Helium shows fascinating quantum phenomena unseen in any other element. In its liquid phase, it is the only known superfluid. The smallest aggregates of helium, the dimer (He 2 ) and the trimer (He 3 ) are, in their predicted structure, unique natural quantum objects. While one might intuitively expect the structure of 4 He 3 to be an equilateral triangle, a manifold of predictions on its shape have yielded an ongoing dispute for more than 20 years. These predictions range from 4 He 3 being mainly linear to being mainly an equilateral triangle. Here we show experimental images of the wave functions of 4 He 3 and 3 He 4 He 2 obtained by Coulomb explosion imaging of mass-selected clusters. We propose that 4 He 3 is a structureless random cloud and that 3 He 4 He 2 exists as a quantum halo state.
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.
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.
We investigate the contribution of Interatomic Coulombic Decay induced by ion impact in neon and argon dimers (Ne 2 and Ar 2 ) to the production of low energy electrons. Our experiments cover a broad range of perturbation strengths and reaction channels. We use 11.37 MeV/u S 14+ , 0.125 MeV/u He 1+ , 0.1625 MeV/u He 1+ and 0.150 MeV/u He 2+ as projectiles and study ionization, single and double electron transfer to the projectile as well as projectile electron loss processes.The application of a COLTRIMS reaction microscope enables us to retrieve the three-dimensional momentum vectors of the ion pairs of the fragmenting dimer into Ne q+ /Ne 1+ and Ar q+ /Ar 1+ (q = 1, 2, 3) in coincidence with at least one emitted electron.
The front cover artwork is provided by the groups of Reinhard Dörner (University of Frankfurt), Robert Berger (University of Marburg) and Jürgen Stohner (Zurich University for Applied Sciences, Wädenswil). The image shows how a single X‐ray photon from a synchrotron source induces the Coulomb Explosion of a prototypical chiral molecule (CHBrClF), allowing to distinguish the enantiomers and determine the absolute configuration. Read the full text of the article at 10.1002/cphc.201501118.
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