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C. Gutt

Publications and source records attributed to C. Gutt.

11 recordsLinked to original sources

Transient laser-induced periodic surface structures revealed by time-resolved EUV diffuse scattering

The formation of permanent laser-induced periodic surface structures (LIPSS) on solid surfaces under impulsive laser irradiation above the damage threshold has been subject of extensive research. We demonstrate the formation of transient surface displacement patterns under femtosecond laser irradiation at fluences well below this threshold. Time-resolved extreme ultraviolet scattering measurements reveal distinct reciprocal-space features similar to those observed for permanent LIPSS but dissipating on the hundreds-of-picoseconds time scale. We show that the transient surface displacement patterns responsible for these features are produced via thermal expansion by the spatial modulation of absorbed laser intensity caused by scattering of the laser radiation by surface roughness and present a model accounting for the experimental observations. We suggest that our experiment revealed a universal phenomenon that will be observed on any strongly absorbing material under ultrafast laser irradiation.

physics.optics

Time-domain extreme ultraviolet diffuse scattering spectroscopy of nanoscale surface phonons

We report the observation of dynamic fringe patterns in the diffuse scattering of extreme ultraviolet light from surfaces, following femtosecond optical excitation. At each point on the detector, the diffuse scattering intensity exhibits oscillations at well-defined frequencies that correspond to surface phonons with wave vectors determined by the scattering geometry, indicating that the optical excitation generates coherent surface phonons propagating in all directions and spanning a wavelength range from 60 to 300 nm. This phenomenon is observed on a variety of samples, including single-layer and multilayer metal films, as well as bulk semiconductors. The measured surface phonon dispersions show good agreement with theoretical calculations. By comparing signal amplitudes from samples with different surface morphologies, we find that the excitation mechanism is linked to the natural surface roughness of the samples. However, the signal is still detectable on extremely smooth surfaces with sub-nanometer roughness. Our findings demonstrate a simple and effective method for optically exciting coherent surface phonons with nanoscale wavelengths on a wide range of solid samples and establish a foundation for surface phonon spectroscopy in a wave vector range well beyond the limit of conventional surface Brillouin scattering.

cond-mat.mtrl-sci

Gelation dynamics upon pressure-induced liquid-liquid phase separation in a water-lysozyme solution

Employing X-ray photon correlation spectroscopy we measure the kinetics and dynamics of a pressure-induced liquid-liquid phase separation (LLPS) in a water-lysozyme solution. Scattering invariants and kinetic information provide evidence that the system reaches the phase boundary upon pressure-induced LLPS with no sign of arrest. The coarsening slows down with increasing quench depths. The $g_2$-functions display a two-step decay with a gradually increasing non-ergodicity parameter typical for gelation. We observe fast superdiffusive ($\gamma \geq 3/2$) and slow subdiffusive ($\gamma < 0.6$) motion associated with fast viscoelastic fluctuations of the network and a slow viscous coarsening process, respectively. The dynamics age linear with time $\tau \propto t_\mathrm{w}$ and we observe the onset of viscoelastic relaxation for deeper quenches. Our results suggest that the protein solution gels upon reaching the phase boundary.

cond-mat.soft

Automated matching of two-time X-ray photon correlation maps from protein dynamics with Cahn-Hilliard type simulations using autoencoder networks

We use machine learning methods for an automated classification of experimental XPCS two-time correlation functions from an arrested liquid-liquid phase separation of a protein solution. We couple simulations based on the Cahn-Hilliard equation with a glass transition scenario and classify the measured correlation maps automatically according to quench depth and critical concentration at a glass/gel transition. We introduce routines and methodologies using an autoencoder network and a differential evolution based algorithm for classification of the measured correlation functions. The here presented method is a first step towards handling large amounts of dynamic data measured at high brilliance synchrotron and X-ray free-electron laser sources facilitating fast comparison to phase field models of phase separation.

cond-mat.soft

Nanoscale Rigidity in Cross-Linked Micelle Networks Revealed by XPCS Nanorheology

Solutions of wormlike micelles can form cross-linked networks on microscopic length scales. The unique mechanical properties of these complex fluids are driven by the interplay between the network structure and dynamics which are investigated by plate-plate rheometry and X-ray photon correlation spectroscopy~(XPCS) nanorheology. Intensity auto-correlation functions of tracer nanoparticles~(NPs) dispersed in micelle solutions were recorded which captured both the slow structural network relaxation and the short-time dynamics of NPs trapped in the network. The results are indicative of a resonance-like dynamic behavior of the network on the nanoscale that develops as a consequence of the intrinsic short-range rigidity of individual micelle chains.

cond-mat.soft

Nanoscale transient magnetization gratings excited and probed by femtosecond extreme ultraviolet pulses

We utilize coherent femtosecond extreme ultraviolet (EUV) pulses derived from a free electron laser (FEL) to generate transient periodic magnetization patterns with periods as short as 44 nm. Combining spatially periodic excitation with resonant probing at the dichroic M-edge of cobalt allows us to create and probe transient gratings of electronic and magnetic excitations in a CoGd alloy. In a demagnetized sample, we observe an electronic excitation with 50 fs rise time close to the FEL pulse duration and ~0.5 ps decay time within the range for the electron-phonon relaxation in metals. When the experiment is performed on a sample magnetized to saturation in an external field, we observe a magnetization grating, which appears on a sub-picosecond time scale as the sample is demagnetized at the maxima of the EUV intensity and then decays on the time scale of tens of picoseconds via thermal diffusion. The described approach opens prospects for studying dynamics of ultrafast magnetic phenomena on nanometer length scales.

cond-mat.mes-hall

Wave vector dependence of the dynamics in supercooled metallic liquids

We present a detailed investigation of the wave vector dependence of collective atomic motion in Au49Cu26.9Si16.3Ag5.5Pd2.3 and Pd42.5Cu27Ni9.5P21 supercooled liquids close to the glass transition temperature. Using x-ray photon correlation spectroscopy in a precedent uncovered spatial range of only few interatomic distances, we show that the microscopic structural relaxation process follows in phase the structure with a marked slowing down at the main average inter-particle distance. This behavior is accompanied by dramatic changes in the shape of the intermediate scattering functions which suggest the presence of large dynamical heterogeneities at length-scales corresponding to few particle diameters. A ballistic-like mechanism of particle motion seems to govern the structural relaxation of the two systems in the highly viscous phase, likely associated to hopping of caged particles in agreement with theoretical studies.

cond-mat.soft

Intermittent dynamics of antiferromagnetic phase in inhomogeneous iron-based chalcogenide superconductor

Coexistence of phases, characterized by different electronic degrees of freedom, commonly occurs in layered superconductors. Among them, alkaline intercalated chalcogenides are model systems showing microscale coexistence of paramagnetic (PAR) and antiferromagnetic (AFM) phases, however, temporal behavior of different phases is still unknown. Here, we report the first visualization of the atomic motion in the granular phase of K$_{x}$Fe$_{2-y}$Se$_2$ using X-ray photon correlation spectroscopy. Unlike the PAR phase, the AFM texture reveals an intermittent dynamics with avalanches as in martensites. When cooled down across the superconducting transition temperature T$_c$, the AFM phase goes through an anomalous slowing behavior suggesting a direct relationship between the atomic motions in the AFM phase and the superconductivity. In addition of providing a compelling evidence of avalanche-like dynamics in a layered superconductor, the results provide a basis for new theoretical models to describe quantum states in inhomogeneous solids.

cond-mat.supr-con

Nanoscale femtosecond imaging of transient hot solid density plasmas with elemental and charge state sensitivity using resonant coherent diffraction

Here we propose to exploit the low energy bandwidth, small wavelength and penetration power of ultrashort pulses from XFELs for resonant Small Angle Scattering (SAXS) on plasma structures in laser excited plasmas. Small angle scattering allows to detect nanoscale density fluctuations in forward scattering direction. Typically, the SAXS signal from laser excited plasmas is expected to be dominated by the free electron distribution. We propose that the ionic scattering signal becomes visible when the X-ray energy is in resonance with an electron transition between two bound states (Resonant coherent X-ray diffraction, RCXD). In this case the scattering cross-section dramatically increases so that the signal of X-ray scattering from ions silhouettes against the free electron scattering background which allows to measure the opacity and derived quantities with high spatial and temporal resolution, being fundamentally limited only by the X-ray wavelength and timing. Deriving quantities such as ion spatial distribution, charge state distribution and plasma temperature with such high spatial and temporal resolution will make a vast number of processes in shortpulse laser-solid interaction accessible for direct experimental observation e.g. hole-boring and shock propagation, filamentation and instability dynamics, electron transport, heating and ultrafast ionization dynamics.

physics.plasm-ph

High Contrast X-ray Speckle from Atomic-Scale Order in Liquids and Glasses

The availability of ultrafast pulses of coherent hard x-rays from the Linac Coherent Light Source opens new opportunities for studies of atomic-scale dynamics in amorphous materials. Here we show that single ultrafast coherent x-ray pulses can be used to observe the speckle contrast in the high-angle diffraction from liquid Ga and glassy Ni2Pd2P and B2O3. We determine the thresholds above which the x-ray pulses disturb the atomic arrangements. Furthermore, high contrast speckle is observed in scattering patterns from the glasses integrated over many pulses, demonstrating that the source and optics are sufficiently stable for x-ray photon correlation spectroscopy studies of dynamics over a wide range of time scales.

cond-mat.mtrl-sci