arXiv subjects

Marika Schleberger

Publications and source records attributed to Marika Schleberger.

At least 19 recordsLinked to original sources

arXiv2026

Phenomenological Growth Regimes in Liquid-Precursor CVD of MoS$_2$ on Functional Substrates

The integration of two-dimensional transition-metal dichalcogenides (TMDCs) onto functional substrates remains constrained by stochastic vapor-phase growth dynamics. Here, we show that liquid-phase precursor chemical vapor deposition (CVD) of MoS$_2$ introduces growth conditions that are consistent with a substrate-influenced reaction-diffusion process. By utilizing pre-growth spin-coated MoO$_3$ intermediates across a diverse crystalline library (sapphire, SrTiO$_3$, rutile TiO$_2$, MgO, and 6H-SiC), we find that substrate-dependent variations in precursor wetting, surface chemistry, and inferred mass-transport constraints correlate with distinct growth morphologies. These substrate-dependent growth regimes are interpreted in terms of reduced effective lateral growth length on SrTiO$_3$, possible precursor anchoring on TiO$_2$, likely chemical surface restructuring on MgO, and possible step-edge growth on SiC. Raman and photoluminescence spectroscopy reveal substrate-dependent variations in vibrational and optical response that correlate with differences in strain, charge environment, and dielectric screening. Ultimately, this work highlights a substrate-dependent reaction-diffusion framework as a potentially useful route for tuning the structural and optical properties of large-area 2D materials.

cond-mat.mtrl-sci↗

arXiv2026

Quantitative Analysis of Composition and Contamination of Atomically Thin Materials by Recoil-Projectile Coincidence in Ion Transmission

Surface contamination strongly affects the intrinsic properties of nanoscale materials, making its reliable identification and quantification crucial for both accurate experimental interpretation and nanofabrication. Although scanning transmission electron microscopy can resolve contaminants at atomic resolution within nanometer-scale regions, it cannot easily provide a quantitative, large-area contamination measure. Here, we introduce a minimally destructive recoil-projectile coincidence method for ion transmission experiments that enables element-specific identification and quantification of surface contaminants with isotopic resolution. We demonstrate this approach by comparing self-supporting graphene samples prepared using either a polymethylmethacrylate (PMMA)-based or a PMMA-free transfer process. Carbon and hydrogen are identified as the dominant surface contaminants. PMMA-free transferred graphene exhibits the lowest native contamination levels. Following in-situ thermal annealing at 400 °C for 1 h, the measured carbon areal density approaches the value expected for atomically clean single-layer graphene within the experimental uncertainty, while hydrogen coverage is strongly reduced. Unlike PMMA-transferred graphene, which rapidly recontaminates after annealing, PMMA-free transferred graphene remains nearly contamination-free for at least 140 min under ultra-high vacuum conditions ($p_{\mathrm{base}} = 2 \times 10^{-8}$ mbar). Beyond graphene, the presented method establishes a quantitative characterization platform for ultrathin materials, enabling studies of surface cleanliness, adsorption, implantation and surface interaction dynamics in such systems.

cond-mat.mtrl-sci↗

arXiv2026

Spot Profile Analysis Low Energy Electron Diffraction of Plasma-Enhanced Chemical Vapor Deposition Grown Epitaxial Few-Layer Graphene on Sapphire

We demonstrate the use of high-resolution spot-profile analysis low-energy electron diffraction to determine the mean grain size of plasma-enhanced chemical vapor deposition grown few-layer graphene on sapphire (Al$_2$O$_3$). The diffraction patterns exhibit broadened graphene spots, pronounced diffuse scattering, and azimuthally extended features, indicating finite crystallite size and rotational disorder. By analyzing the finite-size broadening of the specular (00) spot with an Airy-type diffraction profile, we determine a mean grain diameter of 3.7$\,$nm for the as-grown graphene layer. Post-growth annealing under ultrahigh-vacuum conditions increases the mean grain size to about 5.7$\,$nm and 6.8$\,$nm, respectively. These results establish SPA-LEED as a sensitive reciprocal-space method for quantifying the structural coherence of directly grown graphene on insulating substrates.

cond-mat.mtrl-sci↗

arXiv2026

Rainbow Scattering from Graphene

We report the experimental observation of atomic rainbow scattering of 40 keV Xe$^+$ ions transmitted through self-supporting single-layer graphene using time-of-flight medium energy ion scattering. Supported by molecular dynamics and binary collision approximation simulations, we show that the rainbow pattern of graphene consists of a small hexagonal inner rainbow, arising from projectiles with characteristic trajectories interacting with multiple carbon atoms, and a larger circular outer rainbow, arising from close binary collisions between projectiles and individual carbon atoms.

cond-mat.mtrl-sci↗

arXiv2025

Mechanism of Oleic Acid-Mediated Sulfur Vacancy Healing in monolayer WS$_2$

We uncover the mechanism behind the enhancement of photoluminescence yield in monolayer WS$_2$ through oleic acid treatment, a promising scalable strategy for defect healing. By inducing sulfur vacancies through thermal treatment and monitoring the changes in photoluminescence yield and emission spectra, we demonstrate that oleic acid heals the sulfur vacancy by providing substitutional oxygen. Using density functional theory calculations, we provide insight into the underlying mechanism governing the oleic acid-mediated sulfur vacancy healing process. Our findings suggest that effective defect passivation by oxygen doping can be achieved through chemical treatment, opening a pathway for oxygen doping in transition metal dichalcogenides. However, we also highlight the limitations of chemical treatment, which may only lead to small increases in photoluminescence yield beyond a certain point.

cond-mat.mtrl-sci↗

arXiv2024

Ultrafast Charge Transfer Dynamics at the MoS$_2$/Au Interface Observed via Optical Spectroscopy under Ambient Conditions

To take advantage of the exceptional properties of atomically thin transition metal dichalcogenides (TMDC) for advanced devices and catalysts, integration with metallic surfaces is an efficacious approach for facilitating charge carrier injection and extraction from TMDC monolayers. Light-matter interactions predominantly occur at the K point in TMDC monolayers, making the charge carrier dynamics at this point essential for their optimal performance. However, direct access to and comprehensive understanding of the charge carrier dynamics at the K point of TMDC monolayer on a metal substrate remains challenging. In this study, we employed azimuth- and polarization-dependent final-state sum frequency generation (FS-SFG) spectroscopy to investigate the ultrafast dynamics of charge transfer at the K point of a MoS$_2$ monolayer interfaced with an Au substrate. We observed an ultrafast injection (sub-20 fs) of photoexcited hot electrons from the Au substrate to the conduction band minimum (CBM) of the MoS$_2$ monolayer. Subsequently, driven by an internal electric field induced by charge redistribution, injected hot electrons in MoS$_2$ experience a relaxation and fast return ($\sim2$ ps) from the CBM and a trap state mediated slow return ($\sim60$ ps) process. The direct optical observation of the full electron dynamics at the K point of MoS$_2$ monolayer in ambient conditions provides valuable insights into the mechanisms of charge carrier transfer across the TMDC-metal interface, informing the design of advanced TMDC-based devices with enhanced charge transfer rates.

cond-mat.mes-hall↗

arXiv2024

Non-equilibrium dynamics of electron emission from cold and hot graphene under proton irradiation

Characteristic properties of secondary electrons emitted from irradiated two-dimensional materials arise from multi-length and time-scale relaxation processes that connect the initial non-equilibrium excited electron distribution with their eventual emission. To understand these processes, which are critical for using secondary electrons as high-resolution thermalization probes, we combine first-principles real-time electron dynamics with modern experiments. Our data for cold and hot proton-irradiated graphene shows signatures of kinetic and potential emission and generally good agreement for electron yields between experiment and theory. The duration of the emission pulse is about 1.5 femtoseconds, indicating high time resolution when used as a probe. Our newly developed method to predict kinetic energy spectra shows good agreement with electron and ion irradiation experiments and prior models. We find that lattice temperature significantly increases secondary electron emission, whereas electron temperature has a negligible effect.

cond-mat.mtrl-sci↗

arXiv2023

Isolating the Nonlinear Optical Response of a MoS$_2$ Monolayer under Extreme Screening of a Metal Substrate

Transition metal dichalcogenides (TMDCs) monolayers, as two-dimensional (2D) direct bandgap semiconductors, hold promise for advanced optoelectronic and photocatalytic devices. Interaction with three-dimensional (3D) metals, like Au, profoundly affects their optical properties, posing challenges in characterizing the monolayer's optical responses within the semiconductor-metal junction. In this study, using precise polarization-controlled final-state sum frequency generation (FS-SFG), we successfully isolated the optical responses of a MoS$_2$ monolayer from a MoS$_2$/Au junction. The resulting SFG spectra exhibit a linear lineshape, devoid of A or B exciton features, attributed to the strong dielectric screening and substrate induced doping. The linear lineshape illustrates the expected constant density of states (DOS) at the band edge of the 2D semiconductor, a feature often obscured by excitonic interactions in week-screening conditions such as in a free-standing monolayer. Extrapolation yields the onset of a direct quasiparticle bandgap of about $1.65\pm0.20$ eV, indicating a strong bandgap renormalization. This study not only enriches our understanding of the optical responses of a 2D semiconductor in extreme screening conditions but also provides a critical reference for advancing 2D semiconductor-based photocatalytic applications.

cond-mat.mes-hall↗

arXiv2023

Manipulation of the electrical and memory properties of MoS$_2$ field-effect transistors by highly charged ion irradiation

Field-effect transistors based on molybdenum disulfide (MoS$_2$) exhibit a hysteresis in their transfer characteristics, which can be utilized to realize 2D memory devices. This hysteresis has been attributed to charge trapping due to adsorbates, or defects either in the MoS$_2$ lattice or in the underlying substrate. We fabricated MoS$_2$ field-effect transistors on SiO$_2$/Si substrates, irradiated these devices with Xe$^{30+}$ ions at a kinetic energy of 180 keV to deliberately introduce defects and studied the resulting changes of their electrical and hysteretic properties. We find clear influences of the irradiation: While the charge carrier mobility decreases linearly with increasing ion fluence (up to only 20% of its initial value) the conductivity actually increases again after an initial drop of around two orders of magnitude, likely due to the occurence of hopping transport via localized states. We also find a significantly reduced $n$-doping ($\approx$ 10$^{12}$ per cm$^{2}$) and a well-developed hysteresis after the irradiation. The hysteresis height increases with increasing ion fluence and enables us to characterize the irradiated MoS$_2$ field-effect transistor as a memory device with remarkably longer relaxation times ($\approx$ minutes) compared to previous works.

physics.app-ph↗

arXiv2022

Velocity distributions of particles sputtered from supported 2D-MoS$_2$ during highly charged ion irradiation

The interaction of highly charged ions (HCI) with solids leads to particle sputtering, which can be used for defect-mediated engineering of the properties of the material. Ions can store energy in the form of kinetic and potential energy (sum of the ionization energies) and transfer it to the solid upon impact. The interaction and sputtering mechanisms depend significantly on the projectile energies. However, the relevance of various interaction mechanisms is unknown. Here we show that for slow HCI (5 keV) the interaction mechanisms leading to particle emission by electronic excitation and transferred kinetic energy are independent from each other, which is consistent with our atomistic simulations. We have irradiated substrate supported (Au, SiO$_2$) monolayers of MoS$_2$ with highly charged xenon ions (charge state: 17$+$ - 40$+$), extracted the emitted neutral, post-ionized Mo particles into a time-of-flight mass spectrometer and determined their velocity distributions. We find two main contributions, one at high velocities and a second one at lower velocities, and assign them to kinetic and potential effects respectively. Our data suggests that the dominant mechanism for potential sputtering is related to electron-phonon coupling, while non-thermal processes play no significant role. We anticipate that our work will be a starting point for further experiments and simulations to determine whether the different processes resulting from E$_{pot}$ and E$_{kin}$ can be separated or whether synergistic effects play a role.

cond-mat.mtrl-sci↗

arXiv2022

Out-of-plane longitudinal sound velocity in SnS$_2$ determined via broadband time-domain Brillouin scattering

Here we report time-resolved broadband transient reflectivity measurements performed in a single crystal of SnS$_2$. We made use of time-domain Brillouin scattering and a broadband probe to measure the out-of-plane longitudinal sound velocity $v_L$ = (2950 $\pm$ 100) m s$^{-1}$, in this semiconducting two-dimensional transition metal dichalcogenide. Our study illustrates the potential of this non-invasive all-optical pump-probe technique for the study of the elastic properties of transparent brittle materials and provides the value of the elastic constant $c_{33}$ = (39 $\pm$ 3) GPa.

cond-mat.mtrl-sci↗

arXiv2022

Growth of p-doped 2D-MoS$_2$ on metal oxides from spatial atomic layer deposition

In this letter we report on the synthesis of monolayers of MoS$_2$ via chemical vapor deposition directly on thin films of Al$_2$O$_3$ grown by spatial atomic layer deposition. The synthesized monolayers are characterized by atomic force microscopy as well as confocal Raman and photoluminescence spectroscopies. Our data reveals that the morphology and properties of the 2D material differ strongly depending on its position on the substrate. Close to the material source, we find individual flakes with an edge length of several hundred microns exhibiting a tensile strain of 0.3%, n-doping on the order of $n_e=0.2 \cdot 10^{13}$ cm$^{-2}$ and a dominant trion contribution to the photoluminescence signal. In contrast to this, we identify a mm-sized region downstream, that is made up from densely packed, small MoS$_2$ crystallites with an edge length of several microns down to the nanometer regime and a coverage of more than 70%. This nano-crystalline layer shows a significantly reduced strain of only <0.02%, photoluminescence emission at an energy of 1.86 eV with a reduced trion contribution, and appears to be p-doped with a carrier density of $n_h=0.1 \cdot 10^{13}$ cm$^{-2}$. The unusual p-type doping achieved here in a standard CVD process without substitutional doping, post-processing, or the use of additional chemicals may prove useful for applications.

cond-mat.mtrl-sci↗

arXiv2022

Mass transport via in-plane nanopores in graphene oxide membranes

Angstrom confined solvents in two-dimensional laminates travel through interlayer spacings, gaps between adjacent sheets, and via in plane pores. Among these, experimental access to investigate the mass transport through in plane pores is lacking. Here, we create these nanopores in graphene oxide membranes via ion irradiation with precise control over functional groups, pore size and pore density. Low ion induced pore densities result in mild reduction and increased water permeation for the membranes. Higher pore densities lead to pronounced reduction and complete blockage of pure water however allows permeation of ethanol water mixture due to weakening of hydrogen network. We confirm with simulations, that the attraction of the solvents towards the pores with functional groups and disruption of the angstrom confined hydrogen network is crucial to allow in plane pore transport.

cond-mat.mtrl-sci↗

arXiv2021

Lifetime of Excitons in Janus Monolayer MoSSe Prepared from Exfoliated MoSe_2

Janus monolayer transition metal dichalcogenides, where one of the two chalcogen layers is substituted with a different kind of chalcogen atoms, are pushing the properties of two dimensional materials into new territories. Yet only little is known about this new kind of material class, mainly due to the challenging synthesis. In this work we propose a method to prepare high quality Janus MoSSe monolayers from as-exfoliated MoSe2 by thermal sulfurization. With this we aim to pave a way for more exotic Janus monolayers, which have been out of the experimental reach thus far. The synthesized MoSSe is diligently characterized by room- and low-temperature Raman and photoluminescence spectroscopy, atomic force microscopy correlated with Raman mappings, and time-correlated single-photon counting. The latter providing new information on the lifetime of excitons in Janus MoSSe monolayers. In addition, we report an enhanced trion formation at low temperatures and a relatively high excitonic transition energy that is indicative of less defect states and strain, and therefore a high sample quality.

cond-mat.mtrl-sci↗

arXiv2021

Memory effects in black phosphorus field effect transistors

We report the fabrication and the electrical characterization of back-gated field effect transistors with black phosphorus channel. We show that the hysteresis of the transfer characteristic, due to intrinsic defects, can be exploited to realize non-volatile memories. We demonstrate that gate voltage pulses allow to trap and store charge inside the defect states, which enable memory devices with endurance over 200 cycles and retention longer than 30 minutes. We show that the use of a protective poly (methyl methacrylate) layer, positioned on top of the black phosphorus channel, does not affect the electrical properties of the device but avoids the degradation caused by the exposure to air.

cond-mat.mes-hall↗

arXiv2020

Gate-controlled field emission current from MoS$_2$ nanosheets

Monolayer molybdenum disulfide (MoS$_2$) nanosheets, obtained via chemical vapor deposition onto SiO$_2$/Si substrates, are exploited to fabricate field-effect transistors with n-type conduction, high on/off ratio, steep subthreshold slope and good mobility. The transistor channel conductance increases with the reducing air pressure due to oxygen and water desorption. Local field emission measurements from the edges of the MoS$_2$ nanosheets are performed in high vacuum using a tip-shaped anode. It is demonstrated that the voltage applied to the Si substrate back-gate modulates the field emission current. Such a finding, that we attribute to gate-bias lowering of the MoS$_2$ electron affinity, enables a new field-effect transistor based on field emission.

physics.app-ph↗

arXiv2020

Mechanisms of surface nanostructuring of Al2O3 and MgO by grazing incidence irradiation with swift heavy ions

We experimentally discovered that Al2O3 and MgO exhibit well-pronounced nanometric modifications on the surfaces when irradiated under grazing incidence with 23 MeV I beam, in contrast to normal incidence irradiation with the same ion beam when no damage was found. Moreover, ions in these two materials produce notably different structures: grooves surrounded with nanohillocks on MgO surfaces vs. smoother, roll-like discontinuous structures on the surfaces of Al2O3. To explain these results, detailed numerical simulations were performed. We identified that a presence of the surface inhibits recrystallization process, thereby preventing transient tracks from recovery, and thus forming observable nanopatterns. Furthermore, a difference in the viscosities in molten states in Al2O3 vs. MgO explains the differences in the created nanostructures. Our results thus provide a deeper understanding of the fundamental processes of surface nanostructuring, potentially allowing for controlled production of periodic surface nanopatterns.

cond-mat.mtrl-sci↗

arXiv2020

Graphene Effusion-based Gas Sensor

Porous, atomically thin graphene membranes have interesting properties for filtration and sieving applications because they can accommodate small pore sizes, while maintaining high permeability. These membranes are therefore receiving much attention for novel gas and water purification applications. Here we show that the atomic thickness and high resonance frequency of porous graphene membranes enables an effusion based gas sensing method that distinguishes gases based on their molecular mass. Graphene membranes are used to pump gases through nanopores using optothermal forces. By monitoring the time delay between the actuation force and the membrane mechanical motion, the permeation time-constants of various gases are shown to be significantly different. The measured linear relation between the effusion time constant and the square root of the molecular mass provides a method for sensing gases based on their molecular mass. The presented microscopic effusion based gas sensor can provide a small, low-power alternative for large, high-power, mass-spectrometry and optical spectrometry based gas sensing methods.

physics.app-ph↗