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研究生： 林俊成
Lin, Chun-Cheng
論文名稱： 氧化鋅:鋰薄膜特性探討及其在電阻式記憶體與聲波感測器之應用
Characterization of Li-Doped ZnO Thin Films and Their Application to Resistive Random Access Memory Devices and Acoustic-Based Sensors
指導教授： 朱聖緣
Chu, Sheng-Yuan
學位類別： 博士
Doctor
系所名稱： 電機資訊學院 - 電機工程學系
Department of Electrical Engineering
論文出版年： 2016
畢業學年度： 105
語文別： 英文
論文頁數： 134
中文關鍵詞： 鋰摻雜 、電阻式記憶體 、薄膜體聲波諧振器 、感測器 、氧化鋅
外文關鍵詞： Li-doped, resistive random access memory (ReRAM), thin-film bulk acoustic-wave resonator (TFBAR), sensor, zinc oxide (ZnO)
相關次數： 點閱：86  下載：6 
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    • 氧化鋅為一具有寬能隙及高激子束缚能的N型多功能半導體，具備獨特的光學、電學、聲波及機械特性。因此，提升氧化鋅薄膜品質，乃其在實際應用上的重大課題。首先，本文利用「真空後退火法」及「同步直流偏壓濺鍍法」改善氧化鋅薄膜的微結構，藉此提升薄膜的壓電、鐵電及介電特性。
    再者，本文研究鋰摻雜氧化鋅薄膜製作之「非揮發性電阻式記憶體元件」，以調變鋰摻雜的原子百分比，藉此改變薄膜內部各種缺陷的比例，進而提升記憶體元件的「電阻切換比」；此外，藉由調變「限流大小」改變記憶體元件之電阻切換行為，使記憶體元件具備「多位元切換功能」，有效提升儲存效能。
    最後，本文研究以「紫外光臭氧後退火處理法」改善鋰摻雜氧化鋅薄膜之微結構與壓電特性，輔以「濕式蝕刻法」與「掀離法」，將鋰摻雜氧化鋅薄膜與金屬電極製作成「薄膜體聲波諧振器」， 並透過自建系統以量測薄膜體聲波諧振器對於「真空度」與「相對溼度」之感測功能。

    Zinc oxide (ZnO) is a direct wide-bandgap (Eg ~ 3.37 eV) n-type multifunctional semiconductor material with many unique electrical, optical, acoustic and mechanical properties. The literature contains many proposals for enhancing the structural and electrical properties of ZnO thin films and extending their applications. The present thesis focuses on improving the microstructure of Li-doped ZnO (LZO) thin films with particular regard to their potential application to resistive random access memory (ReRAM) devices and thin-film bulk acoustic-wave resonator (TFBAR) sensors.
    The thesis commences by investigating the use of an in-situ post-sputtering annealing process performed under vacuum conditions to improve the piezoelectric and ferroelectric properties of 3 at% LZO thin films grown by radio frequency (RF) magnetron sputtering. The results confirm that the piezoelectric and ferroelectric properties of the LZO thin film are both improved through a careful control of the annealing conditions. An enhanced RF magnetron sputtering process is then proposed in which 3 at% LZO thin films are prepared with a synchronous DC-bias voltage applied to the substrate in order to improve the structural, piezoelectric and dielectric properties of the films.
    In the second stage of the thesis, an investigation is performed into the potential of LZO films for non-volatile memory (NVM) applications. The investigations focus particularly on the effects of the Li dopant level on the formation and distribution of defects in the LixZn1-xO structure and the subsequent impact of these defects on the resistive random access memory (ReRAM) device performance. It is shown that the Li dopant concentration has a direct influence on the distribution of the defects in the LixZn1-xO film, and thus has a critical effect on the resistance ratio of the device. The multi-step (i.e., normal, 2-, 3-, and 4-step) RESET behavior of a 6 at% LZO ReRAM device is systematically explored under various compliance currents (CC) in terms of current-voltage (I-V) curves (RS cycles and linear fitting results), in-situ transmission electron microscopy (TEM) observations (evolution of the conductive filaments (CFs) within the ReRAM device), electrochemical impedance spectroscopy (EIS) measurements (Nyquist plot and equivalent circuit), and chemical bonds (Li+ ions).
    Finally, longitudinal-mode and contour-mode TFBARs are synthesized incorporating LZO films treated by UV-ozone illumination for 30 ~ 120 min. The microstructural, piezoelectric and energy binding properties of the various LZO films are examined and compared. The results show that the UV illumination process improves both the crystallization properties of the LZO films and their piezoelectric performance. In addition, it is shown that given an appropriate UV illumination time, the TFBARs exhibit a high resolution for atmospheric sensing and an approximately linear response for relative humilities in the range of 30 ~ 90%.

    Abstract I 中文摘要 III 致 謝 IV List of Author’s Journal Paper Publications V Table of Contents VI List of Figures IX List of Tables XIV Chapter 1: Introduction 1 1.1 Background 1 1.2 Motivation 2 1.3 Aims of thesis 5 Chapter 2: Theory and literature review 9 2.1 Properties of ZnO 9 2.1.1 Crystal structures and lattice parameters 9 2.1.2 Mechanical properties 11 2.1.3 Piezoelectric properties 12 2.1.4 Native defects in ZnO 16 2.1.5 Li dopants as donors or acceptors 17 2.2 Growth of ZnO thin-films by RF magnetron sputtering 18 2.2.1 Principles of RF magnetron sputtering 18 2.2.2 History of ZnO thin-films grown by RF magnetron sputtering systems 20 2.3 ZnO-based ReRAM devices 22 2.3.1 Basic concepts of ReRAM devices 22 2.3.2 Classification of switching mechanisms 24 2.3.3 Leakage current mechanisms 26 2.3.3.1 Ohmic behavior 26 2.3.3.2 Hopping conduction 27 2.3.3.3 Space charge limited current 27 2.3.3.4 Schottky emission 28 2.3.3.5 Poole-Frenkel emission 29 2.3.3.6 Fowler-Nordheim tunneling 29 2.3.3.7 Trap-assisted tunneling 30 2.4 ZnO-based TFBAR devices 31 2.4.1 Basic concepts and types of TFBAR 31 2.4.2 TFBAR device as sensors 33 Chapter 3: Improvements of LZO thin films 47 3.1 In-situ post-annealing technique 47 3.1.1 Target synthesis, substrate cleaning procedures, and sputtering conditions 47 3.1.2 Equipments setup, experimental results and discussion 47 3.2 Synchronous DC-bias voltages 52 3.2.1 Experimental procedures 52 3.2.2 Results and discussion 53 Chapter 4: LZO-based ReRAM devices 65 4.1 Unipolar RS behavior controlled by defect types 65 4.1.1 Experimental procedures 65 4.1.2 Results and discussion 65 4.2 Multi-step RS behavior controlled by compliance current 72 4.2.1 Experimental procedures 72 4.2.2 Results and discussion 74 Chapter 5: LZO-based TFBARs for sensing applications 93 5.1 Longitudinal-mode TFBAR for atmospheric sensing 93 5.1.1 Experimental procedures 93 5.1.2 Results and discussion 93 5.2 Contour-mode TFBAR for humidity sensing 96 5.2.1 Experimental procedures 96 5.2.2 Results and discussion 98 Chapter 6: Conclusions and future works 110 6.1 Conclusions 110 6.1.1 Improvements of LZO thin films 110 6.1.1.1 In-situ post-annealing technique 110 6.1.1.2 Synchronous DC-bias voltages 110 6.1.2 LZO-based ReRAM devices 111 6.1.2.1 Unipolar RS behavior controlled by defect types 111 6.1.2.2 Multi-step RS behavior controlled by compliance current 111 6.1.3 LZO-based TFBARs for sensing applications 112 6.1.3.1 Longitudinal-mode TFBAR for atmospheric sensing 112 6.1.3.2 Contour-mode TFBAR for humidity sensing 112 6.2 Future works 113 6.2.1 Conductance quantization behaviors in LZO-based ReRAM device 113 6.2.2 Piezoelectric sensor for touchscreen applications 113 References 118

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