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Photoluminescence and Resonance Raman Spectroscopy of MOCVD Grown Photoluminescence and Resonance Raman Spectroscopy of MOCVD Grown GaAs/AlGaAs Core-Shell Nanowires A Thesis Submitted to the Faculty of Drexel University by Oren D. Leaer in partial fulllment of the requirements for the degree of Doctorate of Philosophy February 2013 © Copyright 2013 Oren D. Leaer. Figure 5.1 is reproduced from an article copyrighted by the American Physical Society and used with their permission. The original article may be found at: http://link.aps.org/doi/10.1103/PhysRevB.80.245324 Regarding only gure 5.1, the following notice is included as part of the terms of use: Readers may view, browse, and/or download material for temporary copying purposes only, provided these uses are for noncommercial personal purposes. Except as provided by law, this material may not be further reproduced, distributed, transmitted, modied, adapted, performed, displayed, published, or sold in whole or part, without prior written permission from the American Physical Society. The rest of this work is licensed under the terms of the Creative Commons Attribution-ShareAlike license Version 3.0. The license is available at: http://creativecommons.org/licenses/by-sa/3.0/. i Dedications To my family: my parents, my sister, and Bubby and Dan. Your support made this possible. Thank you. ii Acknowledgments It is with great pleasure that I am able to thank and acknowledge the individuals and organizations that helped me in the course of my graduate studies. I should begin by thanking my advisor, Dr. Spanier, and my committee, Drs. Livneh, May, Shih, Taheri, and Zavaliangos for supporting me through this rather long process. Working for Dr. Spanier helped me grow as a scientist and learn things that extend well beyond the lab. And Dr. Spanier, thank you again for the opportunities for collaboration and travel. I would like to additionally thank Dr. May for allowing me to take advantage of his open oce door and drop in and ask questions on a number of occasions. And, Tsachi, thank you for your support and advice; I don’t know how this dissertation would have been completed without your help. I would like to acknowledge my funding sources: I was supported by the GAANN fellowship from the Department of Education, the Dean’s fellowship, and the National Science Foundation (NSF) EAPSI fellowship for summer 2011. The work presented here was part of an ongoing collaboration with our Italian colleagues who I had the pleasure of visiting in Lecce, Italy. Nico Lovergine and Paola Prete supplied the nanowires that are the topic of this work. In addition to providing us with samples, they graciously shared their data and allowed me to reproduce it in gure 2.2. Adriano Cola hosted me at the lab in Lecce and made sure that I saw the lab’s fantastic surroundings. In the lab, I learned to use the FIB from Enrico Melissano. Thanks to Anna Fontcuberta i Morral and the American Physical Society for granting permission to reproduce the gure that appears in gure 5.1. I also gratefully acknowledge the help of Dr. Craig Johnson and Stephanie Johnson in acquiring the TEM micrograph presented in gure 2.4 A number of people at Drexel enriched my graduate experience. I would like to thank Dr. Barsoum for the chance to be part of the MAX-phase collaboration; I feel fortunate to have been part of such a productive collaboration. Volker Presser generously provided access to the Renishaw Raman system at the William Keck Institute; in addition to taking the time to iii train me on the instrument, he also took the time to help nd the right conguration for the instrument. My colleagues in the lab – Chris Hawley, Jennifer Atchison, Mohammad Islam, Maria Torres, Sean Chen, Stephanie Johnson, Stephen Nonnenmann, and Terrence McGuckin – helped keep standards high and worked to keep things fun as we toiled away and I hope to collaborate with them in the future. Kevin Siegl and Alex Juskovic both taught me quite a bit when I mentored them. Judy Trachtman, Dorilona Rose, Keiko Nakazawa, Yeneeka Long, and Sarit Kunz helped me navigate the university bureaucracy. Andrew Marx provided various acts of technical support over the years. Scott Currie was a great help in building my experiments, as were Mark Shiber and the sta at the Drexel machine shop. And thank you to Dr. Knight for your continued eorts to keep our labs safe. I was fortunate to be able to take classes from Nader Engheta, Andrea Liu, and Vaclav Vitek at the University of Pennsylvania. I am grateful for how welcome I was made to feel in those classes. The highlight of my time as a graduate student was spending a few months at the Australian National Fabrication Facility’s New South Wales Node (ANFF-NSW) in Sydney, Australia as an EAPSI fellow during the summer of 2011. I would like to thank the NSF and the Australian Academy of Sciences (AAS) for the funding and logistical support. Meaghan O’Brien of the AAS did a wonderful job of helping with many of the arrangements in Australia. I am deeply indebted to my host at the ANFF-NSW Facility, Prof. Andrew Dzurak, and to Rosie Hicks for helping to arrange my visit. Dr. Fay Hudson generously shared her nanofabrication expertise with me. And it was a great experience working with the sta at the ANFF-NSW: Frank Wright, Gordon Bates, Warren McKenzie, Joanna Szymanska, and El van Zeijl. Prof. Chennupati Jagadish of the Australian National University graciously hosted me when I visited for a day. He and his team showed me great hospitality and were extremely generous with their technical knowledge. Evan Malone and the sta at NextFab Studio were a great help with building experimental equipment and also provided a pleasant work environment. Matt Blaze, Andrew, Sandy, Perry, and Sam made me feel at home in their lab. Leslie Mitts saw that I needed a place to sit Acknowledgments iv and write and invited me to work from the SBDC. And Babak, Dev, and Q kindly let me camp out in their lab space. A number of people helped make Sydney feel like home. I was privileged to live with Oliver and Beun who shared their home with me. Dov Rosenfeld helped me nd the ANFF and introduced me to his family in Sydney: Shula, Peter, and Ronny took good care of me while I was there. I would like to thank my friends Tim Verstynen and Jesse Engel for giving me some much-needed perspective. Dan and Ashlee, Ian and Alexis, Billy and Mimi, Micah, Cookie, Adriana, and Rich Grote hosted me at dierent times while I attended conferences. Nick Vacirca and Andrew Bohl helped keep the atmosphere at Drexel light. Linda Anderson and Howard Baker helped me get through this intact. Terrence, Amy, Zoë, and Calyx were patient with me as a housemate for an intended few months that turned into much longer. Matt Robinson and my father helped with the editing. Any mistakes that remain are mine, but there are denitely fewer thanks to their help. And I am extremely grateful to my family for not only putting up with me through my rather long periods of graduate school related crankiness, but also being consistently supportive and helping me see this through to completion. v Table of Contents List of Figures ...................................... vii Abstract ......................................... xi 1. Introduction .................................... 1 1.1 Semiconductor Heterostructures........................ 1 1.1.1 The Double Heterostructure Laser................... 3 1.1.2 Quantum Well Devices......................... 5 2. Fundamentals of Core-Shell Nanowires ................... 8 2.1 Our Samples and Hypothesis.......................... 8 2.2 VLS Growth of Nanowires ........................... 12 2.3 Impurities and Defects ............................. 15 2.3.1 Carbon.................................. 15 2.3.2 Wurtzite and Planar Defects...................... 17 3. Photoluminescence of GaAs/AlGaAs Nanowires . 18 3.1 Introduction ................................... 18 3.2 Experimental Procedures............................ 19 3.2.1 Sample Preparation........................... 19 3.2.2 Experimental Conditions........................ 20 3.3 Photoluminescence Results........................... 21 3.3.1 PL From GaAs Wafer.......................... 21 3.3.2 Bare GaAs Nanowires.......................... 22 3.3.3 Core-Shell Nanowires.......................... 23 3.4 Interpretation of Results and Relevant Eects................. 28 3.4.1 Bandgap Narrowing .......................... 28 3.4.2 Donor-Acceptor Pair Luminescence.................. 29 3.4.3 The Role of Hydrogen ......................... 30 3.5 Conclusions from PL .............................. 31 4. Resonance Raman of GaAs/AlGaAs Nanowires . 34 4.1 Raman Spectroscopy............................... 34 4.2 Experimental Procedures............................ 39 4.3 Results and Interpretation............................ 44 4.3.1 Summary of Results........................... 44 4.3.2 Incoming vs. Outgoing Resonance................... 47 vi 4.3.3 The Missing TO Mode ......................... 49 4.3.4 Variation of the LO Peak Position................... 51 5. Single Nanowire Raman Spectroscopy .................... 55 5.1 Experimental Rationale............................. 55 5.2 Procedure..................................... 57 5.3 Theoretical Considerations........................... 59 5.4 Results and Discussion ............................. 68 5.5 Conclusions ................................... 71 6. Conclusions, Open estions, and Future Work . 72 6.1 Conclusions ................................... 72 6.2 Open Questions and Future Work ....................... 73 Appendix
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