一、鈀氧化亞銅及金奈米棒氧化亞銅核殼結構與其晶面相關之光學探討二、金氧化亞銅核殼結構之可調性近紅外光表面電漿吸收產生之有效光熱作用

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研究生：	王祥儒
論文名稱：	一、鈀氧化亞銅及金奈米棒氧化亞銅核殼結構與其晶面相關之光學探討二、金氧化亞銅核殼結構之可調性近紅外光表面電漿吸收產生之有效光熱作用 I. Facet-Dependent Optical Properties of Pd-Cu2O and Au rod-Cu2O Core-Shell Nanocrystals II. Photothermal Effects Generated from Au-Cu2O Core-Shell Nanocrystals with Tunable NIR SPR Absorption Band
指導教授：	黃暄益
口試委員:	朱立岡郭俊宏黃暄益
學位類別：	碩士 Master
系所名稱：	理學院 - 化學系 Department of Chemistry
論文出版年：	2014
畢業學年度：	102
語文別：	英文
論文頁數：	100
中文關鍵詞：	鈀、金、氧化亞銅、表面電漿共振、光熱
外文關鍵詞：	Pd, Au, Cu2O, surface plasmon resonance, photothermal
相關次數：	點閱：2 下載：0
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先前我們透過以八面體的金核合成奈米立方體、截半立方體及八面體的金氧化亞銅核殼結構，已證實氧化亞銅晶體其與晶面有關之光學性質。金的表面電漿共振吸收峰因為氧化亞銅的高折射率而大幅紅位移且保持在固定的位置而無關乎殼的厚度改變。然而，改變殼的表面晶面，金的表面電漿共振吸收峰在立方體及八面體的金氧化亞銅核殼結構相差達到26奈米，且氧化亞銅的殼本身也出現與晶面有關之光學性質。在第一個環節中，我們同樣觀察到光學性質的晶面相關性也出現在鈀氧化亞銅及金奈米棒氧化亞銅核殼結構中。但是，在正方體中，鈀的表面電漿共振吸收峰卻比八面體更為藍位移，與在金氧化亞銅結構中相反。金奈米短棒的長軸電漿共振吸收峰也因氧化亞銅而紅位移至第二生物窗口。第二個部分中，小尺寸的金氧化亞銅核殼結構第一次被應用在光熱效應中，以近紅外光雷射加熱經過300秒後溫度可從室溫提升至 65 ºC，此現象可應用於將太陽能轉換為熱能。藉由包上氧化亞銅可增加吸收截面積且調控金的表面電漿吸收，此外，金奈米粒子穩定性也可得到提升，而非於照射後會發生變形。這些結構有潛力可發展為極小且高效能的電漿加熱器。

Previously we showed that the optical properties of Cu2O crystals are facet-dependent by examining Au‒Cu2O core‒shell nanocubes, cuboctahedra, and octahedra with octahedral gold cores. The substantially red-shifted Au surface plasmon resonance (SPR) absorption band due to the Cu2O shell with a large refractive index remains fixed despite changes in the shell thickness. However, tuning the shell shape, and hence the surface facet, the Au SPR band can differ by as much as 26 nm. The Cu2O shells also display facet-dependent optical properties. Here in the first study, we examined if the same facet-dependent optical properties are observable in Pd‒Cu2O and Au nanorod‒Cu2O core‒shell nanocrystals. Nicely, the same facet-dependent optical properties are observed in these nanostructures. However, the Pd SPR band in Pd‒Cu2O cubes is more blue-shifted than Pd‒Cu2O truncated octahedra, whereas in the Au‒Cu2O case the Au SPR band of cubes is more red-shifted than octahedra. The short Au nanorod cores shift the SPR band directly to 1010‒1235 nm into the second biological window with the Cu2O shells. The small Au‒Cu2O core‒shell nanocrystals were tested for photothermal effect for the first time. Remarkably, giving enough near-IR irradiation energy, the ethanol solvent containing Au‒Cu2O nanoparticles can raise the temperature to 65 ºC after 300 sec from room temperature. This property can be exploited for converting sun light to thermal energy. Au nanoparticles can deform after long illumination time. By coating Cu2O shells outside Au cores, the stability and absorption cross section will increase and the LSPR property is tunable by changing the shell morphology and using short rods. These structures have potential as ultrasmall and highly efficient plasmonic heaters.

摘要   i 
Abstract   ii 
Table of Contents   iv 
List of Figures   vii 
List of Tables   xii 
List of Schemes   xiii 
CHAPTER 1 Overview of the Thesis and the Background Knowledge   1 
1  Overview of the Thesis   1 
2  Background Knowledge   4 
2.1  Fundamental Optics   4 
2.2  Plasmonics   9 
2.3  Photothermal Effects on Nanoscale   16 
2.4  Cuprous Oxide   20 
3  Paper Review   25 
3.1  Optical and Plasmonic Properties of Nanoparticles   25 
3.2  Photothermal Properties of Nanoparticles   30 
4  Conclusion   36 
5  References   37 
CHAPTER 2 Facet-Dependent Optical Properties of Pd−Cu2O and Au rod−Cu2O Core−Shell 
Nanocrystals   40 
1  Introduction   40
2  Experimental Section   42 
2.1  Chemicals   42 
2.2  Synthesis of Au Nanorods   42 
2.3  Synthesis of Au Nanorod‒Cu2O Core‒Shell Nanocrystals   43 
2.4  Synthesis of Pd Nanocubes   44 
2.5  Synthesis of Pd‒Cu2O Core‒Shell Nanocrystals   45 
2.6  Instrumentation   46 
3  Results and Discussion   47 
3.1  Pd−Cu2O Nanocrystals   47 
3.2  Au Nanorod−Cu2O Nanocrystals   55 
4  Conclusion   67 
5  References   68  
2  Experimental Section   42 
2.1  Chemicals   42 
2.2  Synthesis of Au Nanorods   42 
2.3  Synthesis of Au Nanorod‒Cu2O Core‒Shell Nanocrystals   43 
2.4  Synthesis of Pd Nanocubes   44 
2.5  Synthesis of Pd‒Cu2O Core‒Shell Nanocrystals   45 
2.6  Instrumentation   46 
3  Results and Discussion   47 
3.1  Pd−Cu2O Nanocrystals   47 
3.2  Au Nanorod−Cu2O Nanocrystals   55 
4  Conclusion   67 
5  References   68 
CHAPTER 3 Photothermal Effects Generated from Au−Cu2O Core−Shell Nanocrystals with 
Tunable NIR SPR Absorption Band   69 
1  Introduction   69 
2  Experimental Section   71 
2.1  Chemicals   71 
2.2  Synthesis of Au Octahedra   71 
2.3  Synthesis of Au−Cu2O Core−Shell Heterostuctures   72 
2.4  Synthesis of Au Nanorod−Cu2O Core−Shell Heterostuctures   74 
2.5  Photothermal Measurement   75 
2.6  Instrumentation   75 
3  Results and Discussion   77 
4  Conclusion   97   
5  References   98 
Appendix   99 
                                

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