聚矽氮烷液態高分子陶瓷前驅物(Polysilazane preceramic precursor)在經過熱解後會形成固態的聚合物衍生性陶瓷(Polymer derived ceramic,PDC)，PDC聚有許多優異的性質，且對於任何材料的附著力皆佳，又因其前驅物為液態相，有利於各種沉積形成鍍膜，有機會替代聚醯亞胺在半導體封裝中做為介電層。
本文探討了透過旋塗技術將聚矽氮烷液態高分子陶瓷前驅物(PSZ)與聚醯亞胺(PI)沉積在矽晶圓上，並通過不同溫度進行熱固化交聯(分別為200°C、250°C、300°C)、氧電漿處理時間和陶瓷前驅物濃度對薄膜表面能、粗糙度及黏著力特性的影響。結果顯示，PSZ與PI的接觸角隨固化溫度上升而增加，且經氧電漿處理後水接觸角顯著降低，表明氧電漿引入了極性基團，提高了表面能。稀釋的PSZ在固化後隨濃度降低，有接觸角提高、表面能及黏著力降低的趨勢。氧電漿處理時間增加會進一步降低二碘甲烷接觸角，增加表面能。
AFM分析顯示，PI的粗糙度隨溫度增加而上升，而PSZ在250°C時粗糙度最高，但兩者粗糙度皆隨電漿處理時間增加而增加。膠帶剝離試驗表明，未經電漿處理的PSZ和PI在200°C時黏著力最佳，並隨著溫度上升而黏著力降低，且PSZ在相同溫度下的最佳黏著力皆優於PI。不同厚度的PSZ薄膜黏著力隨厚度增加而增大。另外，通過表面能和粗糙度的量測結果與黏著力的比較，發現表面能、粗糙度與黏著力之間的關係不直觀，表面能和粗糙度皆隨電漿處理時間增加而提高，但黏著力不一定符合此趨勢，需綜合考慮薄膜厚度、固化溫度及電漿處理等因素以選擇最佳製程。

Polysilazane liquid polymer ceramic precursor, upon pyrolysis, forms solid polymer-derived ceramics (PDCs), which possess many excellent properties, including good adhesion to various materials. Due to its liquid-phase precursor, it facilitates diverse deposition methods for film formation and has the potential to replace PI as a dielectric layer in semiconductor packaging.
This study investigates the deposition of liquid-phase polysilazane preceramic precursor and polyimide onto silicon wafers via spin coating. The effects of different curing temperatures (200°C, 250°C, 300°C), oxygen plasma treatment durations, and ceramic precursor concentrations on the surface energy, roughness, and adhesion properties of the films were analyzed. The results show that the contact angles of PSZ and PI increased with curing temperature. However, the water contact angles significantly decreased after oxygen plasma treatment, indicating that oxygen plasma introduced polar functional groups, thus enhancing surface energy. Diluted PSZ, after curing, showed a trend of increased contact angles and decreased surface energy and adhesion with reduced concentration. Extended oxygen plasma treatment further reduced the diiodomethane contact angle and increased surface energy.
AFM analysis revealed that the roughness of PI increased with temperature, while PSZ exhibited the highest roughness at 250°C. The roughness of both materials increased with the duration of plasma treatment. The tape peel test indicated that the adhesion of untreated PSZ and PI was optimal at 200°C and decreased with higher temperatures. Thicker PSZ films showed increased adhesion. Additionally, comparing surface energy and roughness measurements with adhesion results revealed a non-intuitive relationship: surface energy and roughness increased with plasma treatment time, but adhesion did not necessarily follow this trend. Thus, film thickness, curing temperature, and plasma treatment must be considered comprehensively to select the optimal process.

論文審定書 i
摘要 ii
ABSTRACT iii
目錄 v
圖次 viii
表次 xi
第一章 緒論 1
1.1 前言 1
1.2 研究動機與目的 2
第二章 文獻回顧 3
2.1 聚合物衍生性陶瓷(Polymer derived ceramic, PDC) 3
2.1.1 聚合物衍生性陶瓷(PDC)的合成 4
2.1.2 聚合物衍生性陶瓷(PDC)的轉化 6
2.1.3 聚合物衍生性陶瓷(PDC)的沉積 8
2.1.4 聚矽氮烷(Polysilazane, PSZ) 11
2.2 聚醯亞胺(Polyimide) 13
2.2.1 聚醯亞胺在微電子業和半導體業的應用 14
2.3 高分子材料與金屬間的黏附力 15
2.3.1 不同薄膜厚度和不同金屬與黏附性之關係 15
2.3.2 塗層沉積方式與黏附性之關係 16
2.3.3 熱處理與黏附性之關係 16
2.3.4 表面改質 17
第三章 實驗用品 18
3.1 實驗用品 18
3.2 實驗設備 19
3.3 實驗流程與方法 21
3.3.1 準備聚醯亞胺與調配聚矽氮烷液態高分子前驅物溶液 22
3.3.2 聚醯亞胺與聚矽氮烷液態高分子前驅物旋轉塗佈 22
3.3.3 熱處理 25
3.3.4 電漿處理 27
3.3.5 濺鍍鈦銅 28
3.4 分析設備與方法 30
3.4.1 接觸角量測儀 30
3.4.2 接觸角定義 31
3.4.3 多功能原子力顯微鏡(atomic force microscope,AFM) 35
3.4.4 黏著力測試 37
第四章 結果與討論 39
4.1 聚醯亞胺(PI)與聚矽氮烷(PSZ)薄膜之表面能分析 39
4.1.1 固化溫度與電漿處理前後之接觸角比較 39
4.1.2 稀釋PSZ之接觸角與表面能 41
4.1.3 電漿處理時間對於水接觸角(Water contact angle WCA) 43
4.1.4 二碘甲烷接觸角(Diiodomethane contact angle DCA) 45
4.1.5 電漿處理時間對於表面能之關係 47
4.2 聚醯亞胺(PI)與聚矽氮烷(PSZ)薄膜之表面粗糙度分析 50
4.2.1 固化溫度與電漿處理對於粗糙度之影響 50
4.2.2 電漿處理時間對於粗糙度之關係 52
4.3 聚醯亞胺(PI)與聚矽氮烷(PSZ)薄膜和金屬間黏著力分析 55
4.3.1 PSZ與PI之黏著力比較 55
4.3.2 不同厚度之PSZ薄膜黏著力 63
4.3.3 稀釋PSZ之黏著力 65
第五章 結論與未來展望 67
5.1 結論 67
5.2 未來展望 69
參考文獻 70

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