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Hauke Höppner

Publications and source records attributed to Hauke Höppner.

15 recordsLinked to original sources

Probing laser-driven surface and subsurface dynamics via grazing-incidence XFEL scattering and diffraction

We demonstrate a grazing-incidence x-ray platform that simultaneously records time-resolved grazing-incidence small-angle x-ray scattering (GISAXS) and grazing-incidence x-ray diffraction (GID) from a femtosecond laser-irradiated gold film above the melting threshold, with picosecond resolution at an x-ray free-electron laser (XFEL). By tuning the x-ray incidence angle, the probe depth is set to tens of nanometers, enabling depth-selective sensitivity to near-surface dynamics. GISAXS resolves ultrafast changes in surface nanomorphology (correlation length, roughness), while GID quantifies subsurface lattice compression, grain orientation, melting, and recrystallization. The approach overcomes photon-flux limitations of synchrotron grazing-incidence geometries and provides stringent, time-resolved benchmarks for complex theoretical models of ultrafast laser-matter interaction and warm dense matter. Looking ahead, the same depth-selective methodology is well suited to inertial confinement fusion (ICF): it can visualize buried-interface perturbations and interfacial thermal resistance on micron to sub-micron scales that affect instability seeding and burn propagation.

physics.optics↗

Direct High-Magnetic-Field Coupling to Stripe Order in a Cuprate Superconductor

Superconductivity in cuprates emerges out of a complex normal state that hosts density waves, pseudogap physics, and strange metal properties. Here, we access this normal state by synchronizing free-electron laser x-rays with high-magnetic-field pulses up to 44 T. We observe a linear increase in charge order amplitude and correlation length that persists far above the vortex melting transition. This behavior is incompatible with standard phase competition between charge order and superconductivity. By means of conventional hard x-ray diffraction and magnetostriction, we show that applied fields also enhance monoclinic lattice distortions. However, this magnetoelastic response is weaker and an epiphenomenon of the stripe order enhancement. Combined with recent observations of field-linear spin freezing, our results point to a direct coupling between magnetic field and the spin component of stripe order in the high-field normal state -- a mechanism independent of superconductivity suppression that has so far remained hidden from scattering probes.

cond-mat.str-el↗

A Momentum-Resolved X-ray Thomson Scattering Benchmark of Electronic-Response Models in Warm Dense Aluminium

The robust diagnosis of conditions generated in warm dense matter (WDM) experiments remains a persistent challenge. Here we describe the measurement of shock-compressed aluminium at 50 GPa with angle-resolved femtosecond x-ray Thomson scattering (XRTS) over a wide range of scattering wavevectors at the European XFEL. The measured plasmon dispersion and line shape show that the de facto standard approach for analysing XRTS spectra, based on uniform-electron-gas models, systematically overestimates the resonance energy by up to 8 eV. We present an ab initio approach that agrees within the experimental uncertainty and demonstrates that accounting for shock-induced disorder is critical for interpreting shock-compressed systems, providing evidence that ab initio treatments are required for reliable XRTS inference in warm dense aluminium.

physics.plasm-ph↗

Probing ultrafast heating and ionization dynamics in solid density plasmas with time-resolved resonant X-ray absorption and emission

Heating and ionization are among the most fundamental processes in relativistic laser--solid interactions; however, their spatiotemporal evolution remains challenging to capture experimentally. Here we present detailed diagnosis of high-intensity laser interactions with wire targets, leveraging the extreme spectral brightness of an X-ray free-electron laser in sub-picosecond time-resolved resonant X-ray emission spectroscopy and absorption imaging. Experimental results are compared with comprehensive simulations using atomic collisional--radiative models, particle-in-cell, and magnetohydrodynamics codes to elucidate the underlying physics. These multi-scale simulations reveal extreme sensitivity of basic plasma parameters with widely used models, such as temperature and ionization depth, which are able to be constrained by incorporating a detailed accounting of laser spatial profiles, pre-plasma conditions, and collisional processes. These results provide new insights into heating and ionization dynamics in the high-energy-density regime relevant to inertial fusion energy research, both as an experimental platform for accessing theoretically challenging conditions and as a benchmark for improving models of high-power laser--plasma interactions.

physics.plasm-ph↗

XFEL Imaging Techniques for High Energy Density and Inertial Fusion Energy Research at HED-HiBEF

The imaging platform developed at the High Energy Density - Helmholtz International Beamline for Extreme Fields (HED-HiBEF) instrument at the European XFEL and its applications to high energy density and fusion related research are presented. The platform combines the XFEL beam with the high-intensity short-pulse laser ReLaX and the high-energy nanosecond-pulse laser DiPOLE-100X. The spatial resolution is better than 500 nm and the temporal resolution of the order of 50 fs. We show examples of blast waves and converging cylindrical shocks in aluminium, resonant absorption measurements of specific charged states in copper with ReLaX and planar shocks in polystyrene material generated by DiPOLE-100X. We also discuss the possibilities introduced by combining this imaging platform with a kJ-class laser.

physics.plasm-ph↗

Structural evolution of iron oxides melts at Earth's outer-core pressures

Oxygen and other light elements comprise up to 5 wt% of the Earth's outer-core, and may significantly influence its physical properties and the operation of the geodynamo. Here we report in situ x-ray diffraction measurements of Fe, Fe + 4.5 FeO (atomic proportion), and Fe2O3 melts at 177-438 GPa, achieved using laser-driven shock compression at an x-ray free-electron laser. The melts exhibit Fe-O coordination numbers between 4.0(0.4) and 4.5(0.4), indicating predominantly four-fold coordination environments. These coordination states are significantly smaller than those of Fe-bearing lower-mantle phases such as bridgmanite and ferropericlase. Shorter Fe-Fe interatomic distances in compressed iron oxide melts drive the denser packing relative to ambient melts, while the structural differences between Fe + 4.5 FeO and Fe2O3 melts under shock indicate that the oxidation state modulates oxygen solubility in liquid Fe. At around 177 GPa (380 km below the core-mantle boundary), Fe2O3 melts exhibit higher Fe-O coordination, suggesting that local variations in oxygen content could contribute to the stratification in the uppermost outer-core inferred from seismological and geomagnetic observations.

cond-mat.mtrl-sci↗

High-Quality Ultra-Fast Total Scattering and Pair Distribution Function Data using an X-ray Free Electron Laser

High-quality total scattering data, a key tool for understanding atomic-scale structure in disordered materials, require stable instrumentation and access to high momentum transfers. This is now routine at dedicated synchrotron instrumentation using high-energy X-ray beams, but it is very challenging to measure a total scattering dataset in less than a few microseconds. This limits their effectiveness for capturing structural changes that occur at the much faster timescales of atomic motion. Current X-ray free-electron lasers (XFELs) provide femtosecond-pulsed X-ray beams with maximum energies of approximately 24 keV, giving the potential to measure total scattering and the attendant pair distribution functions (PDFs) on femtosecond timescales. Here, we show that this potential has been realised using the HED scientific instrument at the European XFEL and present normalised total scattering data for 0.35 Å-1 < Q < 16.6 Å-1 and their PDFs from a broad spectrum of materials, including crystalline, nanocrystalline and amorphous solids, liquids, and clusters in solution. We analyse the data using a variety of methods, including Rietveld refinement, small-box PDF refinement, joint reciprocal-real space refinement, cluster refinement, and Debye scattering analysis. The resolution function of the setup is also characterised. We conclusively show that high-quality data can be obtained from a single approximately 30 fs XFEL pulse. Our efforts not only significantly increase the existing maximum reported Q-range for an S(Q) measured at an XFEL but also mean that XFELs are now a viable X-ray source for the broad community of people using reciprocal space total scattering and PDF methods in their research.

cond-mat.mtrl-sci↗

Demonstration of full-scale spatio-temporal diagnostics of solid-density plasmas driven by an ultra-short relativistic laser pulse using an X-ray free-electron laser

Understanding the complex plasma dynamics in ultra-intense relativistic laser-solid interactions is of fundamental importance to the applications of laser plasma-based particle accelerators, creation of high energy-density matter, understanding of planetary science and laser-driven fusion energy. However, experimental efforts in this regime have been limited by the accessibility of over-critical density and spatio-temporal resolution of conventional diagnostics. Over the last decade, the advent of femtosecond brilliant hard X-ray free electron lasers (XFELs) is opening new horizons to break these limitations. Here, for the first time we present full-scale spatio-temporal measurements of solid-density plasma dynamics, including preplasma generation with tens of nanometer-scale length driven by the leading edge of a relativistic laser pulse, ultrafast heating and ionization at the main pulse arrival, laser-driven blast shock waves and transient surface return current-induced compression dynamics up to hundreds of picoseconds after interaction. These observations are enabled by utilizing a novel combination of advanced X-ray diagnostics such as small-angle X-ray scattering (SAXS), resonant X-ray emission spectroscopy (RXES), and propagation-based X-ray phase-contrast imaging (XPCI) simultaneously at the European XFEL-HED beamline station.

physics.plasm-ph↗

Effects of Mosaic Crystal Instrument Functions on X-ray Thomson Scattering Diagnostics

Mosaic crystals, with their high integrated reflectivities, are widely-employed in spectrometers used to diagnose high energy density systems. X-ray Thomson scattering (XRTS) has emerged as a powerful diagnostic tool of these systems, providing in principle direct access to important properties such as the temperature via detailed balance. However, the measured XRTS spectrum is broadened by the spectrometer instrument function (IF), and without careful consideration of the IF one risks misdiagnosing system conditions. Here, we consider in detail the IF of 40 $μ$m and 100 $μ$m mosaic HAPG crystals, and how the broadening varies across the spectrometer in an energy range of 6.7-8.6 keV. Notably, we find a strong asymmetry in the shape of the IF towards higher energies. As an example, we consider the effect of the asymmetry in the IF on the temperature inferred via XRTS for simulated 80 eV CH plasmas, and find that the temperature can be overestimated if an approximate symmetric IF is used. We therefore expect a detailed consideration of the full IF will have an important impact on system properties inferred via XRTS in both forward modelling and model-free approaches.

physics.plasm-ph↗

Cylindrical compression of thin wires by irradiation with a Joule-class short pulse laser

Equation of state measurements at Jovian or stellar conditions are currently conducted by dynamic shock compression driven by multi-kilojoule multi-beam nanosecond-duration lasers. These experiments require precise design of the target and specific tailoring of the spatial and temporal laser profiles to reach the highest pressures. At the same time, the studies are limited by the low repetition rate of the lasers. Here, we show that by the irradiation of a thin wire with single beam Joule-class short-pulse laser, a converging cylindrical shock is generated compressing the wire material to conditions relevant for the above applications. The shockwave was observed using Phase Contrast Imaging employing a hard X-ray Free Electron Laser with unprecedented temporal and spatial sensitivity. The data collected for Cu wires is in agreement with hydrodynamic simulations of an ablative shock launched by a highly-impulsive and transient resistive heating of the wire surface. The subsequent cylindrical shockwave travels towards the wire axis and is predicted to reach a compression factor of 9 and pressures above 800 Mbar. Simulations for astrophysical relevant materials underline the potential of this compression technique as a new tool for high energy density studies at high repetition rates.

physics.plasm-ph↗

Visualizing Plasmons and Ultrafast Kinetic Instabilities in Laser-Driven Solids using X-ray Scattering

Ultra-intense lasers that ionize and accelerate electrons in solids to near the speed of light can lead to kinetic instabilities that alter the laser absorption and subsequent electron transport, isochoric heating, and ion acceleration. These instabilities can be difficult to characterize, but a novel approach using X-ray scattering at keV energies allows for their visualization with femtosecond temporal resolution on the few nanometer mesoscale. Our experiments on laser-driven flat silicon membranes show the development of structure with a dominant scale of $~60\unit{nm}$ in the plane of the laser axis and laser polarization, and $~95\unit{nm}$ in the vertical direction with a growth rate faster than $0.1/\mathrm{fs}$. Combining the XFEL experiments with simulations provides a complete picture of the structural evolution of ultra-fast laser-induced instability development, indicating the excitation of surface plasmons and the growth of a new type of filamentation instability. These findings provide new insight into the ultra-fast instability processes in solids under extreme conditions at the nanometer level with important implications for inertial confinement fusion and laboratory astrophysics.

physics.plasm-ph↗

Resonant inelastic x-ray scattering in warm-dense Fe compounds beyond the SASE FEL resolution limit

Resonant inelastic x-ray scattering (RIXS) is a widely used spectroscopic technique, providing access to the electronic structure and dynamics of atoms, molecules, and solids. However, RIXS requires a narrow bandwidth x-ray probe to achieve high spectral resolution. The challenges in delivering an energetic monochromated beam from an x-ray free electron laser (XFEL) thus limit its use in few-shot experiments, including for the study of high energy density systems. Here we demonstrate that by correlating the measurements of the self-amplified spontaneous emission (SASE) spectrum of an XFEL with the RIXS signal, using a dynamic kernel deconvolution with a neural surrogate, we can achieve electronic structure resolutions substantially higher than those normally afforded by the bandwidth of the incoming x-ray beam. We further show how this technique allows us to discriminate between the valence structures of Fe and Fe$_2$O$_3$, and provides access to temperature measurements as well as M-shell binding energies estimates in warm-dense Fe compounds.

cond-mat.mtrl-sci↗

Probing the UV-Induced Photodissociation of CH$_\text{3}$I and C$_\text{6}$H$_\text{3}$F$_\text{2}$I with Femtosecond Time-Resolved Coulomb Explosion Imaging at FLASH

We explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from the FLASH free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267\,nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon--iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules.

physics.atom-ph↗

Alignment, Orientation, and Coulomb Explosion of Difluoroiodobenzene Studied with the Pixel Imaging Mass Spectrometry (PImMS) Camera

Laser-induced adiabatic alignment and mixed-field orientation of 2,6-difluoroiodobenzene (C6H3F2I) molecules are probed by Coulomb explosion imaging following either near-infrared strong-field ionization or extreme-ultraviolet multi-photon inner-shell ionization using free-electron laser pulses. The resulting photoelectrons and fragment ions are captured by a double-sided velocity map imaging spectrometer and projected onto two position-sensitive detectors. The ion side of the spectrometer is equipped with the Pixel Imaging Mass Spectrometry (PImMS) camera, a time-stamping pixelated detector that can record the hit positions and arrival times of up to four ions per pixel per acquisition cycle. Thus, the time-of-flight trace and ion momentum distributions for all fragments can be recorded simultaneously. We show that we can obtain a high degree of one- and three-dimensional alignment and mixed- field orientation, and compare the Coulomb explosion process induced at both wavelengths.

physics.chem-ph↗

Soft x-rays induce femtosecond solid-to-solid phase transition

Soft x-rays were applied to induce graphitization of diamond through a non-thermal solid-to-solid phase transition. This process was observed within poly-crystalline diamond with a time-resolved experiment using ultrashort soft x-ray pulses of duration 52.5 fs and cross correlated by an optical pulse of duration 32.8 fs. This scheme enabled for the first time the measurement of a phase transition on a timescale of ~150 fs. Excellent agreement between experiment and theoretical predictions was found, using a dedicated code that followed the non-equilibrium evolution of the irradiated diamond including all transient electronic and structural changes. These observations confirm that soft x-rays can induce a non-thermal ultrafast solid-to-solid phase transition on a hundred femtosecond timescale.

physics.atom-ph↗