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Sascha Schäfer

Publications and source records attributed to Sascha Schäfer.

At least 19 recordsLinked to original sources

Floquet density response in laser-assisted fast-electron scattering from solids

We extend the Bethe--Floquet formalism of Joachain and coworkers, originally developed for laser-assisted electron--atom collisions, to inelastic scattering of fast electrons from a many-body condensed-matter target in a time-periodic light field. At first order in the projectile--target interaction, the general Floquet--Fourier cross section separates into exact laser-dressed projectile kernels and a matrix-valued Floquet density response of the target. For spatially structured or translationally non-invariant systems, the latter is the bi-momentum Floquet structure factor; its momentum diagonal defines the Floquet generalization of the dynamic structure factor, constrained by Hermiticity, positivity, and sum rules. As a controlled realization of the general projectile kernel, an eikonal--Volkov approximation for slowly varying inhomogeneous fields yields a finite-momentum-resolution convolution of the target response. In the homogeneous-field dipole limit, the projectile kernel reduces to Bessel-function sidebands and the cross section takes the familiar Bethe--Floquet form. The Floquet density correlator separates exactly into the outer product of the pump-induced coherent mean density and connected fluctuations. In the straight-trajectory nonrecoil limit, the coherent, target-elastic sector defines the weak-coupling PINEM amplitude; repeated coherent insertions generate the PINEM Bessel ladder, with an explicit no-double-counting prescription for combining this channel with connected losses. As worked examples, we evaluate the connected, target-changing cross section analytically for a metal in the Drude and diffusive limits, recovering Bessel-weighted plasmon-loss and diffusive combs, and for a driven two-level model that exhibits off-diagonal Floquet coherences through Bessel-channel interference.

cond-mat.mtrl-sci↗

Vibrational high-harmonics and period-doubling bifurcation probed by time-resolved electron diffraction

Nanoscale mechanical oscillators exhibit a plethora of nonlinear phenomena with promising applications for the sensing and clocking of processes down to atomic length scales. Oscillator dynamics are typically probed by electrical or optical means, providing only limited access to the spatial profile of the oscillator motion. Here, we introduce event-based convergent beam electron diffraction for the spatio-temporal mapping of nanoscale mechanical resonators in ultrafast transmission electron microscopy. Employing an optically driven silicon membrane resonator at various driving strengths, we gain access to nonlinear processes with increasing complexity, ranging from a simple Duffing behavior to nonlinear multimode coupling and period-doubling bifurcations. The time-resolved diffraction probing approach supports a spatial resolution down to a few nanometers and a temporal resolution of 5 ns and provides quantitative information on the local membrane bending. Because the diffraction signal responds to local displacement gradients, which become more pronounced as resonators shrink, this approach offers a route toward probing nonlinear nanomechanics at the atomic scale.

physics.optics↗

Visualizing Transient Ordering Phenomena in Dense Nanoparticle Clouds

The dynamics of nanoparticles within nanoscale liquid environments exhibit a range of complex phenomena driven by the interplay of processes at varying length scales. While these dynamics have profound technical implications, such as in nanoscale catalytic kinetics, ion-transport pathways in energy storage, and macromolecular crowding in biological systems, real-space imaging of dense, confined nanoparticle assemblies remains a significant challenge. Here, we present a liquid-phase transmission electron microscopy approach in which dense clouds of gold nanoparticles are formed within microfluidic channels, rendering the particle ensemble visible in bright-field electron imaging. This strategy enables direct imaging of different density-dependent particle ordering phenomena, including a local structuring of the colloidal liquid in nanoscale spaces, disordered dynamic clouds at high nanoparticle densities and the reversible formation of superlattice structures. Our results provide a unique window into the complex processes of colloidal self-organization at the nanoscale.

cond-mat.soft↗

All-optical stochastic switching of magnetization textures in Fe$_3$Sn$_2$

The all-optical control of magnetization at room temperature broadens the scope of applications of spin degrees-of-freedom in data storage, spintronics, and quantum computing. Topological magnetic spin structures, such as skyrmions, are of particular interest due to their particle-like properties, small size and inherent stability. Controlling skyrmion states without strong magnetic fields or large current densities would create new possibilities for their application. In this work, we utilize femtosecond optical pulses to alter the helicity of the spin configuration in dipolar skyrmions formed in the kagome magnet Fe$_3$Sn$_2$ in the absence of an external magnetic field and at room temperature. In situ Lorentz transmission electron microscopy is used to visualize the stochastic, light-induced switching process of chiral Néel caps, while the internal Bloch component of the dipolar skyrmions remain unchanged. In addition to this switching process, we observe the interconversion between type I skyrmionic and type II bubble configurations depending on the external magnetic field and illumination conditions. To corroborate the spin states and the light-induced magnetization dynamics, micromagnetic modelling and simulations of the resulting electron phase shift maps are conducted to elucidate the spin rearrangement induced by individual femtosecond optical pulses.

physics.optics↗

Laser-driven cold-field emission source for ultrafast transmission electron microscopy

Ultrafast transmission electron microscopy (UTEM) has emerged as a versatile technique for the time-resolved imaging of nanoscale dynamics on timescales down to few-hundred attoseconds but the temporal and spatial resolutions are still limited by the coherence properties of pulsed electron sources. Here, we report the development of a novel laser-driven linear cold-field electron emitter integrated in a state-of-the-art UTEM system. Illuminating the sharp tungsten emitter tip with a UV light pulse generates ultrashort femtosecond electron pulses of 220 fs pulse duration, with energy widths as low as 360 meV. The photoelectron emitter demonstrates exceptional spatial coherence, achieving focal spot sizes down to 2 $\mathring {\mathrm A}$ and a peak normalized brightness exceeding 6.7 $\times 10^{13}$ A/m$^2$sr. With an order-of-magnitude improvement compared to previously employed laser-driven Schottky field emitters, the present development opens up the field of ultrafast atomic-scale electron probing.

physics.ins-det↗

Visualizing Standing Light Waves in Continuous-Beam Transmission Electron Microscopy

The phase-resolved imaging of confined light fields by homodyne detection is a cornerstone of metrology in nano-optics and photonics, but its application in electron microscopy has been limited so far. Here, we report the mapping of optical modes in a waveguide structure by illumination with femtosecond light pulses in a continuous-beam transmission electron microscope. Multi-photon photoemission results in a remanent charging pattern which we image by Lorentz microscopy. The resulting image contrast is linked to the intensity distribution of the standing light wave and quantitatively described within an analytical model. The robustness of the approach is showcased in a wider parameter range and more complex sample geometries including micro- and nanostructures. We discuss further applications of light-interference-based charging for electron microscopy with in-situ optical excitation, laying the foundation for advanced measurement schemes for the phase-resolved imaging of propagating light fields.

cond-mat.mes-hall↗

Spectrally resolved free electron-light coupling strength in a transition metal dichalcogenide

Recent advancements in electron microscopy have introduced innovative techniques enabling the inelastic interaction of fast electrons with tightly confined and intense light fields. These techniques, commonly summarized under the term photon-induced nearfield electron microscopy now offer unprecedented capabilities for a precise mapping of the characteristics of optical near-fields with remarkable spatial resolution but their spectral resolution were only scarcely investigated. In this study, we employ a strongly chirped and temporally broadband light pulse to investigate the interaction between free electrons and light at the edge of a MoS2 thin film. Our approach unveils the details of electron-light coupling, revealing a pronounced dependence of the coupling strength on both the position and photon energy. Employing numerical simulations of a simplified model system we identify these modulations to be caused by optical interferences between the incident and reflected field as well as an optical mode guided within the transition metal dichalcogenide film.

cond-mat.mes-hall↗

Inelastic electron-light scattering at dielectric thin films

In a recently developed methodology termed photon induced near-field electron microscopy (PINEM), the inelastic scattering of electrons off illuminated nanostructures provides direct experimental access to the structure of optical near-field modes and their population. Whereas the inelastic scattering probability can be quantitatively linked to the near field distribution, analytical results for simple light scattering geometries are scarce. Here we derive a fully analytical expression for the coupling strength between free electrons and optical near-fields in planar geometries representing dielectric thin films. Contributions to the overall coupling from the electric field above, below and within the sample are analyzed in detail. By carefully choosing the relative angles between electron beam, light and thin film and by accounting for a broad spectrum of photon energies, we demonstrate that one can imprint optical material properties like the reflectivity onto the electron energy distribution.

cond-mat.mes-hall↗

Electron Imaging of Nanoscale Charge Distributions Induced by Femtosecond Light Pulses

Surface charging is a phenomenon ubiquitously observable in in-situ transmission electron microscopy of non-conducting specimens as a result of electron beam/sample interactions or optical stimuli and often limits the achievable image stability and spatial or spectral resolution. Here, we report on the electron-optical imaging of surface charging on a nanostructured surface following femtosecond-multiphoton photoemission. By quantitatively extracting the light-induced electrostatic potential and studying the charging dynamics on the relevant timescales, we gain insights into the details of the multi-photon photoemission process in the presence of a background field. We study the interaction of the charge distribution with the high-energy electron beam and secondary electrons and propose a simple model to describe the interplay of electron- and light-induced processes. In addition, we demonstrate how to mitigate sample charging by simultaneous optical illumination of the sample.

cond-mat.mes-hall↗

Improving the temporal resolution of event-based electron detectors using neural network cluster analysis

Novel event-based electron detector platforms provide an avenue to extend the temporal resolution of electron microscopy into the ultrafast domain. Here, we characterize the timing accuracy of a detector based on a TimePix3 architecture using femtosecond electron pulse trains as a reference. With a large dataset of event clusters triggered by individual incident electrons, a neural network is trained to predict the electron arrival time. Corrected timings of event clusters show a temporal resolution of 2 ns, a 1.6-fold improvement over cluster-averaged timings. This method is applicable to other fast electron detectors down to sub-nanosecond temporal resolutions, offering a promising solution to enhance the precision of electron timing for various electron microscopy applications.

physics.ins-det↗

Coupling broadband terahertz dipoles to microscale resonators

Spintronic emitters are a unique class of terahertz (THz) sources due to their quasi-two-dimensional geometry and thereby their capability to couple to resonator near fields. Global excitation of the emitters often obstructs the intricate details of the coupling mechanisms between local THz dipoles and the individual modes of resonator structures. Here, we demonstrate the spatial mapping of the coupling strength between a local terahertz source on a spintronic emitter and far-field light mediated by a structured metallic environment. For a bow-tie geometry, experimental results are reproduced by a numerical model providing insights into the microscopic coupling mechanisms. The broad applicability of the technique is showcased by extracting the THz mode structure in split-ring resonator metasurfaces and linear arrays. With these developments, planar THz sources with tailored spectral and angular emission profiles are accessible.

physics.optics↗

Broadband coupling of fast electrons to high-Q whispering-gallery mode resonators

Transmission electron microscopy is an excellent experimental tool to study the interaction of free electrons with nanoscale light fields. However, up to now, applying electron microscopy to quantum optical investigations was hampered by the lack of experimental platforms which allow a strong coupling between fast electrons and high-quality resonators. Here, as a first step, we demonstrate the broad-band excitation of optical whispering-gallery modes in silica microresonators by fast electrons. In the emitted coherent cathodoluminescence spectrum, a comb of equidistant peaks is observed, resulting in cavity quality factors larger than 700. These results enable the study of quantum optical phenomena in electron microscopy with potential applications in quantum electron-light metrology.

physics.optics↗

Dynamics and Structure of Monolayer Polymer Crystallites on Graphene

Graphene-based nanostructured systems and van-der-Waals heterostructures comprise a material class of growing technological and scientific importance. Joining materials with vastly different properties, polymer-graphene heterosystems promise diverse applications in surface- and nanotechnology, including photovoltaics or nanotribology. Fundamentally, molecular adsorbates are prototypical systems to study confinement-induced phase transitions exhibiting intricate dynamics, which require a comprehensive understanding of the dynamical and static properties on molecular time and length scales. Here, we investigate the dynamics and the structure of a single polyethylene chain on free-standing graphene by means of molecular dynamics simulations. In equilibrium, the adsorbed polymer is orientationally linked to the graphene as two-dimensional folded-chain crystallites or, at elevated temperatures, as a floating solid. The associated superstructure can be reversibly melted on a picosecond time scale upon quasi-instantaneous substrate heating, involving ultrafast heterogeneous melting via a transient floating phase. Our findings elucidate time-resolved molecular-scale ordering and disordering phenomena in individual polymers interacting with solids, yielding complementary information to collective friction and viscosity, and linking to recent experimental observables from ultrafast electron diffraction. We anticipate that the approach will help in resolving non-equilibrium phenomena of hybrid polymeric systems over a broad range of time and length scales.

cond-mat.soft↗

Structural dynamics probed by high-coherence electron pulses

Ultrafast measurement technology provides essential contributions to our microscopic understanding of the properties and functions of solids and nanostructures. Atomic-scale vistas with ever-growing spatial and temporal resolution are offered by methods based on short pulses of x-rays and electrons. Time-resolved electron diffraction and microscopy are among the most powerful approaches to investigate non-equilibrium structural dynamics in excited matter. In this article, we discuss recent advances in ultrafast electron imaging enabled by significant improvements in the coherence of pulsed electron beams. Specifically, we review the development and first application of Ultrafast Low-Energy Electron Diffraction (ULEED) for the study of structural dynamics at surfaces, and discuss novel opportunities of Ultrafast Transmission Electron Microscopy (UTEM) facilitated by laser-triggered field emission sources. These and further developments will render coherent electron beams an essential component in the future of ultrafast nanoscale imaging.

cond-mat.mes-hall↗

High-purity free-electron momentum states prepared by three-dimensional optical phase modulation

We demonstrate the quantized transfer of photon energy and transverse momentum to a high-coherence electron beam. In an ultrafast transmission electron microscope, a three-dimensional phase modulation of the electron wavefunction is induced by transmitting the beam through a laser-illuminated thin graphite sheet. This all-optical free-electron phase space control results in high-purity superpositions of linear momentum states, providing an elementary component for optically programmable electron phase plates and beam splitters.

physics.optics↗

Few-nm tracking of magnetic vortex orbits and their decay with ultrafast Lorentz microscopy

Transmission electron microscopy is one of the most powerful techniques to characterize nanoscale magnetic structures. In light of the importance of fast control schemes of magnetic states, time-resolved microscopy techniques are highly sought after in fundamental and applied research. Here, we implement time-resolved Lorentz imaging in combination with synchronous radio-frequency excitation using an ultrafast transmission electron microscope. As a model system, we examine the current-driven gyration of a vortex core in a 2 $\mathrmμ$m-sized magnetic nanoisland. We record the trajectory of the vortex core for continuous-wave excitation, achieving a localization precision of $\pm$2nm with few-minute integration times. Furthermore, by tracking the core position after rapidly switching off the current, we find a temporal hardening of the free oscillation frequency and an increasing orbital decay rate attributed to local disorder in the vortex potential.

cond-mat.mes-hall↗

Nanoscale mapping of ultrafast magnetization dynamics with femtosecond Lorentz microscopy

Novel time-resolved imaging techniques for the investigation of ultrafast nanoscale magnetization dynamics are indispensable for further developments in light-controlled magnetism. Here, we introduce femtosecond Lorentz microscopy, achieving a spatial resolution below 100 nm and a temporal resolution of 700 fs, which gives access to the transiently excited state of the spin system on femtosecond timescales and its subsequent relaxation dynamics. We demonstrate the capabilities of this technique by spatio-temporally mapping the light-induced demagnetization of a single magnetic vortex structure and quantitatively extracting the evolution of the magnetization field after optical excitation. Tunable electron imaging conditions allow for an optimization of spatial resolution or field sensitivity, enabling future investigations of ultrafast internal dynamics of magnetic topological defects on 10-nanometer length scales.

physics.optics↗

Nanoscale diffractive probing of strain dynamics in ultrafast transmission electron microscopy

The control of optically driven high-frequency strain waves in nanostructured systems is an essential ingredient for the further development of nanophononics. However, broadly applicable experimental means to quantitatively map such structural distortion on their intrinsic ultrafast time and nanometer length scales are still lacking. Here, we introduce ultrafast convergent beam electron diffraction (U-CBED) with a nanoscale probe beam for the quantitative retrieval of the time-dependent local distortion tensor. We demonstrate its capabilities by investigating the ultrafast acoustic deformations close to the edge of a single-crystalline graphite membrane. Tracking the structural distortion with a 28-nm/700-fs spatio-temporal resolution, we observe an acoustic membrane breathing mode with spatially modulated amplitude, governed by the optical near field structure at the membrane edge. Furthermore, an in-plane polarized acoustic shock wave is launched at the membrane edge, which triggers secondary acoustic shear waves with a pronounced spatio-temporal dependency. The experimental findings are compared to numerical acoustic wave simulations in the continuous medium limit, highlighting the importance of microscopic dissipation mechanisms and ballistic transport channels.

physics.ins-det↗