Noncolinear Second-Harmonic Generation Pairs and Their Scatterings in Nd3+:SBN Crystals with Needle-Like Ferroelectric Domains

Second-harmonic generation in Nd3＋ ：SBN crystal with needle-like ferroelectric with aperiodic domain structures is investigated. Two pairs of second harmonic （SH） waves appearing in lines are observed in unpoled Nd3＋ ：SBN crystals with aperiodic needle-like domains. A pair of SH waves emit from the exit face, whose intensities are angle-dependent. The angular dependence is corresponding to the spatial frequency spectrum of the aperiodic domain structure. Another pair of SH waves emit from both the side surfaces, which are mainly the scattered SH waves by needle-like domain walls and obey the theory of Rayleigh scattering.

Polarization-dependent optical engineering of ferroelectric domains

Ferroelectric domain engineering with infrared femtosecond laser pulses has been a powerful technique to achieve a spatially modulated second-order nonlinear coefficient in three dimensions.However,studies regarding the in-fluence of laser writing conditions on the light-induced ferroelectric domain inversion remain limited.Herein,an experimental study to reveal the role of laser polarization in light-induced domain inversions is discussed.The dependence of the optical threshold and maximal writing depth of inverted domains on light polarization is ex-perimentally investigated.The results are explained by considering the second-order nonlinear optical properties and birefringence-induced focus splitting in the crystal.These findings are useful in fabricating high-quality and large-scale ferroelectric domain structures for applications in optics,electronics,and quantum technologies.

Imaging ferroelectric domains via charge gradient microscopy enhanced by principal component analysis

Local domain structures of ferroelectrics have been studied extensively using various modes of scanning probes at the nanoscale,including piezoresponse force microscopy(PFM)and Kelvin probe force microscopy(KPFM),though none of these techniques measure the polarization directly,and the fast formation kinetics of domains and screening charges cannot be captured by these quasi-static measurements.In this study,we used charge gradient microscopy(CGM)to image ferroelectric domains of lithium niobate based on current measured during fast scanning,and applied principal component analysis(PCA)to enhance the signal-to-noise ratio of noisy raw data.We found that the CGM signal increases linearly with the scan speed while decreases with the temperature under power-law,consistent with proposed imaging mechanisms of scraping and refilling of surface charges within domains,and polarization change across domain wall.We then,based on CGM mappings,estimated the spontaneous polarization and the density of surface charges with order of magnitude agreement with literature data.The study demonstrates that PCA is a powerful method in imaging analysis of scanning probe microscopy(SPM),with which quantitative analysis of noisy raw data becomes possible.

Shape-induced phase transition of vortex domain structures in ferroelectric nanodots and their controllability by electrical and mechanical loads

Shape-induced phase transition of vortex domain structures （VDSs） in BaTiO3 （BT） nanodots under open circuit boundary condition have been investigated using an effective Hamiltonian method. Our calculation indicates the tetragonal VDS missing in cubic BT nanodots can be induced by varying the shape of a nanodot from cube to platelet. Interestingly, a novel VDS is found in BT nanoplatelets in our simulations. Further investigation shows that it is a result of compromise between the ground state and the symmetry of the shape of the nanodot. Furthermore, based on the novel VDS, routes of controlling VDSs governed by homogeneous electric field and uniform stress are discussed. In particular, our results show the possibility of designing multi-states devices based on a single VDS. ~ 2017 The Authors. Published by Elsevier Ltd on behalf of The Chinese Society of Theoretical and Applied Mechanics.

Effect of electric boundary conditions on crack propagation in ferroelectric ceramics

In this paper, the effect of electric boundary conditions on Mode I crack propagation in ferroelectric ceramics is studied by using both linear and nonlinear piezoelectric fracture mechanics. In linear analysis, impermeable cracks under open circuit and short circuit are analyzed using the Stroh formalism and a rescaling method. It is shown that the energy release rate in short circuit is larger than that in open circuit. In nonlinear analysis, permeable crack conditions are used and the nonlinear effect of domain switching near a crack tip is considered using an energy-based switching criterion proposed by Hwang et al.（Acta Metal. Mater.,1995）. In open circuit, a large depolarization field induced by domain switching makes switching much more diffcult than that in short circuit. Analysis shows that the energy release rate in short circuit is still larger than that in open circuit, and is also larger than the linear result. Consequently,whether using linear or nonlinear fracture analysis, a crack is found easier to propagate in short circuit than in open circuit, which is consistent with the experimental observations of Kounga Njiwa et al.（Eng. Fract. Mech., 2006）.

Two new high-temperature molecular ferroelectrics[1,5-3.2.2-Hdabcn]X(X=ClO_(4)^(-),ReO_(4)^(-))

Molecular ferroelectrics have attracted much attention because of their excellent piezoelectricity,mechanical workability,and second harmonic effect.Here,we successfully prepared two molecular ferroelectrics[1,5-3.2.2-Hdabcn]X(X=ClO_(4)^(-),1;ReO_(4)^(-),2)by reactions of a quasi-spherical amine 1,5-diazabicycle[3.2.2]nonane(1.5-3.2.2-dabcn)with HX aqueous solution.Compounds 1 and 2 undergo hightemperature phase transitions at 381 K(1)and 396 K(2).Before and after the phase transition,they crystallize in the polar point group mm2,and the centrosymmetric point groups mmm and 4/mmm,respectively.According to Aizu rules,these two compounds experience mmm Fmm2 and 4/mmm Fmm2 type ferroelectric phase transitions,respectively.The ferroelectricity of both compounds is well expressed in their polycrystalline film at room temperature with low coercive voltages of 13 V for 1 and 25 V for 2.Using piezoelectric force microscopy(PFM),the 180°anti-parallel ferroelectric domains and the reversible polarization switching can be clearly observed in 1 and 2.This high-temperature molecular ferroelectric material has great application potential in flexible materials,biomechanics,intelligent wearables and other fields.

An unconventional phase field modeling of domains formation and evolution in tetragonal ferroelectrics

Based on characteristic functions of variants, we developed an unconventional phase field modeling for investigating domains formation and evolution in tetragonal ferroelectrics. In order to develop this computational approach, we constructed the anisotropy energy of tetragonal variants, which is used instead of Landau-Devonshire potential in the conventional phase field method, resulting in that much fewer parameters are needed for simulations. This approach is advantageous in simulations of emerging ferroelectric materials. We employ it to study the formation and evolution of domains in tetragonal barium titanate single crystal, as well as the nonlinear behaviors under cyclical stress and electric field loading. A multi-rank laminated ferroelectric domain pattern, 90° domain switching accompanied by polarization rotation, and 180° domain switching accompanied by move of domain wall are predicted. It is found that the speed of 90° domain switching is slower than that of 180° domain switching, due to both polarization and transformation strain changed in 90° domain switching. It also suggests that large strain actuation can be generated in single crystal ferroelectrics via combined electromechanical loading inducing 90° domain switching. The good agreement between simulation results and experimental measurements is observed.

HfAlO-based ferroelectric memristors for artificial synaptic plasticity

Memristors have received much attention for their ability to achieve multi-level storage and synaptic learning.However,the main factor that hinders the application of memristors to simulate neural synapses is the instability of the formation and breakage of conductive filaments inside traditional memristors,which makes it difficult to simulate the function of biological synapses in practice.However,the resistance change of ferroelectric memristors relies on the polarization inversion of the ferroelectric thin film,thus avoiding the above problem.In this study,a Pd/HfAlO/LSMO/STO/Si ferroelectric memristor is proposed,which can achieve resistive switching properties through the combined action of ferroelectricity and oxygen vacancies.The I−V curves show that the device has good stability and uniformity.In addition,the effect of pulse sequence modulation on the conductance was investigated,and the biological synaptic function and learning behavior were simulated successfully.The results of the above studies provide a basis for the development of ferroelectric memristors with neurosynaptic-like behaviors.

On ferroelectric domain polarization switching mechanism subject to an external electric field by simulations with the phase-field method

The ferroelectric domain formation(FDF) and polarization switching(FDPS) subjected to an external electric field are simulated using the phase-field(PF) method,and the FDPS mechanism under different external electric fields is discussed.The results show that the FDF is a process of nucleation and growth in ferroelectric without applying any external stress.Four kinds of parallelogram shaped ferroelectric domains are formed at the steady state,in which the 180° anti-phase domains regularly align along the 45° direction and the 90° anti-phase domains regularly distribute like a stepladder.Steady electric fields can rotate domain polarization by 90° and 180°,and force the orientation-favorite domains and the average polarization to grow into larger ones.The greater the steady electric field,the larger the average polarization at the steady state.In ferroelectrics subject to an alternating electric field,domain polarization switches to cause a hysteresis loop and an associated butterfly loop with the alternating electric field.The coercive field and remnant field are enhanced with the increase of the electric field frequency or strength,or with the decrease of temperature.

The temperature-dependent domains,SHG effect and piezoelectric coefficient of TGS

The temperature-dependent,second-order,nonlinear,optical coefficient（x^（（2）））.piezoelectric coefficient （d_（33））,pyroelectric coefficient（Ps） and domains on triglycine sulfate（TGS） reported herein provide a clue for us to investigate these as a typical second-order phase transition.The symmetry breaking occurrence is definitely confirmed by the temperature-dependent x^（（2）） in which x^（（2）） displays a limited value at the ferroelectric phase,indicating the space group（P2_1） chosen is correct,and when x^（（2）） basically maintains a zero value at the paraelectric phase,indicating the space group should be centric.Interestingly,after normalization of x^（（2））,d_（33） or Ps,the change trend with temperature is basically overlapped,probably abiding by Landau theory.Moreover,temperature-dependent domains directly show the symmetry breaking occurrence.

La_(2)O_(3)-modified BiYbO_(3)–Pb(Zr,Ti)O_(3) ternary piezoelectric ceramics with enhanced electrical properties and thermal depolarization temperature

High-performance Pb(Zr_(1−x)Ti_(x))O_(3)(PZT)piezoceramics are urgently desired by the market in view of their expanded operating temperature range,reduced property temperature dependence,and enhanced sensitivity and acoustic power.In this work,we reported a kind of low-cost and high-performance 0.06BiYbO_(3)–0.94Pb(Zr_(0.48)Ti_(0.52))O_(3) ternary piezoceramics;the modifying effects of La_(2)O_(3) on this perovskite system were investigated in terms of the structures,electrical properties,and thermal depolarization behaviors of ceramics.The field-dependent dielectric and conduction properties indicated that there are close correlations among oxygen vacancies(VO),conducting electrons,and intrinsic conduction process.The degradation in ferroelectric properties observed in those samples doped with more than 0.15 wt%of La_(2)O_(3) indicated that the occupying mechanisms of La^(3+)changed from the donor substitution for Pb^(2+)to the isovalent substitution for Bi^(3+).The thermally depoling micromechanisms of ceramics were revealed from the thermodynamic processes of defect dipoles and intrinsic dipoles within ferroelectric domains.The sample doped with 0.15 wt%of La_(2)O_(3) shows excellent electrical properties with TC=387℃,d33=332 pC/N,TKε=5.81×10^(−3)℃−1,Pr=20.66μC/cm^(2),Td=356℃.The significantly enhanced electrical properties and thermal depolarization temperature benefited from the donor substitution of La3+,decreasing the oxygen vacancy concentration in the lattice and possibly optimizing the ferroelectric domain structure of ceramics.

Determination of polarization states in(K,Na)NbO3 lead-free piezoelectric crystal

Polarization switching in lead-free(K0.40Na0.60)NbO3(KNN)single crystals was studied by switching spectroscopy piezoresponse force microscopy(SS-PFM).Acquisition of multiple hysteresis loops on a closely spaced square grid enables polarization switching parameters to be mapped in real space.Piezoresponse amplitude and phase hysteresis loops show collective symmetric/asymmetric characteristics,affording information regarding the switching behavior of different domains.As such,the out-of-plane polarization states of the domains,including amplitudes and phases can be determined.Our results could contribute to a further understanding of the relationships between polarization switching and polarization vectors at the nanoscale,and provide a feasible method to correlate the polarization hysteresis loops in a domain under an electric field with the polarization vector states.

Locally periodically poled LNOI ridge waveguide for second harmonic generation [Invited]

Periodically poled lithium niobate on insulator(LNOI) ridge waveguides are desirable for high-efficiency nonlinear frequency conversions, and the fabrication process of such waveguides is crucial for device performance. In this work, we report fabrication and characterization of locally periodically poled ridge waveguides. Ridge waveguides were fabricated by dry etching, and then the high-voltage pulses were applied to locally poled ridge waveguides. Second harmonic generation with normalized conversion efficiency of 435.5% W^(-1)·cm^(-2) was obtained in the periodically poled LNOI ridge waveguide,which was consistent with the triangular domain structure revealed by confocal microscopy.

Effect of mechanical force on domain switching in BiFeO3 ultrathin films

Ferroelectric polarization can be switched by an external applied electric field and may also be reversed by a mechanical force via flexoelectricity from the strain gradient.In this study,we report the mechanical writing of an epitaxial BiFeO3(BFO)thin film and the combined action of an applied mechanical force and electric field on domain switching,where the mechanical force and electric field are applied using the tip of atomic force microscopy.When the applied force exceeds the threshold value,the upward polarization of the BFO thin film can be reversed by pure mechanical force via flexoelectricity;when an electric field is simultaneously applied,the mechanical force can reduce the coercive electric field because both the piezoelectricity from the homogeneous strain and the flexoelectricity from strain gradient contribute to the internal electric field in the film.The mechanically switched domains exhibit a slightly lower surface potential when compared with that exhibited by the electrically switched domains due to no charge injection in the mechanical method.Furthermore,both the mechanically and electrically switched domains exhibit a tunneling electroresistance in the BFO ferroelectric tunnel junction.