臺灣博碩士論文加值系統

本篇論文我們探討，濺鍍機沉積出來的鈰鈦氧化層作為EIS感測膜（RF濺鍍瓦數為100)，再經由快速熱退火30秒下進行四種不同的溫度（600°С、700°С、800°С、900°С），經由實驗後我們發現鈰鈦氧化層在100濺鍍瓦數以及700°С的回火溫度下有較大的感測度（73 mV/pH）、較低的時漂現象（0.496 mV/hr）與遲滯現象（13.6 mV），不但感測度高且穩定。
我們將此結果應用在大腸癌基因的檢測，使用GPS以共價鍵的形式固定我們的大腸癌基因並進行量測，比較有無突變基因的電量變化。結果我們發現無突變基因較突變基因的結合率高。未來我們將以改善固定化方式與提升檢測準確度為我們研究的方向。期望此感測器在生物臨床檢驗上有更多的延伸應用。
為了提升在基因量測上的準確率，我們測試另一種EOHOS結構來量測，發現當有加入偏壓的時候，感測度有大量的提升，未來將會對這個結構有更多的研究。

In this thesis, we use sputter (RF power 100) to prepare cerium titanium oxide for the membrane of EIS sensor. Then annealed four temperatures (600°С、700°С、800°С、900°С) for thirty secs. By experiment we found out that CeTixOy sputter power 100 with RTA 700°С have higher sensitivity, lower drift rate and lower hysteresis, not only have high sensitivity but also stability.
We use this result for sensing colorectal cancer gene. We use GPS to fix colorectal cancer gene as covalent bonds and measurement then compare the charge shift between normal and mutant gene. It turns out that normal gene have higher combined rate. The future work is to improve the immobilized and enhance detection accuracy. Hope this sensor can have more extended application on biological clinical laboratory.
In order to improve the accuracy of gene measurement, we tested the EOHOS structure. It turns out that when we added bias on the device, the sensitivity has a lot of increasing. In the future we will have more research on this EOHOS.

Contents
指導教授推薦書
口試委員審定書
致謝 iii
摘要 iv
Abstract v
Contents vi
Figure caption ix
Table caption xii
Chapter 1 1
Introduction 1
1.1 Background 1
1.2 Motivation and Objective 3
1.3 EIS and ISFET 4
Chapter 2 6
Theory Description 6
2.1 EIS structure 6
2.2 Site-binding model 7
2.3 pH-ISFET operation mechanism 12
Chapter 3 17
Physical and Electrical Properties of CeTixOy/Si EIS structure 17
3.1 Material 17
3.2 RF sputtering 18
3.3 The fabrication process of EIS sensor 19
3.4 Physical properties of sensing membrane 20
3.4.1 XRD of CeTixOy film analysis 20
3.4.2 AFM of CeTixOy film analysis 20
3.4.3 XPS of CeTixOy film analysis 21
3.5 Sensing characteristics of EIS structure 22
3.5.1 Sensitivity of sensing membrane 22
3.5.2 Drift of sensing membrane 23
3.5.3 Hysteresis of sensing membrane 24
Chapter 4 38
Ce2TiO5 EIS structure for biosensor application 38
4.1 Introduction 38
4.2 Method of immobilization 40
4.3 Material and method 42
4.3.1 Colorectal cancer 42
4.3.2 Reagents 42
4.3.3 GPS 43
4.3.4 DNA immobilization and Experiment flow 43
4.4 Result and discussion 45
Chapter 5 51
Electrolyte-Oxide-High-k-Oxide-Semiconductor 51
5.1 Introduction 51
5.2 The fabrication process of EOHOS sensor 51
5.3 Sensitivity of sensing membrane 52
5.4 Summary 54
Chapter 6 60
Conclusion and Future Work 60
6.1 Conclusions 60
6.2 Future Works 61
Reference 62


Figure caption
Fig. 1- 1 The picture shows the Schematic cross-section of the ISFET. 5
Fig. 1- 2 Comparison of EIS and ISFET structures. 5
Fig. 2-1 Equivalent capacitance of the EIS structure. 14
Fig. 2- 2 Basic and multi-phase diagram of EIS structure. 14
Fig. 2- 3 Typical C-V curves for electrolyte-SiO2-Si EIS structure. Silicon dioxide thickness is 560Å on a (100) 10Ω-cm p-type. 15
Fig. 2- 4 Schematic representation of the site binding model. 15
Fig. 2- 5 Experimental results of the surface potential ( ) on the SiO2 surface, using the theoretical parameters pHpzc=2.2, β=0.14, pKa=5.7, pKb=1.3, Ns=5×1014 cm2 and CDL=20 μF/cm2. 16
Fig. 2- 6 Experimental results of the threshold voltage variation of the Al2O3 gate ISFET, using the theoretical parameters pHpzc=8, β=4.8, pKa=10, pKb=-6, Ns=8×1014 cm2 and CDL=20 μF/cm2. 16
Fig. 3-1 Schematic diagram of the self-designed RF sputtering system. 26
Fig. 3-2 EIS structure with CeTixOy sensing membrane. 27
Fig. 3- 3 Flow chart of CeTixOy EIS process. 28
Fig. 3-4 XRD analysis of Ce2TiO5 films with different annealing temperatures. 29
Fig. 3-5 XRD analysis of CeTiO3 films with different annealing temperatures. 29
Fig. 3-6 3x3μm AFM three domain image of Ce2TiO5 film with 600°С RTA (Rms=0.847 nm). 30
Fig. 3-7 3x3μm AFM three domain image of CeTiO3 film with 700°С RTA (Rms=3.610 nm). 30
Fig. 3-8 XPS spectra of the corresponding (a) Ce 3d, (b) Ti 2p, (c) O 1s energy levels of Ce2TiO5 sensing film annealed at various temperatures 31
Fig. 3-9 XPS spectra of the corresponding (a) Ce 3d, (b) Ti 2p, (c) O 1s energy levels of CeTiO3 sensing film annealed at various temperatures 31
Fig. 3-10 C-V curves of Ce2TiO5 EIS RTA at 600°C for all standard pH buffer solution. 32
Fig. 3-11 Extracted response voltages for varied pH with fitting the sensitivity and linearity of Ce2TiO5 and anneal with 600°C. 32
Fig. 3-12 C-V curves of CeTiO3 EIS RTA at 700°C for all standard pH buffer solution. 33
Fig. 3-13 Extracted response voltages for varied pH with fitting the sensitivity and linearity of CeTiO3 and anneal with 700°C. 33
Fig. 3-14 Drift rates of Ce2TiO5 layer after RTA at different temperatures. 34
Fig. 3-15 Drift rates of CeTiO3 layer after RTA at different temperatures. 35
Fig. 3-16 Hysteresis voltages of Ce2TiO5 on various RTA temperatures. 36
Fig. 3-17 Hysteresis voltages of CeTiO3 on various RTA temperatures. 36
Fig. 4-1 Structure formula of GPS. 47
Fig. 4-2 Scheme of the elementary activation reaction. 47
Fig. 4-4 The C-V curve of EIS structure for sample A reaction. 48
Fig. 4-5 The detection result of sample B. 49
Fig. 4-7 The detection result of sample C. 50
Fig. 4-8 The C-V curve of EIS structure for sample C reaction. 50
Fig. 5-1 EOHOS structure. 55
Fig. 5-2 EOHOS device structure. 55
Fig. 5-3 The C-V curves of EOHOS structure without bias. 56
Fig. 5-4 Sensitivity and linearity of EOHOS structure without bias. 56
Fig. 5-5 The C-V curves of EOHOS structure with bias 10V. 57
Fig. 5-6 Sensitivity and linearity of EOHOS structure without bias 57
Fig. 5-7 The C-V curve shift after added bias 10V. 58
Fig. 5-8 The C-V curves of EOHOS structure with bias -10V. 58
Fig. 5-9 Sensitivity and linearity of EOHOS structure without bias. 59
Fig. 5-10 The C-V curve shift after added bias -10V. 59


Table caption
Table. 3-1 Deposition conditions of CeTixOy thin film using RF sputtering system. 26
Table. 3-2 Sensitivity of Ce2TiO5 and CeTiO3 thin film after different RTA temperatures. 34
Table. 3-3 Drift of Ce2TiO5 and CeTiO3 thin film after different RTA temperatures. 35
Table. 3-4 Hysteresis of Ce2TiO5 and CeTiO3 thin film after different RTA temperatures. 37
Table. 4- 1 Data on ENFETs developed. 46

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