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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 $\it{in-situ}$ investigate the cubic-to-tetragonal (at $\sim$126$^\circ$C) and the tetragonal-to-orthorhombic (at $\sim$5$^\circ$C) phase transition in single-crystalline BTO via 3-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 the 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 (1st/2nd 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 $\it{in-situ}$ engineering of advanced ferroic devices., Comment: 8 pages, 3 figures, with appended supplementary material (2 pages, 2 figures)

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 emphasis on quantifying the origins for DWC. Very few reports exist when it comes to compare 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 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 (FE) lithium niobate (LN) single crystals of 200 and 300 micrometers thickness, respectively. We show that the domain diameter can be controlled with an error of a few percent. As-grown DWs are then subjected to a standard procedure of current-controlled high-voltage DWC enhancement, repetitively reaching a DWC increase of 6 orders of magnitude. While all resulting DWs show significantly enhanced DWC values, subtle features in their individual current-voltage (I-V) characteristics hint towards different 3D shapes into the bulk, with variations probably reflecting local heterogeneities by defects, DW pinning, and surface-near DW inclination, which seem to have a larger impact than expected., Comment: 12 pages, 7 figures, with appended supplement (9 pages, 7 figures)

Conductive ferroelectric domain walls (DWs) represent a promising topical system for the development of nanoelectronic components and devices. DWs show very different properties as compared to their bulk counterparts. Of central interest here is the domain wall current (DWC) of charged DWs in 5mol\% Mg-doped lithium niobate single crystals; in contrast to former works, we extend the DWC study here to temperatures as high as 400$^\circ$C. Both the temporal stability and the thermal activation energies of 90 - 160 meV are readily deduced from current-voltage sweeps as recorded over multiple heating cycles. Our experimental work is backed up by atomistic modelling of the DWC. The latter suggests that a large band bending renders head-to-head and tail-to-tail DWs semimetallic. These detailed investigations underline the potential to extend DWC-based nanoelectronic applications even into the so-far unexplored high-temperature regime., Comment: 5 pages, 4 figures; with included supplementary material (6 pages, 9 figures)

Lithium niobate (LNO) and lithium tantalate (LTO) see widespread use in fundamental research and commercial technologies reaching from electronics over classical optics to integrated quantum communication. In recent years, the mixed crystal system lithium niobate tantalate (LNT) allows for the dedicate engineering of material properties by combining the advantages of the two parental materials LNO and LTO. Vibrational spectroscopies such as Raman spectroscopy or (Fourier transform) infrared spectroscopy are vital techniques to provide detailed insight into the material properties, which is central to the analysis and optimization of devices. In this work, we present a joint experimental-theoretical approach allowing to unambiguously assign the spectral features in the LNT material family through both Raman and IR spectroscopy, as well as to provide an in-depth explanation for the observed scattering efficiencies based on first-principles calculations. The phononic contribution to the static dielectric tensor is calculated from the experimental and theoretical data using the generalized Lyddane-Sachs-Teller relation and compared with the results of the first-principles calculations. The joint methodology can be readily expanded to other materials and serves, e.g., as the basis for studying the role of point defects or doping.

We report THz-pump / mid-infrared probe near-field studies on Si-doped GaAs-InGaAs core-shell nanowires utilizing THz radiation from the free-electron laser FELBE. Upon THz excitation of free carriers, we observe a red shift of the plasma resonance in both amplitude and phase spectra, which we attribute to the heating up of electrons in the conduction band. The simulation of heated electron distributions anticipates a significant electron population in both L- and X-valleys. The two-temperature model is utilized for a quantitative analysis of the dynamics of the electron gas temperature under THz pumping at various power levels., Comment: Manuscript + Supplementary Information

Lithium niobate and lithium tantalate are among the most widespread materials for nonlinear, integrated photonics. Mixed crystals with arbitrary Nb-Ta ratios provide a new degree of freedom to tune materials properties, such as the birefringence, but also leverage the advantages of the singular compounds, for example, by combining the thermal stability of lithium tantalate with the larger nonlinear or piezoelectric constants of lithium niobate. Periodic poling is the prerequisite for any nonlinear optical application. For mixed crystals this has been challenging so far due to the lack of homogeneous, mono-domain crystals, which severely inhibit domain growth and nucleation. In this work we demonstrate that surface-near ($< 1$~$\mu$m depth) periodic poling on x-cut lithium niobate tantalate mixed crystals can be achieved via electric field poling and lithographically structured electrodes. We find that naturally occurring head-to-head or tail-to-tail domain walls in the as-grown crystal inhibit domain inversion at a larger scale. However, periodic poling is possible, if the gap size between the poling electrodes is of the same order of magnitude or smaller than the average size of naturally occurring domains. This work provides the basis for the nonlinear optical application of lithium niobate tantalate mixed crystals.

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 is most often applied to spatially map the 3-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-$\mu$m-penetration depth into the sample.

Ferroelectric domain wall conductivity (DWC) is an intriguing functional property, that can be controlled through external stimuli such as electric and mechanical fields. Optical-field control, as a non-invasive flexible handle, has rarely been applied so far, but significantly expands the possibility for both tuning and probing DWC. On the one hand, as known from Second-Harmonic, Raman, and CARS micro-spectroscopy, the optical in-and-out approach delivers parameters on the DW distribution, the DW inclination, and probes the DW vibrational modes; on the other hand, photons might be applied also to directly generate charge carriers within the DW, hence acting as a functional and spectrally tunable probe to deduce the integral or local absorption properties and bandgaps of conductive DWs. Here, we report on such an optoelectronic approach by investigating the photo-induced DWC (PI-DWC) in DWs of the model system lithium niobate, a material that is well known for hosting conductive DWs. We compare three different crystals containing different numbers of domain walls: (A) none, (B) one, and (C) many conductive DWs. All samples are inspected for their current-voltage (I-V) behavior (i) in darkness, and (ii) for different illumination wavelengths swept from 500 nm down to 310 nm. All samples show their maximum PI-DWC at 310 nm, i.e., at the optical bandgap of lithium niobate; moreover, sample (C) reaches PI-DWCs of several $\mu$A. Interestingly, a noticeable PI-DWC is also observed for sub-bandgap illumination, i.e., wavelengths as high as 500 nm, hinting towards the existence and decisive role of electronic in-gap states that contribute to the electronic transport along DWs. Finally, conductive atomic force microscopy (c-AFM) investigations under illumination proved that the PI-DWC is confined to the DW area, and does not originate from photo-induced bulk conductivity., Comment: 18 pages, 3 figures, and Supplementary Material (with 10 pages, 4 figures)

Magnetic force microscopy (MFM) is long established as a powerful tool for probing the local manifestation 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 samples 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 new method of detecting in-plane magnetic stray field components, by utilizing a home made 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 (V-MFM) images and a lateral MFM (L-MFM) where the tip-cantilever system is only sensitive to stray fields acting perpendicular to the torsional axis of the cantilever.

Electric field enhancement mediated through sharp tips in scattering-type scanning near-field optical microscopy (s-SNOM) enables optical material analysis down to the 10-nm length scale, and even below. Nevertheless, mostly the out-of-plane electric field component is considered here due to the lightning rod effect of the elongated s-SNOM tip being orders of magnitude stronger as compared to any in-plane field component. Nonetheless, the fundamental understanding of resonantly excited near-field coupled systems clearly allows us to take profit from all vectorial components, especially also from the in-plane ones. In this paper, we theoretically and experimentally explore how linear polarization control of both near-field illumination and detection, can constructively be implemented to (non-)resonantly couple to selected sample permittivity tensor components, e.g. explicitly also to the in-plane directions. When applying the point-dipole model, we show that resonantly excited samples respond with a strong near-field signal, to all linear polarization angles. We then experimentally investigate the polarization-dependent responses for both non-resonant (Au) and phonon-resonant (3C-SiC) sample excitations at a 10.6~$\mu$m and 10.7~$\mu$m incident wavelength using a tabletop CO$_2$ laser. Varying the illumination polarization angle thus allows for quantitatively comparing the scattered near-field signatures for the two wavelengths. Finally, we compare our experimental data to simulation results, and thus gain the fundamental understanding of the polarization's influence on the near-field interaction. As a result, the near-field components parallel and perpendicular to the sample surface can be easily disentangled and quantified through their polarization signatures, connecting them directly to the sample's local permittivity., Comment: 11 pages, 5 figures

The terahertz (THz) frequency range is key to study collective excitations in many crystals and organic molecules. However, due to the large wavelength of THz radiation, the local probing of these excitations in smaller crystalline structures or few-molecular arrangements, requires sophisticated methods to confine THz light down to the nanometer length scale, as well as to manipulate such a confined radiation. For this purpose, in recent years, taking advantage of hyperbolic phonon polaritons (HPhP) in highly anisotropic van der Waals (vdW) materials has emerged as a promising approach, offering a multitude of manipulation options such as control over the wavefront shape and propagation direction. Here, we demonstrate the first THz application of twist-angle-induced HPhP manipulation, designing the propagation of confined THz radiation between 8.39 and 8.98 THz in the vdW material alpha-molybdenum trioxide ($\alpha-MoO_{3}$), hence extending twistoptics to this intriguing frequency range. Our images, recorded by near-field optical microscopy, show the frequency- and twist-angle-dependent change between hyperbolic and elliptic polariton propagation, revealing a polaritonic transition at THz frequencies. As a result, we are able to allocate canalization (highly collimated propagation) of confined THz radiation by carefully adjusting these two parameters, i.e. frequency and twist angle. Specifically, we report polariton canalization in $\alpha-MoO_{3}$ at 8.67 THz for a twist angle of 50{\deg}. Our results demonstrate an unprecedented control and the manipulation of highly-confined collective excitations at THz frequencies, offering novel possibilities for nanophotonic applications., Comment: 25 pages, 4 figures, article, submitted

For the last decade, conductive domain walls (CDWs) in single crystals of the uniaxial model ferroelectric lithium niobate (LiNbO$_3$, LNO) have shown to reach resistances more than 10 orders of magnitude lower as compared to the surrounding bulk, with charge carriers being firmly confined to sheets of a few nanometers in width. LNO thus currently witnesses an increased attention since bearing the potential for variably designing room-temperature nanoelectronic circuits and devices based on such CDWs. In this context, the reliable determination of the fundamental transport parameters of LNO CDWs, in particular the 2D charge carrier density $n_{2D}$ and the Hall mobility $\mu_{H}$ of the majority carriers, are of highest interest. In this contribution, we present and apply a robust and easy-to-prepare Hall-effect measurement setup by adapting the standard 4-probe van-der-Pauw method to contact a single, hexagonally-shaped domain wall that fully penetrates the 200-$\mu$m-thick LNO bulk single crystal. We then determine $n_{2D}$ and $\mu_{H}$ for a set of external magnetic fields $B$ and prove the expected cosine-like angular dependence of the Hall voltage. Lastly, we present photo-Hall measurements of one and the same DW, by determining the impact of super-bandgap illumination on the 2D charge carrier density $n_{2D}$.

Ferroelectric domain wall (DW) conductivity (DWC) can be attributed to two separate mechanisms: (a) the injection/ejection of charge carriers across the Schottky barrier formed at the (metal-) electrode-DW junction and (b) the transport of those charge carriers along the DW. Current-voltage (IU) characteristics, recorded at variable temperatures from LiNbO$_3$ (LNO) DWs, are clearly able to differentiate between these two contributions. Practically, they allow us here to directly quantify the physical parameters relevant for the two mechanisms (a) and (b) mentioned above. These are, e.g., the resistance of the DW, the saturation current, the ideality factor, and the Schottky barrier height of the electrode/DW junction. Furthermore, the activation energies needed to initiate the thermally-activated electronic transport along the DWs, can be extracted. In addition, we show that electronic transport along LiNbO$_3$ DWs can be elegantly viewed and interpreted in an adapted semiconductor picture based on a double-diode/double-resistor equivalent circuit model, the R2D2 model. Finally, our R2D2 model was checked for its universality by fitting the DWC data not only to z-cut LNO bulk DWs, but equally to z-cut thin-film LNO DWs, and DWC from x-cut DWs as reported in literature., Comment: 10 pages, 7 figures; with included supporting information (6 pages, 4 figures)

Broadband coherent anti-Stokes Raman scattering (BCARS) is an advanced Raman spectroscopy method that combines the spectral sensitivity of spontaneous Raman scattering (SR) with the increased signal intensity of single-frequency coherent Raman techniques. These two features make BCARS particularly suitable for ultra-fast imaging of heterogeneous samples, as already shown in biomedicine. Recent studies demonstrated that BCARS also shows exceptional spectroscopic capabilities when inspecting crystalline materials like lithium niobate and lithium tantalate, and can be used for fast imaging of ferroelectric domain walls. These results strongly suggest the extension of BCARS towards new imaging applications like mapping defects, strain, or dopant levels, similar to standard SR imaging. Despite these advantages, BCARS suffers from a spurious and chemically unspecific non-resonant background (NRB) that distorts and shifts the Raman peaks. Post-processing numerical algorithms are then used to remove the NRB and to obtain spectra comparable to SR results. Here, we show the reproducibility of BCARS by conducting an internal Round Robin with two different BCARS experimental setups, comparing the results on different crystalline materials of increasing structural complexity: diamond, 6H-SiC, KDP, and KTP. First, we compare the detected and phase-retrieved signals, the setup-specific NRB-removal steps, and the mode assignment. Subsequently, we demonstrate the versatility of BCARS by showcasing how the selection of pump wavelength, pulse width, and detection geometry can be tailored to suit the specific objectives of the experiment. Finally, we compare and optimize measurement parameters for the high-speed, hyperspectral imaging of ferroelectric domain walls in lithium niobate., Comment: 12 pages, 8 figures

Coherent nonlinear optical micro-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, that 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-harmonic 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.

Structural strain severely impacts material properties such as the linear and non-linear optical response. Moreover, strain plays a key role, e.g., in the physics of ferroelectrics and in particular of their domain walls. $\mu$-Raman spectroscopy is a well-suited technique for the investigation of such strain effects, as it allows to measure the lattice dynamics locally. However, quantifying and reconstructing strain fields from Raman maps requires knowledge on the strain dependence of phonon frequencies. In this work, we have analyzed both theoretically and experimentally the phonon frequencies in the widely used ferroelectrics lithium niobate and lithium tantalate as a function of uniaxial strain via density functional theory and $\mu$-Raman spectroscopy. Overall, we find a good agreement between our $ab$ $initio$ models and the experimental data performed with a stress cell. The majority of phonons show an increase in frequency under compressive strain, while the opposite is observed for tensile strains. Moreover, for E-type phonons, we observe the lifting of degeneracy already at moderate strain fields (i.e. at $\pm0.2~\%$) along the x and y directions. This work hence allows for the systematic analysis of 3D strains in modern-type bulk and thin-film devices assembled from lithium niobate and tantalate., Comment: 12 pages, 7 figures, Supplementary Information, submitted to Physical Review Materials

Ferroelectric domain boundaries are quasi-two-dimensional functional interfaces with high prospects for nanoelectronic applications. Despite their reduced dimensionality, they can exhibit complex non-Ising polarization configurations and unexpected physical properties. Here, the impact of the three-dimensional (3D) curvature on the polarization profile of nominally uncharged 180{\deg} domain walls in LiNbO3 is studied using second-harmonic generation microscopy and 3D polarimetry analysis. Correlations between the domain wall curvature and the variation of its internal polarization unfold in the form of modulations of the N\'eel-like character, which we attribute to the flexoelectric effect. While the N\'eel-like character originates mainly from the tilting of the domain wall, the internal polarization adjusts its orientation due to the synergetic upshot of dipolar and monopolar bound charges and their variation with the 3D curvature. Our results show that curved interfaces in solid crystals may offer a rich playground for tailoring nanoscale polar states., Comment: 35 pages, 4 figures and Supporting Information

Conductive domain walls (CDWs) in insulating ferroelectrics have recently attracted considerable attention due to their unique topological, optical, and electronic properties, and offer potential applications such as in memory devices or re-writable circuitry. The electronic properties of domain walls (DWs) can be tuned by the application of strain, hence controlling the charge carrier density at DWs. In this work, we study the influence of uniaxial stress on the conductivity of DWs in the bulk single crystal lithium niobate (LiNbO$_3$). Using conductive atomic force microscopy (cAFM), we observe a large asymmetry in the conductivity of DWs, where only negatively screened walls, so called head-to-head DWs, are becoming increasingly conductive, while positively screened, tail-to-tails DWs, show a decrease in conductivity. This asymmetry of DW conductivity agrees with our theoretical model based on the piezoelectric effect. In addition, we observed that the current in the DW increases up to an order of magnitude for smaller compressive stresses of 100 MPa. This response of DWs remained intact for multiple stress cycles over 2 months, opening a path for future applications.

Strongly charged head-to-head (H2H) domain walls (DWs) that are purposely engineered along the [110] crystallographic orientation into ferroelectric BaTiO$_3$ single crystals have been proposed as novel 2-dimensional electron gases (2DEGs) due to their significant domain wall conductivity (DWC). Here, we quantify these 2DEG properties through dedicated Hall-transport measurements in van-der-Pauw 4-point geometry at room temperature, finding the electron mobility to reach around 400~cm$^2$(Vs)$^{-1}$, while the 2-dimensional charge density amounts to ~7$\times$10$^3$cm$^{-2}$. We underline the necessity to take account of thermal and geometrical-misalignment offset voltages by evaluating the Hall resistance under magnetic-field sweeps, since otherwise dramatic errors of several hundred percent in the derived mobility and charge density values can occur. Apart from the specific characterization of the conducting BaTiO$_3$ DW, we propose the method as an easy and fast way to quantitatively characterize ferroic conducting DWs, complementary to previously proposed scanning-probe-based Hall-potential analyses., Comment: 8 pages, 4 figures; with included supporting information (4 pages, 5 figures)

Skyrmionic materials hold the potential for future information technologies, such as racetrack memories. Key to that advancement are systems that exhibit high tunability and scalability, with stored information being easy to read and write by means of all-electrical techniques. Topological magnetic excitations such as skyrmions and antiskyrmions, give rise to a characteristic topological Hall effect. However, the electrical detection of antiskyrmions, in both thin films and bulk samples has been challenging to date. Here, we apply magneto-optical microscopy combined with electrical transport to explore the antiskyrmion phase as it emerges in crystalline mesoscale structures of the Heusler magnet Mn$_{1.4}$PtSn. We reveal the Hall signature of antiskyrmions in line with our theoretical model, comprising anomalous and topological components. We examine its dependence on the vertical device thickness, field orientation, and temperature. Our atomistic simulations and experimental anisotropy studies demonstrate the link between antiskyrmions and a complex magnetism that consists of competing ferromagnetic, antiferromagnetic, and chiral exchange interactions, not captured by micromagnetic simulations., Comment: 30 pages, 4 figures, Supplementary Information with additional 22 pages and 16 figures

Terahertz (THz) electromagnetic radiation is key to optically access collective excitations such as magnons (spins), plasmons (electrons), or phonons (atomic vibrations), thus bridging between optics and solid-state physics. Confinement of THz light to the nanometer length scale is desirable for local probing of such excitations in low dimensional systems, thereby inherently circumventing the large footprint and low spectral density of far-field THz optics. For that purpose, phonon polaritons (PhPs, i.e., light coupled to lattice vibrations in polar crystals) in anisotropic van der Waals (vdW) materials have recently emerged as a promising platform for THz nanooptics; yet the amount of explored, viable materials is still exiguous. Hence, there is a demand for the exploration of novel materials that feature not only THz PhPs at different spectral regimes, but also exhibit unique anisotropic (directional) electrical, thermoelectric, and vibronic properties. To that end, we introduce here the semiconducting alpha-germanium(II) sulfide (GeS) as an intriguing candidate. By employing THz nano-spectroscopy supported by theoretical analysis, we provide a thorough characterization of the different in-plane hyperbolic and elliptical PhP modes in GeS. We find not only PhPs with long life times ($\tau$ > 2 ps) and excellent THz light confinement ($\lambda_0/\lambda$ > 45), but also an intrinsic, phonon-induced anomalous dispersion as well as signatures of naturally occurring PhP canalization within one single GeS slab.

Thin-film lithium niobate (TFLN) in the form of x- or z-cut lithium-niobate-on-insulator (LNOI) has recently popped up 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 (SH) 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 $\approx$ 50 nm. SH microscopy is a very powerful and non-invasive tool for the investigation of structural properties in the biological and solid-state sciences, especially also for visualizing and analyzing ferroelectric domains and domain walls. However, unlike bulk LN, SH microscopy in TFLN is largely affected by interfacial reflections and resonant enhancement that both rely on film thickness and substrate material. In this paper we show that the dominant SHG contribution measured in back-reflection, is the co-propagating phase-matched SH signal and \textit{not} the counter-propagating SH portion as is the case for bulk LN samples. Moreover, $l_{c}$ dramatically depends also on the incident pump laser wavelength (sample dispersion) but even more 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.

Cu$_2$OSeO$_3$ is an insulating skyrmion-host material with a magnetoelectric coupling giving rise to an electric polarization with a characteristic dependence on the magnetic field $\vec H$. We report magnetic force microscopy imaging of the helical real-space spin structure on the surface of a bulk single crystal of Cu$_2$OSeO$_3$. In the presence of a magnetic field, the helimagnetic order in general reorients and acquires a homogeneous component of the magnetization, resulting in a conical arrangement at larger fields. We investigate this reorientation process at a temperature of 10~K for fields close to the crystallographic $\langle 110\rangle$ direction that involves a phase transition at $H_{c1}$. Experimental evidence is presented for the formation of magnetic domains in real space as well as for the microscopic origin of relaxation events that accompany the reorientation process. In addition, the electric polarization is measured by means of Kelvin-probe force microscopy. We show that the characteristic field dependency of the electric polarization originates in this helimagnetic reorientation process. Our experimental results are well described by an effective Landau theory previously invoked for MnSi, that captures the competition between magnetocrystalline anisotropies and Zeeman energy.

In the cubic chiral magnet Fe$_{1-x}$Co$_{x}$Si a metastable state comprising of topologically nontrivial spin whirls, so-called skyrmions, may be preserved down to low temperatures by means of field cooling the sample. This metastable skyrmion state is energetically separated from the topologically trivial ground state by a considerable potential barrier, a phenomenon also referred to as topological protection. Using magnetic force microscopy on the surface of a bulk crystal, we show that certain positions are preferentially and reproducibly decorated with metastable skyrmions, indicating that surface pinning plays a crucial role. Increasing the magnetic field allows an increasing number of skyrmions to overcome the potential barrier, and hence to transform into the ground state. Most notably, we find that the unwinding of individual skyrmions may be triggered by the magnetic tip itself, however, only when its magnetization is aligned parallel to the external field. This implies that the stray field of the tip is key for locally overcoming the topological protection. Both the control of the position of topologically nontrivial states as well as their creation and annihilation on demand pose important challenges in the context of potential skyrmionic applications.

Local-probe imaging of the ferroelectric domain structure and auxiliary bulk pyroelectric measurements were conducted at low temperatures with the aim to clarify the essential aspects of the orbitally driven phase transition in GaMo4S8, a lacunar spinel crystal that can be viewed as a spin-hole analogue of its GaV4S8 counterpart. We employed multiple scanning probe techniques combined with symmetry and mechanical compatibility analysis to uncover the hierarchical domain structures, developing on the 10-100 nm scale. The identified domain architecture involves a plethora of ferroelectric domain boundaries and junctions, including primary and secondary domain walls in both electrically neutral and charged configurations, and topological line defects transforming neutral secondary walls into two oppositely charged ones., Comment: This is the Accepted Manuscript version of an article accepted for publication in Journal of Physics: Condensed Matter. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at https://doi.org/10.1088/1361-648X/aae448

Electromagnetic field confinement is crucial for nanophotonic technologies, since it allows for enhancing light-matter interactions, thus enabling light manipulation in deep sub-wavelength scales. In the terahertz (THz) spectral range, radiation confinement is conventionally achieved with specially designed metallic structures - such as antennas or nanoslits - with large footprints due to the rather long wavelengths of THz radiation. In this context, phonon polaritons - light coupled to lattice vibrations - in van der Waals (vdW) crystals have emerged as a promising solution for controlling light beyond the diffraction limit, as they feature extreme field confinements and low optical losses. However, experimental demonstration of nanoscale-confined phonon polaritons at THz frequencies has so far remained elusive. Here, we provide it by employing scattering-type scanning near-field optical microscopy (s-SNOM) combined with a free-electron laser (FEL) to reveal a range of low-loss polaritonic excitations at frequencies from 8 to 12 THz in the vdW semiconductor ${\alpha}-MoO_3$. We visualize THz polaritons with i) in-plane hyperbolic dispersion, ii) extreme nanoscale field confinement (below ${\lambda}_o/75$) and iii) long polariton lifetimes, with a lower limit of > 2 ps.

We investigated the structural and magnetic properties of bare SrRuO$_3$ (SRO) ultra-thin films and SrRuO$_3$/SrIrO$_3$/SrZrO$_3$ (SRO/SIO/SZO: RIZ) trilayer heterostructures between 10 K and 80 K, by comparing macroscopic data using magneto-optical Kerr effect (MOKE) and magneto-transport (anomalous Hall effect: AHE), with nanoscale fingerprints when applying non-contact scanning force microscopy (nc-SFM) and magnetic force microscopy (MFM). SRO and RIZ ultra-thin films were epitaxially grown at 650C onto vicinal SrTiO$_3$ (100) single-crystalline substrates to a nominal thickness of 4 and 4/2/2 unit cells (uc), respectively. Our correlated analysis allows associating topographic sample features of overgrown individual layers to their residual magnetization, as is shown here to be relevant for interpreting the macroscopic AHE data. Although the hump-like features in the AHE suggest a magnetically extured skyrmion phase to exist around 55 K associated to the topological Hall effect (THE), both our MOKE and MFM data cannot support this theory. In contrast, our SFM/MFM local-scale analysis finds the local coercive field to be strongly dependent on the effective layer thickness and stoichiometry in both the SRO and RIZ samples, with huge impact on the local band-structure. In fact, it is these variations that in turn mimic a potential THE through anomalies in the AHE resistivity loops., Comment: 16 pages

Surface Acoustic Wave (SAW) resonances were imaged within a closed domain in the ferroelectric LiTaO$_3$ via scanning Microwave Impedance Microscopy (MIM). The MIM probe is used for both SAW generation and measurement, allowing 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., Comment: 5 pages, 3 figures

GaV$_4$S$_8$ is a multiferroic semiconductor hosting N{\'e}el-type magnetic skyrmions dressed with electric polarization. At T$_s$ = 42K, the compound undergoes a structural phase transition of weakly first-order, from a non-centrosymmetric cubic phase at high temperatures to a polar rhombohedral structure at low temperatures. Below T$_s$, ferroelectric domains are formed with the electric polarization pointing along any of the four $\left< 111 \right>$ axes. Although in this material the size and the shape of the ferroelectric-ferroelastic domains may act as important limiting factors in the formation of the N{\'e}el-type skyrmion lattice emerging below T$_C$=13\:K, the characteristics of polar domains in GaV$_4$S$_8$ have not been studied yet. Here, we report on the inspection of the local-scale ferroelectric domain distribution in rhombohedral GaV$_4$S$_8$ using low-temperature piezoresponse force microscopy. We observed mechanically and electrically compatible lamellar domain patterns, where the lamellae are aligned parallel to the (100)-type planes with a typical spacing between 100 nm-1.2 $\mu$m. We expect that the control of ferroelectric domain size in polar skyrmion hosts can be exploited for the spatial confinement and manupulation of N{\'e}el-type skyrmions.

Recently, the fundamental and nanoscale understanding of complex phenomena in materials research and the life sciences, witnessed considerable progress. However, elucidating the underlying mechanisms, governed by entangled degrees of freedom such as lattice, spin, orbit, and charge for solids or conformation, electric potentials, and ligands for proteins, has remained challenging. Techniques that allow for distinguishing between different contributions to these processes are hence urgently required. In this paper we demonstrate the application of scattering-type scanning near-field optical microscopy (s-SNOM) as a novel type of nano-probe for tracking transient states of matter. We introduce a sideband-demodulation technique that allows for probing exclusively the stimuli-induced change of near-field optical properties. We exemplify this development by inspecting the decay of an electron-hole plasma generated in SiGe thin films through near-infrared laser pulses. Our approach can universally be applied to optically track ultrafast/-slow processes over the whole spectral range from UV to THz frequencies.

La$_{0.7}$Ce$_{0.3}$MnO$_3$ thin films of different thicknesses, degrees of CeO$_2$-phase segregation and oxygen deficiency, grown on SrTiO$_3$ single crystal substrates, were comparatively investigated with respect to both their spectral and temperature-dependent photoconductivity (PC) and their magnetoresistance (MR) behaviour under photoexcitation. While as-grown films were insensitive to optical excitation, oxygen reduction appeared to be an effective way to decrease the film resistance, but the film thickness was found to play a minor role. However, from the evaluation of the spectral behaviour of the PC and the comparison of the MR of the LCeMO/substrate-samples with a bare substrate under illumination we find that the photoconductivity data reflects not only contributions from (i) photogenerated charge carriers in the film and (ii) carriers injected from the photoconductive substrate (as concluded from earlier works), but also (iii) a decisive parallel photoconduction in the SrTiO$_3$ substrate. Furthermore -- also by analyzing the MR characteristics -- the unexpected occurence of a strong electroresistive effect in the sample with the highest degree of CeO$_2$ segregation and oxygen deficiency could be attributed to the electroresistance of the SrTiO$_3$ substrate as well. The results suggest a critical reconsideration and possibly a reinterpretation of several previous photoconductivity and electroresistance investigations of manganite thin films on SrTiO$_3$., Comment: 11 pages, 11 figures

Presently, cerium-doped LaMnO$_3$ is vividly discussed as an electron-doped counterpart prototype to the well-established hole-doped mixed-valence manganites. Here, La$_{0.7}$Ce$_{0.3}$MnO$_3$ thin films of different thicknesses, degrees of CeO$_2$ phase segregation, and oxygen deficiency, grown on SrTiO$_3$ single crystal substrates, are compared with respect to their resistance-vs.-temperature (R vs. T) behavior from 300~K down to 90~K. While the variation of the film thickness (and thus the degree of epitaxial strain) in the range between 10~nm and 100~nm has only a weak impact on the electrical transport, the degree of oxygen deficiency as well as the existence of CeO$_2$ clusters can completely change the type of hopping mechanism. This is shown by fitting the respective \textit{R-T} curves with three different transport models (adiabatic polaron hopping, Mott variable-range hopping, Efros-Shklovskii variable-range hopping), which are commonly used for the mixed-valence manganites. Several characteristic transport parameters, such as the hopping energies, the carrier localization lengths, as well as the Mn valences are derived from the fitting procedures., Comment: 9 pages, 3 figures

Surface photovoltage (SPV) spectroscopy, which is a versatile method to analyze the energetic distribution of electronic defect states at surfaces and interfaces of wide-bandgap semiconductor (hetero-)structures, is applied to comparatively investigate heterostructures made of 5-unit-cell-thick LaAlO$_3$ films grown either on TiO$_2$- or on SrO-terminated SrTiO$_3$. As shown in a number of experimental and theoretical investigations in the past, these two interfaces exhibit dramatically different properties with the first being conducting and the second insulating. Our present SPV investigation reveals clearly distinguishable interface defect state distributions for both configurations when interpreted within the framework of a classical semiconductor band scheme. Furthermore, bare SrTiO$_3$ crystals with TiO$_2$ or mixed SrO/TiO$_2$ terminations show similar SPV spectra and transients as do LaAlO$_3$-covered samples with the respective termination of the SrTiO$_3$ substrate. This is in accordance with a number of recent works that stress the decisive role of SrTiO$_3$ and the minor role of LaAlO$_3$ with respect to the electronic interface properties., Comment: 8 pages, 6 figures; supplement not uploaded to arXiv, see ref. [44] for a possible download link; submitted to J. Appl. Phys

Films of cerium-doped LaMnO$_3$, which has been intensively discussed as an electron-doped counterpart to hole-doped mixed-valence lanthanum manganites during the past decade, were analyzed by x-ray photoemission spectroscopy with respect to their manganese valence under photoexcitation. The comparative analysis of the Mn 3s exchange splitting of La$_{0.7}$Ce$_{0.3}$MnO$_3$ (LCeMO) films in the dark and under illumination clearly shows that both oxygen reduction and illumination are able to decrease the Mn valence towards a mixed 2$+$/3$+$ state, independently of the film thickness and the degree of CeO$_2$ segregation. Charge injection from the photoconductive SrTiO$_3$ substrate into the Mn e$_g$ band with carrier lifetimes in the range of tens of seconds and intrinsic generation of electron-hole pairs within the films are discussed as two possible sources of the Mn valence shift and the subsequent electron doping., Comment: 6 pages, 2 figures