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Unlocking the Potential of Half-Metallic Sr2femoo6 Thin Films Through Controlled Stoichiometry and Double Perovskite Ordering

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Unlocking the Potential of Half-Metallic Sr2femoo6 Thin Films Through Controlled Stoichiometry and Double Perovskite Ordering Unlocking the potential of half-metallic Sr2FeMoO6 thin films through controlled stoichiometry and double perovskite ordering DISSERTATION Presented in Partial Fulfillment of the Requirements for the Degree Doctor of Philosophy in the Graduate School of The Ohio State University By Adam Joseph Hauser Graduate Program in Physics The Ohio State University 2010 Dissertation Committee: Professor Fengyuan Yang, Advisor Professor Leonard J. Brillson Professor Nandini Trivedi Professor Klaus Honscheid Copyright by Adam Joseph Hauser 2010 Abstract Sr2FeMoO6 is the most studied half-metallic double perovskite with the potential for room-temperature magnetoelectronic applications due to its Curie temperature above 400 K. Despite its promise, researchers have not yet succeeded in growing films of sufficient quality to realize its potential. By identifying and controlling critical factors that complicate attempts to grow thin films of Sr2FeMoO6, we have overcome the obstacles of non-stoichiometry, impurity phase formation and poor double perovskite ordering, all of which must be overcome to achieve half-metallicity. This dissertation reports an in-depth investigation that addresses several critical issues about the deposition of Sr2FeMoO6 epitaxial films using off-axis ultrahigh vacuum sputtering. High quality Sr2FeMoO6 films have been grown by off-axis ultrahigh vacuum DC magnetron sputtering, and characterized by a wide variety of techniques. We have discovered that sputtering gas pressure plays a dominant role in the stoichiometry and phase formation of Sr2FeMoO6 films. Film stoichiometry was found via Rutherford backscattering spectroscopy (RBS) and electron dispersive x-ray (EDX) spectroscopy to be both position dependent and pressure dependent in off-axis magnetron sputtering, changing from a Mo:Fe ratio of 1.43:1 at PTot = 70 mTorr to 1.12:1 at PTot = 6.7 mTorr. Our Sr2FeMoO6 films exhibit a combination of desired properties expected for its half-metallicity. X-ray-diffractometry (XRD) shows the films to be epitaxial, pure-phase, and well ordered by Reitveld refinement (ξ = 85.4%). High angle annular dark field ii scanning transmission microscopy (HAADF STEM) was performed to give the first direct observation of double perovskite ordering in a film, as well as a low defect level. Magnetic characterization was done via vibrating sample magnetometry (VSM) and superconducting quantum interference device (SQUID) magnetometry to find a saturation magnetization of 2.6 µB per formula unit at T = 5 K and a Curie temperature TC of 380 K, roughly in line with expectation for the film stoichiometry and ordering level. This dissertation also reports the first known report of distinct magnetic shape anisotropy, suggesting a high quality film with long-range magnetic ordering. The Sr2FeMoO6 films with these attributes will provide the material base for magnetoelectronic applications that will eventually achieve its half-metallic potential. iii Dedication This dissertation is dedicated to my parents, Mr. Glenn W. Hauser and Mrs. Elizabeth S. Hauser. Thank you for keeping me from being too much of an idiot. I love you both. iv Acknowledgments First and foremost, I would like to thank my advisor Professor Fengyuan Yang, who for some reason saw it fit to take in and mold a second-rate graduate student into something resembling a real physicist. Thank you for everything. To my parents, Mr. Glenn W. Hauser and Mrs. Elizabeth S. Hauser, for keeping me in line and providing a constant source of support and warmth to carry me through tough stretches. To my little sisters Ms. Erica J. Hauser and Ms. Samantha S. Hauser, thank you for tolerating my nonsense. To the Myers Clan (in no particular order, before the “favorite aunt” argument even starts): my godmother Ms. Patricia Myers, my aunts Mrs. Jeanne Kolakowski, Mrs. Theresa Puretz, Mrs. Rose Marie O’Hara, and my uncles Mr. Joe Kolakowski, Mr. Jeffrey S. Puretz, and Mr. Mike O’Hara. And of course, to my cousins Jacqueline and Matthew Puretz, Sean and Scott O’Hara, and my Goddaughter Claire Kolakowski. Thank you all. I would like to also thank my advisory committee, Dr. Leonard J. Brillson, Dr. Klaus Honscheid, and Dr. Nandini Trivedi, for their help and guidance over the past few years, as well as sitting through the painful ignorance displayed in both my candidacy and final oral examination. The financial support for the work in this dissertation came from the Center for Emergent Materials at The Ohio State University, an NSF MRSEC (Award No. DMR- v 0820414). Between the access to amazing interdisciplinary faculty and facilities and the unwavering support for formerly unreachable research avenues, the impact of the CEM on my graduate education cannot be understated. A special thank you to the CEM Program Director, Ms. Lisa Jones, who deals with much of our nonsense on a daily basis and cannot be thanked enough by us. Through the Center and other collaborations, the number of faculty I must thank are truly numerous. With apologies to anyone I may have missed, thank you all for tolerating my insolence over the last six years: Prof. Tom R. Lemberger, Prof. Leonard J. Brillson, Prof. Ratnasingham Sooryakumar, Prof. Patrick M. Woodward, Prof. P. Chris Hammel, Prof. Terry L. Gustafson, Prof. Nandini Trivedi, Prof. Mohit Randeria, Prof. Hamish L. Fraser, Prof. Ezekiel Johnston- Halperin, Prof. D.D. Sarma, Prof. Patricia A. Morris, Prof. Wolfgang Windl, and Prof. David G. Stroud, Prof. Nitin P. Padture, and Prof. Jonathan P. Pelz. I am truly fortunate to have been able to gain the varied experiences I have through all of you, and I find myself in each or your debts. Of course, the rabblerousing group of miscreants I call friends must be acknowledged. Thank you all for making my life so rich and fun. In rough temporal order, though the list is sure to be incomplete: Robert Tilley, Jason Stambaugh, Umair Suri, Jaime Lopez, John Reading, Stephen Gelb, Greg Montalbano, Scott Boyd, Jeff Schadt, Xianwei Xiao, William Schneider, Kevin Knobbe, Nicholas Harmon, Rakesh Tiwari, John Kerry Morrison, Rob Guidry, Mark Murphy, Sarah Parks, Jeffrey Stevens, Gregory Vieira, Gregory Sollenberger, Steven Avery, Christopher Porter, Kevin Driver, Grayson Williams, Taeyoung Choi, George B. Dundee, Michael Fellinger, Jeremy Lucy, vi Michael Hinton, Charles Ruggiero, Lei Fang, Brian Peters, Jie Yong, Turhan Carroll, James P. Mathis, Rebecca Ricciardo, Tricia Meyer, Matt Stolzfus, and the entire gang we call the Columbus Red Devilz baseball team. To everyone I may have missed, know that I truly appreciate you, but I am spilling onto the third page already and do not want to make this any more gratuitous than it already is. Finally, to Ms. Katherine Marie Schmidt, thank you for the love, support, confidence, and encouragement you have given me through everything. You were there for me and I will always be there for you, because we belong together. I am so lucky to be with you every day, and I want to be with you every day until death do us part. Will you marry me? vii Vita 2000................................................................Livingston High School, NJ 2004................................................................B.S. Physics (Honors), Rutgers University 2004................................................................B.S. Astrophysics, Rutgers University 2008................................................................M.S. Physics, The Ohio State University Publications M. Rutkowski, A. J. Hauser, F. Y. Yang, R. Ricciardo, T. Meyer, P. M. Woodward, A Holcombe, P. A. Morris, and L. J. Brillson. X-ray photoemission spectroscopy of Sr2FeMoO6 film stoichiometry and valence state. J. Vac. Sci. Technol. A 28, 1240 (2010) Inhee Lee, Yuri Obukhov, Gang Xiang, Adam Hauser, Fengyuan Yang, Palash Banerjee, Denis V. Pelekhov, and P. Chris Hammel. Nanoscale scanning probe ferromagnetic resonance imaging using localized modes. Nature 466, 845-848 (2010) T. Henighan, A. Chen, G. Vieira, A.J. Hauser, F.Y. Yang, J.J. Chalmers, R. Sooryakumar. Manipulation of Magnetically Labeled and Unlabeled Cells with Mobile Magnetic Traps. Biophysical Journal 98, 412-417 (2010) J. Pak, W. Lin, K. Wang, A. Chinchore, M. Shi, D. C. Ingram, A. R. Smith, K. Sun, J. M. Lucy, A. J. Hauser, and F. Y. Yang. Growth of epitaxial iron nitride ultrathin film on zinc-blende gallium nitride. J. Vac. Sci. Technol. A 28, 536 (2010) G. Vieira, T. Henighan, A. Chen, A.J. Hauser, F.Y. Yang, J.J. Chalmers, and R. Sooryakumar. Magnetic Wire Traps and Programmable Manipulation of Biological Cells. Phys. Rev. Lett. 76, 128101 (2009) Kangkang Wang, Abhijit Chinchore, Wenzhi Lin, David C. Ingram, Arthur R. Smith, Adam J. Hauser, and Fengyuan Yang. Epitaxial growth of ferromagnetic δ-phase manganese gallium on semiconducting scandium nitride (001). Journal of Crystal Growth 311, 2265-2268 (2009) R.A. Ricciardo, A.J. Hauser, F.Y. Yang, H. Kim, W. Lu and P.M. Woodward. Structural, magnetic, and electronic characterization of double perovskites BixLa2-xMnMO6 (M = Ni, Co; x = 0.25, 0.50). Materials Research Bulletin 44, 239-247 (2009) viii A.J. Hauser, J, Zhang, L. Mier, R. Ricciardo, P.M. Woodward, T. L. Gustafson, L.J.Brillson, and F.Y. Yang. Characterization of electronic structure and defect states of thin epitaxial BiFeO3 films by UV-visible absorption and cathodoluminescence spectroscopies. Appl. Phys. Lett. 92, 222901 (2008) W.C. Liu, C.L. Mak, K.H. Wong, C.Y. Lo, S.W. Or, W. Zhou, A. Hauser, F.Y. Yang and R. Sooryakumar. Magnetoelectric and dielectric relaxation
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