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- ItemSoft-mode driven polarity reversal in ferroelectrics mapped by ultrafast x-ray diffraction(Melville, NY : AIP Publishing LLC, 2018) Hauf, Christoph; Hernandez Salvador, Antonio-Andres; Holtz, Marcel; Woerner, Michael; Elsaesser, ThomasQuantum theory has linked microscopic currents and macroscopic polarizations of ferroelectrics, but the interplay of lattice excitations and charge dynamics on atomic length and time scales is an open problem. Upon phonon excitation in the prototypical ferroelectric ammonium sulfate [(NH4)2SO4], we determine transient charge density maps by femtosecond x-ray diffraction. A newly discovered low frequency-mode with a 3 ps period and sub-picometer amplitudes induces periodic charge relocations over some 100 pm, a hallmark of soft-mode behavior. The transient charge density allows for deriving the macroscopic polarization, showing a periodic reversal of polarity.
- ItemToward ultrafast magnetic depth profiling using time-resolved x-ray resonant magnetic reflectivity(Melville, NY : AIP Publishing LLC, 2021) Chardonnet, Valentin; Hennes, Marcel; Jarrier, Romain; Delaunay, Renaud; Jaouen, Nicolas; Kuhlmann, Marion; Ekanayake, Nagitha; Léveillé, Cyril; von Korff Schmising, Clemens; Schick, Daniel; Yao, Kelvin; Liu, Xuan; Chiuzbăian, Gheorghe S.; Lüning, Jan; Vodungbo, Boris; Jal, EmmanuelleDuring the last two decades, a variety of models have been developed to explain the ultrafast quenching of magnetization following femtosecond optical excitation. These models can be classified into two broad categories, relying either on a local or a non-local transfer of angular momentum. The acquisition of the magnetic depth profiles with femtosecond resolution, using time-resolved x-ray resonant magnetic reflectivity, can distinguish local and non-local effects. Here, we demonstrate the feasibility of this technique in a pump–probe geometry using a custom-built reflectometer at the FLASH2 free-electron laser (FEL). Although FLASH2 is limited to the production of photons with a fundamental wavelength of 4 nm (≃310 eV), we were able to probe close to the Fe L3 edge (706.8 eV) of a magnetic thin film employing the third harmonic of the FEL. Our approach allows us to extract structural and magnetic asymmetry signals revealing two dynamics on different time scales which underpin a non-homogeneous loss of magnetization and a significant dilation of 2 Å of the layer thickness followed by oscillations. Future analysis of the data will pave the way to a full quantitative description of the transient magnetic depth profile combining femtosecond with nanometer resolution, which will provide further insight into the microscopic mechanisms underlying ultrafast demagnetization.
- ItemThe sequence to hydrogenate coronene cations: A journey guided by magic numbers([London] : Macmillan Publishers Limited, part of Springer Nature, 2016) Cazaux, Stéphanie; Boschman, Leon; Rougeau, Nathalie; Reitsma, Geert; Hoekstra, Ronnie; Teillet-Billy, Dominique; Morisset, Sabine; Spaans, Marco; Schlathölter, ThomasThe understanding of hydrogen attachment to carbonaceous surfaces is essential to a wide variety of research fields and technologies such as hydrogen storage for transportation, precise localization of hydrogen in electronic devices and the formation of cosmic H2. For coronene cations as prototypical Polycyclic Aromatic Hydrocarbon (PAH) molecules, the existence of magic numbers upon hydrogenation was uncovered experimentally. Quantum chemistry calculations show that hydrogenation follows a site-specific sequence leading to the appearance of cations having 5, 11, or 17 hydrogen atoms attached, exactly the magic numbers found in the experiments. For these closed-shell cations, further hydrogenation requires appreciable structural changes associated with a high transition barrier. Controlling specific hydrogenation pathways would provide the possibility to tune the location of hydrogen attachment and the stability of the system. The sequence to hydrogenate PAHs, leading to PAHs with magic numbers of H atoms attached, provides clues to understand that carbon in space is mostly aromatic and partially aliphatic in PAHs. PAH hydrogenation is fundamental to assess the contribution of PAHs to the formation of cosmic H2.
- ItemDirect measurement of Coulomb-laser coupling([London] : Macmillan Publishers Limited, part of Springer Nature, 2021) Azoury, Doron; Krüger, Michael; Bruner, Barry D.; Smirnova, Olga; Dudovich, NiritThe Coulomb interaction between a photoelectron and its parent ion plays an important role in a large range of light-matter interactions. In this paper we obtain a direct insight into the Coulomb interaction and resolve, for the first time, the phase accumulated by the laser-driven electron as it interacts with the Coulomb potential. Applying extreme-ultraviolet interferometry enables us to resolve this phase with attosecond precision over a large energy range. Our findings identify a strong laser-Coulomb coupling, going beyond the standard recollision picture within the strong-field framework. Transformation of the results to the time domain reveals Coulomb-induced delays of the electrons along their trajectories, which vary by tens of attoseconds with the laser field intensity.
- ItemStructural relaxation phenomena in silicate glasses modified by irradiation with femtosecond laser pulses(London : Nature Publishing Group, 2017) Seuthe, Thomas; Mermillod-Blondin, Alexandre; Grehn, Moritz; Bonse, Jörn; Wondraczek, Lothar; Eberstein, MarkusStructural relaxation phenomena in binary and multicomponent lithium silicate glasses were studied upon irradiation with femtosecond (fs) laser pulses (800 nm central wavelength, 130 fs pulse duration) and subsequent thermal annealing experiments. Depending on the annealing temperature, micro-Raman spectroscopy analyses evidenced different relaxation behaviours, associated to bridging and non-bridging oxygen structures present in the glass network. The results indicate that the mobility of lithium ions is an important factor during the glass modification with fs-laser pulses. Quantitative phase contrast imaging (spatial light interference microscopy) revealed that these fs-laser induced structural modifications are closely related to local changes in the refractive index of the material. The results establish a promising strategy for tailoring fs-laser sensitivity of glasses through structural mobility.
- ItemPhonon anharmonicities and ultrafast dynamics in epitaxial Sb2Te3([London] : Macmillan Publishers Limited, part of Springer Nature, 2020) Bragaglia, V.; Ramsteiner, M.; Schick, D.; Boschker, J.E.; Mitzner, R.; Calarco, R.; Holldack, K.In this study we report on the investigation of epitaxially grown Sb2Te3 by employing Fourier-Transform transmission Spectroscopy (FTS) with laser-induced Coherent Synchrotron Radiation (CSR) in the Terahertz (THz) spectral range. Static spectra in the range between 20 and 120 cm−1 highlight a peculiar softening of an in-plane IR-active phonon mode upon temperature decrease, as opposed to all Raman active modes which instead show a hardening upon temperature decrease in the same energy range. The phonon mode softening is found to be accompanied by an increase of free carrier concentration. A strong coupling of the two systems (free carriers and phonons) is observed and further evidenced by exciting the same phonon mode at 62 cm−1 within an ultrafast pump-probe scheme employing a femtosecond laser as pump and a CSR single cycle THz pulse as probe. Separation of the free carrier contribution and the phonon resonance in the investigated THz range reveals that, both damping of the phonon mode and relaxation of hot carriers in the time domain happen on the same time scale of 5 ps. This relaxation is about a factor of 10 slower than expected from the Lorentz time-bandwidth limit. The results are discussed in the framework of phonon scattering at thermal and laser induced transient free carriers.
- ItemGeneration and collective interaction of giant magnetic dipoles in laser cluster plasma([London] : Macmillan Publishers Limited, part of Springer Nature, 2021) Andreev, A.; Platonov, K.; Lécz, Z.; Hafz, N.Interaction of circularly polarized laser pulses with spherical nano-droplets generates nanometer-size magnets with lifetime on the order of hundreds of femtoseconds. Such magnetic dipoles are close enough in a cluster target and magnetic interaction takes place. We investigate such system of several magnetic dipoles and describe their rotation in the framework of Lagrangian formalism. The semi-analytical results are compared to particle-in-cell simulations, which confirm the theoretically obtained terrahertz frequency of the dipole oscillation.
- ItemTowards shot-noise limited diffraction experiments with table-top femtosecond hard x-ray sources(Melville, NY : AIP Publishing LLC, 2017) Holtz, Marcel; Hauf, Christoph; Weisshaupt, Jannick; Salvador, Antonio-Andres Hernandez; Woerner, Michael; Elsaesser, ThomasTable-top laser-driven hard x-ray sources with kilohertz repetition rates are an attractive alternative to large-scale accelerator-based systems and have found widespread applications in x-ray studies of ultrafast structural dynamics. Hard x-ray pulses of 100 fs duration have been generated at the Cu Kα wavelength with a photon flux of up to 109 photons per pulse into the full solid angle, perfectly synchronized to the sub- 100-fs optical pulses from the driving laser system. Based on spontaneous x-ray emission, such sources display a particular noise behavior which impacts the sensitivity of x-ray diffraction experiments. We present a detailed analysis of the photon statistics and temporal fluctuations of the x-ray flux, together with experimental strategies to optimize the sensitivity of optical pump/x-ray probe experiments. We demonstrate measurements close to the shot-noise limit of the x-ray source.
- ItemA liquid flatjet system for solution phase soft-x-ray spectroscopy(Melville, NY : AIP Publishing LLC, 2015) Ekimova, Maria; Quevedo, Wilson; Faubel, Manfred; Wernet, Philippe; Nibbering, Erik T. J.We present a liquid flatjet system for solution phase soft-x-ray spectroscopy. The flatjet set-up utilises the phenomenon of formation of stable liquid sheets upon collision of two identical laminar jets. Colliding the two single water jets, coming out of the nozzles with 50 μm orifices, under an impact angle of 48° leads to double sheet formation, of which the first sheet is 4.6 mm long and 1.0 mm wide. The liquid flatjet operates fully functional under vacuum conditions (<10(-3) mbar), allowing soft-x-ray spectroscopy of aqueous solutions in transmission mode. We analyse the liquid water flatjet thickness under atmospheric pressure using interferomeric or mid-infrared transmission measurements and under vacuum conditions by measuring the absorbance of the O K-edge of water in transmission, and comparing our results with previously published data obtained with standing cells with Si3N4 membrane windows. The thickness of the first liquid sheet is found to vary between 1.4-3 μm, depending on the transverse and longitudinal position in the liquid sheet. We observe that the derived thickness is of similar magnitude under 1 bar and under vacuum conditions. A catcher unit facilitates the recycling of the solutions, allowing measurements on small sample volumes (∼10 ml). We demonstrate the applicability of this approach by presenting measurements on the N K-edge of aqueous NH4 (+). Our results suggest the high potential of using liquid flatjets in steady-state and time-resolved studies in the soft-x-ray regime.
- ItemMulti-color imaging of magnetic Co/Pt heterostructures(Melville, NY : AIP Publishing LLC, 2017) Willems, Felix; von Korff Schmising, Clemens; Weder, David; Günther, Christian M.; Schneider, Michael; Pfau, Bastian; Meise, Sven; Guehrs, Erik; Geilhufe, Jan; Merhe, Alaa El Din; Jal, Emmanuelle; Vodungbo, Boris; Lüning, Jan; Mahieu, Benoit; Capotondi, Flavio; Pedersoli, Emanuele; Gauthier, David; Manfredda, Michele; Eisebitt, StefanWe present an element specific and spatially resolved view of magnetic domainsin Co/Pt heterostructures in the extreme ultraviolet spectral range. Resonantsmall-angle scattering and coherent imaging with Fourier-transform holographyreveal nanoscale magnetic domain networks via magnetic dichroism of Co at theM2,3 edges as well as via strong dichroic signals at the O2,3 and N6,7 edges of Pt.We demonstrate for the first time simultaneous, two-color coherent imaging at afree-electron laser facility paving the way for a direct real space access toultrafast magnetization dynamics in complex multicomponent material systems.