能量源照射星際冰晶之光脫附作用與光化學反應

以作者查詢圖書館館藏

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姓名

謝妮恩(Ni-En Sie) 查詢紙本館藏

畢業系所

物理學系

論文名稱

能量源照射星際冰晶之光脫附作用與光化學反應
(Photodesorption and photochemistry of the interstellar ice under energetic radiation processing)

相關論文

★ A Complete Quantification of Photon-induced Desorption Processes of CO2 Ice	★ X射線與電子能量作用下星際冰晶的化學衍化
★ VUV and EUV irradiation of CH4+NH3 ice mixtures	★ Wavelength-dependent photodesorption of VUV-inactive molecular ices (N2 Ar, Kr) induced by VUV-excited CO ice
★ Temperature dependent photodesorption of CO ices	★ Force between Contacting PDMS Surfaces upon Steady Sliding: Speed Dependence and Fluctuations
★ Diffusion in Realistic-Like Double-Layered Ices	★ Chemical evolution of CO:H2S ice mixture under 1 keV electron irradiation
★ 不同電子能量作用下對N2O冰晶的衍化影響	★ 一氧化二氮冰晶在真空紫外光照射下其生成溫度對耗散截面的影響

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本電子論文使用權限為同意立即開放。
已達開放權限電子全文僅授權使用者為學術研究之目的，進行個人非營利性質之檢索、閱讀、列印。
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摘要(中)

在太空環境中許多易揮發性分子已被觀測到以固態冰晶形式存在，但是在溫度極低的冷星雲與星系際空間（< 20 K），天文學家卻觀測到易揮發性分子以超乎預期豐富含量的氣態形式存在，這樣的觀測結果與吸積模型的預測大相徑庭，因此天文學家提出非熱效應導致易揮發性分子脫附的可能性。在溫度極低的天文環境中，星際冰晶受到不同能量來源的作用（宇宙射線與能量光子），除了誘發冰晶分子的化學作用外，也能導致冰晶分子的脫附效應。根據天文學家的模擬計算，真空紫外光子誘發冰晶分子脫附的過程，對於星際冰晶是一個相當重要的非熱脫附來源。本論文著重於研究星際冰晶在真空紫外光與X光作用下所引發的光脫附與光化學反應，其中更致力於了解主宰光脫附效率的參數。此外，冰晶分子生長溫度條件對於冰晶的光物理特性也是本論文探討的重點之一。

本論文的研究方式是利用一套低溫超高真空系統模擬天文環境的低溫與低壓。藉由傅立葉轉換紅外光譜儀與四極柱質譜儀監控冰晶分子在能量作用下所產生的化學演化與脫附過程。在冰晶成分上，我們選擇了天文學家相當關注的一氧化碳、二氧化碳、氮與甲烷等分子，以單一分子冰晶或是混和冰晶的方式進行能量作用實驗。在此研究中能量來源分為微波氣體放電管搭配氟化鎂光窗所產生的真空紫外光源（114--170 nm；7.9--10.9 eV）與同步輻射研究中心TLS 08B光束線所提供的X光光源（250--1250 eV）。本論文嘗試改變冰晶分子的生長溫度、生長角度與、混和冰晶比例與光通量等參數，進而討論上述參數對冰晶分子的化學衍化與光脫附效應的影響。

光脫附的研究結果顯示一氧化碳冰晶與二氧化碳冰晶對於生長溫度的反應截然不同。一氧化碳冰晶隨著生長溫度越高其光脫率值越低，尤其是在臨界相變溫度的區域會有更加顯著的冰晶結構影響光脫附率。二氧化碳冰晶的光脫附率不論是在勻相結構或是晶質結構下，幾乎沒有差異。不論是溫度對於一氧化碳冰晶的光脫附影響，或是二氧化碳冰晶光脫附率與文獻的差異，皆能在考慮冰晶分子的真空紫外光吸收截面與光源能量譜分布的影響下獲得完美的詮釋。此外，在一氧化碳與氮分子及二氧化碳的混和冰晶，實驗結果證實冰晶中的能量傳遞是經由間接電子躍遷造成冰晶分子的脫附現象。

在能量光子照射冰晶的研究中，根據不同成分的冰晶樣本與能量源可以從紅外光譜上偵測到各式各樣的光化產物，其中質量較大的複雜有機分子能同時經由紅外光譜與質譜來標定分子的種類。除了照光過程外，一些大質量的分子也能在回溫過程中被偵測到，而這些複雜有機分子增添了天文環境中化學衍化的多樣性。冰晶的紅外光譜對於天文觀測中的分子標定是不可或缺的，也能提供星際冰晶生成溫度歷史的參考。本論文所設計的研究實驗，是追求對於天文物理與天文化學能有更完整的認知。

摘要(英)

Numerous solid molecules have been observed in various interstellar regions, and the abundant gaseous molecules are also detected in some environments with low temperatures beyond expectation, like the interstellar medium (ISM) and cold dense clouds. The radiation of the energetic cosmic rays, VUV photons, electrons, and X-rays impinge on the dust grains, resulting in the desorption of the ice mantles. The non-thermal photodesorption process has been seen as an indispensable origin of the overabundance of molecules in the gas phase in the cold regions.

Hence, energetic radiation experiments are of significance for studying the details of photodesorption and photochemical processes. The VUV and X-ray photo-processing on the pure and ice mixtures are focused to figure out the governing parameters on the photodesorption yield, as well as the photochemistry happening simultaneously during irradiation. The fundamental physical properties of the ice are involved in the discussion.

The experiments are conducted through the ultra-high vacuum (UHV) chamber, equipped with a closed-cycle helium cryostat to mimic the low pressure and low temperature near the cold dense clouds and the interstellar medium. The evolution of the solid ice is observed by a transmission Fourier transform infrared spectrometer (FTIR), while a quadrupole mass spectrometer (QMS) is used to detect the gaseous desorbing signals. Different kinds of ice samples are selected to be the sample, such as pure CO2, CO, CH4, the mixtures with N2, and the H2O:CO:NH3. The samples are irradiated by the VUV photons, generated by the Microwave-Discharge Hydrogen-flow Lamp (MDHL) produced in the laboratory with the wavelength 110--180 nm. The other energetic source performed in this thesis is the X-ray, provided by the National Synchrotron Radiation Research Center (NSRRC) with the energy 250 to 1250 eV. Various parameters are designed to investigate the photon-induced desorption and chemical reactions, including the different deposition temperatures, deposition angles, ice mixing ratios, and photon fluxes.

The parameters affecting photodesorption are revealed in detail. In the case of deposition temperature issue on the pure CO2 and CO ice, only the latter one shows the temperature dependency, and the desorption factors are developed for determining the photodesorption yields. Another important role is the absorption cross section of the solid ice, which should be considered when we discuss photodesorption. Moreover, we found that the angle between gas inlet and the substrate falls at 70$degree$ can create a maximum photodesorption yield of CO ice, along with a columnar structure of ice. The energy transfer between CO2/CO ice with N2 is discussed, confirming that the indirect desorption induced by electronic transition (DIET) dominates the photodesorption processes. During irradiation, the solid products are observed on the IR spectra according to the ice samples and the radiation sources. There are Complex Organic Molecules (COMs) identified by both the IR spectra and the mass spectra, and the chemical formation routes of these molecules are represented. Some larger molecules are detected during the temperature-programmed desorption (TPD) processes, supporting the molecular diversity in the interstellar regions. The infrared spectra of the ice at different temperature environments are required not only to identify the peak position of the molecules but also to provide information to track the temperature history of the ice mantles on the dust grains. With the experiments performed in this thesis, we hope to contribute to a more complete knowledge of astrophysics and astrochemistry.

關鍵字(中)

★ 光脫附
★ 光化學反應
★ 真空紫外光
★ X光
★ 星際冰晶

關鍵字(英)

★ Photodesorption
★ Photochemistry
★ VUV
★ X-ray
★ Interstellar ice

論文目次

摘要 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . viii
Abstract . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . x
Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xii
Table of Contents . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xiii
List of Figures . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xviii
List of Tables . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xxvi
1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
1.1 Interstellar environments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
1.2 Interstellar molecules . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
1.2.1 Solid ice abundances . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
1.2.2 Gas phase molecules . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
1.2.3 Complex organic molecules . . . . . . . . . . . . . . . . . . . . . . . 5
1.3 Energetic sources . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5
1.4 Photodesorption process . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
1.5 Thesis outline . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9
2 Experimental procedures . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
2.1 Experimental Set-up . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
2.2 Detection system . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
2.2.1 Infrared spectroscopy . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
2.2.2 Mass spectrometer . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
2.3 Energetic sources . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
2.3.1 Vacuum ultraviolet (VUV) . . . . . . . . . . . . . . . . . . . . . . . . 16
2.3.2 X-ray . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 17
2.4 Experiments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
2.5 Experimental protocol . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
I Photodesorption 21
3 On the Photodesorption of CO2 Ice Analogs: The Formation of Atomic C in the
Ice and the Effect of the VUV Emission Spectrum . . . . . . . . . . . . . . . . . . . 24
3.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
3.2 Experimental Methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26
3.2.1 Experimental procedure . . . . . . . . . . . . . . . . . . . . . . . . . 26
3.2.2 Quantitative calibration of mass spectrometer . . . . . . . . . . . . . . 27
3.3 Results and Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
3.3.1 VUV irradiation for CO2 ice . . . . . . . . . . . . . . . . . . . . . . . 28
3.3.2 The discrepancy in the CO2 photodesorption yield measured by infrared
spectrometer and mass spectrometer . . . . . . . . . . . . . . . . . . . 33
3.3.3 Photodesorption yield . . . . . . . . . . . . . . . . . . . . . . . . . . 38
3.4 Conclusions and Astrophysical implications . . . . . . . . . . . . . . . . . . . 41
4 Key parameters controlling the photodesorption yield in interstellar CO ice analogs:
The Influence of ice deposition temperature and thickness . . . . . . . . . . . . . . . 46
4.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 47
4.2 Experiment Setup and Procedures . . . . . . . . . . . . . . . . . . . . . . . . 49
4.3 Results and Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50
4.3.1 Thickness effect . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 50
4.3.2 Temperature effect . . . . . . . . . . . . . . . . . . . . . . . . . . . . 52
4.3.3 Photodesorption estimation . . . . . . . . . . . . . . . . . . . . . . . . 54
4.3.4 Dominating parameters for photodesorption . . . . . . . . . . . . . . . 56
4.4 Astrophysical Implications and Conclusions . . . . . . . . . . . . . . . . . . . 58
5 Accretion and photodesorption of CO ice as a function of the incident angle of
deposition . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 61
5.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 62
5.2 Experimental protocol . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 64
5.3 Experimental Results . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 66
5.4 Astrophysical Implications and Conclusions . . . . . . . . . . . . . . . . . . . 70
6 13CO and 13CO2 ice mixtures with N2 in photon energy transfer studies . . . . . 77
6.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78
6.2 Experimental Set-up . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 79
6.3 Results and Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 82
6.3.1 13CO:N2 results . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 83
6.3.2 13CO2:N2 ice mixtures . . . . . . . . . . . . . . . . . . . . . . . . . . 86
6.3.3 Comparison between 13CO:N2 and 13CO2:N2 mixtures . . . . . . . . . 93
6.4 Astrophysical Implications and Conclusions . . . . . . . . . . . . . . . . . . . 95
7 X-Ray Photo-desorption of H2O:CO:NH3 Circumstellar Ice Analogs: Gas-phase
Enrichment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 98
7.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 98
7.2 Experiments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 101
7.3 Photo-desorbing Fragments Induced by X-Rays . . . . . . . . . . . . . . . . . 103
7.4 Photo-desorption Yield . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 109
7.5 Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 114
7.6 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 117
II Photochemistry 120
8 Formation Mechanism of CO2 in VUV-Irradiated CO Ice . . . . . . . . . . . . . 122
8.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 122
8.2 Experimental procedure . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 124
8.3 Results and Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 126
8.3.1 Formation of C16O18O . . . . . . . . . . . . . . . . . . . . . . . . . . 127
8.3.2 Formation of C18O2 . . . . . . . . . . . . . . . . . . . . . . . . . . . 128
8.3.3 Effect of deposition rate . . . . . . . . . . . . . . . . . . . . . . . . . 129
8.4 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 132
9 Synthesis of Complex Organic Molecules in Soft X-Ray Irradiated Ices . . . . . . 133
9.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 134
9.2 Experiment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 136
9.3 Results and Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 137
9.3.1 Irradiation and Products . . . . . . . . . . . . . . . . . . . . . . . . . 137
9.3.2 Warm Up: Infrared and Mass Spectra . . . . . . . . . . . . . . . . . . 144
9.3.3 The Refractory Residue . . . . . . . . . . . . . . . . . . . . . . . . . 152
9.4 Conclusions and Astrophysical Implications . . . . . . . . . . . . . . . . . . . 154
III Temperature effect on infrared structural changes 158
10 Pure CO2 ice . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 161
10.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 161
10.2 Experimental set-up and procedures . . . . . . . . . . . . . . . . . . . . . . . 163
10.3 Results and Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 163
10.3.1 Different deposition temperatures . . . . . . . . . . . . . . . . . . . . 163
10.3.2 During cooling and TPD process . . . . . . . . . . . . . . . . . . . . . 166
10.3.3 Molecular dynamics (MD) simulations . . . . . . . . . . . . . . . . . 167
10.3.4 Deconvolution of IR features . . . . . . . . . . . . . . . . . . . . . . . 168
10.4 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 173
11 Pure CH4 ice . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 175
11.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 175
11.2 Experimental Procedures . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 176
11.3 Results and Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 176
11.3.1 Different deposition temperatures . . . . . . . . . . . . . . . . . . . . 176
11.3.2 During cooling and TPD processes . . . . . . . . . . . . . . . . . . . . 178
11.3.3 Effect of the deposition rate . . . . . . . . . . . . . . . . . . . . . . . 179
11.4 Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 180
IV Conclusions 181
12 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 182
12.1 I. Photodesorption . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 182
12.1.1 Deposition temperature effect . . . . . . . . . . . . . . . . . . . . . . 182
12.1.2 Parameters influencing the photodesorption yield . . . . . . . . . . . . 183
12.1.3 Photodesorption yield of CO ice . . . . . . . . . . . . . . . . . . . . . 187
12.1.4 Energy transfer . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 188
12.1.5 X-ray induced photodesorption . . . . . . . . . . . . . . . . . . . . . . 189
12.2 II. Photochemistry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 190
12.2.1 VUV — Pure CO2, ice mixture 13CO2:N2 . . . . . . . . . . . . . . . . 190
12.2.2 VUV — Pure CO/C18O, ice mixture 13CO:N2 . . . . . . . . . . . . . . 190
12.2.3 X-ray — Ice mixture H2O:CO:NH3 . . . . . . . . . . . . . . . . . . . 191
12.3 III. Temperature effect on infrared structural changes . . . . . . . . . . . . . . 191
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 194

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指導教授

陳俞融(Yu-Jung Chen)

審核日期

2022-12-30

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