arXiv subjects

Elke Beyreuther

Publications and source records attributed to Elke Beyreuther.

18 recordsLinked to original sources

arXiv2026

On the temperature dependence of the optical band gap in the material system of lithium niobate and lithium tantalate

Lithium niobate and lithium tantalate see widespread use in optics and electronics, and are increasingly used for cryogenic applications. Despite their broad deployment, their optical band gap and its relation to the crystal stoichiometry are not well characterised as a function of temperature. In this work, we study the optical absorption properties of congruent, stoichiometric, MgO-doped and Er-doped lithium niobate as well as congruent lithium tantalate across the temperature range between 7~K and 1000~K by means of optical transmission spectroscopy. Our results demonstrate that the difference of the optical band gap typically observed at room temperature between different stoichiometries is not primarily attributable to the intrinsic electronic structure, but rather to different electron-phonon couplings and the average phonon energies. Additionally, we exemplarily study the temperature shift of the 523 nm absorption line in Er-doped lithium niobate due to the increased interest in optically active dopants. To facilitate future analyses, we present the open-source software suite PhoQS-Treat (Tauc Regression Edge Analysis Tool), which enables automated Tauc regressions alongside additional analytical capabilities. This work advances the development of high-performance lithium niobate-based devices.

cond-mat.mtrl-sci↗

arXiv2026

The domain-wall/metal-electrode injection barrier in lithium niobate: Which electrical transport model fits best?

The comprehensive description of both the electrical transport along conductive domain walls (CDWs) in lithium niobate (LNO) single crystals and the charge injection at the interfacing metal electrodes, emerged to be a complex challenge. Recently, a heuristic evaluation allowed to postulate the "R2D2" equivalent-circuit model (consisting of two parallel resistor-diode pairs) to appropriately match the DC current-voltage (I-V) characteristics. Here, we carefully revisit the interfacial electrical behavior, i.e., the diode part of the equivalent circuit model, since many more processes beyond the diode-related electron hopping transport (HT) assumed so far, may concurrently occur, such as thermionic emission (TE), Fowler-Nordheim tunneling (FNT), space-charge limited conduction (SCLC), and others more. The "R2D2" model thus needs to be generalized into an "R2X2" circuit model (with X = HT, TE, FNT, and others) to fit to the experimental data. Moreover, to double check for the best I-V curve fitting to the different theories, we apply a higher-harmonic DW current-contribution (HHCC) analysis, i.e., an AC I-V inspection, that allows us to discriminate between all these possible models with much higher precision than from pure DC I-V curve fitting. Both the AC and DC analysis reveal well consistent results, finally finding that the FNT model accounts best for the domain-wall/electrode junctions investigated here.

cond-mat.mtrl-sci↗

arXiv2025

Demonstration of domain wall current in MgO-doped lithium niobate single crystals up to 400 °C

Conductive ferroelectric domain walls (DWs) represent a promising topical system for the development of nanoelectronic components and device sensors to be operational at elevated temperatures. DWs show very different properties as compared to their hosting bulk crystal, in particular with respect to the high local electrical conductivity. The objective of this work is to demonstrate DW conductivity up to temperatures as high as \SI{400}{\degreeCelsius} which extends previous studies significantly. Experimental investigation of the DW conductivity of charged, inclined DWs is performed using \SI{5}{\mole\percent} MgO-doped lithium niobate single crystals. \CR{Current-voltage (\IV) curves are determined by DC electrometer measurements and impedance spectroscopy and found to be identical. Moreover, impedance spectroscopy enables to recognize artifacts such as damaged electrodes. Temperature dependent measurements} over repeated heating cycles reveal two distinct thermal activation energies for a given DW, with the higher of the activation energies only measured at higher temperatures. Depending on the specific sample, the higher activation energy is found above \SI{160}{\degreeCelsius}~to~\SI{230}{\degreeCelsius}. This suggests, in turn, that more than one type of defect/polaron is involved, and that the dominant transport mechanism changes with increasing temperature. First principles atomistic modelling suggests that the conductivity of inclined domain walls cannot be solely explained by the formation of a 2D carrier gas and must be supported by hopping processes. This holds true even at temperatures as high as \SI{400}{\degreeCelsius}. Our investigations underline the potential to extend \DWC based nanoelectronic and sensor applications even into the so-far unexplored temperature range up to \SI{400}{\degreeCelsius}.

physics.app-ph↗

arXiv2025

In-situ SHG microscopy investigation of the domain-wall-conductivity enhancement procedure in lithium niobate

Conductive domain walls (CDWs) in the uniaxial ferroelectric lithium niobate (LiNbO$_3$, LN) have attracted a lot of interest as potential elements in 2D nanoelectronics, due to their orders-of-magnitude larger electronic AC and DC conductivities as compared to the host material. On the way towards generating standardized CDWs into z-cut bulk LN crystals with controllable geometry and electrical properties, we have encountered setbacks recently: Although the first preparation step, i.e., the established UV-light-assisted liquid-electrode poling, reliably creates fully penetrating hexagonal domains with the DWs being aligned almost parallel to the polarization axis, the second step in the DW 'conductivity-enhancement' process through post-growth voltage ramping, resulted in randomly-shaped DWs as reflected in their different current-voltage (I-V) characteristics even after having applied the same process parameters. To clarify this phenomenon, we present here an \textit{in-situ} and time-resolved second-harmonic-generation (SHG) microscopy investigation of DW samples of different sizes, monitoring the DW evolution during that critical voltage ramping, which allowed us to reconstruct the 3D DW shapes both prior to and after the enhancement process. As a result, we are able to map the temporal changes of the local DW inclination angle $α$, and to quantify the DW velocity. As a consequence, we need to re-assess and re-think the origin of the DW conductivity (DWC) in LN: The hitherto assumed simple connection between $α$ and the DWC can not be generalized, since point defects accumulating along DWs act as extra sources for charge carrier trapping/release, significantly contributing to the DW current.

cond-mat.mtrl-sci↗

arXiv2024

Probing Ferroelectric Phase Transitions in Barium Titanate Single Crystals via $\it{in-situ}$ Second Harmonic Generation Microscopy

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.

cond-mat.mtrl-sci↗

arXiv2024

Towards the reproducible fabrication of conductive ferroelectric domain walls into lithium niobate bulk single crystals

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.

cond-mat.mtrl-sci↗

arXiv2024

High-temperature domain wall current in Mg-doped lithium niobate single crystals up to 400°C

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.

cond-mat.mtrl-sci↗

arXiv2024

Comparative study of photo-induced electronic transport along ferroelectric domain walls in lithium niobate single crystals

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 $μ$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.

physics.app-ph↗

arXiv2023

R2D2 -- An equivalent-circuit model that quantitatively describes domain wall conductivity in ferroelectric LiNbO$_3$

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.

cond-mat.mtrl-sci↗

arXiv2023

Hall mobilities and sheet carrier densities in a single LiNbO$_3$ conductive ferroelectric domain wall

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 $μ_{H}$ 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-$μ$m-thick LNO bulk single crystal. We then determine $n_{2D}$ and $μ_{H}$ 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 $n_{2D}$.

cond-mat.mtrl-sci↗

arXiv2022

Large Hall electron mobilities in head-to-head BaTiO$_3$-domain walls

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.

cond-mat.mtrl-sci↗

arXiv2021

Does FLASH deplete Oxygen? Experimental Evaluation for Photons, Protons and Carbon Ions

Purpose: To investigate experimentally, if FLASH irradiation depletes oxygen within water for different radiation types such as photons, protons and carbon ions. Methods: This study presents measurements of the oxygen consumption in sealed, 3D printed water phantoms during irradiation with X-rays, protons and carbon ions at varying dose rates up to 340 Gy/s. The oxygen measurement was performed using an optical sensor allowing for non-invasive measurements. Results: Oxygen consumption in water only depends on dose, dose rate and linear energy transfer (LET) of the irradiation. The total amount of oxygen depleted per 10 Gy was found to be 0.04 - 0.18 % atm for 225 kV photons, 0.04 - 0.25 % atm for 224 MeV protons and 0.09 - 0.17 % atm for carbon ions. consumption depends on dose rate by an inverse power law and saturates for higher dose rates because of self-interactions of radicals. Higher dose rates yield lower oxygen consumption. No total depletion of oxygen was found for clinical doses. Conclusions: FLASH irradiation does consume oxygen, but not enough to deplete all the oxygen present. For higher dose rates, less oxygen was consumed than at standard radiotherapy dose rates. No total depletion was found for any of the analyzed radiation types for 10 Gy dose delivery using FLASH.

physics.med-ph↗

arXiv2020

Optical-Field Driven Charge-Transfer Modulations near Composite Nanostructures

Optical activation of material properties illustrates the potentials held by tuning light-matter interactions with impacts ranging from basic science to technological applications. Here, we demonstrate for the first time that composite nanostructures providing nonlocal environments can be engineered to optically trigger photoinduced charge transfer dynamic (CTD) modulations in the solid state. The nanostructures herein explored lead to unprecedented out-of-phase behaviour between charge separation and recombination dynamics, along with linear CTD variations with the optical-field amplitude. Using transient absorption spectroscopy, up to 270 % increase in charge separation rate is obtained in organic semiconductor thin films. We provide evidences that composite nanostructures allow for surface photovoltages to be created, which kinetics vary with the composite architecture and last beyond optical pulse temporal characteristics. Furthermore, by generalizing Marcus theory framework, we explain why CTD modulations can only be unveiled when optic field effects are enhanced by nonlocal image dipole interactions. Demonstrating that composite nanostructures can be designed to use optical fields as CTD remote actuators opens the path for their use in practical and original applications ranging from photochemistry to optoelectronics.

cond-mat.mtrl-sci↗

arXiv2020

Spectral and spatial shaping of laser-driven proton beams using a pulsed high-field magnet beamline

Intense laser-driven proton pulses, inherently broadband and highly divergent, pose a challenge to established beamline concepts on the path to application-adapted irradiation field formation, particularly for 3D. Here we experimentally show the successful implementation of a highly efficient (50% transmission) and tuneable dual pulsed solenoid setup to generate a homogeneous (8.5% uniformity laterally and in depth) volumetric dose distribution (cylindrical volume of 5 mm diameter and depth) at a single pulse dose of 0.7 Gy via multi-energy slice selection from the broad input spectrum. The experiments have been conducted at the Petawatt beam of the Dresden Laser Acceleration Source Draco and were aided by a predictive simulation model verified by proton transport studies. With the characterised beamline we investigated manipulation and matching of lateral and depth dose profiles to various desired applications and targets. Using a specifically adapted dose profile, we successfully performed first proof-of-concept laser-driven proton irradiation studies of volumetric in-vivo normal tissue (zebrafish embryos) and in-vitro tumour tissue (SAS spheroids) samples.

physics.acc-ph↗

arXiv2014

Electrical-transport characteristics of as-grown and oxygen-reduced La$_{0.7}$Ce$_{0.3}$MnO$_3$ films: calculation of hopping energies, Mn valences, and carrier localization lengths

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.

cond-mat.mtrl-sci↗

arXiv2014

Conductivity and magnetoresistance of La$_{0.7}$Ce$_{0.3}$MnO$_3$ thin films under photoexcitation

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$_3$.

cond-mat.mtrl-sci↗

arXiv2013

Mn$^{2+}$/Mn$^{3+}$ state of La$_{0.7}$Ce$_{0.3}$MnO$_3$ by oxygen reduction and photodoping

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.

cond-mat.mtrl-sci↗

arXiv2013

Conducting and insulating LaAlO$_3$/SrTiO$_3$ interfaces: A comparative surface photovoltage investigation

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.

cond-mat.mtrl-sci↗