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- ItemA Mechanistic Perspective on Plastically Flexible Coordination Polymers(Weinheim : Wiley-VCH, 2019) Bhattacharya, Biswajit; Michalchuk, Adam A.L.; Silbernagl, Dorothee; Rautenberg, Max; Schmid, Thomas; Feiler, Torvid; Reimann, Klaus; Ghalgaoui, Ahmed; Sturm, Heinz; Paulus, Beate; Emmerling, FranziskaMechanical flexibility in single crystals of covalently bound materials is a fascinating and poorly understood phenomenon. We present here the first example of a plastically flexible one-dimensional (1D) coordination polymer. The compound [Zn(μ-Cl)2(3,5-dichloropyridine)2]n is flexible over two crystallographic faces. Remarkably, the single crystal remains intact when bent to 180°. A combination of microscopy, diffraction, and spectroscopic studies have been used to probe the structural response of the crystal lattice to mechanical bending. Deformation of the covalent polymer chains does not appear to be responsible for the observed macroscopic bending. Instead, our results suggest that mechanical bending occurs by displacement of the coordination polymer chains. Based on experimental and theoretical evidence, we propose a new model for mechanical flexibility in 1D coordination polymers. Moreover, our calculations propose a cause of the different mechanical properties of this compound and a structurally similar elastic material. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
- ItemCovalency-Driven Preservation of Local Charge Densities in a Metal-to-Ligand Charge-Transfer Excited Iron Photosensitizer(Weinheim : Wiley-VCH, 2019) Jay, Raphael M.; Eckert, Sebastian; Vaz da Cruz, Vinicius; Fondell, Mattis; Mitzner, Rolf; Föhlisch, AlexanderCovalency is found to even out charge separation after photo-oxidation of the metal center in the metal-to-ligand charge-transfer state of an iron photosensitizer. The σ-donation ability of the ligands compensates for the loss of iron 3d electronic charge, thereby upholding the initial metal charge density and preserving the local noble-gas configuration. These findings are enabled through element-specific and orbital-selective time-resolved X-ray absorption spectroscopy at the iron L-edge. Thus, valence orbital populations around the central metal are directly accessible. In conjunction with density functional theory we conclude that the picture of a localized charge-separation is inadequate. However, the unpaired spin density provides a suitable representation of the electron–hole pair associated with the electron-transfer process. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
- ItemAirborne high spectral resolution lidar observation of pollution aerosol during EUCAARI-LONGREX(Göttingen : Copernicus, 2013) Groß, S.; Esselborn, M.; Abicht, F.; Wirth, M.; Fix, A.; Minikin, A.Airborne high spectral resolution lidar observations over Europe during the EUCAARI-LONGREX field experiment in May 2008 are analysed with respect to the optical properties of continental pollution aerosol. Continental pollution aerosol is characterized by its depolarisation and lidar ratio. Over all, the measurements of the lidar ratio and the particle linear depolarization ratio of pollution aerosols provide a narrow range of values. Therefore, this data set allows for a distinct characterization of the aerosol type "pollution aerosol" and thus is valuable both to distinguish continental pollution aerosol from other aerosol types and to determine mixtures with other types of aerosols.
- ItemGraphene Q-switched Yb:KYW planar waveguide laser(New York, NY : American Inst. of Physics, 2015) Kim, Jun Wan; Young Choi, Sun; Aravazhi, Shanmugam; Pollnau, Markus; Griebner, Uwe; Petrov, Valentin; Bae, Sukang; Jun Ahn, Kwang; Yeom, Dong-Il; Rotermund, FabianA diode-pumped Yb:KYW planar waveguide laser, single-mode Q-switched by evanescent-field interaction with graphene, is demonstrated for the first time. Few-layer graphene grown by chemical vapor deposition is transferred onto the top of a guiding layer, which initiates stable Q-switched operation in a 2.4-cm-long waveguide laser operating near 1027 nm. Average output powers up to 34 mW and pulse durations as short as 349 ns are achieved. The measured output beam profile, clearly exhibiting a single mode, agrees well with the theoretically calculated mode intensity distribution inside the waveguide. As the pump power is increased, the repetition rate and pulse energy increase from 191 to 607 kHz and from 7.4 to 58.6 nJ, respectively, whereas the pulse duration decreases from 2.09 μs to 349 ns.
- ItemPhotoluminescence lineshape of ZnO(New York, NY : American Inst. of Physics, 2014) Ullrich, B.; Singh, A.K.; Bhowmick, M.; Barik, P.; Ariza-Flores, D.; Xi, H.; Tomm, J.W.The merger of the absorption coefficient dispersion, retrieved from transmission by the modified Urbach rule introduced by Ullrich and Bouchenaki [Jpn. J. Appl. Phys. 30, L1285, 1991], with the extended Roosbroeck-Shockley relation reveals that the optical absorption in ZnO distinctively determines the photoluminescence lineshape. Additionally, the ab initio principles employed enable the accurate determination of the carrier lifetime without further specific probing techniques.
- ItemInfrared spectroscopy in superfluid helium droplets(Abingdon : Taylor and Francis Ltd., 2019) Verma D.; Tanyag R.M.P.; O’Connell S.M.O.; Vilesov A.F.For more than two decades, encapsulation in superfluid helium nanodroplets has served as a reliable technique for probing the structure and dynamics of molecules and clusters at a low temperature of ≈0.37 K. Due to weak interactions between molecules and the host liquid helium, good spectral resolution can usually be achieved, making helium droplets an ideal matrix for spectroscopy in a wide spectral range from infrared to ultraviolet. Furthermore, rotational structure in the spectra of small molecules provides a unique probe for interactions with the superfluid on an atomic scale. This review presents a summary of results and a discussion of recent experimental developments in helium droplet spectroscopy with the emphasis laid on infrared studies. Initially, studies focused on single molecules and have been expanded to larger species, such as metal-molecular clusters, biomolecules, free radicals, ions, and proteins. © 2018 The Author(s). Published by Informa UK Limited, trading as Taylor & Francis Group.
- ItemNear-field dynamics of broad area diode laser at very high pump levels(New York, NY : American Inst. of Physics, 2011) Hempel, M.; Tomm, J.W.; Baeumler, M.; Konstanzer, H.; Mukherjee, J.; Elsaesser, T.Near-field properties of the emission of broad area semiconductor diode lasers under extremely high pumping of up to ∼50 times the threshold are investigated. A transition from a gain to thermally-induced index guiding is shown under operation with single pulses of 300 ns duration. At highest output powers, catastrophic optical damage is observed which is studied in conjunction with the evolution of time-averaged filamentary near-field properties. Dynamics of the process is resolved on a picosecond time scale.
- 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.
- ItemDynamical studies on the generation of periodic surface structures by femtosecond laser pulses(Les Ulis : EDP Sciences, 2013) Rosenfeld, A.; Höhm, S.; Bonse, J.; Krüger, J.The dynamics of the formation of laser-induced periodic surface structures (LIPSS) on fused silica upon irradiation with linearly polarized fs-laser pulses (50 fs pulse duration, 800 nm center wavelength) is studied experimentally using a double pulse experiment with cross polarized pulse sequences and a trans illumination femtosecond time-resolved (0.1 ps - 1 ns) pump-probe diffraction approach. The results in both experiments confirm the importance of the ultrafast energy deposition and the laser-induced free-electron plasma in the conduction band of the solids for the formation of LIPSS.