arXiv subjects

Mario Sauppe

Publications and source records attributed to Mario Sauppe.

9 recordsLinked to original sources

arXiv2026

Laser-induced transient opacity in helium nanodroplets probed by single-shot coherent diffraction

Single-shot coherent diffractive imaging (CDI) with intense short-wavelength light pulses enables the structural characterization of individual nanoparticles in free flight with high spatial and temporal resolution. Conventional CDI assumes that the target object exhibits a linear scattering response and static electronic properties. Here, we extend this approach to investigate transient laser-driven modifications of the electronic structure in individual nanoparticles, imprinted in their time-resolved diffraction patterns. In the presence of a near-infrared laser pulse, we observe a pronounced reduction in the diffraction signal from helium nanodroplets when probed with ultrashort extreme ultraviolet (XUV) pulses. This effect is attributed to a light-field-induced modification of the electronic structure of the droplets, which substantially increases their XUV absorption. Our results demonstrate that single-particle diffraction can capture ultrafast light-driven electron dynamics in nanoscale systems. This paves the way for the spatiotemporal tracking of reversible changes in the electronic properties of nanoscale structures with potential applications in ultrafast X-ray optics, materials science, and all-optical signal processing.

physics.optics↗

arXiv2025

Dichography: Two-frame Ultrafast Imaging from a Single Diffraction Pattern

We experimentally demonstrate that pairs of time-delayed ultrabright and ultrashort X-ray pulses of two different colors, delivered by modern X-ray Free Electron Lasers, can provide two time-delayed snapshots of a sample. We introduce Dichography, a method that algorithmically separates the diffraction signals overlapping on the detector and independently retrieves the two images of the specimen. We employ Dichography to reconstruct two views of individual xenon-doped helium nanodroplets with 20 nm spatial resolution. The consistency of structures observed in both images at delays up to 750 fs provides evidence that, under these illumination conditions, significant structural damage only occurs at longer timescales. We further validate the method by imaging pairs of silver nanoparticles intercepted by the same light pulse. Dichography enables a new class of experiments across physics, chemistry, and materials science, making a significant step toward the original promise of X-ray free-electron lasers to capture ultrafast movies of nanomatter.

physics.optics↗

arXiv2025

SPRING: an effective and reliable framework for image reconstruction in single-particle Coherent Diffraction Imaging

Coherent Diffraction Imaging (CDI) is an experimental technique to gain images of isolated structures by recording the light scattered off the sample. In principle, the sample density can be recovered from the scattered light field through a straightforward Fourier Transform operation. However, only the amplitude of the field is recorded, while the phase is lost during the measurement process and has to be retrieved by means of suitable, well-established phase retrieval algorithms. In this work, we present SPRING, an analysis framework tailored to X-ray Free Electron Laser (XFEL) single-shot single-particle diffraction data that implements the Memetic Phase Retrieval method to mitigate the shortcomings of conventional algorithms. We benchmark the approach on experimental data acquired in two experimental campaigns at SwissFEL and European XFEL. Imaging results on isolated nanostructures reveal unprecedented stability and resilience of the algorithm's behavior on the input parameters, as well as the capability of identifying the solution in conditions hardly treatable so far with conventional methods. A user-friendly implementation of SPRING is released as open-source software, aiming at being a reference tool for the coherent diffraction imaging community at XFEL and synchrotron facilities.

physics.optics↗

arXiv2023

Melting, bubble-like expansion and explosion of superheated plasmonic nanoparticles

We report on time-resolved coherent diffraction imaging of gas-phase silver nanoparticles, strongly heated via their plasmon resonance. The x-ray diffraction images reveal a broad range of phenomena for different excitation strengths, from simple melting over strong cavitation to explosive disintegration. Molecular dynamics simulations fully reproduce this behavior and show that the heating induces rather similar trajectories through the phase diagram in all cases, with the very different outcomes being due only to whether and where the stability limit of the metastable superheated liquid is crossed.

physics.atm-clus↗

arXiv2022

Three-Dimensional Coherent Diffractive Imaging of Isolated Faceted Nanostructures

The structure and dynamics of isolated nanosamples in free flight can be directly visualized via single-shot coherent diffractive imaging using the intense and short pulses of X-ray free-electron lasers. Wide-angle scattering images even encode three-dimensional morphological information of the samples, but the retrieval of this information remains a challenge. Up to now, effective three-dimensional morphology reconstructions from single shots were only achieved via fitting with highly constrained models, requiring a priori knowledge about possible geometrical shapes. Here we present a much more generic imaging approach. Relying on a model that allows for any sample morphology described by a convex polyhedron, we reconstruct wide-angle diffraction patterns from individual silver nanoparticles. In addition to known structural motives with high symmetries, we retrieve imperfect shapes and agglomerates which were not accessible previously. Our results open new routes towards true 3D structure determination of single nanoparticles and, ultimately, 3D movies of ultrafast nanoscale dynamics.

physics.atm-clus↗

arXiv2020

Highly nonlinear ionization of atoms induced by intense high-harmonic pulses

Intense extreme-ultraviolet (XUV) pulses enable the investigation of XUV-induced nonlinear processes and are a prerequisite for the development of attosecond pump - attosecond probe experiments. While highly nonlinear processes in the XUV range have been studied at free-electron lasers (FELs), high-harmonic generation (HHG) has allowed the investigation of low-order nonlinear processes. Here we suggest a concept to optimize the HHG intensity, which surprisingly requires a scaling of the experimental parameters that differs substantially from optimizing the HHG pulse energy. As a result, we are able to study highly nonlinear processes in the XUV range using a driving laser with a modest ($\approx 10$ mJ) pulse energy. We demonstrate our approach by ionizing Ar atoms up to Ar$^{5+}$, requiring the absorption of at least 10 XUV photons.

physics.atom-ph↗

arXiv2017

Diffractive imaging of transient electronic core-shell structures in a nanoplasma

We have recorded the coherent diffraction images of individual xenon clusters with intense extreme ultraviolet pulses to elucidate the influence of light-induced electronic changes on the diffraction pattern. Using the FLASH free-electron laser we tuned the wavelength to specific xenon atomic and ionic resonances. The data show the emergence of a transient core-shell structure within the otherwise homogeneous sample. Simulations indicate that ionization and nanoplasma formation result in a cluster shell with strongly altered refraction. The presented resonant scattering approach enables imaging of ultrafast electron dynamics on their natural time scale.

physics.atm-clus↗

arXiv2017

Femtosecond X-ray Fourier holography imaging of free-flying nanoparticles

Ultrafast X-ray imaging provides high resolution information on individual fragile specimens such as aerosols, metastable particles, superfluid quantum systems and live biospecimen, which is inaccessible with conventional imaging techniques. Coherent X-ray diffractive imaging, however, suffers from intrinsic loss of phase, and therefore structure recovery is often complicated and not always uniquely-defined. Here, we introduce the method of in-flight holography, where we use nanoclusters as reference X-ray scatterers in order to encode relative phase information into diffraction patterns of a virus. The resulting hologram contains an unambiguous three-dimensional map of a virus and two nanoclusters with the highest lat- eral resolution so far achieved via single shot X-ray holography. Our approach unlocks the benefits of holography for ultrafast X-ray imaging of nanoscale, non-periodic systems and paves the way to direct observation of complex electron dynamics down to the attosecond time scale.

physics.atm-clus↗

arXiv2017

Coherent diffractive imaging of single helium nanodroplets with a high harmonic generation source

Coherent diffractive imaging of individual free nanoparticles has opened novel routes for the in-situ analysis of their transient structural, optical, and electronic properties. So far, single-shot single-particle diffraction was assumed to be feasible only at extreme ultraviolet (XUV) and X-ray free-electron lasers, restricting this research field to large-scale facilities. Here we demonstrate single-shot imaging of isolated helium nanodroplets using XUV pulses from a femtosecond-laser driven high harmonic source. We obtain bright wide-angle scattering patterns, that allow us to uniquely identify hitherto unresolved prolate shapes of superfluid helium droplets. Our results mark the advent of single-shot gas-phase nanoscopy with lab-based short-wavelength pulses and pave the way to ultrafast coherent diffractive imaging with phase-controlled multicolor fields and attosecond pulses.

physics.atm-clus↗