Daniela Rupp

ETH Zurich

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T. Möller

Technische Universität Berlin

Tais Gorkhover

SLAC National Accelerator Laboratory

Mario Sauppe

Technische Universität Berlin

M. Adolph

Hensoldt (Germany)

Sebastian Schorb

Technische Universität Berlin

Bruno Langbehn

Technische Universität Berlin

Yevheniy Ovcharenko

European X-Ray Free-Electron Laser

Rico Mayro P. Tanyag

Aarhus University

Anatoli Ulmer

Universität Hamburg

Christoph Bostedt

Argonne National Laboratory

Cooperative Institutions

SLAC National Accelerator Laboratory

107

Deutsches Elektronen-Synchrotron DESY

103

Universität Hamburg

Center for Free-Electron Laser Science

European X-Ray Free-Electron Laser

Technische Universität Berlin

Linac Coherent Light Source

Max Planck Society

Menlo School

Max-Born-Institute for Nonlinear Optics and Short Pulse Spectroscopy

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Zusammenhang von Metaboliten im Thalamus und Verarbeitungsgeschwindigkeit in der frühen Adoleszenz: Vorläufige Ergebnisse

Christoph Hamann Daniela Rupp St Leuenberger R.L 'Gorman Leila Tarokh

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Three-dimensional femtosecond snapshots of isolated faceted nanostructures

Science Advances (2023)

Alessandro Colombo Simon Dold Patrice Kolb Nils Bernhardt Patrick Behrens

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.

Polyhedron

10.1126/sciadv.ade5839

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Finding the semantic similarity in single-particle diffraction images using self-supervised contrastive projection learning

arXiv (Cornell University) (2022)

Julian Zimmermann Fabien Beguet Daniel Guthruf Bruno Langbehn Daniela Rupp

Single-shot diffraction imaging of isolated nanosized particles has seen remarkable success in recent years, yielding in-situ measurements with ultra-high spatial and temporal resolution. The progress of high-repetition-rate sources for intense X-ray pulses has further enabled recording datasets containing millions of diffraction images, which are needed for structure determination of specimens with greater structural variety and for dynamic experiments. The size of the datasets, however, represents a monumental problem for their analysis. Here, we present an automatized approach for finding semantic similarities in coherent diffraction images without relying on human expert labeling. By introducing the concept of projection learning, we extend self-supervised contrastive learning to the context of coherent diffraction imaging. As a result, we achieve a semantic dimensionality reduction producing meaningful embeddings that align with the physical intuition of an experienced human researcher. The method yields a substantial improvement compared to previous approaches, paving the way toward real-time and large-scale analysis of coherent diffraction experiments at X-ray free-electron lasers.

10.48550/arxiv.2208.11752

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

arXiv (Cornell University) (2019)

Björn Senfftleben Martin Kretschmar Andreas Hoffmann Mario Sauppe J. Tümmler

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.

Extreme ultraviolet

Attosecond

Photon energy

Water window

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

arXiv (Cornell University) (2023)

Simon Dold Thomas Reichenbach Alessandro Colombo Jakob Jordan Ingo Barke

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.

Metastability

10.48550/arxiv.2309.00433

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Theoretical Concepts for Single Cluster Imaging

Springer theses (2016)

Daniela Rupp

Free electron model

10.1007/978-3-319-28649-5_1

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Ionization dynamics of Xe nanoplasma formation studied with XUV fluorescence spectroscopy

Journal of Physics B Atomic Molecular and Optical Physics (2015)

Andreas Przystawik L. Schroedter Márcia Müller M. Adolph C. Bostedt

Intense pulses from a short wavelength free-electron laser turn xenon nanoparticles into a high energy density nanoplasma within femtoseconds. Recently, the generation of multiply charged xenon ions during the initial phase of plasma evolution has been studied by energy-resolved XUV fluorescence detection as a function of cluster size and cluster composition [1]. In the present contribution we give a detailed analysis of the corresponding radiative transitions after resonant excitation of the 4d electron shell at intensities of 2 × 1012 − 2.45 × 1015 W cm−2. The evaluation of charge-state specific fluorescence yields as a function of FEL power density demonstrates that plasma effects such as ionization potential lowering, electron impact excitation, ionization, and energy redistribution govern the laser-induced non-equilibrium dynamics in xenon clusters.

Extreme ultraviolet

Dynamics

10.1088/0953-4075/48/18/184002

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The Scatman: an approximate method for fast wide-angle scattering simulations

arXiv (Cornell University) (2022)

Alessandro Colombo Julian Zimmermann Bruno Langbehn T. Möller Christian Peltz

Single-shot Coherent Diffraction Imaging (CDI) is a powerful approach to characterize the structure and dynamics of isolated nanoscale objects such as single viruses, aerosols, nanocrystals or droplets. Using X-ray wavelengths, the diffraction images in CDI experiments usually cover only small scattering angles of few degrees. These small-angle patterns represent the magnitude of the Fourier transform of the two-dimensional projection of the sample's electron density, which can be reconstructed efficiently but lacks any depth information. In cases where the diffracted signal can be measured up to scattering angles exceeding 10 degrees, i.e. in the wide-angle regime, three-dimensional morphological information of the target is contained in a single-shot diffraction pattern. However, the extraction of the 3D structural information is no longer straightforward and defines the key challenge in wide-angle CDI. So far, the most convenient approach relies on iterative forward fitting of the scattering pattern using scattering simulations. Here we present the Scatman, an approximate and fast numerical tool for the simulation and iterative fitting of wide-angle scattering images of isolated samples. Furthermore, we publish and describe in detail our Open Source software implementation of the Scatman algorithm, PyScatman. The Scatman approach yields quantitative results for weakly scattering samples. PyScatman is capable of computing wide-angle scattering patterns in few milliseconds even on consumer-level computing hardware. The high computational efficiency of PyScatman enables effective data analysis based on model fitting, thus representing an important step towards a systematic application of 3D Coherent Diffraction Imaging from single wide-angle diffraction patterns in various scientific communities.

Biological small-angle scattering

10.48550/arxiv.2202.03411

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Explosions of Methane Clusters Driven by Intense X-Ray FEL Pulses

Nirmala Kandadai Kay Hoffmann H. Thomas A. Helal J. W. Keto

Get PDF Email Share Share with Facebook Tweet This Post on reddit Share with LinkedIn Add to CiteULike Add to Mendeley Add to BibSonomy Get Citation Copy Citation Text N. Kandadai, K. Hoffmann, H. Thomas, A. Helal, J. Keto, T. Ditmire, B. Iwan, N. Timneanu, J. Andreasson, M. Seibert, D. van der Spoel, J. Hajdu, S. Schorb, T. Gorkhover, D. Rupp, M. Adolph, T. Möller, G. Doumy, L. F. DiMauro, C. Bostedt, J. Bozek, M. Hoener, B. Murphy, and N. Berrah, "Explosions of Methane Clusters Driven by Intense X-Ray FEL Pulses," in CLEO:2011 - Laser Applications to Photonic Applications, OSA Technical Digest (CD) (Optica Publishing Group, 2011), paper QTuC2. Export Citation BibTex Endnote (RIS) HTML Plain Text Citation alert Save article

10.1364/qels.2011.qtuc2

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X-Ray and XUV Imaging of Helium Nanodroplets

Topics in applied physics (2022)

Rico Mayro P. Tanyag Bruno Langbehn T. Möller Daniela Rupp

Abstract X-ray and extreme ultraviolet (XUV) coherent diffractive imaging (CDI) have the advantage of producing high resolution images with current spatial resolution of tens of nanometers and temporal resolution of tens of femtoseconds. Modern developments in the production of coherent, ultra-bright, and ultra-short X-ray and XUV pulses have even enabled lensless, single-shot imaging of individual, transient, non-periodic objects. The data collected in this technique are diffraction images, which are intensity distributions of the scattered photons from the object. Superfluid helium droplets are ideal systems to study with CDI, since each droplet is unique on its own. It is also not immediately apparent what shapes the droplets would take or what structures are formed by dopant particles inside the droplet. In this chapter, we review the current state of research on helium droplets using CDI, particularly, the study of droplet shape deformation, the in-situ configurations of dopant nanostructures, and their dynamics after being excited by an intense laser pulse. Since CDI is a rather new technique for helium nanodroplet research, we also give a short introduction on this method and on the different light sources available for X-ray and XUV experiments.

Extreme ultraviolet

Temporal resolution

10.1007/978-3-030-94896-2_7

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