本研究使用脈衝雷射剝熔蝕置於四乙基正矽酸鹽(TEOS)液體的碳化矽(6H-SiC)單晶片，合成含Si-C-O-H成分的鑽石態奈米凝聚物/微粒和包裹亂層石墨烯。從分析式電子顯微鏡觀察得知這種奈米凝聚物/微粒有不同的晶格常數(0.523-0.548 nm)，以至於有特徵拉曼光譜(487, 511 cm-1)、光致螢光(532, 603 nm)、和紫色吸收光譜(對應最小能隙值為3.1eV)。這種富含矽的奈米微粒具來自缺陷團簇(defect cluster) 的順晶結構分布(paracrystalline distribution)和衝擊引起的4x(111)的斷層。一般來說，Si-C合金的鑽石態微粒有發達的~{111}和~{110}鄰近表面(例如311, 331, 123)，以特定的(hkl)聚簇成特殊晶界，即(110)70.5º的扭轉晶界和 [111](123)/(011) 傾轉晶界。而歷經成分過冷(constitutional supercooling) 以至於 Si-O-H摻雜的亂層石墨烯球晶，則具有0.341和0.366nm兩種層間距。至於尺寸達幾微米的莫桑石(Moissanite，即3C-SiC)和鑽石多晶體，則具有固相燒結的特徵三接點(triple junction)，以及特徵拉曼光譜和光致螢光光譜。矽結晶的高溫相，例如立方晶和四方晶的方矽石(cristobalite)，並不容易在TEOS的動態 脈衝雷射剝熔蝕環境中存在。

Pulsed laser ablation of 6H-type SiC single crystal wafer in TEOS was employed to synthesize diamond-type nanocondensates/particulates with varied Si-C-O-H content and turbostratic graphene coverage. Analytical electron microscopic observations indicated that such nanocondensates/particulates have varied lattice parameters (0.523-0.548 nm) with accompanied modification of optoelectronic properties, i.e. Raman shift (487, 511 cm-1), photoluminescence (532, 603 nm)and violet light absorbance corresponding to a minimum band gap of 3.1 eV. The Si-rich nanoparticles have paracrystalline distribution of defect clusters and occasional shock-induced 4x(111) faulting. In general, the Si-C alloyed diamond type particles have well-developed ~{111} and ~{110} vicinal surfaces (such as 311, 331, 123) for (hkl)-specific coalescence as special grain boundaries, i.e. (110) 70.5º twist boundary and [111](123)/(011) tilt boundary. Turbostratic graphene also occurred as folding belts and spherulite which typically retained bimodal basal spacings 0.341 nm and 0.366 nm after Si-O-H doping and/or layer corrugations upon constitutional supercooling. Moissanite (3C-SiC) and diamond polycrystals up to several microns in size with triple junctions, a characteristic of solid-state sintering, were also identified by scanning electron microscopy coupled with Raman and PL spectroscopy. High-temperature formation of crystalline silica, such as cristobalite with cubic and/or tetragonal structures, was not favored in TEOS environment.

目錄

論文審定書 i
誌謝 ii
中文摘要 iv
英文摘要 v
目錄 vi
圖目錄 vii
附錄目錄 xi

壹、 前言 1
貳、 實驗流程 4
參、 實驗步驟及方法 5
肆、 實驗結果 8
伍、 討論 15
陸、 結論 21
柒、 參考文獻 22

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