本論文的核心在於提供了以分子束磊晶法成長岩鹽礦結構的氧化鋅及摻鎂氧化鋅之成長參數、分析方法及重要結果。研究裡先是提供成長岩鹽礦結構的氧化鋅及摻鎂氧化鋅的參數，並且把岩鹽礦結構的氧化鋅及摻鎂氧化鋅關鍵的物理性質和材料性質量化。綜合研究的結果，歸納出益於岩鹽礦結構的氧化鋅及摻鎂氧化鋅的成長參數，這些成長參數被侷限於低的鋅等效流量比和低的成長速率。此外，針對不同鋅含量的岩鹽礦結構氧化鋅及摻鎂氧化鋅磊晶層，將其晶格常數、能隙、磊晶的品質等物理性質和材料性質特徵量測，並予以討論。論文中另有一部分從岩鹽礦結構氧化鋅及摻鎂氧化鋅磊晶層的臨界厚度、應力釋放、鋅含量極限等的理論和計算，討論了可能的成長模型。因此，接下來的三段為此論文最重要的結果與發現。
首先，在論文的第一部分，探討以分子束磊晶法在(100)面的氧化鎂基板上成長氧化鋅磊晶的磊晶成長行為。結果顯示在600 oc，氧化鋅磊晶層以(10-10)方位的非極性纖鋅礦成長。此磊晶層由四個變種的晶域組成，其磊晶關係為：(10-10)ZnO//(100)MgO和 <1-213>ZnO~//<011>MgO差異約為+/-1.5o。磊晶中發現有相當高密度的缺陷。因此在基板上先成長一層Zn0.6Mg0.4O的岩鹽礦結構摻鎂氧化鋅磊晶層後，其晶格失配可降低幾乎至零，在其上成長的纖鋅礦氧化鋅磊晶中缺陷密度大幅下降，因此，其光致發光的特性則大幅改善。
第二部分的實驗主要變數為磊晶成長的鋅鎂流量比。當鋅鎂流量比在0.94以下時，磊晶層維持為岩鹽礦結構，而其鋅含量可達0.83；反之，鋅鎂流量比在0.95以上時，磊晶層則為纖鋅礦結構。此部分的亮點，在於(100)面的氧化鎂基板上成功以分子束磊晶法成長的高鋅含量的岩鹽礦結構礦摻鎂氧化鋅磊晶層，其中一個試片鋅含量可高達0.83。此外，藉由X光繞射方法的鑑定，確定了不同鋅含量摻鎂氧化鋅磊晶層，始終保持岩鹽礦結構，並且得知鋅含量為0.5及0.83的晶格參數分別為0.4256及0.4278奈米，並從(200)面的X光搖擺曲線半高寬介於0.30o ~ 0.47o。磊晶的表面擁有原子級的平坦度，其方均根粗糙值約為1奈米。利用X光倒格子空間分析和穿透式電子顯微鏡的分析，顯示110 ~ 130奈米厚的磊晶層，晶格已呈現部分應力鬆弛的現象。除此之外，鋅含量達0.83的磊晶層在製備穿透式電子顯微鏡試片時，在削薄的過程中，磊晶層即從岩鹽礦結構相變化成纖鋅礦結構。在能隙方面，鋅含量0.5和0.83的岩鹽礦結構摻鎂氧化鋅磊晶層分別為5.33及4.73電子伏特。
最後一個部分是在(100)面的氧化鎂基板上成長岩鹽礦結構氧化鋅、摻鎂氧化鋅及氧化鎂異質結構的研究。結果顯示在七組異質結構試片中，除了H-ZMO-5之外，其餘試片上均有部分區域在成長異質結構階段相變態成纖鋅礦結構，而且量測到的能隙與模擬計算的結果十分相近。這些試片當中，有一項非常值得關注的是H-ZnO-30的試片，其岩鹽礦結構氧化鋅磊晶，它成功地和氧化鎂的互相堆疊成三十個週期的異質接面，並以大約在數個原子層的厚度存在著；此外，纖鋅礦氧化鋅及氧化鎂交互堆疊的異質結構也被觀察到，纖鋅礦氧化鎂穩定的被氧化鋅夾在其中，而其中可能有互擴散發生在這些磊晶層中。這兩種結構的異質結構同時存在於同一片試片但不同位置，其互相接合的介面，可推得與第一個部分相同的結果，關係式如下：(10-10)wurtzite//(100)rock-salt和 <1-213>wurtzite ~//<011>rock-salt。更重要的是，針對異質結構能隙的調變，讓能隙更降低到4.5電子伏特左右，增加了在紫外光區的範圍。

This thesis provides an overall experiments and discussions of depositing rock-salt (RS) type ZnO/ZnxMg1-xO epilayers and heterostructures in a plasma assisted molecular beam epitaxy system. The experiments support regardless of processing and characterizing the RS type ZnO/ZnxMg1-xO. A discussion of the processing was given, the growth of RS type ZnO/ZnxMg1-xO films is limited to low beam equivalent pressure ratios of Zn and growth rates. The ZnO/ZnxMg1-xO films are characterized to have specific lattice parameters, band gap energies, and the film quality with different Zn contents. In addition, several models are proposed to discuss the RS type ZnO/ZnxMg1-xO, such as critical thicknesses, strain relaxation, limitation of the Zn content. The total phenomena are then summarized to give a simple growth model. This thesis therefore reports three major results.
In the first part, the growth were focused on the ZnO on (100)MgO substrate at 600 oC by plasma-assisted molecular beam epitaxy. Nonpolar (10-10)-oriented ZnO was grown epitaxially which was composed of four variant domains having an orientation relationship with the substrate as: (10-10)ZnO//(100)MgO and <1-213>ZnO~//<011>MgO with a +/-1.5o deviation. By introducing a RS type Zn0.6Mg0.4O buffer layer, the lattice mismatch was eliminated almost completely based on the extended coincidence lattice model. The crystal quality is therefore improved and the epilayer reveal better photoluminescence characteristics.
Following, the ZnxMg1-xO epitaxial layers were prepared with different beam equivalent pressure ratios by plasma-assisted molecular beam epitaxy on MgO (100) substrate. X-ray diffraction characterization revealed that both samples retain the RS structure and the lattice parameters are 0.4256 and 0.4278 nm for x = 0.52 and 0.83, respectively. In addition, the epilayers are with low FWHM values (0.30o ~ 0.47o) of the (200) rocking curves. The epilayer surfaces are flat having a root mean square roughness of 1.0 nm. According to reciprocal space map and transmission electron microscopy analyses, the epitaxial strains have been partly relaxed at film thicknesses of 110 ~ 130 nm. In fact, a further relaxation of the strain when preparing the TEM specimen from the Zn0.8Mg0.2O epitaxial layer triggers back transformation of the RS to the wurtzite structure. The band gap energy of the Zn0.8Mg0.2O epitaxial layer was found to be as low as 4.73 eV.
In the last part, RS type ZnO/ZnxMg1-xO/MgO heterostructures are deposited on lattice-matched MgO substrates. The results revealed six heterostructure samples (excluding sample H-ZMO-5) are facing phase transformation from rock-salt to wurtzite phase during the heterostructure or capping layer growth. In addition, the energy gaps that measured are similar to the values from the simulations. It is worth noting that RS type ZnO is obtained by embedded MgO layers to form a periodic heterojunctions in very thin layers. Besides, the wurtzite ZnO/MgO alternative layers are observed in the heterostructures. The wurtzite MgO sandwiched between ZnO layers was to stabilize as very thin layers. The dual phase of ZnO/MgO epilayers occurred in different areas within a sample. The interface of these areas provide a good opportunity to solve the orientation relationship between wurtzite structure and rock-salt structure, which has the same results as that derived in the (10-10)-oriented ZnO/MgO epilayer as: (10-10)wurtzite//(100)rock-salt and <1-213>wurtzite ~//<011>rock-salt. In addition, the band gap engineering by the present process has narrowed down the energy to 4.5 eV, i.e. extending toward lower UV region.

Dissertation Examination Report i
Acknowledgement ii
中文摘要 iv
English Abstract vi
Contents ix
List of Tables xiv
List of Figures xvi
List of Abbreviations xxvi
List of Symbols xxviii
Chapter I Introduction and Motivation 1
1.1 Introduction 1
1.2 Organization of the dissertation 4
Chapter II Literature Review 6
2.1 Zinc Oxide (ZnO) 6
2.1.1 Zinc blende structure ZnO 7
2.1.2 Epitaxial growth of zinc blende ZnO 8
2.1.3 Rock-salt structure ZnO 8
2.2 Magnesium oxide (MgO) 10
2.3 ZnxMg1-xO (ZMO) Alloy 11
2.3.1 Epitaxial growth of rock-salt structure ZMO 12
2.3.2 Stability of rock-salt structure ZMO 14
2.4 Epitaxial growth mechanism 16
2.4.1 Nucleation and growth modes 17
2.4.2 Lattice mismatch between epitaxial films and substrates 20
2.4.3 Lattice mismatch and the growth model 20
2.4.4 Growth modes and kinetic considerations 22
2.4.5 Critical thickness 23
2.5 Molecular Beam Epitaxy (MBE) 24
2.5.1 Introduction of MBE 24
2.5.2 MBE system 25
2.5.3 Conditions in MBE 27
2.5.4 Growth mechanisms in MBE 29
2.6 Optical and electrical properties of rock-salt ZnO/ZnxMg1-xO 30
2.6.1 Band gap of rock-salt ZnO 31
2.6.2 Band gap of rock-salt ZnxMg1-xO 33
2.6.3 Band gap of rock-salt ZnO/ZnxMg1-xO heterostructures 34
2.6.4 Electrical properties of rock-salt ZnO/ZnxMg1-xO 35
Chapter III Experimental Procedures 38
3.1 Substrate preparation 38
3.2 Growth parameters 39
3.2.1 Growth of SL samples 39
3.2.2 Growth of ML (ZnO) samples 39
3.2.3 Growth of Heterostructure samples 40
3.3 Material Characterization 40
3.3.1 Composition 40
3.3.2 Surface Morphology 42
3.3.3 Crystal Structure 42
3.3.4 Microstructure 46
3.3.5 Optical properties 46
3.3.6 Electrical properties 48
Chapter IV Epitaxial growth of ZMO/ZnO thin films 51
4.1 Substrate pretreatment 51
4.2 Growth of SL and ML samples at 600 oC 52
4.2.1 Surface morphology 52
4.2.2 Crystal structure and orientation relationship 53
4.2.3 Microstructure and Defects 55
4.3 Epilayer growth of single-layer ZMO at 400 oC 58
4.3.1 Composition 58
4.3.2 Surface morphology 59
4.3.3 Crystal structure and orientation relationship 60
4.3.4 Microstructure 61
4.3.5 Strain relaxation 64
4.4 Optical and electrical properties of ZMO/ZnO epilayer 66
4.4.1 Optical properties 66
4.4.2 Electrical properties 68
4.5 Discussion 70
4.5.1 MBE growth of RS type ZMO films 70
4.5.2 Characteristics of RS type ZnO/ZMO epilayer 74
4.5.3 Stability of the RS type ZMO 75
4.5.4 Characteristics of mixed ZMO films 80
4.5.5 WZ ZnO epilayer 81
4.6 Conclusions 82
Chapter V Epitaxial growth of ZMO/ZnO heterostructures 84
5.1 Epitaxial growth of ZMO/ZnO heterostructures 84
5.1.1 In-situ RHEED pattern 85
5.1.2 Surface morphology 86
5.2 Microstructure analysis of ZMO/ZnO heterostructures 88
5.2.1 Composition 89
5.2.2 Crystal structure 89
5.2.3 Phase identification 90
5.2.4 Microstructure 92
5.2.5 Periodicity and thickness in the heterostructures 96
5.3 Simulations of the real-space energy band structure of ZMO/ZnO heterostructure 97
5.4 Optical and electrical properties of ZMO/ZnO heterostructure 100
5.4.1 Optical properties 100
5.4.2 Electrical properties 106
5.5 Discussion 107
5.5.1 RS type ZnO and WZ type of MgO 107
5.5.2 Diffusion in heterostructure 109
5.5.3 Heterostructure growth 110
5.5.4 Band gap energy and transition energy 111
5.5.5 Growth rate 112
5.5.6 Phase transformation 112
5.6 Conclusions 114
Chapter VI Conclusions and Future Prospects 115
6.1 Conclusions 115
References 117
List of Publications and Honors 210

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