Kevin Henrichs

Absolute Configuration from Different Multifragmentation Pathways in Light-Induced Coulomb Explosion Imaging.

The absolute configuration of individual small molecules in the gas phase can be determined directly by light-induced Coulomb explosion imaging (CEI). Herein, this approach is demonstrated for ionization with a single X-ray photon from a synchrotron light source, leading to enhanced efficiency and faster fragmentation as compared to previous experiments with a femtosecond laser. In addition, it is shown that even incomplete fragmentation pathways of individual molecules from a racemic CHBrClF sample can give access to the absolute configuration in CEI. This leads to a significant increase of the applicability of the method as compared to the previously reported complete break-up into atomic ions and can pave the way for routine stereochemical analysis of larger chiral molecules by light-induced CEI.

Electron spin polarization in strong-field ionization of xenon atoms

Electron spin polarization is experimentally detected and investigated via strong-field ionization of xenon atoms.

Observation of Enhanced Chiral Asymmetries in the Inner-Shell Photoionization of Uniaxially Oriented Methyloxirane Enantiomers

Most large molecules are chiral in their structure: they exist as two enantiomers, which are mirror images of each other. Whereas the rovibronic sublevels of two enantiomers are almost identical (neglecting a minuscular effect of the weak interaction), it turns out that the photoelectric effect is sensitive to the absolute configuration of the ionized enantiomer. Indeed, photoionization of randomly oriented enantiomers by left or right circularly polarized light results in a slightly different electron flux parallel or antiparallel with respect to the photon propagation direction-an effect termed photoelectron circular dichroism (PECD). Our comprehensive study demonstrates that the origin of PECD can be found in the molecular frame electron emission pattern connecting PECD to other fundamental photophysical effects such as the circular dichroism in angular distributions (CDAD). Accordingly, distinct spatial orientations of a chiral molecule enhance the PECD by a factor of about 10.

Ultrafast preparation and detection of ring currents in single atoms

Quantum particles can penetrate potential barriers by tunnelling1. If that barrier is rotating, the tunnelling process is modified2,3. This is typical for electrons in atoms, molecules or solids exposed to strong circularly polarized laser pulses4–6. Here we measure how the transmission probability through a rotating tunnel depends on the sign of the magnetic quantum number m of the electron and thus on the initial direction of rotation of its quantum phase. We further show that our findings agree with a semiclassical picture, in which the electron keeps part of that rotary motion on its way through the tunnel by measuring m-dependent modification of the electron emission pattern. These findings are relevant for attosecond metrology as well as for interpretation of strong-field electron emission from atoms and molecules7–14 and directly demonstrate the creation of ring currents in bound states of ions with attosecond precision. In solids, this could open a way to inducing and controlling ring-current-related topological phenomena15.When an electron with specific orbit — either clockwise or anticlockwise — in a rare gas atom is selectively ionized, the remaining ion will possess a stationary ring current, which can be probed in a time-delayed second ionization step.

Born in weak fields: below-threshold photoelectron dynamics

We investigate the dynamics of ultra-low kinetic energy photoelectrons. Many experimental techniques employed for the detection of photoelectrons require the presence of (more or less) weak electric extraction fields in order to perform the measurement. Our studies show that ultra-low energy photoelectrons exhibit a characteristic shift in their apparent measured momentum when the target system is exposed to such static electric fields. Already fields as weak as 1 V cm–1 have an observable influence on the detected electron momentum. This apparent shift is demonstrated by an experiment on zero energy photoelectrons emitted from He and explained through theoretical model calculations.

Electron spin polarization in strong-field ionization and the effect of spin in attoclock measurements

Spin plays a fundamental role in the electronic structure of matter, from single atoms and molecules through to condensed matter. However, spin dynamics and the spin response of electrons to ultra-short, strong laser pulses has remained largely unexplored until today. In 2011 and 2013, pioneering theoretical work [1, 2] extended the fundamental PPT theory [3] to treat ionization of p+ and p” electrons by circular fields. This work predicted the sensitivity of ionization probabilities in strong field ionization using circular fields to the magnetic quantum number, showing that counter rotating electrons can tunnel ionize easier. It also predicted the possibility to obtain spin polarized electrons from strong, circularly polarized fields with a high degree of efficiency. The preference of ionization was later confirmed experimentally by [4], however, the experiment in [4] did not provide a confirmation of the spin polarization predictions.

Direct determination of molecular handedness via coulomb explosion imaging

In this work, we show that the direct determination of a chiral molecules absolute configuration can be achieved with Coulomb Explosion Imaging in a COLTRIMS reaction microscope. We compare the results after ionisation with femto-second laser pulses and with X-ray synchrotron light. Different fragmentation pathways of the prototypical chiral molecule CHBrClF are identified that carry information on the handedness. The applicabilty of the technique towards bigger molecules is discussed.

Transfer ionization of D+ and He+ projectiles with H2-molecules – electron emission dependency on the internuclear axis

Its well known for atomic targets that the ionization in transfer ionization originates from electron knock-off or initial state correlated shake-off. For H2 molecules we have observed a similar behavior and additionally a dependency of the electron emission from the internuclear axis