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Evolution of Intrinsic Point Defects in Fluorite-Based Materials: Insights from Atomic-Level Simulation

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Evolution of Intrinsic Point Defects in Fluorite-Based Materials: Insights from Atomic-Level Simulation EVOLUTION OF INTRINSIC POINT DEFECTS IN FLUORITE-BASED MATERIALS: INSIGHTS FROM ATOMIC-LEVEL SIMULATION By DILPUNEET SINGH AIDHY A DISSERTATION PRESENTED TO THE GRADUATE SCHOOL OF THE UNIVERSITY OF FLORIDA IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF DOCTOR OF PHILOSOPHY UNIVERSITY OF FLORIDA 2009 1 © 2009 Dilpuneet S. Aidhy 2 To my parents with love and gratitude 3 ACKNOWLEDGMENTS At this very juncture of my life, where I now bridge my educational and professional career, I want to take this opportunity to thank some very important people who have made my PhD a wonderful journey. I express my deepest gratitude towards my mentor Prof. Simon Phillpot, whose advising skills, besides scientific knowledge, I find to be exceptional. His enthusiasm towards science, trust and patience with students blended with a great sense of humor has made my PhD thoroughly enjoyable. He has always provided liberty to explore things even not directly related to research and has shared his wisdom. I feel fortunate to have him as an advisor, responsibility of which, he fulfilled perfectly. I also want to thank Dr. Dieter Wolf with whom I have had many thought-provoking discussions from which this thesis has benefited immensely. I have never met a more humble person than him. I admire his love for nature and thank him for stimulating me to explore western US. I also thank Dr. Paul Millet, Dr. Tapan Desai and Srujan, with whom I enjoyed our collaborative work on nuclear materials. Thanks to the friends I made in Idaho, their generosity and warmth softened the blow of Idaho winters. Many thanks to my committee members, Profs. Susan Sinnott, Juan Nino, Eric Wachsman and Jason Weaver for serving on my committee and providing valuable suggestions to my research work. Special thanks to Prof. Sinnott for co-advising me, Prof. Nino for teaching me crystallography and Prof. Wachsman for keeping me honest from experimental standpoint. I want to mention some of the very dear friendships that I feel fortunate to have developed during the years. Special thanks to Tabassum for giving me moral support especially during the semester-ending result times, Rakesh for his always-welcome attitude and 4 exceptionally delicious food, and Sankara for being a perfect roommate. Besides, all current and past members of the Sinpot group, thanks also to Priyank, Chan-Woo, Taku, Peter and Tao. All of you did bear me very kindly. In the end, I want to mention my dad and my mom, to thank whom I do not have enough words. They have been the supporting pillars of my life and have never let the distance of seven seas interfere in keeping their warmth of love around me. I am indebted to you, dad, especially for letting me to pursue a degree in the US, exactly a month after you underwent heart surgery, and you mom, for being especially strong during that time. I do not want to forget my little sister who throughout these years looked forward more to souvenirs than me. It would be inappropriate to not to thank the Almighty for making this journey easy and fruitful. 5 TABLE OF CONTENTS Page ACKNOWLEDGMENTS.................................................................................................................... 4 LIST OF TABLES.............................................................................................................................. 10 LIST OF FIGURES ............................................................................................................................ 11 ABSTRACT ........................................................................................................................................ 15 CHAPTER 1 GENERAL INTRODUCTION .................................................................................................. 17 1.1 Sources of Energy ................................................................................................................. 17 1.2 Energy and Environment ...................................................................................................... 19 1.3 Clean Technology ................................................................................................................. 20 1.4 Challenges in Materials Science .......................................................................................... 22 1.5 Motivation for This Work .................................................................................................... 23 1.6 Significance of Simulation ................................................................................................... 24 1.7 Objective of This Work ........................................................................................................ 25 1.8 Organization of Dissertation ................................................................................................ 26 2 DEFECTS IN SOLIDS ............................................................................................................... 27 2.1 Introduction ........................................................................................................................... 27 2.2 Intrinsic Point Defects .......................................................................................................... 27 2.2.1 Frenkel Defect ............................................................................................................ 28 2.2.2 Schottky Defect .......................................................................................................... 29 2.2.3 Thermodynamics of Point Defects: Equilibrium Concentration ............................. 29 2.3 Transport................................................................................................................................ 32 2.3.1 Atomistic Theory of Diffusion .................................................................................. 32 2.3.2 Diffusion Mechanisms ............................................................................................... 34 2.3.2.1 The vacancy mechanism ................................................................................. 34 2.3.2.2 The interstitial mechanism .............................................................................. 34 2.3.2.3 The interstitialcy mechanism .......................................................................... 35 2.4 Crystallography of Materials ................................................................................................ 36 2.4.1 Fluorite Crystal Structure: δ-Bi2O3 and UO2 ............................................................ 36 2.4.2 Rocksalt Crystal Structure: MgO .............................................................................. 37 2.4.3 Space Group Fm3 m .................................................................................................. 37 2.4.4 Body-Centered Cubic: Space Group Im 3 m ............................................................ 39 3 SIMULATION METHODOLOGY ........................................................................................... 40 3.1 Simulation Methodologies ................................ ................................................................... 40 3.2 Molecular Dynamics Simulation ......................................................................................... 41 6 3.3 General MD Algorithm ........................................................................................................ 41 3.4 Periodic Boundary Condition ............................................................................................... 44 3.5 Interatomic Interactions ........................................................................................................ 45 3.5.1 Long-range Interactions ............................................................................................. 47 3.5.2 Short-Range Interactions ........................................................................................... 53 3.5.3 Electronic Polarizability – Shell Model .................................................................... 55 3.5.4 Thermodynamic Conditions (ensemble) for Materials Simulation ......................... 56 4 IONIC CONDUCTIVITY OF SOLID-OXIDE FUEL CELL ELECTROLYTE................... 58 4.1 Fuel Cell ................................................................................................................................ 58 4.2 Solid Oxide Fuel Cell ........................................................................................................... 59 4.3 Fluorite-Based Cubic Bismuth Oxide .................................................................................. 61 4.3.1 A Model Material ....................................................................................................... 61 4.3.2 δ-Bi2O3 Limitations .................................................................................................... 63 4.3.3 Ionic Radii or Polarizability? ..................................................................................... 64 4.4 Simulation Methodology ...................................................................................................... 66 4.5 Results.................................................................................................................................... 67 4.5.1 Polarizability Indeed .................................................................................................. 67 4.5.1.1 Polarizable and non-polarizable ions.............................................................
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