arXiv subjects

Ursula Wurstbauer

Publications and source records attributed to Ursula Wurstbauer.

At least 19 recordsLinked to original sources

arXiv2026

Resonant Raman signatures of bright and momentum-dark exciton coupled by intervalley phonon scattering in monolayer WSe2

Exciton-phonon coupling in atomically thin transition metal dichalcogenides governs key processes such as exciton thermalization and intervalley scattering and remains challenging to access directly by optical spectroscopy. Here, we employ resonance Raman spectroscopy at cryogenic temperatures to probe exciton-phonon coupling in hBN-encapsulated WSe_2 monolayers. Tuning the excitation laser across the bright exciton X_KK resonance, we observe rich Raman spectra and focus on the resonance profile of the degenerate A_1'/E' optical phonon mode. The profile exhibits two asymmetric resonance peaks whose energetic separation significantly exceeds the phonon energy - a feature that cannot be explained by first-order Raman scattering alone. We demonstrate that this discrepancy is resolved by including third-order Raman scattering, in which intervalley scattering enabled by a finite-momentum phonon couples the bright exciton X_KK to a momentum-dark exciton X_d. Fitting the experimental resonance profiles of two independent samples with a model comprising coherent first- and third-order scattering yields consistent exciton energies and linewidths, with a momentum-dark exciton X_d approximately 45meV to 55meV below the bright exciton X_KK. The results indicate efficient bright-to-dark exciton coupling. Our findings provide a microscopic framework for understanding the anomalously bright emission spectra of WSe_2 monolayers despite its spin-forbidden lowest exciton transition and highlight the role of momentum-dark excitons in resonant light-matter interaction.

cond-mat.mtrl-sci↗

arXiv2026

Identifying Contact Barrier Types in Few-Layer MoS2 Devices Using Correlative IV, LBIC, and Bias-Dependent KPFM

Electrical contacts between metals and two-dimensional (2D) semiconductors such as molybdenum disulfide (MoS2) critically govern device performance, yet their microscopic nature remains difficult to disentangle using any single characterization technique. Here we present an integrated experimental framework that combines current-voltage (IV) characterization, laser beam induced current (LBIC) mapping, and bias-dependent Kelvin probe force microscopy (KPFM) to comprehensively resolve the contact properties of few-layer MoS2-based two-terminal devices under ambient conditions. IV measurements deliver macroscopic transport characteristics as a function of bias voltage and illumination conditions. LBIC maps the local photocurrent response with micrometer spatial resolution, revealing the position and nature of internal electric fields at MoS2-metal interfaces. KPFM, operated under an applied static bias rather than in the conventional work-function mode, provides nanoscale-resolved potential distributions that quantify the relative magnitudes and spatial locations of contact barriers. We apply this framework to three representative devices - one exhibiting ohmic-like and two exhibiting diode-like contact behavior - and demonstrate that the combined analysis can unambiguously identify whether the dominant barrier is of Schottky or tunnel type and determine the asymmetry between the two contacts. We further demonstrate that thermal annealing significantly reduces the total resistance, while contact barriers remain the dominant source of resistance. The methodology is directly transferable to other 2D semiconductor-metal systems and provides a practical yet comprehensive route toward a quantitative microscopic understanding of 2D device contacts.

cond-mat.mtrl-sci↗

arXiv2026

Dielectric Tensor of CrSBr from Spectroscopic Imaging Ellipsometry

Chromium sulfur bromide (CrSBr) is a magnetic van der Waals semiconductor with a direct bandgap and pronounced anisotropy in its electronic, optical, spin and lattice degrees of freedom. Here, we employ spectroscopic imaging ellipsometry (SIE) and Mueller-matrix analysis to determine the full dielectric tensor of paramagnetic CrSBr thin films. Our measurements reveal optical anisotropy, characterized by three distinct diagonal components of the dielectric tensor. The in-plane elements are dominated by prominent excitonic resonances polarized along the two main crystallographic axes. Two main excitonic bands (A and B excitons) centered around 1.3eV and 1.7eV, respectively, are identified; the A-exciton polarized along the b-crystallographic direction, whereas the B-exciton appears to consist of two nearly degenerate contributions polarized along two orthogonal in-plane crystal axes. These results provide fundamental insight into anisotropic light-matter interactions in CrSBr, relevant for future spin-optoelectronic and photonic applications.

cond-mat.mtrl-sci↗

arXiv2026

High-Energy Interlayer Exciton Ensembles in MoSe$_2$/WSe$_2$ Heterostructures by Laguerre-Gaussian Excitation

We reveal the higher energetic luminescence part of interlayer exciton ensembles in MoSe$_2$/WSe$_2$ heterostructures upon excitation by an optical Laguerre-Gaussian mode. The excitation is achieved with the help of a spatial light modulator giving rise to a ring-shaped distribution of interlayer excitons. A hyperspectral analysis of the exciton photoluminescence suggests that the excitation scheme allows the accumulation of high-energetic excitons in the rings' center. We discuss the mechanisms leading to such a distribution, including exciton-exciton interaction, phase-space filling, and an incomplete thermalization.

cond-mat.mes-hall↗

arXiv2025

Optical Readout of Reconfigurable Layered Magnetic Domain Structure in CrSBr

The van der Waals magnetic semiconductor CrSBr combines multistable magnetic order with strong light--matter coupling, enabling optical access to a rich and reconfigurable layered magnetic domain structure. A purely optical, non-destructive, and non-contact readout of layered magnetic configurations is realized here by magneto-reflectance measurements and interpreted using an optical multilayer model. The magnetic state is tunable by applied magnetic fields and by interfacing CrSBr with the antiferromagnet MnPS$_3$. Applying an external magnetic field along the easy axis drives the hysteretic antiferromagnetic--to--ferromagnetic transition, which is not universally binary but instead develops through a cascade of intermediate magnetic configurations whose multiplicity and stability scale systematically with layer thickness and can be tailored by magnetic interfaces. The intertwined optical and magnetic properties of CrSBr provide a readout mechanism for information encoded in and processed through its magnetic configuration that is compatible with modern on- and off-chip photonic and electronic technologies. These properties identify CrSBr as a promising platform for intelligent matter and for spin-optoelectronics, in particular for neuromorphic architectures that can learn and evolve in response to changing environments.

cond-mat.mes-hall↗

arXiv2025

Precise Twist Angle Determination in twisted WSe2 via Optical Moir\'e Phonons

Twisted bilayers of transition metal dichalcogenides (TMDC) form moir\'e superlattices resulting in moir\'e minibands in momentum space and hosting localized excitons in real space. While moir\'e superlattices provide access to Mott-Hubbard physics, their energy potential landscape and electronic correlations are highly sensitive to fluctuations of the twist angle, disorder and lattice reconstructions. However, fast and non-invasive experimental access to local twist angle and its spatial variations is challenging. Here, we systematically correlate twist angle variations of twisted WSe2 bilayers across micrometer length scales using a combined lateral force microscopy (LFM) and a micro- Raman spectroscopy approach. These measurements uncover lateral variations in the twist angle by more than 1{\deg} across length scales relevant to optical and transport measurements. We demonstrate that twist angles in the range of 3{\deg} < $\alpha$ < 12{\deg} show distinct Raman response from scattering on optical moir\'e phonons allowing twist angle determination with high precision and sub-micrometer spatial resolution under ambient conditions. These modes are particularly sensitive in the low-angle twist regime, predicted to host emergent quantum phases. Our results establish micro-Raman spectroscopy of optical moir\'e phonons as a rapid, non-invasive probe to determine twist angle and to screen local twist angle variations with a precision better than $\pm$ 0.3{\deg} and a lateral resolution below one micrometer. This methodology is also applicable to fully hBN-encapsulated heterostructures.

cond-mat.mtrl-sci↗

arXiv2025

Impact of Electrical Contacts on Transition Metal Dichalcogenides-Based Acoustoelectric and Acousto-Photoelectric Devices

We study the impact of electrical contact barriers in hybrid WSe$_2$-LiNbO$_3$-based acoustoelectric and acousto-photoelectric devices using a combination of scanning photocurrent and acousto-electric current spectroscopy. Static scanning photocurrent measurements provide a qualitative measure of the band-bending and spatial distribution of the Schottky barrier between semiconducting WSe$_2$ and gold electrodes whereas the surface acoustic wave-induced acousto-electric current reveals the height of the tunnelling barrier created by the van der Waals gap between the multilayered WSe$_2$ flake and the gold electrodes in addition to the Schottky barrier. The combination of both techniques shows a ten-fold increase in the photocurrent by the acoustic wave. Moreover, the observed spatial redistribution of the current is attributed to the interplay between the contact properties at the source and drain electrodes and the charge carrier dynamics induced by the surface acoustic wave. The ratio of acoustic wavelength to the electrical channel length is found to impact the SAW-induced charge carrier transport. For a channel length shorter than one acoustic wavelength, carriers undergo a seesaw-like motion which changes to charge conveyance for channel lengths comparable or exceeding the acoustic wavelength.

cond-mat.mes-hall↗

arXiv2025

Defect-Mediated Phase Engineering of 2D Ag at the Graphene/SiC Interface

Atomically thin silver (Ag) films offer unique opportunities in plasmonic, quantum optics, and energy harvesting, yet conventional growth methods struggle to achieve structural control at the monolayer limit. Here, we demonstrate phase-selective synthesis of large-area, crystalline 2D Ag films via defect-engineered confinement heteroepitaxy (CHet) at the epitaxial graphene/silicon carbide (EG/SiC) interface. By tuning graphene growth and post-growth defect introduction, two distinct Ag phases are achieved with disparate properties: a nearly commensurate Ag(1) lattice stabilized by vacancy and line defects in epitaxial graphene, and a denser Ag(2) phase preferentially grown with sp3-rich zero-layer graphene. Structural and spectroscopic characterization confirm lattice registry with the SiC substrate, while theoretical calculations reveal a thermodynamic preference for Ag(2) but an easier nucleation for Ag(1). Both phases are found to be semiconducting, with the Ag(2) phase exhibiting slightly enhanced n-doping of graphene. Notably, nonlinear optical measurements reveal a three-order magnitude difference in second-order susceptibility between the two phases, demonstrating promise for phase-tunable 2D metals in reconfigurable optoelectronic and metamaterial platforms.

cond-mat.mtrl-sci↗

arXiv2025

Collective neutral excitations as sensitive probe for the quality of 2D charge carrier systems in ultra-pure GaAs quantum wells

Ultra-clean low-dimensional interacting charge carrier systems are the basis to explore correlated states and phases. We report the observation of very narrow collective intersubband excitations (ISBE) of 2D electron systems (2DESs) with ultra-high mobilities in high quality GaAs quantum well structures. These findings from resonant inelastic light scattering (RILS) experiments are used as tools for exploration of links between transport mobility and collective electron behavior in 2DES of high perfection. We find that the linewidths of collective ISBE modes can be very narrow with values smaller than 80{\mu}eV. Comparison of ISBE measurements from several high-mobility samples exhibits a variation in linewidth of more than a factor of two. There is, however, a surprising lack of direct correlation between ISBE linewidth with mobility in the range 15x10^6 cm^2/Vs<{\mu}<24x10^6 cm^2/Vs. ISBE by RILS are discussed as a sensitive probe to characterize the interacting electron systems for fractional quantum Hall effect (FQHE) studies.

cond-mat.mes-hall↗

arXiv2025

Unambiguous determination of optical constants and thickness of ultrathin films by using optical anisotropic substrates

The unambiguous and universal determination of optical constants such as complex refractive indices (n, k) and thickness (d) in one measurement is typically confined for films with a thickness of more than 10~nm that hampers its application for ultra-thin films such as two-dimensional materials. We demonstrate that the commonly accepted limit of n, k, d coupling is overcome in ellipsometry by utilizing anisotropic substrates. In this way, ellipsometry allows to determine n, k and d simultaneously for thicknesses lower than 1~nm with high accuracy. Extensive simulations proof the potential of using anisotropic substrates for decoupling. The simultaneous determination of n, k and d is of great interest in several fields, two-dimensional materials, their heterostructures, ultra thin films for application in quantum technology, plasmonics and nano-photonics.

physics.optics↗

arXiv2024

Laterally Extended States of Interlayer Excitons in Reconstructed MoSe$_2$/WSe$_2$ Heterostructures

Heterostructures made from 2D transition-metal dichalcogenides are known as ideal platforms to explore excitonic phenomena ranging from correlated moir\'e excitons to degenerate interlayer exciton ensembles. So far, it is assumed that the atomic reconstruction appearing in some of the heterostructures gives rise to a dominating localization of the exciton states. We demonstrate that excitonic states in reconstructed MoSe$_2$/WSe$_2$ heterostructures can extend well beyond the moir\'e periodicity of the investigated heterostructures. The results are based on real-space calculations yielding a lateral potential map for interlayer excitons within the strain-relaxed heterostructures and corresponding real-space excitonic wavefunctions. We combine the theoretical results with cryogenic photoluminescence experiments, which support the computed level structure and relaxation characteristics of the interlayer excitons.

cond-mat.mes-hall↗

arXiv2024

Interlayer and moiré excitons in atomically thin double layers: from individual quantum emitters to degenerate ensembles

Interlayer excitons (IXs), composed of electron and hole states localized in different layers, excel in bilayers composed of atomically thin van der Waals materials such as semiconducting transition metal dichalcogenides (TMDs) due to drastically enlarged exciton binding energies, exciting spin-valley properties, elongated lifetimes, and large permanent dipoles. The latter allows modification by electric fields and the study of thermalized bosonic quasiparticles, from the single particle level to interacting degenerate dense ensembles. Additionally, the freedom to combine bilayers of different van der Waals materials without lattice or relative twist angle constraints leads to layer hybridized and moiré excitons which can be widely engineered. This review covers fundamental aspects of IXs including correlation phenomena as well as the consequence of moiré superlattices with a strong focus on TMD homo- and hetero-bilayers.

cond-mat.mes-hall↗

arXiv2024

Collective charge excitations between moiré-minibands in twisted WSe2 bilayers from resonant inelastic light scattering

We establish low-temperature resonant inelastic light scattering (RILS) spectroscopy as a tool to probe the formation of a series of moiré-bands in twisted WSe_{2} bilayers by accessing collective intermoiré-band excitations (IMBE). We observe resonances in RILS spectra at energies in agreement with inter-moiré band transitions obtained from an ab-initio based continuum model. Transitions between the first and second inter-moiré band for a twist angle of about 8° are reported and between first and second, third and higher bands for a twist of about 3°. The signatures from IMBE for the latter highlight a strong departure from parabolic bands with flat minibands exhibiting very high density of states in accord with theory. These observations allow to quantify the transition energies at the K-point where the states relevant for correlation physics are hosted.

cond-mat.str-el↗

arXiv2024

Quadratic optical response of CrSBr controlled by spin-selective interlayer coupling

The optical properties of the layered magnet CrSBr are dominated by intralayer excitons: the antiferromagnetic order between the layers makes layer-to-layer charge hopping, and therefore interlayer excitons, spin-forbidden. An external magnetic field, however, continuously drives the magnetic order towards layer-to-layer ferromagnetic, which opens spin-allowed charge-transfer channels between the layers. Here we elaborate how their admixture changes the composition and nature of the excitons, leading to an extension over many layers, and causes a quadratic red-shift with respect to the external magnetic field. We address these effects by ab-initio $GW$-BSE calculations as a function of magnetic field and cast the data into a minimal four-band model to elucidate the interplay between the various interaction and coupling mechanisms. Our findings should be generally valid for antiferromagnetic layered magnets with and without external magnetic fields, and moreover for any couple of layers with different spin directions. Our insights help to systematically address excitons and predict their optical signatures in such systems.

cond-mat.mes-hall↗

arXiv2023

Exciton-phonon-scattering: A competition between bosonic and fermionic nature of bound electron-hole pairs

The question of macroscopic occupation and spontaneous emergence of coherence for exciton ensembles has gained renewed attention due to the rise of van der Waals heterostructures made of atomically thin semiconductors. The hosted interlayer excitons exhibit nanosecond lifetimes, long enough to allow for excitonic thermalization in time. Several experimental studies reported signatures of macroscopic occupation effects at elevated exciton densities. With respect to theory, excitons are composite particles formed by fermionic constituents, and a general theoretical argument for a bosonic thermalization of an exciton gas beyond the linear regime is still missing. Here, we derive an equation for the phonon mediated thermalization at densities above the classical limit, and identify which conditions favor the thermalization of fermionic or bosonic character, respectively. In cases where acoustic, quasielastic phonon scattering dominates the dynamics, our theory suggests that transition metal dichalcogenide (TMDC) excitons might be bosonic enough to show bosonic thermalization behaviour and decreasing dephasing for increasing exciton densities. This can be interpreted as a signature of an emerging coherence in the exciton ground state, and agrees well with the experimentally observed features, such as a decreasing linewidth for increasing densities.

cond-mat.mes-hall↗

arXiv2023

The bulk van der Waals layered magnet CrSBr is a quasi-1D material

Correlated quantum phenomena in one-dimensional (1D) systems that exhibit competing electronic and magnetic order are of strong interest for studying fundamental interactions and excitations, such as Tomonaga-Luttinger liquids and topological orders and defects with properties completely different from the quasiparticles expected in their higher-dimensional counterparts. However, clean 1D electronic systems are difficult to realize experimentally, particularly magnetically ordered systems. Here, we show that the van der Waals layered magnetic semiconductor CrSBr behaves like a quasi-1D material embedded in a magnetically ordered environment. The strong 1D electronic character originates from the Cr-S chains and the combination of weak interlayer hybridization and anisotropy in effective mass and dielectric screening with an effective electron mass ratio of $m^e_X/m^e_Y \sim 50$. This extreme anisotropy experimentally manifests in strong electron-phonon and exciton-phonon interactions, a Peierls-like structural instability and a Fano resonance from a van Hove singularity of similar strength of metallic carbon nanotubes. Moreover, due to the reduced dimensionality and interlayer coupling, CrSBr hosts spectrally narrow (1 meV) excitons of high binding energy and oscillator strength that inherit the 1D character. Overall, CrSBr is best understood as a stack of weakly hybridized monolayers and appears to be an experimentally attractive candidate for the study of exotic exciton and 1D correlated many-body physics in the presence of magnetic order.

cond-mat.mes-hall↗

arXiv2023

Extended spatial coherence of interlayer excitons in MoSe$_2$/WSe$_2$ heterobilayers

We report on the spatial coherence of interlayer exciton ensembles as formed in MoSe$_2$/WSe$_2$ heterostructures and characterized by point-inversion Michelson-Morley interferometry. Below 10 K, the measured spatial coherence length of the interlayer excitons reaches values equivalent to the lateral expansion of the exciton ensembles. In this regime, the light emission of the excitons turns out to be homogeneously broadened in energy with a high temporal coherence. At higher temperatures, both the spatial coherence length and the temporal coherence time decrease, most likely because of thermal processes. The presented findings point towards a spatially extended, coherent many-body state of interlayer excitons at low temperature.

cond-mat.mes-hall↗

arXiv2022

Exciton manifolds in highly ambipolar doped WS2

The disentanglement of single and many particle properties in 2D semiconductors and their dependencies on high carrier concentration is challenging to experimentally study by pure optical means. We establish an electrolyte gated WS2 monolayer field-effect structure capable to shift the Fermi level from the valence into the conduction band suitable to optically trace exciton binding as well as the single particle band gap energies in the weakly doped regime. Combined spectroscopic imaging ellipsometry and photoluminescence spectroscopies spanning large n- and p-type doping with charge carrier densities up to 10^14 cm-2 enable to study screening phenomena and doping dependent evolution of the rich exciton manifold whose origin is controversially discussed in literature. We show that the two most prominent emission bands in photoluminescence experiments are due to the recombination of spin-forbidden and momentum-forbidden charge neutral excitons activated by phonons. The observed interband transitions are redshifted and drastically weakened under electron or hole doping. This field-effect platform is not only suitable for studying exciton manifold but is also suitable for combined optical and transport measurements on degenerately doped atomically thin quantum materials at cryogenic temperatures.

cond-mat.mes-hall↗