arXiv subjects

J. Ullrich

Publications and source records attributed to J. Ullrich.

At least 19 recordsLinked to original sources

arXiv2021

Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction

Ubiquitous to most molecular scattering methods is the challenge to retrieve bond distance and angle from the scattering signals since this requires convergence of pattern matching algorithms or fitting methods. This problem is typically exacerbated when imaging larger molecules or for dynamic systems with little a priori knowledge. Here, we employ laser-induced electron diffraction (LIED) which is a powerful means to determine the precise atomic configuration of an isolated gas-phase molecule with picometre spatial and attosecond temporal precision. We introduce a simple molecular retrieval method, which is based only on the identification of critical points in the oscillating molecular interference scattering signal that is extracted directly from the laboratory-frame photoelectron spectrum. The method is compared with a Fourier-based retrieval method, and we show that both methods correctly retrieve the asymmetrically stretched and bent field-dressed configuration of the asymmetric top molecule carbonyl sulfide (OCS), which is confirmed by our quantum-classical calculations.

physics.atom-ph↗

arXiv2019

Vectorial optical field reconstruction by attosecond spectral interferometry

An electrical pulse E(t) is completely defined by its time-dependent amplitude and polarisation direction. For optical pulses the manipulation and characterisation of the light polarisation state is fundamental due to its relevance in several scientific and technological fields. In this work we demonstrate the complete temporal reconstruction of the electric field of few-cycle pulses with a complex time-dependent polarisation. Our experimental approach is based on extreme ultraviolet interferometry with isolated attosecond pulses and on the demonstration that the motion of an attosecond electron wave packet is sensitive to perturbing fields only along the direction of its motion. By exploiting the sensitivity of interferometric techniques and by controlling the emission and acceleration direction of the wave packet, pulses with energies as low as few hundreds of nanojoules can be reconstructed. Our approach opens the possibility to completely characterise the electric field of the pulses typically used in visible pump-probe spectroscopy.

physics.optics↗

arXiv2018

Attosecond electronic recollision as field detector

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.

physics.optics↗

arXiv2016

Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets

The ability to directly follow and time resolve the rearrangement of the nuclei within molecules is a frontier of science that requires atomic spatial and few-femtosecond temporal resolutions. While laser induced electron diffraction can meet these requirements, it was recently concluded that molecules with particular orbital symmetries (such as πg) cannot be imaged using purely backscattering electron wave packets without molecular alignment. Here, we demonstrate, in direct contradiction to these findings, that the orientation and shape of molecular orbitals presents no impediment for retrieving molecular structure with adequate sampling of the momentum transfer space. We overcome previous issues by showcasing retrieval of the structure of randomly oriented O2 and C2H2 molecules, with πg and πu symmetries, respectively, and where their ionisation probabilities do not maximise along their molecular axes. While this removes a serious bottleneck for laser induced diffraction imaging, we find unexpectedly strong back scattering contributions from low-Z atoms.

physics.atom-ph↗

arXiv2014

Imaging Molecular Structure through Femtosecond Photoelectron Diffraction on Aligned and Oriented Gas-Phase Molecules

This paper gives an account of our progress towards performing femtosecond time-resolved photoelectron diffraction on gas-phase molecules in a pump-probe setup combining optical lasers and an X-ray Free-Electron Laser. We present results of two experiments aimed at measuring photoelectron angular distributions of laser-aligned 1-ethynyl-4-fluorobenzene (C8H5F) and dissociating, laseraligned 1,4-dibromobenzene (C6H4Br2) molecules and discuss them in the larger context of photoelectron diffraction on gas-phase molecules. We also show how the strong nanosecond laser pulse used for adiabatically laser-aligning the molecules influences the measured electron and ion spectra and angular distributions, and discuss how this may affect the outcome of future time-resolved photoelectron diffraction experiments.

physics.atom-ph↗

arXiv2014

Absolute cross sections for photoionization of Xe$^{q+}$ ions (1 $\le$ q $\le$ 5) at the 3d ionization threshold

The photon-ion merged-beams technique has been employed at the new Photon-Ion spectrometer at PETRA III (PIPE) for measuring multiple photoionization of Xe$^{q+}$ (q=1-5) ions. Total ionization cross sections have been obtained on an absolute scale for the dominant ionization reactions of the type hν+ Xe$^{q+}$ $\to$ Xe$^{r+}$ + (q-r) e$^-$ with product charge states q+2 $\le$ r $\le$ q+5. Prominent ionization features are observed in the photon-energy range 650-750 eV, which are associated with excitation or ionization of an inner-shell 3d electron. Single-configuration Dirac-Fock calculations agree quantitatively with the experimental cross sections for non-resonant photoabsorption, but fail to reproduce all details of the measured ionization resonance structures.

physics.atom-ph↗

arXiv2014

Watching the acetylene vinylidene intramolecular reaction in real time

It is a long-standing dream of scientists to capture the ultra-fast dynamics of molecular or chemical reactions in real time and to make a molecular movie. With free-electron lasers delivering extreme ultraviolet (XUV) light at unprecedented intensities, in combination with pump-probe schemes, it is now possible to visualize structural changes on the femtosecond time scale in photo-excited molecules. In hydrocarbons the absorption of a single photon may trigger the migration of a hydrogen atom within the molecule. Here, such a reaction was filmed in acetylene molecules (C2H2) showing a partial migration of one of the protons along the carbon backbone which is consistent with dynamics calculations on ab initio potential energy surfaces. Our approach opens attractive perspectives and potential applications for a large variety of XUV-induced ultra-fast phenomena in molecules relevant to physics, chemistry, and biology.

physics.atm-clus↗

arXiv2013

Time-Resolved Measurement of Interatomic Coulombic Decay in Ne_2

The lifetime of interatomic Coulombic decay (ICD) [L. S. Cederbaum et al., Phys. Rev. Lett. 79, 4778 (1997)] in Ne_2 is determined via an extreme ultraviolet pump-probe experiment at the Free-Electron Laser in Hamburg. The pump pulse creates a 2s inner-shell vacancy in one of the two Ne atoms, whereupon the ionized dimer undergoes ICD resulting in a repulsive Ne^{+}(2p^{-1}) - Ne^{+}(2p^{-1}) state, which is probed with a second pulse, removing a further electron. The yield of coincident Ne^{+} - Ne^{2+} pairs is recorded as a function of the pump-probe delay, allowing us to deduce the ICD lifetime of the Ne_{2}^{+}(2s^{-1}) state to be (150 +/- 50) fs in agreement with quantum calculations.

physics.atm-clus↗

arXiv2013

X-ray resonant photoexcitation: line widths and energies of Kα transitions in highly charged Fe ions

Photoabsorption by and fluorescence of the Kα transitions in highly charged iron ions are essential mechanisms for X-ray radiation transfer in astrophysical environments. We study photoabsorption due to the main Kα transitions in highly charged iron ions from heliumlike to fluorinelike (Fe 24+...17+) using monochromatic X-rays around 6.6 keV at the PETRA III synchrotron photon source. Natural linewidths were determined with hitherto unattained accuracy. The observed transitions are of particular interest for the understanding of photoexcited plasmas found in X-ray binaries and active galactic nuclei.

physics.atom-ph↗

arXiv2013

Major role of multielectronic K-L inter-shell resonant recombination processes in Li- to O-like ions of Ar, Fe, and Kr

Dielectronic and higher-order resonant electron recombination processes including a K-shell excitation were systematically measured at high resolution in electron beam ion traps. Storing highly charged Ar, Fe, and Kr ions, the dependence on atomic number Z of the contribution of these processes to the total recombination cross section was studied and compared with theoretical calculations. Large higher-order resonant recombination contributions are found, especially for systems with 10<Z<36. In some cases, they even surpass the strength of the dielectronic channel, which was hitherto presumed to be always the dominant one. These findings have consequences for the modeling of high-temperatur plasmas. Features attributed to inter-shell quadruelectronic recombination were also observed. The experimental data obtained for the He-like to O-like isoelectronic sequences compare well with the results of advanced relativistic distorted-wave calculations employing multiconfiguration Dirac-Fock bound state wave functions that include threefold and fourfold excitations.

physics.atom-ph↗

arXiv2013

Decay rate measurement of the first vibrationally excited state of MgH$^+$ in a cryogenic Paul trap

We present a method to measure the decay rate of the first excited vibrational state of simple polar molecular ions being part of a Coulomb crystal in a cryogenic linear Paul trap. Specifically, we have monitored the decay of the $|ν$=$1,J$=$1 \rangle_X$ towards the $|ν$=$0,J$=$0 \rangle_X$ level in MgH$^+$ by saturated laser excitation of the $|ν$=$0,J$=$2 \rangle_X$-$|ν$=$1,J$=$1 \rangle_X$ transition followed by state selective resonance enhanced two-photon dissociation out of the $|ν$=$0,J$=$2 \rangle_X$ level. The technique enables the determination of decay rates, and thus absorption strengths, with an accuracy at the few percent level.

physics.atom-ph↗

arXiv2013

Enabling high-precision 3D strong-field measurements - Ionization with low-frequency fields in the tunneling regime

Ionization of an atom or molecule presents surprising richness beyond our current understanding: strong-field ionization with low-frequency fields recently revealed unexpected kinetic energy structures (1, 2). A solid grasp on electron dynamics is however pre-requisite for attosecond-resolution recollision imaging (3), orbital tomography (4), for coherent sources of keV light (5), or to produce zeptosecond-duration x-rays (6). We present a methodology that enables scrutinizing strong-field dynamics at an unprecedented level. Our method provides high-precision measurements only 1 meV above the threshold despite 5 orders higher ponderomotive energies. Such feat was realized with a specifically developed ultrafast mid-IR light source in combination with a reaction microscope. We observe electron dynamics in the tunneling regime (γ = 0.3) and show first 3D momentum distributions demonstrating surprising new observations of near-zero momentum electrons and low momentum structures, below the eV, despite quiver energies of 95 eV.

physics.atom-ph↗

arXiv2012

Evolution of dopant-induced helium nanoplasmas

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, droplet size-dependent resonance structure in the pump-probe transients reveal the evolution of the dopant-induced helium nanoplasma. 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.

physics.atm-clus↗

arXiv2011

First Use of High Charge States for Mass Measurements of Short-lived Nuclides in a Penning Trap

Penning trap mass measurements of short-lived nuclides have been performed for the first time with highly-charged ions (HCI), using the TITAN facility at TRIUMF. Compared to singly-charged ions, this provides an improvement in experimental precision that scales with the charge state q. Neutron-deficient Rb-isotopes have been charge bred in an electron beam ion trap to q = 8 - 12+ prior to injection into the Penning trap. In combination with the Ramsey excitation scheme, this unique setup creating low energy, highly-charged ions at a radioactive beam facility opens the door to unrivalled precision with gains of 1-2 orders of magnitude. The method is particularly suited for short-lived nuclides such as the superallowed β emitter 74Rb (T1/2 = 65 ms). The determination of its atomic mass and an improved QEC-value are presented.

nucl-ex↗

arXiv2011

Dopant induced ignition of helium nanodroplets in intense few-cycle laser pulses

We demonstrate ultrafast resonant energy absorption of rare-gas doped He nanodroplets from intense few-cycle (~10 fs) laser pulses. We find that less than 10 dopant atoms "ignite" the droplet to generate a non-spherical electronic nanoplasma resulting ultimately in complete ionization and disintegration of all atoms, although the pristine He droplet is transparent for the laser intensities applied. Our calculations at those intensities reveal that the minimal pulse length required for ignition is about 9 fs.

physics.atm-clus↗

arXiv2009

Imaging Molecules from Within: Ultra-fast, Ångström Scale Structure Determination of Molecules via Photoelectron Holography using Free Electron Lasers

A new scheme based on (i) upcoming brilliant X-ray Free Electron Laser (FEL) sources, (ii) novel energy and angular dispersive, large-area electron imagers and (iii) the well-known photoelectron holography is elaborated that provides time-dependent three-dimensional structure determination of small to medium sized molecules with Ångström spatial and femtosecond time resolution. Inducing molecular dynamics, wave-packet motion, dissociation, passage through conical intersections or isomerization by a pump pulse this motion is visualized by the X-ray FEL probe pulse launching keV photoelectrons within few femtoseconds from specific and well-defined sites, deep core levels of individual atoms, inside the molecule. On their way out the photoelectrons are diffracted generating a hologram on the detector that encodes the molecular structure at the instant of photoionization, thus providing 'femtosecond snapshot images of the molecule from within'. Detailed calculations in various approximations of increasing sophistication are presented and three-dimensional retrieval of the spatial structure of the molecule with Ångström spatial resolution is demonstrated. Due to the large photo-absorption cross sections the method extends X-ray diffraction based, time-dependent structure investigations envisioned at FELs to new classes of samples that are not accessible by any other method. Among them are dilute samples in the gas phase such as aligned, oriented or conformer selected molecules, ultra-cold ensembles and/or molecular or cluster objects containing mainly light atoms that do not scatter X-rays efficiently.

physics.atom-ph↗

arXiv2009

Inelastic collisions of relativistic electrons with atomic targets assisted by a laser field

We consider inelastic collisions between relativistic electrons and atomic targets assisted by a low-frequency laser field in the case when this field is still much weaker than the typical internal fields in the target. Concentrating on target transitions we show that they can be substantially affected by the presence of the laser field. This may occur either via strong modifications in the motion of the relativistic electrons caused by the electron-laser interaction or via the Compton effect when the incident electrons convert laser photon(s) into photons with frequencies equal to target transition frequencies.

physics.atom-ph↗

arXiv2008

A new mechanism for electron transfer in fast ion-atomic collisions

We discuss a new mechanism for the electron capture in fast ion-atom collisions. Similarly like in the radiative capture, where the electron transfer occurs due to photon emission, within the mechanism under consideration the electron capture takes place due to the emission of an additional electron. This first order capture process leads to the so called transfer-ionization and has a number of interesting features, in particular, in the target frame it results in the electron emission mainly into the backward semi-sphere.

physics.atom-ph↗