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We present experimental measurements and theoretical calculations for the photoionization of CH4 at the carbon K-edge. Measurements performed using cold target recoil ion momentum spectroscopy (COLTRIMS) combined with complex Kohn variational calculations of the photoelectron in the molecular frame demonstrate the surprising result that the low energy photoelectrons effectively image the molecule by emerging along the bond axes. Furthermore, we observe a dynamic breakdown of axial recoil behaviour in one of the dissociation pathways of the intermediate dication, which we interpret using electronic structure calculations. [ABSTRACT FROM AUTHOR]

In this paper, we shed new light on the molecular photoionization of a diatomic molecule. We will elaborate the differences and analogy between a quantum optical and light-matter interaction approach in a study of K-shell photoionization of N2 in which the photoelectron and the subsequently emitted Auger electron are both measured in coincidence in the body fixed frame of the molecule. The two electrons form an entangled state inside a double slit. By changing the photon energy we create different types of interference in the photoelectron and the Auger electron wave. [ABSTRACT FROM AUTHOR]

In this paper, we shed new light on the molecular photoionization of a diatomic molecule. We will elaborate the differences and analogy between a quantum optical and light-matter interaction approach in a study of K-shell photoionization of N2 in which the photoelectron and the subsequently emitted Auger electron are both measured in coincidence in the body fixed frame of the molecule. The two electrons form an entangled state inside a double slit. By changing the photon energy we create different types of interference in the photoelectron and the Auger electron wave. [ABSTRACT FROM AUTHOR]

The photon-ion merged-beams technique has been employed at the new Photon-Ion spectrometer at PETRA III for measuring multiple photoionization of Xeq + (q = 1–5) ions. Total ionization cross sections have been obtained on an absolute scale for the dominant ionization reactions of the type hν + Xeq + → Xer + + (q − r)e− with product charge states q + 2 ⩽ r ⩽ 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. [ABSTRACT FROM AUTHOR]

We investigate the ionization of HeNe from below the He ls3p excitation to the He ionization threshold. We observe HeNe+ ions with an enhancement by more than a factor of 60 when the He side couples resonantly to the radiation field. These ions are an experimental proof of a two-center resonant photoionization mechanism predicted by Najjari et al. [Phys. Rev. Lett. 105, 153002 (2010)]. Furthermore, our data provide electronic and vibrational state resolved decay widths of interatomic Coulombic decay in HeNe dimers. We find that the interatomic Coulombic decay lifetime strongly increases with increasing vibrational state. [ABSTRACT FROM AUTHOR]

The wave nature of particles is rarely observed, in part because of their very short de Brogue wavelengths in most situations. However, even with wavelengths close to the size of their surroundings, the particles couple to their environment (for example, by gravity, Coulomb interaction, or thermal radiation). These couplings shift the wave phases, often in an uncontrolled way, and the resulting decoherence, or loss of phase integrity, is thought to be a main cause of the transition from quantum to classical behavior. How much interaction is needed to induce this transition? Here we show that a photoelectron and two protons form a minimum particle/slit system and that a single additional electron constitutes a minimum environment. Interference fringes observed in the angular distribution of a single electron are lost through its Coulomb interaction with a second electron, though the correlated momenta of the entangled electron pair continue to exhibit quantum interference. [ABSTRACT FROM AUTHOR]

We investigate K-shell ionization of N2 at 40 keV photon energy. Using a cold target recoil ion momentum spectroscopy reaction microscope, we determine the vector momenta of the photoelectron, the Auger electron, and both N+ fragments. These fully differential data show that the dissociation process of the N22+ ion is significantly modified not only by the recoil momentum of the photoelectron but also by the photon momentum and the momentum of the emitted Auger electron. We find that the recoil energy introduced by the photon and the photoelectron momentum is partitioned with a ratio of approximately 30:70 between the Auger electron and fragment ion kinetic energies, respectively. We also observe that the photon momentum induces an additional rotation of the molecular ion. [ABSTRACT FROM AUTHOR]

It is commonly accepted that the magnitude of a photoelectron circular dichroism (PECD) is governed by the ability of an outgoing photoelectron wave packet to probe the chiral asymmetry of a molecule. To be able to accumulate this characteristic asymmetry while escaping the chiral ion, photoelectrons need to have relatively small kinetic energies of up to a few tens of electron volts. Here, we demonstrate a substantial PECD for very fast photoelectrons above 500 eV kinetic energy released from methyloxirane by a participator resonant Auger decay of its lowermost O 1s excitation. This effect emerges as a result of the Fano interference between the direct and resonant photoionization pathways, notwithstanding that their individual effects are negligibly small. The resulting dichroic parameter has an anomalous dispersion: It changes its sign across the resonance, which can be considered as an analogue of the Cotton effect in the x-ray regime. [ABSTRACT FROM AUTHOR]

We experimentally study 2p photoionization of neon dimers (Ne2) at a photon energy of hν = 36.56 eV. By postselection of ionization events which lead to a dissociation into Ne+ + Ne we obtain the photoelectron angular emission distribution in the molecular frame. This distribution is symmetric with respect to the direction of the charged vs neutral fragment. It shows an inverted Cohen-Fano double slit interference pattern of two spherical waves emitted coherently but with opposite phases from the two atoms of the dimer. [ABSTRACT FROM AUTHOR]