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- ItemProperties of LiGa0.5In0.5Se2: A Quaternary Chalcogenide Crystal for Nonlinear Optical Applications in the Mid-IR(Basel : MDPI, 2016) Isaenko, Ludmila; Yelisseyev, Alexander; Lobanov, Sergei; Vedenyapin, Vitaliy; Krinitsyn, Pavel; Petrov, ValentinLiGaSe2 (LGSe) and LiInSe2 (LISe) are wide band-gap nonlinear crystals transparent in the mid-IR spectral range. LiGa0.5In0.5Se2 (LGISe) is a new mixed crystal, a solid solution in the system LGSe–LISe, which exhibits the same orthorhombic structure (mm2) as the parent compounds in the same time being more technological with regard to the growth process. In comparison with LGSe and LISe its homogeneity range is broader in the phase diagram. About 10% of the Li ions in LGISe occupy octahedral positions (octapores) with coordination number of 3. The band-gap of LGISe is estimated to be 2.94 eV at room temperature and 3.04 eV at 80 K. The transparency at the 0-level extends from 0.47 to 13 µm. LGISe crystals exhibit luminescence in broad bands centered near 1.7 and 1.25 eV which is excited most effectively by band-to-band transition. From the measured principal refractive indices and the fitted Sellmeier equations second-harmonic generation from 1.75 to 11.8 μm (fundamental wavelength) is predicted. The nonlinear coefficients of LGISe have values between those of LGSe and LISe. 6LGISe crystals are considered promising also for detection of thermal neutrons.
- 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.
- ItemExcited-state relaxation of hydrated thymine and thymidine measured by liquid-jet photoelectron spectroscopy: experiment and simulation(Washington, DC : ACS Publications, 2015) Buchner, Franziska; Nakayama, Akira; Yamazaki, Shohei; Ritze, Hans-Hermann; Lübcke, AndreaTime-resolved photoelectron spectroscopy is performed on thymine and thymidine in aqueous solution to study the excited-state relaxation dynamics of these molecules. We find two contributions with sub-ps lifetimes in line with recent excited-state QM/MM molecular dynamics simulations (J. Chem. Phys.2013, 139, 214304). The temporal evolution of ionization energies for the excited ππ* state along the QM/MM molecular dynamics trajectories were calculated and are compatible with experimental results, where the two contributions correspond to the relaxation paths in the ππ* state involving different conical intersections with the ground state. Theoretical calculations also show that ionization from the nπ* state is possible at the given photon energies, but we have not found any experimental indication for signal from the nπ* state. In contrast to currently accepted relaxation mechanisms, we suggest that the nπ* state is not involved in the relaxation process of thymine in aqueous solution.
- 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.
- ItemMultidimensional high harmonic spectroscopy of polyatomic molecules: detecting sub-cycle laser-driven hole dynamics upon ionization in strong mid-IR laser fields(Cambridge [u.a.] : Soc., 2016) Bruner, Barry D.; Mašín, Zdeněk; Negro, Matteo; Morales, Felipe; Brambila, Danilo; Devetta, Michele; Faccialà, Davide; Harvey, Alex G.; Ivanov, Misha; Mairesse, Yann; Patchkovskii, Serguei; Serbinenko, Valeria; Soifer, Hadas; Stagira, Salvatore; Vozzi, Caterina; Dudovich, Nirit; Smirnova, OlgaHigh harmonic generation (HHG) spectroscopy has opened up a new frontier in ultrafast science, where electronic dynamics can be measured on an attosecond time scale. The strong laser field that triggers the high harmonic response also opens multiple quantum pathways for multielectron dynamics in molecules, resulting in a complex process of multielectron rearrangement during ionization. Using combined experimental and theoretical approaches, we show how multi-dimensional HHG spectroscopy can be used to detect and follow electronic dynamics of core rearrangement on sub-laser cycle time scales. We detect the signatures of laser-driven hole dynamics upon ionization and reconstruct the relative phases and amplitudes for relevant ionization channels in a CO2 molecule on a sub-cycle time scale. Reconstruction of channel-resolved complex ionization amplitudes on attosecond time scales has been a long-standing goal of high harmonic spectroscopy. Our study brings us one step closer to fulfilling this initial promise and developing robust schemes for sub-femtosecond imaging of multielectron rearrangement in complex molecular systems.
- 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.
- ItemAdaptive micro axicons for laser applications(Les Ulis : EDP Sciences, 2015) Wallrabe, Ulrike; Brunne, Jens; Treffer, Alexander; Grunwald, Ruediger; Bellouard, YvesWe report on the design, fabrication and testing of novel types of low-dispersion axicons for the adaptive shaping of ultrashort laser pulses. An overview is given on the basic geometries and operating principles of our purely reflective adaptive MEMS-type devices based on thermal or piezoelectric actuation. The flexible formation of nondiffracting beams at pulse durations down to a few oscillations of the optical field enables new applications in optical communication, pulse diagnostics, laser-matter interaction and particle manipulation. As an example, we show first promising results of adaptive autocorrelation. The combination of excellent pulse transfer, self-reconstruction properties and propagation invariance of nondiffracting beams with an adaptive approach promises to extend the field of practical applications significantly.
- 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.