Ferroelectric Domain Engineering Research Articles

The Creation of a Domain Structure Using Ultrashort Pulse NIR Laser Irradiation in the Bulk of MgO-Doped Lithium Tantalate

The fabrication of stable, tailored domain patterns in ferroelectric crystals has wide applications in optical and electronic industries. All-optical ferroelectric poling by pulse laser irradiation has been developed recently. In this work, we studied the creation of the domain structures in MgO-doped lithium tantalate by focused irradiation with a femtosecond near-infrared laser. Cherenkov-type second harmonic generation microscopy was used for domain imaging of the bulk. We have revealed the creation of enveloped domains around the induced microtracks under the action of the depolarization field. The domain growth is due to a pyroelectric field caused by a nonuniform temperature change. The domains in the bulk were revealed to have a three-ray star-shaped cross-section. It was shown that an increase in the field excess above the threshold leads to consequential changes in domain shape from a three-ray star to a triangular and a circular shape. The appearance of comb-like domains as a result of linear scanning was demonstrated. All effects were considered in terms of a kinetic approach, taking into account the domain wall motion by step generation and kink motion driven by excess of the local field over the threshold. The obtained knowledge is useful for the all-optical methods of domain engineering in ferroelectrics.

All-Optical Domain Inversion in LiNbO3 Crystals by Visible Continuous-Wave Laser Irradiation.

LiNbO3 is a distinguished multifunctional material where ferroelectric domain engineering is of paramount importance. This degree of freedom of the spontaneous polarization remarkably enhances the applicability of LiNbO3, for instance, in photonics. In this work, we report the first method for all-optical domain inversion of LiNbO3 crystals using continuous-wave visible light. While we focus mainly on iron-doped LiNbO3, the applicability of the method is also showcased in undoped congruent LiNbO3. The technique is simple, cheap, and readily accessible. It relies on ubiquitous elements: a light source with low/moderate intensity, basic optics, and a conductive surrounding medium, e.g., water. Light-induced domain inversion is unequivocally demonstrated and characterized by combination of several experimental techniques: selective chemical etching, surface topography profilometry, pyroelectric trapping of charged microparticles, scanning electron microscopy, and 3D Čerenkov microscopy. The influence of light intensity, exposure time, laser spot size, and surrounding medium is thoroughly studied. To explain all-optical domain inversion, we propose a novel physical mechanism based on an anomalous interplay between the bulk photovoltaic effect and external electrostatic screening. Overall, our all-optical method offers straightforward implementation of LiNbO3 ferroelectric domain engineering, potentially sparking new research endeavors aimed at novel optoelectronic applications of photovoltaic LiNbO3 platforms.

High-efficiency nonlinear frequency conversion enabled by optimizing the ferroelectric domain structure in x-cut LNOI ridge waveguide

Abstract Photonic devices based on ferroelectric domain engineering in thin film lithium niobate are key components for both classical and quantum information processing. Periodic poling of ridge waveguide can avoid the selective etching effect of lithium niobate, however, the fabrication of high-quality ferroelectric domain is still a challenge. In this work, we optimized the applied electric field distribution, and rectangular inverted domain structure was obtained in the ridge waveguide which is beneficial for efficient nonlinear frequency conversions. Second harmonic confocal microscope, piezoresponse force microscopy, and chemical selective etching were used to characterize the inverted domain in the ridge waveguide. In addition, the performance of nonlinear frequency conversion of the periodically poled nano-waveguide was investigated through second harmonic generation, and the normalized conversion efficiency was measured to be 1,720 % W−1 cm−2, which is close to 60 % that of the theoretical value. The fabrication technique described in this work will pave the way for the development of high-efficiency, low-loss lithium niobate nonlinear photonic devices.

Engineering the Dielectric Constants of Polymers: From Molecular to Mesoscopic Scales.

Polymers are essential components of modern-day materials and are widely used in various fields. The dielectric constant, a key physical parameter, plays a fundamental role in the light-, electricity-, and magnetism-related applications of polymers, such as dielectric and electrical insulation, battery and photovoltaic fabrication, sensing and electrical contact, and signal transmission and communication. Over the past few decades, numerous efforts have been devoted to engineering the intrinsic dielectric constant of polymers, particularly by tailoring the induced and orientational polarization modes and ferroelectric domain engineering. Investigations into these methods have guided the rational design and on-demand preparation of polymers with desired dielectric constants. This review article exhaustively summarizes the dielectric constant engineering of polymers from molecular to mesoscopic scales, with emphasis on application-driven design and on-demand polymer synthesis rooted in polymer chemistry principles. Additionally, it explores the key polymer applications that can benefit from dielectric constant regulation and outlines the future prospects of this field.

Polar topological superdomain arrays in PMN-PT crystals engineered via a voltage-free method

Domain engineering is an active field of research that aims to enhance the functional properties of ferroelectric materials for various applications. This work presents a voltage-free method for fabricating topological superdomain arrays in 0.72Pb(Mg1/3Nb2/3)O3-0.28PbTiO3 (PMN-28PT) crystals. During the cooling process from high-temperature paraelectric phase to room temperature ferroelectric phase, the out-of-plane polarization of PMN-28PT crystals in contact with aluminum can be fully regulated downward, attributed to the difference in the work function of aluminum and PMN-28PT. In conjunction further with photolithography and ultraviolet light illumination, it is easy to obtain periodic strip domain structures with alternating up and down polarization. Moreover, this method can also control in-plane polarization, resulting in a large-scale central divergent/convergent topological superdomain array. These findings provide insights into ferroelectric domain engineering and have implications for the development of electromechanical, piezoelectronic, and photonic devices.

Pressure Control of Nonferroelastic Ferroelectric Domains in ErMnO3.

Mechanical pressure controls the structural, electric, and magnetic order in solid-state systems, allowing tailoring of their physical properties. A well-established example is ferroelastic ferroelectrics, where the coupling between pressure and the primary symmetry-breaking order parameter enables hysteretic switching of the strain state and ferroelectric domain engineering. Here, we study the pressure-driven response in a nonferroelastic ferroelectric, ErMnO3, where the classical stress-strain coupling is absent and the domain formation is governed by creation-annihilation processes of topological defects. By annealing ErMnO3 polycrystals under variable pressures in the MPa regime, we transform nonferroelastic vortex-like domains into stripe-like domains. The width of the stripe-like domains is determined by the applied pressure as we confirm by three-dimensional phase field simulations, showing that pressure leads to oriented layer-like periodic domains. Our work demonstrates the possibility to utilize mechanical pressure for domain engineering in nonferroelastic ferroelectrics, providing a lever to control their dielectric and piezoelectric responses.

Femtosecond laser writing of lithium niobate ferroelectric nanodomains.

Lithium niobate (LiNbO3) is viewed as a promising material for optical communications and quantum photonic chips1,2. Recent breakthroughs in LiNbO3 nanophotonics have considerably boosted the development of high-speed electro-optic modulators3-5, frequency combs6,7 and broadband spectrometers8. However, the traditional method of electrical poling for ferroelectric domain engineering in optic9-13, acoustic14-17 and electronic applications18,19 is limited to two-dimensional space and micrometre-scale resolution. Here we demonstrate a non-reciprocal near-infrared laser-writing technique for reconfigurable three-dimensional ferroelectric domain engineering in LiNbO3 with nanoscale resolution. The proposed method is based on a laser-induced electric field that can either write or erase domain structures in the crystal, depending on the laser-writing direction. This approach offers a pathway for controllable nanoscale domain engineering in LiNbO3 and other transparent ferroelectric crystals, which has potential applications in high-efficiency frequency mixing20,21, high-frequency acoustic resonators14-17 and high-capacity non-volatile ferroelectric memory19,22.

Domain Engineering in Bulk Ferroelectric Ceramics via Mesoscopic Chemical Inhomogeneity.

Domain engineering in ferroelectrics endows flexibility for different functional applications. Whereas the domain engineering strategy for single crystals and thin films is diverse, there is only a limited number of strategies for bulk ceramics. Here, a domain engineering strategy for achieving a compact domain architecture with increased domain‐wall density in (K,Na)NbO3 (KNN)‐based ferroelectric ceramics via mesoscopic chemical inhomogeneity (MCI) is developed. The MCI‐induced interfaces can effectively hinder domain continuity and modify the domain configuration. Besides, the MCI effect also results in diffused phase transitions, which is beneficial for achieving enhanced thermal stability. Modulation of chemical inhomogeneity demonstrates great potential for engineering desirable domain configuration and properties in ferroelectric ceramics. Additionally, the MCI can be easily controlled by regulating the processing condition during solid‐state synthesis, which is advantageous to industrial production.

Ultra-broadband quadrature squeezing with thin-film lithium niobate nanophotonics

Squeezed light is a key quantum resource that enables quantum advantages for sensing, networking, and computing applications. The scalable generation and manipulation of squeezed light with integrated platforms are highly desired for the development of quantum technology with continuous variables. In this Letter, we demonstrate squeezed light generation with thin-film lithium niobate integrated photonics. Parametric down-conversion is realized with quasi-phase matching using ferroelectric domain engineering. With sub-wavelength mode confinement, efficient nonlinear processes can be observed with single-pass configuration. We measure 0.56 ± 0.09 dB quadrature squeezing (∼2.6 dB inferred on-chip). The single-pass configuration further enables the generation of squeezed light with large spectral bandwidth up to 7 THz. This work represents a significant step towards the on-chip implementation of continuous-variable quantum information processing.

Ferroelectric domain modulated AlGaN/GaN field effect transistor

A two-dimensional electron gas (2DEG) in (Al, Ga) N/GaN heterojunction (AlGaN/GaN) is a key factor that affects the performance of GaN-based high electron mobility transistor (HEMT) devices. Previous studies have shown that the ferroelectric polarization can effectively control the density of the 2DEG at the AlGaN/GaN interface; however, the correlation between two-dimensional distribution of ferroelectric polarization (i.e., ferroelectric domains) and its ability to confine the 2DEG is yet to be investigated. In this work, ferroelectric domain-induced modulation of the 2DEG in the AlGaN/GaN heterostructure was characterized using microscopic as well as local transport measurement techniques. The results suggest direct evidence for effective ferroelectric domain engineering in GaN HEMTs, as predicted by theoretical calculations. Additionally, a prototype device was fabricated, where gating was realized by utilizing the polarization of the ferroelectric domain. Considering the nonvolatile and reconfigurable advantages of a ferroelectric domain, the E-mode, D-mode, and even multi-channel output characteristics were realized in the same device by artificially engineered ferroelectric domain structures. These results offer a promising solution for the contradiction between the 2DEG density and gate controllability in GaN HEMTs, thereby showing a great potential of GaN radio frequency devices with further scaled gate lengths down to a few nanometers in the future.

A critical field study of ferroelectric domain in Al-doped KNbO3 single crystal

-Ferroelectric domain engineering is important for studying the dipolar structure of these materials. This dipolar structure is formed because of defects and imperfections produced using various doping. The KNbO3 ferroelectric single crystal was prepared using flux methods. Al2O3 aluminum trioxide (Al) was used as a dopant in a KNbO3 crystal. The domain structure of the crystal was studied by applying electric fields of 50 V/cm, 60 V/cm, 70 V/cm, 80V/cm, and 100 V/cm in an Al-doped KNbO3 single crystal. Furthermore, the critical field on which domains were nucleated after applying the electric field, was also studied. This work confirmed that the critical field of nucleation of the new domain in an Al-doped KNbO3 single crystal was 70 V/cm, which is slightly less than that of pure KNbO3 single crystal.

Conductive Domain-Wall Temperature Sensors of LiNbO3 Ferroelectric Single-Crystal Thin Films

Domain wall current (DWC) plays a key role in storage devices, logic devices and sensors due to its high on-off ratio and nano structure size in the era of nanoelectronics technology. In this work, the DWC of single crystal LiNbO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> thin film was studied by piezoresponse force microscope (PFM) and conducting atomic force microscope (c-AFM). We mainly focus on voltage and temperature dependence of DWC which increases with the voltage and temperatures. Based on this research, the packaged DWC temperature sensor is fabricated and applied in wide temperature range. The existence of domain walls makes the current on-off ratio as high as 10 <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sup> at the voltage of 15 V. Our study shows that DWC has a negative temperature coefficient (NTC) from 140 K to 500 K. The current increases from 3 pA to <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$57 ~\mu \text{A}$ </tex-math></inline-formula> , which is attributed to the conductivity of switched domain. This work proposes a new type temperature sensor with wide temperature range and high compatibility and sensitivity. In addition, it provides support for harsh environment applications of ferroelectric domain engineering devices.

Reporting Excellent Transverse Piezoelectric and Electro‐Optic Effects in Transparent Rhombohedral PMN‐PT Single Crystal by Engineered Domains

Transparent ferroelectric crystals with high piezoelectricity are challenging to build because of their complex structure and disordered domains in rhombohedral relaxor ferroelectrics. There are eight domains along the <111> direction, which cause light scattering. In this study, perfect transparency is achieved along the [110] and [001] directions in [110]-poled rhombohedral 0.72Pb(Mg1/3 Nb2/3 )O3 -0.28PbTiO3 (PMN-PT) crystals, which have a high d31 value of 1700 pC N-1 and a high electro-optic coefficient γ33 of 320 pm V-1 . This implies that the [110]-oriented rhombohedral PMN-0.28PT crystal can realize the mode of transverse modulation, whereas the [001]-oriented PMN-0.28PT crystal is more suitable for the longitudinal mode. Through piezoresponse force microscopy (PFM), it is confirmed that the [110]-poled rhombohedral PMN-PT crystals form 71° layered domains, which are similar to the 109° layered domains of the [001]-oriented transparent crystal. Combined with PFM and birefringence microscopy, the degradation of domains and thickness dependence of piezoelectricity provide clear evidence for the relationship between the engineered domain structures and piezoelectric properties, which should be considered in the design of piezoelectric or electro-optic devices with excellent performance. This work enriches the research on ferroelectric domain engineering for excellent transparency and high piezoelectricity to provide new ideas for photoacoustic devices.

Ferroelectric domain structure of Bi2FeCrO6 multiferroic thin films

Bi2FeCrO6 (BFCO) multiferroic thin films were deposited on SrRuO3(SRO)/SrTiO3(STO) (001) and STO (001) substrates by a pulsed laser deposition method. High-quality epitaxial BFCO thin films with a typical step-flow surface morphology were successfully prepared. X-ray diffraction reveals that the high phase-purity epitaxial BFCO films with good crystallinity are obtained. Using both piezoelectric force microscopy (PFM) and x-ray reciprocal space mapping, we studied the ferroelectric domain structure and ferroelectricity characterization of BFCO thin films with and without an SRO buffer layer. The ferroelectric domain structure of an epitaxial BFCO film deposited on SRO/STO (001) is characterized by eight polarization variants. However, the ferroelectric domain structure of the epitaxial BFCO film directly grown on the STO (001) substrate is degenerate from eight polarization variants to four or even two. The feasibility of ferroelectric domain engineering is demonstrated by growing BFCO films on STO (001) with and without SRO buffer layers.

Regulation of phase transition and magnetocaloric effect by ferroelectric domains in FeRh/PMN-PT heterojunctions

The narrow temperature span, ΔTspan, of first-order magnetocaloric materials is a serious problem that limits the application as refrigerants. Here we report tunable phase transition and magnetocaloric effect controlled by ferroelectric (FE) domains in FeRh films grown on (001)- and (011)-cut PMN-PT substrates. Adjacent two-step phase transition, and hence significantly broadened ΔTspan, has been achieved in FeRh films by utilizing the multi-domain structure of PMN-PT substrates. The results of aberration corrected (ac)-STEM, EELS and EDX analysis revealed that a 3~4 nm buffer layer with AB2O4-type spinel structure is naturally formed at the interface, which largely reduces the lattice mismatch between FeRh and PMN-PT and plays a key role for the successful growth of epitaxial (oriented) FeRh film on either (001)- or (011)-oriented PMN-PT. The switched FE domains by electric field govern the phase transition of FeRh films. As a result, regulated entropy change and refrigeration capacity in a wide temperature span have been achieved. On this basis, a feasible magnetic refrigeration cycle facilitated by electric field is designed. The present study provides an experimental basis for expanding the refrigeration temperature span by ferroelectric domain engineering, which is significant for promoting refrigeration application of first-order magnetocaloric materials particularly in micro-devices.

Transparent ferroelectric crystals with ultrahigh piezoelectricity.

Transparent piezoelectrics are highly desirable for numerous hybrid ultrasound-optical devices ranging from photoacoustic imaging transducers to transparent actuators for haptic applications1-7. However, it is challenging to achieve high piezoelectricity and perfect transparency simultaneously because most high-performance piezoelectrics are ferroelectrics that contain high-density light-scattering domain walls. Here, through a combination of phase-field simulations and experiments, we demonstrate a relatively simple method of using an alternating-current electric field to engineer the domain structures of originally opaque rhombohedral Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) crystals to simultaneously generate near-perfect transparency, an ultrahigh piezoelectric coefficient d33 (greater than 2,100picocoulombs per newton), an excellent electromechanical coupling factor k33 (about 94 per cent) and a large electro-optical coefficient γ33 (approximately 220picometres per volt), which is far beyond the performance of the commonly used transparent ferroelectric crystal LiNbO3. We find that increasing the domain size leads to a higher d33 value for the [001]-oriented rhombohedral PMN-PT crystals, challenging the conventional wisdom that decreasing the domain size always results in higher piezoelectricity8-10. This work presents a paradigm for achieving high transparency and piezoelectricity by ferroelectricdomain engineering, and we expect the transparent ferroelectric crystals reported here to provide a route to a wide range of hybrid device applications, such as medical imaging, self-energy-harvesting touch screens and invisible robotic devices.

Tip-induced domain growth in the non-polar cuts of SBN:Ce single crystals

The local switching by conductive tip of scanning probe microscope was studied in the non-polar cuts of Ce-doped Sr0.61Ba0.39Nb2O6 single crystals after creation of the single-domain state. The switched domains possessed the egg-shaped heads and wedge-like tails. The dependences of lengths of the domain head and tail and width of the domain head on the voltage and pulse duration were derived. The start voltage for growth of the domain tail was revealed. The fast relaxation of the domain head and slow relaxation of the domain tail were observed. The model of the forward domain growth by step generation and kink motion was used for explanation of the experimental results. The obtained knowledge can be used for the domain engineering in ferroelectrics.

Ferroelectric domain engineering of lithium niobate single crystal confined in glass

Abstract

Realization of rhombohedral, mixed, and tetragonal like phases of BiFeO3 and ferroelectric domain engineering using a strain tuning layer on LaAlO3(001) substrate

BiFeO3 (BFO), a room temperature multiferroic, undergoes a series of structural transformations under varying strain conditions by utilizing appropriate substrates for a specific strain condition. In this study, epitaxial thin films of BFO were grown on La0.7Sr0.3MnO3±δ (LSMO), a strain tuning layer on LaAlO3[LAO (001)] substrates, using pulsed laser ablation. LSMO layers of varying thicknesses from 2 nm to 20 nm were grown followed by a BFO layer of a fixed thickness (20 nm). A strained layer of ∼2 nm thick LSMO stabilizes the tetragonal like phase of BFO. Increasing the thickness of the LSMO layer to 10 nm results in a mixed phase with rhombohedral (R) and tetragonal (T) domains, and a further increment of the LSMO layer thickness to 20 nm stabilizes the rhombohedral phase of BFO. The tetragonal phase with weak monoclinic distortion possessed 180° domains with dominant out-of-plane polarization components. However, the mixed phase (R + T) possessed various plausible polarization components in both out-of-plane and in-plane directions. Further, a thermodynamically consistent model based on the phase field approach was implemented to investigate the role of strain on the formation of domain patterns with various polarization components and piezoelectric coefficients. The simulated domain structure exhibited a similar transformation on the dominant polarization components as observed in experiments across different phases of BFO. Our simulations show that the elastic constraint along the z-direction enhances the tetragonality of BFO. The piezoelectric (d33) coefficient was found to be ∼46 pm/V for the 20 nm mixed phase BFO, which was nearly a 200% increment compared to the single phase BFO thin films on LAO.

Local switching in SBN:Ni single crystals with various initial domain states

ABSTRACTWe present the results of experimental study of the local switching in single crystals of relaxor ferroelectric Ni-doped strontium barium niobate with various initial domain states using conductive tip of scanning probe microscope. We investigated the domain growth in as-grown domain structure and initial domain states created by: (i) scanning by biased tip, (ii) in-field cooling, and (iii) scanning by electron beam. The dependences of effective domain radius on the voltage and pulse duration were derived. The shape factor, domain wall mobility, and start voltage were revealed. The obtained results can be used for the domain engineering in ferroelectrics.