DOE Final Report on Grant DE-FG02-03ER46063 “The Controlled Synthesis of Metastable Oxides Utilizing Epitaxy and Epitaxial Stabilization” August 2003 - February 2007

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DOE Final Report on Grant DE-FG02-03ER46063 “The Controlled Synthesis of Metastable Oxides Utilizing Epitaxy and Epitaxial Stabilization” August 2003 - February 2007 DOE Final Report on Grant DE-FG02-03ER46063 “The Controlled Synthesis of Metastable Oxides Utilizing Epitaxy and Epitaxial Stabilization” August 2003 - February 2007 Principal Investigator: Darrell G. Schlom Period Covered by this Final Report: August 2003 - February 2007 DOE Award Number: DE-FG02-03ER46063 Amount of Unexpended Funds: $0 The research enabled by this DOE grant led to 13 publications in leading refereed journals including Physical Review Letters and Applied Physics Letters as well as feature articles in the Journal of the American Ceramic Society and Physik Journal (the German equivalent of Physics Today distributed to all members of the German Physical Society) on the controlled synthesis of metastable oxides utilizing epitaxy and epitaxial stabilization. In total our results fill over 100 pages of archived journals and are attached. Much of our work has been performed in collaboration with other DOE researchers. Specifically, we have active collaborations with (please see publications on the next page) with the following DOE groups. DOE COLLABORATORS ON THE WORK SUPPORTED BY THIS DOE GRANT DOE Laboratory Collaborators Argonne National Laboratory Stephen K. Streiffer, Mark A. Zurbuchen, and Dillon D. Fong Pacific Northwest National Laboratory Scott A. Chambers Los Alamos National Laboratory Marilyn E. Hawley PERSONNEL SUPPORTED BY THIS DOE GRANT Name Position Darrell G. Schlom Principal Investigator Wei Tian Postdoctoral Researcher PUBLICATIONS AND PRESENTATIONS The support from this DOE program has led to the publications listed below and attached to the end of this document. Publications 1. M.A. Zurbuchen, Y. Jia, S. Knapp, A.H. Carim, D.G. Schlom, and X.Q. Pan, “Defect Generation by Preferred Nucleation in Epitaxial Sr2RuO4 / LaAlO3,” Applied Physics Letters 83 (2003) 3891-3893. 1 2. A.V. Pogrebnyakov, J.M. Redwing, S. Raghavan, V. Vaithyanathan, D.G. Schlom, S.Y. Xu, Q. Li, D.A. Tenne, A. Soukiassian, X.X. Xi, M.D. Johannes, D. Kasinathan, W.E. Pickett, J.S. Wu, and J.C.H. Spence, “Enhancement of Superconducting Transition Temperature of MgB2 by a Strain-Induced Bond-Stretching Mode Softening,” Physical Review Letters 93 (2004) 147006-1 - 147006-4. 3. A.V. Pogrebnyakov, X.X. Xi, J.M. Redwing, V. Vaithyanathan, D.G. Schlom, A. Soukiassian, S.B. Mi, C.L. Jia, J.E. Giencke, C.B. Eom, J. Chen, Y.F. Hu, Y. Cui, and Q. Li, “Properties of MgB2 Thin Films with Carbon Doping,” Applied Physics Letters 85 (2004) 2017-2019. 4. D.A. Tenne, X.X. Xi, Y.L. Li, L.Q. Chen, A. Soukiassian, M.H. Zhu, A.R. James, J. Lettieri, D.G. Schlom, W. Tian, and X.Q. Pan, “Absence of Low-Temperature Phase Transitions in Epitaxial BaTiO3 Thin Films,” Physical Review B 69 (2004) 174101-1 - 174101-5. 5. X.X. Xi, A.V. Pogrebnyakov, X.H. Zeng, J.M. Redwing, S.Y. Xu, Q. Li, Z.K. Liu, J. Lettieri, V. Vaithyanathan, D.G. Schlom, H.M. Christen, H.Y. Zhai, and A. Goyal, “Progress in the Deposition of MgB2 Thin Films,” Superconductor Science and Technology 17 (2004) S196-S201 and in: Applied Superconductivity 2003: Proceedings of the Sixth European Conference on Applied Superconductivity, IOP Vol. 181 (Institute of Physics, Bristol, 2004), pp. 37-44. 6. J. Mannhart and D.G. Schlom, “Oxide—Tausendsassa für die Elektronik,” Physik Journal 4 (2005) 45-51. 7. A. Venimadhav, A. Soukiassian, D.A. Tenne, Q. Li, X.X. Xi, D.G. Schlom, R. Arroyave, Z.K. Liu, H.P. Sun, X.Q. Pan, M.Y. Lee, and N.P. Ong, “Structural and Transport Properties of Epitaxial NaxCoO2 Thin Films,” Applied Physics Letters 87 (2005) 172104-1 – 172104-3. 8. P. Orgiani, Y. Cui, A.V. Pogrebnyakov, J.M. Redwing, V. Vaithyanathan, D.G. Schlom, and X.X. Xi, “Investigations of MgB2 / MgO and MgB2 / AlN Heterostructures for Josephson Devices,” IEEE Transactions on Applied Superconductivity 15 (2005) 228-231. 9. B.T. Liu, X.X. Xi, V. Vaithyanathan, and D.G. Schlom, “MgB2 Thin Films Grown at Different Temperatures by Hybrid Physical-Chemical Vapor Deposition,” IEEE Transactions on Applied Superconductivity 15 (2005) 3249-3252. 10. M.A. Zurbuchen, J. Lettieri, Y. Jia, A.H. Carim, S.K. Streiffer, and D.G. Schlom, “Out-of-phase Boundary (OPB) Nucleation in Layered Oxides,” in: Ferroelectric Thin Films XIII edited by R. Ramesh, J.-P. Maria, M. Alexe, and V. Joshi, Vol. 902E (Materials Research Society, Warrendale, 2006), pp. T10-55.1 – T10-55.6. 11. W. Tian, J.H. Haeni, D.G. Schlom, E. Hutchinson, B.L. Sheu, M.M. Rosario, P. Schiffer, Y. Liu, M.A. Zurbuchen, and X.Q. Pan, “Epitaxial Growth and Magnetic Properties of the First Five Members of the Layered Srn+1RunO3n+1 Oxide Series,” Applied Physics Letters 90 (2007) 022507- 1 – 022507-3. 12. M.A. Zurbuchen, W. Tian, X.Q. Pan, D. Fong, S.K. Streiffer, M.E. Hawley, J. Lettieri, Y. Jia, G. Asayama, S.J. Fulk, D.J. Comstock, S. Knapp, A.H. Carim, and D.G. Schlom, “Morphology, Structure, and Nucleation of Out-of-Phase Boundaries (OPBs) in Epitaxial Films of Layered Oxides,” Journal of Materials Research 22 (2007) 1439-1471. 13. M.A. Zurbuchen, R.S. Freitas, M.J. Wilson, P. Schiffer, M. Roeckerath, J. Schubert, M.D. Biegalski, G.H. Mehta, D.J. Comstock, J.H. Lee, Y. Jia, and D.G. Schlom, “Synthesis and Characterization of an n = 6 Aurivillius Phase Incorporating Magnetically Active Manganese, Bi7(Mn,Ti)6O21,” Applied Physics Letters 91 (2007) 033113-1 – 033113-3. 14. D.G. Schlom, L.Q. Chen, X.Q. Pan, A. Schmehl, and M.A. Zurbuchen, “A Thin Film Approach to Engineering Functionality into Oxides,” Journal of the American Ceramic Society 91 (2008) 2429-2454. (Feature Article with Journal Cover) 2 APPLIED PHYSICS LETTERS VOLUME 83, NUMBER 19 10 NOVEMBER 2003 Õ Defect generation by preferred nucleation in epitaxial Sr2RuO4 LaAlO3 Mark A. Zurbuchen,a) Yunfa Jia, Stacy Knapp, Altaf H. Carim,b) and Darrell G. Schlom Department of Materials Science and Engineering, The Pennsylvania State University, University Park, Pennsylvania 16803-6602 X. Q. Pan Department of Materials Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109-2136 ͑Received 27 May 2003; accepted 12 September 2003͒ ͑ ͒ The atomic structure of the film–substrate interface of a 001 Sr2RuO4/(100)c LaAlO3 film, determined by high-resolution transmission electron microscopy and simulation, is reported. The structure of superconductivity-quenching ⌬cϷ0.25 nm out-of-phase boundaries ͑OPBs͒ in the film is also reported. Growth in one region on the La-terminated surface is observed to nucleate with a SrO layer. Because two structurally equivalent SrO layers exist within the unit cell, two neighboring nuclei with differing growth order (SrO-RuO2-SrO or RuO2-SrO-SrO) will nucleate an OPB where their misaligned growth fronts meet. Strategies to avoid OPB generation by this mechanism are suggested, which it is hoped may ultimately lead to superconducting Sr2RuO4 films. © 2003 American Institute of Physics. ͓DOI: 10.1063/1.1624631͔ Sr2RuO4 is the only known copper-free layered perov- In the heteroepitaxial growth of layered structures, sub- skite superconductor,1 and is believed to have an unconven- strate surface quality has a great effect on final film quality.14 tional spin-triplet (p-wave͒ symmetry of the superconduct- Advances in substrate engineering have enabled the prepara- 2 14,15 ing order parameter. Electrical transport studies of Sr2RuO4 tion of substrates with known atomic terminations. Some are expected to further the understanding of the super- disagreement currently exists regarding the atomic termina- 3 ͑ ͒ 16–19 conducting state. Sr2RuO4 is well lattice-matched to tion of 001 LaAlO3 . YBa2Cu3O7Ϫ␦ and other cuprate superconductors. Epitaxial It would be useful experimentally to determine which heterostructures would be useful for probing the interaction atomic layers are energetically preferred for the nucleation of between d-wave and p-wave superconductors. Although the Sr2RuO4 on a given substrate, so that high-quality films can 4,5 ͓ epitaxial growth of Sr2RuO4 films and epitaxial be grown by sequential deposition techniques e.g., 6 ͑ ͔͒ YBa2Cu3O7Ϫ␦ /Sr2RuO4 heterostructures have been dem- molecular-beam epitaxy MBE . Few studies of the pre- onstrated, no superconducting Sr2RuO4 films have been ferred nucleation layer of epitaxial thin films of complex reported.4,5 As we show in this letter, greater attention to oxides on substrates with known termination have been nucleation and growth is important to reducing defects and to reported.20–22 Understanding defect nucleation mechanisms possibly achieving superconductivity in Sr2RuO4 films. and microstructural development in the growth of complex Both impurities and crystallographic defects can quench oxide films will allow greater control over their growth. Sub- superconductivity in Sr2RuO4 . As little as 300 ppm of alu- strate surface features have been demonstrated to result in minum is sufficient to destroy superconductivity.7 Crystallo- micron-scale crystallographic defects in some similarly graphic defects that quench superconductivity include out- structured layered perovskites (nϭ2 Aurivillius phases͒.23,24 of-phase boundaries ͑OPBs͒.8 These are translation In this letter, the structure of the film–substrate interface of ͑ ͒ 16 boundaries consisting of a fractional misalignment in the an epitaxial 001 Sr2RuO4 /(001)c LaAlO3 film is re- long axis (c-axis͒ direction between two neighboring regions ported, and the mechanism whereby the preferred nucleation of the same crystal. Because any interruption of the structure layer can lead to the generation of superconductivity- can act as a pair-breaker, a linear density of OPBs on the quenching OPBs is described. ␰ ␰ ͑ ͒ order of 1/ ab(0), where ab(0) is the superconducting co- (001)c Sr2RuO4 epitaxial films were grown on 001 ͑ ͒ ␰ Ϸ 9 16 ͑ ͒ herence length in the 001 plane, ab(0) 66 nm, renders a LaAlO3 substrates by pulsed-laser deposition PLD at high-purity film nonsuperconducting.9 A correlation between 1000 °C in a radiatively heated sample chamber.
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