通过多元方法构造功能性有序微结构阵列
摘要
微观的结构和表面图案在现代科技中均发挥了重要的作用。随之而来,各种各样的构造技术与方法应运而生。不断发展的图案化技术,展现丰富的多样性和功能性。但是,单一的图案化技术总是在某一方面存在缺点或不足;与之相对,近期新兴的自组装技术则可以迅速而简单地构造微图案,但这项技术的可控性和精确度较差。而且对复杂的二元结构来说,通过单一的策略是很难得到的。因此,对现有的技术进行合理的搭配或改进,来构筑新颖的图案,是图案化技术中新的机遇和挑战。在本论文中,我们将传统与新兴的图案化技术相结合,通过简单的操作步骤,实现了功能性的二元结构的构筑。首先,我们通过可控的去润湿过程,在化学图案化的基底上构造了大面积二元条带的阵列。随着形貌及尺寸的改变,各向异性的效果也不同。这种二元条带阵列不仅在结构上模仿了水稻叶表面结构,而且水滴在其表面也展现出各向异性的润湿。我们不仅可以构造单一聚合物的二元阵列,还可以构造异质的二元结构阵列。然后,我们通过改良的水汽冷凝辅助法(breath figure)结合可控去润湿,构造了异质的靶心结构微阵列。许多材料都可以用于这个体系,磁性纳米粒子、聚合物、有机发光小分子均可以用来构造靶心结构。而更小的特征尺寸往往带来更优异的性质,所以我们在进一步的实验中用二氧化硅胶体微球代替冷凝的水滴,通过胶体微球刻蚀技术与表面诱导的可控二次去润湿的过程,构造了纳米尺寸的双环阵列。
Micro-structure or surface pattern has played an important role in both modern science and technology. Followed, a variety of construction techniques and methods have emerged. Developing technologies show the rich diversity and functionality in many areas, such as microelectronics, information storage, solid-state physics, materials science, biotechnology and application of fluid science and so on. However, a single pattern technology always has shortcomings or deficiencies in one way, such as laser or particle beam writing techniques. These techniques possess high precision and control capability, but they suffer complicated operation, poor general-purpose, time-consuming and expensive. By contrast, the recent emerging of self-assembly techniques can be quickly and easily construct micro-patterns, but they have less controllable and precision. For the complex binary structure, it is very difficult to fabricate by a single strategy. Accordingly, improving the existing technologies for novel pattern remain new opportunity and challenge in pattern technology. In this paper, through a combination of one or several patterned technologies, we first construct a chemical or physical patterned template. Then, by the template-induce dewetting process on the surface, variety of ordered binary microstructure array had been obtained. This policy strategy for combination of multiple patterned technologies to construct the ordered binary structures array, not only followed the advantages of each patterned technology, but also makes up for their deficiencies, which complement each other. At the same time, this multiplex strategy provides a new approach for design and fabrication of functional and structural structure array.
In chapter 2, we fabricated the large-area surface with ordered binary structures via controllable dewetting of polymer thin films. Firstly, the substrate with stripe patterned resist was obtained by conventional photolithography. By chemical vapor deposition (CVD) of fluoride silane (PFS), the chemical heterogeneous substrate was fabricated. Then the polymer film was spin-coating on the patterned substrate and thermal annealing above its Tg. By regulating the simple conditions including concentration of polymer solution and pattern of PFS modification, the diverse topographies had been obtained finally. And the fabrication process were investigated and calculated in detail. The novel surfaces mimicked the natural rice leaf in surface structure. Moreover, these surfaces with ordered binary stripes exhibited well anisotropic wettability for water droplet as natural rice leaf. After a large number of static contact angle measurements, it was confirmed that the anisotropy had been influenced by the periods of the patterns. For a variety of topographies, the mimicking surfaces all exhibited the anisotropy. This technique will offer an effective new way of designing the wettability of materials, and further to design and fabricate smart controllable devices.
In chapter 3, we have demonstrated a versatile method to fabricate ordered homogeneous and heterogeneous bull's-eye-like arrays on the SAMs-patterned surface of a gold substrate through a simple approach. Firstly, we constructed heterogeneous thioalcohol self-assembly monolayers (SAMs) on the gold substrate by microcontact printing (μCP). Then, we fabricated the PVK dot rings on the SAMs-patterned gold substrate by SAMs-directed dewetting; at the same time, we optimized conditions of the dot formation of different materials. Secondly, as the reservation of chemical properties on SAMs, we obtained the ordered ring arrays on the dot arrays patterned surface under the protecting of water droplets by water-droplets-directed and concentration-controlled dewetting process. Finally, the ordered bull's-eye-like structure arrays had been fabricated on the gold substrate. Since both experimental steps were relatively independent, the bull's-eye-like structure that we fabricated could be not only homogeneous but also heterogeneous. We had fabricated the bull's-eye-like structure arrays of PVK/PVK, PVK/DTQA, and PVK/Fe3O4 nanoparticles separately, and characterized the properties of fluorescence and magnetism. Accordingly, diverse material could be introduced to the current system, such as fluorescent materials, electro-conductive materials and magnetic materials as long as the simple conditions are satisfied. These heterogeneous bull's-eye-like structure arrays may have potential applications including photoelectric devices, catalytic surfaces, field emission devices and integrated magnetic, gas, and biochemical sensors.
In Chapter 4, the ordered rhodamine@PVA/PVK heterogeneous double-rings-like structures array was fabricated via combining colloidal lithography technology with two steps dewetting process. For the swelling property of the PDMS elastomer, non-close-packed (ncp) silica colloidal microspheres had been obtained. Then, by the“hot pressing”method, the ncp microspheres array was transferred on the prepared rhodamine@PVA film; moreover, microspheres array was partially embedded in the film and contacted the substrate. Here, we discussed the influence of film thickness in the transfer processes. Next, through the reactive ion etching (RIE) process under the mask of microspheres array, the ring-like structures array turned up below the microspheres array. The thickness of polymer film and radius of microspheres affected the ring-like structure morphology. We investigated the relationship between the two influence factors in detail. Finally, we dipped the substrate with microspheres and ring-like structures array into the PVK chloroform solution. With chloroform volatilization, the two steps dewetting process happened on the top of microspheres and the surface of substrate respectively. Followed, the PVK ring was fabricated surround the rhodamine@PVA ring. After further RIE etching, the ordered rhodamine@PVA/PVK heterogeneous double-rings-like structures array was constructed successfully. We also proved the heterogeneous double-rings-like structure by the characterization of SEM, AFM and fluorescence spectra. These unique structures array has potential application in optoelectronics device, data storage, surface photo-catalytic and surface enhanced Raman scattering (SERS). In addition, due to its universality, this method could be extended to other materials.
Micro-structure or surface pattern has played an important role in both modern science and technology. Followed, a variety of construction techniques and methods have emerged. Developing technologies show the rich diversity and functionality in many areas, such as microelectronics, information storage, solid-state physics, materials science, biotechnology and application of fluid science and so on. However, a single pattern technology always has shortcomings or deficiencies in one way, such as laser or particle beam writing techniques. These techniques possess high precision and control capability, but they suffer complicated operation, poor general-purpose, time-consuming and expensive. By contrast, the recent emerging of self-assembly techniques can be quickly and easily construct micro-patterns, but they have less controllable and precision. For the complex binary structure, it is very difficult to fabricate by a single strategy. Accordingly, improving the existing technologies for novel pattern remain new opportunity and challenge in pattern technology. In this paper, through a combination of one or several patterned technologies, we first construct a chemical or physical patterned template. Then, by the template-induce dewetting process on the surface, variety of ordered binary microstructure array had been obtained. This policy strategy for combination of multiple patterned technologies to construct the ordered binary structures array, not only followed the advantages of each patterned technology, but also makes up for their deficiencies, which complement each other. At the same time, this multiplex strategy provides a new approach for design and fabrication of functional and structural structure array.
In chapter 2, we fabricated the large-area surface with ordered binary structures via controllable dewetting of polymer thin films. Firstly, the substrate with stripe patterned resist was obtained by conventional photolithography. By chemical vapor deposition (CVD) of fluoride silane (PFS), the chemical heterogeneous substrate was fabricated. Then the polymer film was spin-coating on the patterned substrate and thermal annealing above its Tg. By regulating the simple conditions including concentration of polymer solution and pattern of PFS modification, the diverse topographies had been obtained finally. And the fabrication process were investigated and calculated in detail. The novel surfaces mimicked the natural rice leaf in surface structure. Moreover, these surfaces with ordered binary stripes exhibited well anisotropic wettability for water droplet as natural rice leaf. After a large number of static contact angle measurements, it was confirmed that the anisotropy had been influenced by the periods of the patterns. For a variety of topographies, the mimicking surfaces all exhibited the anisotropy. This technique will offer an effective new way of designing the wettability of materials, and further to design and fabricate smart controllable devices.
In chapter 3, we have demonstrated a versatile method to fabricate ordered homogeneous and heterogeneous bull's-eye-like arrays on the SAMs-patterned surface of a gold substrate through a simple approach. Firstly, we constructed heterogeneous thioalcohol self-assembly monolayers (SAMs) on the gold substrate by microcontact printing (μCP). Then, we fabricated the PVK dot rings on the SAMs-patterned gold substrate by SAMs-directed dewetting; at the same time, we optimized conditions of the dot formation of different materials. Secondly, as the reservation of chemical properties on SAMs, we obtained the ordered ring arrays on the dot arrays patterned surface under the protecting of water droplets by water-droplets-directed and concentration-controlled dewetting process. Finally, the ordered bull's-eye-like structure arrays had been fabricated on the gold substrate. Since both experimental steps were relatively independent, the bull's-eye-like structure that we fabricated could be not only homogeneous but also heterogeneous. We had fabricated the bull's-eye-like structure arrays of PVK/PVK, PVK/DTQA, and PVK/Fe3O4 nanoparticles separately, and characterized the properties of fluorescence and magnetism. Accordingly, diverse material could be introduced to the current system, such as fluorescent materials, electro-conductive materials and magnetic materials as long as the simple conditions are satisfied. These heterogeneous bull's-eye-like structure arrays may have potential applications including photoelectric devices, catalytic surfaces, field emission devices and integrated magnetic, gas, and biochemical sensors.
In Chapter 4, the ordered rhodamine@PVA/PVK heterogeneous double-rings-like structures array was fabricated via combining colloidal lithography technology with two steps dewetting process. For the swelling property of the PDMS elastomer, non-close-packed (ncp) silica colloidal microspheres had been obtained. Then, by the“hot pressing”method, the ncp microspheres array was transferred on the prepared rhodamine@PVA film; moreover, microspheres array was partially embedded in the film and contacted the substrate. Here, we discussed the influence of film thickness in the transfer processes. Next, through the reactive ion etching (RIE) process under the mask of microspheres array, the ring-like structures array turned up below the microspheres array. The thickness of polymer film and radius of microspheres affected the ring-like structure morphology. We investigated the relationship between the two influence factors in detail. Finally, we dipped the substrate with microspheres and ring-like structures array into the PVK chloroform solution. With chloroform volatilization, the two steps dewetting process happened on the top of microspheres and the surface of substrate respectively. Followed, the PVK ring was fabricated surround the rhodamine@PVA ring. After further RIE etching, the ordered rhodamine@PVA/PVK heterogeneous double-rings-like structures array was constructed successfully. We also proved the heterogeneous double-rings-like structure by the characterization of SEM, AFM and fluorescence spectra. These unique structures array has potential application in optoelectronics device, data storage, surface photo-catalytic and surface enhanced Raman scattering (SERS). In addition, due to its universality, this method could be extended to other materials.
引文
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