SearcharxivSearch

arXiv subjects

Gero Storeck

Publications and source records attributed to Gero Storeck.

4 recordsLinked to original sources

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

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

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

Coherent control of a structural phase transition in a solid-state surface system

The desire to exert active optical control over matter is a unifying theme across multiple scientific disciplines, as exemplified by all-optical magnetic switching, light-induced metastable or exotic phases of solids and the coherent control of chemical reactions. Typically, these approaches dynamically steer a system towards states or reaction products far from equilibrium. In solids, metal-insulator transitions are an important target for optical manipulation, offering dramatic and ultrafast changes of the electronic and lattice properties. In this context, essential questions concern the role of coherence in the efficiencies and thresholds of such transitions. Here, we demonstrate coherent vibrational control over a metal-insulator structural phase transition in a quasi-one-dimensional solid-state surface system. An optical double-pulse excitation scheme is used to drive the system from the insulating to a metastable metallic state, and the corresponding structural changes are monitored by ultrafast low-energy electron diffraction. We observe strong oscillations in the switching efficiency as a function of the double-pulse delay, revealing the importance of vibrational coherence in two key structural modes governing the transition on a femtosecond timescale. This mode-selective coherent control of solids and surfaces could open new routes to switching chemical and physical functionalities, facilitated by metastable and non-equilibrium states.

cond-mat.str-el