Domain Wall Evolution in Phase Transforming Oxides cit y sion Mechanical Stress oe lec tri sm eti ag n ism et ectricity xpan mal E Ther n ag om Magnetoel – One of the fundamental structural features that defines functionality in these materials are domain walls (see figure). – However, very few experiments are currently able to characterize domain wall evolution during real operating conditions of sensors and actuators (e.g., cycling fields of low amplitude). ez Pyr ez oele ctri city Pi • Scientific challenge Magnetization Pi – Sensors and actuators are used in several military functions including surveillance, reconnaissance, navigation, etc. – Phase-transforming oxides, including ferroelectric materials, exhibit unique potential for multi- Temperature Change functionality (see figure). Py rom • Motivation Jacob L. Jones, University of Florida Electric Field Ps Ps Domain Wall Evolution in Phase Transforming Oxides • Objectives 1. to enhance the basic understanding which underlies the linkage between domain architectures and macroscopic properties (structure-property relationships) in bulk, phasetransforming oxides, 2. to explore new methods to control domain structures, and 3. to identify unique domain configurations with previously unrealizable properties. Jacob L. Jones, University of Florida Macroscopic property (e.g., e-field-induced strain) grain boundary domain domain wall motion piezoelectric effect V Domain Wall Evolution in Phase Transforming Oxides • Approach Jacob L. Jones, University of Florida – Utilize advanced, real-time characterization techniques including in situ X-ray and neutron diffraction during thermal, electrical, mechanical, and/or magnetic field application. – These unique in situ measurements of domain wall behavior then provide insights into materials development for enhanced functionality. – Prior state-of-the-art involved application of static electric fields at high electric field amplitudes. – Our approach involves studying domain wall motion during dynamic loading and at operation-relevant field amplitudes (often below the coercive field). d33(pm/V) (a) 600 Domain Wall Evolution in Phase Transforming Oxides Lattice strain 400 200 • Scientific Accomplishments Strain from L. Jones, Jacob 90domain wall motion Strain from 90do wall motion Cumulative strain 90 domain wall m and electric-field lattice strain University of Florida Cumulative contributions Cumulative contributions Fractional nonlinear (pm/V) to d33 (pm/V) to d33d33 (pm/V) contribution Apparent piezoele 800 coefficient (a) – Time-resolved observation of800 domain variants {002}/{200} of Strain from 90do (b) tetragonal Pb(Zr,Ti)O3 ceramics of wall motion 600 demonstrate the motion ion t u b i r from latticestrain Cumulative 600 walls duringarapplication cont ferroelectric/ferroelastic domain of weak e Lattice strain n li strain 90 domain wall m Non 400 n and electric-fieldutio electric field amplitudes. ontrib c 400 r a e lattice strain Lin – Quantitative analysis of diffraction data leads to a complete account 200 Strain from ntribution o c r a e from 90 domain n li on 200 90Ndomain wall motion 33 motion wall Linear contribution Relative Contributions: 800 (b) Respective nonlin (c) 0.4 contributions calc ution b i r t from lattice n o 600 c from (a) and (b) r linea strain 0.3 Non tion ibustrain Lattice r t n o c 400 Linear 0.2 ntribution o c r a e from 90 domain n li Non 200 -E 3.87 0.1 Strain from 90 0.0 wall motion +E 3.97 2 Linear contribution -E 0.5 de domain wall motion nds gre 1.0 e co es) 4.07 s 0.0 , e Respective nonlin Tim 200 400 600 800 (c) 0.4 Electric Field Amplitude (V/mm) contributions calc from (a) and (b) Measurement performed at the European Synchrotron Radiation Facility 0.3 linear on Diffracted Intensity of the contributions to the ceramic piezoelectric coefficient, d . d33(pm/V) (a) 600 Domain Wall Evolution in Phase Transforming Oxides Lattice strain 400 200 • Scientific Accomplishments intergranular coupling. – composition is mostly Cumulative contributions Cumulative contributions Fractional nonlinear (pm/V) to d33 (pm/V) to d33d33 (pm/V) contribution – University of Florida Apparent piezoele 800 coefficient (a) The linear component of the 800 e-field-induced lattice strains is the Strain from 90do (b) wall motion only component which may be 600 intrinsic piezoelectricity ion (since t u b i tr from latticestrain Cumulative 600 r con a intrinsic PE is field-independent). e Lattice strain n li strain 90 domain wall m Non 400 n and electric-fieldutio Closer inspection of lattice strain ontrib indicate this is not c 400 measurements r a e lattice strain Lin likely the intrinsic piezoelectric but orather an elastic 200 coefficient, Strain from ntribution c r a e from 90 domain n li on 200 90Ndomain wall motion wall motion Linear contribution Remarkably, the Relative Contributions: 800 (b) Respective nonlin piezoelectric d33 (c) 0.4 contributions calc ution b i r t from lattice n o 600 c from (a) and (b) coefficient in this r linea strain 0.3 Non common soft PZT tion ibustrain Lattice r t n o c 400 Linear 0.2 ntribution o c r a e from 90 domain n li attributed to domain Non 200 0.1 Strain from 90 wall motion Linear contribution wall motion, not the domain wall motion 0.0 intrinsic piezoelectric Respective nonlin 200 400 600 800 (c) 0.4 Electric Field Amplitude (V/mm) contributions calc effect of the lattice. from (a) and (b) In review 0.3 as a Feature Article for J. American Ceramic Society linear on – Strain from L. Jones, Jacob 90domain wall motion Strain from 90do wall motion Cumulative strain 90 domain wall m and electric-field lattice strain Domain Wall Evolution in Phase Transforming Oxides • Scientific Accomplishments Jacob L. Jones, University of Florida – Synthesis, high-resolution structural measurement, and refinement of (1-x)Na0.5Bi0.5TiO3-xBaTiO3 (BNT-xBT) piezoelectric ceramics. – Crystallographic refinement of the NBT indicates a monoclinic Cc space group, not widely-assumed R3c. – Implies complex ferroelectric/ferroelastic domain structure in BNTbased materials. May explain nanodomains and relaxor-like behavior. – Also suggests “monoclinic” not a sufficient condition for high d33. High-resolution X-ray measurements at the Advanced Photon Source, Argonne National Laboratory Domain Wall Evolution in Phase Transforming Oxides • Scientific Accomplishments Jacob L. Jones, University of Florida d33 (pm/V) – Acceptor-doping in Na0.5Bi0.5TiO3(BNT)-based ceramics show unexpected behavior of thermal stability. Enhanced thermal stability – Piezoelectric coefficient 140 d33 as a function of Undoped 0.5 mol% Fe O 120 temperature shows 1.0 mol% Fe O increased thermal stability 1.5 mol% Fe O 100 2.0 mol% Fe O for small (<1%) Fe2O3 80 doping concentration. – Because of negligible 60 lowering of initial 40 (room temperature) d33, this material has a high 20 piezoelectric coefficient at 0 elevated temperatures. 0 50 100 150 200 250 300 350 Temperature (degrees C) 2 3 2 3 2 3 2 3 Domain Wall Evolution in Phase Transforming Oxides • Transitions Jacob L. Jones, University of Florida – The PI gave several seminars at national laboratories including: • User Science Seminar, Advanced Photon Source, Argonne National Laboratory, July 30, 2010. • Lujan Neutron Scattering Center, Los Alamos National Laboratory, July 27, 2010. – The PI participated and delivered an invited talk at a symposium organized by ARL PI Jones and PhD student personnel from the Aberdeen Proving Ground Elena Aksel at Los Alamos National Laboratory (XIX International Materials Research Congress, Cancun, Mexico, August 15-19, 2010.) – The PI hosted Dr. Melanie Cole from the Army Research Laboratory, Aberdeen Proving Ground, on Sept 12, 2008. She met with several faculty members and the PI and gave a departmental research seminar titled, “Compositionally Tailored Material Properties To Enable Performance Enhanced Tunable Microwave Devices.” Domain Wall Evolution in Phase Transforming Oxides • PI Awards Jacob L. Jones, University of Florida – Presidential Early Career Award for Scientists and Engineers (PECASE), Awarded January 13, 2010. – Defense Program Awards of Excellence, nominated through the Los Alamos National Laboratory and presented by Donald Cook (Deputy Administrator for Defense Programs, NNSA), August 30, 2010, “for discovering important new physics in ferroelectric ceramics used in neutron generators through clever neutron scattering experiments.” – Faculty Excellence Award, April 22, 2010. Department of Materials Science and Engineering, University of Florida. – Excellence Award for Assistant Professors, April 27, 2010, one of 10 recipients at the University of Florida. – 11 invited talks acknowledging ARO support at international conferences, national laboratories, and universities. Domain Wall Evolution in Phase Transforming Oxides Jacob L. Jones, University of Florida • Future Research Plans PLZT Longitudinal Strain in Response to Instantaniously Applied E-Fields Normalized Longitudinal Strain – Recent time-dependent pulse poling measurements discriminate between 180° and non-180° domain wall motion (see figure). – Use of pulsed electric fields of various durations during the electrical poling process will coerce domains into unique configurations. – This time-dependent experiment builds upon our existing electromechanical poling studies. 1 2.0 kV/mm 1.9 kV/mm 1.8 kV/mm 1.6 kV/mm 1.5 kV/mm 1.4 kV/mm 0.8 0.6 0.4 0.2 0 0 10 2 4 10 10 Time (microseconds) 6 10 180° domain switching occurs first during pulsed fields Non-180° domain switching occurs last after pulsed field application Domain Wall Evolution in Phase Transforming Oxides • Future Research Plans – Analysis of structure and resulting domain structures in BNT-xBT using high-resolution X-ray diffraction. – In situ X-ray and neutron diffraction measurements to understand origin of electromechanical behavior at x=7. – We hypothesize that high piezoelectric d33 at x=7 is not related to the morphotropic phase boundary, but due to domain wall contributions (similar to PZT). – This implies that the design of highd33 ceramics should include domain wall contributions. Jacob L. Jones, University of Florida Peak in permittivity and d33 at x=7 W. Jo, J. L. Jones, et al., in review at J. Applied Physics
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