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研究生：	何銘軒 He, Ming-Xuan
論文名稱：	透過新型聚合方法進行TiO2和Mg2SiO4薄膜局部直接圖案化及其介電和微波應用 Novel Polymerization Approaches for Localized Direct Patterning of TiO2 and Mg2SiO4 Films and Their Dielectric and Microwave Applications
指導教授：	張高碩 Chang, Kao-Shuo
學位類別：	碩士 Master
系所名稱：	工學院 - 材料科學及工程學系 Department of Materials Science and Engineering
論文出版年：	2024
畢業學年度：	112
語文別：	英文
論文頁數：	107
中文關鍵詞：	新穎聚合方法、直接圖案化、多孔TiO2薄膜、多孔Mg2SiO4薄膜、5G頻段的介電性質
外文關鍵詞：	polymerization, direct patterning, porous TiO2 film, porous Mg2SiO4 film, microwave dielectric property
相關次數：	點閱：148 下載：1
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本研究報告了一種新穎的電化學聚合方法，用於在矽基板上製備TiO2和Mg2SiO4薄膜。這種方法使用均勻分散奈米尺度金屬離子的非導電溶液，實現了薄膜的局部沉積。通過調整電化學系統的參數，可以輕易控制薄膜的生長速率、厚度和質量，展現了良好的控制性和多樣性。
為了確保氧化物薄膜通過聚合直接沉積在矽上而不在陽極氧化，研究開發了一種點對點（陰極對陽極）的設置，將尖銳的銅帶固定在基板邊緣。這種配置有效減少了SiO2的形成，防止了基板的氧化。
研究提出了一個假設的沉積機制。在高壓電場下，前驅體溶液中表面略帶負電的顆粒被吸引到正極基板上沉積。由於使用了超尖銳的陰極尖端，沉積區域的電場強度可達約1000 V/m，導致最初螯合的金屬離子被釋放，隨後與溶液中的O2-離子反應，在基板上形成金屬氧化物。
首先製備了TiO2薄膜，並通過C-V和I-V特性測量了其介電性質。由於製備的薄膜本質上具有多孔性，其介電性能較差。隨後，這種方法被應用於製備Mg2SiO4薄膜，作為超越5G和6G無線通信以及汽車雷達的新型介電材料。在28、40和80 GHz頻率下對其介電性質進行了表徵。與傳統的濺射或CVD技術相比，這種沉積方法在常壓環境下操作，大大降低了設備的環境成本。對於TiO2薄膜，多孔結構導致MOS電容器中存在較大的漏電流。而對於Mg2SiO4薄膜，多孔結構中的空氣進一步降低了材料的介電常數，與聚酰亞胺（PI）的複合結構在高頻段展現出良好的介電性能。
本研究在開發新型多孔薄膜沉積技術方面具有創新性和實用價值。未來還需進一步研究Mg2SiO4與聚合物的複合，製作傳輸線和天線器件來測試其介電特性，為開發高性能的微波通信材料提供重要的實驗和理論基礎。

This study reports the fabrication of TiO2 and Mg2SiO4 films on Si substrates through a novel electrochemical-based polymerization approach using a non-conductive solution with uniformly dispersed metal ions at a nanoscale. This method enables the local deposition of the films with the ease of control and versatility simply by the adjustable parameters of our electrochemical system for the control of growth rates, thicknesses, and quality of the films.
To ensure direct deposition of the oxide films on Si through polymerization without oxidation in an anode, a point (cathode)-to-point (anode) setup was developed involving a pointed copper tape attached to an edge of a substrate. This configuration effectively reduced the formation of SiO2 and prevented oxidation of the substrate.
A hypothetical mechanism was proposed. Under a high-voltage electric field, particles in the precursor solutions with a slightly negative charge on their surface were attracted to the positive electrode substrate to be deposited. Due to the use of an ultrasharp tip (cathode), the electric field strength in the deposition area can reach up to approximately 1000 V/m, which causes the initially chelated metal ions to be released and subsequently react with O2- ions in the solution to form metal oxides on the substrate.
TiO2 films were first fabricated and their dielectric properties were measured through C-V and I-V characteristics. Because of the porosity of the fabricated film in nature, their dielectric performance was poor. The approach was applied to another application of Mg2SiO4 films for novel dielectrics for beyond 5G and 6G wireless telecommunication and automotive radar. Its dielectric properties was characterized at 28, 40 and 80 GHz.

摘要	I
Abstract	II
致謝	III
Contents	V
Figure Contents	X
Chapter 1	Introduction	1
1	Background: film deposition approach though solution processes	1
1.1	Typical electrolyte approach	2
1.1.1	Electroplating (cathode)	2
1.1.1.1	Mechanism	3
1.1.1.2	Application	5
1.1.2	Electrodeposition of oxide films (anode)	8
1.1.2.1	Mechanism	8
1.1.2.2	Application	15
1.2	Nonelectrolyte approach	17
1.2.1	EPD	18
1.2.1.1	Mechanism	18
1.2.1.2	Application	25
1.2.2	Novel polymerization	26
1.2.2.1	Direct deposition of oxide films on substrates (anode) through polymerization: oxidation (point to plate)	27
1.2.2.2	Direct deposition of oxide films on substrates (anode) through polymerization: no oxidation (point to point)	27
1.2.2.3	Experimental setup	28
1.2.2.3.1	Tip prepared by etching	29
1.2.2.4	Hypothetical mechanism	30
2	Polymerization application	32
2.1	Local deposition of TiO2	32
2.1.1	Characteristics	32
2.1.2	Application	32
2.2	Local deposition of Mg2SiO4	33
2.2.1	Characteristics	33
2.2.2	Application	34
3	Motivation	35
Chapter 2	Experimental method	36
1	Material	36
1.1	Chemicals for novel polymerization	36
1.2	Chemicals for cleaning process	36
1.2.1	Tip cleaning	36
1.2.2	Substrate cleaning	37
1.2.3	Substrate material	37
1.2.4	Material for tip preparation	37
2	Preparation of polymerized precursor solution frequency bands	38
2.1	Titanium polymerized precursor solution	38
2.2	Magnesium-silicon polymerized precursor solution	39
3	Experimental setup	40
3.1	Power supply for the preparation of TiO2	40
3.2	Power supply for the preparation of Mg2SiO4	40
3.3	Three-axis linear motion stage	41
3.4	Experiment setup	42
3.5	Tip cleaning setup and process	43
3.6	Tip etching setup	44
3.7	Substrates cleaning setup and process	45
4	Characterization	46
4.1	Optical microscopy (OM)	46
4.2	High resolution scanning electron microscope (HRSEM)	47
4.3	Two-Dimensional X-Ray Diffraction (2DXRD)	48
4.4	X-Ray photoelectron Spectroscopy (XPS)	48
4.5	Zeta potential analyzer	49
4.6	Resonator System	49
4.7	Programmable compact temperature & humidity System	50
Chapter 3	Results and discussion	51
1	Characterization of porous TiO2 film	51
1.1	OM & XRD Results	51
1.2	XPS results	56
1.3	SEM results	57
1.4	Mechanism	59
1.5	TiO2-based Metal Oxide Semiconductor (MOS) Capacitor	61
1.5.1	Resulting Device	61
1.5.2	C-V measurement	61
1.5.3	I-V measurement	62
1.6	Further analysis	63
2	Characterization of porous Mg2SiO4 film	64
2.1	OM Results	64
2.2	XRD Results	65
2.3	XPS results	69
2.4	SEM results	70
2.5	Mechanism	71
2.6	Application	76
(1)	Mg2SiO4/Si	76
(2)	Mg2SiO4/PI	77
I. Dielectric measurement at multiple frequency bands	78
II. Moisture absorption	80
Chapter 4	Conclusions and future works	81
1	Conclusions	81
1.1	TiO2 film	81
1.2	Mg2SiO4 film	82
2	Future work	83
2.1	Preparation of Composite Materials	83
2.2	Fabrication of Devices	83
Chapter 5	References	84
                                    

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