arXiv subjects

Christoph Kastl

Publications and source records attributed to Christoph Kastl.

At least 19 recordsLinked to original sources

arXiv2026

Second-Harmonic Imaging of Magnetic Domains in Thin Film Hematite

Hematite is an antiferromagnetic oxide and candidate altermagnetic insulator whose Néel order reorients from an easy-axis to an easy-plane phase at the Morin transition. Interpreting altermagnetic transport and symmetry sensitive optical responses requires knowledge of the Néel vector orientation relative to the crystal axes and of the domain structure within the probed device. Here, we show that polarization-resolved second-harmonic generation (SHG) microscopy resolves magnetic symmetry and domains in epitaxial (0001)-oriented hematite films. Across the Morin temperature, the SHG polarization anisotropy evolves from an approximately sixfold pattern consistent with the easy-axis orientation to pronounced twofold patterns consistent with the easy-plane orientation. A symmetry analysis based on magnetic-dipole and electric-quadrupole contributions reproduces this evolution. Importantly, the interference between SHG amplitudes that are odd and even under reversal of the magnetic order renders opposite Néel-vector orientations optically distinguishable. Consistently, opposite directions of an applied in-plane magnetic field produce distinct SHG responses in our experiments. Using this magnetic contrast, we image micrometer-scale domains, their reorganization across the Morin transition, and their reconfiguration under magnetic and thermal cycling, including a remanent change after cycling through the spin-flop transition. These results establish SHG microscopy as a local probe of magnetic symmetry, Néel-vector orientation, and domain evolution in hematite films.

cond-mat.mtrl-sci↗

arXiv2026

Ultrafast photo-thermoelectric currents in graphene junctions in the mid-infrared

Graphene is widely recognized for its ultrafast and broadband photocurrent response, but whether the broadband ultrafast characteristics are preserved at mid-infrared wavelengths with photon energies below the optical phonon energy remains an open question. Here, we investigate the carrier dynamics in graphene junctions under mid-infrared excitation using an ultrafast pump-probe photocurrent spectroscopy. We utilize dual split gate devices to demonstrate that the photo-thermoelectric effect can dominate the photoresponse of graphene also for a mid-infrared femtosecond excitation. We observe that graphene retains its broadband photocurrent response in this spectral region, but the photocurrent relaxation time increases from ca. 2 ps below 8-9 micrometer up to 3 ps at longer mid-infrared wavelengths. The absence of a pronounced phonon bottleneck in the decay dynamics at room temperature suggests an efficient interplay of electron-electron and electron-phonon scattering even for photon energies below the optical phonon energy in graphene. The observed wavelength dependence of the photocurrent relaxation times is consistent with energy-dependent theoretical relaxation times as derived from a microscopic transport theory of graphene that includes electron-phonon coupling within a Holstein-Peierls Hamiltonian.

cond-mat.mes-hall↗

arXiv2026

Zero-phonon line emission of single photon emitters in helium-ion treated MoS$_2$

We explore the zero-phonon line of single photon emitters in helium-ion treated monolayer MoS$_2$, which are currently understood in terms of single sulfur-site vacancies. By comparing the linewidths of the zero-phonon line as extracted directly from optical spectra with values inferred from the first-order autocorrelation function of the photoluminescence, we quantify bounds of the homogeneous broadening and of phonon-assisted contributions. The results are discussed in terms of both the independent boson model and ab-initio results as computed from GW and Bethe-Salpeter equation approximations.

cond-mat.mes-hall↗

arXiv2026

Creation and Microscopic Origins of Single-Photon Emitters in Transition Metal Dichalcogenides and Hexagonal Boron Nitride

We highlight recent advances in the controlled creation of single-photon emitters in van der Waals materials and in the understanding of their atomistic origin. We focus on quantum emitters created in monolayer transition-metal dichalcogenide semiconductors, which provide spectrally sharp single-photon emission at cryogenic temperatures, and the ones in insulating hBN, which provide bright and stable single-photon emission up to room temperature. After introducing the different classes of quantum emitters in terms of band-structure properties, we review the defect creation methods based on electron and ion irradiation as well as local strain engineering and plasma treatments. A main focus of the review is put on discussing the microscopic origin of the quantum emitters as revealed by various experimental platforms, including optical and scanning probe methods.

cond-mat.mes-hall↗

arXiv2025

Single-Photon Detection in Few-Layer NbSe$_2$ Superconducting Nanowires

Superconducting Nanowire Single-Photon Detectors (SNSPDs) are key building blocks for photonic quantum technologies due to their ability to detect single photons with ultra-high efficiency, low dark counts and fast temporal resolution. Superconducting materials exhibiting high uniformity, large absorption cross-section and atomic-scale thickness are desirable to extend single-photon detection from the near-infrared up to the terahertz regime, where existing material choices are especially constrained. Substrate independence would further open the way to integrate detectors onto functional materials and heterostructures, enhancing performance and enabling proximal read-out of a wide range of individual excitations. Here, we top-down shape the prototypical two-dimensional superconductor niobium diselenide (NbSe$_2$) into few-layer nanowires less than 100 nm wide and demonstrate single-photon detection at 780 and 1550 nm. At the same time, the dark-count rate remains below 1 Hz up to the switching current and we achieve a timing jitter below 50 ps. We use a diffusive hot-spot model to estimate a theoretical cut-off wavelength that surpasses the millimetre range. Our results open up routes toward quantum limited detectors integrated into quantum-photonic circuits and quantum devices, with the potential for novel detection capabilities and unprecedented energy sensitivity.

cond-mat.supr-con↗

arXiv2025

Quantifying the creation of negatively charged boron vacancies in He-ion irradiated hexagonal boron nitride

Hexagonal boron nitride (hBN) hosts luminescent defects possessing spin qualities compatible with quantum sensing protocols at room temperature. Vacancies, in particular, are readily obtained via exposure to high-energy ion beams. While the defect creation mechanism via such irradiation is well understood, the occurrence rate of optically active negatively charged vacancies ($V_B^-$) is an open question. In this work, we exploit focused helium ions to systematically generate optically active vacancy defects in hBN flakes at varying density. By comparing the density-dependent spin splitting measured by magnetic resonance to calculations based on a microscopic charge model, in which we introduce a correction term due to a constant background charge, we are able to quantify the number of $V_B^-$ defects generated by the ion irradiation. We find a lower bound for the fraction (0.2%) of all vacancies in the optically active, negatively charged state. Our results provide a protocol for measuring the generation efficiency of $V_B^-$, which is necessary for understanding and optimizing luminescent centers in hBN.

cond-mat.mes-hall↗

arXiv2024

Spectrally resolved far-field emission pattern of single photon emitters in MoS2

We explore the optical dipole orientation of single photon emitters in monolayer MoS2 as produced by a focused helium ion beam. The single photon emitters can be understood as single sulfur vacancies. The corresponding far-field luminescence spectra reveal several photoluminescence lines below the dominating luminescence of the exciton in MoS2. These sub-bandgap emission lines were predicted by ab initio theory, but they have never been resolved in luminescence experiments because of their small amplitude. We reveal the lines by their dependence as a function of the photon energy and momentum as measured in the back focal plane of the optical circuitry. The agreement between theory and experiment suggests that the defect states interact strongly within the Brillouin zone.

cond-mat.mes-hall↗

arXiv2023

Combining experiments on luminescent centres in hexagonal boron nitride with the polaron model and ab initio methods towards the identification of their microscopic origin

The two-dimensional material hexagonal boron nitride (hBN) hosts luminescent centres with emission energies of 2 eV which exhibit pronounced phonon sidebands. We investigate the microscopic origin of these luminescent centres by combining ab initio calculations with non-perturbative open quantum system theory to study the emission and absorption properties of 26 defect transitions. Comparing the calculated line shapes with experiments we narrow down the microscopic origin to three carbon-based defects: $\mathrm{C_2C_B}$, $\mathrm{C_2C_N}$, and $\mathrm{V_NC_B}$. The theoretical method developed enables us to calculate so-called photoluminescence excitation (PLE) maps, which show excellent agreement with our experiments. The latter resolves higher-order phonon transitions, thereby confirming both the vibronic structure of the optical transition and the phonon-assisted excitation mechanism with a phonon energy 170 meV. We believe that the presented experiments and polaron-based method accurately describe luminescent centres in hBN and will help to identify their microscopic origin.

cond-mat.mtrl-sci↗

arXiv2023

Spin-defect characteristics of single sulfur vacancies in monolayer $\text{MoS}_2$

Single spin defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2 and Q*) of He-ion induced sulfur vacancies in monolayer $\text{MoS}_2$. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wavefunction extent of $\sim$ 3.5 nm. The distinct valley-Zeeman splitting in out-of-plane $B$-fields and the brightening of dark states through in-plane $B$-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab-initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.

cond-mat.mes-hall↗

arXiv2022

Ultra-Sensitive Extinction Measurements of Optically Active Defects in Monolayer MoS$_2$

We utilize cavity-enhanced extinction spectroscopy to directly quantify the optical absorption of defects in MoS$_2$ generated by helium ion bombardment. We achieve hyperspectral imaging of specific defect patterns with a detection limit below 0.01% extinction, corresponding to a detectable defect density below $10^{11}$ cm$^{-2}$. The corresponding spectra reveal a broad sub-gap absorption, being consistent with theoretical predictions related to sulfur vacancy-bound excitons in MoS$_2$. Our results highlight cavity-enhanced extinction spectroscopy as efficient means for the detection of optical transitions in nanoscale thin films with weak absorption, applicable to a broad range of materials.

cond-mat.mes-hall↗

arXiv2021

Berry curvature-induced local spin polarisation in gated graphene/WTe$_2$ heterostructures

Full experimental control of local spin-charge interconversion is of primary interest for spintronics. Heterostructures combining graphene with a strongly spin-orbit coupled two-dimensional (2D) material enable such functionality by design. Electric spin valve experiments have provided so far global information on such devices, while leaving the local interplay between symmetry breaking, charge flow across the heterointerface and aspects of topology unexplored. Here, we utilize magneto-optical Kerr microscopy to resolve the gate-tunable, local current-induced spin polarisation in graphene/WTe$_2$ van der Waals (vdW) heterostructures. It turns out that even for a nominal in-plane transport, substantial out-of-plane spin accumulation is induced by a corresponding out-of-plane current flow. We develop a theoretical model which explains the gate- and bias-dependent onset and spatial distribution of the massive Kerr signal on the basis of interlayer tunnelling, along with the reduced point group symmetry and inherent Berry curvature of the heterostructure. Our findings unravel the potential of 2D heterostructure engineering for harnessing topological phenomena for spintronics, and constitute an important further step toward electrical spin control on the nanoscale.

cond-mat.mes-hall↗

arXiv2021

Exciton self-trapping causes picoseconds recombination in metal-organic chalcogenides hybrid quantum wells

Metal-organic species can be designed to self-assemble in large-scale, atomically defined, supramolecular architectures. Hybrid quantum wells, where inorganic two-dimensional (2D) planes are separated by organic ligands, are a particular example. The ligands effectively provide an intralayer confinement for charge carriers resulting in a 2D electronic structure, even in multilayered assemblies. Air-stable metal organic chalcogenides hybrid quantum wells have recently been found to host tightly bound 2D excitons with strong optical anisotropy in a bulk matrix. Here, we investigate the excited carrier dynamics in the prototypical metal organic chalcogenide [AgSePh], disentangling three excitonic resonances by low temperature transient absorption spectroscopy. Our analysis suggests a complex relaxation cascade comprising ultrafast screening and renormalization, inter-exciton relaxation, and self-trapping of excitons within few picoseconds. The ps-decay provided by the self-trapping mechanism may be leveraged to unlock the material's potential for ultrafast optoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2020

Vibronic response of a spin-1/2 state from a carbon impurity in two-dimensional WS$_2$

We demonstrate the creation of a spin-1/2 state via the atomically controlled generation of magnetic carbon radical ions (CRIs) in synthetic two-dimensional transition metal dichalcogenides (TMDs). Hydrogenated carbon impurities located at chalcogen sites introduced by chemical doping can be activated with atomic precision by hydrogen depassivation using a scanning probe tip. In its anionic state, the carbon impurity exhibits a magnetic moment of 1 $μ_\text{B}$ resulting from an unpaired electron populating a spin-polarized in-gap orbital of C$^{\bullet -}_\text{S}$. Fermi level control by the underlying graphene substrate can charge and decharge the defect, thereby activating or quenching the defect magnetic moment. By inelastic tunneling spectroscopy and density functional theory calculations we show that the CRI defect states couple to a small number of vibrational modes, including a local, breathing-type mode. Interestingly, the electron-phonon coupling strength critically depends on the spin state and differs for monolayer and bilayer WS$_2$. These carbon radical ions in TMDs comprise a new class of surface-bound, single-atom spin-qubits that can be selectively introduced, are spatially precise, feature a well-understood vibronic spectrum, and are charge state controlled.

cond-mat.mtrl-sci↗

arXiv2020

How Substitutional Point Defects in Two-Dimensional WS$_2$ Induce Charge Localization, Spin-Orbit Splitting, and Strain

Control of impurity concentrations in semiconducting materials is essential to device technology. Because of their intrinsic confinement, the properties of two-dimensional semiconductors such as transition metal dichalcogenides (TMDs) are more sensitive to defects than traditional bulk materials. The technological adoption of TMDs is dependent on the mitigation of deleterious defects and guided incorporation of functional foreign atoms. The first step towards impurity control is the identification of defects and assessment of their electronic properties. Here, we present a comprehensive study of point defects in monolayer tungsten disulfide (WS$_2$) grown by chemical vapor deposition (CVD) using scanning tunneling microscopy/spectroscopy, CO-tip noncontact atomic force microscopy, Kelvin probe force spectroscopy, density functional theory, and tight-binding calculations. We observe four different substitutional defects: chromium (Cr$_{\text{W}}$) and molybdenum (Mo$_{\text{W}}$) at a tungsten site, oxygen at sulfur sites in both bottom and top layers (O$_{\text{S}}$ top/bottom), as well as two negatively charged defects (CDs). Their electronic fingerprints unambiguously corroborate the defect assignment and reveal the presence or absence of in-gap defect states. The important role of charge localization, spin-orbit coupling, and strain for the formation of deep defect states observed at substitutional defects in WS$_2$ as reported here will guide future efforts of targeted defect engineering and doping of TMDs.

cond-mat.mes-hall↗

arXiv2020

Identifying substitutional oxygen as a prolific point defect in monolayer transition metal dichalcogenides with experiment and theory

Chalcogen vacancies are considered to be the most abundant point defects in two-dimensional (2D) transition-metal dichalcogenide (TMD) semiconductors, and predicted to result in deep in-gap states (IGS). As a result, important features in the optical response of 2D-TMDs have typically been attributed to chalcogen vacancies, with indirect support from Transmission Electron Microscopy (TEM) and Scanning Tunneling Microscopy (STM) images. However, TEM imaging measurements do not provide direct access to the electronic structure of individual defects; and while Scanning Tunneling Spectroscopy (STS) is a direct probe of local electronic structure, the interpretation of the chemical nature of atomically-resolved STM images of point defects in 2D-TMDs can be ambiguous. As a result, the assignment of point defects as vacancies or substitutional atoms of different kinds in 2D-TMDs, and their influence on their electronic properties, has been inconsistent and lacks consensus. Here, we combine low-temperature non-contact atomic force microscopy (nc-AFM), STS, and state-of-the-art ab initio density functional theory (DFT) and GW calculations to determine both the structure and electronic properties of the most abundant individual chalcogen-site defects common to 2D-TMDs. Surprisingly, we observe no IGS for any of the chalcogen defects probed. Our results and analysis strongly suggest that the common chalcogen defects in our 2D-TMDs, prepared and measured in standard environments, are substitutional oxygen rather than vacancies.

cond-mat.mtrl-sci↗

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

Characterizing Transition-Metal Dichalcogenide Thin-Films using Hyperspectral Imaging and Machine Learning

Atomically thin polycrystalline transition-metal dichalcogenides (TMDs) are relevant to both fundamental science investigation and applications. TMD thin-films present uniquely difficult challenges to effective nanoscale crystalline characterization. Here we present a method to quickly characterize the nanocrystalline grain structure and texture of monolayer WS2 films using scanning nanobeam electron diffraction coupled with multivariate statistical analysis of the resulting data. Our analysis pipeline is highly generalizable and is a useful alternative to the time consuming, complex, and system-dependent methodology traditionally used to analyze spatially resolved electron diffraction measurements.

cond-mat.mes-hall↗

arXiv2019

Electrically driven photon emission from individual atomic defects in monolayer WS2

Optical quantum emitters are a key component of quantum devices for metrology and information processing. In particular, atomic defects in 2D materials can operate as optical quantum emitters that overcome current limitations of conventional bulk emitters, such as yielding a high single-photon generation rate and offering surface accessibility for excitation and photon extraction. Here we demonstrate electrically stimulated photon emission from individual point defects in a 2D material. Specifically, by bringing a metallic tip into close proximity to a discrete defect state in the band gap of WS2, we induce inelastic tip-to-defect electron tunneling with an excess of transition energy carried by the emitted photons. We gain atomic spatial control over the emission through the position of the tip, while the spectral characteristics are highly customizable by varying the applied tip-sample voltage. Atomically resolved emission maps of individual sulfur vacancies and chromium substituent defects are in excellent agreement with the electron density of their respective defect orbitals as imaged via conventional elastic scanning tunneling microscopy. Inelastic charge-carrier injection into localized defect states of 2D materials thus provides a powerful platform for electrically driven, broadly tunable, atomic-scale single-photon sources.

cond-mat.mes-hall↗