S. Zeller

Imaging the structure of the trimer systems 4He3 and 3He4He2

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 (He2) and the trimer (He3) are, in their predicted structure, unique natural quantum objects. While one might intuitively expect the structure of (4)He3 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)He3 being mainly linear to being mainly an equilateral triangle. Here we show experimental images of the wave functions of (4)He3 and (3)He(4)He2 obtained by Coulomb explosion imaging of mass-selected clusters. We propose that (4)He3 is a structureless random cloud and that (3)He(4)He2 exists as a quantum halo state.

Imaging the He2 quantum halo state using a free electron laser

Significance In bound matter on all length scales, from nuclei to molecules to macroscopic solid objects, most of the density of the bound particles is within the range of the interaction potential which holds the system together. Quantum halos on the contrary are a type of matter where the particle density is mostly outside the range of the interaction potential in the tunneling region of the potential. Few examples of these fascinating systems are known in nuclear and molecular physics. The conceptually simplest halo system is made of only two particles. Here we experimentally image the wavefunction of the He2 quantum halo. It shows the predicted exponential shape of a tunneling wavefunction. Quantum tunneling is a ubiquitous phenomenon in nature and crucial for many technological applications. It allows quantum particles to reach regions in space which are energetically not accessible according to classical mechanics. In this “tunneling region,” the particle density is known to decay exponentially. This behavior is universal across all energy scales from nuclear physics to chemistry and solid state systems. Although typically only a small fraction of a particle wavefunction extends into the tunneling region, we present here an extreme quantum system: a gigantic molecule consisting of two helium atoms, with an 80% probability that its two nuclei will be found in this classical forbidden region. This circumstance allows us to directly image the exponentially decaying density of a tunneling particle, which we achieved for over two orders of magnitude. Imaging a tunneling particle shows one of the few features of our world that is truly universal: the probability to find one of the constituents of bound matter far away is never zero but decreases exponentially. The results were obtained by Coulomb explosion imaging using a free electron laser and furthermore yielded He2’s binding energy of 151.9±13.3 neV, which is in agreement with most recent calculations.

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.

Agreement of Experiment and Theory on the Single Ionization of Helium by Fast Proton Impact

Even though the study of ion-atom collisions is a mature field of atomic physics, large discrepancies between experiment and theoretical calculations are still common. Here we present experimental results with high momentum resolution on the single ionization of helium induced by 1-MeV protons, and we compare these to theoretical calculations. The overall agreement is strikingly good, and even the first Born approximation yields good agreement between theory and experiment. This has been expected for several decades, but so far has not been accomplished. The influence of projectile coherence effects on the measured data is briefly discussed in terms of an ongoing dispute on the existence of nodal structures in the electron angular emission distributions.

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.

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 Localization in Dissociating H2+ by Retroaction of a Photoelectron onto Its Source

We investigate the dissociation of H_{2}^{+} into a proton and a H^{0} after single ionization with photons of an energy close to the threshold. We find that the p^{+} and the H^{0} do not emerge symmetrically in the case of the H_{2}^{+} dissociating along the 1sσ_{g} ground state. Instead, a preference for the ejection of the p^{+} in the direction of the escaping photoelectron can be observed. This symmetry breaking is strongest for very small electron energies. Our experiment is consistent with a recent prediction by Serov and Kheifets [Phys. Rev. A 89, 031402 (2014)]. In their model, which treats the photoelectron classically, the symmetry breaking is induced by the retroaction of the long-range Coulomb potential onto the dissociating H_{2}^{+}.

Determination of Interatomic Potentials of He2, Ne2, Ar2, and H2 by Wave Function Imaging

We report on a direct method to measure the interatomic potential energy curve of diatomic systems. A cold target recoil ion momentum spectroscopy reaction microscope was used to measure the squares of the vibrational wave functions of H_{2}, He_{2}, Ne_{2}, and Ar_{2}. The Schrödinger equation relates the curvature of the wave function to the potential V(R) and therefore offers a simple but elegant way to extract the shape of the potential.

Single ionization of Helium at 0.5-2 MeV proton impact: On the quest for projectile coherence effects

J. Gatzke, F. Navarrete, M. Ciappina, H. Gatzke, O. Chuluunbaatar, S. A. Zaytsev, A. A. Bulychev, K. A. Kouzakov, A. Galstyan, M. Waitz, H.-K. Kim, T. Bauer, A. Laucke, S. Eckart, G. Kastirke, J. Müller, M. Ritzer, E. Bloch, M. Richter, K. Fehre, M. Kunitski, Ch. Müller, J. Voigtsberger, J. Rist, K. Pahl, M. Honig, M. Pitzer, M. Weller, I. Vela Pérez, J. Hoehl, G. Nalin, S. Grundmann, H. Maschkiwitz, C. Janke, S. Zeller, C. Goihl, Y. Herrman, D. Trabert, T. Jahnke, L. Ph. H. Schmidt, Yu. V. Popov, R. Dörner R. O. Barrachina, and M. S. Schöffler 1

Erratum: Electron Localization in Dissociating H2+ by Retroaction of a Photoelectron onto Its Source [Phys. Rev. Lett. 116 , 043001 (2016)]

This corrects the article DOI: 10.1103/PhysRevLett.116.043001.