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Lukas M. Eng

Publications and source records attributed to Lukas M. Eng.

At least 19 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

Uniaxial strain-driven ferroelastic domain control in LaAlO3

Multiferroic domain walls in functional oxides exhibit properties distinct from the bulk and are increasingly exploited as active elements in nanoelectronic and photonic devices. Deterministic control of domain populations has typically remained limited to local control, or removal with temperature. Here we demonstrate continuous, reversible manipulation of the ferroelastic domain structure in single-crystal LaAlO$_3$ using in-situ uniaxial strain. Combining atomic force microscopy, X-ray diffraction, and Raman spectroscopy with first-principles calculations we map the complete microscopic evolution of the twin domain population through the strain-driven transition from the rhombohedral $R\bar{3}c$ ground state toward the predicted orthorhombic $Fmmm$ phase. Applied strains below $0.5\%$ produce pronounced surface flattening and large-scale domain reorganisation, establishing uniaxial strain as a technically accessible control parameter for ferroelastic domain engineering. These results open a route to active, real-time programming of domain architectures in LaAlO$_3$-based heterostructures, with implications for strain-tunable superconducting interfaces, nanoscale phonon-polariton optics, and ultrafast lattice control.

cond-mat.mtrl-sci↗
arXiv2026

Universal material basis for biocompatible printed electrolytes in Organic Electrochemical Transistors

Organic Electrochemical Transistors (OECTs) stand out for their interplay between ionic and electronic conduction, making them ideal analogues to biological synapses for neuromorphic computing and biosensing applications. Furthermore, they can be printed into integrated circuits on flexible substrates, enabling low-cost and high-throughput fabrication of complete electronic systems. However, most OECT electrolytes for integrated circuits still lack biocompatibility and suffer from rheology-related printing challenges. This paper presents a novel material basis that can be combined with an ionic liquid to fabricate an electrolyte for OECTs that only contains biocompatible materials. It allows rheological adjustments to enable the use of electrolyte in both inkjet and screen printing. Furthermore, the electrolyte is UV-curable, enabling it to transition into solid-state structures after printing. Extended ink and device lifetimes for screen-printed structures enable the fabrication of advanced OECTs that can operate in ambient air for over 30 days after fabrication. Ultimately, a fully screen-printed transistor using only biocompatible materials on a leaf substrate is shown

cond-mat.soft↗
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↗
arXiv2026

Ultra-high THz-field-confinement at LaAlO3 twin walls

The control and steering of light at nanometre length scales is crucial for the development of both fundamental science and nanophotonic technologies. Recent advancements have been achieved by exploiting various crystalline anisotropies, allowing for subdiffractional and diffraction-less canalisation of energy. These studies in particular benefit from stacking and twisting of 2D materials, whereas corresponding capabilities of anisotropic bulk crystals are rather unexplored. In this work, we show that ferroelastic twin walls - crystallographically perfect 2D-sheets that separate regions of differently oriented domains - in the distorted perovskite LaAlO3 provide a natural platform for broadband lateral confinement and superb canalisation of light at the nanoscale. Without fabrication processes, the electromagnetic fields localised at such walls exhibit lateral optical sizes up to 260 times smaller than the free-space wavelength. Depending on the adjacent domain orientation and frequency, the twin wall pattern preferentially concentrates or repels the electromagnetic energy, constituting a natural building block towards broadband MIR and THz nanophotonics for polaritonic circuitry.

physics.optics↗
arXiv2026

Uncovering the properties of homo-epitaxial GaN devices through cross-sectional infrared nanoscopy

Validating material performance in electrical devices is crucial to product development. For Gallium Nitride (GaN) devices, evaluating material factors such as defects, dopant concentration, and overall production quality is essential to ensure their performance in advanced electronic and optoelectronic applications. This work demonstrates that scattering-type scanning near-field optical microscopy (s-SNOM) can meet the demanding performance requirements for characterizing homoepitaxial GaN devices. Specifically, we show that combining s-SNOM results in the mid-IR and terahertz (THz) spectral ranges can disentangle carrier and lattice changes in a GaN p-i-n diode, which is not possible using one spectral range alone. We observe strong, resonant near-field signals near the LO phonon mode of GaN that correlate well with point-dipole models. This data shows great sensitivity to the local carrier density, with changes on the order of 1018 cm-3 easily resolved experimentally. Further, we demonstrate high sensitivity to sub-surface defects, which remain a significant challenge for other non-destructive techniques. To validate the power of s-SNOM imaging, our results are compared to traditional metrologies, including micro-Raman mapping and Kelvin Probe Force Microscopy (KPFM). Our results show that s-SNOM shows superior resolution and sensitivity to perturbations, highlighting the power of this technique in semiconductor device characterization.

cond-mat.mtrl-sci↗
arXiv2026

Tailoring phonon-driven responses in {\alpha}-MoO3 through isotopic enrichment

The implementation of polaritonic materials into nanoscale devices requires selective tuning of parameters to realize desired spectral or thermal responses. One robust material is {\alpha}-MoO3, which as an orthorhombic crystal boasts three distinct phonon dispersions, providing three polaritonic dispersions of hyperbolic phonon polaritons (HPhPs) across the mid-infrared (MIR). Here, the tunability of both optical and thermal responses in isotopically enriched {\alpha}-MoO3 (98MoO3, Mo18O3 and 98Mo18O3) are explored. A uniform ~5 % spectral redshift from 18O enrichment is observed in both Raman- and IR-active TO phonons. Both the in- and out-of-plane thermal conductivities for the isotopic variations are reported. Ab initio calculations both replicate experimental findings and analyze the select-mode three-phonon scattering contributions. The HPhPs from each isotopic variation are probed with s-SNOM and their Q- factors are reported. A Q-factor maxima increase of ~50 % along the [100] in the RB2 and ~100 % along the [001] in the RB3 are reported for HPhPs supported in 98Mo18O3. Observations in both real and Fourier space of higher-order HPhP modes propagating in single slabs of isotopically enriched {\alpha}-MoO3 without the use of a subdiffractional surface scatterer are presented here. This work illustrates the tunability of {\alpha}-MoO3 for thermal and nanophotonic applications.

cond-mat.mtrl-sci↗
arXiv2025

Real-space observation of the low-temperature Skyrmion lattice in Cu2OSeO3(100) single crystal

Cu2OSeO3 is a skyrmion host material in which two distinct thermodynamically stable skyrmion phases were identified. We report magnetic force microscopy imaging of the low-temperature magnetic phases in bulk Cu2OSeO3(100) single crystal. Tuning the external magnetic field over the various phase transition at a temperature of 10 K, we observe the formation of helical, conical, tilted conical and skyrmion lattice domains in real space.

cond-mat.mes-hall↗
arXiv2025

Spectral tuning of hyperbolic shear polaritons in monoclinic gallium oxide via isotopic substitution

Hyperbolic phonon polaritons - hybridized modes arising from the ultrastrong coupling of infrared light to strongly anisotropic lattice vibrations in uniaxial or biaxial polar crystals - enable to confine light to the nanoscale with low losses and high directionality. In even lower symmetry materials, such as monoclinic $\beta$-Ga$_2$O$_3$ (bGO), hyperbolic shear polaritons (HShPs) further enhance the directionality. Yet, HShPs are intrinsically supported only within narrow frequency ranges defined by the phonon frequencies of the host material. Here, we report spectral tuning of HShPs in bGO by isotopic substitution. Employing near-field optical microscopy to image HShPs in $^{18}$O bGO films homo-epitaxially grown on a $^{16}$O bGO substrate, we demonstrate a spectral redshift of $\sim~40~$cm$^{-1}$ for the $^{18}$O bGO, compared to $^{16}$O bGO. The technique allows for direct observation and a model-free estimation of the spectral shift driven by isotopic substitution without the need for knowledge of the dielectric tensor. Complementary far-field measurements and ab initio calculations - in good agreement with the near-field data - confirm the effectiveness of this estimation. This multifaceted study demonstrates a significant isotopic substitution induced spectral tuning of HShPs into a previously inaccessible frequency range, creating new avenues for technological applications of such highly directional polaritons.

physics.optics↗
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 $\alpha$, 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 $\alpha$ 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↗
arXiv2025

Phonon dephasing times determined with time-delayed, broadband CARS

Coherent Raman scattering techniques as coherent anti-Stokes Raman scattering (CARS), offer significant advantages in terms of pixel dwell times and speed as compared to spontaneous Raman scattering for investigations of crystalline materials. However, the spectral information in CARS is often hampered by the presence of a non-resonant contribution to the scattering process that shifts and distorts the Raman peaks. In this work, we apply a method to obtain non-resonant background-free spectra based on time-delayed, broadband CARS (TD-BCARS) using an intra-pulse excitation scheme. In particular, this method can measure the phononic dephasing times across the full phonon spectrum at once. We test the methodology on amorphous SiO2 (glass), which is used to characterize the setup-specific and material-independent response times, and then apply TD-BCARS to the analysis of single crystals of diamond and ferroelectrics of potassium titanyl phosphate (KTP) and potassium titanyl arsenate (KTA). For diamond, we determine a dephasing time of t = 7.81 ps for the single sp3 peak.

cond-mat.mtrl-sci↗
arXiv2025

Demonstration of domain wall current in MgO-doped lithium niobate single crystals up to 400 {\deg}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

Two-dimensional talc as a natural hyperbolic material

This study demonstrates that two-dimensional talc, a naturally abundant mineral, supports hyperbolic phonon-polaritons (HPhPs) at mid-infrared wavelengths, thus offering a low-cost alternative to synthetic polaritonic materials. Using scattering scanning near-field optical microscopy (s-SNOM) and synchrotron infrared nano spectroscopy (SINS), we reveal tunable HPhP modes in talc flakes of a long lifetime. These results highlight the potential of natural 2D talc crystals to constituting an effective platform for establishing scalable optoelectronic and photonic devices.

cond-mat.mes-hall↗
arXiv2024

Surface-near domain engineering in multi-domain x-cut lithium niobate tantalate mixed crystals

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 ($< 1$~$μ$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.

physics.optics↗
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↗