Paraelectric Doping Simultaneously Improves the Field Frequency Adaptability and Dielectric Properties of Ferroelectric Materials:A Phase-Field Study

Recent years,the polarization response of ferroelectrics has been entirely studied.However,it is found that the polarization may disappear gradually with the continually applied of electric field.In this paper,taking K0.48Na0.52NbO3(KNN)as an example,it was demonstrated that the residual polarization began to decrease when the electric field frequency increased to a certain extent using a phase-field methods.The results showed that the content of out-of-plane domains increased first and then decreased with the increase of applied electric field frequency,the maximum polarization disappeared at high frequencies,and the hysteresis loop became elliptical.In order to further study the abnormal changes of hysteresis loops of ferroelectrics under high electric field frequency,we analyzed the hysteresis loop and dielectric response of solid solution 0.1SrTiO_(3)-0.9K_(0.48)Na_(0.52)NbO_(3).It was found that the doped hysteresis loop maintained its shape at higher frequency and the dielectric constant increased.This kind of doping has a higher field frequency adaptability,which has a key guiding role in improving the dielectric properties of ferroelectric thin films and expanding the frequency application range of ferroelectric nano memory。

Enhanced ferroelectric and improved leakage of BFO-based thin films through increasing entropy strategy

BiFeO_(3)(BFO)has received considerable attention as a lead-free ferroelectric film due to its large theoretical remnant polariza-tion.However,BFO suffers from a large leakage current,resulting in poor ferroelectric properties.Herein,the sol-gel method was used to deposit a series of BFO-based thin films on fluorine-doped tin oxide substrates,and the effects of the substitution of the elements Co,Cu,Mn(B-site)and Sm,Eu,La(A-site)on the crystal structure,ferroelectricity,and leakage current of the BFO-based thin films were invest-igated.Results confirmed that lattice distortion by X-ray diffraction can be attributed to the substitution of individual elements in the BFO-based films.Sm and Eu substitutions contribute to the lattice distortion in a pseudo-cubic structure,while La is biased toward pseudo-tet-ragonal.Piezoelectric force microscopy confirmed that reversible switching of ferroelectric domains by nearly 180°can be realized through the prepared films.The ferroelectric hysteresis loops showed that the order for the polarization contribution is as follows:Cu>Co>Mn(B-site),Sm>La>Eu(A-site).The current density voltage curves indicated that the order for leakage contribution is as follows:Mn<Cu<Co(B-site),La<Eu<Sm(A-site).Scanning electron microscopy showed that the introduction of Cu elements facilitates the formation of dense grains,and the grain size distribution statistics proved that La element promotes the reduction of grain size,leading to the increase of grain boundaries and the reduction of leakage.Finally,a Bi_(0.985)Sm_(0.045)La_(0.03)Fe_(0.96)Co_(0.02)Cu_(0.02)O_(3)(SmLa-CoCu)thin film with a qualitative leap in the remnant polarization from 25.5(Bi_(0.985)Sm_(0.075)FeO_(3))to 98.8µC/cm^(2)(SmLa-CoCu)was prepared through the syner-gistic action of Sm,La,Co,and Cu elements.The leakage current is also drastically reduced from 160 to 8.4 mA/cm^(2)at a field strength of 150 kV/cm.Thus,based on the increasing entropy strategy of chemical engineering,this study focuses on enhancing ferroelectricity and decreasing leakage current,providing a promising path for the advancement of ferroelectric devices.

Structure,ferroelectric,and enhanced fatigue properties of sol–gel-processed new Bi-based perovskite thin films of Bi(Cu_(1/2)Ti_(1/2))O_(3)–PbTiO_(3)

Bi-based perovskite ferroelectric thin films have wide applications in electronic devices due to their excellent ferroelectric properties.New Bi-based perovskite thin films Bi(Cu_(1/2)Ti_(1/2))O_(3)–PbTiO_(3)(BCT–PT) are deposited on Pt(111)/Ti/SiO_(2)/Si substrates in the present study by the traditional sol–gel method.Their structures and related ferroelectric and fatigue characteristics are studied in-depth.The BCT–PT thin films exhibit good crystallization within the phase-pure perovskite structure,besides,they have a predominant(100) orientation together with a dense and homogeneous microstructure.The remnant polarization(2P_(r)) values at 30 μC/cm^(2) and 16 μC/cm^(2) are observed in 0.1BCT–0.9PT and 0.2BCT–0.8PT thin films,respectively.More intriguingly,although the polarization values are not so high,0.2BCT–0.8PT thin films show outstanding polarization fatigue properties,with a high switchable polarization of 93.6% of the starting values after 10^(8) cycles,indicating promising applications in ferroelectric memories.

Optimal parameter space for stabilizing the ferroelectric phase of Hf_(0.5)Zr_(0.5)O_(2) thin films under strain and electric fields

Hafnia-based ferroelectric materials, like Hf_(0.5)Zr_(0.5)O_(2)(HZO), have received tremendous attention owing to their potentials for building ultra-thin ferroelectric devices. The orthorhombic(O)-phase of HZO is ferroelectric but metastable in its bulk form under ambient conditions, which poses a considerable challenge to maintaining the operation performance of HZO-based ferroelectric devices. Here, we theoretically addressed this issue that provides parameter spaces for stabilizing the O-phase of HZO thin-films under various conditions. Three mechanisms were found to be capable of lowering the relative energy of the O-phase, namely, more significant surface-bulk portion of(111) surfaces, compressive c-axis strain,and positive electric fields. Considering these mechanisms, we plotted two ternary phase diagrams for HZO thin-films where the strain was applied along the in-plane uniaxial and biaxial, respectively. These diagrams indicate the O-phase could be stabilized by solely shrinking the film-thickness below 12.26 nm, ascribed to its lower surface energies. All these results shed considerable light on designing more robust and higher-performance ferroelectric devices.

Influence of lateral size on dielectric properties of ferroelectric thin films with structure transition zones

By taking into account structural transition zones near the lateral and thickness direction edges,this paper uses a modified transverse Ising model to study dielectric properties of a finite size ferroelectric thin film in the framework of the mean-field approximation.The results indicate that the influence of the lateral size on the dielectric susceptibility cannot be neglected and lateral structural transition zones could be a crucial factor that improves the mean susceptibility of the fixed size film.

Strain tunability of dielectric and ferroelectric properties in epitaxial lead titanate thin films

Many distinguished properties of epitaxial ferroelectric thin films can be tunable through the misfit strain.The strain tunability of ferroelectric and dielectric properties in epitaxial lead titanate ultrathin films is numerically investigated by using a phase field model,in which the surface effect of polarization is taken into account.The response of polarization to the applied electric field in the thickness direction is examined with different misfit strains at room temperature.It is found that a compressive misfit strain increases the coercive field and the remanent polarization while a tensile misfit strain decreases both of them.The nonlinear dielectric constants of the thin films with tensile misfit strains are much larger than those of the thin films without misfit strains,which are attributed to the existence of the a/c/a/c multiple domains in the thin films under tensile misfit strains.

Dielectric and Ferroelectric Properties of PZN-4.5PT Nanoparticles Thin Films on Nanostructured Silicon Substrate for Ferrophotovoltaic and Energy Storage Application

The integration of ferroelectric materials as thin films has attracted considerable attention these last years thanks to their outstanding performances that allow considering new features for the realization of photovoltaic devices. Our study focuses on investigating structural, dielectric and ferroelectric properties of undoped and Mn doped PZN-4.5PT nanoparticles thin films on Silicon substrate. We fabricate very stable PZN-4.5PT nanoparticles thin films deposited on nanostructured silicon substrate with giant relative dielectric permittivity of 2.76 × 104 and 17.7 × 104 for respectively the undoped and Mn doped thin films. These values are very large compared to those found in single crystals and might be explained by the influence of the gel in which nanoparticles were dispersed. The SEM images show the crystallization of new hexagonal phases on the film surface probably coming from interaction between Si and the gel. The hysteresis loops permitted to determine the spontaneous polarization (Ps), remnant polarization (Pr) and coercive field Ec which are equal to 11.73 &mu;C/cm2, 10.20 &mu;C/cm2 and 20 V/cm, respectively for the undoped nanoparticles thin film and 22.22 &mu;C/cm2, 19.32 &mu;C/cm2 and 20 V/cm respectively for the Mn doped one. These values are high and correspond to the best ones found in literature compared to typical ferroelectric thin films.

Comment on “Ferroelectric composite-based piezoelectric energy harvester for self-powered detection of obstructive sleep”

SrTi_(2)O_(5) particles were claimed by Panda et al.in J.Materiomics 2023;9:609 as a new lead-free ferroelectric material with orthorhombic symmetry and space group of Cmm2,being,therefore,employed as a base of piezoelectric energy harvesters.However,in this comment we express concerns regarding the presence of the piezoelectricity in the studied material and the interpretation of the structural,microstructural,and ferroelectric results in that publication as those associated with SrTi_(2)O_(5).We also note that the presented dielectric results are contradictory and that many important details are missing.

A Bilayer High-Temperature Dielectric Film with Superior Breakdown Strength and Energy Storage Density

The further electrification of various fields in production and daily life makes it a topic worthy of exploration to improve the performance of capacitors for a long time,including thin-film capacitors.The discharge energy density of thin-film capacitors that serves as one of the important types directly depends on electric field strength and the dielectric constant of the insulation material.However,it has long been a great challenge to improve the breakdown strength and dielectric constant simultaneously.Considering that boron nitride nanosheets(BNNS)possess superior insulation and thermal conductivity owing to wide band gap and 2-dimensional structure,a bilayer polymer film is prepared via coating BNNS by solution casting on surface of polyethylene terephthalate(PET)films.By revealing the bandgap and insulating behavior with UV absorption spectrum,leakage current,and finite element calculation,it is manifested that nanocoating contributes to enhance the bandgap of polymer films,thereby suppressing the charge injection by redirecting their transport from electrodes.Worthy to note that an ultrahigh breakdown field strength(~736 MV m^(−1)),an excellent discharge energy density(~8.77 J cm^(−3))and a prominent charge-discharge efficiency(~96.51%)are achieved concurrently,which is ascribed to the contribution of BNNS ultrathin layer.In addition,the modified PET films also have superior comprehensive performance at high temperatures(~120°C).The materials and methods here selected are easily accessible and facile,which are suitable for large-scale roll-to-roll process production,and are of certain significance to explore the methods about film modification suitable for commercial promotion.

Dielectric properties and relaxor ferroelectric behavior of （1-y）Ba(Zr0.1Ti0.9)O3-yBa(Zn1/3Nb2/3)O3 ceramics

The microstructure,dielectric and ferroelectric properties of(1-y)Ba(Zr0.1Ti0.9)O3-yBa(Zn1/3Nb2/3)O3(y=0-0.05)ceramics prepared by traditional solid state method were investigated by X-ray diffractometer,scanning electron microscope,electric parameter testing system and ferroelectric tester.It is found that the barium zirconate titanate based ceramics are single-phase perovskites as y increases up to 0.05 and their average grain size decreases with the increase of y.The permittivity maximumεr,max is suppressed from 8948 to 1611 at 1 kHz with increasing y,and the ferroelectric-paraelectric phase transition temperature Tm decreases from 93 to-89℃at 1 kHz as y increases.The composition-induced diffuse phase transition is enhanced with increasingy.The relaxor-like ferroelectric behavior with a strong frequency dispersion of Tm and permittivity at T<Tm accompanied by a strong diffuse phase transition is found for the system with high y value.The remnant polarization decreases with increasing y,while the coercive field decreases remarkably and then increases with the increase of y.

Macro-circuit simulation and optimal design for ferroelectric liquid crystal based on dielectric properties

A macro-circuit equivalent model for ferroelectric liquid crystal （FLC） is proposed. The model includes both effects of ferroelectric toque and dielectric torque and is utilized to simulate the switching response and memory behavior of a single FLC cell . Simulation results show that the delay time has a minimum while increasing the amplitude of drive voltage and the amplitude of bipolar pulses should be controlled within a certain range to realize the memory behavior. Also the switching angle is successfully enhanced to the reference value of 22.5° by adopting ＂AC stabihzation＂ addressing method.

Dielectric Characteristics in BiFeO3-Modified SrTiO3 Incipient Ferroelectric Ceramics

We investigate the dielectric and ferroelectric properties of Sr1-xBixTi1-xFex03 solid solutions （x =0, 0.05, 0.1, 0.15 and 0.2） together with their structures. Through the analysis of Rietveld refinement of powder x-ray diffraction, a cubic structure in space group Pm3m is determined for all the compositions. An obvious dielectric relaxation peak differing from SrTiO3 is observed in the present ceramics. The peak temperature Tm increases with increasing x, and it approaches room temperature at x =0.2. The Vogel Fulcher law and Curie Weiss law fittings further confirm the relaxor ferroelectricity in the present ceramics.

Dielectric, piezoelectric, and ferroelectric properties of lanthanum-modified PZTFN ceramics

Specimens of Pb1-1.5xLax（Zr0.53 Ti0.47）1-y-zFeyNb2O3 （x = 0, 0.004, 0.008, 0.012, and 0.016, y = z = 0.01） （PZTFN） ceramics were synthesized by a semi-wet route. In the present study, the effect of La doping was investigated on the structural, microstructural, dielectric, piezoelectric, and ferroelectric properties of the ceramics. The results show that, the tetragonal （space group P4mm） and rhombohedral （space group R3c） phases are observed to coexist in the sample at x = 0.012. Microstructural investigations of all the samples reveal that La doping inhibits grain growth. Doping of La into PZTFN improves the dielectric, ferroelectric, and piezoelectric properties of the ceramics. The hys- teresis loops of all specimens exhibit nonlinear behavior. The dielectric, piezoelectric and ferroelectric properties show a maximum response atx 〉 0.012, which corresponds to the morphotropic phase boundary （MPB）.

Dielectric and ferroelectric properties of Sr_4CaSmTi_3Nb_7O_(30) with tetragonal tungsten bronze structure

Sr4CaSmTi3Nb7O30 ceramics are synthesized and indexed as tetragonal tungsten bronze structure. The dielectric behavior and ferroelectric nature are investigated. Three dielectric anomalies are observed. The phase transition is a displacive phase transition with some diffusive characteristics, which indicates possible compositional variations within the materials on the microscopic scale. The weak distortion disappears in cooling process for differential scanning calorimetry measurement, and the large depression of Curie-Weiss temperature TO indicates the difficulty in forming macroferroelectric domain. The ferroelectric nature in these filled tungsten bronze niobates originates from the off-center displacement of B-site cations, but they are primarily dominated by A-site cation occupation. Both the radius and the valence of A1-site cations play an important role on ferroelectric properties of the filled tungsten bronze compounds. Existence of spontaneous polarization with a remanent polarization of 0.16 μC/cm^2 a coercive field of Ec = 11.74 kV/cm confirms the room-temperature ferroelectric nature of Sr4CaSmTi3Nb7O30 ceramics.

NUMERICAL ANALYSIS OF DIELECTRIC RESPONSE IN RELAXOR FERROELECTRICS

The dielectric response of complex perovskite relaxor ferrolectrics Pb(Mg1/3Nb2/3) O3 with respect to temperature and frequency was carefully measured. Using a normalized method of the 'universal' many-body theory, the relaxation process was analyzed around the temperature of dielectric absorption maximum. There is no structural phase transition near this temperature and the behavior is closely like that of a polar dipole medium. The functional relationship about frequency and temperature of dielectric pormittivity maximum was also fitted to discuss the dynamic behavior of polar microregion. It is confirmed that a new power exponential Arrhenius relation is better to characterize the relaxation behavior than the Vogel-Fulcher and Debye relations. Based on the polarization theory of polar dipoles, we analyzed the relaxation mechanism of ferroelectric microdomains of relaxor ferroelectrics, and get an ideal distribution function of relaxation time. Consequently, a simulated dielectric response dependence on temperature and frequencies can be expressed, which is well coincided with experiment results.

Preparation, Characterization and Dielectric Properties of Sr_5RTi_3Ta_7O_(30) (R=Pr and Eu) Ferroelectric Ceramics

Polycrystalline samples of Sr5PrTi3Ta7O30 （SPTT） and Sr5EuTi3Ta7O30 （SETT） compounds were prepared by high-temperature solid-state reaction method and their formation, structure and dielectric properties were studied. They are found to be ferroelectric phase of filled tetragonal tungsten bronze （TB） structure at room temperature and undergoes diffuse type of ferroelectric-paraelectric phase transition around 34 ℃ and 31 ℃, respectively. At 1 MHz SPTT exhibits high dielectric constants of 177 and low dielectric losses of 3.5×10^-4 and SETT has high dielectric constants of 125 and low dielectric losses of 2.4×10^-3.

Effects of A1 site occupation on dielectric and ferroelectric properties of Sr_4CaRTi_3Nb_7O_(30)(R=Ce,Eu) tungsten bronze ceramics

Sr4Ca RTi3Nb7O30（R = Ce, Eu） tungsten bronze ceramics are prepared by a standard solid state reaction method. The effects of A1 site occupation on the dielectric and ferroelectric properties of Sr4 Ca RTi3Nb7O30（R = Ce, Eu） tetragonal tungsten bronzes are investigated. The Sr4 Ca Ce Ti3Nb7O30 shows a normal transition behavior due to the closer size ion occupation in A1 sites, which could suppress the distortion of B2 octahedra effectively. Sr4 Ca Eu Ti3Nb7O30 ceramic exhibits two dielectric anomalies, which might be related to the fact that the large radius difference between Ca^2＋ and Eu^3＋ could lead to the uneven distribution of Ca^2＋ and Eu^3＋ in A1 sites and form two slightly different kinds of compositions with different transition temperatures in the structure. Our results indicate that the ionic radius difference in A1 sites plays an important role in determining the dielectric and ferroelectric natures of the filled tungsten bronze ceramics. Polarization–electric field（P–E） curves are evaluated at room temperature and both of them show hysteresis loops. Sr4 Ca Ce Ti3Nb7O30 shows a fat hysteresis loop, indicating the long-range ferroelectric order in the ceramic. The current density–electric field（J–E） curves are measured at room temperature with a largest leakage current density of ～ 10^-6A/cm^2, indicating that their leakage currents are rather low.

Study of Dielectric and Mechanical Spectra on Point Defects and Phase Transition in Ferroelectric Ceramics

Ferroelectric materials have enormous potential applications in advanced techniques. However, there are still many problems in its practical application. Dielectric and mechanical (internal friction) measurements are very sensitive to phase transitions, relaxation process of point defects, domain walls and their mobility, which have severe effect on ferroelectric properties. These make them become very good means to investigate substantial information on structural features and to explore the fundamental principles in ferroelectric materials and their applications. In this paper, the dielectric and internal friction measurement were used to investigate the behaviors for point defects and phase transition in ferroelectric ceramics such as Bi_ 4-x La_ x Ti_ 3 O_ 12 , Bi_ 4 Ti_ 3-y Nb_ y O_ 12 , SrBi_ 2 Ti_ 2 O_ 9 , PbZr_ x Ti_ 1-x O_ 3 ,_ PMN-PT. They were used to clarify the mechanism for some ferroelectric behaviors.

Relaxor ferroelectric and dielectric properties of(1-x)Ba(Zr_(1/3)Ti_(2/3))O_(3)-xBaMg_(0.1)Ta_(0.9))O_(3)ceramics

The environmentally-friendly(1-x)Ba(Zr_(1/3)Ti_(2/3))O_(3)-xBaMg_(0.1)Ta_(0.9))O_(3)(x=0,0.02,0.04,0.06,0.08)relaxor ferroelectric ceramics were prepared by the conventional solid-state method and sintered in air at 1400°C for 2 h.SEM and XRD analyses were utilized to study the surface morphologies and the crystalline structures,respectively.The effects of BaMg_(0.1)Ta_(0.9))O_(3)on the phase transformation,dielectric and ferroelectric properties of Ba(Zr_(1/3)Ti_(2/3))O_(3)ceramics were also investigated.It is found that the average grain size of(1-x)Ba(Zr_(1/3)Ti_(2/3))O_(3)-xBaMg_(0.1)Ta_(0.9))O_(3)(BZT-BMT)perovskite single-phase ceramics decreases as the content of BaMg_(0.1)Ta_(0.9))O_(3)(BMT)increases.The relaxor ferroelectric behavior with diffuse phase transition and well-defined frequency dispersion of dielectric maximum temperature is found for the ceramic with increasing x values.0.98BZT-0.02BMT ceramic shows very good dielectric properties with the relative permittivity and the dielectric loss,measured at 100 k Hz as 6034 and 0.01399 respectively at room temperature.Both remnant polarization and coercive field decreased with increasing BMT content,indicating a transition from the ferroelectric phase to the paraelectric phase at room temperature.

Dielectric and Ferroelectric Properties of Complex Perovskite Ceramics Under Compressive Stress

Dielectric and ferroelectric properties of complex perovskite PZT-PZN ceramic system were investigated under the influence of the compressive stress.The results showed that the dielectric properties,i.e.dielectric constant(ε_r)and dielectric loss(tan δ),and the ferroelectric characteristics,i.e.the area of the ferroelectric hysteresis loops,the saturation polarization(P_ sat),and the remnant polarization(P_r)changed significantly with increasing compressive stress.These changes depended strongly on the ceramic compositions.The experimental results on the dielectric properties could be explained by both intrinsic and extrinsic domain-related mechanisms involving domain wall motions,as well as the de-aging phenomenon.The stress-induced domain wall motion suppression and non-180° ferroelectric domain switching processes were responsible for the changes observed in the ferroelectric parameters.In addition,a significant decrease in those parameters after a cycle of stress was observed and attributed to the stress induced decrease in switchable part of spontaneous polarization.This study clearly show that the applied stress had significant influence on the electrical properties of complex perovskite ceramics.