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DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 廖尉斯 | |
dc.contributor.author | Chong-You Chen | en |
dc.contributor.author | 陳重佑 | zh_TW |
dc.date.accessioned | 2021-06-17T06:11:44Z | - |
dc.date.available | 2028-12-31 | |
dc.date.copyright | 2018-11-08 | |
dc.date.issued | 2018 | |
dc.date.submitted | 2018-10-23 | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/71841 | - |
dc.description.abstract | 表面分子環境控制在印刷技術與相關應用方面均扮演極重要的角色,而將其應用在分析平台開發的前端研究中也因其決定性之影響力而受到極大之重視。在本論文中,我們運用化學拔除法可調控分子層缺陷的特性,將其應用於表面生物分子修飾、奈米粒子選擇性排列,微液珠陣列形成等研究。首先,為滿足生物功能性分析平台需仰賴極低之非專一性吸附和足夠分子辨認的介面環境需求,我們利用化學拔除法在基材表面製作出稀釋分子層的環境,提供功能性分子選擇性修飾與後續結合目標物的良好條件。此處所使用之化學拔除法係利用活化後的軟性材料印章與表面單分子層之接觸,在分離兩表面的後續操作中因介面間化學鍵結的形成而導致金屬基材表面分子的拔除現象,同時產生人工的分子層缺陷。這些表面缺陷除能提供功能性生物分子插入的空間,拔除區域內所殘存的分子亦可支撐後插入生物分子展現‟自我站立”的特性,並同時達到分散欲修飾分子之目的。由實驗結果發現,經由這種表面修飾所插入之生物分子和目標物的親合能力可媲美在溶液中無空間結合障礙的自由分子選擇性辨認效率。重要的是,印章與表面單分子層的接觸時間為調控表面分子密度的關鍵條件,因而此實驗條件可被利用來調控分子層的缺陷程度,進一步控制後續所插入的生物分子密度;而利用多次且不同接觸時間的拔除策略,在同一塊基板上更可達到多樣化的分子修飾密度。在研究中我們發現,經化學拔除法所產生的表面缺陷可同時適用於許多不同類型生物分子的修飾,大幅增加了利用此技術以製作分析平台的應用廣度。此外,經化學拔除處理後的區域由於表面親水分子減少與殘存分子疏水性枝幹的暴露,使此區域得可以抑制檸檬酸根包覆的金奈米粒子之吸附,而促使奈米粒子藉由氫鍵吸引力選擇性地沉積在未經化學拔除處理的區域。在最佳的優化條件下,我們便可利用化學拔除法精準地圖樣化奈米粒子於表面之選擇性沉積,使其圖樣解析度最高可達只有一顆奈米粒子的寬度。另一方面,透過化學拔除法於單分子層的高解析圖樣化能力,我們也可簡單地利用親水性與疏水性分子之差異來調控基材表面的親疏水性程度;而藉由不連續性之去濕過程,流經表面之液體可在親水性分子修飾之區域自主聚集而產生微液珠陣列平台。我們進一步利用這些液珠的形成過程來調控不同材料於表面之組裝與排列行為,所產生之材料陣列不但可用以提高所製分析平台的效能,也可利用在降低基質輔助雷射脫附電離質譜分析的定量偏差。藉由這些實驗結果可知,化學拔除法除可提供更簡易且多變性的分析平台設計方法外,並同時具有不同尺度的表面圖樣化能力,且能提供良好的表面分子環境控制與材料介面性質操縱。 | zh_TW |
dc.description.abstract | Surface molecular environment control has attracted much attention due to its importance in both lithographic technologies and practical applications for analytical platform developments. In this dissertation, I demonstrate programmable molecular-level defects control through chemical lift-off lithography (CLL) to manipulate biomolecule anchoring, nanoparticle alignment, and microdroplet formation. First, a straightforward strategy creating diluted matrices by CLL for site-specific probe anchoring and suitable targeting recognition is introduced. This design ensures adequate biomolecules immobilization with minimum nonspecific attachment and provides an appropriate molecular recognition environment. The Au-thiolates lift-off operation in CLL generates artificial self-assembled monolayer (SAM) defects, enabling spatially addressable biomolecules. The created diluted surface molecular environment can assist aptamer probes not only to “self-stand” on the surface but also to be separated from each other. The binding affinity of surface-patterned probes toward targets is found to be comparable to solution-type free probes. The conformal contact-induced reaction between the activated soft material stamp and SAMs in CLL is crucial in offering well-tunable SAM defects, leading to well-controllable anchored probe quantity. With multiple lift off processes, complex probe density gradients are produced and the fabricated arrays are functional for a variety of target recognition. This post-CLL region is found to be suitable for various biological probes’ insertion to benefit different biorecognition array types. Other than bio assays, nanoparticle arrays on a supporting substrate can benefit the development of analytical devices, and a CLL-based strategy for high quality nanoparticle alignment is demonstrated. The unique molecular environment of post-CLL area can resist nonspecific adhesion of citrate-capped Au nanoparticle due to highly reduced number of hydrophilic terminal functional groups and increased exposure of residual molecules’ hydrophobic alkane chains. The nanoparticles are consequently deposited onto hydroxyl-terminated SAM covered areas, where hydrogen-bonding plays a key role in attracting citrate-capped Au nanoparticles. Under appropriate deposition conditions, spatially precise nanoparticle alignment with single-particle-wide resolution is achieved. Taking advantages of CLL-created high fidelity molecular patterns, I also demonstrate regional wettability differences provided by CLL for “wall-less” microdroplet array fabrication. The introduced liquids repel from patterned omniphobic areas and spontaneously condense on hydrophilic regions in the discontinuous dewetting process, resulting in isolated liquid droplet formation. These well-ordered droplet arrays not only increase the throughput of particle-based sensing platform fabrication, but also help matrix-assisted laser desorption/ionization of mass spectrometry with lowered quantification variance. Embracing properties of extensive pattern feature dimension and geometry, great local molecular environments control, and advanced interfacial interactions, this CLL process has moved the fabrication of analytical devices onto a more convenient route. | en |
dc.description.provenance | Made available in DSpace on 2021-06-17T06:11:44Z (GMT). No. of bitstreams: 1 ntu-107-D03223108-1.pdf: 15640679 bytes, checksum: 58c7940ee3687c38e929771148d89a9e (MD5) Previous issue date: 2018 | en |
dc.description.tableofcontents | 中文摘要 i
Abstract iii Contents v Figure Contents vii Table Contents xiii Abbreviation List xiv Chapter 1 Introduction 1 1.1 Chemical Lift-Off Lithography 1 1.2 Molecular Environment Management 3 1.3 Bioactive Matrix 6 1.4 Diverse Applications 9 1.5 References 14 Chapter 2 Self Standing Aptamers by Artificial Defect-Rich Matrix 19 2.1 Introduction 20 2.2 Results and Discussion 21 2.3 Conclusions 26 2.4 Experimental Section 27 2.5 References 43 Chapter 3 Surface Functional DNA Density Control by Programmable Molecular Defects 48 3.1 Introduction 49 3.2 Results and Discussion 50 3.3 Conclusions 54 3.4 Experimental Section 54 3.5 References 71 Chapter 4 Wafer Scale Bioactive Substrate Patterning by Chemical Lift Off Lithography 77 4.1 Introduction 78 4.2 Results and Discussion 80 4.3 Conclusions 85 4.4 Experimental Section 85 4.5 References 97 Chapter 5 Large Area Nanoparticle Alignment by Chemical Lift-Off Lithography 101 5.1 Introduction 102 5.2 Results and Discussion 104 5.3 Conclusions 106 5.4 Experimental Section 107 5.5 References 115 Chapter 6 Finely Tunable Surface Wettability by Two Dimensional Molecular Manipulation 118 6.1 Introduction 119 6.2 Results and Discussion 122 6.3 Conclusions 128 6.4 Experimental Section 129 6.5 References 143 Synopsis and Prospects 151 Publications 153 Appendix I 154 Appendix II 164 | |
dc.language.iso | en | |
dc.title | 應用表面分子環境控制於分析平台奈米製程 | zh_TW |
dc.title | Nanofabrication for Analytical Platforms via
Surface Molecular Environment Control | en |
dc.type | Thesis | |
dc.date.schoolyear | 107-1 | |
dc.description.degree | 博士 | |
dc.contributor.oralexamcommittee | 張煥宗,陳俊顯,張哲政,何佳安,陳珮珊 | |
dc.subject.keyword | 化學拔除法,表面分子環境,分析平台, | zh_TW |
dc.subject.keyword | chemical lift-off lithography,surface molecular environment,analytical platform, | en |
dc.relation.page | 176 | |
dc.identifier.doi | 10.6342/NTU201804233 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2018-10-23 | |
dc.contributor.author-college | 理學院 | zh_TW |
dc.contributor.author-dept | 化學研究所 | zh_TW |
顯示於系所單位: | 化學系 |
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