臺灣博碩士論文加值系統

自主裝奈米顆粒薄膜具有許多有趣的光學與電學特質，例如金屬奈米顆粒薄膜具有很強的表面電漿共振吸收，且吸收共振波長可由奈米粒子之間的間距來調控，此外金屬奈米顆粒間將會產生一強局域電場，並可用來增強拉曼訊號、增強太陽能的效率與影響奈米元件的電荷傳輸等等。奈米顆粒薄膜的穿隧電阻也將會奈米顆粒之間的間距改變，當間距從0.9奈米變成1.8奈米時，薄膜的電學特性將從導電態變為絕緣態。 而奈米顆粒薄膜電阻對於間距變化的靈敏反應和特性可由表面所修飾的分子來定義，使它可被用來感測特定的氣體分子、重金屬、有機物或微小的曲率變化。
在這個研究當中，我們將分子與金屬奈米顆粒組成的奈米顆粒薄膜應用在幾個不同的領域，如可重複使用的SERS基板、高靈敏的濕度(水氣)感測器與量測分子熱電上。在實驗當中，我們也證實可由簡單的臭氧處理來還原已經使用過金奈米顆粒薄膜的SERS基板，並且發現金奈米顆粒薄膜SERS基板在反覆使用50次後，能維持一樣的增強效果。此外，我們也發現當表面接上metal-ptoroporphyrin分子的奈米顆粒薄膜對於水氣有很靈敏的反應，且具有相當短的反應時間和穩定性。最後我們也把分子-金奈米顆粒結構應用於分子的熱電量測，我們將待測分子修飾於奈米金表面，並鋪排於一純金的電極上，並利用自行設計的量測機構來量測待測分子的熱電電壓，並且計算出他的功效與seebeck 係數。從這些不同的領域應用，證明了分子-金屬奈米顆粒結構，在不同領域中將有相當不錯的應用性。

The assembled nanostructures consisting of nanoparticles has many interesting optical, electrical, and photo-electric properties. For instance, the assembled gold and silver nanoparticle film has strong interparticle coupling effect on their local surface plasmon resonance (LSPR), which can be tuned through control interparticle spacing between adjacent nanoparticle. The strong local electromagnetic field adjacent nanoparticles from LSPR created is often applied to the surface enhanced Raman spectroscopy. Similarly, the tunneling resistance of nanoparticle films also has the strong influence of interparticle space s. For example, the electric properties change from Mott-metal to Mott-insulator when interparticle spacing increased. Besides, the characteristics of nanoparticle films also depend on their surface-modified molecules. The specific characteristic and high sensitivity resistance variation for interparticle spacing have power and high potential application at chemisorbed sensors, ion sensors, and bending sensors.
In this reports, we fabricated the assembled nanostructure consisted with molecule functionalized metal nanoparticles by centrifugal assembly method, and applied to reusable SERS substrate, humidity sensor, and molecule thermoelectric properties studies. For reusable SERS substrate, we demonstrate a simple method to reuse SERS substrate of assembled AuNPs and AgNPs films through ozone treatment to remove analyte. The analytes molecules on SERS substrate were easy decomposed with less ozone exposure time, and could renew SERS substrate up to fifty times. In addition, we also found metal-protoporphyrin AuNP films could be apply to humidity sensors. The resistance of metal-protoporphyrin AuNP films would increase when the film exposed in water vapor. In addition, metal-protoporphyrin AuNP films have higher response and much better repeatability than alkanethiol AuNP films. Finally, we also measurement the Seebeck coefficient of molecule junctions by using novel nano-assembly method to fabricate composite molecule-AuNPs films and build up a measurement system. We got the Seebeck coefficient of metal-protoporphyrin-AuNPs films and cysteine/cysteamine-AuNPs films, and found the Seebeck coefficients of metal-protoporphyrin-AuNPs films were positive, but was negative to cysteine/cysteamine-AuNPs films. We also found Heme-AuNPs and Hematin-AuNPs film have similar Seebeck coefficient, this may due to same ceter-metal ion.

Contents
Chapter1. Introduction 1
1.1 Overview 1
1.2 Assembled nanoparticle films 2
1.3 The characteristic and application of Assembled nanoparticle films 3
1.4 Outline of the work 8
1.5 References 9
Chapter 2. Materials and Methods 11
2.1 Gold and silver nanoparticle synthesis 11
2.1.1 Preparation of gold nanoparticle 11
2.1.2 Silver nanoparticle method (15~40 nm) 17
2.2 Gold and silver nanoparticle modification method 18
2.3 Lithography and electrode fabrication 22
2.4 Assembly of nanoparticle films 23
2.5 Reference 24
Chapter 3. Ultra-Sensitive and Reusable SERS Substrate 27
3.1 Introduction 27
3.2 Basic Principles 33
3.2.1 Raman scattering 33
3.2.2 Surface enhanced Raman spectroscopy (SERS) 34
3.3 Experiment method and measurement system 37
3.3.1 SERS measurements 37
3.3.2 Ozone treatment method 38
3.4 Result and Discussion 39
3.4.1 Au-NPs and AgNPs film SERS substrate 39
3.4.2 Ozone treatment method 41
3.4.3 Reusable SERS substrate 51
3.5 Conclusion 55
3.6 Reference 56
Chapter 4. High-Response Humidity Sensor Utilizing Metal- Protoporphyrin Encapsulated Gold Nanoparticles 61
4.1 Introduction 61
4.2 Basic Principles 70
4.3 Experiment method and measurement system 70
4.3.1 Metal-protoporphyrin-AuNP film 70
4.3.2 Measurement system 71
4.4 Result and Discussion 72
4.4.1 Metal-protoporphyrin-AuNP films for humidity sensing 72
4.4.2 Alkanethiol-AuNP film for humidity sensing 78
4.4.3 Repeatability test and response time 80
4.5 Conclusion 84
4.6 Reference 84
Chapter 5. Thermoelectric Properties of Composite Nanoparticle Array with Protoporphyrin Molecule Junctions 87
5.1 Introduction 87
5.2 Basic Principles 93
5.3 Experiment method and measurement system 95
5.3.1 Metal-protoporphyrin-AuNP film 95
5.3.2 Measurement system 95
5.4 Result and Discussion 100
5.5 Conclusion 105
5.6 Reference 105
Chapter6. Summary 107

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Chapter 4.
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