透明金屬氧化物於近紅外及近紫外光波長之應用

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研究生：	張恆睿
論文名稱：	透明金屬氧化物於近紅外及近紫外光波長之應用 Transparent Metal Oxides for Near-Infrared and Near-Ultraviolet Applications
指導教授：	吳孟奇
口試委員:	蘇炎坤劉文超許渭州陳英忠劉柏村劉埃森
學位類別：	博士 Doctor
系所名稱：	電機資訊學院 - 電子工程研究所 Institute of Electronics Engineering
論文出版年：	2014
畢業學年度：	102
語文別：	英文
論文頁數：	118
中文關鍵詞：	透明金屬氧化物、氧化銦鉬、氧化銦鎵鋅、高頻發光二極體、發光電晶體
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在本論文中，我們研製適用於近紅外及近紫外光波段的透明金屬氧化物，並完成其元件製備。透明金屬氧化物中的載子吸收造成其在近紅外光波段穿透率的下降，由於氧化銦鉬具有高價電差的材料特性，其在近紅外光波段的穿透率優於氧化銦錫等商用透明電極。因此，我們研製氧化銦鉬並應用於近紅外光高速發光二極體。藉由共濺鍍沉積之氧化銦鉬薄膜具有低電阻率(3.55 × 10-4 Ω-cm)及近紅外光波長高穿透率(99%)的材料特性。其後，我們應用電晶體概念設計具有雙極性結構的發光二極體晶片。藉由氧化銦鉬透明電極製程的導入，近紅外光發光二極體的發光功率可提昇兩倍；同時，藉由雙極性磊晶結構的設計，近紅外光發光二極體之頻率響應頻寬為649 MHz。此外，由於氧化銦鉬具有高功函數的材料特性，有利於有機元件中的電洞傳輸，因此我們進一步整合氧化銦鉬透明電極與有機太陽能電池。使用氧化銦鉬透明電極之太陽電池，其功率轉換效率可達3.77%；其未來將可和含近紅外吸收材料的有機太樣電池進一步結合應用。在近紫外光波長區段，金屬氧化物的穿透率主要取決於其光能隙大小。因此，我們研製寬能隙之氧化銦鎵鋅薄膜。藉由濺鍍製程的優化，氧化銦鎵鋅薄膜具有低電阻(7.16 × 10-4 Ω-cm)及近紫外光波長高穿透率的優點，未來可進一步應用於近紫外發光二極體及光偵測器等元件應用。

In this thesis, transparent metal oxides for near-infrared (NIR) and near-ultraviolet (NUV) are prepared and discussed, and their applications are further indicated. Indium molybdenum oxide (IMO) exhibited the material characteristic of valence difference of 3 between the In3+ matrix and Mo6+ dopants is feasible for NUV device applications. The optimum IMO film shows the characteristics of low electrical resistivity of 3.55 × 10-4 Ω-cm and high optical transmittance of 99% at 968 nm. Afterwards, a high-speed and high-light-output-power InGaAs/GaAs NIR LED at 968 nm wavelength employing IMO contact is constructed. As compared to NIR LED using AuGe contact, NIR LED using IMO contact produces a light output power with a rate of 5.7 μW/mA, which is twice of 2.7 μW/mA for NIR LED using AuGe contact at corresponding injection current level. These NIR LEDs exhibit the 3-dB optical bandwidth of 649 MHz, which is correlated to the carrier recombination lifetime of 245 ps. Besides, the IMO exhibits characteristic of high work function around 4.93 eV. Thus, the incorporation of IMO contact and P3HT/PCBM organic solar cells is discussed. Solar cell using optimum IMO contact shows an higher electrical power efficiency of 3.77%. Furthermore, indium gallium zinc oxide (IGZO) is constructed for future NUV applications. The optimization of IGZO preparation process is realized. IGZO with the wide optical band gap of 3.7 eV, shows a low electrical resistivity of 7.16 × 10-4 Ω-cm and a high optical transmittance in NUV wavelengths. IGZO is the alluring transparent contact for NUV device applications.

Contents
Acknowledgement    I
Abstrate (Chinese)    Ⅱ
Abstract (English)    Ⅲ
Contents    Ⅴ
Figure Captions    Ⅷ
List of Tables    ⅩⅡ 

Chapter 1 Introduction    1
Chapter 2 The Study of Structural, Electrical, and Optical Characteristics of Co-Sputtered Indium Molybdenum Oxide Films    6
2-1 Introduction    6
2-1-1 Paper Review    6
2-1-2 Drude Model    8
2-1-2 Band Gap Fundamentals    11
2-2 Experimental Methods    14
2-3 Results and Discussion    15
2-3-1 Structural characterization    15
2-3-2 Electrical characterization    18
2-3-3 Optical characterization    21
2-4 Summary    26
Chapter 3 The Applications: High Speed/High Light Output Power InGaAs/GaAs LED and Organic P3HT/PCBM Solar Cells    43
3-1 High Speed and High Light Output Power of InGaAs/GaAs LEDs with an Indium   Molybdenum Oxide Contact    43
    3-1-1 Introduction    43
3-1-2 Experimental    46
3-1-3 Results and Discussion    50
3-1-4 Summary    56
3-2 The Study of Co-Sputtered Indium Molybdenum Oxide Films for the Application to Organic Solar Cells    58
3-2-1 Introduction    58
3-2-2 Material and Methods    59
3-2-3 Results and Discussion    60
3-2-4 Summary    63
Chapter 4 RF Sputtered Low Resistivity and High Transmittance Indium Gallium Zinc Oxide Films for Near-UV Applications    77
4-1 Introduction    77
4-2 Experimental Methods    79
4-3 Results and Discussion    80
4-4 Summary    84
Chapter 5 Conclusions and Future Work    90

References    93
Publications List    103


















Figure Captions

Fig. 2- 1 E-k diagram of conductive In2O3.    30
Fig. 2- 2 The preparation process of IMO thin films.    31
Fig. 2- 3 Growth rate of (a) In2O3 and (b) Mo thin films as a function of RF power.    32
Fig. 2- 4 XRD patterns of IMO thin films as a function of Mo doping concentration.    33
Fig. 2- 5 XRD patterns of IMO thin films as a function of substrate temperature. The X-axis (2θ degree) is offset by 20%.    34
Fig. 2- 6 Effects of substrate temperature on peak intensity and FWHM of IMO films.    34
Fig. 2- 7 Effects of Mo dopant concentration on the resistivity, Hall concentration, and Hall mobility of IMO films.    35
Fig. 2- 8 Effects of post annealing on the resistivity, Hall concentration, and Hall mobility of IMO films.    36
Fig. 2- 9 Effects of substrate temperature on the resistivity, Hall concentration, and Hall mobility of IMO films.    37
Fig. 2- 10 Relationship between resistivity and FWHM.    38
Fig. 2- 11 Relationship between resistivity, Hall concentration, and Hall mobility.    38
Fig. 2- 12 Comparison of optical transmittance of IMO films of 2.36 wt% Mo concentration with and without post annealing.    39
Fig. 2- 13 Comparison of optical energy band gap of IMO films of 2.36 wt% Mo concentration with and without post annealing.    39
Fig. 2- 14 Effects of Mo dopant concentration on the optical transmittance of IMO films. IMO films were post annealed at 300℃ .    40
Fig. 2- 15 Optical transmittance of IMO films with 2.36 wt% Mo prepared at different substrate temperature.    41
Fig. 2- 16 Effect of post annealing on IMO films prepared at different substrate temperature. The Mo concentration in IMO films is 2.36 wt%.    41
Fig. 2- 17 Relationship between Hall concentration and band gap shift.    42
Fig. 2- 18 Plot of figure of merit vs resistivity of IMO films.    42

Fig. 3- 1 Process flow of NIR InGaAs/GaAs LEDs.    65
Fig. 3- 2 Top view of the NIR InGaAs/GaAs LED.    66
Fig. 3- 3 Schematic cross section of fabricated NIR LED structure. The carrier flows are shown as arrows.    66
Fig. 3- 4 The radius of CTLM varies from 4 to 52 μm.    67
Fig. 3- 5 Calculation of CTLM model.    67
Fig. 3- 6 Plot of the measured resistance as the function of the distance difference between the inner circular and the outer IMO contacts    68
Fig. 3- 7 I-V characteristics of IMO/n-type GaAs contacts annealed at different temperatures.    69
Fig. 3- 8 I-V characteristics of IMO/n-type GaAs contact annealed at 600℃. CTLM measurement is used to obtain the specific contact resistance.    69
Fig. 3- 9 Optical transmittance spectrum of IMO contact after annealing at 300℃. The transmittance spectra of as-deposited IMO and ITO are also revealed for comparison.    70
Fig. 3- 10 I-V characteristics of NIR LED using IMO, ITO and AuGe contacts on top GaAs contact layer.    70
Fig. 3- 11 EL characteristics of the NIR LED using an AuGe contact.    71
Fig. 3- 12 EL characteristics of the NIR LED using an IMO contact.    71
Fig. 3- 13 Comparison of EL characteristics of NIR LEDs using IMO and AuGe contacts. Injection current level is 30 mA.    72
Fig. 3- 14 EL intensity of NIR LEDs using IMO and AuGe contacts as a function of injection current level.    72
Fig. 3- 15 Light output power as a function of bias current for NIR LEDs using IMO, ITO and AuGe contacts on the top GaAs contact layer.    73
Fig. 3- 16 Light output efficiency as a function of bias current for NIR LEDs using IMO, ITO and AuGe contacts on the top GaAs contact layer.    73
Fig. 3- 17 Optical response of NIR LED with IMO contact.    74
Fig. 3- 18 The modulation bandwidth and carrier recombination lifetime as a function of injection current for the NIR LED with IMO contact on the top GaAs contact layer.    74
Fig. 3- 19 Effects of Mo concentration on the J-V characteristics of solar cells utilizing IMO electrode. Solar cell utilizing ITO electrode is schematized for comparison.    75
Fig. 3- 20 Effects of IMO electrode post annealing condition on the J-V characteristics of solar cells utilizing IMO electrodes.    75
Fig. 3- 21 Comparison of electrical power density output of solar cells using IMO and ITO electrodes.    76

Fig. 4- 1 XRD patterns of IGZO films deposited on glass substrates at 25 and 175℃ by sputtering process.    87
Fig. 4- 2 Temperature dependence of the electrical resistivity, carrier concentration, and Hall mobility if the IGZO films    87
Fig. 4- 3 Optical transmittance spectra of IGZO films. The deposition temperature varies from 25 to 275℃.    88
Fig. 4- 4 The square of absorption coefficient as a function of photon energy.    88
Fig. 4- 5 XRD patterns of IGZO films with In concentration of (a) 18.91, (b) 23.00, and (c) 24.56 at%.    89
Fig. 4- 6 Optical transmittance of IGZO films of 18.19, 23.00, and 24.56 at% In concentration.    89





















List of Tables
 Table  1. Comparisons of electrical properties of IMO thin films prepared by differentdeposition methods.    29
Table  2. The epitaxial structure of the InGaAs/GaAs NIR LED.    64
Table  3. The deposited parameters of rf power supplied to the In2O3 target, the In contents, and the electrical characteristics for the IGZO films grown at the substrate temperature of 175℃.    86


                                

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