嘧啶混合冰晶之光化作用研究

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胡幃傑(Wei-jie Hu) 查詢紙本館藏

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物理學系

論文名稱

嘧啶混合冰晶之光化作用研究

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摘要(中)

於碳質隕石及球狀碳隕石中，蘊藏了與生命體相關的許多有機分子。而於其中檢測到核鹼基(建構DNA/RNA的基本分子)的存在，說明這些關乎生命體的分子可以在地球外的環境下被生成出來。而於近幾年的實驗結果以及理論計算推演之下，嘧啶加水的混合冰晶在經由真空紫外光的作用後，能生成嘧啶的相關氧化物，其中也包含了核鹼基-尿嘧啶。

本論文主要探討嘧啶加水的混合冰晶在天文環境中(14K，< 10-9 torr)，於不同光子能量作用下的光化機制。光源分別以氫氣微波放電管產生的真空紫外光(VUV)以及同步輻射研究中心提供之極致紫外光(EUV)，並挑選不同的光子能量範圍進行實驗：VUV(114−180 nm)，白光(25−300 nm)，He I (58.4nm)，He II (30.4 nm)。使用紅外光譜儀量測嘧啶的光解速率以及光化產物的種類與生成速率。並以液相及氣相層析圖譜分析受光化作用後回溫至室溫的殘餘物質。

實驗結果中發現嘧啶相當容易受光子作用而被消耗，並且生成諸多已被觀測到的星際分子:CO、CO2、HNCO、OCN-、CN-、H2CO、HCONH2。並於所有實驗結果中明顯地偵測到尿嘧啶以及其前體4(3H)-pyrimidone的生成。而不同入射能量的光子作用對嘧啶光消耗以及光化產物的產率是相當地不同。這些結果說明原生有機分子是可以在VUV/EUV光子作用下生成，並且在被水包覆之下存留而抵達地球表面。

摘要(英)

Carbon-rich meteorites and carbonaceous chondrites are found to contain many biologically relevant organic molecules. The presence of nucleobases (building block of DNA and RNA) in carbonaceous chondrites indicates that molecules of biological components can be formed in non-terrestrial environments via abiotic pathways. Recent laboratory experiments and ab initio calculations had already shown that the VUV irradiation of pyrimidine in H2O ices leads to the formation of oxidized pyrimidine derivatives, including the nucleobase uracil.

In this study, we focus on the different photo-energy effect on photon irradiation of pyrimidine in H2O-rich ice mixtures under astrophysical conditions (<10-9 torr, 14K).The vacuum ultra-violet (VUV) and extreme ultra-violet (EUV) photons provide by microwave-discharged hydrogen-flowed lamp (MDHL) and synchrotron radiation in several ranges: VUV (114−180 nm), 0th order light of synchrotron radiation beamline (25−300 nm), He I (58.4 nm), He II (30.4 nm). The photo-destruction rate of pyrimidine and photo-production rate of products were measured by FTIR spectroscopy. Afterwards, the photo-irradiated samples were warmed up to room temperature and the residues were analyzed by liquid and gas chromatography all together.

The results show that pyrimidine was easy to be depleted by VUV/ EUV photons, and formed many interstellar molecules such as: CO, CO2, HNCO, OCN-, CN-, H2CO, HCONH2, etc. All the photo-products in our experiments evidenced that 4(3H)-pyrimidone and uracil could be conclusively identified. The photo-destruction rate of pyrimidine and photo-production rate of products are found photon energy dependent. These results illustrate that the prebiotic components can be formed and survive in astrophysical environments which is subjected to VUV/EUV irradiation constantly. Finally they can be wrapped by H2O-rich ice matrix and fall down to Earth’s surface.

關鍵字(中)

★ 隕石
★ 核鹼基
★ 嘧啶
★ 星際冰晶
★ 光化作用
★ 紅外光譜
★ 真空紫外光
★ 極致紫外光
★ 氣相層析儀
★ 液相層析儀
★ 尿嘧啶

關鍵字(英)

★ meteorites
★ pyrimidine
★ nucleobases
★ interstellar ice
★ photolysis
★ infrared spectrum
★ VUV
★ EUV
★ gas chromatography
★ liquid chromatography
★ uracil

論文目次

目錄
第1章緒論 …………………………………………………………………..1
1.1 生命的起源 ………………………………………………………1
1.2 起源的另一扇窗…………………………………………………..2
1.3 串起生命的長鏈 – DNA與RNA………………………………..4
1.4 太空環境下的生命探索…………………………………………..8
第2章實驗原理……………………………………………………………...11
2.1 冰晶衍化機制……………………………………………………11
2.1.1 熱能……………………………………………………….11
2.1.2 高能粒子………………………………………….………11
2.1.3 光化作用…………………………………………………12
2.2.1 紅外光譜………………………………………………………14
2.2.2 分子振動模式…………………………………………………15
2.2.3 比爾定律………………………………………………………16
2.3 傅立葉紅外光譜儀…………………………………………...…17
2.3.1 麥克森干涉儀……………………………………………18
2.3.2 干涉圖譜轉換成紅外光譜圖……………………………20
2.4 薄膜干涉術……………………………………………………...21
2.5 四極質譜儀……………………………………………………...23
2.6 高效能液相層析………………………………………………...24
(High Performance Liquid Chromatography,HPLC)
2.7 氣相層析質譜分析儀…………………………………………...25
(Gas chromatography–mass spectrometry,GC-MS)
第3章實驗儀器與架設……………………………………………………..27
3.1 太空環境之模擬………………………………………………...27
3.1.1 超高真空系統…………………………………………….27
3.1.2 低溫冷卻系統（cryostat）……………………………….28
3.1.3 基板…………………………………………………….…30
3.2 氣體預混系統(Gas Handing System) …………………………...30
3.3 傅立葉紅外光譜儀………………………………………………32
3.4 四極質譜儀………………………………………………………33
3.5 真空紫外光………………………………………………………33
3.5.1 微波氫氣放電管(MDHL) ………………………….…….33
3.5.2 同步輻射光源………..…………………………….……..37
3.6 雷射量測薄膜厚度技術…………………………………………39
3.7 高效能液相層析儀(HPLC) ……………………………………..40
3.8氣相層析質譜分析儀 (GC-MS) ………………………………...41
第4章實驗過程與分析…………………………………………………….42
4.1 實驗方法…………………………………………………………43
4.1.1 前置作業與降溫………………………………………….43
4.1.2氣體預混與長冰過程……………………………………..43
4.1.3照光過程…………………………………………………..48
4.1.4 回溫過程………………………………………………….48
4.1.5 殘餘物質………………………………………………….48
4.2 實驗結果與分析-紅外光譜……………………………………...50
4.2.1 水冰晶中的嘧啶光消耗(Photo-depletion)現象………….50
4.2.2 光化產物………………………………………………….60
4.2.3 含氮之光化產物的生成機制…………………………….62
4.2.4不含氮之光化產物的生成機制…………………………..77
4.3殘餘物質實驗與分析…………………………………………….83
4.3.1 雷射冰晶厚度量測………………………………………...84
4.3.2殘餘物質的組成與分析…………………………………….86
4.3.3 HPLC結果與分析…………………………………………..87
4.3.4 GC-MS結果與分析………………………………………...95
第5章應用與結論…………………………………………………………102
5.1 天文生物學應用………………………………………………..102
5.2 結論……………………………………………………………..103
參考文獻…………………………………………………………………….105

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2014-7-29

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