臺灣博碩士論文加值系統

摘 要
本研究透過使用尺寸分布均勻以及相對低蝕刻速率特性的鍺量子點作為虛擬光罩，發展建立金字塔型的量子點包含鍺/矽超晶格結構在大尺寸的區域裡。在螢光激發光譜量測中發現鍺/矽超晶格量子點與原本鍺/矽超晶格的比較中展現出在強度方面的10 倍提升，此一特性可應用在光電元件應用上。在激發光譜方面的提升歸因于量子維度限制影響。這種成長鍺/矽超晶格量子點方法與現有的矽製程整合技術相容。
利用自我組裝的多層鍺量子點(self-assembled Ge QDs/Si spacer multilayers)尺寸分布均勻以及相對低蝕刻速率特性，本研究提出一種方法來發展建立多層堆疊鍺/氧化矽奈米透鏡(multilayered Ge@silica nanolenses) 在大尺寸的區域裡。在波長1.5微米左右，多層堆疊鍺/氧化矽奈米透鏡樣品相較於原本多層鍺量子點樣品展現百分之77反射率的增強。另外，在螢光激發光譜量測中，多層堆疊鍺/氧化矽奈米透鏡樣品在1.5 和1.55微米之間顯示一個發射峰。將多層堆疊鍺/氧化矽奈米透鏡樣品的螢光激發特性和反射率的增強特性相結合可以被應用作為電信通訊上與矽製程相容的光偵測器材料。
本研究提出一種方法從二維的結構轉換到三維結構進而在矽基材表面上形成鎳矽化物/矽鍺的奈米管(NiSi2/SiGe-based nanotubes)。 透過在一種磊晶成長下所造成的晶格應變的調變釋放，發展一種方法從矽基材上捲取的奈米管架構。透過利用受應變的p+-Si/Si0.7Ge0.3的基材可將半導體矽鍺層(SiGe)和金屬矽化物層(NiSi2)結合成一種奈米管的新架構。由於半導體磊晶技術對於材料成份、摻雜濃度、成長厚度擁有成熟良好的控制，使得金屬矽化物/矽鍺的奈米管(metal silicide/SiGe-based nanotubes)適合于廣泛的應用裡，
本研究是利用固相磊晶方式在應變矽(strained Si)基材上成長長程有序異質磊晶的半導體性鐵矽化物奈米點(��-FeSi2 nanodots)。觀察到鐵矽化物奈米點沿著應變矽基材的<110>方向呈現一維的有序排列。這顯然表示由於漸層緩衝層中的差排傳遞一個應變場到試片表面，使得鐵矽化物奈米點傾向沿著應變場的方向磊晶成長排列。另外，在低溫螢光激發光譜量測中鐵矽化物奈米點在波長1.5微米左右顯示一個發射峰。這種成長半導體性鐵矽化物奈米點方法與現有的矽製程整合技術相容，因此可用於光電元件的應用上。
在對於分支的矽奈米線轉變成鎳矽化物奈米線的詳細研究中，證明在奈米尺度成長的鎳/矽系統中鎳原子是主要的擴散元素。在二鎳化矽/鎳化矽原子級平整度的介面上顯示在奈米尺度中相轉變過程裡異質接面的磊晶關係。另外，在溫度上的改變觀察到矽奈米帶轉變成鎳矽化物奈米帶，進而利用Arrhenius公式計算得到鎳矽化物奈米帶(Ni31Si12 nanobelts)的活化能量(1.06 eV)。

Abstract
By the use of comparably low etching-rate of uniform size Ge QDs as mask, a method was developed to fabricate pyramidal nanodots with excellent uniformity over large area, containing Si-Ge superlattice structure. Photoluminescence measurements reveal that Si-Ge superlattice nanodots exhibit about ten fold enhancement in intensity over conventional Si-Ge superlattice heterostructure, which may lead to applications in optoelectronic devices. The enhancement in PL is attributed to quantum confinement effects. An additional incentive is that the method is compatible with the existing Si/SiGe-based integration technology.
Taking advantage of comparably low etching-rate for Si and uniform size of self-assembled Ge QDs/Si spacer multilayers, a method has been developed to fabricate multilayered Ge@silica nanolenses with excellent uniformity over large area. The samples with Ge@silica nanolens stacks exhibited a reflectivity with an increase of about 77 % around 1.5 �慆 over conventional self-assembled Ge QDs/Si spacer multilayers. In addition, it showed an emission peak between 1.5 and 1.55 �慆 in photoluminescence spectrum. The combination of photoluminescence and reflectance properties of multilayered Ge@silica nanolenses promises applications as a Si-compatible photodetector material for telecommunication.
NiSi2/SiGe-based nanotubes have been fabricated on the Si surfaces by precise transformations from two-dimensional structures to three-dimensional objects. By using the strain in a pair of lattice-mismatched epitaxy layers, a method was developed to create nanotube structure released from a substrate. A new structure combining semiconductor (SiGe) and metallic silicide (NiSi2) into a single nanotube structure was achieved by employing strained p+-Si/Si0.7Ge0.3 substrates. SiGe/metal silicide bilayer nanotubes with a wide range of properties are appropriate for many applications since semiconductor epi-layers possess remarkable control over material composition, doping concentration, and layer thicknesses.
Long-range ordered heteroepitaxial ��-FeSi2 nanodots were grown on strained Si/Si0.8Ge0.2 (001) substrates by solid phase epitaxy method. Ordering was observed on surfaces of strained Si/Si0.8Ge0.2 substrate where the ��-FeSi2 nanodots appear to be confined to one-dimensional array along <110> direction. It is shown that dislocation slip originating from compositionally graded Si1-xGex layers can produce local surface-strain variation that can be used for the fabrication of epitaxial ��-FeSi2 nanostructures on the surface of strained Si/Si0.8Ge0.2 substrate. In addition, a photoluminescence peak at 840meV that contributes from ��-FeSi2 nanodots is measured at 11 K. Consequently, the fabrication procedure of ��-FeSi2 nanodots allows the possibility of combining optoelectronic devices with SiGe/Si-based circuits in the same integrated circuit.
Detailed studies of the transformation from branched Si nanowires into Ni2Si nanowires structures demonstrate that the property of dominant diffusing species of Ni atoms and the diffusion-controlled growth mechanism in nanoscale Ni/Si system. The atomically sharp interface of the Ni2Si/NiSi produced in the nanowire heterostructure has revealed the epitaxial relationship in the nanometer-scale transformation process. The investigation of the transformation of silicon nanobelts into nickel silicide nanobelts on the temperature rise is achieved. The activation energy for the growth of Ni31Si12 nanobelts was obtained (1.06 eV)from an Arrhenius plot.

Contents
Acknowledgments …………………………………………………. V
Abstract ………………………………………………………………. VI
List of Abbreviations and Acronyms ……………………………. XII
Chapter 1 SiGe Heterostructures
1.1 An Overview ………………………………………………………. 1
1.2 Material Properties of Si1-xGex ...…………………………………... 3
1.2.1 Lattice Parameters and Lattice Mismatch.....……………....... 3
1.2.2 Critical Thickness of Si1-xGex on Si ...…….…………………. 4
1.3 Electronic Properties of Strained Si1-xGex …...…………………..... 6
1.4 Si1-xGex Epitaxial Growth Techniques .............................................. 9
1.4.1 Ultra-high Vacuum Chemical Vapor Deposition …….………10
1.4.2 Molecular Beam Epitaxy ……………………………………11
Chapter 2 SiGe Nanostructures
2.1 Si/SiGe quantum Well Structures .......................................... 13
2.2 Si/Ge Dot Structures ……………………………..…………… 14
2.3 Self-Ordered Ge Dot Structures ….…………………………….. 20
2.3.1 Vertically Self-Aligned Si/Ge Dot Stacks ……….……......… 21
2.3.2 Laterally Self-Ordered Arrays of Ge Dots………………...... 24
Chapter 3 Experimental Procedures
3.1 Ultra-high Vacuum Chemical Vapor Deposition ……….…….….. 27
3.2 High resolution XRD (HRXRD) Analysis …………………….… 28
3.3 Transmission Electron Microscope Observation …..…….............. 29
3.4 Energy Dispersion Spectrometer (EDS) Analysis ……………….. 30
3.5 Atomic Force Microscope (AFM) Observation ……..…………… 30
3.6 Raman Spectrometer Analysis ……………..………...................... 30
3.7 Field Emission Measurements ………………………………..….. 31
3.8 Photoluminescence Spectroscopy …………..……………………. 31
Chapter 4 Pyramid-Shaped Si-Ge Superlattice Quantum Dots with Strong Photoluminescence Properties
4.1 Motivation ……………………………….………………….……. 33
4.2 Experimental Procedures ……………………..………………... 34
4.3 Results and Discussion ………………………..…………………. 35
4.4 Summary and Conclusions ……………..……..…………………. 40
Chapter 5 Self-Aligned Nanolenses with Multilayered Ge-Silica Core-Shell Structures on Si (001)
5.1 Motivation ………………………………………….…………….. 41
5.2 Experimental Procedures ………………………………….…… 42
5.3 Results and Discussion ……………………………………...…… 43
5.4 Summary and Conclusions ……………..……..…………………. 50
Chapter 6 Strain-Driven Self-Rolling Silicide/SiGe Based Nanotubes on Si (001) Substrates
6.1 Motivation …………………………….………………………….. 51
6.2 Experimental Procedures ……………………………….……… 52
6.3 Results and Discussion …………………………...……………… 53
6.4 Summary and Conclusions ……………..……..…………………. 57
Chapter 7 Formation of Epitaxial ��-FeSi2 Nanodots Array on Strained Si/Si0.8Ge0.2 (001) Substrate
7.1 Motivation ……………………………………………...………… 59
7.2 Experimental Procedures ………………………...…………….. 60
7.3 Results and Discussion …………………..………………………. 61
7.4 Summary and Conclusions ……………..…….…………………. 65
Chapter 8 Formation of the Nickel Silicide Nanowire and Nanobelts by In Situ Transmission Electron Microscope Investigation
8.1 Motivation …………………………………………….………… 67
8.2 Experimental Procedures …………………………...………… 69
8.3 Results and Discussion ……………………………….………… 69
8.4 Summary and Conclusions …………..……. ….………………. 74
Chapter 9 Summary and Conclusions
9.1 Pyramid-Shaped Si-Ge Superlattice Quantum Dots with Strong
Photoluminescence Properties …………………….……….…… 76
9.2 Self-Aligned Nanolenses with Multilayered Ge-Silica Core-Shell Structures on Si (001) ………………………………….. 76
9.3 Strain-Driven Self-Rolling Silicide/SiGe Based Nanotubes on Si (001) Substrates …………………………..……………...……. 77
9.4 Formation of Epitaxial ��-FeSi2 Nanodots Array on Strained Si/Si0.8Ge0.2 (001) Substrate …………………………...……….. 77
9.5 Formation of the Nickel Silicide Nanowire and Nanobelts by In Situ Transmission Electron Microscope Investigation …………...……………….……………...……….. 78
Chapter 10 Future Prospects
10.1 Fabrication of Nanowires Functional Devices ………………..… 80
10.2 The Extension of In-Situ Transmission Electron Microscopy …………………………….…………………...…. 81
References …………………………………………………….….…… 83
Figure Captions ……........................................................................... 114
Figures ................................................................................................. 120
Publication List ................................................................................... 147

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Chapter 3
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Chapter 4
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Chapter 5
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Chapter 6
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6.8 Ch. Deneke, C. Müller, N. Y. Jin-Phillipp, O. G. Schmidt, “Diameter Scalability of Rolled-up In(Ga)As/GaAs Nanotubes,” Semicond. Sci. Technol. 17, 1278-1281 (2002)
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Chapter 7
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Chapter 8
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Chapter 10
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10.2 Josh Goldberger, Allon I. Hochbaum, Rong Fan, and Peidong Yang, “Silicon Vertically Integrated Nanowire Field Effect Transistors,” Nano Lett. 6, 973-977 (2006)
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10.4 Kristian Mølhave, Sven Bjarke Gudnason, Anders Tegtmeier Pedersen, Casper Hyttel Clausen, Andy Horsewell, and Peter Bøggild, “Transmission Electron Microscopy Study of Individual Carbon Nanotube Breakdown Caused by Joule Heating in Air,” Nano Lett. 6, (2006)
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10.6 J. Y. Huang, S. Chen, Z. F. Ren, G. Chen, and M. S. Dresselhaus, “Real-Time Observation of Tubule Formation from Amorphous Carbon Nanowires under High-Bias Joule Heating,” Nano Lett. 6, (2006)