Dielectric investigations in Sr0.75Ba0.25Nb2O6 relaxor ferroelectric thin films

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Mesoscopic structure evidenced by AC dielectric nonlinearities in Sr(0.75)Ba(0.25)Nb(2)O(6) relaxor ferroelectric thin films

The AC electric field and temperature dependences of the dielectric permittivity for strontium barium niobate (Sr(0.75)Ba(0.25)Nb(2)O(6)) relaxor ferroelectric thin films have been investigated. The results indicate the existence of a true mesoscopic structure evidenced by the nonlinear dielectric response of these films, which is similar to those observed for bulk relaxor ferroelectrics. A tendency for a temperature dependent crossover from a linear to a quadratic behaviour of the dielectric nonlinearity was observed, indicating an evolution from paraelectric to glass-like behaviour on cooling the samples towards the freezing temperature transition.

Investigation of nonlinear dielectric properties in Sr0.75Ba0.25Nb2O6 relaxor ferroelectric thin films

The ac and dc driving fields dependence of the dielectric permittivity for the strontium barium niobate relaxor ferroelectric thin films has been investigated. The nonlinear dielectric properties were obtained by using the measurements of the dielectric permittivity of the material as a function of the ac and dc "bias" electric field amplitude in wide frequency (100 Hz-10 MHz) and temperature (50-450 K) intervals. The results hint the existence of a true mesoscopic dielectric relaxor response in the ferroelectric thin film, which is very similar to those observed in bulk relaxor ferroelectrics. An anomalous behavior of the NL dielectric response was observed when submitted to moderate dc electric fields levels,,indicating a crossover from paraelectric to a glasslike behavior on cooling the sample toward the freezing transition. The obtained results were analyzed within the framework of the models proposed in the current literature.

Local structure and hybridization states in Ba0.9Ca0.1Ti1-xZrxO3 ceramic compounds: Correlation with a normal or relaxor ferroelectric character

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Absence of relaxor-like ferroelectric phase transition in (Pb,Sr)TiO3 thin films

We have performed dielectric and micro-Raman spectroscopy measurements in the 298 - 673 K temperature range in polycrystalline Pb0.50Sr0.50TiO3 thin films prepared by a soft chemical method. The phase transition have been investigated by dielectric measurements at various frequencies during the heating cycle. It was found that the temperature corresponding to the peak value of the dielectric constant is frequency-independent, indicating a non-relaxor ferroelectric behavior. However, the dielectric constant versus temperature curves associated with the ferroelectric to paraelectric phase transition showed a broad maximum peak at around 433 K. The observed behavior is explained in terms of a diffuse phase transition. The obtained Raman spectra indicate the presence of a local symmetry disorder, due to a higher strontium concentration in the host lattice. The monitoring of some modes, conducted in the Pb0.50Sr0.50TiO3 thin films, showed that the ferroelectric tetragonal phase undergoes a transition to the paraelectric cubic phase at around 423 K. However, the Raman activity did not disappear, as would be expected from a transition to the cubic paraelectric phase. The strong Raman spectrum observed for this cubic phase is indicative that a diffuse-type phase transition is taking place. This behavior is attributed to distortions of the perovskite structure, allowing the persistence of low-symmetry phase features in cubic phase high above the transition temperature. This result is in contrast to the forbidden first-order Raman spectrum, which would be expected from a cubic paraelectric phase, such as the one observed at high temperature in pure PbTiO3 perovskite.

In situ X-ray diffraction studies of phase transition in Pb1-x La x Zr0.40Ti0.60O3 ferroelectric ceramics

The temperature dependence of the crystalline structure and the lattice parameters of Pb1-xLaxZr0.40Ti0.60O3 ferroelectric ceramic system with 0.00 x 0.21 was determined. The samples with x 0.11 show a cubic-to-tetragonal phase transition at the maximum dielectric permittivity, Tmax. Above this amount and especially for the x = 0.12 sample, a spontaneous phase transition from a relaxor ferroelectric state (cubic phase) to a ferroelectric state (tetragonal phase) is observed upon cooling below the Tmax. Unlike what has been reported in other studies, the x = 0.13, 0.14, and 0.15 samples, which present a more pronounced relaxor behavior, also presents a spontaneous normal-to-relaxor transition, indicated by a cubic to tetragonal symmetry below the Tmax. The origin of this anomaly has been associated with an increase in the degree of tetragonality, confirmed by the measurements of the X-ray diffraction patterns. The differential thermal analysis (DSC) measurements also confirm the existence of these phase transitions.

Phase-transition studies of Ba(0.90)Ca(0.10)(Ti(1-x)Zr(x))O(3) ferroelectric ceramic compounds

Perovskite-structured Ba(0.90)Ca(0.10)(Ti(1-x)Zr(x))O(3) ceramics were prepared in this work and subsequently studied in terms of composition-dependent dielectric and high-resolution long-range order structural properties from 30 to 450 K. The dielectric response of these materials was measured at several frequencies in the range from 1 kHz to 1 MHz. Combining both techniques, including Rietveld refinement of the X-ray diffraction data, allowed observing that, when increasing Zr(4+) content, the materials change from conventional to diffuse and relaxor ferroelectric compounds, the transition occurring spontaneously at the x = 0.18 composition. Interestingly, this spontaneous transition turned out to be prevented for a further increase of Zr(4+). On the basis of all the dielectric and structural results processed, a phase diagram of this system is presented. (C) 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Effect of strontium addition on ferroelectric phase transition of PZT thin films prepared by chemical route

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Investigation on dielectric response of PMN ceramics around paraelectric-ferroelectric diffuse phase transition

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Dielectric relaxation and relaxor behavior in bilayered perovskites

Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)

Ferroelectric phase transition in Pb0.60Sr0.40TiO3 thin films

Polycrystalline Pb-0.Sr-60(0).40TiO3 thin films with the tetragonal perovskite structure were grown on platinum-coated silicon substrates by a chemical method. Raman results reveal that A1 (1 TO) symmetry modes, also known as soft modes, persist above the phase transition 14 temperature. This is due to the high structural distortion caused by the substitution effect of Sr2+ for Pb2+ ions. In contrast, the E(1TO) symmetry mode vanishes at 498 K, characterizing the ferroelectric-paraelectric transition phase. However, the Raman spectra, as a function of temperature, reveal that the ferroelectric-paraelectric phase transition may be correlated with a diffuse phase transition. The experimental data obtained from measurements of the dielectric constant as a function of temperature and frequencies showed a classical behavior of ferroelectric phase transition in Pb-0.Sr-60(0).40TiO3 thin films, rather than a relaxor ferroelectric phase transition. (C) 2004 Elsevier B.V. All rights reserved.

Dielectric properties of Pb Nb2 O6 ferroelectric ceramics at cryogenic temperatures

Complex dielectric permittivity measurements in Pb Nb2 O6 ceramics were performed in a frequency and temperature range of 1 kHz-1 MHz and from 15 to 900 K, respectively. The results revealed two dielectric anomalies showing typical characteristics of relaxor ferroelectric materials at cryogenic temperatures. Comparison with other tetragonal tungsten bronze (TTB) structure-type materials suggests the existence of successive phase transitions, which until now were not reported. The observed low temperature dielectric behaviors seem to be due to intrinsic physical characteristics related to the TTB structure. © 2007 American Institute of Physics.

Local order of Pb1-xLaxZr0.40Ti 0.60O3 ferroelectric ceramic materials probed by X-ray absorption and Raman spectroscopies

This paper reports on the structural characterization of Pb 1-xLaxZr0.40Ti0.60O3 (PLZT) ferroelectric ceramic compositions prepared by the conventional solid state reaction method. X-ray absorption spectroscopy (XAS) and Raman spectroscopy were used to probe the local structure of PLZT samples that exhibits a normal and relaxor ferroelectric behavior. From the Zr K-edge and Pb LIII-edge EXAFS spectra, a considerable dissymmetry of Zr and Pb sites was observed in all samples, including those showing a long-range order cubic symmetry and a relaxor behavior. The Raman spectroscopy results confirmed the existence of a local disorder in all PLZT samples through the observation of Raman active vibrational modes. The variation in the intensity of the E(TO 3) mode in the PLZT relaxor samples indicates that the process of correlation between nanodomains stabilizes at temperatures lower than T m. © 2013 Elsevier B.V. All rights reserved.

X-ray photoelectron spectroscopy study on sintered Pb1-xLaxTiO3 ferroelectric ceramics

The Pb1-xLaxTiO3 sintered ferroelectric ceramics with x equal to 0, 0.10, 0.15, 0.20, and 0.30 were studied by X-ray photoelectron spectroscopy (XPS). The binding energy of the Ti 2p lines is consistent with only one chemical state, Ti4+. on the other hand, in the case of Pb 4f and 0 Is XPS spectra, apart from the main peaks attributed to the lattice ions, minor peaks related to the surface states were also observed. The presence of Pb-0 state on the surface of all samples was due to the reduction of lead ions caused by the preferential removal of the oxygen ions after sputtering. The non observation of Ti3+ ions confirms that the mechanism of charge compensation that should occurs owing to the substitution of Ph2+ by La3+ is due to the preferential formation of Pb site vacancies, and not to a reduction from Ti4+ to Ti3+ states. Within the limits of the present experiment, there is no evidence of the existence of non-equivalent Pb, Ti, and La sites as the Pb1-xLaxTiO3 ceramic changes from a normal to a relaxor ferroelectric state. (c) 2006 Elsevier B.V. All rights reserved.

Lineare und nichtlineare dielektrische Spektroskopie am Relaxor-Ferroelektrikum Bleimagnesiumniobat

Relaxor-Ferroelektrika sind wegen ihrer möglichen technischen Anwendungen und vom Standpunkt der Grundlagenforschung als Beispiel für ungeordnete Systeme von wissenschaftlichem Interesse. Trotz zahlreicher experimenteller Untersuchungen sind die mikroskopischen Ursachen ihrer Eigenschaften aber nach wie vor ungeklärt. Im Rahmen dieser Arbeit wurde das Relaxor-Ferroelektrikum Bleimagnesiumniobat-Bleititanat (PMN-10PT) mittels linearer und nichtlinearer dielektrischer Spektroskopie untersucht. Durch Anregung mit starken elektrischen Wechselfeldern konnten mit der Methode des nichtresonanten dielektrischen Lochbrennens frequenzselektiv einzelne spektrale Bereiche aus dem verbreiterten Relaxationsspektrum herausgegriffen und deren Rückrelaxation separat verfolgt werden. Die experimentellen Ergebnisse zeigten, daß eine langlebige dynamische Heterogenität der dipolaren Reorientierung existiert. Durch ihr ausgeprägt nichtergodisches Verhalten zeigen Relaxor-Ferroelektrika starke Alterungseffekte. Die Untersuchung des Alterungsverhaltens der dielektrischen Suszeptibilität zeigte, daß ein Gedächtnis für die bei einer Alterungstemperatur eingenommene Konfiguration bestehen bleibt, sofern die Temperatur nach einer unvollständigen isothermen Alterung nur um einige Grad abgesenkt oder erhöht wurde.Außerdem wurde die induzierte Polarisation bei stochastischen dielektrischen Anregungen mit elektrischen Feldern, die in sehr guter Näherung ein weißes Rauschen darstellten, untersucht. Über die Bildung der Kreuzkorrelationsfunktion zwischen Feld und Polarisation konnte die Impulsantwortfunktion des Systems berechnet werden.Die experimentellen Ergebnisse am Relaxor-Ferroelektrikum PMN-10PT können sehr gut mit einem Modell eines ungeordneten Ferroelektrikums erklärt werden, dessen Domänenwände unordnungsbedingt an sogenannten Pinning-Zentren festhaften.