位置、尺寸可調控之有序矽單晶奈米線陣列製備及其氧化行為之研究

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姓名

羅健修(Chien-hsiu Lo) 查詢紙本館藏

畢業系所

化學工程與材料工程學系

論文名稱

位置、尺寸可調控之有序矽單晶奈米線陣列製備及其氧化行為之研究
(Fabrication of site- and size-controllable Si nanowire arrays and their oxidation behaviors)

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摘要(中)

本研究成功地利用奈米球微影術結合金屬催化蝕刻法在預置圖案之(001)矽晶基材上製備出位置、尺寸及長度均可控制調變之矽晶奈米線陣列。
經SEM、TEM及選區電子繞射分析，在(001)矽晶基材上定義之Pattern I及Pattern II試片上的矽晶奈米線陣列，其線寬具有很好的均一性，與所使用之奈米球模板球徑大小相當一致，其寬度約為160 nm。利用金屬催化選擇性蝕刻所生成筆直排列之矽晶奈米線陣列均為單晶結構，且軸向方向沿著[001]方向生成。此外，以不同的反應溫度及時間可有效地控制奈米線陣列之生成長度，由阿瑞尼士方程式求得在預置圖案之(001)矽晶基材上製備矽晶奈米線的蝕刻反應活化能為68.3 (kJ/mol)。
經一系列不同試片之水滴接觸角量測觀察，具有矽晶奈米線陣列結構之試片表面會呈現較好的疏水性質，其水滴接觸角為135.3°-147.3°，而造成水滴接觸角提升的現象可用Cassie Model來解釋。另外，利用紫外光-可見光光譜儀分析反應後之試片可發現，表面具有矽晶奈米線陣列結構的試片具有光補捉 ( Light Trapping ) 效果，可大幅降低入射光之反射率。
利用TEM觀察矽晶奈米線氧化之形貌顯示，Core-Shell結構中心之矽晶奈米線半徑會隨著氧化時間及溫度增加而逐漸減少，氧化層厚度則逐漸增厚。此外，矽晶奈米線由於應力的作用，在氧化初期時其氧化速率較快於平板矽晶基材，而其所生成之氧化層厚度與氧化時間呈現一拋物線關係，證明氧化層之生成為一擴散控制的反應機制，且利用氧化層於不同溫度下之生成速率可以得到線寬為160 nm之矽晶奈米線其氧化層生成反應活化能為31.3 (kJ/mol)。

摘要(英)

In the present study, we have demonstrated the successful fabrication of site-, size- and length-controlled Si nanowire arrays on pre-patterned (001)Si substrates using the PS nanosphere lithography technique and Au-assisted selective chemical etching process.
From SEM, TEM, and SAED analyses, the diameter of the Si nanowires produced on Pattern I and Pattern II samples was very uniform and was observed to be approximately 160 nm, corresponding to that of RIE-treated PS sphere mask used. All the vertically-aligned Si nanowires produced were single crystalline in nature and their axial orientations were identified to be parallel to the [001] direction. The length of Si nanowires could be tuned by adjusting the etching temperature and time. In this study, the activation energy for the formation of Si nanowires on pre-patterned (001)Si could be determined from an Arrhenius plot to be about 68.3 kJ/mol.
The results of water contact angle measurements indicated that the surfaces of HF-treated Si nanowire arrays exhibited strong hydrophobicity with water contact angle of 135.3°-147.3°. The hydrophobic behavior of the Si nanowire arrays was explained by the Cassie model. From UV-Vis spectral analysis, it is found that the Si substrate with Si nanowire arrays exhibited low reflection properties. The reduction in reflection of the Si nanowires samples can be attributed to the light trapping effect.
The oxidation characteristics of Si nanowires were investigated by TEM. The core radii and oxide shell thickness were found to decrease and increase with oxidation temperature and time. In addition, the oxidation rate of Si nanowires is faster than that of blank Si due to the stress effects. The thickness of outer SiO2 shell was found to increase parabolically with time, indicating that the growth of outer SiO2 shell is diffusion-controlled. By measuring the growth rate of SiO2 shell at different temperatures, the activation energy for the growth of SiO2 shells on 160-nm-diameter Si nanowires could be determined to be about 31.3 kJ/mol.

關鍵字(中)

★ 金屬催化蝕刻
★ 矽晶奈米線

關鍵字(英)

★ Metal-assisted etching
★ Si nanowires

論文目次

目錄…………………………………………………………………I
第一章前言及文獻回顧…………………………………………1
1-1 前言……………………………………………………………1
1-2 矽晶奈米線製備方法-乾式製程……………………………2
1-2-1 化學氣相沉積法……………………………………2
1-2-2 反應性離子蝕刻法…………………………………5
1-3 矽晶奈米線製備方法-濕式化學蝕刻製程……………………6
1-3-1 金屬輔助化學蝕刻法………………………………6
1-3-2 金屬催化濕式蝕刻法………………………………7
1-4 奈米球微影術……………………………………………8
1-4-1 奈米球微影術的發展……………………………8
1-4-2 奈米球的自組裝行為………………………………9
1-4-3 奈米球模板法製備各式奈米結構…………………9
1-5 金屬催化結合奈米球微影術製備矽晶奈米線之蝕刻反應機制10
1-6 奈米結構表面之濕潤行為………………………………11
1-7 矽晶奈米線於太陽能電池上之應用…………………………12
1-8 矽基結構之氧化行為及機制…………………………………14
1-9 研究動機………………………………………………15
第二章實驗步驟及儀器設備……………………………………17
2-1 實驗步驟……………………………………………………17
2-1-1 矽晶基材使用前處理……………………………17
2-1-2 在矽基材上預置規則圖案………………………17
2-1-3 奈米球模板製備…………………………………18
2-1-4 以電漿蝕刻調變奈米球模板之直徑………………………18
2-1-5 蒸鍍金屬薄膜………………………………………………19
2-1-6 在預置規則圖案之矽晶基材上製備規則單晶矽奈米線陣列19
2-1-7 矽晶奈米線之氧化製程……………………………………20
2-2 試片分析…………………………………………………20
2-2-1 光學顯微鏡 (OM)………………………………20
2-2-2 掃描式電子顯微鏡 (SEM)……………………20
2-2-3 穿透式電子顯微鏡 (TEM)……………………21
2-2-4 高解析穿透式電子顯微鏡 (HRTEM)…………21
2-2-5 X光能量散佈光譜儀 (EDS)…………………21
2-2-6 影像式接觸角量測儀…………………………22
2-2-7 紫外光-可見光光譜儀………………………22
第三章結果與討論………………………………………………23
3-1 預置圖案之矽基材與奈米球模板製備……………………23
3-2 利用電漿蝕刻法調控奈米球陣列之球徑……………………23
3-3 以金屬催化蝕刻法結合奈米球微影術在預置規則圖案之矽晶片上製備矽單晶奈米線陣列………………………………………24
3-4 在預置規則圖案之矽晶基材上製備矽晶奈米線陣列之成長動
力學探討………………………………………………………26
3-5 矽晶奈米線之結構及晶向分析鑑定…………………………31
3-6 接觸角量測分析………………………………………………32
3-7 紫外光-可見光光譜儀量測分析……………………………34
3-8 矽晶奈米線陣列之氧化行為及動力學探討…………………35
第四章結論與未來展望…………………………………………40
4-1 結論………………………………………………………40
4-2 未來展望…………………………………………………42
4-2-1 製備大面積筆直有序排列之金屬矽化物奈米線陣列……42
4-2-2 以濕式蝕刻法結合奈米球微影術製備不同矽基奈米陣列結構.………………………………………………………………………42
參考文獻……………………………………………………………43
表目錄………………………………………………………………53
圖目錄……………………………………………………………55

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指導教授

鄭紹良(Shao-liang Cheng)

審核日期

2010-7-28

推文