臺灣博碩士論文加值系統

本論文利用化學氣相傳導法成功生長三硫化磷鐵和三硒化磷鐵晶體，皆為單晶層狀反鐵磁性材料，樣品表面呈金屬亮面且容易撕薄。首先利用能量散佈光譜儀確認晶體的成分比例為1:1:3與X射線光電子能譜儀確認所含之元素化學態和電子態，結果符合預期。接著利用X射線晶體繞射分析儀分析出材料結構和晶格常數，結果顯示三硫化磷鐵為單斜晶系而三硒化磷鐵為六方晶系，低溫X-光繞射也發現三硫化磷鐵和三硒化磷鐵因結構改變產生新的峰值，而晶格常數也隨著溫度變低而變小，在變溫拉曼實驗中，首先將樣品利用機械撥離法撕成微奈米級通過波長532 奈米的雷射激發，三硫化磷鐵主要顯示四種拉曼振動模態而三硒化磷鐵則有三種拉曼振動模態，隨著溫度下降拉曼模態往高波數位移，實驗結果中也發現三硫化磷鐵在峰值98 cm-1位置當溫度高於120 K時，出現寬且不對稱的峰，且當溫度低於60K時，此98 cm-1的峰分離為兩個尖峰，我們推測此振動模態可能與材料磁性有關，為了找出拉曼光譜與磁性的相關性，我們利用超導量子干涉磁量儀量測三硫化磷鐵和三硒化磷鐵變溫磁特性，結果發現他們的尼爾溫度分別在120K與110K，其中三硫化磷鐵磁矩方向改變的溫度與拉曼峰98 cm-1改變的溫度相近。本論文持續探討三硫化磷鐵和三硒化磷鐵的光學與電學特性，三硫化磷鐵的能隙位置由室溫到低溫為1.32到1.41 eV，三硒化磷鐵能隙位置則在0.75到0.85 eV，它們屬於間接能隙，熱探針實驗中三硫化磷鐵以及三硒化磷鐵的主要載子為電洞，在四點量測變溫電阻率實驗中，三硫化磷鐵和三硒化磷鐵之電阻率分別為1.7k (Ω-cm)和116 (Ω-cm)並且隨著溫度降低而電阻率變大符合一般半導體的特性，經過霍爾量測的計算結果三硒化磷鐵載子濃度為1016 cm-3，載子遷移率為3 (cm2/V·Sec)。

In this thesis, the chemical vapor transport method is used to grow layered single crystals of antiferromagnetic materials FePS3 and FePSe3. The sample surfaces of as grow crystals are bright and the layer are easy to exfoliate. EDS and XPS are used to confirm composition and structure in the crystals. The XRD measurements reveal that FePS3 possesses a monoclinic structure, whereas FePSe3 possesses a hexagonal structure. Some new peaks of FePS3 and FePSe3 in XRD are appeared owing to a result of structural changes at low temperatures. The lattice constant decreases when the temperature is decreased. For the Raman measurement, the exfoliated samples are transferred onto a SiO2 silicon substrate and a 532 nm laser used as the excitation source. The Raman modes for both FePS3 and FePSe3 shift to higher wavenumber as the temperature is decreased. Raman result of FePS3 shows an asymmetrical peak at 98 cm-1 from 300 K to 120 K. After passing through the Neel temperature at 120 K, the peak divided into two sharp peaks as the temperature is lowered. The Raman peak at 98 cm-1 may reflect the magnetic characteristic of FePS3 . To further find out the correlation between Raman result and magnetism, temperature dependent magnetic measurement of superconducting quantum interference device from 5K to 300K was implemented. The difference in temperature between the Raman peak and magnetic moment direction is consistent with the change occurred at Neel temperature of 120K. At room temperature, FePS3 has an indirect bandgap at 1.32 eV, while FePSe3 is at 0.75 eV. The value of resistivity are 1.7k (Ω-cm) and 116 (Ω-cm) for FePS3 and FePSe3 at 300K. According to Hall measurement, both FePS3 and FePSe3 are p-type semiconductors.. the temperature dependent resistivity measurement reveal the carrier activation energies are ΔE = 306 meV for FePS3 and ΔE = 127 meV for FePSe3, respectively.

中文摘要 I
ABSTRACT II
誌謝 III
目錄 IV
圖索引 VI
表索引 X
第一章 緒論 1
第二章 晶體成長 4
2.1 晶體成長方法 4
2.2 單晶成長的系統配置 5
2.2.1 高真空系統 6
2.2.2 高溫長晶爐系統 7
2.3 晶體秤重與成長流程 8
2.3.1 元素比例秤重和石英管玻璃清洗 8
2.3.2 單晶化合及成長 9
第三章 實驗原理及量測技術 11
3.1 能量散佈能譜儀 (EDS) 11
3.2 X射線光電子能譜儀 (XPS) 13
3.3 X-ray晶格繞射分析儀 (XRD) 14
3.4 超導量子干涉磁量儀 (SQUID) 17
3.4.1 磁性的基本理論 18
3.5 拉曼散射系統 (Raman) 23
3.6 光穿透實驗原理 (Transmittance) 26
3.6.1 光穿透系統架構與實驗方法 27
3.7 電阻率量測(Resistivity measurement) 28
3.8.1 熱探針實驗 (Hot probe) 29
3.8.2 照光電阻率量測 (Photo VI measurement) 30
3.8.3 四點電阻率量測 (Van der Pauw method) 31
3.8 霍爾量測 (Hall effect) 33
第四章 實驗結果與討論 35
4.1 能量散佈能譜儀分析 35
4.2 X射線光電子能譜儀分析 37
4.3 X-ray晶格繞射實驗分析 44
4.3.1 變溫X-ray晶格繞射實驗分析 49
4.4 超導量子干涉磁量儀實驗分析 52
4.5 拉曼散射光譜實驗分析 55
4.6 光穿透光譜實驗結果 60
4.7 電阻率量測結果 65
4.7.1 熱探針實驗結果 65
4.7.2 照光電阻率實驗結果 65
4.7.3 四點電阻率量測實驗結果 68
4.8 霍爾量測結果 70
第五章 結論 71
參考文獻 73

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