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研究生:陳鴻志
研究生(外文):Hung-Chih Chen
論文名稱:氣體分子在材料表面的反應及蝕刻化學
論文名稱(外文):The Chemical Reaction of Adsorbed Gas on Material and Corrosion Chemistry
指導教授:張哲政
指導教授(外文):Che-Chen Chang
學位類別:碩士
校院名稱:國立臺灣大學
系所名稱:化學研究所
學門:自然科學學門
學類:化學學類
論文種類:學術論文
論文出版年:1999
畢業學年度:87
語文別:中文
論文頁數:128
中文關鍵詞:X光光電子光譜程溫脫附法重構同步輻射白光蝕刻化學氯氣氮化鎵氯化反應
外文關鍵詞:X-ray photoelectron spectroscopy (SXPS)temperature programmed desorption(TPD)missing row reconstructionsynchrotron radiation white beamcorrosion chemistrychlorineGaNchlorination reaction
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論文摘要
本篇論文共分為兩部分,我們使用低能電子繞射(LEED)、歐傑電子能譜(AES)、程溫脫附法(TPD)、二次離子質譜(SIMS)及同步輻射軟X光光電子光譜(SXPS)等表面分析技術,作為偵測材料表面鍵結狀態、組成以及結構在化學反應過程中改變的工具。在有關氣體分子在材料表面反應的研究,我們觀察在低溫100K時,一氧化碳(CO18)在Pd(110)單晶表面上鍵結吸附的情形,並且藉由改變表面的溫度或是照射同步輻射白光,觀看一氧化碳的吸附位置及狀態的改變,以及Pd(110)表面結構的變化。在低溫100K時,一氧化碳分子主要是吸附在bridge site,形成CO islands 結構。反應溫度升高時, CO islands的面積也隨著增加;當升溫至340K時,Pd(110)表面產生missing row重構面。而若Pd表面先吸附一氧化碳之後再照射同步輻射白光,將會有新的化學產物生成,其化學式分別為Cn(CO)及Cn(CO)2,隨著白光照射時間及Pd表面溫度的改變,這些產物在表面的數目也各有消長。另外,在有關蝕刻化學的研究上,我們選擇目前光電材料研究中最熱門的氮化鎵(GaN)為材質,而以蝕刻上最常使用的氯氣(Cl2)作為反應氣體。在低溫100K時,隨著氯氣曝露量的增加,GaCl為最先生成的產物,而GaCl2與GaCl3則分別在較高的曝露量(2L與6L)產生。當GaN表面達到飽合覆蓋量時,GaCl與GaCl2為主要的產物;隨著表面溫度不斷昇高,GaCl的含量逐漸下降,而GaCl2與GaCl3的含量慢慢多於GaCl,表示升溫過程中,GaCl會再進一步與氯原子形成含氯數較高且揮發性較高的產物。經由實驗結果,我們對於氯氣在GaN上蝕刻反應的機制能有較清楚的瞭解。
Abstract
About the chemical reaction of the adsorbed gas on material, we use the reaction of CO18 with the Pd(110) surface as a model system. The effect of the surface temperature and the exposure on the variation of the chemical state of CO18 present on the surface is measured by soft X-ray photoelectron spectroscopy (SXPS) which employs synchrotron radiation and temperature programmed desorption(TPD). Increasing the exposure at 100 K, the C1s spectrum exhibits two emission bands and is dominated by the photoemission of CO18 in bridge site. It appears that CO islands are formed, which is surrounded by a disordered sea. With increasing surface coverage increases the number and average size of islands reducing the number of molecules left in the disordered sea. When a CO-saturated surface is annealed to about 323 K, a CO-induced missing row reconstruction of the Pd(110)surface occurs. It is confirmed by theα3 state peak of CO18 in thermal desorption spectra data and new emission features at binding energies of 286.0 and 286.3 eV for CO bonding to bridge sites on the ridges and in the grooves of Pd(110).
When a CO-saturated surface is irradiated by synchrotron radiation white beam , the C 1s spectrum exhibits two emission bands and is dominated by lower binding-energy band. The lower binding-energy band which contains three deconvolution peaks assigns to new chemical species with general formula as Cn(CO) and Cn(CO)2. The effect of the irradiation time and the surface temperature on the variation of these new chemical species present on the surface is also discussed.
Regarding to the research of corrosion chemistry, we use GaN as a model substrate to study the etching reaction of chlorine on the nitride surface. The etching process of Cl on the surface is monitored at various substrate temperatures and chlorine exposures. Results from secondary ion mass spectrometric measurements reveal that the GaN surface is chlorinated upon chlorine exposure, with an increasing yield of the GaClx species formed on the surface at higher chlorine exposures. The chlorination reaction occurs stepwise, with gallium monochloride formed prior to the dichloride at 100K. The range of x also increases with the amount of chlorine exposed to GaN. The variation with the substrate temperature of the population of different Cl states on the surface is examined by coupling synchrotron-radiation core-level spectroscopy. A surface etching mechanism of GaN by chlorine is proposed based on the analysis of Ga3d core-level spectra.
第一章 緒論 1
1.1表面科學及其在半導體工業與觸媒催化之應用 1
1.2表面之重構現象(Reconstruction) 4
1.3一氧化碳吸附在Pd(110)單晶之反應機構 6
1.3.1簡介 6
1.3.2 CO-Pd之鍵結軌域研究 8
1.3.3 CO/Pd(110)之吸附位置研究 10
1.3.4 CO /Pd (110)之表面結構研究 13
1.3.5 CO/Pd(110)之氣體表面擴散研究 19
1.4 CO/Ni(110)、CO/Pd(110) 、CO/Pt(110)反應系統之比較 22
1.5 CO/Pd(111)、CO /Pd(110) 、CO/Pd(100)反應系統之比較 28
第二章 實驗儀器、方法與步驟 31
2.1 實驗之超高真空系統 31
2.2樣品處理及清潔 34
2.3實驗之氣體處理與氯氣製造器之製作 36
2.4表面分析技術之量測 37
2.4.1 低能電子繞射(LEED) 37
2.4.2 歐傑電子能譜 37
2.4.3 軟X光光電子發射能譜(SXPS) 39
2.4.4 二次離子質譜 39
2.4.5 層溫脫附法(TPD) 40
2.4.6 資料處理 42
第三章 實驗結果與討論 43
3.1 SXPS於分子吸附及蝕刻化學之研究 43
3.2一氧化碳在低溫吸附於Pd(110)表面之研究 44
3.3溫度對一氧化碳吸附於Pd(110)表面之影響研究 59
3.4 一氧化碳氧同位素於Pd (110)表面之程溫脫附實驗 62
3.5 照射同步輻射白光後對一氧化碳吸附於Pd (110)表面之影響研究
74
3.6蝕刻化學:氯氣(Chlorine)在氮化鎵(Gallium Nitride)表面之蝕刻反應研究 90
3.6.1 前言 90
3.6.2低溫蝕刻 94
3.6.2表面升溫的影響 95
第四章 結論117
Reference 122
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