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Thomas Fennel

Publications and source records attributed to Thomas Fennel.

At least 19 recordsLinked to original sources

X-ray Driven Trihydrogen Formation on Silica Nanosurfaces

The trihydrogen cation ($\mathrm{H_3^+}$) initiates the ion-molecule reactions that build molecular complexity in interstellar space. Whether its canonical formation reaction, $\mathrm{H_2^+ + H_2 \rightarrow H_3^+ + H}$, proceeds on inorganic surfaces under radiation-driven ionization has remained untested. Here we drive $\mathrm{H_3^+}$ formation on hydrated silica nanoparticles using intense 1.88 keV X-ray pulses, combining ion velocity map imaging, electron time-of-flight spectroscopy, and single-particle coherent diffractive imaging to resolve this chemistry on individual particles. The self-induced surface electric field on the V/nm scale drives interfacial charge transfer and water fragmentation. This field is the dominant parameter governing the relative yields of $\mathrm{H^+}$, $\mathrm{H_2^+}$, and $\mathrm{H_3^+}$ across particle size, composition, and aggregation. Density functional theory and nonadiabatic quantum molecular dynamics simulations trace this field-driven charge transfer, directly analogous to band bending at semiconductor photoelectrodes. These results establish surface-field-driven charge transfer as a unifying mechanism between radiation dominated astrophysical environments and field-driven surface catalysis.

physics.chem-ph

A finite-difference model for intense light interactions with dielectrics in the ultrafast ionization regime

We present a computationally efficient model that describes the interaction of intense, ultrashort infrared laser pulses with transparent materials in the strong ionization regime. The model is augmented with a detailed self-consistent description of the local response due to ionization and collisional plasma dynamics. It incorporates the direct solution of Maxwell's equations without approximations and rigorous boundary conditions for the input pulse, allowing us to study the ultrafast formation of over-critical nanoscaled plasmas in dielectric materials under the influence of intense tightly focused laser pulses. We perform a scan of the parameter space, find unexpected optima regimes for different experientially relevant parameters, and explain these maxima based on spatiotemporal dynamics.

physics.plasm-ph

Cross-process interference in single-cycle electron emission from metal needle tips

Though interference from different emission channels enabled a deeper understanding of strong-field photoemission in atoms and molecules, it remained out of reach for solids. Here, we explore metal needle tips under single-cycle pulses via classical trajectories extended by quantum diffusion and interference and numerical solution of the time-dependent Schr\"odinger equation. We find interference of direct and backscattered electrons with fringe pattern encoding sub-cycle information on birth times and near-field driven acceleration dynamics, opening routes for ultrafast solid-state metrology.

physics.optics

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

Model-free pattern separation of two-color ultrafast X-ray diffraction

Two-color X-ray imaging with Free Electron Laser pulses offers a powerful approach for probing ultrafast structural dynamics in nanoscale systems, combining (near-)atomic spatial resolution with femtosecond temporal precision. The first X-ray pulse captures the object's initial state, while the second, time-delayed pulse records its subsequent evolution. A key challenge lies in disentangling the two patterns simultaneously recorded by the same detector. We demonstrate the realization of this approach on structurally varying nanoscale particles using two X-ray pulses of different photon energies, 1 and 1.2 keV. Sub-micrometer helium nanodroplets generated in vacuum are irradiated by the two X-ray pulses separated in time by up to 750 femtoseconds. Taking advantage of the high photon-energy resolution of the imaging detector, we separate the overlapping diffraction signals by analyzing individual pixel counts and applying pattern recognition. The helium nanodroplets' spherical shape allows us to cross-validate this approach by fitting the radial scattering profiles with Mie solutions for abichromatic field. The excellent agreement between the two methods, particularly in the sparsely illuminated outer regions of the diffraction patterns where high-resolution structural information is encoded, highlights the quality of this approach and its potential for future advanced X-ray movie techniques.

physics.optics

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

Fast Simulation of Wide-Angle Coherent Diffractive Imaging

Single-shot coherent diffractive imaging (CDI) using intense XUV and soft X-ray pulses holds the promise to deliver information on the three dimensional shape as well as the optical properties of nano-scale objects in a single diffraction image. This advantage over conventional X-ray diffraction methods comes at the cost of a much more complex description of the underlying scattering process due to the importance of wide-angle scattering and propagation effects. The commonly employed reconstruction of the sample properties via iterative forward fitting of diffraction patterns requires an accurate and fast method to simulate the scattering process. This work introduces the propagation multi-slice Fourier transform method (pMSFT) and demonstrates its superior performance and accuracy against existing methods for wide-angle scattering. A derivation from first principles, a unified physical picture of the approximations underlying pMSFT and the existing methods, as well as a systematic benchmark that provides qualified guidance for the selection of the appropriate scattering method is presented.

physics.optics

Attosecond physics in optical near fields

Attosecond science, the electron control by the field of ultrashort laser pulses, is maturing into lightfield-driven electronics, called petahertz electronics. Based on optical field-driven nanostructures, elements for petahertz electronics have been demonstrated. These hinge on the understanding of the electron dynamics in the optical near field of the nanostructure. Here we show near field-induced low energy stripes (NILES) in carrier-envelope phase-dependent electron spectra, a new spectral feature appearing in the direct electrons emitted from a strongly driven nanostructure, i.e., in the easily accessible energy region between 0 and a few electron volts. NILES emerge due to the sub-cycle sensitivity of ponderomotive acceleration of electrons injected into a strong near field gradient by a few-cycle optical waveform. NILES enables us to track the emission of direct and re-scattered electrons down to sub-cycle time-scales and to infer the electron momentum width at emission. Because NILES shows up in the direct part of the electrons, a large fraction of the emitted electrons can now be steered in new ways, facilitating the isolation of individual electron bursts with high charge density of 430 attosecond duration. These results not only substantially advance the understanding of attosecond physics in optical near fields, but also provide new ways of electron control for the nascent field of petahertz electronics.

physics.optics

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

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

Tracing attosecond electron emission from a nanometric metal tip

Solids exposed to intense electric fields release electrons through tunnelling. This fundamental quantum process lies at the heart of various applications, ranging from high brightness electron sources in DC operation to petahertz vacuum electronics in laser-driven operation. In the latter process, the electron wavepacket undergoes semiclassical dynamics in the strong oscillating laser field, similar to strong-field and attosecond physics in the gas phase. There, the sub-cycle electron dynamics has been determined with a stunning precision of tens of attoseconds, but at solids the quantum dynamics including the emission time window has so far not been measured. Here we show that two-colour modulation spectroscopy of backscattering electrons uncovers the sub-optical-cycle strong-field emission dynamics from nanostructures, with attosecond precision. In our experiment, photoelectron spectra of electrons emitted from a sharp metallic tip are measured as function of the relative phase between the two colours. Projecting the solution of the time-dependent Schr\"odinger equation onto classical trajectories relates phase-dependent signatures in the spectra to the emission dynamics and yield an emission duration of $710\pm30$ attoseconds by matching the quantum model to the experiment. Our results open the door to the quantitative timing and precise active control of strong-field photoemission in solid state and other systems and have direct ramifications for diverse fields such as ultrafast electron sources, quantum degeneracy studies and sub-Poissonian electron beams, nanoplasmonics and petahertz electronics.

physics.optics

Electron energy loss and angular asymmetry induced by elastic scattering in helium droplets

Helium nanodroplets are ideal model systems to unravel the complex interaction of condensed matter with ionizing radiation. Here we study the effect of purely elastic electron scattering on angular and energy distributions of photoelectrons emitted from He nanodroplets of variable size ($10$-$10^9$ atoms per droplets). For large droplets, photoelectrons develop a pronounced anisotropy along the incident light beam due to a shadowing effect within the droplets. In contrast, the detected photoelectron spectra are only weakly perturbed. This opens up possibilities for photoelectron spectroscopy of dopants embedded in droplets provided they are smaller than the penetration depth of the light and the trapping range of emitted electrons.

physics.atm-clus

Generation of Large Vortex-Free Superfluid Helium Nanodroplets

Superfluid helium nanodroplets are an ideal environment for the formation of metastable, self-organized dopant nanostructures. However, the presence of vortices often hinders their formation. Here, we demonstrate the generation of vortex-free helium nanodroplets and explore the size range in which they can be produced. From x-ray diffraction images of xenon-doped droplets, we identify that single compact structures, assigned to vortex-free aggregation, prevail up to $10^8$ atoms per droplet. This finding builds the basis for exploring the assembly of far-from-equilibrium nanostructures at low temperatures.

cond-mat.mes-hall

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

Diffraction imaging of light induced dynamics in xenon-doped helium nanodroplets

We have explored the light induced dynamics in superfluid helium nanodroplets with wide-angle scattering in a pump-probe measurement scheme. The droplets are doped with xenon atoms to facilitate the ignition of a nanoplasma through irradiation with near-infrared laser pulses. After a variable time delay of up to 800 ps, we image the subsequent dynamics using intense extreme ultraviolet pulses from the FERMI free-electron laser. The recorded scattering images exhibit complex intensity fluctuations that are categorized based on their characteristic features. Systematic simulations of wide-angle diffraction patterns are performed, which can qualitatively explain the observed features by employing model shapes with both randomly distributed as well as structured, symmetric distortions. This points to a connection between the dynamics and the positions of the dopants in the droplets. In particular, the structured fluctuations might be governed by an underlying array of quantized vortices in the superfluid droplet as has been observed in previous small-angle diffraction experiments. Our results provide a basis for further investigations of dopant-droplet interactions and associated heating mechanisms.

physics.atm-clus

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

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.

physics.comp-ph

Strong-field physics with nanospheres

When intense laser fields interact with nanoscale targets, strong-field physics meets plasmonic near-field enhancement and sub-wavelength localization of light. Photoemission spectra reflect the associated attosecond optical and electronic response and encode the collisional and collective dynamics of the solid. Nanospheres represent an ideal platform to explore the underlying attosecond nanophysics because of their particularly simple geometry. This review summarizes key results from the last decade and aims to provide the essential stepping stones for students and researchers to enter this field.

physics.optics

Characterization of laser-induced ionization dynamics in solid dielectrics

The formation of an electron-hole plasma during the interaction of intense femtosecond laser pulses with transparent solids lies at the heart of femtosecond laser processing. Advanced micro- and nanomachining applications require improved control over the excitation characteristics. Here, we relate the emission of low-order harmonics to the strong laser-field-induced plasma formation. Together with a measurement of the total plasma density we identify the contribution of two competing ionization mechanisms - strong-field and electron-impact ionization.

physics.optics