We have measured triple differential momentum distributions for electron detachment in collisions of 30- and 300-keV anions (C− and Si−) with atoms and molecules (He, Ar, and N2). The entire angular range of the ejected electrons was covered. The binary encounter ring, well known from positive ion-atom collisions, was observed in most cases. In a quasifree-electron scattering model this structure represents elastic scattering of the active electron from the target. However, especially for the slowest projectiles, this model fails to reproduce the angular distributions. In this regime it is probably necessary to use quasimolecular models to describe the collision. Indications for a projectile cusp are observed, implying that excitation-induced dipole moments in the ion projectile may be important. Published by the American Physical Society 2024

A new experimental setup has been developed to investigate the reactions of molecular ions and charged clusters with a variety of projectile beams. An Electrostatic Ion Beam Trap (EIBT) stores fast ions at keV energies in an oscillatory motion. By crossing it with a projectile beam, e.g., an IR laser, molecular reactions can be induced. We implemented a Reaction Microscope (REMI) in the field-free region of the EIBT to perform coincidence spectroscopy on the resulting reaction products. In contrast to prior experiments, this unique combination of techniques allows us to measure the 3D momentum-vectors of ions, electrons, and neutrals as reaction products in coincidence. At the same time, the EIBT allows for advanced target preparation techniques, e.g., relaxation of hot molecules during storage times of up to seconds, autoresonance cooling, and recycling of target species, which are difficult to prepare. Otherwise, the TrapREMI setup can be connected to a variety of projectile sources, e.g., atomic gas jets, large-scale radiation facilities, and ultrashort laser pulses, which enable even time-resolved studies. Here, we describe the setup and a first photodissociation experiment on H2+, which demonstrates the ion-neutral coincidence detection in the TrapREMI.

We present a compact experimental setup for performing attosecond-pump-infrared-probe experiments with long-time delay stability. The robustness of the setup is demonstrated over a two-day acquisition time in two-photon photoionization of argon in the photon-energy range 17-33 eV. The propagation of the input infrared pulse, as driving pulse for the high-order harmonic generation process and for the generation of the sidebands of the main photoelectron peaks, through the main optical components is simulated and discussed. Our setup allows us to perform attosecond experiments with an overall stability of +/- 40as.

We demonstrate the complete reconstruction of the electric field of visible-infrared pulses with energy as low as a few tens of nanojoules. The technique allows for the reconstruction of the instantaneous electric field vector direction and magnitude, thus giving access to the characterisation of pulses with an arbitrary time-dependent polarisation state. The technique combines extreme ultraviolet interferometry with the generation of isolated attosecond pulses.

A kinematically complete experiment on two-photon double ionization of Ar by free-electron laser radiation with a photon energy of 27.93 eV was performed. The electron energy spectra show that double ionization is dominated by the sequential process. Comparison of the electron angular distributions to our data for single ionization and to theory confirms that even in the sequential process the electrons from both ionization steps are correlated with each other through polarization of the intermediate Ar+ state. Furthermore, a very important role of autoionization in both ionization steps is found.

With a XUV-pump/THz-probe scheme the decay of excited O2 cations that were produced by irradiation with XUV photons has been investigated using a Reaction Microscope (ReMi) at the free-electron-laser FLASH in Hamburg. The temporal profile of electrons emitted due to autoionization of Rydberg states C 4 Σ u − ( n l σ g ) has been traced using THz streaking. This way the relaxation dynamics was followed. The relative shift in phase between photoelectrons and autoionization electrons was analyzed with respect to emission time delays or autoionization lifetimes.

Visualizing chemical reactions as they occur requires atomic spatial and femtosecond temporal resolution. Here, we report imaging of the molecular structure of acetylene (C2H2) 9 femtoseconds after ionization. Using mid-infrared laser-induced electron diffraction (LIED), we obtained snapshots as a proton departs the [C2H2](2+) ion. By introducing an additional laser field, we also demonstrate control over the ultrafast dissociation process and resolve different bond dynamics for molecules oriented parallel versus perpendicular to the LIED field. These measurements are in excellent agreement with a quantum chemical description of field-dressed molecular dynamics.

An electrostatic cryogenic storage ring, CSR, for beams of anions and cations with up to 300 keV kinetic energy per unit charge has been designed, constructed, and put into operation. With a circumference of 35 m, the ion-beam vacuum chambers and all beam optics are in a cryostat and cooled by a closed-cycle liquid helium system. At temperatures as low as (5.5 ± 1) K inside the ring, storage time constants of several minutes up to almost an hour were observed for atomic and molecular, anion and cation beams at an energy of 60 keV. The ion-beam intensity, energy-dependent closed-orbit shifts (dispersion), and the focusing properties of the machine were studied by a system of capacitive pickups. The Schottky-noise spectrum of the stored ions revealed a broadening of the momentum distribution on a time scale of 1000 s. Photodetachment of stored anions was used in the beam lifetime measurements. The detachment rate by anion collisions with residual-gas molecules was found to be extremely low. A residual-gas density below 140 cm(-3) is derived, equivalent to a room-temperature pressure below 10(-14) mbar. Fast atomic, molecular, and cluster ion beams stored for long periods of time in a cryogenic environment will allow experiments on collision- and radiation-induced fragmentation processes of ions in known internal quantum states with merged and crossed photon and particle beams.

Intense long wavelength (λ ≥ 2 μm) laser pulses enable experiments in the tunneling ionization regime (γ ≪ 1) and reveal surprising low electron energy features, which can not be described with the strong-field approximation (SFA). These features, universal for all target species, include the low-energy structure (LES), the very-low-energy structure (VLES) and the zero-energy structure (ZES). Using full 3D electron-ion coincidence detection in combination with our ultrafast 160 kHz mid-IR source, we reveal the entire 3D momentum spectrum well below 1 eV. Quantum and classical simulations allow for an interpretation of the LES, VLES and of the newly identified ZES.

Laser-induced electron diffraction is a developing dynamical imaging technique that is already able to probe molecular dynamics at few-femtosecond temporal resolutions and has the potential to reach the sub-femtosecond level. Here we provide the recipe for the extension of the technique to polyatomic molecules and we demonstrate the method by extracting the structure of aligned and anti-aligned acetylene (C2H2). We show that multiple bond lengths can be simultaneously imaged at high accuracy including elusive hydrogen containing bonds. Our results open the door to the investigation of larger complex molecules and the realization of a true molecular movie.

We report the simultaneous retrieval of multiple bond lengths of the polyatomic molecule C 2 H 2 by coherent “self-electron” wave packets generated by the interaction of the molecular target with intense mid-IR laser pulses [1].

Interatomic Coulombic Decay (ICD) is a relaxation phenomenon, which takes place in weakly bound atomic and molecular systems, typically within a few to hundreds of femtoseconds depending on the system and the particular decay mechanism. The creation of ICD-active states requires the production of highly excited systems, usually populated by innershell ionization or excitation. To this end, XUV and X-ray radiation from synchrotrons was conventionally applied for the majority of experiments due to the desired state-selective ionization of certain sub-shells. The advent of Free-Electron Lasers (FELs) has enabled an entirely new class of experiments, which finally allow to trace ICD directly in the time domain due to the femtosecond pulse duration. Within this paper, the first time-resolved ICD measurement using an XUV-pump–XUV-probe scheme will be discussed in detail. The experiment was performed on neon dimers and ICD was triggered by removing a 2s electron from one of the neon atoms using a 58 eV pulse from the FEL in Hamburg (FLASH). The onset of ICD was probed with a delayed copy of the trigger pulse that further ionized one of the two Ne+ ions emerging after ICD. Thus, the delay-dependent yield of coincident Ne+ + Ne2+ ion pairs contains the lifetime of the 2s-innershell vacancy decaying via ICD. The result of 150 fs ± 50 fs is in good agreement with theory but only for those calculations that explicitly take nuclear motion into account.

The cryogenic storage ring (CSR) for positive and negative atomic, molecular and cluster ions is starting operation at the Max Planck Institute for Nuclear Physics in Heidelberg.

We present time-resolved femtosecond photoelectron momentum images and angular distributions of dissociating, laser-aligned 1,4-dibromobenzene (C6H4Br2) molecules measured in a near-infrared pump, soft-x-ray probe experiment performed at an x-ray free-electron laser. The observed alignment dependence of the bromine 2p photoelectron angular distributions is compared to density functional theory calculations and interpreted in terms of photoelectron diffraction. While no clear time-dependent effects are observed in the angular distribution of the Br(2p) photoelectrons, other, low-energy electrons show a pronounced dependence on the time delay between the near-infrared laser and the x-ray pulse.

The dynamics of multi-photon induced fragmentation of N2 has been investigated in XUV-pump/XUV-probe experiments at the Free-Electron Laser in Hamburg (FLASH) by recording the ion kinetic energy release(KER) and angular distributions for various dissociation- and Coulomb-explosion channels as a function of the pump-probe delay-time.

Few-photon induced ultrafast dynamics in acetylene (C2H2) leading to several dissociation channels-deprotonation (H++C2H+ and H++C2H2+), symmetric break-up (CH++CH+) and isomerization (C++CH2+)-were investigated employing the (XUV; extreme ultra-violet)-pump-(XUV; extreme ultra-violet)-probe scheme at the free-electron laser in Hamburg, combined with multi-hit coincidence detection. The kinetic energy releases and fragment-ion momentum distributions for various decay channels are presented. The C++CH2+ and H++C2H2+ channels reveal clear signatures of ultrafast molecular mechanisms, demonstrating potential applications of our pump-probe technique to complex systems in order to study a large variety of ultrafast phenomena in the XUV regime.

The ionization and fragmentation of two selenium containing hydrocarbon molecules, methylselenol (CH3SeH) and ethylselenol (C2H5SeH), by intense (>1017 W cm−2) 5 fs x-ray pulses with photon energies of 1.7 and 2 keV has been studied by means of coincident ion momentum spectroscopy. Measuring charge states and ion kinetic energies, we find signatures of charge redistribution within the molecular environment. Furthermore, by analyzing fragment ion angular correlations, we can determine the laboratory-frame orientation of individual molecules and thus investigate the fragmentation dynamics in the molecular frame. This allows distinguishing protons originating from different molecular sites along with identifying the reaction channels that lead to their emission.

Using a split-mirror setup attached to a Reaction Microscope at the Free electron LASer in Hamburg (FLASH) we traced as function of time the migration of a hydrogen atom in C2H4+ from one end of the molecule to the other by coincident CH+ + CH3+ fragment detection. In addition, the observed H-3(+)+C2H+ channel provides for the first time evidence for an isomerization-induced formation mechanism of H-3(+) molecules.

Two-component nanoplasmas generated by strong-field ionization of doped helium nanodroplets are studied in a pump–probe experiment using few-cycle laser pulses in combination with molecular dynamics simulations. High yields of helium ions and a pronounced resonance structure in the pump–probe transients which is droplet size dependent reveal the evolution of the dopant-induced helium nanoplasma with an active role for He shells in the ensuing dynamics. The pump–probe dynamics is interpreted in terms of strong inner ionization by the pump pulse and resonant heating by the probe pulse which controls the final charge states detected via the frustration of electron–ion recombination.

Using a split focusing mirror, XUV pump–probe measurements have been performed at the free-electron laser at Hamburg (FLASH). The obtained non-linear autocorrelation signals can be used to characterize the ultra-short photon pulses generated by the machine at different control parameters.