臺灣博碩士論文加值系統

利用第一原理(First-principles)密度泛函理論(density functional theory, DFT)計算GaN(0001)/Ga2O3(-201)異質界面結構(Heterointerface structure)，以及計算繪製氮化鎵(Ga2O3)的電極電位-pH圖。我們考慮各種可能之不同界面鍵結模型，分析價帶偏移(Valence band offset, VBO)大小對異質界面結構之影響，計算出最低價帶偏移(0.872 eV)和最穩定之異質界面結構模型為GaN之N原子與Ga2O3之Ga原子鍵結成N─Ga鍵，證明表面氮化Ga2O3將有助於GaN後續磊晶成長。而價帶偏移量與原子間鍵長壓縮量或異質界面應變量是正比關係。同樣利用第一原理計算氧化鎵與氧化鎵相關化合物的自由能與標準生成能，並透過能斯特方程式(Nernst equation)與熱力學公式求得氧化鎵相關化合物在水溶液化學平衡方程式之電位與酸鹼值pH關係，便以彙整成Pourbaix diagram，本研究理論計算所得之Pourbaix diagram與實驗上的Pourbaix diagram吻合，此一關鍵技術證實了我們有能力解決新穎功能性磊晶層之第一原理Pourbaix相圖研究。

First-principles calculations were used to determine the heteroepitaxial growth behavior of GaN (0001) on Ga2O3(-201) templates and the Pourbaix diagram of Ga2O3. The relative stability of eight different models of the GaN(0001)/Ga2O3(-201) interface is examined as a function of the valence band offset. The most favorable interface consists of N─Ga bonds at the GaN(0001)/Ga2O3(-201) interface. This interface structure agree with previously reported experimental and theoretical results of the surface treatment of N exposure on the Ga2O3 surface. The potential and pH relationships of Ga2O3 systems in aqueous solutions were obtained from Nernst equation and thermodynamic equations. Our results agree with experimental Pourbaix diagrams of Ga2O3.

摘要----------------------------------i
英文摘要-------------------------------ii
目次----------------------------------iii
表目次---------------------------------v
圖目次---------------------------------vi
第一章 緒論-----------------------------1
1-1前言--------------------------------1
1-2研究動機與目的------------------------1
1-3論文架構-----------------------------2
第二章 背景介紹與文獻回--------------------4
2-1前言--------------------------------4
2-2氮化鎵之介紹與文獻回顧------------------4
2-3氧化鎵之介紹與文獻回顧------------------6
2-4能帶偏移之介紹與文獻回顧----------------7
2-5 Pourbaix diagrams之介紹與文獻回顧-----7
第三章 計算方法--------------------------14
3-1前言--------------------------------14
3.2 Born-Oppenheimer Approximation----14
3-3 Hohenberg-Kohn Theorem------------15
3-4 Kohn-Sham Equation----------------17
3-5局域密度近似法(LDA)-------------------18
3-6廣義梯度近似法(GGA)-------------------19
3-7膺勢(Pseudopotential)---------------20
第四章 GaN(0001)/Ga2O3(-201)異質界面研究--22
4-1前言--------------------------------22
4-2研究方法與模型建構---------------------22
4-3結果與討論---------------------------24
4-3-1塊材GaN和Ga2O3結構-----------------24
4-3-2 GaN/LAO宏觀平均位勢----------------24
4-3-3價帶偏移---------------------------25
4-3-4鍵長分析---------------------------25
4-4 結論-------------------------------26
第五章 氧化鎵電極電位與pH圖之研究-----------35
5-1前言--------------------------------35
5-2計算方法-----------------------------35
5-3結果與討論---------------------------38
5-4結論--------------------------------39
第六章 總結論----------------------------42
參考文獻--------------------------------43

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