Large Polarization Near 50 µC/cm2 in a Single Unit Cell Layer SrTiO3.

The generally nonpolar SrTiO3 has attracted more attention recently because of its possibly induced novel polar states and related paraelectric-ferroelectric phase transitions. By using controlled pulsed laser deposition, high-quality, ultrathin, and strained SrTiO3 layers were obtained. Here, transmission electron microscopy and theoretical simulations have unveiled highly polar states in SrTiO3 films even down to one unit cell at room temperature, which were stabilized in the PbTiO3/SrTiO3/PbTiO3 sandwich structures by in-plane tensile strain and interfacial coupling, as evidenced by large tetragonality (∼1.05), notable polar ion displacement (0.019 nm), and thus ultrahigh spontaneous polarization (up to ∼50 µC/cm2). These values are nearly comparable to those of the strong ferroelectrics as the PbZrxTi1-xO3 family. Our findings provide an effective and practical approach for integrating large strain states into oxide films and inducing polarization in nonpolar materials, which may broaden the functionality of nonpolar oxides and pave the way for the discovery of new electronic materials.

A Roadmap for Ferroelectric-Antiferroelectric Phase Transition.

Antiferroelectric materials have shown great potential in electronic devices benefiting from the reversible phase transition between ferroelectric and antiferroelectric phases. Understanding the dipole arrangements and clear phase transition pathways is crucial for design of antiferroelectric materials-based energy storage and conversion devices. However, the specific phase transition details remain largely unclear and even controversial to date. Here, we have grown a series of PbZrO3 on SrTiO3 substrates and elucidated the fine atom structures and phase transition pathways using atomic-resolution transmission electron microscopy. Specifically, a roadmap for ferroelectric to antiferroelectric phase transitions, here with increasing film thickness, is determined as ferroelectric rhombohedral (R3c)-ferroelectric monoclinic (Pc)-ferrielectric orthorhombic (Ima2)-antiferroelectric orthorhombic (Pbam), where Pc and Ima2 phases act as structural bridges. Moreover, the phase transition pathway is strongly related to the synergistic effect of oxygen octahedral tilting and cation displacement. These findings provide an insightful understanding for the theories and related properties of antiferroelectrics.

Evodiamine attenuates oxidative stress and ferroptosis by inhibiting the MAPK signaling to improve bortezomib-induced peripheral neurotoxicity.

BACKGROUND: Bortezomib (BTZ) is a commonly used antitumor drug, but its peripheral neuropathy side effect poses a limitation on its dosage. Evodiamine (EVO) exhibits various biological activities, including antioxidant, anti-inflammatory, and anticancer effects. The purpose of this investigation is to confirm the impact of EVO on BTZ-induced peripheral neurotoxicity. METHODS: GeneCards and HERB were applied to analyze the targets of peripheral neurotoxicity and EVO. The Gene Ontology (GO) and Kyoto Encyclopedia of Genes and Genomes (KEGG) pathways enrichment analysis of the hub genes were identified by DAVID. Rat dorsal root ganglion neurons (DRGs) and rat RSC96 Schwann cells (SCs) were treated with BTZ to simulate peripheral neurotoxicity. BTZ-induced peripheral neurotoxicity was assessed by detecting cell viability, proliferation, oxidative stress, and ferroptosis in DRGs and SCs. The mitogen-activated protein kinase (MAPK) signaling was scrutinized by Western blot assay. RESULTS: The Venn diagram for the overlapping targets of EVO and peripheral neurotoxicity showed that EVO might regulate peripheral neurotoxicity by influencing cell oxidative stress, ferroptosis, and MAPK signaling pathway. EVO attenuated BTZ-induced toxicity in DRGs and SCs. EVO attenuated BTZ-induced oxidative stress damage in DRGs and SCs by reducing reactive oxygen species and malondialdehyde levels and enhancing glutathione level. EVO attenuated BTZ-induced ferroptosis in DRGs and SCs. EVO inhibited BTZ-induced activation of the MAPK signaling in DRGs and SCs. Activation of the MAPK signaling reversed the neuroprotective effect of EVO on BTZ-induced oxidative stress injury and ferroptosis. CONCLUSION: EVO attenuated oxidative stress and ferroptosis by inhibiting the MAPK signaling to improve BTZ-induced peripheral neurotoxicity.

Pure Chiral Polar Vortex Phase in PbTiO3/SrTiO3 Superlattices with Tunable Circular Dichroism.

Nontrivial polarization textures have been demonstrated in ferroelectric/dielectric superlattices, where the electrostatic, elastic, and different gradient energies compete in a delicate balance. When PbTiO3/SrTiO3 superlattices are grown on DyScO3, the coexistence of ferroelectric domains and vortex structure is observed for n = 12-20 unit cells. Here, we report an approach to achieve single-phase vortex structures in superlattices by controlling the epitaxial strain using Sr1.04Al0.12Ga0.35Ta0.50O3 substrates. The domain width follows Kittel's law with the thickness of the ferroelectric PbTiO3 layers. A phase transition from vortex to a disordered phase with temperature is characterized by the correlation length. Resonant soft X-ray diffraction circular dichroism at the titanium L-edge reveals enhanced chirality with the thickness of the ferroelectric layer. These results are supported by second-principles simulations, which demonstrate that the integrated helicity increases with n. The stabilization of chiral single-phase polar vortices in ferroelectric/dielectric superlattices can enable novel optoelectronic devices with enhanced ferroelectric-light interaction.

Atomic Insight into the Successive Antiferroelectric-Ferroelectric Phase Transition in Antiferroelectric Oxides.

Antiferroelectrics characterized by voltage-driven reversible transitions between antiparallel and parallel polarity are promising for cutting-edge electronic and electrical power applications. Wide-ranging explorations revealing the macroscopic performances and microstructural characteristics of typical antiferroelectric systems have been conducted. However, the underlying mechanism has not yet been fully unraveled, which depends largely on the atomistic processes. Herein, based on atomic-resolution transmission electron microscopy, the deterministic phase transition pathway along with the underlying lattice-by-lattice details in lead zirconate thin films was elucidated. Specifically, we identified a new type of ferrielectric-like dipole configuration with both angular and amplitude modulations, which plays the role of a precursor for a subsequent antiferroelectric to ferroelectric transformation. With the participation of the ferrielectric-like phase, the phase transition pathways driven by the phase boundary have been revealed. We provide new insights into the consecutive phase transformation in low-dimensional lead zirconate, which thus would promote potential antiferroelectric-based multifunctional devices.

Direct Observation of Large-Scale Screw Dislocation Grids in Oxide Heteroepitaxies.

Screw dislocation is important not only for understanding plastic deformation of crystals but also for optical and electrical properties of materials. However, characterizations of screw dislocations are still challenging since there is almost no atom distortion when viewed along the dislocation line. In particular, although it is theoretically known that shear strains in heteroepitaxy systems may be relaxed via screw dislocation grids, the specific structures and thickness-dependent evolutions of these grids are still largely unknown. Here, by using orthorhombic [001]-oriented DyScO3 substrates we have directly observed large-scale screw dislocation grids in the DyScO3/BiFeO3 oxide heteroepitaxies exhibiting large shear strain. Pure screw dislocations with a[100] and a[01̅0] Burgers vectors were confirmed by multiscale transmission electron microscopy study. Our results directly confirm screw dislocation grids as a factor to tailor shear strains in epitaxial systems and suggest a practical platform for studying structures and induced responses corresponding to screw dislocations.

Real-Time Transformation of Flux-Closure Domains with Superhigh Thermal Stability.

Polar topologies have received extensive attention due to their exotic configurations and functionalities. Understanding their responsive behaviors to external stimuli, especially thermal excitation, is highly desirable to extend their applications to high temperature, which is still unclear. Here, combining in situ transmission electron microscopy and phase-field simulations, the thermal dynamics of the flux-closure domains were illuminated in PbTiO3/SrTiO3 multilayers. In-depth analyses suggested that the topological transition processes from a/c domains to flux-closure quadrants were influenced by the boundary conditions of PbTiO3 layers. The symmetrical boundary condition stabilized the flux-closure domains at higher temperature than in the asymmetrical case. Furthermore, the reversible thermal responsive behaviors of the flux-closure domains displayed superior thermal stability, which maintained robust up to 450 °C (near the Curie temperature). This work provides new insights into the dynamics of polar topologies under thermal excitation and facilitates their applications as nanoelectronics under extreme conditions.

Atomic-Scale Tunable Flexoelectric Couplings in Oxide Multiferroics.

Flexoelectricity is an effective tool in modulating the crystallographic structures and properties of oxides for multifunctional applications. However, engineering the nonuniform strain to obtain tunable flexoelectric behaviors at the atomic scale remains an ongoing challenge in conventional substrate-imposed ferroelectric films. Here, the regulatable flexoelectric behaviors are demonstrated at atomic scale in [110]-oriented BiFeO3 thin films, which are triggered by the strain-field coupling of high-density interfacial dislocations. Using aberration-corrected scanning transmission electron microscopy, the asymmetric polarization rotation around the single dislocation is revealed, which is induced by the gradient strain fields of the single dislocation. These strain fields are highly correlated to generate huge strain gradients between neighboring dislocations, and thereby, serial flexoelectric responses are engineered as a function of dislocation spacings in thicker BiFeO3 films. This work opens a pathway for the modulation of flexoelectric responses in ferroelectrics, which could be extended to other functional materials to create exotic phenomena.

Periodic Polarization Waves in a Strained, Highly Polar Ultrathin SrTiO3.

SrTiO3 is generally paraelectric with centrosymmetric structure exhibiting unique quantum fluctuation related ferroelectricity. Here we reveal highly polar and periodic polarization waves in SrTiO3 at room temperature, which is stabilized by periodic tensile strains in a sandwiched PbTiO3/SrTiO3/PbTiO3 structure. Scanning transmission electron microscopy reveals that periodic a/c domain structures in PbTiO3 layers exert unique periodic tensile strains in the ultrathin SrTiO3 layer and consequently make the highly polar and periodic states of SrTiO3. The as-received polar SrTiO3 layer features peak polar ion displacement of ∼0.01 nm and peak tetragonality of ∼1.07. These peak values are larger than previous results, which are comparable to that of bulk ferroelectric PbTiO3. Our results suggest that it is possible to integrate large and periodic strain state in oxide films with exotic properties, which in turn could be useful in optical applications and information addressing when used as memory unit.

Synchronous measurement of temperature and deformation by an ultraviolet imaging system and monochromatic pyrometry at extreme temperatures.

Synchronous measurement of temperature and deformation at elevated temperatures is highly critical, yet challenging in evaluating mechanical properties of thermal protection systems. An ultraviolet (UV) imaging system is proposed to obtain noncontact, in situ, synchronous, and full-field temperature and deformation. The established system consists of a monochromatic UV illumination with a bandpass filter for radiation suppressing, a UV CCD camera for image capturing, and an infrared pyrometer for temperature recording. Additionally, an improved monochromatic radiation pyrometry method is proposed, while a deformation measuring method using the UV digital image correlation (UV-DIC) and natural textures-generated speckle is introduced. Furthermore, through camera calibration at room temperature and real-time exposure time adjusted at elevated temperatures, the influence of reflection on radiation pyrometry and unfiltered radiation on DIC analysis is eliminated. Synchronous temperature and deformation fields of C/SiC subjected to flame heating are experimentally measured with a temperature range of 500°C-1500°C, and results demonstrate the efficacy and potential of the proposed system and method. Finally, the importance of exposure time on balancing the light intensity of radiation and reflection is also discussed.

Temperature and deformation measurement for large-scale flat specimens based on image mosaic algorithms.

Synchronous measurement of the temperature and deformation fields of large-scale flat specimens is challenging in engineering experiments, especially for high-temperature environment where the non-contact optical method is attempted. To overcome this difficulty of large-scale flat specimens tested at high temperature in the open arc wind tunnel environment, measurement principles and experiments of large-scale flat specimens based on a multi-camera system are proposed using digital image stitching as well as the improved two-color method for temperature measurement. First, the digital image mosaic method is used to process and evaluate the mosaic effect of multi-camera images, the optimal mosaic parameters are selected, and the calculation results are given. Second, a set of images for large-scale flat specimens are deduced based on an improved two-color method of temperature measurement and digital image mosaic algorithms. A stitching algorithm for full-field temperature measurement and calculation results are given. Finally, full-field displacement of the stitched images is calculated by the digital image correlation method. Synchronous measurement of temperature and deformation established in this paper provides guidance for measurement of large-scale flat specimens with high spatial resolution in engineering tests.

Overcoming high luminance gradient using serial exposure time method for synchronous full-field measurement of temperature and deformation.

The high-temperature optical method has been widely used for evaluating structural materials subjected to high temperature. Obtaining high-quality images of a specimen surface in such a harsh environment is detrimental for the accurate measurement of temperature and strain field. However, the high-temperature environment poses many challenges on these measurements, e.g., the large luminance gradient on the sample surface would jeopardize the image quality when using the full-field optical method. In order to overcome this issue, we propose here a simple and effective algorithm to obtain image sequences with serial exposure times. This algorithm incorporates exponentially decreasing exposure times to successfully reduce the disturbance caused by large luminance gradient, as will be shown by the verification on samples tested both in arc wind tunnel and oxy-propane torch flame. In comparison to the images with single exposure time, further experiment carried out on C/SiC sample up to 1100°C shows that image sequences with different exposure times can be effectively obtained by the image fusion technique. The calculation of the deformation and temperature fields using the image sequence method gives more accurate and reasonable results.

Local Enhancement of Polarization at PbTiO3/BiFeO3 Interfaces Mediated by Charge Transfer.

Ferroelectrics hold promise for sensors, transducers, and telecommunications. With the demand of electronic devices scaling down, they take the form of nanoscale films. However, the polarizations in ultrathin ferroelectric films are usually reduced dramatically due to the depolarization field caused by incomplete charge screening at interfaces, hampering the integrations of ferroelectrics into electric devices. Here, we design and fabricate a ferroelectric/multiferroic PbTiO3/BiFeO3 system, which exhibits discontinuities in both chemical valence and ferroelectric polarization across the interface. Aberration-corrected scanning transmission electron microscopic study reveals an 8% elongation of out-of-plane lattice spacing associated with 104%, 107%, and 39% increments of δTi, δO1, and δO2 in the PbTiO3 layer near the head-to-tail polarized interface, suggesting an over ∼70% enhancement of polarization compared with that of bulk PbTiO3. Besides that in PbTiO3, polarization in the BiFeO3 is also remarkably enhanced. Electron energy loss spectrum and X-ray photoelectron spectroscopy investigations demonstrate the oxygen vacancy accumulation as well as the transfer of Fe3+ to Fe2+ at the interface. On the basis of the polar catastrophe model, FeO2/PbO interface is determined. First-principles calculation manifests that the oxygen vacancy at the interface plays a predominate role in inducing the local polarization enhancement. We propose a charge transfer mechanism that leads to the remarkable polarization increment at the PbTiO3/BiFeO3 interface. This study may facilitate the development of nanoscale ferroelectric devices by tailing the coupling of charge and lattice in oxide heteroepitaxy.

Large Scale Two-Dimensional Flux-Closure Domain Arrays in Oxide Multilayers and Their Controlled Growth.

Ferroelectric flux-closures are very promising in high-density storage and other nanoscale electronic devices. To make the data bits addressable, the nanoscale flux-closures are required to be periodic via a controlled growth. Although flux-closure quadrant arrays with 180° domain walls perpendicular to the interfaces (V-closure) have been observed in strained ferroelectric PbTiO3 films, the flux-closure quadrants therein are rather asymmetric. In this work, we report not only a periodic array of the symmetric flux-closure quadrants with 180° domain walls parallel to the interfaces (H-closure) but also a large scale alternative stacking of the V- and H-closure arrays in PbTiO3/SrTiO3 multilayers. On the basis of a combination of aberration-corrected scanning transmission electron microscopic imaging and phase field modeling, we establish the phase diagram in the layer-by-layer two-dimensional arrays versus the thickness ratio of adjacent PbTiO3 films, in which energy competitions play dominant roles. The manipulation of these flux-closures may stimulate the design and development of novel nanoscale ferroelectric devices with exotic properties.

Single-cell sequencing in diffuse large B-cell lymphoma: C1qC is a potential tumor-promoting factor.

BACKGROUND: Complement component 1q (C1q) is central to the classical complement pathway. High C1q expression has been linked to poor prognosis in patients with cancer. However, the precise mechanism via which C1q contributes to diffuse large B-cell lymphoma (DLBCL) is still unknown. We aimed to explore the potential mechanism by which C1qC promoting DLBCL. METHODS: Using multiplex immunohistochemistry (mIHC) to identify immunocyte subgroups associated with prognosis in DLBCL tissues. Constructing a risk prediction model based on immunocytes using least absolute shrinkage and selection operator (LASSO) regression. Single-cell sequencing detects the expression level of C1qC in immunocytes in the DLBCL microenvironment. Using Wb and qPCR to detect markers of M2 macrophages after knocking down C1qC, and exploring the interactions between lymphoma cells and macrophages through co-culture. Analyzing clinical data from DLBCL patients to investigate the clinical significance of C1qC+ M2 macrophages. Lastly, using bioinformatics in conjunction with mIHC to elucidate the potential pro-tumor mechanism of C1qC. RESULTS: First, we found T cell subtypes, neutrophils, and M2 macrophages are associated with prognosis. Subsequently, the risk model identified C1qC as a differential gene relevant to DLBCL prognosis. Furthermore, single-cell sequencing suggested high C1qC expression in M2 macrophages. The expression level of CD163 is significantly lower following siC1qC. Co-culture experiments have shown that M2 macrophages can promote the proliferation of tumor cells and reduce their drug sensitivity. Furthermore, as an independent predictive indicator, high expression of C1qC+ M2 macrophages is associated with poor prognosis in patients. Finally, a positive correlation between increased C1qC expression and immune checkpoints, as well as an increase in the infiltration of regulatory T cells (Tregs) and M2 macrophages. CONCLUSIONS: C1qC offering new insights into pathogenesis and presenting a potential therapeutic target in DLBCL.

Polar Bloch points in strained ferroelectric films.

Topological domain structures have drawn great attention as they have potential applications in future electronic devices. As an important concept linking the quantum and classical magnetism, a magnetic Bloch point, predicted in 1960s but not observed directly so far, is a singular point around which magnetization vectors orient to nearly all directions. Here we show polar Bloch points in tensile-strained ultrathin ferroelectric PbTiO3 films, which are alternatively visualized by phase-field simulations and aberration-corrected scanning transmission electron microscopic imaging. The phase-field simulations indicate local steady-state negative capacitance around the Bloch points. The observation of polar Bloch points and their emergent properties consequently implies novel applications in future integrated circuits and low power electronic devices.

Epitaxial Strain Enhanced Ferroelectric Polarization toward a Giant Tunneling Electroresistance.

A substantial ferroelectric polarization is the key for designing high-performance ferroelectric nonvolatile memories. As a promising candidate system, the BaTiO3/La0.67Sr0.33MnO3 (BTO/LSMO) ferroelectric/ferromagnetic heterostructure has attracted a lot of attention thanks to the merits of high Curie temperature, large spin polarization, and low ferroelectric coercivity. Nevertheless, the BTO/LSMO heterostructure suffers from a moderate FE polarization, primarily due to the quick film-thickness-driven strain relaxation. In response to this challenge, we propose an approach for enhancing the FE properties of BTO films by using a Sr3Al2O6 (SAO) buffering layer to mitigate the interfacial strain relaxation. The continuously tunable strain allows us to illustrate the linear dependence of polarization on epitaxial strain with a large strain-sensitive coefficient of ∼27 µC/cm2 per percent strain. This results in a giant polarization of ∼80 µC/cm2 on the BTO/LSMO interface. Leveraging this large polarization, we achieved a giant tunneling electroresistance (TER) of ∼105 in SAO-buffered Pt/BTO/LSMO ferroelectric tunnel junctions (FTJs). Our research uncovers the fundamental interplay between strain, polarization magnitude, and device performance, such as on/off ratio, thereby advancing the potential of FTJs for next-generation information storage applications.

Absence of critical thickness for polar skyrmions with breaking the Kittel's law.

The period of polar domain (d) in ferroics was commonly believed to scale with corresponding film thicknesses (h), following the classical Kittel's law of d ∝ [Formula: see text]. Here, we have not only observed that this relationship fails in the case of polar skyrmions, where the period shrinks nearly to a constant value, or even experiences a slight increase, but also discovered that skyrmions have further persisted in [(PbTiO3)2/(SrTiO3)2]10 ultrathin superlattices. Both experimental and theoretical results indicate that the skyrmion periods (d) and PbTiO3 layer thicknesses in superlattice (h) obey the hyperbolic function of d = Ah + [Formula: see text] other than previous believed, simple square root law. Phase-field analysis indicates that the relationship originates from the different energy competitions of the superlattices with PbTiO3 layer thicknesses. This work exemplified the critical size problems faced by nanoscale ferroelectric device designing in the post-Moore era.

Enhanced Exchange Bias in Epitaxial High-Entropy Oxide Heterostructures.

High-entropy oxides (HEOs) have gained significant interest in recent years due to their unique structural characteristics and potential to tailor functional properties. However, the electronic structure of the HEOs currently remains vastly unknown. In this work, combining magnetometry measurements, scanning transmission electron microscopy, and element-specific X-ray absorption spectroscopy, the electronic structure and magnetic properties of the perovskite-HEO La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 epitaxial thin films are systemically studied. It is found that enhanced magnetic frustration emerges from competing exchange interactions of the five transition-metal cations with energetically favorable half-filled/full-filled electron configurations, resulting in an unprecedented large vertical exchange bias effect in the single-crystalline films. Furthermore, our findings demonstrate that the La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 layer with a thickness down to 1 nm can be used as a pinning layer and strongly coupled with a ferromagnetic La0.7Sr0.3MnO3 layer, leading to a notable exchange bias and coercivity enhancement in a cooling field as small as 5 Oe. Our studies not only provide invaluable insight into the electronic structure of HEOs but also pave the way for a new era of large bias materials for spintronics devices.

Room-Temperature Ferroelectricity of Paraelectric Oxides Tailored by Nano-Engineering.

Inducing clear ferroelectricity in the quantum paraelectric SrTiO3 is important for triggering methods to discover hidden phases in condensed matter physics. Several methods such as isotope substitution and freestanding membranes could introduce ferroelectricity in SrTiO3 toward nonvolatile memory applications. However, the stable transformation from quantum paraelectric SrTiO3 to ferroelectricity SrTiO3 at room temperature still remains challenging. Here, we used multiple nano-engineering in (SrTiO3)0.65/(CeO2)0.35 films to achieve an emergent room-temperature ferroelectricity. It is shown that the CeO2 nanocolumns impose large out-of-plane strains and induce Sr/O deficiency in the SrTiO3 matrix to form a clear tetragonal structure, which leads to an apparent room-temperature ferroelectric polarization up to 2.5 µC/cm2. In collaboration with density functional theory calculations, it is proposed that the compressive strains combined with elemental deficiency give rise to local redistribution of charge density and orbital order, which induce emergent tetragonality of the strained SrTiO3. Our work thus paves a pathway for architecting functional systems in perovskite oxides using a multiple nano-design.