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Ferroelectric materials play a crucial role in a broad range of technologies due to their unique properties that are deeply connected to the pattern and behavior of their ferroelectric (FE) domains. Chief among them, barium titanate (BaTiO 3 ; BTO) sees widespread applications such as in electronics but equally is a ferroelectric model system for fundamental research, e.g., to study the interplay of such FE domains, the domain walls (DWs), and their macroscopic properties, owed to BTO's multiple and experimentally accessible phase transitions. Here, we employ Second Harmonic Generation Microscopy (SHGM) to in situ investigate the cubic-to-tetragonal (at ∼ 126 ° C) and the tetragonal-to-orthorhombic (at ∼ 5 ° C) phase transition in single-crystalline BTO via three-dimensional (3D) DW mapping. We demonstrate that SHGM imaging provides the direct visualization of FE domain switching as well as the domain dynamics in 3D, shedding light on the interplay of the domain structure and phase transition. These results allow us to extract the different transition temperatures locally, to unveil the hysteresis behavior, and to determine the type of phase transition at play (first/second order) from the recorded SHGM data. The capabilities of SHGM in uncovering these crucial phenomena can easily be applied to other ferroelectrics to provide new possibilities for in situ engineering of advanced ferroic devices. [ABSTRACT FROM AUTHOR]

Magnetic force microscopy (MFM) is long established as a powerful tool for probing the local stray fields of magnetic nanostructures across a range of temperatures and applied stimuli. A major drawback of the technique, however, is that the detection of stray fields emanating from a sample's surface rely on a uniaxial vertical cantilever oscillation, and thus are only sensitive to vertically oriented stray field components. The last two decades have shown an ever-increasing literature fascination for exotic topological windings where particular attention to in-plane magnetic moment rotation is highly valuable when identifying and understanding such systems. Here, we present a method of detecting in-plane magnetic stray field components, by utilizing a split-electrode excitation piezo that allows the simultaneous excitation of a cantilever at its fundamental flexural and torsional modes. This allows for the joint acquisition of traditional vertical mode images and a lateral MFM where the tip–cantilever system is only sensitive to stray fields acting perpendicular to the torsional axis of the cantilever. [ABSTRACT FROM AUTHOR]

Ferroelectric domain walls (DWs) are promising structures for assembling future nano-electronic circuit elements on a larger scale since reporting domain wall currents of up to 1 mA per single DW. One key requirement hereto is their reproducible manufacturing by gaining preparative control over domain size and domain wall conductivity (DWC). To date, most works on DWC have focused on exploring the fundamental electrical properties of individual DWs within single-shot experiments, with an emphasis on quantifying the origins of DWC. Very few reports exist when it comes to comparing the DWC properties between two separate DWs, and literally nothing exists where issues of reproducibility in DWC devices have been addressed. To fill this gap while facing the challenge of finding guidelines for achieving predictable DWC performance, we report on a procedure that allows us to reproducibly prepare single hexagonal domains of a predefined diameter into uniaxial ferroelectric lithium niobate single crystals of 200 and 300 μ m thickness, respectively. We show that the domain diameter can be controlled with an uncertainty of a few percent. As-grown DWs are then subjected to a standard procedure of current-limited high-voltage DWC enhancement, and they repetitively reach a DWC increase of six orders of magnitude. While all resulting DWs show significantly enhanced DWC values, their individual current–voltage (I–V) characteristics exhibit different shapes, which can be explained by variations in their 3D real structure reflecting local heterogeneities by defects, DW pinning, and surface-near DW inclination. [ABSTRACT FROM AUTHOR]

Piezoresponse force microscopy (PFM) is one of the most widespread methods for investigating and visualizing ferroelectric domain structures down to the nanometer length scale. PFM makes use of the direct coupling of the piezoelectric response to the crystal lattice, and hence, it is most often applied to spatially map the three-dimensional (3D) near-surface domain distribution of any polar or ferroic sample. Nonetheless, since most samples investigated by PFM are at least semiconducting or fully insulating, the electric ac field emerging from the conductive scanning force microscopy (SFM) tip penetrates the sample and, hence, may also couple to polar features that are deeply buried into the bulk of the sample under investigation. Thus, in the work presented here, we experimentally and theoretically explore the contrast and depth resolution capabilities of PFM, by analyzing the dependence of several key parameters. These key parameters include the depth of the buried feature, i.e., here a domain wall (DW), as well as PFM-relevant technical parameters such as the tip radius, the PFM drive voltage and frequency, and the signal-to-noise ratio. The theoretical predictions are experimentally verified using x-cut periodically poled lithium niobate single crystals that are specially prepared into wedge-shaped samples, in order to allow the buried feature, here the DW, to be "positioned" at any depth into the bulk. This inspection essentially contributes to the fundamental understanding in PFM contrast analysis and to the reconstruction of 3D domain structures down to a 1 μ m-penetration depth into the sample. [ABSTRACT FROM AUTHOR]

Coherent nonlinear optical μ -spectroscopy is a frequently used tool in modern material science as it is sensitive to many different local observables, which comprise, among others, crystal symmetry and vibrational properties. The richness in information, however, may come with challenges in data interpretation, as one has to disentangle the many different effects like multiple reflections, phase jumps at interfaces, or the influence of the Guoy-phase. In order to facilitate interpretation, the work presented here proposes an easy-to-use semi-analytical modeling Ansatz, which bases upon known analytical solutions using Gaussian beams. Specifically, we apply this Ansatz to compute nonlinear optical responses of (thin film) optical materials. We try to conserve the meaning of intuitive parameters like the Gouy-phase and the nonlinear coherent interaction length. In particular, the concept of coherence length is extended, which is a must when using focal beams. The model is subsequently applied to exemplary cases of second- and third-harmonic generation. We observe a very good agreement with experimental data, and furthermore, despite the constraints and limits of the analytical Ansatz, our model performs similarly well as when using more rigorous simulations. However, it outperforms the latter in terms of computational power, requiring more than three orders less computational time and less performant computer systems. [ABSTRACT FROM AUTHOR]

Second harmonic (SH) microscopy represents a powerful tool for the investigation of crystalline systems, such as ferroelectrics and their domain walls (DWs). Under the condition of normal dispersion, i.e., the refractive index at the SH wavelength is larger as compared to the refractive index at the fundamental wavelength, n (2 ω) > --> n (ω) , bulk crystals will generate no SH signal. Should the bulk, however, contain DWs, an appreciable SH signal will still be detectable at the location of DWs stemming from the Čerenkov mechanism. In this work, we demonstrate both how SH signals are generated in bulk media and how the Čerenkov mechanism can be inhibited by using anomalous dispersion, i.e., n (ω) > --> n (2 ω). This allows us to quantitatively estimate the relative strength of the Čerenkov compared to other SH contrast mechanisms in DWs, such as the interference contrast. The results are in agreement with previous experiments based on the geometric separation of the signals. Due to the observed, strong Čerenkov contrast, such signal contributions may not be neglected in polarimetry studies of ferroelectric DWs in the future. [ABSTRACT FROM AUTHOR]

Thin-film materials from μ m thickness down to single-atomic-layered 2D materials play a central role in many novel electronic and optical applications. Coherent, nonlinear optical (NLO) μ -spectroscopy offers insight into the local thickness, stacking order, symmetry, or electronic and vibrational properties. Thin films and 2D materials are usually supported on multi-layered substrates leading to (multi-)reflections, interference, or phase jumps at interfaces during μ -spectroscopy, which all can make the interpretation of experiments particularly challenging. The disentanglement of the influence parameters can be achieved via rigorous theoretical analysis. In this work, we compare two self-developed modeling approaches, a semi-analytical and a fully vectorial model, to experiments carried out in thin-film geometry for two archetypal NLO processes, second-harmonic and third-harmonic generation. In particular, we demonstrate that thin-film interference and phase matching do heavily influence the signal strength. Furthermore, we work out key differences between three and four photon processes, such as the role of the Gouy-phase shift and the focal position. Last, we can show that a relatively simple semi-analytical model, despite its limitations, is able to accurately describe experiments at a significantly lower computational cost as compared to a full vectorial modeling. This study lays the groundwork for performing quantitative NLO μ -spectroscopy on thin films and 2D materials, as it identifies and quantifies the impact of the corresponding sample and setup parameters on the NLO signal, in order to distinguish them from genuine material properties. [ABSTRACT FROM AUTHOR]

Recent analyses by polarization resolved second-harmonic (SH) microscopy have demonstrated that ferroelectric (FE) domain walls (DWs) can possess non-Ising wall characteristics and topological nature. These analyses rely on locally analyzing the properties, directionality, and magnitude of the second-order nonlinear tensor. However, when inspecting FE DWs with SH microscopy, a manifold of different effects may contribute to the observed signal difference between domains and DWs, i.e., far-field interference, Čerenkov-type phase-matching (CSHG), and changes in the aforementioned local nonlinear optical properties. They all might be present at the same time and, therefore, require careful interpretation and separation. In this work, we demonstrate how the particularly strong Čerenkov-type contrast can selectively be blocked using dark- and bright-field SH microscopy. Based on this approach, we show that other contrast mechanisms emerge that were previously overlayed by CSHG but can now be readily selected through the appropriate experimental geometry. Using the methods presented, we show that the strength of the CSHG contrast compared to the other mechanisms is approximately 22 times higher. This work lays the foundation for the in-depth analysis of FE DW topologies by SH microscopy. [ABSTRACT FROM AUTHOR]

Thin-film lithium niobate (TFLN) in the form of x- or z-cut lithium-niobate-on-insulator has attracted considerable interest as a very promising and novel platform for developing integrated optoelectronic (nano)devices and exploring fundamental research. Here, we investigate the coherent interaction length l c of optical second-harmonic generation (SHG) microscopy in such samples, that are purposely prepared into a wedge shape, in order to elegantly tune the geometrical confinement from bulk thicknesses down to approximately 50 nm. SHG microscopy is a very powerful and non-invasive tool for the investigation of structural properties in the biological and solid-state sciences, especially for visualizing and analyzing ferroelectric domains and domain walls. However, unlike in bulk lithium niobate (LN), SHG microscopy in TFLN is impacted by interfacial reflections and resonant enhancement, both of which rely on film thickness and substrate material. In this paper, we show that the dominant SHG contribution measured on TFLN in backreflection is the co-propagating phase-matched SHG signal and not the counter-propagating SHG portion as is the case for bulk LN samples. Moreover, l c depends on the incident pump laser wavelength (sample dispersion) but also on the numerical aperture of the focussing objective in use. These experimental findings on x- and z-cut TFLN are excellently backed up by our advanced numerical simulations. [ABSTRACT FROM AUTHOR]

Quasi-phase-matched grating structures in lithium niobate waveguides with sub-micrometer periodicities will benefit the development of short-wavelength nonlinear optical devices. Here, we report on the reproducible formation of periodically poled domains in x-cut single-crystalline thin-film lithium niobate with periodicities as short as 600 nm. Shaped single-voltage poling pulses were applied to electrode structures that were fabricated by a combination of electron-beam and direct-writing laser lithography. Evidence of successful poling with good quality was obtained through second-harmonic microscopy and piezoresponse force microscopy imaging. For the sub-micrometer period structures, we observed patterns with a double periodicity formed by domain interactions and features with sizes < 200 nm. [ABSTRACT FROM AUTHOR]

High throughput method is described which is applicable to the development of ferroelectric thin films. The chemical solution deposition techniques containing 90 samples are used to prepare thin film libraries for an automated synthesis route.

Surface Acoustic Wave (SAW) resonances were imaged within a closed domain in the ferroelectric LiTaO3 via scanning Microwave Impedance Microscopy (MIM). The MIM probe is used for both SAW generation and measurement, allowing the contact-less measurement within a mesoscopic structure. Measurements taken over a range of microwave frequencies are consistent with a constant acoustic velocity, demonstrating the acoustic nature of the measurement. [ABSTRACT FROM AUTHOR]

Piezoresponse force microscopy (PFM) is a well-established method to study ferroelectric domains on the nanometer length scale. Here, we apply low-temperature PFM and Kelvin probe force microscopy (KPFM) to investigate the domain configuration of (111)-oriented barium titanate in the temperature range from 150K to 290 K. We are able to identify all three ferroelectric phases and domain orientations from the combined PFM, KPFM, and topographic data. Ferroelectric phase transitions manifest in changes of the piezoelectric tensor elements as well as in variations of the spatial domain arrangement. A complete reordering of domains occurs exclusively upon the rhombohedral-to-orthorhombic phase transition during heating. [ABSTRACT FROM AUTHOR]

In order to match the high-density requirement of ferroelectric memories, ferroelectric Bi3.15Nd0.85Ti3O12 nanotubes with outer diameter of about 100 nm and wall thickness of about 30 nm were synthesized using a sol-gel method. Transmission electron microscope images and Raman spectra revealed the Bi-layered perovskite structure of these nanotubes. Their dielectric constant and remnant polarization were comparable with those of thin film form. Piezoelectric hysteresis loops of individual nanotube measured by piezoresponse force microscope indicate their asymmetry, and the switched nanotubes show long term retention. [ABSTRACT FROM AUTHOR]

The idealized system of an atomically flat metallic surface [highly oriented pyrolytic graphite (HOPG)] and an organic monolayer (porphyrin) was used to determine whether the dielectric function and associated properties of thin films can be accessed with scanning–near-field scanning optical microscopy (s-NSOM). Here, we demonstrate the use of harmonics up to fourth order and the polarization dependence of incident light to probe dielectric properties on idealized samples of monolayers of organic molecules on atomically smooth substrates. An analytical treatment of light/sample interaction using the s-NSOM tip was developed in order to quantify the dielectric properties. The theoretical analysis and numerical modeling, as well as experimental data, demonstrate that higher order harmonic scattering can be used to extract the dielectric properties of materials with tens of nanometer spatial resolution. To date, the third harmonic provides the best lateral resolution(∼50 nm) and dielectric constant contrast for a porphyrin film on HOPG. [ABSTRACT FROM AUTHOR]