Light Source Free Electron Laser Research Articles

Focal shift induced by source displacements and optical figure errors.

In this work the longitudinal shifts of the focal plane of an ellipsoidal mirror induced by longitudinal shifts of the source and by the optical figure error of the mirror itself are investigated. The case of an ideal mirror illuminated by a Gaussian beam is considered first, deriving an analytical formula predicting the source-to-focus shift. Then the realistic case of a mirror affected by surface shape defects is examined, by taking into account metrological data and numerically solving the Huygens-Fresnel integral. The analytical and numerical solutions in the ideal and real cases are compared. Finally, it is shown that an additional dependence of the focal shift is introduced on the wavelength and the pointing angle of the source. Both effects are investigated by numerical computations. We limit the treatment in the XUV spectral range, choosing as a test bench the Kirkpatrick-Baez mirror system of the DiProI and LDM end-stations and at the FERMI seeded free-electron laser (FEL). The work is primarily aimed at disentangling the different causes of focal shift at FEL light sources, where source position, wavelength and pointing angle are either tunable or rapidly fluctuating. The method can be easily extended to parabolic reflectors and refractors (lenses) with other kinds of illuminating sources and wavelengths.

Harmonic Generation in Planar Undulators in Single-Pass Free Electron Lasers

The paper presents a theoretical study of the harmonic power evolution in a single-pass free-electron laser (FEL) and a comparison with some of the experimental results. The phenomenological approach which considers the main FEL parameters (current density, the Lorentz factor, electron energy spread, and the beam geometry) provides a description of any undulator. With due regard to the real laser beam parameters, the effect from high-order harmonic radiation and the beam deviation from the undulator axis on the FEL irradiation is investigated. The Bessel coefficients are calculated for the undulator in the presence of the second periodic field. The phenomenological approach provides the free-electron laser simulation experiments at Sorgente Pulsata Auto-amplificata di Radiazione Coerente (SPARC), SPring-8 Angstrom Compact Free-Electron Laser (SACLA) and Linac Coherent Light Source (LCLS). These studies include the high-harmonic generation, a comparison of the emission power evolution with the experimentally obtained data on the harmonic generation including even and odd high-order harmonics, gain and saturation lengths and the respective power. A possible effect from the third harmonic of the planar undulator magnetic field is studied in relation to the FEL irradiation. It is shown that this effect is insignificant even at the magnetic-field harmonic amplitude equaling ~1/10 of the amplitude of the ideal magnetic field in the periodic undulator. It is found that the second-harmonic generation in FEL lasing is rather weak, that is in good agreement with the measurement results as well as the behavior of the high-order harmonics.

Stitching techniques for measuring X-ray synchrotron mirror topography.

Optical metrology and polishing techniques are continuously evolving to satisfy the increasingly stringent specifications required for X-ray optical components for synchrotron and free-electron laser light source beamlines. For both spherical and aspherical geometries, the most demanding applications may have target residual figure errors close to 1 nm. To achieve such specifications and maintain them in the optomechanical mount, it is critical to develop methods capable of measuring the topography of the optical surface over the clear aperture of the mirror. The European Synchrotron Radiation Facility optical metrology laboratory has developed a stitching tool initially aimed at measuring long flat mirrors up to 1 m long with a Fizeau interferometer. The system is routinely used providing 2D maps of the optical surface. The instrument capabilities have been extended to characterize moderately curved optics using a transmission flat element, and results obtained on a high quality spherical mirror with 120 m of radius of curvature are presented. As a novel approach of stitching application, the technique has been used to improve the measurement accuracy of the Fizeau interferometer when measuring short plane mirrors. Acquisition of 2D topographies on a short plane mirror by micro-stitching interferometry is also presented and discussed.

The Percival 2-Megapixel monolithic active pixel imager

The peak brilliance reached by today's Free-Electron Laser and Synchrotron light sources requires photon detectors matching their output intensity and other characteristics in order to fully realize the sources' potential. The Pixellated Energy Resolving CMOS Imager, Versatile And Large (Percival) is a dedicated soft X-ray imager (0.25–1 keV) developed for this purpose by a collaboration of DESY, Rutherford Appleton Laboratory/STFC, Elettra Sincrotrone Trieste, Diamond Light Source, and Pohang Accelerator Laboratory. Following several generations of prototypes, the Percival “P2M” 2-Megapixel imager—a 4.5×5 cm monolithic, stitched sensor with an uninterrupted imaging area of 4×4 cm2 (1408×1484 pixels of 27×27 μm—was produced and has demonstrated basic functionality with a first-light image using visible light. It is currently being brought to full operation in a front-illuminated configuration. The readout system being commissioned in parallel has been developed specifically for this imager which will produce—at full 300 Hz frame rate—data at 20 Gbit/s. A first wafer with eight Percival P2M chips has undergone backthinning to enable soft X-ray detection. It has been diced and chips are currently being wirebonded. We summarize here the P2M system, the project status, and show the P2M sensor's first response to visible light.

A convolutional neural network-based screening tool for X-ray serial crystallography.

A new tool is introduced for screening macromolecular X-ray crystallography diffraction images produced at an X-ray free-electron laser light source. Based on a data-driven deep learning approach, the proposed tool executes a convolutional neural network to detect Bragg spots. Automatic image processing algorithms described can enable the classification of large data sets, acquired under realistic conditions consisting of noisy data with experimental artifacts. Outcomes are compared for different data regimes, including samples from multiple instruments and differing amounts of training data for neural network optimization.

Generation and characterization of ultrathin free-flowing liquid sheets

The physics and chemistry of liquid solutions play a central role in science, and our understanding of life on Earth. Unfortunately, key tools for interrogating aqueous systems, such as infrared and soft X-ray spectroscopy, cannot readily be applied because of strong absorption in water. Here we use gas-dynamic forces to generate free-flowing, sub-micron, liquid sheets which are two orders of magnitude thinner than anything previously reported. Optical, infrared, and X-ray spectroscopies are used to characterize the sheets, which are found to be tunable in thickness from over 1 μm down to less than 20 nm, which corresponds to fewer than 100 water molecules thick. At this thickness, aqueous sheets can readily transmit photons across the spectrum, leading to potentially transformative applications in infrared, X-ray, electron spectroscopies and beyond. The ultrathin sheets are stable for days in vacuum, and we demonstrate their use at free-electron laser and synchrotron light sources.

The LAMP instrument at the Linac Coherent Light Source free-electron laser.

The Laser Applications in Materials Processing (LAMP) instrument is a new end-station for soft X-ray imaging, high-field physics, and ultrafast X-ray science experiments that is available to users at the Linac Coherent Light Source (LCLS) free-electron laser. While the instrument resides in the Atomic, Molecular and Optical science hutch, its components can be used at any LCLS beamline. The end-station has a modular design that provides high flexibility in order to meet user-defined experimental requirements and specifications. The ultra-high-vacuum environment supports different sample delivery systems, including pulsed and continuous atomic, molecular, and cluster jets; liquid and aerosols jets; and effusive metal vapor beams. It also houses movable, large-format, high-speed pnCCD X-ray detectors for detecting scattered and fluorescent photons. Multiple charged-particle spectrometer options are compatible with the LAMP chamber, including a double-sided spectrometer for simultaneous and even coincident measurements of electrons, ions, and photons produced by the interaction of the high-intensity X-ray beam with the various samples. Here we describe the design and capabilities of the spectrometers along with some general aspects of the LAMP chamber and show some results from the initial instrument commissioning.

Infrared nanoscopy down to liquid helium temperatures.

We introduce a scattering-type scanning near-field infrared microscope (s-SNIM) for the local scale near-field sample analysis and spectroscopy from room temperature down to liquid helium (LHe) temperature. The extension of s-SNIM down to T = 5 K is in particular crucial for low-temperature phase transitions, e.g., for the examination of superconductors, as well as low energy excitations. The low temperature (LT) s-SNIM performance is tested with CO2-IR excitation at T = 7 K using a bare Au reference and a structured Si/SiO2-sample. Furthermore, we quantify the impact of local laser heating under the s-SNIM tip apex by monitoring the light-induced ferroelectric-to-paraelectric phase transition of the skyrmion-hosting multiferroic material GaV4S8 at Tc = 42 K. We apply LT s-SNIM to study the spectral response of GaV4S8 and its lateral domain structure in the ferroelectric phase by the mid-IR to THz free-electron laser-light source FELBE at the Helmholtz-Zentrum Dresden-Rossendorf, Germany. Notably, our s-SNIM is based on a non-contact atomic force microscope (AFM) and thus can be complemented in situ by various other AFM techniques, such as topography profiling, piezo-response force microscopy (PFM), and/or Kelvin-probe force microscopy (KPFM). The combination of these methods supports the comprehensive study of the mutual interplay in the topographic, electronic, and optical properties of surfaces from room temperature down to 5 K.

Measurement of transformer ratio from ramped beams in the blowout regime

We present the plans for a UCLA-Argonne collaborative plasma wakefield acceleration (PWFA) experiment aimed at demonstrating the dependence of transformer ratio – the relation between maximum acceleration observed in a plasma wake to the maximum deceleration of the driving beam – on beam shape. Utilizing the unique capabilities of the emittance exchange (EEX) beamline, we may obtain transformer ratios in excess of six in a 120 MeV/m PWFA. These experiments are a crucial step in enabling applications ranging from compact X-ray free electron laser (FEL) light sources to TeV-class linear colliders for high energy physics.

Characterisation of Redlen high-flux CdZnTe

CdZnTe is a promising material for the current generation of free electron laser light sources and future laser-driven γ-ray sources which require detectors capable of high flux imaging at X-ray and γ-ray energies (> 10 keV) . However, at high fluxes CdZnTe has been shown to polarise due to hole trapping, leading to poor performance. Novel Redlen CdZnTe material with improved hole transport properties has been designed for high flux applications. Small pixel CdZnTe detectors were fabricated by Redlen Technologies and flip-chip bonded to PIXIE ASICs. An XIA Digital Gamma Finder PIXIE-16 system was used to digitise each of the nine analogue signals with a timing resolution of 10 ns. Pulse shape analysis was used to extract the rise times and amplitude of signals. These were measured as a function of applied bias voltage and used to calculate the mobility (μ) and mobility-lifetime (μτ) of electrons and holes in the material for three identical detectors. The measured values of the transport properties of electrons in the high-flux-capable material was lower than previously reported for Redlen CdZnTe material (μeτe ∼ 1 × 10−3 cm2V−1 and μe ∼ 1000 cm2V−1s−1) while the hole transport properties were found to have improved (μhτh ∼ 3 × 10−4 cm2V−1 and μh ∼ 100 cm2V−1s−1).

How Cubic Can Ice Be?

Using an X-ray laser, we investigated the crystal structure of ice formed by homogeneous ice nucleation in deeply supercooled water nanodrops (r ≈ 10 nm) at ∼225 K. The nanodrops were formed by condensation of vapor in a supersonic nozzle, and the ice was probed within 100 μs of freezing using femtosecond wide-angle X-ray scattering at the Linac Coherent Light Source free-electron X-ray laser. The X-ray diffraction spectra indicate that this ice has a metastable, predominantly cubic structure; the shape of the first ice diffraction peak suggests stacking-disordered ice with a cubicity value, χ, in the range of 0.78 ± 0.05. The cubicity value determined here is higher than those determined in experiments with micron-sized drops but comparable to those found in molecular dynamics simulations. The high cubicity is most likely caused by the extremely low freezing temperatures and by the rapid freezing, which occurs on a ∼1 μs time scale in single nanodroplets.

Start-to-end simulation of the shot-noise driven microbunching instability experiment at the Linac Coherent Light Source

The shot-noise driven microbunching instability can significantly degrade electron beam quality in x-ray free electron laser light sources. Experiments were carried out at the Linac Coherent Light Source (LCLS) to study this instability. In this paper, we present start-to-end simulations of the shot-noise driven microbunching instability experiment at the LCLS using the real number of electrons. The simulation results reproduce the measurements quite well. A microbunching self-heating mechanism is also illustrated in the simulation, which helps explain the experimental observation.

Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses

New x-ray free electron laser (XFEL) and high harmonic generation (HHG) light sources are capable of generating short and intense pulses that make x-ray nonlinear spectroscopy possible. Multidimensional spectroscopic techniques, which have long been used in the nuclear magnetic resonance, infrared, and optical regimes to probe the electronic structure and nuclear dynamics of molecules by sequences of short pulses with variable delays, can thus be extended to the attosecond x-ray regime. This opens up the possibility of probing core-electronic structure and couplings, the real-time tracking of impulsively created valence-electronic wavepackets and electronic coherences, and monitoring ultrafast processes such as nonadiabatic electron-nuclear dynamics near conical-intersection crossings. We survey various possible types of multidimensional x-ray spectroscopy techniques and demonstrate the novel information they can provide about molecules.

A liquid jet setup for x-ray scattering experiments on complex liquids at free-electron laser sources.

In this paper we describe a setup for x-ray scattering experiments on complex fluids using a liquid jet. The setup supports Small and Wide Angle X-ray Scattering (SAXS/WAXS) geometries. The jet is formed by a gas-dynamic virtual nozzle (GDVN) allowing for diameters ranging between 1 μm and 20 μm at a jet length of several hundred μm. To control jet properties such as jet length, diameter, or flow rate, the instrument is equipped with several diagnostic tools. Three microscopes are installed to quantify jet dimensions and stability in situ. The setup has been used at several beamlines performing both SAXS and WAXS experiments. As a typical example we show an experiment on a colloidal dispersion in a liquid jet at the X-ray Correlation Spectroscopy instrument at the Linac Coherent Light Source free-electron laser.

Two mirror X-ray pulse split and delay instrument for femtosecond time resolved investigations at the LCLS free electron laser facility.

We built a two-mirror based X-ray split and delay (XRSD) device for soft X-rays at the Linac Coherent Light Source free electron laser facility. The instrument is based on an edge-polished mirror design covering an energy range of 250 eV-1800 eV and producing a delay between the two split pulses variable up to 400 femtoseconds with a sub-100 attosecond resolution. We present experimental and simulation results regarding molecular dissociation dynamics in CH3I and CO probed by the XRSD device. We observed ion kinetic energy and branching ratio dependence on the delay times which were reliably produced by the XRSD instrument.

Charge transfer in dissociating iodomethane and fluoromethane molecules ionized by intense femtosecond X-ray pulses.

Ultrafast electron transfer in dissociating iodomethane and fluoromethane molecules was studied at the Linac Coherent Light Source free-electron laser using an ultraviolet-pump, X-ray-probe scheme. The results for both molecules are discussed with respect to the nature of their UV excitation and different chemical properties. Signatures of long-distance intramolecular charge transfer are observed for both species, and a quantitative analysis of its distance dependence in iodomethane is carried out for charge states up to I21+. The reconstructed critical distances for electron transfer are in good agreement with a classical over-the-barrier model and with an earlier experiment employing a near-infrared pump pulse.

Rate equations for nitrogen molecules in ultrashort and intense x-ray pulses

We study theoretically the quantum dynamics of nitrogen molecules (N2) exposed to intense and ultrafast x-rays at a wavelength of ( photon energy) from the Linac Coherent Light Source (LCLS) free electron laser. Molecular rate equations are derived to describe the intertwined photoionization, decay, and dissociation processes occurring for N2. This model complements our earlier phenomenological approaches, the single-atom, symmetric-sharing, and fragmentation-matrix models of 2012 (J. Chem. Phys. 136 214310). Our rate-equations are used to obtain the effective pulse energy at the sample and the time scale for the dissociation of the metastable dication . This leads to a very good agreement between the theoretically and experimentally determined ion yields and, consequently, the average charge states. The effective pulse energy is found to decrease with shortening pulse duration. This variation together with a change in the molecular fragmentation pattern and frustrated absorption—an effect that reduces absorption of x-rays due to (double) core hole formation—are the causes for the drop of the average charge state with shortening LCLS pulse duration discovered previously.

Molecular dynamics induced by short and intense x-ray pulses from the LCLS

The past six years have led to a wealth of experimental and theoretical data revealing the nature of the interaction between gas-phase molecules and short and intense x-ray pulses, from the Linac coherent light source free electron laser (FEL). We present here a few highlights that describe some of the first photoabsorption measurements of gas-phase molecules. In particular, we report on a three decades long prediction of single-site double core holes (ss-DCH) and two-site double core holes (ts-DCH) in diatomic and triatomic molecules. We also describe recent measurements that validate a simple theory regarding femtosecond intense x-ray induced fragmentation dynamics of C60 as well as photoabsorption measurements of encapsulated fullerenes, Ho3N@C80. The latter investigation opens the way for even more complex molecular studies with FELs. In all of the described highlights, working in close collaboration with theorists enabled the interpretation of, or predicted our measurements, and in some cases our experiments guided the modeling. We conclude this article by describing the potential of new instrumentation for chemical and biological sciences especially in light of new or improved FELs.

Narrow-band near-field nanoscopy in the spectral range from 1.3 to 8.5 THz

Nano-spectroscopy in the terahertz frequency range remains challenging despite recent technological progress in developing both THz emitter sources and near-field optical microscopy (SNOM). Here, we combine scattering-type SNOM with a free-electron laser light source, to tune into the 1.3–8.5 THz range. A significant portion of this range, namely, the frequencies above ∼3 THz, is not covered by previously reported near-field microscopy systems. However, it constitutes an indispensable regime where many elementary processes in solids including collective lattice excitations, charge, and spin transport occur. Our approach of nano-spectroscopy and nano-imaging provides a versatile analysis of nanostructures as small as 50 nm, hence beating the optical diffraction limit by λ/4600.

Coulomb frustration of the multiphoton ionization of metallic clusters under intense EUV FEL evidenced by ion spectrometry

Free electron laser light sources delivering high intensity pulses of short wavelength radiation are opening novel possibilities for the investigation of matter at the nanoscale and for the discovery and understanding of new physical processes occurring at the exotic transient states they make accessible. Strong ionization of atomic constituents of a nano-sized sample is a representative example of such processes and the understanding of ionization dynamics is crucial for a realistic description of the experiments. We report here on multiple ionization experiments on free clusters of titanium, a high cohesive energy metal. The time of flight ion spectra reveal a saturation of the cluster ionization at ∼1016 photons per pulse per cm2. Our results also show a clear lack of any explosion process, opposite to what is observed for a rare-gas cluster under similar conditions. A simple and generalized multi-step ionization model including Coulomb frustration of the photoemission process effectively reproduces with a good agreement the main features of the experimental observation and points to an interpretation of the data involving a substantial energy deposition into the cluster through electronic system heating upon scattering events within photoemission.