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研究生：	林俊廷 Lin, Chun-Ting
論文名稱：	氧化鋅摻鈮薄膜製備、表面改質及其運用於電阻式記憶體、光感測器:紫外光臭氧處理與真空退火 The Fabrication of ZnO:Nb Films, Surface Modifications for RRAMs and Photodetectors: UV-Ozone and Vacuum Annealing Effects
指導教授：	朱聖緣 Chu, Sheng-Yuan
學位類別：	碩士 Master
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：	2018
畢業學年度：	106
語文別：	英文
論文頁數：	87
中文關鍵詞：	鈮摻雜、氧化鋅、電阻式記憶體、後處理、光感測器
外文關鍵詞：	Nb-doped, Zinc oxide (ZnO), resistive random access memory (RRAM), post treatment, photodetector
相關次數：	點閱：90 下載：2
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氧化鋅是具有寬能隙及高激子束缚能的半導體材料，擁有優異的電學、光學、聲波及機械特性。文獻中有許多致力於改善氧化鋅薄膜結構和電性的方法。其中，摻雜是在半導體製程中被廣泛運用於提升電性的方法。在本論文，我們使用射頻濺鍍法製備氧化鋅摻雜鈮薄膜(NZO)並將其運用在電阻式記憶體及光感測器上以改善其元件特性。
在本實驗的第一部分，藉由濺鍍製備不同鈮摻雜濃度之氧化鋅摻鈮薄膜並探討其材料特性，後將不同濃度的薄膜應用在電阻式記憶體上。實驗發現藉由摻雜鈮可以減少元件功率消耗並增加其穩定度，相較原先純氧化鋅元件可以擁有比較低的1.21V set操作電壓。
而在本實驗的第二部分，為了呈現出較低的位元錯位率而提高記憶窗，我們使用二種不同後處理方法以改善NZO薄膜特性並運用於元件上，包括UV ozone 及真空退火，可以使記憶窗分別從102 提升至 5×103 和 104。
最後，我們探討氧化鋅薄膜運用於光感測器的傳導機制，並藉由摻雜鈮以改善光感測器的元件特性。

Zinc oxide (ZnO) is a conventional semiconductor material exhibiting a large exciton energy (~ 60 meV), direct band gap (~3.3 eV) which has many unique electrical, optical, acoustic and mechanical properties. There are many proposals for enhancing the structural and electrical properties of ZnO thin films in the literature. Among them, doping is a crucial process for the semi-conductor fabrication and it is widely used to modulate the electrical properties. In this study, we attempt to improve the structural and electrical properties of ZnO thin films by doping niobium (Nb) with regard to their potential application to resistive random access memory (RRAM) and photodetectors.
In the first part of this study, various concentration of Nb-doped ZnO (NZO) thin films are deposited on Pt/TiO2/SiO2/Si substrates by radio frequency (RF) magnetron sputtering system. The detailed investigation of material characteristics in all NZO thin films is presented.
In the second part of this study, the proposed NZO thin films are applied to the solid-electrolyte of RRAMs. The electrical characteristic, reliability test, conduction mechanism of the devices is also examined. NZO films show low power consumption and high stability with a low set voltage of 1.21V compared with ZnO films.
In the third part of this study, in order to have low bit error rate with a high memory window, we use two post treatments to our NZO films, including UV ozone and vacuum annealing, which make memory window improved from 102 to 5×103 and 104, respectively.
Finally, the corresponding mechanism of ZnO thin film based photodetectors is investigated and the device performance improved by Nb doping is also examined.
Keyword: Nb-doped, Zinc oxide (ZnO), resistive random access memory (RRAM), post treatment, photodetector

Table of contents
ABSTRACT	I
摘要	II
誌謝	III
Table of contents	IV
List of Tables	VIII
List of Figures	X
Chapter 1 Introduction	1
1.1 Background	1
1.1.1 Characteristics of Zinc oxide	1
1.1.2 Introduction to Non-Volatile Memory (NVM)	2
1.2 Motivation	4
Chapter 2 Theory and Literature Review	5
2.1 Nonvolatile memory	5
2.1.1 Ferroelectric random access memory (FeRAM)	5
2.1.2 Phase-change random access memory (PCRAM)	6
2.1.3 Magnetic random access memory (MRAM)	6
2.1.4 Resistive random access memory (RRAM)	7
2.3 Electrical properties of valence change memory (VCM)	11
2.3.1 Forming voltage	11
2.3.2 Operation method	11
2.3.3 Resistance ratio	12
2.3.4 Retention	12
2.3.5 Endurance	12
2.4 The Mechanism of Current Conduction	13
2.4.1 Ohmic Conduction	13
2.4.2 Tunneling Conduction	14
2.4.2.1 Direction Tunneling	14
2.4.2.2 Fowler-Nordheim (FN) Tunneling	14
2.4.3 Hopping Conduction	15
2.4.4 Space-Charge-Limited-Current (SCLC)	15
2.4.5 Schottky Emission	16
2.4.6 Poole-Frankel (PF) Emission	17
2.5 Basic concepts of and types of Photodetectors	18
2.5.1 Metal-Semiconductor junction	18
2.5.2 Semiconductor type of Photodetector	19
2.5.2.1 Principle of operation of the photodetector	19
2.5.2.2 Photoconductive detector	19
2.5.3 Electrical properties of photodetectors	20
2.5.3.1 Responsivity	20
2.5.3.2 Response time	20
Chapter 3 Experiments and Measurement Techniques	21
3.1 Experimental Methods	21
3.1.1 Synthesis of Zinc oxide: Nb (NZO)targets	21
3.1.2 ZnO: Nb thin films fabrication process	21
3.1.3 ZnO: Nb thin films post treatment process	22
3.1.4 ZnO: Nb RRAM fabrication process	22
3.2 Characterization for Materials and Devices	24
3.2.1 Alpha Step	24
3.2.2 RRAM characteristics Measurement	24
3.2.3 X-ray Diffraction (XRD) Spectroscopy	25
3.2.4 Scanning Electron Microscope (SEM)	25
3.2.5 X-ray Photoelectron Spectroscopy (XPS)	26
3.2.6 Atomic Force Microscope (AFM)	27
3.2.7 Photoelectron Spectrometer (model AC-II from Riken Keiki Co. Ltd.)	27
Chapter 4 Results and Discussions	28
4.1 Material Characteristics of ZnO doping Nb (NZO) Thin Films	28
4.1.1 Analysis of ZnO: Nb Crystallinity	28
4.1.2 Morphology of ZnO doping Nb Thin Films	31
4.1.3 Chemical Composition of ZnO: Nb Thin Films	33
4.1.4 Work Function of ZnO doping Nb Thin Films	37
4.2 Influence of the doping content on the electrical properties of NZO	38
4.2.1 RRAM’s characteristics	38
4.2.2 Switching mechanism of Pt/NZO/Pt devices	50
4.2.3 Reliability measurement	54
4.2.4 Summary	59
4.3 Influence of post treatment to NZO thin films on the electrical properties of NZO Resistive Random Access Memory	60
4.3.1 Material Characteristics of NZO Thin films under UV ozone treatment	60
4.3.1.1 Chemical Composition of NZO UV Thin films under UV ozone treatment	60
4.3.1.2 Work Function of NZO Thin films under UV ozone treatment	64
4.3.2 NZO dielectric layer under UV ozone treatment for RRAMs	64
4.3.2.1 RRAM’s characteristics	64
4.3.2.2 Reliability measurement	66
4.3.3 Material Characteristics of NZO Thin films with post annealing treatment	68
4.3.3.1 Material Characteristics of NZO Thin films with post annealing treatment	68
4.3.4 Post annealing treated NZO dielectric layer for RRAMs	71
4.3.4.1 RRAM’s characteristics	71
4.3.3.2 Reliability measurement	73
4.4 NZO thin films for photodetectors	75
4.4.1 The photoconduction mechanisms of ZnO thin films	75
4.4.2 Influence of the Nb doping on the responsivity of ZnO-based photodetectors	77
Chapter 5 Conclusions and Future Works	80
5.1 Conclusions	80
5.2 Future works	81
References	82








List of Tables
Table 1.1 Performance parameters projected for the fully scaled emerging research memory technologies.	3
Table 2.1 The overview of doping in ZnO-Based RRAM	9
Table 2.2 The work function of metal and ITO	18
Table 3.1 Sputtering parameters of ZnO: Nb thin films.	22
Table 4.1 The average crystalline size and FWHM with different Nb content.	30
Table 4.2 Roughness values of NZO films with different contents.	32
Table 4.3 Work function of NZO films with different contents.	37
Table 4.4 Operation voltage of NZO films with different contents.	39
Table 4.5 Characteristics of the LRS state and the HRS state in Pt/NZO/Pt devices with different Nb contents.	42
Table 4.6 Properties of Pt/NZO/Pt devices in set process with different Nb contents.	45
Table 4.7 Properties of Pt/NZO/Pt devices in reset process with different Nb contents.	45
Table 4.8 The set voltage and switching stability of ZnO-based RRAMs.	59
Table 4.9 Work function of NZO films without/with UV ozone	64
Table 4.10 Characteristics of the LRS state and the HRS state in Pt/NZO-0.5/Pt devices with or without UV-ozone illumination	65
Table 4.11 Distribution of resistances in HRS of RRAM with/ without UV-ozone.	66
Table 4.12 FWHM of NZO films without/with vacuum annealing.	69
Table 4.13 Work function of NZO films without/with vacuum annealing.	71
Table 4.14 Characteristics of the LRS state and the HRS state in Pt/NZO-0.5/Pt devices with or without post annealing.	72
Table 4.15 Distribution of resistances in HRS with/ without annealing.	73
Table 4.16 The Responsivity of the ZnO device (a) without (b) with Nb doping.	77
Table 4.17 The Responsivity of ZnO-based photodetectors.	78

























List of Figures
Fig. 1.1 (a) Hexagonal wurtzite crystal structure of ZnO. (b) Hexagonal prism of ZnO crystal showing different crystallographic faces.	2
Fig 2.1 Magnetic random access memory operation method.	7
Fig 2.2 (a) metal-insulator-metal sandwich structure of RRAM. Schematic I-V curves of (b) unipolar (c) bipolar switching.	8
Fig 2.3 photoconductive detector.	20
Fig. 3.1 Fabrication processes and measurement of ZnO: Nb thin film and ZnO: Nb memory devices.	23
Fig. 3.2 The structure of NZO films based RRAM devices.	23
Fig. 3.3 Semiconductor parameter analyzer (Agilent 4155 C).	24
Fig. 3.4 Scanning electron microscopy measurement system.	25
Fig. 3.5 X-ray photoelectron spectroscopy.	26
Fig. 3.6 Atomic force microscope.	27
Fig 4.1 The X-ray diffraction patterns of NZO films with different Nb contents	29
Fig 4.2 FWHM of NZO thin films with different Nb contents	29
Fig 4.3 The peaks of the 2θ angles of NZO films with different Nb contents	30
Fig 4.4 SEM images of NZO films with different contents: (a) 0 (b) 0.2 (c) 0.5 and (d) 0.8 at%.	31
Fig 4.5 AFM images of NZO films with different content (a) 0 (b) 0.2 (c) 0.5 (d) 0.8 at%	33
Fig 4.6 XPS spectra of O-1s core levels of different Nb content: (a) 0 (b) 0.2 (c) 0.5 (d) 0.8 at%	36
Fig. 4.7 Typical unipolar I-V curves in linear scale of the Pt/NZO/Pt device with different content NZO films: (a) 0 (b) 0.2 (c) 0.5 and (d) 0.8 at%.	41
Fig. 4.8 Distribution of the switching voltages of the with different content NZO films: (a) 0 (b) 0.2 (c) 0.5 and (d) 0.8 at%.	44
Fig.4.9 Distribution of the resistances in the LRS and the HRS state with the different content NZO films: (a) 0 (b) 0.2 (c) 0.5 and (d) 0.8 at%.	47
Fig. 4.10 Schematic diagrams to illustrate the process of conductive filament formation in Nb-doped ZnO thin films. (a) Pt/ZnO:Nb(0.2%)/Pt, (c) Pt/ZnO: Nb (0.5%)/Pt, (e) Pt/ZnO: Nb (0.8%)/Pt in pristine state and (b) Pt/ZnO: Nb (0.2%)/Pt, (d) Pt/ZnO:Nb (0.5%)/Pt, (f) Pt/ZnO:Nb (0.8%)/Pt in low resistance state.	49
Fig.4.11 The switching curve of the different content NZO film devices are re-plotted in a double-logarithmic coordinate: (a) 0 (b) 0.2 (c) 0.5 and (d) 0.8 at%	52
Fig. 4.12 Current-Voltage behavior for a unipolar ReRAM during (1) Forming; (2) Reset and (3) Set processes.	53
Fig. 4.13 Reliability performances up to 100 switching cycles in Pt/NZO/Pt devices with different content NZO films: (a) 0 (b) 0.2 (c) 0.5 and (d) 0.8 at%.	56
Fig. 4.14 Retention time of the Pt/NZO/Pt memory cell with different content NZO films: (a) 0 (b) 0.2 (c) 0.5 and (d) 0.8 at%.	58
Fig.4.15 XPS spectra of: (a) Zn-2p (b) O-1s core levels as function of UV-ozone 30 min illumination.	61
Fig.4.16 XPS spectra of O-1s core levels of different UV-ozone illumination time: (a) 0 min (b) 30 min.	63
Fig 4.17 Typical unipolar I-V curves in linear scale of the Pt/NZO/Pt device with or without UV-ozone illumination.	65
Fig. 4.18 Reliability performances up to 100 switching cycles in Pt/NZO/Pt devices of different UV-ozone illumination time: (a) 0 min (b) 30 min.	67
Fig 4.19 The X-ray diffraction patterns of NZO films: (a) without (b) with 200。C annealing.	68
Fig 4.20 SEM images of NZO films: (a) without (b) with 200。C annealing.	69
Fig 4.21 XPS spectra of O-1s core levels of NZO films: (a) without (b) with 200。C annealing.	70
Fig 4.22 Typical unipolar I-V curves in linear scale of the Pt/NZO/Pt device with or without post annealing.	72
Fig. 4.23 Reliability performances up to 100 switching cycles in Pt/NZO/Pt devices (a) with (b) without annealing.	74
Fig. 4.24 Schematic band diagram of the Pt–ZnO thin film Schottky contact under UV light illumination.	76
Fig. 4.25 The current response curves of the ZnO device (a) without (b) with Nb doping.	79
                                    

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校內：2023-08-30公開
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