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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.
- ItemUnusual terahertz waveforms from a resonant medium controlled by diffractive optical elements([London] : Macmillan Publishers Limited, part of Springer Nature, 2019) Pakhomov, A.V.; Arkhipov, R.M.; Arkhipov, M.V.; Demircan, A.; Morgner, U.; Rosanov, N.N.; Babushkin, I.Up to now, full tunability of waveforms was possible only in electronics, up to radio-frequencies. Here we propose a new concept of producing few-cycle terahertz (THz) pulses with widely tunable waveforms. It is based on control of the phase delay between different parts of the THz wavefront using linear diffractive optical elements. Suitable subcycle THz wavefronts can be generated via coherent excitation of nonlinear low-frequency oscillators by few-cycle optical pulses. Using this approach it is possible to shape the electric field rather than the slow pulse envelope, obtaining, for instance, rectangular or triangular waveforms in the THz range. The method is upscalable to the optical range if the attosecond pump pulses are used.
- 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.
- ItemTailoring optical properties and stimulated emission in nanostructured polythiophene([London] : Macmillan Publishers Limited, part of Springer Nature, 2019) Portone, Alberto; Ganzer, Lucia; Branchi, Federico; Ramos, Rodrigo; Caldas, Marília J.; Pisignano, Dario; Molinari, Elisa; Cerullo, Giulio; Persano, Luana; Prezzi, Deborah; Virgili, TersillaPolythiophenes are the most widely utilized semiconducting polymers in organic electronics, but they are scarcely exploited in photonics due to their high photo-induced absorption caused by interchain polaron pairs, which prevents the establishment of a window of net optical gain. Here we study the photophysics of poly(3-hexylthiophene) configured with different degrees of supramolecular ordering, spin-coated thin films and templated nanowires, and find marked differences in their optical properties. Transient absorption measurements evidence a partially-polarized stimulated emission band in the nanowire samples, in contrast with the photo-induced absorption band observed in spin-coated thin films. In combination with theoretical modeling, our experimental results reveal the origin of the primary photoexcitations dominating the dynamics for different supramolecular ordering, with singlet excitons in the nanostructured samples superseding the presence of polaron pairs, which are present in the disordered films. Our approach demonstrates a viable strategy to direct optical properties through structural control, and the observation of optical gain opens the possibility to the use of polythiophene nanostructures as building blocks of organic optical amplifiers and active photonic devices. © 2019, The Author(s).
- ItemRole of hole confinement in the recombination properties of InGaN quantum structures([London] : Macmillan Publishers Limited, part of Springer Nature, 2019) Anikeeva, M.; Albrecht, M.; Mahler, F.; Tomm, J. W.; Lymperakis, L.; Chèze, C.; Calarco, R.; Neugebauer, J.; Schulz, T.We study the isolated contribution of hole localization for well-known charge carrier recombination properties observed in conventional, polar InGaN quantum wells (QWs). This involves the interplay of charge carrier localization and non-radiative transitions, a non-exponential decay of the emission and a specific temperature dependence of the emission, denoted as “s-shape”. We investigate two dimensional In0.25Ga0.75N QWs of single monolayer (ML) thickness, stacked in a superlattice with GaN barriers of 6, 12, 25 and 50 MLs. Our results are based on scanning and high-resolution transmission electron microscopy (STEM and HR-TEM), continuous-wave (CW) and time-resolved photoluminescence (TRPL) measurements as well as density functional theory (DFT) calculations. We show that the recombination processes in our structures are not affected by polarization fields and electron localization. Nevertheless, we observe all the aforementioned recombination properties typically found in standard polar InGaN quantum wells. Via decreasing the GaN barrier width to 6 MLs and below, the localization of holes in our QWs is strongly reduced. This enhances the influence of non-radiative recombination, resulting in a decreased lifetime of the emission, a weaker spectral dependence of the decay time and a reduced s-shape of the emission peak. These findings suggest that single exponential decay observed in non-polar QWs might be related to an increasing influence of non-radiative transitions.
- ItemPhonon driven charge dynamics in polycrystalline acetylsalicylic acid mapped by ultrafast x-ray diffraction(Melville, NY : AIP Publishing LLC, 2019) Hauf, Christoph; Hernandez Salvador, Antonio-Andres; Holtz, Marcel; Woerner, Michael; Elsaesser, ThomasThe coupled lattice and charge dynamics induced by phonon excitation in polycrystalline acetylsalicylic acid (aspirin) are mapped by femtosecond x-ray powder diffraction. The hybrid-mode character of the 0.9 ± 0.1 THz methyl rotation in the aspirin molecules is evident from collective charge relocations over distances of some 100 pm, much larger than the sub-picometer nuclear displacements. Oscillatory charge relocations around the methyl group generate a torque on the latter, thus coupling electronic and nuclear motions.
- ItemDynamics of Broadband Lasing Cascade from a Single Dot-in-well InGaAs Microdisk([London] : Macmillan Publishers Limited, part of Springer Nature, 2019) Talalaev, Vadim; Kryzhanovskaya, Natalia; Tomm, Jens W.; Rutckaia, Viktoriia; Schilling, Joerg; Zhukov, AlexeyThe development of a fast semiconductor laser is required for the realization of next-generation telecommunication applications. Since lasers operating on quantum dot ground state transitions exhibit only limited gain due to the saturation effect, we investigate lasing from excited states and compare its corresponding static and dynamic behavior to the one from the ground state. InAs quantum dots (QDs) grown in dot-in-well (DWELL) structures allowed to obtain light emission from ground and three excited states in a spectral range of 1.0–1.3 μm. This emission was coupled to whispering gallery modes (WGMs) of a 6 μm microdisk resonator and studied at room temperature by steady-state and time-resolved micro-photoluminescence. We demonstrate a cascade development of lasing arising from the ladder of quantum dot states, and compare the lasing behavior of ground and excited state emission. While the lasing threshold is being increased from the ground state to the highest excited state, the dynamic behavior is improved: turn-on times and lifetimes of WGMs become shorter paving the way towards high frequency direct driven microlasers. © 2019, The Author(s).
- ItemExcitation of H2 at large internuclear separation: F1∑+g outer well states and continuum resonances(London : Taylor & Francis, 2019) Trivikram, T.M.; Salumbides, E.J.; Jungen, Ch.; Ubachs, W.Bound and free quantum resonances of molecular hydrogen exhibiting wave-function density at large internuclear separation, (Formula presented.) 4–5 a.u., are excited via multi-step laser spectroscopy. Highly excited vibrational levels of H (Formula presented.) are prepared via two-photon UV-photolysis of H (Formula presented.) S. Subsequent two-photon Doppler-free precision measurements are performed connecting (Formula presented.) levels with (Formula presented.) outer-well levels. Detection and spectroscopic labelling of the quantum states is assisted by further laser excitation into the auto-ionisation continuum employing a third UV-laser. Level energies of high rotational states ((Formula presented.)) in the outer-well state (Formula presented.) are accurately determined. The three-laser study demonstrates a method for probing resonances in the H (Formula presented.) ionisation continuum with wave-function density at large internuclear separation (Formula presented.) 4–5 a.u., large angular momenta J, and energy range 131,100–133,000 cm-1, a hitherto unexplored territory. © 2019, © 2019 The Author(s). Published by Informa UK Limited, trading as Taylor & Francis Group.
- ItemEmittance Reduction of RF Photoinjector Generated Electron Beams by Transverse Laser Beam Shaping(Bristol : IOP Publ., 2019) Gross, M.; Qian, H.J.; Boonpornprasert, P.; Chen, Y.; Good, J.D.; Huck, H.; Isaev, I.; Koschitzki, C.; Krasilnikov, M.; Lal, S.; Li, X.; Lishilin, O.; Loisch, G.; Melkumyan, D.; Mohanty, S.K.; Niemczyk, R.; Oppelt, A.; Shaker, H.; Shu, G.; Stephan, F.; Vashchenko, G.; Will, I.Laser pulse shaping is one of the key elements to generate low emittance electron beams with RF photoinjectors. Ultimately high performance can be achieved with ellipsoidal laser pulses, but 3-dimensional shaping is challenging. High beam quality can also be reached by simple transverse pulse shaping, which has demonstrated improved beam emittance compared to a transversely uniform laser in the 'pancake' photoemission regime. In this contribution we present the truncation of a Gaussian laser at a radius of approximately one sigma in the intermediate (electron bunch length directly after emission about the same as radius) photoemission regime with high acceleration gradients (up to 60 MV/m). This type of electron bunch is used e.g. at the European XFEL and FLASH free electron lasers at DESY, Hamburg site and is being investigated in detail at the Photoinjector Test facility at DESY in Zeuthen (PITZ). Here we present ray-tracing simulations and experimental data of a laser beamline upgrade enabling variable transverse truncation. Initial projected emittance measurements taken with help of this setup are shown, as well as supporting beam dynamics simulations. Additional simulations show the potential for substantial reduction of slice emittance at PITZ. © Published under licence by IOP Publishing Ltd.
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