TY - JOUR A1 - Pontius, Niko A1 - Beye, Martin A1 - Trabant, Christoph A1 - Mitzner, Rolf A1 - Sorgenfrei, Nomi A1 - Kachel, Torsten A1 - Woestmann, Michael A1 - Roling, Sebastian A1 - Zacharias, Helmut A1 - Ivanov, Rosen A1 - Treusch, Rolf A1 - Buchholz, Marcel A1 - Metcalf, Pete A1 - Schuessler-Langeheine, Christian A1 - Föhlisch, Alexander T1 - Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment JF - Structural dynamics N2 - We present a general experimental concept for jitter-free pump and probe experiments at free electron lasers. By generating pump and probe pulse from one and the same X-ray pulse using an optical split-and-delay unit, we obtain a temporal resolution that is limited only by the X-ray pulse lengths. In a two-color X-ray pump and X-ray probe experiment with sub 70 fs temporal resolution, we selectively probe the response of orbital and charge degree of freedom in the prototypical functional oxide magnetite after photoexcitation. We find electronic order to be quenched on a time scale of (30 +/- 30) fs and hence most likely faster than what is to be expected for any lattice dynamics. Our experimental result hints to the formation of a short lived transient state with decoupled electronic and lattice degree of freedom in magnetite. The excitation and relaxation mechanism for X-ray pumping is discussed within a simple model leading to the conclusion that within the first 10 fs the original photoexcitation decays into low-energy electronic excitations comparable to what is achieved by optical pump pulse excitation. Our findings show on which time scales dynamical decoupling of degrees of freedom in functional oxides can be expected and how to probe this selectively with soft X-ray pulses. Results can be expected to provide crucial information for theories for ultrafast behavior of materials and help to develop concepts for novel switching devices. (C) 2018 Author(s). Y1 - 2018 U6 - https://doi.org/10.1063/1.5042847 SN - 2329-7778 VL - 5 IS - 5 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Kühn, Danilo A1 - Giangrisostomi, Erika A1 - Jay, Raphael Martin A1 - Sorgenfrei, Nomi A1 - Föhlisch, Alexander T1 - The influence of x-ray pulse length on space-charge effects in optical pump/x-ray probe photoemission JF - New journal of physics : the open-access journal for physics N2 - Pump-probe photoelectron spectroscopy (PES) is a versatile tool to investigate the dynamics of transient states of excited matter. Vacuum space-charge effects can mask these dynamics and complicate the interpretation of electron spectra. Here we report on space-charge effects in Au 4f photoemission from a polycrystalline gold surface, excited with moderately intense 90 ps (FWHM) soft x-ray probe pulses, under the influence of the Coulomb forces exerted by a pump electron cloud, which was produced by intense 40 fs laser pulses. The experimentally observed kinetic energy shift and spectral broadening of the Au 4f lines, measured with highly-efficient time-of-flight spectroscopy, are in good agreement with simulations utilizing a mean-field model of the electrostatic pump electron potential. This confirms that the line broadening is predominantly caused by variations in the take-off time of the probe electrons without appreciable influence of local scattering events. Our findings might be of general interest for pump-probe PES with picosecond-pulse-length sources. KW - space-charge effects KW - mean-field model KW - x-ray photoemission KW - electron spectroscopy KW - pump-probe KW - ARTOF Y1 - 2019 U6 - https://doi.org/10.1088/1367-2630/ab2f5c SN - 1367-2630 VL - 21 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Li, Tian-yi A1 - Benduhn, Johannes A1 - Li, Yue A1 - Jaiser, Frank A1 - Spoltore, Donato A1 - Zeika, Olaf A1 - Ma, Zaifei A1 - Neher, Dieter A1 - Vandewal, Koen A1 - Leo, Karl T1 - Boron dipyrromethene (BODIPY) with meso-perfluorinated alkyl substituents as near infrared donors in organic solar cells JF - Journal of materials chemistry : A, Materials for energy and sustainability N2 - Three furan-fused BODIPYs were synthesized with perfluorinated methyl, ethyl and n-propyl groups on the meso-carbon. They were obtained with high yields by reacting the furan-fused 2-carboxylpyrrole in corresponding perfluorinated acid and anhydride. With the increase in perfluorinated alkyl chain length, the molecular packing in the single crystal is influenced, showing increasing stacking distance and decreasing slope angle. All the BODIPYs were characterized as intense absorbers in near infrared region in solid state, peaking at similar to 800 nm with absorption coefficient of over 280 000 cm(-1). Facilitated by high thermal stability, the furan-fused BODIPYs were employed in vacuum-deposited organic solar cells as electron donors. All devices exhibit PCE over 6.0% with the EQE maximum reaching 70% at similar to 790 nm. The chemical modification of the BODIPY donors have certain influence on the active layer morphology, and the highest PCE of 6.4% was obtained with a notably high jsc of 13.6 mA cm(-2). Sensitive EQE and electroluminance studies indicated that the energy losses generated by the formation of a charge transfer state and the radiative recombination at the donor-acceptor interface were comparable in the range of 0.14-0.19 V, while non-radiative recombination energy loss of 0.38 V was the main energy loss route resulting in the moderate V-oc of 0.76 V. Y1 - 2018 U6 - https://doi.org/10.1039/c8ta06261g SN - 2050-7488 SN - 2050-7496 VL - 6 IS - 38 SP - 18583 EP - 18591 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Liebig, Ferenc A1 - Sarhan, Radwan Mohamed A1 - Prietzel, Claudia Christina A1 - Thünemann, Andreas F. A1 - Bargheer, Matias A1 - Koetz, Joachim T1 - Undulated Gold Nanoplatelet Superstructures BT - In Situ Growth of Hemispherical Gold Nanoparticles onto the Surface of Gold Nanotriangles JF - Langmuir N2 - Negatively charged flat gold nanotriangles, formed in a vesicular template phase and separated by an AOT-micelle-based depletion flocculation, were reloaded by adding a cationic polyelectrolyte, that is, a hyperbranched polyethylenimine (PEI). Heating the system to 100 degrees C in the presence of a gold chloride solution, the reduction process leads to the formation of gold nanoparticles inside the polymer shell surrounding the nanoplatelets. The gold nanoparticle formation is investigated by UV-vis spectroscopy, small-angle X-ray scattering, and dynamic light scattering measurements in combination with transmission electron microscopy. Spontaneously formed gold clusters in the hyperbranched PEI shell with an absorption maximum at 350 nm grow on the surface of the nanotriangles as hemispherical particles with diameters of similar to 6 nm. High-resolution micrographs show that the hemispherical gold particles are crystallized onto the {111} facets on the bottom and top of the platelet as well as on the edges without a grain boundary. Undulated gold nanoplatelet superstructures with special properties become available, which show a significantly modified performance in SERS-detected photocatalysis regarding both reactivity and enhancement factor. Y1 - 2018 U6 - https://doi.org/10.1021/acs.langmuir.7b02898 SN - 0743-7463 VL - 34 IS - 15 SP - 4584 EP - 4594 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Tchoumba Kwamen, Christelle Larodia A1 - Rössle, Matthias A1 - Leitenberger, Wolfram A1 - Alexe, Marin A1 - Bargheer, Matias T1 - Time-resolved X-ray diffraction study of the structural dynamics in an epitaxial ferroelectric thin Pb(Zr0.2Ti0.8)O-3 film induced by sub-coercive fields JF - Applied physics letters N2 - The electric field-dependence of structural dynamics in a tetragonal ferroelectric lead zirconate titanate thin film is investigated under subcoercive and above-coercive fields using time-resolved X-ray diffraction. The domain nucleation and growth are monitored in real time during the application of an external field to the prepoled thin film capacitor. We propose the observed broadening of the in-plane peak width of the symmetric 002 Bragg reflection as an indicator of the domain disorder and discuss the processes that change the measured peak intensity. Subcoercive field switching results in remnant disordered domain configurations. Published under license by AIP Publishing. Y1 - 2019 U6 - https://doi.org/10.1063/1.5084104 SN - 0003-6951 SN - 1077-3118 VL - 114 IS - 16 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Stete, Felix A1 - Koopman, Wouter-Willem Adriaan A1 - Bargheer, Matias T1 - Signatures of strong coupling on nanoparticles BT - revealing absorption anticrossing by tuning the dielectric environment JF - ACS Photonics N2 - In the strong coupling regime, exciton and plasmon excitations are hybridized into combined system excitations. The correct identification of the coupling regime in these systems is currently debated, from both experimental and theoretical perspectives. In this article we show that the extinction spectra may show a large peak splitting, although the energy loss encoded in the absorption spectra clearly rules out the strong coupling regime. We investigate the coupling of J-aggregate excitons to the localized surface plasmon polaritons on gold nanospheres and nanorods by fine-tuning the plasmon resonance via layer-by-layer deposition of polyelectrolytes. While both structures show a characteristic anticrossing in extinction and scattering experiments, the careful assessment of the systems’ light absorption reveals that strong coupling of the plasmon to the exciton is not present in the nanosphere system. In a phenomenological model of two classical coupled oscillators, a Fano-like regime causes only the resonance of the light-driven oscillator to split up, while the other one still dissipates energy at its original frequency. Only in the strong-coupling limit do both oscillators split up the frequencies at which they dissipate energy, qualitatively explaining our experimental finding. KW - hybrid nanoparticles KW - exciton plasmon coupling KW - layer-by-layer deposition KW - strong coupling KW - absorption measurements Y1 - 2017 U6 - https://doi.org/10.1021/acsphotonics.7b00113 SN - 2330-4022 VL - 4 SP - 1669 EP - 1676 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Mattern, Maximilian A1 - Pudell, Jan-Etienne A1 - Laskin, Gennadii A1 - Reppert, Alexander von A1 - Bargheer, Matias T1 - Analysis of the temperature- and fluence-dependent magnetic stress in laser-excited SrRuO3 JF - Structural dynamics N2 - We use ultrafast x-ray diffraction to investigate the effect of expansive phononic and contractive magnetic stress driving the picosecond strain response of a metallic perovskite SrRuO3 thin film upon femtosecond laser excitation. We exemplify how the anisotropic bulk equilibrium thermal expansion can be used to predict the response of the thin film to ultrafast deposition of energy. It is key to consider that the laterally homogeneous laser excitation changes the strain response compared to the near-equilibrium thermal expansion because the balanced in-plane stresses suppress the Poisson stress on the picosecond timescale. We find a very large negative Grüneisen constant describing the large contractive stress imposed by a small amount of energy in the spin system. The temperature and fluence dependence of the strain response for a double-pulse excitation scheme demonstrates the saturation of the magnetic stress in the high-fluence regime. KW - Thin films KW - Thermodynamic properties KW - Bragg peak KW - Ultrafast X-ray diffraction KW - Thermal effects KW - Phonons KW - Magnetism KW - Lattice dynamics KW - Lasers KW - Perovskites Y1 - 2020 U6 - https://doi.org/10.1063/4.0000072 SN - 2329-7778 VL - 8 IS - 2 PB - AIP Publishing LLC CY - Melville, NY ER - TY - JOUR A1 - Zeuschner, Steffen Peer A1 - Wang, Xi-Guang A1 - Deb, Marwan A1 - Popova, Elena A1 - Malinowski, Gregory A1 - Hehn, Michel A1 - Keller, Niels A1 - Berakdar, Jamal A1 - Bargheer, Matias T1 - Standing spin wave excitation in Bi BT - YIG films via temperature-induced anisotropy changes and magneto-elastic coupling JF - Physical review : B, Condensed matter and materials physics N2 - Based on micromagnetic simulations and experimental observations of the magnetization and lattice dynamics after the direct optical excitation of the magnetic insulator Bi : YIG or indirect excitation via an optically opaque Pt/Cu double layer, we disentangle the dynamical effects of magnetic anisotropy and magneto-elastic coupling. The strain and temperature of the lattice are quantified via modeling ultrafast x-ray diffraction data. Measurements of the time-resolved magneto-optical Kerr effect agree well with the magnetization dynamics simulated according to the excitation via two mechanisms: the magneto-elastic coupling to the experimentally verified strain dynamics and the ultrafast temperature-induced transient change in the magnetic anisotropy. The numerical modeling proves that, for direct excitation, both mechanisms drive the fundamental mode with opposite phase. The relative ratio of standing spin wave amplitudes of higher-order modes indicates that both mechanisms are substantially active. Y1 - 2022 U6 - https://doi.org/10.1103/PhysRevB.106.134401 SN - 2469-9950 SN - 2469-9969 VL - 106 IS - 13 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Liebig, Ferenc A1 - Henning, Ricky A1 - Sarhan, Radwan Mohamed A1 - Prietzel, Claudia Christina A1 - Bargheer, Matias A1 - Koetz, Joachim T1 - A new route to gold nanoflowers JF - Nanotechnology N2 - Catanionic vesicles spontaneously formed by mixing the anionic surfactant bis(2-ethylhexyl)sulfosuccinate sodium salt with the cationic surfactant cetyltrimethylammonium bromide were used as a reducing medium to produce gold clusters, which are embedded and well-ordered into the template phase. The gold clusters can be used as seeds in the growth process that follows by adding ascorbic acid as a mild reducing component. When the ascorbic acid was added very slowly in an ice bath round-edged gold nanoflowers were produced. When the same experiments were performed at room temperature in the presence of Ag+ ions, sharp-edged nanoflowers could be synthesized. The mechanism of nanoparticle formation can be understood to be a non-diffusion-limited Ostwald ripening process of preordered gold nanoparticles embedded in catanionic vesicle fragments. Surface-enhanced Raman scattering experiments show an excellent enhancement factor of 1.7 . 10(5) for the nanoflowers deposited on a silicon wafer. KW - catanionic vesicles KW - gold cluster KW - gold nanoflowers KW - crystal growth KW - HRTEM KW - SEM Y1 - 2018 U6 - https://doi.org/10.1088/1361-6528/aaaffd SN - 0957-4484 SN - 1361-6528 VL - 29 IS - 18 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Pudell, Jan-Etienne A1 - Sander, M. A1 - Bauer, R. A1 - Bargheer, Matias A1 - Herzog, Marc A1 - Gaál, Peter T1 - Full Spatiotemporal Control of Laser-Excited Periodic Surface Deformations JF - Physical review applied N2 - We demonstrate full control of acoustic and thermal periodic deformations at solid surfaces down to subnanosecond time scales and few-micrometer length scales via independent variation of the temporal and spatial phase of two optical transient grating (TG) excitations. For this purpose, we introduce an experimental setup that exerts control of the spatial phase of subsequent time-delayed TG excitations depending on their polarization state. Specific exemplary coherent control cases are discussed theoretically and corresponding experimental data are presented in which time-resolved x-ray reflectivity measures the spatiotemporal surface distortion of nanolayered heterostructures. Finally, we discuss examples where the application of our method may enable the control of functional material properties via tailored spatiotemporal strain fields. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevApplied.12.024036 SN - 2331-7019 VL - 12 IS - 2 PB - American Physical Society CY - College Park ER -