Single-shot temporal characterization of XUV pulses with duration from ~10 fs to ~350 fs at FLASH

Ultra-short extreme ultraviolet pulses from the free-electron laser FLASH are characterized using terahertz-field driven streaking. Measurements at different ultra-short extreme ultraviolet wavelengths and pulse durations as well as numerical simulations were performed to explore the application range and accuracy of the method. For the simulation of streaking, a standard classical approach is used which is compared to quantum mechanical theory, based on strong field approximation. Various factors limiting the temporal resolution of the presented terahertz streaking setup are investigated and discussed. Special attention is paid to the cases of very short (similar to 10 fs) and long (up to similar to 350 fs) pulses.We want to acknowledge the work of the scientific and technical team at FLASH. NMK acknowledges the hospitality and financial support from DESY and from the theory group in cooperation with the SQS research group of the European XFEL (Hamburg). KW and MD acknowledge support by the SFB925-A1. UF and AD acknowledge support by the excellence cluster `The Hamburg Center for Ultrafast Imaging-Structure, Dynamics and Control of Matter at the Atomic Scale' (DFG)-EXC 1074 project ID 194651731. SW acknowledges support by the DFG Forschergruppe FOR 1789. Editoria

Ultrafast dynamics in (TaSe4)2I triggered by valence and core-level excitation

Dimensionality plays a key role in the emergence of ordered phases, such as charge density-waves (CDW), which can couple to, and modulate, the topological properties of matter. In this work, we study the out-of-equilibrium dynamics of the paradigmatic quasi-one-dimensional material (TaSe4)2I, which exhibits a transition into an incommensurate CDW phase when cooled to just below room temperature, namely at TCDW = 263 K. We make use of both optical laser and free-electron laser (FEL) based time-resolved spectroscopies in order to study the effect of a selective excitation on the normal-state and on the CDW phases by probing the near-infrared/visible optical properties both along and perpendicularly to the direction of the CDW, where the system is metallic and insulating, respectively. Excitation of the core-levels by ultrashort X-ray FEL pulses at 47 eV and 119 eV induces reflectivity transients resembling those recorded when only exciting the valence band of the compound - by near-infrared pulses at 1.55 eV - in the case of the insulating sub-system. Conversely, the metallic sub-system displays relaxation dynamics which depend on the energy of photo-excitation. Moreover, excitation of the CDW amplitude mode is recorded only for excitation at a low-photon-energy. This fact suggests that the coupling of light to ordered states of matter can predominantly be achieved when directly injecting delocalized carriers in the valence band, rather than localized excitations in the core levels. Complementing this, table-top experiments allow us to prove the quasi-unidirectional nature of the CDW phase in (TaSe4)2I, whose fingerprints are detected along its c-axis only. Our results provide new insights into the symmetry of the ordered phase of (TaSe4)2I perturbed by a selective excitation, and suggest a novel approach based on complementary table-top and FEL spectroscopies for the study of complex materials

Terahertz-wave decoding of femtosecond extreme-ultraviolet light pulses

In recent years, femtosecond extreme-ultraviolet (XUV) and x-ray pulses from free-electron lasers have developed into important probes to monitor processes and dynamics in matter on femtosecond-time and angstrom-length scales. With the rapid progress of versatile ultrafast x-ray spectroscopy techniques and more sophisticated data analysis tools, accurate single-pulse information on the arrival time, duration, and shape of the probing x-ray and XUV pulses becomes essential. Here, we demonstrate that XUV pulses can be converted into terahertz electromagnetic pulses using a spintronic terahertz emitter. We observe that the duration, arrival time, and energy of each individual XUV pulse is encoded in the waveform of the associated terahertz pulses, and thus can be readily deduced from single-shot terahertz time-domain detection

Transient EUV Reflectivity Measurements of Carbon upon Ultrafast Laser Heating

Time resolved extreme ultraviolet (EUV) transient reflectivity measurements on non-equilibrium amorphous carbon (a-C) have been carried out by combining optical and free electron laser (FEL) sources. The EUV probing was specifically sensitive to lattice dynamics, since the EUV reflectivity is essentially unaffected by the photo-excited surface plasma. Data have been interpreted in terms of the dynamics of an expanding surface, i.e., a density gradient rapidly forming along the normal surface. This allowed us to determine the characteristic time ( τ ≲ 1 ps) for hydrodynamic expansion in photo-excited a-C. This finding suggests an extremely narrow time window during which the system can be assumed to be in the isochoric regime, a situation that may complicate the study of photo-induced metastable phases of carbon. Data also showed a weak dependence on the probing EUV wavelength, which was used to estimate the electronic temperature ( T e ≈ 0.8 eV) of the excited sample. This experimental finding compares fairly well with the results of calculations, while a comparison of our data and calculations with previous transient optical reflectivity measurements highlights the complementarities between optical and EUV probing

Free Electron Laser Measurement of Liquid Carbon Reflectivity in the Extreme Ultraviolet

Ultrafast time-resolved extreme ultraviolet (EUV) reflectivity measurements of optically pumped amorphous carbon (a-C) have been performed with the FERMI free electron laser (FEL). This work extends the energy range used in previous reflectivity studies and adds polarization dependence. The EUV probe is known to be sensitive to lattice dynamics, since in this range the reflectivity is essentially unaffected by the photo-excited surface plasma. The exploitation of both s- and p-polarized EUV radiation permits variation of the penetration depth of the probe; a significant increase in the characteristic time is observed upon increasing the probing depth (1 vs. 5 ps) due to hydrodynamic expansion and consequent destruction of the excited region, implying that there is only a short window during which the probed region is in the isochoric regime. A weak wavelength dependence of the reflectivity is found, consistent with previous measurements and implying a maximum electronic temperature of 0.8 eV ± 0.4

Multimodal near-infrared-emitting PluS Silica nanoparticles with fluorescent, photoacoustic, and photothermal capabilities

Purpose: The aim of the present study was to develop nanoprobes with theranostic features, including \u2013 at the same time \u2013 photoacoustic, near-infrared (NIR) optical imaging, and photothermal properties, in a versatile and stable core\u2013shell silica-polyethylene glycol (PEG) nanoparticle architecture. Materials and methods: We synthesized core\u2013shell silica-PEG nanoparticles by a one-pot direct micelles approach. Fluorescence emission and photoacoustic and photothermal properties were obtained at the same time by appropriate doping with triethoxysilane-derivatized cyanine 5.5 (Cy5.5) and cyanine 7 (Cy7) dyes. The performances of these nanoprobes were measured in vitro, using nanoparticle suspensions in phosphate-buffered saline and blood, dedicated phantoms, and after incubation with MDA-MB-231 cells. Results: We obtained core\u2013shell silica-PEG nanoparticles endowed with very high colloidal stability in water and in biological environment, with absorption and fluorescence emission in the NIR field. The presence of Cy5.5 and Cy7 dyes made it possible to reach a more reproducible and higher doping regime, producing fluorescence emission at a single excitation wavelength in two different channels, owing to the energy transfer processes within the nanoparticle. The nanoarchitecture and the presence of both Cy5.5 and Cy7 dyes provided a favorable agreement between fluorescence emission and quenching, to achieve optical imaging and photoacoustic and photothermal properties. Conclusion: We obtained rationally designed nanoparticles with outstanding stability in biological environment. At appropriate doping regimes, the presence of Cy5.5 and Cy7 dyes allowed us to tune fluorescence emission in the NIR for optical imaging and to exploit quenching processes for photoacoustic and photothermal capabilities. These nanostructures are promising in vivo theranostic tools for the near future

Toward an integrated device for spatiotemporal superposition of free-electron lasers and laser pulses

Free-electron lasers (FELs) currently represent a step forward on time-resolved investigations on any phase of matter through pump-probe methods involving FELs and laser beams. That class of experiments requires an accurate spatial and temporal superposition of pump and probe beams on the sample, which at present is still a critical procedure. More efficient approaches are demanded to quickly achieve the superposition and synchronization of the beams. Here, we present what we believe is a novel technique based on an integrated device allowing the simultaneous characterization and the fast spatial and temporal overlapping of the beams, reducing the alignment procedure from hours to minutes

Research data: Terahertz-wave decoding of femtosecond extreme-ultraviolet light pulses

This repository entry contains the research data used for generating the publication "Terahertz-wave decoding of femtosecond extreme-ultraviolet light pulses"

Media 1: Towards jitter-free pump-probe measurements at seeded free electron laser facilities

Originally published in Optics Express on 02 June 2014 (oe-22-11-12869