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請用此 Handle URI 來引用此文件: http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/66434
完整後設資料紀錄
DC 欄位值語言
dc.contributor.advisor陳銘堯
dc.contributor.authorChun-Tsung Suen
dc.contributor.author蘇俊聰zh_TW
dc.date.accessioned2021-06-17T00:35:38Z-
dc.date.available2017-03-19
dc.date.copyright2012-03-19
dc.date.issued2012
dc.date.submitted2012-02-06
dc.identifier.citationReferences
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dc.identifier.urihttp://tdr.lib.ntu.edu.tw/jspui/handle/123456789/66434-
dc.description.abstractIn this thesis, we investigate the development of phase-pure CuAlO2 film. CuAlO2 films were deposited on the c-plane sapphire substrates by radio-frequency (RF) magnetron sputtering using a CuAlO2 ceramic target at different deposition temperatures. The as-deposited films were found to be amorphous regardless of the deposition temperatures. After annealing at 1050 °C in air, only the film deposited at 700 °C showed the crystalline CuAlO2 structure but with a small amount of CuAl2O4 impurity. During post-annealing, Al in the sapphire substrate reacted with the as-deposited Cu–Al–O film so the whole film contained excess of Al, leading to the formation of CuAl2O4. To suppress CuAl2O4, a layer of 100 nm Cu2O film was deposited between the Cu–Al–O film and sapphire. In the annealing process, Cu2O reacted with sapphire to form CuAlO2 so the ratio of Cu to Al of the whole film was maintained, and a phase-pure CuAlO2 film without impurity was fabricated.
After the successful fabrication of phase-pure CuAlO2 film, the film was characterized, focusing on the crystal structure, electric and optical properties, and the surface morphology. In XRD, the film shows a highly preferred c-oriented structure. The electric conductivity of the phase-pure CuAlO2 thin film at room temperature is 1.01 S cm-1, which is almost two orders of magnitude better than that of the film with CuAl2O4 impurity. The p-type conduction was also confirmed by using the hot probe and Hall effect method. In the optical properties, the phase-pure CuAlO2 film is reasonably transparent in the visible region. The direct band gap fitted by the Tauc plot was found to be 3.3 eV. In the photoluminescence measurement, a near-band-edge (NBE) emission occurred at 3.27 eV was also found. The surface morphology was investigated by using FESEM and AFM. The specular surface of the as-deposited film was lost and the roughness increased after post-annealing. The surface morphology of phase-pure CuAlO2 film consists of stacked hexagonal facets with parallel edges, suggesting that the film may be grown epitaxially.
Finally, we try to find out whether the film was grown epitaxially or not by using the phi-scan measurement. The detail procedures of the phi-scan measurement performed by using the Bede D3 diffraction system were reported. We use a tricky method to exceed the hardware limit of the instrument. The film was confirmed to be grown epitaxially in the phi-scan measurement. We also found that 2H-CuAlO2, the relatively rare prototype of CuAlO2, coexisted in the epitaxial films in addition to 3R-CuAlO2
en
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dc.description.tableofcontentsContents
口試委員會審定書 i
誌謝 ii
中文摘要 iii
Abstract v
Chapter 1 Introduction 1
1.1 Introduction to Transparent Conducting Oxides 1
1.2 Development of p-type TCOs 1
1.3 The crystal structure of Delafossites 3
1.4 The chemical modulation of the valence band method 7
1.5 The lattice constant of CuAlO2 11
1.6 The origins of p-type conduction of CuAlO2 11
1.7 The previous works about the preparations of CuAlO2 thin films 14
1.7.1 PLD 18
1.7.2 DC sputtering 19
1.7.3 RF sputtering 21
1.7.4 The chemical solution methods 22
1.7.5 Summary 22
1.8 The phase diagram of CuAlO2 23
1.9 Our strategy to prepare CuAlO2 thin film 29
Chapter 2 The deposition instruments and experiment procedures 30
2.1 The deposition chamber 30
2.2 Sputtering 31
2.2.1 The principle of sputtering 31
2.2.2 The power supply of sputtering 32
2.2.3 Magnetron sputtering and the magnet design 33
2.2.4 The reactive sputtering 34
2.3 The preparation of CuAlO2 ceramic target 37
2.4 The experiment procedures 39
2.5 The post-annealing 41
Chapter 3 Characterization techniques 43
3.1 XRD 43
3.1.1 The x-ray generator 43
3.1.2 Bede D3 diffraction system 45
3.1.3 Bragg diffraction law 47
3.2 Electric analysis 48
3.3 Transmittance 52
3.4 Photoluminescence 53
3.5 Atomic force microscopy 55
Chapter 4 Phase development of phase-pure CuAlO2 thin films 58
4.1 The as-deposited and in-situ annealed Cu–Al–O film 58
4.2 Ex-situ annealing 60
4.3 The possible causes of the formation of CuAl2O4 64
4.4 The preparation of the phase-pure CuAlO2 films 71
4.5 HRXRD of CuAlO2 films 74
4.6 Similar structure and the thickness of Cu2O 77
4.7 Summary 78
Chapter 5 Characterization of CuAlO2 thin films 80
5.1 Optical properties analysis 80
5.1.1 The transmittance 80
5.1.2 The fitting of the band gap (the Tauc plot) 82
5.1.3 Photoluminescence 85
5.2 Electric properties 86
5.2.1 The room temperature conductivity 86
5.2.2 The carrier properties 87
5.2.3 The temperature-dependence conductivity of phase-pure CuAlO2 film 89
5.3 Surface morphology 95
5.3.1 Field-Emission SEM 95
5.3.2 Atomic force microscopy 97
Chapter 6 The phi-scan measurement 101
6.1 Epitaxy or highly preferred orientation 101
6.2 The procedures of phi-scan 102
6.3 The result of the phi-scan 110
6.4 Discussion about the rotational symmetry of CuAlO2 115
6.5 3R-CuAlO2 or 2H-CuAlO2 120
Chapter 7 Conclusion 125
Appendix 128
Appendix A: The CuAlO2 films prepared on A, M and R-plane sapphire substrates 128
A.1 XRD 128
A.2 The Raman spectrum 130
Appendix B: The variable range hopping 135
References 138
dc.language.isoen
dc.subject氧化銅鋁zh_TW
dc.subject快速退火zh_TW
dc.subject透明導電氧化物薄膜zh_TW
dc.subject射頻磁控濺鍍zh_TW
dc.subject磊晶zh_TW
dc.subjectEpitaxyen
dc.subjectTransparent conducting oxidesen
dc.subjectDelafossitesen
dc.subjectCuAlO2en
dc.subjectAnnealingen
dc.subjectRF sputteringen
dc.subjectPhi-scanen
dc.title利用射頻濺鍍法於c面氧化鋁基板上成長純相CuAlO2薄膜及其特性分析zh_TW
dc.titleDevelopment and characterization of phase-pure CuAlO2 thin films grown on c-plane sapphire substrates prepared by using RF sputteringen
dc.typeThesis
dc.date.schoolyear100-1
dc.description.degree博士
dc.contributor.oralexamcommittee楊鴻昌,陳政維,王立民,梁啟德
dc.subject.keyword透明導電氧化物薄膜,射頻磁控濺鍍,氧化銅鋁,快速退火,磊晶,zh_TW
dc.subject.keywordTransparent conducting oxides,Delafossites,CuAlO2,Annealing,RF sputtering,Epitaxy,Phi-scan,en
dc.relation.page151
dc.rights.note有償授權
dc.date.accepted2012-02-06
dc.contributor.author-college理學院zh_TW
dc.contributor.author-dept物理研究所zh_TW
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