arXiv subjects

Ursula Wurstbauer

Publications and source records attributed to Ursula Wurstbauer.

At least 37 records · Page 2Linked to original sources

arXiv2022

Spectroscopic imaging ellipsometry of two-dimensional TMDC heterostructures

Semiconducting two-dimensional materials and their heterostructures gained a lot of interest for applications as well as fundamental studies due to their rich optical properties. Assembly in van der Waals heterostacks can significantly alter the intrinsic optical properties as well as the wavelength-dependent absorption and emission efficiencies making a direct comparison of e.g. photoluminescence intensities difficult. Here, we determine the dielectric function for the prototypical MoSe2/WSe2 heterobilayer and their individual layers. Apart from a redshift of 18 meV - 44 meV of the energetically lowest interband transitions, we find that for larger energies the dielectric function can only be described by treating the van der Waals heterobilayer as a new artificial homobilayer crystal rather than a stack of individual layers. The determined dielectric functions are applied to calculate the Michelson contrast of the individual layers and the bilayer in dependence of the oxide thickness of often used Si/SiO2 substrates. Our results highlight the need to consider the altered dielectric functions impacting the Michelson interference in the interpretation of intensities in optical measurements such as Raman scattering or photoluminescence.

cond-mat.mtrl-sci↗

arXiv2022

Domain Textures in the Fractional Quantum Hall Effect

Impacts of domain textures on low-lying neutral excitations in the bulk of fractional quantum Hall effect (FQHE) systems are probed by resonant inelastic light scattering. We demonstrate that large domains of quantum fluids support long-wavelength neutral collective excitations with well-defined wave vector (momentum) dispersion that could be interpreted by theories for uniform phases. Access to dispersive low-lying neutral collective modes in large domains of FQHE fluids such as long wavelength magnetorotons at filling factor v=1/3 offer significant experimental access to strong electron correlation physics in the FQHE.

cond-mat.mes-hall↗

arXiv2021

Optical dipole orientation of interlayer excitons in MoSe$_{2}$-WSe$_{2}$ heterostacks

We report on the far-field photoluminescence intensity distribution of interlayer excitons in MoSe$_{2}$-WSe$_{2}$ heterostacks as measured by back focal plane imaging in the temperature range between 1.7 K and 20 K. By comparing the data with an analytical model describing the dipolar emission pattern in a dielectric environment, we are able to obtain the relative contributions of the in- and out-of-plane transition dipole moments associated to the interlayer exciton photon emission. We determine the transition dipole moments for all observed interlayer exciton transitions to be (99 $\pm$ 1)% in-plane for R- and H-type stacking, independent of the excitation power and therefore the density of the exciton ensemble in the experimentally examined range. Finally, we discuss the limitations of the presented measurement technique to observe correlation effects in exciton ensembles.

cond-mat.mes-hall↗

arXiv2021

Tunable Two-Dimensional Group-III Metal Alloys

Chemically stable quantum-confined 2D metals are of interest in next-generation nanoscale quantum devices. Bottom-up design and synthesis of such metals could enable the creation of materials with tailored, on-demand, electronic and optical properties for applications that utilize tunable plasmonic coupling, optical non-linearity, epsilon-near-zero behavior, or wavelength-specific light trapping. In this work, we demonstrate that the electronic, superconducting and optical properties of air-stable two-dimensional metals can be controllably tuned by the formation of alloys. Environmentally robust large-area two-dimensional InxGa1-x alloys are synthesized by Confinement Heteroepitaxy (CHet). Near-complete solid solubility is achieved with no evidence of phase segregation, and the composition is tunable over the full range of x by changing the relative elemental composition of the precursor. The optical and electronic properties directly correlate with alloy composition, wherein the dielectric function, band structure, superconductivity, and charge transfer from the metal to graphene are all controlled by the indium/gallium ratio in the 2D metal layer.

cond-mat.mtrl-sci↗

arXiv2020

Unexpected Near-Infrared to Visible Non-linear Optical Properties from Two-Dimensional Polar Metals

Near-infrared-to-visible second harmonic generation from air-stable two-dimensional polar gallium and indium metals is described. The photonic properties of 2D metals - including the largest second-order susceptibilities reported for metals (approaching 10nm$^2$/V) - are determined by the atomic-level structure and bonding of two-to-three-atom-thick crystalline films. The bond character evolved from covalent to metallic over a few atomic layers, changing the out-of-plane metal-metal bond distances by approximately ten percent (0.2 $\unicode{x212B}$), resulting in symmetry breaking and an axial electrostatic dipole that mediated the large nonlinear response. Two different orientations of the crystalline metal atoms, corresponding to lateral displacements < 2 $\unicode{x212B}$, persisted in separate micron-scale terraces to generate distinct harmonic polarizations. This strong atomic-level structure-property interplay suggests metal photonic properties can be controlled with atomic precision.

cond-mat.mtrl-sci↗

arXiv2020

Photo-physics and electronic structure of lateral graphene/MoS2 and metal/MoS2 junctions

Integration of semiconducting transition metal dichalcogenides (TMDs) into functional optoelectronic circuitries requires an understanding of the charge transfer across the interface between the TMD and the contacting material. Here, we use spatially resolved photocurrent microscopy to demonstrate electronic uniformity at the epitaxial graphene/molybdenum disulfide (EG/MoS2) interface. A 10x larger photocurrent is extracted at the EG/MoS2 interface when compared to metal (Ti/Au) /MoS2 interface. This is supported by semi-local density-functional theory (DFT), which predicts the Schottky barrier at the EG/MoS2 interface to be ~2x lower than Ti/MoS2. We provide a direct visualization of a 2D material Schottky barrier through combination of angle resolved photoemission spectroscopy with spatial resolution selected to be ~300 nm (nano-ARPES) and DFT calculations. A bending of ~500 meV over a length scale of ~2-3 micrometer in the valence band maximum of MoS2 is observed via nano-ARPES. We explicate a correlation between experimental demonstration and theoretical predictions of barriers at graphene/TMD interfaces. Spatially resolved photocurrent mapping allows for directly visualizing the uniformity of built-in electric fields at heterostructure interfaces, providing a guide for microscopic engineering of charge transport across heterointerfaces. This simple probe-based technique also speaks directly to the 2D synthesis community to elucidate electronic uniformity at domain boundaries alongside morphological uniformity over large areas.

physics.app-ph↗

arXiv2020

Scalable single-photon sources in atomically thin MoS2

Real-world quantum applications, eg. on-chip quantum networks and quantum cryptography, necessitate large scale integrated single-photon sources with nanoscale footprint for modern information technology. While on-demand and high fidelity implantation of atomic scale single-photon sources in conventional 3D materials suffer from uncertainties due to the crystals dimensionality, layered 2D materials can host point-like centers with inherent confinement to a sub-nm plane. However, previous attempts to truly deterministically control spatial position and spectral homogeneity while maintaining the 2D character have not been realized. Here, we demonstrate the on-demand creation and precise positioning of single-photon sources in atomically thin MoS2 with very narrow ensemble broadening and near-unity fabrication yield. Focused ion beam irradiation creates 100s to 1000s of mono-typical atomistic defects with anti-bunched emission lines with sub-10 nm lateral and 0.7 nm axial positioning accuracy. Our results firmly establish 2D materials as a scalable platform for single-photon emitters with unprecedented control of position as well as photophysical properties owing to the all-interfacial nature.

cond-mat.mes-hall↗

arXiv2020

Light-matter interaction in van der Waals heterostructures

Even if individual two-dimensional materials own various interesting and unexpected properties, the stacking of such layers leads to van der Waals solids which unite the characteristics of two dimensions with novel features originating from the interlayer interactions. In this topical review, we cover fabrication and characterization of van der Waals heterosructures with a focus on heterobilayers made of monolayers of semiconducting transition metal dichalcogenides. Experimental and theoretical techniques to investigate those heterobilayers are introduced. Most recent findings focusing on different transition metal dichalcogenides heterostructures are presented and possible optical transitions between different valleys, appearance of moire patterns and signatures of moire excitons are discussed. The fascinating and fast growing research on van der Waals hetero-bilayers provide promising insights required for their application as emerging quantum-nano materials.

cond-mat.mes-hall↗

arXiv2020

Condensation signatures of photogenerated interlayer excitons in a van der Waals heterostack

Atomistic van der Waals heterostacks are ideal systems for high-temperature exciton condensation because of large exciton binding energies and long lifetimes. Charge transport and electron energy-loss spectroscopy showed first evidence of excitonic many-body states in such two-dimensional materials. Pure optical studies, the most obvious way to access the phase diagram of photogenerated excitons have been elusive. We observe several criticalities in photogenerated exciton ensembles hosted in MoSe2-WSe2 heterostacks with respect to photoluminescence intensity, linewidth, and temporal coherence pointing towards the transition to a coherent quantum state. For this state, the occupation is 100 percent and the exciton diffusion length is increased. The phenomena survive above 10 kelvin, consistent with the predicted critical condensation temperature. Our study provides a first phase-diagram of many-body interlayer exciton states including Bose Einstein condensation.

cond-mat.quant-gas↗

arXiv2019

Control of the orbital character of indirect excitons in MoS2/WS2 heterobilayers

Valley selective hybridization and residual coupling of electronic states in commensurate van der Waals heterobilayers enable the control of the orbital character of interlayer excitons. We demonstrate electric field control of layer index, orbital character, lifetime and emission energy of indirect excitons in MoS2/WS2 heterobilayers embedded in an vdW field effect structure. Different excitonic dipoles normal to the layers are found to stem from bound electrons and holes located in different valleys of MoS2/WS2 with a valley selective degree of hybridization. For the energetically lowest emission lines, coupling of electronic states causes a field-dependent level anticrossing that goes along with a change of the IX lifetime from 400 ns to 100 ns. In the hybridized regime the exiton is delocalized between the two constituent layers, whereas for large positive or negative electric fields, the layer index of the bound hole is field-dependent. Our results demonstrate the design of novel van der Waals solids with the possibility to in-situ control their physical properties via external stimuli such as electric fields.

cond-mat.mes-hall↗

arXiv2019

Observation of new plasmons in the fractional quantum Hall effect: interplay of topological and nematic orders

Collective modes of exotic quantum fluids reveal underlying physical mechanisms responsible for emergent complex quantum ground states. We observe unexpected new collective modes in the fractional quantum Hall (FQH) regime: intra-Landau-level plasmons in the second Landau level measured by resonant inelastic light scattering. The plasmons herald rotational-symmetry-breaking phases in tilted magnetic fields and reveal long-range translational invariance in these phases. The fascinating dependence of plasmon features on filling factor provide new insights on interplays between topological quantum Hall order and nematic electronic liquid crystal phases. A marked intensity minimum in the plasmon spectrum at Landau level filling factor v = 5/2 strongly suggests that this paired state, which could support non-Abelian excitations, overwhelms competing nematic phases, unveiling the robustness of the 5/2 superfluid state for small tilt angles. At v = 7/3, a sharp and strong plasmon peak that links to emerging macroscopic coherence supports the proposed model of a FQH nematic state at this filling factor.

cond-mat.mes-hall↗

arXiv2019

Atomistic defect states as quantum emitters in monolayer MoS$_2$

Quantum light sources in solid-state systems are of major interest as a basic ingredient for integrated quantum device technologies. The ability to tailor quantum emission through deterministic defect engineering is of growing importance for realizing scalable quantum architectures. However, a major difficulty is that defects need to be positioned site-selectively within the solid. Here, we overcome this challenge by controllably irradiating single-layer MoS$_{2}$ using a sub-nm focused helium ion beam to deterministically create defects. Subsequent encapsulation of the ion bombarded MoS$_{2}$ flake with high-quality hBN reveals spectrally narrow emission lines that produce photons at optical wavelengths in an energy window of one to two hundred meV below the neutral 2D exciton of MoS$_{2}$. Based on ab-initio calculations we interpret these emission lines as stemming from the recombination of highly localized electron-hole complexes at defect states generated by the helium ion bombardment. Our approach to deterministically write optically active defect states in a single transition metal dichalcogenide layer provides a platform for realizing exotic many-body systems, including coupled single-photon sources and exotic Hubbard systems.

cond-mat.mes-hall↗

arXiv2018

Hybridized indirect excitons in MoS2/WS2 heterobilayers

Ensembles of indirect or interlayer excitons (IXs) are intriguing systems to explore classical and quantum phases of interacting bosonic ensembles. IXs are composite bosons that feature enlarged lifetimes due to the reduced overlap of the electron-hole wave functions. We demonstrate electric Field control of indirect excitons in MoS2/WS2 hetero-bilayers embedded in a field effect structure with few-layer hexagonal boron nitrite as insulator and few-layer graphene as gate-electrodes. The different strength of the excitonic dipoles and a distinct temperature dependence identify the indirect excitons to stem from optical interband transitions with electrons and holes located in different valleys of the hetero-bilayer featuring highly hybridized electronic states. For the energetically lowest emission lines, we observe a field-dependent level anticrossing at low temperatures. We discuss this behavior in terms of coupling of electronic states from the two semiconducting monolayers resulting in spatially delocalized excitons of the hetero-bilayer behaving like an artificial van der Waals solid. Our results demonstrate the design of novel nano-quantum materials prepared from artificial van der Waals solids with the possibility to in-situ control their physical properties via external stimuli such as electric fields.

cond-mat.mes-hall↗

arXiv2018

Tuning the Fröhlich exciton-phonon scattering in monolayer MoS2

A direct band gap, remarkable light-matter coupling as well as strong spin-orbit and Coulomb interaction establish two-dimensional (2D) crystals of transition metal dichalcogenides (TMDs) as an emerging material class for fundamental studies as well as novel technological concepts. Valley selective optical excitation allows for optoelectronic applications based on the momentum of excitons. In addition to lattice imperfections and disorder, scattering by phonons is a significant mechanism for valley depolarization and decoherence in TMDs at elevated temperatures preventing high-temperature valley polarization required for realistic applications. Thus, a detailed knowledge about strength and nature of the interaction of excitons with phonons is vital. We directly access exciton-phonon coupling in charge tunable single layer MoS2 devices by polarization resolved Raman spectroscopy. We observe a strong defect mediated coupling between the long-range oscillating electric field induced by the longitudinal optical (LO) phonon in the dipolar medium and the exciton. We find that this so-called Fröhlich exciton LO-phonon interaction is suppressed by doping. This suppression correlates with a distinct increase of the degree of valley polarization of up to 20 % even at elevated temperatures of 220 K. Our result demonstrates a promising strategy to increase the degree of valley polarization towards room temperature valleytronic applications.

cond-mat.mes-hall↗

arXiv2018

Photo-induced anomalous Hall effect in the type-II Weyl-semimetal WTe2 at room-temperature

Using Hall photovoltage measurements, we demonstrate that an anomalous Hall-voltage can be induced in few layer WTe2 under circularly polarized light illumination. By applying a bias voltage along different crystal axes, we find that the photo-induced anomalous Hall conductivity coincides with a particular crystal axis. Our results are consistent with the underlying Berry-curvature exhibiting a dipolar distribution due to the breaking of crystal inversion symmetry. Using a time-resolved optoelectronic auto-correlation spectroscopy, we find that the decay time of the anomalous Hall voltage exceeds the electron-phonon scattering time by orders of magnitude but is consistent with the comparatively long spin-lifetime of carriers in the momentum-indirect electron and hole pockets in WTe2. Our observation suggests, that a helical modulation of an otherwise isotropic spin-current is the underlying mechanism of the anomalous Hall effect.

cond-mat.mtrl-sci↗

arXiv2018

Robust valley polarization of helium ion modified atomically thin MoS$_{2}$

Atomically thin semiconductors have dimensions that are commensurate with critical feature sizes of future optoelectronic devices defined using electron/ion beam lithography. Robustness of their emergent optical and valleytronic properties is essential for typical exposure doses used during fabrication. Here, we explore how focused helium ion bombardment affects the intrinsic vibrational, luminescence and valleytronic properties of atomically thin MoS$_{2}$. By probing the disorder dependent vibrational response we deduce the interdefect distance by applying a phonon confinement model. We show that the increasing interdefect distance correlates with disorder-related luminescence arising 180 meV below the neutral exciton emission. We perform ab-initio density functional theory of a variety of defect related morphologies, which yield first indications on the origin of the observed additional luminescence. Remarkably, no significant reduction of free exciton valley polarization is observed until the interdefect distance approaches a few nanometers, namely the size of the free exciton Bohr radius. Our findings pave the way for direct writing of sub-10 nm nanoscale valleytronic devices and circuits using focused helium ions.

cond-mat.mes-hall↗

arXiv2017

Contact morphology and revisited photocurrent dynamics in monolayer MoS2

Two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have emerged as promising materials for electronic, optoelectronic, and valleytronic applications. Recent work suggests drastic changes of the band gap and exciton binding energies of photo-excited TMDs with ultrafast non-radiative relaxation processes effectively heating the crystal lattice. Such phenomena have not been considered in the context of optoelectronic devices yet. We resolve corresponding ultrafast photo-conductance dynamics within monolayer MoS2 and demonstrate that a bolometric contribution dominates the overall photoconductance. We further reveal that a focused laser illumination, as is used in many standard optoelectronic measurements of MoS2, modifies and anneals the morphology of metal contacts. We show that a junction evolves with lateral built-in electric fields, although Raman- and photoluminescence spectra indicate no significant changes such as a crystal phase transition. We highlight how such optimized devices can drive ultrafast electromagnetic signals in on-chip high-frequency and THz circuits.

cond-mat.mes-hall↗

arXiv2017

Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit

We demonstrate the reduction of the inhomogeneous linewidth of the free excitons in atomically thin transition metal dichalcogenides (TMDCs) MoSe$_{2}$, WSe$_{2}$ and MoS$_{2}$ by encapsulation within few nanometer thick hBN. Encapsulation is shown to result in a significant reduction of the 10K excitonic linewidths down to $\sim3.5 \text{ meV}$ for n-MoSe$_{2}$, $\sim5.0 \text{ meV}$ for p-WSe$_{2}$ and $\sim4.8 \text{ meV}$ for n-MoS$_{2}$. Evidence is obtained that the hBN environment effectively lowers the Fermi level since the relative spectral weight shifts towards the neutral exciton emission in n-doped TMDCs and towards charged exciton emission in p-doped TMDCs. Moreover, we find that fully encapsulated MoS$_{2}$ shows resolvable exciton and trion emission even after high power density excitation in contrast to non-encapsulated materials. Our findings suggest that encapsulation of mechanically exfoliated few-monolayer TMDCs within nanometer thick hBN dramatically enhances optical quality, producing ultra-narrow linewidths that approach the homogeneous limit.

cond-mat.mes-hall↗