臺灣博碩士論文加值系統

於下一世代元件結構中，奈米電子、光子晶體與磁性元件的整合研發具有高度的發展潛力。其中氧化鋅半導體具有無毒、低成本、直接寬能隙、極化等特性，因此ZnO被認為是非常重要且具有未來光電元件應用的材料。本論文研究金屬摻雜氧化鋅材料之特性、並在不同材質的基板研製光電元件、場效電晶體與其他元件整合成OEIC之應用、以及元件的撓曲特性測試。論文的主要研究可以分為以下四個部分討論。
首先，我們探討氧化鋅為基礎製作的金屬-半導體-金屬(MSM)光偵測器比較單層與加上氧化鋅覆蓋層在可撓式高分子基板-聚對苯二甲酸乙二醇酯（PET）進行比較分析，其中以低溫濺鍍法濺鍍ZnO薄膜並加以分析。金屬銀與氧化鋅之間的蕭特基能障為0.782 eV。光偵測器元件結構具有氧化鋅覆蓋層（堆疊結構：氧化鋅/銀/氧化鋅/PET）顯示了一個比單層結構更高的紫外光-可見光互斥比為1.56×103。不僅是在紫外區域光電流顯著增加，而且在可見光區也有抑制效果。元件在370 nm波長和3 V偏壓下顯示出很高的紫外光響應度，在具有氧化鋅覆蓋層和氧化鋅單層結構的光偵測器元件分別為3.8×10-2和2.36×10-3 A/W，其對應於量子效率則分別為1.13和0.07 ％。
另外，探討Ti/Au與 Mg0.24Zn0.76O和ZnO薄膜的歐姆接觸特性，並應用MSM光偵測器於玻璃基板上的元件特性分析。由UV/Vis光譜測量的光學能隙顯示出Mg0.24Zn0.76O薄膜具有較大於氧化鋅薄膜(3.25 eV)的光學能隙3.54 eV。在以Mg0.24Zn0.76O製作MSM結構紫外光UV光偵測器，結果表示相比於氧化鋅薄膜元件有較高的紫外光-可見光互斥比2.78×103，可歸因於Mg0.24Zn0.76O光偵測器具有較低的暗電流0.08 pA和在XRD於(002)方向具有較小半高寬0.34°結果，表示Mg0.24Zn0.76O比氧化鋅具有更好的晶體品質。在5 V偏壓下和分別照光於350和380 nm時，顯示出，以Mg0.24Zn0.76O和ZnO的MSM光偵測器元件表現出的光響應度分別為0.4和0.32 A/W。
其次，我們成長具方向性氧化鋅奈米柱陣列，利用X射線繞射、掃描式電子顯微鏡、UV/Vis光譜、光致發光量測（PL）和微拉曼光譜量測結構和光電特性。顯示出擇優取向成長的纖鋅礦ZnO奈米柱結構成長方向為(002) C軸的方向。並應用至蕭特基光電二極體的製作。元件在370 nm波長和5 V偏壓下顯示出紫外光響應值(0.051 A/W)，這相當於21%的量子效率。
我們也在可撓式（PET）基板製作氧化鋅奈米柱MSM UV光偵測器並進行特性分析。結果顯示，相較於傳統的氧化鋅薄膜光感測元件，氧化鋅奈米柱的光感測元件有較高的光響應值和紫外光-可見光互斥比，分別是0.0409 A/W和282.59。製作新結構的光偵測元件顯示出較高的光響應值，可歸因於氧化鋅奈米柱的高比表面積特性。而氧化鋅表面存在的高密度的表面電洞缺陷對氧的吸附和解吸附導致了持續光導效應，促進載子傳送至元件。
另外，我們也探討了往深紫外光工作的MgZnO奈米柱光偵測元件的特性分析。結果也顯示出在UV/Vis光譜光吸收邊界，MgZnO奈米柱有短波長的光吸收特性（4.76 eV，260 nm）。MgZnO奈米柱光偵測元件的光響應值和紫外光-可見光互斥比分別為2.01 A/W和6.24×102。可歸因為MgZnO奈米柱高表面體積比和鎂的摻雜。實驗結果說明了MgZnO奈米柱有很大的潛力應用在深紫外線光電元件。
我們也研究利用液相沉積法(六水硝酸鋅，硝酸鎂，硝酸鋁)在90 °C成長溫度製作鎂-鋁共摻雜氧化鋅奈米柱陣列的結構和光學特性。在不同實驗條件生長的鎂-鋁共摻雜氧化鋅奈米柱的物理性能和光學特性，以X射線繞射、掃描式電子顯微鏡、紫外可見分光光度計、能量色散光譜儀，和光致發光光譜儀分析。結果顯示鎂-鋁共摻雜氧化鋅奈米柱棒具有成長方向(002) 的纖鋅礦結構，其中鎂原子沿c軸方向替代了鋅的位置和鋁共摻雜。我們在鎂-鋁共摻雜氧化鋅奈米柱陣列成功地結合了低電阻率的ZnO：Al和能隙調變的MgZnO。UV/Vis光譜光吸收邊界顯示了AlMgZnO奈米柱具有在短波長的光吸收反應（3.92 eV，316 nm）。而AlMgZnO奈米柱光偵測元件有深紫外線的光響應值和紫外光-可見光互斥比，分別為0.3 A / W和636.3。這些結果表明了氧化鋅為基礎的寬帶隙材料獨特的光學和電學可調性，有潛力作為未來的電子元件。
最後我們製作在可撓式基板(聚對苯二甲酸乙二醇酯，PET)以氧化鋅薄膜作為通道和銦錫氧化物(ITO)作為源、漏極的高性能半透明的薄膜電晶體(TFTs)。利用低溫濺射法在可撓式基板上製作元件。半透明電晶體元件具有低工作電壓(5 V)，高開/關比(4.1 × 108)，以及元件柵極長度(L)為8 μm於可撓式基板的閘極漏電流和透明度分別為12 nA和75 % (550 nm)。另外，氧化鉿閘極介電層製作ZnO-TFTs可撓式的元件，並探討不同的彎曲的條件下閘極漏電流(IG)，漏源電流(IDS)，開/關電流比(Ion/off)，和臨界電壓(Vth)元件特性分析。
最後，我們還探討了ZnO-TFT 元件之應用，利用ZnO-TFT 製作顯示器相關應用電路驅動LED和ZnO-TFT以電極連接於紫外線探測器，ZnO-TFT通過調整柵極電壓的以提高後者的光電流效率。當ZnO-TFT接通閘極偏壓 5 V時，相較於由偏壓為 0 V關閉通道，光電二極管的光電流效率增加了3倍。此外，我們成功地製作出可撓式元件(氧化鋅透明電薄膜電晶體，氧化鋅奈米柱光偵測元件)和操作在不同的彎曲條件下電流-電壓量測，並以原子力顯微鏡、紫外可見分光光度計去分析特性變化。

Developing integrated nanoelectronic, nanophotonic and nanomagnetic devices draw highly attractive potential as next-generation device architecture. ZnO-based semiconductors have been regarded as one of the strongest candidates for optoelectronic device considering their non-toxic, low cost, a direct wide band gap, electronic, optical, and piezoelectric properties. This dissertation describes the fabrication and characterization of optoelectronic devices (photodetectors, photoconductor, and field-effect transistors) with metal doping ZnO in glass and flexible substrates. The main investigation can be divided into the following four parts.
First, we elucidate the characteristics of ZnO-based metal-semiconductor-metal photodetectors with and without a ZnO cap layer were fabricated on flexible substrates of poly(ethylene terephthalate) (PET) for comparative analysis. The ZnO films were prepared by a low-temperature sputtering process. The Schottky barrier height at the Ag/ZnO interface is also determined to be 0.782 eV. The photodetector with a ZnO cap layer (stack structure: ZnO/Ag/ZnO/PET) shows a much higher UV-to-visible rejection ratio of 1.56×103 than that without. This can be attributed to the photocurrents that are not only significantly increased in the UV region but also slightly suppressed in the visible region for such a novel structure. With an incident wavelength of 370nm and an applied bias of 3 V, the responsivities of both photodetectors with and without a ZnO cap layer are 3.8×10-2 and 2.36×10-3 A/W, which correspond to quantum efficiencies of 1.13 and 0.07 %, respectively.
Additionally, the Ti/Au Ohmic contacts to both Mg0.24Zn0.76O and ZnO film-based metal-semiconductor-metal (MSM) photodetectors (PDs) were fabricated on glass substrates for comparative analysis. The transmittance spectra measured around the optical energy gap revealed that Mg0.24Zn0.76O films have a larger optical energy gap (3.54 eV) than ZnO films (3.25 eV). Mg0.24Zn0.76O MSM-structured ultraviolet (UV) PDs show a much higher UV-to-visible rejection ratio of 2.78×103 than those made of ZnO films. This can be attributed to the low dark current (0.08 pA) of the Mg0.24Zn0.76O UV PDs and the small full width at half maximum (0.34°) of the Mg0.24Zn0.76O (002) x-ray diffraction peak, indicating better crystal quality than that of ZnO. With an applied bias of 5 V and illuminations at 350 and 380 nm, the Mg0.24Zn0.76O and ZnO film-based MSM PDs exhibited responsivities of 0.4 and 0.32 A/W, respectively.
Second, we demonstrate the structural and optoelectronic characteristics of the well-aligned ZnO nanorod arrays were achieved by means of X-ray diffraction, scanning electron microscopy, transmission electron microscopy, photoluminescence (PL) and micro-Raman spectroscopy. The results indicated that the well-aligned ZnO nanorod with wurtzite structure was preferred oriented in the (002) c-axis direction. ZnO nanorod-based Schottky-barrier photodiodes has been also fabricated and characterized. With an incident wavelength of 370 nm and 5 V applied bias, it was found that maximum photoresponsivity of the photodiode was 0.051 A/W, which corresponded to a quantum efficiency of 21 %.
We also describe the fabrication of metal-semiconductor-metal ultraviolet photodetectors on flexible polyethylene terephthalate (PET) substrates with ZnO nanorods have been characterized. The photoresponsity and UV-to-visible rejection ratio of the ZnO nanorod-based sensor were 0.0409 A/W and 282.59, respectively. Compared to a traditional ZnO photodetector without nanorods, the fabricated novel photodetector showed much higher photoresponsity which could strongly depend on oxygen adsorption and desorption in the presence of trap states at the nanorods surface. It can be attributed to high surfaceto-volume ratio of ZnO nanorods.
Additionally, the deep-ultraviolet photodetectors on glass substrates with MgZnO nanorods have been characterized. The measured transmittance spectra around the absorption edge results reveal that the MgZnO nanorods have the absorption edge (4.76 eV, 260 nm). The photoresponsity and UV-to-visible rejection ratio of the MgZnO nanorod-based photodetectors were 2.01 A/W and 6.24×102, respectively. It can be attributed to high surface-to-volume ratio of MgZnO nanorods and doping the Mg. The improved performance reveals that the MgZnO nanorods have great potential applications in deep-ultraviolet optoelectronic devices.
We also describe the structural and Optical characteristics of the Mg-Al codoping ZnO nanorod arrays were fabricated at temperatures as low as 90 °C via a liquid phase deposition using zinc nitrate hexahydrate, magnesium nitrate, aluminium nitrate. Physical properties of the as grown ZnO nanorod arrays and optical properties of the fabricated devices will be also discussed by means of X-ray diffraction, scanning electron microscopy, UV-Vis spectrophotometer, energy dispersive spectrometer, and photoluminescence. The results indicated that the well-aligned Mg-Al codoping ZnO nanorod with wurtzite structure was preferred oriented in the (002) c-axis direction. The structural optical characteristics observed in this study are the result of the combined effect of structural defects, the substitution of Mg into Zn site along the c axis, and codoping of Al. Finally, we succeeded in combining the low resistivity of ZnO:Al and the band gap shift of MgZnO in Mg-Al codoping ZnO nanorod arrays. The measured transmittance spectra around the absorption edge results reveal that the AlMgZnO nanorods have the absorption edge (3.92 eV, 316 nm). The photoresponsity and UV-to-visible rejection ratio of the AlMgZnO nanorod-based photodetectors were 0.3 A/W and 636.3, respectively. These results demonstrate the unique tunability of the optical and electrical properties of the ZnO-based wideband gap material for future electronic devices.
Finally, we demonstrate high-performance semitransparent thin-film transistors (TFTs) on flexible substrates (polyethylene terephthalate, PET) with ZnO thin films as the active channel and indium tin oxide (ITO) as the source, drain, and gate electrodes. The transistors were prepared through low-temperature sputtering, which allowed device fabrication even on flexible substrates. Transparent transistors with a low operating voltage (5 V), high on/off ratio (4.1 × 108), and a gate length of 8-µm were built on flexible substrates; the gate leakage current and transparency were found to be approximately 12 nA and 75 % (550 nm) on average, respectively. In addition, the flexible device sputter-HfO2 gate dielectric layer was fabricated and successfully operated under different bend conditions for gate leakage current (IG), drain-source current (IDS), current on/off ratio (Ion/off), and threshold voltage (Vth).
Additionally, we also describe the fabrication of driving LED(Light Emitting Diode) of ZnO-TFT for display applications and ZnO -TFT is connected electrically to the ultraviolet photodetectors in order to enhance the latter’s photocurrent efficiency by adjusting the gate voltage of the TFT. When the TFT is switched on by biasing a gate voltage of 5 V, the photocurrent efficiency of the photodiode is three times higher than that when the TFT is switched off by biasing a gate voltage of 0 V. In addition, the flexible device (ZnO-TFTs and ZnO nanorod-PDs)fabricated and successfully operated under different bend conditions for I-V, AFM, and UV/Vis.

中文摘要 ………………………………………………… i
英文摘要 ………………………………………………… iv
誌謝 ………………………………………………… vii
表目錄 ………………………………………………… x
圖目錄 ………………………………………………… xi
第一章 緒論…………………………………………… 1
1.1 光偵測器與電晶體之發展…………………… 1
1.2 軟性電子發展及特性………………………… 8
1.2.1 塑膠基板的發展……………………………… 8
1.2.2 塑膠基板特性………………………………… 9
1.3 研究動機……………………………………… 12
第二章 文獻探討……………………………………… 16
2.1 氧化鋅基本特性……………………………… 16
2.1.1 化學性質……………………………………… 16
2.1.2 物理性質……………………………………… 17
2.1.3 製作方法……………………………………… 18
2.1.4 應用領域……………………………………… 19
2.2 氧化鋅奈米結構及摻雜特性………………… 23
2.3. 軟電技術與檢測標準………………………… 26
2.3.1 標準制訂掌握先機…………………………… 26
2.3.2 撓曲檢測機台的發展與應用………………… 26
2.3.3 軟性薄膜基板檢測技術……………………… 27
2.4 氧化鋅國內外相關研究……………………… 29
2.4.1 國外部份……………………………………… 29
2.4.2 國內部分……………………………………… 34
第三章 研究內容與方法……………………………… 41
3.1 金屬半導體接觸理論………………………… 41
3.2 接觸電阻……………………………………… 42
3.3 基本操作原理………………………………… 44
3.3.1 光偵測器……………………………………… 44
3.3.2 電晶體工作原理……………………………… 44
3.3.3 薄膜應力生成之原理………………………… 47
3.3.4 液相沉積法成長奈米結構…………………… 48
第四章 實驗架構及步驟……………………………… 52
4.1 實驗架構……………………………………… 52
4.2 氧化鋅薄膜和奈米結構……………………… 56
4.2.1 氧化鋅薄膜及摻雜金屬……………………… 56
4.2.2 氧化鋅奈米結構及摻雜金屬………………… 56
4.3 材料分析及金屬摻雜影響…………………… 59
第五章 氧化鋅薄膜及摻雜應用於光偵測器………… 69
5.1 前言…………………………………………… 69
5.2 實驗方法……………………………………… 70
5.3 結果與討論…………………………………… 71
第六章 氧化鋅奈米結構及摻雜應用於光偵測器…… 75
6.1 前言…………………………………………… 75
6.2 實驗方法……………………………………… 77
6.3 結果與討論…………………………………… 78
第七章 氧化鋅薄膜場效電晶體及OEIC應用………… 83
7.1 前言…………………………………………… 83
7.2 實驗方法……………………………………… 83
7.3 結果與討論…………………………………… 84
7.4 OEIC應用……………………………………… 85
7.4.1 OEIC分類……………………………………… 85
7.4.2 以ZnO-TFT驅動發光二極體(LED)元件之應用 86
7.4.3 以ZnO-TFT放大器光電元件之應用……………86
第八章 基板撓曲於元件特性影響…………………… 93
8.1 彎曲條件定義………………………………… 93
8.2 元件撓曲特性影響…………………………… 94
第九章 結論與未來展望……………………………… 100
9.1 結論…………………………………………… 100
9.2 未來展望……………………………………… 101
參考文獻 ………………………………………………… 104
英文論文大綱…………………………………………… 118
簡歷 ………………………………………………… 123

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