Polarization Switching Behavior Research Articles

Optical Modulation of MoTe2/Ferroelectric Heterostructure via Interface Doping.

Optical modulation through interface doping offers a convenient and efficient way to control ferroelectric polarization, thereby advancing the utilization of ferroelectric heterostructures in nanoelectronic and optoelectronic devices. In this work, we fabricated heterostructures of MoTe2/BaTiO3/La0.7Sr0.3MnO3 (MoTe2/BTO/LSMO) and demonstrated opposite ultraviolet (UV) light-induced polarization switching behaviors depending on the varied thicknesses of MoTe2. The thickness-dependent band structure of MoTe2 film results in interface doping with opposite polarity in the respective heterostructures. The polarization field of BTO interacts with the interface charges, and an enhanced effective built-in field (Ebi) can trigger the transfer of massive UV light-induced carriers in both MoTe2 and BTO films. As a result, the interplay among the contact field of MoTe2/BTO, the polarization field, and the optically excited carriers determines the UV light-induced polarization switching behavior of the heterostructures. In addition, the electric transport characteristics of MoTe2/BTO/LSMO heterostructures reveal the interface barrier height and Ebi under opposite polarization states, as well as the presence of inherent in-gap trap states in MoTe2 and BTO films. These findings represent a further step toward achieving multifield modulation of the ferroelectric polarization and promote the potential applications in optoelectronic, logic, memory, and synaptic ferroelectric devices.

Polarization switching pathways of ferroelectric Zr-doped HfO2 based on the first-principles calculation

Based on the first principles calculation, the mechanisms of polarization switching behavior in ferroelectric Zr-doped HfO2 are investigated. Seven switching pathways, divided into two categories by the identified orientation of polarization switching and value, are analyzed based on atomic migration and energy barrier. The effects of Zr dopant on switching energy barrier (Eb) and spontaneous polarization (Ps) are analyzed as well. In one of the categories, two pathways with tetragonal-like transition states show low energy barriers and can be further minimized with higher Zr dopant proportion, which originates from the stabilizing effect of Zr dopant on the tetragonal phase (T, P42/nmc). Especially, in the two tetragonal-like pathways, a distorted tetragonal-like transient state (T′, Pbcn) resulting from distinct atomic displacement is transformed to a highly symmetric T-phase along with the incorporation of Zr, elucidating this pathway as energy favorable as the regular T-pathway. This work provides an atomic insight for ferroelectric switching behavior and predicts the probable ferroelectric switching pathway in Zr-doped HfO2 films.

Terahertz bi-functional polarization converter based on interference mechanism supported by diatomic metasurfaces

Polarization manipulation based on the Jones matrix facilitates the enhancement of light-matter interactions. Recently, arbitrarily tailorable polarization states generated with the assistance of a diatomic metasurface effectively reduce the complexity of the system. Nevertheless, a single polarization switching behavior hinders the application of meta-platforms in cryptographic imaging. Here, we theoretically propose and design a single-layer diatomic all-dielectric metasurface working in the terahertz band, which can efficiently realize bi-functional polarization switching according to the Jones matrix. Such a meta-platform is assembled from two anisotropic silicon pillars with carefully optimized lateral dimensions and in-plane twist angles. Benefiting from the flexible assembly of half-wave plate and quarter-wave plate, the polarization states generated by the constructed metasurfaces in the transmission mode can be arbitrarily tailored. The feasibility of this diatomic metasurface is further validated by a broadband near-field imaging device, paving the way for broader system applications in cryptographic imaging, data storage, and chiral sensing.

Electrically induced cancellation and inversion of piezoelectricity in ferroelectric Hf0.5Zr0.5O2

HfO2-based thin films hold huge promise for integrated devices as they show full compatibility with semiconductor technologies and robust ferroelectric properties at nanometer scale. While their polarization switching behavior has been widely investigated, their electromechanical response received much less attention so far. Here, we demonstrate that piezoelectricity in Hf0.5Zr0.5O2 ferroelectric capacitors is not an invariable property but, in fact, can be intrinsically changed by electrical field cycling. Hf0.5Zr0.5O2 capacitors subjected to ac cycling undergo a continuous transition from a positive effective piezoelectric coefficient d33 in the pristine state to a fully inverted negative d33 state, while, in parallel, the polarization monotonically increases. Not only can the sign of d33 be uniformly inverted in the whole capacitor volume, but also, with proper ac training, the net effective piezoresponse can be nullified while the polarization is kept fully switchable. Moreover, the local piezoresponse force microscopy signal also gradually goes through the zero value upon ac cycling. Density functional theory calculations suggest that the observed behavior is a result of a structural transformation from a weakly-developed polar orthorhombic phase towards a well-developed polar orthorhombic phase. The calculations also suggest the possible occurrence of a non-piezoelectric ferroelectric Hf0.5Zr0.5O2. Our experimental findings create an unprecedented potential for tuning the electromechanical functionality of ferroelectric HfO2-based devices.

A physics-based predictive model for pulse design to realize high-performance memristive neural networks

Memristive neural networks have extensively been investigated for their capability in handling various artificial intelligence tasks. The training performance of memristive neural networks depends on the pulse scheme applied to the constituent memristors. However, the design of the pulse scheme in most previous studies was approached in an empirical manner or through a trial-and-error method. Here, we choose ferroelectric tunnel junction (FTJ) as a model memristor and demonstrate a physics-based predictive model for the pulse design to achieve high training performance. This predictive model comprises a physical model for FTJ that can adequately describe the polarization switching and memristive switching behaviors of the FTJ and an FTJ-based neural network that uses the long-term potentiation (LTP)/long-term depression (LTD) characteristics of the FTJ for the weight update. Simulation results based on the predictive model demonstrate that the LTP/LTD characteristics with a good trade-off between ON/OFF ratio, nonlinearity, and asymmetry can lead to high training accuracies for the FTJ-based neural network. Moreover, it is revealed that an amplitude-increasing pulse scheme may be the most favorable pulse scheme as it offers the widest ranges of pulse amplitudes and widths for achieving high accuracies. This study may provide useful guidance for the pulse design in the experimental development of high-performance memristive neural networks.

In Situ Observation of Domain Wall Lateral Creeping in a Ferroelectric Capacitor

AbstractAs a promising candidate for next‐generation nonvolatile memory devices, ferroelectric oxide films exhibit many emergent phenomena with functional applications, making understanding polarization switching and domain evolution behaviors of fundamental importance. However, tracking domain wall motion in ferroelectric oxide films with high spatial resolution remains challenging. Here, an in situ biasing approach for direct atomic‐scale observations of domain nucleation and sideways motion is presented. By accurately controlling the applied electric field, the lateral translational speed of the domain wall can decrease to less than 2.2 Å s−1, which is observable with atomic resolution STEM imaging. In situ observations on a capacitor structured PbZr0.1Ti0.9O3/La0.7Sr0.3MnO3 heterojunction demonstrate the unique creeping behavior of a domain wall under a critical electric field, with the atomic structure of the creeping domain wall revealed. Moreover, the evolution of the metastable domain wall forms an elongated morphology, which contains a large proportion of charged segments. Phase‐field simulations unveil the competition between gradient, elastic, and electrostatic energies that decide this unique domain wall creeping and morphology variation. This work paves the way toward a complete fundamental understanding of domain wall physics and potential modulations of domain wall properties in real devices.

Features of spontaneous ferroelectric domain nucleation in Ti:LiNbO3 modulators

Integrated optical modulators based on lithium niobate Ti-indiffused waveguides (Ti:LiNbO3) are used extensively for broadband devices that have a high coupling efficiency with optical fibers at a 1.5 μm wavelength window. However, the ferroelectric nature of lithium niobate crystal results in some undesirable effects causing parameters fluctuations. For example, the pyroelectric effect leads to thermal dependent DC-drift and excess optical losses. Therefore, to develop effective compensation methods, it is important to understand the origin of instability. In the interelectrode gap of phase modulators we found needle-like domain defects with switched polarization along a surface layer of the monodomain X-cut lithium niobate substrate. Based on domain nucleation theory and polarization switching behavior, the spontaneous nature of domain nucleation caused by the pyroelectric field was shown and described for the interelectrode gap of the modulator along electrode edges. Considering the corona effect, models of domain nucleation and growth are proposed, and the morphology of needle-like domains is describes based on numerical simulation of the pyroelectric field distribution in the crystal volume. Experimental studies of industrial optical phase modulators characterize the shape and size of domains not only in the interelectrode gap, but also along the boundary of external electrodes proving the pyroelectric type of domain nucleation. Several methods were used for domain visualization-selective chemical etching, piezoresponse force microscopy, and electron scanning microscopy. The present work provides a theoretical and practical basis for future research on stabilization of the parameters for optical phase modulators.

Spin polarization gate device based on the chirality-induced spin selectivity and robust nonlocal spin polarization.

Nonlocal spin polarization phenomena are thoroughly investigated in the devices made of chiral metallic single crystals of CrNb3S6 and NbSi2 as well as of polycrystalline NbSi2. We demonstrate that simultaneous injection of charge currents in the opposite ends of the device with the nonlocal setup induces the switching behavior of spin polarization in a controllable manner. Such a nonlocal spin polarization appears regardless of the difference in the materials and device dimensions, implying that the current injection in the nonlocal configuration splits spin-dependent chemical potentials throughout the chiral crystal even though the current is injected into only a part of the crystal. We show that the proposed model of the spin dependent chemical potentials explains the experimental data successfully. The nonlocal double-injection device may offer significant potential to control the spin polarization to large areas because of the nature of long-range nonlocal spin polarization in chiral materials.

Defect-Induced, Ferroelectric-Like Switching and Adjustable Dielectric Tunability in Antiferroelectrics.

Antiferroelectrics, which undergo a field-induced phase transition to ferroelectric order that manifests as double-hysteresis polarization switching, exhibit great potential for dielectric, electromechanical, and electrothermal applications. Compared to their ferroelectric cousins, however, considerably fewer efforts have been made to understand and control antiferroelectrics. Here, it is demonstrated that the polarization switching behavior of an antiferroelectric can be strongly influenced and effectively regulated by point defects. In films of the canonical antiferroelectric PbZrO3 , decreasing oxygen pressure during deposition (and thus increasing adatom kinetic energy) causes unexpected "ferroelectric-like" polarization switching although the films remain in the expected antiferroelectric orthorhombic phase. This "ferroelectric-like" switching is correlated with the creation of bombardment-induced point-defect complexes which pin the antiferroelectric-ferroelectric phase boundaries, and thus effectively delay the phase transition under changing field. The effective pinning energy is extracted via temperature-dependent switching-kinetics studies. In turn, by controlling the concentration of defect complexes, the dielectric tunability of the PbZrO3 can be adjusted, including being able to convert between "positive" and "negative" tunability near zero field. This work reveals the important role and strong capability of defects to engineer antiferroelectrics for new performance and functionalities.

Insight into the evolutions of microstructure and performance in bismuth ferrite modified potassium sodium niobate lead-free ceramics

In consideration of growing human health and ecological environment issues, lead-free piezoelectric ceramics have aroused heated research to develop their potential applications in electronic fields instead of toxic lead-based ones. In the present work, a ternary lead-free material system of (0.97- x )K 0.48 Na 0.52 Nb 0.96 Sb 0.04 O 3 –0.03Bi 0.5 Na 0.5 Zr 0.8 Sn 0.2 O 3 - x BiFeO 3 (KNNS-BNZS- x BF, 0 ≤ x ≤ 0.007) ceramics was designed, and the evolution mechanisms of microstructures and electrical behaviors at multiple applied fields were revealed in detail. The bimodal microstructure with an alternative fine and coarse grain size distribution feature is generally observed, while the BF doping tends to decrease grain size and increase the diffusion phase transition behaviors. As x = 0.005, the R-O-T multiphase boundary is formed at room temperature, accompanied by the presence of striped nanodomains with smaller size and regular distribution feature that exhibit the better polarization switching and the fast domain wall movement under external stimuli. In particular, an enhanced d 33 ~ 470 pC/N and a simultaneous higher T c ~ 260 °C are achieved in KNNS-BNZS-0.005BF, reflecting a better balanced development of performance by the present doping strategy. Most importantly, benefiting from the coexistence of R-O-T multiphase boundary and the lower domain wall energy, an excellent d 33 ⁎ ~ 530 pm/V is attained as well in this ceramic, which favors the better applications in high precision displacement or strain actuators. This work sheds insight into understanding the underlying physical mechanism of enhanced performance of KNN-based ceramics, substantially expanding the more applications of lead-free piezoelectric materials in electronic fields. • A new lead-free material system of KNNS-BNZS- x BF is designed. • Enhanced comprehensive performance is obtained by constructing R-O-T multiphase boundary. • The domain structures and polarization switching behaviors are revealed in detail. • The physical origin of enhanced performance is elaborated.

Design for the reconfigurable polarization rotator by inhibiting Fano resonance with graphene-metal grating structures

In this paper, the Fano resonance associated with the integrated grating-enhanced transmissive cross-polarization rotator (TCPR) superimposed via two polarization plates operating in disparate frequency bands is observed. The metal resonance frequency dramatically impacts the Fano effect, which triggers alterations in polarization conversion ratio (PCR). Through the analysis for the surface current distributions, the spring vibrator model driven by external forces in two orthogonal directions is employed to figure out the internal mechanism of the Fano line shape in the PCR curve. Subsequently, the symmetrical lateral current branches on the two gold polarization sheets are accessible. The relative bandwidth (RBW) value and the operating region of the ultimate optimized TCPR are 84.6% and 0.563 THz–1.388 THz, respectively. In other words, the PCR band is expanded successfully. Intended to obtain the fabulous polarization switching behavior to enhance the reconfigurability, the gated voltagedriven graphene is doped in grating gaps with the chemical potential fluctuating uniformly between 0.01 and 0.50 eV. The proposed optimizations with the PCR and the final TCPR are distinguished from precedented instances in the RBW and tunability, which is universally applicable in multitudinous terahertz-controlled scenarios.

Ferroelectric properties of BaTiO3 nanocube self-assembled monolayers: an investigation using piezoresponse force microscopy

We investigated the ferroelectric properties of barium titanate (BTO) nanocube self-assembled monolayers with and without heat treatment using piezoresponse force microscopy (PFM). Observations of polarization switching behavior confirmed that BTO nanocube monolayers about 15 nm thick are ferroelectric, even without heat treatment. Vertical PFM phase imaging of the monolayers revealed that heat treatment changed the ferroelectric polarization distribution in the monolayers at 800 °C. Atomic force microscopy and transmission electron microscopy suggested that this change originated from the residual stress caused by mechanical interactions between neighboring BTO nanocubes and between the monolayers and the substrate.

Scaling behavior of ferroelectric FET with reduction in number of domains in ferroelectric layer

With the gate-length scaling, the number of domains in FeFET is reduced to a few or a single domain. In this paper, we investigate the effect of multi-domains versus few/single-domain behavior in FeFET. The abrupt polarization switching behavior of a single-domain is obtained by modifying the Preisach model in which the difference between saturation and remnant polarization (P s−P r) is reduced. We show that for the same program/erase voltage, a two-times higher memory window can be achieved with single/few-domains FeFET than the multi-domain FeFET. Further, at fixed program/erase voltage, the scaling behavior shows improved variability due to increased polarization-induced vertical field with single-domain FeFET. We present an optimized device with a single-domain FeFET having a low operating voltage of ±2.4 V but with the same device performance that can be achieved for multi-domain FeFET having a higher operating voltage of ±5 V, which is highly promising for low power applications.

Frequency dependence on polarization switching measurement in ferroelectric capacitors

Ferroelectric hysteresis loop measurement under high driving frequency generally faces great challenges. Parasitic factors in testing circuits such as leakage current and RC delay could result in abnormal hysteresis loops with erroneous remnant polarization (P r) and coercive field (E c). In this study, positive-up-negative-down (PUND) measurement under a wide frequency range was performed on a 10-nm thick Hf0.5Zr0.5O2 ferroelectric film. Detailed analysis on the leakage current and RC delay was conducted as the polarization switching occurs in the FE capacitor. After considering the time lag caused by RC delay, reasonable calibration of current response over the voltage pulse stimulus was employed in the integral of polarization current over time. In such a method, rational P–V loops measured at high frequencies (>1 MHz) was successfully achieved. This work provides a comprehensive understanding on the effect of parasitic factors on the polarization switching behavior of FE films.

Effect of Film Microstructure on Domain Nucleation and Intrinsic Switching in Ferroelectric Y:HfO2 Thin Film Capacitors

AbstractOne of the general features of ferroelectric systems is a complex nature of polarization reversal, which involves domain nucleation and motion of domain walls. Here, time‐resolved nanoscale domain imaging is applied in conjunction with the integral switching current measurements to investigate the mechanism of polarization reversal in yttrium‐doped HfO2 (Y:HfO2)—currently one of the most actively studied ferroelectric systems. More specifically, the effect of film microstructure on the nucleation process is investigated by performing a comparative study of the polarization switching behavior in the epitaxial and polycrystalline Y:HfO2 thin film capacitors. It is found that although the epitaxial Y:HfO2 capacitors tend to switch slower than their polycrystalline counterparts, they exhibit a significantly higher nucleation density and rate, suggesting that this is a rate‐limiting mechanism. In addition, it is observed that under the external fields approaching the activation field value, the switching kinetics can be described equally well by the nucleation limited switching and the Kolmogorov‐Avrami‐Ishibashi models for both types of capacitors. This signifies convergence of two different mechanisms implying that the polarization reversal proceeds via a homogeneous nucleation process unaffected by the film microstructure, which can be considered as approaching the intrinsic switching limit.

Mutually induced soliton polarization instability in a bidirectional ultrafast fiber laser.

The bidirectional ultrafast fiber laser is a promising light source for dual-comb applications. The counter-propagating geometry could lead to soliton interaction through gain sharing, as well as the possible outcome of polarization instability. However, the polarization dynamics hidden behind the soliton interaction process in bidirectional fiber lasers were rarely investigated. Herein, we report on the polarization instability induced by the mutual soliton interactions through fiber gain in a bidirectional mode-locked fiber laser. Depending on the adjustment of the intracavity birefringence, the polarization states of two counter-propagating solitons can exhibit similar periodical polarization switching behaviors with a polarization-rotating transition state. The successive interactions of the bidirectional solitons mediated by the polarization cross-saturation effect of gain fiber could be responsible for the soliton polarization instability. These findings, in addition to the fundamental interest of the soliton nonlinear dynamics in dissipative optical systems, also open up new possibilities for creating dynamical control of the soliton polarization state and performance improvement in bidirectional ultrafast fiber lasers.

Quantitative Characterization of Ferroelectric/Dielectric Interface Traps by Pulse Measurements

The ferroelectric (FE) polarization switching behavior in the HfZrO <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> (HZO) FE/dielectric (FE/DE) stack is investigated systematically by charge responses from pulse measurements. The trapped charge density at the FE/DE interface related with the FE polarization switching is found to be 1.2 × 10 <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">14</sup> cm <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">-2</sup> according to the leakage-current-assist polarization switching mechanism. Furthermore, by the time-dependent nonswitching charge responses, the extra FE/DE interface trap density of 1.1 × 10 <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">13</sup> cm <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">-2</sup> is confirmed, which is not related but can be detected along with the FE polarization switching. The quantitative characterization reveals the huge amount of FE/DE interface traps and their dominant role in the FE operation of HZO FE/DE stack, which improves the proposed leakagecurrent-assist polarization switching model. This improved model provides a more comprehensive understanding of the polarization switching in the HZO FE/DE stack and new insights on HZO negative-capacitance (NC) and FE fieldeffect transistors (FETs).

Defect model of domain nucleation growth induced by interlayers in poly (vinylidene fluoride-trifluoroethylene) ultrathin films

The polarization switching behaviors of ultrathin films of ferroelectric poly(vinylidene fluoride-trifluoroethylene) capacitors with different electroactive interlayers have been studied. The polarization switching results are related to the high local electric field and complete microdynamic switching behavior can be ensured by optimizing the defect model. Weiss mean field theory was introduced to analyze the nucleation process of defect states. The spatial defects around the ferroelectric domain were aligned, resulting in a stable space configuration with low energy. Three hypothetical effects are proposed based on the recovery mechanism of dipole defects, including the obedience effect, cooperation effect and antagonism effect. Understanding and controlling defect functionality in ferroelectric materials is critical for realizing reliable applications in ferroelectric memories.

First-order reversal curve diagram and its application in investigation of polarization switching behavior of HfO&lt;sub&gt;2&lt;/sub&gt;-based ferroelectric thin films

&lt;sec&gt; From physical point of view, the “0, 1” read/write operation of ferroelectric memory is based on the polarization switching of ferroelectric memory. Therefore, the reliability of device relies directly on the stability of polarization switching behavior. The polarization behaviors of HfO&lt;sub&gt;2&lt;/sub&gt;-based ferroelectric thin films subjected to bipolar cyclic electric field often exhibit wake-up, fatigue and split-up of transient switching current. These unstable switching properties seriously restrict the practical application of this new-type ferroelectric material in memory devices. It therefore becomes the critical task to explore the mechanism behind the complex evolution of polarization switching and find out possible approaches to optimizing the stability. However, it will be extremely difficult to accomplish the task by the traditional characterization methods. First-order reversal curve (FORC) diagram is regarded as “fingerprint identification” in the study of hysteresis systems, and has been used successfully to analyze the characteristic parameters of magnetic materials. The FORC diagram can intuitively determine the type, size and domain status of magnetic particles from distribution of both coercive field and interaction field. Moreover, it is also found that the FORC diagram is sensitive to measuring temperature. &lt;/sec&gt;&lt;sec&gt; In this work, first, the Preisach model and implementation method of the FORC diagram are introduced. Then using Keithley 4200-SCS equipped with a remote pulse measurement unit, 60 FORCs are recorded for Si-doped HfO&lt;sub&gt;2&lt;/sub&gt; ferroelectric thin films experiencing different external field loading histories. By the mathematical treatment, switching density distributions determined by FORC measurements are obtained to explore the evolution of coercive field and bias field. The FORC diagram of pristine film contains three distribution regions with different bias fields, which merge into one distribution with an almost zero bias field after 10&lt;sup&gt;4&lt;/sup&gt; wake-up cycles. Two oppositely biased regions can be observed after 2 × 10&lt;sup&gt;9&lt;/sup&gt; sub-cycling treatments. Surprisingly, the bias fields nearly vanish again after 10&lt;sup&gt;4&lt;/sup&gt; wake-up cycles. The main change of bias field instead of coercive field indicates that the migration of oxygen vacancies is likely to be the dominant mechanism behind the complex polarization switching behavior for HfO&lt;sub&gt;2&lt;/sub&gt;-based ferroelectric thin films.&lt;/sec&gt;

Ferroelectric state and polarization switching behaviour of ultrafine BaTiO3 nanoparticles with large-scale size uniformity

A coherently non-centrosymmetric structure and remarkable macroscopic ferroelectric response of 4.5 nm BTO nanocrystals are reported.