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Polarization dynamics and domain structure evolution in ferroelectric Al0.93B0.07N are studied using piezoresponse force microscopy and spectroscopies in ambient and controlled atmosphere environments. The application of negative unipolar and bipolar first‐order reverse curve (FORC) waveforms leads to a protrusion‐like feature on the Al0.93B0.07N surface and a reduction of electromechanical response due to electrochemical reactivity. A surface change is also observed on the application of fast alternating current bias. At the same time, the application of positive biases does not lead to surface changes. Comparatively in a controlled glove box atmosphere, stable polarization patterns can be observed, with minuscule changes in surface morphology. This surface morphology change is not isolated to applying biases to free surface, a similar topographical change is also observed at the electrode edges when cycling a capacitor in an ambient environment. The study suggests that surface electrochemical reactivity may have a significant impact on the functionality of this material in the ambient environment. However, even in the controlled atmosphere, the participation of the surface ions in polarization switching phenomena and ionic compensation is possible. [ABSTRACT FROM AUTHOR]

Ferroelectricity in van der Waals (vdW) layered material has attracted a great deal of interest recently. CuInP2S6 (CIPS), the only vdW layered material whose ferroelectricity in the bulk was demonstrated by direct polarization measurements, was shown to remain ferroelectric down to a thickness of a few nanometers. However, its ferroelectric properties have just started to be explored in the context of potential device applications. We report here the preparation and measurements of metal-ferroelectric semiconductor-metal heterostructures using nanosheets of CIPS obtained by mechanical exfoliation. Four bias voltage and polarization dependent resistive states were observed in the current–voltage characteristics, which we attribute to the formation of ferroelectric Schottky diode, along with switching behavior. [ABSTRACT FROM AUTHOR]

Polarization domains in ferroelectric materials and the ability to orient them with an external electric field lead to the development of a variety of applications from information storage to actuation. The development of piezoresponse force microscopy (PFM) has enabled researchers to investigate ferroelectric domains and ferroelectric domain switching on the nanoscale, which offers a pathway to study structure-function relationships in this important material class. Due to its commercial availability and ease of use, PFM has become a widely used research tool. However, measurement artifacts, i.e., alternative signal origins besides the piezoelectric effect are barely discussed or considered. This becomes especially important for materials with a small piezoelectric coefficient or materials with unknown ferroelectric properties, including non-ferroelectric materials. Here, the role of surface charges and current flow during PFM measurements on classical ferroelectrics are discussed and it will be shown how they alter the PFM hysteresis loop shape. This will help to better address alternative signal origins in PFM-type experiments and offer a pathway to study additional phenomena besides ferroelectricity. [ABSTRACT FROM AUTHOR]

Metal halide perovskites (MHPs) as one of the most active materials gained tremendous attention in the past decade because of their outstanding performance in optoelectronics. Owing to their perovskite structure, ferroelectricity is anticipated in this class of materials. However, whether MHPs are ferroelectric or not remains elusive. Recently, discussion regarding ferroelasticity in MHPs has been also raised. In addition, ionic motion and structural dynamics are well known in MHPs. The interplay of these phenomena including electric polarization, strain, ionic motion, and structural dynamics can have a significant impact on optoelectronics. Therefore, understanding the mechanism behind these phenomena and their interactions is critical in addressing the controversy about ferroicity of MHPs and developing functional devices. Here, the current findings about MHP's ferroicity are summarized and evaluated and a perspective for the future is provided. It is suggested that ionic motion and associated phenomena, coupled with ferroic behavior, are the main drivers behind MHPs functionality. The challenges are also discussed in probing MHPs' ferroicity and what new measurement modalities are needed to fully understand and characterize MHP behavior. Finally, it is discussed how ferroic and strain can affect the optoelectronic performance of MHPs and how they can be used for engineering of higher performance devices. [ABSTRACT FROM AUTHOR]

General features of finite size effects in the ferroelectric-semiconductor film under open-circuit electric boundary conditions are analyzed using Landau-Ginzburg-Devonshire theory and continuum media electrostatics. The temperature dependence of the film critical thickness, spontaneous polarization, and depolarization field profiles of the open-circuited films are found to be significantly different from the characteristics of short-circuited ones. In particular, we predict the re-entrant type transition boundary between the mono-domain and poly-domain ferroelectric states due to reduced internal screening efficiency and analyzed possible experimental scenarios created by this mechanism. Performed analysis is relevant for the quantitative description of free-standing ferroelectric films phase diagrams and polar properties. Also our results can be useful for the explanation of the scanning-probe microscopy experiments on free ferroelectric surfaces. [ABSTRACT FROM AUTHOR]

Metal halide perovskites (MHPs) have attracted broad research interest due to their outstanding optoelectronic performance. This performance has been attributed in part to the presence of polarization in these materials. However, the precise effects of chemical environment and strain condition on the polar states in MHPs have largely been missing. It is revealed for the first time that chemical gradient is directly coupled with strain gradient in CH3NH3PbI3. This strain–chemical gradient induces an electric polarization that can potentially affect charge carrier dynamics. Furthermore, it is unveiled that this electric polarization—unlike ferroelectricity that only exists in noncentrosymmetric materials—can be present in both tetragonal and cubic phases of CH3NH3PbI3. This suggests that the strain–chemical gradient induced polarization is a more convincing explanation of the outstanding photovoltaic properties of MHPs than the hotly debated ferroelectric polarization. Finally, a mechanism of how this polarization impacts photovoltaic action is proposed, which offers insightful advances in the development of MHPs. [ABSTRACT FROM AUTHOR]

Ferroelectric domain nucleation and growth in multiferroic BiFeO3 films is observed directly by applying a local electric field with a conductive tip inside a scanning transmission electron microscope. The nucleation and growth of a ferroelastic domain and its interaction with pre-existing 71° domain walls are observed and compared with the results of phase-field modeling. In particular, a preferential nucleation site and direction-dependent pinning of domain walls are observed due to slow kinetics of metastable switching in the sample without a bottom electrode. These in situ spatially resolved observations of a first-order bias-induced phase transition reveal the mesoscopic mechanisms underpinning functionality of a wide range of multiferroic materials. [ABSTRACT FROM AUTHOR]

We study the effect of the depolarization field on a domain wall structure near the surface of a ferroelectric. Since in real situation bound and screening charges form an electric double layer, the breaking of this layer by the domain wall induces stray depolarization field, which in turn changes the domain wall structure. Power law decay of the stray field results in the power law of polarization saturation near the surface, as compared to exponential saturation in the bulk. Obtained results predict that the surface broadening of ferroelectric domain walls appeared near Curie temperature as well as describe domain wall depth profile in weak ferroelectrics. We qualitatively describe extra-broad domain walls near LiNbO3 and LiTaO3 surfaces observed experimentally at room temperature, which probably originate at high temperatures but did not fully relax their width with temperature decrease allowing for lattice pinning and defect centers. Thus results have broad implication for fundamental issues such as maximal information storage density in ferroelectric data storage, domain wall pinning mechanisms at surfaces and interfaces, and nucleation dynamics. [ABSTRACT FROM AUTHOR]

The structure of a single antiparallel ferroelectric domain wall in LiNbO3 is quantitatively mapped by piezoelectric force microscopy (PFM) with calibrated probe geometry. The PFM measurements are performed for 49 probes with the radius varying from 10 to 300 nm. The magnitude and variation of the experimental piezoelectric coefficient across a domain wall match the profiles calculated from a comprehensive analytical theory, as well as three-dimensional finite element method simulations. Quantitative agreement between experimental and theoretical profile widths is obtained only when a finite disk-type tip radius that is in true contact with the sample surface is considered, which is in agreement with scanning electron microscopy images of the actual tips after imaging. The magnitude of the piezoelectric coefficient is shown to be independent of the tip radius, and the PFM profile width is linearly proportional to the tip radius. Finally we demonstrate a method to extract any intrinsic material broadening of the ferroelectric wall width. Surprisingly wide wall widths of up to 100 nm are observed in the limit of zero tip radius. [ABSTRACT FROM AUTHOR]

Ferroelectric single-crystal-architecture-in-glass is a new class of metamaterials that would enable active integrated optics if the ferroelectric behavior is preserved within the confines of glass. We demonstrate using lithium niobate crystals fabricated in lithium niobosilicate glass by femtosecond laser irradiation that not only such behavior is preserved, the ferroelectric domains can be engineered with a DC bias. A piezoresponse force microscope is used to characterize the piezoelectric and ferroelectric behavior. The piezoresponse correlates with the orientation of the crystal lattice as expected for unconfined crystal, and a complex micro- and nano-scale ferroelectric domain structure of the as-grown crystals is revealed. [ABSTRACT FROM AUTHOR]

A preface for the topic piezoresponse force microscopy and nanoscale phenomena in polar materials is presented.

The recent discovery of twin domains in MAPbI3 perovskites has initiated contentious discussion on the ferroic nature of hybrid perovskites. Ferroelectric polarization is thought to facilitate the dissociation of photoinduced electron-hole pairs, helping to explain the extraordinary photovoltaic performance exhibited by this class of materials. Alternate to ferroelectricity, which has yet to be unambiguously established despite considerable efforts to do so, ferroelasticity was also proposed in these materials. Meanwhile, given the coupling of ionic states and ferroelectricity and the interconnected nature of defect chemistry and ferroelasticity, the electrochemical reactivity can no longer be ignored. In this work, using band excitation piezoresponse force microscopy, we reveal the variation in elasticity between adjacent domains, indicating the ferroelasticity and the difference in the crystallographic states of the twin domain. Moreover, using band excitation contact Kelvin probe force microscopy, we dynamically map the evolution of the twinning structure under electric bias. These results help decipher the effect of the twin domains on ionic mobility and ion diffusion pathways. Combining these results, we reveal the interaction of twin domains and ionic activity in this material. Overall, this work provides insights into the twinning structure in MAPbI3 and its potential effects on the hybrid perovskite optoelectronics. [ABSTRACT FROM AUTHOR]

Ferroelectric materials have remained one of the major focal points of condensed matter physics and materials science for over 50 years. In the last 20 years, the development of voltage-modulated scanning probe microscopy techniques, exemplified by Piezoresponse force microscopy (PFM) and associated time- and voltage spectroscopies, opened a pathway to explore these materials on a singledigit nanometer level. Consequently, domain structures and walls and polarization dynamics can now be imaged in real space. More generally, PFM has allowed studying electromechanical coupling in a broad variety of materials ranging from ionics to biological systems. It can also be anticipated that the recent Nobel prize ["The Nobel Prize in Chemistry 2016," http://www.nobelprize.org/ nobel_prizes/chemistry/laureates/2016/ (Nobel Media, 2016)] in molecular electromechanical machines will result in rapid growth in interest in PFM as a method to probe their behavior on single device and device assembly levels. However, the broad introduction of PFM also resulted in a growing number of reports on the nearly ubiquitous presence of ferroelectric-like phenomena including remnant polar states and electromechanical hysteresis loops in materials which are non-ferroelectric in the bulk or in cases where size effects are expected to suppress ferroelectricity. While in certain cases plausible physical mechanisms can be suggested, there is remarkable similarity in observed behaviors, irrespective of the materials system. In this review, we summarize the basic principles of PFM, briefly discuss the features of ferroelectric surfaces salient to PFM imaging and spectroscopy, and summarize existing reports on ferroelectric-like responses in non-classical ferroelectric materials. We further discuss possible mechanisms behind observed behaviors and possible experimental strategies for their identification. [ABSTRACT FROM AUTHOR]

Ferroelectric and ferroelastic domain walls play important roles in ferroelectric properties. However, their couplings with flexoelectricity have been less understood. In this work, we applied phase-field simulation to investigate the flexoelectric coupling with ferroelectric a/c twin structures in lead ziconate titanate thin films. Local stress gradients were found to exist near twin walls that created both lateral and vertical electric fields through the flexoelectric effect, resulting in polarization inclinations from either horizontal or normal orientation, polarization rotation angles deviated from 90°, and consequently highly asymmetric a/c twin walls. By tuning the flexoelectric strengths in a reasonable range from first-principles calculations, we found that the transverse flexoelectric coefficient has a larger influence on the polarization rotation than longitudinal and shear coefficients. As polar rotations that commonly occur at compositional morphotropic phase boundaries contribute to the piezoelectric enhancement, this work calls for further exploration of alternative strain-engineered polar rotations via flexoelectricity in ferroelectric thin films. [ABSTRACT FROM AUTHOR]

The interplay between electrochemical surface charges and bulk ferroelectricity in thin films gives rise to a continuum of coupled ferro-ionic states. These states are exquisitely sensitive to chemical and electric conditions at the surfaces, applied voltage, and oxygen pressure. Using the analytical approach combining the Ginzburg-Landau-Devonshire description of the ferroelectricity with the Langmuir adsorption isotherm for the ions at the film surface, we have studied the temperature-, time- and field-dependent polarization changes and electromechanical response of the ferro-ionic states. The responses are found to be inseparable in thermodynamic equilibrium and at low frequencies of applied voltage. The states become separable in the high frequency dynamic mode due to the several orders of magnitude difference in the relaxation times of ferroelectric polarization and surface ion charge density. These studies provide an insight into the dynamic behavior of nanoscale ferroelectrics with an open surface exposed to different kinds of the electrochemically active gaseous surrounding. [ABSTRACT FROM AUTHOR]

A three-dimensional phenomenological model is proposed to describe both ferroelectricity and antiferroelectricity based on the Ginzburg-Landau-Devonshire theory. Its application to the multiferroic Sm-doped BiFeO3 system describes the temperature-, pressure-, and composition-induced ferroelectric to antiferroelectric phase transitions. The constructed temperature-composition and temperature-pressure phase diagrams show that compressive hydrostatic pressure and Sm doping have similar effects on the ferroelectric and antiferroelectric phase transitions. It is also indicated from the temperature-pressure phase diagram that the experimentally observed phase of BiFeO3 under the hydrostatic pressure from 3GPa to 10GPa is a PbZrO3-like antiferroelectric phase. [ABSTRACT FROM AUTHOR]

The development of interface-based magnetoelectric devices necessitates an understanding of polarization-mediated electronic phenomena and atomistic polarization screening mechanisms. In this work, the LSMO/BFO interface is studied on a single unit-cell level through a combination of direct order parameter mapping by scanning transmission electron microscopy and electron energy-loss spectroscopy. We demonstrate an unexpected ~5% lattice expansion for regions with negative polarization charge, with a concurrent anomalous decrease of the Mn valence and change in oxygen K-edge intensity. We interpret this behaviour as direct evidence for screening by oxygen vacancies. The vacancies are predominantly accumulated at the second atomic layer of BFO, reflecting the difference of ionic conductivity between the components. This vacancy exclusion from the interface leads to the formation of a tail-to-tail domain wall. At the same time, purely electronic screening is realized for positive polarization charge, with insignificant changes in lattice and electronic properties. These results underline the non-trivial role of electrochemical phenomena in determining the functional properties of oxide interfaces. Furthermore, these behaviours suggest that vacancy dynamics and exclusion play major roles in determining interface functionality in oxide multilayers, providing clear implications for novel functionalities in potential electronic devices. [ABSTRACT FROM AUTHOR]

The influence of an electrically inhomogeneous epitaxial bottom layer on the ferroelectric and electrical properties has been explored in epitaxial PbTiO3 (PTO)/La0.7Sr0.3MnO3 (LSMO) submicron structures using atomic force microscopy. The submicron LSMO-dot structures underneath the ferroelectric PTO film allow exploring gradual changes in material properties. The LSMO interfacial layer influences significantly both electrical and ferroelectric properties of the upper PTO layer. The obtained results show that the as-grown polarization state of an epitaxial ferroelectric layer is strongly influenced by the properties of the layer on top of which it is deposited. [ABSTRACT FROM AUTHOR]

Ferroelectrics and multiferroics have recently emerged as perspective materials for information technology and data storage applications. The combination of extremely narrow domain wall width and the capability to manipulate polarization by electric field opens the pathway toward ultrahigh (>10 TBit inch-2) storage densities and small (sub-10 nm) feature sizes. The coupling between polarization and chemical and transport properties enables applications in ferroelectric lithography and electroresistive devices. The progress in these applications, as well as fundamental studies of polarization dynamics and the role of defects and disorder on domain nucleation and wall motion, requires the capability to probe these effects on the nanometer scale. In this review, we summarize the recent progress in applications of piezoresponse force microscopy (PFM) for imaging, manipulation and spectroscopy of ferroelectric switching processes. We briefly introduce the principles and relevant instrumental aspects of PFM, with special emphasis on resolution and information limits. The local imaging studies of domain dynamics, including local switching and relaxation accessed through imaging experiments and spectroscopic studies of polarization switching, are discussed in detail. Finally, we review the recent progress on understanding and exploiting photochemical processes on ferroelectric surfaces, the role of surface adsorbates, and imaging and switching in liquids. Beyond classical applications, probing local bias-induced transition dynamics by PFM opens the pathway to studies of the influence of a single defect on electrochemical and solid state processes, thus providing model systems for batteries, fuel cells and supercapacitor applications. [ABSTRACT FROM AUTHOR]

Piezoresponse force microscopy (PFM) has emerged as a powerful and versatile tool for probing nanoscale phenomena in ferroelectric materials on the nanometer and micrometer scales. In this review, we summarize the fundamentals and recent advances in PFM, and describe the nanoscale electromechanical properties of several important ferroelectric ceramic materials widely used in memory and microelectromechanical systems applications. Probing static and dynamic polarization behavior of individual grains in PZT films and ceramics is discussed. Switching spectroscopy PFM is introduced as a useful tool for studying defects and interfaces in ceramic materials. The results on local switching and domain pinning behavior, as well as nanoscale fatigue and imprint mapping are presented. Probing domain structures and polarization dynamics in polycrystalline relaxors (PMN-PT, PLZT, doped BaTiO3) are briefly outlined. Finally, applications of PFM to dimensionally confined ferroelectrics are demonstrated. The potential of PFM for studying local electromechanical phenomena in polycrystalline ferroelectrics where defects and other inhomogeneities are essential for the interpretation of their macroscopic properties is illustrated. [ABSTRACT FROM AUTHOR]

Macroscopic ferroelectric polarization switching, similar to other first-order phase transitions, is controlled by nucleation centres. Despite 50 years of extensive theoretical and experimental effort, the microstructural origins of the Landauer paradox, that is, the experimentally observed low values of coercive fields in ferroelectrics corresponding to implausibly large nucleation activation energies, are still a mystery. Here, we develop an approach to visualize the nucleation centres controlling polarization switching processes with nanometre resolution, determine their spatial and energy distribution and correlate them to local microstructure. The random-bond and random-field components of the disorder potential are extracted from positive and negative nucleation biases. Observation of enhanced nucleation activity at the 90∘ domain wall boundaries and intersections combined with phase-field modelling identifies them as a class of nucleation centres that control switching in structural-defect-free materials. [ABSTRACT FROM AUTHOR]

The effective piezoelectric coefficients of twin walls in tetragonal ferroelectric are calculated in the framework of decoupling approximation and Landau-Ginzburg-Devonshire theory allowing for polarization gradient terms, electrostriction and flexoelectric coupling. Using an example of piezoelectric response of a1-a2 twins to a homogeneous electric field, we show that the response is almost independent on the flexoelectric coupling, but is very sensitive to the values of polarization gradient coefficients. This behavior originates from the strong coupling between local dielectric susceptibility and the gradient coefficients. The enhancement of piezoelectric response from 10% up to a factor of 103 times is predicted. The local electromechanical response of the domain walls can thus provide information on the gradient terms in Ginzburg-Landau-Devonshire expansion and pinning mechanisms of the ferroelectric domain walls. The observability of these effects by the piezoresponse force microscopy of electroded structures and impact on the functional properties of the systems with dense domain structures are analyzed. [ABSTRACT FROM AUTHOR]

The role of elastic defects on the kinetics of 180° uncharged ferroelectric domain wall motion is explored using continuum time-dependent Landau-Ginzburg-Devonshire equation with elastic dipole coupling. In one dimensional case, ripples, steps, and oscillations of the domain wall velocity appear due to the wall-defect interactions. While the defects do not affect the limiting-wall velocity vs. field dependence, they result in the minimal threshold field required to activate the wall motions. The analytical expressions for the threshold field are derived and the latter is shown to be much smaller than the thermodynamic coercive field. The threshold field is linearly proportional to the concentration of defects and non-monotonically depends on the average distance between them. The obtained results provide the insight into the mesoscopic mechanism of the domain wall pinning by elastic defects in ferroelectrics. [ABSTRACT FROM AUTHOR]

Time-resolved piezoresponse force spectroscopy (TR-PFS) and spectroscopic imaging are developed to probe the spatial variability of relaxation behavior in nanoscale ferroelectric materials and structures. TR-PFS was applied to study polarization dynamics in polyvinylidine fluoride and trifluoroethylene nanomesas. We demonstrate that polarization relaxation in ferroelectric polymers is slow even on the ∼10 nm length scale of piezoresponse force microscopy (PFM) signal generation. Furthermore, the relaxation times are found to be nonuniform within the nanomesa, indicative of a complex internal structure. The applicability of TR-PFM for studies of polarization dynamics in ferroelectric polymers and relaxors is discussed. [ABSTRACT FROM AUTHOR]

One of the key limiting factors in the quantitative interpretation of piezoresponse force microscopy (PFM) is the lack of knowledge on the effective tip geometry. Here the authors derive analytical expressions for a 180° domain wall profile in PFM for the point charge, sphere plane, and disk electrode models of the tip. An approach for the determination of the effective tip parameters from the wall profile is suggested and illustrated for several ferroelectric materials. The calculated tip parameters can be used self-consistently for the interpretation of PFM resolution and spectroscopy data, i.e., linear imaging processes. [ABSTRACT FROM AUTHOR]

Piezoresponse force microscopy has been used to manipulate and image polarization of ferroelectric polymer Langmuir-Blodgett films at the nanoscale, achieving polarization control with a resolution below 50 nm and imaging resolution below 5 nm. Individual regions showed square polarization-voltage hysteresis loops, demonstrating bistability of the polarization state. Arbitrary polarization patterns could be repeatedly written and erased with a resolution of 25 to 50 nm, limited by grain size, demonstrating the potential for high-density data storage and retrieval at densities exceeding 250 Gbits/in2. [ABSTRACT FROM AUTHOR]

Applications of ferroelectric materials for nonvolatile memory, data storage devices, nanosensors, and nanoactuators necessitate fundamental studies of ferroelectric behavior, including the presence of switchable polarization and switching behavior, on the nanoscale. Here the authors investigated the switching properties of (Na½Bi½)0.9Ba0.1TiO3 nanocrystals prepared by a mist deposition technique using piezoresponse force microscopy (PFM) and spectroscopy. By using stiff cantilevers, reliable PFM data have been obtained and local electromechanical response was measured. The transition from ferroelectric to superparaelectric behavior in these nanocrystals was observed at sizes of ∼10 nm. The effects of particle shape on the PFM imaging are also discussed. [ABSTRACT FROM AUTHOR]

Piezoresponse force microscopy (PFM) and spectroscopy of domain structure and switching dynamics at small excitation voltages require resonance enhancement of the surface displacements. The contact stiffness depends strongly on local elastic properties and topography resulting in significant variations of the resonant frequency. Moreover, the resonant response is determined both by the Q factor and the electromechanical activity. Here we develop a resonance-enhanced PFM that allows mapping of the local electromechanical activity, contact stiffness, and loss factor, thus avoiding limitations inherent to conventional frequency tracking. We anticipate that this method will be instrumental in imaging weakly piezoelectric materials and probing inelastic phenomena in ferroelectrics. [ABSTRACT FROM AUTHOR]

The application of ferroelectric materials for electronic devices necessitates the quantitative study of local switching behavior, including imprint, coercive bias, remanent and saturation responses, and work of switching. Here we introduce switching spectroscopy piezoresponse force microscopy as a tool for real-space imaging of switching properties on the nanoscale. The hysteresis curves, acquired at each point in the image, are analyzed in the thermodynamic and kinetic limits. We expect that this approach will further understanding of the relationships between material microstructure and polarization switching phenomena on the nanoscale, and provide a quantitative tool for ferroelectric-based device characterization. [ABSTRACT FROM AUTHOR]

LaBGeO5 is a model transparent ferroelectric glass-ceramic (TFGC) material, developed as an inexpensive alternative to single-crystal nonlinear optical materials. The optical activity of the TFGC originates from the ferroelectric phase which remains under a hydrostatic pressure exerted by the surrounding glass matrix. A combination of two techniques, electron-backscattered diffraction (EBSD) and piezoresponse force microscopy (PFM), is employed to monitor the development of the ferroelectric phase. A method is proposed to theoretically construct PFM amplitude maps from EBSD orientation maps. The theoretical vertical piezoresponse map is compared with the experimental piezoresponse map from PFM. A good correlation between the theoretical and experimental maps is observed. [ABSTRACT FROM AUTHOR]

We have developed a multisample film growth method on a temperature-gradient substrate holder to quickly optimize the film growth temperature in pulsed-laser deposition. A smooth temperature gradient is achieved, covering a range of temperatures from 200 to 830 °C. In a single growth run, the optimal growth temperature for Sr[sub x]Ba[sub 1-x]Nb[sub 2]O[sub 6] thin films on MgO(001) substrates was determined to be 750 °C, based on results from ellipsometry and piezoresponse force microscopy. Variations in optical properties and ferroelectric domains structures were clearly observed as function of growth temperature, and these physical properties can be related to their different crystalline quality. Piezoresponse force microscopy indicated the formation of uniform ferroelectric film for deposition temperatures above 750 °C. At 660 °C, isolated micron-sized ferroelectric islands were observed, while samples deposited below 550 °C did not exhibit clear piezoelectric contrast. © 2004 American Institute of Physics. [ABSTRACT FROM AUTHOR]

SrTiO3 epitaxial growth by molecular beam epitaxy (MBE) on silicon has opened up the route to the monolithic integration of various complex oxides on the complementary metal-oxide–semiconductor silicon platform. Among functional oxides, ferroelectric perovskite oxides offer promising perspectives to improve or add functionalities on-chip. We review the growth by MBE of the ferroelectric compound BaTiO3 on silicon (Si), germanium (Ge) and gallium arsenide (GaAs) and we discuss the film properties in terms of crystalline structure, microstructure and ferroelectricity. Finally, we review the last developments in two areas of interest for the applications of BaTiO3 films on silicon, namely integrated photonics, which benefits from the large Pockels effect of BaTiO3, and low power logic devices, which may benefit from the negative capacitance of the ferroelectric. [ABSTRACT FROM AUTHOR]

A correction to the article "Influence of a Single Grain Boundary on Domain Wall Motion in Ferroelectrics" that was published in a 2014 issue is presented.

Abstract Ferroelectric surfaces and interfaces are unique physical objects for fundamental studies of various screening mechanisms of spontaneous polarization by free carriers and possible ion exchange between the polar surface and ambient media. The theory of the polarization charge compensation at ferroelectric surface by ambient screening charges requires a detailed comparison of different screening models. In the article, we study the free energy of a thin ferroelectric film covered by a screening charge layer of different nature and calculate hysteresis loops of polarization and screening charge in the system at different temperatures. The dependence of the screening charge density on electric potential was considered for three basic models, namely for the linear Bardeen-type surface states (BS) and nonlinear the Fermi-Dirac (FD) density of states describing two-dimensional electron gas at the film surface, and the strongly nonlinear electrochemical Stephenson-Highland (SH) model describing the surface charge density of absorbed ions. Among considered surface screening models, the most various behavior of polarization and screening charge hysteresis loops is inherent to SH model. Obtained results give new insight to the understanding of bound charge compensation at ferroelectric surfaces at different temperatures, as well as they open the way to control the polarization reversal in thin ferroelectric films by appropriate choice of the surface charge nature and screening mechanism. Graphical abstract Image 1 [ABSTRACT FROM AUTHOR]

This work explores a nontrivial temperature behavior of the carriers concentration, which governs the conductance of the graphene channel on ferroelectric substrate with domain walls that is a basic element for field effect transistors of new generation. We revealed the transition from a single to double antiferroelectric-like hysteresis loop of the concentration voltage dependence that happens with the temperature increase and then exist in a wide temperature range (350–500) K. We have shown that the double loops of polarization and concentration can have irregular shape that remains irregular as long as the computation takes place, and the voltage position of the different features (jumps, secondary maxima, etc) changes from one period to another, leading to the impression of quasi-chaotic behavior. It appeared that these effects originate from the nonlinear screening of ferroelectric polarization by graphene carriers, as well as it is conditioned by the temperature evolution of the domain structure kinetics in ferroelectric substrate. The nonlinearity rules the voltage behavior of polarization screening by graphene 2D-layer and at the same time induces the motion of separated domain walls accompanied by the motion of p-n junction along the graphene channel. Since the domain walls structure, period and kinetics can be controlled by changing the temperature, we concluded that the considered nano-structures based on graphene-on-ferroelectric are promising for the fabrication of new generation of modulators based on the graphene p-n junctions. [ABSTRACT FROM AUTHOR]

Polarization reversal in ferroelectric nanomesas of polyvinylidene fluoride with trifluoroethylene has been probed by ultrahigh vacuum piezoresponse force microscopy in a wide temperature range from 89 to 326 K. In dramatic contrast to the macroscopic data, the piezoresponse force microscopy local switching was nonthermally activated and, at the same time, occurring at electric fields significantly lower than the intrinsic switching threshold. A "cold-field" defect-mediated extrinsic switching is shown to be an adequate scenario describing this peculiar switching behavior. The extrinsic character of the observed polarization reversal suggests that there is no fundamental bar for lowering the coercive field in ferroelectric polymer nanostmctures, which is of importance for their applications in functional electronics. [ABSTRACT FROM AUTHOR]

Using piezoresponse force microscopy in an ultrahigh vacuum, polarization switching has been detected and quantified in epitaxial BiFeO3 films from 200 to about 4 unit cells thick. Local remnant piezoresponse was utilized to probe both ferroelectric properties and effects of imperfect electrical contacts. It was found that the shape of electromechanical hysteresis loops is strongly influenced by an extrinsic dielectric gap. primarily through the suppressing effect of the depolarizing field on the spontaneous polarization in the ultrathin films. Furthermore, statistical analysis o( the hysteresis loops has revealed lateral variation of the extrinsic dielectric-gap with sub-10-nm resolution. Robust and reproducible ferroelectric properties of nanoscale BiFeO3 indicate its potential for nanoscale applications in information storage and spintmnics. [ABSTRACT FROM AUTHOR]

Abstract: Grain-to-grain long-range interactions and the ensuing collective dynamics in the domain behavior of nanostructured polycrystalline Pb(Zr,Ti)O3 ferroelectric thin films have been investigated. To identify the key factors and interactions controlling local polarization dynamics we utilize a synergistic approach based on focused ion beam (FIB) milled damage-free nanostructures to isolate single grains and grain clusters, time-resolved piezoresponse force microscopy and switching spectroscopy PFM (SSPFM) (PFM) to address polarization dynamics within individual grains, and finite-element simulations to quantify the local ferroelectric interactions and hence assess the weight of several possible switching mechanisms. The experiments find that of the three possible switching mechanisms, namely direct electromechanical coupling, local built-in electric field and strain, and grain boundary electrostatic charges, the last one is the dominant mechanism. Although finite-element simulations find that direct electromechanical coupling and local built-in field-induced switching are possible, calculations confirm that for the utilized material properties, the aforementioned mechanisms are energetically unfavored. [Copyright &y& Elsevier]

Recent observations of unusual ferroelectricity in thin films of HfO 2 and related materials has attracted broad interest to the materials and led to the emergence of a number of competing models for observed behaviors. Here we develop the analytical description for a possible electrochemical mechanism of observed ferroelectric-like behaviors, namely the collective phenomena of elastic and electric dipoles originated from oxygen vacancies. The vacancies are formed initially in the vicinity of film surfaces, grain boundaries, and other types of inhomogeneities inside the film including those induced by the film treatment. Electric cycling makes the distribution of electric dipoles more homogeneous than it was initially, providing at the same time the significant decrease in depolarization field. The ferroelectric phase is induced by the "electrochemical" coupling, that is the joint action of the omnipresent electrostriction and "chemical" pressure, which lead to the sign change of the positive coefficient α at P 2 in the order-disorder type thermodynamic functional. Negative coefficient α becomes the driving force of the transition to the long-range ordered ferroelectric phase with the spontaneous polarization P in the direction normal to the film surface. Using the above ideas, we estimated that the reversible ferroelectric polarization, as high as (5–20) μC/cm2, can be induced by oxygen vacancies in HfO 2 films of thickness less than (20–30) nm. Semi-quantitative agreement with available experimental data is demonstrated. ∙ Origin of ferroelectricity in HfO2 films is established. ∙ Elastic and electric dipoles originated from oxygen vacancies. ∙ Ferroelectricity is induced by electrochemical coupling. [ABSTRACT FROM AUTHOR]

Using the Landau-Ginzburg-Devonshire theory, we considered the impact of the flexoelectrochemical coupling on the size effects in polar properties and phase transitions of thin ferroelectric films with a layer of elastic defects. We investigated a typical case, when defects fill a thin layer below the top film surface with a constant concentration creating an additional gradient of elastic fields. The defective surface of the film is not covered with an electrode, but instead with an ultrathin layer of ambient screening charges, characterized by a surface screening length. Obtained results revealed an unexpectedly strong effect of the joint action of Vegard stresses and flexoelectric effect (shortly flexochemical coupling) on the ferroelectric transition temperature, distribution of the spontaneous polarization and elastic fields, domain wall structure and period in thin PbTi O3 films containing a layer of elastic defects. A nontrivial result is the persistence of ferroelectricity at film thicknesses below 4 nm, temperatures lower than 350 K, and relatively high surface screening length ( ~ 0.1 nm ) . The origin of this phenomenon is the flexoelectric coupling leading to the rebuilding of the domain structure in the film (namely the cross-over from c-domain stripes to a-type closure domains) when its thickness decreases below 4 nm. The ferroelectricity persistence is facilitated by negative Vegard effect. For positive Vegard effect, thicker films exhibit the appearance of pronounced maxima on the thickness dependence of the transition temperature, whose position and height can be controlled by the defect type and concentration. The revealed features may have important implications for miniaturization of ferroelectric-based devices. [ABSTRACT FROM AUTHOR]