Evolution of dielectric and optical properties in PbIn1/2Nb1/2O3-PbMg1/3Nb2/3O3-PbTiO3 single crystals in an electric field

A study is reported of various modes of dc electric field application (0 < E < 3 kV/cm) on structural phase transformations and behavior of the phase boundary in [001]-oriented 30PbIn_1/2Nb_1/2O₃-37PbMg_1/3Nb_2/3O₃-33PbTiO₃ single crystals located close to the morphotropic phase boundary. Dielectric methods of investigation have been complemented for the first time with optical methods. It has been found that the number, symmetry, and stability of the phases formed in the field depend on the actual mode of field application. The E-T phase diagrams have been constructed for different field application modes. It has been shown that phase diagrams obtained for the same crystal are different for different field application modes.     

Complex Studies of the Kinetics of Induced Phase Transition in [001], [011], and [111]-Oriented Single Crystal Relaxor Solid Solutions

The kinetics of an induced phase transition in single-crystal relaxor solid solutions 33PbIn_1/2Nb_1/2O₃–35PbMg_1/3Nb_2/3O₃–32PbTiO₃ and PbMg_1/3Nb_2/3O₃–29PbTiO₃ under application of an electric field along three directions [001], [011], and [111] at room temperature is studied. Joint measurements of optical transmission at different wavelengths, dielectric properties, and attenuation of sound are carried out. It was found that, even in small fields (E ~ 2 kV/cm) applied in the [011] and [111] directions, the maximum changes in all three characteristics as well as the coincidence of the time dependences of the optical transmission at different wavelengths of light occur in the same time interval. It is established that, in the same interval of fields along the [001] direction, the anomalies of the optical properties do not coincide in time with the anomalies of the acoustic and dielectric properties. The results obtained are explained by the induction of single-domain and multidomain phases.     

Influence of the electric field on structural transformations and phase boundary for PMg1/3Nb2/3O3-xPbTiO3 single crystals

The influence of different regimes of application of a dc electric field (0 < E < 4 kV/cm) on structural phase transformations and behavior of the phase boundary in [001]-oriented single crystals PMg_1/3Nb_2/3O₃-xPbTiO₃ (PMN-xPT) with compositions near the morphotropic phase boundary (x = 28 and 32%) and far from it (x = 13%) has been investigated. The studies have been performed using optical methods, namely, optical transmittance and small-angle light scattering. It has been revealed that the number, symmetry, and stability of field-induced phases depend on the regime of electric field application. During cooling of the PMN-28PT crystals from the cubic phase in the field (FC regime), the tetragonal phase is induced already in weak fields of ∼0.5 kV/cm, whereas even a field of 3 kV/cm is insufficient for inducing this phase by applying the field in the ferroelectric phase. In the PMN-32PT crystal (which has a composition closer to the morphotropic phase boundary as compared to that of the PMN-28PT crystal) in the FC regime and when the field is applied in the ferroelectric phase, the tetragonal phase is induced already in weak electric fields, even though this phase in the latter case appears to be unstable. The E-T phase diagrams have been constructed for different regimes of field application. The possible factors responsible for the observed differences have been discussed.     

Optical and dielectric anomalies in PbIn1/2Nb1/2O3-xPbTiO3 crystals in an electric field

A study is reported of the effect produced by application of a dc electric field (0 < E < 5 kV/cm) in different regimes on structural phase transformations and behavior of the phase boundary in [001]-oriented PbIn_1/2Nb_1/2O₃-37PbTiO₃ single crystals (starting composition) near the morphotropic phase boundary. The dielectric methods have been complemented for the first time by optical probing. It has been demonstrated that the content of PbTiO₃ in the samples under study is less than that in the starting composition. A suggestion is advanced that, in the samples studied, the stable room-temperature state with no electric field applied is that formed in the mixture of the rhombohedral R and monoclinic M _a phases. It has been found that the number, symmetry, and stability of the phases formed in a field depend on the regime of field application. The E-T phase diagrams have been constructed for different field application regimes. Phase diagrams obtained for the same crystal have been shown to differ for different regimes of field application.     

In-situ X-ray investigation of a PbMg1/3Nb2/3O3-28%PbTiO3 single-crystal plate in an external electric field

A (001) single-crystal plate PbMg_1/3Nb_2/3O₃28 mol %PbTiO₃ was investigated by wide-angle X-ray scattering at room temperature in situ under the influence of an external static electric field E, applied along the [001] direction of the specimen. Excluding an initial stage of the electric field processing, the induced strain s calculated from the change of interplanar spacing, exhibited a symmetrical increase with |E|, and an anhysteretic character of the s(E) dependence, during unidirectional loops of the applied electric field. Reasons for the observed s(E) behaviour are discussed.Dedicated to Professor Hartmut Fuess (TU Darmstadt, Germany) on the ocassion of his 65th birthdayPACS 61.10.NZ; 61.50.-f; 83.60.Np; 84.37.+q     

Effect of electric field on the smeared phase transition in crystals PbIn1/2Nb1/2O3-28PbTiO3 and PbIn1/2Nb1/2O3-37PbTiO3

The effect of a direct-current electric field (0 < E < 3 kV/cm) on the smearing of the phase transition and the Curie-Weiss exponent (γ) for two PbIn_1/2Nb_1/2O₃-28PbTiO₃ and PbIn_1/2Nb_1/2O₃-37PbTiO₃ crystals lying at different distances from the morphotropic phase boundary has been investigated. The universal Curie-Weiss law has been used to approximate the temperature dependences of the dielectric permittivity. It has been shown that the more remote is the crystal from the morphotropic phase boundary, the larger is the exponent γ and, consequently, the more smeared is the phase transition (in the zero field, γ = 1.67 and 1.49 for PbIn_1/2Nb_1/2O₃-28PbTiO₃ and PbIn_1/2Nb_1/2O₃-37PbTiO₃, respectively). It has been found that a weak electric field (no greater than 2–3 kV/cm) in the case of the more smeared phase transition almost does not affect the Curie-Weiss exponent, whereas for the PbIn_1/2Nb_1/2O₃-37PbTiO₃ crystal, this exponent decreases with increasing electric field strength and approaches γ = 1, which is characteristic of the conventional ferroelectric.     

E-T phase diagrams of a solid solution of the multicomponent PbZn1/3Nb2/3O3-PbMg1/3Nb2/3O3-PbNi1/3Nb2/3O3-PbTiO3 system near the morphotropic phase boundary

The specific features of the dielectric and pyroelectric responses of a solid solution in the barium-doped multicomponent yPbZn_1/3Nb_2/3O₃-mPbMg_1/3Nb_2/3O₃-nPbNi_1/3Nb_2/3O₃-xPbTiO₃ system of the composition y = 0.0982, m = 0.4541, n = 0.1477, and x = 0.3 near the morphotropic phase boundary have been investigated. It has been assumed that the maxima revealed in the dependences of the reversible permittivity on the electric field strength with both the forward and backward changes in the field (E ₌) are associated with the induced phase transition. Based on the experimental results, the E-T phase diagrams are constructed in the temperature range from ?100 to 150°C for different temperature-field regimes: (i) variation in the electric field E ₌ at a fixed temperature of the sample and (ii) variation in the temperature of the sample at a constant value of E ₌. It has been found that there is a singular point in the E-T phase diagram and that, in the vicinity of this point, the dielectric and pyroelectric responses of the studied ceramics exhibit specific features.     

Field-induced piezoelectric response in Pb(Mg1/3Nb2/3)O3–PbTiO3 single crystals

The electric field induced strain, piezoelectric and electromechanical response in relaxor based single crystal piezoelectrics (1−x)Pb(Mg_1/3Nb_2/3)O₃–xPbTiO₃(PMNT100x) were investigated as a function of dc bias and temperature along the crystallographic [001] orientation. With increasing temperature and dc bias, monoclinic and rhombohedral phases were found to coexist in the crystals, exhibiting large strain hysteresis, while above a threshold temperature and dc bias, the induced monoclinic and tetragonal phases were found to show very low strain hysteresis. The electric field level for the monoclinic to tetragonal phase transformation was found to exponentially decay with temperature. The mechanical quality factor Q for the tetragonal phase exhibits higher values when compared to rhombohedral and monoclinic phases, displaying improved domain stability. The domain stability of tetragonal crystals as a function of sample thickness was also studied, it was found that a higher dc bias was needed for thinner tetragonal crystals in order to stabilize the single domain configuration and reduce the strain hysteresis.     

Orientation effects on the bandgap and dispersion behavior of 0.91Pb（Zn_（1/3）Nb_（2/3））O_3-0.09PbTiO_3 single crystals

0.91Pb(Zn_1/3Nb_2/3)O₃--0.09PbTiO₃ (PZN--9%PT) single crystals with different orientations are investigated by using a spectroscopic ellipsometer, and the refractive indices and the extinction coefficients are obtained. The Sellmeier dispersion equations for the refractive indices are obtained by the least square fitting, which can be used to calculate the refractive indices in a low absorption wavelength range. Average Sellmeier oscillator parameters E_o, $\lambda$_o, S_o, and E_d are calculated by fitting with the single-term oscillator equation, which are related directly to the electronic energy band structure. The optical energy bandgaps are obtained from the absorption coefficient spectra. Our results show that the optical properties of [001] and [111] poled crystals are very similar, but quite different from those of the [011] poled crystal.     

Electric field effects on the dielectric and acoustic anomalies of Pb[(Mg1/3Nb2/3)0.83Ti0.17]O3 single crystals studied by dielectric and Brillouin spectroscopies

The effect of the electric field on the dielectric and acoustic properties of Pb[(Mg_1/3Nb_2/3)_0.83Ti_0.17]O₃ single crystals was investigated as functions of temperature and the electric field strength. The dielectric constant and the acoustic mode behaviors exhibited typical relaxor behaviors when there was no bias field. The longitudinal acoustic mode showed splitting under a moderate electric field of 1 kV/cm applied along the [001] direction, indicating coexistence of macroscopic/mesoscopic ferroelectric states and relaxor states. Further increase in the electric field up to 2 kV/cm induced a clear ferroelectric phase transition, which became smeared out due to the proximity of the electric field to the critical point. The electric field-temperature phase diagram of Pb[(Mg_1/3Nb_2/3)_0.83Ti_0.17]O₃ was suggested based on the observed field-induced changes in the dielectric and the acoustic properties.     

Bias field effects on the dielectric properties of 0.67Pb(Mg1/3Nb2/3)O3-0.33PbTiO3 single crystals with different orientations

The domain states and phase transitions in 0.67Pb(Mg_1/3Nb_2/3)O₃-0.33PbTiO₃ single crystals were investigated by studying their relative permittivity under various dc bias at constant heating and cooling rates. The orientation dependence of the bias field effect was revealed by examining the temperature dependence of relative permittivity as a function of crystal orientation (the 〈111〉, 〈011〉 and 〈001〉 directions) and dc bias field. The crystals basically have a macrodomain rhombohedral ferroelectric state in the ferroelectric phase under zero dc bias. External bias field could modulate the domain state and induce a stable macrodomain state in the crystals. Also, it is proposed that the dc bias applied along the 〈001〉 or 〈011〉 direction could induce a tetragonal ferroelectric phase or an orthorhombic ferroelectric phase, respectively, in an intermediate temperature range.     

Theoretical study on the fine structure of PbFe0.5Nb0.5O3

The full potential linearized augmented plane wave method within the generalized gradient approximation was used to determine the tetragonal fine structure for PbFe_0.5Nb_0.5O₃, i.e., the equilibrium configuration of B-site compound cations (Fe and Nb). It was found that the displacement of atom Fe along [001] direction is 0.022 nm and that of Nb is 0.0020 nm. The ferroelectric instability of complex compound PbFe_0.5Nb_0.5O₃ is mainly coming from the displacement of atom Fe along [001] direction.     

Magnetoelectricity in the PbFe1/2Nb1/2O3 Ceramics

The magnetodielectric effect (the influence of a magnetic field H on the dielectric constant ?) and the magnetoelectric effect (the influence of an electric field E on the magnetoelectric constant ??) of the PbFe_1/2Nb_1/2O₃ ceramics have been investigated at temperatures T in the range from 50 to 200°C, including the Curie point T _C ? 98°C. It has been demonstrated that there is a correlation of these effects with the shift of the ferroelectric-paraelectric phase transition temperature in a magnetic field.     

Ferroelectric phase transitions in Pb0.96Ba0.04Sc0.5Nb0.5O3 and Pb0.94Ba0.06Sc0.5Nb0.5O3 solid-solution single crystals

The optical properties of Pb_0.96Ba_0.04Sc_0.5Nb_0.5O₃ (PBSN-4) and Pb_0.94Ba_0.06Sc_0.5Nb_0.5O₃ (PBSN-6) single-crystal solid solutions were studied for the first time. It was shown that the spontaneous phase transition occurring in PBSN-4 with no electric field present is accompanied by a sharp minimum in optical transmission, which indicates the percolation nature of the transition. No sharp changes were observed in the temperature dependence of optical transmission in PBSN-6 single crystals with no electric field applied. However, a very weak electric field, ～0.4 kV/cm, is sufficient to induce the ferroelectric state in PBSN-6 single crystals. It was shown that the destruction of the induced ferroelectric state is a first-order phase transition which is accompanied by an anomalously narrow peak in the small-angle light scattering intensity (or by a minimum in optical transmission) and occurs through the percolation mechanism.     

Successive phase transitions in the highly ordered complex perovskite PbLu1/2Nb1/2O3

The structural phase transitions and the electrical behaviour of the complex perovskite PbLu_1/2Nb_1/2O₃ have been investigated using X-ray powder diffraction, dielectric constant measurements, differential scanning calorimetry and measurement of the polarisation as a function of applied electric field. The high-temperature paraelectric phase is highly ordered. A first-order paraelectric-antiferroelectric phase transition occurs at 270°C and an antiferroelectric-ferroelectric phase transition, characterised by dispersion in the curves of dielectric constant as a function of temperature, occurs at ≈ 30°C. The antiferroelectric phase is isostructural with the orthorhombic form of PbYb1/₂Nb1/₂O₃. The low-temperature ferroelectric phase also has an orthorhombic crystal structure.     

Evolution of the ferroelectric phase in ?001?-oriented (100 ? x )PbMg1/3Nb2/3O3- x PbTiO3 single crystals

The effect of a dc electric field on the nucleation and evolution of the phase with long-range order in a cubic nonpolar matrix in 〈001〉-oriented (100 − x)PbMg_1/3Nb_2/3O₃-xPbTiO₃ single-crystal relaxors as the content of PbTiO₃ is gradually increased (6 ≤ x ≤ 20, where x is the PbTiO₃ content given in molecular percent) is investigated. The optical properties of these solid solutions are studied in different modes of application of an electric field. It is shown that an applied electric field with a strength above a threshold value induces a first-order ferroelectric phase transition with a temperature hysteresis occurring between measurements performed under cooling and heating of the crystal in the electric field. As the PbTiO₃ content or electric field strength increases, the hysteresis becomes less pronounced and the first-order phase transition is suppressed. At x ∼ 20, the induced transition resembles a second-order rather than first-order transformation. It is assumed that, for compositions with x > 10 in electric fields higher than 4 kV/cm, the formation of the rhombohedral phase is accompanied by the appearance of another (possibly, monoclinic) phase associated with the rotation of the polarization vector from the [111] direction of the rhombohedral phase to the [001] direction of the tetragonal phase. Original Russian Text ? L.S. Kamzina, E.V. Snetkova, I.P. Raevskiĭ, A.S. Emel’yanov, Jiayue Xu, Weidong Xiang, 2007, published in Fizika Tverdogo Tela, 2007, Vol. 49, No. 4, pp. 725–730.     

Effect of bias field on the dielectric properties of 0.7Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 single crystals with different orientations

Microdomain-macrodomain transformations and phase transitions in 0.7Pb(Mg_1/3Nb_2/3)O₃-0.3PbTiO₃ single crystals were investigated by studying their relative permittivity under various dc bias at constant heating and cooling rates. The orientation dependence of the bias field effect was revealed by examining the temperature dependence of relative permittivity as a function of crystal orientation (the 111, 011 and 001 directions) and dc bias field. The crystals have a microdomain rhombohedral ferroelectric state in the ferroelectric phase under zero dc bias. External bias field could modulate the domain state and induce a macrodomain state in the crystals. Also, it is proposed that the dc bias applied along the 001 or 011 direction could induce a tetragonal ferroelectric phase or an orthorhombic ferroelectric phase, respectively, in an intermediate temperature range. PACS 77.80.-e; 77.22.-d; 81.40.-z     

C-oriented SrBi2Nb2O9 films grown on YBa2Cu3O7−δ /SrTiO3 and NdGaO3

Epitaxial SrBi₂Nb₂O₉ films were grown by laser ablation on (001)YBa₂Cu₃O_7?δ /(100)SrTiO₃ and (001)NdGaO₃, with c axis normal to the substrate plane. The SrBi₂Nb₂O₉ films were grown in a layer-by-layer regime on NdGaO₃ substrates in 25-Å steps at a condensation temperature of 700 °C. Microinclusions of secondary phases and a-oriented grains were observed to exist on the surface of (001)SrBi₂Nb₂O₉ films grown on (001)YBa₂Cu₃O_7?δ /(100)SrTiO₃. The dielectric permittivity of the SrBi₂Nb₂O₉ films measured along the c axis is 123 (T=300 K, f=100 kHz), and tan δ≈0.04.     

Polarization switching by stretched exponential functions in 0.7Pb(Mg1/3Nb2/3)O3–0.3PbTiO3

Polarization reversal and domain dynamics have been investigated in 0.7Pb(Mg_1/3Nb_2/3)O₃–0.3PbTiO₃ using a method of current transients. Investigations were performed as a function of applied electric field. The kinetics of the transients have been modelled by a stretched-exponential-type function.     

Composition Dependence of Electrocaloric Effect in (1-x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 Single Crystals

Composition dependence of electrocaloric effect is investigated in (1-x)Pb(Mg_1/3Nb_2/3)O_3-xPbTiO₃ single crystals by using an eighth-order Landau—Devonshire theory. The applied electric field along [001] direction reduces the ferroelectric-ferroelectric phase transition temperatures, but increases the Curie temperatures. The electrocaloric coefficients of tetragonal phase are much larger than that of rhombohedral and monoclinic phase. A negative electrocaloric effect is observed near the M_C-T phase transition in 0.69 Pb(Mg_1/3Nb_2/3)O₃-0.31 PbTiO₃ single crystal. The application of a strong enough electric field results in a high adiabatic temperature change over a broad range of temperature. Therefore, it would be useful to construct a solid state cooling cycle over a broad temperature range for practical applications.