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Title: Synthesis of the ferroelectric solid solution, Pb(Zr{sub 1-x}Ti{sub x})O{sub 3} on a single substrate using a modified molecular beam epitaxy technique

Abstract

High-throughput synthesis of the ferroelectric solid solution Pb(Zr{sub 1-x}Ti{sub x})O{sub 3} (PZT) on single Pt/Ti/SiO{sub 2}/Si substrates was demonstrated using a modified molecular beam epitaxy (MBE) system. The PZT films exhibited a phase transition from rhombohehdral to tetragonal symmetry as a function of Zr:Ti ratio, across the substrate diagonal. This was consistent with the presence of a morphotropic phase boundary at Zr:Ti ratio of 0.64:0.36, different from the value of 0.53:0.47 observed for bulk ceramics. All points on the films exhibited ferroelectric hysteresis. Results demonstrate the feasibility of high-throughput MBE for deposition of complex ferroelectric oxides, and pave the way for further materials discovery.

Authors:
; ; ; ; ; ; ; ;  [1];  [2];  [2];  [2]
  1. Ilika Technologies Ltd., University of Southampton Science Park, Kenneth Dibben House, Enterprise Road, Chilworth, Southampton, Hampshire SO16 7NS (United Kingdom)
  2. (United Kingdom)
Publication Date:
OSTI Identifier:
20971930
Resource Type:
Journal Article
Resource Relation:
Journal Name: Applied Physics Letters; Journal Volume: 90; Journal Issue: 20; Other Information: DOI: 10.1063/1.2738191; (c) 2007 American Institute of Physics; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; CERAMICS; CRYSTAL GROWTH; DEPOSITION; FERROELECTRIC MATERIALS; HYSTERESIS; LAYERS; MOLECULAR BEAM EPITAXY; OZONE; PHASE TRANSFORMATIONS; PZT; SILICON OXIDES; SOLID SOLUTIONS; SUBSTRATES; SYNTHESIS; THIN FILMS

Citation Formats

Anderson, P. S., Guerin, S., Hayden, B. E., Khan, M. A., Bell, A. J., Han, Y., Pasha, M., Whittle, K. R., Reaney, I. M., School of Chemistry, University of Southampton, Southampton, Hampshire SO17 1BJ, School of Process, Environmental and Materials Engineering, Institute of Materials Research, University of Leeds, Houldsworth Building, Leeds LS2 9JT, and Department of Engineering Materials, University of Sheffield, Sir Robert Hadfield Building, Mappin Street, Sheffield S1 3JD. Synthesis of the ferroelectric solid solution, Pb(Zr{sub 1-x}Ti{sub x})O{sub 3} on a single substrate using a modified molecular beam epitaxy technique. United States: N. p., 2007. Web. doi:10.1063/1.2738191.
Anderson, P. S., Guerin, S., Hayden, B. E., Khan, M. A., Bell, A. J., Han, Y., Pasha, M., Whittle, K. R., Reaney, I. M., School of Chemistry, University of Southampton, Southampton, Hampshire SO17 1BJ, School of Process, Environmental and Materials Engineering, Institute of Materials Research, University of Leeds, Houldsworth Building, Leeds LS2 9JT, & Department of Engineering Materials, University of Sheffield, Sir Robert Hadfield Building, Mappin Street, Sheffield S1 3JD. Synthesis of the ferroelectric solid solution, Pb(Zr{sub 1-x}Ti{sub x})O{sub 3} on a single substrate using a modified molecular beam epitaxy technique. United States. doi:10.1063/1.2738191.
Anderson, P. S., Guerin, S., Hayden, B. E., Khan, M. A., Bell, A. J., Han, Y., Pasha, M., Whittle, K. R., Reaney, I. M., School of Chemistry, University of Southampton, Southampton, Hampshire SO17 1BJ, School of Process, Environmental and Materials Engineering, Institute of Materials Research, University of Leeds, Houldsworth Building, Leeds LS2 9JT, and Department of Engineering Materials, University of Sheffield, Sir Robert Hadfield Building, Mappin Street, Sheffield S1 3JD. Mon . "Synthesis of the ferroelectric solid solution, Pb(Zr{sub 1-x}Ti{sub x})O{sub 3} on a single substrate using a modified molecular beam epitaxy technique". United States. doi:10.1063/1.2738191.
@article{osti_20971930,
title = {Synthesis of the ferroelectric solid solution, Pb(Zr{sub 1-x}Ti{sub x})O{sub 3} on a single substrate using a modified molecular beam epitaxy technique},
author = {Anderson, P. S. and Guerin, S. and Hayden, B. E. and Khan, M. A. and Bell, A. J. and Han, Y. and Pasha, M. and Whittle, K. R. and Reaney, I. M. and School of Chemistry, University of Southampton, Southampton, Hampshire SO17 1BJ and School of Process, Environmental and Materials Engineering, Institute of Materials Research, University of Leeds, Houldsworth Building, Leeds LS2 9JT and Department of Engineering Materials, University of Sheffield, Sir Robert Hadfield Building, Mappin Street, Sheffield S1 3JD},
abstractNote = {High-throughput synthesis of the ferroelectric solid solution Pb(Zr{sub 1-x}Ti{sub x})O{sub 3} (PZT) on single Pt/Ti/SiO{sub 2}/Si substrates was demonstrated using a modified molecular beam epitaxy (MBE) system. The PZT films exhibited a phase transition from rhombohehdral to tetragonal symmetry as a function of Zr:Ti ratio, across the substrate diagonal. This was consistent with the presence of a morphotropic phase boundary at Zr:Ti ratio of 0.64:0.36, different from the value of 0.53:0.47 observed for bulk ceramics. All points on the films exhibited ferroelectric hysteresis. Results demonstrate the feasibility of high-throughput MBE for deposition of complex ferroelectric oxides, and pave the way for further materials discovery.},
doi = {10.1063/1.2738191},
journal = {Applied Physics Letters},
number = 20,
volume = 90,
place = {United States},
year = {Mon May 14 00:00:00 EDT 2007},
month = {Mon May 14 00:00:00 EDT 2007}
}
  • A previously unreported ferroelectric phase has been discovered in a highly homogeneous sample of PbZr{sub 0.52}Ti{sub 0.48}O{sub 3} by high-resolution synchrotron x-ray powder diffraction measurements. At ambient temperature the sample has tetragonal symmetry (a{sub t}=4.037{Angstrom}, c{sub t}=4.138{Angstrom}), and transforms below {approximately}250 K into a phase which, unexpectedly, has monoclinic symmetry (a{sub m}=5.717{Angstrom}, b{sub m}=5.703{Angstrom}, c{sub m}=4.143{Angstrom}, {beta}=90.53{degree}, at 20 K). The intensity data strongly indicate that the polar axis lies in the monoclinic {ital ac} plane close to the pseudocubic [111] direction, which would be an example of the species m3m(12)A2Fm predicted on symmetry grounds by Shuvalov. {copyright} {ital 1999more » American Institute of Physics.}« less
  • A quantitative model is developed to explain the antihysteretic behavior of the electrical resistivity of graphene on a ferroelectric Pb(Zr{sub x}Ti{sub 1-x})O{sub 3} substrate as a function of the gate voltage. The model takes into account the trapping of the electrons from the graphene layer by the states related to the graphene-ferroelectric interface. The finite energy gap of impurity states is also taken into account, which makes it possible to describe the well-known experimental dependences, including an increase and the subsequent saturation of a 'memory window' with the switching gate voltage. The obtained estimates can be important for creating next-generationmore » nonvolatile memory elements, which use the two stable values of electrical resistivity (one of them is attributed to logical '0' and the other, to '1') that result from the antihysteresis effect.« less
  • The solid solution between the normal ferroelectric Pb(Zr{sub 1/2}Ti{sub 1/2})O{sub 3} (PZT) and relaxor ferroelectric Pb(Ni{sub 1/3}Nb{sub 2/3})O{sub 3} (PNN) was synthesized by the columbite method. The phase structure and dielectric properties of xPZT-(1-x)PNN where x=0.4-0.9 and the Zr/Ti composition was fixed close to the morphotropic phase boundary (MPB) were investigated. With these data, the ferroelectric phase diagram between PZT and PNN has been established. The relaxor ferroelectric nature of PNN gradually transformed towards a normal ferroelectric state towards the composition 0.7PZT-0.3PNN, in which the permittivity was characterized by a sharp peak and the disappearance of dispersive behavior. X-ray diffractionmore » analysis demonstrated the coexistence of both the rhombohedral and tetragonal phases at the composition 0.8PZT-0.2PNN, a new morphotropic phase boundary within this system. Examination of the dielectric spectra indicates that PZT-PNN exhibits an extremely high relative permittivity near the MPB composition. The permittivity shows a shoulder at the rhombohedral to tetragonal phase transition temperature T{sub RT}=195 deg. C, and then a maximum permittivity (36 000 at 10 kHz) at the transition temperature T{sub max}=277 deg. C at the MPB composition. The maximum transition temperature of this system was 326 deg. C at the composition x=0.9 with the relative permittivity of 32 000 at 10 kHz.« less
  • Phase transitions and field-induced preferred orientation in (Pb 1-xLa x)(Zr 0.90Ti 0.10) 1–x/ 4O 3 (PLZT x/90/10) ceramics upon electric field cycling using in situ X-ray diffraction were studied. The evolution of the {200} pc and {111} pc diffraction line profiles indicate that PLZT 4/90/10 and PLZT 3/90/10 compositions undergo an antiferroelectric (AFE)–ferroelectric (FE) phase switching. Both PLZT 4/90/10 and PLZT 3/90/10 exhibit irreversible preferred orientation after experiencing the field-induced AFE-to-FE phase switching. An electric field-induced structure develops in both compositions which has a reversible character during the field decreasing in PLZT 4/90/10 and an irreversible character in PLZT 3/90/10.more » In addition, structural analysis of pre-poled PLZT 3/90/10 ceramics show that it is possible to induce consecutive FE-to-AFE and AFE-to-FE transitions when fields of reversed polarity are applied in sequence. The field range required to induce the AFE phase is broad, and the phase transition is kinetically slow. In conclusion, this kind of transition has rarely been reported before.« less
  • Landau-Ginzburg thermodynamic formalism is used for the description of the anomalous ferroelectric, ferromagnetic, and magnetoelectric properties of Pb(Fe{sub 1/2}Ta{sub 1/2}){sub x}(Zr{sub 0.53}Ti{sub 0.47}){sub 1−x}O{sub 3} and Pb(Fe{sub 1/2}Nb{sub 1/2}){sub x}(Zr{sub 0.53}Ti{sub 0.47}){sub 1−x}O{sub 3} micro-ceramics. We calculated temperature, composition, and external field dependences of ferroelectric, ferromagnetic, and antiferromagnetic phases transition temperatures, remanent polarization, magnetization, hysteresis loops, dielectric permittivity, and magnetoelectric coupling. Special attention was paid to the comparison of developed theory with experiments. It appeared possible to describe adequately main experimental results including a reasonable agreement between the shape of calculated and measured hysteresis loops and remnant polarization. Since Landau-Ginzburgmore » thermodynamic formalism appertains to single domain properties of a ferroic, we did not aim to describe quantitatively the coercive field under the presence of realistic poly-domain switching. Information about linear and nonlinear magnetoelectric coupling coefficients was extracted from the experimental data. From the fitting of experimental data with theoretical formula, we obtained the composition dependence of Curie-Weiss constant that is known to be inversely proportional to harmonic (linear) dielectric stiffness, as well as the strong nonlinear dependence of anharmonic parameters in free energy. Keeping in mind the essential influence of these parameters on multiferroic properties, the obtained results open the way to govern practically all the material properties with the help of suitable composition choice. A forecast of the strong enough influence of antiferrodistortive order parameter on the transition temperatures and so on the phase diagrams and properties of multiferroics are made on the basis of the developed theory.« less