Because ICD is expected to take place universally in weakly bound aggregates containing light atoms between carbon and neon in the periodic table 2,3 , these results could have implications for our understanding of ionization damage in living tissues. NPHYS-2009-06-00979a 2 Electronic vacancy states can be produced in matter by ionizing radiation, such as X-ray photons or fast charged particles. When a state with a high electronic excitation energy has been produced by impact of such particles, electron correlation can cause the ejection of electrons. Auger decay is the best known representative of this class of secondary processes that is more generally termed autoionization. In other words, the mechanism is a concerted transition in which a single hole in an inner shell is replaced by two vacancies in the outer valence shells of two adjacent molecules, and a free electron. This decay channel was termed Intermolecular (Interatomic, in the case of atomic clusters) Coulombic Decay and was subsequently observed in rare gas clusters 4-7 .The process is shown schematically in Fig. 1. A resonant variant of ICD, which may take place after photoexcitation into an unoccupied orbital, has also been discussed [7][8][9] . In the present paper, we consider ICD of inner valence vacancy states, for which case the ejected electrons have a low kinetic energy.On the basis of energetic considerations, ICD can take place whenever the binding energy of the ionized state lies above the double ionization threshold of the corresponding cluster or liquid. This prerequisite for ICD is fulfilled in hydrogen-bonded systems 2,10 , but so far the process has not been seen. Calculations of the energy spectrum of electrons ejected by ICD of small water clusters give a hint as to why it has escaped observation: A broad, rather unstructured distribution of energies is expected, which peaks at zero eV 10 . Ifwe consider an experiment with a conventional electron energy analyser on a bulk or liquid NPHYS-2009-06-00979a 3 sample, an electron spectrum with this shape can hardly be distinguished from the "universal curve" 1 for secondary electrons (Fig. 2). In this respect our work differs from earlier experiments, which were either restricted to dimers 5-7 , or dealt with simpler cases where an ICD feature appears from simple electron kinetic energy spectra 4,8,9 . Producing primary electrons of a well-defined energy by photoionization and detecting them in coincidence with the ICD electron has allowed us to overcome the aforementioned problem. Here, we demonstrate that ICD follows the photoionization of medium-sized water clusters and show that -above the corresponding photoionization threshold -ICD electrons make an important contribution to the low kinetic energy spectrum.In our experiment, a jet of water clusters with a mean size 〈N〉 of 40 or 200 was used.Such clusters are believed to form amorphous structures, which resemble the hydrogenbonded network of liquid water rather than that of crystalline ice 11 . Inner valence vacancies were p...

Because of inversion symmetry and particle exchange, all constituents of homonuclear diatomic molecules are in a quantum mechanically non-local coherent state; this includes the nuclei and deep-lying core electrons. Hence, the molecular photoemission can be regarded as a natural double-slit experiment: coherent electron emission originates from two identical sites, and should give rise to characteristic interference patterns. However, the quantum coherence is obscured if the two possible symmetry states of the electronic wavefunction ('gerade' and 'ungerade') are degenerate; the sum of the two exactly resembles the distinguishable, incoherent emission from two localized core sites. Here we observe the coherence of core electrons in N(2) through a direct measurement of the interference exhibited in their emission. We also explore the gradual transition to a symmetry-broken system of localized electrons by comparing different isotope-substituted species--a phenomenon analogous to the acquisition of partial 'which-way' information in macroscopic double-slit experiments.

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 He 2 's binding energy of 151.9 ± 13.3 neV, which is in agreement with most recent calculations.clusters | helium dimer | wavefunction | tunneling A ttractive forces allow particles to condense into stable bound systems such as molecules or nuclei with a ground state and (in most cases) energetically excited bound states, as shown in Fig. 1. Classical particles situated in such a binding potential oscillate back and forth between two turning points. The regions beyond these points are inaccessible for a classical particle due to a lack of energy. Quantum particles, however, can penetrate into the potential barrier by a phenomenon known as "tunneling." Tunneling is omnipresent in nature and occurs on all energy scales from megaelectron volts in nuclear physics to electron volts in molecules and solids and to nanoelectron volts in optical lattices. For bound matter, the fraction of the probability density distribution in this classically forbidden region is usually small. For shallow short-range potentials, this situation can change dramatically: upon decreasing the potential depth, excited states are expelled one after the other as they become unbound (transition from A to B in Fig. 1). A further decrease of the potential depth effects the ground state as well, as more and more of its wavefunction expands into the tunneling region ( Fig. 1 C and D). Consequently, at the threshold (i.e., in the limit of vanishing binding energy), the size of the quantum system expands to infinity. For short-range potentials, this expansion is accompanied by the fact that the system becomes less "classical" and more quantumlike. Systems existing near that threshold (and therefore being dominated by the tunneling part of their wavefunction) are called "quantum halo states" (1). These states are known, for example, from nuclear physics where 11 Be and 11 Li form ...

For emission out of the molecule along the molecular axis, the direct wave interferes with an electron wave that is scattered an odd number of times and dominated by singlescattering (66% back-scattering), whereas for emission into the molecule, the direct

Extreme-ultraviolet to x-ray free-electron lasers (FELs) in operation for scientific applications are up to now single-user facilities. While most FELs generate around 100 photon pulses per second, FLASH at DESY can deliver almost two orders of magnitude more pulses in this time span due to its superconducting accelerator technology. This makes the facility a prime candidate to realize the next step in FELs-dividing the electron pulse trains into several FEL lines and delivering photon pulses to several users at the same time. Hence, FLASH has been extended with a second undulator line and self-amplified spontaneous emission (SASE) is demonstrated in both FELs simultaneously. FLASH can now deliver MHz pulse trains to two user experiments in parallel with individually selected photon beam characteristics. First results of the capabilities of this extension are shown with emphasis on independent variation of wavelength, repetition rate, and photon pulse length.

All the different Auger decay paths of Argon 2p holes have been characterized using a time of flight spectrometer of the magnetic bottle type. All electrons (the photoelectron and up to three Auger electrons) are detected in coincidence and resolved in energy. Double Auger decay is shown to proceed either through a direct process or by intense cascade paths, implying highly excited autoionizing Ar 2+ states, which are identified as Ar 2+ 3s -2 correlation satellites. TripleAuger decay is also observed and estimated to account for 0.2 % only of all Auger decay.

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The relaxation processes after non-resonant inner-shell photoionization are studied experimentally using electron–electron time-of-flight coincidence spectroscopy. Results for krypton 3d and xenon 4d as well as 3d photoionization are presented. The experimental data make it possible to disentangle sequential from simultaneous processes using the different electron emission characteristics as the differentiating property. For the population of final states having charges higher than 2, the measurements show a strong preference for sequential Auger cascade decay. Clear evidence for direct double Auger processes is found in the case of Xe 3d photoionization only.