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PDF (Shuster Thesis Final.Pdf) APPLICATION OF SPALLOGENIC NOBLE GASES INDUCED BY ENERGETIC PROTON IRRADIATION TO PROBLEMS IN GEOCHEMISTRY AND THERMOCHRONOMETRY Thesis by David Lawrence Shuster In Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy CALIFORNIA INSTITUTE OF TECHNOLOGY Pasadena, California 2005 (Defended May 12, 2005) ii © 2005 David Lawrence Shuster All Rights Reserved iii ACKNOWLEDGEMENTS I thank Prof. Ken Farley for the scientific opportunities, intellectual stimulation, encouragement, and friendship he provided me as my thesis advisor. I also thank Prof. Don Burnett for the countless times I dropped into his office with “quick” questions on nuclear physics and for his invaluable input to my work. I am grateful to Prof. Jess Adkins, who acted as my academic advisor and personal confidant throughout my five years at Caltech, and to Prof. John Eiler for numerous discussions and for serving on my thesis committee. I thank Prof. Tapio Schneider for his help with the inversion mathematics presented in Chapter I. I also benefited from insightful discussions with Prof. Jerry Wasserburg, who gave me a taste of the “old school,” grilling me with difficult questions about my work while at the white board in his office. I am grateful for the efforts and input of my collaborators Dr. Janet Sisterson (Northeast Proton Therapy Center), Prof. Paulo Vasconcelos (University of Queensland, Brisbane), and Mr. Jonathan Heim (University of Queensland, Brisbane) whose work is presented in this dissertation. I am also grateful for the collaborative relationships I have developed with (former) fellow Caltech grad students Prof. Ben Weiss (MIT), Prof. Sujoy Mukhopadhyay (Harvard), and Prof. Sarah Stewart-Mukhopadhyay (Harvard). These three, in particular, have taught me much about doing science and set a high bar for me. I will forever be indebted to my officemates and dear friends (future Drs.) Julie O’Leary, Juliane Fry, and John Crounse for countless discussions on all matters imaginable. It has been a remarkable experience to share workspace with such a diverse group of creative young scientists. I am happy to give special acknowledgement to Ms. Lindsey Hedges, who worked many hours helping to prepare my samples both before and after proton iv irradiations. Without her expertise and patience much of the work presented here would not have been completed (at least in a timely fashion). I also thank Dr. Mack Kennedy (Lawrence Berkeley National Laboratory), Prof. Don DePaolo (UC Berkeley), and Prof. Martha House (Pasadena City College). Each of these people played an important role in my decision to become a Ph.D. student at Caltech. I was introduced to and learned how to do noble gas geochemistry in Mack’s lab, an experience that has been invaluable to me as a grad student. I was encouraged to go to Caltech by Don, and Martha’s work sufficiently inspired me to seal the deal. I acknowledge the financial support of the Caltech Special Institute Fellowship program and the National Science Foundation Graduate Research Fellowship program, both of which provided me a little more intellectual freedom than I may have otherwise had. Lastly, I thank my family, my mother, my sisters, and Rick and Aldeana Saber. They have always supported me emotionally and have been patient when I haven’t always been available to them during these last five years. I dedicate this dissertation to my grandfather, David W. Anderson (BS ’32), who initially put the Caltech bug in my head when I was a high school student and whose influence has caused a high priority to be placed on intellectual pursuit within my family. Although he did not live to read this work, I know that he would be very proud. v ABSTRACT Synthetic components of 3He, 4He, and 21Ne were generated within natural minerals via irradiation with 150 and 220 MeV proton beams. Fluences of ~1014 and ~1016 protons/cm2 induced 3He concentrations of ~108 and ~109 atoms/mg, respectively. Controlled degassing experiments on irradiated samples of terrestrial apatite (Ca5(PO4)3F), titanite (Ca(TiO)(SiO4)), olivine ((Mg,Fe)2SiO4), goethite (FeOOH), and quartz (SiO2) demonstrate that the proton-induced nuclides are spatially uniform across samples ≤ 1 mm in diameter and sequential degassing quantifies solid-state diffusion kinetics of helium and neon. Diffusion 3 kinetics of proton-induced He in Durango apatite (Ea = 147.9 ± 1.3 kJ/mol; 2 -1 ln(Do/a ) = 16.0 ± 0.3 ln(s )) and Fish Canyon tuff titanite (Ea = 183.7 ± 2.7 2 -1 kJ/mol; ln(Do/a ) = 13.3 ± 0.5 ln(s )), are indistinguishable from those determined for natural radiogenic 4He in the same samples. Experiments indicate that lattice damage potentially introduced via proton irradiation did not significantly modify the natural 4He diffusion kinetics in the two samples, and that the proton-induced 4He component is relatively negligible in abundance. Therefore, sequentially measured 4He/3He ratios reflect the natural spatial distribution of radiogenic 4He. Combined with a (U-Th)/He age and helium diffusion kinetics, the distribution limits the time-temperature (t-T) path a mineral experienced through geologic time. This is the basis for a new methodology called 4He/3He thermochronometry, which for apatite constrains continuous t-T paths between 80 oC and 20 oC. Proton-induced 3He diffusion parameters in olivine 2 -1 o are: Ea = 153.8 ± 1.1 kJ/mol and ln(Do/a ) = 3.0 ± 0.2 ln(s ). At 25 C, the 2 helium diffusion kinetics in a goethite sample (Ea = 163 ± 2.4 kJ/mol; ln(Do/a ) = 26.0 ± 0.6 ln(s-1)) predict 90% 4He retention over 11.8 Ma, consistent with the observed deficit gas fraction and (U-Th)/He age of 10.7 Ma. This indicates that goethite (U-Th)/He dating is a viable weathering geochronometer. In quartz, the vi 21 3 diffusion kinetics for proton-induced Ne and He (Ea = 153.7 ± 1.5 (kJ/mol); 2 -1 2 ln(Do/a ) = 15.9 ± 0.3 (ln(s )) and Ea = 84.5 ± 1.2 (kJ/mol); ln(Do/a ) = 11.1 ± 0.3 (ln(s-1), respectively), indicate that cosmogenic neon will be quantitatively retained in inclusion-free quartz at Earth surface temperatures whereas cosmogenic helium will not. vii TABLE OF CONTENTS Acknowledgements............................................................................................................ iii Abstract.................................................................................................................................v Table of Contents..............................................................................................................vii List of Tables........................................................................................................................x List of Figures .....................................................................................................................xi Introduction .........................................................................................................................1 Chapter I: 4He/3He thermochronometry .......................................................................8 Introduction ................................................................................................................10 Theory ..........................................................................................................................13 Uniform 3He distribution..............................................................................13 Constraining an initial profile with a stepwise degassing experiment...14 Forward model matching and inversion.........................................17 Chronometric implications of the initial profile .......................................20 Methods - simulations...............................................................................................21 Results ..........................................................................................................................25 Forward models..............................................................................................25 Isothermal profiles..............................................................................25 Monotonic cooling..............................................................................28 Monotonic cooling followed by 5 Myr at 25 oC............................29 Distinct thermal histories for samples with a common He age.31 Inversions.........................................................................................................32 Discussion ...................................................................................................................35 Forward model matching..............................................................................37 Inversion accuracy and resolution...............................................................38 Plotting space ..................................................................................................40 Correcting (U-Th)/He ages..........................................................................44 Constraining thermal histories .....................................................................44 Conclusion...................................................................................................................46 Acknowledgements....................................................................................................46 Chapter II: Quantifying the diffusion kinetics and spatial distributions of radiogenic 4He in minerals containing proton-induced 3He .....................................48 Introduction ................................................................................................................49
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