University of Calgary PRISM: University of Calgary's Digital Repository Graduate Studies The Vault: Electronic Theses and Dissertations 2019-08-20 Ice Nucleation: Sulfate and Its Influence in Arctic and Rural and Urban NW Continental Precipitation Derksen, Mark Derksen, M. (2019). Ice Nucleation: Sulfate and Its Influence in Arctic and Rural and Urban NW Continental Precipitation (Unpublished master's thesis). University of Calgary, Calgary, AB. http://hdl.handle.net/1880/110824 master thesis University of Calgary graduate students retain copyright ownership and moral rights for their thesis. You may use this material in any way that is permitted by the Copyright Act or through licensing that has been assigned to the document. For uses that are not allowable under copyright legislation or licensing, you are required to seek permission. Downloaded from PRISM: https://prism.ucalgary.ca UNIVERSITY OF CALGARY Ice Nucleation: Sulfate and Its Influence in Arctic and Rural and Urban NW Continental Precipitation by Mark Derksen A THESIS SUBMITTED TO THE FACULTY OF GRADUATE STUDIES IN PARTIAL FUFULMENT OF THE REQUIREMENTS FOR THE DEGREE OF MASTER OF SCIENCE GRADUATE PROGRAM IN PHYSICS AND ASTRONOMY CALGARY, ALBERTA AUGUST, 2019 © Mark Derksen 2019 Abstract With the growth of urban centers and decline of natural ecosystems, the increasing presence of aerosol particles has the potential to have major impacts on climate. This study assessed the ice nucleation characteristics of anthropogenic and organic/biogenic sulfate sources in precipitation samples from the Arctic, Kananaskis (rural continental), and Calgary (Urban continental). Samples were analyzed using droplet freezing technique, isotopic analysis, and anion/cation measurements. Comparisons between deposition-based precipitation sampler and passive fog/rain sampler yielded no significant differences in ice nucleation characteristics. Arctic fog samples had distinct ice nucleating particle characteristics compared to rain and dry deposition samples. A 32% increase in the influence of biogenic matter was apparent in 2016 Arctic samples relative to 2014 samples. The influence of a continental biogenic and/or organic material was apparent in the ice nucleating characteristics of both rural and urban continental samples. Snow samples exhibited the greatest biogenic influence, followed by rain samples, and then dry deposition samples. ii Acknowledgements This thesis would not have been possible with the help of so many people, and I am very grateful to you all! First and foremost, I would like to thank my supervisor Dr. Ann-Lise Norman for the extensive guidance, mentorship, motivation, and encouragement. This project provided me with amazing opportunities to grow and learn as a researcher. Thank you to Dr. Mike Wieser and Dr. David Hobill for the invaluable feedback, and lending your expertise, time, and support. Thank you to my lab colleagues Roghayeh Ghahremaninezhadgharelar, Chenqi Ge, and Neda Amiri. You were always happy to lend a hand or answer my questions. Thank you to Farzin Malekani for the technical assistance in laboratory sample analysis. Thank you to my longtime mentor and friend Dr. Trent Hoover, for your endless advice and support. I would like to dedicate a special thanks towards my friends and family, who were always supportive and encouraging during my project. iii Table of Contents Abstract.......................................................................................................................................... ii Acknowledgement........................................................................................................................ iii Table of Contents ......................................................................................................................... iv List of Tables ....................................................................................................………………....vii List of Figures and Illustrations .......................................................................……………….viii List of Abbreviations………….........................................................................………………...xii Chapter One: Introduction ...........................................................................................................1 1.1 Atmospheric Aerosol Impacts and Sulfate Influences ……………………..............1 Chapter Two: Atmospheric Aerosols...........................................................................................4 2.1 Arctic Amplification and Aerosol Influences…………………………………….....4 2.2 Radiative Influences………………………………………………………………….6 2.3 Cloud Condensation and Ice Nuclei…………………………………………………8 2.4 Mixed-phase Clouds………………………………………………………………….8 2.5 Ice Nucleation……………………………………………………………………….10 2.6 Ice Nucleation Measurement Techniques………………………………………….12 2.6.1 Wet Dispersion Methods………………………………………………….13 2.6.2 Dry Dispersion Methods………………………………………………….13 2.7 Effective Ice Nuclei Properties……………………………………………………...14 2.8 Aerosol Sources……………………………………………………………………...18 2.9 Arctic Biogenic Sulfate……………………………………………………………...22 2.10 Arctic DMS and the CLAW Hypothesis………………………………...………..23 2.11 Sulfur Isotopes……………………………………………………………….…….26 2.12 Study Objectives…………………………………………………………………...28 Chapter Three: Study Site, Sampling and Analysis Methodology…………………………...30 3.1 Arctic Precipitation Samples.....................................................................................30 3.2 Kananaskis/Calgary Precipitation Samples………................................................33 3.3 Ice Nucleation Experiments……...............................................................................33 iv 3.4 Cation/Anion Analysis...............................................................................................37 3.5 Sulfate Analysis...........................................................................................................38 3.6 HYSPLIT Analysis.....................................................................................................38 3.7 Uncertainty and Statistics..........................................................................................38 Chapter Four: Ice Nucleation Concentrations and Isotope Results.........................................40 4.1 Filtered versus Unfiltered Samples...........................................................................40 4.2 Precipitation Blanks and Samples.............................................................................43 4.3 2014 versus 2016 Arctic Samples...............................................................................46 4.3.1 Ion/Cation Results: Arctic 2016..................................................................46 4.3.2 INP Concentrations: 2014, 2016 Fog + Rain..............................................48 4.4 Rural and Urban Continental Samples……….........................................................52 4.4.1 Ion/Cation Results.......................................................................................52 4.4.2 Kananaskis/Calgary Air Mass Back Trajectories.....................................54 4.4.3 INP Concentrations: Urban and Rural Concentrations...........................57 4.5 Sulfur Isotope Results................................................................................................61 Chapter Five: Discussion ............................................................................................................63 5.1 Comparison of Filtered and Unfiltered INP.............................................................63 5.2 Blanks Versus Samples..............................................................................................65 5.3 Arctic Sampling Observations...................................................................................66 5.4 Alberta Sampling Observations................................................................................68 5.5 Arctic versus Alberta..................................................................................................69 5.6 Sulfur Isotopes............................................................................................................70 5.7 Ice Nucleation Characteristics...................................................................................72 5.7.1 Ice Nucleation Curves.................................................................................72 5.7.2 Arctic Rain, Fog, and Dry Deposition........................................................73 5.7.3 Contrasts in Urban/Rural Continental Samples.......................................76 5.7.4 Comparison of Continental with Arctic INP.............................................77 v Chapter Six: Summary and Recommendations.........................................................................79 6.1 Summary.....................................................................................................................79 6.2 Recommendations for Future Works........................................................................81 References.....................................................................................................................................83 Appendix.......................................................................................................................................92 Table of slopes calculated from INP(T) data…………………………...……………...92 vi List of Tables Table 5.1 Differences between filtered and unfiltered samples for a 2013 Calgary flood precipitation