arXiv subjects

Kerstin Volz

Publications and source records attributed to Kerstin Volz.

At least 19 recordsLinked to original sources

arXiv2026

Energy-time entanglement from a monolithically integrated quantum dot on silicon

Scalable quantum photonic technologies require deterministic sources of entangled photons that are compatible with established semiconductor manufacturing platforms. While self-assembled III--V semiconductor quantum dots are among the most promising sources of on-demand entanglement generation, their integration with silicon-based architectures remains a central challenge. Here, we demonstrate energy--time entanglement from a single InGaAs/GaAs quantum dot monolithically grown on a silicon substrate. Under coherent two-photon excitation, we achieve coherent control of the biexciton--exciton cascade, evidenced by Rabi oscillations and dressed-state formation. Using a four-channel Franson interferometer, we observe phase-dependent two-photon interference with visibilities up to $(64.0 \pm 7.0)\%$ for an 80 ps integration window (and $(49.4 \pm 1.9)\%$ for a 1600 ps window), approaching the threshold for Bell inequality violation at short time scales. These results establish monolithically integrated III--V-on-silicon quantum dots as promising sources of energy--time entangled photons for scalable quantum photonic technologies.

cond-mat.mes-hall↗

arXiv2026

Orientation Mapping via Dictionary Indexing of AC-STEM Kikuchi patterns using Open-source Software

The properties of polycrystalline materials are strongly influenced by the spatial arrangement and orientations of individual grains within the microstructure, making nanoscale characterization of grain orientation essential. This is also often the case for small grains in the nm regime explored using scanning transmission electron microscopy (STEM). Automated crystal orientation mapping (ACOM) is traditionally performed using spot-like diffraction patterns. In contrast, orientation mapping based on transmission Kikuchi diffraction (TKD) using an aberration-corrected (AC) convergent STEM probe remains relatively underexplored, despite its superior orientation sensitivity and higher spatial resolution. In this work, we present an open-source software-based template-matching approach for orientation mapping using AC-STEM TKD. A master pattern (a simulated angular distribution of Kikuchi band intensities on the unit sphere) is first generated through a dynamical simulation implemented in open-source software. This resulting pattern is subsequently imported into another open-source package for geometric simulations and orientation indexing. We demonstrate the capability of the proposed method by applying it to orientation mapping in BaZr0.4Ce0.4Y0.1Yb0.1O3-{\delta} (BZCYYb4411) fuel-cell material and LiNiO2 (LNO) lithium-ion battery cathode material. The best-matched simulated patterns exhibit strong agreement with experimental data, even under the challenging conditions with limited diffraction space available for matching.

cond-mat.mtrl-sci↗

arXiv2026

Localized Excitonic Emission in Wafer-Scale MOCVD-Grown GaSe 2D Nanosheets for Classical and Non-Classical Light Sources

Wafer-scale growth of two-dimensional semiconductors remains a key challenge for their integration into photonic technologies. While most studies of two-dimensional semiconductors have focused on transition metal dichalcogenides and their scalable fabrication, comparatively little attention has been given to III-VI monochalcogenides. Here, we report wafer-scale growth of gallium selenide (GaSe) by metal-organic chemical vapor deposition (MOCVD) and investigate its structural and optical properties for visible-range classical and quantum light emission. Two samples with thicknesses ranging from a few monolayers to several micrometers, controlled via the growth time, were investigated. The 30-minute grown sample yields intense, broad photoluminescence spanning 1.7--2.0$\,$eV, whereas the thinner 3-minute sample exhibits discrete narrow emission lines and single-photon emission with $(g^{(2)}(0) = 0.15 \pm 0.10)$. Remarkably, cathodoluminescence mapping reveals pronounced spatial localization of both spectrally narrow and broad emission centers. Together with temperature-dependent power-law analysis and Raman mapping, our results indicate defect-induced emission rather than intrinsic excitonic recombination. These findings establish wafer-scale MOCVD grown 2D GaSe as a platform for classical and non-classical light sources and highlight defect-engineered localization as a route toward scalable quantum photonics.

cond-mat.mes-hall↗

arXiv2026

Stark-tunable O-band single-photon sources based on deterministically fabricated quantum dot--circular Bragg gratings on silicon

Semiconductor quantum dots (QDs) offer outstanding quantum-optical properties, making them highly attractive for quantum information technologies. However, combining wide-range electrical tunability, efficient photon extraction, elevated-temperature operation, monolithic silicon integration, and telecom-wavelength compatibility remains a major challenge. Here, we demonstrate electrically contacted circular Bragg grating (eCBG) resonators incorporating InGaAs QDs directly grown on silicon, enabling bright single-photon emission in the telecom O-band. Deterministic electron-beam lithography and a ridge-based vertical p--i--n diode architecture enable precise device integration and electrical control of individual emitters. The QD--eCBGs exhibit a quantum-confined Stark shift of approximately 16 nm (11 meV) at 4 K, representing a record for QDs embedded in nanophotonic structures at telecom wavelengths. This is achieved alongside a photon extraction efficiency of $(21.7 \pm 3.0)\%$ into the first lens, while maintaining excellent radiative properties and high single-photon purity, with $g^{(2)}(0)=0.0078 \pm 0.0012$ below saturation and $g^{(2)}(0)=0.0183 \pm 0.0021$ at saturation under pulsed excitation. Robust antibunching persists up to 77 K, with $g^{(2)}(0)=0.0663 \pm 0.0056$, enabling operation with liquid-nitrogen or compact Stirling cryocoolers. Furthermore, spatially separated QD--eCBGs can be electrically tuned into spectral resonance without degrading photon statistics. These results establish a silicon-compatible, electrically addressable telecom O-band quantum light platform combining wide spectral tunability, high single-photon purity, and elevated-temperature operation, providing a scalable route toward practical photonic quantum networks.

physics.optics↗

arXiv2025

Direct Epitaxial Growth and Deterministic Device Integration of high-quality Telecom O-Band InGaAs Quantum Dots on Silicon Substrate

Semiconductor quantum dots (QDs) are key building blocks for photonic quantum technologies, enabling practical sources of non-classical light. A central challenge for scalable integration is the direct epitaxial growth of high-quality emitters on industry-compatible silicon platforms. Furthermore, for long-distance fiber-based quantum communication, emission in the telecom O- or C-band is essential. Here, we demonstrate the direct growth of high-quality InGaAs/GaAs QDs emitting in the telecom O-band using a strain-reducing layer approach on silicon. Deterministic integration of individual QDs into circular Bragg grating resonators is achieved via in-situ electron-beam lithography. The resulting devices exhibit strong out-coupling enhancement, with photon extraction efficiencies up to $(40 \pm 2)\%$, in excellent agreement with numerical simulations. These results highlight the high material quality of both the epitaxial platform and the photonic nanostructure, as well as the precise lateral positioning of the emitter within 20~nm of the resonator center. At cryogenic temperature (4~K) and low excitation power ($0.027\times P_\text{sat}$), the devices show excellent single-photon purity, exceeding 99\%. Operation at elevated temperatures of 40~K and 77~K, compatible with compact Stirling cryo-coolers and liquid-nitrogen cooling, reveals robust performance, with single-photon purity maintained at $(88.4 \pm 0.6)\%$ at 77~K. These results demonstrate a practical and scalable route toward silicon-based quantum light sources and provide a promising path for cost-effective fabrication and seamless integration of quantum photonics with classical electronics, representing an important step toward large-scale, chip-based quantum information systems.

cond-mat.mes-hall↗

arXiv2025

Robust coherent phonon mode at GaP/Si(001) heterointerface

Lattice-matched GaP layers without extended defects can be grown on Si(001) substrate via a two-step growth procedure, consisting of low-temperature nucleation followed by high-temperature overgrowth. A transient reflectivity experiment on a thin, low-temperature nucleation layer discovered a previously unknown phonon mode at 2 THz upon below-bandgap optical excitation (Adv. Mater. Interfaces 2025, 2400573). Here we examine the influence of the two-step growth process on the ultrafast carrier and phonon dynamics of the GaP/Si interface. We find that the discrete electronic state, which governed the interfacial carrier dynamics of the thin nucleation layer, becomes suppressed when a thicker layer is formed by high-temperature overgrowth. The coherent 2-THz oscillation is observed also in the high-temperature overgrown structures, at the constant frequency regardless of the GaP layer thickness. Its resonance behavior closely follows that of the carrier dynamics at the respective growth stage. This supports its assignment to a phonon mode generated at the heterointerface and strongly coupled to the interfacial carriers. The phonon amplitude exhibits a non-monotonic dependence on the GaP layer thickness, and its optical polarization-dependence is qualitatively altered by the high-temperature overgrowth, neither of which is accounted for by the carrier-phonon coupling alone. Our results demonstrate that the 2-THz interfacial phonon mode is robust against high-temperature overgrowth, while its amplitude is determined by both coupling to interfacial electronic transitions and atomic-scale structural reorganization at the interface.

cond-mat.mtrl-sci↗

arXiv2025

Low Temperature MOCVD Synthesis of high-mobility 2D InSe

Two-dimensional (2D) indium selenide (InSe) is a layered semiconductor with high electron mobility and a tunable band gap ranging from 1.25 eV in the bulk to 2.8 eV in the monolayer limit. These properties make these materials strong candidates for future logic and optoelectronic devices. However, growing phase-pure InSe remains challenging due to the complex indium-selenium (In-Se) phase diagram. This complexity and the sensitivity of chemical precursors to growth conditions make it difficult to control which In-Se phase forms during synthesis during, e.g., metal-organic chemical vapor deposition (MOCVD). Despite the challenges, MOCVD is considered the most promising approach for growing InSe, as it enables wafer-scale, uniform, and controllable deposition-key requirements for device integration. In this study, we present a systematic investigation of InSe synthesis via MOCVD on c-plane sapphire substrates at low temperatures, which are highly relevant for various integration schemes. By varying the Se/In precursor ratio and the growth temperature, we create a phase diagram that covers the In-rich, equal stoichiometric, and Se-rich InxSey phases. Raman spectroscopy and atomic force microscopy, supported by energy dispersive X-ray spectroscopy and scanning transmission electron microscopy, confirm conditions, under which the formation of 2D InSe is observed. Atomically-resolved cross-sectional scanning transmission electron microscopy also reveals an epitaxial alignment of the InSe with the sapphire substrate mediated by a specific interface reconstruction. The epitaxial alignment is verified by in-plane X-ray diffraction across large length scales. Samples grown under optimized conditions exhibit a strong optical absorption in the visible range and especially a comparably high electron mobility underlining the potential of the MOCVD-grown material for future applications.

cond-mat.mtrl-sci↗

arXiv2025

Microstructure of Silicon Anodes in Solid-State Batteries -- From Crystalline to Amorphous

Silicon offers great promise as a potential anode active material and the optimum alternative to lithium metal in all-solid-state lithium-ion batteries. However, its practical application is limited by severe volume expansion (~300%) during lithiation, leading to cracking upon delithiation. In this study, we investigated the microstructural evolution of microcrystalline silicon electrodes in a solid-electrolyte-free environment using cryogenic scanning transmission electron microscopy (STEM) during electrochemical cycling. A controlled workflow prevents ambient exposure, and cryo-TEM ensures structural integrity. After the first lithiation, the electrode shows a heterogeneous mix of crystalline Li15Si4, various amorphous LixSi phases, and residual crystalline silicon. After delithiation, the structure becomes predominantly amorphous with thread-like features and minimal remaining crystallinity. By the 10th delithiation, the microstructure is more uniform, with thread-like regions mainly at grain boundaries. Our results reveal that starting from a crystalline phase, a stationary microstructure emerges in bulk silicon only after several cycles. Thus, to have a more controlled behavior of the electrode and minimize cracking, the starting material should be carefully chosen along with an optimized electrode architecture to help stabilize the microstructure throughout cycling.

cond-mat.mtrl-sci↗

arXiv2025

STEM Diffraction Pattern Analysis with Deep Learning Networks

Accurate grain orientation mapping is essential for understanding and optimizing the performance of polycrystalline materials, particularly in energy-related applications. Lithium nickel oxide (LiNiO$_{2}$) is a promising cathode material for next-generation lithium-ion batteries, and its electrochemical behaviour is closely linked to microstructural features such as grain size and crystallographic orientations. Traditional orientation mapping methods--such as manual indexing, template matching (TM), or Hough transform-based techniques--are often slow and noise-sensitive when handling complex or overlapping patterns, creating a bottleneck in large-scale microstructural analysis. This work presents a machine learning-based approach for predicting Euler angles directly from scanning transmission electron microscopy (STEM) diffraction patterns (DPs). This enables the automated generation of high-resolution crystal orientation maps, facilitating the analysis of internal microstructures at the nanoscale. Three deep learning architectures--convolutional neural networks (CNNs), Dense Convolutional Networks (DenseNets), and Shifted Windows (Swin) Transformers--are evaluated, using an experimentally acquired dataset labelled via a commercial TM algorithm. While the CNN model serves as a baseline, both DenseNets and Swin Transformers demonstrate superior performance, with the Swin Transformer achieving the highest evaluation scores and the most consistent microstructural predictions. The resulting crystal maps exhibit clear grain boundary delineation and coherent intra-grain orientation distributions, underscoring the potential of attention-based architectures for analyzing diffraction-based image data. These findings highlight the promise of combining advanced machine learning models with STEM data for robust, high-throughput microstructural characterization.

cond-mat.dis-nn↗

arXiv2025

Determining the grain orientations of battery materials from electron diffraction patterns using convolutional neural networks

Polycrystalline materials have numerous applications due to their unique properties, which are often determined by the grain boundaries. Hence, quantitative characterization of grain as well as interface orientation is essential to optimize these materials, particularly energy materials. Using scanning transmission electron microscopy, matter can be analysed in an extremely fine grid of scan points via electron diffraction patterns at each scan point. By matching the diffraction patterns to a simulated database, the crystal orientation of the material as well as the orientation of the grain boundaries at each scan point can be determined. This pattern matching approach is highly time intensive. Artificial intelligence promises to be a very powerful tool for pattern recognition. In this work, we train convolutional neural networks (CNNs) on dynamically simulated diffraction patterns of LiNiO2, an important cathode-active material for Lithium-ion batteries, to predict the orientation of grains in terms of three Euler angles for the complete fundamental orientation region. Results demonstrate that these networks outperform the conventional pattern matching algorithm with increased accuracy and efficiency. The increased accuracy of the CNN models can be attributed to the fact that these models are trained by data incorporating dynamical effects. This work is the first attempt to apply deep learning for analysis of electron diffraction data and enlightens the great potential of ML to accelerate the analysis of electron microscopy data, toward high-throughput characterization technique.

cond-mat.mtrl-sci↗

arXiv2025

Sequential tilting 4D-STEM for improved momentum-resolved STEM field mapping

Momentum-resolved scanning transmission electron microscopy (MRSTEM) is a powerful phase-contrast technique that can map lateral magnetic and electric fields ranging from the micrometer to the subatomic scale. Resolving fields ranging from a few nanometers to a few hundred nanometers, as well as across material junctions, is particularly important since these fields often determine the functional properties of devices. However, it is also challenging since they are orders of magnitude smaller than atomic electric fields. Thus, subtle changes in diffraction conditions lead to significant changes in the measured MRSTEM signal. One established approach to partially overcome this problem is precession electron diffraction, in which the incident electron beam is continuously precessed while precession-averaged diffraction patterns are acquired. Here, we present an alternative approach in which we sequentially tilt the incident electron beam and record a full diffraction pattern for each tilt and spatial position. This approach requires no hardware modification of the instrument and enables the use of arbitrary beam tilt patterns that can be optimized for specific applications. Furthermore, recording diffraction patterns for every beam tilt allows access to additional information. In this work, we use this information to create virtual large-angle convergent beam electron diffraction (vLACBED) patterns to assess MRSTEM data quality and improve field measurements by applying different data analysis methods beyond simple averaging. The presented data acquisition concept can readily be applied to other 4D-STEM applications.

cond-mat.mtrl-sci↗

arXiv2024

Excitons in epitaxially grown WS2 on Graphene: a nanometer-resolved EELS and DFT study

In this study, we investigate excitonic properties of epitaxially grown WS2, which is of particular interest for various applications due to its potential for upscaling to wafer sized structures. Understanding the effect of the dielectric environment due to changing layer numbers and multi-material heterostructures on the optical properties is crucial for tailoring device properties. Monochromated electron energy loss spectroscopy in a scanning transmission electron microscope is employed to characterize the excitonic spectrum of WS2 on graphene grown by metal organic chemical vapor deposition. This technique provides the required spatial resolution at the nanometer scale in combination with high quality spectra. To complement the experimental results, theoretical investigations using density functional theory and applying the Bethe-Salpeter equations are conducted. We find that by transitioning from mono- to bi- to multilayers of WS2 the spectra show redshifts for both, the K-valley excitons at about 2.0 and 2.4 eV as well as excitonic features of higher energies. The latter features originate from so called band nesting of transitions between the Gamma- and K-point. In summary, this study provides valuable insights into the excitonic properties of WS2 in different layer configurations and environments, which are realistically needed for future device fabrication and property tuning. Finally, we can show that nanometer scale electron spectroscopy supported by careful theoretical modelling can successfully link atomic structure and optical properties, such as exciton shifts, in non-idealized complex material systems like multilayer 2D heterostructures.

cond-mat.mtrl-sci↗

arXiv2024

A Small Step for Epitaxy, a Large Step Towards Twist Angle Control in 2D Heterostructures

Two-dimensional (2D) materials have received a lot of interest over the past decade. Especially van der Waals (vdW) 2D materials, such as transition metal dichalcogenides (TMDCs), and their heterostructures exhibit semiconducting properties that make them highly suitable for novel device applications. Controllable mixing and matching of the 2D materials with different properties and a precise control of the in-plane twist angle in these heterostructures are essential to achieve superior properties and need to be established through large-scale device fabrication. To gain fundamental insight into the control of these twist angles, 2D heterostructures of tungsten disulfide (WS2) and graphene grown by bottom-up synthesis via metal-organic chemical vapor deposition (MOCVD) are investigated using a scanning transmission electron microscope (STEM). Specifically, the combination of conventional high-resolution imaging with scanning nano beam diffraction (SNBD) using advanced 4D STEM techniques is used to analyze moiré structures. The latter technique is used to reveal the epitaxial alignment within the WS2/Gr heterostructure, showing a direct influence of the underlying graphene layers on the moiré formation in the subsequent WS2 layers. In particular, the importance of grain boundaries within the underlying WS2 and Gr layers for the formation of moiré patterns with rotation angles below 2° is discussed.

cond-mat.mtrl-sci↗

arXiv2023

Accurate first-principle bandgap predictions in strain-engineered ternary III-V semiconductors

Tuning the bandgap in ternary III-V semiconductors via modification of the composition or the strain in the material is a major approach for the design of optoelectronic materials. Experimental approaches screening a large range of possible target structures are hampered by the tremendous effort to optimize the material synthesis for every target structure. We present an approach based on density functional theory efficiently capable of providing the bandgap as a function of composition and strain. Using a specific density functional designed for accurate bandgap computation (TB09) together with a band unfolding procedure and special quasirandom structures, we develop a computational protocol efficiently able to predict bandgaps. The approach's accuracy is validated by comparison to selected experimental data. We thus map the phase space of composition and strain (we call this the ``bandgap phase diagram'') for several important III-V compound semiconductors: GaAsP, GaAsN, GaPSb, GaAsSb, GaPBi, and GaAsBi. We show the application of these diagrams for identifying the most promising materials for device design. Furthermore, our computational protocol can easily be generalized to explore the vast chemical space of III-V materials with all other possible combinations of III- and V-elements.

cond-mat.mtrl-sci↗

arXiv2023

Strongly coupled interface electronic states and interface phonon mode at GaP/Si(001)

Ultrafast carrier and phonon dynamics at the buried heterointerface of GaP/Si(001) are investigated by means of two-color pump-probe reflectivity measurements. The carrier-induced reflectivity signal exhibits a resonant enhancement at pump-photon energies of 1.4 eV, which can be assigned to an optical transition between electronic interface states. The transient reflectivity is modulated by a coherent oscillation at 2 THz, whose amplitude also becomes maximum at 1.4 eV. The observed resonant behavior of the phonon mode in combination with a characteristic wavelength-dependence of, both, its frequency and initial phase, strongly indicate that the 2-THz mode is a difference-combination mode of a GaP-like and a Si-like phonon at the heterointerface and that this second-order scattering process can be enhanced by a double resonance involving the interfacial electronic states.

cond-mat.mtrl-sci↗

arXiv2023

Structure Determination in a new Type of Amorphous Molecular Solids with Different Nonlinear Optical Properties: A Comparative Structural Analysis

The microscopic structure of two amorphous materials with extreme nonlinear optical properties has been studied. One of these materials exhibits second harmonic generation, while another material of similar molecular structure emits brilliant white light if being irradiated with a simple IR laser diode. Structural differences were investigated using X-ray scattering and EXAFS combined with molecular RMC. Transmission electron microscopy and scanning precession electron diffraction were used to understand specific structural differences on all length scales, from mesoscopic down to mutual molecular arrangements. Characteristic differences were found at all scales. Close core-core spacing between {SnS} clusters as well as characteristic cluster distortions appear to be characteristic features of the white light emitting material. In the other material, cores are undistorted and core distances are larger. There, the formation of nanocrystalline structures in the amorphous matrix could also be identified as reason for the WLG suppression.

cond-mat.mtrl-sci↗

arXiv2023

Measuring spatially-resolved potential drops at semiconductor hetero-interfaces using 4D-STEM

Characterizing long-range electric fields and built-in potentials in functional materials at nano- to micrometer scales is of supreme importance for optimizing devices. E.g., the functionality of semiconductor heterostructures or battery materials is determined by the electric fields established at interfaces which can also vary spatially. In this study, we propose momentum-resolved four-dimensional scanning transmission electron microscopy (4D-STEM) for the quantification of these potentials and show the optimization steps required to reach quantitative agreement with simulations for the GaAs / AlAs hetero-junction model system. Using STEM the differences in the mean inner potentials (DELTA MIP) of two materials forming an interface and resulting dynamic diffraction effects have to be considered. We show that the measurement quality is significantly improved by precession, energy filtering and a non-zone-axis alignment of the specimen. Complementary simulations yielding a DELTA MIP of 1.3 V confirm that the potential drop due to charge transfer at the intrinsic interface is about 0.1 V, in agreement with experimental and theoretical values found in literture. These results show the feasibility of accurately measuring built-in potentials across hetero-interfaces of real device structures and its promising application for more complex interfaces of other polycrystalline materials on the nanometer scale.

cond-mat.mtrl-sci↗

arXiv2022

Ultra-Broadband Visible and Infrared Light Generation Driven by Far Infrared Light in the Broad Region from 8μm to 240μm

The most commonly used nonlinear optical process is the conversion of infrared light at 1064nm to green light at 532nm, as performed in common laser pointers. However, more relevant for future applications are nonlinear optical processes that generate a broad spectrum, a so called supercontinuum. A desirable goal is generating a spectrum that covers the whole visible range (400 -900nm), i.e., white light. Nowadays, white-light generation is usually achieved in specially designed photonic fibres requiring high laser intensities. However, in previous studies we showed that amorphous powders of $(PhSn)_4S_6$ cluster-molecules generate white light when they are irradiated by low-intensity near-infrared light. In this study, we use the mid- and far-infrared radiation of a free-electron laser to investigate the same molecules. White-light generation is observed for excitation with wavelength between 8 and 240$μ$ m. While the emitted radiation shows only slight variations, its intensity strongly depends on the excitation wavelength. We then match the wavelength dependent efficiency with the infrared absorption spectra of the material. This comparison shows: whenever the excitation can introduce molecular vibrations, less white light is generated. For all other wavelengths the excitation interacts mostly with the electron system. This shows that the electron system and the molecular backbone are decoupled to a large extent. Our work contributes to the understanding of the nonlinear process that underlies white-light generation in $(PhSn)_4S_6$ cluster molecules. Additionally, it shows the high potential of this material in applications where a broad laser spectrum is desired.

physics.optics↗