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     

Multiferroic properties of Bi0.8La0.2FeO3/CoFe2O4 multilayer thin films

Bi_0.8La_0.2FeO₃/CoFe₂O₄ (BLFO/CFO) multilayer thin films (totally 20 layers BLFO and 19 layers CFO) were prepared on Pt/Ti/SiO₂/Si substrates by pulsed laser deposition. X-ray diffraction and transmission electron microscope measurements show that the films are polycrystalline and consisted of multilayered structure. Ferroelectric hysteresis loops with remnant polarization and saturated polarization of 4.2 and 13.3 μC/cm², respectively, were observed. On the other hand, the films show well-shaped magnetization hysteresis loops with saturated and remnant magnetization of 34.7 and 11.4 emu/cm³, respectively, which are significantly larger than pure BLFO thin films deposited under the same conditions. These results indicate that constructing epitaxial superlattice might be a promising way to fabricate multiferroics with improved properties.     

Recording of domains and regular domain patterns in strontium–barium niobate crystals in the field of atomic force microscope

The recording of microdomains and regular 1D- (linear) and 2D- (square) domain arrays was performed in SBN crystals by means of applying low (within 10 V) DC voltages to an AFM tip. The ferroelectric phenomena under AFM-tip fields (P–E hysteresis loops, the domain dynamics, etc.) agree qualitatively with the polarization processes observed at the macroscopic level and reveal peculiarities obviously related to the relaxor origin of SBN crystals. Particularly, the domain formation and the domain-wall lateral motion occur under fields much lower than E _c , which founds no explanation in terms of the model approach to the ferroelectric switching. The formation of linear and square domains results from overlapping closely spaced individual domains. For the first time a drastic dependence of the temporal stability on the domain topology was found. Namely, at identical exposure conditions of recording, the lifetimes of individual domains, domain lines, and domain squares (“chessboards”) are, respectively, several minutes, tens of hours, and no less than a month.     

Rochelle salt in an inhomogeneous electric field

The parameters of the hysteresis loop in the ferroelectric Rochelle salt were investigated using a sample with two pairs of electrodes: measurement electrodes and the side ones. It has been shown that the difference between the potentials of the measurement and the side electrodes (generating an inhomogeneous electric field) leads to gradual decay in time t of the remanent polarization P_r. The time required for the hysteresis loop to disappear in the inhomogeneous electric field (not parallel to the ferroelectric axis) decreases with temperature increase from 44±3 h at – 9°C to 2.3±0.1 h at 21.9 °C. On the other hand, the crystal placed for a sufficiently long time simultaneously in the measuring electric field and in the constant inhomogeneous one may finally exhibit a stationary hysteresis loop with a reduced remanent polarization and the unchanged coercive field. It has been shown that the crystal as a whole does not have to be polarized perpendicularly to the ferroelectric axis in order for its hysteresis loop to be reduced.     

Polarization switching process of soft lead zirconate titanate bulk ceramics

The domain switching dynamics was investigated in Nb-doped Pb(Zr_0.52Ti_0.48)O₃ bulk ceramics through observing systematically the evolution of the hysteresis loops at frequencies ranging from 0.01 to 100 Hz and in a field of 7.5–35 kV/cm. The experimental results indicate that the hysteresis loops are remarkably dependent on the fields and the frequencies. The data are analyzed by the Merz equation. The analysis results reveal that the requirement to satisfy the Merz equation is saturated loops. Based on these results, we divided the polarization switching process into three regions.     

Simulation of thickness dependence in ferroelectric thin films

The thickness dependence of coercive field (E_C) and remanent polarization (P_r) in ferroelectric thin films has been numerically simulated using a two-dimensional four-state Potts model. In this model, each of the dipoles in the film is assigned to one of the four states corresponding to the four different mutually perpendicular orientations. Neighboring dipoles with the same orientation are then grouped together to form a domain. Four different kinds of domains exist. In the presence of the surface layer near the electrode/film interface, the thickness dependence of both coercive field and remanent polarization are simulated.     

Piezoresponse imaging and local characterization of ferroelectric domains in Pb(Zn1/3Nb2/3)O3–7%PbTiO3 single crystals

Ferroelectric domain structures of (001)‐oriented Pb(Zn_1/3Nb_2/3)O₃–7%PbTiO₃ (PZN‐7%PT) single crystals were visualized and characterized by piezoresponse force microscopy (PFM). Locally regular domain configurations are found to be possibly related to the stable macroscopic properties in the PZN‐7%PT single crystals. Nanoscale piezoresponse hysteresis loops measured by PFM tip revealed no evidence of local domain switching behavior in the PZN‐7%PT single crystal. (© 2007 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Relaxor behaviour in PZN-PT-BT ferroelectric ceramics

The relaxor behaviour of the (Pb_0.8Ba_0.2)[(Zn_1/3Nb_2/3)_0.7Ti_0.3]O₃ ferroelectric ceramic is presented. A strong dispersion of the maximum of the dielectric permittivity (ε′) below the transition temperature (T_m) is observed, which shift towards higher temperatures with increasing frequency. There is a strong deviation from the Curie-Weiss law. The results are fitted by using the Volger-Fulcher relationship, showing typical behaviour of a spin glass system. The hysteresis loops suggest relaxor behaviour.     

Dielectric properties of ferroelectric/DMS heterointerface using YMnO3 and Ce doped Si

Bottom gate type Al/Si:8.2 at%Ce/YMnO₃/Pt capacitor was fabricated. Although it was polycrystalline, we successfully obtained Si:8.2 at%Ce film on ferroelectric YMnO₃. The dielectric properties of the capacitor were carefully investigated. Although the capacitance shows frequency dispersion, the capacitor exhibits a ferroelectric type C-V hysteresis loop. From the PUND and P-V measurements, ferroelectric polarization was distinguished from the another polarization, Based on these dielectric measurements, effect of polarization induced by the ferroelectric YMnO₃ on the carrier modulation in the diluted magnetic semiconductor, Ce doped Si film was discussed.     

Dependence of high electric-field-induced strain on the composition and orientation of Pb(Mg1/3Nb2/3)O3-PbTiO3 crystals

Electric-field-induced strain behavior of (1−x)Pb(Mg_1/3Nb_2/3)O₃-xPbTiO₃ (PMNT) crystals with different orientations and compositions was investigated for use as electromechanical actuators. Crystallographically, high strains with low hysteresis were achieved for 〈001〉 oriented rhombohedral crystals (29%≤x≤31%) near a morphotropic phase boundary, rather than 〈110〉 and 〈111〉. Domain instability could explain inferior strain levels and large hysteresis for 〈110〉 and 〈111〉 oriented crystals. Ultrahigh strain levels up to 1.8% could be achieved for 〈001〉 oriented PMNT crystals, being related to an E-field induced phase transition. −2 kV/cm negative E-field can be applied to PMNT ferroelectric material with low hysteresis. High strain with low hysteresis makes PMNT crystals promising candidates for high performance solid-state actuators.     

Artificial Modulation of Ferroelectric Thin Films into Antiferroelectric through H+ Implantation for High-Density Charge Storage

Hydrogen ions are implanted into Pb（Zro.3Tio.7）03 1014 ions/cm^2. Pseudo-antiferroelectric behaviour in thin films at the energy of 40keV with a flux of 5 x the implanted thin films is observed, as confirmed by the measurements of polarization versus electric hysteresis loops and capacitance versus voltage curves. X-ray diffrac- tion patterns show the film structures before and after H＋ implantation both to be perovskite of a tetragonal symmetry. These findings indicate that hydrogen ions exist as stable dopants within the films. It is believed that the dopants change domain-switching behaviour via the boundary charge compensation. Meanwhile, time dependence of leakage current density after time longer than lOs indicates the enhancement of the leakage cur- rent nearly in one order for the implanted film, but the current at time shorter than i s is mostly the same as that of the original film without the ionic implantation. The artificial tailoring of the antiferroelectric behaviour through H＋ implantation in ferroelectric thin films is finally proven to be achievable for the device application of high-density charge storage.     

Sub-coercive field dynamic hysteresis in morphotropic phase boundary composition of Pb(Zr1/2Ti1/2)O3-Pb(Zn1/3Nb2/3)O3 ceramic and its scaling behavior

Sub-coercive field dynamic ferroelectric hysteresis of a morphotropic phase boundary composition of the PZT-PZN ceramic was investigated under influence of the compressive stress. The scaling relation of hysteresis area 〈A〉 against frequency f, field amplitude E₀, and stress σ took a form of , which is not different significantly to that of other PZT-PZN compositions with pure tetragonal or rhombohedral structure, as well as to that of soft and hard PZT bulk ceramics. This study suggested that the domain structures, not ceramic compositions, played a key role in controlling dynamic hysteresis behavior of ferroelectric materials.     

Domain wall thickness variations of ferroelectric BaMgF4 single crystals in the tip fields of an atomic force microscope

The ferroelectric domain wall thickness of a fluoride BaMgF₄ single crystal was investigated by piezoresponse force microscopy. It was found that the domain wall thickness shows a strong spatial variation in the as‐grown crystal and the polarization reversal process. The original wall thickness is greater (about two to seven times) than that switched by the tip fields of the atomic force microscope. A significantly narrower domain wall was obtained in the higher tip‐field. The trapped defects at the domain wall play an important role in the spatial variation of the polarization width of 180° domain wall in the BaMgF₄ single crystal. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Hysteresis phenomena in the course of polarization evolution in a sinusoidal electric field in lead magnesium niobate crystals

The processes of polarization evolution in single crystals of the PbMg_1/3Nb_2/3O₃ model ferroelectric relaxor in a sinusoidal electric field are investigated at temperatures near and above the temperature T _d 0 of destruction of the induced ferroelectric state upon heating in zero electric field. The polarization switching current loops are measured in the ac electric field applied along the 〈111〉 and 〈110〉 pseudocubic directions. The electroluminescence intensity loops are obtained under the combined action of ac and dc electric fields applied along the 〈100〉 direction. In a certain temperature range above T _d 0 and the freezing temperature T _f in lead magnesium niobate, there are electric current anomalies, that correspond to the dynamic formation and subsequent destruction of the ferroelectric macroregions throughout each half-cycle of the ac electric field. The measurements of electroluminescence hysteresis loops demonstrate that the observed depolarization delay (related to the ac electric field amplitude) increases with an increase in the dc electric field and decreases as the ac field amplitude increases. The nature of the observed phenomena is discussed.     

Multiferroic magnetoelectric coupling and relaxor ferroelectric behavior in 0.7BiFeO3-0.3BaTiO3 nanocrystals

The structural, microstructural, polarization, magnetization, dielectric constant, and relaxor characteristics of 0.7BiFeO₃-0.3BaTiO₃ (BF-BT) nanocrystals have been studied. BF-BT nanocrystals were prepared by a chemical route using polyvinyl alcohol as surfactant. The phase structure is confirmed by X-ray diffraction and average particle size by transmission and scanning electron microscopy. The magnetoelectric coupling is studied by polarization hysteresis loops under the influence of applied magnetic field and the phase transition anomaly. The diffuse phase transition is studied by modified Curie-Weiss law and relaxor characteristics by Vogel-Fulcher relation.     

Recent advances in studies of magnetically soft amorphous microwires

In this paper, we present the giant magneto-impedance (GMI) effect (real part of longitudinal impedance, Z, and of the off-diagonal impedance) and hysteretic magnetic properties of amorphous glass-coated microwires with different compositions possessing nearly zero, positive and negative magnetostriction constant and metallic nucleus diameter ranging between 6 and 16 μm. Enhanced soft magnetic properties (low coercivity of about 4 A/m) and high-GMI effect have been observed in Co-rich microwires with vanishing magnetostriction constant. The magnetic anisotropy field of these microwires depends on the ratio between metallic diameter, d and total microwires diameter, D. Stress-sensitive magnetic properties have been obtained in Fe-rich microwires after stress annealing: hysteresis loop stress-annealed (SA) microwires drastically changes under applied stress. A variety of hysteresis loops with different hysteresis loops can be obtained in Fe-rich microwires changing the conditions (time and/or temperature) of the stress annealing. The obtained results allow us to tailor the microwire magnetic properties for magnetic sensors applications through selection of their composition and/or geometry and by thermal treatment.     

Effect of illumination on magnetization and microwave absorption of La1−xCaxMnO3 (x<0.2) films

Light-induced changes of the hysteresis loops of magnetization and microwave absorption are investigated in low-doped La_1−xCa_xMnO₃ (x<0.2) thin films. The width of the hysteresis loops decreases clearly under illumination with visible or near-infrared light at temperatures below 50 K. The microwave conductivity has a minimum value at magnetic fields corresponding to the magnetization reversal and is shifted towards weaker fields under illumination. These effects show complex nonexponential time evolution and dependence on strength of the magnetic field. The results can be explained by assuming that small ferromagnetic metallic regions exist within the insulating ferromagnetic phase of the sample, and that these regions are expanded by optically induced charge transfer between Jahn–Teller split e_g states of neighboring Mn³⁺ ions. Decrease of the Mn³⁺ XPS core level spectrum is observed in the samples under illumination with a HeNe laser.     

Ferroelectric Properties of Polycrystalline Ceramics with Dipolar Defect Simulated from the Potts--Ising Model

Physical properties of polycrystailine ferroelectrics including the contributions of the fixed dipolar defects and the average grain size in the Potts-Ising model are simulated by using the Monte Carlo method. Domain pattern, hysteresis loop and switching current of the polarization reversal process are obtained. Two processes are considered in our simulation. In the first one, the grain texture of ferroelectric ceramics are produced from the Ports model, and then the Ising model is implemented in the obtained polycrystailine texture to produce the domain pattern, hysteresis loop and switching current. It is concluded that the defect has the ability to decrease the remnant polarization P~ as well as the coercive field E~. The back switching is obviously observed after the electric field is off, and it shows some variation after introducing the fixed dipolar defect. Meanwhile, the spike of the switching current is found to lower with the increasing defect concentration and the decreasing average grain size.     

Piezoelectric evaluation of ion beam etched Pb(Zr,Ti)O3 thin films by piezoresponse force microscopy

The evolution of piezoelectric properties of Pb(Zr,Ti)O₃ (PZT) thin films after ion beam etching have been investigated at the nanoscale level by piezoelectric force microscopy. A comparison of the piezoelectric properties on etched and unetched films is realized. Piezoelectric contrasts imaging evidences a modification of the domain architecture at the film surface. Local piezoelectric hysteresis loops measurements on grains indicate that the coercive voltage for switching is much higher for the etched films (2.3 V) compared to the unetched ones (1.0 V) while the average piezoelectric activity is slightly lower. The results are explained in terms of grain-damaging during etching and domain-wall pinning.     

Properties of K0.5Bi0.5TiO3 thin films deposited on different substrates

K_0.5Bi_0.5TiO₃ thin films were deposited on fused quartz, n-type Si(100) and Pt/TiO₂/SiO₂/Si substrates by repeated coating/dying cycles. X-ray diffraction analysis shows that the films annealed at 700 °C for 10 min present perovskite phase. Atomic force microscopy reveals that the surface morphology is smooth, the grain sizes of the films on Si(100) are quite larger than on fused quartz. The capacitance-voltage hysteresis loops at various sweeping speed are collected as are polarization types. The films in the ON and OFF states are relatively stable. The films also exhibit a hysteresis loop at an applied voltage of 4 V, with a remanent polarization of 9.3 μC/cm² and a coercive voltage of 2 V. The insulating property of negative bias voltage is better than that of positive bias voltage. The transmittance of the films is between 74 and 82% in the wavelength range of 200-2000 nm.