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Electronically excited atoms or molecules may deexcite by emission of a secondary electron through an Auger-Meitner decay. This deexcitation process is typically considered to be exponential in time. This is strictly speaking, however, only true for the case of an atom. Here, we present a study experimentally demonstrating the non-exponential time dependence of the decay of an inner-shell hole in a diatomic molecule. In addition, we provide an intuitive explanation for the origin of the observed variation of the molecular lifetimes and their dependence on the kinetic energy of the ionic fragments measured in coincidence with the photoelectrons., Comment: 5 pages, 4 figures

We present the momentum distributions of the nucleus and of the electrons from double ionization of the helium atom by Compton scattering of photons with $h\nu=40$ keV. We find that the doubly charged ion momentum distribution is very close to the Compton profile of the nucleus in the ground state of the helium atom, and the momentum distribution of the singly charged ion to give a precise image of the electron Compton profile. To reproduce these results, non-relativistic calculations require the use of highly correlated initial- and final-state wavefunctions., Comment: 5 pages, 3 figures

We report on a joint experimental and theoretical study of photoelectron circular dichroism (PECD) in methyloxirane. By detecting O 1s-photoelectrons in coincidence with fragment ions, we deduce the molecule's orientation and photoelectron emission direction in the laboratory frame. Thereby, we retrieve a fourfold differential PECD clearly beyond 50%. This strong chiral asymmetry is reproduced by ab initio electronic structure calculations. Providing such a pronounced contrast makes PECD of fixed-in-space chiral molecules an even more sensitive tool for chiral recognition in the gas phase., Comment: 5 figures

X-ray as well as electron diffraction are powerful tools for structure determination of molecules. Studies on randomly oriented molecules in the gas-phase address cases in which molecular crystals cannot be generated or the interaction-free molecular structure is to be addressed. Such studies usually yield partial geometrical information, such as interatomic distances. Here, we present a complementary approach, which allows obtaining insight to the structure, handedness and even detailed geometrical features of molecules in the gas phase. Our approach combines Coulomb explosion imaging, the information that is encoded in the molecular frame diffraction pattern of core-shell photoelectrons and ab initio computations. Using a loop-like analysis scheme we are able to deduce specific molecular coordinates with sensitivity even to the handedness of chiral molecules and the positions of individual atoms, as, e.g., protons., Comment: 13 pages, 3 figures

We investigate the differential ionization probability of chiral molecules in the strong field regime as a function of the helicity of the incident light. To this end, we analyze the fourfold ionization of bromochlorofluoromethane (CHBrClF) with subsequent fragmentation into four charged fragments and different dissociation channels of the singly ionized methyloxirane. We observe a variation of the differential ionization probability in a range of several percent. Accordingly, we conclude that the helicity of light is a quantity that should be considered for the theoretical description of the strong field ionization rate of chiral molecules., Comment: 12 pages, 6 figures, submitted

We report on kinematically complete measurements and ab initio non-perturbative calculations of double ionization of He and H2 by a single 800 eV circularly polarized photon. We confirm the quasifree mechanism of photoionization for H2 and show how it originates from the two-electron cusp in the ground state of a two-electron target. Our approach establishes a new method for mapping electrons relative to each other and provides valuable insight into photoionization beyond the electric-dipole approximation., Comment: 7 pages, 4 figures

Lead halide perovskites are causing a change of paradigm in photovoltaics. Among other peculiarities, these perovskites exhibit an atypical temperature dependence of the fundamental optical gap: It decreases in energy with decreasing temperature. So far reports ascribe such a behavior to a particularly strong electron-phonon renormalization of the band gap, neglecting completely contributions from thermal expansion effects. However, high pressure experiments performed, for instance, on the archetypal perovskite MAPbI$_3$, where MA stands for methylammonium, yield a negative pressure coefficient for the gap of the tetragonal room-temperature phase, which speaks against the assumption of a negligible gap shift due to thermal expansion. On the basis of the high pressure results, we show here that for MAPbI$_3$ the temperature-induced gap renormalization due to electron-phonon interaction can only account for about 40\% of the total energy shift, thus implying thermal expansion to be the dominant term. Furthermore, this result possesses general validity, holding also for the tetragonal or cubic phase, stable at ambient conditions, of other halide perovskite counterparts., Comment: 24 pages (manuscript 17 pages + supplementary information 7 pages), 5 figures (manuscript 4 figures + supplementary information 1 figure), submitted to J. Phys. Chem. Lett

We suggest that low energy electrons, released by resonant decay processes, experience substantial scattering on the electron density of excited electrons, which remain a spectator during the decay. As a result, the angular emission distribution is altered significantly. This effect is expected to be a common feature of low energy secondary electron emission. In this letter, we exemplify our idea by examining the spectator resonant interatomic Coulombic decay (sRICD) of Ne dimers. Our theoretical predictions are confirmed by a corresponding coincidence experiment., Comment: 5 pages two figures

Almost ten years ago, energetic neutral hydrogen atoms were detected after a strong-field double ionization of H$_2$. This process, called 'frustrated tunneling ionization', occurs when an ionized electron is recaptured after being driven back to its parent ion by the electric field of a femtosecond laser. In the present study we demonstrate that a related process naturally occurs in clusters without the need of an external field: we observe a charge hopping that occurs during a Coulomb explosion of a small helium cluster, which leads to an energetic neutral helium atom. This claim is supported by theoretical evidence. As an analog to 'frustrated tunneling ionization', we term this process 'frustrated Coulomb explosion'.

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 case of the $H_2^+$ dissociating along the $1s\sigma_g$ 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 $H_2^+$., Comment: Accepted for publication in Phys.Rev.Lett. 1/11/2016

We report on coulomb explosion imaging of the wavefunction of the quantum halo system He$_2$. Each atom of this system is ionized by tunnelionization in a femto second laser pulse and in a second experiment by single photon ionization employing a free electron laser. We visualize the exponential decay of the probability density of the tunneling particle over distance for over two orders of magnitude up to an internuclear distance of 250 {\AA}. By fitting the slope of the density in the tunneling regime we obtain a binding energy of 151.9 $\pm$ 13.3 neV, which is in agreement with most recent calculations., Comment: 11 pages, 5 figures

Even though ion/atom-collision is a mature field of atomic physics great discrepancies between experiment and theoretical calculations are still common. Here we present experimental results with highest momentum resolution on single ionization of helium induced by 1\,MeV protons and compare these to different theoretical calculations. The overall agreement is strikingly good and already the first Born approximation yields good agreement between theory and experiment. This has been expected since several decades, but so far has not been accomplished. The influence of projectile coherence effects on the measured data is shortly discussed in line with an ongoing dispute on the existence of nodal structures in the electron angular emission distributions., Comment: 15 pages, 4 figures

We investigate the onset of photoionization shakeup induced interatomic Coulombic decay (ICD) in He2 at the He+*(n = 2) threshold by detecting two He+ ions in coincidence. We find this threshold to be shifted towards higher energies compared to the same threshold in the monomer. The shifted onset of ion pairs created by ICD is attributed to a recapture of the threshold photoelectron after the emission of the faster ICD electron., Comment: 5 Pages, 2 Figures

We investigate the ionization of HeNe from below the He 1s3p 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 (ICD) in HeNe dimers. We find that the ICD lifetime strongly increases with increasing vibrational state., Comment: 7 pages, 5 figures

During the last 15 years a novel decay mechanism of excited atoms has been discovered and investigated. This so called ''Interatomic Coulombic Decay'' (ICD) involves the chemical environment of the electronically excited atom: the excitation energy is transferred (in many cases over long distances) to a neighbor of the initially excited particle usually ionizing that neighbor. It turned out that ICD is a very common decay route in nature as it occurs across van-der-Waals and hydrogen bonds. The time evolution of ICD is predicted to be highly complex, as its efficiency strongly depends on the distance of the atoms involved and this distance typically changes during the decay. Here we present the first direct measurement of the temporal evolution of ICD using a novel experimental approach., Comment: 6 pages, 4 figures, submitted to PRL

We report a study of the low-temperature high-pressure phase diagram of the intermetallic compound PrCu$_2$, by means of molecular-field calculations and $^{63,65}$Cu nuclear-quadrupole-resonance (NQR) measurements under pressure. The pressure-induced magnetically-ordered phase can be accounted for by considering the influence of the crystal electric field on the $4f$ electron orbitals of the Pr$^{3+}$ ions and by introducing a pressure-dependent exchange interaction between the corresponding local magnetic moments. Our experimental data suggest that the order in the induced antiferromagnetic phase is incommensurate. The role of magnetic fluctuations both at high and low pressures is also discussed., Comment: 7 pages, 6 figures, submitted to Eur. Phys. J. B

Data of 23Na NMR spectra- and relaxation measurements are interpreted as suggesting that, upon increasing temperature the Na layers in Na0.8CoO2 adopt a 2D liquid state at T=291 K. The corresponding first order phase transition is preceded by a rapidly increasing mobility and diffusion of Na ions above 200K. Above 291 K the 23Na NMR response is similar to that previously observed in superionic conductors with planar Na layers., Comment: 4 pages, 4 figures

Pressure-induced variations of $^{27}$Al NMR spectra of CeAl$_3$ indicate significant changes in the ground-state characteristics of this prototypical heavy-electron compound. Previously reported magnetic and electronic inhomogeneities at ambient pressure and very low temperatures are removed with external pressures exceeding 1.2 kbar. The spectra and results of corresponding measurements of the NMR spin-lattice relaxation rates indicate a pressure-induced emergence of a simple paramagnetic state involving electrons with moderately enhanced masses and no magnetic order above 65 mK., Comment: 4 pages, 4 figures, 2 tables submitted to Physical Review B

We report the results of a $^{63,65}$Cu NMR/NQR study probing the intermetallic compound PrCu$_2$. The previously claimed onset of magnetic order at 65 K, indicated in a $\mu$SR study, is not confirmed. Based on our data we discuss different possible reasons for this apparent discrepancy, including a non negligible influence of the implanted muons on their environment. Competing dipolar and quadrupolar interactions lead to unusual features of the magnetic-ion/conduction-electron system, different from those of common intermetallics exhibiting structural or magnetic instabilities., Comment: 8 pages, 7 figures, submitted to Phys Rev B