這篇博士論文，重點是通過了解源到襯底距離的作用及其對反應的影響來預測物理氣相傳輸過程 (PVT) 中碳化矽單晶生長的生長速率和 Si/C 比。 PVT 過程。例如，如果源與襯底的距離保持緊密，則源中的昇華物質表現理想，PVT 系統中的矽通量會變高，這對於 4H-SiC 多型穩定性是不利的。相反，如果源到襯底的距離保持相對較遠，昇華物質有足夠的時間擴散，與石墨坩堝壁碰撞並在靠近襯底的降低溫度下表現非理想，通過橫向相互作用其他形成較大的含碳物質（簇）的中間化合物。因此，我們之所以研究橫向相互作用反應的動力學和熱力學，它們對生長的產物貢獻和 Si/C 比。為了確定 Si/C 比，我們首先構建了實驗觀察到的 4H-SiC (000-1) 重建 π 鍵鏈 (π-BC) 襯底，然後，我們通過 ab 估計了該襯底上簇的粘附係數從頭開始。最後，將係數的結果用於計算 SiC 晶錠在不同襯底溫度下的 Si/C 比，我們的研究結果表明，對於 4H-SiC 生長，在降低的生長溫度下達到 1.98 的 Si/C 比.然而，這種化學計量比是不夠的，因為這種多型穩定性需要更多的碳通量，因此，我們建議將襯底放置在 2296 K 以上的轉變溫度，此時 Si/C 比變得統一。此外，爐坩​​堝由石墨製成這一事實也提高了該溫度下的 Si/C 比，因為坩堝中的一些碳會在此過程中溶解在主體流體中。此外，分析和確定了生長動力學路徑，並使用從頭耦合有限元方法 (FEM) 來估計不同 (PVT) 壓力水平下物種的個體生長貢獻和總生長速率。

This doctoral dissertation, focused on predicting the growth rate and Si/C ratio of silicon carbide single crystal growth in the physical vapor transport process (PVT), by understanding the role of the source-to-substrate distance and its effect on the reactions in the PVT process. For instance, if the source-to-substrate distance is maintained closely, sublime species from the source behave ideally and the amount of silicon flux in the PVT system becomes high, which is undesirable for 4H-SiC polytype stability. On the contrast, if the source-to-substrate distance is maintained relatively far apart, sublime species have sufficient time to diffuse, collide with the graphite crucible walls and behave non-ideally at reduced temperature close to the substrate, by laterally interacting with each other to form larger intermediate compounds of carbon containing species (clusters). Therefore, the reason we studied the kinetics and thermodynamics of the lateral interaction reactions, their product contribution to growth and Si/C ratio. To determine the Si/C ratio, we first built the experimentally observed 4H-SiC (000-1) reconstructed π-bonded chain (π-BC) substrate, and thereafter, we estimate the sticking coefficients of the clusters on this substrate by ab initio. Finally, the results of the coefficients, is used to calculate the Si/C ratio of the SiC boule at different substrate temperature, and our findings shows that, a Si/C ratio of 1.98 is achieved at reduced growth temperature for 4H-SiC growth. However, this stoichiometric ratio isn’t enough, as more carbon flux is required for this polytype stability, hence, we recommend the substrate placed at the transition temperature just above 2296 K where the Si/C ratio becomes unity. In addition, the fact that, the furnace crucible is made of graphite, also improves the Si/C ratio at this temperature, as some carbon from the crucible will dissolve in the bulk fluid during the process. Furthermore, growth kinetics pathway are analyzed and determined, and an ab initio coupled finite element method (FEM) is used in estimating the individual growth contribution of species and total growth rate at different (PVT) pressure levels.

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