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The motion of domain walls is a crucial factor in piezoelectric properties and is usually related to the irreversible and hysteretic behaviors. Herein, we report on the investigation of inverse and transverse piezoelectric coefficients of capacitor-based and microcantilever-based Pb(Zr0.52Ti0.48)O3 films with a change in the DC bias and the AC applied voltage. A large inverse piezoelectric strain coefficient of about 350 p.m./V, and a low strain hysteresis of about 7.1%, are achieved in the film capacitors under a low applied voltage of 2 V (20 kV/cm) which can benefit the actuators for motion control in high-precision systems. The field-dependences of the transverse piezoelectric coefficients, obtained from four-point bending and microcantilever displacement, are in good agreement with each other. The results also reveal that the irreversible domain-wall motion is attributed to the nonlinearity in the field-dependent piezoelectric strain and cantilever displacement.

As the employment of halide perovskite films in single-junction and tandem solar cells continues to soar, there is a strong drive -from academia to industry- to produce these films using dry processes, avoiding the use of toxic solvents. Vapor deposition methods such as co-evaporation have shown advantages of solvent-free approaches to produce high-efficiency solar cells. However, co-evaporation requires the use of multiple sources that challenge the deposition rate control of complex halide perovskite compositions. Here, Pulsed Laser Deposition (PLD) is proposed as an alternative method to deposit hybrid halide perovskites films from a single-source and following a fully dry approach. We use the archetypical methylammonium lead iodide (MAPbI3) to demonstrate the formation of high-quality films with optimal optoelectronic properties by PLD on various substrates for single-junction and tandem devices. Furthermore, the important role of the PLD target composition and deposition parameters to achieve control over film microstructure and optoelectronic properties is discussed. The controlled conformal growth provided by PLD demonstrated in this work with MAPbI3 on device-relevant substrates will broaden opportunities to explore PLD of more complex hybrid halide perovskite compositions for efficient, stable, and scalable solar cell devices.

Lead-free Bi0.5K0.5TiO3 (BKT) ferroelectric films were synthesized on Pt/Ti/SiO2/Si substrates via the chemical solution deposition. The influence of the excess potassium on the microstructures and the ferroelectric properties of the films was investigated in detail. The results showed that the BKT films have reached the well-crystallized state in the single-phase perovskite structure with 20 mol.% excess amount of potassium. For this film, the ferroelectric properties of the films were significantly enhanced. The remnant polarization (Pr) and maximum polarization (Pm) reached the highest values of 9.4 μC/cm2 and 32.2 μC/cm2, respectively, under the electric field of 400 kV/cm.

The properties of correlated oxides can be manipulated by forming short-period superlattices since the layer thicknesses are comparable with the typical length scales of the involved correlations and interface effects. Herein, we studied the metal–insulator transitions (MITs) in tetragonal NdNiO3/SrTiO3 superlattices by controlling the NdNiO3 layer thickness, n in the unit cell, spanning the length scale of the interfacial octahedral coupling. Scanning transmission electron microscopy reveals a crossover from a modulated octahedral superstructure at n = 8 to a uniform nontilt pattern at n = 4, accompanied by a drastically weakened insulating ground state. Upon further reducing n the predominant dimensionality effect continuously raises the MIT temperature, while leaving the antiferromagnetic transition temperature unaltered down to n = 2. Remarkably, the MIT can be enhanced by imposing a sufficiently large strain even with strongly suppressed octahedral rotations. Our results demonstrate the relevance for the control of oxide functionalities at reduced dimensions.

To benefit from the diverse functionalities of perovskite oxides in silicon-based complementary metal oxide semiconductor (CMOS) technology, integrating oxides into a silicon platform has become one of the major tasks for oxide research. Using the deposition of LaMnO3/SrTiO3 (STO) superlattices (SLs) as a case study, we demonstrate that (001) single oriented oxide SLs can be integrated on Si using various template techniques, including a single-layer buffer of STO prepared by molecular beam epitaxy (MBE) and pulsed laser deposition, a multilayer buffer of Y-stabilized zirconia/CeO2/LaNiO3/STO, and STO-coated two-dimensional nanosheets of Ca2Nb3O10 (CNO) and reduced graphene oxide. The textured SL grown on STO-coated CNO nanosheets shows the highest crystallinity, owing to the small lattice mismatch between CNO and STO as well as less clamping from a Si substrate. The epitaxial SL grown on STO buffer prepared by MBE suffers the largest thermal strain, giving rise to a strongly suppressed saturation magnetization but an enhanced coercive field, as compared to the reference SL grown on an STO single crystal. These optional template techniques used for integrating oxides on Si are of significance to fulfill practical applications of oxide films in different fields.

Excellent energy storage performance in combination with a low operating voltage is a very important factor for pulse-power dielectric capacitor devices to achieve miniaturization and integration. Here the heterostructure of the relaxor ferroelectric Pb0.9La0.1(Zr0.52Ti0.48)O3 (PL), with a slim hysteresis loop, on the normal ferroelectric Pb(Zr0.52Ti0.48)0.99Nb0.01O3 (PN), causing a large voltage imprint, is shown to improve the energy-storage performance. A large recoverable energy-storage density of 43.5 J/cm3 and a high energy-storage efficiency of 84.1%, under an electric field of 2450 kV/cm (i.e. a 49 V voltage bias), are obtained in the 180 nm PL/20 nm PN thin film heterostructure. Due to the small total film thickness the excellent energy-storage properties are obtained at a low operating voltage of 49 V. Moreover, the PL/PN heterostructure also exhibits an excellent charge-discharge endurance up to 1010 cycles and good thermal stability in a wide temperature range from room temperature to 200 °C. These performances show that these heterostructures form a promising design for high-temperature pulse-power capacitors, with superior energy-storage performance at low operating voltages.

The dielectric properties, tunability and figure-of-merit (FOM) of relaxor Pb0.9La0.1(Zr0.52Ti0.48)O3 (PLZT) films have been investigated. Dielectric measurements indicated that the dielectric constant (at zero-bias field), tunability and FOM are enhanced as the film thickness increases, which are mainly attributed to the presence of an interfacial layer near the film-electrode interface. Experimental results illustrated that a slight reduction is observed in both dielectric constant and tunability (−2%) in a wide-frequency range (10 kHz–1 MHz), meanwhile, the FOM value decreases significantly (−17%) with increasing frequency, arising from the higher dielectric loss value. The 1000-nm PLZT film shows the largest tunability of 94.6% at a maximum electric-field of 1450 kV/cm, while the highest FOM factor is 37.6 at 1000 kV/cm, due to the combination of medium tunability (88.7%) and low dielectric loss (0.0236). All these excellent results indicated that the relaxor PLZT films are promising candidates for specific applications in microwave devices.

The interface between the insulators LaAlO$_3$ and SrTiO$_3$ accommodates a two-dimensional electron liquid (2DEL) -- a high mobility electron system exhibiting superconductivity as well as indications of magnetism and correlations. While this flagship oxide heterostructure shows promise for electronics applications, the origin and microscopic properties of the 2DEL remain unclear. The uncertainty remains in part because the electronic structures of such nanoscale buried interfaces are difficult to probe, and is compounded by the variable presence of oxygen vacancies and coexistence of both localized and delocalized charges. These various complications have precluded decisive tests of intrinsic electronic and orbital reconstruction at this interface. Here we overcome prior difficulties by developing an interface analysis based on the inherently interface-sensitive resonant x-ray reflectometry. We discover a high charge density of 0.5 electrons per interfacial unit cell for samples above the critical LaAlO$_3$ thickness, and extract the depth dependence of both the orbital and electronic reconstructions near the buried interface. We find that the majority of the reconstruction phenomena are confined to within 2 unit cells of the interface, and we quantify how oxygen vacancies significantly affect the electronic system. Our results provide strong support for the existence of polarity induced electronic reconstruction, clearly separating its effects from those of oxygen vacancies., Accepted in Physical Review Materials

The growth of α-quartz-based piezoelectric thin films opens the door to higher-frequency electromechanical devices than those available through top-down approaches. We report on the growth of SiO2/GeO2 thin films by pulsed laser deposition and their subsequent crystallization. By introducing a devitrifying agent uniformly within the film, we are able to obtain the α-quartz phase in the form of platelets with lateral sizes above 100 μm at accessible temperatures. Films containing different amounts of devitrifying agent are investigated, and their crystallinity is ascertained with X-ray diffraction and electron back-scatter diffraction. Our work highlights the difficulty in crystallization when competing phases arise that have markedly different crystalline orientation.

For thin film synthesis of complex oxides, one of the most important issues has always been how to oxidise the material. For a technique like pulsed laser deposition, a key benefit is the relatively high oxygen background pressure one can operate at, and therefor oxidation should be relatively straightforward. However, understanding the microscopic oxidation mechanisms turns out to be rather difficult. In this perspective, we give a brief overview of the sources of oxidation for complex oxide thin films grown by pulsed laser deposition. While it is clear what these sources are, their role in the kinetics of the formation of the crystal structure and oxygen stoichiometry is not fully understood.

Thin PbZrO3 (PZO) antiferroelectric films with (001)-preferred orientation were deposited on SrRuO3/Ca2Nb3O10-nanosheet/Si substrates using pulsed laser deposition. Variation of the deposition temperature was found to play a key role in the control of the microstructure and strongly influence the energy storage performance of the thin film. The critical phase switching field, where the aligned antiferroelectric (AFE) domains start to transform into the ferroelectric (FE) state, decreased with increasing temperature. On the other hand, the content of the FE phase in the AFE PZO thin films increased with increasing deposition temperature. A large recoverable energy-storage density of 16.8 J/cm3 and high energy-storage efficiency of 69.2% under an electric field of 1000 kV/cm were achieved in the films deposited at 525 °C. This performance was due to the high forward switching field and backward switching field values and the low difference between these two fields. Moreover, the PZO thin films showed great charge-discharge cycling life with fatigue-free performance up to 1010 cycles and good thermal stability from room temperature to 100 °C.

Functional oxides on silicon have been the subject of in-depth research for more than 20 years. Much of this research has been focused on the quality of the integration of materials due to their intrinsic thermodynamic incompatibility, which has hindered the flourishing of the field of research. Nevertheless, growth of epitaxial transition metal oxides on silicon with a sharp interface has been achieved by elaborated kinetically controlled sequential deposition while the crystalline quality of different functional oxides has been considerably improved. In this Research Update, we focus on three applications in which epitaxial ferroelectric oxides on silicon are at the forefront, and in each of these applications, other aspects of the integration of materials play an important role. These are the fields of piezoelectric microelectromechanical system devices, electro-optical components, and catalysis. The overview is supported by a brief analysis of the synthesis processes that enable epitaxial growth of oxides on silicon. This Research Update concludes with a theoretical description of the interfaces and the possibility of manipulating their electronic structure to achieve the desired coupling between (ferroelectric) oxides and semiconductors, which opens up a remarkable perspective for many advanced applications. © 2021 Author(s).

Polarization fatigue, i.e., the loss of polarization of ferroelectric capacitors upon field cycling, has been widely discussed as an interface related effect. However, mechanism(s) behind the development of fatigue have not been fully identified. Here, we study the fatigue mechanisms in Pt/PbZr0.52Ti0.48O3/SrRuO3 (Pt/PZT/SRO) capacitors in which all layers are fabricated by pulsed laser deposition without breaking the vacuum. With scanning transmission electron microscopy, we observed that in the fatigued capacitor, the Pt/PZT interface becomes structurally degraded, forming a 5 nm–10 nm thick non-ferroelectric layer of crystalline ZrO2 and diffused Pt grains. We then found that the fatigued capacitors can regain the full initial polarization switching if the externally applied field is increased to at least 10 times the switching field of the pristine capacitor. These findings suggest that polarization fatigue is driven by a two-step mechanism. First, the transient depolarization field that repeatedly appears during the domain switching under field cycling causes decomposition of the metal/ferroelectric interface, resulting in a non-ferroelectric degraded layer. Second, this interfacial non-ferroelectric layer screens the external applied field causing an increase in the coercive field beyond the usually applied maximum field and consequently suppresses the polarization switching in the cycled capacitor. Our work clearly confirms the key role of the electrode/ferroelectric interface in the endurance of ferroelectric-based devices.

The phenomena of hysteresis, ferroelectric loss, and nonlinearity are investigated for the strain and polarization of a monoclinic, epitaxial Pb(Zr,Ti)O3 film over the 70 Hz to 5 kHz frequency range at sub-coercive excitation fields and zero electrical bias. For the strain, a linear hysteretic behavior is found, whereas the polarization shows a strongly nonlinear hysteretic behavior. In contrast to polycrystalline structures (for instance in ceramics or chemical solution deposited thin films), the commonly referred Rayleigh model cannot explain the observed behavior. A new model is presented, based on the rotation of the polarization vector within the monoclinic or rhombohedral unit cell under an applied electric field, with the viscous interaction of domains accompanying the unit cell deformation. The model explains the amplitude and frequency scaling of the strain, polarization, and loss tangent as well as the observed higher harmonics of polarization in the measured epitaxial Pb(Zr,Ti)O3 films. It is concluded that the nonlinear response and the hysteretic loss originate from two separate physical processes. The nonlinear response is attributed to the nonlinear angular rotation of the polarization vector, whereas the hysteresis and ferroelectric loss are due to a viscous interaction of domains while the polarization vector is rotating.

Pulsed laser deposition is widely used to synthesize complex oxide thin films with advanced functional properties because of the versatility of the process, although the actual processes and mechanisms that take place are highly dynamic and nontrivial. Detailed understanding of the plume dynamics is required to achieve enhanced control of the growth of complex oxide thin films. However, analytical models of the plasma plume proposed in previous studies, the so-called shockwave model, drag model, and adiabatic thermalization model, only apply to a specific pressure regime and only focus on the propagation of the plasma front. Numerical modeling of the plasma dynamics has previously been pursued for the one-dimensional propagation of a Si plasma plume in a noble background gas. Here we have explored a more generalized numerical model for the dynamics of a ${\mathrm{TiO}}_{2}$ plasma plume by extending to three dimensions, multiple elements in the plasma plume, and including chemical reactions in an oxygen environment without the use of adaptive parameters, other than used for the description of the initial plume shape. Comparison between the simulations and the self-emission measurements of the ${\mathrm{TiO}}_{2}$ plasma plume shows good agreement. Our model enables detailed simulation of the oxidation state of the arriving particles (Ti, TiO, and ${\mathrm{TiO}}_{2}$) on the substrate surface depending on oxygen background pressure. Interestingly, low pressures of about 0.02 mbar result in fast oxygen particles arriving prior to the slower titanium particles, which could significantly influence the oxidation state of the initial substrate surface. The enhanced number of collisions for higher pressures of about 0.1 mbar leads to a large amount of the low-mass oxygen particles coming to a standstill 1--2 cm away from the ablated target. Furthermore, the three-dimensional nature of our model has enabled simulation of the lateral variations in composition of the deposited particles on the substrate surface. Although negligible variations in the Ti:TiO and Ti:${\mathrm{TiO}}_{2}$ ratios are present for high pressures over deposition areas with diameters up to 5 cm, significant variations can be observed for low pressures. These insights could play an important role in upscaling pulsed laser deposition from a scientific laboratory-based scale to an industrial large-area scale.

Magnetic domain engineering in ferromagnetic thin films is a very important route toward the rational design of spintronics and memory devices. Although the magnetic domain formation has been extensively studied, artificial control of magnetic domain remains challenging. Here, we present the control of magnetic domain formation in paradigmatic SrRuO3/SrTiO3 heterostructures via structural domain engineering. The formation of structural twin domains in SrRuO3 films can be well controlled by breaking the SrTiO3 substrate symmetry through engineering miscut direction. The combination of x-ray diffraction analysis of structural twin domains and magnetic imaging of reversal process demonstrates a one-to-one correspondence between structural domains and magnetic domains, which results in multi-step magnetization switching and anomalous Hall effect in films with twin domains. Our work sheds light on the control of the magnetic domain formation via structural domain engineering, which will pave a path toward desired properties and devices applications.

Reflection high-energy electron diffraction is a widely used tool to study the growth dynamics of thin films, in situ and operando. Here it is applied after deposition, revealing that the morphological state of the surface is connected to the amount of material underneath. We focus on the growth of ${\mathrm{LaAlO}}_{3}$ thin films on a ${\mathrm{SrTiO}}_{3}$ substrate by pulsed laser deposition, utilizing a geometrically anisotropic plasma plume. After deposition, oscillations in the intensity and width of the specular spot as a function of position are observed along the short axis of the plasma plume. Each complete oscillation represents a unit-cell difference in film thickness, as confirmed by local x-ray reflectivity measurements. We apply this approach to demonstrate the critical thickness for conductivity at the ${\mathrm{LaAlO}}_{3}/{\mathrm{SrTiO}}_{3}$ interface on a single sample. Our results introduce a straightforward method to engineer and study thickness-dependent properties of epitaxial thin films on a highly detailed level.

Pure perovskite phase, (001)-oriented, epitaxial thin films of (Pb(Mg1/3Nb2/3)O3)0.67-(PbTiO3)0.33 (PMN-PT) were fabricated on single crystal, (001)-oriented SrTiO3 substrates using a hard (Fe-doped) and soft doped (Nb-doped) PZT(52/48) interfacial layer. The effect of different interface layers on the structural and ferroelectric properties of the PMN-PT films was investigated in detail. A significant self-bias voltage in the PMN-PT films can be introduced by using an appropriate interfacial layer. There are significant differences in polarization for different types of doped and undoped interface layers and a doubling of the relative dielectric constant was observed for the Nb-doped interfacial layer. Device properties remain stable up to at least 108 cycles.

Integrating functional complex oxides with conventional (“non-oxide”) semiconductors emerges to be an important research field and has been attracting great interest. Because of their superior intrinsic material properties, such as a relatively high dielectric constant and polarization, the utilization of PbZr1- xTixO3 (PZT) materials as a dielectric layer is expected to greatly improve the performance of the GaN high electron mobility transistor. The functional PbZr1- xTixO3 exhibits quite different crystal structures and consequently physical properties depending on the composition. In this work we report the growth of full range of compositions of PZT films on MgO buffered GaN substrates. Besides revealing the temperature effect on phase formation and surface morphology, we demonstrated the strong effect of composition on the growth: pure (1 1 1) phase is formed in Ti-rich PZT (x > 0.48) while pyrochlore impurity phase is found in Zr-rich PZT (x < 0.48). By introducing an ultrathin Ti-rich PZT seed layer, we are able to achieve epitaxial growth of Zr-rich PZT. The epitaxial PZT films of different composition all exhibit good ferroelectric properties, showing great promise for future GaN device applications.

Origins of polarization fatigue in ferroelectric capacitors under electric field cycling still remain unclear. Here, we experimentally identify origins of polarization fatigue in ferroelectric PbZr0.52Ti0.48O3 (PZT) thin-film capacitors by investigating their fatigue behaviours and interface structures. The PZT layers are epitaxially grown on SrRuO3-buffered SrTiO3 substrates by a pulsed laser deposition (PLD), and the capacitor top-electrodes are various, including SrRuO3 (SRO) made by in-situ PLD, Pt by in-situ PLD (Pt-inPLD) and ex-situ sputtering (Pt-sputtered). We found that fatigue behaviour of the capacitor is directly related to the top-electrode/PZT interface structure. The Pt-sputtered/PZT/SRO capacitor has a thin defective layer at the top interface and shows early fatigue while the Pt-inPLD/PZT/SRO and SRO/PZT/SRO capacitor have clean top-interfaces and show much more fatigue resistance. The defective dielectric layer at the Pt-sputtered/PZT interface mainly contains carbon contaminants, which form during the capacitor ex-situ fabrication. Removal of this dielectric layer significantly delays the fatigue onset. Our results clearly indicate that dielectric layer at ferroelectric capacitor interfaces is the main origin of polarization fatigue, as previously proposed in the charge injection model.

The presence of a non-optically active polymorph (yellow-phase) competing with the optically active polymorph (black $\gamma$-phase) at room temperature in CsSnI3 and the susceptibility of Sn to oxidation, represent two of the biggest obstacles for the exploitation of CsSnI3 in optoelectronic devices. Here room-temperature single-source in vacuum deposition of smooth black $\gamma$ - CsSnI3 thin films is reported. This has been done by fabricating a solid target by completely solvent-free mixing of CsI and SnI2 powders and isostatic pressing. By controlled laser ablation of the solid target on an arbitrary substrate at room temperature, the formation of CsSnI3 thin films with optimal optical properties is demonstrated. The films present a band gap of 1.32 eV, a sharp absorption edge and near-infrared photoluminescence emission. These properties and X-ray diffraction of the thin films confirmed the formation of the orthorhombic (B-$\gamma$) perovskite phase. The thermal stability of the phase was ensured by applying in situ an Al2O$_3$ capping layer. This work demonstrates the potential of pulsed laser deposition as a volatility-insensitive single-source growth technique of halide perovskites and represents a critical step forward in the development and future scalability of inorganic lead-free halide perovskites., Comment: Accepted by Advanced Materials Interfaces, 16 pages, 4 figures, and supplement

Controlling the crystalline structure of hafnium zirconate and its epitaxial relationship to a semiconducting electrode has high technological interest, as ferroelectric materials are key ingredients for emerging electronic devices. Using pulsed laser deposition, a phase-pure, ultrathin film of HfZrO4 is grown epitaxially on a GaN(0001)/Si(111) template. Since standard microscopy techniques do not allow us to determine with certitude the crystalline structure of the film due to the weak scattering of oxygen, differentiated differential phase contrast scanning transmission electron microscopy is used to allow the direct imaging of oxygen columns in the film. Combined with x-ray diffraction analysis, the polar nature and rhombohedral R3 symmetry of the film are demonstrated.

Despite its interest for CMOS applications, Atomic Layer Deposition (ALD) of GeO$_{2}$ thin films, by itself or in combination with SiO$_{2}$, has not been widely investigated yet. Here we report the ALD growth of SiO$_{2}$/GeO$_{2}$ multilayers on Silicon substrates using a so far unreported Ge precursor. The characterization of multilayers with various periodicities reveals successful layer-by-layer growth with electron density contrast and absence of chemical intermixing, down to a periodicity of 2 atomic layers., This manuscript has been submitted to Applied Physics Letters

The integration of oxides on Si remains challenging, which largely hampers the practical applications of oxide-based electronic devices with superior performance. Recently, $\mathrm{LaMn}{\mathrm{O}}_{3}/\mathrm{SrTi}{\mathrm{O}}_{3}$ (LMO/STO) heterostructures have gained renewed interest for the debating origin of the ferromagnetic-insulating ground state as well as for their spin-filter applications. Here we report on the structural and magnetic properties of high-quality LMO/STO heterostructures grown on silicon. The chemical abruptness across the interface was investigated by atomic-resolution scanning transmission electron microscopy. The difference in the thermal expansion coefficients between LMO and Si imposed a large biaxial tensile strain to the LMO film, resulting in a tetragonal structure with $c/a\ensuremath{\sim}0.983$. Consequently, we observed a significantly suppressed ferromagnetism along with an enhanced coercive field, as compared to the less distorted LMO film ($c/a\ensuremath{\sim}1.004$) grown on STO single crystal. The results are discussed in terms of tensile-strain enhanced antiferromagnetic instabilities. Moreover, the ferromagnetism of LMO on Si sharply disappeared below a thickness of 5 unit cells, in agreement with the LMO/STO case, pointing to a robust critical behavior irrespective of the strain state. Our results demonstrate that the growth of oxide films on Si can be a promising way to study the tensile-strain effects in correlated oxides, and also pave the way towards the integration of multifunctional oxides on Si with atomic-layer control.

Epitaxial growth of SrTiO3 (STO) on silicon greatly accelerates the monolithic integration of multifunctional oxides into the mainstream semiconductor electronics. However, oxide superlattices (SLs), the birthplace of many exciting discoveries, remain largely unexplored on silicon. In this work, LaNiO3/LaFeO3 SLs are synthesized on STO-buffered silicon (Si/STO) and STO single-crystal substrates, and their electronic properties are compared using dc transport and X-ray absorption spectroscopy. Both sets of SLs show a similar thickness-driven metal-to-insulator transition, albeit with resistivity and transition temperature modified by the different amounts of strain. In particular, the large tensile strain promotes a pronounced Ni (Formula presented.) orbital polarization for the SL grown on Si/STO, comparable to that reported for LaNiO3 SL epitaxially strained to DyScO3 substrate. Those results illustrate the ability to integrate oxide SLs on silicon with structure and property approaching their counterparts grown on STO single crystal, and also open up new prospects of strain engineering in functional oxides based on the Si platform. © 2020 The Authors. Advanced Materials published by Wiley-VCH GmbH

It is important to understand the effect of the interfaces between the oxide electrode layers and the ferroelectric layer on the polarization response for optimizing the device performance of all-oxide ferroelectric devices. Herein, the effects of the oxide La0.07Ba0.93SnO3 (LBSO) as an electrode material in an PbZr0.52Ti0.48O3 (PZT) ferroelectric capacitor are compared with those of the more commonly used SrRuO3 (SRO) electrode. SRO (top)/PZT/SRO (bottom), SRO/PZT/LBSO, and SRO/PZT/2 nm SRO/LBSO devices are fabricated. Only marginal differences in crystalline properties, determined by X-ray diffraction and scanning transmission electron microscopy, are found. High-quality polarization loops are obtained, but with a much larger coercive field for the SRO/PZT/LBSO device. In contrast to the SRO/PZT/SRO device, the polarization decreases strongly with increasing field cycling. This fatigue problem can be remedied by inserting a 2 nm SRO layer between PZT and LBSO. It is argued that strongly increased charge injection into the PZT occurs at the bottom interface, because of the low PZT/LBSO interfacial barrier and the much lower carrier density in LBSO, as compared with that in SRO, causing a low dielectric constant, depleted layer in LBSO. The charge injection creates a trapped space charge in the PZT, causing the difference in fatigue behavior.

We report the energy-storage performance and electric breakdown field of antiferroelectric PbZrO3 (PZ) and relaxor ferroelectric Pb0.9La0.1(Zr0.52Ti0.48)O3 (PLZT) single films, as well as PLZT/PZ and PZ/PLZT heterolayered films grown on SrRuO3/Ca2Nb3O10–nanosheet/Si substrates using pulsed laser deposition. These films show the highly textured (001) orientation. The ‘square’ hysteresis loop with very sharp electric field–induced antiferroelectric–ferroelectric (AFE–FE) phase transition is observed for the PZ/Si film, meanwhile the heterolayerd PLZT/PZ/Si and PZ/PLZT/Si films show the ‘slanted’ hysteresis loops with gradual phase transition. Moreover, the electric field-induced AFE-FE phase transition in the hererolayered films is occurred at lower applied electric fields (~275 kV/cm) than that in the PZ/Si (~425 kV/cm), due to the presence of the PLZT layers in the heterolayered films. Owing to the dense structure in PLZT layer, the large electric breakdown strength of 2000 and 1825 kV/cm, and then the high recoverable energy-storage density of 28.8 and 23.8 J/cm3, respectively, are obtained for the PLZT/Si and PZ/PLZT/Si films.

Thin relaxor-ferroelectric Pb0.9La0.1(Zr0.52Ti0.48)O3 (PLZT) films were deposited on Si substrates using Ca2Nb3O10 (CNOns) and Ti0.87O2 (TiOns) nanosheets as the growth template layer and SrRuO3 (SRO) as the base electrode layer, using pulsed laser deposition. XRD and cross-sectional SEM results show that the structure of the PLZT layers changes from very dense with (001)-orientation to columnar with (110)-orientation for CNOns and TiOns, respectively. The recoverable energy-storage density (Ureco) is nearly proportional to the critical electric breakdown field (EBD), which increases with PLZT film thickness. A very high Ureco value of 58.4 J cm-3 and energy-storage efficiency (η) of 81.2% were obtained at an EBD of 3400 kV cm-1 for the 1000 nm thick PLZT film on CNOns/Si, significantly higher than for the film on TiOns/Si (Ureco = 44.0 J cm-3 and η = 59.6% for EBD = 2800 kV cm-1). This excellent energy storage performance in the PLZT/SRO/CNOns/Si is due to the dense film structure and nearly hysteresis-free relaxor behavior. These results are important for improving the performance of relaxor-ferroelectric thin films for high-power capacitor applications.

The hysteresis, loss, and nonlinearity of the strain and polarization response of an epitaxial PbZr0.55Ti0.45O3 film are experimentally investigated for non-switching AC excitation fields at a DC bias of 20 kV cm−1 in the 70 Hz to 5 kHz range. The measured strain is hysteretic and linear, whereas the polarization is hysteretic and highly nonlinear with excitation amplitude. Furthermore, compared to the case with zero bias, the effective piezoelectric coefficient that is extracted from the strain response is almost not changed for the investigated field range. In contrast, the loss tangent and nonlinearity of the polarization response are strongly reduced. The observations can not be explained by the Rayleigh model and its extensions, but are very well explained by the recently proposed polarization rotation model through addition of a non-zero bias field term to the model. This model describes the film properties as the result of the nonlinear rotation of the polarization vector within the unit-cell in response to the applied field, which is accompanied with viscous domain interaction. These results demonstrate that the polarization rotation model can describe the film response in a broad range of excitation frequencies and amplitudes, which far the applicable range of the Rayleigh model.

Nanosheet Ca2Nb3O10 (CNOns) layers were deposited on ultralow expansion glass substrates by the Langmuir–Blodgett method to obtain preferential (001)-oriented growth of Pb(Zr0.52Ti0.48)O3 (PZT) thin films using pulsed laser deposition (PLD) to enhance the ferroelectric and piezoelectric properties of the films. The PLD deposition temperature and repetition frequency used for the deposition of the PZT films were found to play a key role in the precise control of the microstructure and therefore of the ferroelectric and piezoelectric properties. A film deposited at a high repetition frequency has a columnar grain structure, which helps to increase the longitudinal piezoelectric coefficient (d33f). An enhanced d33f value of 356 pm V–1 was obtained for 2-μm-thick PZT films on CNOns/glass substrates. This high value is ascribed to the preferential alignment of the crystalline [001] axis normal to the substrate surface and the open columnar structure. Large displacement actuators based on such PZT films grown on CNOns/glass substrates should be useful in smart X-ray optics applications.

An anisotropic double exchange interaction driven giant transport anisotropy is demonstrated in a canonic double exchange system of La2/3Sr1/3MnO3 ultrathin films epitaxially grown on NdGaO3 (110) substrates. The oxygen octahedral coupling at the La2/3Sr1/3MnO3/NdGaO3 interface induces a planar anisotropic Mn-O-Mn bond bending, which causes a significant anisotropic overlap of neighboring Mn orbitals. Due to the anisotropic double exchange interaction, it is found that the conductivity of the La2/3Sr1/3MnO3 film is enhanced when current is applied along the in-plane short crystalline axis. However, the anisotropic behavior is absent in the high temperature paramagnetic phase. Our results demonstrate anisotropic transport in the clean limit where phase separation is absent and the role of anisotropic phase percolation can be excluded.

Relaxor ferroelectric Pb0.9La0.1(Zr0.52Ti0.48)O3 (PLZT) thin films have been epitaxially grown via pulsed laser deposition on SrRuO3/SrTiO3 single crystal with different orientations. The high recoverable energy-storage density and energy-storage efficiency in the epitaxial PLZT thin films are mainly caused by the coexistence of relaxor and antiferroelectric-like behaviors. The recoverable energy-storage density of 12.03, 12.51 and 12.74 J/cm3 and energy-storage efficiency of 86.50, 88.14 and 88.44%, respectively, for the PLZT(001), PLZT(011) and PLZT(111) thin films measured at 1000 kV/cm. The high energy density and high efficiency indicate that the relaxor epitaxial PLZT(111) thin film is a promising candidate for high pulsed power capacitors.

Pb(Zr0.52Ti0.48)O3 (PZT) films with (001) orientation were deposited on Pt(111)/Ti/SiO2/Si(100) substrates using pulsed laser deposition. Variation of the laser pulse rate during the deposition of the PZT films was found to play a key role in the control of the microstructure and to change strongly the piezoelectric response of the thin film. The film deposited at low pulse rate has a denser columnar microstructure, which improves the transverse piezoelectric coefficient (d31f) and ferroelectric remanent polarization (Pr), whereas the less densely packed columnar grains in the film deposited at high pulse rates give rise to a significantly higher longitudinal piezoelectric coefficient (d33f) value. The effect of film thickness on the ferroelectric and piezoelectric properties of the PZT films was also investigated. With increasing film thickness, the grain column diameter gradually increases, and also the average Pr and d33f values become larger. The largest piezoelectric coefficient of d33f = 408 pm V–1 was found for a 4-μm film thickness. From a series of films in the thickness range 0.5–5 μm, the z-position dependence of the piezoelectric coefficient could be deduced. A local maximum value of 600 pm V–1 was deduced in the 3.5–4.5 μm section of the thickest films. The dependence of the film properties on film thickness is attributed to the decreasing effect of the clamping constraint imposed by the substrate and the increasing spatial separation between the grains with increasing film thickness.

Extreme ultraviolet and soft x-ray wavelengths have ever-increasing applications in photolithography, imaging, and spectroscopy. Adaptive schemes for wavefront correction at such a short wavelength range have recently gained much attention. In this Letter we report, to the best of our knowledge, the first demonstration of a functional actuator based on piezoelectric thin films. We introduce a new approach that allows producing a gradually varying surface deformation. White light interferometery is used to show the level of control in generating arbitrary surface profiles at the nanoscale.

The two-dimensional electron liquid which forms between the band insulators LaAlO3 (LAO) and SrTiO3 (STO) is a promising component for oxide electronics, but the requirement of using single crystal SrTiO3 substrates for the growth limits its applications in terms of device fabrication. It is therefore important to find ways to deposit these materials on other substrates, preferably Si, or Si-based, in order to facilitate integration with existing technology. Interesting candidates are micron-sized nanosheets of Ca2Nb3O10 which can be used as seed layers for perovskite materials on any substrate. We have used low-energy electron microscopy (LEEM) with in-situ pulsed laser deposition to study the subsequent growth of STO and LAO on such flakes which were deposited on Si. We can follow the morphology and crystallinity of the layers during growth, as well as fingerprint their electronic properties with angle resolved reflected electron spectroscopy. We find that STO layers, deposited on the nanosheets, can be made crystalline and flat; that LAO can be grown in a layer-by-layer fashion; and that the full heterostructure shows the signature of the formation of a conducting interface., 11 pages, 7 figures

Normal-ferroelectric Pb(Zr0.52Ti0.48)O3 (PZT) and relaxor-ferroelectric Pb0.9La0.1(Zr0.52Ti0.48)O3 (PLZT) thin-films are deposited on SrRuO3-covered SrTiO3/Si substrates. An ultrahigh recoverable energy-storage density (Ureco) of 68.2 J/cm3 and energy efficiency (η) of 80.4% are achieved in the PLZT thin-films under a large breakdown strength (EBD) of 3600 kV/cm. These values are much lower in the PZT thin-films (Ureco of 10.3 J/cm3 and η of 62.4% at EBD of 1000 kV/cm). In addition, the remanent polarization (Pr) and dielectric-constant are also investigated to evaluate the breakdown strength in thin-films. Polar nano-regions (PNRs) are created in the PLZT thin-films to enable relaxor behavior and lead to slim polarization loops along with very small Pr. The excellent operating temperature of energy-storage performance and also the breakdown strength obtained in the PLZT thin-films are mainly ascribed to the presence of PNRs. Moreover, both PZT and PLZT thin-films exhibit superior performance up to 1010 times of charge-discharge cycling.

Vanadium dioxide (VO2) is a much-discussed material for oxide electronics and neuromorphic computing applications. Here, heteroepitaxy of VO2 is realized on top of oxide nanosheets that cover either the amorphous silicon dioxide surfaces of Si substrates or X-ray transparent silicon nitride membranes. The out-of-plane orientation of the VO2 thin films is controlled at will between (011)M1/(110)R and (−402)M1/(002)R by coating the bulk substrates with Ti0.87O2 and NbWO6 nanosheets, respectively, prior to VO2 growth. Temperature-dependent X-ray diffraction and automated crystal orientation mapping in microprobe transmission electron microscope mode (ACOM-TEM) characterize the high phase purity, the crystallographic and orientational properties of the VO2 films. Transport measurements and soft X-ray absorption in transmission are used to probe the VO2 metal–insulator transition, showing results of a quality equal to those from epitaxial films on bulk single-crystal substrates. Successful local manipulation of two different VO2 orientations on a single substrate is demonstrated using VO2 grown on lithographically patterned lines of Ti0.87O2 and NbWO6 nanosheets investigated by electron backscatter diffraction. Finally, the excellent suitability of these nanosheet-templated VO2 films for advanced lensless imaging of the metal–insulator transition using coherent soft X-rays is discussed.

Non-coplanar spin textures with scalar spin chirality can generate effective magnetic field that deflects the motion of charge carriers, resulting in topological Hall effect (THE), a powerful probe of the ground state and low-energy excitations of correlated systems. However, spin chirality fluctuation in two-dimensional ferromagnets with perpendicular anisotropy has not been considered in prior studies. Herein, we report direct evidence of universal spin chirality fluctuation by probing the THE above the transition temperatures in two different ferromagnetic ultra-thin films, SrRuO$_3$ and V doped Sb$_2$Te$_3$. The temperature, magnetic field, thickness, and carrier type dependences of the THE signal, along with our Monte-Carlo simulations, unambiguously demonstrate that the spin chirality fluctuation is a universal phenomenon in two-dimensional Ising ferromagnets. Our discovery opens a new paradigm of exploring the spin chirality with topological Hall transport in two-dimensional magnets and beyond, Comment: accepted by nature materials

To control the pulsed laser deposition synthesis, knowledge on the relationship between the plasma plume and the grown thin film is required. We show that the oxidation of species in the plasma plume still affects the SrVO3 growth even at low oxygen partial pressures. Optical emission spectroscopy measurements for the plasma plume at different growth conditions were correlated with the film properties determined by Atomic force microscopy, X-ray diffraction, and transport. At reducing oxygen pressures, the background argon pressure can affect the oxidation in the plasma plume, which in turn controls the growth kinetics, stoichiometry, and electrical properties of the films.

Lead-free (1-x)Bi0.5Na0.4K0.2TiO3-xBiFeO3 (abbreviated as BNKT-xBFO) ferroelectric films with x in the range from 0.00 to 0.10, were synthesized by the chemical solution deposition technique on Pt/Ti/SiO2/Si substrates. The microstructures and magnetic behaviors of BNKT-xBFO films were analyzed in detail as a function of BFO concentration. X-ray diffraction patterns indicated that BNKT-xBFO films were grown with a single-phase perovskite structure. The pure films showed an antiferromagnetic behavior. The magnetic properties of the films were gradually transferred from antiferromagnetic to ferromagnetic properties when BFO concentration was raised. The saturated magnetization (M S) reached the highest value of 10.3 emu cm−3 at the BFO-doped concentration x = 0.10. Our work will contribute to illuminate the impact of BFO (ABO3 perovskite structure) on the magnetic properties of BNKT materials at room temperature.

Ferroelectric domain formation is an essential feature in ferroelectric thin films. These domains and domain walls can be manipulated depending on the growth conditions. In rhombohedral BiFeO3 thin films, the ordering of the domains and the presence of specific types of domain walls play a crucial role in attaining unique ferroelectric and magnetic properties. In this study, controlled ordering of domains in BiFeO3 film is presented, as well as a controlled selectivity between two types of domain walls is presented, i.e., 71 degrees and 109 degrees, by modifying the substrate termination. The experiments on two different substrates, namely SrTiO3 and TbScO3, strongly indicate that the domain selectivity is determined by the growth kinetics of the initial BiFeO3 layers.

Epitaxial (PbMg1/3Nb2/3O3)2/3-(PbTiO3)1/3 (PMN-PT) films with different out-of-plane orientations were prepared using a CeO2/yttria stabilized ZrO2 bilayer buffer and symmetric SrRuO3 electrodes on silicon substrates by pulsed laser deposition. The orientation of the SrRuO3 bottom electrode, either (110) or (001), was controlled by the deposition conditions and the subsequent PMN-PT layer followed the orientation of the bottom electrode. The ferroelectric, dielectric and piezoelectric properties of the (SrRuO3/PMN-PT/SrRuO3) ferroelectric capacitors exhibit orientation dependence. The properties of the films are explained in terms of a model based on polarization rotation. At low applied fields domain switching dominates the polarization change. The model indicates that polarization rotation is easier in the (110) film, which is ascribed to a smaller effect of the clamping on the shearing of the pseudo-cubic unit cell compared to the (001) case.

Thin film capacitors of the lead-free (K0.5Na0.5)NbO3 (KNN) with (100) orientation were grown on Pt/Ti/SiO2/SOI (silicon-on-insulator) substrates by pulsed laser deposition. The films are pure phases and do not show other crystal orientations. The remnant polarization Pr, saturation polarization Psat, longitudinal d33,f and transverse (d31,f and e31,f) piezoelectric coefficients of the KNN films were determined (Pr=12.6 µC/cm2, Psat=25.0 µC/cm2, d33,f=58 pm/V, d31,f=−42 pm/V and e31,f=−5.6 C/m2). These values are well comparable with the highest values reported for lead-free films of different compositions and therefore these KNN films form a potential alternative to PZT films in lead-free MEMS applications.

The layered perovskite-type niobate KCa2Nb3O10 and its derivatives show advantages in several fields, such as templated film growth and (photo)catalysis. Conventional synthesis routes generally yield crystal size smaller than 2 μm. We report a flux synthesis method to obtain KCa2Nb3O10 crystals with significantly larger sizes. By using different flux materials (K2SO4 and K2MoO4), crystals with average sizes of 8 and 20 μm, respectively, were obtained. The KCa2Nb3O10 crystals from K2SO4 and K2MoO4 assisted synthesis were protonated and exfoliated into monolayer nanosheets, and the optimal exfoliation conditions were determined. Using pulsed laser deposition, highly (001)-oriented piezoelectric stacks (SrRuO3/PbZr0.52Ti0.48O3/SrRuO3, SRO/PZT/SRO) were deposited onto Langmuir-Blodgett films of Ca2Nb3O10- (CNO) nanosheets with varying lateral nanosheet sizes on Si substrates. The resulting PZT thin films showed high crystallinity irrespective of nanosheet size. The small sized nanosheets yielded a high longitudinal piezoelectric coefficient d33 of 100 pm/V, while the larger sized sheets had a d33 of 72 pm/V. An enhanced transverse piezoelectric coefficient d31 of -107 pm/V, an important input parameter for the actuation of active structures in microelectromechanical systems (MEMS) devices, was obtained for PZT films grown on CNO nanosheets with large lateral size, while the corresponding value on small sized sheets was -96 pm/V.

Near-infrared absorption in transparent conducting oxides (TCOs) is usually caused by electronic intraband transition at high doping levels. Improved infrared transparency is commonly explained by enhanced drift mobility in these TCOs. Here, an alternative cause behind the high infrared transparency of La-doped barium stannate (LBSO) transparent electrodes is presented. Following the Drude model formalism, we reconstructed spectrally resolved dielectric permittivity for a set of thin films with different free electron concentrations. A comparison of optical properties of LBSO with the tin-doped indium oxide thin films with identical carrier concentrations suggests that the redshift of the screened plasma wavelength for LBSO originates from its large high-frequency dielectric constant of 4.4, one of the highest reported for the s-orbital-based TCOs. Moreover, our measurements confirm an optical mobility significantly higher (>300 cm2/V s) than the drift mobility, effectively suppressing the free carrier absorption. These factors enable high infrared transparency of LBSO films and motivate further exploration of LBSO as broadband TCOs for solar cells and nanophotonics.

The energy-storage performance and piezoelectric properties were determined for epitaxial antiferroelectric (AFE) PbZrO3 (PZ), ferroelectric (FE) PbZr0.52Ti0.48O3 (PZT), and relaxor ferroelectric (RFE) Pb0.9La0.1Zr0.52Ti0.48O3 (PLZT) thin films that were deposited on to SrTiO3 buffered Si substrates. The films were investigated by directly measuring the polarization hysteresis loops and piezoelectric strain curves. The square polarization loop with a high remanent polarization and a large piezoelectric coefficient obtained in PZT thin films allow them to be useful for various applications in ferroelectric field effect transistors and/or in MEMS actuators. Meanwhile, there is a jump of about 0.9% in the strain curve of PZ thin films around the field-induced AFE-FE phase transition, which is useful in digital displacement transducers due to a good ON/OFF strain state. The large recoverable energy-storage density, excellent energy-storage efficiency, and low strain hysteresis due to a slim hysteresis loop combine to make PLZT thin films as a potential candidate for a broad range of applications from energy storage to nano-positioning precision systems.

In transition metal perovskites ABO(3), the physical properties are largely driven by the rotations of the BO6 octahedra, which can be tuned in thin films through strain and dimensionality control. However, both approaches have fundamental and practical limitations due to discrete and indirect variations in bond angles, bond lengths, and film symmetry by using commercially available substrates. Here, we introduce modulation tilt control as an approach to tune the ground state of perovskite oxide thin films by acting explicitly on the oxygen octahedra rotation modes-that is, directly on the bond angles. By intercalating the prototype SmNiO3 target material with a tilt-control layer, we cause the system to change the natural amplitude of a given rotation mode without affecting the interactions. In contrast to strain and dimensionality engineering, our method enables a continuous fine-tuning of the materials' properties. This is achieved through two independent adjustable parameters: the nature of the tilt-control material (through its symmetry, elastic constants, and oxygen rotation angles), and the relative thicknesses of the target and tilt-controlmaterials. As a result, a magnetic and electronic phase diagram can be obtained, normally only accessible by A-site element substitution, within the single SmNiO3 compound. With this unique approach, we successfully adjusted the metal-insulator transition (MIT) to room temperature to fulfill the desired conditions for optical switching applications.

Just Accepted Manuscript, In the present work, we study the hysteretic behavior in the electric-field-dependent capacitance and the current characteristics of 0.5Ba(Zr0.2Ti0.8)O3-0.5(Ba0.7Ca0.3)TiO3 (BCZT)/ZnO bilayers deposited on 0.7 wt % Nb-doped (001)-SrTiO3 (Nb:STO) substrates in a metal-ferroelectric-semiconductor (MFS) configuration. The X-ray diffraction measurements show that the BCZT and ZnO layers are highly oriented along the c-axis and have a single perovskite and wurtzite phases, respectively, whereas high-resolution transmission electron microscopy revealed very sharp Nb:STO/BCZT/ZnO interfaces. The capacitance-electric field ( C- E) characteristics of the bilayers exhibit a memory window of 47 kV/cm and a capacitance decrease of 22%, at a negative bias. The later result is explained by the formation of a depletion region in the ZnO layer. Moreover, an unusual resistive switching (RS) behavior is observed in the BCZT films, where the RS ratio can be 500 times enhanced in the BCZT/ZnO bilayers. The RS enhancement can be understood by the barrier potential profile modulation at the depletion region, in the BCZT/ZnO junction, via ferroelectric polarization switching of the BCZT layer. This work builds a bridge between the hysteretic behavior observed either in the C- E and current-electric field characteristics on a MFS structure., Portuguese Foundation for Science and Technology (FCT) in the framework of the Strategic Funding UID/FIS/04650/2013 and (ii) Project Norte-070124-FEDER-000070 Nanomateriais Multifuncionais. This research was partially supported by the COST Action MP1308 "Towards Oxide-Based Electronics (TO-BE)". The authors acknowledge the CERIC-ERIC Consortium for access to experimental facilities and financial support under proposal 20157018. The author J.P.B.S. is grateful for financial support through the FCT Grant SFRH/BPD/92896/2013. The author K.C.S. acknowledge UGC and DST-SERB, Govt. of India for the funds through the grant No.F.4-5(59-FRP/2014(BSR)) and ECR/2017/000068, respectively. The authors R.F.N. and C.G. acknowledge the financial support from Romanian Ministry of Research and Innovation in the frame of the Core Program PN18-11, info:eu-repo/semantics/publishedVersion

The epitaxial growth of yttria-stabilized zirconia (YSZ) on silicon with native oxide was investigated in order to gain more insight in the growth mechanism. Specifically, attention was paid to the possibilities to control the chemical interactions between YSZ, silicon and oxygen during initial growth. The sources of oxygen during growth proved to play an important role in the growth process, as shown by individual manipulation of all sources present during Pulsed Laser Deposition. Partial oxidation of the YSZ plasma and sufficient delivery of oxygen to the growing film were necessary to prevent silicide formation and obtain optimal YSZ crystalline qualities. In these conditions, thickness increase of the silicon native oxide before growth just started to occur, while a much faster regrowth of silicon oxide at the YSZ-Si interface occurred during growth. Control of all these contributions to the growth process is necessary to obtain reproducible growth of high quality YSZ.

The relaxor ferroelectric Pb 0.9 La 0.1 (Zr 0.52 Ti 0.48 )O 3 (PLZT) thin films were deposited using pulsed laser deposition, and their microstructures, break-down field strengths and energy storage performances were investigated as a function of the buffer layer and electrode. A large recoverable energy-storage density ( U reco ) of 23.2 J/cm 3 and high energy-storage efficiency ( η ) of 91.6% obtained in the epitaxial PLZT film grown on SrRuO 3 /SrTiO 3 /Si are much higher than those in the textured PLZT film ( U reco = 21.9 J/cm 3 , η = 87.8%) on SrRuO 3 /Ca 2 Nb 3 O 10 -nanosheet/Si and the polycrystalline PLZT film ( U reco = 17.6 J/cm 3 , η = 82.6%) on Pt/Ti/SiO 2 /Si, under the same condition of 1500 kV/cm and 1 kHz, due to the slim polarization loop and significant antiferroelectric-like behavior. Owing to the high break-down strength (BDS) of 2500 kV/cm, a giant U reco value of 40.2 J/cm 3 was obtained for the epitaxial PLZT film, in which U reco values of 28.4 J/cm 3 (at BDS of 2000 kV/cm) and 20.2 J/cm 3 (at BDS of 1700 kV/cm), respectively, were obtained in the textured and polycrystalline PLZT films. The excellent fatigue-free properties and high thermal stability were also observed in these films.