WO2021219005A1 - 一种微纳结构的制备方法 - Google Patents

一种微纳结构的制备方法 Download PDF

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Publication number
WO2021219005A1
WO2021219005A1 PCT/CN2021/090554 CN2021090554W WO2021219005A1 WO 2021219005 A1 WO2021219005 A1 WO 2021219005A1 CN 2021090554 W CN2021090554 W CN 2021090554W WO 2021219005 A1 WO2021219005 A1 WO 2021219005A1
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Prior art keywords
micro
nano
fluid polymer
substrate
layer
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PCT/CN2021/090554
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English (en)
French (fr)
Inventor
罗先刚
郭迎辉
蒲明博
李雄
马晓亮
高平
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Institute of Optics and Electronics of CAS
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Institute of Optics and Electronics of CAS
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Priority to US17/997,102 priority Critical patent/US11675273B2/en
Priority to EP21795876.8A priority patent/EP4134743A4/en
Priority to JP2022551796A priority patent/JP7333676B2/ja
Publication of WO2021219005A1 publication Critical patent/WO2021219005A1/zh
Anticipated expiration legal-status Critical
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    • G—PHYSICS
    • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03F—PHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00—Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/0002—Lithographic processes using patterning methods other than those involving the exposure to radiation, e.g. by stamping
    • G—PHYSICS
    • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03F—PHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00—Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/70—Microphotolithographic exposure; Apparatus therefor
    • G03F7/70425—Imaging strategies, e.g. for increasing throughput or resolution, printing product fields larger than the image field or compensating lithography- or non-lithography errors, e.g. proximity correction, mix-and-match, stitching or double patterning
    • G03F7/70433—Layout for increasing efficiency or for compensating imaging errors, e.g. layout of exposure fields for reducing focus errors; Use of mask features for increasing efficiency or for compensating imaging errors
    • G—PHYSICS
    • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03F—PHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00—Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/16—Coating processes; Apparatus therefor
    • G03F7/162—Coating on a rotating support, e.g. using a whirler or a spinner
    • G—PHYSICS
    • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03F—PHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00—Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/16—Coating processes; Apparatus therefor
    • G03F7/168—Finishing the coated layer, e.g. drying, baking, soaking
    • G—PHYSICS
    • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03F—PHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00—Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/70—Microphotolithographic exposure; Apparatus therefor
    • G03F7/70216—Mask projection systems
    • G03F7/7035—Proximity or contact printers

Definitions

  • the present disclosure relates to the technical field of micro-nano manufacturing, in particular to a method for preparing a micro-nano structure.
  • micro-nano manufacturing technologies are mainly divided into three categories: direct writing, photolithography and imprinting.
  • the direct-write micro-nano manufacturing technology has high resolution, its processing efficiency is low, and it is not suitable for mass production.
  • Lithography-type micro-nano manufacturing technology has strong technical advantages in terms of efficiency, material and process compatibility, but due to the theoretical limitation of the Rayleigh criterion, to improve the exposure resolution, shorter exposure wavelengths and higher exposure wavelengths are required.
  • the numerical aperture of the objective lens but the continuous reduction of the exposure wavelength and the increase of the objective lens numerical aperture are accompanied by a continuous surge in cost.
  • Imprinting micro-nano manufacturing technology is a low-cost processing technology developed in recent years.
  • the shape and quality of the graphics are directly determined by the stamper, so the processing resolution has no physical limits and proximity effects; but due to high The manufacturing cost of the resolving stamper is high, and the copied pattern has many defects, the alignment and over-engraving accuracy is not high, and the multi-layer micro-nano structure pattern cannot be processed, which restricts its large-scale popularization and application.
  • the present disclosure provides a method for manufacturing a micro-nano structure, which is used to at least partially solve the technical problems of the traditional micro-nano manufacturing method such as low processing efficiency, high manufacturing cost, and many pattern defects.
  • One aspect of the present disclosure provides a method for preparing a micro-nano structure, which includes: forming a reflective layer and a fluid polymer layer on the surface of a substrate; The material layer is squeezed into the light-transmitting area of the mask, and the fluid polymer layer is cured; exposing, the fluid polymer in the light-transmitting area is sensitized under the combined action of the transmitted light and the reflected light of the reflective layer to obtain a micro-nano structure.
  • press-fitting the substrate and the reticle with micro-nano patterns includes: press-fitting the substrate and the reticle with micro-nano patterns through precise pressure transfer, so that the fluid polymer layer is evenly pressed into the mask.
  • the light-transmitting area of the template includes: press-fitting the substrate and the reticle with micro-nano patterns through precise pressure transfer, so that the fluid polymer layer is evenly pressed into the mask. The light-transmitting area of the template.
  • the precision pressure transmission methods include piston mechanical transmission, piezoelectric actuator transmission, air film transmission, and air pressure transmission.
  • the pressure bonding of the substrate and the reticle with micro-nano graphics also includes: leveling and contacting the substrate with the reticle with micro-nano graphics.
  • curing the fluid polymer in the light-transmitting area further includes: placing the substrate in a developing solution for development, and removing the fluid polymer that has not been photocured to obtain a micro-nano structure.
  • the micro-nano pattern of the mask plate also includes an anti-adhesion layer, and the material of the anti-adhesion layer includes diamond-like carbon film and fluorine-doped silane.
  • the fluid polymer layer is a high-resolution fluid polymer material, including fluorine-doped silicon-based copolymers or derivatives, vinyl ether-based copolymers, acrylic-based copolymers, calixarene-based molecular glass, and high acidolytic activity Acetal polymer, poly(p-hydroxystyrene-based copolymer).
  • the method for forming the reflective layer on the surface of the substrate includes molecular beam epitaxy combined with low-temperature annealing, co-sputtering, and high-temperature sputtering.
  • forming a fluid polymer layer on the surface of the substrate includes spin coating the fluid polymer on the surface of the reflective layer to form a fluid polymer layer.
  • the reflective layer includes a low-loss silver reflective layer and a low-loss aluminum reflective layer.
  • Step 1 Deposit a low-loss reflective layer on the surface of the substrate;
  • Step 2. The fluid polymer material is spin-coated on the surface of the reflective layer;
  • step 3, an anti-adhesion layer is made on the surface of the micro-nano mask;
  • step 4 a high-resolution fluid polymer material is spin-coated on the surface of the reflective layer through a mechanical device
  • the substrate and the micro-nano mask pattern surface are leveled and contacted;
  • step 5 the high-resolution fluid polymer material surface is squeezed into the light-transmitting area of the mask pattern by a precision pressure transfer method;
  • step 6 exposure, in Under the action of the reflective layer, the light field passing through the reticle pattern is localized in the light-transmitting area, and the local fluid polymer material extruded into the light-transmitting area of the reticle pattern and between the reflective layer is sensitized and cured;
  • step 7 After
  • the low-loss reflective layer preparation method in step 1 is molecular beam epitaxy combined with low-temperature annealing, co-sputtering, and high-temperature sputtering.
  • the high-resolution fluid polymer material in step 2 is fluorine-doped silicon-based copolymers or derivatives, vinyl ether-based copolymers, acrylic acid-based copolymers, calixarene-based molecular glass, and high acidolytic activity acetal polymers , Poly-p-hydroxystyrene-based copolymer.
  • the anti-adhesion layer is a diamond-like carbon film and fluorine-doped silane.
  • the precision pressure transmission method in step 5 is piston mechanical transmission, piezoelectric actuator transmission, air film transmission, and air pressure transmission.
  • the pressure transmission method in step 5 includes piston mechanical transmission, piezoelectric actuator transmission, air film transmission, and air pressure transmission.
  • Fig. 1 schematically shows a schematic flow chart of a method for preparing a micro-nano structure according to an embodiment of the present disclosure
  • Fig. 2 schematically shows a schematic diagram of the preparation of a micro-nano structure according to an embodiment of the present disclosure
  • FIG. 3 schematically shows a schematic diagram of a cross-sectional structure after depositing a reflective layer on the surface of a substrate and spin-coating a fluid polymer material according to an embodiment of the present disclosure
  • FIG. 4 schematically shows a cross-sectional structure diagram after an anti-adhesion layer is fabricated on the surface of a mask according to an embodiment of the present disclosure
  • FIG. 5 schematically shows a cross-sectional structure diagram of a substrate spin-coated with a fluid polymer material on the surface of a reflective layer and a micro-nano mask pattern surface after leveling and contacting according to an embodiment of the present disclosure
  • FIG. 6 schematically shows a cross-sectional structure diagram after a shallow layer of a fluid polymer material surface is extruded into a light-transmitting area of a reticle pattern according to an embodiment of the present disclosure
  • Fig. 7 schematically shows a cross-sectional structure diagram of demolding after exposure is completed according to an embodiment of the present disclosure
  • FIG. 8 schematically shows a schematic cross-sectional structure diagram of a pattern after development after development according to an embodiment of the present disclosure
  • the embodiment of the present disclosure provides a method for preparing a micro-nano structure, forming a reflective layer on a substrate, and adopting a shallow pressure combined exposure method, and a method for manufacturing a micro-nano photoprint based on a reflective light field enhancement is proposed.
  • the solution provides technical support for the solution of the aforementioned problems.
  • Fig. 1 schematically shows a flow chart of a method for preparing a micro-nano structure according to an embodiment of the present disclosure.
  • Fig. 2 schematically shows a schematic diagram of a manufacturing method of a micro-nano structure according to an embodiment of the present disclosure.
  • a low-loss reflective layer 7 is deposited on the surface of the substrate 8; then a high-resolution fluid polymer material is spin-coated on the surface of the reflective layer 7, see FIG. 3.
  • the reflective layer 7 can reflect the transmitted ultraviolet light to make the fluid polymer 6 in the transmission area sensitive to reduce the transmission loss of the evanescent wave, improve the processing resolution, and do not need to shorten the exposure wavelength And increase the numerical aperture of the objective lens, reducing the production cost.
  • the fluid polymer material in the fluid polymer layer 6 has a high resolution and is suitable for preparing micro-nano structures.
  • FIG. 4 is a schematic diagram of a cross-sectional structure of a mask 2 with a micro-nano pattern.
  • the imprinting process is to squeeze the imprinting glue into the template, and then form the pattern through thermal curing or ultraviolet curing.
  • the depth of the pattern is determined by the stamping mold, so The manufacturing difficulty and cost are relatively high; while the present disclosure adopts a shallow pressure combined exposure method, and the depth of the pattern is mainly determined by the depth of exposure, which reduces the difficulty and cost of mask processing.
  • the embossing pattern needs to ensure a certain aspect ratio, the pattern structure will inevitably be separated from the middle stamper due to stress during the demolding process, resulting in pattern defects; while this method squeezes the pattern into the mask
  • the depth is relatively shallow, mainly through exposure to increase the depth of the graphics, thus greatly reducing the graphics defects.
  • pressing the fluid polymer layer 6 into the light-transmitting area 5 of the reticle by means of pressure does not make the fluid polymer layer 6 completely fill the entire light-transmitting area 5, but partially fill the reticle.
  • the light-transmitting area 5 there is still a certain gap between the fluid polymer layer 6 and the substrate of the mask 2 after extrusion. The manufacturing cost of the die is reduced.
  • the depth of the pattern extruded into the mask is shallow, the pattern defects caused by uneven force during the separation process of the stamper and the substrate 8 are reduced.
  • the fluid polymer in the light-transmitting area is exposed to light under the combined action of the transmitted light and the reflected light of the reflective layer to obtain a micro-nano structure.
  • FIG. 8 is a schematic diagram of the cross-sectional structure of the copied pattern after development, that is, the cross-sectional view of the obtained micro-nano structure.
  • pressing and bonding the substrate 8 and the reticle 2 with micro-nano patterns includes: pressing and bonding the substrate 8 and the reticle 2 with micro-nano patterns through precise pressure transfer to make The fluid polymer layer 6 is evenly pressed into the light-transmitting area 5 of the mask.
  • the fluid polymer layer 6 can be evenly pressed into the light-transmitting area 5, and the depth Controllable.
  • the precision pressure transmission methods include piston mechanical transmission, piezoelectric actuator transmission, and gas film Transmission, air pressure transmission.
  • Piezoelectric actuator transmission is pressure transmission based on the piezoelectric effect.
  • the diaphragm transmits the measured pressure to the piezoelectric element, and then the piezoelectric element outputs an electrical signal that has a certain relationship with the measured pressure, thereby precisely controlling the base
  • the pressure exerted by the sheet Air film transfer is when the pressure inside the air film is greater than the outside pressure of the air film, a certain pressure difference is generated, and the gas in the air film can support the film material to exert pressure on the substrate.
  • the air pressure transfer is achieved by compressing the gas to increase the pressure and apply pressure to the substrate.
  • the above methods can control the size of the pressure applied to the substrate, and the applied pressure is evenly distributed on the surface of the substrate, so as to achieve precise control of the depth of the extrusion, and finally make the micro-nano structure obtained with high resolution.
  • the substrate 8 and the reticle 2 with micro-nano patterns before pressing and bonding the substrate 8 and the reticle 2 with micro-nano patterns, it further includes: leveling and contacting the substrate 8 and the reticle 2 with micro-nano patterns.
  • the substrate 8 spin-coated with high-resolution fluid polymer material on the surface of the reflective layer 7 needs to be leveled and contacted with the pattern surface of the micro-nano mask through a mechanical device. Please refer to Figure 5 to avoid Because of the uneven contact surface, the depth of the fluid polymer 6 pressed into it is uneven, which brings about the problem of pattern defects.
  • curing the fluid polymer in the light-transmitting area further includes: placing the substrate 8 in a developing solution for development, and removing the fluid polymer that is not photocured to obtain a micro-nano structure.
  • Figure 7 is a schematic diagram of the cross-sectional structure of demolding after the exposure is completed.
  • the substrate is placed in a developer for development, and the non-sensitized and cured polymer materials are removed.
  • the non-sensitized and cured materials are mainly located in the mask pattern area 3 and Between the reflective layers 7, that is, the pattern area of the reticle is copied to the substrate 8, the pattern left is the light-transmitting area of the reticle 2, and finally the copied pattern is obtained on the substrate, and the pattern is realized from the reticle 2.
  • Figure 8 is a schematic diagram of the cross-sectional structure of the copied pattern after development.
  • the micro-nano pattern 3 of the mask 2 further includes an anti-adhesion layer 4, and the material of the anti-adhesion layer 4 includes diamond-like carbon film and fluorine-doped silane.
  • FIG. 4 is a schematic diagram of a cross-sectional structure after the anti-adhesion layer 4 is fabricated on the surface of the micro-nano mask.
  • the diamond-like carbon film has both the excellent characteristics of diamond and graphite.
  • the diamond-like carbon film is used as the anti-adhesion layer because of its high hardness and good optical transparency, which makes it difficult to bond with the fluid polymer layer 6 and does not Affect the subsequent exposure process. Since the fluorine-containing polysiloxane has low surface energy, solvent resistance, flexibility, high and low temperature resistance, and has good hydrophobic, oleophobic and anti-fouling properties, it can improve the anti-sticking performance of the mask 2.
  • the fluid polymer layer 6 is a high-resolution fluid polymer material, including fluorine-doped silicon-based copolymers or derivatives, vinyl ether-based copolymers, acrylic-based copolymers, calixarene-based molecules Glass, high acid hydrolysis activity acetal polymer, poly(p-hydroxystyrene-based copolymer).
  • fluid polymer materials usually have certain requirements for material properties. For example, including resolution less than 100 nanometers, viscosity less than 5 ⁇ 10-3Pa ⁇ s, molecular weight less than 40, contrast greater than 4, etc., fluorine-doped silicon-based copolymers or derivatives, vinyl ether-based copolymers, acrylic-based copolymers, Calixarene-based molecular glass, high acidolytic activity acetal polymer, poly(p-hydroxystyrene-based copolymer) and other materials can be used to prepare the fluid polymer layer 6 of the present disclosure.
  • the method for forming the reflective layer 7 on the surface of the substrate 8 includes molecular beam epitaxy combined with low-temperature annealing, co-sputtering, and high-temperature sputtering.
  • the material of the reflective layer 7 is usually metal or alloy metal, and deposition is mainly achieved by vacuum coating and sputtering.
  • Molecular beam epitaxy can prepare single crystal films as thin as dozens of atomic layers, with high growth quality and easy to obtain high-quality reflective layer 7.
  • Sputtering has the advantages of easy control, large coating area and strong adhesion, and it is also easy to obtain a high-quality reflective layer 7.
  • forming the fluid polymer layer 6 on the surface of the substrate 8 includes spin coating the fluid polymer on the surface of the reflective layer 7 to form a fluid polymer layer.
  • the main advantage of spin coating is that it is easy to obtain a denser coating, and the thickness of the coating is relatively uniform.
  • the method of spin coating the fluid polymer layer 6 is mainly to obtain a coating of uniform thickness to ensure the depth of the subsequent extrusion fluid. Unanimous.
  • the reflective layer 7 includes a low-loss silver reflective layer and a low-loss aluminum reflective layer.
  • the materials used here for the reflective layer include silver, silver alloys (such as Ag-Pd alloy), aluminum, and aluminum alloys (such as Al-Ti alloy). These materials all exhibit high reflectivity and can minimize evanescent waves. The transmission loss improves the processing resolution.
  • a uniform monomolecular anti-adhesive layer is formed on the surface of the 200nm line width resolution chromium mask by heating and evaporation.
  • a passive leveling mechanical structure is used to level and contact the spin-coated substrate with high-resolution fluid polymer material and the chromium mask pattern surface with a line width resolution of 200 nm.
  • step S3 After the exposure is completed, separate the substrate from the mask to achieve demolding; put the substrate in the developer solution and develop it for 20 seconds at 22°C to remove the unsensitized and cured polymer material to obtain 200nm
  • the resolution and 300nm depth photoprint pattern is equivalent to the aforementioned step S3.
  • a silicon wafer with a thickness of 0.21 mm is selected as the substrate; a coating method of aluminum and copper co-sputtering is used to deposit a 60-nm-thick low-loss aluminum reflective layer on the surface of the substrate.
  • a uniform monomolecular anti-adhesive layer is formed on the surface of the molybdenum mask with 30nm line width resolution by heating and evaporation.
  • a three-point active leveling system is used to level and contact the spin-coated substrate with high-resolution fluid polymer material and the molybdenum mask pattern surface with a line width resolution of 30 nm.
  • the leveling process monitors and adjusts the three-point gap value in real time.
  • a pressure of 200N is applied to the back of the substrate through the piezoelectric actuator, and the surface of the high-resolution fluid polymer material with a thickness of 20nm is extruded into the light-transmitting area of the reticle pattern and heated and cured, which is equivalent to the aforementioned step S2.
  • the present disclosure also needs to use the direct writing method to make the mask, but the micro-nano structure can be copied in batches at low cost through the mask, and the processing efficiency is much higher than that of the traditional direct writing Micro-nano-like manufacturing technology: Compared with traditional lithography-like micro-nano manufacturing technology, this method solves the problem of limited diffraction, reduces the transmission loss of evanescent waves through reflective optical field enhancement, and improves the processing resolution. Shorten the exposure wavelength and increase the numerical aperture of the objective lens. Compared with the traditional imprinting micro-nano manufacturing technology, the imprinting process is to squeeze the imprinting glue into the template, and then heat or UV cure to form a pattern.
  • the depth is determined by the stamper, so the manufacturing difficulty and cost of the stamper are relatively high; and this method uses a combination of shallow pressure and exposure, and the depth of the pattern is mainly determined by the depth of exposure, which reduces the difficulty and cost of mask processing;
  • the embossing pattern needs to ensure a certain aspect ratio.
  • the pattern structure is inevitably separated from the middle stamper due to stress, causing pattern defects; while the depth of the pattern squeezed into the mask by this method is relatively low. Shallow, mainly through exposure to increase the depth of the graphics, thus greatly reducing the graphics defects.

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Abstract

一种微纳结构的制备方法，包括：在基片（8）表面依次形成反射层（7）、流体聚合物层（6）；将基片（8）与带微纳图形的掩模版（2）加压贴合，使流体聚合物层（6）挤压进入掩模版（2）的透光区（5），并使流体聚合物层（6）固化；曝光，在透射光以及反射层（7）反射光的共同作用下使透光区（5）的流体聚合物感光，得到微纳结构。这种方法解决了衍射受限的问题，通过反射式光场增强降低倏逝波的传输损耗，提高了加工分辨力，采用浅压结合曝光的方法，降低了掩模加工难度及成本，也降低了图形缺陷。

Description

一种微纳结构的制备方法
本公开要求于2020年04月29日提交的、申请号为202010354559.X的中国专利申请的优先权，其全部内容通过引用结合在本公开中。
技术领域
本公开涉及微纳米制造技术领域，具体涉及一种微纳结构的制备方法。
背景技术
近年来，大量的研究报道表明具有微纳米特征尺度的人工结构可以极大的增强微纳光子器件、微纳电子器件、微纳机电系统、微纳米能源及显示器件的性能。而作为这些微纳米尺度结构和器件制造的基础，低成本、高分辨力、高产出、大面积的新型纳米加工技术/方法的需求极为迫切。
传统微纳制造技术主要分为三类：直写类、光刻类和压印类。直写类微纳制造技术虽然具有高的分辨力，但加工效率较低，不适用于大规模批量生产。光刻类微纳制造技术在效率、材料和工艺的兼容性等方面具有较强的技术优势，但受瑞利准则的理论限制，要提高曝光分辨力，需要采用更短的曝光波长和更高数值孔径的物镜，但是不断的缩小曝光波长及提高物镜数值孔径伴随着的是成本的不断激增。压印类微纳制造技术是近年来发展到一种低成本的加工技术，由于不涉及曝光过程，图形形状和质量直接由压模决定，因此加工分辨力没有物理极限及邻近效应；但由于高分辨力的压模制造成本高昂，且复制图形存在缺陷多，对准和套刻精度不高，不能加工多层微纳结构图形，制约了其大规模推广应用。
发明内容
(一)要解决的技术问题
针对上述问题，本公开提供了一种微纳结构的制备方法，用于至少部分解决传统微纳制造方法加工效率较低、制造成本高、图形缺陷多等技术问题。
(二)技术方案
本公开一方面提供了一种微纳结构的制备方法，包括：在基片表面依次形成反射层、流体聚合物层；将基片与带微纳图形的掩模版加压贴合，使流体聚合物层挤压进入掩模版的透光区，并使流体聚合物层固化；曝光，在透射光以及反射层反射光的共同作用下使透光区的流体聚合物感光，得到微纳结构。
进一步地，将基片与带微纳图形的掩模版加压贴合包括：通过精密压力传递将基片与带微纳图形的掩模版加压贴合，使流体聚合物层均匀受压进入掩模版的透光区。
进一步地，通过精密压力传递将基片与带微纳图形的掩模版加压贴合中，精密压力传递的方法包括活塞类机械传递、压电执行机构传递、气膜传递、气压传递。
进一步地，将基片与带微纳图形的掩模版加压贴合之前还包括：将基片与带微纳图形的掩模版调平并接触。
进一步地，使透光区的流体聚合物固化还包括：将基片置于显影液中显影，去除未感光固化的流体聚合物，得到微纳结构。
进一步地，掩模版的微纳图形上还包括一层抗粘接层，抗粘接层的材料包括类金刚石薄膜、掺氟硅烷。
进一步地，流体聚合物层为高分辨力的流体聚合物材料，包括氟掺杂硅基共聚物或衍生物、乙烯醚基共聚物、丙烯酸基共聚物、杯芳烃基分子玻璃、高酸解活性缩醛聚合物、聚对羟基苯乙烯基共聚物。
进一步地，在基片表面形成反射层的方法包括分子束外延结合低温退火、共溅射、高温溅射法。
进一步地，在基片表面形成流体聚合物层包括将流体聚合物旋涂在 反射层表面，形成流体聚合物层。
进一步地，反射层包括低损耗银反射层、低损耗铝反射层。
本公开另一方面提供了一种基于反射式光场增强的微纳光印制造方法，步骤如下：步骤1、在基片表面沉积一层低损耗的反射层；步骤2、将高分辨力的流体聚合物材料旋涂在反射层表面；步骤3、在微纳米掩模版表面制作一层抗粘接层；步骤4、通过机械装置将在反射层表面旋涂有高分辨力流体聚合物材料的基片与微纳米掩模版图形面调平并接触；步骤5、通过精密压力传递方法将高分辨力的流体聚合物材料表面浅层挤压进入掩模版图形透光区；步骤6、曝光，在反射层的作用下使穿过掩模版图形的光场局域在透光区，使挤压进入掩模版图形透光区及到反射层之间的局部流体聚合物材料感光及固化；步骤7、脱模后将基片放入显影液中显影，去掉未感光及固化的聚合物材料，得到复制后的图形。
进一步地，步骤1中低损耗的反射层制备方法为分子束外延结合低温退火、共溅射、高温溅射法。
进一步地，步骤2中高分辨力的流体聚合物材料为氟掺杂硅基共聚物或衍生物、乙烯醚基共聚物、丙烯酸基共聚物、杯芳烃基分子玻璃、高酸解活性缩醛聚合物、聚对羟基苯乙烯基共聚物。
进一步地，步骤3中抗粘接层为类金刚石薄膜、掺氟硅烷。
进一步地，步骤5中精密压力传递方法为活塞类机械传递、压电执行机构传递、气膜传递、气压传递。
进一步地，步骤5中压力传递方法为活塞类机械传递、压电执行机构传递、气膜传递、气压传递。
(三)有益效果
本公开实施例提供的一种微纳结构的制备方法，通过反射式光场增强降低倏逝波的传输损耗，提高了加工分辨力，解决了衍射受限的问题；采用浅压结合曝光的方法，图形的深度主要由曝光的深度决定，降低了掩模加工难度及成本，同时挤压进入掩模的图形深度较浅，主要通过曝光提高图形的深度，因而极大程度的降低了图形缺陷。
附图说明
图1示意性示出了根据本公开实施例中微纳结构制备方法的流程示意图；
图2示意性示出了根据本公开实施例中微纳结构的制备示意图；
图3示意性示出了根据本公开实施例在基片表面沉积反射层并旋涂流体聚合物材料后的剖面结构示意图；
图4示意性示出了根据本公开实施例在掩模版表面制作抗粘接层后的剖面结构示意图；
图5示意性示出了根据本公开实施例将在反射层表面旋涂有流体聚合物材料的基片与微纳米掩模版图形面调平并接触后的剖面结构示意图；
图6示意性示出了根据本公开实施例将流体聚合物材料表面浅层挤压进入掩模版图形透光区后的剖面结构示意图；
图7示意性示出了根据本公开实施例曝光完成后脱模的剖面结构示意图；
图8示意性示出了根据本公开实施例显影后得到复制后的图形剖面结构示意图；
附图标记说明：
1 紫外照明光源；
2 掩模版；
3 微纳图形；
4 抗粘接层；
5 透光区；
6 流体聚合物层；
7 反射层；
8 基片。
具体实施方式
为使本公开的目的、技术方案和优点更加清楚明白，以下结合具体实施例，并参照附图，对本公开进一步详细说明。
本公开的实施例提供了一种微纳结构的制备方法，于基底上形成一层反射层，并采用浅压结合曝光的方法，提出了基于反射式光场增强的微纳光印制造方法的方案，对于前文问题的解决，提供了技术支撑。
图1示意性示出了根据本公开实施例中微纳结构的制备方法的流程图。
S1，在基片8表面依次形成反射层7、流体聚合物层6。
图2示意性示出了根据本公开实施例中微纳结构的制造方法示意图。在基片8表面沉积一层低损耗的反射层7；再将高分辨率的流体聚合物材料旋涂在反射层7表面，请参见图3。在进行紫外光曝光时，反射层7可将透射过来的紫外光进行反射，使透射区域的流体聚合物6感光，以降低倏逝波的传输损耗，提高了加工分辨力，不需要缩短曝光波长和提高物镜的数值孔径，降低了生产成本。流体聚合物层6中的流体聚合物材料具有高分辨率，适合用于制备微纳结构。
S2，将基片8与带微纳图形的掩模版2加压贴合，使流体聚合物层6挤压进入掩模版的透光区5，并使流体聚合物层6固化。
图4为带微纳图形的掩模版2的剖面结构示意图。相比于传统的压印类微纳制造技术，压印过程中是将压印胶挤压进入模板中，再通过热固化或紫外固化形成图形，图形的深度由压模决定，因而压模的制造难度及成本较高；而本公开是采用浅压结合曝光的方法，图形的深度主要由曝光的深度决定，降低了掩模加工难度及成本。其次由于压印图形需要保证一定的深宽比，在脱模的过程中图形结构不可避免的由于受力原因，未中压模上分离，造成图形缺陷；而本方法挤压进入掩模的图形深度较浅，主要通过曝光提高图形的深度，因而极大程度的降低了图形缺陷。
需要说明的是，这里通过加压的方式使流体聚合物层6挤压进入掩模版的透光区5并不是使流体聚合物层6完全填充整个透光区5，而是 部分填充掩模版的透光区5，挤压之后流体聚合物层6与掩模版2的基底之间还存在一定间隙，请参见图6，通过该浅压的方式降低了对压模的高分辨率的要求，降低了压模的制造成本。同时，由于挤压进入掩模的图形深度较浅，降低了由于压模和基片8分离过程中由于受力不均匀而造成的图形缺陷。
S3，曝光，在透射光以及反射层反射光的共同作用下使透光区的流体聚合物感光，得到微纳结构。
在掩模版2上方使用紫外照明光源进行曝光，掩模版2上的掩模图形区3不透光，无掩模图形3的区域为透光区5，光束穿透该透光区对该透光区中的流体聚合物层6进行感光，同时还有一部分光经过基片8上的反射层7进行反射，并使靠近反射层7的流体聚合物层6也进行感光，图2中的5为模拟得到的局域光场，类似于沙漏型，通过该反射层7的使用强降了低倏逝波的传输损耗，提高了加工分辨力。图8为显影后得到复制后的图形剖面结构示意图，即得到的微纳结构的剖面图。
在上述实施例的基础上，将基片8与带微纳图形的掩模版2加压贴合包括：通过精密压力传递将基片8与带微纳图形的掩模版2加压贴合，使流体聚合物层6均匀受压进入掩模版的透光区5。
为了使得流体聚合物材料表面浅层挤压进入掩模版图形透光区，需要精确控制挤压的深度，通过压力传递的方式可以使得流体聚合物层6均匀受压进入透光区5，且深度可控。
在上述实施例的基础上，通过精密压力传递将基片8与带微纳图形的掩模版2加压贴合中，精密压力传递的方法包括活塞类机械传递、压电执行机构传递、气膜传递、气压传递。
活塞类机械传递通过活塞单元沿着缸筒往复移动，通过精密控制将压力传导至基片8上，从而与掩模版2加压贴合。压电执行机构传递是基于压电效应的压力传递，由膜片将被测压力传递给压电元件，再由压电元件输出与被测压力成一定关系的电信号，由此精密控制对基片施加的压力。气膜传递是当气膜内压力大于气膜外压力时，就产生一定的气压差，气膜内气体就能将膜材支撑起来对基片施加压力。气压传递是通 过压缩气体实现压强变大，对基片施加压力。以上方式均可控制对基片施加压力的大小，且施加的压力均匀分布于基片表面，实现对挤压的深度精确控制，最终使得到的微纳结构具有高分辨率。
在上述实施例的基础上，将基片8与带微纳图形的掩模版2加压贴合之前还包括：将基片8与带微纳图形的掩模版2调平并接触。
在加压贴合之前，还需要通过机械装置将在反射层7表面旋涂有高分辨力流体聚合物材料的基片8与微纳米掩模版图形面调平并接触，请参见图5，避免因为接触面不平造成的压入流体聚合物6的深度不均一，而带来图形的缺陷问题。
在上述实施例的基础上，使透光区的流体聚合物固化还包括：将基片8置于显影液中显影，去除未感光固化的流体聚合物，得到微纳结构。
图7为曝光完成后脱模的剖面结构示意图，脱模后将基片放入显影液中显影，去掉未感光及固化的聚合物材料，未感光及固化的材料主要位于掩模图形区3和反射层7之间，即掩模版图形区则复制到了基片8，留下的图形即为掩模版2的透光区，最终在基片上得到复制后的图形，实现了图形从掩模版2上的转移，图8为显影后得到复制后的图形剖面结构示意图。
在上述实施例的基础上，将掩模版2的微纳图形3上还包括一层抗粘接层4，抗粘接层4的材料包括类金刚石薄膜、掺氟硅烷。
图4为在微纳米掩模版表面制作抗粘接层4后的剖面结构示意图。类金刚石薄膜兼具了金刚石和石墨的优良特性，这里使用类金刚石薄膜作为抗粘接层，是因为其具有高硬度、良好的光学透明性，使之与流体聚合物层6不易黏结，且不影响后续的曝光过程。由于含氟聚硅氧烷具有低表面能、耐溶剂性、柔顺性、耐高低温性，具有良好的疏水疏油及抗污性，可以提高掩模版2的抗粘性能。
在上述实施例的基础上，流体聚合物层6为高分辨力的流体聚合物材料，包括氟掺杂硅基共聚物或衍生物、乙烯醚基共聚物、丙烯酸基共聚物、杯芳烃基分子玻璃、高酸解活性缩醛聚合物、聚对羟基苯乙烯基共聚物。
为了制备高分辨力的微纳结构，流体聚合物材料通常对材料性能有一定要求。例如包括分辨率小于100纳米，粘度小于5×10-3Pa·s，分子量小于40，对比度大于4等等，氟掺杂硅基共聚物或衍生物、乙烯醚基共聚物、丙烯酸基共聚物、杯芳烃基分子玻璃、高酸解活性缩醛聚合物、聚对羟基苯乙烯基共聚物等等材料可用来制备本公开的流体聚合物层6。
在上述实施例的基础上，在基片8表面形成反射层7的方法包括分子束外延结合低温退火、共溅射、高温溅射法。
反射层7的材料通常为金属或者是合金金属，主要通过真空镀膜、溅射的方式来实现沉积。分子束外延可以制备薄到几十个原子层的单晶薄膜，生长质量高，易于得到高质量的反射层7。溅射具有易于控制、镀膜面积大和附着力强等优点，也易于得到高质量的反射层7。
在上述实施例的基础上，在基片8表面形成流体聚合物层6包括将流体聚合物旋涂在反射层7表面，形成流体聚合物层。
旋涂的主要优点是易于获得密度较大的涂层，涂层厚度比较均匀，这里采用旋涂流体聚合物层6的方式主要是为了获得厚度均匀的涂层，以保证后续挤压流体的深度一致。
在上述实施例的基础上，反射层7包括低损耗银反射层、低损耗铝反射层。
这里用于反射层的材料有银、银合金(如Ag-Pd合金)、铝、铝合金(如Al-Ti合金)，该类材料均表现出高反射率，能最大限度地减少倏逝波的传输损耗，提高了加工分辨力。
下面以两个具体实施例对本公开进行详细描述。
实施例1
制作200nm线宽分辨力、300nm深度的光印图形，其具体的制作过程如下：
(1)选择厚度为0.35mm厚度的石英基片作为衬底；采用分子束外延结合低温退火镀膜方式在基片表面沉积一层50nm厚度的低损耗银反射层。
(2)在银反射层表面旋涂一层300nm厚度的高分辨力流体聚合物材料，相当于前述步骤S1。
(3)通过加热蒸发的方式在200nm线宽分辨力的铬掩模版表面形成一层均匀的单分子抗粘剂层。
(4)采用被动调平机械结构将旋涂有高分辨力流体聚合物材料的基片与在200nm线宽分辨力的铬掩模版图形面调平并接触。
(5)通过在基片背面施加0.2MPa的气压方式，将厚度为100nm的高分辨力流体聚合物材料表面挤压进入掩模版图形透光区，并加热固化，相当于前述步骤S2。
(6)打开中心波长为365nm的紫外曝光光源，在功率为0.2mW/cm2的条件下，曝光20s；在反射层的作用下使穿过掩模版图形的光场局域在透光区，使挤压进入掩模版图形透光区及到反射层之间的局部流体聚合物材料感光。
(7)曝光完成后，将基片与掩模分离，实现脱模；并将基片放入显影液中在22℃温度条件下显影20s，以去掉未感光及固化的聚合物材料，得到200nm分辨力、300nm深度的光印图形，相当于前述步骤S3。
实施例2
制作30nm线宽分辨力、50nm深度的光印图形，其具体的制作过程如下：
(1)选择厚度为0.21mm厚度的硅片作为衬底；采用铝和铜共溅射的镀膜方式在基片表面沉积一层60nm厚度的低损耗铝反射层。
(2)在铝反射层表面旋涂一层50nm厚度的高分辨力流体聚合物材料，相当于前述步骤S1。
(3)通过加热蒸发的方式在30nm线宽分辨力的钼掩模版表面形成一层均匀的单分子抗粘剂层。
(4)采用三点主动调平系统将旋涂有高分辨力流体聚合物材料的基片与在30nm线宽分辨力的钼掩模版图形面调平并接触。调平过程实时监测并调整三点的间隙值。
(5)通过压电执行机构在基片背面施加200N的压力，将厚度为 20nm的高分辨力流体聚合物材料表面挤压进入掩模版图形透光区，并加热固化，相当于前述步骤S2。
(6)打开中心波长为365nm的紫外曝光光源，在功率为0.2mW/cm2的条件下，曝光10s；在反射层的作用下使穿过掩模版图形的光场局域在透光区，使挤压进入掩模版图形透光区及到反射层之间的局部流体聚合物材料感光。
(7)曝光完成后，将基片与掩模分离，实现脱模；并将基片放入显影液中在0℃温度条件下显影40s，以去掉未感光及固化的聚合物材料，得到30nm分辨力、50nm深度的光印图形，相当于前述步骤S3。
本公开相比于传统直写类微纳制造技术，虽然本方法也需采用直写方法制作掩模，但通过该掩模可以低成本批量复制微纳结构，加工效率远远高于传统直写类微纳制造技术；相比于传统光刻类微纳制造技术，本方法解决了衍射受限的问题，通过反射式光场增强降低倏逝波的传输损耗，提高了加工分辨力，不需要缩短曝光波长和提高物镜的数值孔径；相比于传统的压印类微纳制造技术，压印过程中是将压印胶挤压进入模板中，再通过热固化或紫外固化形成图形，图形的深度由压模决定，因而压模的制造难度及成本较高；而本方法是采用浅压结合曝光的方法，图形的深度主要由曝光的深度决定，降低了掩模加工难度及成本；其次由于压印图形需要保证一定的深宽比，在脱模的过程中图形结构不可避免的由于受力原因，未中压模上分离，造成图形缺陷；而本方法挤压进入掩模的图形深度较浅，主要通过曝光提高图形的深度，因而极大程度的降低了图形缺陷。
以上所述的具体实施例，对本公开的目的、技术方案和有益效果进行了进一步详细说明，所应理解的是，以上所述仅为本公开的具体实施例而已，并不用于限制本公开，凡在本公开的精神和原则之内，所做的任何修改、等同替换、改进等，均应包含在本公开的保护范围之内。

Claims (16)

  1. 一种微纳结构的制备方法，其特征在于，包括：
    在基片(8)表面依次形成反射层(7)、流体聚合物层(6)；
    将所述基片(8)与带微纳图形的掩模版(2)加压贴合，使所述流体聚合物层(6)挤压进入所述掩模版的透光区(5)，并使所述流体聚合物层(6)固化；
    曝光，在透射光以及所述反射层反射光的共同作用下使所述透光区的流体聚合物感光，得到所述微纳结构。
  2. 根据权利要求1所述的微纳结构的制备方法，其特征在于，所述将所述基片(8)与带微纳图形的掩模版(2)加压贴合包括：
    通过精密压力传递将所述基片(8)与带微纳图形的掩模版(2)加压贴合，使所述流体聚合物层(6)均匀受压进入所述掩模版的透光区(5)。
  3. 根据权利要求2所述的微纳结构的制备方法，其特征在于，所述通过精密压力传递将所述基片(8)与带微纳图形的掩模版(2)加压贴合中，精密压力传递的方法包括活塞类机械传递、压电执行机构传递、气膜传递、气压传递。
  4. 根据权利要求1所述的微纳结构的制备方法，其特征在于，所述将所述基片(8)与带微纳图形的掩模版(2)加压贴合之前还包括：
    将所述基片(8)与带微纳图形的掩模版(2)调平并接触。
  5. 根据权利要求4所述的微纳结构的制备方法，其特征在于，所述使所述透光区的流体聚合物固化还包括：
    将所述基片(8)置于显影液中显影，去除未感光固化的流体聚合物，得到所述微纳结构。
  6. 根据权利要求1所述的微纳结构的制备方法，其特征在于，所述掩模版(2)的微纳图形(3)上还包括一层抗粘接层(4)，所述抗粘接层(4)的材料包括类金刚石薄膜、掺氟硅烷。
  7. 根据权利要求1所述的微纳结构的制备方法，其特征在于，所述流体聚合物层(6)为高分辨力的流体聚合物材料，包括氟掺杂硅基共聚物或衍生物、乙烯醚基共聚物、丙烯酸基共聚物、杯芳烃基分子玻璃、高酸解活性缩醛聚合物、聚对羟基苯乙烯基共聚物。
  8. 根据权利要求1所述的微纳结构的制备方法，其特征在于，所述在基片(8)表面形成反射层(7)的方法包括分子束外延结合低温退火、共溅射、高温溅射法。
  9. 根据权利要求8所述的微纳结构的制备方法，其特征在于，所述在基片(8)表面形成流体聚合物层(6)包括将所述流体聚合物旋涂在所述反射层(7)表面，形成流体聚合物层。
  10. 根据权利要求8所述的微纳结构的制备方法，其特征在于，所述反射层(7)包括低损耗银反射层、低损耗铝反射层。
  11. 一种基于反射式光场增强的微纳光印制造方法，其特征在于，步骤如下：
    步骤1、在基片表面沉积一层低损耗的反射层；
    步骤2、将高分辨力的流体聚合物材料旋涂在反射层表面；
    步骤3、在微纳米掩模版表面制作一层抗粘接层；
    步骤4、通过机械装置将在反射层表面旋涂有高分辨力流体聚合物材料的基片与微纳米掩模版图形面调平并接触；
    步骤5、通过精密压力传递方法将高分辨力的流体聚合物材料表面浅层挤压进入掩模版图形透光区；
    步骤6、曝光，在反射层的作用下使穿过掩模版图形的光场局域在透光区，使挤压进入掩模版图形透光区及到反射层之间的局部流体聚合物材料感光及固化；
    步骤7、脱模后将基片放入显影液中显影，去掉未感光及固化的聚合物材料，得到复制后的图形。
  12. 根据权利要求11所述的一种基于反射式光场增强的微纳光印制造方法，其特征在于：所述步骤1中低损耗的反射层制备方法为分子束外延结合低温退火、共溅射、高温溅射法。
  13. 根据权利要求11所述的一种基于反射式光场增强的微纳光印制造方法，其特征在于：所述步骤2中高分辨力的流体聚合物材料为氟掺杂硅基共聚物或衍生物、乙烯醚基共聚物、丙烯酸基共聚物、杯芳烃基分子玻璃、高酸解活性缩醛聚合物、聚对羟基苯乙烯基共聚物。
  14. 根据权利要求11所述的一种基于反射式光场增强的微纳光印制造方法，其特征在于：所述步骤3中抗粘接层为类金刚石薄膜、掺氟硅烷。
  15. 根据权利要求11所述的一种基于反射式光场增强的微纳光印制造方法，其特征在于：所述步骤5中精密压力传递方法为活塞类机械传递、压电执行机构传递、气膜传递、气压传递。
  16. 根据权利要求11所述的一种基于反射式光场增强的微纳光印制造方法，其特征在于：所述步骤5中压力传递方法为活塞类机械传递、压电执行机构传递、气膜传递、气压传递。
PCT/CN2021/090554 2020-04-29 2021-04-28 一种微纳结构的制备方法 Ceased WO2021219005A1 (zh)

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