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Investigation of Structure-Property Relationships of Heavy-Fermion Materials Robin Macaluso Louisiana State University and Agricultural and Mechanical College

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Investigation of Structure-Property Relationships of Heavy-Fermion Materials Robin Macaluso Louisiana State University and Agricultural and Mechanical College Louisiana State University LSU Digital Commons LSU Doctoral Dissertations Graduate School 2004 Investigation of structure-property relationships of heavy-fermion materials Robin Macaluso Louisiana State University and Agricultural and Mechanical College Follow this and additional works at: https://digitalcommons.lsu.edu/gradschool_dissertations Part of the Chemistry Commons Recommended Citation Macaluso, Robin, "Investigation of structure-property relationships of heavy-fermion materials" (2004). LSU Doctoral Dissertations. 1732. https://digitalcommons.lsu.edu/gradschool_dissertations/1732 This Dissertation is brought to you for free and open access by the Graduate School at LSU Digital Commons. It has been accepted for inclusion in LSU Doctoral Dissertations by an authorized graduate school editor of LSU Digital Commons. For more information, please [email protected]. INVESTIGATION OF STRUCTURE-PROPERTY RELATIONSHIPS OF HEAVY-FERMION MATERIALS A Dissertation Submitted to the Graduate Faculty of the Louisiana State University and Agricultural and Mechanical College in partial fulfillment of the requirements for the degree of Doctor of Philosophy in The Department of Chemistry by Robin Macaluso B.S., L.S.U., December 1998 December 2004 ACKNOWLEDGEMENTS The past four years as a graduate student have been a very rewarding experience, in part, because of family and friends, scientists, and collaborators with whom I have interacted. Firstly, I must state my deep appreciation for my husband, Joseph Macaluso. Although it must have been difficult at times, Joey always encouraged me to pursue my education and career. He was my primary support when I traveled for months at a time to Los Alamos, New Mexico and even to Japan in order to conduct research. In addition to his many sacrifices, Joey has shared his knowledge and interest in cultural and historic aspects of life, which, in turn, has kept my life more interesting. I am very thankful for many supportive family members and friends, especially my parents and parents-in-law. They have shown a genuine interest in my life successes and have wholly encouraged me to pursue my aspirations. Also, it is partly due to the optimism and wisdom of Mrs. Charlene Ross (a former mentor during my brief stint as a high school teacher) that I overcame my personal fears to initiate doctoral studies. There are many individuals at Louisiana State University and other professional institutions to whom I am indebted. My advisor, Prof. Julia Chan has provided many opportunities and resources for success. Dr. Frank Fronczek, the staff crystallographer encouraged me not just to use the diffractometer for routine data collection, but to analyze the data to solve crystal structures. He was also always very willing to share his knowledge of crystallography with students. I must also thank many collaborators: Prof. David Young and Dr. Monica Moldovan (Louisiana State University), Prof. Zachary Fisk (University of California, Davis) and his graduate student, Hanoh Lee, and the research group of Prof. Yoshiteru Maeno ii (Kyoto University, Japan), particularly Lecturer Satoru Nakatsuji. Lastly, the camaraderie and scientific curiosity of fellow group members have also enhanced my graduate experience. The work presented here was performed in part due to partial funding from NSF Career (Division of Materials Research DMR-0237664), NSF Japan ACS - PRF Type G, BoR- LEQSF RCS: LEQSF(2001-04)-RD-A-05, and the Charles E. Coates Memorial, and the Charles E. Coates Memorial Scholar Research Grant. iii TABLE OF CONTENTS ACKNOWLEDGEMENTS...............................................................................................................i ABSTRACT....................................................................................................................................vii CHAPTER 1. INTRODUCTION ..................................................................................................1 1.1 Heavy Fermion Intermetallic Materials ..............................................................................1 1.2 Magnetic Ordering in Heavy Fermion Materials................................................................1 1.3 Electronic and Transport Properties of Heavy-Fermion Materials.....................................3 1.3.1 Theory of Specific Heat.............................................................................................3 1.3.2 Electronic Effective Mass..........................................................................................5 1.3.3 Experimental Determination of Specific Heat...........................................................6 1.3.4 Resistivity ..................................................................................................................7 1.4 Fundamentals of Magnetism..............................................................................................8 1.4.1 RKKY Mechanism.....................................................................................................8 1.4.2 The Kondo Effect.......................................................................................................9 1.4.3 Curie-Weiss Law .....................................................................................................10 1.4.4 Determination of Effective Moment........................................................................11 1.5 Single Crystal X-Ray Diffraction ....................................................................................12 1.5.1 Bragg’s Law.............................................................................................................12 1.5.2 Reciprocal Lattice ....................................................................................................12 1.5.3 Sample Preparation ..................................................................................................14 1.5.4 Instrumentation ........................................................................................................14 1.5.5 Data Processing........................................................................................................15 1.5.6 Space Group Determination.....................................................................................16 1.5.7 Structure Solution ....................................................................................................16 1.5.8 Other Parameters for Refinement ............................................................................17 1.6 References ........................................................................................................................19 CHAPTER 2. CRYSTAL GROWTH AND STRUCTURE DETERMINATION OF LaMIn5 (M=Co, Rh, Ir)................................................................................................................................22 2.1 Introduction......................................................................................................................22 2.2 Experimental....................................................................................................................23 2.2.1 Flux Growth Techniques..........................................................................................23 2.2.2 Single Crystal X-Ray Diffraction ............................................................................26 2.2.3 Physical Property Measurements.............................................................................27 2.3 Results and Discussion .................................................................................................... 27 2.3.1 Crystal Structure ......................................................................................................27 2.3.2 Calculations..............................................................................................................31 2.4 References ........................................................................................................................33 CHAPTER 3. SINGLE-CRYSTAL GROWTH OF Ln2MIn8 (Ln = La, Ce; M = Rh, Ir): IMPLICATIONS FOR THE HEAVY-FERMION GROUND STATE.........................................35 3.1 Introduction......................................................................................................................35 3.2 Experimental....................................................................................................................36 iv 3.2.1 Synthesis.................................................................................................................36 3.2.2 Single Crystal X-Ray Diffraction ...........................................................................37 3.2.3 Electron Microprobe Analysis ................................................................................40 3.2.4 Physical Property Measurements............................................................................41 3.3 Results and Discusison .................................................................................................... 41 3.3.1 Crystal Structure .....................................................................................................42 3.3.2 Relationship of Structure Parameters to Physical Properties – Resistivity.............44 3.3.3 Relationship of Structure Parameters to Physical Properties – Magnetism............45 3.4 Conclusion.......................................................................................................................46 3.5 References ........................................................................................................................48
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