本論文以溶膠－凝膠法及快速熱處理技術製備鉭酸鋰[LiTaO3，簡稱LT]焦電薄膜以作為紅外線感測元件之應用；利用旋鍍法將薄膜沈積於Pt/Ti/SiO2/Si(100)基板上，同時選擇1,3丙二醇為溶劑以減少達到薄膜所需厚度之披覆次數，並改變熱處理溫度(500~800℃)及升溫速率(600~3000℃/min)，探討不同製程參數對薄膜成長之影響，找出最佳製程參數並製作成紅外線感測器，另一方面為了減少元件熱傳導效應，利用非等向性溼式蝕刻法在感測元件之基板上作背部蝕刻，藉由蝕刻時間控制背部矽基板厚度(20~350μm)，研究矽基板厚度對於LiTaO3焦電薄膜紅外線感測器的影響。
實驗結果顯示，薄膜中製程升溫速率的快慢直接影響到LT薄膜的晶粒大小、介電性、鐵電性及焦電性；在薄膜特性方面，隨升溫速率的增加，LT薄膜的晶粒會有變小而緻密的趨勢，C軸優選排向有增強的趨勢，相對介電常數從28增加到45.6，介電損失則從0.009減少到0.003，而矯頑電場從122 KV/cm下降到60 KV/cm，殘留極化量從7.45

In this thesis, the lithium tantalite [LiTaO3, abbreviated to LT] thin films were deposited on Pt/Ti/SiO2/Si substrates by spin coating with sol-gel processing and rapid thermal processing. 1,3 propanediol was used as solvent to minimize the number of cycles of spin coating and drying processes to obtain the desired thickness of thin film. By changing the heating rate (600~3000℃/min) and the heating temperature (500~800℃), the effects of various processing parameters on the thin films growth are studied. In addition, the thermal isolation of detecting elements was achieved by the anisotropic wet etching of back silicon substrate. In order to reduce the thermal mass and thermal time constant of detector, the sensing element was built-up on a thin membrane. By changing the membrane thickness (20~350 μm), the effects of various membrane thickness on the response of pyroelectric IR detector devices are studied also.
Experimental results reveal that the heating rate will influence strongly on grain size, dielectricity, ferroelectricity and pyroelectricity of LT thin films. With the increase of heating rate, the grain size of LT thin film decreases slightly, and the c-axis orientation is enhanced. The relative dielectric constant (εr ) of LT thin film increases from 28 up to 45.6, the dielectric loss (tan

Abstract I
Content V
Chapter 1 Introduction 1
1.1 General background and motivation 1
1.2 Organization of this thesis 3
Chapter 2 Theory 6
2.1 The structure of LiTaO3 6
2.2 Ferroelectricity 6
2.3 Sol-Gel processing 7
2.4 The choice of precursor 8
2.5 Fabrication of the film 8
2.6 Rapid thermal annealing 9
2.7 Pyroelectric effect 9
2.8 Pyrolelctric response 11
2.9 Wet etching mechanism 16
2.9 Silicon etching 17
2.10 Sputtering 18
2.11 DC glow discharge 19
Chapter 3 Experiments 21
3.1 Fabrications of LiTaO3 thin films 21
3.1.1 Properties of precursors 21
3.1.2 Thin film deposition 22
3.1.3 Thermal processing 23
3.2 RTA furnace 24
3.2.1 Infrared gold image furnace 24
3.2.2 Comparison of the CTA and RTA 24
3.3 XRD analysis 25
3.4 SEM analysis 25
3.5 AFM analysis 25
3.6 Thickness analysis 26
3.7 SIMS (Secondary Ion Mass Spectroscopy) 26
3.8 Electrical measurements 26
3.9 Fabrication of traditional IR detectors without back surface etching 26
3.10 Fabrication of IR detectors with back etching 27
3.11 Dynamic response measurement 29
Chapter 4 Results and discussion 31
4.1 The analysis of the solution 31
4.1.1 The composition analysis of the solution 31
4.1.2 Differential thermal analysis (DTA) and Thermogravimetric analysis (TGA) 31
4.2 The thickness analysis of the film 32
4.3 Orientation analysis of the films 32
4.3.1 The effects of annealing temperature 32
4.3.2 The effects of heating rate 32
4.3.3 XRD comparisons of RTA and CTA 33
4.4 Surface morphology analysis 34
4.4.1 The effect of the annealing temperature 34
4.4.2 The effect of the heating rate 34
4.4.3 SEM comparisons of RTA and CTA 35
4.5 AFM analysis 35
4.6 SIMS analysis 35
4.7 Dielectric constant 36
4.8 Dielectric loss 36
4.9 Current-Voltage measurement 37
4.10 Leakage Current mechanisms 37
4.11 P-E measurement 39
4.12 Pyroelectric coefficient measurement 39
4.13 The characteristics of the thin film detectors without back surface etching 40
4.13.1 Voltage responsivity (RV) and current reponsivity (RI) 40
4.13.2 The noise voltages (Vn) 42
4.13.3 The noise equivalent power (NEP) and the specific detectivity (D*) 42
4.14 The characteristics of the thin film detectors with back surface etching 43
4.14.1 Si3N4 etching 43
4.14.2 SiO2 etching 44
4.14.3 Si etching in KOH solution 44
4.14.4 The microstructure of silicon etching 45
4.14.5 Voltage responsivity (RV) 45
4.14.6 Thermal time constant (τt) 46
4.14.7 The Noise voltages (Vn) 46
4.14.8 The specific detectivity (D*) 47
4.14.9 Comparison of the IR detector with and without back etching 47
4.15 Comparisons of this work with published studies 48
Chapter 5 Conclusion 49
Chapter 6 Future works 51
References 52
Fig. 2-1 Stereoscopic view of the lithium tantalite crystal structure. 63
Fig. 2-2 Stereoscopic view of the bonding topography around tantalum 64
Fig. 2-3 Hysteresis loop of ferroelectric material. 65
Fig. 2-4 The schematic diagram of the spin coating process. 66
Fig. 2-5 Pyroelectric effect. 67
Fig. 2-6 A pyroelectric detector element. 68
Fig. 2-7 A common pyroelectric detecting system. 69
Fig. 2-8 Variation in voltage responsitivity RV with frequency. 70
Fig. 2-9 Orientation-dependent etching. (a) Through window patterns on <100>-oriented silicon; (b) through window patterns on <110>-oriented silicon. 71
Fig. 2-10 Voltage versus current characteristic for three types of self-sustained discharges (p= 2 to 30 Pa). 72
Fig. 2-11 Features of a dc glow discharge system. 73
Fig. 3-1. The flow diagram for preparation of LiTaO3 films. 74
Fig. 3-2 The schematic diagram of the DC magnetron sputtering system. 75
Fig. 3-3 The schematic diagram of the infrared gold image furnace. 76
Fig. 3-4 The metal foil mask(mm). 77
Fig. 3-5 The traditional single IR detector. 78
Fig. 3-6 Fabrication process of the LiTaO3 thin film IR detector with back surface etching, (a) Pt/Ti bottom electrode deposition, (b) Al/LiTaO3 deposition, (c) backside etch-window patterning, and (d) backside bulk-silicon etching. 79
Fig. 3-7 (a)Cross section of etching fixture used to protect front devices during etch in hot KOH, and (b) top view of detector. 80
Fig. 3-8 The schematic diagram of the IR detector measurement system. 81
Fig.4-1 TGA-DTA curves of the LiTaO3 solution. 82
Fig.4-2 A cross-sectional photograph of LiTaO3 film annealed at 700℃ 83
Fig.4-3 XRD results as a function of annealing temperature for LiTaO3 films annealed by CTA for 1 hour. 84
Fig.4-4 XRD results as a function of heating rate for LiTaO3 films annealed at 700℃ for 2 min. 85
Fig. 4-5 The f factor as a function of heating rate for LiTaO3 films annealed at 700℃ for 2 min. 86
Fig. 4-6 XRD results of the LiTaO3 thin films annealed by CTA method at 700 oC for 1h (a), and RTA method at 700oC for 2min (b). 87
Fig. 4-7 The SEM surface morphologies of LiTaO3 films annealed at, (a) 500 oC, (b) 600 oC, (c) 700 oC, and (d) 800 oC with heating rate of 1800oC/min. 88
Fig. 4-8 The SEM surface morphologies of LiTaO3 films annealed at 700℃ with heating rate of, (a) 600 ℃/min, (b) 1200 ℃/min, (c) 1800 ℃/min, (d) 2400 ℃/min, and (e) 3000 ℃/min. 89
Fig. 4-9 SEM of the LiTaO3 thin films annealed by CTA method at 700 oC for 1h (a), and RTA method at 700oC for 2min (b). 90
Fig. 4-10 AFM images of LiTaO3 films annealed at 700℃ with heating rate of, (a) 600 ℃/min, (b) 1800 ℃/min, and (c) 3000 ℃/min. 91
Fig. 4-11The SIMS analysis for LiTaO3 thin film. 92
Fig. 4-12 Heating rate dependence of dielectric properties for the LiTaO3 thin films 93
Fig. 4-13 Heating rate dependence of leakage current density for LiTaO3 thin films 94
Fig. 4-14 Log J-E1/2 plots of LiTaO3 thin films annealed at heating rate of, (a) 600 oC /min, (b) 1800 oC /min, and (c) 3000 oC/min. 95
Fig.4-15 The Sawyer-Tower circuit. 96
Fig. 4-16 Ferroelectric hysteresis loops of LiTaO3 thin films annealed at 700℃ with heating rate of, (a) 600℃/min, (b) 1800℃/min, and (c) 3000℃/min. 97
Fig. 4-17 Heating rate dependence of the coercive field (Ec) and remnant polarization (Pr) for LiTaO3 thin films 98
Fig. 4-18 The schematic diagram of the pyroelectric current measurement system. 99
Fig. 4-19 Heating rate dependence of pyroelectric coefficient for LiTaO3 thin films. 100
Fig. 4-20 Dependences of the figures of merit Fv and Fm on heating rate. 101
Fig. 4-21 Frequency dependence of the voltage responsivity (RV) and current reponsivity (RI) of LiTaO3 thin film IR detector with heating rate of 600℃/min. 102
Fig. 4-22 Frequency dependence of the voltage responsivity (RV) and current reponsivity (RI) of LiTaO3 thin film IR detector with heating rate of 1800℃/min. 103
Fig. 4-23 Frequency dependence of the voltage responsivity (RV) and current reponsivity (RI) of LiTaO3 thin film IR detector with heating rate of 3000℃/min. 104
Fig. 4-24 Dependence of the maximum voltage reponsivity on heating rate at 20Hz. 105
Fig. 4-25 Frequency dependence of the noise voltage per unit bandwidth for LiTaO3 thin film IR detectors without back side etching. 106
Fig. 4-26 Frequency dependence of the noise equivalent power and the specific detectivity of LiTaO3 thin film IR detector with heating rate of 600℃/min. 107
Fig. 4-27 Frequency dependence of the noise equivalent power and the specific detectivity of LiTaO3 thin film IR detector with heating rate of 1800℃/min. 108
Fig. 4-28 Frequency dependence of the noise equivalent power and the specific detectivity of LiTaO3 thin film IR detector with heating rate of 3000℃/min. 109
Fig. 4-29 Dependence of the maximum specific detectivity on heating rate at 300Hz. 110
Fig. 4-30 Etch rate as a function of temperature for Si3N4 in H3PO4 etchant. 111
Fig. 4-31 Etch rate as a function of temperature for SiO2 in BOE etchant. 112
Fig. 4-32 Etch rate as a function of temperature for silicon in KOH etchant. 113
Fig. 4-33 Etch rates as a function of stirred speed for silicon in KOH etchant. 114
Fig. 4-34 The photograph of backside bulk-silicon etching. 115
Fig. 4-35 Various etched depths of silicon, (a) 120μm, (b) 150μm, (c) 170μm, (d) 270μm, (e) 370μm, (f) 470μm. 116
Fig. 4-36 The modulation frequency dependence of Rv for the LiTaO3 thin film IR detectors on various thickness of membrane. 117
Fig. 4-37 Membrane thickness dependence of the thermal time constant (τt) for detectors. 118
Fig. 4-38 Dependence of the voltage responsivity on membrane thickness at 20 Hz. 119
Fig. 4-39 Frequency dependence of the noise voltage per unit bandwidth for LiTaO3 thin film IR detectors. 120
Fig. 4-40 The modulation frequency dependence of the specific detectivity for LiTaO3 thin film IR detectors. 121
Fig. 4-41 Dependence of the specific detectivity on membrane thickness at 100 Hz. 122
Fig. 4-42 Modulation frequency depended Rv, D* and Vn for LiTaO3 thin film IR detector with and without back etching. 123
Table 1 The characteristic parameters of LiTaO3 and LiNbO3. 124
Table 2 Deposition conditions of Pt film. 125
Table 3 The ratios of the XRD intensities of LiTaO3 films with various heating rates. 126
Table 4 The electrical and pyroelectric properties of the LiTaO3 thin films. 127
Table 5 The measured dielectric constants and β values of LiTaO3 thin films annealed at various heating rates. 128
Table 6 Comparison of electrical and pyroelectric properties of LiTaO3 film with published materials. 128
Table 7 Comparison of dynamic respones of this work with published reports 129

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