Search

We present the first lasing results of SwissFEL, a hard X-ray free-electron laser (FEL) that recently came into operation at the Paul Scherrer Institute in Switzerland. SwissFEL is a very stable, compact and cost-effective X-ray FEL facility driven by a low-energy and ultra-low-emittance electron beam travelling through short-period undulators. It delivers stable hard X-ray FEL radiation at 1-A wavelength with pulse energies of more than 500 μJ, pulse durations of ~30 fs (root mean square) and spectral bandwidth below the per-mil level. Using special configurations, we have produced pulses shorter than 1 fs and, in a different set-up, broadband radiation with an unprecedented bandwidth of ~2%. The extremely small emittance demonstrated at SwissFEL paves the way for even more compact and affordable hard X-ray FELs, potentially boosting the number of facilities worldwide and thereby expanding the population of the scientific community that has access to X-ray FEL radiation. The first lasing results at SwissFEL, an X-ray free-electron laser, are presented, highlighting the facility’s unique capabilities. A general comparison to other major facilities is also provided.

Long-wavelength pulses from the Swiss X-ray free-electron laser (XFEL) have been used for de novo protein structure determination by native single-wavelength anomalous diffraction (native-SAD) phasing of serial femtosecond crystallography (SFX) data. In this work, sensitive anomalous data-quality indicators and model proteins were used to quantify improvements in native-SAD at XFELs such as utilization of longer wavelengths, careful experimental geometry optimization, and better post-refinement and partiality correction. Compared with studies using shorter wavelengths at other XFELs and older software versions, up to one order of magnitude reduction in the required number of indexed images for native-SAD was achieved, hence lowering sample consumption and beam-time requirements significantly. Improved data quality and higher anomalous signal facilitate so-far underutilized de novo structure determination of challenging proteins at XFELs. Improvements presented in this work can be used in other types of SFX experiments that require accurate measurements of weak signals, for example time-resolved studies., IUCrJ, 7 (6), ISSN:2052-2525

Optical-domain Transient Grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique used to probe vibrational, magnetic and electronic degrees of freedom in the time domain. The newly developed coherent X-ray Free Electron Laser sources allow its extension to the X-ray regime. Xrays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element-specificity can address core-excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. We demonstrate for the first time TG excitation in the hard X-ray range at 7.1 keV. In Bismuth Germanate (BGO), the nonresonant TG excitation generates coherent optical phonons detected as a function of time by diffraction of an optical probe pulse. This experiment demonstrates the ability to probe bulk properties of materials and paves the way for ultrafast coherent four-wave-mixing techniques using X-ray probes and involving nanoscale TG spatial periods., Comment: 11 pages, 4 figures

A multidisciplinary concept has been developed to compare advanced wastewater treatment processes for their efficacy of eliminating micropollutants and pathogens. The concept is based on (i) the removal/formation of selected indicator substances and their transformation products (TPs), (ii) the assessment of ecotoxicity via in vitro tests, and (iii) the removal of pathogens and antibiotic resistant bacteria. It includes substances passing biological wastewater treatment plants regulated or proposed to be regulated in the European Water Framework Directive, TPs formed in biological processes or during ozonation, agonistic/antagonistic endocrine activities, mutagenic/genotoxic activities, cytotoxic activities, further activities like neurotoxicity as well as antibiotics resistance genes, and taxonomic gene markers for pathogens. At a pilot plant, ozonation of conventionally treated wastewater resulted in the removal of micropollutants and pathogens and the reduction of estrogenic effects, whereas the in vitro mutagenicity increased. Subsequent post-treatment of the ozonated water by granular activated carbon (GAC) significantly reduced the mutagenic effects as well as the concentrations of remaining micropollutants, whereas this was not the case for biofiltration. The results demonstrate the suitability of the evaluation concept to assess processes of advanced wastewater treatment including ozonation and GAC by considering chemical, ecotoxicological, and microbiological parameters.

The extension of transient grating spectroscopy to the x-ray regime will create numerous opportunities, ranging from the study of thermal transport in the ballistic regime to charge, spin, and energy transfer processes with atomic spatial and femtosecond temporal resolution. Studies involving complicated split-and-delay lines have not yet been successful in achieving this goal. Here we propose a novel, simple method based on the Talbot effect for converging beams, which can easily be implemented at current x-ray free electron lasers. We validate our proposal by analyzing printed interference patterns on polymethyl methacrylate and gold samples using similar to 3 keV X-ray pulses. (C) 2019 Optical Society of America

Many of the scientific applications for X-ray free-electron lasers seek to exploit the ultrashort pulse durations of intense X-rays to obtain femtosecond time resolution of various processes in a “pump-probe” scheme. One of the limiting factors for such experiments is the timing jitter between the X-rays and ultrashort pulses from more conventional lasers operating at near-optical wavelengths. In this work, we investigate the potential of using X-ray-induced changes in the optical second harmonic generation efficiency of a nonlinear crystal to retrieve single-shot arrival times of X-ray pulses with respect to optical laser pulses. Our experimental results and simulations show changes to the efficiency of the second harmonic generation of 12%, approximately three times larger than the measured changes in the transmission of the 800 nm center-wavelength fundamental pulse. Further experiments showing even larger changes in the transmission of 400 nm center-wavelength pulses show that the mechanism of the second harmonic generation efficiency modulation is mainly the result of X-ray-induced changes in the linear absorption coefficients near 400 nm. We demonstrate and characterize a cross-correlation tool based on this effect in reference to a previously demonstrated method of X-ray/optical cross-correlation.

We investigate the excitation of coherent acoustic and optical phonons by ultrashort extreme ultraviolet (EUV) pulses produced by a free electron laser. Two crossed femtosecond EUV (wavelength 12.7 nm) pulses are used to excite coherent phonons at a wavelength of 280 nm, which are detected via diffraction of an optical probe beam. Longitudinal and surface acoustic waves are measured in BK-7 glass, diamond, and Bi4Ge3O12; in the latter material, the excitation of a coherent optical phonon mode is also observed. We discuss probing different acoustic modes in reflection and transmission geometries and frequency mixing of surface and bulk acoustic waves in the signal. The use of extreme ultraviolet radiation will allow the creation of tunable GHz to THz acoustic sources in any material without the need to fabricate transducer structures. The contribution by the MIT group was supported by the U.S. Department of Energy, Office of Basic Energy Sciences under Award No. DE-FG02-00ER15087. The JILA group graciously acknowledges support from the Department of Energy BES Award No. DE-FG02-99ER14982 and the Gordon and Betty Moore Foundation's EPiQS Initiative through Grant No. GBMF: 4538, and J.K. acknowledges support from an SRC Fellowship. The Elettra group acknowledges the European Research Council Grant No. 202804-TIMER. A.C. and T.F. acknowledge the Swiss NSF through the NCCR-MUST.

We report on the application of a short working distance von Hamos geometry spectrometer to measure the inelastic X-ray scattering (IXS) signals from solids and liquids. In contrast to typical IXS instruments where the spectrometer geometry is fixed and the incoming beam energy is scanned, the von Hamos geometry allows measurements to be made using a fixed optical arrangement with no moving parts. Thanks to the shot-to-shot capability of the spectrometer setup, we anticipate its application for the IXS technique at X-ray free electron lasers (XFELs). We discuss the capability of the spectrometer setup for IXS studies in terms of efficiency and required total incident photon flux for a given signal-to-noise ratio. The ultimate energy resolution of the spectrometer, which is a key parameter for IXS studies, was measured to the level of 150 meV at short crystal radius thanks to the application of segmented crystals for X-ray diffraction. The short working distance is a key parameter for spectrometer efficiency that is necessary to measure weak IXS signals.

The use of lasers to generate acoustic waves revolutionized the field of ultrasound and enabled numerous key developments in both fundamental research and applications. In the past decade, remarkable progress has been achieved in developing coherent sources of radiation operating in the extreme ultraviolet (EUV) and x-ray ranges, such as free electron lasers, which already yielded many breakthroughs in different fields of science. We expect that the field of ultrasonics will also greatly benefit from the availability of coherent EUV and x-ray sources. So far, a number of studies explored the use of coherent EUV and x-ray radiation for detection of acoustic waves. In this report, we describe the first experiment on the generation of surface and bulk acoustic waves in the tens of GHz range by EUV light.

The SwissFEL X-ray Free Electron Laser (XFEL) facility started construction at the Paul Scherrer Institute (Villigen, Switzerland) in 2013 and will be ready to accept its first users in 2018 on the Aramis hard X-ray branch. In the following sections we will summarize the various aspects of the project, including the design of the soft and hard X-ray branches of the accelerator, the results of SwissFEL performance simulations, details of the photon beamlines and experimental stations, and our first commissioning results.

The development of free electron laser (FEL) sources has provided an unprecedented bridge between the scientific communities working with ultrafast lasers and extreme ultraviolet (XUV) and X-ray radiation. Indeed, in recent years an increasing number of FEL-based applications have exploited methods and concepts typical of advanced optical approaches. In this context, we recently used a seeded FEL to demonstrate a four-wave-mixing (FWM) process stimulated by coherent XUV radiation, namely the XUV transient grating (X-TG). We hereby report on X-TG measurements carried out on a sample of silicon nitride (Si3N4). The recorded data bears evidence for two distinct signal decay mechanisms: one occurring on a sub-ps timescale and one following slower dynamics extending throughout and beyond the probed timescale range (100 ps). The latter is compatible with a slower relaxation (time decay > ns), that may be interpreted as the signature of thermal diffusion modes. From the peak intensity of the X-TG signal we could estimate a value of the effective third-order susceptibility which is substantially larger than that found in SiO2, so far the only sample with available X-TG data. Furthermore, the intensity of the time-coincidence peak shows a linear dependence on the intensity of the three input beams, indicating that the measurements were performed in the weak field regime. However, the timescale of the ultrafast relaxation exhibits a dependence on the intensity of the XUV radiation. We interpreted the observed behaviour as the generation of a population grating of free-electrons and holes that, on the sub-ps timescale, relaxes to generate lattice excitations. The background free detection inherent to the X-TG approach allowed the determination of FEL-induced electron dynamics with a sensitivity largely exceeding that of transient reflectivity and transmissivity measurements, usually employed for this purpose. This journal is © The Royal Society of Chemistry.

X-ray techniques have evolved over decades to become highly refined tools for a broad range of investigations. Importantly, these approaches rely on X-ray measurements that depend linearly on the number of incident X-ray photons. The advent of X-ray free electron lasers (XFELs) is opening the ability to reach extremely high photon numbers within ultrashort X-ray pulse durations and is leading to a paradigm shift in our ability to explore nonlinear X-ray signals. However, the enormous increase in X-ray peak power is a double-edged sword with new and exciting methods being developed but at the same time well-established techniques proving unreliable. Consequently, accurate knowledge about the threshold for nonlinear X-ray signals is essential. Herein we report an X-ray spectroscopic study that reveals important details on the thresholds for nonlinear X-ray interactions. By varying both the incident X-ray intensity and photon energy, we establish the regimes at which the simplest nonlinear process, two-photon X-ray absorption (TPA), can be observed. From these measurements we can extract the probability of this process as a function of photon energy and confirm both the nature and sub-femtosecond lifetime of the virtual intermediate electronic state., Scientific Reports, 6, ISSN:2045-2322

Simultaneous time and frequency detection in off-resonant femtosecond degenerate four-wave mixing (fs-DFWM) experiments displays spectral features that are covered in standard, nondispersed, frequency-integrated measurements. The application of laser fields with finite bandwidths, narrower than or comparable to the rotational Raman bands, affects the observed coherent signals. Information available from such experiments is split between the time and frequency domains and an improved measurement necessitates a combined detection. Rotational recurrences of oxygen (O2), measured by dispersed fs-DFWM at room temperature, exhibit spectral characteristics, using 800-nm laser pulses with ∼100 fs duration. Analysis of the detected signals in both dimensions incorporating temporal and spectral trends can assist in the extraction and interpretation of chemicophysical quantities from the experiment. The dispersed recurrent signals are in accordance with simulations. Copyright © 2011 John Wiley & Sons, Ltd.

The applicability of several femtosecond time resolved non-linear coherent techniques such as Raman induced polarization spectroscopy (RIPS), degenerate four-wave mixing (DFWM) and coherent anti-Stokes Raman spectroscopy (CARS) for molecular spectroscopy is presented. All methods rely on the initial coherent excitation of molecular states producing wavepackets, whose time evolution is then measured. In the case of RIPS and DFWM only pure rotational transitions are involved, whereas in CARS vibrational states can be excited. First the methodology of concentration and temperature measurements using RIPS in gas mixtures involving N2, CO2, O2, and N2O is shown. In addition some applications are given for the two closely related techniques DFWM and CARS. DFWM is suitable to extract the rotational constants of molecules to a high accuracy as is demonstrated by measurements on CO2 and pyrimidine, which is a biological building block. CARS can be used to study higher order molecular constants and to sensitively determine temperature in, e.g., H2 up to 2000 K. Finally, CARS is applied for the investigation of pressure dependent lineshape models, which are important for the temperature evaluation from spectroscopic data. To cite this article: B. Lavorel et al., C. R. Physique 5 (2004).

We show that the technique of femtosecond time-resolved coherent anti-Stokes Raman scattering (CARS) spectroscopy provides a powerful tool for the investigation of collision-induced linewidths and the validation of rotational energy transfer (RET) models. The fs-CARS method is applied to the N2–N2 collision system, and a comparison between the commonly used exponential gap (ECS-E), power gap (ECS-P), frequency corrected (EFCS), and the recently proposed angular momentum and energy corrected (AECS) variants of the ECS model is presented. As result we show that the AECS scaling law requires only two free parameters, and is appropriate for the determination of RET rates from the measured fs-CARS signals. The AECS model is also applied to the more complex C2H2–C2H2 collision system. As vibrational energy transfer and dephasing is not negligible in this case, the model has to be modified by introducing a vibrational relaxation factor. With this modification the fs-CARS signals from acetylene can be described s...

Knopp et al. [J. Raman Spectrosc. 31, 51 (2000)] have recently used resonant femtosecond coherent anti-Stokes Raman spectroscopy (CARS) to prepare and probe highly excited vibrational wave packets on the ground electronic potential surface of molecular iodine. The experiment uses a sequence of three resonant femtosecond pulses with two independently variable time delays. The first two pulses act as a pump and dump sequence to create a predefined, highly excited wave packet on the ground electronic state, whose amplitude is optimized by selecting the proper pump–dump (Raman) frequency difference and varying the time delay. The third pulse promotes the pump–dump wave packet to an excited electronic state, resulting in subsequent coherent emission of light at the anti-Stokes frequency. This fully-resonant CARS signal, measured as a function of time delay between the second and third pulses, oscillates at a frequency characteristic of the pump–dump wave packet. Due to anharmonicity, this frequency is a sensit...

Femtosecond time-delayed coherent anti-Stokes Raman scattering is presented not only as a tool for monitoring but also as a viable method for the preparation of vibrational wavepackets with very high quantum numbers in the ground electronic state of molecules. We experimentally demonstrate a particularly useful approach of using two separate time delays between the pulses for preparing vibrational wavepackets as high as v″=38 [ΔEv=7000 cm−1] in bulk gas-phase molecular iodine. By means of an ultrashort laser pulse, we prepare a wavepacket in an electronic excited state, optimize the frequency and timing of a second pulse to efficiently generate the targeted ground-state vibrational wavepacket, and monitor the wavepacket by coherent scattering from a third pulse. The method is further used to probe interference effects in femtosecond four-wave-mixing signals generated by molecular wavepackets.

Femtosecond time-resolved four-wave mixing (FWM) spectroscopy is performed using degenerate laser frequencies in order to investigate molecular dynamics in iodine molecules in the gas phase. It is demonstrated that by varying the timing as well as the wavenumber position for the signal detection different dynamics can be accessed. This is due to a selection of contributions (e.g. described by Feynman diagrams) to the nonlinear polarization of the process. The wave packet dynamics of the electronic excited B as well as the X ground state of iodine can be monitored by degenerate FWM, coherent anti-Stokes Raman scattering or coherent Stokes Raman scattering (CSRS) processes all included in the same experiment.

Femtosecond time-resolved coherent anti-Stokes Raman scattering (CARS) is applied in order to investigate molecular dynamics in the gas phase. As model system iodine vapour is chosen. By changing the timing of the laser pulses of this non-degenerate four-wave mixing technique, the wavepacket motion on both the electronically excited and the ground states can be detected as oscillations in the coherent anti-Stokes signal. Different decay times are found for the amplitudes of the excited and ground-state beats. The results are compared with transients obtained from a conventional pump-probe technique, where laser-induced fluorescence is used for detection.

Velocity map imaging (VMI) is used in mass spectrometry and in angle resolved photo-electron spectroscopy to determine the lateral momentum distributions of charged particles accelerated towards a detector. VM-images are composed of projected Newton spheres with a common centre. The 2D images are usually evaluated by a decomposition into base vectors each representing the 2D projection of a set of particles starting from a centre with a specific velocity distribution. We propose to evaluate 1D projections of VM-images in terms of 1D projections of spherical functions, instead. The proposed evaluation algorithm shows that all distribution information can be retrieved from an adequately chosen set of 1D projections, alleviating the numerical effort for the interpretation of VM-images considerably. The obtained results produce directly the coefficients of the involved spherical functions, making the reconstruction of sliced Newton spheres obsolete.

Field emitters are investigated for use as a low emittance electron gun. Two available field emitter technologies are currently explored; the field emitter arrays (FEAs) with individual focusing and single tip cathode with robust and fairly blunt apex. The challenge is to achieve several amperes of peak current without tip destructions. Very good cathode and environmental conditioning procedures with extremely short emission duration (ns) at low repetition rate (10 Hz) gave encouraging results to reach high peak current emission. For a free electron laser application, very short emission durations are preferred. Such operation regime should prevent the tip from overheating so that higher current densities could be reached. Another possible low emittance electron sources are single needle tips made from etched wires and which can be coated and formed in order to carry high current emission. One way to achieve short emission duration is to use pulsed laser light illuminating the tip while high electric field is applied.

The properties of the electron source define the ultimate limit of the beam quality in linear accelerators like Free Electron Lasers (FEL). The goal is to develop an electron gun delivering beam emittance lower than current state of the art. Such a gun should reduce the cost and size of an X-ray Free Electron Laser (XFEL). In this paper we present two concepts of field emitter cathodes which could potentially produce low emittance beam. The first challenging parameter for such cathode is to emit peak current as high as 5 A. This is the minimum current requirement for the XFEL concept from Paul Scherrer Institut.1 Maximum current of 0.12 A and 0.58 A have been reached respectively with field emitter arrays (FEA) and single needle cathodes. Laser assisted field emission gave encouraging results to reach even higher peak current and to pre-bunch the beam., 23 pages, 1 table, 9 figures Accepted for publication in JVST B

We report on the feasibility and expected performance of a sub-picosecond X-ray source at the Swiss Light Source (SLS), based on the electron-beam slicing method. This method has recently been demonstrated at the Advanced Light Source (ALS), using a bending magnet to produce ultrafast optical pulses. To improve the flux of such a source for user experiments, we have studied its realization both in the hard and soft X-ray regime, employing small gap insertion devices (IDs) installed either in one or in two successive straight sections. The most favourable geometry is one in which the modulator and the radiator are positioned in the same straight section of the storage ring.

The ultrafast dynamics of the second singlet electronically excited state (Ssub2/sub) in ethylbenzene has been studied by femtosecond time-resolved photoelectron imaging. The time evolution of the photoelectron signal can be well described by a biexponential decay: a rapid relaxation pathway with a time constant of 60 ( ± 9) fs and a longer-lived channel on a timescale of 2.58 ( ± 0.22) ps. The rapid relaxation is ascribed to the ultrafast internal conversion from the Ssub2/substate to the vibrationally hot Ssub1/substate. This internal conversion process has been observed in real time. The slow photoelectron signal reflects the depopulation of secondarily populated high vibronic Ssub1/substate.

We demonstrate the feasibility of the time-delayed femtosecond CARS (fs-CARS) technique in a dense gas environment. The experiments were performed on N2 molecules between 0.2 and 5 bar pressure. The method provides several advantages compared with its wavenumber-resolved counterpart, e.g. the possible separation of the non-resonant contributions to the signal, and is more suitable when the isolated lines approximations collapse and complex line mixing and energy transfer models have to be implemented in the signal description. The experimental results are in good agreement with theoretical considerations based on collision-induced rotational energy transfer (RET) models such as the common energy-corrected sudden approximation (ECS). Moreover, it is shown that the structure of the time-delayed signals is very sensitive to the applied pressures. Therefore, fs-CARS is an ideal supplementary tool for investigations of collision-induced spectroscopic effects, which are decisive for temperature and concentration determination in combustion processes. Copyright © 2002 John Wiley & Sons, Ltd.

We present an approach to determine the absolute thickness profile of flat liquid jets, which takes advantage of the information of thin film interference combined with light absorption, both captured in a single microscopic image. The feasibility of the proposed method is demonstrated on our compact experimental setup used to generate micrometer thin, free-flowing liquid jet sheets upon collision of two identical laminar cylindrical jets. Stable operation was achieved over several hours of the flat jet in vacuum (10-4 mbar), making the system ideally suitable for soft x-ray photon spectroscopy of liquid solutions. We characterize the flat jet size and thickness generated with two solvents, water and ethanol, employing different flow rates and nozzles of variable sizes. Our results show that a gradient of thickness ranging from a minimal thickness of 2 µm to over 10 µm can be found within the jet surface area. This enables the tunability of the sample thickness in situ, allowing the optimization of the transmitted photon flux for the chosen photon energy and sample. We demonstrate the feasibility of x-ray absorption spectroscopy experiments in transmission mode by measuring at the oxygen K-edge of ethanol. Our characterization method and the description of the experimental setup and its reported performance are expected to expand the range of applications and facilitate the use of flat liquid jets for spectroscopy experiments.