本研究中，探討蠶絲蛋白混摻金屬奈米粒子 (金奈米粒子、銀奈米粒子以及中空金奈米粒子) 之複合薄膜的光學行為、在白光燈源照射下之光熱行為以及利用光誘導熱產生電流之響應。據我們所知，目前尚未有以高分子/金屬奈米粒子系統開發寬頻且高吸收之複合薄膜，同樣的，選擇白光光源探討光熱效應的研究也相當有限。本研究藉由增加金屬奈米粒子在薄膜中的含量，希望能將增加侷域表面電漿共振 (LSPR) 吸收波段附近的吸收值之外，更重要的是希望增加在非LSPR吸收波段之吸收值，得到具有寬頻吸收特性的複合薄膜。當大量的吸收子存在時，有助於光熱效應速率。本研究比較了三種不同的金屬奈米粒子，其中，蠶絲蛋白/中空金奈米粒子複合薄膜表現出優異的光學性質，此複合薄膜具有寬頻且高吸收的特性，在350-2000 nm波段之吸收值皆>90%，因此在同樣光強度的入射光之下，此複合薄膜可以吸收涵蓋這個範圍的所有入射光，將光能量轉換成熱能。此外，由實驗結果發現到不管是利用LED燈或是鹵素燈做為白光光源，都可以快速地讓溫度上升到超過100 oC，此外，蠶絲蛋白/金屬奈米粒子複合薄膜皆對光強度呈現線性關係，且因為蠶絲蛋白具有高玻璃轉換溫度，因此在較高的光強度照射下，具有良好的光熱穩定性。為了進一步證實蠶絲蛋白/金屬奈米粒子複合薄膜在光-熱-電流的響應，本研究將整合寬頻吸收複合薄膜以及鋁/矽蕭特基二極體，分別以鹵素燈以及單一波長做為光源，探討光-熱-電流響應。在上述所提兩種型態光源的照射下，皆得到電流值對光強度呈現線性關係，此外，經由重複性的光─熱─電流響應測試，在經過10個循環之後，蠶絲蛋白/金屬奈米粒子複合薄膜仍舊有穩定的光─熱─電流響應。本研究中所開發的蠶絲蛋白/金屬奈米粒子複合薄膜系統具有寬頻高吸收特性、良好的光熱穩定性以及穩定的光熱電流響應，由於蠶絲蛋白為高生物相容性以及生物可降解性的材料，未來可與同樣為高生物相容性的熱電材料 (例如: 聚二氧乙基噻吩，簡稱PEDOT) 結合，應用於生物體內之充電材料。

In this study, the phenomenon of white-light-induced heating in silk fibroin (SF) films embedded with metal nanoparticles [Gold nanoparticles (Au NPs), Silver nanoparticles (AGNs), Hollow gold nanoaparticles (HGNs)] is systematically investigated. As far as we are aware, this study is the first to employ metal nanoparticles to develop an ultrahigh broadband absorber and also the first to use a white light source for the photothermal generation. By increasing the metal nanoparticle content in the composite films, the absorbance could be enhanced significantly around the localized surface plasmon resonance (LSPR) wavelength and also raised dramatically at the non-LSPR wavelengths. The greater amount of absorbed light led to an increase in the photoheating rate. Here, we compare three different metal nanoparticles including Au NPs, AGNs and HGNs with different LSPR wacelength at ca. 410 nm, 520 nm and 800 nm, respectively. For SF/HGNs, the optimized composite film exhibits an ultrahigh absorbance of ca.>90% over a wide spectral range of 350-2000 nm. In this case, the composite film could absorb almost all of the incident light and accordingly convert the optical energy to local heat. Therefore, significant temperature increases on the order of ca. >100 °C could be readily obtained when the composite film is irradiated by a LED light a halogen lamp. Moreover, the composite films also display a linear light-to-heat response with light intensity and a great photothermal stability. Finally, the broadband absorptive film is coated on a simply Al/Si Schottky diode and displays a linear, significant, stable photo-thermo-electronic response with varying light intensity. Here, we demonstrate the broadband absorptive film have photo-thermo-electronic response under either white light sources or single wavelength light exposure since its ultrahigh absorbance over a wide spectral range of 350-2000 nm.

中文摘要 I
Abstract II
圖目錄 IX
表目錄 XIV
第一章、緒論 1
1.1 研究動機 1
1.2 論文架構 3
第二章 文獻回顧 5
2.1 蠶絲蛋白 5
2.1.1 蠶絲蛋白之簡介 5
2.1.2 蠶絲蛋白在生物醫學之應用 6
2.1.3 蠶絲蛋白在光學材料之應用 11
2.2 金屬奈米粒子 12
2.2.1 金屬奈米粒子合成 12
2.2.1.1 實心金奈米粒子 (Gold nanoparticle, Au NP) 12
2.1.1.2 實心銀奈米粒子 (Silver nanoparticle, AGN) 13
2.1.1.3 中空金奈米粒子 (Hollow gold nanoparticle, HGN) 13
2.2.2金屬奈米粒子之物化性質 15
2.2.2.1 金屬奈米粒子之簡介 15
2.2.2.2 金屬奈米粒子之光學性質 (Optical property) 15
2.2.3 金屬奈米粒子之光熱性質 (Photothermal property) 18
2.3 無機熱電材料 21
2.4 有機熱電材料 22
2.5 矽基光電偵測器 24
2.5.1 p-n接面二極體 (p-n junction) 24
2.5.2 蕭特基二極體 (Schottky diode) 25
2.5.3 矽基近紅外光電偵測器 30
第三章、實驗材料與方法 34
3.1 材料 34
3.2 純化蠶絲蛋白 34
3.3 金屬奈米粒子合成 35
3.3.1 金奈米粒子 (Gold nanoparticle, Au NP) 35
3.3.2 銀奈米粒子 (Silver nanoparticle, AGN) 35
3.3.3 中空金奈米粒子 (Hollow gold nanoparticle, HGN) 36
3.4 製備蠶絲蛋白/金屬奈米粒子薄膜於基材上 36
3.5 鋁/矽元件製備 36
3.6 材料特性分析 37
3.6.1形貌分析 37
3.6.2光學量測 37
3.6.3光學模擬 37
3.6.4光熱現象 38
3.6.5光-熱-電流響應 39
第四章、開發寬頻吸收之蠶絲蛋白/金奈米粒子複合薄膜於白光光源照射下之光熱行為 40
4.1 蠶絲蛋白/實心金奈米粒子溶液之光學特性以及金屬奈米粒子之表面形貌 41
4.2 蠶絲蛋白/實心金奈米粒子複合薄膜之形貌 42
4.3 蠶絲蛋白/實心金奈米粒子複合薄膜之光學量測 45
4.4 蠶絲蛋白/實心金奈米粒子複合薄膜之光學模擬 49
4.5 蠶絲蛋白/實心金奈米粒子複合薄膜之光熱效應 53
4.6 結合鋁/矽蕭特基元件 (Schottky diode) 60
4.6.1 白光光源-熱-電流響應 60
第五章、開發寬頻吸收之蠶絲蛋白/金奈米粒子複合薄膜於通訊波段之光-熱-電偵測器 64
5.1蠶絲蛋白/金屬奈米粒子溶液之光學特性以及金屬奈米粒子之表面形貌 65
5.2蠶絲蛋白/金屬奈米粒子複合薄膜之形貌 66
5.3 蠶絲蛋白/金屬奈米粒子複合薄膜之光學量測 66
5.4 蠶絲蛋白/金屬奈米粒子複合薄膜之光學模擬 69
5.5 蠶絲蛋白/金屬奈米粒子複合薄膜之光熱效應 71
5.6 結合鋁矽蕭特基元件 (Schottky diode) 76
5.6.1單一波長光源-熱-電流響應 76
第六章、結論 79
未來工作 81
參考文獻 82

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