Modeling of the evolution of dielectric loss with processing temperature in ferroelectric and dielectric thin oxide films
X. H. Zhu, B. Guigues, E. Defay, M. Aid
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The experimentally observed dielectric loss responses in ferroelectric and dielectric thin oxide films have been theoretically addressed in this work, which paves the way for seeking methods in order to tailor the dielectric loss effectively for practical applications. Accepted for publication in Journal of Applied Physics
It was experimentally found that the evolution of dielectric loss with processing temperature displays a common trend in ferroelectric and dielectric thin oxide films: firstly an increase and then a decrease in dielectric loss when the processing temperature is gradually raised. Such a dielectric response of ferroelectric/dielectric thin films has been theoretically addressed in this work. We propose that at the initial stage of the crystallization process in thin films, the transformation from amorphous to crystalline phase should increase substantially the dielectric loss; then, with further increase in the processing temperature, the coalescent growth of small crystalline grains into big ones could be helpful in reducing the dielectric loss by lowering grain boundary densities. The obtained experimental data for (Ba,Sr)TiO3 thin films with 500 nm in thickness were analyzed in terms of the model developed and shown to be in a reasonable agreement with the theoretical results.
We report that an energetic plasma process is extremely effective in enlarging the unit cell volume and ferroelectric distortion of the ferroelectric oxides, resulting in a significant increase in its Tc. We demonstrate experimentally that c-axis oriented BaTiO3 films can be deposited directly on quartz glass and Si substrates using such a process and that the material shows an approximately 5% expansion of its unit cell volume and approximately 4 times the ferroelectric tetragonal distortion of the bulk crystals. Such a frozen negative pressure results in a Tc value that is approximately 580 …
We report the observation of a "transparency window" in the dielectric resonant absorption spectrum of the relaxor ferroelectric K1-xLixTaO3 (KLT) in the vicinity of its weakly first order transition. This phenomenon is shown to be conceptually similar to the electro-magnetically induced transparency (EIT) phenomenon observed in atomic vapors, which can be modeled classically by a driven master -slave oscillator system. In KLT, it reveals the presence of macroscopic hetero-phase fluctuations and provides unique information on the nature and mechanism of the phase transition in relaxors.
The aim of this Chapter is to provide an account of recent advances in the first-principles modeling of ferroelectric oxide nanostructures. Starting from a microscopic description of ferroelectricity in bulk materials and considering then, successively, different kinds of nanostructures (films, multilayers, wires, and particles), we try to identify the main trends and to provide a coherent picture of the role of finite size effects in ferroelectric oxides.
The alkaline earth binary oxides adopt a simple rocksalt structure and form an important family of compounds because of their large presence in the earth's mantle and their potential use in microelectronic devices. In comparison to the class of multifunctional ferroelectric perovskite oxides, however, their practical applications remain limited and the emergence of ferroelectricity and related functional properties in simple binary oxides seems so unlikely that it was never previously considered. Here, we show using first-principles density functional calculations that ferroelectricity can be …
Relaxor ferroelectrics are complex materials with distinct properties different from classic ferroelectrics. Probing frequency depended dielectric susceptibility is its trait. Other empirical laws build on classic ferroelectrics are still applicable to relaxor ferroelectrics. Here we report an abnormal improved dielectric in La doped relaxor ferroelectric 0.4PNN-0.6PHT, which deviated from the consistent variation relationship with piezoelectric coefficient. A mesoscale mechanism is proposed to reveal the origin of the improved dielectric response in 0.4PNN-0.6PHT, where the polar nanoregions …
The conductive domain wall (CDW) is extensively investigated in ferroelectrics, which can be considered as a quasi-two-dimensional reconfigurable conducting channel embedded into an insulating material. Therefore, it is highly important for the application of ferroelectric nanoelectronics. Hitherto, most CDW investigations are restricted in oxides, and limited work has been reported in non-oxides to the contrary. Here, by successfully synthesizing the non-oxide ferroelectric Sn2P2S6 single crystal, we observed and confirmed the domain wall conductivity by using different scanning probe techniq…
We fabricated ultrathin ferroelectric/correlated electron oxide heterostructures composed of the ferroelectric Pb(Zr0.2Ti0.8)O3 and the correlated electron oxide (CEO) La0.8Sr0.2MnO3 on SrTiO3 substrates by pulsed laser epitaxy. The hole accumulation in the ultrathin CEO layer was substantially modified by heterostructuring with the ferroelectric layer, resulting in an insulator-metal transition. In particular, our thickness dependent study showed that drastic changes in transport and magnetic properties were strongly coupled to the modulation of charge carriers by ferroelectric field effect, …
A dielectric nonlinear response in model two-phase composites, prepared from a displacive ferroelectric material with a dominant dielectric response due to a single oscillator ferroelectric mode and a dielectric material, is characterized by the existence of new modes due to geometric resonances below the percolation threshold in the ferroelectric matrix. The geometric nature of oscilations depends on composition and geometric properties of the mixture. Generation of higher frequency modes is studied within our model and discussed for displacive ferroelectric materials of the $BaTiO_{3}$ type.…
The epitaxial growth of multifunctional oxides on semiconductors has opened a pathway to introduce new functionalities to semiconductor device technologies. In particular, ferroelectric materials integrated on semiconductors could lead to low-power field-effect devices that can be used for logic and memory. Essential to realizing such field-effect devices is the development of ferroelectric metal-oxide-semiconductor (MOS) capacitors, in which the polarization of a ferroelectric gate is coupled to the surface potential of a semiconducting channel. Here we demonstrate that ferroelectric MOS capa…
This review covers the important advances in recent years in the physics of thin film ferroelectric oxides, the strongest emphasis being on those aspects particular to ferroelectrics in thin film form. We introduce the current state of development in the application of ferroelectric thin films for electronic devices and discuss the physics relevant for the performance and failure of these devices. Following this we cover the enormous progress that has been made in the first principles computational approach to understanding ferroelectrics. We then discuss in detail the important role that stra…
We report the ferroelectric property in Tb2Ti2O7 pyrochlore, prepared by a two-step solid-state reaction method. A concave P-E (polarisation vs electric field) loop observed from 382 K confirms ferroelectricity, below which the loop remains as pointed or banana-shaped. Dielectric plots clearly show an anomaly at 383 K and the magnetic data reveals a deviation from 380 K supporting the observed ferroelectric ordering. The origin of ferroelectricity in Tb2Ti2O7 is discussed which is due to the structural distortion in TiO6 octahedron.
This article reviews the polarizability model and its applications to ferroelectric perovskite oxides. The motivation for the introduction of the model is discussed and nonlinear oxygen ion polarizability effects and their lattice dynamical implementation outlined. While a large part of this work is dedicated to results obtained within the self-consistent-phonon approximation (SPA), also nonlinear solutions of the model are handled which are of interest to the physics of relaxor ferroelectrics, domain wall motions, incommensurate phase transitions. The main emphasis is to compare the results o…
There are two silver perovskite oxides: AgNbO3 and AgTaO3. AgNbO3 has a noncentrosymmetric group of Pmc21 at room temperature with a ferri-electric ordering of polarization. Such a ferri-electric state with small polarization can be changed into a ferroelectric state with very large polarization by a high electric field or by a chemical modification. The induced ferroelectric phase shows promising electromechanical response for applications in piezoelectric devices. In contrast, AgTaO3 is a quantum paraelectric, but ferroelectricity also can be induced through chemical substitution. The findin…
In this review, we propose a summary of the most recent advances in the first-principles study of ferroelectric oxide epitaxial thin films and multilayers. We discuss in detail the key roles of mechanical and electrical boundary conditions, providing to the reader the basic background for a simple and intuitive understanding of the evolution of the ferroelectric properties in many nanostructures. Going further we also highlight promising new avenues and future challenges within this exciting field or researches.
The ferroelectric polarization switching in ferroelectric hafnium zirconium oxide (Hf0.5Zr0.5O2, HZO) in the HZO/Al2O3 ferroelectric/dielectric stack is investigated systematically by capacitance-voltage and polarization-voltage measurements. The thickness of dielectric layer is found to have a determinant impact on the ferroelectric polarization switching of ferroelectric HZO. A suppression of ferroelectricity is observed with thick dielectric layer. In the gate stacks with thin dielectric layers, a full polarization switching of the ferroelectric layer is found possible by the proposed leaka…
A strategy for obtaining low band gap oxide ferroelectrics based on charge imbalance is described and illustrated by first principles studies of the hypothetical compound Bi$_6$Ti$_4$O$_{17}$, which is an alternate stacking of the ferroelectric Bi$_4$Ti$_3$O$_{12}$. We find that this compound is ferroelectric, similar to Bi$_4$Ti$_3$O$_{12}$ although with a reduced polarization. Importantly, calculations of the electronic structure with the recently developed functional of Tran and Blaha yield a much reduced band gap of 1.83 eV for this material compared to Bi$_4$Ti$_3$O$_{12}$. Therefore, Bi$…
We calculate the pyrocoefficient, static dielectric susceptibility profiles and its thickness dependence of ferroelectric thin films. Also, the temperature dependences of above quantities have been calculated. For the calculations we use Landau phenomenological theory, leading to Lame equations. These equations subject to boundary conditions with different extrapolation length on the surfaces have been solved numerically. The divergency of pyroelectric coefficient and static dielectric susceptibility in the vicinity of thickness induced ferroelectric phase transition (i.e. at $l\approx l_c$ or…
Ferroelectric hafnium zirconium oxide (HZO) thin films show significant promise for applications in ferroelectric random-access memory, ferroelectric field-effect transistors, and ferroelectric tunneling junctions. However, there are shortcomings in understanding ferroelectric switching, which is crucial in the operation of these devices. Here a computational model based on phase field method is developed to simulate the switching behavior of polycrystalline HZO thin films. Furthermore, we introduce a novel approach to optimize the effective Landau coefficients describing the free energy of HZ…
An analysis of the dynamic dielectric and electro-optic relaxation response of thin film ferroelectrics is presented. The analysis is based upon the relaxation of ferroelectric domains with a continuous distribution of sizes given by percolation theory. The resulting temporal response is described by the expression (t^-m) exp(-(t/tau)^beta). The analysis was applied to KNbO3 thin films. Measurements of the polarization, birefringence and dielectric transients show qualitative agreement with the model over 11 orders of magnitude in time.
It has been recently suggested that the coexistence of ferroelectricity and Rashba-like spin-splitting effects due to spin-orbit coupling in a single material may allow for a non-volatile electric control of spin degrees of freedom. In the present work, we compared the structural and ferroelectric properties of tetragonal and rhombohedral phases of ferroelectric BiAlO$_3$ by means of density-functional calculations. In both phases, we carefully investigated Rashba and Dresselhaus effects, giving rise to spin-splitting in their bulk electronic structure, particularly near the conduction band mi…
We report far-infrared dielectric properties of powder form ferroelectric SrTiO3. Terahertz time-domain spectroscopy (THz-TDS) measurement reveals that the low-frequency dielectric response of SrTiO3 is a consequence of the lowest transverse optical (TO) soft mode TO1 at 2.70 THz (90.0 1/cm), which is directly verified by Raman spectroscopy. This result provides a better understanding of the relation of low-frequency dielectric function with the optical phonon soft mode for ferroelectric materials. Combining THz-TDS with Raman spectra, the overall low-frequency optical phonon response of SrTiO…
GaFeO3, AlFeO3 and related oxides are ferrimagnetic exhibiting magnetodielectric effect. There has been no evidence to date for ferroelectricity and hence multiferroicity in these oxides. We have investigated these oxides as well as oxides of the composition Al1-x-yGaxFe1+yO3 (x = 0.2, y = 0.2) for possible ferroelectricity by carrying out pyroelectric measurements. These measurements establish the occurrence of ferroelectricity at low temperatures below the Nèel temperature in these oxides. They also exhibit significant magnetoelectric effect. We have tried to understand the origin of ferroel…
An accurate estimate of the ferroelectric polarization in ferroelectric-dielectric stacks is important from a materials science perspective, and it is also crucial for the development of ferroelectric based electron devices. This paper revisits the theory and application of the PUND technique in Metal-Ferroelectric-Dielectric-Metal (MFDM) structures by using analytical derivations and numerical simulations. In an MFDM structure the results of the PUND technique may largely differ from the polarization actually switched in the stack, which in turn is different from the remnant polarization of t…
Polycrystals of CaxBa1-xNb2O6(CBN) tungsten bronze type oxides have been prepared and their structural, dielectric, and thermal properties have been investigated. It was found that CBN alloys with ferroelectric tetragonal tungsten bronze structure were only available in a composition range of 0.19 <= x <= 0.32. It was also showed that CBN can be classified as a ferroelectric with a first-order thermal phase transition showing polarization precursor dynamics before transition into the ferroelectric phase, in sharp contrast to an isostructural alloy SrxBa1-xNb2O6(SBN) that shows typical relaxor …
Cubic structure is one of the most commonly found structures for oxides at high temperature. As the temperature is lowered only a handful of these oxides exhibit ferroelectricity which is rather surprising. In this paper, we use the example of YCrO3 (YCO), an incipient ferroelectric material to show that in most oxides there are two competing phenomenon -onset of ferroelectricity due to rotation of CrO6 octahedra and displacement of Y atom leading to suppression of ferroelectricity. This competition reveals that while the octahedral rotations favor a lower symmetry state, the Y atom displaceme…
By performing first-principles calculations on four capacitor structures based on BaTiO3 and PbTiO3, we determine the intrinsic interfacial effects that are responsible for the destabilization of the polar state in thin-film ferroelectric devices. We show that, contrary to the established interpretation, the interfacial capacitance depends crucially on the local chemical environment of the interface through the force constants of the metal-oxide bonds, and is not necessarily related to the bulk screening properties of the electrode material. In particular, in the case of interfaces between AO-…
All-oxide magnetic tunnel junctions (MTJs) incorporating functional materials as insulating barriers have the potential of becoming the founding technology for novel multi-functional devices. We investigate, by first-principles density functional theory, the bias-dependent transport properties of an all-oxide SrRuO3/BaTiO3/SrRuO3 MTJ. This incorporates a BaTiO3 barrier which can be found either in a non-ferroic or in a ferroelectric state. In such an MTJ not only can the tunneling magnetoresistance reach enormous values, but also, for certain voltages, its sign can be changed by altering the b…
We have proposed the phenomenological description of dielectric hysteresis loops in ferroelectric semiconductors with charged defects and prevailing extrinsic conductivity. Exactly we have modified Landau-Ginsburg approach and shown that the macroscopic state of the aforementioned inhomogeneous system can be described by three coupled equations for three order parameters. Both the experimentally observed coercive field values well below the thermodynamic one and the various hysteresis loop deformations (constricted and double loops) have been obtained in the framework of our model. The obtaine…
Recently, based on the phase-field modeling, it was predicted that Hf1-xZrxO2 (HZO) exhibits the morphotropic phase boundary (MPB) in its compositional phase diagram. Here, we investigate the effect of structural changes between tetragonal (t) and orthorhombic (o) phases on the ferroelectric and dielectric properties of HZO films to probe the existence of MPB region. The structural analysis show that by adjusting the ozone dosage during the atomic layer deposition process and annealing conditions, different ratios of t- to o-phases (f_(t/o) ) were achieved which consequently affect the ferroel…
Ferroelectric domain structure evolution induced by an external electric field was investigated by means of nematic liquid crystal (NLC) method in two strontium-barium niobate single crystals of nominal composition: Sr_{0.70}Ba_{0.30}Nb_{2}O_{6} (SBN:70 - relaxor) and Sr_{0.26}Ba_{0.74}Nb_{2}O_{6} (SBN:26 - ferroelectric). Our results provide evidence that the broad phase transition and frequency dispersion that are exhibited in SBN:70 crystal have a strong link to the configuration of ferroelectric microdomains. The large leakage current revealed in SBN:26 may compensate internal charges acti…
Atomic-scale understanding of HfO2 ferroelectricity is important to help address many challenges in developing reliable and high-performance ferroelectric HfO2 (fe-HfO2) based devices. Though investigated from different angles, a factor that is real device-relevant and clearly deserves more attention has largely been overlooked by previous research, namely, the fe-HfO2/dielectric interface. Here, we investigate the electronic structures of several typical interfaces formed between ultrathin fe-HfO2 and oxide dielectrics in the sub-3-nm region. We find that interface formation introduces strong…
Lead-free Ba0.85Ca0.15Zr0.10Ti0.90O3 (BCZT) ceramics have demonstrated excellent dielectric, ferroelectric and piezoelectric properties in comparison to lead-based materials. The synthesis of pure and crystalline BCZT nanopowders at low temperatures of 25, 80 and 160 C was reported previously by using a sol-gel method followed by a hydrothermal route. In this study, the structural, dielectric and ferroelectric properties of sintered BCZT ceramics at 1250 °C for 10h were investigated. XRD measurements revealed the presence of a single perovskite phase at room temperature with the coexistence of…
The momentum-dependent Rashba and Dresselhaus spin-splitting has gained much attention for its highly promising applications in spintronics. In the present work, ab initio density functional theory calculations are performed to study the spin-splitting effect in ferroelectric oxide perovskite KIO3. Our calculations are additionally supported by symmetry adapted two-band k.p Hamiltonian. Non-negligible spin-splitting effect is observed at conduction band minimum (CBm) and valence band maximum (VBM) for rhombohedral R3m and R3c phases. Linear Rashba terms successfully explain the splitting at VB…
We propose a device model that elucidates the role of domain walls in the photovoltaic effect in multi-domain ferroelectric perovskites. The model accounts for the intricate interplay between ferroelectric polarization, space charges, photo-generation and electronic transport. When applied to bismuth ferrite, results show a significant electric potential step across both 71-degree and 109-degree domain walls, which in turn contributes to the photovoltaic (PV) effect. We also find a strong correlation between polarization and oxygen octahedra tilts, which indicates the nontrivial role of the la…
The origin of the functional properties of complex oxide superlattices can be resolved using time-resolved synchrotron x-ray diffraction into contributions from the component layers making up the repeating unit. The CaTiO3 layers of a CaTiO3/BaTiO3 superlattice have a piezoelectric response to an applied electric field, consistent with a large continuous polarization throughout the superlattice. The overall piezoelectric coefficient at large strains, 54 pm/V, agrees with first-principles predictions in which a tetragonal symmetry is imposed on the superlattice by the SrTiO3 substrate.
CuCrS2, a Heisenberg antiferromagnet with layered edge sharing triangular lattice, exhibits a spiral magnetic order. Dielectric (E) and polarization studies show magnetoelectric (ME) coupling at Neel temperature (T_N=38 K) where simultaneous dielectric and magnetic long range order occur. The compound shows a diffused ferroelectric (FE) transition and slow relaxation dynamics above T_N, indicative of relaxor FE behavior. Interestingly, memory effect and magnetic field induced rejuvenation are also observed in E, establishing cooperative glassy dynamics and ME coupling even above T_N. We discus…
New relaxor ferroelectric system has been synthesized. BLTN exhibits a smeared maximum of permittivity, characteristic of classic relaxor behaviour, with a peak shift from 185 K at 100 Hz to 300 K at 1 GHz. BNTN undergoes a first order ferroelectric phase transition at 389 K and BLNTN exhibits both a ferroelectric phase transition at 274 K and relaxor behaviour at higher temperatures.
We present a method to compute the electrooptic tensor from first principles, explicitly taking into account the electronic, ionic and piezoelectric contributions. It allows us to study the non-linear optic behavior of three ferroelectric ABO_3 compounds : LiNbO_3, BaTiO_3 and PbTiO_3. Our calculations reveal the dominant contribution of the soft mode to the electrooptic coefficients in LiNbO_3 and BaTiO_3 and identify the coupling between the electric field and the polar atomic displacements along the B-O chains as the origin of the large electrooptic response in these compounds.
Two-dimensional (2D) ferroelectricity has attracted extensive attention since its discovery in the monolayers of van der Waals materials. Here we show that 2D ferroelectricity induced by octahedral rotation distortion is widely present in the perovskite bilayer system through first-principles calculations. The perovskite tolerance factor plays a crucial role in the lattice dynamics and ground-state structure of the perovskite monolayers and bilayers, thus providing an important indicator for screening this hybrid improper ferroelectricity. Generally, the ferroelectric switching via an orthorho…
Magnetism and transport are two key functional ingredients in modern electronic devices. In oxide heterostructures, ferroelectricity can provide a new route to control these two properties via electrical operations, which is scientifically interesting and technologically important. In this Brief Review, we will introduce recent progresses on this fast developing research field. Several subtopics will be covered. First, the ferroelectric polarization tuning of interfacial magnetism will be introduced, which includes the tuning of magnetization, easy axis, magnetic phases, as well as exchange bi…
The nanodomain pattern in ferroelectric/dielectric superlattices transforms to a uniform polarization state under above-bandgap optical excitation. X-ray scattering reveals a disappearance of domain diffuse scattering and an expansion of the lattice. The reappearance of the domain pattern occurs over a period of seconds at room temperature, suggesting a transformation mechanism in which charge carriers in long-lived trap states screen the depolarization field. A Landau-Ginzburg-Devonshire model predicts changes in lattice parameter and a critical carrier concentration for the transformation.
A series of Pb-free ferroelectric materials Ba0.9Sr0.1Ti1-xSnxO3 (BSTS-x) with 0 < x < 0.15 was successfully prepared via solid-state reaction method. The effect of Sn substitution on the crystal structure, microstructure, dielectric behavior, ferroelectric and tunable features of BSTS-x ceramics were systematically investigated. Room temperature (RT) x-ray diffraction (XRD) analysis using the Rietveld refinement method reveals that all the synthesized BSTS-x ceramics were well crystallized into single perovskite structure. The results show a tetragonal phase for 0.00 < x < 0.02, which evolves…
A microscopic model Hamiltonian for the ferroelectric field effect is introduced for the study of oxide heterostructures with ferroelectric components. The long-range Coulomb interaction is incorporated as an electrostatic potential, solved self-consistently together with the charge distribution. A generic double-exchange system is used as the conducting channel, epitaxially attached to the ferroelectric gate. The observed ferroelectric screening effect, namely the charge accumulation/depletion near the interface, is shown to drive interfacial phase transitions that give rise to robust magneto…
An ab initio structure optimization technique is newly developed to determine the valley line on a total-energy surface for zone-center distortions of ferroelectric perovskite oxides and is applied to barium titanate BaTiO3 and lead titanate PbTiO3. The proposed technique is an improvement over King-Smith and Vanderbilt's scheme [Phys. Rev. B 49, p.5828 (1994)] of evaluating total energy as a function of the amplitude of atomic displacements. The results of numerical calculations show that total energy can be expressed as a fourth-order function of the amplitude of atomic displacements in BaTi…
Polar discontinuities and structural changes at oxide interfaces can give rise to a large variety of electronic and ionic phenomena. Related effects have been intensively studied in epitaxial systems, including ferroelectric domain walls and interfaces in superlattices. Here, we investigate the relation between polar discontinuities and the local chemistry at grain boundaries in polycrystalline ferroelectric ErMnO3. Using orientation mapping and different scanning probe microscopy techniques, we demonstrate that the polycrystalline material develops charged grain boundaries with enhanced elect…
Within the modified model of proton ordering of one-dimensional ferroelectric having hydrogen bonds of PbHPO$_4$-type, their thermodynamic and dynamic characteristics are studied and calculated taking into account the linear (by crystal deformations $\varepsilon_i$ ($i=1,3$) and $\varepsilon_4$) contributions into the energy of a proton system but without taking into account the tunneling in the two-particle cluster approximation. There has been obtained a good quantitative description of the temperature dependence of polarization, static dielectric permittivity, heat capacity and frequency de…
A method for the calculation of the temperature dependence of dielectric and piezoelectric responses, based on the use of a first-principles effective Hamiltonian, is described. Results are presented for the ferroelectric perovskite PbTiO3. While the method includes only the soft-mode contributions to the responses, it is argued to give a good description of the divergences or near-divergences of the response functions near the cubic-tetragonal transition. The expression of the response functions in terms of correlation functions is used to provide a real-space interpretation of the responses …
We describe the static dielectric response of ferroelastic-dielectric microcomposites. Dependence on temperature, pressure and concentration is considered for temperatures in the paraelastic transition. In recent years there has been considerable interest in perovskite oxides for application in solid oxide fuel cells (SOFC), exhaust gas sensors in automobiles, membranes for separation processes and as catalysts, which are of the ferroeleastic nature, f.e. of the ($ LaSrCoO_{3}$) type. Ferroelastic-dielectric microcomposites and measurement of their properties may improve properties of perovski…
The second and third order nonlinear susceptibilities of the ferroelectric oxides LiNbO$_3$, LiTaO$_3$, and KNbO$_3$ are calculated from first principles. Two distinct methodologies are compared, one approach is based on a perturbative approach within the frequency-domain, another on the time-evolution of the electric polarization. The frequency dependence of the second harmonic coefficients of the ferroelectric phase of LiNbO$_3$ calculated within the two approaches is in excellent agreement. This is further validated by experimental data for LiNbO$_3$ and LiTaO$_3$, measured for an incident …
The discovery of ferroelectric HfO2 in thin films and more recently in bulk is an important breakthrough because of its silicon-compatibility and unexpectedly persistent polarization at low dimensions, but the origin of its ferroelectricity is still under debate. The stabilization of the metastable polar orthorhombic phase was often considered as the cumulative result of various extrinsic factors such as stress, grain boundary, and oxygen vacancies as well as phase transition kinetics during the annealing process. We propose a novel mechanism to stabilize the polar orthorhombic phase over the …
Prediction of properties from composition is a fundamental goal of materials science and can greatly accelerate development of functional materials. It is particularly relevant for ferroelectric perovskite solid solutions where compositional variation is a primary tool for materials design. To advance beyond the commonly used Landau-Ginzburg-Devonshire and density functional theory methods that despite their power are not predictive, we elucidate the key interactions that govern ferroelectrics using 5-atom bulk unit cells and non-ground-state defect-like ferroelectric domain walls as a simple …
Advances in complex oxide heteroepitaxy have highlighted the enormous potential of utilizing strain engineering via lattice mismatch to control ferroelectricity in thin-film heterostructures. This approach, however, lacks the ability to produce large and continuously variable strain states, thus limiting the potential for designing and tuning the desired properties of ferroelectric films. Here, we observe and explore dynamic strain-induced ferroelectricity in SrTiO$_3$ by laminating freestanding oxide films onto a stretchable polymer substrate. Using a combination of scanning probe microscopy,…
The radiofrequency dielectric response of the lead-free Ba(Zr$_{0.5}$Ti$_{0.5}$)O$_3$ relaxor ferroelectric is simulated using a coarse-grained Hamiltonian. This concept, taken from Real-Space Renormalization Group theories, allows depicting the collective behavior of correlated local modes gathered in blocks. Free-energy barriers for their thermally activated collective hopping are deduced from this {\it ab-initio}-based approach, and used as input data of Kinetic Monte Carlo simulations. The resulting numerical scheme allows to simulate the dielectric response for external field frequencies …
We present the first analytical study of phase transitions in ferroelastic-ferroelectric epitaxial thin films on exactly solvable model. The emerging domain structure with domains of equal width (which may be exponentially large on a "soft" substrate) always remains stable irrespective of the film thickness. The dielectric response of an epitaxial film is {\em smaller} than that of a free film, in striking contrast with assertions in the literature.
