Dielectric capacitors are widely used in pulsed power electronic devices due to their ultrahigh power densities and extremely fast charge/discharge speed. To achieve enhanced energy storage density, both maximum polarization (Pmax) and breakdown strength (Eb) need to be improved simultaneously. However, these two key parameters are inversely correlated. In this study, order-disorder transition induced polar nanoregions (PNRs) have been achieved in PbZrO3 thin films by making use of the low-energy ion implantation, enabling us overcome the trade-off between high polarizability and breakdown strength, which leads to the tripling of the energy storage density from 20.5 J/cm3 to 62.3 J/cm3 as well as the great enhancement of breakdown strength. This approach could be extended to other dielectric oxides to improve the energy storage performance, providing a new pathway for tailoring the oxide functionalities.

The deterministic creation and modification of domain walls in ferroelectric films have attracted broad interest due to their unprecedented potential as the active element in non-volatile memory, logic computation and energy-harvesting technologies. However, the correlation between charged and antiphase states, and their hybridization into a single domain wall still remain elusive. Here we demonstrate the facile fabrication of antiphase boundaries in BiFeO 3 thin films using a He-ion implantation process. Cross-sectional electron microscopy, spectroscopy and piezoresponse force measurement reveal the creation of a continuous in-plane charged antiphase boundaries around the implanted depth and a variety of atomic bonding configurations at the antiphase interface, showing the atomically sharp 180° polarization reversal across the boundary. Therefore, this work not only inspires a domain-wall fabrication strategy using He-ion implantation, which is compatible with the wafer-scale patterning, but also provides atomic-scale structural insights for its future utilization in domain-wall nanoelectronics.

Exotic topological domains in BiFeO3 nanoislands have attracted much attention regarding their potential applications in advanced electronic devices. Here, different from the earlier reported disordered distributed BiFeO3 nanoislands formed by a self-assembly method, we fabricated an ordered BiFeO3 nanoisland array by mask-assisted pulsed laser deposition on a SrTiO3 substrate, which exhibits a center-converged in-plane polarization component and a monodomain pattern along the vertical direction. Such center-type quad-domain structures exhibit high stability, maintaining their topological structures after heating to 250 °C and subsequently cooling to room temperature. Moreover, they can be switched by applying a scanning electric field and recovered by applying a heating and cooling process. Observing this topological structure in BiFeO3 nanoislands might provide a suitable platform for further exploration of its topological phase transition properties, new functions, and potential applications.

Optical second harmonic generation (SHG) is a sensitive and powerful technique to probe various symmetry breaking, especially ferroelectric/magnetic domains, in artificial thin films or heterostructures. In a wide range of ferroelectric crystals, a non‐trivial broken symmetry will emerge at domain boundaries, however, the contribution of such symmetry breaking to SHG is often neglected due to its random orientation. Here, a co‐polarized SHG effect from the well‐aligned domain wall arrays is observed in BiFeO 3 thin films. This SHG component is highly dependent on the local orientation of the wall arrays, and its polarization feature reveals the Néel‐like evolution of electric polar vectors in the wall region. Based on this intriguing effect, mixed‐phase patches with four possible orientations in the quasi‐tetragonal stripes are identified by polarization‐sensitive SHG mapping. These findings not only clarify a critical SHG contribution in this multiferroic material, but also demonstrate an optical approach for exploring phase‐determined function unit.

As a high-k material, hafnium oxide (HfO2) has been used in gate dielectrics for decades. Since the discovery of polar phase in Si-doped HfO2 films, chemical doping has been widely demonstrated as an effective approach to stabilize the ferroelectric phase in HfO2 based thin films. However, the extra capping layer deposition, post-growth annealing and wake-up effect are usually required to arouse the ferroelectricity in HfO2 based thin films, resulting in the increase of complexity for sample synthesis and the impediment of device application. In this study, the ferroelectricity is observed in non-capped dopant-free HfO2 thin films prepared by pulsed laser deposition (PLD) without post-growth annealing. By adjusting the deposited temperature, oxygen pressure and thickness, the maximum polarization up to 14.7 μC/cm2 was obtained in 7.4 nm-thick film. The fraction of orthorhombic phase, concentrations of defects and size effects are considered as possible mechanisms for the influences of ferroelectric properties. This study indicates that PLD is an effective technique to fabricate high-quality ferroelectric HfO2 thin films in the absence of chemical doping, capping layer deposition and post-growth annealing, which may boost the process of nonvolatile memory device application.

The coexistence of two phases across a morphotropic phase boundary (MPB), in piezoelectric materials, usually possess high electromechanical coupling response owing to the electrically controllable of transition between the two phases. Conventionally, morphotropic phase boundary is compositionally driven such as in PbZrO3–PbTiO3 system. Recent study has demonstrated it can be strain-induced in BiFeO3 as well. Using a combination of strain engineering in conjunction with chemical doping, we reveal the coexistence of multiple morphotropic phase boundaries (multi-MPBs) in highly strained BiFeO3 thin films through La doping. By applying an electric field, we show the reversible switching of these multi-MPBs. The discovery of these multi-MPBs in La-doped BiFeO3 thin films further enhance the electromechanical coupling response comparing with the previous observed MPB in pure BiFeO3, opening a new field to obtain high-performance piezoelectric materials.

Ferroelectric topological objects provide a fertile ground for exploring emerging physical properties that could potentially be utilized in future nanoelectronic devices. Here, we demonstrate quasi-one-dimensional metallic high conduction channels associated with the topological cores of quadrant vortex domain and center domain (monopole-like) states confined in high quality BiFeO 3 nanoislands, abbreviated as the vortex core and the center core. We unveil via the phase-field simulation that the superfine metallic conduction channels along the center cores arise from the screening charge carriers confined at the core region, whereas the high conductance of vortex cores results from a field-induced twisted state. These conducting channels can be reversibly created and deleted by manipulating the two topological states via electric field, leading to an apparent electroresistance effect with an on/off ratio higher than 10 3 . These results open up the possibility of utilizing these functional one-dimensional topological objects in high-density nanoelectronic devices, e.g. nonvolatile memory.

In recent years, there is a surge of research interest in exotic ferroelectric topological states, motivated by their rich emerging physical properties and potential applications in nanoelectronic devices. Here, we demonstrate the observation of a sort of complex center-type topological domain structures, which exhibit a quadrant center-type (with polarization pointing to the center) topological texture for an in-plane polarization component and a cylinder domain pattern along the vertical direction, in rhombohedral structured Pb(Zr0.7Ti0.3)O-3 (R-PZT) nanoislands. Such a center domain state exhibits a rather high stability, which can well maintain its topological texture after heating to above curie temperature and subsequently cooling down to room temperature. Moreover, it allows erasure by a scanning electric field, yet it can also be recovered by a similar heating and cooling process. The observation of these unique topological textures in R-PZT nanoislands might provide a good playground for further exploring their topological phase transition properties, emerging novel functionalities, and application potential.

The topological Hall effect (THE) has been discovered in ultrathin SrRuO 3 (SRO) films, where the interface between the SRO layer and another oxide layer breaks the inversion symmetry resulting in the appearance of THE. Thus, THE only occurs in ultrathin SRO films of several unit cells. In addition to employing a heterostructure, the inversion symmetry can be broken intrinsically in bulk SRO by introducing defects. In this study, THE is observed in 60‐nm‐thick SRO films, in which defects and lattice distortions are introduced by helium ion irradiation. The irradiated SRO films exhibit a pronounced THE in a wide temperature range from 5 to 80 K. These observations can be attributed to the emergence of Dzyaloshinskii–Moriya interaction as a result of artificial inversion symmetry breaking associated with the lattice defect engineering. The creation and control of the THE in oxide single layers can be realized by ex situ film processing. Therefore, this work provides new insights into the THE and illustrates a promising strategy to design novel spintronic devices.

Ferroelectric heterostructures with bi-stable state of polarization are appealing for data storage as well as tunable functionalities such as memristor behavior. While an increasing number of experimental and theoretical studies suggest that polarization persists in ultrathin epitaxial heterostructures approaching just a couple of unit cells, the switching of such polar order is much less well understood, and whether polarization can be reversed in ultrathin ferroelectric heterostructures remains to be answered. Here we fabricate high-quality 7-unit cell thick BaTiO3 (BTO) films on Nb-doped single crystalline SrTiO3 (NSTO) substrate, and demonstrate their apparent yet unambiguously false polarization reversal due to charge injection using comprehensive piezoresponse force microscopy (PFM) studies. The presence of weak polar order consistent with linear piezoelectricity is confirmed at the atomic scale by high resolution integrated differential phase contrast (IDPC) of transmission electron microscopy (TEM) as well as macroscopic second harmonic generation (SHG), while the lack of polarization reversal under the voltage applied is supported by density functional theory calculation showing the persistence of dead layer on the surface. Nevertheless, poling-induced electric conduction differing by two orders of magnitude is observed, demonstrating resistive switching in ferroelectric heterostructure in the absence of polarization reversal, even with weak polar order. Our finding has technological implications on emerging memristor applications with potentially more accessible states than bi-stable polarization modulated mechanism, and raises technical challenges to unambiguously demonstrate polarization switching in ultrathin films at their critical size limit.

Defect engineering has been a powerful tool to enable the creation of exotic phases and the discovery of intriguing phenomena in ferroelectric oxides. However, accurate control the concentration of defects remains a big challenge. In this work, ion implantation, that can provide controllable point defects, allows us the ability to produce a controlled defect-driven true super-tetragonal (T) phase with enhanced tetragonality in ferroelectric BiFeO3 thin films. This point defect engineering is found to drive the phase transition from the as-grown mixed rhombohedral-like (R) and tetragonal-like (MC) phase to true tetragonal (T) symmetry. By further increasing the injected dose of He ion, we demonstrate an enhanced tetragonality super-tetragonal (super-T) phase with the largest c/a ratio (~ 1.3) that has ever been experimentally achieved in BiFeO3. A combination of morphology change and domain evolution further confirm that the mixed R/MC phase structure transforms to the single-domain-state true tetragonal phase. Moreover, the re-emergence of R phase and in-plane stripe nanodomains after heat treatment reveal the memory effect and reversible phase transition. Our findings demonstrate the control of R-Mc-T-super T symmetry changes and the creation of true T phase BiFeO3 with enhanced tetragonality through controllable defect engineering. This work also provides a pathway to generate large tetragonality (or c/a ratio) that could be extended to other ferroelectric material systems (such as PbTiO3, BaTiO3 and HfO2) which may lead to strong polarization enhancement.

Defect engineering has been a powerful tool to enable the creation of exotic phases and the discovery of intriguing phenomena in ferroelectric oxides. However, the accurate control of the concentration of defects remains a big challenge. In this work, ion implantation, which can provide controllable point defects, allows us to produce a controlled defect driven true super-tetragonal (T) phase with a single-domain-state in ferroelectric BiFeO3 thin films. This point-defect engineering is found to drive the phase transition from the as-grown mixed rhombohedral-like (R) and tetragonal-like (MC) phase to true tetragonal (T) symmetry and induce the stripe multi-nanodomains to a single domain state. By further increasing the injected dose of the He ion, we demonstrate an enhanced tetragonality super-tetragonal (super-T) phase with the largest c/a ratio of ∼1.3 that has ever been experimentally achieved in BiFeO3. A combination of the morphology change and domain evolution further confirms that the mixed R/MC phase structure transforms to the single-domain-state true tetragonal phase. Moreover, the re-emergence of the R phase and in-plane nanoscale multi-domains after heat treatment reveal the memory effect and reversible phase transition and domain evolution. Our findings demonstrate the reversible control of R-Mc-T-super T symmetry changes (leading to the creation of true T phase BiFeO3 with enhanced tetragonality) and multidomain-single domain structure evolution through controllable defect engineering. This work also provides a pathway to generate large tetragonality (or c/a ratio) that could be extended to other ferroelectric material systems (such as PbTiO3, BaTiO3 and HfO2) which might lead to strong polarization enhancement.

Conductive ferroelectric domain walls-ultranarrow configurable conduction paths-have been considered as essential building blocks for future programmable domain wall electronics. For applications in high-density devices, it is imperative to explore the conductive domain walls in small confined systems, while earlier investigations have hitherto focused on thin films or bulk single. Here, an observation and manipulation of conductive domain walls confined within small BiFeO3 nanoislands aligned in high-density arrays are demonstrated. Using conductive atomic force microscopy, various types of conductive domain walls, including the head-to-head charged domain walls (CDWs), zigzag domain walls, and typical 71 degrees head-to-tail neutral domain walls (NDWs), are distinctly visualized. The CDWs exhibit remarkably enhanced metallic conductivity with current of approximate to nA order in magnitude and 10(4) times larger than that inside domains (0.01-0.1 pA), while the semiconducting NDWs allow much smaller current (approximate to 10 pA) than the CDWs. The substantial difference in conductivity for dissimilar walls enables manipulations of various wall conduction states for individual addressable nanoislands via electrical tuning of domain structures. A controllable writing of four distinctive states in individual nanoislands can be achieved, showing application potentials for developing multilevel high-density memories.

We propose a novel method to drive phase transitions by etching strained BiFeO3 thin films to nanoislands. Atomic force microscopy (AFM) measurements reveal that the amount of rhombohedral-like (R) phase increases as the BiFeO3 thin films with tetragonal-like (T) matrix are etched to nanoislands and larger fraction of R phase can be obtained with the size reduction from 1 pm to 200 nm, indicating the T to R phase transitions induced by partial release of substrate clamping. Using piezoresponse force microscopy (PFM), it is demonstrated that rhombohedral-like (R) to tetragonal-like (T) phase transitions can be reversibly achieved under DC electric field in BFO nanoislands. Large electromechanical response has been observed in BFO nanoislands as well. This approach can be extended to other strained oxide films and provide guidance for the development of high-performance electromechanical lead-free materials.

The recent discovery of efficient charge separation in tetragonal–rhombohedral (T‐R) polymorphic phase boundaries (PPBs) in strained BiFeO3 (BFO) films is of great interest, and also raised a question of whether the PPBs could enhance the performance of BFO‐based planar photodetectors. To address it, we prepare BFO films with thickness ranging from 8 to 90 nm on the LaAlO3 substrates, in which the BFO evolves from a pure T phase (without PPBs) to a T‐R mixed phase (with PPBs) due to the strain relaxation. Then, we comparatively investigate the photoconductive properties of these BFO films with the planar device geometry. It is found that the photoconductance first increases and then decreases with increasing film thickness. Particularly, the 50‐nm film containing the pure T phase without any detectable PPBs exhibits the highest photoconductance. This unexpected observation can be understood by analyzing the effects of increasing film thickness and associated phase evolution on the photoconduction‐related parameters.

A new driving method for a liquid crystal (LC) lens with a hole-patterned electrode is proposed to increase the range of the variable power of the lens. The optical properties of the LC lens are analyzed by an interferometer, and the combination of the driving parameters including the amplitudes and the frequency of the driving voltages are optimized to extend the focus range and keep the aberration below 0.07 wave. For the LC tens used in the experiment with an aperture of 2.0 mm diameter and an LC (Delta n = 0.2) layer of 15 pm thickness, the focus range is extended from approximately 3.4 to 5.7 diopters. (C) 2018 The Japan Society of Applied Physics

Photodetectors, which convert incident light into electricity, are the key components to many optoelectronic technologies in use today. How well the photodetectors perform depends on how efficiently the photo-excited electron–hole pairs are separated. Efficient charge separation was recently discovered in tetragonal–rhombohedral (T-R) polymorphic phase boundaries (PPBs) in strained BiFeO3 (BFO) films, which also raised the question of whether the PPBs could enhance the performance of BFO-based planar photodetectors. In their Letter (article no. 1700301), Zhen Fan, Xingsen Gao and co-workers systematically investigate the photoconductive characteristics of strained BFO films with different thicknesses, in which the BFO evolves from a pure T phase (without PPBs) to a T-R mixed phase (with PPBs), by using the planar device geometry. Interestingly, the 50-nm film containing the pure T phase without any detectable PPBs exhibits the highest photoconductance. To understand this unexpected observation, the authors analyze the effects of increasing film thickness and associated phase evolution on the photoconduction process, with particular attention paid to the role of PPBs. This study provides insights into the physics of photoconduction in the BFO-based planar devices, which may benefit the development of high-performance photodetectors.

Exchange bias stems from the interaction between different magnetic phases, and therefore, it generally occurs in magnetic multilayers. Here, we present a large exchange bias in a single SrRuO3 layer induced by helium ion irradiation. When the fluence increases, the induced defects not only suppress the magnetization and the Curie temperature but also drive a metal-insulator transition at a low temperature. In particular, a large exchange bias field up to ∼0.36 T can be created by the irradiation. This large exchange bias is related to the coexistence of different magnetic and structural phases that are introduced by embedded defects. Our work demonstrates that spintronic properties in complex oxides can be created and enhanced by applying ion irradiation.

Ferroelectric diodes with polarization-modulated Schottky barriers are promising for applications in resistive switching (RS) memories. However, they have not achieved satisfactory performance reliability as originally hoped. The physical origins underlying this issue have not been well studied, although they deserve much attention. Here, by means of scanning Kelvin probe microscopy we show that the electrical poling of ferroelectric diodes can cause significant charge injection and trapping besides polarization switching. We further show that the reproducibility and stability of switchable diode-type RS behavior are significantly affected by the interfacial traps. A theoretical model is then proposed to quantitatively describe the modifications of Schottky barriers by charge injection and trapping. This model is able to reproduce various types of hysteretic current-voltage characteristics as experimentally observed. It is further revealed that the charge injection and trapping can significantly modify the electroresistance ratio, RS polarity, and high-or low-resistance states initially defined by the polarization direction. Several approaches are suggested to suppress the effect of charge injection and trapping so as to realize high-performance polarization-reversal-induced RS. This study, therefore, reveals the microscopic mechanisms for the RS behavior comodulated by polarization reversal and charge trapping in ferroelectric diodes, and also provides useful suggestions for developing reliable ferroelectric RS memories.

We have comparatively studied the dielectric, ferroelectric, conduction, and photovoltaic properties of Ti/BaTiO3 (BTO)/SrRuO3 (SRO) and Pt/BTO/SRO capacitors. The resistive switching (RS) is observed in the Pt/BTO/SRO capacitor while it is absent in the Ti/BTO/SRO capacitor, which may be attributed to the interfacial layer existing between Pt and BTO and the Ti/BTO Ohmic interface, respectively. Further analyses on the conduction mechanisms suggest that the RS may be caused by the opening/closing of conduction paths in the Pt/BTO interfacial layer, whereas the polarization is ruled out as the origin of RS because of the inconsistency between the RS switching voltages and coercive voltages. On the other hand, it is observed that the photovoltaic effects (PVEs) in both Ti/BTO/SRO and Pt/BTO/SRO capacitors are electrically unswitchable and the open-circuit voltages of the two capacitors are similar in magnitude, implying that the PVE is driven by an internal bias field rather than the polarization-induced field. The existence of such an internal bias field is indicated by the self-polarization and imprint phenomena. Our study demonstrates that the interfacial layer and the internal bias field can be the major causes for the RS and PVE in certain ferroelectric capacitors, respectively, whereas the polarization may not necessarily play a role. Published by AIP Publishing.