2014, Stodolna, A., Huismans, Y., Rouzée, A., Lépine, F., Vrakking, M.J.J.

The application of velocity map imaging for the detection of photoelectrons resulting from atomic or molecular ionization allows the observation of interferometric, and in some cases holographic structures that contain detailed information on the target from which the photoelecrons are extracted. In this contribution we present three recent examples of the use of photoelectron velocity map imaging in experiments where atoms are exposed to strong optical and dc electric fields. We discuss (i) observations of the nodal structure of Stark states of hydrogen measured in a dc electric field, (ii) mid-infrared strong-field ionization of metastable Xe atoms and (iii) the reconstruction of helium electronic wavepackets in an attosecond pump-probe experiment. In each case, the interference between direct and indirect electron pathways, reminiscent of the reference and signal waves in holography, is seen to play an important role.

2015, Schütte, Bernd, Arbeiter, Mathias, Fennel, Thomas, Jabbari, Ghazal, Gokhberg, Kirill, Kuleff, Alexander I., Vrakking, Marc J. J., Rouzée, Arnaud

We report on the observation of a novel intracluster Coulombic decay process following Rydberg atom formation in clusters ionized by intense near-infrared fields. A new decay channel emerges, in which a Rydberg atom relaxes to the ground state by transferring its excess energy to a weakly bound electron in the environment that is emitted from the cluster. We find evidence for this process in the electron spectra, where a peak close to the corresponding atomic ionization potential is observed. For Ar clusters, a decay time of 87 ps is measured, which is significantly longer than in previous time-resolved studies of interatomic Coulombic decay.

2015, Schütte, Bernd, Vrakking, Marc J. J., Rouzée, Arnaud

We report on the observation of a transient C4+ ion charge state in nanoplasmas produced by the interaction of intense near-infrared (NIR) laser pulses with CH4 clusters. The underlying dynamics are studied by pump-probe spectroscopy, which reveals that the ion charge states are lowered by electron-ion recombination. Furthermore, we present direct evidence that autoionization of multiply-excited ions plays an important role in expanding nanoplasmas, in contrast to models that neglect quantum phenomena.

2015, Zimmermann, Henri, Eilzer, Sebastian, Eichmann, Ulli

We investigated the principal quantum number n distribution of excited states resulting from the interaction of Helium with strong, short laser pulses. We find excellent agreement with predictions of the semiclassical frustrated tunneling ionization (FTI) model [1] as well as fully quantum mechanical calculations. Furthermore, the excitation process directly populates triplet excited states due to the breakdown of the Russel-Saunders coupling scheme for high orbital angular momentum l states of Helium, which are predominantly populated in the strong laser field.

2014, McFarland, B.K., Berrah, N., Bostedt, C., Bozek, J., Bucksbaum, P.H., Castagna, J.C., Coffee, R.N., Cryan, J.P., Fang, L., Farrell, J.P., Feifel, R., Gaffney, K.J., Glownia, J.M., Martinez, T.J., Miyabe, S., Mucke, M., Murphy, B., Natan, A., Osipov, T., Petrovic, V.S., Schorb, S., Schultz, T., Spector, L.S., Swiggers, M., Tarantelli, F., Tenney, I., Wang, S., White, J.L., White, W., Gühr, M.

Free electron laser (FEL) based x-ray sources show great promise for use in ultrafast molecular studies due to the short pulse durations and site/element sensitivity in this spectral range. However, the self amplified spontaneous emission (SASE) process mostly used in FELs is intrinsically noisy resulting in highly fluctuating beam parameters. Additionally timing synchronization of optical and FEL sources adds delay jitter in pump-probe experiments. We show how we mitigate the effects of source noise for the case of ultrafast molecular spectroscopy of the nucleobase thymine. Using binning and resorting techniques allows us to increase time and spectral resolution. In addition, choosing observables independent of noisy beam parameters enhances the signal fidelity.

2015, Schütte, Bernd, Arbeiter, Mathias, Fennel, Thomas, Jabbari, Ghazal, Kuleff, Alexander I., Vrakking, Marc J. J., Rouzée, Arnaud

We report on a novel correlated electronic decay process following extensive Rydberg atom formation in clusters ionized by intense near-infrared fields. A peak close to the atomic ionization potential is found in the electron kinetic energy spectrum. This new contribution is attributed to an energy transfer between two electrons, where one electron decays from a Rydberg state to the ground state and transfers its excess energy to a weakly bound cluster electron in the environment that can escape from the cluster. The process is a result of nanoplasma formation and is therefore expected to be important, whenever intense laser pulses interact with nanometer-sized particles.

2015, Brambila, Danilo S., Harvey, Alex G., Mašín, Zdeněk, Smirnova, Olga

We present R-matrix calculations of photoionization from NO2, resolved in energy, angle, and both neutral and ionic state, for a range of molecular geometries, including in the vicinity of the 2A1/2B2 conical intersection.

2014, Baumbach, S., Kanngießer, B., Malzer, W., Stiel, H., Bjeoumikhova, S., Wilhein, T.

This article presents a concept and the first results for the setup of an 8keV laboratory transmission x-ray microscope with a polycapillary optic as condenser at the BliX in Berlin. The incentive of building such a microscope is that the penetration depth for hard x-rays is much higher than in the soft x-ray range, e.g. The water window. Therefore, it is possible to investigate even dense materials such as metal compounds, bones or geological samples. The future aim is to achieve a spatial resolution better than 200 nm.

2015, Iablonskyi, D., Nagaya, K., Fukuzawa, H., Motomura, K., Kumagai, Y., Mondal, S., Tachibana, T., Takanashi, T., Nishiyama, T., Matsunami, K., Johnsson, P., Piseri, P., Sansone, G., Dubrouil, A., Reduzzi, M., Carpeggiani, P., Vozzi, C., Devetta, M., Negro, M., Faccialà, D., Calegari, F., Trabattoni, A., Castrovilli, M., Ovcharenko, Y., Möller, T., Mudrich, M., Stienkemeier, F., Coreno, M., Alagia, M., Schütte, B., Berrah, N., Callegari, C., Plekan, O., Finetti, P., Spezzani, C., Ferrari, E., Allaria, E., Penco, G., Serpico, C., De Ninno, G., Diviacco, B., Di Mitri, S., Giannessi, L., Prince, K.., Yao, M., Ueda, K.

We present a comprehensive analysis of autoionization processes in Ne clusters (~5000 atoms) after multiple valence excitations by free electron laser radiation. The evolution from 2-body interatomic Coulombic decay (ICD) to 3-body ICD is demonstrated when changing from surface to bulk Frenkel exciton excitation. Super Coster-Kronig type 2-body ICD is observed at Wannier exciton which quenches the main ICD channel.

2015, Hasović, Elvedin, Milošević, Dejan B., Gazibegović-Busuladži, Azra, Čerkić, Aner, Busuladžić, Mustafa

We consider high-order above-threshold ionization (HATI) of polyatomic molecules ionized by a strong linearly polarized laser field. Improved molecular strong-field approximation by which the HATI process on polyatomic molecular species can be described is developed. Using this theory we calculate photoelectron angular-energy spectra for different triatomic molecules. Special attention is devoted to the minima that are observed in the calculated high-energy electron spectra of the ozone and carbon dioxide molecules. A key difference between these minima and minima that are observed in the corresponding spectra of diatomic molecules are presented.