arXiv subjects

Benjamin Erk

Publications and source records attributed to Benjamin Erk.

At least 19 recordsLinked to original sources

arXiv2026

Probing the structure of cyclic hydrocarbon molecules with X-ray-induced Coulomb explosion imaging

Coulomb explosion imaging (CEI) is a powerful experimental technique that maps a molecule's geometric structure onto the momenta of ionic molecular fragments produced by rapid multiple ionization. Here, we apply CEI induced by pulses from an X-ray free-electron laser in order to image and distinguish complex hydrocarbon isomers with the chemical formula C7H8: toluene, cycloheptatriene, and 1,6-heptadiyne. The measured fragment-ion momentum distributions show discernible differences between the three isomers and provide signatures of specific carbon and hydrogen sites in the molecule. In contrast to previous work, we demonstrate that distinct 'marker atoms' are not strictly required for constructing a meaningful molecular frame of reference for the interpretation of the momentum-space data. Our work paves the way for tracking the ultrafast motion of nuclei during isomerization reactions in pure hydrocarbons.

physics.chem-ph↗

arXiv2025

Wavelength-Dependent Photodissociation of Iodomethylbutane

Ultrashort XUV pulses of the Free-Electron-LASer in Hamburg (FLASH) were used to investigate laser-induced fragmentation patterns of the prototypical chiral molecule 1-iodo-2-methyl-butane (C$_5$H$_{11}$I) in a pump-probe scheme. Ion velocity-map images and mass spectra of optical-laser-induced fragmentation were obtained for subsequent FEL exposure with photon energies of 63 eV and 75 eV. These energies specifically address the iodine 4d edge of neutral and singly charged iodine, respectively. The presented ion spectra for two optical pump-laser wavelengths, i.e., 800 nm and 267 nm, reveal substantially different cationic fragment yields in dependence on the wavelength and intensity. For the case of 800-nm-initiated fragmentation, the molecule dissociates notably slower than for the 267-nm pump. The results underscore the importance of considering optical-laser wavelength and intensity in the dissociation dynamics of this prototypical chiral molecule that is a promising candidate for future studies of its asymmetric nature.

physics.chem-ph↗

arXiv2024

Attosecond soft X-ray pulses generated by chirp-dispersed manipulation in an XFEL reveal nonlinear core-electron dynamics in neon

Free-electron lasers have demonstrated their capability of generating intense attosecond X-ray pulses, which are the key to studying electron dynamics at their natural time scale and in specifically targeted electronic states, but come at the expanse of complicated generation schemes and stochastic pulse shapes. Here, we demonstrate a novel and simple operation concept based on the manipulation of the electron-bunch chirp-dispersion and working with the full 4.5 MHz repetition rate at the European XFEL in Germany. With a high-fidelity single-shot temporal characterisation, we detect X-ray pulses with durations of down to 200 attoseconds and peak powers reaching into the terawatt regime at ~1 keV photon energy. As a direct application, we present simultaneous measurements of nonlinear X-ray-matter interaction via time-resolved electron spectroscopy. Using the derived temporal pulse information and restricting the durations to a regime where individual X-ray pulses are shorter than the single-core-hole life time in neon atoms, we reveal an otherwise hidden peak-intensity dependence in the nonlinear dynamics of double-core-hole formation. Our results open the field of attosecond science to the investigation of electronic processes not only in the ground state but also in systems driven far off their equilibrium. They shed light on highly transient intermediate steps in complex electronic dynamics and thus promise to help build the conceptual bridge between fundamental physical processes and chemical photo-reactions.

physics.optics↗

arXiv2024

Controlled molecule injector for cold, dense, and pure molecular beams at the European x-ray free-electron laser

A permanently available molecular-beam injection setup for controlled molecules (COMO) was installed and commissioned at the small quantum systems (SQS) instrument at the European x-ray free-electron laser (EuXFEL). A $b$-type electrostatic deflector allows for pure state-, size-, and isomer-selected samples of polar molecules and clusters. The source provides a rotationally cold ($T\approx1$~K) and dense ($\rho\approx10^8$~cm$^{-3}$) molecular beam with pulse durations up to 100~\us generated by a new version of the Even-Lavie valve. Here, a performance overview of the COMO setup is presented along with characterization experiments performed both, with an optical laser at the Center for Free-Electron-Laser Science and with x-rays at EuXFEL under burst-mode operation. COMO was designed to be attached to different instruments at the EuXFEL, in particular at the small quantum systems (SQS) and single particles, clusters, and biomolecules (SPB) instruments. This advanced controlled-molecules injection setup enables XFEL studies using highly defined samples with soft and hard x-ray FEL radiation for applications ranging from atomic, molecular, and cluster physics to elementary processes in chemistry and biology.

physics.chem-ph↗

arXiv2023

Monitoring the evolution of relative product populations at early times during a photochemical reaction

Identifying multiple rival reaction products and transient species formed during ultrafast photochemical reactions and determining their time-evolving relative populations are key steps towards understanding and predicting photochemical outcomes. Yet, most contemporary ultrafast studies struggle with clearly identifying and quantifying competing molecular structures/species amongst the emerging reaction products. Here, we show that mega-electronvolt ultrafast electron diffraction in combination with ab initio molecular dynamics calculations offer a powerful route to determining time-resolved populations of the various isomeric products formed after UV (266 nm) excitation of the five-membered heterocyclic molecule 2(5H)-thiophenone. This strategy provides experimental validation of the predicted high (~50%) yield of an episulfide isomer containing a strained 3-membered ring within ~1 ps of photoexcitation and highlights the rapidity of interconversion between the rival highly vibrationally excited photoproducts in their ground electronic state.

physics.chem-ph↗

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↗

arXiv2023

Multiple-core-hole resonance spectroscopy with ultraintense X-ray pulses

Understanding the interaction of intense, femtosecond X-ray pulses with heavy atoms is crucial for gaining insights into the structure and dynamics of matter. One key aspect of nonlinear light-matter interaction was, so far, not studied systematically at free-electron lasers -- its dependence on the photon energy. Using resonant ion spectroscopy, we map out the transient electronic structures occurring during the complex charge-up pathways. Massively hollow atoms featuring up to six simultaneous core holes determine the spectra at specific photon energies and charge states. We also illustrate how the influence of different X-ray pulse parameters that are usually intertwined can be partially disentangled. The extraction of resonance spectra is facilitated by the fact that the ion yields become independent of the peak fluence beyond a saturation point. Our study lays the groundwork for novel spectroscopies of transient atomic species in exotic, multiple-core-hole states that have not been explored previously.

physics.atom-ph↗

arXiv2023

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↗

arXiv2022

Photon Energy-Resolved Velocity Map Imaging from Spectral Domain Ghost Imaging

We present an approach that combines photon spectrum correlation analysis with the reconstruction of three-dimensional momentum distribution from velocity map images in an efficient, single-step procedure. We demonstrate its efficacy with the results from the photoionization of the $2p$-shell of argon using the FLASH free-electron laser~(FEL). Distinct spectral features due to the spin-orbit splitting of Ar$^+(2p^{-1})$ are resolved, despite the large average bandwidth of the ionizing pulses from the FEL. This demonstrates a clear advantage over the conventional analysis method, and it will be broadly beneficial for velocity map imaging experiments with FEL sources. The retrieved linewidth of the binding energy spectrum approaches the resolution limitation prescribed by the spectrometers used to collect the data. Our approach presents a path to extend spectral-domain ghost imaging to the case where the photoproduct observable is high-dimensional.

physics.atom-ph↗

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↗

arXiv2022

The Kinetic Energy of PAH Dication and Trication Dissociation Determined by Recoil-Frame Covariance Map Imaging

We investigated the dissociation of dications and trications of three polycyclic aromatic hydrocarbons (PAHs), fluorene, phenanthrene, and pyrene. PAHs are a family of molecules ubiquitous in space and involved in much of the chemistry of the interstellar medium. In our experiments, ions are formed by interaction with 30.3 nm extreme ultraviolet (XUV) photons, and their velocity map images are recorded using a PImMS2 multi-mass imaging sensor. Application of recoil-frame covariance analysis allows the total kinetic energy release (TKER) associated with multiple fragmentation channels to be determined to high precision, ranging 1.94-2.60 eV and 2.95-5.29 eV for the dications and trications, respectively. Experimental measurements are supported by Born-Oppenheimer molecular dynamics (BOMD) simulations.

physics.chem-ph↗

arXiv2021

Single-shot MHz velocity-map-imaging using two Timepix3 cameras

We demonstrate the application of event-driven Timepix3-based detectors in combination with a double-sided velocity-map-imaging spectrometer to record the full 3D momentum of charged particles at the free-electron-laser facility FLASH. We measured the XUV induced fragmentation of $\text{N}_2$ using 250 kHz FLASH bursts with sub-pixel spatial resolution and up to 1.7~ns temporal resolution for photoelectrons. To further demonstrate the capabilities of this camera at even higher repetition rates we measured single-shot images of He($1s$) photoelectrons for bursts with a repetition rate of 1 MHz. Overall, with the Timepix3 camera we overcome limitations of standard-camera technology for advanced-imaging experiments with requirements on high event-rates and high spatio-temporal resolution.

physics.ins-det↗

arXiv2020

New aerodynamic lens injector for single particle diffractive imaging

An aerodynamic lens injector was developed specifically for the needs of single-particle diffractive imaging experiments at free-electron lasers. Its design allows for quick changes of injector geometries and focusing properties in order to optimize injection for specific individual samples. Here, we present results of its first use at the FLASH free-electron-laser facility. Recorded diffraction patterns of polystyrene spheres are modeled using Mie scattering, which allowed for the characterization of the particle beam under diffractive-imaging conditions and yield good agreement with particle-trajectory simulations.

physics.ins-det↗

arXiv2019

Tracking the Ultraviolet Photochemistry of Thiophenone During and Beyond the Initial Ultrafast Ring Opening

Photoinduced isomerization reactions, including ring-opening reactions, lie at the heart of many processes in nature. The mechanisms of such reactions are determined by a delicate interplay of coupled electronic and nuclear dynamics unfolding on the femtosecond scale, followed by the slower redistribution of energy into different vibrational degrees of freedom. Here we apply time-resolved photoelectron spectroscopy with a seeded extreme ultraviolet free electron laser to trace the ultrafast ring opening of gas phase thiophenone molecules following photoexcitation at 265 nm. When combined with cutting edge ab initio electronic structure and molecular dynamics calculations of both the excited and ground state molecules, the results provide unprecedented insights into both electronic and nuclear dynamics of this fundamental class of reactions. The initial ring opening and non-adiabatic coupling to the electronic ground state is shown to be driven by ballistic SC bond extension and to be complete within 350 femtoseconds. Theory and experiment also allow clear visualization of the rich ground-state dynamics involving formation of, and interconversion between, several ring opened isomers and the reformed cyclic structure, and fragmentation (CO loss) over much longer timescales.

physics.chem-ph↗

arXiv2019

Time-resolved inner-shell photoelectron spectroscopy: from a bound molecule to an isolated atom

Due to its element- and site-specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH$_3$I) is investigated by ionization above the iodine 4d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.

physics.chem-ph↗

arXiv2018

Photophysics of indole upon x-ray absorption

A photofragmentation study of gas-phase indole (C$_8$H$_7$N) upon single-photon ionization at a photon energy of 420 eV is presented. Indole was primarily inner-shell ionized at its nitrogen and carbon $1s$ orbitals. Electrons and ions were measured in coincidence by means of velocity map imaging. The angular relationship between ionic fragments is discussed along with the possibility to use the angle-resolved coincidence detection to perform experiments on molecules that are strongly oriented in their recoil-frame. The coincident measurement of electrons and ions revealed fragmentation-pathway-dependent electron spectra, linking the structural fragmentation dynamics to different electronic excitations. Evidence for photoelectron-impact self-ionization was observed.

physics.atm-clus↗

arXiv2017

Coulomb explosion imaging of concurrent CH$_{2}$BrI photodissociation dynamics

The dynamics following laser-induced molecular photodissociation of gas-phase CH$_{2}$BrI at 271.6 nm were investigated by time-resolved Coulomb explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment momenta reveal that CH$_{2}$BrI undergoes C-I cleavage, depositing 65.6% of the available energy into internal product states, and that absorption of a second UV photon breaks the C-Br bond of CH$_{2}$Br. Simulations confirm that this mechanism is consistent with previous data recorded at 248 nm, demonstrating the sensitivity of Coulomb explosion imaging as a real-time probe of chemical dynamics.

physics.chem-ph↗

arXiv2017

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↗