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High-Resolution Spectroscopic Studies Of HIGH-RESOLUTION SPECTROSCOPIC STUDIES OF 15 ATMOSPHERIC GASES (C2H2-N2, O2, and NH3) HOIMONTI IMMACULATA ROZARIO Master of Science, University of Lethbridge, 2012 Master of Science, Jahangirnagar University, 2010 Bachelor of Science, Jahangirnagar University, 2009 A Thesis Submitted to the School of Graduate Studies of the University of Lethbridge in Partial Fulfillment of the Requirements for the Degree DOCTOR OF PHILOSOPHY Department of Physics and Astronomy University of Lethbridge LETHBRIDGE, ALBERTA, CANADA © Hoimonti Immacualata Rozario, 2019 HIGH-RESOLUTION SPECTROSCOPIC STUDIES OF ATMOSPHERIC GASES 15 (C2H2-N2, O2, and NH3) HOIMONTI IMMACULATA ROZARIO Date of Defence: March 27, 2019 Dr. Brant Billinghurst Senior Scientist PhD Co-supervisor Canadian Light Source Saskatoon, Saskatchewan Dr. Karl Staenz Professor PhD Co-supervisor Dr. Locke Spencer Associate Professor PhD Thesis Examination Committee Member Dr. Arundhati Dasgupta Associate Professor PhD Thesis Examination Committee Member Dr. Michael Gerken Professor PhD Internal External Examiner Dr. Ann-Lise Norman Professor PhD External Examiner University of Calgary Calgary, Alberta Dr. Craig Coburn Associate Professor PhD Chair, Thesis Examination Committee Dedication Page I would like to dedicate my PhD thesis work to my mother. iii Abstract With the modern technology and availability of spectrometer systems, it is possible to provide more accurate and new parameters to the spectroscopic databases. Accordingly, three spectroscopic studies were carried out in this thesis. The first study is intended to find the suitable line-shape models that can reproduce C2H2-N2 spectra best as well as retrieve reliable parameters, which are very useful for spectroscopic studies. The second project of oxygen A-band spectra is dedicated to retrieving a new parameter, called the speed- dependent parameter. The main goal of the third study is to obtain a better ground state line 15 list of NH3, which has never been studied as extensively as in this thesis. Performing the acetylene study will improve the use of line-shape profiles based on the spectral pressure regions. The new speed-dependent parameter and extended (439) lines 15 of NH3 spectroscopic results will progress the retrievals of atmospheric spectra and enrich spectroscopic databases. iv Acknowledgements My deepest gratefulness goes to the individuals who had always been supportive and encouraging me in any situation during my Ph.D. program. Drs. Brant Billinghurst and Karl Staenz were very kind with their suggestions and time frame. I truly appreciate their help and generosity. As my former supervisor, I am very thankful to Dr. Adriana Predoi- Cross for her support and guiding me through the various projects. My thankfulness goes to the Ph.D. committee members Drs. Arundhati Das Gupta and Locke Spencer for supporting my Ph.D. program and showing their interest in my research projects. I would like to take the opportunity to show my gratitude to Drs. Gianfranco Di Lonardo of the University of Bologna, Italy and Georg Mellau of the Justus-Liebig University of Giessen, Germany who were my internship supervisors. I really appreciate the opportunity provided by the Canadian Light Source, Saskatoon, Canada to use their facility. I want to thank all my lab colleagues for being helpful and supportive. A special appreciation goes to Dr. Chad Povey for his help and being available for discussions regarding the various research topics. My thanks go to my friends who have been understandable and supportive during the different stages of this program. I am very grateful to my family, because they have always encouraged me to explore and expand my skills and inspired me in continuing my dedication to work. Final appreciation goes to the School of Graduate Studies, the Faculty of Arts and Science, and the Department of Physics and Astronomy for being very helpful and supportive. This will not be fulfilled without thanking the NSERC CREATE Advanced v Methods, Education and Training in Hyperspectral Science and Technology (AMETHYST) program and the Alberta Terrestrial Imaging Centre (ATIC) for all the funding and opportunities. vi Contents Dedication Page ..................................................................................................... iii Abstract ................................................................................................................... iv Acknowledgements .................................................................................................. v List of Figures ...................................................................................................... xiii List of Tables ..................................................................................................... xviii List of Abbreviations ............................................................................................ xxi List of Symbols .................................................................................................. xxiii Chapter 1 Introduction........................................................................................... 1 1.1 Overview .................................................................................................... 1 1.2 History of Spectroscopy ............................................................................. 2 1.3 Spectroscopy .............................................................................................. 2 1.4 Purpose and Literature Review of the Spectroscopic Studies .................... 6 1.4.1 Line-Shape Models Testing on Acetylene Transitions ........................ 6 1.4.1.1 Literature Review………………………………………...……….7 1.4.2 Line-shape Parameters of Oxygen A-band Transitions ..................... 10 1.4.2.1 Current State of Knowledge of the Oxygen A-band……..………12 15 1.4.3 Far-Infrared Assignment Study of Ammonia ( NH3) ....................... 17 1.4.3.1 Previous Studies……………..…………………..………………18 vii 1.5 Contribution to Other Studies and Publications ....................................... 19 1.6 Summary .................................................................................................. 22 Chapter 2 Theoretical background ...................................................................... 24 2.1 Overview .................................................................................................. 24 2.2 Introduction .............................................................................................. 24 2.2.1 Fundamentals of Spectroscopy ........................................................... 25 2.2.2 Normal Modes of Molecules .............................................................. 28 2.2.3 Rotational Spectroscopy ..................................................................... 29 2.2.4 Vibrational Spectroscopy ................................................................... 34 2.2.5 Rotational-vibrational Spectra and Band Structure ............................ 38 2.2.6 Types of Molecular Bands ................................................................. 41 2.3 Line-shape Theory .................................................................................... 42 2.3.1 Beer-Lambert Law ............................................................................. 42 2.3.2 Line-shape Function ........................................................................... 43 2.4 Different Types of Line-shape Models/Profiles and Parameters ............. 45 2.4.1 Line Position, Shift, and Intensity ...................................................... 45 2.4.2 Natural Line Width (Natural Broadening) ......................................... 48 2.4.3 Doppler Width (Doppler Broadening), Gaussian Profile ................... 49 2.4.4 Pressure-Induced Collisional Broadening .......................................... 50 2.4.5 The Voigt Profile ................................................................................ 51 viii 2.4.6 Molecular Speed-dependency Effects ................................................ 54 2.4.7 Speed-dependent Voigt Profile .......................................................... 55 2.4.8 Dicke Narrowing Effect and the Diffusion Coefficient ..................... 56 2.4.9 Galatry and Rautian-Sobel’man Profiles ............................................ 57 2.4.10 Speed-Dependent Galatry (SDG) and Speed-Dependent Rautian- Sobel’man (SDR) Profiles ......................................................................................... 59 2.4.11 Line-mixing ...................................................................................... 61 2.4.12 Exponential Power Gap Scaling Law (EPG) ................................... 63 2.5 Summary .................................................................................................. 65 Chapter 3 Experimental Procedures .................................................................... 66 3.1 Overview .................................................................................................. 66 3.2 Tunable Diode-Laser Spectrometer System (C2H2-N2 study) .................. 66 3.2.1 Temperature and Pressure (T-P) Controlled Gas Cell (Channel-1) ... 70 3.2.2 Reference Gas Cell and the Background Signal ................................ 71 3.2.3 Pressure Measurements and Monitoring ............................................ 72 3.2.4 Detectors ............................................................................................. 73 3.2.5 Instrumental Line-Shape Function ....................................................
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