate 21 may have 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. Further, the transfer substrate 21 may not have the convex structure portion 24 protruding from the periphery on one surface 22a of the base portion 22.
Next, an embodiment of the method for manufacturing a pattern structure 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 one embodiment of the method for manufacturing the pattern structure of the present invention, and are shown in cross sections corresponding to FIGS. 2 and 4. The method for manufacturing the pattern structure of the present invention will be described below with reference to FIGS. 5 to 8.

<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 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). By pressurizing the transfer substrate 21, the thin portion 28 of the transfer substrate 21 is curved so that the convex structure 24 side has a convex shape (FIG. 5 (A)).
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 mechanical holding method, and an electrostatic adsorption holding method, and the substrate holding member 121 and the recessed portion 27 of the transfer substrate 21 Any space S formed by can be made liquid-tight or airtight. Further, the fluid supply / exhaust mechanism supplies 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 portion 28 of the transfer substrate 21, and also to bend the thin portion 28 of the transfer substrate 21. Anything can be used as long as it is possible to discharge the fluid from the transfer substrate 21 and flatten the thin portion 28 of the transfer substrate 21 to the original state.

In the supply step, the droplet 31 of the resin composition to be molded is supplied to the desired unit imprint region of the transfer substrate 21 (FIG. 5 (B)). In the illustrated example, the droplet 31 of the resin composition to be molded is supplied to the unit imprint region 23A. The droplet 31 can be supplied by ejecting the droplet from the inkjet head, supplying the droplet 31 from the dispenser, or the like.
The resin composition to be molded may be any as long as it has 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 cross-linking agent, and if necessary, a mold release agent for suppressing adhesion to the mold 11 and adhesion to the transfer substrate 21. It may contain an adhesive for improving the properties. Then, the resin composition to be molded can be appropriately selected according to the intended use, required properties, physical properties, etc. of the pattern structure to be manufactured. For example, if the application 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 application of the pattern structure is an optical member, a specific refractive index, Light transmission is required, and the 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. In addition, the viscosity, surface tension, etc. of the compatible liquid of the inkjet head differ depending on the structure, material, and the like. Therefore, it is preferable to appropriately adjust the viscosity, surface tension, etc. of the resin composition to be used, or to appropriately select an inkjet head suitable for the resin composition to be used.

Further, the number of droplets 31 of the resin composition to be molded supplied onto the unit imprint region 23A of the transfer substrate 21, the distance between adjacent droplets is the amount of individual droplets dropped, and the required resin to be molded. It can be appropriately set from the total amount of the composition, the wettability of the resin composition to be molded with respect to the transfer substrate 21, the size of the gap between the transfer substrate 21 and the mold 11 in the contact step which is a subsequent step, and the like.
After supplying the droplet 31 of the resin composition to be molded 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 into the 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) to pressurize the mold 11. As a result, the thin portion 18 of the mold 11 is curved so that the convex structure 14 side has a convex shape (FIG. 5 (C)).
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 mechanical holding method, and an electrostatic suction holding method, and is formed by the mold holding member 111 and the recessed portion 17 of the mold 11. Any space S'that can be made liquid-tight and airtight will be used. Further, the fluid supply / exhaust mechanism supplies fluid to the space S'formed by the mold holding member 111 and the recessed portion 17 of the mold 11 to bend the thin portion 18 of the mold 11 and also to bend this space S'. Anything can be used as long as it is possible to discharge the fluid from the mold 11 and flatten the thin portion 18 of the mold 11 to the original state.

In the contact step, the transfer substrate 21 in which the thin-walled portion 28 is curved so that the convex structure 24 side has a convex shape as described above, and the thin-walled portion 18 has a convex structure 14 side as described above. The mold 11 curved so as to be close to the mold 11. In the present invention, the proximity of the transfer substrate 21 and the mold 11 is measured 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, as shown in FIG. 6 (A). 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 concave-convex structure region 15 of the mold 11 coincide with each other. In FIG. 6A, the normal line N is shown by a solid line and the normal line N'is shown by a chain double-dashed 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 matches the normal line N'at the center C'of the uneven structure region 15 of the mold 11. Means that, in addition to the case where the normal N and the normal N'are completely matched, the case where there is a difference of 0.002 ° or less between the direction of the normal N and the direction of the normal N'. It is a concept to be included.
FIG. 9 is a partial plan view showing the imprint region 23 of the transfer substrate 21. In FIG. 9, in the imprint region 23 in which the four unit imprint regions 23A, 23B, 23C, and 23D are defined, the droplet 31 of the resin composition to be molded is supplied, and the mold 11 is close to the target. It shows the center C of the unit imprint areas 23A, 23B, 23C, and 23D. 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 outer shell of each unit imprint area. Similarly, the center C'of the concave-convex structure region 15 of the mold 11 can also be the center of gravity of the figure determined by the outer shell of the concave-convex structure region 15.

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

In the example shown in FIG. 6A, since the direction of the normal line N at the center C of the unit imprint area 23A of the transfer substrate 21 deviates from the vertical direction, the direction of the normal line N and the normal line N' The mold holding member 111 is operated so that the directions match. Further, for example, the substrate holding member 121 is operated so that the normal N at the center C of the unit imprint region 23A of the transfer substrate 21 in which the thin wall portion 28 is curved is set in the vertical direction, and then the center C of the concave-convex structure region 15 is set. The mold holding member 111 holding the mold 11 is operated so that the normal N ′ in ′ is in the vertical direction, and the mold 11 is brought close to the transfer substrate 21 so that the normal N and the normal N ′ match. You may let me.
By bringing the transfer substrate 21 and the mold 11 close to each other in this way, the resin composition to be molded is developed between the mold 11 and the unit imprint region 23A of the transfer substrate 21 to form the resin layer 32 to be molded ( FIG. 6 (B). In such proximity of the transfer substrate 21 and the mold 11, the position where the droplet 31 of the resin composition to be molded supplied to the unit imprint region 23A and the mold 11 first come into contact is the center of the unit imprint region 23A. As a result, the development of the resin composition to be molded in the unit imprint region 23A becomes uniform, and the thickness of the residual film portion (the portion existing in the gap between the mold 11 and the transfer substrate 21) in the resin layer 32 to be molded is formed. The distribution will be uniform.

Further, in the present embodiment, in the contacting step, after the transfer substrate 21 and the mold 11 are brought close to each other to form the resin layer 32 to be molded as described above, the normal line N at the center C of the unit imprint region 23A is displayed. While keeping the normal line N'at the center C'of the concave-convex structure region 15 of the mold 11 aligned, the thin portion 28 of the region where the recess 27 of the transfer substrate 21 exists is flattened, and the recess 17 of the mold 11 is formed. The thin portion 18 of the existing region is flattened (FIG. 7 (A)). 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 recessed portion 17 of the mold 11 by a fluid supply / discharge mechanism (not shown). Can be done. Similarly, the flattening of the thin portion 28 of the transfer substrate 21 is performed 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, since the direction of the normal line N at the center C of the unit imprint region 23A of the transfer substrate 21 deviates from the vertical direction, the flattening of the thin portion 28 of the transfer substrate 21 progresses. Along with this, the direction of the normal N changes so as to be the vertical direction. Therefore, while advancing the flattening of the thin portion 18 of the mold 11, the mold holding member 111 so that the normal N'at the center C'of the mold 11 coincides with the normal N at the center C of the unit imprint area 23A. To operate.

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

<Curing process>
Next, light irradiation is performed from the mold 11 side to cure the resin layer 32 to be molded to obtain a transfer resin layer 33 to which the uneven structure 16 of the mold 11 is transferred (FIG. 7 (B)). 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.
When the resin composition to be molded is a thermosetting resin, it can be cured by subjecting the resin layer 32 to be molded to heat treatment.

<Release process>
Next, in the mold release step, the transfer substrate 21 is provided with 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 concave-convex structure region 15 of the mold 11 being matched. The thin-walled portion 28 in the region where the recessed portion 27 exists is curved, and the thin-walled portion 18 in the region where the recessed portion 17 exists in the mold 11 is curved (FIG. 8 (A)). The curvature of the thin portion 18 of the mold 11 is formed by press-fitting the fluid into the 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). It can be carried out. Similarly, the curvature of the thin portion 28 of the transfer substrate 21 is such that a fluid is press-fitted into 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) to pressurize the transfer substrate 21. Can be done by In the example shown in FIG. 8A, the direction of the normal line N at the center C of the unit imprint region 23A of the transfer substrate 21 deviates from the vertical direction as the bending of the thin-walled portion 28 progresses. Therefore, while advancing the curvature of the thin portion 18 of the mold 11, the mold holding member 111 is set so that the normal N'at the center C'of the mold 11 coincides with the normal N at the center C of the unit imprint area 23A. Manipulate.

Next, the transfer resin layer 31 and the mold 11 are separated from each other so that the pattern structure 35, which is the transfer resin layer 33, is positioned on the unit imprint area 23A of the transfer substrate 21 (FIG. 8B). The thin-walled portion 18 of the mold 11 is curved as described above, and the thin-walled portion 28 of the transfer substrate 21 is curved, and then the transfer resin layer 31 and the mold 11 are separated from each other to separate the transfer resin layer 31 and the mold 11. It becomes easy to separate the region in contact with the outer peripheral side from the outer peripheral side, and it is possible to prevent the formation of defects in the formed pattern structure 35 and damage to the mold 11.
After that, the pattern structure 35 is sequentially formed in the other unit imprint areas 23B, 23C, 23D constituting the imprint area 23 by repeating the above supply step, contact step, curing step, and mold release step.
In such a method for manufacturing a pattern structure, a highly accurate pattern structure can be stably manufactured by multi-imposition on a transfer substrate having a recessed portion.

In the present invention, when the transfer substrate 21 has the hard mask material layer on the surface 22a of the base portion 22 and the surface 24a of the convex structure portion 24, all the units constituting the imprint region 23 as described above. After forming the pattern structure 35 on the hard mask material layer in the imprint areas 23A, 23B, 23C, 23D, the pattern structure is used as an etching mask at four unit imprint areas 23A, 23B, 23C, 23D. At the same time, the hard mask material layer can be etched. Further, the pattern structure 35 may be formed and the hard mask material layer using the pattern structure as an etching mask may be etched for each unit imprint region at one location.
Further, in the present invention, for example, the mold 11 used in the above-described embodiment is provided with alignment marks 51 at the four corners around the convex structure portion 14, as shown in FIG. 10, and the transfer substrate 11 is provided. , As shown in FIG. 11, an alignment mark 55 corresponding to each unit imprint area 23A, 23B, 23C, 23D may be provided around the convex structure portion 24. Then, in the contact step, in the imprint using the mold 11 for the desired unit imprint area, for example, the unit imprint area 23A shown in FIG. 11, the imprint is circled in the alignment mark 55 of the transfer substrate 21. 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 example, and the present invention is not limited to such an embodiment. For example, the mold 11 may not have the recessed portion 17. FIG. 12 is a diagram for explaining a contact process using the mold 11'which does not have such a recessed portion 17, and is a diagram corresponding 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 concave-convex structure region 15 of the mold 11' The operation of matching the normal N'at the center C'with the normal N at the center C of the unit imprint region 23A of the transfer substrate 21 needs to be performed in the same manner. As a result, the position where the droplet 31 of the resin composition to be molded supplied to the unit imprint region 23A and the mold 11'first come into contact with each other is at the center of the unit imprint region 23A. Therefore, the development of the resin composition to be molded in the unit imprint region 23A becomes uniform, and the thickness distribution of the residual film portion (the portion existing in the gap between the mold 11'and the transfer substrate 21) in the formed resin layer to be molded. It will be uniform.

Further, in the contacting step, after the transfer substrate 21 and the mold 11 are brought close to each other to form the resin layer 32 to be molded, the thin-walled portion 28 in the region where the recessed portion 27 of the transfer substrate 21 exists is flattened, and the mold 11 is recessed. Even when the thin-walled portion 18 in the region where the portion 17 exists is flattened, the thin-walled portion 18 of the mold 11 is not curved and the thin-walled portion 28 of the transfer substrate 21 is not curved in the mold release step. The resin layer 31 and the mold 11 may be separated from each other.

[Manufacturing method of 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 the line III-III of the mold shown in FIG. The mold 41 shown in FIGS. 13 and 14 has a base portion 42 and a convex structure portion 44 projecting from the periphery on one surface 42a of the base portion 42. On the surface 44a of the convex structure portion 44, a concavo-convex structure region 43 composed of four unit concavo-convex structure regions 43A, 43B, 43C, 43D is defined, and four unit concavo-convex structure regions 43A, 43B, 43C, The uneven structure 46 is located on the 43D. Further, the surface 42b on the opposite side of the base portion 42 has a recessed portion 47 having a plan-view shape having a wider area than the plan-view shape of the concave-convex structure region 43 so as to include the concave-convex structure region 43. In FIG. 13, the peripheral edge of the recessed portion 47 is shown by a alternate long and short dash line, and the concave-convex structure 46 is omitted. Further, in the illustrated example, the concavo-convex structure region 43 is composed of four unit concavo-convex structure regions 43A, 43B, 43C, and 43D, but the number and arrangement of the unit concavo-convex structure regions are not particularly limited.

Next, an example of the method for manufacturing the imprint mold of the present invention will be described by taking the manufacturing of the mold 41 as an example. FIG. 15 is a process diagram showing an embodiment of the method for manufacturing 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 on the surface 24a of the convex structure portion 24 is used as the mold manufacturing substrate 21'. Therefore, in the mold manufacturing substrate 21', the same member as the transfer substrate 21 is designated with the same member number. The four unit imprint areas 23A, 23B, 23C, 23D in the mold manufacturing substrate 21'are the four unit uneven structure regions 43A, 43B, 43C, 43D in the imprint mold 41. Further, the recessed portion 27 in the mold manufacturing substrate 21'is a recessed portion 47 in the imprint mold 41.
In the method for manufacturing an imprint mold of the present invention, four unit imprint regions 23A, 23B, 23C, on the hard mask material layer 29 of the mold manufacturing substrate 21'by the method for manufacturing a pattern structure of the present invention. A pattern structure 35, which is a resist pattern layer, is formed on 23D (FIG. 15 (A)).

Next, the hard mask material layer 29 is etched through the pattern structure 35 to form the hard mask 29'(FIG. 15B).
Next, the imprint mold 41 as shown in FIGS. 13 and 14 can be obtained by etching the mold manufacturing substrate 21'through the hard mask 29' to form the concave-convex structure 46. Since the mold manufacturing substrate 21'is etched at the same time in the four unit imprint regions 23A, 23B, 23C, and 23D using the formed hard mask 29'as a mask, the four unit uneven structure regions 43A , 43B, 43C, 43D have a uniform recess depth of the concave-convex structure 46.
In such a method for manufacturing an imprint mold of the present invention, it is possible to manufacture an imprint mold having a unit uneven structure region in which a concave-convex structure is located on multiple surfaces with high accuracy.
The above-described embodiment is an example, 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.

It can be used for various processes that require the formation of a pattern structure having a fine uneven structure on multiple surfaces, such as a replica mold used in the imprint method.

11 ... Mold 14 ... Convex structure part 15 ... Concavo-convex structure area 16 ... Concavo-convex structure 17 ... Recessed part 21 ... Transfer substrate 23 ... Imprint area 23A, 23B, 23C, 23D ... Unit imprint area 24 ... Convex structure part 27 ... Recessed part Part 31 ... Droplet 32 ... Resin layer to be molded 33 ... Transfer resin layer 35 ... Pattern structure 21'... Mold manufacturing substrate 29 ... Hard mask material layer 29' ... Hard mask 41 ... Imprint mold 43 ... Concavo-convex structure area 43A, 43B, 43C, 43D ... Unit uneven structure area 46 ... Concavo-convex structure 47 ... Recessed portion

Claims (12)

A recess having a unit imprint area on one surface and a plan view shape having an area wider than the plan view shape of the unit imprint area on the opposite surface is included in the unit imprint area. A supply step of supplying the resin composition to be molded to the unit imprint area of the transfer substrate using the transfer substrate having the transfer substrate.
A contact step of developing the resin composition to be molded between the mold and the transfer substrate by bringing the mold having the concave-convex structure and the transfer substrate close to each other in the concave-convex structure region to form a resin layer to be molded.
A curing step of curing the resin layer to be molded to form a transfer resin layer,
It has a mold release step of separating the transfer resin layer and the mold so that the pattern structure, which is the transfer resin layer, is positioned on the transfer substrate.
In a plan view from one surface side of the transfer substrate, the center of the unit imprint region does not coincide with the center of the region where the recess portion of the transfer substrate exists.
In the contact step, the region where the recessed portion of the transfer substrate exists is curved toward the mold side so as to have a convex shape, and is located at the center of the unit imprint region to which the resin composition to be molded is supplied. It is characterized in that the mold and the transfer substrate are brought close to each other in a state where the transfer substrate and / or the mold is inclined so that the normal and the normal at the center of the uneven structure region of the mold coincide with each other. A method for manufacturing a pattern structure. The transfer substrate has an imprint area composed of a plurality of the unit imprint areas, and the center of at least one unit imprint area of the plurality of unit imprint areas is a recessed portion of the transfer substrate. It does not coincide with the center of the existing region, the area of the recessed portion in the plan view is wider than the area of the imprinted region in the plan view , and the center of the region where the recessed portion of the transfer substrate exists. The production of the pattern structure according to claim 1, wherein the supply step, the contact step, the curing step, and the mold release step are performed on each unit imprint area having the center that does not match. Method. In the contact step, after the mold and the resin composition to be molded are brought into contact with each other, the normal at the center of the unit imprint region and the normal at the center of the concavo-convex structure region of the mold remain aligned. The method for manufacturing a pattern structure according to claim 1 or 2, wherein the region where the recessed portion of the transfer substrate exists is flattened. In the mold release step, the region where the recessed portion of the transfer substrate exists is defined while keeping the normal at the center of the unit imprint region and the normal at the center of the concave-convex structure region of the mold coincident with each other. The method for manufacturing a pattern structure according to claim 3, wherein the transfer resin layer and the mold are separated from each other after being curved so as to have a convex shape on the mold side. The mold has the concave-convex structure region in which the concave-convex structure is located on one surface, and the concave-convex portion having a plan-view shape having an area wider than the plan-view shape of the concave-convex structure region on the opposite surface. Have to include the structural area
In the contact step, the region where the recessed portion of the mold exists is curved toward the transfer substrate side so as to have a convex shape, and the normal at the center of the concave-convex structure region and the resin composition to be molded are formed. The pattern according to any one of claims 1 to 4, wherein the mold and the transfer substrate are brought close to each other so as to coincide with the normal at the center of the supplied unit imprint region. How to manufacture the structure. In the contact step, after the mold and the resin composition to be molded are brought into contact with each other, the normal at the center of the concave-convex structure region of the mold and the normal at the center of the unit imprint region remain aligned. The method for manufacturing a pattern structure according to claim 5, wherein the region where the recess portion of the mold exists is flattened, and the imprint region of the transfer substrate is flattened. In the mold release step, the region where the recessed portion of the mold exists is transferred while keeping the normal at the center of the concave-convex structure region of the mold and the normal at the center of the unit imprint region coincide with each other. It is curved so as to have a convex shape on the substrate side, and the region where the recess portion of the transfer substrate exists is curved so as to have a convex shape on the mold side, and then the transfer resin layer and the transfer resin layer and the said. The method for manufacturing a pattern structure according to claim 6, wherein the mold is separated. In the mold, the concave-convex structure region in which the concave-convex structure is located exists on the surface of the convex structure portion protruding from the periphery, and the area of the convex structure portion in the plan view is the plan view shape of the recessed portion. The method for manufacturing a pattern structure according to any one of claims 5 to 7, wherein the area is smaller than the area of. In the transfer substrate, the imprint region exists on the surface of the convex structure portion protruding from the periphery, and the area of the convex structure portion in the plan view is smaller than the area of the recess portion in the plan view. The method for manufacturing a pattern structure according to any one of claims 1 to 8, wherein the pattern structure is manufactured. The mold has a plurality of alignment marks located around the uneven structure region.
The transfer substrate has a plurality of alignment marks around the unit imprint area.
Any of claims 1 to 9, wherein in the contact step, alignment is performed using the plurality of alignment marks of the transfer substrate and the plurality of alignment marks of the mold. The method for manufacturing a pattern structure according to the above. A recess having a concavo-convex structure region consisting of a plurality of unit concavo-convex structure regions in which the concavo-convex structure is located is provided on one surface, and a recess having a plan-view shape having an area wider than the plan-view shape of the concavo-convex structure region is formed on the opposite surface. In the method for manufacturing 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 located at least in the imprint area, and has a plan view of the imprint area on the opposite surface. Claims 1 to 1 to use a mold manufacturing substrate having a recess portion having a plan view shape having a larger area than the shape so as to include the imprint region, on the hard mask material layer of each unit imprint region. A pattern structure which is a resist pattern layer is formed by the method for producing a pattern structure according to any one of claims 10.
A method for manufacturing an imprint mold, which comprises 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 exists on the surface of the convex structure portion protruding from the periphery, and the area of the convex structure portion in the plan view is larger than the area of the recess portion in the plan view. The method for manufacturing an imprint mold according to claim 11, wherein the size is also small.

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