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High Resolution Spectra of Carbon Monoxide, Propane and Ammonia for Atmospheric Remote Sensing Old Dominion University ODU Digital Commons OES Theses and Dissertations Ocean & Earth Sciences Summer 2017 High Resolution Spectra of Carbon Monoxide, Propane and Ammonia for Atmospheric Remote Sensing Christopher Andrew Beale Old Dominion University, [email protected] Follow this and additional works at: https://digitalcommons.odu.edu/oeas_etds Part of the Atmospheric Sciences Commons, Physical Chemistry Commons, and the Remote Sensing Commons Recommended Citation Beale, Christopher A.. "High Resolution Spectra of Carbon Monoxide, Propane and Ammonia for Atmospheric Remote Sensing" (2017). Doctor of Philosophy (PhD), Dissertation, Ocean & Earth Sciences, Old Dominion University, DOI: 10.25777/ev91-0796 https://digitalcommons.odu.edu/oeas_etds/7 This Dissertation is brought to you for free and open access by the Ocean & Earth Sciences at ODU Digital Commons. It has been accepted for inclusion in OES Theses and Dissertations by an authorized administrator of ODU Digital Commons. For more information, please contact [email protected]. HIGH RESOLUTION SPECTRA OF CARBON MONOXIDE, PROPANE AND AMMONIA FOR ATMOSPHERIC REMOTE SENSING By Christopher Andrew Beale B.Sc. July 2010, University of York, UK M.Sc. July 2012, University of York, UK A Dissertation Submitted to the Faculty of Old Dominion University in Partial Fulfillment of the Requirements for the Degree of DOCTOR OF PHILOSOPHY OCEANOGRAPHY OLD DOMINION UNIVERSITY August 2017 Approved by: Peter F. Bernath (Director) John Klinck (Member) Charles I. Sukenik (Member) ABSTRACT HIGH RESOLUTION SPECTRA OF CARBON MONOXIDE, PROPANE AND AMMONIA FOR ATMOSPHERIC REMOTE SENSING Christopher Andrew Beale Old Dominion University, 2017 Director: Dr. Peter F. Bernath Spectroscopy is a critical tool for analyzing atmospheric data. Identification of atmospheric parameters such as temperature, pressure and the existence and concentrations of constituent gases via remote sensing techniques are only possible with spectroscopic data. These form the basis of model atmospheres which may be compared to observations to determine such parameters. To this end, this dissertation explores the spectroscopy of three molecules: ammonia, propane and carbon monoxide. Infrared spectra have been recorded for ammonia in the region 2400-9000 cm-1. These spectra were recorded at elevated temperatures (from 293-973 K) using a Fourier Transform Spectrometer (FTS). Comparison between the spectra recorded at different temperatures yielded experimental lower state energies. These spectra resulted in the measurement of roughly 30000 lines and about 3000 quantum assignments. In addition spectra of propane were recorded at elevated temperatures (296-700 K) using an FTS. Atmospheres with high temperatures require molecular data at appropriate conditions. This dissertation describes collection of such data and the potential application to atmospheres in our solar system, such as auroral regions in Jupiter, to those of planets orbiting around other stars and cool sub-stellar objects known as brown dwarfs. The spectra of propane and ammonia provide the highest resolution and most complete experimental study of these gases in their respective spectral regions at elevated temperatures. Detection of ammonia in an exoplanet or detection of propane in the atmosphere of Jupiter will most likely rely on the work presented here. The best laboratory that we have to study atmospheres is our own planet. The same techniques that are applied to these alien atmospheres originated on Earth. As such it is appropriate to discuss remote sensing of our own atmosphere. This idea is explored through analysis of spectroscopic data recorded by an FTS on the Atmospheric Chemistry Experiment satellite of carbon monoxide. The effect of the atmosphere’s chemistry and physics on this molecule is measured through its isotopologues, primarily 13CO (carbon-13 substituted carbon monoxide). Isotopic chemistry allows a key analysis of the atmosphere as it may be used as a tracer for chemical reactions and dynamical processes. The carbon monoxide fractionation results in Chapter IV present the first global measurements of isotopic fractionation of CO, showing significant fractionation in the upper atmosphere (60-80 km) as a result of the photolysis of carbon dioxide (CO2). iv For my family v ACKNOWLEDGEMENTS My journey through graduate school has not been a short one. Throughout the seven years from starting my M.Sc. at York to finishing my Ph.D. at Old Dominion University I have been indebted to my advisor, Professor Peter Bernath. My development as a scientist is primarily due to being part of the Bernath group. It has been a privilege to be a part of a diverse and entertaining team! Many of the methods used for my research were first developed by Dr. Robert Hargreaves and having him in the group helped my professional progression. For much of the ACE research, the constant back and forth between Eric Buzan and me helped me immensely and I hope this was reciprocated! Other members of the group who deserve thanks are Mike Dulick for organizing the lab and making things run smoothly, the postdocs who have come and gone during my time here, Drs. Dan Frohman, Andy Wong, Jamie Hodges and Dror Bittner. Even though my research and that of other students in the group may have not always overlapped, I’m thankful to have had Anton Fernando and Mehdi Yousefi as well as Eric for making the group a great place to work. I also thank Professor Hans-Peter Plag for the significant edits suggested after the first draft. For life outside of work and study I thank all of the graduate students in the Ocean. Earth and Atmospheric Sciences Department, especially Bonnie, Will, Malee and Brittany as well as Rob, Andy and Dan from the group for their friendship and for enabling me to take some well needed time from the office. I am immensely grateful to the Torrillo family for being a real home away from home, being so far away from my own family was never easy and to be extended the kind of love and care that I was means a great deal to me and certainly made this journey of mine possible. vi As for my own family, I cannot express my gratitude easily. As difficult as my time at ODU has been for me, my family have always been there for me, in every capacity possible. For family members lost and for those gained, I dedicate this dissertation to you. vii TABLE OF CONTENTS Page LIST OF TABLES ...........................................................................................................................x LIST OF FIGURES ...................................................................................................................... xii Chapter I. INTRODUCTION ...............................................................................................................1 II. ATMOSPHERIC CHEMISTRY BACKGROUND ............................................................4 VERTICAL STRUCTURE OF THE ATMOSPHERE ...........................................4 COMPOSITION OF THE ATMOSPHERE ............................................................6 METHODS OF ATMOSPHERIC MEASUREMENT ...........................................7 SATELLITE REMOTE SENSING .........................................................................7 THE ATMOSPHERIC CHEMISTRY EXPERIMENT ..........................................8 ATMOSPHERIC MODELS ..................................................................................11 ASTRONOMICAL ATMOSPHERES ..................................................................12 SOLAR SYSTEM PLANETS ...............................................................................13 BROWN DWARFS ...............................................................................................14 EXOPLANET ATMOSPHERES ..........................................................................18 III. SPECTROSCOPY BACKGROUND ................................................................................21 INTRODUCTION .................................................................................................21 ROTATIONAL SPECTROSCOPY ......................................................................22 VIBRATIONAL SPECTROSCOPY .....................................................................24 FUNDAMENTAL, OVERTONE, HOT BAND AND COMBINATION TRANSITIONS .....................................................................................................25 SELECTION RULES ............................................................................................27 SPECTRAL LINESHAPE .....................................................................................29 LINELISTS ............................................................................................................31 viii Page FOURIER TRANSFORM SPECTROSCOPY......................................................32 IV. ISOTOPIC FRACTIONATION OF CARBON MONOXIDE .........................................41 INTRODUCTION .................................................................................................41 EXPERIMENTAL .................................................................................................45 ISOTOPIC EFFECTS ON INFRARED SPECTRA..............................................52 WACCM ................................................................................................................55 RESULTS FOR 13CO ............................................................................................58 ISOTOPIC FRACTIONATION OF C17O AND C18O ..........................................65
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