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Kim, Young-Min,He, Jun,Biegalski, Michael D.,Ambaye, Hailemariam,Lauter, Valeria,Christen, Hans M.,Pantelides, Sokrates T.,Pennycook, Stephen J.,Kalinin, Sergei V.,Borisevich, Albina Y. Nature Publishing Group, a division of Macmillan P 2012 NATURE MATERIALS Vol.11 No.10
Oxygen vacancy distributions and dynamics directly control the operation of solid-oxide fuel cells and are intrinsically coupled with magnetic, electronic and transport properties of oxides. For understanding the atomistic mechanisms involved during operation of the cell it is highly desirable to know the distribution of vacancies on the unit-cell scale. Here, we develop an approach for direct mapping of oxygen vacancy concentrations based on local lattice parameter measurements by scanning transmission electron microscopy. The concept of chemical expansivity is demonstrated to be applicable on the subunit-cell level: local stoichiometry variations produce local lattice expansion that can be quantified. This approach was successfully applied to lanthanum strontium cobaltite thin films epitaxially grown on substrates of different symmetry, where polarized neutron reflectometry revealed a strong difference in magnetic properties. The different vacancy content found in the two films suggests the change in oxygen chemical potential as a source of distinct magnetic properties, opening pathways for structural tuning of the vacancy concentrations and their gradients.
Kim, Young-Min,Morozovska, Anna,Eliseev, Eugene,Oxley, Mark P.,Mishra, Rohan,Selbach, Sverre M.,Grande, Tor,Pantelides, S. T.,Kalinin, Sergei V.,Borisevich, Albina Y. Nature Publishing Group, a division of Macmillan P 2014 NATURE MATERIALS Vol.13 No.11
The development of interface-based magnetoelectric devices necessitates an understanding of polarization-mediated electronic phenomena and atomistic polarization screening mechanisms. In this work, the LSMO/BFO interface is studied on a single unit-cell level through a combination of direct order parameter mapping by scanning transmission electron microscopy and electron energy-loss spectroscopy. We demonstrate an unexpected ~5% lattice expansion for regions with negative polarization charge, with a concurrent anomalous decrease of the Mn valence and change in oxygen K-edge intensity. We interpret this behaviour as direct evidence for screening by oxygen vacancies. The vacancies are predominantly accumulated at the second atomic layer of BFO, reflecting the difference of ionic conductivity between the components. This vacancy exclusion from the interface leads to the formation of a tail-to-tail domain wall. At the same time, purely electronic screening is realized for positive polarization charge, with insignificant changes in lattice and electronic properties. These results underline the non-trivial role of electrochemical phenomena in determining the functional properties of oxide interfaces. Furthermore, these behaviours suggest that vacancy dynamics and exclusion play major roles in determining interface functionality in oxide multilayers, providing clear implications for novel functionalities in potential electronic devices.
Jang, Jae Hyuck,Kim, Young-Min,He, Qian,Mishra, Rohan,Qiao, Liang,Biegalski, Michael D.,Lupini, Andrew R.,Pantelides, Sokrates T.,Pennycook, Stephen J.,Kalinin, Sergei V.,Borisevich, Albina Y. American Chemical Society 2017 ACS NANO Vol.11 No.7
<P>Vacancy dynamics and ordering underpin the electrochemical functionality of complex oxides and strongly couple to their physical properties. In the field of the epitaxial thin films, where connection between chemistry and film properties can be most clearly revealed, the effects related to oxygen vacancies are attracting increasing attention. In this article, we report a direct, real-time, atomic level observation of the formation of oxygen vacancies in the epitaxial LaCoO3 thin films and heterostructures under the influence of the electron beam utilizing scanning transmission electron microscopy (STEM). In the case of LaCoO3/SrTiO3 superlattice, the formation of the oxygen vacancies is shown to produce quantifiable changes in the interatomic distances, as well as qualitative changes in the symmetry of the Co sites manifested as off-center displacements. The onset of these changes was observed in both the [100](pc) and [110](pc) orientations in real time. Additionally, annular bright field images directly show the formation of oxygen vacancy channels along [110](pc) direction. In the case of 15 u.c. LaCoO3 thin film, we observe the sequence of events during beam-induced formation of oxygen vacancy ordered phases and find them consistent with similar processes in the bulk. Moreover, we record the dynamics of the nucleation, growth, and defect interaction at the atomic scale as these transformations happen. These results demonstrate that we can track dynamic oxygen vacancy behavior with STEM, generating atomic-level quantitative information on phase transformation and oxygen diffusion.</P>
Mishra, Rohan,Kim, Young-Min,He, Qian,Huang, Xing,Kim, Seong Keun,Susner, Michael A.,Bhattacharya, Anand,Fong, Dillon D.,Pantelides, Sokrates T.,Borisevich, Albina Y. American Physical Society 2016 Physical Review B Vol.94 No.4
<P>The surfaces of transition-metal oxides with the perovskite structure are fertile grounds for the discovery of novel electronic and magnetic phenomena. In this article, we combine scanning transmission electron microscopy (STEM) with density functional theory (DFT) calculations to obtain the electronic and magnetic properties of the (001) surface of a (LaFeO3)(8)/(SrFeO3)(1) superlattice film capped with four layers of LaFeO3. Simultaneously acquired STEM images and electron-energy-loss spectra reveal the surface structure and a reduction in the oxidation state of iron from Fe3+ in the bulk to Fe2+ at the surface, extending over several atomic layers, which signals the presence of oxygen vacancies. The DFT calculations confirm the reduction in terms of oxygen vacancies and further demonstrate the stabilization of an exotic phase in which the surface layer is half metallic and ferromagnetic, while the bulk remains antiferromagnetic and insulating. Based on the calculations, we predict that the surface magnetism and conductivity can be controlled by tuning the partial pressure of oxygen.</P>
Mishra, Rohan,Kim, Young-Min,Salafranca, Juan,Kim, Seong Keun,Chang, Seo Hyoung,Bhattacharya, Anand,Fong, Dillon D.,Pennycook, Stephen J.,Pantelides, Sokrates T.,Borisevich, Albina Y. American Chemical Society 2014 NANO LETTERS Vol.14 No.5
<P>Complex oxides displaying ferroelectric and/or multiferroic behavior are of high fundamental and applied interest. In this work, we show that it is possible to achieve polar order in a superlattice made up of two nonpolar oxides by means of oxygen vacancy ordering. Using scanning transmission electron microscopy imaging, we show the polar displacement of magnetic Fe ions in a superlattice of (LaFeO<SUB>3</SUB>)<SUB>2</SUB>/(SrFeO<SUB>3</SUB>) grown on a SrTiO<SUB>3</SUB> substrate. Using density functional theory calculations, we systematically study the effect of epitaxial strain, octahedral rotations, and surface terminations in the superlattice and find them to have a negligible effect on the antipolar displacements of the Fe ions lying in between SrO and LaO layers of the superlattice (i.e., within La<SUB>0.5</SUB>Sr<SUB>0.5</SUB>FeO<SUB>3</SUB> unit cells). The introduction of oxygen vacancies, on the other hand, triggers a polar displacement of the Fe ions. We confirm this important result using electron energy loss spectroscopy, which shows partial oxygen vacancy ordering in the region where polar displacements are observed and an absence of vacancy ordering outside of that area.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/nalefd/2014/nalefd.2014.14.issue-5/nl500601d/production/images/medium/nl-2014-00601d_0006.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/nl500601d'>ACS Electronic Supporting Info</A></P>
Point Defect Configurations of Supersaturated Au Atoms Inside Si Nanowires
Oh, Sang Ho,Benthem, Klaus van,Molina, Sergio I.,Borisevich, Albina Y.,Luo, Weidong,Werner, Peter,Zakharov, Nikolai D.,Kumar, Dhananjay,Pantelides, Sokrates T.,Pennycook, Stephen J. American Chemical Society 2008 NANO LETTERS Vol.8 No.4
Interface control of bulk ferroelectric polarization.
Yu, P,Luo, W,Yi, D,Zhang, J X,Rossell, M D,Yang, C-H,You, L,Singh-Bhalla, G,Yang, S Y,He, Q,Ramasse, Q M,Erni, R,Martin, L W,Chu, Y H,Pantelides, S T,Pennycook, S J,Ramesh, R National Academy of Sciences 2012 PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF Vol.109 No.25
<P>The control of material interfaces at the atomic level has led to novel interfacial properties and functionalities. In particular, the study of polar discontinuities at interfaces between complex oxides lies at the frontier of modern condensed matter research. Here we employ a combination of experimental measurements and theoretical calculations to demonstrate the control of a bulk property, namely ferroelectric polarization, of a heteroepitaxial bilayer by precise atomic-scale interface engineering. More specifically, the control is achieved by exploiting the interfacial valence mismatch to influence the electrostatic potential step across the interface, which manifests itself as the biased-voltage in ferroelectric hysteresis loops and determines the ferroelectric state. A broad study of diverse systems comprising different ferroelectrics and conducting perovskite underlayers extends the generality of this phenomenon.</P>