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- ItemWater Dynamics in the Hydration Shells of Biomolecules(Washington, DC : ACS Publ., 2017) Laage, Damien; Elsaesser, Thomas; Hynes, James T.The structure and function of biomolecules are strongly influenced by their hydration shells. Structural fluctuations and molecular excitations of hydrating water molecules cover a broad range in space and time, from individual water molecules to larger pools and from femtosecond to microsecond time scales. Recent progress in theory and molecular dynamics simulations as well as in ultrafast vibrational spectroscopy has led to new and detailed insight into fluctuations of water structure, elementary water motions, electric fields at hydrated biointerfaces, and processes of vibrational relaxation and energy dissipation. Here, we review recent advances in both theory and experiment, focusing on hydrated DNA, proteins, and phospholipids, and compare dynamics in the hydration shells to bulk water.
- ItemXUV double-pulses with femtosecond to 650 ps separation from a multilayer-mirror-based split-and-delay unit at FLASH(Chester : IUCr, 2018-8-3) Sauppe, Mario; Rompotis, Dimitrios; Erk, Benjamin; Bari, Sadia; Bischoff, Tobias; Boll, Rebecca; Bomme, Cédric; Bostedt, Christoph; Dörner, Simon; Düsterer, Stefan; Feigl, Torsten; Flückiger, Leonie; Gorkhover, Tais; Kolatzki, Katharina; Langbehn, Bruno; Monserud, Nils; Müller, Erland; Müller, Jan P.; Passow, Christopher; Ramm, Daniel; Rolles, Daniel; Schubert, Kaja; Schwob, Lucas; Senfftleben, Björn; Treusch, Rolf; Ulmer, Anatoli; Weigelt, Holger; Zimbalski, Jannis; Zimmermann, Julian; Möller, Thomas; Rupp, DanielaExtreme ultraviolet (XUV) and X-ray free-electron lasers enable new scientific opportunities. Their ultra-intense coherent femtosecond pulses give unprecedented access to the structure of undepositable nanoscale objects and to transient states of highly excited matter. In order to probe the ultrafast complex light-induced dynamics on the relevant time scales, the multi-purpose end-station CAMP at the free-electron laser FLASH has been complemented by the novel multilayer-mirror-based split-and-delay unit DESC (DElay Stage for CAMP) for time-resolved experiments. XUV double-pulses with delays adjustable from zero femtoseconds up to 650 picoseconds are generated by reflecting under near-normal incidence, exceeding the time range accessible with existing XUV split-and-delay units. Procedures to establish temporal and spatial overlap of the two pulses in CAMP are presented, with emphasis on the optimization of the spatial overlap at long time-delays via time-dependent features, for example in ion spectra of atomic clusters.
- ItemCAMP@FLASH: an end-station for imaging, electron- and ion-spectroscopy, and pump–probe experiments at the FLASH free-electron laser(Chester : IUCr, 2018-8-2) Erk, Benjamin; Müller, Jan P.; Bomme, Cédric; Boll, Rebecca; Brenner, Günter; Chapman, Henry N.; Correa, Jonathan; Düsterer, Stefan; Dziarzhytski, Siarhei; Eisebitt, Stefan; Graafsma, Heinz; Grunewald, Sören; Gumprecht, Lars; Hartmann, Robert; Hauser, Günter; Keitel, Barbara; von Korff Schmising, Clemens; Kuhlmann, Marion; Manschwetus, Bastian; Mercadier, Laurent; Müller, Erland; Passow, Christopher; Plönjes, Elke; Ramm, Daniel; Rompotis, Dimitrios; Rudenko, Artem; Rupp, Daniela; Sauppe, Mario; Siewert, Frank; Schlosser, Dieter; Strüder, Lothar; Swiderski, Angad; Techert, Simone; Tiedtke, Kai; Tilp, Thomas; Treusch, Rolf; Schlichting, Ilme; Ullrich, Joachim; Moshammer, Robert; Möller, Thomas; Rolles, DanielThe non-monochromatic beamline BL1 at the FLASH free-electron laser facility at DESY was upgraded with new transport and focusing optics, and a new permanent end-station, CAMP, was installed. This multi-purpose instrument is optimized for electron- and ion-spectroscopy, imaging and pump–probe experiments at free-electron lasers. It can be equipped with various electron- and ion-spectrometers, along with large-area single-photon-counting pnCCD X-ray detectors, thus enabling a wide range of experiments from atomic, molecular, and cluster physics to material and energy science, chemistry and biology. Here, an overview of the layout, the beam transport and focusing capabilities, and the experimental possibilities of this new end-station are presented, as well as results from its commissioning.
- ItemRole of electronic correlations in photoionization of NO2 in the vicinity of the 2A1/2B2 conical intersection(Cambridge : The Royal Soc. of Chemistry, 2017) Brambila, Danilo S.; Harvey, Alex G.; Houfek, Karel; Mašín, Zdeněk; Smirnova, OlgaWe present the first ab initio multi-channel photoionization calculations for NO2 in the vicinity of the 2A1/2B2 conical intersection, for a range of nuclear geometries, using our newly developed set of tools based on the ab initio multichannel R-matrix method. Electronic correlation is included in both the neutral and the scattering states of the molecule via configuration interaction. Configuration mixing is especially important around conical intersections and avoided crossings, both pertinent for NO2, and manifests itself via significant variations in photoelectron angular distributions. The method allows for a balanced and accurate description of the photoionization/photorecombination for a number of different ionic channels in a wide range of photoelectron energies up to 100 eV. Proper account of electron correlations is crucial for interpreting time-resolved signals in photoelectron spectroscopy and high harmonic generation (HHG) from polyatomic molecules.
- ItemQuantification of silver nanoparticle uptake and distribution within individual human macrophages by FIB/SEM slice and view(London : Biomed Central, 2017-3-21) Guehrs, Erik; Schneider, Michael; Günther, Christian M.; Hessing, Piet; Heitz, Karen; Wittke, Doreen; López-Serrano Oliver, Ana; Jakubowski, Norbert; Plendl, Johanna; Eisebitt, Stefan; Haase, AndreaBackground: Quantification of nanoparticle (NP) uptake in cells or tissues is very important for safety assessment. Often, electron microscopy based approaches are used for this purpose, which allow imaging at very high resolution. However, precise quantification of NP numbers in cells and tissues remains challenging. The aim of this study was to present a novel approach, that combines precise quantification of NPs in individual cells together with high resolution imaging of their intracellular distribution based on focused ion beam/ scanning electron microscopy (FIB/SEM) slice and view approaches. Results: We quantified cellular uptake of 75 nm diameter citrate stabilized silver NPs (Ag 75 Cit) into an individual human macrophage derived from monocytic THP-1 cells using a FIB/SEM slice and view approach. Cells were treated with 10 μg/ml for 24 h. We investigated a single cell and found in total 3138 ± 722 silver NPs inside this cell. Most of the silver NPs were located in large agglomerates, only a few were found in clusters of fewer than five NPs. Furthermore, we cross-checked our results by using inductively coupled plasma mass spectrometry and could confirm the FIB/SEM results. Conclusions: Our approach based on FIB/SEM slice and view is currently the only one that allows the quantification of the absolute dose of silver NPs in individual cells and at the same time to assess their intracellular distribution at high resolution. We therefore propose to use FIB/SEM slice and view to systematically analyse the cellular uptake of various NPs as a function of size, concentration and incubation time.
- ItemOriented zinc oxide nanorods: A novel saturable absorber for lasers in the near-infrared(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2018-10-23) Loiko, Pavel; Bora, Tanujjal; Serres, Josep Maria; Yu, Haohai; Aguiló, Magdalena; Díaz, Francesc; Griebner, Uwe; Petrov, Valentin; Mateos, Xavier; Dutta, JoydeepZinc oxide (ZnO) nanorods (NRs) oriented along the crystallographic [001] axis are grown by the hydrothermal method on glass substrates. The ZnO NRs exhibit a broadband (1–2 µm) near-IR absorption ascribed to the singly charged zinc vacancy VZn−1. The saturable absorption of the ZnO NRs is studied at ≈1 µm under picosecond excitation, revealing a low saturation intensity, ≈10 kW/cm2, and high fraction of the saturable losses. The ZnO NRs are applied as saturable absorbers in diode-pumped Yb (≈1.03 µm) and Tm (≈1.94 µm) lasers generating nanosecond pulses. The ZnO NRs grown on various optical surfaces are promising broadband saturable absorbers for nanosecond near-IR lasers in bulk and waveguide geometries.
- ItemVibrational sum-frequency generation spectroscopy of lipid bilayers at repetition rates up to 100 kHz(Melville, NY : American Institute of Physics, 2018) Yesudas, Freeda; Mero, Mark; Kneipp, Janina; Heiner, ZsuzsannaBroadband vibrational sum-frequency generation (BB-VSFG) spectroscopy has become a well-established surface analytical tool capable of identifying the orientation and structure of molecular layers. A straightforward way to boost the sensitivity of the technique could be to increase the laser repetition rate beyond that of standard BB-VSFG spectrometers, which rely on Ti:sapphire lasers operating at repetition rates of 1-5 kHz. Nevertheless, possible thermally induced artifacts in the vibrational spectra due to higher laser average powers are unexplored. Here, we discuss laser power induced temperature accumulation effects that distort the BB-VSFG spectra of 1,2-diacyl-sn-glycero-3-phosphocholine at an interface between two transparent phases at repetition rates of 5, 10, 50, and 100 kHz at constant pulse energy. No heat-induced distortions were found in the spectra, suggesting that the increase in the laser repetition rate provides a feasible route to an improved signal-to-noise ratio or shorter data acquisition times in BB-VSFG spectroscopy for thin films on transparent substrates. The results have implications for future BB-VSFG spectrometers pushing the detection limit for molecular layers with low surface coverage.