skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Size-driven relaxation and polar states in PbMg{sub 1/3}Nb{sub 2/3}O{sub 3}-based system

Abstract

Nanocrystalline powders and ceramics with controlled grain size from 15 to 3000 nm of PbMg{sub 1/3}Nb{sub 2/3}O{sub 3}(PMN) and (PMN){sub 0.65}-(PbTiO{sub 3}){sub 0.35} (PMN-PT35) have been synthesized using the ball milling method. Dielectric experiments have revealed in PMN a disappearance of relaxation below {approx_equal}30 nm grain size and combined x-ray and Raman experiments the vanishing of correlations between polar nanoregions (PNRs). A similar study in morphotropic compound PMN-PT35 has shown the appearance of a relaxor state below {approx_equal}200 nm, associated to a destruction of the ferroelectric domains state towards PNRs in a paraelectric matrix. These phenomena are discussed in connection with pressure experiments from the literature and on the basis of polar states destabilization by both elastic and electric random fields changes associated with the size reduction.

Authors:
; ; ;  [1];  [1];  [2]; ;  [3]
  1. Laboratoire Structures, Proprietes et Modelisation des Solides, Ecole Centrale Paris, Grande Voie des Vignes 92295 Chatenay-Malabry Cedex (France)
  2. (France)
  3. Jozef Stefan Institute, Jamova 39, 1001 Ljubljana (Slovenia)
Publication Date:
OSTI Identifier:
20719781
Resource Type:
Journal Article
Resource Relation:
Journal Name: Physical Review. B, Condensed Matter and Materials Physics; Journal Volume: 72; Journal Issue: 17; Other Information: DOI: 10.1103/PhysRevB.72.174115; (c) 2005 The American Physical Society; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; CERAMICS; CORRELATIONS; CRYSTALS; FERROELECTRIC MATERIALS; GRAIN SIZE; LEAD COMPOUNDS; MILLING; NANOSTRUCTURES; POWDERS; RAMAN SPECTRA; RANDOMNESS; RELAXATION; TITANATES; X RADIATION; X-RAY DIFFRACTION

Citation Formats

Carreaud, J., Gemeiner, P., Dkhil, B., Bogicevic, C., Kiat, J.M., Laboratoire Leon Brillouin, CE Saclay, 91191 Gif-sur-Yvette Cedex, Rojac, T., and Malic, B.. Size-driven relaxation and polar states in PbMg{sub 1/3}Nb{sub 2/3}O{sub 3}-based system. United States: N. p., 2005. Web. doi:10.1103/PhysRevB.72.174115.
Carreaud, J., Gemeiner, P., Dkhil, B., Bogicevic, C., Kiat, J.M., Laboratoire Leon Brillouin, CE Saclay, 91191 Gif-sur-Yvette Cedex, Rojac, T., & Malic, B.. Size-driven relaxation and polar states in PbMg{sub 1/3}Nb{sub 2/3}O{sub 3}-based system. United States. doi:10.1103/PhysRevB.72.174115.
Carreaud, J., Gemeiner, P., Dkhil, B., Bogicevic, C., Kiat, J.M., Laboratoire Leon Brillouin, CE Saclay, 91191 Gif-sur-Yvette Cedex, Rojac, T., and Malic, B.. Tue . "Size-driven relaxation and polar states in PbMg{sub 1/3}Nb{sub 2/3}O{sub 3}-based system". United States. doi:10.1103/PhysRevB.72.174115.
@article{osti_20719781,
title = {Size-driven relaxation and polar states in PbMg{sub 1/3}Nb{sub 2/3}O{sub 3}-based system},
author = {Carreaud, J. and Gemeiner, P. and Dkhil, B. and Bogicevic, C. and Kiat, J.M. and Laboratoire Leon Brillouin, CE Saclay, 91191 Gif-sur-Yvette Cedex and Rojac, T. and Malic, B.},
abstractNote = {Nanocrystalline powders and ceramics with controlled grain size from 15 to 3000 nm of PbMg{sub 1/3}Nb{sub 2/3}O{sub 3}(PMN) and (PMN){sub 0.65}-(PbTiO{sub 3}){sub 0.35} (PMN-PT35) have been synthesized using the ball milling method. Dielectric experiments have revealed in PMN a disappearance of relaxation below {approx_equal}30 nm grain size and combined x-ray and Raman experiments the vanishing of correlations between polar nanoregions (PNRs). A similar study in morphotropic compound PMN-PT35 has shown the appearance of a relaxor state below {approx_equal}200 nm, associated to a destruction of the ferroelectric domains state towards PNRs in a paraelectric matrix. These phenomena are discussed in connection with pressure experiments from the literature and on the basis of polar states destabilization by both elastic and electric random fields changes associated with the size reduction.},
doi = {10.1103/PhysRevB.72.174115},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 17,
volume = 72,
place = {United States},
year = {Tue Nov 01 00:00:00 EST 2005},
month = {Tue Nov 01 00:00:00 EST 2005}
}
  • Photoluminescence for PbMg{sub 1/3}Nb{sub 2/3}O{sub 3} (PMN){endash}PbIn{sub 1/2}Nb{sub 1/2}O{sub 3} (PIN) solid solutions in the temperature ranging from 35 to 295 K have been obtained for the first time. An abrupt photoluminescence enhancement of the system has been observed to occur at {approximately}210 K, which can be attributed to the growing and merging of dynamic polar microregions or to the phase transformation of the material at this temperature. The PIN content has been found to affect the photoluminescence of the PMN-PIN system significantly. The photoluminescence mechanism for PMN-PIN has been studied. {copyright} {ital 1998 Materials Research Society.}
  • The pulsed laser deposition process of 300 nm thick films of Pb(Mg{sub 1/3}Nb{sub 2/3})O{sub 3}){sub 0.67}-(PbTiO{sub 3}){sub 0.33} on (001)-oriented SrTiO{sub 3} was studied by varying deposition pressure, substrate deposition temperature, laser fluence on the target and target-substrate distance. Perovskite phase pure, (001)-oriented, epitaxial smooth films were obtained in a narrow range of deposition parameters. The ferroelectric and dielectric properties of films fabricated within this parameter range still vary significantly. This shows the sensitivity of the system for growth conditions. The best film has a polarization value close to that expected for a (001) poled, stress free single crystal film.more » All films show deposition conditions dependent variations in the self-bias field. The self-bias is very stable during long cycling for films made at optimum deposition conditions. The piezoelectric coefficients of the films are strongly reduced with respect to bulk single crystal values due to the film clamping. The properties variations are ascribed to changes in the grain boundary properties in which film defects are expected to accumulate. Notably slight off-stoichiometry may cause localized screening charges, affecting specifically the polarization and dielectric constant.« less
  • Dielectric permittivities, Brillouin backscattering spectra, polarization-electric field hysteresis loops, and domain structures have been measured as a function of temperature in relaxor-based ferroelectric single crystals (PbMg{sub 1/3}Nb{sub 2/3}O{sub 3}){sub 1{minus}x}(PbTiO{sub 3}){sub x}(PMN-xPT) for x=0.24 and 0.34. For PMN-24%PT, a diffuse phase transition which is associated with a broad frequency-dependent dielectric maximum was observed near 380 K. As the temperature increases, the PMN-24%PT crystal gradually develops cubic regions and is fully converted into the cubic state near 375 K. An extra dielectric anomaly appears at 370 K, possibly due to the percolating polar cluster induced by an external electric field. PMN-34%PTmore » exhibits a nearly normal ferroelectric phase transition near 445 K from the tetragonal to the cubic phase. In addition, a weak diffuse phase transition observed near 280 K may result from partial conversion of rhombohedral phase to tetragonal phase. The dielectric thermal hysteresis confirms that the transitions near 280 and 445 K are diffuse first order and first order, respectively. The dielectric permittivities of PMN-24%PT and PMN-34%PT obey the relation, {var_epsilon}{sub m}{sup {prime}}/{var_epsilon}{sup {prime}}(f,T)=1+[T{minus}T{sub m}(f)]{sup {gamma}}/2{delta}{sub {gamma}}{sup 2}, above the temperature of permittivity maximum T{sub m}. {copyright} 2001 American Institute of Physics.« less
  • Dielectric anomalies observed in heterostructures of the epitaxial thin films of (PbMg{sub 1/3}Nb{sub 2/3}O{sub 3}){sub 0.68}-(PbTiO{sub 3}){sub 0.32}, fabricated by in situ pulsed laser deposition on La{sub 0.5}Sr{sub 0.5}CoO{sub 3}/MgO (100), and with metal top electrodes, were analyzed. The contribution of the film-electrode interfaces to the properties of the heterostructures was evaluated and the true properties of the films were reconstructed. Deviation from Curie-Weiss behavior, temperature evolution of the local order parameter, the Vogel-Fulcher relationship, and temperature evolution of the relaxation time spectrum were found in the films. The relaxor ferroelectric properties of the films were essentially similar to thosemore » of the single crystal. Also, it was shown that an apparent {open_quotes}relaxorlike{close_quotes} behavior in ferroelectric thin film heterostructures, evidenced only by a broad maximum and frequency dispersion of the dielectric permittivity, can be determined by the film-electrode interface rather than by the relaxor properties of the films.« less
  • X-ray and neutron diffraction patterns of lead magnesium niobate (PMN) were recorded between 800 and 5 K. The evolution of the cubic cell parameter and the thermal expansion coefficient was analyzed and structural refinements were carried out by the Rietveld method. In the cubic phase of space group Pm3m the atoms exhibit important shifts from their special positions. A disordered structural model leading to a discrepancy factor R{sub wp} = 7.21% is proposed. The nucleation of polar microregions begins at 600K; it is revealed on the X-ray and neutron diffraction patterns only by some line tails which increase when themore » temperature is lowered. A structural refinement at 5K leads to a R{sub wp} factor of about 11%. Therefore this model has to be improved in order to take into account the existence of polar microregions with very small correlation lengths.« less