Browsing by Author "Ramesh, R."

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A Strain-Driven Morphotropic Phase Boundary in BiFeO(3)
(2009-11-13)
Zeches, R. J.
;
Rossell, M. D.
;
Zhang, J. X.
;
Hatt, A. J.
;
He, Q.
Piezoelectric materials, which convert mechanical to electrical energy and vice versa, are typically characterized by the intimate coexistence of two phases across a morphotropic phase boundary. Electrically switching one to the other yields large electromechanical coupling coefficients. Driven by global environmental concerns, there is currently a strong push to discover practical lead-free piezoelectrics for device engineering. Using a combination of epitaxial growth techniques in conjunction with theoretical approaches, we show the formation of a morphotropic phase boundary through epitaxial constraint in lead-free piezoelectric bismuth ferrite (BiFeO(3)) films. Electric field-dependent studies show that a tetragonal-like phase can be reversibly converted into a rhombohedral-like phase, accompanied by measurable displacements of the surface, making this new lead-free system of interest for probe-based data storage and actuator applications.
A Strain-Driven Morphotropic Phase Boundary in BiFeO3
(2009-11-13)
Zeches, R. J.
;
Rossell, M. D.
;
Zhang, J. X.
;
Hatt, A. J.
;
He, Q.
Piezoelectric materials, which convert mechanical to electrical energy and vice versa, are typically characterized by the intimate coexistence of two phases across a morphotropic phase boundary. Electrically switching one to the other yields large electromechanical coupling coefficients. Driven by global environmental concerns, there is currently a strong push to discover practical lead-free piezoelectrics for device engineering. Using a combination of epitaxial growth techniques in conjunction with theoretical approaches, we show the formation of a morphotropic phase boundary through epitaxial constraint in lead-free piezoelectric bismuth ferrite (BiFeO3) films. Electric field-dependent studies show that a tetragonal-like phase can be reversibly converted into a rhombohedral-like phase, accompanied by measurable displacements of the surface, making this new lead-free system of interest for probe-based data storage and actuator applications.
Above-bandgap voltages from ferroelectric photovoltaic devices
(2010-02-01)
Yang, S. Y.
;
Seidel, J.
;
Byrnes, S. J.
;
Shafer, P.
;
Yang, C. -H.
In conventional solid-state photovoltaics, electron-hole pairs are created by light absorption in a semiconductor and separated by the electric field spaning a micrometre-thick depletion region. The maximum voltage these devices can produce is equal to the semiconductor electronic bandgap. Here, we report the discovery of a fundamentally different mechanism for photovoltaic charge separation, which operates over a distance of 1-2 nm and produces voltages that are significantly higher than the bandgap. The separation happens at previously unobserved nanoscale steps of the electrostatic potential that naturally occur at ferroelectric domain walls in the complex oxide BiFeO(3). Electric-field control over domain structure allows the photovoltaic effect to be reversed in polarity or turned off. This new degree of control, and the high voltages produced, may find application in optoelectronic devices.
Advances in the growth and characterization of magnetic, ferroelectric, and multiferroic oxide thin films
(2010-05-20)
Martin, L. W.
;
Chu, Y-H.
;
Ramesh, R.
;
材料科學與工程學系
;
Department of Materials Science and Engineering
The growth and characterization of functional oxide thin films that are ferroelectric, magnetic, or both at the same time are reviewed. The evolution of synthesis techniques and how advances in in situ characterization have enabled significant acceleration in improvements to these materials are described. Methods for enhancing the properties of functional materials or creating entirely new functionality at interfaces are covered, including strain engineering and layering control at the atomic-layer level. Emerging applications of these functional oxides such as achieving electrical control of ferromagnetism and the future of these complex functional oxides is discussed. (C) 2010 Elsevier B.V. All rights reserved.
Conduction at domain walls in oxide multiferroics
(2009-03-01)
Seidel, J.
;
Martin, L. W.
;
He, Q.
;
Zhan, Q.
;
Chu, Y. -H.
Domain walls may play an important role in future electronic devices, given their small size as well as the fact that their location can be controlled. Here, we report the observation of room-temperature electronic conductivity at ferroelectric domain walls in the insulating multiferroic BiFeO(3). The origin and nature of the observed conductivity are probed using a combination of conductive atomic force microscopy, high-resolution transmission electron microscopy and first-principles density functional computations. Our analyses indicate that the conductivity correlates with structurally driven changes in both the electrostatic potential and the local electronic structure, which shows a decrease in the bandgap at the domain wall. Additionally, we demonstrate the potential for device applications of such conducting nanoscale features.
Correlation between nanoscale and nanosecond resolved ferroelectric domain dynamics and local mechanical compliance
(2011-05-01)
Polomoff, N. A.
;
Rakin, A.
;
Lee, S.
;
Palumbo, V.
;
Yu, P.
The local dynamics of ferroelectric domain polarization are uniquely investigated with sub-20-nm resolved maps of switching times, growth velocities, and growth directions. This is achieved by analyzing movies of hundreds of consecutive high speed piezo force microscopy images, which record domain switching dynamics through repeatedly alternating between high speed domain imaging and the application of 20-nanosecond voltage pulses. Recurrent switching patterns are revealed, and domain wall velocities for nascent domains are uniquely reported to be up to four times faster than for mature domains with radii greater than approximately 100 nm. Switching times, speeds, and directions are also shown to correlate with local mechanical compliance, with domains preferentially nucleating and growing in compliant sample regions while clearly shunting around locations with higher stiffness. This deterministic switching behavior strongly supports a defect-mediated energy landscape which controls polarization reversal, and that can therefore be predicted, modeled, and even manipulated through composition, processing, and geometry. Such results have important implications for the practical performance of ferroelectric devices by enabling guided optimization of switching times and feature densities, while the methods employed provide a new means to investigate and correlate dynamic functionality with mechanical properties at the nanoscale. (C) 2011 American Institute of Physics. [doi:10.1063/1.3581205]
Critical thickness and orbital ordering in ultrathin La(0.7)Sr(0.3)MnO(3) films
(2008-09-01)
Huijben, M.
;
Martin, L. W.
;
Chu, Y. -H.
;
Holcomb, M. B.
;
Yu, P.
Detailed analysis of transport, magnetism, and x-ray absorption spectroscopy measurements on ultrathin La(0.7)Sr(0.3)MnO(3) films with thicknesses from 3 to 70 unit cells resulted in the identification of a lower critical thickness for a nonmetallic nonferromagnetic layer at the interface with the SrTiO(3) (001) substrate of only three unit cells (similar to 12 angstrom). Furthermore, linear-dichroism measurements demonstrate the presence of a preferred (x(2)-y(2)) in-plane orbital ordering for all layer thicknesses without any orbital reconstruction at the interface. A crucial requirement for the accurate study of these ultrathin films is a controlled growth process, offering the coexistence of layer-by-layer growth and bulklike magnetic/transport properties.
Critical thickness and orbital ordering in ultrathin La0.7Sr0.3MnO3 films
(2008-09-01)
Huijben, M.
;
Martin, L. W.
;
Chu, Y. -H.
;
Holcomb, M. B.
;
Yu, P.
Detailed analysis of transport, magnetism, and x-ray absorption spectroscopy measurements on ultrathin La0.7Sr0.3MnO3 films with thicknesses from 3 to 70 unit cells resulted in the identification of a lower critical thickness for a nonmetallic nonferromagnetic layer at the interface with the SrTiO3 (001) substrate of only three unit cells (similar to 12 angstrom). Furthermore, linear-dichroism measurements demonstrate the presence of a preferred (x(2)-y(2)) in-plane orbital ordering for all layer thicknesses without any orbital reconstruction at the interface. A crucial requirement for the accurate study of these ultrathin films is a controlled growth process, offering the coexistence of layer-by-layer growth and bulklike magnetic/transport properties.
Deterministic control of ferroelastic switching in multiferroic materials
(2009-12-01)
Balke, N.
;
Choudhury, S.
;
Jesse, S.
;
Huijben, M.
;
Chu, Y. H.
Multiferroic materials showing coupled electric, magnetic and elastic orderings provide a platform to explore complexity and new paradigms for memory and logic devices. Until now, the deterministic control of non-ferroelectric order parameters in multiferroics has been elusive. Here, we demonstrate deterministic ferroelastic switching in rhombohedral BiFeO(3) by domain nucleation with a scanning probe. We are able to select among final states that have the same electrostatic energy, but differ dramatically in elastic or magnetic order, by applying voltage to the probe while it is in lateral motion. We also demonstrate the controlled creation of a ferrotoroidal order parameter. The ability to control local elastic, magnetic and torroidal order parameters with an electric field will make it possible to probe local strain and magnetic ordering, and engineer various magnetoelectric, domain-wall-based and strain-coupled devices.
Direct spectroscopic evidence of charge reversal at the Pb(Zr(0.2)Ti(0.8))O(3)/La(0.7)Sr(0.3)MnO(3) heterointerface
(2011-01-21)
Wu, Chung-Lin
;
Lee, Pei-Wei
;
Chen, Yi-Chun
;
Chang, Lo-Yueh
;
Chen, Chia-Hao
At the heterointerface of a top ferroelectric Pb(Zr(0.2)Ti(0.8))O(3) (PZT) ultrathin film and a bottom La(0.7)Sr(0.3)MnO(3) (LSMO) electrode, we used continuous synchrotron-radiation photoelectron spectroscopy to probe in situ and demonstrated that the interfacial charges are reversible and their affected valence-band barrier height becomes modulated upon switching the polarization in the top layer. By monitoring the core-level shifting of the buried LSMO layer under continuous illumination of synchrotron radiation, we directly observed a temporal screening of polarization induced by the photon-generated carriers in the top PZT layer. This dynamic characterization of the core-level shifting of the buried layer demonstrates an effective method to probe the electric conduction and ferroelectric polarization of an ultrathin ferroelectric oxide thin film.
Direct spectroscopic evidence of charge reversal at the Pb(Zr0.2Ti0.8)O-3/La0.7Sr0.3MnO3 heterointerface
(2011-01-21)
Wu, Chung-Lin
;
Lee, Pei-Wei
;
Chen, Yi-Chun
;
Chang, Lo-Yueh
;
Chen, Chia-Hao
At the heterointerface of a top ferroelectric Pb(Zr0.2Ti0.8)O-3 (PZT) ultrathin film and a bottom La0.7Sr0.3MnO3 (LSMO) electrode, we used continuous synchrotron-radiation photoelectron spectroscopy to probe in situ and demonstrated that the interfacial charges are reversible and their affected valence-band barrier height becomes modulated upon switching the polarization in the top layer. By monitoring the core-level shifting of the buried LSMO layer under continuous illumination of synchrotron radiation, we directly observed a temporal screening of polarization induced by the photon-generated carriers in the top PZT layer. This dynamic characterization of the core-level shifting of the buried layer demonstrates an effective method to probe the electric conduction and ferroelectric polarization of an ultrathin ferroelectric oxide thin film.
Domain Wall Conductivity in La-Doped BiFeO(3)
(2010-11-05)
Seidel, J.
;
Maksymovych, P.
;
Batra, Y.
;
Katan, A.
;
Yang, S. -Y.
The transport physics of domain wall conductivity in La-doped bismuth ferrite (BiFeO(3)) has been probed using variable temperature conducting atomic force microscopy and piezoresponse force microscopy in samples with arrays of domain walls in the as-grown state. Nanoscale current measurements are investigated as a function of bias and temperature and are shown to be consistent with distinct electronic properties at the domain walls leading to changes in the observed local conductivity. Our observation is well described within a band picture of the observed electronic conduction. Finally, we demonstrate an additional degree of control of the wall conductivity through chemical doping with oxygen vacancies, thus influencing the local conductive state.
Domain Wall Conductivity in La-Doped BiFeO3
(2010-11-05)
Seidel, J.
;
Maksymovych, P.
;
Batra, Y.
;
Katan, A.
;
Yang, S. -Y.
The transport physics of domain wall conductivity in La-doped bismuth ferrite (BiFeO3) has been probed using variable temperature conducting atomic force microscopy and piezoresponse force microscopy in samples with arrays of domain walls in the as-grown state. Nanoscale current measurements are investigated as a function of bias and temperature and are shown to be consistent with distinct electronic properties at the domain walls leading to changes in the observed local conductivity. Our observation is well described within a band picture of the observed electronic conduction. Finally, we demonstrate an additional degree of control of the wall conductivity through chemical doping with oxygen vacancies, thus influencing the local conductive state.
Electric modulation of conduction in multiferroic Ca-doped BiFeO(3) films
(2009-06-01)
Yang, C. -H.
;
Seidel, J.
;
Kim, S. Y.
;
Rossen, P. B.
;
Yu, P.
Many interesting materials phenomena such as the emergence of high-T(c) superconductivity in the cuprates and colossal magnetoresistance in the manganites arise out of a doping-driven competition between energetically similar ground states. Doped multiferroics present a tantalizing evolution of this generic concept of phase competition. Here, we present the observation of an electronic conductor-insulator transition by control of band-filling in the model antiferromagnetic ferroelectric BiFeO(3) through Ca doping. Application of electric field enables us to control and manipulate this electronic transition to the extent that a p-n junction can be created, erased and inverted in this material. A 'dome-like' feature in the doping dependence of the ferroelectric transition is observed around a Ca concentration of similar to 1/8, where a new pseudo-tetragonal phase appears and the electric modulation of conduction is optimized. Possible mechanisms for the observed effects are discussed on the basis of the interplay of ionic and electronic conduction. This observation opens the door to merging magnetoelectrics and magnetoelectronics at room temperature by combining electronic conduction with electric and magnetic degrees of freedom already present in the multiferroic BiFeO(3).
Electric modulation of conduction in multiferroic Ca-doped BiFeO3 films
(2009-06-01)
Yang, C. -H.
;
Seidel, J.
;
Kim, S. Y.
;
Rossen, P. B.
;
Yu, P.
Many interesting materials phenomena such as the emergence of high-T-c superconductivity in the cuprates and colossal magnetoresistance in the manganites arise out of a doping-driven competition between energetically similar ground states. Doped multiferroics present a tantalizing evolution of this generic concept of phase competition. Here, we present the observation of an electronic conductor-insulator transition by control of band-filling in the model antiferromagnetic ferroelectric BiFeO3 through Ca doping. Application of electric field enables us to control and manipulate this electronic transition to the extent that a p-n junction can be created, erased and inverted in this material. A 'dome-like' feature in the doping dependence of the ferroelectric transition is observed around a Ca concentration of similar to 1/8, where a new pseudo-tetragonal phase appears and the electric modulation of conduction is optimized. Possible mechanisms for the observed effects are discussed on the basis of the interplay of ionic and electronic conduction. This observation opens the door to merging magnetoelectrics and magnetoelectronics at room temperature by combining electronic conduction with electric and magnetic degrees of freedom already present in the multiferroic BiFeO3.
Electric-Field-Induced Magnetization Reversal in a Ferromagnet-Multiferroic Heterostructure
(2011-11-14)
Heron, J. T.
;
Trassin, M.
;
Ashraf, K.
;
Gajek, M.
;
He, Q.
A reversal of magnetization requiring only the application of an electric field can lead to low-power spintronic devices by eliminating conventional magnetic switching methods. Here we show a nonvolatile, room temperature magnetization reversal determined by an electric field in a ferromagnet-multiferroic system. The effect is reversible and mediated by an interfacial magnetic coupling dictated by the multiferroic. Such electric-field control of a magnetoelectric device demonstrates an avenue for next-generation, low-energy consumption spintronics.
Electrically controllable spontaneous magnetism in nanoscale mixed phase multiferroics
(2011-03-01)
He, Q.
;
Chu, Y. -H.
;
Heron, J. T.
;
Yang, S. Y.
;
Liang, W. I.
Magnetoelectrics and multiferroics present exciting opportunities for electric-field control of magnetism. However, there are few room-temperature ferromagnetic-ferroelectrics. Among the various types of multiferroics the bismuth ferrite system has received much attention primarily because both the ferroelectric and the antiferromagnetic orders are quite robust at room temperature. Here we demonstrate the emergence of an enhanced spontaneous magnetization in a strain-driven rhombohedral and super-tetragonal mixed phase of BiFeO(3). Using X-ray magnetic circular dichroism-based photoemission electron microscopy coupled with macroscopic magnetic measurements, we find that the spontaneous magnetization of the rhombohedral phase is significantly enhanced above the canted antiferromagnetic moment in the bulk phase, as a consequence of a piezomagnetic coupling to the adjacent tetragonal-like phase and the epitaxial constraint. Reversible electric-field control and manipulation of this magnetic moment at room temperature is also shown.
Electromechanical Coupling among Edge Dislocations, Domain Walls, and Nanodomains in BiFeO3 Revealed by Unit-Cell-Wise Strain and Polarization Maps
(2013-04-01)
Lubk, A.
;
Rossell, M. D.
;
Seidel, J.
;
Chu, Y. H.
;
Ramesh, R.
The performance of ferroelectric devices, for example, the ferroelectric field effect transistor, is reduced by the presence of crystal defects such as edge dislocations. For example, it is well-known that edge dislocations play a crucial role in the formation of ferroelectric dead-layers at interfaces and hence finite size effects in ferroelectric thin films. The detailed lattice structure including the relevant electromechanical coupling mechanisms in close vicinity of the edge dislocations is, however, not well-understood, which hampers device optimization. Here, we investigate edge dislocations in ferroelectric BiFeO3 by means of spherical aberration-corrected scanning transmission electron microscopy, a dedicated model-based structure analysis, and phase field simulations. Unit-cell-wise resolved strain and polarization profiles around edge dislocation reveal a wealth of material states including polymorph nanodomains and multiple domain walls characteristically pinned to the dislocation. We locally determine the piezoelectric tensor and identify piezoelectric coupling as the driving force for the observed phenomena, explaining, for example, the orientation of the domain wall with respect to the edge dislocation. Furthermore, an atomic model for the dislocation core is derived.
Emergent phenomena at multiferroic heterointerfaces
(2012-10-28)
Yu, P.
;
Chu, Y. H.
;
Ramesh, R.
;
材料科學與工程學系
;
Department of Materials Science and Engineering
The coupling and reconstruction of electronic degrees of freedom (such as charge, spin and orbital) at a heterointerface can lead to unexpected and exotic states of matter. In this study, using model systems consisting of multiferroic BiFeO3 and ferromagnetic La0.7Sr0.3MnO3, we review the current understanding of a novel interfacial magnetic state formed at the interface, and highlight some possible mechanisms responsible for this interesting phenomenon and identify open questions for future studies.
Evidence of Sharp and Diffuse Domain Walls in BiFeO3 by Means of Unit-Cell-Wise Strain and Polarization Maps Obtained with High Resolution Scanning Transmission Electron Microscopy
(2012-07-25)
Lubk, A.
;
Rossell, M. D.
;
Seidel, J.
;
He, Q.
;
Yang, S. Y.
Domain walls (DWs) substantially influence a large number of applications involving ferroelectric materials due to their limited mobility when shifted during polarization switching. The discovery of greatly enhanced conduction at BiFeO3 DWs has highlighted yet another role of DWs as a local material state with unique properties. However, the lack of precise information on the local atomic structure is still hampering microscopical understanding of DW properties. Here, we examine the atomic structure of BiFeO3 109 degrees DWs with pm precision by a combination of high-angle annular dark-field scanning transmission electron microscopy and a dedicated structural analysis. By measuring simultaneously local polarization and strain, we provide direct experimental proof for the straight DW structure predicted by ab initio calculations as well as the recently proposed theory of diffuse DWs, thus resolving a long-standing discrepancy between experimentally measured and theoretically predicted DW mobilities.