Effect of electric field on electrocaloric effect in Pb(Zr1 − xTix)O3 solid solution

A thermodynamic analysis is employed to investigate the intrinsic electrocaloric effect of Pb(Zr_1 − xTi_x)O₃ solid solution system under the different electric field. Theoretical analysis indicates that Pb(Zr_1 − xTi_x)O₃ system has the giant electrocaloric coefficient and the large adiabatic temperature change near its ferroelectric Curie temperature. The applied electric field decreases not only the electrocaloric coefficient but also its temperature dependence. Furthermore, it increases the adiabatic temperature change as well as its dependence of temperature. The temperature corresponding to the maximum of electrocaloric coefficient and adiabatic temperature change increases with the enhancement of electric field because of its first-order phase transition between ferroelectric phase and paraelectric phase.     

Dynamic hysteresis in ferroelectric systems: experiment and Monte Carlo simulation

A Monte Carlo algorithm for dynamic hysteresis simulation in ferroelectric spin systems is developed based on a DIFFOUR model in which the local spontaneous polarization is defined by the double-well potential energy and the nearest-neighbor spin interaction as well as an external electrical field of variable amplitude and frequency. A direct measurement of the hysteresis loop for ferroelectric Pb(Zr_0.52Ti_0.48)O₃ thin film capacitors using the Sawyer–Tower technique is performed. Significant dependence of the hysteresis shape and pattern on the external field is revealed. Direct imaging of the simulated domain pattern indicates serious suppression of the domain switching over the high-frequency range. The evaluated scaling relations from the simulation for remanence, coercivity, and the area of the hysteresis over the low-frequency range are supported by theoretical predictions and experiments, but the high-frequency scaling behaviors as derived are different from one and another. Received: 23 January 2001 / Accepted: 17 August 2001 / Published online: 20 December 2001     

Soft modes and phonon interactions in studied by neutron scattering

The low frequency lattice dynamics and its relationship to the second order paraelectric-to-ferroelectric transition in Sn₂P₂S₆ is studied. The dispersion branches of the acoustic and lowest lying optical phonons in the a^*-c^* plane have been obtained in the ferroelectric phase, for x-polarized phonons. Close to the phase transition a considerable softening is found for the lowest optical mode (P_x), comparable to the behaviour observed in previous Raman investigations. As found previously in Sn₂P₂Se₆, a strong coupling between the TO(P_x) and TA(u_xz) phonons is observed, although, apparently, not strong enough to lead to an incommensurate phase. The soft TO(P_x) mode at the zone center is observed. The temperature dependence of its frequency and damping shows that the transition is not entirely displacive. At low temperatures an unusual apparent negative LO-TO splitting is observed which is shown to arise from the coupling of the x-polarized soft mode to the nearby z-polarized optical phonon. For comparison, the soft TO(P_x) dispersion in the a^*-b^* plane is measured in both the paraelectric and ferroelectric phases. Consistent frequency changes and LO-TO splitting are observed, revealing a significant interaction between the TA(u_yx) and LA(u_xx) acoustics branches and the TO and LO soft optic branches, respectively. In contrast, the nearby y-polarized optic branch shows almost no temperature dependence. Finally, the influence of piezoelectric effects on the limiting acoustic slopes in the ferroelectric phase is discussed. Received: 11 May 1998 / Revised and Accepted: 15 June 1998     

Compositional dependence of the Curie temperature in mixed ferroelectrics: effective field approach

An effective field approach is used to investigate the compositon depedence of the Curie temperature T_C(x) for mixed ferroelectric systems of partially deuterated triglycine sulfate (TGS)_1−x(DTGS)_x, and partially deuterated triglycine selenate (TGSe)_1−x(DTGSe)_x. We found that the coupling strength between the two sub systems is weaker than the average value of the effective field within each system, this can account for the non-linearity of composition dependence of the Curie temperature in these mixed ferroelectric systems.     

Frequency dependence of aging, rejuvenation and memory in a disordered ferroelectric

We characterize in details the aging properties of the ferroelectric phase of KTa_1-xNb_x O₃ (KTN), where both rejuvenation and (partial) memory are observed. In particular, we carefully examine the frequency dependence of several quantities that characterize aging, rejuvenation and memory. We find a marked subaging behaviour, with an a.c. dielectric susceptiblity scaling as ω, where t _w is the waiting time. We suggest an interpretation in terms of pinned domain walls, much along the lines proposed for aging in a disordered ferromagnet, where both domain wall reconformations and overall (cumulative) domain growth are needed to rationalize the experimental findings. Received 10 November 2000 and Received in final form 20 February 2001     

Coexistence of the relaxor-like and ferroelectric behavior in K1-xLixTaO3

ABSTRACT

The results of low-temperature linear and nonlinear susceptibilities, polarization measurements and the dc electric field dependence of the dielectric properties of the lithium-doped potassium tantalate K_1-xLi_xTaO₃, x = 0.034 (KLT-3.4%Li) solid solution are presented. The coexistence of the relaxor-like and ferroelectric behavior and different mechanisms leading to either of them are discussed. The observed ferroelectric phase transition is of the first-order type with temperature hysteresis. This transition is due to the off-center motions of Ta ions in the octahedral environment of oxygen ions. Clusters of Li⁺ ions produce a relaxor-like behavior and random electric field. This field reduces the depolarization field and allows off-center motions of Ta ions and an appearance of spontaneous polarization.     

Coupling of ferroelectric and antiferromagnetic order parameters in hexagonal RMnO3

Second-harmonic generation (SHG) is used as a probe for the coexisting ferroelectric and antiferromagnetic orders in hexagonal RMnO₃. SH contributions coupling to the electric and/or magnetic order parameters are identified on the basis of their spectral dependence and the symmetries of the corresponding order parameters. The SH signals from the ferroelectric and antiferromagnetic orders were employed to image the electric and magnetic domain structures separately. The transformation properties of electric and magnetic domains are discussed with respect to the transformation properties of the corresponding order parameters. An investigation of the mutual coupling between the coexisting electric and magnetic orders reveals apparently independent domain structures, which contradicts the symmetry and transformation properties of electric-dipole-induced SHG in this ferroelectromagnetic group of compounds. Apart from higher-order multipole contributions to SHG, interface contributions from clamped electric and magnetic domains can solve the contradiction. Received: 16 October 2001 / Published online: 24 April 2002     

Size dependence of dielectric properties and structural metastability in ferroelectrics

The size effect of the dielectric properties and the barrier height was investigated in the ferroelectric solid solution Ba_xSr_1-xTiO₃ system. The decrease of the grain size causes the suppression of the ferroelectricity, and the increase of the relaxation frequency. Barrier heights increase with increasing grain size. The result is analogous to magnetic phase transitions in nanocrystals and other solid-solid phase transitions in nanocrystals. It suggests a general rule that may be of use in the discovery of new metastable phases. An explanation of this phenomenon was given by an electric potential model that agrees well with the experimental results. For Ba_xSr_1-xTiO₃ system, the decrease of xcauses the decrease of the barrier height. Received 3 August 1998 and Received in final form 22 November 1998     

Optical second harmonic generation and ordering effects in the system of ferroelectric barium titanate nanocrystals

The temperature dependence of the optical second harmonic generation in nanocrystalline BaTiO₃:Eu³⁺ revealed a strong hysteresis in the C_4v-O_h ferroelectric phase transition region. The explanation of the effect by the ordering processes in the system of ferroelectric nanocrystals is confirmed by the experiments in an external electric field.     

Variation of the soft-mode frequency in ferroelectric semiconductors in a static electric field

The action of a static electric field on the soft-mode frequency in narrow-gap ferroelectric semiconductors, as a result of the contribution of the electron subsystem, is investigated within the framework of the vibronic mechanism. It is shown that the frequency of the soft mode varies directly as the square of the electric field strength under the action of the field, and the soft-mode frequency is determined in the vibronic model by the electron distribution function, whose parameters also vary under the action of the electric field. The effect is stronger for crystals with a one-dimensional electron spectrum than for those with an isotropic three-dimensional spectrum; according to estimates for ferroelectric semiconductors of the type Pb_1–xGe_xTe, a frequency variation of the order of the soft-mode frequency itself is attained in fields of the order of tens of volts per centimeter.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 1, pp. 33–37, January, 1988.     

Processing,Structure, Properties,and Applications of PZT Thin Films

There has been a resurgence of complex oxides of late owing to their ferroelectric and ferromagnetic properties. Although these properties had been recognized decades ago, the renewed interest stems from modern deposition techniques that can produce high quality materials and attractive proposed device concepts. In addition to their use on their own, the interest is building on the use of these materials in a stack also. Ferroelectrics are dielectric materials that have spontaneous polarization in certain temperature range and show nonlinear polarization–electric field dependence called a hysteresis loop. The outstanding properties of the ferroelectrics are due to non-centro-symmetric crystal structure resulting from slight distortion of the cubic perovskite structure. The ferroelectric materials are ferroelastic also in that a change in shape results in a change in the electric polarization (thus electric field) developed in the crystal and vice versa. Therefore they can be used to transform acoustic waves to electrical signal in sonar detectors and convert electric field into motion in actuators and mechanical scanners requiring fine control. In a broader sense the ferroelectric materials can be used for pyroelectric and piezoelectric sensors, voltage tunable capacitors, infrared detectors, surface acoustic wave (SAW) devices, microactuators, and nonvolatile random-access memories (NVRAMs), including the potential production of one transistor memory cells, and applications requiring nonlinear optic components. Another set of potential applications seeks to exploit the ferroelastic properties in stacked templates where they are juxtaposed to ferromagnetic materials. Doing so would allow the control of magnetic properties with electric field, which is novel. Such templates taking advantage two or more properties acquired a new name and now goes by multiferroics. After a brief historical development, this article discusses technological issues such as growth and processing, electrical and optical properties, piezo, pyro, and ferroelectric properties, degradation, measurements methods, and application of mainly lead-zirconate-titanate (PZT = PbZr_1?xTi_xO₃). The focus on PZT stems from its large electromechanical constant, large saturation polarization and large dielectric constant.     

Relation between vortex excitation and thermal conductivity in superconductors

Thermal conductivity κ _xx(T) under a field is investigated in d _{x2 - y2}-wave superconductors and isotropic s-wave superconductors by the linear response theory, using a microscopic wave function of the vortex lattice states. To study the origin of the different field dependence of κ_xx(T) between higher and lower temperature regions, we analyze the spatially-resolved thermal conductivity around a vortex at each temperature, which is related to the spectrum of the local density of states. We also discuss the electric conductivity in the same formulation for a comparison. Received 8 December 2001 and Received in final form 20 March 2002 Published online 6 June 2002     

CH4/air/SO2 premixed flame spectroscopy with a 7.5-μm diode laser

As sulfur dioxide (SO₂) is often involved in combustion processes, we present here SO₂-concentration measurements in the post-flame region of a CH₄/air/SO₂ premixed flame. SO₂ concentrations were deduced from high-resolution absorption spectra recorded with a mid-infrared tunable diode-laser (TDL) source operating at liquid nitrogen temperature. Single-mode, continuous frequency tuning around 1384.5 cm^-1 (or 7.5 μm) is achieved by a fine TDL temperature ramp. These experiments lead us to develop in situ combustion-pollutant measurements with compact apparatus. We show that this non-intrusive method is efficient for detection and allows the retrieval of SO₂ concentration and temperature. Received: 19 February 2001 / Revised version: 18 April 2001 / Published online: 7 June 2001     

1/<Emphasis Type="Italic">E</Emphasis><Superscript>2</Superscript> Law: Solution of the Unsolved Problem in the Physics of Ferroelectrics

An unusual frequency dependence of a coercive field observed in polycrystalline ferroelectric films of Pb(Zr_{1 ? x}Ti_x)O₃ solid solutions in a wide frequency range has been explained within the model of surface sources emitting thin ferroelectric domains with reversed polarization. This model makes it possible to interpret experimental data as the manifestation of the coercivity paradox in polycrystalline films and predicts the existence of the limiting frequency for switching of domains in agreement with the experiment. The proposed mechanism of polarization switching explains the observed temperature dependence of the activation field E_a ∝ T^?1/2. Furthermore, it predicts an increase in the activation energy for the nucleation of domains with an increase in the size of the source, indicating that the coercive field increases with the degradation of small     

Kinetics of nucleation of thermodynamically ordered ferroelectric phases in PbMg<Subscript>1/3</Subscript>Nb<Subscript>2/3</Subscript>O<Subscript>3</Subscript>–<Emphasis Type="Italic">x</Emphasis>PbTiO<Subscript>3</Subscript> crystals with different compositions

The kinetics of electric field-induced nucleation of ordered ferroelectric phases from a mixed glassy relaxor state has been studied in a number of single-crystal (1–x)PbMg_1/3Nb_2/3O₃–xPbTiO₃ (PMN–xPT) solid solutions (x = 29, 33, 35%) lying in a morphotropic phase region. It is shown that the formation of these phases and fast establishment of a macroscopic polarization are preceded by some delay time, depending on the electric field strength and temperature. It is found that the monoclinic phase is thermodynamically stable at room temperature in all the compounds in the time (~3000 s) and electric field (~1 kV/cm) ranges under study, whereas the monoclinic phase of the compound with x = 35% transforms, at temperatures near the temperature of the morphotropic phase transition after insignificant time interval of ~100 s, to another stable ferroelectric tetragonal phase.     

Electrocaloric response of a ferroelectric capacitor to a periodic electric field

The electrocaloric response of a ferroelectric capacitor to a periodic electric field has been analyzed in terms of the nonstationary heat conduction equation. A linear physical model is considered for an electrocaloric element in which one end (x = 0) is thermally insulated and a constant temperature T ₀ is maintained at the boundary x = l. The effect of a periodic electric field on the capacitor gives rise to temperature oscillations about a decreasing average value that reaches saturation. A relatively simple analytic expression is derived for the temperature distribution along the electrocaloric element and the heat flux density under stationary conditions. The calculations are carried out using the results obtained from measurements performed for a PMN-PT relaxor ferroelectric in the temperature range of the phase transition. A temperature gradient and a heat flux of ～150 W/cm² are observed in an electric field of 2.4 V/μm at a frequency of 10 Hz.     

Ferroelectricity in antiferromagnetic phases of Eu1−xY xMnO3

This work reports an experimental investigation of the ferroelectric character of magnetic phases of the orthorhombic Eu_1−xY _xMnO₃ system at low temperatures. The temperature dependence of the polarization curves clearly reveals the existence of a re-entrant improper ferroelectric phase for x=0.2, 0.3 and 0.5. A ferroelectric phase is also stable for x=0.4, and we have no experimental evidence for its vanishing down to 7 K. From these and early results obtained using other experimental techniques, the corresponding (x,T) phase diagram was traced, yielding significant differences with regard to the ones previously reported.     

Griffiths phase manifestation in disordered dielectrics

We predict the existence of a Griffiths phase in dielectrics with a concentrational crossover between dipole glass (electric analog of spin glass) and ferroelectricity. Particular representatives of the above substances are KTaO₃:Li, Nb, Na, or relaxor ferroelectrics like Pb_1–xLa_xZr_0.65Ti_0.35O₃. Since this phase exists above the ferroelectric phase-transition temperature (but below that temperature for ordered substances), we call it a “para-glass phase”. We assert that the difference between paraelectric and para-glass phases in the above substances is the existence of clusters (inherent to the “ordinary” Griffiths phase of Ising magnets) of correlated dipoles. We show that randomness plays a decisive role in the Griffiths (para-glass) phase formation: this phase does not exist in a mean field approximation. To investigate the Griffiths phase properties, we calculate the density of Yang-Lee (YL) zeros in the partition function and find that it has “tails” inherent to the Griffiths phase in the above temperature interval. We perform calculations on the basis of our self-consistent equation for the long-range order parameter in an external electric field. This equation has been derived in the framework of the random field theory. The latter automatically incorporates both short-range (due to indirect interaction via transverse optical phonons of the host lattice) and long-range (ordinary dipole-dipole) interactions between impurity dipoles, so that the problem of long-range interaction considerations does not appear in it. Received 17 May 2000     

37BiScO_3-63PbTiO_3铁电陶瓷的极化翻转行为研究

在正弦电场E=E0sin(2πft)加载下,通过改变电场E0(5—55kV/cm)和频率f(0.1—100Hz),测量了37BiScO3-63PbTiO3铁电陶瓷材料的电滞回线.数据拟合结果表明:在低电场和高电场阶段,剩余极化强度Pr的对数和矫顽场强Ec的对数都与电场强度E0的对数存在线性关系,而介于高电场与低电场之间则无线性关系存在,这种三阶段行为有别于现有的两阶段行为.这可归结于铁电陶瓷在不同的电场作用下铁电极化机理的不同.     

Temperature-dependent ferroelectric and dielectric properties of Bi3.25La0.75Ti3O12 thin films

To investigate temperature-dependent ferroelectric and dielectric properties of ferroelectric films, Bi_3.25La_0.75Ti₃O₁₂ (BLT) thin films were prepared on Pt-coated silicon substrates by pulsed laser deposition. The ferroelectric and dielectric behaviors have been studied in a wide temperature range from 80 K to room temperature. The saturated polarization (P_sat) decreases with decreasing temperature and decreasing electric field, whereas remnant polarization (P_r) shows a more complex temperature dependence. These results, which can be well explained based on a temperature-dependent charged defects-domain wall interaction model, might be helpful for further understanding the domain switching behavior. Based on these results, an alternative way to investigate temperature-dependent ferroelectric fatigue is proposed and experimentally carried out. The measured fatigue rate is found to be linearly dependent on temperature, consistent with the report on Pb(Zr,Ti)O₃ films. Temperature-dependent dielectric measurements of the films further confirm the above explanation.