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The manipulation of low-energy matter properties such as superconductivity, ferromagnetism, and ferroelectricity via cavity quantum electrodynamics engineering has been suggested as a way to enhance these many-body collective phenomena. In this work, we investigate the effective interactions between low-energy matter excitations induced by the off-resonant coupling with cavity electromagnetic modes. We extend a previous work by going beyond the dipole approximation accounting for the full polarization and magnetization densities of matter. We further include the often neglected diamagnetic interaction and, for the cavity, we consider general linear absorbing media with possibly non-local and non-reciprocal response. We demonstrate that, even in this general scenario, the effective cavity-induced interactions between the matter degrees of freedom are of electrostatic and magnetostatic nature. This confirms the necessity of a multimode description for cavity engineering of matter systems where the low-energy assumption holds. Our findings provide a theoretical framework for studying the influence of general optical environments on extended low-energy matter excitations. [ABSTRACT FROM AUTHOR]

Two-dimensional ferroelectric materials are beneficial for power-efficient memory devices and transistor applications. Here, we predict out-of-plane ferroelectricity in a new family of buckled metal oxide (MO; M: Ge, Sn, Pb) monolayers with significant spontaneous polarization. Additionally, these monolayers have a narrow valence band, which is energetically separated from the rest of the low-lying valence bands. Such a unique band structure limits the long thermal tail of the hot carriers, mitigating subthreshold thermionic leakage and allowing field-effect transistors (FETs) to function beyond the bounds imposed on conventional FETs by thermodynamics. Our quantum transport simulations reveal that the FETs based on these MO monolayers exhibit a large ON/OFF ratio with an average subthreshold swing of less than 60 mV/decade at room temperature, even for short gate lengths. Our work motivates further exploration of the MO monolayers for developing advanced, high-performance memory and logic devices. [ABSTRACT FROM AUTHOR]

Despite the extensive research on HfO2-based thin films, the ferroelectric orthorhombic phase formation remains unclear. This work proposes a physical picture throughout the entire annealing process to describe the phase transition. Subsequently, the phase evolution at various doping and annealing temperatures is illustrated based on a kinetic model formalized from the classical nucleation theory. It is found that the formation of the ferroelectric orthorhombic phase depends not only on a modest doping concentration but also on the thermal activation of the t-to-o phase transition provided by a sufficient annealing temperature. In addition, phase transition rates correlated to the monoclinic phase formation are effectively suppressed by doping. The exploration of combined effects of annealing parameters indicates a more decisive role of the annealing temperature rather than the keeping time for induced ferroelectricity, and the doping impact becomes significant when a critical annealing temperature is reached. This work provides an understanding for exploring the kinetic effect on the phase transition in HfO2-based thin films, which helps improve ferroelectricity in doped HfO2 ferroelectric films. [ABSTRACT FROM AUTHOR]

Recent studies have shown that proximity effects are able to substantially modulate the superconducting properties of various quasi-two-dimensional layered materials such as FeSe, FeSeTe, NbSe2, and NbS2. Due to their high surface charge concentration and high dielectric constants, ferroelectric materials provide an interesting avenue for inducing proximity effects in layered superconductors. In this study, we explore the interactions between FeSeTe and the two-dimensional ferroelectrics CuInP2S6 and CuInP2Se6. We found that contrary to the normal behavior of FeSeTe, FeSeTe/CuInP2S6, and FeSeTe/CuInP2Se6 heterostructures display a peculiar two-step superconducting transition. Further testing revealed a hysteresis loop in the IV curves of these samples when measured below the critical temperature indicating the presence of disorder and domains within FeSeTe. We conclude that these domains are responsible for the two-step transition in FeSeTe and hypothesize that they are induced by the domain structure of the aforementioned ferroelectric materials. [ABSTRACT FROM AUTHOR]

Improving piezoelectric and ferroelectric responses of group III-nitrides is desired for their potential applications in the emerging microelectromechanical-based systems. One possible approach to realize the optimization and control of functionalities is to bring together compounds with different properties to form the ordered multilayer superlattices. In this work, we systematically investigate the phase stability, piezoelectricity, and ferroelectricity in a class of wurtzite-structure-derived nitride superlattices with a periodic alternation of chemically and/or structurally different layers. The structural heterogeneity and phase stability of the ordered wurtzite-structure-derived superlattices are intimately related to the ionic radii mismatch between the substitutional compounds and the parent nitrides. Moreover, the internal structural distortion of the nitride superlattices has a crucial impact on the ferroelectricity and piezoelectricity, namely, piezoelectric and ferroelectric responses become increasingly enhanced as the buckled atomic layers becomes flatter. This work offers fundamental physical insights into the structure–property relationships in nitride superlattices and may propose some material design strategies for achieving high-performance materials with desired responses. [ABSTRACT FROM AUTHOR]

Ferroelectric properties of hafnium-based thin films have gained significant interest, yet the fundamental mechanisms responsible for the emergence of the ferroelectric phase continue to be inadequately investigated. In contrast with polycrystalline films fabricated by atomic layer deposition or sputter methods, which possess uncertainty in polarization orientation, epitaxial ferroelectric HfO2-based materials are less investigated, especially for factors such as electric field and oxygen vacancy, which are proposed and examined for their potential impacts on phase stability. In this study, Y-doped hafnium oxide (HYO) ferroelectric epitaxial films were fabricated using pulsed laser deposition, with variations in oxygen pressure during the deposition process. Structural and electrical analyses of HYO epitaxial ferroelectric films prepared under differing oxygen pressures revealed a correlation between the ferroelectric properties of the films and the oxygen content. An optimal selection of oxygen pressure was found to be conducive to the formation of HYO epitaxial ferroelectric films, presenting a promising avenue for future ferroelectric memory applications. [ABSTRACT FROM AUTHOR]

Ferroelectric properties of hafnium-based thin films have gained significant interest, yet the fundamental mechanisms responsible for the emergence of the ferroelectric phase continue to be inadequately investigated. In contrast with polycrystalline films fabricated by atomic layer deposition or sputter methods, which possess uncertainty in polarization orientation, epitaxial ferroelectric HfO2-based materials are less investigated, especially for factors such as electric field and oxygen vacancy, which are proposed and examined for their potential impacts on phase stability. In this study, Y-doped hafnium oxide (HYO) ferroelectric epitaxial films were fabricated using pulsed laser deposition, with variations in oxygen pressure during the deposition process. Structural and electrical analyses of HYO epitaxial ferroelectric films prepared under differing oxygen pressures revealed a correlation between the ferroelectric properties of the films and the oxygen content. An optimal selection of oxygen pressure was found to be conducive to the formation of HYO epitaxial ferroelectric films, presenting a promising avenue for future ferroelectric memory applications. [ABSTRACT FROM AUTHOR]

Ferroelectric HfO2-based thin films have attracted much interest in the utilization of ferroelectricity at the nanoscale for next-generation electronic devices. However, the structural origin and stabilization mechanism of the ferroelectric phase are not understood because the film is typically nanocrystalline with active yet stochastic ferroelectric domains. Here, electron microscopy is used to map the in-plane domain network structures of epitaxially grown ferroelectric Y:HfO2 films in atomic resolution. The ferroelectricity is confirmed in free-standing Y:HfO2 films, allowing for investigating the structural origin for their ferroelectricity by 4D-STEM, high-resolution STEM, and iDPC-STEM. At the grain boundaries of -oriented Pca21 orthorhombic grains, a high-symmetry mixed-(R3m, Pnm21) phase is induced, exhibiting enhanced polarization due to in-plane compressive strain. Nanoscale Pca21 orthorhombic grains and their grain boundaries with mixed-(R3m, Pnm21) phases of higher symmetry cooperatively determine the ferroelectricity of the Y:HfO2 film. It is also found that such ferroelectric domain networks emerge when the film thickness is beyond a finite value. Furthermore, in-plane mapping of oxygen positions overlaid on ferroelectric domains discloses that polarization is suppressed at vertical domain walls, while it is active when domains are aligned horizontally with subangstrom domain walls. In addition, randomly distributed 180° charged domain walls are confined by spacer layers.

Ferroelectricity in hafnium zirconium oxide (Hf1 − xZrxO2) and the factors that impact it have been a popular research topic since its discovery in 2011. Although the general trends are known, the interactions between fabrication parameters and their effect on the ferroelectricity of Hf1 − xZrxO2 require further investigation. In this paper, we present a statistical study and a model that relates Zr concentration (x), film thickness (tf), and annealing temperature (Ta) with the remanent polarization (Pr) in tungsten (W)-capped Hf1 − xZrxO2. This work involved the fabrication and characterization of 36 samples containing multiple sets of metal-ferroelectric-metal capacitors while varying x (0.26, 0.48, and 0.57), tf (10 and 19 nm), and Ta (300, 400, 500, and 600 ° C). In addition to the well-understood effects of x and Ta on the ferroelectricity of Hf1 − xZrxO2, the statistical analysis showed that thicker Hf1 − xZrxO2 films or films with higher x require lower Ta to crystallize and demonstrated that there is no statistical difference between samples annealed to 500 and 600 ° C, thus suggesting that most films fully crystallize with Ta ∼ 500 ° C for 60 s. Our model explains 95% of the variability in the Pr data for the films fabricated, presents the estimates of the phase composition of the film, and provides a starting point for selecting fabrication parameters when a specific Pr is desired. [ABSTRACT FROM AUTHOR]

Ever since ferroelectricity was discovered in HfO 2 , the question of its origin remains controversial. Here, we probe this question using a combination of Landau theory of phase transitions and first-principles computations. In such an approach, the energy landscape associated with the phase transition between cubic and different experimentally demonstrated phases of HfO 2 (tetragonal, monoclinic, orthorhombic Pbca, orthorhombic Pnma, and orthorhombic Pca 2 1) is explored using density functional theory calculations. Computations revealed that stabilization of all but orthorhombic Pbca phase is driven by a single unstable zone-boundary antipolar mode X 2 −. When coupled with zone-center modes (Γ 1 + and Γ 3 +), it stabilizes the tetragonal phase. Coupling with four additional modes (Γ 5 + , X 3 − , X 5 − , X 5 +) results in the monoclinic phase, which is the ground state of the material. If, however, Γ 5 + mode is replaced with Γ 4 − mode, orthorhombic polar phase Pca 2 1 is stabilized. The application of this framework to examine the effect of electric field on the ferroelectric phase of hafnia reveals that the field of 5 MV/cm is capable of stabilizing ferroelectric phase over the monoclinic one at 0 K. [ABSTRACT FROM AUTHOR]

Ferroelectric (Al, Sc)N thin films have the potential for use in low-power memory applications. This study demonstrates the thickness scalability of ferroelectricity down to an approximately 20 nm-thick (Al0.8Sc0.2)N film sandwiched between microfabricable TiN electrodes. The impact of the deposition gas atmosphere during the sputtering process and the top electrode materials on the crystal structures and ferroelectric properties was investigated for 20–30 nm-thick (Al0.8Sc0.2)N thin films deposited on Si substrates covered with a TiN layer by radio frequency magnetron sputtering. The deposition atmosphere did not strongly affect the crystal structures of the 30 nm-thick (Al0.8Sc0.2)N films but significantly affected their ferroelectric properties. The leakage current density decreased for films deposited under pure N2 gas compared to the films deposited under a gas mixture of 0.67Ar + 0.33N2. The ferroelectric properties of 20 nm-thick (Al0.8Sc0.2)N films were changed by the top electrode materials; both the switching electric field and its maximum applicable electric field increased for the TiN top electrodes compared with the Pt top electrodes, improving the saturation characteristics of the remnant polarization (Pr) against the applied electric field. Consequently, the 20 nm-thick (Al0.8Sc0.2)N film sandwiched between the microfabricable TiN top and bottom electrodes showed ferroelectricity without noticeable degradation with decreasing film thickness; the film maintained large Pr values of over 100 μC/cm2 in the temperature range from room temperature to 150 °C. The present data open the door to scalable ferroelectric random-access memories using almost thickness-degradation-free thin (Al, Sc)N films with microfabricable TiN electrodes. [ABSTRACT FROM AUTHOR]

κ-Ga2O3 has been predicted to be a potential ferroelectric material. In this work, undoped Ga2O3 films were grown by either plasma-enhanced atomic layer deposition (PEALD) or metal organic chemical vapor deposition (MOCVD) on platinized sapphire substrates. 50 nm thick PEALD films with a mixture of κ-Ga2O3 and β-Ga2O3 had a relative permittivity of ∼27, a loss tangent below 2%, and high electrical resistivity up to ∼1.5 MV/cm. 700 nm thick MOCVD films with predominantly the κ-Ga2O3 phase had relative permittivities of ∼18 and a loss tangent of 1% at 10 kHz. Neither film showed compelling evidence for ferroelectricity measured at fields up to 1.5 MV/cm, even after hundreds of cycles. Piezoresponse force microscopy measurements on bare κ-Ga2O3 showed a finite piezoelectric response that could not be reoriented for electric fields up to 1.33 MV/cm. [ABSTRACT FROM AUTHOR]

We conducted a comprehensive investigation on the influence of TiN thickness and stress on the ferroelectric properties of Hf 0.5 Zr 0.5 O 2 thin films. TiN top electrode layers with varying thicknesses of 2, 5, 10, 30, 50, 75, and 100 nm were deposited and analyzed. It was observed that the in-plane tensile stress in TiN films increased with the thickness of the TiN top electrode. This is expected to elevate the tensile stress in the Hf 0.5 Zr 0.5 O 2 film, consequently leading to an enhancement in ferroelectric polarization. However, the effect of stress on the ferroelectric behavior of Hf 0.5 Zr 0.5 O 2 films exhibited distinct stages: improvement, saturation, and degradation. Our study presents novel findings revealing a saturation and degradation phenomenon of in-plane tensile stress on the ferroelectric properties of polycrystalline Hf 0.5 Zr 0.5 O 2 films, thereby partially resolving the discrepancies between experimental observations and theoretical predictions. The observed phase transformation induced by tensile stress in Hf 0.5 Zr 0.5 O 2 films played a crucial role in these effects. Furthermore, we found that the impact of the TiN top electrode thickness on other factors influencing ferroelectricity, such as grain size and oxygen vacancies, was negligible. These comprehensive results offer valuable insights into the influence of stress and TiN top electrode thickness on the ferroelectric behavior of Hf 0.5 Zr 0.5 O 2 films. [ABSTRACT FROM AUTHOR]

Ferroelectric (FE) electrocaloric materials research has been blossoming worldwide for solid-state refrigeration and potential cooling systems replacing thermoelectric Peltier coolers in microelectronics. In this work, we report the outcomes from a systematic study of combined phase transition (thermodynamics) based on the phenomenological Landau theory and distributed electric field (electrostatics of thin film interfaces) in FE bilayer films. Specifically, the compositional variation of ferroelectric bilayers results in broken spatial inversion symmetry leading to asymmetric thermodynamic potentials due to a combination of normal (first- and second-order phase transition) and relaxor (dispersive dielectric constant) ferroelectric behaviors devised for efficient electrocaloric cooling effects. Extensive theoretical analyses conducted for bilayers consisting of insulating materials highlight modified phase transition temperature behavior and self-poling by effective electric field amplification arising due to bilayers' electrostatic coupling yielding significant changes in isothermal entropy (ΔS) and adiabatic temperature (ΔT). The theoretical calculation insights supported with experimental results signify, through case studies for a combination of materials experimental parameters, that amplification of the local electric field and materials engineering maximize the number of coexisting phases at or away from the morphotropic phase boundary of constituent layers in bilayer thin film architectures, which can be applicable toward other classes of materials and multilayer systems. These are effective ways for efficient cooling, in general, and for microelectronics thermal management either directly or by developing a thermal switch with phase change materials integrated with thermoelectric coolers for residual heat dissipation, both at the system and on-chip levels. [ABSTRACT FROM AUTHOR]

While the influence of various fabrication parameters during deposition on the ferroelectricity of hafnium oxide has been extensively studied, the effect of different atmospheres on the actual switching process has not yet been investigated. In this work, we characterized the ferroelectric properties of undoped hafnium oxide prepared by reactive sputtering under three different atmospheres: dry oxygen/nitrogen, wet nitrogen, and vacuum conditions. We found a significant correlation between dry and wet atmospheres and resulting polarization. Specifically, we observed a direct effect on ferroelectric switching when the film was exposed to dry atmospheres and vacuum, resulting in a higher electric field necessary to initialize the wake-up effect due to an initial imprint effect. Increasing the amount of wet nitrogen during switching decreased the imprint and lowered the necessary voltage required for the wake up. We present a simple model that explains and discusses the incorporation of moisture and its resulting consequences on the ferroelectric properties of hafnium oxide. Additionally, kinetic Monte Carlo simulations showed that the addition of protons to the oxide thin film leads to a lowering of the potential and to a redistribution of protons and oxygen vacancies, which reduces the initial imprint. [ABSTRACT FROM AUTHOR]

Hf0.5Zr0.5O2 (HZO) is a promising candidate for low-power non-volatile memory due to its nanoscale ferroelectricity and compatibility with silicon-based technologies. Stress and oxygen vacancy (VO) are key factors that impact the ferroelectricity of HZO. However, their combined effects have not been extensively studied. In this study, we investigated the impact of the VO content on HZO thin films' ferroelectricity under different electrode stresses by using TiN and tungsten (W) top electrodes and controlling ozone dose time during HZO deposition. The HZO thin films with W top electrodes exhibit elevated stress levels and a greater abundance of orthorhombic/tetragonal phases, and the HZO thin films with TiN top electrode shows an increase in the monoclinic phase with increasing ozone dose time. The residual polarization (Pr) of the capacitors with TiN and W top electrodes displayed different or even opposing trends with increasing ozone dose time, and the VO content decreases with increasing ozone dose time for both sets of capacitor samples. We propose a model to explain these observations, considering the combined influence of electrode stresses and VO on the free and formation energy of the crystalline phase. Increasing the VO content promotes the transformation of the tetragonal phase to the orthorhombic phase in HZO films with TiN top electrodes, and with W top electrodes, a higher VO content prevents the tetragonal phase from transforming into the orthorhombic/monoclinic phase. Additionally, an alternative explanation is proposed solely from the perspective of stress. These findings provide valuable insights into the regulation of ferroelectricity in HZO thin films. [ABSTRACT FROM AUTHOR]

Ferroelectric topological structures have broad application prospects for high-density information storage for long-term data retention via topological protection. However, the high-density memory component might generate tremendous power consumption, causing the failure of ferroelectric devices due to the severe thermal effect. There remains an emergent issue on the synchronous achievement of high-density data storage with the decreasing influences of the thermal effects in ferroelectric topological domain structures. Here, we introduce dual-probe excitation to control the symmetry of the electric field and integrate the phase field simulation for modulating the flux-closure ferroelectric domain configuration to simultaneously improve the memory storage unit and thermal conductivity at the nanoscale in PbTiO3 thin film under a piezoresponse force microscopy experiment. It is found that the grown flux-closure polar state in both in-plane directions encourages us to enhance the storage density during dual-probe excitation in topological ferroelectric memory devices. Moreover, the increased number of flux-closure polar states and the decreased density of the domain walls can be obtained by using dual-probe excitation. Finally, we figured out that both the double-staircase-like and paddle-like domain configurations exhibit large storage units and effective thermal conductivity simultaneously under dual-probe excitation. Our study gives a guideline to synchronously improve storage performance and thermal conductivity through multiple-probe excitations in topological ferroelectric materials and devices. [ABSTRACT FROM AUTHOR]

Non-toxic molecular ferroelectrics have attracted significant interest due to their unique flexibility, low costs, and environmental friendliness. However, such materials with narrow bandgaps and ferroelectricity above room temperature (RT) are still scarce. Herein, we present a brand-new lead-free molecular ferroelectric [C8N2H22]1.5[Bi2I9] synthesized hydrothermally. [C8N2H22]1.5[Bi2I9] features a zero-dimensional (0D) structure with a polar space group of Pc, as confirmed by single-crystal X-ray diffraction and second-harmonic generation (SHG) analyses. The RT hysteresis loop reveals the intrinsic ferroelectricity of [C8N2H22]1.5[Bi2I9] with a spontaneous polarization (Ps) of 1.3 μC cm−2. A visible-light optical bandgap has been confirmed by UV-vis spectroscopy and theoretical calculations. A notable ferroelectric photovoltaic (PV) effect has been revealed in [C8N2H22]1.5[Bi2I9]-based photoelectric devices with an open-circuit voltage (Voc) of 0.39 V and a short-circuit current density (Jsc) of 2.3 μA cm−2 under AM 1.5G illumination. The PV performance can be significantly enhanced by tuning the ferroelectric polarization, achieving a maximum Voc of 0.47 V and Jsc of about 50 μA cm−2. This study offers a novel member of the 0D lead-free hybrid organic–inorganic molecular ferroelectric family possessing great promise for optoelectronic devices. [ABSTRACT FROM AUTHOR]

Solid polymer electrolytes offer great promise for all‐solid‐state batteries, but their advancement is constrained due to the low ionic conductivity at ambient temperature and non‐uniform ion transport, which hampers fast‐charging capabilities. In this study, a ferroelectric heterojunction composite is incorporated into poly(vinylidene difluoride) (PVDF) based solid electrolytes to establish an interfacial electric field that enhances lithium salt dissociation and promotes uniform ion deposition. Electrospun 1D BaTiO3 nanofibers serve as a long‐range organic/inorganic (polymer/filler) interface for ion transport, while MoSe2 hydrothermally grown on BaTiO3 forms Li2Se‐rich high‐speed ion conductors. The piezoelectric effect of the ferroelectric material helps suppress lithium dendrite growth by reversing internal charges and reducing local overpotentials. Consequently, the PVBM electrolyte achieves a substantia ionic conductivity of 6.5 × 10−4 S cm−1 and a Li‐ion transference number of 0.61 at 25 °C. The LiFePO4/PVBM/Li solid‐state batteries demonstrate an initial discharge capacity of 146 mAh g−1 at 1 C, with a capacity preservation of 80.2% upon completion of 1200 cycles, and an initial discharge capacity of 110.7 mAh g−1 at 5 C. These findings highlight the prospect of ferroelectric ceramic fillers to significantly improve ion transport and fast‐charging performance in polymer electrolytes. [ABSTRACT FROM AUTHOR]

Electric polarization typically originates from non-centrosymmetric charge distributions in compounds. In elemental crystalline materials, chemical bonds between atoms of the same element favor symmetrically distributed electron charges and centrosymmetric structures, making elemental ferroelectrics rare. Compared to atoms, elemental clusters are intrinsically less symmetric and can have various preferred orientations when they are assembled to form crystals. Consequently, the assembly of clusters with different orientations tends to break the inversion symmetry. By exploiting this concept, we show that sliding ferroelectricity naturally emerges in trilayer quasi-hexagonal phase (qHP) C60, a cluster-assembled carbon allotrope recently synthesized. Compared to many metallic or semi-metallic elemental ferroelectrics, trilayer qHP C60's have sizable band gaps and several ferroelectric structures, which are distinguishable by measuring their second-harmonic generation (SHG) responses. Some of these phases show both switchable out-of-plane and in-plane polarizations on the order of 0.2 pC/m. The out-of-plane and in-plane polarizations can be switched independently and enable an easy-to-implement construction of Van der Waals homostructures with ferroelectrically switchable chirality. [ABSTRACT FROM AUTHOR]

Non-toxic molecular ferroelectrics have attracted significant interest due to their unique flexibility, low costs, and environmental friendliness. However, such materials with narrow bandgaps and ferroelectricity above room temperature (RT) are still scarce. Herein, we present a brand-new lead-free molecular ferroelectric [C8N2H22]1.5[Bi2I9] synthesized hydrothermally. [C8N2H22]1.5[Bi2I9] features a zero-dimensional (0D) structure with a polar space group of Pc, as confirmed by single-crystal X-ray diffraction and second-harmonic generation (SHG) analyses. The RT hysteresis loop reveals the intrinsic ferroelectricity of [C8N2H22]1.5[Bi2I9] with a spontaneous polarization (Ps) of 1.3 μC cm−2. A visible-light optical bandgap has been confirmed by UV-vis spectroscopy and theoretical calculations. A notable ferroelectric photovoltaic (PV) effect has been revealed in [C8N2H22]1.5[Bi2I9]-based photoelectric devices with an open-circuit voltage (Voc) of 0.39 V and a short-circuit current density (Jsc) of 2.3 μA cm−2 under AM 1.5G illumination. The PV performance can be significantly enhanced by tuning the ferroelectric polarization, achieving a maximum Voc of 0.47 V and Jsc of about 50 μA cm−2. This study offers a novel member of the 0D lead-free hybrid organic–inorganic molecular ferroelectric family possessing great promise for optoelectronic devices. [ABSTRACT FROM AUTHOR]

BiFeO3 (BFO) thin films are well‐known for their multiferroic and photovoltaic properties, driving extensive research into potential applications. Highly ordered pyrolytic graphite (HOPG) substrates, with a graphene‐like surface structure, provide an ideal platform for assessing the impact of graphene electrodes. This study investigates the photovoltaic properties of ITO/BFO/HOPG devices with La‐doped BFO thin films at concentrations of 5, 10, and 15 mol%. The polycrystalline BFO thin films exhibited a preferential (111) orientation, with the 10 mol% La‐doped thin films demonstrating optimal crystallinity and the highest remanent polarization of 50.8 µC/cm2. Photovoltaically, the 5 mol% La‐doped BFO thin film exhibited an open‐circuit voltage (Voc) of 0.46 V and the highest short‐circuit current (Jsc) of 0.38 mA/cm2. The 10 mol% La‐doped BFO thin film achieved the highest Voc of 0.57 V with a Jsc of 0.35 mA/cm2, likely because of enhanced ferroelectric polarization. In contrast, the 15 mol% La‐doped BFO thin film showed a reduced band gap but diminished photovoltaic performance. The minimal variation in the band gap (within 0.1 eV) suggests that the improved photovoltaic performance is primarily driven by increased polarization resulting from enhanced tetragonality. [ABSTRACT FROM AUTHOR]

Pristine ZnO and Sm-doped ZnO nanoparticles were synthesized using a wet chemical co-precipitation technique. The morphological and structural characteristics of pristine and Sm-doped ZnO were studied by field-emission scanning electron microscopy (FESEM) and X-ray diffraction (XRD) techniques. Increases in lattice parameters, interplanar spacing, and volume was observed from the XRD patterns compared to its JCPDS card. Crystallite size, dislocation density, deformation stress, lattice strain, and energy density for both pristine and Sm-ZnO nanoparticles were calculated using Scherrer and Williamson–Hall (W–H) methods. An energy bandgap reduction was observed in the Sm-doped ZnO (Eg ~ 2.7 eV), which played a crucial role in explaining the increased leakage currents in Sm-ZnO. The Sm-doped ZnO nanoparticles exhibited a remnant polarization (Pr ~ 0.163 µC/cm2) and a coercive field (Ec ~ 25.33 kV/cm). Current–voltage (I–V) characteristics show maximum current generated on applying varying voltages (Vmax = 40 V, Imax = ~600 μA). Frequency- and temperature-dependent dielectric studies were conducted to examine the change in the values of the dielectric constant and dielectric loss with the variation in frequency and temperature. The Sm-doped ZnO-based nanogenerator generated an output voltage ~ 400 mV at tapping force of ~ 0.02 kgf, which makes it a prominent candidate for self-powered devices. [ABSTRACT FROM AUTHOR]

The discovery of nanoscale ferroelectricity in hafnia (HfO2) has paved the way for next generation high‐density, non‐volatile devices. Although the surface conditions of nanoscale HfO2 present one of the fundamental mechanism origins, the impact of external environment on HfO2 ferroelectricity remains unknown. In this study, the deleterious effect of ambient moisture is examined on the stability of ferroelectricity using Hf0.5Zr0.5O2 (HZO) films as a model system. It is found that the development of an intrinsic electric field due to the adsorption of atmospheric water molecules onto the film's surface significantly impairs the properties of domain retention and polarization stability. Nonetheless, vacuum heating efficiently counteracts the adverse effects of water adsorption, which restores the symmetric electrical characteristics and polarization stability. This work furnishes a novel perspective on previous extensive studies, demonstrating significant impact of surface water on HfO2‐based ferroelectrics, and establishes the design paradigm for the future evolution of HfO2‐based multifunctional electronic devices. [ABSTRACT FROM AUTHOR]

This study employs a data‐driven machine learning approach to investigate specific ferroelectric properties of Al1−xScxN thin films, targeting their application in next‐generation nonvolatile memory (NVM) devices. This approach analyzes a vast design space, encompassing over a million data points, to predict a wide range of coercive field values that are crucial for optimizing Al1−xScxN‐based NVM devices. We evaluated seven machine learning models to predict the coercive field across a range of conditions, identifying the random forest algorithm as the most accurate, with a test R2 value of 0.88. The model utilized five key features: film thickness, measurement frequency, operating temperature, scandium concentration, and growth temperature to predict the design space. Our analysis spans 13 distinct scandium concentrations and 13 growth temperatures, encompassing thicknesses from 9–1000 nm, frequencies from 1 to 100 kHz, and operating temperatures from 273 to 700 K. The predictions revealed dominant coercive field values between 3.0 and 4.5 MV/cm, offering valuable insights for the precise engineering of Al1−xScxN‐based NVM devices. This work underscores the potential of machine learning in guiding the development of advanced ferroelectric materials with tailored properties for enhanced device performance. [ABSTRACT FROM AUTHOR]

Extending ferroelectric materials to two-dimensional limit provides versatile applications for the development of next-generation nonvolatile devices. Conventional ferroelectricity requires materials consisting of at least two constituent elements associated with polar crystalline structures. Monolayer graphene as an elementary two-dimensional material unlikely exhibits ferroelectric order due to its highly centrosymmetric hexagonal lattices. Here, we report the observations of electronic ferroelectricity in monolayer graphene by introducing asymmetric moiré superlattice at the graphene/h-BN interface, in which the electric polarization stems from electron-hole dipoles. The polarization switching is probed through the measurements of itinerant Hall carrier density up to room temperature, manifesting as standard polarization-electric field hysteresis loops. We find ferroelectricity in graphene moiré systems exhibits generally similar characteristics in monolayer, bilayer, and trilayer graphene, which indicates layer polarization is not essential to observe the ferroelectricity. Furthermore, we demonstrate the applications of this ferroelectric moiré structures in multi-state nonvolatile data storage with high retention and the emulation of versatile synaptic behaviors. Our work not only provides insights into the fundamental understanding of ferroelectricity, but also demonstrates the potential of graphene for high-speed and multi-state nonvolatile memory applications. Monolayer graphene, with its highly centrosymmetric hexagonal lattice, is typically not considered ferroelectric. Here, the authors observe ferroelectricity in monolayer graphene by introducing asymmetric moiré superlattices, where polarization arises from electron-hole dipoles. [ABSTRACT FROM AUTHOR]

Integrating free‐standing complex oxides with two‐dimensional (2D) materials has recently attracted great interest, due to the rich physics evolving from such structures. Enhancing and tuning the opto–electronic properties of these systems is of high importance for a multitude of applications, such as sensors, memory devices or optical communications. The electrostatic control of photoluminescence of monolayer MoS2 at room temperature via integration of free‐standing BaTiO3 (BTO), a ferroelectric perovskite oxide is presented. It is shown that the use of BTO leads to highly tunable exciton emission of MoS2 in a minimal range of gate voltages. Due to BTO's ferroelectric polarization‐induced doping, large peak emission shifts as well as a large and tunable A trion binding energy in the range of 40–100 meV are observed. These measurements are compared with those carried out when the BTO is replaced by a hexagonal boron nitride (hBN) dielectric layer, confirming BTO's superior gating properties and thus lower power consumption. Additionally, advantage of the ferroelectric switching of BTO is taken by fabricating devices where the BTO layer is decoupled from the gate electrode with a SiO2 layer. Choosing to isolate the BTO allows to induce large remanent behavior of MoS2's excitonic features. [ABSTRACT FROM AUTHOR]

Miniaturizing van der Waals (vdW) ferroelectric materials to atomic scales is essential for modern devices like nonvolatile memory and sensors. To unlock their full potential, their growth mechanisms, interface effects, and stabilization are preferably investigated, particularly for ultrathin 2D nanosheets with single‐unit cell thickness. This study focuses on Bi2TeO5 (BTO) and utilizes precise control over growth kinetics at the nucleation temperature to create specific interfacial reconfiguration layers. Ultrathin BTO nanosheets with planar ferroelectricity at a single‐unit cell thickness are successfully grown. Atomic‐scale characterization reveals a disordered distribution of elements in the interfacial layer, which buffers strain from lattice mismatch. The theoretical calculations support these observations. Furthermore, this strategy also can be extended to the growth of a variety of 2D ternary oxide nanosheets. This work contributes to a better understanding of growth and stability mechanisms in 2D ultrathin nanosheets. [ABSTRACT FROM AUTHOR]

The development of ultrathin (≤5 nm) hafnia‐based ferroelectric (FE) films is essential for achieving low operating voltages, facilitating their integration into advanced process nodes for low‐power and non‐volatile memory applications. However, challenges in ultrathin FE films arise from the depolarization field and interface‐related issues, leading to an antiferroelectric‐like (AFE‐like) polarization switching behavior and more significant wake‐up effects, causing operational inconvenience and reliability concerns. Here, interface‐modulated ferroelectricity is reported in 4 nm Hf0.5Zr0.5O2 (HZO) thin films, demonstrating excellent properties with low operating voltage, enhanced switching speed, and high reliability. Electrical and structural characterizations reveal that adjusting interface asymmetry may introduce a substantial built‐in field (Ebi) and an AFE‐like switching behavior can exhibit a robust FE‐like characteristic. This AFE‐to‐FE‐like transition is driven by switching kinetics rather than commonly proposed phase transitions. Furthermore, a comprehensive model is developed to elucidate the intricate physics of the modulation mechanism by asymmetric interfaces, emphasizing the critical roles of depolarizing effects and Ebi on ferroelectricity. This work underscores the importance of interfaces in engineering ferroelectricity for advanced electronic applications. [ABSTRACT FROM AUTHOR]

Hybrid improper ferroelectrics (HIFs), characterized by ferroelectric polarization arising from the rotation of two symmetry inequivalent antiferrodistortive modes, exhibit exotic properties such as T-independent dielectric constants and robustness against depolarizing field. Here, using first-principles simulations, we report a new P 2 1 phase in a Si-compatible CeO2/HfO2 superlattice that exhibits remarkably robust hybrid improper ferroelectricity, induced by the in-plane oxygen rotations of two antiferrodistortive distortion modes. These non-polar distortions are coupled with a polar distortion through a trilinear coupling in the superlattice, stabilizing ferroelectricity as the competing ground state with the assistance of epitaxial strain. The estimated out-of-plane polarization ( P = 30.3 μ C / c m 2 ) is switchable with a remarkably small energy barrier of 8.5 meV/atom and relatively smaller coercive field relative to bulk HfO2, expected to reduce the operational voltage of ferroelectric devices. Our discovery may offer unexpected opportunities for innovating high-performance, low-voltage devices, and promising advancements in next-generation CMOS compatible oxide-based electronics. [ABSTRACT FROM AUTHOR]

Multiferroic BaTiO 3 exhibiting ferroelectric and ferromagnetic behavior was synthesized via the high-energy ball milling of pure BaTiO 3 (BTO) powders for durations ranging from 15 to 60 min, followed by pressing and sintering at 1200 °C X-ray diffraction patterns of all synthesized samples predominantly revealed a BTO phase with a tetragonal structure and a secondary Ba 12 Fe 28 Ti 15 O 84 (BFTO) phase. The BFTO phase was formed after milling for more than 30 min because of chemical interactions between the BTO powder and milling media. Vibrating sample magnetometry confirmed the ferromagnetic nature of the sintered pellets. The specific magnetization increased with increasing milling duration, reaching a maximum value of 1.15 emu/g after 60 min of milling. This increase can be attributed to the distortion of the crystal structure and presence of a secondary phase, as confirmed by scanning electron microscopy and energy-dispersive X-ray spectroscopy. Additionally, electrical characterization revealed the dielectric nature of the materials, with relative permittivity ranging from 500 to 1800, maximum spontaneous polarization from 9.77 to 11.31 μC/cm2, coercive field from 3.86 to 11.12 kV/cm, and AC conductivity from 1 × 10−6 to 1 × 10−3 S/cm. The method described in this study is a simple and cost-effective approach to produce multiferroic materials with ferroelectric and relaxor ferroelectric behavior at room temperature, broadening their potential for technological applications. [ABSTRACT FROM AUTHOR]

CeO 2 -HfO 2 solid solution thin films (Hf 1-x Ce x O 2) were deposited on Pt(111)/TiO 2 /SiO 2 /Si(100) substrates using the chemical solution deposition method. This study investigates the influence of CeO 2 content and annealing temperature on the structure and ferroelectric properties of Hf 1-x Ce x O 2 films. Ferroelectric behavior is demonstrated in polycrystalline Hf 0.80 Ce 0.20 O 2 films with thicknesses ranging from 163 to 524 nm. And the structure of the films is analyzed using glancing incidence X-ray diffraction. The comprehensive results indicate that Hf 0.80 Ce 0.20 O 2 films annealed at 850 °C exhibit excellent ferroelectricity. Square hysteresis loops associated with the ferroelectric orthorhombic phase are observed, even in the 524-nm-thick film. The remnant polarization (P r) and coercive field (E c) range from 16 to 18 μC/cm2 and 1100–1250 kV/cm, respectively, under a maximum applied electric field of 2 MV/cm for all Hf 0.80 Ce 0.20 O 2 films. Furthermore, the film presents thickness-insensitive characteristic. The current work paves the new way to design high-performance thick HfO 2 -based ferroelectric films. [ABSTRACT FROM AUTHOR]

Multiferroic materials that exhibit interacting and coexisting properties, like ferroelectricity and ferromagnetism, possess significant potential in the development of novel technologies that can be controlled through the application of external fields. They also exhibit varying regions of polarity, known as domains, with the interfaces that separate the domains referred to as domain walls. In this study, using three-dimensional (3D) bragg coherent diffractive imaging (BCDI), we investigate the dynamics of multiferroic domain walls in a single hexagonal dysprosium manganite (h-DyMnO 3 ) nanocrystal under varying applied electric field. Our analysis reveals that domain wall motion is influenced by the pinning effects, and a threshold voltage of +3 V is required to overcome them. Using circular mean analysis and phase gradient mapping, we identified localised phase realignment and high-gradient regions corresponding to domain walls, providing insights into the behaviour of multiferroic systems under external stimuli. [ABSTRACT FROM AUTHOR]

Noncollinear ferroic materials are sought after as testbeds to explore the intimate connections between topology and symmetry, which result in electronic, optical, and magnetic functionalities not observed in collinear ferroic materials. For example, ferroaxial materials have rotational structural distortions that break mirror symmetry and induce chirality. When ferroaxial order is coupled with ferroelectricity arising from a broken inversion symmetry, it offers the prospect of electric‐field‐control of the ferroaxial distortions and opens up new tunable functionalities. However, chiral multiferroics, especially ones stable at room temperature, are rare. A strain‐stabilized, room‐temperature chiral multiferroic phase in single crystals of BaTiS3 is reported here. Using first‐principles calculations, the stabilization of this multiferroic phase having P63 space group for biaxial tensile strains exceeding 1.5% applied on the basal ab‐plane of the room temperature P63cm phase of BaTiS3 is predicted. The chiral multiferroic phase is characterized by rotational distortions of TiS6 octahedra around the long c‐axis and polar displacement of Ti atoms along the c‐axis. The ferroaxial and ferroelectric distortions and their domains in P63‐BaTiS3 are directly resolved using atomic resolution scanning transmission electron microscopy. Landau‐based phenomenological modeling predicts a strong coupling between the ferroelectric and the ferroaxial order making P63‐BaTiS3 an attractive test bed for achieving electric‐field‐control of chirality. [ABSTRACT FROM AUTHOR]

A synergistic realization of high electrocaloric effect (ECE) and excellent temperature stability in ferroelectrics are foundation for practical applications, which is, however, a major challenge in ferroelectric cooling community thus far. In confront with this long‐standing issue, an emergent monomorphic ferrodistortion strategy in NaNbO3‐based relaxor is proposed with flexible tetragonal polar nanoregions immersing in short‐range oxygen octahedral tilt. This not only contributes to large quantities of polar entities to increase entropy change but also produces highly robust oxygen octahedral tilt to persist ferroelectricity and obstruct thermal agitations. Therefore, a high ΔT of 0.96 K and an ultrawide temperature span ΔTspan of 110 K with a record‐high figure of merit of 4.74 is achieved in Ta‐doped NaNbO3‐BaTiO3 ceramics and these superior EC performances present a remarkable breakthrough in ferroelectric bulks cooling. This work thus provides an innovative way of utilizing ferrodistortive relaxor feature with polar nanoregions immersing in oxygen octahedral tilt to simultaneously boost EC value and temperature stability and thus monomorphic ferrodistortion is proposed as an effective strategy to develop high‐performance entropy‐change materials. [ABSTRACT FROM AUTHOR]

The pursuit of extreme device miniaturization and the exploration of associated physical phenomena has spurred significant interest in crystallographic phase control and ferroelectric switching in reduced dimensions. The recently discovered wurtzite ferroelectrics offer intriguing piezoelectric and ferroelectric properties, CMOS compatibility, and seamless integration with mainstream semiconductor technology. In this study, we present a comprehensive investigation of the crystallographic phase transition of ScAlN nanowires across the full Sc compositional range. While a gradual transition from wurtzite to cubic phase was observed with increasing Sc composition, we further demonstrate that a highly ordered wurtzite phase ScAlN can be confined at the ScAlN/GaN interface for Sc contents surpassing what is possible in conventional films. We provide the first evidence of ferroelectric switching in ScAlN nanowires, a result that holds significant implications for future device miniaturization. Our demonstration of tunable ferroelectric ScAlN nanowires opens new possibilities for nanoscale, domain, alloy, strain, and quantum engineering of wurtzite ferroelectrics, representing a significant stride toward the development of next-generation, miniaturized devices based on wurtzite ferroelectrics. [ABSTRACT FROM AUTHOR]

Pb-based perovskites play pivotal roles in ferroelectric research. In the search for new Pb-based ferroelectrics, we investigated the ferroelectric properties of Dion–Jacobson type CsPb2Nb3O10 and exfoliated 2D nanosheets. Ferroelectricity in CsPb2Nb3O10 was demonstrated for the first time. CsPb2Nb3O10 adopted a polar tetragonal structure with a modest TC = 260 °C and polarization PS = 7.93 μC cm−2; the polarization mainly arose from the out-of-plane displacements of Nb5+ ions and nearby oxygens. CsPb2Nb3O10 layered perovskite offers additional advantages for tailoring ferroelectric nanomaterials, as exfoliated 2D nanosheets provide novel platforms for investigating ferroelectric properties down to the 2D limit. Piezoresponse force microscopy confirmed stable ferroelectricity even in exfoliated 2D Pb2Nb3O10 nanosheets. [ABSTRACT FROM AUTHOR]

2D materials have been interested in recent years due to their unique properties and enormous potential in various fields. In particular, 2D ferroionics with both ferroelectricity and ionic conductivity shed light on new possibilities for van der Waals nanoelectronics. Here, supported by theoretical calculations and electrical characterizations, the reconfigurable van der Waals ferroionic barristor that can be used in multifunctional electronics including resistive devices and steep‐slope transistors is reported. Large modulation on the device properties is achieved by electrically driven migration and redistribution of mobile ions. The memory device shows an unprecedented long‐term stability with a switching ratio of ≈1010. Utilizing this ferroionic nature, 2D transistors able to beat the Boltzmann tyranny, with different gate configurations, are designed. The subthreshold swing (SS) exhibits sub‐60 mV per decade values over five decades of the drain current with a minimum of 12.1 mV per decade. This work paves the way for investigating the symbiotic relationship of ferroelectricity and ionic activities in van der Waals ferroionics and highlights their applications in advanced nanoelectronics. [ABSTRACT FROM AUTHOR]

Ferroelectric (FE)‐antiferromagnetic (AFM) multiferroic materials have sparked growing interest due to their huge possibilities in energy‐saving, photoelectric devices, nonvolatile storage, and switches. However, realizing FE‐AFM properties in a hybrid molecular material is difficult because ferroelectric and magnetic orders are commonly mutually exclusive. Here, we report an FE‐AFM multiferroic semiconductor [NH4(18‐crown‐6)]2[Mn(SCN)4] (NCMS) by supramolecular assembly approach via molecular rotor synthon [NH4(18‐crown‐6)] and inorganic magnetic module [Mn(SCN)4]. Interestingly, NCMS shows good ferroelectricity with a spontaneous polarization (Ps) of 5.94 μC cm−2 higher than most crown‐ether‐based ferroelectrics. Especially, the realization of antiferromagnetism is for the first time in the crown ether hybrid perovskite ferroic systems. Additionally, semiconductor NCMS displays an X‐ray radiation detection response with a large photo/dark current on‐off ratio (197). Our study not only gives a deep insight into understanding multiferroic properties but also provides a novel and efficient approach to realizing high‐performance hybrid multiferroic materials. [ABSTRACT FROM AUTHOR]

Developing efficient photo‐piezocatalytic systems to achieve the conversion of renewable energy to chemical energy emerges enormous potential. However, poor catalytic efficiency remains a significant obstacle to future practical applications. Herein, a series of unique Au@BaTiO3 (Au@BT) yolk‐shell nanostructure photo‐piezocatalyst is constructed with single Au nanoparticle (Au NP) embedded in different positions within ferroelectric BaTiO3 hollow nanosphere (BT‐HNS). This special structure showcases excellent mechanical force sensitivity and provides ample plasmon‐induced interfacial charge‐transfer pathways. In addition, the powerful piezoelectric polarization electric field induced by the enhanced ferroelectric polarization electric field via corona poling treatment in BT‐HNS further promotes charge separation, CO2 adsorption and key intermediate conversion. Notably, BT with single Au NP encapsulated into hollow nanosphere shell with reinforced polarization (Au@BT‐1‐P) shows synergistically improved photo‐piezocatalytic CO2 reduction activity for producing CO with a high production rate of 31.29 µmol g−1 h−1 under visible light irradiation and ultrasonic vibration. This work highlights a generic tactic for optimized design of high‐performance and multifunctional nanostructured photo‐piezocatalyst. Meanwhile, these yolk‐in‐shell nanostructures with single Au nanoparticle as an ideal model may hold great promise to inspire in‐depth exploration of carrier dynamics and mechanistic understanding of the catalytic reaction. [ABSTRACT FROM AUTHOR]