arXiv subjects

Claus Ropers

Publications and source records attributed to Claus Ropers.

At least 55 records · Page 3Linked to original sources

arXiv2020

Phase space manipulation of free-electron pulses from metal nanotips using combined THz near-fields and external biasing

We present a comprehensive experimental and numerical study of photoelectron streaking at metallic nanotips using single-cycle Terahertz (THz) transients and a static bias voltage as an external control parameter. Analyzing bias voltage dependent streaking spectrograms, we explore the THz-induced reshaping of photoelectron energy spectra, governed by the superimposed static field. Numerical simulations are employed to determine the local field strengths and spatial decay lengths of the field contributions, demonstrating electron trajectory control and the manipulation of the phase space distributions in confined fields with both dynamic and static components.

physics.optics↗

arXiv2020

Surface structure and stacking of the commensurate $\left(\sqrt{13}\times\sqrt{13}\right)$R13.9° charge density wave phase of 1T-TaS$_2$(0001)

By quantitative low-energy electron diffraction (LEED) we investigate the extensively studied commensurate charge density wave (CDW) phase of trigonal tantalum disulphide (1T-TaS$_2$), which develops at low temperatures with a $\left(\sqrt{13}\times\sqrt{13}\right)$R13.9° periodicity. A full-dynamical analysis of the energy dependence of diffraction spot intensities reveals the entire crystallographic surface structure, i.e. the detailed atomic positions within the outermost two trilayers consisting of 78 atoms as well as the CDW stacking. The analysis is based on an unusually large data set consisting of spectra for 128 inequivalent beams taken in the energy range 20-250 eV and an excellent fit quality expressed by a bestfit Pendry R-factor of R=0.110. The LEED intensity analysis reveals that the well-accepted model of star-of-David-shaped clusters of Ta atoms for the bulk structure also holds for the outermost two TaS$_2$ trilayers. Specifically, in both layers the clusters of Ta atoms contract laterally by up to 0.25 $Å$ and also slightly rotate within the superstructure cell, causing respective distortions as well as heavy bucklings (up to 0.23 $Å$) in the adjacent sulphur layers. Most importantly, our analysis finds that the CDWs of the 1$^{\text{st}}$ and 2$^{\text{nd}}$ trilayer are vertically aligned, while there is a lateral shift of two units of the basic hexagonal lattice (6.71 $Å$) between the 2$^{\text{nd}}$ and 3$^{\text{rd}}$ trilayer. The results may contribute to a better understanding of the intricate electronic structure of the reference compound 1T-TaS$_2$ and guide the way to the analysis of complex structures in similar quantum materials.

cond-mat.str-el↗

arXiv2020

Structure and Non-Equilibrium Heat-Transfer of a Physisorbed Molecular Layer on Graphene

The structure of a physisorbed sub-monolayer of 1,2-bis(4-pyridyl)ethylene (bpe) on epitaxial graphene is investigated by Low-Energy Electron Diffraction and Scanning Tunneling Microscopy. Additionally, non-equilibrium heat-transfer between bpe and the surface is studied by Ultrafast Low-Energy Electron Diffraction. Bpe arranges in an oblique unit cell which is not commensurate with the substrate. Six different rotational and/or mirror domains, in which the molecular unit cell is rotated by 28{\pm}0.1° with respect to the graphene surface, are identified. The molecules are weakly physisorbed, as evidenced by the fact that they readily desorb at room temperature. At liquid nitrogen temperature, however, the layers are stable and time-resolved experiments can be performed. The temperature changes of the molecules and the surface can be measured independently through the Debye-Waller factor of their individual diffraction features. Thus, the heat flow between bpe and the surface can be monitored on a picosecond timescale. The time-resolved measurements, in combination with model simulations, show the existence of three relevant thermal barriers between the different layers. The thermal boundary resistance between the molecular layer and graphene was found to be 2{\pm}1{\cdot}10-8 K m2 W-1.

cond-mat.mtrl-sci↗

arXiv2020

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↗

arXiv2020

Clocking plasmon nanofocusing by THz near-field streaking

We apply terahertz (THz) near-field streaking in a nanofocusing geometry to investigate plasmon polariton propagation on the shaft of a conical nanotip. By evaluating the delay between a streaking spectrogram for plasmon-induced photoemission with a measurement for direct apex excitation, we obtain an average plasmon group velocity, which is in agreement with numerical simulations. Combining plasmon-induced photoemission with THz near-field streaking facilitates extensive control over localized photoelectron sources for time-resolved imaging and diffraction.

physics.optics↗

arXiv2020

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↗

arXiv2020

Spontaneous and Stimulated Electron-Photon Interactions in Nanoscale Plasmonic Near Fields

We demonstrate spatially-resolved measurements of spontaneous and stimulated electron-photon interactions in nanoscale optical near fields using electron energy-loss spectroscopy (EELS), cathodoluminescence spectroscopy (CL), and photon-induced near-field electron microscopy (PINEM). Specifically, we study resonant surface plasmon modes that are tightly confined to the tip apexes of an Au nanostar, enabling a direct correlation of EELS, CL, and PINEM on the same physical structure at the nanometer length scale. Complemented by numerical electromagnetic boundary-element method calculations, we discuss the spontaneous and stimulated electron-photon interaction strength and spatial dependence of our EELS, CL and PINEM distributions. We demonstrate that in the limit of an isolated tip mode, spatial variations in the electron-near field coupling are fully determined by the modal electric field profile, irrespective of the spontaneous (in EELS and CL) or stimulated nature (in PINEM) of the process. Yet we show that coupling to the tip modes crucially depends on the incident electron energy with a maximum at a few keV, depending on the proximity of the interaction to the tip apex. Our results provide elementary insights into spontaneous and stimulated electron-light-matter interactions at the nanoscale that have key implications for research on (quantum) coherent optical phenomena in electron microscopy.

physics.optics↗

arXiv2020

Ultrafast nano-imaging of the order parameter in a structural phase transition

Understanding microscopic processes in materials and devices that can be switched by light requires experimental access to dynamics on nanometer length and femtosecond time scales. Here, we introduce ultrafast dark-field electron microscopy, tailored to map the order parameter across a structural phase transition. We track the evolution of charge-density wave domains in 1T-TaS2 after ultrashort laser excitation, elucidating relaxation pathways and domain wall dynamics. The unique benefits of selective contrast enhancement will inspire future beam shaping technology in ultrafast transmission electron microscopy.

cond-mat.mtrl-sci↗

arXiv2020

Structural Dynamics of incommensurate Charge-Density Waves tracked by Ultrafast Low-Energy Electron Diffraction

We study the non-equilibrium structural dynamics of the incommensurate and nearly-commensurate charge-density wave phases in 1T-TaS$_2$. Employing ultrafast low-energy electron diffraction (ULEED) with 1 ps temporal resolution, we investigate the ultrafast quench and recovery of the CDW-coupled periodic lattice distortion. Sequential structural relaxation processes are observed by tracking the intensities of main lattice as well as satellite diffraction peaks as well as the diffuse scattering background. Comparing distinct groups of diffraction peaks, we disentangle the ultrafast quench of the PLD amplitude from phonon-related reductions of the diffraction intensity. Fluence-dependent relaxation cycles reveal a long-lived partial suppression of the order parameter for up to 60 picoseconds, far outlasting the initial amplitude recovery and electron-phonon scattering times. This delayed return to a quasi-thermal level is controlled by lattice thermalization and coincides with the population of zone-center acoustic modes, as evidenced by a structured diffuse background. The long-lived non-equilibrium order parameter suppression suggests hot populations of CDW-coupled lattice modes. Finally, a broadening of the superlattice peaks is observed at high fluences, pointing to a nonlinear generation of phase fluctuations.

cond-mat.str-el↗

arXiv2020

Probing chirality with inelastic electron-light scattering

Circular dichroism spectroscopy is an essential technique for understanding molecular structure and magnetic materials, but spatial resolution is limited by the wavelength of light, and sensitivity sufficient for single-molecule spectroscopy is challenging. We demonstrate that electrons can efficiently measure the interaction between circularly polarized light and chiral materials with deeply sub-wavelength resolution. By scanning a nanometer-sized focused electron beam across an optically-excited chiral nanostructure and measuring the electron energy spectrum at each probe position, we produce a high-spatial-resolution map of near-field dichroism. This technique offers a nanoscale view of a fundamental symmetry and could be employed as "photon staining" to increase biomolecular material contrast in electron microscopy.

physics.optics↗

arXiv2020

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↗

arXiv2019

Nanoscale Nonlinear Spectroscopy with Electron Beams

We theoretically demonstrate the ability of electron beams to probe the nonlinear photonic response with nanometer spatial resolution, well beyond the capabilities of existing optical techniques. Although the interaction of electron beams with photonic modes is generally weak, the use of optical pumping produces stimulated electron-light interactions that can reach order-unity probabilities in photon-induded near field electron microscopy (PINEM). Here, we demonstrate that PINEM can locally and quantitatively probe the nonlinear optical response. Specifically, we predict a dependence of PINEM electron spectra on the sample nonlinearity that can reveal the second-harmonic (SH) response of optical materials with nanometer resolution, observed through asymmetries between electron energy losses and gains. We illustrate this concept by showing that PINEM spectra are sensitive to the SH near field of centrosymmetric structures and by finding substantial spectral asymmetries in geometries for which the linear interaction is reduced.

cond-mat.mes-hall↗

arXiv2019

Controlling free electrons with optical whispering-gallery modes

Free-electron beams serve as uniquely versatile probes of microscopic structure and composition, and have repeatedly revolutionized atomic-scale imaging, from solid-state physics to structural biology. Over the past decade, the manipulation and interaction of electrons with optical fields has seen significant progress, enabling novel imaging methods, schemes of near-field electron acceleration, and culminating in 4D microscopy techniques with both high temporal and spatial resolution. However, weak coupling strengths of electron beams to optical excitations are a standing issue for existing and emerging applications of optical free-electron control. Here, we demonstrate phase matched near-field coupling of a free-electron beam to optical whispering gallery modes of dielectric microresonators. The cavity-enhanced interaction with these optically excited modes imprints a strong phase modulation on co-propagating electrons, which leads to electron-energy sidebands up to hundreds of photon orders and a spectral broadening of 700 eV. Mapping the near-field interaction with ultrashort electron pulses in space and time, we trace the temporal ring-down of the microresonator following a femtosecond excitation and observe the cavity's resonant spectral response. Resonantly enhancing the coupling of electrons and light via optical cavities, with efficient injection and extraction, can open up novel applications such as continuous-wave acceleration, attosecond structuring, and real-time all-optical electron detection.

physics.optics↗

arXiv2019

Nonlinear Spectroscopy and All-Optical Switching of Femtosecond Soliton Molecules

The emergence of confined structures and pattern formation are exceptional manifestations of concurring nonlinear interactions found in a variety of physical, chemical and biological systems[1]. Optical solitons are a hallmark of extreme spatial or temporal confinement enabled by a variety of nonlinearities. Such particle-like structures can assemble in complex stable arrangements, forming "soliton molecules"[2,3]. Recent works revealed oscillatory internal motions of these bound states, akin to molecular vibrations[4-8]. These observations beg the question as to how far the "molecular" analogy reaches, whether further concepts from molecular spectroscopy apply in this scenario, and if such intra-molecular dynamics can be externally driven or manipulated. Here, we probe and control such ultrashort bound-states in an optical oscillator, utilizing real-time spectroscopy and time-dependent external perturbations. We introduce two-dimensional spectroscopy of the linear and nonlinear bound-state response and resolve anharmonicities in the soliton interaction leading to overtone and sub-harmonic generation. Employing a non-perturbative interaction, we demonstrate all-optical switching between distinct states with different binding separation, opening up novel schemes of ultrafast spectroscopy, optical logic operations and all-optical memory.

physics.optics↗

arXiv2019

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↗

arXiv2019

Density Matrix Reconstructions in Ultrafast Transmission Electron Microscopy: Uniqueness, Stability, and Convergence Rates

In the recent paper [17] the first experimental determination of the density matrix of a free electron beam has been reported. The employed method leads to a linear inverse problem with a positive semidefinite operator as unknown. The purpose of this paper is to complement the experimental and algorithmic results in the work mentioned above by a mathematical analysis of the inverse problem concerning uniqueness, stability, and rates of convergence under different types of a-priori information.

math.AP↗

arXiv2017

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↗

arXiv2017

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↗